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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Modeling of different scenarios of thin current sheet equilibria in the Earth’s magnetotail

The Earth’s magnetosphere is an open dynamic system permanently interacting with the solar wind, i.e., the plasma flow from the Sun. Some plasma processes in the magnetosphere are of spontaneous explosive character, while others develop rather slowly as compared to the characteristic times of plasma particle motion in it. The large-scale current sheet in the magnetotail can be in an almost equilibrium state both in quiet periods and during geomagnetic perturbations, and its variations can be considered quasistatic. Thus, under some conditions, the magnetotail current sheet can be described as an equilibrium plasma system. Its state depends on various parameters, in particular, on those determining the dynamics of charged particles. Knowing the main governing parameters, one can study the structure and properties of the current sheet equilibrium. This work is devoted to the self-consistent modeling of the equilibrium thin current sheet (TCS) of the Earth’s magnetotail, the thickness of which is comparable with the ion gyroradius. The main objective of this work is to examine how the TCS structure depends on the parameters characterizing the particle dynamics and magnetic field geometry. A numerical hybrid self-consistent TCS model in which the tension of magnetic field lines is counterbalanced by the inertia of ions moving through the sheet is constructed. The ion dynamics is considered in the quasi-adiabatic approximation, while the electron motion, in the conductive fluid approximation. Depending on the values of the adiabaticity parameter κ (which determines the character of plasma particle motion) and the dimensionless normal component of the magnetic field b{sub z}, the following two scenarios are considered: (A) the adiabaticity parameter is proportional to the particle energy and b{sub z} = const and (B) the particle energy is fixed and the adiabaticity parameter is proportional to b{sub z}. The structure of the current sheet and particle dynamics in it are studied as functions of the parameters κ and b{sub z}. It is shown that, in scenario A, the current sheet thickness decreases with increasing adiabaticity parameter due to a decrease in the ion gyroradius. Accordingly, the radius of curvature of magnetic field lines decreases, which leads to an increase in the contribution of electron drift currents near the neutral plane z = 0. Numerical simulations demonstrate that current equilibria can exist if the adiabaticity parameter lies in the range 0.05 ≤ κ ≤ 0.7. At κ ∼ 0.7, the contribution of electron drift currents to the total current density is much larger than the contribution of ions and the ion motion becomes chaotic. At larger values of the adiabaticity parameter, no equilibrium solutions were found in the framework of the given one-dimensional model. Therefore, the value κ = 0.7 corresponds to the upper applicability limit of the quasi-adiabatic model of the current sheet. In scenario B, an increase in the parameter κ leads to the appearance of a large number of quasi-trapped ions in the current sheet, due to which the current sheet thickens and the amplitude of the current density decreases. As a result, equilibrium solutions exist in a much narrower range of the adiabaticity parameter, 0.05≤ κ ≤ 0.25. Consequences of the existence of parametric boundaries of equilibrium solutions for the TCS under actual geomagnetic conditions are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Stochastic Ion Acceleration by the Ion-cyclotron Instability in a Growing Magnetic Field

