Submitted by Irene Nascimento (irene.kessia@ufpe.br) on 2017-04-12T17:11:36Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Ammis.pdf: 2193663 bytes, checksum: 132bcda3d18c7d64c2a148645f123479 (MD5) / Made available in DSpace on 2017-04-12T17:11:36Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Ammis.pdf: 2193663 bytes, checksum: 132bcda3d18c7d64c2a148645f123479 (MD5) Previous issue date: 2016-05-04 / Facepe / Neste trabalho apresentamos a caracterização de uma armadilha magneto ótica de átomos de Rb construída em nosso laboratório, juntamente com o seu princípio de funcionamento. O resfriamento é feito com lasers de diodo e tem como mecanismo básico a força de pressão de radiação, que é gerada pelos processos de absorção e emissão de fótons, juntamente com a ação de um campo magnético e a polarização dos feixes. O sistema consiste em três pares de feixes contrapropagantes nas direções x, y e z, com polarizações s+ e s, e um campo magnético que varía linearmente no espaço. Conseguimos armadilhar aproximadamente 108 átomos com um tempo de carga da ordem de 2 seg. Em paralelo realizamos medidas de mistura de quatro ondas degenerada em um vapor de átomos de Rb, na configuração de feixes quase-copropagantes. O sinal gerado no processo não linear foi estudado em função da frequência de um dos feixes enquanto o outro tinha sua frequência fixa; e se mostrou independe de qual dos feixes esta sendo sintonizado. Medidas simultâneas da transmissão do feixe de prova indicam que o processo não linear ocorre só na transição cíclica e envolve o grupo de átomos selecionados pelo feixe de frequência fixa. / In this work we present a characterization of magneto optical trap of 87Rb atoms built in our lab, along with its operating principle. The cooling is done with a diode laser and its basic mechanism is the force of radiation pressure, which is generated by the processes of absorption and emission of photons, together with the action of a magnetic field and polarization of the beams. The system consists of three pairs of counterpropagating beams in the x, y and z directions with s+ and s polarizations, and a magnetic field that varies linearly in space. We were able to trap about 108 atoms with a charging time of approximately 2 sec. In parallel we performed degenerate four wave mixing measures in a Rb vapor atoms using a quasi-copropagating beams configuration. The signal generated in the nonlinear process was studied as a function of one of laser’s while keep the other with a fixed frequency; and it showed independent of which of the beams is being tuned. Simultaneous measurements of the transmission of the probe beam indicates that the nonlinear process occurs only in the cyclic transition and involves the group of atoms selected by the beam with fixed frequency.

<p dir="ltr">Knowledge of transport processes plays a critical role in the development and application of materials in many technologies. As manufacturing technologies continue to push the geometries of materials to smaller scales, traditional means of predicting and measuring transport properties begin to fail. Micro and nanoscopic effects tend to alter transport phenomena in materials, leading to new physics and different properties from the bulk state. In particular, the dynamics of thermal transport of a material varies greatly in both spatial and temporal senses. Different energy carriers have intrinsically different mechanisms of thermal transport; depending on the time and lengths scales in question, the contribution to the overall thermal transport by one carrier may be vastly different than others. To characterize and understand the dynamics of thermal transport at these small scales, novel ultrafast experimental techniques and theories are crucially needed. This work will discuss the efforts made to develop a framework to measure and differentiate the dynamics of transport processes of a material due to different energy carriers using ultrafast optical techniques. This dissertation is organized as follows.</p><p dir="ltr">Chapter 1 gives a background in the theory of thermal transport. This will serve as the foundation for the physical models that are used to extract thermal properties from experimental works. A brief review of the advances in ultrafast experimental and theoretical works will also be given. This will assist in placing this work in the context of ongoing work in the thermal transport community. Chapter 2 illustrates the experimental setups and physical models used to measure the effective thermal transport properties of thin film materials. Steady-state optical measurements are used to quantify the effective, in-plane, anisotropic, thermal conductivity of a 2D material. Time resolved, ultrafast optical measurements are used to quantify the effective, out-of-plane, thermal conductivity of a material. Chapters 3 and 4 demonstrate the capabilities of an ultrafast spatiotemporal scanning pump-probe system, where the high temporal and nanometric resolution measurements directly probe the electron contribution to thermal transport in metals as well as the ambipolar diffusion of carriers in semiconductors. Lastly, Chapter 5 summarizes this dissertation and provides a discussion on the use of the developed experimental capabilities to probe transport of emerging materials.</p>

