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Coupled optical and electrical study of thin-film InGaAs photodetector integrated with surface InP Mie resonators

High-index dielectric and semiconductor nanostructures with characteristics of low absorption loss and artificially controlled scattering properties have grasped an increasing attention for improving the performance of thin-film photovoltaic devices. In this work, combined optical and electrical simulations were performed for thin-film InP/In{sub 0.53}Ga{sub 0.47}As/InP hetero-junction photodetector with periodically arranged InP nano-cylinders in the in-coupling configuration. It is found that the carefully designed InP nano-cylinders possess strongly substrate-coupled Mie resonances and can effectively couple incident light into the guided mode, both of which significantly increase optical absorption. Further study from the electrical aspects shows that enhancement of external quantum efficiency is as high as 82% and 83% in the configurations with the optimized nano-cylinders and the optimized period, respectively. Moreover, we demonstrate that the integration of InP nano-cylinders does not degrade the electrical performance, since the surface recombination is effectively suppressed by separating the absorber layer where carriers generate and the air/semiconductor interface. The comprehensive modeling including optical and electrical perspectives provides a more practical description for device performance than the optical-only simulation and is expected to advance the design of thin-film absorber layer based optoelectronic devices for fast response and high efficiency.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Computational analysis of metamaterial–aluminum–silicon solar cell model

In this paper, the optical parameters of an improved waveguide structure for a more efficient silicon solar cell are studied. Despite its favorable electronic, physical, and chemical properties, silicon remains a poor absorber of light. The optical losses due to the reflection at the air/glass interface of the cell and the transmission at its back are other factors, which limit the cell conversion efficiency. Consequently, several mechanisms for light trapping capable to increase the collection of the incident photons as electrical current and to decrease the transmission loss, have been developed. In this context, we propose a multilayer waveguide structure in which the sunlight is guided by a metamaterial layer and the transmission loss is eliminated by an aluminum back reflector. The reflection and transmission coefficients are derived by using the Generalized Transfer Matrix Method. The application of the law of conservation of energy allowed the determination of the absorption coefficient. These optical parameters are examined for several angles of incidence for s-polarized light, p-polarized light and unpolarized light. Simulation results show a significant reduction of reflection and a complete suppression of transmission.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ground and Airborne Methane Measurements with an Optical Parametric Amplifier

We report on ground and airborne atmospheric methane measurements with a differential absorption lidar using an optical parametric amplifier (OPA). Methane is a strong greenhouse gas on Earth and its accurate global mapping is urgently needed to understand climate change. We are developing a nanosecond-pulsed OPA for remote measurements of methane from an Earth-orbiting satellite. We have successfully demonstrated the detection of methane on the ground and from an airplane at approximately 11-km altitude.

Numata, Kenji↗

A new sample of obscured AGNs selected from the XMM-Newton and AKARI surveys

We report a new sample of obscured active galactic nuclei (AGNs) selected from the XMM-Newton serendipitous source and AKARI point-source catalogs. We match X-ray sources with infrared (18 and 90 μm) sources located at |b|>10{sup ∘} to create a sample consisting of 173 objects. Their optical classifications and absorption column densities measured by X-ray spectra are compiled and study efficient selection criteria to find obscured AGNs. We apply the criteria (1) X-ray hardness ratio defined by using the 2–4.5 keV and 4.5–12 keV bands > −0.1 and (2) EPIC-PN count rate (CR) in the 0.2–12 keV to infrared flux ratio CR/F{sub 90}<0.1 or CR/F{sub 18}<1, where F{sub 18} and F{sub 90} are infrared fluxes at 18 and 90 μm in Jy, respectively, to search for obscured AGNs. X-ray spectra of 48 candidates, for which no X-ray results have been published, are analyzed and X-ray evidence for the presence of obscured AGNs such as a convex shape X-ray spectrum indicative of absorption of N{sub H} ∼ 10{sup 22–24} cm{sup −2}, a very flat continuum, or a strong Fe–K emission line with an equivalent width of >700 eV is found in 26 objects. Six of them are classified as Compton-thick AGNs, and four are represented by either Compton-thin or Compton-thick spectral models. The success rate of finding obscured AGNs combining our analysis and the literature is 92% if the 18 μm condition is used. Of the 26 objects, 4 are optically classified as an H ii nucleus and are new “elusive AGNs” in which star formation activity likely overwhelms AGN emission in the optical and infrared bands.