Using 1D and 2D particle-in-cell simulations of a plasma with a growing magnetic field ${\boldsymbol{B}}$, we show herein that ions can be stochastically accelerated by the ion-cyclotron (IC) instability. As ${\boldsymbol{B}}$ grows, an ion pressure anisotropy ${p}_{\perp ,i}\gt {p}_{| | ,i}$ arises due to the adiabatic invariance of the ion magnetic moment (${p}_{| | ,i}$ and $p_{⊥,i}$ are the ion pressures parallel and perpendicular to ${\boldsymbol{B}}$). When initially $β_ i$ = 0.5 (${\beta }_{i}\equiv 8\pi {p}_{i}/| {\boldsymbol{B}}{| }^{2}$, where $p_i$ is the ion isotropic pressure), the pressure anisotropy is limited mainly by inelastic pitch-angle scattering provided by the IC instability, which in turn produces a nonthermal tail in the ion energy spectrum. After ${\boldsymbol{B}}$ is amplified by a factor of ~2.7, this tail can be approximated as a power law of index ~3.4 plus two nonthermal bumps and accounts for 2%–3% of the ions and ~18% of their kinetic energy. On the contrary, when initially $β_i$ = 2, the ion scattering is dominated by the mirror instability, and the acceleration is suppressed. This implies that efficient ion acceleration requires that initially, $β_{i} \lesssim$ 1. Although we focus on cases where ${\boldsymbol{B}}$ is amplified by plasma shear, we check that the acceleration occurs similarly if ${\boldsymbol{B}}$ grows due to plasma compression. Our results are valid in a subrelativistic regime where the ion thermal energy is ~10% of the ion rest-mass energy. This acceleration process can thus be relevant in the inner region of low-luminosity accretion flows around black holes.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Communication: Global flux surface hopping in Liouville space

Recent years have witnessed substantial progress in the surface hopping (SH) formulation of non-adiabatic molecular dynamics. A generalization of the traditional fewest switches SH (FSSH), global flux SH (GFSH) utilizes the gross population flow between states to derive SH probabilities. The Liouville space formulation of FSSH puts state populations and coherences on equal footing, by shifting the hopping dynamics from Hilbert to Liouville space. Both ideas have shown superior results relative to the standard FSSH in Hilbert space, which has been the most popular approach over the past two and a half decades. By merging the two ideas, we develop GFSH in Liouville space. The new method is nearly as straightforward as the standard FSSH, and carries comparable computational expense. Tested with a representative super-exchange model, it gives the best performance among all existing techniques in the FSSH series. The obtained numerical results match almost perfectly the exact quantum mechanical solutions. Moreover, the results are nearly invariant under the choice of a basis state representation for SH, in contrast to the earlier techniques which exhibit notable basis set dependence. Unique to the developed approach, this property is particularly encouraging, because exact quantum dynamics is representation independent. GFSH in Liouville space significantly improves accuracy and applicability of SH for a broad range of chemical and physical processes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2018

Parameterization of Mixed Layer and Deep-Ocean Mesoscales Including Nonlinearity

In 2011, Chelton et al. carried out a comprehensive census of mesoscales using altimetry data and reached the following conclusions: "essentially all of the observed mesoscale features are nonlinear" and "mesoscales do not move with the mean velocity but with their own drift velocity," which is "the most germane of all the nonlinear metrics." Accounting for these results in a mesoscale parameterization presents conceptual and practical challenges since linear analysis is no longer usable and one needs a model of nonlinearity. A mesoscale parameterization is presented that has the following features: 1) it is based on the solutions of the nonlinear mesoscale dynamical equations, 2) it describes arbitrary tracers, 3) it includes adiabatic (A) and diabatic (D) regimes, 4) the eddy-induced velocity is the sum of a Gent and McWilliams (GM) term plus a new term representing the difference between drift and mean velocities, 5) the new term lowers the transfer of mean potential energy to mesoscales, 6) the isopycnal slopes are not as flat as in the GM case, 7) deep-ocean stratification is enhanced compared to previous parameterizations where being more weakly stratified allowed a large heat uptake that is not observed, 8) the strength of the Deacon cell is reduced. The numerical results are from a stand-alone ocean code with Coordinated Ocean-Ice Reference Experiment I (CORE-I) normal-year forcing.

