A Strategy to Identify Materials Exhibiting a Large Nonlinear Phononics Response: Tuning the Ultrafast Structural Response of LaAlO$_3$ with Pressure

TL;DR

This paper combines theory and first-principles calculations to explore how hydrostatic pressure influences ultrafast structural changes in LaAlO$_3$, identifying conditions for large nonlinear phononics responses near phase boundaries.

Contribution

It introduces a systematic approach to identify materials with large ultrafast structural responses by analyzing pressure-dependent phononic behavior using a new figure of merit.

Findings

Structural changes are highly sensitive to pressure, especially near phase boundaries.

The peak nonlinear response depends on specific microscopic material properties.

The method can guide the discovery of materials with large optically induced structural changes.

Abstract

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 LaAlO$_3$. 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.