Engineering â€ș Electrical and Electronic Engineering

Organic Electronics and Photovoltaics

Description

This cluster of papers represents a collection of research on advances in organic solar cell technology, focusing on topics such as conjugated polymers, bulk heterojunction solar cells, efficiency enhancement, non-fullerene acceptors, solution processing, charge transport, morphology control, high-efficiency solar cells, and field-effect transistors.

Keywords

Conjugated Polymers; Bulk Heterojunction; Efficiency Enhancement; Non-Fullerene Acceptors; Solution Processing; Polymer Blends; Charge Transport; Morphology Control; High-Efficiency Solar Cells; Field-Effect Transistors

Fossil fuel alternatives, such as solar energy, are moving to the forefront in a variety of research fields. Polymer-based organic photovoltaic systems hold the promise for a cost-effective, lightweight solar 
 Fossil fuel alternatives, such as solar energy, are moving to the forefront in a variety of research fields. Polymer-based organic photovoltaic systems hold the promise for a cost-effective, lightweight solar energy conversion platform, which could benefit from simple solution processing of the active layer. The function of such excitonic solar cells is based on photoinduced electron transfer from a donor to an acceptor. Fullerenes have become the ubiquitous acceptors because of their high electron affinity and ability to transport charge effectively. The most effective solar cells have been made from bicontinuous polymer-fullerene composites, or so-called bulk heterojunctions. The best solar cells currently achieve an efficiency of about 5%, thus significant advances in the fundamental understanding of the complex interplay between the active layer morphology and electronic properties are required if this technology is to find viable application.
Abstract By applying the specific fabrication conditions summarized in the Experimental section and post‐production annealing at 150 °C, polymer solar cells with power‐conversion efficiency approaching 5 % are demonstrated. These 
 Abstract By applying the specific fabrication conditions summarized in the Experimental section and post‐production annealing at 150 °C, polymer solar cells with power‐conversion efficiency approaching 5 % are demonstrated. These devices exhibit remarkable thermal stability. We attribute the improved performance to changes in the bulk heterojunction material induced by thermal annealing. The improved nanoscale morphology, the increased crystallinity of the semiconducting polymer, and the improved contact to the electron‐collecting electrode facilitate charge generation, charge transport to, and charge collection at the electrodes, thereby enhancing the device efficiency by lowering the series resistance of the polymer solar cells.
A thin-film, two-layer organic photovoltaic cell has been fabricated from copper phthalocyanine and a perylene tetracarboxylic derivative. A power conversion efficiency of about 1% has been achieved under simulated AM2 
 A thin-film, two-layer organic photovoltaic cell has been fabricated from copper phthalocyanine and a perylene tetracarboxylic derivative. A power conversion efficiency of about 1% has been achieved under simulated AM2 illumination. A novel feature of the device is that the charge-generation efficiency is relatively independent of the bias voltage, resulting in cells with fill factor values as high as 0.65. The interface between the two organic materials, rather than the electrode/organic contacts, is crucial in determining the photovoltaic properties of the cell.
Over the past 25 years, organic field‐effect transistors (OFETs) have witnessed impressive improvements in materials performance by 3–4 orders of magnitude, and many of the key materials discoveries have been 
 Over the past 25 years, organic field‐effect transistors (OFETs) have witnessed impressive improvements in materials performance by 3–4 orders of magnitude, and many of the key materials discoveries have been published in Advanced Materials . This includes some of the most recent demonstrations of organic field‐effect transistors with performance that clearly exceeds that of benchmark amorphous silicon‐based devices. In this article, state‐of‐the‐art in OFETs are reviewed in light of requirements for demanding future applications, in particular active‐matrix addressing for flexible organic light‐emitting diode (OLED) displays. An overview is provided over both small molecule and conjugated polymer materials for which field‐effect mobilities exceeding > 1 cm 2 V –1 s –1 have been reported. Current understanding is also reviewed of their charge transport physics that allows reaching such unexpectedly high mobilities in these weakly van der Waals bonded and structurally comparatively disordered materials with a view towards understanding the potential for further improvement in performance in the future.
Self-organization of liquid crystalline and crystalline-conjugated materials has been used to create, directly from solution, thin films with structures optimized for use in photodiodes. The discotic liquid crystal hexa-peri-hexabenzocoronene was 
 Self-organization of liquid crystalline and crystalline-conjugated materials has been used to create, directly from solution, thin films with structures optimized for use in photodiodes. The discotic liquid crystal hexa-peri-hexabenzocoronene was used in combination with a perylene dye to produce thin films with vertically segregated perylene and hexabenzocoronene, with large interfacial surface area. When incorporated into diode structures, these films show photovoltaic response with external quantum efficiencies of more than 34 percent near 490 nanometers. These efficiencies result from efficient photoinduced charge transfer between the hexabenzocoronene and perylene, as well as from effective transport of charges through vertically segregated perylene and hexabenzocoronene π systems. This development demonstrates that complex structures can be engineered from novel materials by means of simple solution-processing steps and may enable inexpensive, high-performance, thin-film photovoltaic technology.
In this review, we discuss the physics underlying the operation of single and multiple heterojunction, vacuum-deposited organic solar cells based on small molecular weight thin films. For single heterojunction cells, 
 In this review, we discuss the physics underlying the operation of single and multiple heterojunction, vacuum-deposited organic solar cells based on small molecular weight thin films. For single heterojunction cells, we find that the need for direct contact between the deposited electrode and the active organics leads to quenching of excitons. An improved device architecture, the double heterojunction, is shown to confine excitons within the active layers, allowing substantially higher internal efficiencies to be achieved. A full optical and electrical analysis of the double heterostructure architecture leads to optimal cell design as a function of the optical properties and exciton diffusion lengths of the photoactive materials. Combining the double heterostructure with novel light trapping schemes, devices with external efficiencies approaching their internal efficiency are obtained. When applied to an organic photovoltaic cell with a power conversion efficiency of 1.0%±0.1% under 1 sun AM1.5 illumination, devices with external power conversion efficiencies of 2.4%±0.3% are reported. In addition, we show that by using materials with extended exciton diffusion lengths LD, highly efficient double heterojunction photovoltaic cells are obtained, even in the absence of a light trapping geometry. Using C60 as an acceptor material, double heterostructure external power conversion efficiencies of 3.6%±0.4% under 1 sun AM1.5 illumination are obtained. Stacking of single heterojunction devices leads to thin film multiple heterojunction photovoltaic and photodetector structures. Thin bilayer photovoltaic cells can be stacked with ultrathin (∌5 Å), discontinuous Ag layers between adjacent cells serving as efficient recombination sites for electrons and holes generated in the neighboring cells. Such stacked cells have open circuit voltages that are n times the open circuit voltage of a single cell, where n is the number of cells in the stack. In optimized structures, the short circuit photocurrent remains approximately constant upon stacking thin cells, leading to higher achievable power conversion efficiencies, as confirmed by modelling optical interference effects and exciton migration. A 2.5%±0.3% power efficiency under 100 mW/cm2 AM1.5 illumination conditions is obtained by stacking two ∌1% efficient devices. Alternatively, when the contact layers between the stacked cells are eliminated, a multilayer structure consisting of alternating films of donor and acceptor-type materials is obtained. Since the thicknesses of the individual layers (∌5 Å) can be substantially smaller than the exciton diffusion length, nearly 100% of the photogenerated excitons are dissociated, and the resulting free charges are detected. In addition, the ultrathin organic layers facilitate electron and hole transport through the multilayer stack by tunneling. When these devices are operated as photodetectors under applied fields >106 V/cm, the carrier collection efficiency reaches 80%, leading to external quantum efficiencies of 75%±1% across the visible spectrum in cells containing the thinnest layers. We find that due to the fast carrier tunneling process, the temporal response of these multilayer detectors is a direct measure of exciton dynamics. Response times of 720±50 ps are achieved, leading to a 3 dB bandwidth of 430±30 MHz. A summary of representative results obtained for both polymer and small molecule photovoltaic cells and photodetectors is included in this review. Prospects for further improvements in organic solar cells and photodetectors are considered.
Abstract Although the field of polymer solar cell has seen much progress in device performance in the past few years, several limitations are holding back its further development. For instance, 
 Abstract Although the field of polymer solar cell has seen much progress in device performance in the past few years, several limitations are holding back its further development. For instance, current high-efficiency (>9.0%) cells are restricted to material combinations that are based on limited donor polymers and only one specific fullerene acceptor. Here we report the achievement of high-performance (efficiencies up to 10.8%, fill factors up to 77%) thick-film polymer solar cells for multiple polymer:fullerene combinations via the formation of a near-ideal polymer:fullerene morphology that contains highly crystalline yet reasonably small polymer domains. This morphology is controlled by the temperature-dependent aggregation behaviour of the donor polymers and is insensitive to the choice of fullerenes. The uncovered aggregation and design rules yield three high-efficiency (>10%) donor polymers and will allow further synthetic advances and matching of both the polymer and fullerene materials, potentially leading to significantly improved performance and increased design flexibility.
For bulk-heterojunction photovoltaic cells fabricated from conjugated polymers and a fullerene derivative, the relation between the open-circuit voltage (Voc) and the oxidation potential for different conjugated polymers is studied. A 
 For bulk-heterojunction photovoltaic cells fabricated from conjugated polymers and a fullerene derivative, the relation between the open-circuit voltage (Voc) and the oxidation potential for different conjugated polymers is studied. A linear relation between Voc and the oxidation potential is found (see figure). Based on this relation, the energy-conversion efficiency of a bulk-heterojunction solar cell is derived as a function of the bandgap and the energy levels of the conjugated polymer.