Baroclinic flows; Mesoscale processes; Mixing; Sub↗
DOE OSTI2019

Onset of magnetic reconnection in a collisionless, high-β plasma

In a magnetized, collisionless plasma, the magnetic moment of the constituent particles is an adiabatic invariant. An increase in the magnetic-field strength in such a plasma hence leads to an increase in the thermal pressure perpendicular to the field lines. Above a $\unicode[STIX]{x1D6FD}$ -dependent threshold (where $\unicode[STIX]{x1D6FD}$ is the ratio of thermal to magnetic pressure), this pressure anisotropy drives the mirror instability, producing strong distortions in the field lines on ion-Larmor scales. The effect of this instability on magnetic reconnection is investigated using a simple analytical model for the formation of a current sheet (CS) and the associated production of pressure anisotropy. The difficulty in maintaining an isotropic, Maxwellian particle distribution during the formation and subsequent thinning of a CS in a collisionless plasma, coupled with the low threshold for the mirror instability in a high- $\unicode[STIX]{x1D6FD}$ plasma, imply that the geometry of reconnecting magnetic fields can differ radically from the standard Harris-sheet profile often used in simulations of collisionless reconnection. Because of this, depending on the rate of CS formation and the initial CS thickness, tearing modes whose growth rates and wavenumbers are boosted by this difference may disrupt the mirror-infested CS before standard tearing modes can develop. A quantitative theory is developed to illustrate this process, which may find application in the tearing-mediated disruption of kinetic magnetorotational ‘channel’ modes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Surface Charge Effects on Fe(II) Sorption and Oxidation at (110) Goethite Surfaces

Iron(III) oxides and oxyhydroxides are among the most reactive minerals in the environment, with surfaces that become charged when immersed in water. The governing role of surface charge over interfacial processes such as metal sorption is well understood. However, its role in interfacial redox reactions, such as when metal sorption is coupled to interfacial electron transfer (ET), is not. This is mainly because surface charge affects not only the types and densities of surface complexes formed but also their respective driving forces for ET. An important case is Fe(II)-catalyzed recrystallization of Fe(III)-oxyhydroxides, in which Fe(II) sorption and interfacial ET are closely linked. We used replica-exchange constant-pH molecular dynamics simulations (Zarzycki, P.; Smith, D. M.; Rosso, K. M. J. Chem. Theory Comput. 2015, 11, 1715–1724) to calculate the distance-dependent electrostatic potential at charged (110) surfaces of goethite particles, assessing its effect on previously computed Fe(II) sorption and interfacial ET free energies (Zarzycki, P.; Kerisit, S.; Rosso, K. M. J. Phys. Chem. C 2015, 119, 3111–3123). We show that Fe(II) adsorbs preferentially as an inner-sphere complex on the negatively charged surface, and as an outer-sphere complex on the positively charged surface because of both electrostatic repulsion and high energy barriers that arise from ordered water layers at the interface. The separation distance between adsorbed Fe(II) and the surface largely dictates adiabatic versus nonadiabatic ET regimes for this interface. The findings help unravel the pH dependence of Fe(II)-catalyzed recrystallization of goethite.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

EFFECT OF ADIABATIC FOCUSING ON THE DIFFUSION OF ENERGETIC CHARGED PARTICLES

An approximate analytic description of a diffusion coefficient, including the effect of adiabatic focusing, has been developed. This description is formulated with the aid of stochastic differential equations and the steady perturbation solution of the Fokker–Plank transport equation. The analytical formula is based on three important assumptions. First, the pitch-angle diffusion coefficient is set to be separable from the spatial coordinate and the pitch-angle cosine. Second, the spatial dependence of the ratio between the mean-free path and focusing length is assumed to be weak. Third, the pitch-angle distribution relaxes quickly to a steady state. The new analytic formula could be applied to calculate the spatial diffusion coefficient in the interplanetary and interstellar space.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Damping of density oscillations in neutrino-transparent nuclear matter

We calculate the bulk-viscous dissipation time for adiabatic density oscillations in nuclear matter at densities of one to seven times the nuclear saturation density and at temperatures ranging from 1 MeV, where corrections to previous low-temperature calculations become important, up to 10 MeV, where the assumption of neutrino transparency is no longer valid. Under these conditions, which are expected to occur in neutron star mergers, damping of density oscillations arises from β equilibration via weak interactions. Here, we find that for 1-kHz oscillations the shortest dissipation times are in the 5- to 20-ms range, depending on the equation of state, which means that bulk viscous damping could affect the dynamics of a neutron star merger. For higher frequencies, the dissipation time can be even shorter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Transient hydroperoxyalkyl intermediates (•QOOH) in isopentane oxidation. II. Isomer-resolved unimolecular dynamics

