Energy transfer between molecules and electronically excited atoms. II.
Relative rate constants for energy transfer from excited argon atoms to various organic molecules
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Relative rate constants for energy transfer from excited argon atoms to various organic molecules
Linear energy transfer spectra and dose equivalents of galactic radiation exposure in space
Zeaxanthin (Zea) is a key component in the energy-dependent, rapidly reversible, nonphotochemical quenching process (qE) that regulates photosynthetic light harvesting. Previous transient absorption (TA) studies suggested that Zea can participate in direct quenching via chlorophyll (Chl) to Zea energy transfer. However, the contamination of intrinsic exciton–exciton annihilation (EEA) makes the assignment of TA signal ambiguous. In this study, we present EEA-free TA data using Nicotiana benthamiana thylakoid membranes, including the wild type and three NPQ mutants (npq1, npq4, and lut2) generated by CRISPR/Cas9 mutagenesis. The results show a strong correlation between excitation energy transfer from excited Chl Q y to Zea S 1 and the xanthophyll cycle during qE activation. Notably, a Lut S 1 signal is absent in the npq1 thylakoids which lack zeaxanthin. Additionally, the fifth-order response analysis shows a reduction in the exciton diffusion length (L D ) from 62 ± 6 nm to 43 ± 3 nm under high light illumination, consistent with the reduced range of exciton motion being a key aspect of plants’ response to excess light.
A series of experiments has been conducted in order to examine the nature of the energy transfer process between the Cr(3+) and Tm(3+) ions in YAG. Data are obtained on various samples doped with Cr(3+) and/or Tm(3+). These data include absorption, luminescence, excitation spectra and time-resolved response to pulsed excitation. The measurements were carried out over a range of temperatures from 78 to 350 K. The rate of nonradiative energy transfer from Cr(3+) to Tm(3+) depends on temperature, and in the region from 200 to 350 K, this dependence is due primarily to the thermal variation in the radiative decay probability of the Cr ion.
Detailed measurements were made of energy transfer among the scales of motion in incompressible turbulent fields at low Reynolds numbers generated by direct numerical simulation. It was observed that although the transfer resulted from triad interactions that were non-local in k space, the energy always transferred locally. The results are consistent with the notion of non-uniform advection of small weak eddies by larger and stronger ones, similar to transfer processes in the far dissipation range at high Reynolds numbers.
Gas-surface energy transfer experiment on OGO-F satellite, measuring upper atmosphere kinetic energy flux to determine accommodation and drag coefficients, density, etc
The nonlinear physics of cross-beam energy transfer (CBET) for multi-speckled laser beams is examined using large-scale particle-in-cell simulations for a range of laser and plasma conditions relevant to indirect-drive inertial confinement fusion (ICF) experiments. The time-dependent growth and saturation of CBET involve complex, nonlinear ion and electron dynamics, including ion trapping-induced enhancement and detuning, ion acoustic wave (IAW) nonlinearity, oblique forward stimulated Raman scattering (FSRS), and backward stimulated Brillouin scattering (BSBS) in a CBET-amplified seed beam. Ion-trapping-induced detuning of CBET is captured in the kinetic linear response by a new δf-Gaussian-mixture algorithm, enabling an accurate characterization of trapping-induced non-Maxwellian distributions. Ion trapping induces nonlinear processes, such as changes to the IAW dispersion and nonlinearities (e.g., bowing and self-focusing), which, together with pump depletion, FSRS, and BSBS, determine the time-dependent nature and level of CBET gain as the system approaches a steady state. Using VPIC simulations at intensities at and above the onset threshold for ion trapping and the insight from the time-dependent saturation analyses, we construct a nonlinear CBET model from local laser and plasma conditions that predicts the CBET gain and the energy deposition into the plasma. This model is intended to provide a more accurate, physics-based description of CBET saturation over a wide range of conditions encountered in ICF hohlraums compared with linear CBET gain models with ad hoc saturation clamps often used in laser ray-based methods in multi-physics codes.
