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At least 109 records · Page 6

Ion momentum and energy transfer rates for charge exchange collisions

The rates of momentum and energy transfer have been obtained for charge exchange collisions between ion and neutral gases having arbitrary Maxwellian temperatures and bulk transport velocities. The results are directly applicable to the F-region of the ionosphere where 0+ - 0 charge is the dominant mechanism affecting ion momentum and energy transfer.

Horwitz, J.↗

Energy Transfer in Rotating Turbulence

The influence or rotation on the spectral energy transfer of homogeneous turbulence is investigated in this paper. Given the fact that linear dynamics, e.g. the inertial waves regime tackled in an RDT (Rapid Distortion Theory) fashion, cannot Affect st homogeneous isotropic turbulent flow, the study of nonlinear dynamics is of prime importance in the case of rotating flows. Previous theoretical (including both weakly nonlinear and EDQNM theories), experimental and DNS (Direct Numerical Simulation) results are gathered here and compared in order to give a self-consistent picture of the nonlinear effects of rotation on tile turbulence. The inhibition of the energy cascade, which is linked to a reduction of the dissipation rate, is shown to be related to a damping due to rotation of the energy transfer. A model for this effect is quantified by a model equation for the derivative-skewness factor, which only involves a micro-Rossby number Ro(sup omega) = omega'/(2(OMEGA))-ratio of rms vorticity and background vorticity as the relevant rotation parameter, in accordance with DNS and EDQNM results fit addition, anisotropy is shown also to develop through nonlinear interactions modified by rotation, in an intermediate range of Rossby numbers (Ro(omega) = (omega)' and Ro(omega)w greater than 1), which is characterized by a marco-Rossby number Ro(sup L) less than 1 and Ro(omega) greater than 1 which is characterized by a macro-Rossby number based on an integral lengthscale L and the micro-Rossby number previously defined. This anisotropy is mainly an angular drain of spectral energy which tends to concentrate energy in tile wave-plane normal to the rotation axis, which is exactly both the slow and the two-dimensional manifold. In Addition, a polarization of the energy distribution in this slow 2D manifold enhances horizontal (normal to the rotation axis) velocity components, and underlies the anisotropic structure of the integral lengthscales. Finally is demonstrated the ability of a generalized EDQNM (Eddy Damped Quasi-Normal Markovian) model to predict the underlying spectral transfer structure and all the subsequent developments of classic anisotropy indicators in physical space, when compared to recent LES results. Even if the applications mainly concern developed strong turbulence, a particular emphasis is given to the strong formal analogy of this EDQNM2 model with recent weakly nonlinear approaches to wave-turbulence.

Cambon, Claude↗

Excitation energy transfer in proteoliposomes reconstituted with LH2 and RC-LH1 complexes from Rhodobacter sphaeroides

Abstract Light-harvesting 2 (LH2) and reaction-centre light-harvesting 1 (RC-LH1) complexes purified from the photosynthetic bacterium Rhodobacter (Rba.) sphaeroides were reconstituted into proteoliposomes either separately, or together at three different LH2:RC-LH1 ratios, for excitation energy transfer studies. Atomic force microscopy (AFM) was used to investigate the distribution and association of the complexes within the proteoliposome membranes. Absorption and fluorescence emission spectra were similar for LH2 complexes in detergent and liposomes, indicating that reconstitution retains the structural and optical properties of the LH2 complexes. Analysis of fluorescence emission shows that when LH2 forms an extensive series of contacts with other such complexes, fluorescence is quenched by 52.6 ± 1.4%. In mixed proteoliposomes, specific excitation of carotenoids in LH2 donor complexes resulted in emission of fluorescence from acceptor RC-LH1 complexes engineered to assemble with no carotenoids. Extents of energy transfer were measured by fluorescence lifetime microscopy; the 0.72 ± 0.08 ns lifetime in LH2-only membranes decreases to 0.43 ± 0.04 ns with a ratio of 2:1 LH2 to RC-LH1, and to 0.35 ± 0.05 ns for a 1:1 ratio, corresponding to energy transfer efficiencies of 40 ± 14% and 51 ± 18%, respectively. No further improvement is seen with a 0.5:1 LH2 to RC-LH1 ratio. Thus, LH2 and RC-LH1 complexes perform their light harvesting and energy transfer roles when reconstituted into proteoliposomes, providing a way to integrate native, non-native, engineered and de novo designed light-harvesting complexes into functional photosynthetic systems.

