On Ultrafast Time-Domain TeraHertz Spectroscopy in the Condensed Phase: Linear Spectroscopic Measurements of Hydrogen-Bond Dynamics of Astrochemical Ice Analogs and Nonlinear TeraHertz Kerr Effect Measurements of Vibrational Quantum Beats

Much of the chemistry that affects life on planet Earth occurs in the condensed phase. The TeraHertz (THz) or far-infrared (far-IR) region of the electromagnetic spectrum (from 0.1 THz to 10 THz, 3 cm^-1 to 300 cm^-1, or 3000 μm to 30 μm) has been shown to provide unique possibilities in the study of condensed-phase processes. The goal of this work is to expand the possibilities available in the THz region and undertake new investigations of fundamental interest to chemistry. Since we are fundamentally interested in condensed-phase processes, this thesis focuses on two areas where THz spectroscopy can provide new understanding: astrochemistry and solvation science. To advance these fields, we had to develop new instrumentation that would enable the experiments necessary to answer new questions in either astrochemistry or solvation science. We first developed a new experimental setup capable of studying astrochemical ice analogs in both the TeraHertz (THz), or far-Infrared (far-IR), region (0.3 - 7.5 THz; 10 - 250 cm^-1) and the mid-IR (400 - 4000 cm^-1). The importance of astrochemical ices lies in their key role in the formation of complex organic molecules, such as amino acids and sugars in space. Thus, the instruments are capable of performing variety of spectroscopic studies that can provide especially relevant laboratory data to support astronomical observations from telescopes such as the Herschel Space Telescope, the Stratospheric Observatory for Infrared Astronomy (SOFIA), and the Atacama Large Millimeter Array (ALMA). The experimental apparatus uses a THz time-domain spectrometer, with a 1750/875 nm plasma source and a GaP detector crystal, to cover the bandwidth mentioned above with ~10 GHz (~0.3 cm^-1) resolution.

Using the above instrumentation, experimental spectra of astrochemical ice analogs of water and carbon dioxide in pure, mixed, and layered ices were collected at different temperatures under high vacuum conditions with the goal of investigating the structure of the ice. We tentatively observe a new feature in both amorphous solid water and crystalline water at 33 cm^-1 (1 THz). In addition, our studies of mixed and layered ices show how it is possible to identify the location of carbon dioxide as it segregates within the ice by observing its effect on the THz spectrum of water ice. The THz spectra of mixed and layered ices are further analyzed by fitting their spectra features to those of pure amorphous solid water and crystalline water ice to quantify the effects of temperature changes on structure. From the results of this work, it appears that THz spectroscopy is potentially well suited to study thermal transformations within the ice.

To advance the study of liquids with THz spectroscopy, we developed a new ultrafast nonlinear THz spectroscopic technique: heterodyne-detected, ultrafast THz Kerr effect (TKE) spectroscopy. We implemented a heterodyne-detection scheme into a TKE spectrometer that uses a stilbazoiumbased THz emitter, 4-N,N-dimethylamino-4-N-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate (DSTMS), and high numerical aperture optics which generates THz electric field in excess of 300 kV/cm, in the sample. This allows us to report the first measurement of quantum beats at terahertz (THz) frequencies that result from vibrational coherences initiated by the nonlinear, dipolar interaction of a broadband, high-energy, (sub)picosecond THz pulse with the sample. Our instrument improves on both the frequency coverage, and sensitivity previously reported; it also ensures a backgroundless measurement of the THz Kerr effect in pure liquids. For liquid diiodomethane, we observe a quantum beat at 3.66 THz (122 cm^-1), in exact agreement with the fundamental transition frequency of the υ4 vibration of the molecule. This result provides new insight into dipolar vs. Raman selection rules at terahertz frequencies.

