All-optical time-resolved measurement techniques provide a powerful tool for investigating critical parameters that determine the performance of infrared photodetector and emitter semiconductor materials. Narrow-bandgap InAs/GaSb type-II superlattices (T2SLs) have shown great promise as next generation materials, due to superior intrinsic properties and versatility. Unfortunately, InAs/GaSb T2SLs are plagued by parasitic Shockley-Read-Hall recombination centers that shorten the carrier lifetime and limit device performance. Ultrafast pump-probe techniques and time-resolved differential-transmission measurements are used here to demonstrate that "Ga-free" InAs/InAs₁₋xSbx T2SLs and InAsSb alloys do not have this same limitation and thus have significantly longer carrier lifetimes. Measurements of unintentionally doped MWIR and LWIR InAs/InAs₁₋xSbx T2SLs demonstrate minority carrier (MC) lifetimes of 18.4 µs and 4.5 µs at 77 K, respectively. This represents a more than two order of magnitude increase compared to the 90 ns MC lifetime measured in a comparable MWIR and LWIR InAs/GaSb T2SL. Through temperature-dependent differential-transmission measurements, the various carrier recombination processes are differentiated and the dominant recombination mechanisms identified for InAs/InAs₁₋xSbx T2SLs. These results demonstrate that these Ga-free materials are viable options over InAs/GaSb T2SLs and potentially bulk Hg₁₋xCdxTe photodetectors. In addition to carrier lifetimes, the drift and diusion of excited charge carriers through the superlattice layers (i.e. in-plane transport) directly aects the performance of photo-detectors and emitters. All-optical ultrafast techniques were successfully used for a direct measure of in-plane diffusion coeffcients in MWIR InAs/InAsSb T2SLs using a photo-generated transient grating technique at various temperatures. Ambipolar diffusion coefficients of approximately 60 cm²/s were reported for MWIR InAs/InAs₁₋xSbxT2SLs at 293 K.

Thulium (Tm) based high repetition rate compact optical frequency comb sources operating in the 2 µm regime with femtosecond pulse durations enable a wide range of applications such as precise micro-machining, spectroscopy and metrology. Applications such as metrology and spectroscopy rely on the stability of mode-locked lasers (MLLs) which provide extreme precision, yet, the complex dynamics of such highly nonlinear systems result in unstable events which could hinder the normal operation of a MLL. MLL as a nonlinear system inherently exists a wide variety of complex attractors, which are sets of states that the system tends to evolve toward, exhibiting unique behaviors. Complex phenomena including pulsating solitons, chaotic solitons, period-doubling, soliton explosion, etc., have been predicted theoretically and observed experimentally in the past decade. However, most experimental observations rely on conventional characterization methods, which are limited to the scanning speed of the spectrometer and the electronic speed of photodetector and digitizer, so that the details of the non-repetitive events can be buried. In recent years, a technique called dispersive Fourier transform (DFT) has been developed and allows consecutive recordings of the pulse-to-pulse spectral evolution of a femtosecond pulse train, opening a whole new world of nonlinear dynamics in MLL. In this dissertation, we first demonstrate the ability of scaling the repetition rate of a Tm MLL to repetition rate as high as 1.25 GHz through miniaturizing the cavity. Our approach of maintaining comparable pulse energies while scaling the repetition rates allows a high-quality femtosecond mode-locking performance with low noise performance in Tm soliton lasers. Then we experimentally study the transition dynamics between consecutive multi-pulsing states through adjusting pump power with a constant rate in an erbium-doped fiber laser, specifically the build-up and annihilation of soliton pulses between a double pulsing and a three-pulse state utilizing DFT. To investigate real-time laser dynamics in Tm based laser systems, we propose and develop a DFT system that up-converts the signal to the 1 µm regime via second harmonics generation (SHG) and stretches the signal in a long spool of single-mode fiber to realize DFT. This approach overcomes the limitation of bandwidth of 2 µm photodetector and high intrinsic absorption of 2 µm light in fused silica fibers. The SHG-DFT system is used to study dynamics of both explosions in a chaotic state between stable single-pulsing and double-pulsing state, and explosions induced by soliton collision in a dual-wavelength vector soliton state. We also study dynamics of transient regimes in a Tm-doped fiber ring laser that can be switched between conventional soliton and dissipative soliton, revealing how spectral filtering plays a role in obtaining stable stationary states. / 2022-11-23T00:00:00Z

