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Item Thermalization and exciton localization in 2D semiconductors(Montana State University - Bozeman, College of Letters & Science, 2023) Strasbourg, Matthew Christopher; Chairperson, Graduate Committee: Nick Borys; This is a manuscript style paper that includes co-authored chapters.2D semiconductors are a promising class of materials to investigate for applications in the next generation of photonic devices. They can be used to generate quantum light and also exhibit correlated many-body phenomena. Many of the novel optoelectronic properties of 2D semiconductors are associated with strongly-bound hydrogen-like states known as excitons. Excitons in 2D semiconductors have binding energies on the order of 100s of meV and are stable at room temperature. At low temperatures, higher-order excitonic states such as charged excitons and biexcitons--multiple-bound excitons that are like hydrogen molecules-- and localized excitons that emit quantum light are also observed. Whether excited optically or electronically, a diversity of high-energy excitons and free carriers are produced directly after excitation. The relaxation and thermalization of these initial states influence the formation of excitons, biexcitons, and localized excitons. Here, I present work that (i) investigates the thermalization of excited states in a prototypical 2D semiconductor, monolayer (1L-) WSe2, and reports the discovery that the generation of charged biexcitons is enhanced with increasing photoexcitation energy, (ii) shows the emergence of quantum emitters (QEs) in a new 2D QE platform: 1L-WSe2 nanowrinkle arrays induced by Au nano stressors, and (iii) uses a novel method to classify the excited-state dynamics of 2D QEs and differentiate emitter populations. A suite of low-temperature energy- and time- resolved optical spectroscopies are used to conduct this work. This work shows how excited state thermalization affects the formation of exciton and biexcitons and investigates the optical properties of an emergent class of 2D quantum light emitters.Item X-ray analysis and modeling of NGC 3227(Montana State University - Bozeman, College of Letters & Science, 2022) Newman, Jared James; Chairperson, Graduate Committee: Yves U. Idzerda and Sachiko Tsuruta (co-chair)The 1.5 Seyfert galaxy NGC 3227 has been observed by several X-ray missions. We carried out combined analysis of the data from a total of twenty one observations. Six of the observations were preformed by Suzaku, eight by XMM-Newton, and seven by NuStar. A unified model was constructed which is consistent with all twenty one of the observations by the three satellites with large intensity and spectral changes. The model consists of a hard power law which is interpreted as the Comptonized emission from the corona above an accretion disk. In the high flux states an additional soft excess component dominates, which is consistent with a model with either a steeper power law or a warm Comptonization component. These emissions from the central engine are absorbed by multiple distinct absorbers at various ionization levels. A reflection component and several emission lines are also present. This is the most robust model of this source to date.Item Novel models and observations of energetic events in the solar transition region(Montana State University - Bozeman, College of Letters & Science, 2021) Parker, Jacob Douglas; Chairperson, Graduate Committee: Charles C. Kankelborg; Dana Longcope was a co-author of the article, 'Modeling a propagating sawtooth flare ribbon as a tearing mode in the presence of velocity shear' in the journal 'Astrophysical journal' which is contained within this dissertation.; Charles Kankelborg was a co-author of the article, 'Determining the spectral content of MOSES images' submitted to the journal 'Astrophysical journal' which is contained within this dissertation.; Roy Smart, Charles Kankelborg, Amy Winebarger and Nelson Goldsworth were co-authors of the article, 'First flight of the EUV snapshot imaging spectrograph (ESIS)' submitted to the journal 'Astrophysical journal' which is contained within this dissertation.The solar atmosphere is an energetic and violent place capable of producing eruptions that affect us on earth. In order to better understand these events, so that we might improve out ability to model and predict them, we observe the sun from space to diagnose the local plasma conditions and track its evolution. The transition region, a thin region of the solar atmosphere separating the chromosphere from the corona, is where the solar atmosphere transitions rapidly from ten thousand, to one million kelvin and is therefore thought to play an important roll in the transfer of mass and energy to the hot corona. The sun's magnetic field, and magnetic reconnection, are thought to contribute to the increased temperature of the corona, since the cooler lower solar atmosphere cannot heat it via thermal conduction or convection. Explosive events, small solar eruptions likely driven by magnetic reconnection, are