59 BASIC BIOLOGICAL SCIENCES↗

The influence of molecular rotation on vibration-translation energy transfer

A three-dimensional vibration-rotation collision model is formulated within a semiclassical framework to study the effect of coupled rotational motion on the rate of vibrational energy transfer for collisions between anharmonic diatomic molecules and structureless atoms. Emphasis is on the net rates of vibrational energy transfer summed over all final rotational states rather than those for individual vibration-rotation transitions. The corresponding three-dimensional rate parameters are cast into forms that may be identified with equivalent parameters associated with the collinear approximation. Their comparisons allow the validity of a collinear model to be evaluated and some constraints on its application to be implied. The mechanisms of vibrational energy transfer including rotational transitions are shown to be separable into three classes which are identified and discussed

Mckenzie, R. L.↗

Response of silicon-Based Linear Energy Transfer Spectrometers

Silicon-based linear energy transfer (LET) telescope,(e. g., DOSTEL and RRMD) have recently been flown in space. LET spectra measured using tissue equivalent proportional counters show differences that need to be fully understood. A Monte Carlo technique based on: 1. radiation transport cluster intra-cascade model. 2. Landau-Vavilov distribution, 3. telescope geometry and detector coincidence & discriminator settings, 4. spacecraft shielding geometry, and 5. the external free space radiation environment, including recent albedo measurements, was developed.

Aman, A.↗

The role of energy transfer and competing bimolecular reactions in characterizing the unimolecular dissociations of allylic radicals

Resonantly stabilized radicals (RSR's) such as allylic radicals typically have bond energies exceeding 45 kcal/mol and are therefore reasonably long-lived up to quite high temperatures. Consequently, kinetics of the unimolecular dissociations and bimolecular reactions of these long-lived RSR's assume significance in high temperature chemically reacting systems such as in flames. Our recent analyses (J. Cho et al., Proc. Comb. Inst., 2022) of the uncertainty propagated by the energy transfer parameters for 1-methylallyl (1MA) dissociation to the laminar flame speed, indicates an intricate coupling between the kinetics of 1MA dissociation (chain propagation) and its reaction with H-atoms (chain-termination). Here, this work extends such analyses to other C 3 – C 5 allylic radicals: allyl, 2-methylallyl, 1,1-dimethylallyl, 1,2-dimethylallyl, and 1,3-dimethylallyl. Theoretical kinetics for the C 3 – C 4 allylic radicals were taken from prior literature studies (J.A. Miller et al., J. Phys. Chem., 2008; J. Cho et al., Proc. Comb. Inst., 2022; R.S. Tranter et al., Proc. Comb. Inst., 2017). Potential energy surfaces were newly computed for the dissociations of the larger C5 allylic radicals and the reactions of these radicals with H-atoms. These PES's were then used to calculate rate constants for the relevant unimolecular and bimolecular reactions. Energy transfer has a crucial role to play in these pressure-dependent reactions and therefore the present kinetics calculations relied on a-priori predictions of collisional energy transfer parameters to best characterize the branching between chain propagating unimolecular dissociations of these allylic radicals and chain terminating bimolecular reactions of these RSR's with H-atoms. Prompt dissociations are now established to be a universal feature of free radical dissociations. Here we have also characterized the propensity for prompt dissociations in these more-stable allylic RSR's and their role in combustion simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pump with Broadband Probe Experiments for Single-Shot Measurements of Plasma Conditions and Crossed-Beam Energy Transfer

Here, a novel technique for measuring plasma conditions using monochromatic pump-broadband-probe laser interactions has been experimentally demonstrated. Originally proposed in Ludwig et al. [Phys. Plasmas 26, 113108 (2019)], this method utilizes crossed-beam energy transfer between the broadband probe and the pump, mediated by plasma ion acoustic waves. The complete energy transfer spectrum can be captured in a single shot, enabling the inference of plasma parameters such as density, electron and ion temperatures, and flow velocity. Compared to Thomson scattering, this technique offers signal enhancements typically larger than 9 orders of magnitude, significantly reducing the required probe laser intensity and facilitating interactions that are linear and measurements that are nonperturbative of the plasma. Furthermore, it provides a powerful tool for advancing studies of crossed-beam energy transfer under conditions relevant to inertial confinement fusion experiments.

