Monitoring Wavepacket Dynamics at Conical Intersections by Entangled Two-Photon Absorption
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Materials Science↗
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Results for “Photon absorption”
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Nondegenerate two-photon absorption in GaAs/AlGaAs multiple quantum well waveguides
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Cox, Nicholas (ORCID:0000000328523092)↗
Terahertz Photoconductive Metasurface Detector with enhanced Two-Step Photon Absorption at 1550 nm
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Jung, Hyunseung↗
Multi-photon Absorption Based Method to Detect and Quantify Electric Fields.
Abstract not provided.
Barnat, Edward↗
Streaming in a Nuclear Grade Sandwich Composite for Microreactor Shielding
The NGSC is a new approach to develop a shield structure for microreactors which combines the biological shielding with the reactor pressure vessel. Six layers of SS316 skins and core materials are present in the NGSC, where the core materials are reduce the neutron and gamma dose. Previous work has examined how a simplified NGSC can be optimized for cost, dose, and weight. This work explored the inclusion of SS36 ribs, which helps maintain the structural integrity of the NGSC, affects the transportation of radiation through the NGSC. For B$_4$C layers, the addition of ribs reduces neutron absorption but increase photon absorption. For WB$_4$-cermet layers, the addition of ribs reduces neutron absorption and reduces photon absorption.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Decay of a laser beam under stimulated temperature scattering in toluene as a result of two-photon pump absorption and nonsteady-state laser pulse interaction with matter
The decay of the pump-beam spatial structure under conditions of stimulated temperature scattering of a pulsed laser beam in toluene as a result of two-photon absorption of pump radiation and time-dependent interaction of a laser pulse with a medium is considered. (paper)
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Role of Metal Cocatalysts in the Photocatalytic Production of Hydrogen from Water Revisited
The use of photocatalysts to promote the production of molecular hydrogen from water, following the so-called water splitting reaction, continues to be a promising route for the green production of fuels. The molecular basis of this photocatalysis is the photoexcitation of electrons from the valence band of semiconductors to their conduction band, from which they can be transferred to chemical reactants, protons in the case of water, to promote a reduction reaction. The mechanism by which such a process takes place has been studied extensively using titanium oxide, a simple material that fulfills most requirements for water splitting. However, photocatalysis with TiO 2 tends to be highly inefficient; a cocatalyst, commonly a late transition metal (Au, Pt) in nanoparticle form, needs to be added to facilitate the production of H 2 . The metal is widely believed to help with the scavenging of the excited electrons from the conduction band of the semiconductor in order to prevent their recombination with the accompanying hole formed in the valence band, a step that cancels the initial photon absorption and competes with the photolytic chemical reduction. Here we review and analyze the molecular basis for that mechanism and argue for an alternative explanation, that the role of the metal is to help with the recombination of the atomic hydrogen atoms produced by proton reduction on the semiconductor surface instead. First, we summarize what is known about the electronic structure of these photocatalysts and how the electronic levels need to line up for the reduction of protons in water to be feasible. Next, we review the current understanding of the dynamics of the steps associated with the absorption of photons, the de-excitation via electron–hole pair recombination and fluorescence decay, and the electronic transitions that lead to proton reduction, and contrast those with the rates of the chemical steps required to produce molecular hydrogen. The following section addresses the changes introduced by the addition of the metal cocatalyst, comparatively evaluating its role as either an electron scavenger or a promoter of the recombination of hydrogen atoms. A discussion of the viable chemical mechanisms for the latter pathway is included. Finally, we briefly mention other associated aspects of this photocatalysis, including the possible promotion of H 2 production with visible light via resonant excitation of the surface plasmon of Au nanoparticles, the use of single-metal (Au, Pt) atom catalysts and of yolk–shell nanostructures, and the reduction of organic molecules. We end with a brief personal perspective on the possible generality of the concepts introduced in this Critical Review.
08 HYDROGEN↗
Entangled light–matter interactions and spectroscopy
Entangled photons exhibit non-classical light–matter interactions that create new opportunities in materials and molecular science. Notably, in entangled two-photon absorption, the intensity-dependence scales linearly as if only one photon was present. The entangled two-photon absorption cross section approaches but does not match the one-photon absorption cross section. The entangled two-photon cross section also does not follow classical two-photon molecular design motifs. Questions such as these seed the rich but nascent field of entangled light–matter interactions. In this work, we use the experimental developments in entangled photon spectroscopy to outline the current status of the field. Now that the fundamental tools are outlined, it is time to start the exploration of how materials, molecules, and devices can control or utilize interactions with entangled photons.