79 ASTRONOMY AND ASTROPHYSICS↗

Understanding the unique optical and vibrational signatures of sequential infiltration synthesis derived indium oxyhydroxide clusters for CO 2 absorption

Sequential infiltration synthesis (SIS) is a vapor phase synthesis technique with potential to exert precise control over metal oxyhydroxide incorporation into polymer scaffolds. Here, we observe strong size-dependent properties of InO x (OH) y few-atom clusters deposited with variable SIS cycle numbers within a polymethylmethacrylate (PMMA) matrix. Infrared spectroscopy and ultraviolet-visible absorption spectroscopy reveal that the metal atom coordination and optical properties of the clusters depend on the number of SIS cycles performed as well as the choice of processing parameters. The incorporation of indium oxyhydroxide in PMMA via SIS presents an opportunity to improve the CO 2 absorption capacity and gas selectivity of inexpensive polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

X-RAY SPECTRAL RESIDUALS IN NGC 5408 X-1: DIFFUSE EMISSION FROM STAR FORMATION, OR THE SIGNATURE OF A SUPER-EDDINGTON WIND?

If ultraluminous X-ray sources (ULXs) are powered by accretion onto stellar remnant black holes, then many must be accreting at super-Eddington rates. It is predicted that such high accretion rates should give rise to massive, radiatively driven winds. However, observational evidence of a wind, in the form of absorption or emission features, has remained elusive. As such, the reported detection of X-ray spectral residuals in XMM-Newton spectra of NGC 5408 X-1, which could be related to absorption in a wind is potentially very exciting. However, it has previously been assumed by several authors that these features simply originate from background diffuse plasma emission related to star formation in the ULX’s host galaxy. In this work we utilize the spatial resolving power of Chandra to test whether we can rule out this latter interpretation. We demonstrate that the majority of the luminosity in these spectral features is emitted from a highly localized region close to the ULX, and appears point-like even with Chandra. It is therefore highly likely that the spectral features are associated with the ULX itself, and little of the flux in this spectral component originates from spatially extended emission in the host galaxy. This may be consistent with the suggestion of absorption in an optically thin phase of a super-Eddington wind. Alternatively, we could be seeing emission from collisionally ionized material close to the black hole, but critically this would be difficult to reconcile with models where the source inclination largely determines the observed X-ray spectral and timing properties.

79 ASTRONOMY AND ASTROPHYSICS↗

Unraveling electronic absorption spectra using nuclear quantum effects: Photoactive yellow protein and green fluorescent protein chromophores in water

Many physical phenomena must be accounted for to accurately model solution-phase optical spectra line shapes, from the sampling of chromophore-solvent configurations to the electronic-vibrational transitions leading to vibronic fine structure. Here we thoroughly explore the role of nuclear quantum effects, direct and indirect solvent effects, and vibronic effects in the computation of the optical spectrum of the aqueously solvated anionic chromophores of green fluorescent protein (GFP) and photoactive yellow protein (PYP). By analyzing the chromophore and solvent configurations, the distributions of vertical excitation energies, the absorption spectra computed within the ensemble approach, and the absorption spectra computed within the ensemble plus zero-temperature Franck-Condon approach, we introduce how solvent, nuclear quantum effects, and vibronic transitions alter the optical absorption spectra. We discover that including nuclear quantum effects in the sampling of chromophore-solvent configurations using ab initio path integral molecular dynamics simulations leads to improved spectral shapes through three mechanisms. The three mechanisms that lead to line shape broadening and a better description of the high-energy tail are softening of heavy atom bonds in the chromophore that couple to the optically bright state, widening the distribution of vertical excitation energies from more diverse solvation environments, and redistributing spectral weight from the 0-0 vibronic transition to higher energy vibronic transitions when computing the Franck-Condon spectrum in a frozen solvent pocket. The absorption spectra computed using the combined ensemble plus zero-temperature Franck-Condon approach yield significant improvements in spectral shape and width compared to spectra computed with the ensemble approach. Using the combined approach with configurations sampled from path integral molecular dynamics trajectories presents a significant step forward in accurately modeling the absorption spectra of aqueously solvated chromophores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Method of increasing power within an optical cavity with long path lengths

A cavity-enhanced absorption spectroscopy instrument has an optical cavity with two or more cavity mirrors, one mirror of which having a hole or other aperture for injecting a light beam, and the same or another mirror of which being partially transmissive to allow exit of light to a detector. A spherical-spherical configuration with at least one astigmatic mirror or a spherical-cylindrical configuration where the spherical mirror could also be astigmatic prevents a reentrant condition wherein the injected beam would prematurely exit the cavity through the aperture. This combination substantially increases the number of passes of the injected beam through a sample volume for sensitive detection of chemical species even in less than ideal conditions including low power laser or LED sources, poor mirror reflectivity or detector noise at the wavelengths of interest, or cavity alignment issues such as vibration or temperature and pressure changes.