<p dir="ltr">The increasing availability of spatio-temporal information in the form of detailed time-resolved images sampled at very high framing rates has resulted in a search for mathematical techniques capable of extracting and relaying the pertinent underlying physics governing complex flows. Analysis relying on the usage of a solitary spectral, correlation, or modal decomposition techniques to identify dynamically significant information from large datasets may give an incomplete description of these phenomena. Moreover, fully resolved spatio-temporal measurements of these complex flow fields are needed for a complete and accurate description across a wide spectrum of length and time scales. The primary goals of this dissertation are address these challenges in two key aspects: (1) to improve and demonstrate the novel application of complementary data analysis and modal decomposition techniques to quantify the dynamics of flow systems that exhibit intricate patterns and behaviors in both space and time, and (2) to make advancements in achieving and characterizing high-resolution and high-speed quantitative measurements of turbulent mixing fields.</p><p dir="ltr">In the first goal, two canonical flow fields are considered, including an acoustically excited co-axial jet and a bluff-body stabilized flame. The local susceptibility of a nonreacting, cryogenic, coaxial-jet, rocket injector to transverse acoustics is characterized by applying dynamical systems theory in conjunction with complementary wavelet-based spectral decomposition to high-speed backlit images of flow field. The local coupling of the jet with external acoustics is studied as a function of the relative momentum flux ratio between the outer and inner jets, giving a quantitative description of the dynamical response of each jet to external acoustics as a function of the downstream distance from the nozzle.</p><p dir="ltr">Bluff bodies are a common feature in the design of propulsion systems owing to their ability to act as flame holders. The reacting wake behind the bluff body consists of a recirculation bubble laden with hot-products and wrapped between separated shear layers. The wake region of a bluff body is systematically investigated utilizing a technique known as robust dynamic mode decomposition (DMD) to discern the onset of the thermoacoustic instability mode, which is highly detrimental to aerospace propulsion systems. The approach enables quantification of the spatial distribution and behavior of coherent structures observed from different flows as a function of the equivalence ratio.</p><p dir="ltr">As modal decomposition techniques employ a certain degree of averaging in time, a novel space-and-time local filtering technique utilizing the well-defined characteristics of wavelets is introduced with a goal of temporally resolving the spatial evolution of irregular flow instabilities associated with specific frequencies. This provides insight into the existence of transient sub-modal characteristics representing intermittencies within seemingly stable modes. The flow fields obtained from the same two canonical flows are interrogated to demonstrate the utility of the technique. It has been shown that temporally resolved flow features obtained from wavelet filtering satisfactorily track the same modal featured derived from DMD, but reveal sub-modal spatial distortions or local non-stationarity of specific modal frequencies on a frame-by-frame basis.</p><p dir="ltr">Finally, to improve the ability to study the dynamical behavior of complex flows across the full range of spatio-temporal scales present, advancements are reported in the spatial and temporal quantitative measurement of the scalar quantities in turbulent mixing fields utilizing 100 kHz planar laser-induced fluorescence (PLIF) and Rayleigh scattering imaging of acetone. The imaging system provided a resolution of 55 µm with a field-of-view mapping of 18.5 µm/pixel on the camera sensor, which is three times better spatial resolution than the previous reported work to-date for similar flow fields that were investigated at 1/10^th the current measurement rate. The power spectra of instantaneous mixture fraction fluctuations adhere to Kolmogorov's well-established -5/3 law, showing that the technique captures a significant range of dissipation scales. This observation underscores the ability to study mixing dynamics throughout the turbulent by fully resolving scalar fluctuations up to 30 kHz. This enhanced spatio-temporal resolution allows for a more detailed investigation of the dynamical behavior of turbulent flows with complex modal interactions down to the smallest diffusion limited mixing scales.</p>