Bulk heterojunction (BHJ) polymer solar cells (PSCs) sandwich a blend layer of conjugated polymer donor and fullerene derivative acceptor between a transparent ITO positive electrode and a low work function 
 Bulk heterojunction (BHJ) polymer solar cells (PSCs) sandwich a blend layer of conjugated polymer donor and fullerene derivative acceptor between a transparent ITO positive electrode and a low work function metal negative electrode. In comparison with traditional inorganic semiconductor solar cells, PSCs offer a simpler device structure, easier fabrication, lower cost, and lighter weight, and these structures can be fabricated into flexible devices. But currently the power conversion efficiency (PCE) of the PSCs is not sufficient for future commercialization. The polymer donors and fullerene derivative acceptors are the key photovoltaic materials that will need to be optimized for high-performance PSCs. In this Account, I discuss the basic requirements and scientific issues in the molecular design of high efficiency photovoltaic molecules. I also summarize recent progress in electronic energy level engineering and absorption spectral broadening of the donor and acceptor photovoltaic materials by my research group and others. For high-efficiency conjugated polymer donors, key requirements are a narrower energy bandgap (E(g)) and broad absorption, relatively lower-lying HOMO (the highest occupied molecular orbital) level, and higher hole mobility. There are three strategies to meet these requirements: D-A copolymerization for narrower E(g) and lower-lying HOMO, substitution with electron-withdrawing groups for lower-lying HOMO, and two-dimensional conjugation for broad absorption and higher hole mobility. Moreover, better main chain planarity and less side chain steric hindrance could strengthen π-π stacking and increase hole mobility. Furthermore, the molecular weight of the polymers also influences their photovoltaic performance. To produce high efficiency photovoltaic polymers, researchers should attempt to increase molecular weight while maintaining solubility. High-efficiency D-A copolymers have been obtained by using benzodithiophene (BDT), dithienosilole (DTS), or indacenodithiophene (IDT) donor unit and benzothiadiazole (BT), thienopyrrole-dione (TPD), or thiazolothiazole (TTz) acceptor units. The BDT unit with two thienyl conjugated side chains is a highly promising unit in constructing high-efficiency copolymer donor materials. The electron-withdrawing groups of ester, ketone, fluorine, or sulfonyl can effectively tune the HOMO energy levels downward. To improve the performance of fullerene derivative acceptors, researchers will need to strengthen absorption in the visible spectrum, upshift the LUMO (the lowest unoccupied molecular orbital) energy level, and increase the electron mobility. [6,6]-Phenyl-C(71)-butyric acid methyl ester (PC(70)BM) is superior to [6,6]-phenyl-C(61)-butyric acid methyl ester (PCBM) because C(70) absorbs visible light more efficiently. Indene-C(60) bisadduct (ICBA) and Indene-C(70) bisadduct (IC(70)BA) show 0.17 and 0.19 eV higher LUMO energy levels, respectively, than PCBM, due to the electron-rich character of indene and the effect of bisadduct. ICBA and IC(70)BA are excellent acceptors for the P3HT-based PSCs.
ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTSynthesis of Conjugated Polymers for Organic Solar Cell ApplicationsYen-Ju Cheng*, Sheng-Hsiung Yang, and Chain-Shu Hsu*View Author Information Department of Applied Chemistry, National Chiao Tung University, 1001 Ta 
 ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTSynthesis of Conjugated Polymers for Organic Solar Cell ApplicationsYen-Ju Cheng*, Sheng-Hsiung Yang, and Chain-Shu Hsu*View Author Information Department of Applied Chemistry, National Chiao Tung University, 1001 Ta Hsueh Road, Hsin-Chu 30049, Taiwan* To whom correspondence should be addressed. Phone: +886-3513-1523. Fax: +886-3513-1523. E-mail: [email protected] (Y.-J.C.); [email protected] (C.-S.H.).Cite this: Chem. Rev. 2009, 109, 11, 5868–5923Publication Date (Web):September 28, 2009Publication History Received7 May 2009Published online28 September 2009Published inissue 11 November 2009https://pubs.acs.org/doi/10.1021/cr900182shttps://doi.org/10.1021/cr900182sreview-articleACS PublicationsCopyright © 2009 American Chemical SocietyRequest reuse permissionsArticle Views51034Altmetric-Citations3652LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Conjugated polymers,Electrical conductivity,Polymers,Power conversion efficiency,Solar cells Get e-Alerts
We show that the power conversion efficiency of organic photovoltaic devices based on a conjugated polymer/methanofullerene blend is dramatically affected by molecular morphology. By structuring the blend to be a 
 We show that the power conversion efficiency of organic photovoltaic devices based on a conjugated polymer/methanofullerene blend is dramatically affected by molecular morphology. By structuring the blend to be a more intimate mixture that contains less phase segregation of methanofullerenes, and simultaneously increasing the degree of interactions between conjugated polymer chains, we have fabricated a device with a power conversion efficiency of 2.5% under AM1.5 illumination. This is a nearly threefold enhancement over previously reported values for such a device, and it approaches what is needed for the practical use of these devices for harvesting energy from sunlight.
ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTCharge Photogeneration in Organic Solar CellsTracey M. Clarke and James R. Durrant*View Author Information Centre for Plastic Electronics, Department of Chemistry, Imperial College London, London, SW7 2AZ, 
 ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTCharge Photogeneration in Organic Solar CellsTracey M. Clarke and James R. Durrant*View Author Information Centre for Plastic Electronics, Department of Chemistry, Imperial College London, London, SW7 2AZ, United Kingdom* To whom correspondence should be addressed. E-mail: [email protected]Cite this: Chem. Rev. 2010, 110, 11, 6736–6767Publication Date (Web):January 11, 2010Publication History Received5 August 2009Published online11 January 2010Published inissue 10 November 2010https://pubs.acs.org/doi/10.1021/cr900271shttps://doi.org/10.1021/cr900271sreview-articleACS PublicationsCopyright © 2010 American Chemical SocietyRequest reuse permissionsArticle Views37531Altmetric-Citations1996LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Charge transfer,Dissociation,Excitons,Photogeneration,Recombination Get e-Alerts
Direct printing of functional electronic materials may provide a new route to low-cost fabrication of integrated circuits. However, to be useful it must allow continuous manufacturing of all circuit components 
 Direct printing of functional electronic materials may provide a new route to low-cost fabrication of integrated circuits. However, to be useful it must allow continuous manufacturing of all circuit components by successive solution deposition and printing steps in the same environment. We demonstrate direct inkjet printing of complete transistor circuits, including via-hole interconnections based on solution-processed polymer conductors, insulators, and self-organizing semiconductors. We show that the use of substrate surface energy patterning to direct the flow of water-based conducting polymer inkjet droplets enables high-resolution definition of practical channel lengths of 5 micrometers. High mobilities of 0.02 square centimeters per volt second and on-off current switching ratios of 10(5) were achieved.
The optoelectronic properties of polymeric semiconductor materials can be utilized for the fabrication of organic electronic and photonic devices. When key structural requirements are met, these materials exhibit unique properties 
 The optoelectronic properties of polymeric semiconductor materials can be utilized for the fabrication of organic electronic and photonic devices. When key structural requirements are met, these materials exhibit unique properties such as solution processability, large charge transporting capabilities, and/or broad optical absorption. In this review recent developments in the area of π-conjugated polymeric semiconductors for organic thin-film (or field-effect) transistors (OTFTs or OFETs) and bulk-heterojunction photovoltaic (or solar) cell (BHJ-OPV or OSC) applications are summarized and analyzed.
The carrier collection efficiency (η c ) and energy conversion efficiency (η e ) of polymer photovoltaic cells were improved by blending of the semiconducting polymer with C 60 or 
 The carrier collection efficiency (η c ) and energy conversion efficiency (η e ) of polymer photovoltaic cells were improved by blending of the semiconducting polymer with C 60 or its functionalized derivatives. Composite films of poly(2-methoxy-5-(2â€Č-ethyl-hexyloxy)-1,4-phenylene vinylene) (MEH-PPV) and fullerenes exhibit η c of about 29 percent of electrons per photon and η e of about 2.9 percent, efficiencies that are better by more than two orders of magnitude than those that have been achieved with devices made with pure MEH-PPV. The efficient charge separation results from photoinduced electron transfer from the MEH-PPV (as donor) to C 60 (as acceptor); the high collection efficiency results from a bicontinuous network of internal donor-acceptor heterojunctions.
ADVERTISEMENT RETURN TO ISSUEPREVArticleNEXTCharge-Transfer and Energy-Transfer Processes in π-Conjugated Oligomers and Polymers: A Molecular PictureJean-Luc BrĂ©das, David Beljonne, Veaceslav Coropceanu, and JĂ©rĂŽme CornilView Author Information School of Chemistry and Biochemistry, 
 ADVERTISEMENT RETURN TO ISSUEPREVArticleNEXTCharge-Transfer and Energy-Transfer Processes in π-Conjugated Oligomers and Polymers: A Molecular PictureJean-Luc BrĂ©das, David Beljonne, Veaceslav Coropceanu, and JĂ©rĂŽme CornilView Author Information School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, and Laboratory for Chemistry of Novel Materials, University of Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium Cite this: Chem. Rev. 2004, 104, 11, 4971–5004Publication Date (Web):September 28, 2004Publication History Received9 June 2004Published online28 September 2004Published inissue 1 November 2004https://pubs.acs.org/doi/10.1021/cr040084khttps://doi.org/10.1021/cr040084kresearch-articleACS PublicationsCopyright © 2004 American Chemical SocietyRequest reuse permissionsArticle Views34788Altmetric-Citations2480LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Aromatic compounds,Excited states,Excitons,Hydrocarbons,Oligomers Get e-Alerts
A novel non-fullerene electron acceptor (ITIC) that overcomes some of the shortcomings of fullerene acceptors, for example, weak absorption in the visible spectral region and limited energy-level variability, is designed 
 A novel non-fullerene electron acceptor (ITIC) that overcomes some of the shortcomings of fullerene acceptors, for example, weak absorption in the visible spectral region and limited energy-level variability, is designed and synthesized. Fullerene-free polymer solar cells (PSCs) based on the ITIC acceptor are demonstrated to exhibit power conversion efficiencies of up to 6.8%, a record for fullerene-free PSCs.