47 OTHER INSTRUMENTATION↗

Quantum Mechanical Simulations of Dynamics of Electronic Excitations in Low-Dimensional Photovoltaics Materials

Dynamics of electronically excited states including exciton generation and relaxation, exciton-exciton interaction, and charge/energy transfer and transport, are critical to understanding and optimizing photovoltaic materials. Although considerable progress has been made, accurate experimental characterization of such crucial dynamics remains extremely challenging, especially in low-dimensional materials. In this talk, I will discuss how the advancement of quantum mechanical simulations of the dynamics of electronic excitations can reveal the physical mechanisms hindering or improving solar energy harvest. Specifically, we find that surface dangling-bond defects on silicon quantum dots cause rapid charge recombination and low carrier mobility in the inorganic-organic PV cells. Although small quantum dots are essentially free of defects, their optical gaps are too large. To solve this issue, a full-spectrum-light-absorption scheme is computationally designed, taking advantage of complexity and flexibility of low-dimensional materials consisting of different characteristics and dimensions. In this scheme the multifunctional ligands are used to (1) passivate against oxidation, (2) facilitate interfacial charge transfer, and (3) improve both charge transport and optical absorption. A joint theoretical and experimental study has demonstrated the feasibility of this approach. Finally, I will briefly talk about how this scheme and the well-tested quantum mechanical simulations can be employed to help improve energy-conversion efficiency in perovskite photovoltaics including perovskite-based tandem cells.

Zhigang Wu↗

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in 17 manuscripts published in refereed journals.

54 ENVIRONMENTAL SCIENCES↗

Sensitive Thermochromic Behavior of InSeI, a Highly Anisotropic and Tubular 1D van der Waals Crystal

Thermochromism, the change in color of a material with temperature, is the fundamental basis of optical thermometry. A longstanding challenge in realizing sensitive optical thermometers for widespread use is identifying materials with pronounced thermometric optical performance in the visible range. Herein, it is demonstrated that single crystals of indium selenium iodide (InSeI), a 1D van der Waals (vdW) solid consisting of weakly bound helical chains, exhibit considerable visible range thermochromism. A strong temperature-dependent optical band edge absorption shift ranging from 450 to 530 nm (2.8 to 2.3 eV) over a 380 K temperature range with an experimental (dE g /dT) max value extracted to be 1.26 × 10 −3 eV K −1 is shown. This value lies appreciably above most dense conventional semiconductors in the visible range and is comparable to soft lattice solids. The authors further seek to understand the origin of this unusually sensitive thermochromic behavior and find that it arises from strong electron–phonon interactions and anharmonic phonons that significantly broaden band edges and lower the E g with increasing temperature. The identification of structural signatures resulting in sensitive thermochromism in 1D vdW crystals opens avenues in discovering low-dimensional solids with strong temperature-dependent optical responses across broad spectral windows, dimensionalities, and size regimes.

36 MATERIALS SCIENCE↗

Structural and optical studies of hydrothermally synthesized MoS{sub 2} nanostructures

Transition-metal dichalcogenides like molybdenum disulphide have intrigued intensive interest as two-dimensional (2D) materials beyond extensively studied graphene due to their unique electronic and optical properties. Here we report the hydrothermal synthesis of MoS{sub 2} nanostructures without the addition of any surfactants. The structural and optical properties of the synthesized samples were characterized by various techniques, including X-ray diffraction (XRD), UV-Vis absorption, photoluminescence (PL), and Raman analysis. XRD and Raman spectroscopic studies confirm the formation of hexagonal phase and well ordered stacking of S-Mo-S layers. The increased lattice parameters of MoS{sub 2} samples are due to the stress or strain induced bending and folding of the layers. The synthesized MoS{sub 2} nanostructures shows a large optical absorption in 300-700 nm region and strong luminescence at 640 nm. In addition, the optical results demonstrates the quantum confinement in layered d-electron material MoS{sub 2} that can lead to engineer its various properties for electronic and optoelectronic applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Graphene vertical hot-electron terahertz detectors