<div>Vibrational spectroscopic imaging has become an emerging platform for chemical visualization of biomolecules and materials in complex systems. For over a century, both Raman and infrared spectroscopy have demonstrated the capability to recognize molecules of interest by harnessing the characteristic features from molecular fingerprints. With the recent development of hyperspectral vibrational spectroscopy imaging, which records the chemical information without sacrificing the spatial-temporal resolution, numerous discoveries has been achieved in the field of molecular and cellular biology. Despite the ability to provide complimentary chemical information to Raman-based approaches, infrared spectroscopy has not been extensively applied in routine studies due to several fundamental limitations: 1). the poor spatial resolution; 2). inevitable strong water absorption; 3). lack of depth resolution.</div><div>Mid-infrared photothermal (MIP) microscopy overcame all the above mentioned problems and for the first time, enabled depth-resolved in vivo infrared imaging of live cells, microorganisms with submicrometer spatial resolution. The development of epi-detected MIP microscopy further extends its application in pharmaceutical and materials sciences. With the deployment of difference frequency generation and other nonlinear optical techniques, the spectral coverage of the MIP microscopy was significantly enhanced to enable chemical differentiation in complex systems across the broad mid-infrared region. In addition to the efforts to directly improve the performance of MIP microscopy, a novel quantitative phase imaging approach based on polarization wavefront shaping via custom-designed micro-retarder arrays was developed to take advantage of the highly sensitive phase measurement in combination with the photothermal effect. Besides, the extended depth-of-field and multifocus imaging enabled by polarization wavefront shaping could both improve the performance of MIP microscopy for volumetric imaging.</div>

<p dir="ltr">The objective of this research is to advance the development and application of laser diagnostics in gas phase medium, which ranges from atmospheric non-reacting flows to turbulent reacting flows in high-pressure, high-temperature environments. Laser diagnostic techniques are powerful tools for non-intrusive and in-situ measurements of important chemical parameters, such as temperature, pressure, and species mole fractions, in harsh environments. These measurements significantly advance the knowledge across various research disciplines, such as combustion dynamics, chemical kinetics, and molecular spectroscopy. In this thesis, detailed theoretical models and experimental analysis are presented for three different techniques: 1. Chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CPP fs CARS); 2. Two-color polarization spectroscopy (TCPS); 3. Ultrafast-laser-absorption-spectroscopy (ULAS). The first chapter provides a brief survey of laser diagnostics, including both linear and nonlinear methods. The motivations behind the three studies covered in this dissertation are also discussed. </p><p dir="ltr">In the second chapter, single-shot CPP fs CARS thermometry is developed for the hydrogen molecule at 5 kHz. The results are divided into two parts. The first part concentrates on the development of H₂ CPP fs CARS thermometry for high-pressure and high-temperature conditions. The second part demonstrates the application of H₂ CPP fs CARS in a model rocket combustor at pressures up to 70 bar. In the first part, H₂ fs CARS thermometry was performed in Hencken burner flames up to 2300 K, as well as in a heated gas-cell at temperatures up to 1000 K. It was observed that the H₂ fs CARS spectra are highly sensitive to the pump and Stokes chirp. Chirp typically originates from optical components such as windows and polarizers. As a result, the pump delay is modeled to provide a shift to the Raman excitation efficiency curve. With the updated theoretical model, excellent agreement was found between the simulated and experimental spectra. The averaged error and precision are 2.8% and 2.3%, respectively. In addition, the spectral phase and pump delay determined from the experimental spectra closely align with the theoretical predictions. It is also found that pressure does not have significant effects on the H₂ fs CARS spectra up to 50 bar at 1000 K. The collision model provides excellent agreement with the experiment. This allows the use of low-pressure laser parameters for high-pressure thermometry measurements. In the second part, spatially resolved H₂ temperature was measured in a rocket chamber at pressures up to 70 bar. This is the first demonstration of fs CARS thermometry inside a high-pressure rocket combustor. These results highlight the potential of using H₂ CPP fs CARS thermometry to provide quantitative data in high-pressure experiments for the study of combustion dynamics and model validation efforts at application relevant operating conditions.