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Femtosecond laser filamentation in gaseous media is a new source of broadband, ultrashort radiation that has the potential for application to many fields of research. In this dissertation filamentation is studied with a view to understanding the underlying physics governing the formation and propagation dynamics of filamentation, as well as to developing a method for vibrational spectroscopy based on the filament-induced impulsive vibrational excitation of molecules in the filamentation region. In pursuit of a better understanding of the underlying physical processes driving filamentation, the development of a new method for characterizing high intensity ultrashort laser pulses is presented, wherein two laser beams generate a transient grating in a noble gas, causing the pulse undergoing filamentation to diffract from the grating. Measuring the spectrum as a function of time delay between the filament and probe beams generates a spectrogram that can be inverted to recover the spectral and temporal phase and amplitude of the filamentary pulse. This technique enables measurement of the filamentary pulse in its native environment, offering a window into the pulse dynamics as a function of propagation distance. The intrinsic pulse shortening observed during filamentation leads to the impulsive excitation of molecular vibrations, which can be used to understand the dynamics of filamentation as well. Combined measurements of the longitudinally-resolved filament Raman spectrum, power spectrum, and fluorescence intensity confirm the propagation dynamics inferred from pulse measurements and show that filamentation provides a viable route to impulsive vibrational spectroscopy at remote distances from the laser source. The technique is applied to thermometry in air and in flames, and an analytical expression is derived to describe the short-time dynamics of the rovibrational wave-packet dispersion experienced by diatomic molecules in the wave of the filament. It is found that no energy is initially partitioned into the distribution of rovibrational states during the filamentation process. Filament-assisted impulsive stimulated Raman spectroscopy of more complex systems is also performed, showing that filament-assisted vibrational measurements can be used as an analytical tool for gas phase measurements and has potential for use as a method for standoff detection. Finally, a study of the nonlinear optical mechanisms driving the filamentation process is conducted using spectrally-resolved pump-probe measurements of the transient birefringence of air. Comparison to two proposed theories shows that a newly described effect, ionization grating-induced birefringence, is largely responsible for saturation and sign inversion of the birefringence at 400 nm and 800 nm, while the magnitude of contributions described by a competing theory that relies on negative terms in the power series expansion of the bound electron response remain undetermined. / Chemistry

Metallic nano-structures provide for new and exciting domains to investigate light-matter interactions. The coupling of these metallic nano-structures to semiconductor emitters allows for the observation of cavity QED effects including Purcell enhancement and Vacuum Rabi splitting. The focus of this dissertation will be to present an introduction and background to semiconductor optics, and metallic metamaterial systems. This will be followed by the presentation of the spectroscopy systems designed and constructed during my tenure as graduate student and the experimental data obtained with these systems. Some of the results have been published, while some of the presented material is still actively being pursued for publication. More specifically, the dissertation will cover the research at hand, experimental techniques, and results.

Doctor of Philosophy / Department of Physics / Daniel Rolles / Modern laser sources can produce bursts of light that surpass even the fastest molecular vibrations. With durations this short even moderate pulse energies generate peak powers exceeding the average power output of the entire globe. When focused, this can result in an ultrafast electric field greater than the Coulomb potential that binds electrons to nuclei. This strong electric field strips electrons away from atoms in a process known as strong-field ionization. The first experimental realization of photoionization with intense laser pulses occurred only a few years after the invention of the laser. Yet, despite decades of intensive investigation, open questions remain. At the same time, the knowledge gained has led to the creation of multiple exciting fields such as attoscience, femtochemistry, and ultrafast nano-photonics. In this thesis I present my work to advance the fundamental understanding of intense, ultrafast light-matter interactions as well as efforts to expand the technological capabilities of ultrafast light sources and measurement techniques. This includes the photoionization pro- cess of atoms and nanoparticles subject to intense, mid-infrared laser fields. The resulting photoelectron emission is measured, with high precision, in a velocity map imaging spec- trometer. Other parts of this thesis detail my work on the generation and characterization of non-Gaussian optical pulses. Femtosecond Bessel beams are used to drive and study high harmonic generation with the ultimate goal of creating a compact, high-flux XUV source. Further studies include few-cycle pulses and the carrier-envelope phase, specifically methods of locking and tagging the carrier-envelope phase. A single-shot, all optical tagging method is developed and directly compared to the standard tagging method, the carrier-envelope phase meter. Finally, both experimental and computational studies are presented investigating the ultrafast thermal response cycle of nanowires undergoing femtosecond heating.

