Disentangling Electronic and Ionic Nonlinear Polarization Effects in the THz Kerr Response of LaAlO$_{3}$

TL;DR

This study uses 2D Terahertz Kerr effect spectroscopy and modeling to distinguish genuine ionic oscillations from electronic responses in LaAlO$_{3}$, revealing complex propagation effects and refining interpretation of THz polarization dynamics.

Contribution

It introduces a combined experimental and modeling approach to disentangle electronic and ionic nonlinear polarization effects in THz Kerr responses of birefringent crystals.

Findings

Identified the 1.1 THz mode as $E_g$ Raman phonon.

Attributed 0.86 THz and 0.36 THz signals to propagation effects.

Showed $E_g$ mode is excited via a two-photon process.

Abstract

Nonlinear responses to intense terahertz (THz) fields provide unique insights into complex dynamics of contemporary material systems. However, the interpretation of the obtained data, in particular, distinguishing genuine ionic oscillations from the instantaneous electronic responses in THz Kerr effect remains challenging. Here, we combine two-dimensional Terahertz Kerr effect (2D-TKE) spectroscopy experiments and their modeling to unravel complex THz-induced temporal oscillations in twinned LaAlO$_3$ crystals at low temperatures. We identify the 1.1 THz mode as $E_g$ Raman phonon, while 0.86 THz and 0.36 THz signals are due to spurious effects resulting from the co- and counter-propagation of THz and optical probe pulses in birefringent twin domains. Furthermore, we determine that the $E_g$ mode is excited via a two-photon process, whereas THz pulse reflections at the sample surface produce a temporal response that can mimic anharmonic phonon coupling. Our findings highlight the importance of propagation effects in nonlinear THz experiments and provide a refined framework for interpreting THz polarization dynamics in birefringent crystals.