</p><p dir="ltr">The third chapter presents the development of a TCPS system for the study of the NO (<i>A</i>²Σ⁺-<i>X</i>²Π) state-to-state collision dynamics with He, Ar, and N₂. Two sets of TCPS spectra for 1% NO, diluted in different buffer gases at 295 K and 1 atm, were obtained with the pump beam tuned to the R₁₁(11.5) and ^OP₁₂(1.5) transitions. The probe was scanned while the pump beam was tuned to the line center. Collision induced transitions were observed in the spectra as the probe scanned over transitions that were not coupled with the pump frequency. The strength and structure of the collision induced transitions in the TCPS spectra were compared between the three colliding partners. Theoretical TCPS spectra, calculated by solving the density matrix formulation of the time-dependent Schrödinger wave equation, were compared with the experimental spectra. A collision model based on the modified exponential-gap law was used to model the rotational level-to-rotational level collision dynamics. An unique aspect of this work is that the collisional transfer from an initial to a final Zeeman state was modeled based on the difference in the cosine of the rotational quantum number <i>J</i> projection angle with the z-axis for the two Zeeman states. Rotational energy transfer rates and Zeeman state collisional dynamics were varied to obtain good agreement between theory and experiment for the two different TCPS pump transitions and for the three different buffer gases. One key finding, in agreement with quasi-classical trajectory calculations, is that the spin-rotation changing transition rate in the <i>A</i>²Σ⁺ level of NO is almost zero for rotational quantum numbers ≥ 8. It was necessary to set this rate to near zero to obtain agreement with the TCPS spectra. </p><p dir="ltr">The fourth chapter presents the development and application of a broadband ULAS technique operating in the mid-infrared for simultaneous measurements of temperature, methane (CH₄), and propane (C₃H₈) mole fractions. Single-shot measurements targeting the C-H stretch fundamental vibration bands of CH₄ and C₃H₈ near 3.3 μm were acquired in both a heated gas cell up to ~650 K and laminar diffusion flames at 5 kHz. The average temperature error is 0.6%. The average species mole fraction error are 5.4% for CH₄, and 9.9% for C₃H₈. This demonstrates that ULAS is capable of providing high-fidelity hydrocarbon-based thermometry and simultaneous measurements of both large and small hydrocarbons in combustion gases. </p>

<p dir="ltr">Optical frequency combs have revolutionized metrology and advanced other fields such as RF photonics and astronomy. While powerful, they can be bulky, expensive, and difficult to manufacture. This tends to limit uses in real-world scenarios. Within the last decade or so, coherent frequency combs have begun to be generated in millimeter-scale, CMOS fabrication-compatible nonlinear crystals. These so-called “microcombs” have led to hopes of overcoming deployability constraints of more traditional bulk combs.</p><p dir="ltr">One of the first applications for \textit{bulk} frequency combs after their explosion in 2000 was the optical atomic clock. It promised extreme long-term time stability better than that of the Cesium clock that currently defines the SI second. More recently, interest in a fully portable optical atomic clock has grown. Such a device could reliably keep time even without the aid of GPS references, and potentially with greater accuracy than current GPS synchronization can provide.</p><p dir="ltr">Frequency combs have also been used to sample electrical signals more rapidly than traditional electronics can accomplish. This has been used to achieve dramatically increased effective frequency bandwidths for signal detection architectures. One can imagine how this capability would be beneficial in a portable (microcomb-driven) form: a lightweight, comb-enhanced receiver able to capture a broadband snapshot of its surrounding electromagnetic environment could be a powerful tool.</p><p dir="ltr">Timekeeping and RF photonics are the primary applications of microcombs focused upon here. I will attempt to roughly summarize important concepts and highlight relevant work in both subjects in the Introduction. Then I will move a step closer to the hands-on lab work that has largely kept me preoccupied over the last several years and describe important or commonly-employed Methods for experiments. A collection of three journal manuscripts (two published, and the third recently submitted) will follow in the Publications chapter, highlighting some experimental results. Finally, I will conclude with a brief Outlook.</p>