To conclude we discuss future directions for the nonlinear THz spectroscopy in the Blake lab. We report the first results from an experiment using a plasma-based THz source for nonlinear spectroscopy that has the potential to enable nonlinear THz spectra with a sub-100 fs temporal resolution, and how the optics involved in the plasma mechanism can enable THz pulse shaping. Finally, we discuss how a single-shot THz detection scheme could improve the acquisition of THz data and how such a scheme could be implemented in the Blake lab. The instruments developed herein will hopefully remain a part of the groups core competencies and serve as building blocks for the next generation of THz instrumentation that pushes the frontiers of both chemistry and the scientific enterprise as a whole.

星间激光通信中复合轴系统的带宽设计研究

星间激光通信中，由粗跟踪系统和精跟踪系统组成的复合轴系统完成了系统的大范围、高精度跟踪任务。对复合轴系统进行了基于Z变换的数字模拟以研究其带宽设计。根据计算的卫星轨迹和粗跟踪系统机械误差，得到了粗跟踪系统的带宽设计结果；给出了粗跟踪系统和精跟踪系统的配合工作关系；得到了精跟踪系统的带宽设计结果；最后研究了在中高频扰动下，复合轴系统的带宽设计。以上结果为星间激光通信中的复合轴系统控制系统设计提供了重要依据。

Stability of Hypervelocity Boundary Layers

The early stage of laminar-turbulent transition in a hypervelocity boundary layer is studied using a combination of modal linear stability analysis, transient growth analysis, and direct numerical simulation. Modal stability analysis is used to clarify the behavior of first and second mode instabilities on flat plates and sharp cones for a wide range of high enthalpy flow conditions relevant to experiments in impulse facilities. Vibrational nonequilibrium is included in this analysis, its influence on the stability properties is investigated, and simple models for predicting when it is important are described.

Transient growth analysis is used to determine the optimal initial conditions that lead to the largest possible energy amplification within the flow. Such analysis is performed for both spatially and temporally evolving disturbances. The analysis again targets flows that have large stagnation enthalpy, such as those found in shock tunnels, expansion tubes, and atmospheric flight at high Mach numbers, and clarifies the effects of Mach number and wall temperature on the amplification achieved. Direct comparisons between modal and non-modal growth are made to determine the relative importance of these mechanisms under different flow regimes.

Conventional stability analysis employs the assumption that disturbances evolve with either a fixed frequency (spatial analysis) or a fixed wavenumber (temporal analysis). Direct numerical simulations are employed to relax these assumptions and investigate the downstream propagation of wave packets that are localized in space and time, and hence contain a distribution of frequencies and wavenumbers. Such wave packets are commonly observed in experiments and hence their amplification is highly relevant to boundary layer transition prediction. It is demonstrated that such localized wave packets experience much less growth than is predicted by spatial stability analysis, and therefore it is essential that the bandwidth of localized noise sources that excite the instability be taken into account in making transition estimates. A simple model based on linear stability theory is also developed which yields comparable results with an enormous reduction in computational expense. This enables the amplification of finite-width wave packets to be taken into account in transition prediction.

Two-step digit-set-restricted modified signed-digit addition-subtraction algorithm and its optoelectronic implementation

A novel, to our knowledge, two-step digit-set-restricted modified signed-digit (MSD) addition-subtraction algorithm is proposed. With the introduction of the reference digits, the operand words are mapped into an intermediate carry word with all digits restricted to the set {(1) over bar, 0} and an intermediate sum word with all digits restricted to the set {0, 1}, which can be summed to form the final result without carry generation. The operation can be performed in parallel by use of binary logic. An optical system that utilizes an electron-trapping device is suggested for accomplishing the required binary logic operations. By programming of the illumination of data arrays, any complex logic operations of multiple variables can be realized without additional temporal latency of the intermediate results. This technique has a high space-bandwidth product and signal-to-noise ratio. The main structure can be stacked to construct a compact optoelectronic MSD adder-subtracter. (C) 1999 Optical Society of America.