Abstract Solution‐processed bulk heterojunction organic photovoltaic (OPV) devices have gained serious attention during the last few years and are established as one of the leading next generation photovoltaic technologies for 
 Abstract Solution‐processed bulk heterojunction organic photovoltaic (OPV) devices have gained serious attention during the last few years and are established as one of the leading next generation photovoltaic technologies for low cost power production. This article reviews the OPV development highlights of the last two decades, and summarizes the key milestones that have brought the technology to today’s efficiency performance of over 7%. An outlook is presented on what will be required to drive this young photovoltaic technology towards the next major milestone, a 10% power conversion efficiency, considered by many to represent the efficiency at which OPV can be adopted in wide‐spread applications. With first products already entering the market, sufficient lifetime for the intended application becomes more and more critical, and the status of OPV stability as well as the current understanding of degradation mechanisms will be reviewed in the second part of this article.
An all-polymer semiconductor integrated device is demonstrated with a high-mobility conjugated polymer field-effect transistor (FET) driving a polymer light-emitting diode (LED) of similar size. The FET uses regioregular poly(hexylthiophene). Its 
 An all-polymer semiconductor integrated device is demonstrated with a high-mobility conjugated polymer field-effect transistor (FET) driving a polymer light-emitting diode (LED) of similar size. The FET uses regioregular poly(hexylthiophene). Its performance approaches that of inorganic amorphous silicon FETs, with field-effect mobilities of 0.05 to 0.1 square centimeters per volt second and ON-OFF current ratios of >10(6). The high mobility is attributed to the formation of extended polaron states as a result of local self-organization, in contrast to the variable-range hopping of self-localized polarons found in more disordered polymers. The FET-LED device represents a step toward all-polymer optoelectronic integrated circuits such as active-matrix polymer LED displays.
An effective way to improve polymer solar cell efficiency is to use a tandem structure, as a broader part of the spectrum of solar radiation is used and the thermalization 
 An effective way to improve polymer solar cell efficiency is to use a tandem structure, as a broader part of the spectrum of solar radiation is used and the thermalization loss of photon energy is minimized. In the past, the lack of high-performance low-bandgap polymers was the major limiting factor for achieving high-performance tandem solar cell. Here we report the development of a high-performance low bandgap polymer (bandgap <1.4 eV), poly[2,7-(5,5-bis-(3,7-dimethyloctyl)-5H-dithieno[3,2-b:2â€Č,3â€Č-d]pyran)-alt-4,7-(5,6-difluoro-2,1,3-benzothia diazole)] with a bandgap of 1.38 eV, high mobility, deep highest occupied molecular orbital. As a result, a single-junction device shows high external quantum efficiency of >60% and spectral response that extends to 900 nm, with a power conversion efficiency of 7.9%. The polymer enables a solution processed tandem solar cell with certified 10.6% power conversion efficiency under standard reporting conditions (25 °C, 1,000 Wm−2, IEC 60904-3 global), which is the first certified polymer solar cell efficiency over 10%. Tandem solar cell structures combine high- and low-bandgap materials, allowing a broader spectral absorption of solar radiation. The authors report the synthesis of a high performance low-bandgap polymer which enables fabrication of a tandem solar cell with a certified power conversion efficiency of 10.6%.
The photovoltaic performance of polymer bulk heterojunction solar cells is studied systematically. Using a new benzodithiophene polymer (PTB7) and PC71BM (see figure) a power conversion efficiency of 7.4% has been 
 The photovoltaic performance of polymer bulk heterojunction solar cells is studied systematically. Using a new benzodithiophene polymer (PTB7) and PC71BM (see figure) a power conversion efficiency of 7.4% has been achieved in PTB7/PC71BM-blend film, indicating a great potential and bright future for polymer solar cells (FF = fill factor, PCE ;= power-conversion efficiency). Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer-reviewed, but not copy-edited or typeset. They are made available as submitted by the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
Tandem solar cells, in which two solar cells with different absorption characteristics are linked to use a wider range of the solar spectrum, were fabricated with each layer processed from 
 Tandem solar cells, in which two solar cells with different absorption characteristics are linked to use a wider range of the solar spectrum, were fabricated with each layer processed from solution with the use of bulk heterojunction materials comprising semiconducting polymers and fullerene derivatives. A transparent titanium oxide (TiO(x)) layer separates and connects the front cell and the back cell. The TiO(x) layer serves as an electron transport and collecting layer for the first cell and as a stable foundation that enables the fabrication of the second cell to complete the tandem cell architecture. We use an inverted structure with the low band-gap polymer-fullerene composite as the charge-separating layer in the front cell and the high band-gap polymer composite as that in the back cell. Power-conversion efficiencies of more than 6% were achieved at illuminations of 200 milliwatts per square centimeter.
Organic field-effect transistors (OFETs) were first described in 1987. Their characteristics have undergone spectacular improvements during the last two or three years. At the same time, several models have been 
 Organic field-effect transistors (OFETs) were first described in 1987. Their characteristics have undergone spectacular improvements during the last two or three years. At the same time, several models have been developed to rationalize their operating mode. In this review, we examine the performance of OFETs as revealed by recently published data, mainly in terms of field-effect mobility and on–off current ratio. We compare the various compounds that have been used as the active component, and describe the most prominent fabrication techniques. Finally, we analyze the charge transport mechanisms in organic solids, and the resulting models of OFETs.
ADVERTISEMENT RETURN TO ISSUEPREVArticleNEXTCharge Transport in Organic SemiconductorsVeaceslav Coropceanu, JĂ©rĂŽme Cornil, Demetrio A. da Silva Filho, Yoann Olivier, Robert Silbey, and Jean-Luc BrĂ©dasView Author Information School of Chemistry and Biochemistry 
 ADVERTISEMENT RETURN TO ISSUEPREVArticleNEXTCharge Transport in Organic SemiconductorsVeaceslav Coropceanu, JĂ©rĂŽme Cornil, Demetrio A. da Silva Filho, Yoann Olivier, Robert Silbey, and Jean-Luc BrĂ©dasView Author Information School of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, Laboratory for Chemistry of Novel Materials, University of Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium, and Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 Cite this: Chem. Rev. 2007, 107, 4, 926–952Publication Date (Web):March 23, 2007Publication History Received8 November 2006Published online23 March 2007Published inissue 1 April 2007https://pubs.acs.org/doi/10.1021/cr050140xhttps://doi.org/10.1021/cr050140xresearch-articleACS PublicationsCopyright © 2007 American Chemical SocietyRequest reuse permissionsArticle Views66183Altmetric-Citations3771LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Coupling reactions,Diseases and disorders,Electrical energy,Mobility,Molecules Get e-Alerts
Organic thin-film transistors (OTFTs) have lived to see great improvements in recent years. This review presents new insight into conduction mechanisms and performance characteristics, as well as opportunities for modeling 
 Organic thin-film transistors (OTFTs) have lived to see great improvements in recent years. This review presents new insight into conduction mechanisms and performance characteristics, as well as opportunities for modeling properties of OTFTs. The shifted focus in research from novel chemical structures to fabrication technologies that optimize morphology and structural order is underscored by chapters on vacuum-deposited and solution-processed organic semiconducting films. Finally, progress in the growing field of the n-type OTFTs is discussed in ample detail. The Figure, showing a pentacene film edge on SiO2, illustrates the morphology issue.
ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTRecent Advances in Bulk Heterojunction Polymer Solar CellsLuyao Lu, Tianyue Zheng, Qinghe Wu, Alexander M. Schneider, Donglin Zhao, and Luping Yu*View Author Information Department of Chemistry and 
 ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTRecent Advances in Bulk Heterojunction Polymer Solar CellsLuyao Lu, Tianyue Zheng, Qinghe Wu, Alexander M. Schneider, Donglin Zhao, and Luping Yu*View Author Information Department of Chemistry and The James Franck Institute, The University of Chicago, 929 East 57th Street, Chicago, Illinois 60637, United States*E-mail: [email protected]Cite this: Chem. Rev. 2015, 115, 23, 12666–12731Publication Date (Web):August 7, 2015Publication History Received13 February 2015Published online7 August 2015Published inissue 9 December 2015https://pubs.acs.org/doi/10.1021/acs.chemrev.5b00098https://doi.org/10.1021/acs.chemrev.5b00098review-articleACS PublicationsCopyright © 2015 American Chemical SocietyRequest reuse permissionsArticle Views31232Altmetric-Citations2296LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Conjugated polymers,Layers,Polymers,Power conversion efficiency,Solar cells Get e-Alerts
ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTSemiconducting π-Conjugated Systems in Field-Effect Transistors: A Material Odyssey of Organic ElectronicsChengliang Wang, Huanli Dong, Wenping Hu*, Yunqi Liu, and Daoben ZhuView Author Information Beijing National Laboratory 
 ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTSemiconducting π-Conjugated Systems in Field-Effect Transistors: A Material Odyssey of Organic ElectronicsChengliang Wang, Huanli Dong, Wenping Hu*, Yunqi Liu, and Daoben ZhuView Author Information Beijing National Laboratory for Molecular Sciences, Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China*Address: Zhongguancun North First No 2, Beijing, 100190, China. E-mail: [email protected]Cite this: Chem. Rev. 2012, 112, 4, 2208–2267Publication Date (Web):November 23, 2011Publication History Received15 November 2010Published online23 November 2011Published inissue 11 April 2012https://pubs.acs.org/doi/10.1021/cr100380zhttps://doi.org/10.1021/cr100380zreview-articleACS PublicationsCopyright © 2011 American Chemical SocietyRequest reuse permissionsArticle Views44410Altmetric-Citations3145LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Aromatic compounds,Hydrocarbons,Mobility,Reaction products,Thin films Get e-Alerts
A new polymer donor (PBDB-T-SF) and a new small molecule acceptor (IT-4F) for fullerene-free organic solar cells (OSCs) were designed and synthesized. The influences of fluorination on the absorption spectra, 
 A new polymer donor (PBDB-T-SF) and a new small molecule acceptor (IT-4F) for fullerene-free organic solar cells (OSCs) were designed and synthesized. The influences of fluorination on the absorption spectra, molecular energy levels, and charge mobilities of the donor and acceptor were systematically studied. The PBDB-T-SF:IT-4F-based OSC device showed a record high efficiency of 13.1%, and an efficiency of over 12% can be obtained with a thickness of 100-200 nm, suggesting the promise of fullerene-free OSCs in practical applications.