<p dir="ltr">Laser absorption spectroscopy (LAS) is a widely used technique to acquire path-integrated measurements of gas properties such as temperature and mole fraction. Although extremely useful, the application of LAS to study heterogeneous combustion environments can be challenging. For example, beam steering can be one such challenge that arises during measurements in heterogeneous combustion environments such as metallized propellant flames or measurements at high-pressure conditions. The ability to only obtain path integrated measurements has been a major challenge of conventional LAS techniques, especially in characterizing combustion environments with a non-uniform thermo-chemical distribution along the line of sight (LOS). Additionally, simultaneous measurements of multiple species using LAS with narrow-bandwidth lasers often necessitates employing multiple light sources. Aerospace applications, such as characterizing hypersonic flows may require ultrashort time resolution to study fast-evolving chemistry. Similarly, atmospheric entry most often requires measurements of atoms and molecules that absorb at wavelengths ranging from ultraviolet to mid-infrared. The availability of appropriate light sources for such measurements has been limited. In the past, several researchers have come up with diagnostic techniques to overcome the above-mentioned challenges to a certain extent. Most often, these solutions have been need-based while compromising on other diagnostic capabilities. Therefore, LAS diagnostics capable of acquiring broadband measurements with ultrafast time resolution and the ability to acquire measurements at wavelengths in ultraviolet through mid-infrared is required to study advanced combustion systems and for the development of advanced aerospace systems for future space missions. Ultrafast laser absorption spectroscopy is one such technique that provides broadband measurements, enabling simultaneous multi-species and high-pressure measurements. The light source utilized for ULAS provides the ultrafast time resolution necessary for resolving fast-occurring chemistry and more importantly the ability to acquire measurements at a wide range of wavelengths ranging from ultraviolet to far-infrared. The development and application of ULAS for characterizing propellant flames and hypersonic flows under non-equilibrium conditions by overcoming the above-mentioned challenges is presented here. </p><p>This work describes the development of a single-shot ultrafast laser absorption spectroscopy (ULAS) diagnostic for simultaneous measurements of temperature and concentrations of CO, NO, and H₂O in flames and aluminized fireballs of HMX (C₄H₈N₈O₈). Ultrashort (55 fs) pulses from a Ti:Sapphire oscillator emitting near 800 nm were amplified and converted into the mid-infrared through optical parametric amplification (OPA) at a repetition rate of 5 kHz. Ultimately, pulses with a spectral bandwidth of ≈600 cm^-1 centered near 4.9 µm were utilized in combination with a mid-infrared spectrograph to measure absorbance spectra of CO, NO, and H₂O across a 30 nm bandwidth with a spectral resolution of 0.3 nm. The gas temperature and species concentrations were determined by least-squares fitting simulated absorbance spectra to measured absorbance spectra. Measurements of temperature, CO, NO, and H₂O were acquired in an HMX flame burning in air at atmospheric pressure and the measurements agree well with previously published results. Measurements were also acquired in fireballs of HMX with and without 16.7 wt% H-5 micro-aluminum. Time histories of temperature and column densities are reported with a 1-σ precision of 0.4% for temperature and 0.3% (CO), 0.6% (NO), and 0.5% (H₂O), and 95% confidence intervals (C.I.) of 2.5% for temperature and 2.5% (CO), 11% (NO), and 7% (H₂O), thereby demonstrating the ability of ULAS to provide high-fidelity, multi-parameter measurements in harsh combustion environments. The results indicate that the addition of the micron-aluminum increases the fireball peak temperature by ≈100 K and leads to larger concentrations of CO. The addition of aluminum also increases the duration fireballs remain at elevated temperatures above 2000 K.</p><p dir="ltr">Next, the application of ULAS for dual-zone temperature and multi-species (CO, NO, H₂O, CO₂, HCl, and HF) measurements in solid-propellant flames is presented. ULAS measurements were acquired at three different central wavelengths (5.121 µm, 4.18 µm, and 3.044 µm) for simultaneous measurements of temperature and: 1) CO, NO, and H₂O, 2) CO₂ and HCl, and 3) HF and H₂O. Absorption measurements with a spectral resolution of 0.35 nm and bandwidth of 7 cm^-1, 18 cm^-1, and 35 cm^-1, respectively were acquired. In some cases, a dual-zone absorption spectroscopy model was implemented to accurately determine the gas temperature in the hot flame core and cold flame boundary layer via broadband absorption measurements of CO₂, thereby overcoming the impact of line-of-sight non-uniformities. Results illustrate that the hot-zone temperature of CO₂ agrees well with the equilibrium flame temperature and single-zone thermometry of CO, the latter of which is insensitive to the cold boundary layer due to the corresponding oxidation of CO to CO₂.