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Pressure tuning of bond-directional exchange interactions and magnetic frustration in the hyperhoneycomb iridate <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>β</mml:mi><mml:mo>−</mml:mo><mml:msub><mml:mi>Li</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi>IrO</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>
We explore the response of Ir $5d$ orbitals to pressure in $\ensuremath{\beta}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$, a hyperhoneycomb iridate in proximity to a Kitaev quantum spin-liquid (QSL) ground state. X-ray absorption spectroscopy reveals a reconstruction of the electronic ground state below 2 GPa, the same pressure range where x-ray magnetic circular dichroism shows an …