Although organic photovoltaic (OPV) cells have many advantages, their performance still lags far behind that of other photovoltaic platforms. A fundamental reason for their low performance is the low charge 
 Although organic photovoltaic (OPV) cells have many advantages, their performance still lags far behind that of other photovoltaic platforms. A fundamental reason for their low performance is the low charge mobility of organic materials, leading to a limit on the active-layer thickness and efficient light absorption. In this work, guided by a semi-empirical model analysis and using the tandem cell strategy to overcome such issues, and taking advantage of the high diversity and easily tunable band structure of organic materials, a record and certified 17.29% power conversion efficiency for a two-terminal monolithic solution-processed tandem OPV is achieved.
Abstract Solution‐processed bulk‐heterojunction solar cells have gained serious attention during the last few years and are becoming established as one of the future photovoltaic technologies for low‐cost power production. This 
 Abstract Solution‐processed bulk‐heterojunction solar cells have gained serious attention during the last few years and are becoming established as one of the future photovoltaic technologies for low‐cost power production. This article reviews the highlights of the last few years, and summarizes today's state‐of‐the‐art performance. An outlook is given on relevant future materials and technologies that have the potential to guide this young photovoltaic technology towards the magic 10% regime. A cost model supplements the technical discussions, with practical aspects any photovoltaic technology needs to fulfil, and answers to the question as to whether low module costs can compensate lower lifetimes and performances.
Abstract Pristine PEDOT: PSS is a p-type material with salient features. However, studies have revealed that the electrical property of pristine PEDOT: PSS can be switched to n-type by solvent 
 Abstract Pristine PEDOT: PSS is a p-type material with salient features. However, studies have revealed that the electrical property of pristine PEDOT: PSS can be switched to n-type by solvent treatment. Notwithstanding that this method is simple, it performs inconsistently and primarily affects the samples’ surfaces due to the migration of the solvent molecules into the polymer network. These solvents are also hazardous and unfavourable to the environment. In this work, we report solvent-free switching electrical characteristics of pristine PEDOT: PSS to n-type using a spray coating technique. The obtained n-PEDOT: PSS exhibits excellent optical and electrical characteristics. In addition, high Seebeck coefficient of – 1320.06 ± 38.42 ”VK −1 and power factor of 4.32 ± 0.25 ”Wm −1 K −2 were found. The obtained n-PEDOT: PSS was used in the fabrication of a homojunction diode. The I-V curve showed rectification characteristics with rectification ratio and barrier height of 17.2 and 0.047 eV, respectively, which is one of the best reported values in the literature for all PEDOT: PSS-based diode.
The ternary strategy represents a promising approach to improving the power conversion efficiency (PCE) of organic solar cells (OSCs). However, the mechanism of the third component in optimizing both the 
 The ternary strategy represents a promising approach to improving the power conversion efficiency (PCE) of organic solar cells (OSCs). However, the mechanism of the third component in optimizing both the active layer morphology and charge transfer processes remains elusive. Here, we employ a multiscale computational framework integrating first-principles calculations, molecular dynamics (MD), and kinetic Monte Carlo (KMC) simulations to elucidate the critical function of PC71BM as a third component in the PM6/L8-BO blend. Our findings reveal that PC71BM primarily localizes at the PM6/L8-BO interface, forming an additional high-energy charge transfer (H-CT) state between PM6 and PC71BM, alongside the intrinsic low-energy CT (L-CT) state between PM6 and L8-BO. This H-CT establishes a new high-efficiency pathway for PM6 exciton dissociation, succeeding in leading to a much larger charge separation (CS) rate (6 × 1012 s-1) than that (5 × 109 s-1) via the L-CT state. Furthermore, PC71BM incorporation improves electron and hole mobilities as well as ambipolar transport, thereby suppressing charge recombination loss. This work unveils the dual role of PC71BM in optimizing interfacial charge-transfer kinetics and bulk carrier transport, offering fundamental guidelines for a third-component design in high-performance ternary OSCs.
Charge carriers in amorphous semiconducting polymers diffuse rapidly along the polymer chains, hopping less frequently to neighboring chains. The escape time required on average to hop to a neighboring chain 
 Charge carriers in amorphous semiconducting polymers diffuse rapidly along the polymer chains, hopping less frequently to neighboring chains. The escape time required on average to hop to a neighboring chain affects the design of new polymers and determines the relative importance of other system parameters such as polymer rigidity or polymer molecular weight. We provide a general expression for the escape rate, which lends itself to a more simplified and transparent expression in the limit of vanishing reorganization energy. The escape rate appears to be more sensitive to disorder and temperature than the intra-chain transport. We show how the parameters required for the evaluation of this rate can be derived from a combination of classical and quantum chemical models already used to characterize semiconducting polymers, and we provide an illustration based on two realistic polymeric materials.
The utilization of near-infrared (NIR) organic photodetectors (OPDs) holds considerable promise, primarily owing to their solution processability and flexibility characteristics. The recent reduction of dark current in the NIR-OPDs is 
 The utilization of near-infrared (NIR) organic photodetectors (OPDs) holds considerable promise, primarily owing to their solution processability and flexibility characteristics. The recent reduction of dark current in the NIR-OPDs is critical for achieving high performance in OPDs using the narrow bandgap of the active layer. However, recent NIR-OPDs with excellent low-dark current exhibit measurement limitations, particularly regarding noise and trap measurements, which are crucial for evaluating specific detectivity and understanding the physics of the NIR-OPDs. This study comprehensively analyzes precise noise and trap measurements at varying inert annealing temperatures applied to the electron-transport layer. The optimized annealing process led to a high specific detectivity of 1.3 × 1013 cm Hz1/2 W-1 at 850 nm and a low trap density of 9.9 × 1013 cm-3 at a shallow-trap-energy level of 0.37 eV. The inert annealing process offers an example of typical issues, such as water-induced trap analysis. Our research explains some pitfalls of noise and trap measurements, addresses them adequately, and demonstrates their limitations. Noise-spectrum measurements should be conducted in a specific range limited by the shot-noise current and the gain bandwidth. In addition, the shallow and slight trap-density reduction can be captured by capacitance-voltage and capacitance-frequency measurements using a series resistance correction. The adequate measurement settings play a vital role in extracting the key physical characteristics of the recent high-performance OPD.
Broadband photomultiplication-type organic photodetectors (PM-OPDs) were fabricated by employing a wide bandgap donor P3HT and narrow bandgap acceptor QxIC as the photoactive layers. The optimal weight ratio of P3HT to 
 Broadband photomultiplication-type organic photodetectors (PM-OPDs) were fabricated by employing a wide bandgap donor P3HT and narrow bandgap acceptor QxIC as the photoactive layers. The optimal weight ratio of P3HT to QxIC is adjusted as approximately 100:1 to achieve numerous isolated electron traps formed by P3HT/QxIC/P3HT and an efficient hole transport channel in the photoactive layers. The trapped photogenerated electrons in QxIC near the Al electrode will induce interfacial band bending for more efficient hole tunneling injection to obtain a large light current density (JL), resulting in the external quantum efficiency (EQE) over 100% of the PM-OPDs. The dark current density (JD) of broadband PM-OPDs can be further suppressed by employing MPA2FPh-BT-BA as an interfacial layer instead of a PEDOT:PSS layer on the ITO electrode. The optimal PM-OPDs display a rather low JD of 5.7 × 10-7 A cm-2 under a -8 V bias, which is lower than 5.3 × 10-6 A cm-2 for PM-OPDs with PEDOT:PSS as an interfacial layer under the same bias. Additionally, the JL of broadband PM-OPDs exhibits a slightly decreased trend by using the MPA2FPh-BT-BA interfacial layer. The signal-to-noise ratio (SNR) of broadband PM-OPDs can be increased from 667 to 3788 by replacing PEDOT:PSS with MPA2FPh-BT-BA as the interfacial layer, benefiting from the markedly decreased JD and relatively high JL. The optimal broadband PM-OPDs exhibit EQE values of 8010% at 355 nm and 2170% at 835 nm, as well as specific detectivity values of 9.1 × 1012 Jones at 355 nm and 5.8 × 1012 Jones at 835 nm under a -8 V bias.
Abstract It is proposed organic photodetectors (OPDs) with immiscible planar heterojunction (PHJ) interfaces can address the air stability challenges of bulk heterojunction (BHJ) and pseudo‐PHJ OPDs, which suffer from nanomorphology 
 Abstract It is proposed organic photodetectors (OPDs) with immiscible planar heterojunction (PHJ) interfaces can address the air stability challenges of bulk heterojunction (BHJ) and pseudo‐PHJ OPDs, which suffer from nanomorphology instability. A random polythiophene (RP‐T50) containing ≈50 mol% thiophene units with thermocleavable side chains (TCSs) is employed as the electron donor, while [6,6]‐phenyl‐C 71 ‐butyric acid methyl ester (PC 71 BM) served as the electron acceptor. Thermal annealing of RP‐T50 (RP‐T50‐COOH) thin films cleaved the TCSs, rendering the films insoluble and forming a stable, unmixed interface with PC 71 BM. This approach prevented the formation of partially mixed pseudo‐PHJ interfaces that compromise air stability in conventional PHJ OPDs. The insoluble RP‐T50‐COOH thin films enabled all‐green‐solvent processing, resulting in high performance, including a responsivity of ≈138 mA W −1 , a specific detectivity of ≈1.68 × 10Âč 2 Jones, and a linear dynamic range of ≈100 dB without external bias. Notably, the devices exhibited exceptional air stability, maintaining performance for ≈250 days in ambient storage without encapsulation. These findings demonstrate a simple and scalable strategy for enhancing OPD stability, paving the way for their commercial application across diverse fields.
