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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states {sup 1}L{sub a} and {sup 1}L{sub b} and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τ{sub f}, and rotation correlation time τ{sub rot} have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that {sup 1}L{sub b}–{sup 1}L{sub a} inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the {sup 1}L{sub a} state at all excitation wavelengths but in the 287–289 nm area which contained an absorption hump of the {sup 1}L{sub b} state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τ{sub f} and the rotation correlation time τ{sub rot} showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τ{sub f} = 3.83 ± 0.14 ns and τ{sub rot} = 0.74 ± 0.06 ns.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

New Insights into the Charge-Transfer-to-Solvent Spectrum of Aqueous Iodide: Surface versus Bulk

Liquid phase charge-transfer-to-solvent (CTTS) transitions are important, as they serve as photochemical routes to solvated electrons. Here in this work, broadband deep-ultraviolet electronic sum frequency generation (DUV-ESFG) and two-photon absorption (2PA) spectroscopic techniques were used to assign and compare the nature of the aqueous iodide CTTS excitations at the air/water interface and in bulk solution. In the one-photon absorption (1PA) spectrum, excitation to the 6s Rydberg-like orbital (5p → 6s) gives rise to a pair of spin–orbit split iodine states, 2 P 3/2 and 2 P 1/2 . In the 2PA spectra, the lower-energy 2 P 3/2 peak is absent and the observed 2PA peak, which is ~0.14 eV blue-shifted relative to the upper 2 P 1/2 CTTS peak seen in 1PA, arises from 5p → 6p electronic promotion. The band observed in the ESFG spectrum is attributed to mixing of excited states involving 5p → 6p and 5p → 6s promotions caused by both vibronic coupling and the external electric field generated by asymmetric interfacial solvation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Calibration of hydrogen atoms measurement using femtosecond two-photon laser-induced fluorescence

What we believe to be a new calibration method for H-fs-TALIF is proposed, and the ratio of two-photon absorption cross-sections, σ (2) , for atomic hydrogen (H) and krypton (Kr) is determined using the broadband emission of a femtosecond laser system. The estimated ratio of the two-photon absorption cross-sections for H and Kr is σ (2) (Kr)/σ (2) (H) = 0.027 ± 20%, which is nearly twenty times lower than values previously obtained with narrowband nanosecond lasers. This discrepancy highlights the need for independent calibration of TALIF measurements for a specific laser pulsewidth range.

Starikovskiy, Andrey [Princeton Univ., NJ (United ↗
DOE OSTI2012

Characterization of Photochemical Processes for H2 Production by CdS Nanorod-[FeFe] Hydrogenase Complexes

We have developed complexes of CdS nanorods capped with 3-mercaptopropionic acid (MPA) and Clostridium acetobutylicum [FeFe]-hydrogenase I (CaI) that photocatalyze reduction of H{sup +} to H{sub 2} at a CaI turnover frequency of 380-900 s{sup -1} and photon conversion efficiencies of up to 20% under illumination at 405 nm. In this paper, we focus on the compositional and mechanistic aspects of CdS:CaI complexes that control the photochemical conversion of solar energy into H{sub 2}. Self-assembly of CdS with CaI was driven by electrostatics, demonstrated as the inhibition of ferredoxin-mediated H{sub 2} evolution by CaI. Production of H{sub 2} by CdS:CaI was observed only under illumination and only in the presence of a sacrificial donor. We explored the effects of the CdS:CaI molar ratio, sacrificial donor concentration, and light intensity on photocatalytic H{sub 2} production, which were interpreted on the basis of contributions to electron transfer, hole transfer, or rate of photon absorption, respectively. Each parameter was found to have pronounced effects on the CdS:CaI photocatalytic activity. Specifically, we found that under 405 nm light at an intensity equivalent to total AM 1.5 solar flux, H{sub 2} production was limited by the rate of photon absorption ({approx}1 ms{sup -1}) and not by the turnover of CaI. Complexes were capable of H{sub 2} production for up to 4 h with a total turnover number of 106 before photocatalytic activity was lost. This loss correlated with inactivation of CaI, resulting from the photo-oxidation of the CdS capping ligand MPA.

