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We present magnetization measurements carried out on polycrystalline andsingle-crystalline samples of $\alpha$-Li$_2$IrO$_3$ under hydrostaticpressures up to 2 GPa and establish the temperature-pressure phase diagram ofthis material. The N\'eel temperature ($T_{\rm{N}}$) of $\alpha$-Li$_2$IrO$_3$is slightly enhanced upon compression with $dT_{\rm{N}}/dp$ = 1.5 K/GPa. Above1.2 GPa, $\alpha$-Li$_2$IrO$_3$ undergoes a first-order phase transition towarda nonmagnetic dimerized phase, with no traces of the magnetic phase observedabove 1.8 GPa at low temperatures. The critical pressure of the structuraldimerization is strongly temperature-dependent. This temperature dependence iswell reproduced on the ab initio level by taking into account lower phononentropy in the nonmagnetic phase. We further show that the initial increase in$T_{\rm{N}}$ of the magnetic phase is due to a weakening of the Kitaevinteraction $K$ along with the enhancement of the Heisenberg term $J$ andoff-diagonal anisotropy $\Gamma$. Our study reveals a common thread in theinterplay of magnetism and dimerization in pressured Kitaev materials.

Pressure-induced dimerization and collapse of antiferromagnetism in the Kitaev material $\alpha$-Li$_2$IrO$_3$