Experimental study of the Talbot effect under femtosecond laser illumination

Experimental results of the Talbot effect of an amplitude grating under femtosecond laser illumination are reported. Compared with Talbot image under continuous wave (CW) illumination, Talbot images under femtosecond laser illumination are different due to the wide spectral bandwidth and the Talbot images are more distorted at longer Talbot distances. The spectrums and the pulsewidths of femtosecond laser pulses are measured with the frequency-resolved optical gating (FROG) apparatus. Experimental results are in good agreement with the theoretical analysis. (c) 2005 Elsevier B.V. All rights reserved.

Femtosecond laser speckles

The concept of femtosecond laser speckles is put forward. The theory of a speckle pattern in light of finite bandwidth is applied to describe femtosecond laser speckles. Basic representations of the contrast and the spectral correlation of femtosecond laser speckles are presented. The relationship between the speckle contrast and the bandwidth of a femtosecond laser is given. Experimental results are given that indicate an obvious difference between the speckle patterns produced by a continuous-wave laser and those produced by a femtosecond laser. (c) 2005 Optical Society of America

Coherence measurement of a Ti:sapphire femtosecond pulsed laser

The interference patterns produced by Gaussian-shaped broad-bandwidth femtosecond pulsed laser sources are derived. The interference pattern contains both spatial and temporal properties of laser beam. Interference intensity dependent on the bandwidth of femtosecond laser are given. We demonstrate experimentally both the spatial and the temporal coherence properties of a Ti:sapphire femtosecond pulse laser, as well as its power spectrum by using a pinhole pair.

一种新型光纤光栅无啁啾调谐方法

分析了基于弹性梁的光纤光栅调谐原理，引入了轴向直变传递系数的概念，提出利用部分纯弯曲调谐方法，可实现光纤光栅宽带无啁嗽调谐。在实验中，利用部分纯弯曲调谐法，获得了20．1nm的光纤光栅无啁嗽调谐范围，调谐线性拟合度为0．9996，调谐过程中光栅反射谱的3dB带宽变化小于0．07nm，峰值反射率变化小于0．2dB，基本无啁嗽现象产生，实验结果和理论分析一致。

有源波导环形谐振腔滤波特性分析

将掺铒有源波导材料引入环形谐振腔结构，从理论上分析了有源波导环形谐振腔的滤波特性。结果表明由于抽运光提供的增益补偿了腔内损耗，使得环形谐振腔满足临界耦合条件，实现对信号光的最佳陷波，同时发现通过改变抽运光功率，可以对精细度和带宽进行动态调谐。分析了铒离子掺杂浓度、信号光功率以及抽运光耦合系数对最佳陷波抽运功率的影响，为有源波导器件设计制作提供了理论依据。

平面弯曲波导耦合器的特性分析

根据耦合模理论和弯曲波导耦合器的结构特点,对平面弯曲波导耦合器的特性进行了分析,结果表明弯曲波导耦合器的弯曲半径和最小间距两个可调变量,增加了波导器件设计的灵活性;同时由于等效耦合长度的调制作用使得弯曲波导耦合器在波分复用/解复用中比平行直波导耦合器具有更大的复用带宽;分析了弯曲半径和最小间距对弯曲波导耦合器复用带宽的影响,为实际波导器件的设计制作提供了一定的理论依据.

Pulse shaping properties of volume holographic gratings in anisotropic media

Based on a modified coupled wave theory, the pulse shaping properties of volume holographic gratings (VHGs) in anisotropic media VHGs are studied systematically. Taking photorefractive LiNbO3 crystals as an example, the combined effect that the grating parameters, the dispersion and optical anisotropy of the crystal, the pulse width, and the polarization state of the input ultrashort pulsed beam (UPB) have on the pulse shaping properties are considered when the input UPB with arbitrary polarization state propagates through the VHG. Under the combined effect, the diffraction bandwidth, pulse profiles of the diffracted and transmitted pulsed beams, and the total diffraction efficiency are shown. The studies indicate that the properties of the shaping of the o and e components of the input UPB in the crystal are greatly different; this difference can be used for pulse shaping applications. (c) 2006 Optical Society of America.

