High-amplitude, ultrashort strain solitons in solids

In recent years, pressure pulses of very short (picosecond) time duration have found wide application as a diagnostic tool in the semiconductor industry and in fundamental condensed matter research. Next to their application in the studies of nanometer-sized structures, propagation of these short acoustic pulses over millimeter distances at low temperatures has revealed a new field of picosecond acoustics. It has been shown that, for very short strain pulses, phonon dispersion destroys the internal structure of the coherent wavepacket by pulling apart its different frequency components. However, when strain amplitudes are sufficiently increased, a nonlinear pulse-steepening mechanism emerges, that leads to the formation of shock waves. The combined action of the nonlinear and dispersive effects then results in the formation of stable, highly localized solitary waves. In this thesis, we study the development of picosecond pressure pulses into trains of ultrashort acoustic solitons in a bulk crystal. The high-amplitude, bipolar strain wavepackets are generated by femtosecond optical excitation of a thin chromium film evaporated onto the crystal, using high-power optical pulses from an amplified Ti:sapphire laser. Propagation over millimeter distances at low temperatures is studied by means of two complementary experimental methods. First, the development of low-frequency, gigahertz strain components is monitored using Brillouin light-scattering. By monitoring the scattered intensity against traveled distance of the packets, we demonstrate the breakup of the initial single-cycle pulse into an ultrashort acoustic soliton train, reaching transient pressures up to tens of kilobars and soliton widths less than 0.5 picoseconds, corresponding to only several nanometers in the crystal. Further, we show that the ultrashort strain solitons interact coherently with local electronic two-level systems at terahertz frequency, in optically excited ruby. The strain-induced electronic population can be monitored using the well-known R1- and R2-luminescence lines of the excited Cr3+ impurity-ions in the ruby crystal. Coherent manipulation, and even amplification, of terahertz strain wavepackets using an electronic two-level medium appears well within reach. Finally, we present a novel picosecond ultrasonics setup based on our low-repetition laser system and demonstrate its operation by determining the initial shape of the acoustic wavepacket in the chromium transducer