We have used ultrafast optics, primarily focused on the nonlinear processes of Polarization Gating and of Optical Parametric Amplification, one for measurement and the other for imaging purposes. For measurement, we have demonstrated a robust method of measurement to simultaneously measure both optical pulses used in a pump-probe type configuration. We refer to this method of pulse measurement as Double Blind Polarization Gating FROG. We have demonstrated this single-shot method for measuring two unknown pulses using one device. In addition to pulse measurement, we have demonstrated the processes of Optical Parametric Amplification (OPA) applicability to imaging of complex objects. We have done this where the Fourier transform plane is used during the interaction. We have amplified and wavelength converted a complex image. We observe a gain of ~100, and, although our images were averaged over many shots, we used a single-shot geometry, capable of true single-shot OPA imaging. To our knowledge, this is the first Fourier-plane OPA imaging of more than a single spatial-frequency component of an image. We observe more than 30 distinct spatial frequency components in both our amplified image and our wavelength shifted image. We have demonstrated all-optical spatial filtering for these complex images. We have demonstrated that direct Fourier filtering of spatial features is possible by using a shaped pump beam. We can isolate certain portions of the image simply by rotating the crystal.

In this thesis a powerful and practical method for characterizing ultrashort pulses in space and time is described (called SEA TADPOLE). First we focus on measuring pulses that are spatially uniform but very complicated in time or frequency. We demonstrate and verify that SEA TADPOLE can measure temporal features as small as 30 femtoseconds over durations as long as 14 picoseconds. The spectral resolution of this device is carefully studied and we demonstrate that for certain pulses, we achieve spectral super resolution. We also develop and test an algorithm for measuring polarization shaped pulses with SEA TADPOLE. Our simple interferometer can even be used to measure the spatiotemporal electric field of ultrashort pulses at a focus. This is because SEA TADPOLE samples the field with an optical fiber which has a small core size. Therefore this fiber can be used to spatially sample the beam, so that the temporal electric field can be measured at every position to obtain E(x, y, z, t). The single mode fiber can be replaced with an NSOM (Near Field Scanning Optical Microscopy) fiber so that spatial resolution as low as 500nm (and possibly lower) can be achieved. Using this device we make the first direct measurements of the compete field of focusing ultrashort pulses. These measurement can be viewed as "snap shots" in flight of the focusing pulse. Also, for the first time, we have observed some of the interesting distortions that have been predicted for focusing ultrashort pulses such as the "forerunner" pulse, radially varying group delay dispersion, and the Bessel-like X-shaped pulse. We have also made the first direct measurements of the electric field of Bessel X-pulses and their propagation invariance is demonstrated. We also use SEA TADPOLE to study the "boundary wave pulses" which are due to diffraction.

付記する学位プログラム名: 京都大学卓越大学院プログラム「先端光・電子デバイス創成学」 / 京都大学 / 新制・課程博士 / 博士(理学) / 甲第23690号 / 理博第4780号 / 新制||理||1684(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)教授 田中 耕一郎, 教授 金光 義彦, 教授 柳瀬 陽一 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

The topic of this proposal is the development of high peak power laser sources with a focus on linearly chirped pulse laser sources. In the past decade chirped optical pulses have found a plethora of applications such as photonic analog-to-digital conversion, optical coherence tomography, laser ranging, etc. This dissertation analyzes the aforementioned applications of linearly chirped pulses and their technical requirements, as well as the performance of previously demonstrated parabolic pulse shaping approaches. The experimental research addresses the topic of parabolic pulse generation in two distinct ways. First, pulse shaping technique involving a time domain approach is presented, that results in stretched pulses with parabolic profiles with temporal duration of 15 ns. After pulse is shaped into a parabolic intensity profile, the pulse is compressed with DCF fiber spool by 100 times to 80 ps duration at FWHM. A different approach of pulse shaping in frequency domain is performed, in which a spectral processor based on Liquid Crystal on Silicon technology is used. The pulse is stretched to 1.5 ns before intensity mask is applied, resulting in a parabolic intensity profile. Due to frequency to time mapping, its temporal profile is also parabolic. After pulse shaping, the pulse is compressed with a bulk compressor, and subsequently analyzed with a Frequency Resolved Optical Gating (FROG). The spectral content of the compressed pulse is feedback to the spectral processor and used to adjust the spectral phase mask applied on the pulse. The resultant pulse iv after pulse shaping with feedback mechanism is a Fourier transform, sub-picosecond ultrashort pulse with 5 times increase in peak power. The appendices in this dissertation provide additional material used for the realization of the main research focus of the dissertation. Specification and characterization of major components of equipments and devices used in the experiment are present. The description of Matlab algorithms that was used to calculate required signals for pulse shaping are shown. A brief description of the Labview code used to control the spectral processor will also be illustrated.