Diffraction properties of volume holographic gratings for an ultrashort pulsed beam with different polarization states readout

The diffraction properties of volume holographic gratings are studied when the gratings are illuminated by an ultrashort pulsed beam with different polarization states. The developed coupled wave theory of Kogelnik is used. Considering the dispersion effect of the grating media, solutions for the diffracted and transmitted intensities, diffraction efficiencies and the bandwidths of the gratings are given in transmission volume holographic gratings and reflection volume holographic gratings. The bandwidths of the gratings are reduced by the dispersion effect of the grating media. They also have different influences on the diffraction of an ultrashort pulsed beam with different polarization states. For different values of the ratio of the spectral bandwidth of the input pulse to that of the grating, the changes of the spectral and temporal distributions of the diffracted intensities, as well as the diffraction efficiencies of the gratings are shown.

A Multiwavelength Study of the Intracluster Medium and the Characterization of the Multiwavelength Sub/millimeter Inductance Camera

The first part of this thesis combines Bolocam observations of the thermal Sunyaev-Zel’dovich (SZ) effect at 140 GHz with X-ray observations from Chandra, strong lensing data from the Hubble Space Telescope (HST), and weak lensing data from HST and Subaru to constrain parametric models for the distribution of dark and baryonic matter in a sample of six massive, dynamically relaxed galaxy clusters. For five of the six clusters, the full multiwavelength dataset is well described by a relatively simple model that assumes spherical symmetry, hydrostatic equilibrium, and entirely thermal pressure support. The multiwavelength analysis yields considerably better constraints on the total mass and concentration compared to analysis of any one dataset individually. The subsample of five galaxy clusters is used to place an upper limit on the fraction of pressure support in the intracluster medium (ICM) due to nonthermal processes, such as turbulent and bulk flow of the gas. We constrain the nonthermal pressure fraction at r500c to be less than 0.11 at 95% confidence, where r500c refers to radius at which the average enclosed density is 500 times the critical density of the Universe. This is in tension with state-of-the-art hydrodynamical simulations, which predict a nonthermal pressure fraction of approximately 0.25 at r500c for the clusters in this sample.

The second part of this thesis focuses on the characterization of the Multiwavelength Sub/millimeter Inductance Camera (MUSIC), a photometric imaging camera that was commissioned at the Caltech Submillimeter Observatory (CSO) in 2012. MUSIC is designed to have a 14 arcminute, diffraction-limited field of view populated with 576 spatial pixels that are simultaneously sensitive to four bands at 150, 220, 290, and 350 GHz. It is well-suited for studies of dusty star forming galaxies, galaxy clusters via the SZ Effect, and galactic star formation. MUSIC employs a number of novel detector technologies: broadband phased-arrays of slot dipole antennas for beam formation, on-chip lumped element filters for band definition, and Microwave Kinetic Inductance Detectors (MKIDs) for transduction of incoming light to electric signal. MKIDs are superconducting micro-resonators coupled to a feedline. Incoming light breaks apart Cooper pairs in the superconductor, causing a change in the quality factor and frequency of the resonator. This is read out as amplitude and phase modulation of a microwave probe signal centered on the resonant frequency. By tuning each resonator to a slightly different frequency and sending out a superposition of probe signals, hundreds of detectors can be read out on a single feedline. This natural capability for large scale, frequency domain multiplexing combined with relatively simple fabrication makes MKIDs a promising low temperature detector for future kilopixel sub/millimeter instruments. There is also considerable interest in using MKIDs for optical through near-infrared spectrophotometry due to their fast microsecond response time and modest energy resolution. In order to optimize the MKID design to obtain suitable performance for any particular application, it is critical to have a well-understood physical model for the detectors and the sources of noise to which they are susceptible. MUSIC has collected many hours of on-sky data with over 1000 MKIDs. This work studies the performance of the detectors in the context of one such physical model. Chapter 2 describes the theoretical model for the responsivity and noise of MKIDs. Chapter 3 outlines the set of measurements used to calibrate this model for the MUSIC detectors. Chapter 4 presents the resulting estimates of the spectral response, optical efficiency, and on-sky loading. The measured detector response to Uranus is compared to the calibrated model prediction in order to determine how well the model describes the propagation of signal through the full instrument. Chapter 5 examines the noise present in the detector timestreams during recent science observations. Noise due to fluctuations in atmospheric emission dominate at long timescales (less than 0.5 Hz). Fluctuations in the amplitude and phase of the microwave probe signal due to the readout electronics contribute significant 1/f and drift-type noise at shorter timescales. The atmospheric noise is removed by creating a template for the fluctuations in atmospheric emission from weighted averages of the detector timestreams. The electronics noise is removed by using probe signals centered off-resonance to construct templates for the amplitude and phase fluctuations. The algorithms that perform the atmospheric and electronic noise removal are described. After removal, we find good agreement between the observed residual noise and our expectation for intrinsic detector noise over a significant fraction of the signal bandwidth.