<title>Abstract</title> The commercialization of organic solar cells (OSCs) requires eliminating halogenated solvents from their production. However, the disordered molecular aggregation of nonfullerene acceptors in nonhalogenated solvents hinders the realization of 
 <title>Abstract</title> The commercialization of organic solar cells (OSCs) requires eliminating halogenated solvents from their production. However, the disordered molecular aggregation of nonfullerene acceptors in nonhalogenated solvents hinders the realization of OSCs with high power conversion efficiencies (PCEs). Herein, this problem is addressed using an external physical field modulation strategy involving the sonication of nonfullerene acceptor solutions. The application of ultrasound field induces a transformation from disordered molecular aggregation to ordered J-aggregation via microstreaming and shear stress in nonhalogenated solvents. The aggregation is effectively preserved within films, causing the formation of a fibril network with enhanced π-π stacking interactions. Moreover, sonication promotes the conversion of localized excitons to intra-moiety delocalized excitons and suppresses molecular vibrations, thus favoring charge separation and reducing nonradiative recombination. Consequently, the PCEs of PM6:L8-BO-based binary and ternary devices fabricated using <italic>o</italic>-xylene as a nonhalogenated solvent are 19.43% and 20.41% (certified 19.84%), which is among the highest values reported for OSCs produced without halogenated solvents. The binary devices also exhibit high thermal stabilities, with the <italic>T</italic><sub>80</sub> lifetime exceeding 10000 h. The developed strategy is applicable to various small-molecule acceptor and polymer acceptor systems, facilitating control disordered aggregation in nonfullerene acceptor solutions and thus paving the way for practical industrial applications.
Two polymer donors, PATz3T-o6BO and PATz3T-o6HD, incorporating alkoxy-substituted anthra[1,2-c:5,6-c']bis([1,2,5]thiadiazole), were strategically designed and synthesized. The unique wavy backbone of these polymers effectively reduced aggregation, leading to enhanced solubility and significantly 
 Two polymer donors, PATz3T-o6BO and PATz3T-o6HD, incorporating alkoxy-substituted anthra[1,2-c:5,6-c']bis([1,2,5]thiadiazole), were strategically designed and synthesized. The unique wavy backbone of these polymers effectively reduced aggregation, leading to enhanced solubility and significantly improved molecular ordering. Consequently, the PATz3T-o6HD:Y12-based solar cells achieved a power conversion efficiency (PCE) of 7.94%. These findings provide valuable insights into the molecular design of high-performance polymer donors for organic photovoltaics (OPVs).
Modifying the polymer backbone through N⋯S non-covalent interactions is an effective approach to enhance the properties of organic semiconducting polymers. Following this strategy, we designed and synthesized two new quinoidal 
 Modifying the polymer backbone through N⋯S non-covalent interactions is an effective approach to enhance the properties of organic semiconducting polymers. Following this strategy, we designed and synthesized two new quinoidal polymers based on asymmetric and symmetric thiazole-flanked para-azaquinodimethane (p-AQM), named PAQM-TTTz and PAQM-TzTTz. To assess the impact of the thiazole unit, we also synthesized a reference polymer, PAQM-TTT, and compared its optoelectronic, thermal, and polymer backbone planarity properties with those of PAQM-TTTz and PAQM-TzTTz. Both PAQM-TTTz and PAQM-TzTTz exhibited dual-band absorption in solution, indicating pre-aggregation due to enhanced intermolecular interactions. Both polymers exhibited a low band gap. Density functional theory (DFT) studies revealed that while the thiazole unit does not alter the bond lengths of adjacent thiophenes, but it reduces torsional disorder by forming N⋯S non-covalent interactions with adjacent thiophenes in PAQM-TTTz and PAQM-TzTTz. However, due to the reduced electron richness of the conjugated backbone, a lower charge carrier mobility was observed in field-effect transistors for PAQM-TTTz and PAQM-TzTTz in comparison to PAQM-TTT. Our results highlighted the interest of non-covalent interactions in quinoidal polymers and present an alternative design strategy to control the properties of p-AQM-based quinoidal semiconducting polymers.
Semitransparent organic modules (STOMs) are of particular interest due to potential applications in building-integrated photovoltaics though upscaling without significant performance losses while ensuring an aesthetic appearance for window applications remains 
 Semitransparent organic modules (STOMs) are of particular interest due to potential applications in building-integrated photovoltaics though upscaling without significant performance losses while ensuring an aesthetic appearance for window applications remains a major research obstacle. This study presents two types of STOMs with an area of 11.4 cm2, exhibiting homogeneous appearance while retaining up to 92% of their respective small-area cell power conversion efficiency (PCE). Precise laser structuring minimized the area loss originating from the sub-cell series interconnection, allowing narrow cell stripes down to 1.25 mm. This enables a metal-less top electrode composed solely of PEDOT:PSS without compromising fill factor. For a module, an additional challenge is to ensure a low resistance series interconnection between sub-cells. This is realized with a novel approach based on a direct contact between PEDOT:PSS and a thin Ag layer within the back electrode. For the first design, the latter incorporates Al-doped ZnO and Ag attaining a PCE of 6.1% with an average visible transmission (AVT) of 47.5%. A more elaborate design features an extended back electrode using TiO2 and SiO2 for improved optical performance (PCE = 7.9%), reaching an unprecedented AVT of 50.8% and a light utilization efficiency (LUE = AVT x PCE) of 4.0%.
Optimizing the morphology of the active layer is crucial for achieving high photovoltaic conversion efficiency in all-polymer solar cells (APSCs). Solvent vapor annealing (SVA) is an essential post-treatment strategy for 
 Optimizing the morphology of the active layer is crucial for achieving high photovoltaic conversion efficiency in all-polymer solar cells (APSCs). Solvent vapor annealing (SVA) is an essential post-treatment strategy for controlling active layer morphology. However, most current SVA are conducted ex situ, limiting their ability to accurately reveal the morphological evolution of active layers of APSCs. In this study, in situ synchrotron radiation GIWAXS and in situ UV-vis spectroscopy combined with GISAXS is used to monitor the morphological evolution of PM6/PY-IT blends during the SVA process in real-time. Results showed that the PY-IT absorption peak exhibited a red shift under a nonpolar carbon disulfide vapor, while a blue shift is observed during the SVA process with a polar chloroform vapor. The SVA process can be divided into three stages: solvent swelling, recrystallization, and molecular rearrangement. For thermally pre-annealed samples subjected to chloroform SVA, the power conversion efficiency (PCE) increased by 15.1%. The improved PCE stems from reduced crystal plane spacing (d-spacing), enhanced crystal coherence length, and optimal phase separation via SVA. Pre-annealing suppresses excessive swelling, emphasizing the reordering dynamical role in the morphology of APSCs. This study offers insights into balancing SVA conditions to maximize performance and minimize adverse effects.
Light‐harvesting layers in organic bulk‐heterojunction solar cells are commonly fabricated from aromatic or even chlorinated solvents, which are often toxic or otherwise hazardous. In this work, nanoparticle dispersions of a 
 Light‐harvesting layers in organic bulk‐heterojunction solar cells are commonly fabricated from aromatic or even chlorinated solvents, which are often toxic or otherwise hazardous. In this work, nanoparticle dispersions of a blend of poly(3‐hexylthiophene) and [6,6]‐phenyl C 71 ‐butric acid methyl ester (P3HT:PC 71 BM) are synthesized in water, omitting any stabilizing surfactants which would remain in the layer and hamper the device performance. To overcome wetting issues and to master the deposition of thin films from aqueous dispersions, co‐solvents are employed. The solar cells exhibit power conversion efficiencies of 2.7% and show excellent long‐term stability, paving a promising way towards the all‐eco‐friendly production of organic solar cells in the future.
The capability of cathode interlayer (CIL) in regulating the conductivity, interfacial dipole, and work function of electrode plays a critical role in determining the photovoltaic performance of organic solar cells 
 The capability of cathode interlayer (CIL) in regulating the conductivity, interfacial dipole, and work function of electrode plays a critical role in determining the photovoltaic performance of organic solar cells (OSCs). The widely used perylene‐diimide‐based CILs suffered from the inbuilt limitation of finite conductivity and poor thickness tolerance. To address this issue, we develop a universal strategy to finely optimize the functionality of perylene‐diimide‐type CIL (PDINN) by incorporating polyfluorine‐substituted copper phthalocyanine (CuPc) derivative to form hybrid CIL. It is found that the hydrogen bonding and π‐π interaction between PDINN and CuPc can address the solvent processability issue of CuPc used as CIL. The incorporation of CuPc in the PDINN layer leads to better film morphology, increased conductivity, and reduced cathode work function, enabling greater CIL thickness tolerance and significantly improved photovoltaic performance of OSCs. Notably, the PM6:D18:L8‐BO‐based device using PDINN:F16CuPc as hybrid CIL yields a remarkable power conversion efficiency (PCE) of 20.17%, which is a significant improvement with regard to the PCE of 19.29% for the control device based on PDINN CIL. Particularly, this strategy demonstrates a universality in multiple photoactive layers and various perylene‐diimide‐based CILs, offering an effective approach to developing highly efficient OSCs.
