A strategy to identify materials exhibiting a large nonlinear phononics response: tuning the ultrafast structural...

We use theory and first-principles calculations to investigate how structural changes induced by ultrafast optical excitation of infrared-active phonons change with hydrostatic pressure in LaAlO₃. Our calculations show that the observed structural changes are sensitive to pressure, with the largest changes occurring at pressures near the boundary between the cubic perovskite and rhombohedral phases. We rationalize our findings by defining a figure of merit that depends only on intrinsic materials quantities, and show that the peak response near the phase boundary is dictated by different microscopic materials properties depending on the particular phonon mode being excited. Our work demonstrates how it is possible to systematically identify materials that may exhibit particularly large changes in structure and properties due to optical excitation of infrared-active phonons.