Transient carbon-centered hydroperoxyalkyl intermediates (•QOOH) in isopentane oxidation are characterized by their time- and energy-resolved unimolecular dissociation dynamics to hydroxyl (OH) and cyclic ether products. Two distinct •QOOH isomers are examined with radical sites at a primary carbon of one of the methyl groups (β-Me) or a secondary carbon (β-Et) of the ethyl group. Energy-dependent unimolecular rates are obtained from the time-dependent appearance of OH products for the two isomers and compared with statistical microcanonical rates computed using RRKM theory, including heavy-atom tunneling, based on high-level theoretical calculations. A benchmark-corrected approach is utilized to compute high-accuracy stationary-point energies, most importantly, transition-state barriers, for the •QOOH_Me and •QOOH_Et isomers in isopentane oxidation, building on higher-level reference calculations for the oxidation of ethane (C 2 H 5 O 2 ) and propane (C 3 H 7 O 2 ), respectively. Here, the measured rates are compared with RRKM calculations incorporating the benchmark-corrected transition-state parameters, a vibrationally adiabatic multidimensional hindered-rotor treatment of key torsions, and quantum tunneling. Agreement between experiment and theory validates the statistical description and shows faster decay for •QOOH_Et due to its lower barrier. Both β-QOOH isomers decay almost exclusively to OH + cyclic ether products under the conditions studied.

Oxidation processes↗
NASA NTRS1999

Effects of Structure and Hydrodynamics on the Sooting Behavior of Spherical Microgravity Diffusion Flames

Recent experimental, numerical and analytical work has shown that the stoichiometric mixture fraction (Z(sub st)) can have a profound effect on soot formation in diffusion flames. These findings were obtained at constant flame temperature (T(sub ad)), employing the approach described in Du and Axelbaum (1995, 1996). For example, a fuel mixture containing 1 mole of ethylene and 11.28 moles of nitrogen burning in pure oxygen ((Z(sub st)) = 0.78) has the same adiabatic flame temperature (2370 K) as that of pure ethylene burning in air ((Z(sub st)) = 0.064). An important finding of these works was that at sufficiently high (Z(sub st)), flames remain blue as strain rate approaches zero in counterflow flames, or as flame height and residence time approach infinity in coflowing flames. Lin and Faeth (1996a) coined the term permanently blue to describe such flames. Two theories have been proposed to explain the appearance of permanently-blue flames at high (Z(sub st)). They are based on (1) hydrodynamics and (2) flame structure. Previous experimental studies in normal gravity are not definitive as to which, if either, mechanism is dominant because both hydrodynamics and structure suppress soot formation at high (Z(sub st)) in coflowing and counterflowing diffusion flames. In counterflow flames with (Z(sub st)) < 0.5 streamlines at the flame sheet are directed toward the fuel. Newly formed soot is convected into richer regions, favoring soot growth over oxidation. For (Z(sub st)) > 0.5, convection at the flame is toward the oxidizer, thus enhancing soot oxidization. Thus, in counterflow flames, hydrodynamics causes soot to be convected towards the oxidizer at high (Z(sub st)) which suppresses soot formation. Axelbaum and co-workers maintain that while the direction of convection can impact soot growth and oxidation, these processes alone cannot cause permanently-blue flames. Soot growth and oxidation are dependent on the existence of soot particles and the presence of soot is invariably accompanied by yellow luminosity. Soot-particle inception, on the other hand, arises from gas-phase reactions and its dependence on flow direction is weak, similar to that of other gas-phase reactions in flames. For example, when the flame moves across the stagnation plane no significant changes in flame chemistry are observed. Furthermore, since the soot-inception zone has a finite thickness, soot has been produced in counterflow flames with (Z(sub st)) > 0.5. For large (Z(sub st)) the fuel concentration decreases and oxygen concentration increases in the soot forming regions of the flame. This yields a shift in the OH profile toward the fuel side of the flame, and this shift can dramatically influence soot inception because it essentially narrows the soot inception zone. Soot-free (permanently-blue) conditions can be realized when the structure of the flame is adjusted to the extent that significant oxidizing species exist on the fuel side of the flame at temperatures above the critical temperature for soot inception, ca. 1250 K. In previously considered flames it was impossible to independently vary flame structure and convection direction. In contrast, spherical diffusion flames (which generally require microgravity) allow both properties to be varied independently. We altered structure (Z(sub st)) by exchanging inert between the oxidizer and the fuel and we independently varied convection direction at the flame sheet by interchanging the injected and ambient gases. In this work we established four flames: (a) ethylene issuing into air, (b) diluted ethylene issuing into oxygen, (c) air issuing into ethylene, and (d) oxygen issuing into diluted ethylene. (Z(sub st)) is 0.064 in flames (a) and (c) and 0.78 in flames (b) and (d). The convection direction is from fuel to oxidizer in flames (a) and (b) and from oxidizer to fuel in flames (c) and (d). Under the assumption of equal diffusivities of all species and heat, the stoichiometric contours of these flames have identical temperatures and nitrogen concentrations.

