Andrea Cavalleri

Abstract:

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa₂Cu₃O_6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO₂ planes. The empty chain Cu dy²-z² orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these results, we calculate changes in the soft x-ray absorption spectra at the Cu L-edge. Femtosecond x-ray pulses from a free electron laser are used to probe changes in absorption at two photon energies along this spectrum and provide data consistent with these predictions.

Abstract:

We report on the demonstration of ultrafast optical reversal of the ferroelectric polarization in LiNbO_{3}. Rather than driving the ferroelectric mode directly, we couple to it indirectly by resonant excitation of an auxiliary high-frequency phonon mode with femtosecond midinfrared pulses. Because of strong anharmonic coupling between these modes, the atoms are directionally displaced along the ferroelectric mode and the polarization is transiently reversed, as revealed by time-resolved, phase-sensitive, second-harmonic generation. This reversal can be induced in both directions, a key prerequisite for practical applications.

Abstract:

We study the response of the one-dimensional charge density wave in K_{0.3}MoO_{3} to different types of excitation with femtosecond optical pulses. We compare direct excitation of the lattice at midinfrared frequencies with injection of quasiparticles across the low energy charge density wave gap and with charge transfer excitation in the near infrared. For all three cases, we observe a fluence threshold above which the amplitude-mode oscillation frequency is softened and the mode becomes increasingly damped. We show that all the data can be collapsed onto a universal curve in which the melting of the charge density wave occurs abruptly at a critical lattice excursion. These data highlight the existence of a universal stability limit for a charge density wave, reminiscent of the Lindemann criterion for the melting of a crystal lattice.