frequent in the transition region, making it an attractive area of the atmosphere to study and gather information on the processes. Using Computed Tomography Imaging Spectrographs (CTIS), capable of measuring spectral line profiles over a wide fields of view at every exposure, we find many eruptive events in the transition region to be spatially complex, three dimensional, and to evolve on rapid timescales. This demonstrates the utility of, and need to continue developing, CTIS style instruments for solar study since they provide a more complete picture of solar events, allowing us to improve our understanding of our closest star.Item Exploration of rare-earth ion transitions and host materials for spectral hole burning applications and quantum information science(Montana State University - Bozeman, College of Letters & Science, 2021) Marsh, Aaron Daniel; Chairperson, Graduate Committee: Rufus L. ConeDue to their capacity for generating and manipulating light, the rare-earths are a foundational part of many cutting-edge technologies, ranging from lighting to quantum communications. Optical applications based on rare-earth doped materials are restricted to their transition energies. There are large bands, including the telecom window, where available rare-earth transitions typically have poor properties at liquid helium temperatures. The limitations are determined by the fundamental interactions between rare-earth ions and their host materials; comprehension of the interactions can be leveraged to significantly improve the properties of rare-earth quantum states. Three unexplored rare-earth optical transitions are investigated in this thesis: the Tm 3+ 3 H6<-->3 F3 at ~690 nm, the Pr 3+ 3 H 4<-->3 F 3 at ~1584 nm, and the Tm 3+ 3 F4<-->3 H 4 at ~1451 nm. The first transition suppresses non-radiative relaxation through engineering of the host material phonon spectrum. The 3 F 3 lifetime is extended to ~100 microsecond in Tm 3+ :KPb 2Br 5. The material Tm 3+:LaF 3 is also prepared for high-contrast spectral filtering in ultrasound-optical medical imaging sensitive to blood oxygenation at ~690 nm. Narrow 380 kHz holes are burned; simulations of hole burning indicate that ~60 dB of filtering contrast at ~3MHz is possible. Likewise, non-radiative relaxation is suppressed on the Pr 3+ transition at ~1584 nm in the low-phonon energy host RbPb 2Br 5. Four sites are revealed, with ~2-5 GHz spectrally resolved inhomogeneous broadenings, ~0.5-1 ms T 1 lifetimes, pseudoquadrupole level storage, and ~750 ns coherence times. This material is discussed for use as an L-band quantum memory. The excited state transition of Tm 3+ at ~1451 nm is then explored for quantum memories. High-resolution spectroscopy finds ~1 GHz inhomogeneous broadenings, ~6 ms lifetimes, and laser-limited ~30 MHz holes are burned. Techniques for measuring the properties of excited state transitions are described. Throughout, experimental methods and applications demonstrate the close relationship between lanthanide research and devices. Rare-earth doped crystals are used as an all-optical, high-resolution sensor package for characterizing cryostats in situ, and spectral hole burning characterizes laser performance as a real-time, ~1 MHz resolution spectrum analyzer. The exploration of rare-earth transitions is found to enable new research and new applications, with many other transitions yet to be explored.Item Exploring the origin of the Magellanic periphery with SMASH photometric metallicities(Montana State University - Bozeman, College of Letters & Science, 2019) Miller, Amy Elizabeth; Chairperson, Graduate Committee: David L. NideverThe distribution of stellar metallicities across the Large and Small Magellanic Clouds is a key ingredient to understanding the processes that have shaped their evolution, and remains a rich ground for exploration. I use data from the Survey of Magellanic Stellar History (SMASH), a photometric survey of the Magellanic Clouds that contains approximately 400 million objects in 197 fields that were obtained with DECam on the CTIO Blanco 4m telescope. SMASH covers 2400 square degrees to 24th magnitude in ugriz, encompassing a depth of 2 magnitudes below the oldest main-sequence turnoff stars. The DECam u-band is sensitive to metallicity for main-sequence turn-off stars, which is calibrated using SDSS and LAMOST spectroscopy in overlapping regions. This analysis is used to make accurate metallicity maps of the main bodies of the Clouds and their peripheries. Ultimately, these metallicity maps will help us trace out population gradients in the Clouds and uncover the origin of their very extended stellar peripheries.Item Characterizing excited state dynamics and carrier transport in hybrid organic-inorganic lead halide perovskites via ultrafast microscopy(Montana State University - Bozeman, The Graduate School, 2018) Hill, Andrew Hinson; Chairperson, Graduate Committee: Erik Grumstrup; Kori E. Smyser, Casey L. Kennedy, Eric S. Massaro and Erik M. Grumstrup were co-authors of the article, 'Ultrafast microscopy of methylammonium