Sunderland, P. B.↗
DOE OSTI2019

Efficient construction of generalized master equation memory kernels for multi-state systems from nonadiabatic quantum-classical dynamics

Techniques derived from the generalized quantum master equation (GQME) framework have provided the basis for elucidating energy and charge transfer in systems ranging from molecular solids to photosynthetic complexes. Recently, the nonperturbative combination of the GQME with quantum-classical methods has resulted in approaches whose accuracy and efficiency exceed those of the original quantumclassical schemes while offering significant accuracy improvements over perturbative expansions of the GQME. In this work, we show that, while the non-Markovian memory kernel required to propagate the GQME scales quartically with the number of subsystem states, the number of trajectories required scales at most quadratically when using quantum-classical methods to construct the kernel. We then present an algorithm that allows further acceleration of the quantum-classical GQME by offering a way to selectively sample the kernel matrix elements that are most important to the process of interest. We demonstrate the utility of these advances by applying the combination of Ehrenfest mean field theory with the GQME (MF-GQME) to models of the Fenna-Matthews-Olson (FMO) complex and the light harvesting complex II (LHCII), with 7 and 14 states, respectively. This allows us to show that the MF-GQME is able to accurately capture all the relevant dynamical time scales in LHCII: the initial nonequilibrium population transfer on the femtosecond time scale, the steady state-type trapping on the picosecond time scale, and the long time population relaxation. Remarkably, all of these physical effects spanning tens of picoseconds can be encoded in a memory kernel that decays only after ~65 fs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Causes of fuel–ablator mix inferred from modeling of monochromatic time-gated radiography of OMEGA cryogenic implosions

Here, we present evidence, in the context of OMEGA cryogenic target implosions, that laser imprint, known to be capable of degrading laser-direct-drive target performance, plays a major role in generating fuel–ablator mix. OMEGA cryogenic target implosions show a performance boundary correlated with acceleration-phase shell stability; for sufficiently low adiabats (where the adiabat is the ratio of the pressure to the Fermi pressure) and high in-flight aspect ratios (IFAR's), the neutron-weighted shell areal density and neutron yield relative to the clean simulated values sharply decline. Direct evidence of Rayleigh–Taylor fuel–ablator mixing was previously obtained using a Si Heα backlighter driven by an ~20-ps short pulse generated by OMEGA EP. The shadow cast by the shell shortly prior to stagnation, as diagnosed using backlit radiographs, shows a softening near the limb, which is evidence of an ablator–fuel mix region for a low-adiabat implosion (α ~ 1.9, IFAR = 14) but not for a moderate adiabat implosion (α ~ 2.5, IFAR = 10). We find good agreement between experimental and synthetic radiographs in simulations that model laser imprint and account for uncertainty in the initial ablator thickness. Furthermore, we further explore the role of other mechanisms such as classical instability growth at the fuel–ablator interface, species concentration diffusion, and long-wavelength drive and target asymmetries.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Reaction studies of neutral atomic C with H{sub 3}{sup +} using a merged-beams apparatus