We propose and analyze the concept of the vertical hot-electron terahertz (THz) graphene-layer detectors (GLDs) based on the double-GL and multiple-GL structures with the barrier layers made of materials with a moderate conduction band off-set (such as tungsten disulfide and related materials). The operation of these detectors is enabled by the thermionic emissions from the GLs enhanced by the electrons heated by incoming THz radiation. Hence, these detectors are the hot-electron bolometric detectors. The electron heating is primarily associated with the intraband absorption (the Drude absorption). In the frame of the developed model, we calculate the responsivity and detectivity as functions of the photon energy, GL doping, and the applied voltage for the GLDs with different number of GLs. The detectors based on the cascade multiple-GL structures can exhibit a substantial photoelectric gain resulting in the elevated responsivity and detectivity. The advantages of the THz detectors under consideration are associated with their high sensitivity to the normal incident radiation and efficient operation at room temperature at the low end of the THz frequency range. Such GLDs with a metal grating, supporting the excitation of plasma oscillations in the GL-structures by the incident THz radiation, can exhibit a strong resonant response at the frequencies of several THz (in the range, where the operation of the conventional detectors based on A{sub 3}B{sub 5} materials, in particular, THz quantum-well detectors, is hindered due to a strong optical phonon radiation absorption in such materials). We also evaluate the characteristics of GLDs in the mid- and far-infrared ranges where the electron heating is due to the interband absorption in GLs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correction to “Ruthenium Dye Excitations and Relaxations in Natural Sunlight”

An error in computing the optical rate coefficients for dye RuP was discovered in Table S4 of the Supporting Information Section S8 Model S? for this article, published in J. Phys. Chem. A, 2021, 125, 4365-4372, 10.1021/acs.jpca.1c02386. The optical rate coefficients include absorption, stimulated emission, and ground-state bleach associated with the ground state and the singlet and triplet excited states as well as for the excited-state absorption between the excited states and implicit higher-energy excited states. The optical rate coefficients for continuous solar irradiance were computed using eq 3 of the main text in which the product of the individual signal components and the solar spectrum are integrated and multiplied by the fundamental optical rate coefficient. We determined the incorrect signal components were used for RuP in the published Supporting Information Table S4. The corrected Table S4 column for RuP is presented with the reported values from the original paper in the corrected Supporting Information. New simulations have been performed using the corrected values, and the results were used to update Figures 5 and 6 and also Figure S9 in the corrected Supporting Information. The published conclusions are unchanged. The populations of RuP excited states, Figure 5, are only marginally smaller, which should be expected with minor changes to the optical rate coefficients. There is not a significant change in the results for the number of radiative and nonradiative interactions per dye per second (the optical transitions and nonradiative transitions increased, respectively, by approximately 2% and 10%, Figure 6A). The occurrence of excited-state absorption (ESA) and excited-state emission (ESE) events, Figure 6C, both decreased from the original simulation results by 20% and 33%. The most notable difference is exhibited in Figure 6B; the fraction of population moving from the lowest-energy singlet state (i.e., intersystem crossing or ultrafast nonradiative relaxation) and nonradiative relaxation from the triplet state have decreased from ~0.45 to ~0.4 and increased from ~0.35 to ~0.4, respectively..

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bound Exciton Complexes in Near-Infrared Emitting Quantum Shells

Near-infrared (NIR) light sources based on colloidal semiconductor nanocrystals (NCs) represent a scalable, low-cost alternative to epitaxial semiconductor platforms. However, their performance remains hindered by rapid Auger recombination, a problem that is particularly pronounced in narrow-bandgap materials. Here, we report on CdS/HgS/CdS and CdS/HgCdSe/ ZnS quantum shells (QSs), a class of spherical quantum wells specifically engineered for a suppression of nonradiative Auger processes. Fabricated QSs exhibit tunable NIR emission with photoluminescence quantum yields reaching ∼60% below 1000 nm and up to 30% near 1300 nm. Optical gain and stimulated emission were observed in CdS/HgS/CdS QSs. In contrast, CdS/HgCdSe/ZnS QSs displayed a photoinduced absorption in lieu of optical gain despite demonstrating a comparatively stronger Auger suppression. Transient absorption spectroscopy revealed that this phenomenon arises from the formation of bound multiexciton complexes that induce long-lived sub-bandgap multiexciton states. The observation of such bound excitonic clusters at room temperature offers a pathway toward nonlinear NIR photonic phenomena, including biexciton−exciton cascade emission, optical modulation, and singleexciton gain.

