Author: Wilhelm KühnPublisher:
ISBN:
Category :
Languages : en
Pages : 165
Book Description
Nonlinear Terahertz Spectroscopy in One and Two Dimensions
Author: Wilhelm KühnConcepts and Applications of Nonlinear Terahertz Spectroscopy
Author: Thomas ElsaesserPublisher: Morgan & Claypool Publishers
ISBN: 1643272160
Category : Science
Languages : en
Pages : 159
Book Description
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.
Nonlinear Low-frequency Excitations of Condensed Matter Studied by Two-dimensional Terahertz Spectroscopy
Author: Matthias RungePublisher:
ISBN:
Category :
Languages : en
Pages : 0
Book Description
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.[...].
Developments and Advances in Nonlinear Terahertz Spectroscopy
Author: Nathaniel Curran BrandtPublisher:
ISBN:
Category :
Languages : en
Pages : 176
Book Description
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.
Nonlinear Terahertz Interactions in Two Dimensional Systems
Author: Sayyed Hadi Razavi-PourPublisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
"Reducing the dimensionality of a material from 3D to 2D introduces new quantum effects that can be exploited to see new physics and produce new devices. Two examples of such materials are graphene, a single layer of carbon atoms, and quantum well heterostructures confining charges to a planar potential well. A powerful method for observing charge transport in these 2D materials is time-resolved terahertz (THz) spectroscopy, using picosecond pulses of far-infrared light to measure the complex valued ac conductivity. In this thesis, THz spectroscopy is used to study the linear and nonlinear electrodynamic response of two 2D systems: graphene and self-assembled metal halide perovskite quantum wells. In graphene, THz field-induced bleaching is studied, found to be well described by simple phenomenological reduction in intraband absorption using a free carrier Drude model that includes neutral and charged impurity scattering as well as optical phonon scattering. The Fermi level dependence of this nonlinearity is studied for the first time, which allows us to separate the contributions of long and short range momentum scattering and map their dependence on the field amplitude. We find, contrary to previous work, that the increase in scattering cannot be explained by an increase in the lattice temperature alone and that other mechanisms such as carrier-carrier scattering must be accounted for to explain the effect. Our results provide a deeper understanding of transport in graphene devices operating at THz frequencies and in modest kV/cm field strengths present in most devices. Second, time-resolved multi-THz spectroscopy was used to investigate carrier dynamics in 2D organic metallic halide perovskite (OMHP) systems. The 2D OMHPs are promising photovoltaic materials showing reduced sensitivity to environmental degradation, however their photoconductivity response has been unexplored on ultrafast time scales. We observed a rapid decay of injected photocarriers on a 10-100 ps time scale, indicating a significant trap/decay channel that limits device performance. Supporting hyperspectral photoluminescent imaging measurements confirm the band gap shift of the naturally formed quantum wells, however also show significant surface structural defects serving as monomolecular traps. We show how mono-molecular, bimolecular and Auger constants are sensitive to the changes in the electronic confinement of the quantum wells, of importance to devices attempting to exploit their tunable optical properties and environmental stability." --
Nonlinear Terahertz Spectroscopy of Electronic and Vibrational Responses in Condensed Matter Systems
Author: Harold Young HwangPublisher:
ISBN:
Category :
Languages : en
Pages : 231
Book Description
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.
Nonlinear Terahertz Spectroscopy and Imaging of Carbon Nanomaterials
Author: Byounghwak LeePublisher:
ISBN:
Category : Carbon nanotubes
Languages : en
Pages : 118
Book Description
This dissertation presents nonlinear terahertz (THz) properties of carbon nanomaterials investigated by time-resolved high-field THz spectroscopy. In order to determine THz characteristics of nanomaterials, we performed THz power spectrum measurement, THz raster imaging, THz time-domain spectroscopy (THz-TDS) and time-resolved pump-probe experiment on two different types of single layer graphene and a free standing multi-walled carbon nanotubes (MWCNTs), utilizing strong single-cycle THz pulses (central frequency, 0.9 THz; bandwidth, 1 THz; THz field amplitude, E_THz>1 MV/cm) generated by optical rectification (a second order nonlinear optical process) of femtosecond laser pulses (pulse energy, 1 mJ; pulse duration, 100 fs; repetition rate, 1 kHz) with titled pulse front for phase matching between optical and THz pulses in LiNbO3 crystal. Strong and broadband THz pulses induce transparency single layer graphene grown by catalytic chemical vapor deposition (CVD). A substrate-free homogeneous graphene becomes more transparent to the THz radiation than an inhomogeneous graphene on silicon as the peak strength of THz field increases over 50kV/cm considered as the threshold of the nonlinear transparency effect. The experimental results show that suspended graphene is more efficient to manipulate THz signal than one with a substrate. Free-standing MWCNTs drawn from a forest of MWCNTs synthesized by CVD exhibit highly anisotropic linear and nonlinear THz responses. There are no nonlinear effects for the polarization perpendicular to the MWCNT axis, whereas, in the parallel polarization configuration, intense THz pulses induce nonlinear absorption in the quasi-one-dimensional conducting media. That is, it is revealed via time-resolved measurements of transmitted THz pulses and a theoretical analysis of the data that strong THz fields enhance permittivity in carbon nanotubes by generating charge carriers. Optical-Pump/THz-probe (OPTP) spectroscopy shows that optical pump pulses induce interband transitions in MWCNTs: Its conductivity is increased by generating photo-excited hot-carriers as the optical pump energy increases. On the other hand, Optical-Pump/Intense THz-Pump spectroscopy (OPITP) exhibits three carrier dynamics phenomena which are optical pump-induced absorption, THz field-induced absorption and transparency in MWCNTs: Intense THz and optical pump energies (E_THz
Terahertz-field-induced Nonlinearity in Phonons, Electrons and Spins
Author: Xian Li (Ph.D.)Publisher:
ISBN:
Category :
Languages : en
Pages : 210
Book Description
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.
Author: Peter Gaál
Author: Qijun Liang