36 MATERIALS SCIENCE↗
Role of water vapour in the absorption of nanosecond 266-nm laser pulses by atmospheric air
The absorption of the Nd : YAG fourth harmonic in air and binary mixtures of water vapour with nitrogen and oxygen at atmospheric pressure has been measured as a function of pulse energy (peak intensity). The mixtures obtained by adding equal amounts of water vapour to dry nitrogen and oxygen have been found to differ significantly in absorption. Preliminary quantitative data have been obtained for two- and three-photon absorption cross sections of water and oxygen molecules: σ{sup (2)}(H{sub 2}O) = (4 ± 1) ± 10{sup –49} cm{sup 4} s and σ{sup (3)}(O{sub 2}) = (5.6 ± 1.4) ± 10{sup –78} cm{sup 6} s{sup 2}. The absorption of 266-nm pulses with peak intensities from 0.05 to 2 GW cm{sup –2} in the near-surface atmosphere has been shown to be determined by two-photon absorption in water vapour and three-photon absorption in oxygen. In moist air containing 1 % water vapour, the absorption coefficient for 266-nm laser pulses exceeds that in dry air by four to five times. There is no absorption in nitrogen. We have developed a technique for photoacoustic measurements of multiphoton absorption cross sections in single-component gases and gas mixtures. (paper)
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Two-photon excited deep-red and near-infrared emissive organic co-crystals
Abstract Two-photon excited near-infrared fluorescence materials have garnered considerable attention because of their superior optical penetration, higher spatial resolution, and lower optical scattering compared with other optical materials. Herein, a convenient and efficient supramolecular approach is used to synthesize a two-photon excited near-infrared emissive co-crystalline material. A naphthalenediimide-based triangular macrocycle and coronene form selectively two co-crystals. The triangle-shaped co-crystal emits deep-red fluorescence, while the quadrangle-shaped co-crystal displays deep-red and near-infrared emission centered on 668 nm, which represents a 162 nm red-shift compared with its precursors. Benefiting from intermolecular charge transfer interactions, the two co-crystals possess higher calculated two-photon absorption cross-sections than those of their individual constituents. Their two-photon absorption bands reach into the NIR-II region of the electromagnetic spectrum. The quadrangle-shaped co-crystal constitutes a unique material that exhibits two-photon absorption and near-infrared emission simultaneously. This co-crystallization strategy holds considerable promise for the future design and synthesis of more advanced optical materials.
36 MATERIALS SCIENCE↗
Avalanche photodiode and an optical receiver having the same
Examples described herein relate to an avalanche photodiode (APD) and an optical receiver including the APD. The APD may include a substrate and a photon absorption region disposed on the substrate. The substrate may include a charge carrier acceleration region under the photon absorption region; a charge region adjacent to the charge carrier acceleration region; and a charge carrier multiplication region adjacent to the charge region. The charge carrier acceleration region, the charge region, and the charge carrier multiplication region are laterally formed in the substrate. When a biasing voltage is applied to the optoelectronic device, photon-generated free charge carriers may be generated in the photon absorption region and are diffused into the charge carrier acceleration region. The charge carrier acceleration region is configured to accelerate the photon-generated free charge carriers prior to the photon-generated free charge carriers entering into the charge region and undergoing impact ionization in the charge carrier multiplication region.
Yuan, Yuan↗
Longitudinal position dependence of dark line defect growth rate in high-power diode lasers at 790 nm
Using a nondestructive, in situ near-infrared defect imaging technique, we obtained time-resolved images of dark line defect (DLD) growth in the cavities of several high-power 790-nm diode lasers and calculated individual DLD growth rates. A clear longitudinal spatial dependence in the DLD growth rate was observed, in which the DLD growth rate was faster near the anti-reflective (AR) facet. Longitudinal spatial hole burning simulation results indicate that the total photon density increases toward the AR facet, while the carrier density decreases toward the AR facet. Here, these results suggest that photon absorption plays a key role in enhancing DLD growth beyond the contribution of the traditional carrier capture mechanism. Asymmetric DLD growth that was preferentially directed toward the high-reflectivity facet was also observed, providing further support for the role of photon absorption in the growth process. To account for these findings, we propose a photon-accelerated mechanism for the enhancement of DLD growth in which the slower carrier capture process in the traditional recombination-enhanced dislocation glide mechanism is replaced by a faster photon absorption process.