ABSORPTION↗
DOE OSTI2018

Nonlinear Optical Properties of CdS/ZnS Quantum Dots in a High-Molecular-Weight Polyvinylpyrrolidone Matrix

Sols containing core/shell CdS/ZnS semiconductor quantum dots are synthesized and their nonlinear properties, which are interesting for a large variety of applications in nanophotonics, are studied. The quantum dots produced are smaller in dimensions than the exciton Bohr radius and, therefore, exhibit a well-pronounced quantum-confinement effect. The nonlinear optical properties of low-concentration sols are studied upon exposure to laser pulses with an emission wavelength of 532 nm and a duration of 5 ns by the z-scan technique. The dependences of nonlinear optical coefficients on the concentration of CdS/ZnS quantum dots are obtained. The intensity dependence of two-photon absorption coefficients is presented. The dependence determines the boundary of the influence of high-order nonlinearities on the nonlinear transmittance of the samples. The mechanisms of optical limitation exhibited by sols, specifically, two-photon absorption, nonlinear refraction, and nonlinear scattering are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Simulating dust grain-radiation coupling on a moving mesh

ABSTRACT We present a model for the interaction between dust and radiation fields in the radiation hydrodynamic code arepo-rt, which solves the moment-based radiative transfer equations on an unstructured moving mesh. Dust is directly treated using live simulation particles, each of which represent a population of grains that are coupled to hydrodynamic motion through a drag force. We introduce methods to calculate radiation pressure on and photon absorption by dust grains. By including a direct treatment of dust, we are able to calculate dust opacities and update radiation fields self-consistently based on the local dust distribution. This hybrid scheme coupling dust particles to an unstructured mesh for radiation is validated using several test problems with known analytic solutions, including dust driven via spherically symmetric flux from a constant luminosity source and photon absorption from radiation incident on a thin layer of dust. Our methods are compatible with the multifrequency scheme in arepo-rt, which treats UV, optical photons as single scattered and IR photons as multi scattered. At IR wavelengths, we model heating of and thermal emission from dust. Dust and gas are not assumed to be in local thermodynamic equilibrium but transfer energy through collisional exchange. We estimate dust temperatures by balancing these dust-radiation and dust-gas energy exchange rates. This framework for coupling dust and radiation can be applied in future radiation hydrodynamic simulations of galaxy formation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Enhanced photocurrent density in graphene/Si based solar cell (GSSC) by optimizing active layer thickness

Thickness dependent photocurrent density in active layer of graphene/Si based solar cell has been investigated via analytical – simulation study. This report is a preliminary comparison of experimental and analytical investigation of graphene/Si based solar cell. Graphene sheet was interfaced with Si thin film forming heterojunction solar cell that was treated as a device model for photocurrent generator. Such current can be enhanced by optimizing active layer thickness and involving metal oxide as supporting layer to shift photons absorption. In this case there are two type of devices model with and without TiO{sub 2} in which the silicon thickness varied at 20 – 100 nm. All of them have examined and also compared with each other to obtain an optimum value. From this calculation it found that generated currents almost linear with thickness but there are saturated conditions that no more enhancements will be achieved. Furthermore TiO{sub 2} layer is effectively increases photon absorption but reducing device stability, maximum current is fluctuates enough. This may caused by the disturbance of excitons diffusion and resistivity inside each layer. Finally by controlling active layer thickness, it is quite useful to estimate optimization in order to develop the next solar cell devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Development of III-Sb Quantum Dot Systems for High Efficiency Intermediate Band Solar Cells