We have investigated the chemistry of C+H{sub 3}{sup +} forming CH{sup +}, CH{sub 2}{sup +}, and CH{sub 3}{sup +}. These reactions are believed to be some of the key gas-phase astrochemical processes initiating the formation of organic molecules in molecular clouds. For this work, we have constructed a novel merged fast-beams apparatus which overlaps a beam of molecular ions onto a beam of ground-term neutral atoms. Here, we describe the apparatus in detail and present cross section data for forming CH{sup +} and CH{sub 2}{sup +} at relative energies from ≈9 meV to ≈20 and 3 eV, respectively. Measurements were performed for statistically populated C ({sup 3}P{sub J}) in the ground term reacting with hot H{sub 3}{sup +} (at an internal temperature of ∼2550 K). Using these data, we have derived rate coefficients for translational temperatures from ≈72 K to ∼2.3×10{sup 5} and 3.4×10{sup 4} K, respectively. For the formation of CH{sub 3}{sup +}, we are only able to place an upper limit on the rate coefficient. Our results for CH{sup +} and CH{sub 2}{sup +} are in good agreement with the mass-scaled results from a previous ion trap study of C + D{sub 3}{sup +}, at a translational temperature of ∼1000 K. That work also used statistically populated C ({sup 3}P{sub J}) but internally cold D{sub 3}{sup +} (∼77 K). The good agreement between the two experiments implies that the internal excitation of the H{sub 3}{sup +} is not significant so long as the reaction proceeds adiabatically. At 300 K, the C fine-structure levels are predicted to be essentially statistically populated, enabling us to compare our translational temperature results to thermal equilibrium calculations. At this temperature, our rate coefficient for forming CH{sup +} lies a factor of ≈2.9 below the Langevin rate coefficient currently given in astrochemical databases, and a factor of ∼1.8−3.3 below the published classical trajectory studies using quantum mechanical potential energy surfaces. Our results for CH{sub 2}{sup +} formation at 300 K are a factor of ≈26.7 above these semi-classical results. Astrochemical databases do not currently include this channel. We also present a method for converting our translational temperature results to thermal rate coefficients for temperatures below ∼300 K. The results indicated that CH{sub 2}{sup +} formation dominates over that of CH{sup +} at temperatures ≲50 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2018

Instability Wave–Streak Interactions in a High Mach Number Boundary Layer at Flight Conditions