Engineering - Electronic and electrical engineerin↗
Mechanism and dynamics of fatty acid photodecarboxylase
Photoenzymes are rare biocatalysts driven by absorption of a photon at each catalytic cycle; they inspire development of artificial photoenzymes with valuable activities. Fatty acid photodecarboxylase (FAP) is a natural photoenzyme that has potential applications in the bio-based production of hydrocarbons, yet its mechanism is far from fully understood. RATIONALE To elucidate the mechanism of FAP, we studied the wild-type (WT) enzyme from Chlorella variabilis (CvFAP) and variants with altered active-site residues using a wealth of techniques, including static and time-resolved crystallography and spectroscopy, as well as biochemical and computational approaches. RESULTS A 1.8-Å-resolution CvFAP x-ray crystal structure revealed a dense hydrogen-bonding network positioning the fatty acid carboxyl group in the vicinity of the flavin adenine dinucleotide (FAD) cofactor. Structures solved from free electron laser and low-dose synchrotron x-ray crystal data further highlighted an unusual bent shape of the oxidized flavin chromophore, and showed that the bending angle (14°) did not change upon photon absorption (step 1) or throughout the photocycle. Calculations showed that bending substantially affected the energy levels of the flavin. Structural and spectroscopic analysis of WT and mutant proteins targeting two conserved active-site residues, R451 and C432, demonstrated that both residues were crucial for proper positioning of the substrate and water molecules and for oxidation of the fatty acid carboxylate by 1 FAD* (~300 ps in WT FAP) to form FAD ∙– (step 2). Time-resolved infrared spectroscopy demonstrated that decarboxylation occured quasi-instantaneously upon this forward electron transfer, consistent with barrierless bond cleavage predicted by quantum chemistry calculations and with snapshots obtained by time-resolved crystallography. Transient absorption spectroscopy in H 2 O and D 2 O buffers indicated that back electron transfer from FAD ∙– was coupled to and limited by transfer of an exchangeable proton or hydrogen atom (step 3). Unexpectedly, concomitant with FAD ∙– reoxidation (to a red-shifted form FAD RS ) in 100 ns, most of the CO 2 product was converted, most likely into bicarbonate (as inferred from FTIR spectra of the cryotrapped FAD RS intermediate). Calculations indicated that this catalytic transformation involved an active-site water molecule. Cryo-Fourier transform infrared spectroscopy studies suggested that bicarbonate formation (step 4) was preceded by deprotonation of an arginine residue (step 3). At room temperature, the remaining CO 2 left the protein in 1.5 μs (step 4'). The observation of residual electron density close to C432 in electron density maps derived from time-resolved and cryocrystallography data suggests that this residue may play a role in stabilizing CO 2 and/or bicarbonate. Three routes for alkane formation were identified by quantum chemistry calculations; the one shown in the figure is favored by the ensemble of experimental data. CONCLUSION Finally, we provide a detailed and comprehensive characterization of light-driven hydrocarbon formation by FAP, which uses a remarkably complex mechanism including unique catalytic steps. We anticipate that our results will help to expand the green chemistry toolkit.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Measurements of atoms and metastable species in N 2 and H 2 –N 2 nanosecond pulse plasmas
We report time-resolved, absolute number densities of metastable N 2 (A 3 Σ u + , v = 0, 1) molecules, ground state N 2 and H atoms, and rotational–translational temperature have been measured by tunable diode laser absorption spectroscopy and two-photon absorption laser-induced fluorescence in diffuse N 2 and N 2 –H 2 plasmas during and after a nanosecond pulse discharge burst. Comparison of the measurement results with the kinetic modeling predictions, specifically the significant reduction of the N 2 (A 3 Σ u + ) populations and the rate of N atom generation during the burst, suggests that these two trends are related. The slow N atom decay in the afterglow, on a time scale longer than the discharge burst, demonstrates that the latter trend is not affected by N atom recombination, diffusion to the walls, or convection with the flow. This leads to the conclusion that the energy pooling in collisions of N 2 (A 3 Σ u + ) molecules is a major channel of N 2 dissociation in electric discharges where a significant fraction of the input energy goes to electronic excitation of N 2 . Additional measurements in a 1% H 2 –N 2 mixture demonstrate a further significant reduction of N 2 (A 3 Σ u + , v = 0, 1) populations, due to the rapid quenching by H atoms accumulating in the plasma. Comparison with the modeling predictions suggests that the N 2 (A 3 Σ u + ) molecules may be initially formed in the highly vibrationally excited states. The reduction of the N 2 (A 3 Σ u + ) number density also diminishes the contribution of the energy pooling process into N2 dissociation, thus reducing the N atom number density. The rate of N atom generation during the burst also decreases, due to its strong coupling to N 2 (A 3 Σ u + , v) populations. On the other hand, the rate of H atom generation, produced predominantly by the dissociative quenching of the excited electronic states of N 2 by H 2 , remains about the same during the burst, resulting in a nearly linear rise in the H atom number density. Comparison of the kinetic model predictions with the experimental results suggests that the yield of H atoms during the quenching of the excited electronic state of N 2 by molecular H 2 is significantly less than 100%. The present results quantify the yield of N and H atoms in high-pressure H 2 –N 2 plasmas, which have significant potential for ammonia generation using plasma-assisted catalysis
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
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↗
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 ↗
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↗