Ray-based cross-beam energy transfer (CBET) models have become a common feature of the radiation-hydrodynamic codes used to simulate inertial confinement fusion experiments. Here, these models are necessary for achieving better agreement with experimental measurements, but their detailed implementation can vary widely between the codes and often rely on artificial multipliers. To address this, a series of 2D and 3D test cases has been developed with validated solutions from wave-based calculations. Comparisons of various ray-based CBET models to the wave-based calculations highlight the essential physics that is required for accurate ray-based CBET modeling. Quantitative comparison metrics and/or field data from the wave-based calculations have been made available for use in the validation of other ray-based CBET codes.
Crossed-beam energy transfer (CBET) is a consequential process in inertial confinement fusion (ICF) experiments. CBET depends on the polarization state of the interacting lasers and can, in turn, alter their polarization. Here, we derive analytical expressions for two-beam CBET with linearly and circularly polarized light, and present simulations of CBET that include polarization effects for ICF conditions relevant to experiments on the National Ignition Facility. The results show that CBET mixes the polarization of the beams as they propagate through the target and leads to azimuthal power imbalances between beams within a given cone (i.e., at the same polar angle in the target chamber). These variations are shown to correlate with variations in measured backscatter between beams of a same quadruplet. Using circularly polarized, instead of linearly polarized, light produces similar overall levels of CBET within a cone of beams but tends to reduce the azimuthal variations. This is expected to slightly improve irradiation symmetry and reduce the risk of backscatter from stimulated Brillouin scattering. Circular polarization may therefore be beneficial for the next generation of laser fusion drivers.
Energy transfer and ion cost in hydrogen plasma
Radiant energy transfer in absorbing and emitting media, noting approximate equations reduced to correct optically thin and thick limits for multidimensional problems
Electronic to vibrational energy transfer in mercury vapor reaction with hydrogen fluoride, studying IR emission and scattering cross section
A systematic analysis of energy transfer processes in crystals of YAG doped with varying concentrations of Cr and Tm is described. Both spectral measurements and measurements of the temporal response to pulsed excitation are used to give independent determinations of the microscopic interaction parameter for Cr to Tm transfer. The different factors in influencing the temperature dependence of the Cr to Tm transfer are discussed. The dependence of the Tm cross-relaxation rate on Tm concentration is determined.
Integral linear energy transfer (LET) spectra of cosmic radiation (CR) particles were measured on five Cosmos series spacecraft in low Earth orbit (LEO). Particular emphasis is placed on results of the Cosmos 1887 biosatellite which carried a set of joint U.S.S.R.-U.S.A. radiation experiments involving passive detectors that included thermoluminescent detectors (TLDs), plastic nuclear track detectors (PNTDs), fission foils, nuclear photo-emulsions, etc. which were located both inside and outside the spacecraft. Measured LET spectra are compared with those theoretically calculated. Results show that there is some dependence of LET spectra on orbital parameters. The results are used to estimate the CR quality factor (QF) for the Cosmos 1887 mission.