Physics - Plasma physics↗

Dynamic control of the spatial frequency content of an intense laser via intra-beam energy transfer

We present theory and simulations demonstrating that bandwidth-inducing optical smoothing techniques such as smoothing by spectral dispersion (SSD) can initiate intra-beam energy transfer (IBET) within a single beam. IBET consists of energy transfer between the different frequency components of the beam and results in a simultaneous and correlated redistribution of the temporal and spatial frequencies of the laser's electric field. We identify a threshold in bandwidth for IBET to occur and validate the theory with simulations. The bandwidth and the color cycling of SSD can result in IBET in conditions relevant for high-energy density experiments at the National Ignition Facility and Omega Laser. We show that IBET could be used to manipulate a laser's spatial frequency content within a plasma. In particular, this technique could be used to increase a laser's effective f-number, with potential applications for self-guiding in plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Experimental and theoretical study of energy transfer in a chromophore triad: What makes modeling dynamics successful?

Simulation of electronic dynamics in realistically large molecular systems is a demanding task that has not yet achieved the same level of quantitative prediction already realized for its static counterpart. This is particularly true for processes occurring beyond the Born–Oppenheimer regime. Non-adiabatic molecular dynamics (NAMD) simulations suffer from two convoluted sources of error: numerical algorithms for dynamics and electronic structure calculations. While the former has gained increasing attention, particularly addressing the validity of ad hoc methodologies, the effect of the latter remains relatively unexplored. Indeed, the required accuracy for electronic structure calculations to reach quantitative agreement with experiment in dynamics may be even more strict than that required for static simulations. In this study, we address this issue by modeling the electronic energy transfer in a donor–acceptor–donor (D–A–D) molecular light harvesting system using fewest switches surface hopping NAMD simulations. In the studied system, time-resolved experimental measurements deliver complete information on spectra and energy transfer rates. Subsequent modeling shows that the calculated electronic transition energies are “sufficiently good” to reproduce experimental spectra but produce over an order of magnitude error in simulated dynamical rates. We further perform simulations using artificially shifted energy gaps to investigate the complex relationship between transition energies and modeled dynamics to understand factors affecting non-radiative relaxation and energy transfer rates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Energy Transfer in Aqueous Light Harvesting Antennae Based on Brush-like Inter-Conjugated Polyelectrolyte Complexes

Conjugated polyelectrolytes (CPEs) have the potential to serve as building blocks of artificial light-harvesting systems. This is primarily due to their delocalized electronic states and potential for hierarchical self-assembly. We showed previously that inter-CPE complexes composed of oppositely charged exciton-donor and exciton-acceptor CPEs displayed efficient electronic energy transfer. However, near ionic charge equivalence, complexed CPE chains become net-neutral and thus experience a precipitous drop in aqueous solubility. To increase the stability and to rationally manipulate the phase behavior of inter-CPE complexes, we synthesized a series of highly water-soluble exciton-donor CPEs composed of alternating ionic and polar nonionic fluorene monomers. The nonionic monomer contained oligo(ethyleneglycol) sidechains of variable length. We then formed exciton donor-acceptor complexes and investigated their relative energy transfer efficiencies in the presence of a fixed exciton-acceptor CPE. We find that, even when the polar nonionic sidechains become quite long (nine ethyleneglycol units), the energy transfer efficiency is hardly affected so long as the inter-CPE network retains a net polyelectrolyte charge. However, near the onset of spontaneous phase separation, we observe a clear influence of the length of the oligo(ethyleneglycol) sidechains on the photophysics of the complex. Our results have implications for the use of polyelectrolyte phase separation to produce aqueous light-harvesting soft materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Local intermodal energy transfer of the secondary instability in a plane channel

A mathematical technique for analyzing local energy-transfer rates among wave-vector triads is developed and applied to the data generated by direct numerical simulations of waves with various types of initial conditions. Starting the simulation with a primary two-dimensional wave and random noise produced structures very similar to those which evolved from three-dimensional center modes. The local transfer rates determined in this case help to explain the eventual deformation of the primary two-dimensional wave which was observed in wind-tunnel experiments. Including weak streamwise vortices in the initial flow field results in large amounts of energy being transferred to the K-type modes early in the simulation. The later development of the waves (and hence the energy-transfer rates) is similar to the previous case.