lead iodide perovskite thin films: heterogeneity of excited state spatial and temporal evolution' which is contained within this thesis.; Kori E. Smyser, Casey L. Kennedy, Eric S. Massaro and Erik M. Grumstrup were co-authors of the article, 'Screened charge carrier transport in methylammonium lead iodide perovskite thin films' in the journal 'Journal of physical chemistry letters' which is contained within this thesis.; Casey L. Kennedy, Eric S. Massaro and Erik M. Grumstrup were co-authors of the article, 'Perovskite carrier transport: disentangling the impacts of effective mass and scattering time through microscopic optical detection' in the journal 'Journal of physical chemistry letters' which is contained within this thesis.; Casey L. Kennedy and Erik M. Grumstrup were co-authors of the article, 'Determining the effects of A-site cation substitution on the optical response and transport properties of lead tri-bromide perovskites' submitted to the journal 'Journal of physical chemistry letters' which is contained within this thesis.Lead tri-halide perovskites have recently emerged as cost-effective alternatives to silicon for use in photovoltaic devices. A large contributor to their reduced cost compared to silicon is the simple solution processed techniques employed in their fabrication. While these methods can produce effective photovoltaic devices, heterogeneity endemic to solution processing makes characterization of tri-halide perovskites a challenging task. Most spectroscopic techniques use large sample interrogation volumes which often results in the indiscriminate sampling of grain boundaries and other heterogeneities which impact the spectroscopic observable. To circumvent this issue, pump-probe microscopy is used to dramatically shrink the sample volume, reducing the contributions from chemical and morphological heterogeneities and providing a more accurate measure of the sample's inherent properties. This work begins with a study of the recombination and transport dynamics methylammonium lead tri-iodide (MAPbI 3) perovskite. After identifying the main recombination pathways and contributions to the transient signal, experimental focus is shifted to the transport properties of MAPbI 3. The key contributing factors to the high diffusivities reported in MAPbI 3 are found to be strong electron-phonon coupling and a high static dielectric constant which serves to screen carriers from interactions with charged defects and other carriers. Then the development a new all-optical method capable of uniquely determining the two fundamental parameters that govern carrier transport (the mean scattering time and optical mass of photogenerated carriers) is reported. This method was applied to a series of different perovskite materials including MAPbI 3, cesium lead bromide di-iodide (CsPbBrI 2), methylammonium lead tri-bromide (MAPbBr 3), formamidinium lead tri-bromide (FAPbBr 3), and cesium lead tri-bromide (CsPbBr 3). The results of these experiments have led to the characterization of the role each perovskite constituent (namely, the identity of the organic cation and the halide stoichiometry) plays in determining the transport properties of the resulting material. The work presented in this dissertation characterizes the transport properties of lead halide perovskites. Measurements collected across multiple discrete and highly crystalline domains of multiple perovskite species have helped establish a relationship between the functionality and the local structure of these materials. Additionally, the design and first application of a new methodology to disentangle the effects of mean scattering time and the photogenerated carrier mass on carrier transport is reported. This technique will not only continue to aid in the characterization of lead-halide perovskites but will likely also see use on a host of other material systems to advance understanding of carrier transport in a variety of materials.Item Combining spectral and polarimetric methods to classify cloud thermodynamic phase(Montana State University - Bozeman, College of Engineering, 2019) Tauc, Martin Jan; Chairperson, Graduate Committee: Joseph A. Shaw; David W. Riesland, Laura M. Eshelman, Wataru Nakagawa and Joseph A. Shaw were co-authors of the article, 'Radiance ratios for CTP discrimination' submitted to the journal 'Journal of applied remote sensing' which is contained within this thesis.; Wataru Nakagawa and Joseph A. Shaw were co-authors of the article, 'The SWIR three-channel polarimeter for cloud thermodynamic phase detection' in the journal 'Optical engineering' which is contained within this thesis.Cloud thermodynamic phase--whether a cloud is composed of spherical water droplets or polyhedral ice crystals--is an important parameter for optical communication with space-based instruments, remote sensing of the atmosphere, and, perhaps most importantly, understanding weather and climate. Although some methods exist to detect the phase of clouds, there is still a need for passive remote sensing of cloud thermodynamic phase due to its