</p><p dir="ltr">The initial development and implementation of an ultraviolet and broadband ultrafast-laser-absorption-imaging (UV-ULAI) diagnostic for one dimensional (1D) imaging of temperature and CN via its <i>B</i>²Σ⁺←<i>X</i>²Σ⁺absorption bands near 385 nm. The diagnostic was demonstrated by acquiring single-shot measurements of 1D temperature and CN profiles in HMX flames at a repetition rate of 25 Hz. Ultrashort pulses (55 fs) at 800 nm were generated using a Ti:Sapphire oscillator and then amplification and wavelength conversion to the ultraviolet was carried out utilizing an optical parametric amplifier and frequency doubling crystals. The broadband pulses were spectrally resolved using a 1200 l/mm grating and imaged on an EMCCD camera to obtain CN absorbance spectra with a resolution of ≈0.065 nm and a bandwidth of ≈4 nm (i.e. 260 cm^-1). Simulated absorbance spectra of CN were fit to the measured absorbance spectra using non-linear curve fitting to determine the gas properties. The spatial evolution of gas temperature and CN concentration near the burning surface of an HMX flame was measured with a spatial resolution of ≈10 µm. 1D profiles of temperature and CN concentration were obtained with a 1-σ spatial precision of 49.3 K and 4 ppm. This work demonstrates the ability of UV-ULAI to acquire high-precision, spatially resolved absorption measurements with unprecedented temporal and spatial resolution. Further, this work lays the foundation for ultraviolet imaging of numerous atomic and molecular species with ultrafast time resolution.</p><p dir="ltr">Ultraviolet ULAS was applied to characterize the temporal evolution of non-Boltzmann CN (<i>X</i>²Σ⁺) formed behind strong shock waves in N₂-CH₄ mixtures at conditions relevant to entry into Titan's atmosphere. An ultrafast (femtosecond) light source was utilized to produce 55 fs pulses near 385 nm at a repetition rate of 5 kHz and a spectrometer with a 2400 lines/mm grating was utilized to spectrally resolve the pulses after passing through the Purdue High-Pressure Shock Tube. This enabled broadband single-shot absorption measurements of CN to be acquired with a spectral resolution and bandwidth of ≈0.02 nm and ≈6 nm (≈402 cm^-1 at these wavelengths), respectively. A line-by-line absorption spectroscopy model for the <i>B</i>²Σ⁺←<i>X</i>²Σ⁺ system of CN was developed and utilized to determine six internal temperatures (two vibrational temperatures, four rotational) of CN from the (0,0), (1,1), (2,2) and (3,3) absorption bands. Measurements were acquired behind reflected shock waves in 5.65% CH₄ and 94.35% N₂ with an initial pressure of 1.56 mbar and incident shock speed of ≈2.1 km/s. For this test condition, the chemically and vibrationally frozen temperature of the mixture behind the reflected shock was 5000 K and the pressure was 0.6 atm. The high repeatability of the shock-tube experiments (0.3% variation in shock speed across tests) enabled multi-shock time histories of CN mole fraction and six internal temperatures to be acquired with a single-shot time resolution of less than 1 ns. The measurements revealed that CN <i>X</i>²Σ⁺ is non-Boltzmann rotationally and vibrationally for greater than 200 µs, thereby strongly suggesting that chemical reactions are responsible for the non-Boltzmann population distributions. </p><p><br></p>

<p dir="ltr">In recent years, nanosecond repetitively pulsed (NRP) plasma discharges have garnered significant interest due to their rapid generation of reactive excited-state species, reactive radicals, and localized heat release within nanosecond (ns) timescale. To effectively harness these plasmas for altering system-level thermal and chemical behavior, a thorough understanding of their governing physics is crucial. This knowledge enables the development of predictive plasma kinetic models for tailoring NRP plasmas to specific applications. However, achieving this requires high-fidelity experimental data to validate models and deepen our understanding of fundamental plasma physics. Advancing experimental spectroscopy and laser diagnostics methods is essential for probing such temporally highly dynamic and optically complex nonequilibrium environments. This includes developing novel <i>test platforms</i>, conducting <i>fundamental research</i> to address existing knowledge gaps, and constructing custom <i>ultrafast laser architectures</i> for probing plasma properties. </p><p dir="ltr">The pioneering development of Streak-based <i>test platform</i> in the diagnostics field of nanosecond pulsed plasmas and its successful application towards inferring the underlying ultrafast spatio-temporal evolution of nanosecond pulsed plasma discharges with an unprecedented time-resolution as short as ~25 ps is presented for the first time. Spectrally filtered, 1D line-imaging of nanosecond pulsed plasma discharges in a single-shot, jitter-free, continuously sweeping manner is obtained, and differences in discharge dynamics of air and N2 plasma environments are studied. Successive <i>test