Nonlinear Terahertz Spectroscopy of Electronic and Vibrational Responses in Condensed Matter Systems

Nonlinear Terahertz Spectroscopy of Electronic and Vibrational Responses in Condensed Matter Systems

Author: Harold Young Hwang

Publisher:

Published: 2012

Total Pages: 231

ISBN-13:

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In this work, I describe experiments utilizing high-field terahertz (THz) pulses to initiate nonlinear responses in several classes of materials. We have developed several methods for interrogating the nonlinear THz response of materials including collinear and noncollinear THz-pump/THz-probe spectroscopy, and THz-pump/optical probe spectroscopies including THz Kerr effect spectroscopy. We have observed nonlinear free-carrier absorption, occurring through the saturation of free-carrier mobility in bulk semiconductors. We have demonstrated that highly energetic electrons in the conduction band can generate electron-hole pairs in indium antimonide, and have elucidated the dynamics of the carrier generation process. We have observed nonlinear conductivity responses in graphene, showing that a strong THz pulse can heat the electron distribution leading to saturable absorption in the THz range. We have demonstrated THz-induced optical anisotropy in simple liquids, allowing for the measurement of subsequent orientational dynamics. We have driven nonlinear vibrational dynamics in ferroelectrics, demonstrating that the strong anharmonicity of lattice vibrational modes can induce an anisotropic optical response. We have begun to study nonlinear vibrational responses in molecular crystals, which is of importance in mode coupling and energy transfer processes in the THz range. Finally, we have driven nonlinear metamaterial responses in gallium arsenide and vanadium dioxide. In GaAs, we have shown that metamaterial properties may be tuned by an intense THz field if the substrate material (GaAs) is changed by the incident THz pulse, and we have demonstrated carrier multiplication locally in the metamaterial split ring resonator gaps where substantial electric field enhancement occurs. In VO2, we have shown that THz radiation can drive an insulator-to-metal phase transition, opening up new possibilities in the control of the states of matter with THz fields. This work has demonstrated only a few of the capabilities made possible by the interaction of intense THz radiation with matter, and provides a general framework to open up new research in a nascent field.


Concepts and Applications of Nonlinear Terahertz Spectroscopy

Concepts and Applications of Nonlinear Terahertz Spectroscopy

Author: Thomas Elsaesser

Publisher: Morgan & Claypool Publishers

Published: 2019-02-22

Total Pages: 159

ISBN-13: 1643272160

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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 in a tutorial way, 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.


Terahertz-field-induced Nonlinearity in Phonons, Electrons and Spins

Terahertz-field-induced Nonlinearity in Phonons, Electrons and Spins

Author: Xian Li (Ph.D.)

Publisher:

Published: 2019

Total Pages: 210

ISBN-13:

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In this thesis, I describe work aimed at understanding nonlinear material responses initiated by strong terahertz (THz) field excitation. I discuss two aspects of nonlinear THz spectroscopy in condensed-matter materials: developments of experimental THz capabilities and spectroscopy methods and their applications in investigating ultrafast nonlinear dynamics in different classes of materials. I first describe the THz generation, detection and spectroscopy methods, which are the basis of all of our studies. We have generated strong single- and multi-cycle THz pulses covering several spectral ranges using inorganic and organic crystals and developed linear and nonlinear THz spectroscopy techniques to interrogate light-matter interactions based on different observables and/or symmetry criteria. We have demonstrated a new method for studying time-domain electron paramagnetic resonance that allows us to measure THz-frequency fine structures of spin energy levels on a tabletop and have developed nonlinear two-dimensional (2D) magnetic resonance spectroscopy to distinguish nonlinear THz-spin interaction pathways. We also show that THz-pump, optical-probe spectroscopy, including THz field-induced second-harmonic generation spectroscopy and THz Kerr effect spectroscopy, can be extended to study phase transitions in quantum paraelectric and topological materials. We have employed the THz methods to drive and detect nonlinear responses from several degrees of freedom in the materials. We have demonstrated collective coherent control over material structure by inducing a quantum paraelectric to ferroelectric phase transition using intense THz electric fields in strontium titanate. We show that a single-cycle THz field is able to drive ions along the microscopic pathway leading directly to their locations in a new crystalline phase on an ultrafast timescale. We have driven highly nonlinear lattice and electronic responses in a topological crystalline insulator by dynamically perturbing the protecting crystalline symmetry through THz phonon excitation. We have observed oscillations in optical reflectivity that may be associated with electronic gap opening and modulation in the topological surface states. Finally, we have demonstrated nonlinear manipulation of collective spin waves in a canted antiferromagnet using strong THz magnetic fields and we have observed full sets of the second- and third-order nonlinear responses in 2D THz magnetic resonance spectra, which are accurately reproduced in our numerical simulations.