The interaction of stationary streaks undergoing nonmodal growth with modally unstable instability waves in a hypersonic boundary-layer flow is studied using numerical computations. The geometry and flow conditions are selected to match a relevant trajectory location from the ascent phase of the HIFiRE-1 flight experiment; namely, a 7 degree half-angle, circular cone with 2.5 mm nose radius, freestream Mach number equal to 5.30, unit Reynolds number equal to 13.42 m -1 , and wall-to-adiabatic temperature ratio of approximately 0.35 over most of the vehicle. This paper investigates the nonlinear evolution of initially linear optimal disturbances that evolve into finite-amplitude streaks, followed by an analysis of the modal instability characteristics of the perturbed, streaky boundary-layer flow. The investigation is performed with stationary direct numerical simulations (DNS) and plane-marching parabolized stability equations (PSE), in conjunction with partial-differential-equation-based planar eigenvalue analysis. The overall effect of streaks is to reduce the peak amplification factors of instability waves, indicating a possible downstream shift in the onset of laminar-turbulent transition. The present study confirms previous findings that the mean flow distortion of the nonlinear streak perturbation reduces the amplification rates of the Mack-mode instability. More importantly, however, the present results demonstrate that the spanwise varying component of the streak can produce a larger effect on the Mack-mode amplification. The study with selected azimuthal wavenumbers for the stationary streaks reveals that a wavenumber of approximately 1.4 times larger than the optimal wavenumber is more effective in stabilizing the planar Mack-mode instabilities. In the absence of unstable first-mode waves for the present cold-wall condition, transition onset is expected to be delayed until the peak streak amplitude increases to nearly 35 percent of the freestream velocity, when intrinsic instabilities of the boundary-layer streaks begin to dominate the transition process. For streak amplitudes below that limit a significant net stabilization is achieved, yielding a potential transition delay that can exceed 100 percent of the length of the laminar region in the uncontrolled case.

Boundary layer stability↗
DOE OSTI2022

High-resolution CH stretch spectroscopy of jet-cooled cyclopentyl radical: First insights into equilibrium structure, out-of-plane puckering, and IVR dynamics

First, high-resolution sub-Doppler infrared spectroscopic results for cyclopentyl radical (C 5 H 9 ) are reported on the α-CH stretch fundamental with suppression of spectral congestion achieved by adiabatic cooling to T rot ≈ 19(4) K in a slit jet expansion. Surprisingly, cyclopentyl radical exhibits a rotationally assignable infrared spectrum, despite 3N – 6 = 36 vibrational modes and an upper vibrational state density (ρ ≈ 40–90 #/cm –1 ) in the critical regime (ρ ≈ 100 #/cm –1 ) necessary for onset of intramolecular vibrational relaxation (IVR) dynamics. Such high-resolution data for cyclopentyl radical permit detailed fits to a rigid-rotor asymmetric top Hamiltonian, initial structural information for ground and vibrationally excited states, and opportunities for detailed comparison with theoretical predictions. Specifically, high level ab initio calculations at the coupled-cluster singles, doubles, and perturbative triples (CCSD(T))/ANO0, 1 level are used to calculate an out-of-plane bending potential, which reveals a C 2 symmetry double minimum 1D energy surface over a C 2v transition state. Here, the inversion barrier [V barrier ≈ 3.7(1) kcal/mol] is much larger than the effective moment of inertia for out-of-plane bending, resulting in localization of the cyclopentyl wavefunction near its C 2 symmetry equilibrium geometry and tunneling splittings for the ground state too small (<1 MHz) to be resolved under sub-Doppler slit jet conditions. The persistence of fully resolved high-resolution infrared spectroscopy for such large cyclic polyatomic radicals at high vibrational state densities suggests a “deceleration” of IVR for a cycloalkane ring topology, much as low frequency torsion/methyl rotation degrees of freedom have demonstrated a corresponding “acceleration” of IVR processes in linear hydrocarbons.

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

Polariton spectra under the collective coupling regime. II. 2D non-linear spectra

In our previous work [Mondal et al., J. Chem. Phys. 162, 014114 (2025)], we developed several efficient computational approaches to simulate exciton–polariton dynamics described by the Holstein–Tavis–Cummings (HTC) Hamiltonian under the collective coupling regime. Here, we incorporated these strategies into the previously developed Lindblad-partially linearized density matrix (⁠$\mathscr{L}$-PLDM) approach for simulating 2D electronic spectroscopy (2DES) of exciton–polariton under the collective coupling regime. In particular, we apply the efficient quantum dynamics propagation scheme developed in Paper I to both the forward and the backward propagations in the PLDM and develop an efficient importance sampling scheme and graphics processing unit vectorization scheme that allow us to reduce the computational costs from $\mathscr{O}$($\mathscr{K}$ 2 )$\mathscr{O}$(T 3 ) to $\mathscr{O}$($\mathscr{K}$)$\mathscr{O}$(T 0 ) for the 2DES simulation, where $\mathscr{K}$ is the number of states and T is the number of time steps of propagation. As a result, we further simulated the 2DES for an HTC Hamiltonian under the collective coupling regime and analyzed the signal from both rephasing and non-rephasing contributions of the ground state bleaching, excited state emission, and stimulated emission pathways.