Auger recombination↗

Recovering Interstellar Gas Properties with Hi Spectral Lines: A Comparison between Synthetic Spectra and 21-SPONGE

We analyze synthetic neutral hydrogen (H i) absorption and emission spectral lines from a high-resolution, three-dimensional hydrodynamical simulation to quantify how well observational methods recover the physical properties of interstellar gas. We present a new method for uniformly decomposing H i spectral lines and estimating the properties of associated gas using the Autonomous Gaussian Decomposition (AGD) algorithm. We find that H i spectral lines recover physical structures in the simulation with excellent completeness at high Galactic latitude, and this completeness declines with decreasing latitude due to strong velocity-blending of spectral lines. The temperature and column density inferred from our decomposition and radiative transfer method agree with the simulated values within a factor of <2 for the majority of gas structures. We next compare synthetic spectra with observations from the 21-SPONGE survey at the Karl G. Jansky Very Large Array using AGD. We find more components per line of sight in 21-SPONGE than in synthetic spectra, which reflects insufficient simulated gas scale heights and the limitations of local box simulations. In addition, we find a significant population of low-optical depth, broad absorption components in the synthetic data which are not seen in 21-SPONGE. This population is not obvious in integrated or per-channel diagnostics, and reflects the benefit of studying velocity-resolved components. The discrepant components correspond to the highest spin temperatures (1000<T{sub s}<4000 K), which are not seen in 21-SPONGE despite sufficient observational sensitivity. We demonstrate that our analysis method is a powerful tool for diagnosing neutral interstellar medium conditions, and future work is needed to improve observational statistics and implementation of simulated physics.

79 ASTRONOMY AND ASTROPHYSICS↗

Using Plasmon Peaks in Electron Energy-Loss Spectroscopy to Determine the Physical and Mechanical Properties of Nanoscale Materials

In this program, we developed new theoretical and experimental insights into understanding the relationships among fundamental universality and scaling phenomena, the solid-state physical and mechanical properties of materials, and the volume plasmon energy as measured by electron energy-loss spectroscopy (EELS). Particular achievements in these areas are summarized as follows: (i) Using a previously proposed physical model based on the universal binding-energy relation (UBER), we established close phenomenological connections regarding the influence of the valence electrons in materials on the longitudinal plasma oscillations (plasmons) and various solid-state properties such as the optical constants (including absorption and dispersion), elastic constants, cohesive energy, etc. (ii) We found that carbon materials, e.g., diamond, graphite, diamond-like carbons, hydrogenated and amorphous carbon films, exhibit strong correlations in density vs. E p (or maximum of the volume plasmon peak) and density vs. hardness, both from available experimental data and ab initio DFT calculations. This allowed us to derive a three-dimensional relationship between hardness and the plasmon energy, that can be used to determine experimentally both hardness and density of carbon materials based on measurements of the plasmon peak position. (iii) As major experimental accomplishments, we demonstrated the possibility of in-situ monitoring of changes in the physical properties of materials with conditions, e.g., temperature, and we also applied a new plasmon ratio-imaging technique to map multiple physical properties of materials, such as the elastic moduli, cohesive energy and bonding electron density, with a sub-nanometer lateral resolution. This presents new capability for understanding material behavior. (iv) Lastly, we demonstrated a new physical phenomenon - electron-beam trapping, or electron tweezers - of a solid metal nanoparticle inside a liquid metal. This phenomenon is analogous to that of optical trapping of solid microparticles in solution known as "optical tweezers", which is currently being used to manipulate molecules and inorganic materials in a variety of nanotechnology applications.

36 MATERIALS SCIENCE↗

Determination of local concentration of H{sub 2}O molecules and gas temperature in the process of hydrogen - oxygen gas mixture heating by means of linear and nonlinear laser spectroscopy

Employing the methods of linear absorption spectroscopy and nonlinear four-wave mixing spectroscopy using laserinduced gratings we have simultaneously measured the local concentrations of H{sub 2}O molecules and the gas temperature in the process of the H{sub 2} - O{sub 2} mixture heating. During the measurements of the deactivation rates of pulsed-laser excited singlet oxygen O{sub 2} (b {sup 1}{Sigma}{sup +}{sub g}) in collisions with H{sub 2} in the range 294 - 850 K, the joint use of the two methods made it possible to determine the degree of hydrogen oxidation at a given temperature. As the mixture is heated, H{sub 2}O molecules are formed by 'dark' reactions of H{sub 2} with O{sub 2} in the ground state. The experiments have shown that the measurements of tunable diode laser radiation absorption along an optical path through the inhomogeneously heated gas mixture in a cell allows high-accuracy determination of the local H{sub 2}O concentration in the O{sub 2} laser excitation volume, if the gas temperature in this volume is known. When studying the collisional deactivation of O{sub 2} (b {sup 1}{Sigma}{sup +}{sub g}) molecules, the necessary measurements of the local temperature can be implemented using laser-induced gratings, arising due to spatially periodic excitation of O{sub 2} (X{sup 3}{Sigma}{sup -}{sub g}) molecules to the b {sup 1}{Sigma}{sup +}{sub g} state by radiation of the pump laser of the four-wave mixing spectrometer. (laser spectroscopy)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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