Nonlinear Low-frequency Excitations of Condensed Matter Studied by Two-dimensional Terahertz Spectroscopy

Nonlinear Low-frequency Excitations of Condensed Matter Studied by Two-dimensional Terahertz Spectroscopy

Author: Matthias Runge

Publisher:

Published: 2024*

Total Pages: 0

ISBN-13:

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Englische Version: This thesis exploits techniques of terahertz (THz) spectroscopy to investigate nonlinear low-frequency excitations of condensed matter. In particular, application of two-dimensional (2D) THz spectroscopy allows to disentangle different nonlinear signal contributions. The nonlinear polaronic response of solvated electrons and their surrounding solvent molecules in the polar liquid isopronal is studied. Solvated electrons are generated via multiphoton ionization. Longitudinal polaron oscillations with THz frequencies are impulsively excited during the ultrafast localization of the electrons. Perturbation of such polaron oscillations with an external THz pulse induces nonlinear changes of the transverse polaron polarizability, reflected in distinct modifications to the oscillation phase as mapped in 2D-THz experiments. Further, the generation of mono-cycle THz pulses from asymmetric semiconductor quantum wells upon resonant intersubband excitation in the mid-infrared (MIR) range is demonstrated. The temporal shape of the emitted THz electric field is modified by controlling pulse duration and peak electric field of the MIR driving pulses. Phase-resolved 2D-MIR experiments confirm that the THz emission is predominantly due to a nonlinear shift current generated upon femtosecond intersubband excitation. The influence of combined intra- and interband currents on symmetry properties, which opens novel quantum pathways for phonon excitation in narrow-band-gap materials, is demonstrated by 2D-THz experiments on bismuth. Nonperturbative long-wavelength excitation of charge carriers close to the L points leads to an anisotropic carrier distribution, reflected in a six-fold azimuthal angular dependence of the pump-induced change of THz transmission.[...].


Enhanced Polarisation Control and Extreme Electric Fields

Enhanced Polarisation Control and Extreme Electric Fields

Author: Connor Devyn William Mosley

Publisher: Springer Nature

Published: 2021-03-25

Total Pages: 125

ISBN-13: 3030669025

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This thesis reports advances in terahertz time-domain spectroscopy, relating to the development of new techniques and components that enhance the experimentalist’s control over the terahertz polarisation state produced by photoconductive emitters. It describes how utilising the dynamic magnetoelectric response at THz frequencies, in the form of electromagnons, can probe material properties at a transition between two magnetically ordered phases. Additionally, preliminary investigations into the properties of materials exposed to extreme terahertz optical electric fields are reported. The work presented in this thesis may have immediate impacts on the study of anisotropic media at THz frequencies, with photoconductive emitters and detectors being the most commonly used components for commercially available terahertz spectroscopy and imaging systems, and by providing a new way to study the nature of magnetic phase transitions in multiferroics. In the longer term the increased understanding of multiferroics yielded by ultrafast spectroscopic methods, including terahertz time-domain spectroscopy, may help develop new magnetoelectric and multiferroic materials for applications such as spintronics.