Five bismuth(III)-organic phases that consist of supramolecular assemblies of Bi-2,6-pyridinedicarboxylate structural units and substituted 1,10-phenanthroline molecules (R-Phen; R = H, 5-methyl, 5-chloro, 2,9-dimethyl, and 2,9-dicholoro) were synthesized. All five compounds exhibited solid-state photoluminescence. Whereas the phases containing 2,9-dimethylphenanthroline (Me 2 Phen) and 2,9-dichlorophenanthroline (Cl 2 Phen) displayed solely phosphorescence, the structures built from 5-methylphenanthroline and 5-chlorophenanthroline showed exclusively fluorescence. The remaining phase, consisting of phenanthrolinium, exhibited both fluorescence and phosphoresence. It was determined that phosphorescence arises from triplet state emission (T 1 → S 0 ) of substituted R-Phen units while fluorescence originates from Bi(III) coordinated pyrdinedicarboxylate ligands. Bismuth induces spin–orbit coupling for triplet state population and additionally acts as a heavy metal attenuator for X-ray luminescence (radioluminescence). The electronic structure was mapped and excitation pathway investigated via density functional theory calculations. Computational findings indicate favorable conditions for triplet energy transfer from donor Bi(III)-organic units to acceptor R-Phen derivatives. It is proposed that for the phosphorescent compounds, strong π–π interactions promote electron transfer, whereas the compounds that exhibit purely fluorescence lack any such π–π interactions and undergo triplet energy transfer. In conclusion, these results provide a useful platform for probing structure–property relationships of luminescent bismuth-organic compounds, and specifically highlights the role of noncovalent interactions in achieving room temperature phosphorescence and radioluminescence.
Conjugated polymers offer unprecedented chemical tunability for modulating energy transfer in a multitude of infrared light applications. In this work, we use a combination of time-resolved spectroscopic experiments and nonadiabatic molecular dynamics calculations to probe the photochemistry and nonradiative transitions in a recently synthesized narrow bandgap donor–acceptor conjugated polymer based on alternating cyclopentadithiophene and electronegative benzothiadiazole heterocycles. Using large-scale semi-empirical nonadiabatic molecular dynamics, which can treat a large 260-atom hexamer, we calculate an S 5 → S 1 lifetime of 34.75 fs, which is consistent with our time-resolved spectroscopic data. Our simulations suggest that vibronic motions of the central carbons in the cyclopentadithiophene functional groups are predominantly involved in the nonradiative transitions, and the excitation becomes more localized on a monomer fragment over time. The combined use of time-resolved experiments and nonadiabatic molecular dynamics calculations in this work provides mechanistic insight into chemical functionalities that can be tuned to enhance energy transfer in other prospective low-bandgap polymer materials.
We introduce a heterodimer model in which multiple mechanisms of vibronic coupling and their impact on energy transfer can be explicitly studied. We consider vibronic coupling that arises through either Franck-Condon activity in which each site in the heterodimer has a local electron-phonon coupling or Herzberg-Teller activity in which the transition dipole moment coupling the sites has an explicit vibrational mode-dependence. We have computed two-dimensional electronic-vibrational (2DEV) spectra for this model while varying the magnitude of these two effects and find that 2DEV spectra contain static and dynamic signatures of both types of vibronic coupling. Franck-Condon activity emerges through a change in the observed excitonic structure, while Herzberg-Teller activity is evident in the appearance of significant side-band transitions that mimic the lower-energy excitonic structure. A comparison of quantum beating patterns obtained from analysis of the simulated 2DEV spectra shows that this technique can report on the mechanism of energy transfer, elucidating a means of experimentally determining the role of specific vibronic coupling mechanisms in such processes.
In this paper, we introduce a realistic modeling of laser beams smoothed by random phase plates to investigate cross-beam energy transfer (CBET). We compute the total field of the smoothed laser beams, which allows us to perform accurate simulations and to build a model accounting for the realistic structure of the speckles. This lets us confirm the results already discussed in a previous work given by Oudin et al. [Phys. Plasmas 29, 112112 (2022)]. When CBET is induced by a plasma flow, plane wave models can predict the exchange between smoothed laser beams. By contrast, when the exchange is caused by a wavelength shift between the laser fields of each beam, plane wave models overestimate the energy transfer, even for strongly Landau-damped ion acoustic waves. We also show that the laser angular spread, which results from its focusing, affects the resonance between the ponderomotive force induced by the laser fields and the ion acoustic wave. It increases the resonance width, which weakly depends on the Landau damping rate when there is a wavelength shift and no flow. In addition, the power transfer obtained with or without a phase plate is essentially the same in the perturbative regime and for small crossing angles.