This project aimed to develop solar cells that can help reduce cost per watt. This work focused on developing solar cells that utilize quantum dot (QD) nanomaterials to provide multijunction solar cell efficiency at the cost of single junction solar cell. We focused on a novel concept known as intermediate band solar cells (IBSC) where an additional energy band is inserted in a single solar cell to accommodate sub-bandgap photons absorption which otherwise are lost through transmission. The additional energy band can be achieved by growing QDs within a solar cell p-n junction. Though numerous studies have been conducted to develop such QD systems, very small improvements in solar energy conversion efficiency have been reported. This is mainly due to non-optimal material parameters such as band gap, band offset etc. In this work, we identified and developed a novel QD material system that meets the requirements of IBSC more closely than the current state-of-the-art technology. To achieve these goals, we focused on three important areas of solar cell design: band structure calculations of new materials, efficient device design for high efficiency, and development of new semiconductor materials. In this project, we focused on III-Sb materials as they possess a wide range of energy bandgaps from 0.2 eV to 2eV. Despite the difficulty involved in realizing these materials, we were successfully developed these materials through a systematic approach. Materials studied in this work are AlAsSb (Aluminum Arsenide Antimonide), InAlAs (Indium Aluminum Arsenide) and InAs (Indium Arsenide). InAs was used to develop QD layers within AlAsSb and InAlAs p-n junctions. As the QDs have very small volume, up to 30 QD layers been inserted into the p-n junction to enhance light absorption. These QD multi-stack devices helped in understanding the challenges associated with the development of quantum dot solar cells. The results from this work show that the quantum dot solar cells indeed improve the efficiency via sub-bandgap photon absorption but much lower than the expected theoretical efficiencies. Yet, these devices serve as a proof of concept and the results provide vital information for future IBSC work. With further understanding of the operation of intermediate band solar cells and the identification of less expensive materials can substantially improve the solar cell efficiency and drastically cut the cell cost thereby reducing the dollar/watt cost.

14 SOLAR ENERGY↗
NASA NTRS1981

Two-photon excitation of nitric oxide fluorescence as a temperature indicator in unsteady gasdynamic processes

A laser-induced fluorescence technique based on the pulsed two-photon excitation of NO is presented which is especially suited for the measurement of fluctuating temperatures in cold turbulent flows. The technique uses the fluorescence from the UV gamma bands of NO produced by two-photon excitation of NO (A 2 Sigma +, nu-prime = 0 - X 2 Pi, nu-double prime = 0) to obtain a rotational temperature. An analysis is presented of relevant aspects of the two-photon absorption process including microphysical processes, spectral intensities as a function of transition and laser spectral widths, line-shape integrals, the nonequilibrium response of the medium to a laser pulse, fluorescence energies, signal to noise ratio, and focusing effects. An analysis of absolute two-photon absorptivity measured in a nonflowing cell is then presented and used to predict signal to noise ratios greater than 50 for supersonic flows at temperatures below 300 K.

Mckenzie, R. L.↗
NASA NTRS1980

Two-photon excitation cross section in light and intermediate atoms in frozen-core LS-coupling approximation

Using the method of explicit summation over the intermediate states two-photon absorption cross sections in light and intermediate atoms based on the simplistic frozen-core approximation and LS coupling have been formulated. Formulas for the cross section in terms of integrals over radial wave functions are given. Two selection rules, one exact and one approximate, valid within the stated approximations are derived. The formulas are applied to two-photon absorptions in nitrogen, oxygen, and chlorine. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum-defect method have been used. A relationship between the cross section and the oscillator strengths is derived.

Omidvar, K.↗
DOE OSTI2016

Pinning down high-performance Cu-chalcogenides as thin-film solar cell absorbers: A successive screening approach

Photovoltaic performances of Cu-chalcogenides solar cells are strongly correlated with the absorber fundamental properties such as optimal bandgap, desired band alignment with window material, and high photon absorption ability. According to these criteria, we carry out a successive screening for 90 Cu-chalcogenides using efficient theoretical approaches. Besides the well-recognized CuInSe{sub 2} and Cu{sub 2}ZnSnSe{sub 4} materials, several novel candidates are identified to have optimal bandgaps of around 1.0–1.5 eV, spike-like band alignments with CdS window layer, sharp photon absorption edges, and high absorption coefficients. These new systems have great potential to be superior absorbers for photovolatic applications if their carrrier transport and defect properties are properly optimized.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on the properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Effect of Proximity of Features on the Damage Threshold During Submicron Additive Manufacturing Via Two-Photon Polymerization