low-cost, scalability, and ease of use. Two methods for cloud thermodynamic phase classification employ spectral radiance ratios in the short-wave infrared, and the S 1 Stokes parameter, a polarimetric quantity. In this dissertation, the combination of the two methods is realized in an instrument called the short-wave infrared three-channel polarimeter. The coalescence of radiance ratios in the short-wave infrared and polarization channels oriented parallel and perpendicular to the scattering plane provides better classification of cloud phase than either method independently. Despite the improvement, the low-cost system suffered from hardware and software limitations, which caused an increase in noise and polarimetric artifacts. These errors are analyzed and a subset of low-noise data shows even better classification ability. All together, the results attained from the deployment of the polarimeter in early 2019 showed promise that the combination of the two methods is an improvement over past techniques.Item The development of superresolution spectroscopic techniques and characterization of microscale exciton diffusion in organic semiconducting polymers(Montana State University - Bozeman, College of Letters & Science, 2018) Massaro, Eric Stephen; Chairperson, Graduate Committee: Erik Grumstrup; Andrew H. Hill and Erik M. Grumstrup were co-authors of the article, 'Superresolution structured pump-probe microscopy' in the journal 'ACS Photonics' which is contained within this thesis.; Andrew H. Hill, Casey L. Kennedy and Erik M. Grumstrup were co-authors of the article, 'Imaging theory of structured pump-probe microscopy' in the journal 'Optics Express' which is contained within this thesis.; Erik M. Grumstrup was a co-author of the article, 'Label-free saturated structured excitation microscopy' in the journal 'Photonics' which is contained within this thesis.; Erik M. Grumstrup was a co-author of the article, 'Exceptionally fast nanoscale exciton diffusion in donor-acceptor polymer thin films' which is contained within this thesis.; Erik M. Grumstrup was a co-author of the article, 'Toward direct imaging of sub-10 nm carrier diffusion lengths by differential detection pump-probe microscopy' which is contained within this thesis.Disordered semiconducting materials offer cost effective, solution processable alternatives to highly crystalline semiconducting materials for utilization in a variety of optoelectronic devices. However, characterization of these complex materials systems using bulk spectroscopic methods is heavily influenced by chemical and morphological heterogeneity inherent to the material. The experiments described in this thesis are designed to improve the fundamental understanding of the photophysical processes in disordered solution processed semiconducting materials by developing and utilizing high spatial resolution spectroscopic methods. Chapters 2-4 will outline the experimental and theoretical development of two superresolution spectroscopic techniques. First (chapters 2 & 3), structured pump-probe microscopy (SPPM) utilizes a structured excitation profile along with a diffraction limited probe pulse to achieve ~100 nm spatial resolution. Using SPPM it is also possible to collect time resolved spectroscopic data from a sub-diffraction limited volume. Second (chapter 4), label-free saturated structured excitation microscopy (LF-SSEM) is theoretically developed. LF-SSEM is experimentally similar to SPPM but exploits the saturation of the absorption process to achieve even greater resolution enhancement. Here, simulated LF-SSEM is shown to achieve ~33 nm spatial resolution. Chapter 5 demonstrates the utilization of PPM to investigate exciton transport in the organic semiconducting polymer (OSP), poly [N-9''-hepta-decanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT). Although OSPs have shown great promise for use in a variety of optoelectronic applications, much remains un-known about their excited state dynamics. The data reported here represents a significant contribution to the rapidly growing wealth of knowledge pertaining to OSP systems. Specifically, the microscale exciton diffusivity observed in PCDTBT thin films using PPM is found to reach 3.2 cm 2/s. Chapter 6 examines a technique in the early stages of development and optimization that is able to detect excited state carrier diffusion with increased sensitivity and accuracy compared to PPM. Differential detection pump-probe microscopy (DDPPM) uses two probe pulses to selectively eliminate the signal of carriers that have not diffused beyond the boundaries of the initial excitation. The experiments described within this dissertation are diverse, yet the common goal is to increase and improve the knowledge of photophysical properties in disordered semi-conducting materials. This goal takes two forms in the development of novel spectroscopic methodology and the characterization of complex materials using PPM. The singular result is the advancement of basic science pertaining to complex semiconducting materials systems.Item Organic