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Concepts and Applications of Nonlinear Terahertz Spectroscopy

Thomas Elsaesser, Klaus Reimann, Michael Woerner


Terahertz (THz) radiation with frequencies between 100 GHz and 30 THz has developed into an important tool of science and technology, with numerous applications in materials characterization, imaging, sensor technologies and telecommunications. Recent progress in THz generation has provided ultrashort THz pulses with electric field amplitudes of up to several megavolts/cm. This development opens the new research field of nonlinear THz spectroscopy, in which strong light-matter interactions are exploited to induce quantum excitations and/or charge transport and follow their nonequilibrium dynamics in time-resolved experiments. This book introduces methods of THz generation and nonlinear THz spectroscopy; discusses the relevant theoretical concepts; and presents prototypical, experimental and theoretical results in condensed matter physics. The potential of nonlinear THz spectroscopy is illustrated by recent research, including an overview of the relevant literature.

About Editors

Thomas Elsaesser is a director at the Max Born Institute in Germany, and a professor of experimental physics at the Humboldt University of Berlin.

Klaus Reimann has worked as a scientist at the Max Born Institute, in the field of ultrafast mid-infrared and THz spectroscopy, since 1999.

Michael Woerner is a department head at the Max Born Institute, and holds a lecturer qualification (habilitation) in physics at the Humboldt University of Berlin.

Table of Contents

About the Authors
1 Introduction
1.1 Linear Optical Response
1.2 Low-Energy Excitations in Condensed Matter
1.2.1 Electronic excitations
1.2.2 Vibrational excitations
1.3 Charge Transport in Solids
2 Terahertz Technology
2.1 Generation of Coherent Terahertz Radiation
2.1.1 Terahertz lasers
2.1.2 THz generation by optical frequency conversion
2.1.3 Photoconductive switches
2.2 Phase-Resolved Detection of Terahertz Transients
2.2.1 Photoconductive antennas
2.2.2 Electro-optic sampling
2.3 Linear Terahertz Spectroscopy and Imaging
3 Nonlinear Light-Matter Interactions
3.1 Nonlinear Optical Response in the THz Range
3.1.1 Theoretical framework
3.1.2 Approximations
3.2 Nonlinear Currents in Condensed Matter
3.2.1 Shift currents in systems lacking inversion symmetry
3.2.2 Nonlinear currents of electrons in a periodic potential
3.2.3 Nonlinear currents without real-space transfer of carriers
3.3 Quantum Coherences in Coupled Multi-Level Systems
3.4 Nonperturbative Regime of Light-Matter Interaction
4 Methods of Nonlinear Terahertz Spectroscopy
4.1 Concepts and Experimental Implementation
4.1.1 Optical geometries for nonlinear THz experiments
4.1.2 Interaction schemes and pulse sequences
4.2 Two-Dimensional Spectroscopy
4.2.1 Experimental methods of two-dimensional THz spectroscopy
4.2.2 Data representation and analysis
5 Nonlinear THz Spectroscopy of Condensed Matter
5.1 Low-Energy Excitations in Liquids and Solids
5.1.1 Condensed-phase molecular systems
5.1.2 Solids and nanostructures
5.2 Field-Driven Nonlinear Response and Charge Transport
5.2.1 Nonlinear THz response of softmodes in a molecular crystal
5.2.2 Polaron transport
5.2.3 Coherent high-field transport in GaAs on femtosecond time scales
5.2.4 THz-induced interband tunneling of carriers
5.2.5 Shift current in LiNbO3
5.2.6 Nonlinear transport in graphene
5.3 Conclusions and Outlook


Paperback ISBN: 9780750329682

Ebook ISBN: 9781643272153

DOI: 10.1088/2053-2571/aae931

Publisher: Morgan & Claypool Publishers


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