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Type-II multiferroic materials, in which ferroelectric polarization isinduced by inversion non-symmetric magnetic order, promise new and highlyefficient multifunctional applications based on the mutual control of magneticand electric properties. Although this phenomenon has to date been limited tolow temperatures, here we report a giant pressure-dependence of themultiferroic critical temperature in CuBr$_2$. At 4.5 GPa, $T_\mathrm{C}$ isenhanced from 73.5 to 162 K, to our knowledge the highest value yet reportedfor a non-oxide type-II multiferroic. This growth shows no sign of saturatingand the dielectric loss remains small under these high pressures. We establishthe structure under pressure and demonstrate a 60\% increase in the two-magnonRaman energy scale up to 3.6 GPa. First-principles structural and magneticenergy calculations provide a quantitative explanation in terms of dramaticallypressure-enhanced interactions between CuBr$_2$ chains. These large,pressure-tuned magnetic interactions motivate structural control in cuproushalides as a route to applied high-temperature multiferroicity.

Giant pressure-enhancement of multiferroicity in CuBr2