Developments and Advances in Nonlinear Terahertz Spectroscopy

Developments and Advances in Nonlinear Terahertz Spectroscopy

Author: Nathaniel Curran Brandt

Publisher:

Published: 2014

Total Pages: 176

ISBN-13:

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Nonlinear terahertz (THz) spectroscopy is a rapidly developing field, which is concerned with driving and observing nonlinear material responses in the THz range of the electromagnetic spectrum. In this thesis, I present several advances in nonlinear THz spectroscopy that expand the range of systems in which responses may be driven, the types of responses that may be initiated, and the way in which these responses may be observed. Sufficiently strong THz pulses are generated using the tilted-pulse-front technique, and are collected, focused, and detected using a THz spectrometer specifically designed for maximum peak THz electric field strength and maximum flexibility, allowing for a wide range of experimental geometries to be implemented. Further enhancement in the peak THz electric field strength is obtained through the use of metamaterial structures, which concentrate free-space THz fields in their antenna gaps. Impact ionization was observed in high-resistivity silicon, a material in which no nonlinear THz response had been previously seen, using metamaterial structures to enhance free space THz electric fields. Using three-dimensional metamaterial structures, the THz magnetic field is shown to also be capable of driving ionization processes both in high-resistivity silicon as well as air. Using metamaterial structures with open gaps, the THz electric field is shown to induce breakdown in air at both high and low pressures due to field ionization processes involving the gold metamaterial antennas. Furthermore, THz-driven electromigration of the gold metamaterial antennas is observed. Probing of THz-driven structural changes in both vanadium dioxide and perovskite ferroelectrics is demonstrated using femtosecond Xray pulses from the LCLS facility at the SLAC National Accelerator Laboratory. Finally, ongoing results involving energetic materials, stimulated Raman measurements, and Stark effect measurements are discussed. This work, coupled with the ongoing expansion of nonlinear THz techniques and potential applications demonstrates the continued development of nonlinear THz spectroscopy into a robust and valuable method for investigating fundamental processes in a multitude of systems.


Time-resolved THz Studies of Carrier Dynamics in Semiconductors, Superconductors, and Strongly-correlated Electron Materials

Time-resolved THz Studies of Carrier Dynamics in Semiconductors, Superconductors, and Strongly-correlated Electron Materials

Author:

Publisher:

Published: 2006

Total Pages:

ISBN-13:

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Perhaps the most important aspect of contemporary condensed matter physics involves understanding strong Coulomb interactions between the large number of electrons in a solid. Electronic correlations lead to the emergence of new system properties, such as metal-insulator transitions, superconductivity, magneto-resistance, Bose-Einstein condensation, the formation of excitonic gases, or the integer and fractional Quantum Hall effects. The discovery of high-Tc superconductivity in particular was a watershed event, leading to dramatic experimental and theoretical advances in the field of correlated-electron systems. Such materials often exhibit competition between the charge, lattice, spin, and orbital degrees of freedom, whose cause-effect relationships are difficult to ascertain. Experimental insight into the properties of solids is traditionally obtained by time-averaged probes, which measure e.g., linear optical spectra, electrical conduction properties, or the occupied band structure in thermal equilibrium. Many novel physical properties arise from excitations out of the ground state into energetically higher states by thermal, optical, or electrical means. This leads to fundamental interactions between the system's constituents, such as electron-phonon and electron-electron interactions, which occur on ultrafast timescales. While these interactions underlie the physical properties of solids, they are often only indirectly inferred from time-averaged measurements. Time-resolved spectroscopy, consequently, is playing an ever increasing role to provide insight into light-matter interaction, microscopic processes, or cause-effect relationships that determine the physics of complex materials. In the past, experiments using visible and near-infrared femtosecond pulses have been extensively employed, e.g. to follow relaxation and dephasing processes in metals and semiconductors. However, many basic excitations in strongly-correlated electron systems and nanoscale materials occur at lower energies. The terahertz (THz) regime is particularly rich in such fundamental resonances. This includes ubiquitous lattice vibrations and low-energy collective oscillations of conduction charges. In nanoscale materials, band structure quantization also yields novel infrared and THz transitions, including intersubband absorption in quantum wells. The formation of excitons in turn leads to low-energy excitations analogous to inter-level transitions in atoms. In transition-metal oxides, fundamental excitation gaps arise from charge pairing into superconducting condensates and other correlated states. This motivates the use of ultrafast THz spectroscopy as a powerful tool to study light-matter interactions and microscopic processes in nanoscale and correlated-electron materials. A distinct advantage of coherent THz pulses is that the amplitude and phase of the electric field can be measured directly, as the THz fields are coherent with the fs pulses from which they are generated. Using THz time-domain spectroscopy (THz-TDS), both the real and imaginary parts of the response functions (such as the dielectric function) are obtained directly without the need for Kramers?Kronig transforms. The THz response can also be expressed in terms of absorption and refractive index, or as the optical conductivity. The optical conductivity describes the current response of a many-body system to an electric field, an ideal tool to study conducting systems. A second important advantage is the ultrafast time resolution that results from the short temporal duration of the THz time-domain sources. In particular, optical-pump THz-probe spectroscopy enables a delicate probe of the transient THz conductivity after optical photoexcitation. These experiments can provide insight into quasiparticle interactions, phase transitions, or nonequilibrium dynamics. In this chapter we will provide many such examples. Since THz spectroscopy of solids is a quickly expanding field.