2D non-linear spectra↗
DOE OSTI2016

Surface hopping investigation of the relaxation dynamics in radical cations

Ionization processes can lead to the formation of radical cations with population in several ionic states. In this study, we examine the dynamics of three radical cations starting from an excited ionic state using trajectory surface hopping dynamics in combination with multiconfigurational electronic structure methods. The efficiency of relaxation to the ground state is examined in an effort to understand better whether fragmentation of cations is likely to occur directly on excited states or after relaxation to the ground state. The results on cyclohexadiene, hexatriene, and uracil indicate that relaxation to the ground ionic state is very fast in these systems, while fragmentation before relaxation is rare. Ultrafast relaxation is facilitated by the close proximity of electronic states and the presence of two- and three-state conical intersections. Examining the properties of the systems in the Franck-Condon region can give some insight into the subsequent dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Enhanced axial confinement in a monolithically integrated self-rolled-up SiN x vertical microring photonic coupler

We report an efficient method to introduce enhanced axial confinement in the self-rolled-up SiN x vertical microtube coupler by depositing a thin layer of high refractive index material strip within the coupling section and effectively forming a vertical microring. Three times wider mode spacing is observed in such a vertical microring coupler monolithically integrated with a silicon nitride ridge waveguide as compared to the one without such axial confinement. More importantly, single mode operation within the telecomm C-band and S-band is achieved. The self-rolled-up microtube has been demonstrated to be a versatile device platform, which has found application in a number of areas including nanophotonics,1–7 microelectronics,8 chemical and biological sensing,9–11 and intelligent synthetic neural circuits.12 Because the microtube is a three dimensional (3D) structure readily fabricated using two dimensional processing technology, it may serve naturally as a component in 3D-integrated devices. We had previously demonstrated a vertical microtube coupler (VμTC) monolithically integrated with planar ridge waveguides in silicon photonic platform to achieve 3D photonic coupling and observed greatly enhanced coupling between the microtube and the underlying ridge waveguide.1,13 A similar result was reported independently by another research group shortly thereafter.2 One limitation of the VμTC used in previous experiments is that it supports many modes within the telecommunication C-band because of poor axial confinement. For example, we found multiple resonant coupling peaks, which is not desirable for wavelength division multiplexing (WDM) switches. In order to increase the mode spacing of this 3D photonic coupler and to achieve single mode operation within the C-band, we propose efficient axial confinement in the microtube to suppress the higher order modes. Axial confinement in self-rolled-up microtubes had been studied both theoretically and experimentally by a couple of research groups.14–17 In all these previous cases, the axial confinement was introduced by a specially designed geometrical shape of a section of the microtube. After being rolled up, the microtube wall will have different thicknesses at different axial locations. The different wall thicknesses result in a slightly varying effective refractive index of the supported whispering gallery modes (WGMs) along the axial direction of the microtube. When a parabolic shape is used, the effective index of the WGM at the center of the parabola will be the highest and decrease adiabatically along both sides. However, the refractive index change due to different wall thicknesses is very small; hence, the axial confinement is rather weak. Here in this paper, we present our experimental endeavor to incorporate a different axial confinement scheme in the monolithically integrated vertical microtube (VμT) to form a vertical microring (VμR) resonator and demonstrate 3 times wider mode spacing than the microtube based vertical photonic coupler and the potential to achieve a higher Q-factor.

36 MATERIALS SCIENCE↗