The capability of cathode interlayer (CIL) in regulating the conductivity, interfacial dipole, and work function of electrode plays a critical role in determining the photovoltaic performance of organic solar cells 
 The capability of cathode interlayer (CIL) in regulating the conductivity, interfacial dipole, and work function of electrode plays a critical role in determining the photovoltaic performance of organic solar cells (OSCs). The widely used perylene‐diimide‐based CILs suffered from the inbuilt limitation of finite conductivity and poor thickness tolerance. To address this issue, we develop a universal strategy to finely optimize the functionality of perylene‐diimide‐type CIL (PDINN) by incorporating polyfluorine‐substituted copper phthalocyanine (CuPc) derivative to form hybrid CIL. It is found that the hydrogen bonding and π‐π interaction between PDINN and CuPc can address the solvent processability issue of CuPc used as CIL. The incorporation of CuPc in the PDINN layer leads to better film morphology, increased conductivity, and reduced cathode work function, enabling greater CIL thickness tolerance and significantly improved photovoltaic performance of OSCs. Notably, the PM6:D18:L8‐BO‐based device using PDINN:F16CuPc as hybrid CIL yields a remarkable power conversion efficiency (PCE) of 20.17%, which is a significant improvement with regard to the PCE of 19.29% for the control device based on PDINN CIL. Particularly, this strategy demonstrates a universality in multiple photoactive layers and various perylene‐diimide‐based CILs, offering an effective approach to developing highly efficient OSCs.
Abstract This study addresses the role of energetic offsets resulting from non‐fullerene acceptor crystallization/aggregation in stabilizing charge separation in organic bulk heterojunction (BHJ) solar cells. Devices are fabricated using PM6 
 Abstract This study addresses the role of energetic offsets resulting from non‐fullerene acceptor crystallization/aggregation in stabilizing charge separation in organic bulk heterojunction (BHJ) solar cells. Devices are fabricated using PM6 as electron donor and either IDIC or Y6 as acceptor, with blend ratios from 5:1 to 1:1. Reducing acceptor content significantly lowers device performance, most notably for initially higher performing PM6:Y6 BHJ's (from 14.31% to 0.95%) compared to PM6:IDIC (from 11.28% to 3.40%). Optical, optoelectronic, and morphological characterizations reveal that lower acceptor content PM6:Y6 devices exhibit suppressed acceptor aggregation/crystallinity, correlated with increased recombination losses and lower efficiency. Charge separation in optimal (1:1) PM6:Y6 devices is found to be stabilized by a LUMO level energetic offset between intermixed and pure, more crystalline, Y6 domains, driven by strong electronic interactions between Y6 molecules. In contrast, PM6:IDIC devices show minimal changes in energetics and recombination kinetics, aligning with their smaller performance decline, and consistent with IDIC's weaker electronic interactions. As such strong electronic interactions between Y6 molecules are concluded to provide an energetic stabilization of electrons in more aggregated/crystalline Y6 domains, suppressing charge recombination, and analogous to that observed for the highest performing fullerene acceptor PCBM.
Heterostructures are widely used in organic phototransistors (OPTs) to balance carrier dynamics, including exciton dissociation, transport, and recombination inhibition. Planar heterojunctions (PHJs) offer direct pathways and fewer recombination sites for 
 Heterostructures are widely used in organic phototransistors (OPTs) to balance carrier dynamics, including exciton dissociation, transport, and recombination inhibition. Planar heterojunctions (PHJs) offer direct pathways and fewer recombination sites for photo‐induced carriers. However, PHJ‐based OPTs' performance remains unsatisfactory due to challenges in achieving high‐quality organic planar interfaces with uniformity, large area, low roughness, and low defect density. Herein, a PHJ structure is designed for near‐infrared (NIR) photodetection. The PHJ consists of a polymer semiconductor, PDPPBTT, and a fullerene derivative, PC 61 BM. The PDPPBTT acts as the NIR photoactive layer, electron donor, and channel, while PC 61 BM is the acceptor. A simple evaporation technique is developed to deposit the PC 61 BM film on PDPPBTT to form a stable and uniform planar interface. Owing to the balanced dynamic characteristics, highly sensitive NIR photodetection is achieved as demonstrated by peak photosensitivity of 2.59 × 10 4 , photoresponsivity of 1.42 × 10 5 A W −1 , detectivity of 1.83 × 10 16 Jones upon weak irradiation of 0.072 ÎŒW cm −2 . To confirm the practicality of NIR imaging, a 7 × 7 array device is demonstrated. The results reveal a simple and effective strategy to prepare high‐performance PHJ‐based OPTs and provide insights into the development of advanced photodetection and imaging systems.
Abstract The cyano group is extensively employed in the molecular engineering of high‐performance small‐molecule acceptors (SMAs) for organic solar cells (OSCs) to fine‐tune energy levels and optimize molecular packing. To 
 Abstract The cyano group is extensively employed in the molecular engineering of high‐performance small‐molecule acceptors (SMAs) for organic solar cells (OSCs) to fine‐tune energy levels and optimize molecular packing. To date, the application of cyano group has predominantly been confined to end‐group modification in SMAs, with limited investigation in central unit engineering. Herein, in this work, the role of cyano substitution is systematically investigated in the central unit of SMAs and design a novel cyano‐functionalized wide‐bandgap acceptor UF‐BCN. The introduction of the cyano group significantly enhances the surface energy of the molecule and substantially deepens the highest occupied molecular orbital (HOMO) energy level due to its strong electron‐withdrawing capability, then leading to a blue‐shifted absorption. When introduced as the third component in the D18:BTP‐eC9, UF‐BCN demonstrates complementary light absorption, strong intermolecular interactions, and excellent compatibility with BTP‐eC9 to form a mixed acceptor phase, enabling it to function as an effective morphological modulator within the ternary system. Consequently, the ternary OSC based on D18:BTP‐eC9:UF‐BCN achieves an impressive power conversion efficiency (PCE) of 19.34%. This study underscores the effectiveness of cyano substitution in central unit engineering and highlights its potential for optimizing active layer morphology and enhancing the performance of ternary OSCs.
Dmitry Vyacheslavovich Kusaykin , V. T. Kuanyshev , Н. М. Đ‘Đ°Ń€Đ±ĐžĐœ | The Herald of the Siberian State University of Telecommunications and Information Science
Abstract This research employs inner side‐chain engineering in C‐shaped ortho‐benzodipyrrole‐based (CB) A‐D‐A non‐fullerene acceptors (NFAs) CB8, CB12, CB16, and CB20, where side‐chain configuration crucially influences self‐assembly, single‐crystal structures, and optoelectronic 
 Abstract This research employs inner side‐chain engineering in C‐shaped ortho‐benzodipyrrole‐based (CB) A‐D‐A non‐fullerene acceptors (NFAs) CB8, CB12, CB16, and CB20, where side‐chain configuration crucially influences self‐assembly, single‐crystal structures, and optoelectronic properties. The enthalpy of fusion at the melting point, combined with the intensity of the 730 nm solid‐state absorption shoulder, suggests that the acceptor–acceptor (A–A) interactions follow the order: CB8 &gt; CB12 &gt; CB20 &gt; CB16. Solution small‐ and wide‐angle X‐ray scattering (SWAXS) quantitatively reveals the successively increased donor–acceptor (D–A) association numbers of these CB derivatives with PM6, consistent with the reduction of their A–A self‐assembly. Complementarily and comprehensively, transient absorption spectroscopy (TAS) shows a systematically shortened decay‐time of charge transfer in the series of the binary PM6:CB (1:1.2 wt%) thin films, from 25.40 ps (CB8), to 16.13 ps (CB12), to 15.03 ps (CB20), and to 11.97 ps (CB16), following the increasing trend of CB‐PM6 interaction strength. Correspondingly, the photovoltaic efficiency improves with the enhanced CB‐PM6 interactions from PM6:CB8 (15.24%), to PM6:CB12 (16.66%), to PM6:CB20 (17.12%), and to PM6:CB16 (18.13%). These close correlations between the structures and photovoltaic properties elucidate the importance of minimizing A–A self‐aggregation and enhancing D (PM6)‐A (CBs) interactions via engineering the side chains in the CB‐based acceptors.
Abstract Measuring photoluminescence (PL) of free charge carriers under operation conditions is a valuable tool for characterizing solar cells. However, in organic solar cells, free charge carrier PL is typically 
 Abstract Measuring photoluminescence (PL) of free charge carriers under operation conditions is a valuable tool for characterizing solar cells. However, in organic solar cells, free charge carrier PL is typically obscured by the emission from non‐dissociated excitons. To overcome this, an adaptation of the time‐resolved PL measurement method is introduced that allows for the separate observation of the effects of applied voltage on the PL of excitons and free charge carriers. Using state‐of‐the‐art D18:Y6 and PM6:Y6 organic solar cells (power conversion efficiencies: and ), this study demonstrated: I) the determination of the implied voltage from free charge carrier PL under operation conditions providing insights into transport losses under steady‐state and transient conditions, II) the construction of a PL‐based current‐implied voltage curve revealing implied efficiencies of and ; III) an estimation of the photogenerated current at the maximum power point by combining PL and electroluminescence measurements, showing a reduction compared to the short‐circuit current, and IV) a discussion of possible origins of this reduction, including recombination due to limited transport, electrode‐induced charges and field‐dependent exciton dissociation. The introduced method thus provides a valuable diagnostic tool for identifying both transport and current losses in high‐efficiency organic solar cells.