enrichment at aqueous interfaces studied with non-linear spectroscopy: cooperative adsorption of soluble saccharides to lipid monolayers(Montana State University - Bozeman, College of Letters & Science, 2019) Link, Katie Ann; Chairperson, Graduate Committee: Robert Walker; Chia-Yun Hsieh, Aashish Tuladhar, Zizwe Chase, Zheming Wang, Hongfei Wang and Robert A. Walker were co-authors of the article, 'Vibrational studies of saccharide-induced lipid film reorganization at aqueous/vapor interfaces' in the journal 'Chemical physics' which is contained within this thesis.; Gabrielle N. Spurzem, Aashish Tuladhar, Zizwe Chase, Zheming Wang, Hongfei Wang and Robert A. Walker were co-authors of the article, 'Organic enrichment at aqueous interfaces: cooperative adsorption of glucuronic acid to DPPC monolayers studied with vibrational sum frequency generation' submitted to the journal 'Journal of physical chemistry B' which is contained within this thesis.; Gabrielle N. Spurzem, Aashish Tuladhar, Zizwe Chase, Zheming Wang, Hongfei Wang, and Robert A. Walker were co-authors of the article, 'Cooperative adsorption of trehalose to DPPC studied with vibrational sum frequency generation' which is contained within this thesis.Field measurements of sea spray aerosols have reported high concentrations of soluble organic material that are in excess of the concentration of soluble organics in the ocean. The studies described in this dissertation investigated a possible mechanism for this increase deemed cooperative adsorption. The cooperative adsorption mechanism describes an interaction between an insoluble Langmuir monolayer at the aqueous/vapor interface and soluble organic molecules that would not normally be enriched at the surface. In this model, the soluble organics are drawn to the surface through non-covalent interactions with the lipid surfactant. This mechanism was investigated with the surface specific nonlinear optical technique, vibrational sum frequency generation spectroscopy. These optical measurements were coupled with surface tension measurements and differential scanning calorimetry measurements. To study cooperative adsorption, model systems were used; these were composed of a phosphatidylcholine lipid surfactant, DPPC, and soluble saccharides including glucosamine, glucuronic acid, and trehalose. Glucosamine, in both a positive and neutral state, induced ordering in both expanded and condensed DPPC monolayers, supporting cooperative adsorption as a mechanism. Glucuronic acid, an anion, ordered lipid monolayers in the limits that the lipid DPPC was moderately packed and there were no competing ions in solution. Trehalose, a larger, uncharged saccharide showed, through ordering the DPPC monolayer, indications of cooperative adsorption in moderately packed DPPC when the trehalose concentration was sufficiently high. These results support cooperative adsorption as a mechanism for the accumulation of soluble organics in sea spray aerosols with some limitations.Item Nonlinear correction of spectrally recovered, RF spectral features, readout with high frequency-chirped laser fields(Montana State University - Bozeman, College of Letters & Science, 2017) Oberto, Louis Joseph; Chairperson, Graduate Committee: Wm. Randall BabbittFrequency-chirped readout of spectral features from spatial-spectral (S2) materials, as a result of spectral hole-burning, has been in use as a radio-frequency (RF) spectrum analyzer for well over a decade. Previously, a signal processing deconvolution algorithm had been developed that enabled faster chirping, such that the chirp rate 'K' could be much greater than the desired resolution bandwidth (RBW). This broke past conventional limits for spectroscopic detection, which states that one needs to dwell on a spectral feature of width gamma for a time 1/gamma. For a chirp, this would mean that the square root of the chirp rate would need to be less than the RBW. For chirp rates on the order of gamma 2 or higher, nonlinearities begin to appear in detected signals depending on optical absorption depth, the chirp rate, and burned hole depths. Even with this algorithm, distortions still persist when very deep holes are burned in a high absorbing material, while the chirp rate is still very high. However, resolving spectral features under these conditions is desirable to increase the dynamic range of the SA. A new nonlinear signal processing technique that removes the nonlinearity has been developed, recovering the distorted signals. It was applied to RF signals spectrally absorbed in two different Tm 3+: YAG crystals, with measured absorption lengths of 1.9 and 2.5. The new algorithm is shown to work on multiple spectral holes simultaneously. Signals as wide as 1 MHz and as small as 300 kHz were recovered for a chirp rate of about 11.88 MHz/microsecond. These results show that very fast chirp rates could be used for highly absorbing materials, with deeply burned spectral holes. This could enable ultra-sensitive readout of a spectrum spanning hundreds of gigahertz, while pushing the dynamic range higher.