Andrea Cavalleri

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.

Abstract:

We report on the generation of narrowband carrier-envelope phase stable mid-infrared (MIR) pulses between 10 and 15 μm. High pulse energies and narrow bandwidths are required for the selective nonlinear excitation of collective modes of matter that is not possible with current sources. We demonstrate bandwidths of <2% at 12.5 μm wavelength through difference frequency generation between two near-infrared (NIR) pulses, which are linearly chirped. We obtain a reduction in bandwidth by one order of magnitude, compared to schemes that make use of transform-limited NIR pulses. The wavelength of the narrowband MIR pulse can be tuned by changing the optical delay between the two chirped NIR pulses.