Intense Terahertz Excitation of Semiconductors

Intense Terahertz Excitation of Semiconductors

Author: Sergey Ganichev

Publisher: OUP Oxford

Published: 2005-12-15

Total Pages: 432

ISBN-13: 0191523747

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Intense Terahertz Excitation of Semiconductors presents the first comprehensive treatment of high-power terahertz applications to semiconductors and low-dimensional semiconductor structures. Terahertz properties of semiconductors are in the center of scientific activities because of the need of high-speed electronics. This research monograph brigdes the gap between microwave physics and photonics. It focuses on a core topic of semiconductor physics providing a full description of the state of the art of the field. _ The reader is introduced to new physical phenomena which occur in the terahertz frequency range at the transition from semi-classical physics with a classical field amplitude to the fully quantized limit with photons. The book covers a wide range of optical, optoelectronic, and nonlinear transport processes, presenting experimental results, clearly visualizing models and basic theories. Background information for future work and exhaustive references of current literature are given. A particularly valuable feature is through the discussion of various technical aspects of the terahertz range like the generation of high-power coherent radiation, optical components, instrumentation, and detection schemes of short intense radiation impulses. The book complements, for the first time in form of a monograph, previous books on infrared physics which dealt with low-power optical and opto-electronic processes. It will be useful not only to scientists but also to advanced students who are interested in terahertz research.


The Generation of High Field Terahertz Radiation and Its Application in Terahertz Nonlinear Spectroscopy

The Generation of High Field Terahertz Radiation and Its Application in Terahertz Nonlinear Spectroscopy

Author: Ka-Lo Yeh

Publisher:

Published: 2009

Total Pages: 155

ISBN-13:

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In this thesis research, I implemented a terahertz generation scheme that enables high-field near-single-cycle terahertz (THz) pulse generation via optical rectification in a LiNbO3 (LN) crystal. I also developed a method for the non reconfigurable generation of high-intensity multiple-cycle THz fields aimed to more efficiently deliver THz energy to resonant samples. A novel free-space THz-pump/THz-probe setup enabled time-resolved measurement of ultrafast nonlinear electronic responses in doped bulk semiconductor samples. The ability to spectrally and temporally resolve the response of the semiconductor sample using a THz probe allowed us to uncover both the dynamics of impact ionization and interesting phonon-plasma interactions in indium antimonide (InSb) for the first time. Nonlinear vibrational responses in LN were ob-served first in a dual THz beam setup on an integrated LN waveguide platform with optical probing to reveal the generation of terahertz second harmonic signals and also in THz transmission measurements in cooled LN where THz intensity-dependent self-phase modulation and harmonic generation were observed. An outlook and preliminary results toward implementation and observation of high-field THz-driven responses in ferroelectric materials are given in the final chapter of this thesis.