ABSTRACT The aim of this study is to present a challenging insight into the molecular design and architecture optimization of two cost‐effective conjugated polymers and their adoptions in bulk heterojunction 
 ABSTRACT The aim of this study is to present a challenging insight into the molecular design and architecture optimization of two cost‐effective conjugated polymers and their adoptions in bulk heterojunction fullerene‐based solar cells. The new polymers, with repeating units based on symmetrically disubstituted polyalkyloxythiophenes have been prepared with simple procedures and have been employed as electron‐donor materials for polymer solar cells. A comparative study with monosubstituted polyalkyloxythiophene has evidenced a more favorable active morphology, improved charge mobility, and higher power conversion efficiency for the newly prepared disubstituted polymers. Photoconversion ability further increases when a thin layer of a cationic polyelectrolyte is coated on the surface of the photoactive blend, thus facilitating electron transport. Finally, the prepared polymers were evaluated according to a figure of merit based on their synthetic complexity and conversion efficiency, resulting in particularly suitable for large‐scale production.
Abstract The non-fullerene acceptors (NFAs) are dominating thin-film organic solar cells (TFOSCs) research, in recent years, because of their record high power conversion efficiency (PCE). Currently, the PCE of NFAs-based 
 Abstract The non-fullerene acceptors (NFAs) are dominating thin-film organic solar cells (TFOSCs) research, in recent years, because of their record high power conversion efficiency (PCE). Currently, the PCE of NFAs-based solar cells reaches 19.36%, which is much higher than the fullerene-based counterparts. The NFAs offer several advantages over the fullerene, and consequently, attracted a growing interest in the field of TFOSCs. The vast majority of the research reports are based on electron deficient acceptor–donor-acceptor (A-D-A) type small molecules that follow a simple synthesis route. A-D-A offers low photons energy losses resulting in high open-circuit voltage $$({V}_{oc})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mo>(</mml:mo> <mml:msub> <mml:mi>V</mml:mi> <mml:mrow> <mml:mi>oc</mml:mi> </mml:mrow> </mml:msub> <mml:mo>)</mml:mo> </mml:mrow> </mml:math> and tunable energy bandgaps for efficient collection of the charges. The effect of energy loss on the performance of non-fullerene based TFOSCs was deliberated in terms of changes in energy offset and morphology of the acceptor and donor molecules blend films. Controlling the energy loss and film morphology through material synthesis and new device structure can lead to more successful performance in TFOSCs. This review focuses on the recent research progress based on indacenodithiophene (IDT) and perylene diimides (PDIs) core donor moieties for the purpose of solar energy harvesting via solution-processed TFOSCs. The influence of the new molecule acceptors’ chemical and structural properties was deliberated based on tuning energy levels, film morphology, and charge mobility. Finally, the challenges of NFAs are also presented in summary and perspective.
The electrical performance of organic thin-film transistors (OTFTs) based on DNTT as the semiconductor active layer (DNTT, which stands for dinaphtho [2,3-b:2',3'-f] thieno [3,2-b] thiophene) is investigated and related to 
 The electrical performance of organic thin-film transistors (OTFTs) based on DNTT as the semiconductor active layer (DNTT, which stands for dinaphtho [2,3-b:2',3'-f] thieno [3,2-b] thiophene) is investigated and related to the structural properties of the organic films grown on SiO2 and Cytop substrates. Conventional current-voltage measurements and high-sensitivity low-frequency measurements show a lower mobility and correspondingly higher defect density for DNTT/SiO2 devices. Morphological and structural characterizations of DNTT films grown on the two dielectrics were performed using atomic force microscopy (AFM) and X-ray diffraction (XRD), revealing a highly ordered crystalline structure. Consistent with DFT simulation results, morphological analysis shows that the semiconductor films are layered, with DNTT molecules arranged with their longest axis perpendicular to the substrate. However, in only DNTT/SiO2 films, some molecules were found to be ordered and arranged parallel to the substrate. This "horizontal" orientation causes differences in charge transport properties in the semiconductor films grown on SiO2, reducing the field-effect mobility. TCAD simulations indicate that this horizontal molecular orientation can be modeled as highly defective regions at semiconductor grain boundaries, consistent with low-frequency noise measurement results.
The enhancement of the optoelectronic properties of organic conjugation materials through boron doping may reshape current understanding, with boron-doped polycyclic aromatic hydrocarbons (PAHs) poised to be high-performance organic optoelectronic materials. 
 The enhancement of the optoelectronic properties of organic conjugation materials through boron doping may reshape current understanding, with boron-doped polycyclic aromatic hydrocarbons (PAHs) poised to be high-performance organic optoelectronic materials. However, the impact of boron doping on charge transport remains underexplored. In this study, the effects of diboron doping, including both dense and dispersed doping, along with further π-extension on the electronic structure, stacking pattern, and charge transport of perylene-based PAHs were systematically investigated using density-functional theory. The results indicate that diboron doping can switch the molecular packing from herringbone to π-stacking, which increases the transfer integrals and significantly improves the mobility. Furthermore, it is revealed that intermolecular B···B and B···C interactions promote the formation of π-π stacking by symmetry-adapted perturbation theory and Hirshfeld surface analysis. In addition, densely doped B2-TBPA exhibits a one-dimensional intrinsic hole mobility of up to 40.86 cm2 V-1 s-1, while B2-HBP with π-extension and dispersed diboron doping exhibits pitched-π stacking, allowing it to display potential for bipolar transport. Monte Carlo and molecular dynamics simulations further demonstrate that diboron-doped PAHs offer more stable charge transport with reduced thermal disorder. This research provides new insights for the experimental design and synthesis of high-performance organic semiconductor devices.
We present a 3D multiparticle Monte Carlo simulation approach to model hopping transport in disordered organic materials and study the effect of organic magnetoresistance (OMAR). The model is based on 
 We present a 3D multiparticle Monte Carlo simulation approach to model hopping transport in disordered organic materials and study the effect of organic magnetoresistance (OMAR). The model is based on the bipolaron mechanism within a framework of strongly correlated disordered systems, incorporating both random hyperfine fields and an external magnetic field. The model includes the effects of exchange and short-range Coulomb interactions on magnetoresistance. Our results demonstrate that the shape of the magnetoresistance curve closely matches the experimentally observed Lorentzian profile. In particular, we identify a critical dependence of the OMAR sign on the interplay between the exchange interaction, Coulomb repulsion, and charge carrier concentration at room temperature. A transition from a positive to a negative OMAR is observed, correlated with the phase change from a paramagnetic phase at zero magnetic field to the formation of ferromagnetic ordering clusters under a finite magnetic field (B = 100 mT). These results highlight the essential role of carrier density in controlling the sign of OMAR, providing new insights into spin-dependent transport in organic semiconductors.
Abstract This study outlines a molecular design approach that entails integrating 3D structural motifs into the central core or terminal groups of fused‐ring acceptor molecules, specifically, LLZ1, LLZ2, and LLZ3–by 
 Abstract This study outlines a molecular design approach that entails integrating 3D structural motifs into the central core or terminal groups of fused‐ring acceptor molecules, specifically, LLZ1, LLZ2, and LLZ3–by incorporating a 3D architecture unit of norbornene. The objective is to modulate the aggregation behavior of these molecules by modifying their molecular structure, thereby enhancing the photoluminescence quantum yield (PLQY) values of the acceptor materials and reducing the non‐radiative recombination voltage loss in the corresponding devices. Our research findings demonstrate that the introduction of norbornene units effectively suppresses excessive molecular aggregation and significantly improves the PLQY values of the acceptor molecules. Further research has demonstrated that only the acceptor molecule LLZ1, characterized by both high PLQY and moderate crystallinity, can strike an optimal balance between the dual requirements of reducing voltage loss and enhancing charge transport in the device. Utilizing the preferred molecule LLZ1, we achieved a power conversion efficiency (PCE) of 18.0% in binary system and 20.4% in ternary device with much‐reduced voltage loss of 0.508V, which is among the highest values of current OSCs. In summary, this work provides novel insights and research directions for the development of OSCs with low voltage loss and high PCE.
Abstract In organic photovoltaics, even small morphological changes on the sub‐nanometer scale can significantly impact the device's performance. Such structural changes intrinsically occur due to the thermal response of a 
 Abstract In organic photovoltaics, even small morphological changes on the sub‐nanometer scale can significantly impact the device's performance. Such structural changes intrinsically occur due to the thermal response of a material, making a fundamental understanding of these processes essential. In this study, the thermal expansion of the high‐performance donor material PDBD‐T‐2F (PM6) is characterized using in situ transmission and grazing incidence wide‐angle X‐ray scattering (WAXS and GIWAXS) over the temperature range of 30–300 °C. By systematically increasing the complexity of the sample, multiple influencing factors are deciphered. Significantly, distinct structural differences and temperature expansion behavior is observed for the face‐on and edge‐on crystallite fraction. In particular, the initial lamellar stacking d ‐spacings differ for the two fractions and moreover, the face‐on fraction exhibits significantly lower thermal expansion in lamellar direction compared to the edge‐on fraction. In situ GIWAXS measurements performed during solution coating show that these differences are formed during film formation. Additionally, an impact of the thermal expansion mismatch between the substrate and the sample is observed, limiting the in‐plane π–π stacking expansion. The results emphasize the interplay between molecular packing, substrate interaction, and thermal response.
Comprehensive Summary The design and synthesis of high‐mobility n‐type near‐amorphous conjugated polymers (NACPs) represent a prominent research focus in organic semiconductors. The diketopyrrolopyrrole (DPP) unit is a widely used building 
 Comprehensive Summary The design and synthesis of high‐mobility n‐type near‐amorphous conjugated polymers (NACPs) represent a prominent research focus in organic semiconductors. The diketopyrrolopyrrole (DPP) unit is a widely used building block for constructing high‐mobility conjugated polymers. However, DPP‐based polymers often exhibit semi‐crystalline structures and inherent p‐type charge‐transport characteristics, which hinder their application in n‐type flexible electronic devices. To overcome these challenges, this study employs acceptor modulation and terpolymerization by integrating pyridine‐flanked DPP with 3,4‐difluorothiophene (2FT) and selenophene (Se) as comonomers. Besides, the incorporation of oligo(ethylene glycol) side chains is strategically designed to enhance polymer solubility and favorably modulate the morphology. Thus, a series of polymers, P2FT x ( x = 100–0), are synthesized via Stille polycondensation, enabling systematic investigation of the composition‐structure‐property relationships. It reveals that optimal Se incorporation minimizes torsional barriers and reduces backbone regularity, inducing a near‐amorphous phase with locally ordered domains while maintaining suitable energy levels for efficient electron transport. Notably, P2FT90 achieves the highest electron mobility of 0.47 cm 2 ·V ‐1 ·s ‐1 , highlighting the efficacy of this compositional engineering approach. This study exemplifies a synergistic approach that combines precise control of backbone regioregularity and energy‐level engineering to realize high‐performance n‐type NACPs.