Wave induced oscillations in harbors of arbitrary shape

Theoretical and experimental studies were conducted to investigate the wave induced oscillations in an arbitrary shaped harbor with constant depth which is connected to the open-sea.

A theory termed the “arbitrary shaped harbor” theory is developed. The solution of the Helmholtz equation, ∇²f + k²f = 0, is formulated as an integral equation; an approximate method is employed to solve the integral equation by converting it to a matrix equation. The final solution is obtained by equating, at the harbor entrance, the wave amplitude and its normal derivative obtained from the solutions for the regions outside and inside the harbor.

Two special theories called the circular harbor theory and the rectangular harbor theory are also developed. The coordinates inside a circular and a rectangular harbor are separable; therefore, the solution for the region inside these harbors is obtained by the method of separation of variables. For the solution in the open-sea region, the same method is used as that employed for the arbitrary shaped harbor theory. The final solution is also obtained by a matching procedure similar to that used for the arbitrary shaped harbor theory. These two special theories provide a useful analytical check on the arbitrary shaped harbor theory.

Experiments were conducted to verify the theories in a wave basin 15 ft wide by 31 ft long with an effective system of wave energy dissipators mounted along the boundary to simulate the open-sea condition.

Four harbors were investigated theoretically and experimentally: circular harbors with a 10° opening and a 60° opening, a rectangular harbor, and a model of the East and West Basins of Long Beach Harbor located in Long Beach, California.

Theoretical solutions for these four harbors using the arbitrary shaped harbor theory were obtained. In addition, the theoretical solutions for the circular harbors and the rectangular harbor using the two special theories were also obtained. In each case, the theories have proven to agree well with the experimental data.

It is found that: (1) the resonant frequencies for a specific harbor are predicted correctly by the theory, although the amplification factors at resonance are somewhat larger than those found experimentally,(2) for the circular harbors, as the width of the harbor entrance increases, the amplification at resonance decreases, but the wave number bandwidth at resonance increases, (3) each peak in the curve of entrance velocity vs incident wave period corresponds to a distinct mode of resonant oscillation inside the harbor, thus the velocity at the harbor entrance appears to be a good indicator for resonance in harbors of complicated shape, (4) the results show that the present theory can be applied with confidence to prototype harbors with relatively uniform depth and reflective interior boundaries.

Diffraction of an ultrashort pulsed beam with arbitrary polarization state from a volume holographic grating in LiNbO3 crystals

Based on a modified coupled wave theory of Kogelnik, we have studied the diffraction of an ultrashort pulsed beam with an arbitrary polarization state from a volume holographic grating in photorefractive LiNbO3 crystals. The results indicate that the diffracted intensity distributions in the spectral and temporal domains and the diffraction efficiency of the grating are both changed by the polarization state and spectral bandwidth of the input pulsed beam. A method is given of choosing the grating parameters and input conditions to obtain a large variation range of the spectral bandwidth of the diffracted pulsed beam with an appropriate diffraction efficiency. Our study presents a possibility of using a volume holographic grating recorded in anisotropic materials to shape a broadband ultrashort pulsed beam by modulating its polarization state.