Two-photon polymerization (TPP) is a laser writing process that enables fabrication of millimeter scale three-dimensional (3D) structures with submicron features. In TPP, writing is achieved via nonlinear two-photon absorption that occurs at high laser intensities. Thus, it is essential to carefully select the incident power to prevent laser damage during polymerization. Currently, the feasible range of laser power is identified by writing small test patterns at varying power levels. Here in this paper, we demonstrate that the results of these tests cannot be generalized, because the damage threshold power depends on the proximity of features and reduces by as much as 47% for overlapping features. We have identified that this reduction occurs primarily due to an increase in the single-photon absorptivity of the resin after curing. We have captured the damage from proximity effects via X-ray 3D computed tomography (CT) images of a non-homogenous part that has varying feature density. Part damage manifests as internal spherical voids that arise due to boiling of the resist. We have empirically quantified this proximity effect by identifying the damage threshold power at different writing speeds and feature overlap spacings. In addition, we present a first-order analytical model that captures the scaling of this proximity effect. Based on this model and the experiments, we have identified that the proximity effect is more significant at high writing speeds; therefore, it adversely affects the scalability of manufacturing. The scaling laws and the empirical data generated here can be used to select the appropriate TPP writing parameters.

36 MATERIALS SCIENCE↗
NASA NTRS1980

Two-photon excitation cross-section in light and intermediate atoms

The method of explicit summation over the intermediate states is used along with LS coupling to derive an expression for two-photon absorption cross section in light and intermediate atoms in terms of integrals over radial wave functions. Two selection rules, one exact and one approximate, are also derived. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum defect method are used. A relationship between the cross section and the oscillator strengths is derived. Cross sections due to selected transitions in nitrogen, oxygen, and chlorine are given. The expression for the cross section is useful in calculating the two-photon absorption in light and intermediate atoms.

Omidvar, K.↗
DOE OSTI2012

Investigations on the electrical, thermal and optical properties of the nonlinear optical allylthiourea mercury chloride single crystals

Graphical abstract: Display Omitted Highlights: ► The single crystals of dimension 10 × 5 × 5 mm{sup 3} of allylthiourea mercury chloride are synthesized using slow evaporation technique. ► The bandgap of allylthiourea mercury chloride crystal is found to be about 3.18 eV. ► The optical nonlinearity of the crystal sample are studied using the open aperture Z-scan technique employing a nanosecond laser at 532 nm, and three photon absorption effect has been found. ► An improved photo pyroelectric is used to find the thermal parameters of the crystal. ► The piezoelectric charge coefficient is determined. -- Abstract: Single crystals of dimension 10 × 5 × 5 mm{sup 3} of allylthiourea mercury chloride were synthesized from aqueous solution using slow evaporation technique at ambient temperature. The grown crystals are confirmed by elemental analysis. The band gap of Allylthiourea mercury chloride crystal was found to be about 3.18 eV. The optical nonlinearity of the crystal sample was studied using the open aperture Z-scan technique employing a nanosecond laser at 532 nm, and a three-photon absorption effect has been found. The electrical properties such as dielectric constant, dielectric loss and ac conductivity of the sample were carried out by Agillent E 4980 A LCR meter at different temperatures. An improved photopyroelectric technique was used to find the thermal parameters of the crystal. The piezo electric charge coefficient is also determined.

36 MATERIALS SCIENCE↗
NASA NTRS2011

Hypersonic Wake Diagnostics Using Laser Induced Fluorescence Techniques

A review of recent research performed in iodine that involves a two photon absorption of light at 193 nm will be discussed, and it's potential application to velocimetry measurements in a hypersonic flow field will be described. An alternative seed atom, Krypton, will be presented as a good candidate for performing nonintrusive hypersonic flow diagnostics. Krypton has a metastable state with a lifetime of approximately 43 s which would prove useful for time of flight measurement (TOF) and a sensitivity to collisions that can be utilized for density measurements. Calculations using modest laser energies and experimental values show an efficiency of excited state production to be on the order of 10(exp -6) for a two photon absorption at 193 nm.

Mills, Jack L.↗
DOE OSTI2023

Realization of a wide steering end-fire facet optical phased array using silicon rich silicon nitride

The design, fabrication, and characterization of a 16-element optical phased array (OPA) using a high index (n = 3.1) silicon-rich silicon nitride (SRN) is demonstrated. Here, we present one-dimensional beam steering with end-fire facet antennas over a wide steering range of >115° at a fixed wavelength of 1525 nm. A beam width of 6.3° has been measured at boresight, consistent with theory. We demonstrate SRN as a viable material choice for chip-scale OPA applications due to its high thermo-optic coefficient, high optical power handling capacity [negligible two-photon absorption (TPA)], wide transparency window, and CMOS compatibility.

Nejadriahi, Hani↗