A study of electron and phonon dynamics by broadband two-dimensional THz time-domain spectroscopy

Abstract

In this thesis, the coherent phonons excited by THz pulses are experimentally demonstrated for the first time in both GaAs and InSb. The resonant excitation using THz pulses enables the coherent control of the lattice motion via direct interaction of atoms and electromagnetic wave, without inducing electronic transition as reported in the optical excitation of coherent phonons. The classic model is used to explain both excitation and detection mechanisms. An increase of the damping rate of the coherent lattice motion due to higher carrier density is observed in our experiment.

This thesis focuses on the linear and nonlinear interaction of the THz wave with semiconductors. Since a great many physical processes, including vibrational motion of lattice and plasma oscillation, has resonant frequency in the THz range, rich physics can be studies in our experiment. The thesis starts from the linear interaction of the THz wave with semiconductors. In the narrow band gap semiconductor InSb, the plasma absorption edge, Restrahlen band and dispersion of polaritons are observed. The nonlinear response of InSb in high THz field is verified in the frequency-resolved THz Z-scan experiment. The third harmonic generations due to the anharmonicity of plasma oscillation and the second order signal due to the plasma-phonon interaction are observed in 2D THz transmission spectra.

Terahertz (THz) wave interacts with semiconductors in many ways, such as resonant excitation of lattice vibration, intraband transition and polaron formation. Different from the optical waves, THz wave has lower photon energy (1 THz = 4.14 meV) and is suitable for studying dynamics of low-energy excitations. Recently the studies of the interaction of THz wave and semiconductors have been extending from the linear regime to the nonlinear regime, owing to the advance of the high-intensity THz generation and detection methods. Two-dimensional (2D) spectroscopy, as a useful tool to unravel the nonlinearity of materials, has been well developed in nuclear magnetic resonance and infrared region. However, the counterpart in THz region has not been well developed and was only demonstrated at frequency around 20 THz due to the lack of intense broadband THz sources. Using laser-induced plasma as the THz source, we developed collinear broadband 2D THz time-domain spectroscopy covering from 0.5 THz to 20 THz. Broadband intense THz pulses emitted from laser-induced plasma provide access to a variety of nonlinear properties of materials. Ultrafast optical and THz pulses make it possible to resolve the transient change of the material properties with temporal resolution of tens of femtoseconds.

Transient reflectivity change of GaAs induced by THz pulses is studied in 2D THz-pump/optical-probe configuration. Using the perturbative analysis of nonlinear electro-optic effect, we conclude that the nonlinear response of GaAs to two phase-locked THz pulses is mainly caused by the nonlinearity of the electronic response.