Abstract Organic photovoltaics (OPVs) offer a promising solution for indoor energy harvesting. However, fundamental investigations to understand and optimize industrial processes such as roll‐to‐roll lamination for upscaling remain limited. This 
 Abstract Organic photovoltaics (OPVs) offer a promising solution for indoor energy harvesting. However, fundamental investigations to understand and optimize industrial processes such as roll‐to‐roll lamination for upscaling remain limited. This study investigates a critical failure mode in the upscaling of OPVs. One major challenge for thick semitransparent laminated OPV devices is current–voltage ( J–V ) asymmetry, where performance under cathode‐side illumination exceeds that under anode‐side illumination. X‐ray reflectivity, neutron reflectivity, and drift‐diffusion simulations reveal that a vertically stratified polymer‐rich region within the bulk of photoactive layers is the main cause of asymmetric J–V characteristics. Based on this fundamental understanding, a model is proposed to explain the mechanism, wherein electron extraction is hindered by the polymer‐rich region during anode illumination. By exploring upscaling‐compatible blends, cathode/anode‐balanced, high‐performing, and air‐stable semitransparent laminated OPVs are developed for indoor applications using commercially available PV‐X‐plus material. These findings provide valuable guidance for designing OPVs with balanced performance, facilitating roll‐to‐roll adoption and commercialization.
ConspectusOrganic π-conjugated molecules and polymers have emerged as some of the most promising candidates of semiconductors for future information, intelligent technology, and smart manufacturing because of their unique properties such 
 ConspectusOrganic π-conjugated molecules and polymers have emerged as some of the most promising candidates of semiconductors for future information, intelligent technology, and smart manufacturing because of their unique properties such as structural diversity, flexibility, stretchability, ultrathinness, light weight, low-cost and large-area fabrication procedures, and excellent biocompatibility. However, several severe challenges remain, including inferior optical and electronic properties compared to inorganic materials, poor stability and lifespan, low yields in solution processing patterning techniques, inadequate mechanical endurance, and difficulties in multifunctionalization. Particularly, there are still no big breakthroughs in terms of the common and long-term challenges, such as flexible organic light-emitting diodes (OLEDs) with printing procedures that could not be achieved at the calibration of commercialization, electrically pumped lasers that become the open global question, and organic integrated circuits and brain-like computing technologies at the conceptual stage. The nanosization of the molecular π systems is one crucial way to address the dilemmas that stem from the molecular limitation of organic semiconductors. Covalent nanoscale strategies of organic semiconducting π backbones enable not only effective suppression of phonon behavior, thereby significantly improving their charge transport capacity and exciton efficiency, but also facilitate functional integration for intelligent semiconductors.In this Account, the molecular gridization of the π backbone has been proposed to lock conformation and to reduce the entropy for ordering since the first reported discovery of organic nanogridarenes (ONGAs) in 2014. We comprehensively summarize the progress in the structural diversity of ONGAs, gridization rules, gridization effects on electron or exciton properties, and their application in organic devices within organic electronics. To date, we have defined six types of monogrids and synthesized a series of ONGA-based nanoatoms, including ladder-type, A-type, angle-lost-type, windmill-type, diamond-type, and tic-tac-toe ("[Formula: see text]")-type, as well as their nanomolecules of multigrids. The shape-sensitive gridization rule has been explored with the establishment of Friedel-Crafts, superelectrophile, C-H activation, and other C-C coupling gridizations, enabling precise control over their configuration and stereochemistry while achieving efficient yields. These gridization strategies not only allow for the exploration of ONGAs' diversity but also endow them with unique properties. Specifically, gridization effectively reduces the reorganization energy (ROE), and multigridization breaks through the lowest ROE of ∌28 meV in organic semiconductors. Moreover, gridization can modulate not only the glassy transition temperature and thermal stability but also the excited-state pathways, hole/electron mobility, dielectric characteristics, and ionic-electronic coupling behaviors. These unique attributes render ONGAs as organic quantum grid-dots with potential applications in flexible OLEDs and organic neuromorphic computing devices. Ultraviolet OLEDs have been achieved with a nanohydrocarbon of triangle ONGA that exhibits an external quantum efficiency (EQE) of ∌4.12%. Organic field-effect transistor (OFET) memory based on ladder-type ONGAs, which serve as single-component charge-memorable materials (CMMs), exhibit long-term retention time and fast writing speeds compared to those in devices based on ungridized counterparts, demonstrating the dramatic gridization effects at the device level. Finally, we discuss their future opportunities and challenges along the direction of organic electronic intelligence and their scaling supercycles based on artificially intelligent and robotic chemists (AiRCs).
Exciton dissociation in organic solar cells (OSCs) is primarily achieved through interfacial charge-transfer (CT) states, leading to a trade-off between open-circuit voltage ( V OC ) and short-circuit current ( 
 Exciton dissociation in organic solar cells (OSCs) is primarily achieved through interfacial charge-transfer (CT) states, leading to a trade-off between open-circuit voltage ( V OC ) and short-circuit current ( J SC ). Spatially dispersed delocalized singlet excitons (DSEs) in nonfullerene acceptors (NFAs) provide an alternative channel to promote charge generation without interfacial CT state. Here, we manipulate intermolecular interactions, carrier dynamics, and photovoltaic properties through selective asymmetric fluorination. Two asymmetric molecules, Z12 and Z13, were synthesized by substituting the terminal group with different fluorine atoms compared with the symmetrical molecule, Z11. Z12 showed enhanced molecular interactions, promoting to more compact and ordered stacking, which in turn promotes the DSE formation, benefiting the synergistic enhancement of V OC and J SC . The D18:Z12-based device achieved a remarkable power conversion efficiency of 19.5%, notably outperforming the other two devices. Our study indicates that controlling the molecular configuration by selective fluorination to enhance the DSE formation in NFAs is an effective strategy to achieve efficient OSCs.
Abstract Polymer solar cells, which include a blend of electron-donating conjugated polymers and electron-accepting molecules in the photovoltaic layer, have been widely studied as next-generation solar cells. To improve photocurrent 
 Abstract Polymer solar cells, which include a blend of electron-donating conjugated polymers and electron-accepting molecules in the photovoltaic layer, have been widely studied as next-generation solar cells. To improve photocurrent generation, it is necessary to harvest as many photons as possible in solar light, which distributes over a wide wavelength including the ultraviolet, visible, and near-infrared (near-IR) regions. However, covering such a wide solar spectrum by using binary blend polymer solar cells is inherently difficult because most organic materials (e.g., conjugated polymers) have a narrow absorption bandwidth (less than 200 nm). Ternary blend polymer solar cells can overcome this limitation by combining near-IR light-harvesting materials with the electron-donor conjugated polymer and the electron-acceptor molecule. In this review, recent progress in the development of polymer solar cells is briefly overviewed, followed by a detailed description of ternary blend polymer solar cells.
Abstract The efficiency of small‐area organic solar cells (OSCs) has now exceeded 20%, while mini‐modules have achieved efficiencies of over 17%. However, the performance of large area modules over 100 
 Abstract The efficiency of small‐area organic solar cells (OSCs) has now exceeded 20%, while mini‐modules have achieved efficiencies of over 17%. However, the performance of large area modules over 100 cm 2 still lags behind, largely due to the limitation of precisely controlling the film formation dynamics to achieve optimal crystallinity and nanomorphology. In this study, phase separation and polymer rheology are synergistically investigated during film formation. Using computational fluid dynamics (CFD) simulations and theoretical calculations, the film formation dynamics are thoroughly investigated in large‐area modules and propose a heat‐enhanced fast morphological evolution strategy (HF). This method mitigates excessive phase separation during large‐area film deposition, reduces non‐radiative recombination, and enhances charge carrier transport. Devices based on PM1:L8‐BO:BTP‐eC9 processed using a non‐halogenated high‐boiling point solvent exhibit a power conversion efficiency (PCE) of 20.3%, with the corresponding 110 cm 2 (active area of 100 cm 2 ) module achieving an efficiency of 13.1% (certified PCE of 12.7%). Finally, the potential applications of organic solar cell modules in environmental protection and medical fields are demonstrated.
Abstract Thermal processing is widely used in solution‐based coating techniques or to enhance solubility, yet the impact on supramolecular self‐assembly and thin film properties remains largely unexplored. Here, we demonstrate 
 Abstract Thermal processing is widely used in solution‐based coating techniques or to enhance solubility, yet the impact on supramolecular self‐assembly and thin film properties remains largely unexplored. Here, we demonstrate how heating and cooling cycles modulate the self‐assembly of amino acid‐appended perylene bisimides (PBIs), influencing their structural and optoelectronic properties. Using small‐angle neutron scattering (SANS), rheology, and absorption spectroscopy, we show that heating increases fibre flexibility while cooling results in spherical aggregate formation. Additionally, we demonstrate the impact of these changes on thin film performance using nanoindentation and voltammetry. When incorporated as electron transport layers (ETLs) in perovskite solar cells, heat‐cooling reduces the series resistance from 6.33 to 4.40 Ω∙cm 2 , enhancing device efficiency. Our findings highlight the importance of thermal history in supramolecular materials and emphasise the need for strict temperature control in solution‐based coating techniques to optimise optoelectronic device performance.