platform</i> advancement includes spectrally resolved Streak-spectroscopy measurements of thermal regime-transition evolution from early-nonequilibrium to local-thermal-equilibrium (LTE) to attain time-resolved quantitative insights into N2(C) state rotational/vibrational nonequilibrium temperatures, electron temperature/density, and spectral lifetime dynamics. </p><p dir="ltr">Ultrafast laser-based progression includes detailed <i>fundamental</i> investigation of higher-order optical nonlinearity perturbations of fs-EFISH by considering of – self-phase modulation induced spectral characteristic of fs-EFISH signal, calibration mapping during-below-and-beyond optical breakdown regime, optical Kerr effect consequences, impact of femtosecond (fs) laser seeding on the noninvasiveness of fs-EFISH, and spectral emission characteristics of fs laser filaments. To infer N2(X) state nonequilibrium of NRP pulsed plasmas, two hybrid fs/ps ro-vibrational coherent anti-Stokes Raman scattering (CARS) <i>ultrafast laser architectures</i> are developed. First architecture, single-laser-solution, reduces system’s energy budget by ~3 mJ/pulse for generating narrowband (~21 ps), high-energy (~420 μJ/pulse), 532 nm probe pulses through incorporation of custom built visible fs optical parametric amplifier (OPA) coupled with an Nd:YAG power amplifier module. The second architecture, two-laser-solution, improves system’s robustness through the development of a 1 kHz, 532 nm, high-energy (~600 μJ/pulse), low-jitter (<1 ps), narrowband (~27 ps), master-oscillator-power-amplification (MOPA) based picosecond probe pulse laser time-synchronized with fs master-oscillator. Single-shot, hybrid fs/ps narrowband ro-vibrational CARS demonstration in a combusting flame up to temperatures of ~2400 K is demonstrated. Experimental ro-vibrational CARS investigation includes polarization based nonresonant background suppression and demonstration of preferential Raman coherence excitation shift, a temperature sensitivity enhancing strategy for vibrationally hot mediums like nanosecond pulsed plasmas. Lastly, an ultrafast pulse-friendly optically accessible vacuum cell is designed and fabricated for controlled experiments of NRP fs/ps CARS. Special care is taken to prevent self-focusing and spectral-temporal chirp of fs CARS beams while maintaining Gaussian focusing beam caustic.</p>

<p>Ultrafast laser-based diagnostic techniques are powerful tools for the detailed understanding of highly dynamic combustion chemistry and physics. The ultrashort pulses provide unprecedented temporal resolution along with high peak power for broad spectral range−ideal for nonlinear signal generation at high repetition rate−with applications including next-generation combustors for gas turbines, plasma-assisted combustion, hypersonic flows and rotating detonation engines. The current work focuses on advancing (i) femtosecond (fs) two-photon laser-induced fluorescence, and (ii) hybrid femtosecond/picosecond vibrational and rotational coherent anti-Stokes Raman scattering (fs/ps RCARS and VCARS) to higher pressures for the first time. </p><p>Quantitative single-laser-shot kHz-rate concentration measurements of key atomic (O-atom) and molecular (CO) species is presented using femtosecond two-photon laser-induced fluorescence (TP-LIF) for a range of equivalence ratios and pressures in diffusion flames. A multitude of signal-interfering sources and loss mechanisms−relevant to high-pressure fs TP-LIF applications−are also quantified up to 20 atm to ensure high accuracy. The pressure scaling of interferences take into account degradation, attenuation and wave-front distortion of the excitation laser pulse; collisional quenching and pressure dependent transition line-broadening and shifting; photolytic interferences; multi-photon ionization; stimulated emission; and radiation trapping. </p><p>Hybrid fs/ps VCARS of N₂ is reported for interference-free temperature measurement at 1300-2300 K in high-pressure, laminar diffusion flames up to 10 atm. A time asymmetric probe pulse allowed for detection of spectrally resolved CARS signals at probe delays as early as ~200-300 fs while being independent of collisions for the full range of pressures and temperatures. Limits of collisional independence, accuracy and precision of the measurement is explored at various probe-pulse delays, pressures and temperatures. </p><p> </p><p>Additionally, a novel all diode-pumped Nd:YAG amplifier design is presented for generation of time-synchronized ps-probe pulses for hybrid fs/ps RCARS of N₂. High-energy, nearly transform-limited, single-mode, chirp-free ps probe-pulses are generated at variable pulsewidths. The detailed architecture and characterization of the laser is presented. kHz-rate RCARS thermometry is presented up to 2400 K. Excellent spatial, spectral, and temporal beam quality allowed for fitting the theoretical spectra with a simple Gaussian model for the probe pulse with temperature accuracies of 1-2%. </p> <p><br></p>