Singer, Bart A.↗

Cellular and molecular analysis of mutagenesis induced by charged particles of defined linear energy transfer

Mutation induction by charged particles of defined linear energy transfer (LET) and gamma rays was scored using human-hamster hybrid AL cells. The LET values for charged particles accelerated at the Radiological Research Accelerator Facility ranged from 10 keV/microm protons to 150 keV/microm 4He ions. The induced mutant fractions at both the S1 and HGPRT loci were dependent on the dose and LET. In addition, for each dose examined, the mutant yield at the S1 locus was 30-60 fold higher than at the corresponding HGPRT locus. To determine whether the mutation spectrum was comparably dependent on dose and LET, independent S1- and HGPRT- mutants induced by 150 keV/microm 4He ions and gamma rays were isolated, and their DNA was analyzed by both Southern blotting and multiplex PCR methods. While the majority of radiation-induced mutants showed deletions of varying sizes, the relative percentage of large deletions was found to be related to both the dose and LET of the radiation examined. Using a mutation system that can detect multilocus changes, results of the present study show that radiation-induced chromosomal loss can be in the millions of base pairs.

NASA Discipline Radiation Health↗

Cross-beam energy transfer in conditions relevant to direct-drive implosions on OMEGA

In cross-beam energy transfer (CBET), the interference of two laser beams ponderomotively drives an ion-acoustic wave that coherently scatters light from one beam into the other. This redirection of laser beam energy can severely inhibit the performance of direct-drive inertial confinement fusion (ICF) implosions. To assess the role of nonlinear and kinetic processes in direct-drive-relevant CBET, the energy transfer between two laser beams in the plasma conditions of an ICF implosion at the OMEGA laser facility was modeled using particle-in-cell simulations. For typical laser beam intensities, the simulations are in excellent agreement with linear kinetic theory, indicating that nonlinear processes do not play a role in direct-drive implosions. At higher intensities, CBET can be modified by pump depletion, backward stimulated Raman scattering, or ion trapping, depending on the plasma density.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonadiabatic Electronic Energy Transfer in Chemical Oxygen-Iodine Laser: Powered by Derivative Coupling or Spin-Orbit Coupling?

Derivative couplings near a conical intersection and spin-orbit couplings between different spin states are known to facilitate nonadiabatic transitions in molecular systems. In this report, we investigate a prototypical electronic energy transfer process, I( 2 P 3/2 )+O 2 (a 1 Δ g )→I( 2 P 1/2 )+ O 2 (X 3 Σ g - ), which is of great importance for the chemical oxygen-iodine laser. To understand the nonadiabatic dynamics, this multistate process is investigated in full dimensionality with quantum wave packets using diabatic potential energy surfaces coupled by both derivative and spin-orbit couplings, all determined from first principles. A near quantitative agreement with structural, energetic, and kinetic measurements is achieved. Detailed analyses suggest that the nonadiabatic dynamics is largely controlled by derivative coupling near conical intersections, which leads to a small effective barrier and hence a slightly positive temperature dependence of the rate coefficient. The new findings should extend our understanding of energy transfer, provide a quantitative basis for numerical simulations of the chemical oxygen-iodine laser, and have important implications in other electronic energy transfer processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Degrees of locality of energy transfer in the inertial range

Measured raw transfer interactions from which local energy transfer is argued to result are summed in a way that directly indicates the scale disparity (s) of contributions to the net energy flux across the spectrum. It is found that the dependence upon s closely follows the s exp -4/3 form predicted by classical arguments. As a result, it is concluded that direct numerical simulation measurements lend support to the classical Kolmogorov phenomenology of local interactions and local transfer in an inertial range.

Zhou, YE↗