Andrea Cavalleri

Abstract:

Crystal lattice fluctuations, which are known to influence phase transitions of quantum materials in equilibrium, are also expected to determine the dynamics of light-induced phase changes. However, they have only rarely been explored in these dynamical settings. Here we study the time evolution of lattice fluctuations in the quantum paraelectric SrTiO3, in which mid-infrared drives have been shown to induce a metastable ferroelectric state. Crucial in these physics is the competition between polar instabilities and antiferrodistortive rotations, which in equilibrium frustrate the formation of long-range ferroelectricity. We make use of high-intensity mid-infrared optical pulses to resonantly drive the Ti–O-stretching mode at 17 THz, and we measure the resulting change in lattice fluctuations using time-resolved X-ray diffuse scattering at a free-electron laser. After a prompt increase, we observe a long-lived quench in R-point antiferrodistortive lattice fluctuations. Their enhancement and reduction are theoretically explained by considering the fourth-order nonlinear phononic interactions to the driven optical phonon and third-order coupling to lattice strain, respectively. These observations provide a number of testable hypotheses for the physics of light-induced ferroelectricity.

Abstract:

Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena, which to date have been primarily studied with ultrafast optical, X-Ray and photo-emission spectroscopy. However, little has been done to characterize their transient electrical responses, which are directly associated with the functionality of these materials. Especially interesting are linear and nonlinear current-voltage characteristics at frequencies below 1 THz, which are not easily measured at picosecond temporal resolution. Here, we report on ultrafast transport measurements in photo-excited K₃C₆₀. Thin films of this compound were connected to photo-conductive switches with co-planar waveguides. We observe characteristic nonlinear current-voltage responses, which in these films point to photo-induced granular superconductivity. Although these dynamics are not necessarily identical to those reported for the powder samples studied so far, they provide valuable new information on the nature of the light-induced superconducting-like state above equilibrium T_c. Furthermore, integration of non-equilibrium superconductivity into optoelectronic platforms may lead to integration in high-speed devices based on this effect.