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DOE OSTI2015

Influences of Quantum Mechanically Mixed Electronic and Vibrational Pigment States in 2D Electronic Spectra of Photosynthetic Systems: Strong Electronic Coupling Cases

In 2D electronic spectroscopy studies, long-lived quantum beats have recently been observed in photosynthetic systems, and several theoretical studies have suggested that the beats are produced by quantum mechanically mixed electronic and vibrational states. Concerning the electronic-vibrational quantum mixtures, the impact of protein-induced fluctuations was examined by calculating the 2D electronic spectra of a weakly coupled dimer with the Franck-Condon active vibrational modes in the resonant condition. This analysis demonstrated that quantum mixtures of the vibronic resonance are rather robust under the influence of the fluctuations at cryogenic temperatures, whereas the mixtures are eradicated by the fluctuations at physiological temperatures. However, this conclusion cannot be generalized because the magnitude of the coupling inducing the quantum mixtures is proportional to the inter-pigment electronic coupling. In this paper, we explore the impact of the fluctuations on electronic-vibrational quantum mixtures in a strongly coupled dimer with an off-resonant vibrational mode. Toward this end, we calculate energy transfer dynamics and 2D electronic spectra of a model dimer that corresponds to the most strongly coupled bacteriochlorophyll molecules in the Fenna-Matthews-Olson complex in a numerically accurate manner. The quantum mixtures are found to be robust under the exposure of protein-induced fluctuations at cryogenic temperatures, irrespective of the resonance. At 300 K, however, the quantum mixing is disturbed more strongly by the fluctuations, and therefore, the beats in the 2D spectra become obscure even in a strongly coupled dimer with a resonant vibrational mode. Further, the overall behaviors of the energy transfer dynamics are demonstrated to be dominated by the environment and coupling between the 0 0 vibronic transitions as long as the Huang-Rhys factor of the vibrational mode is small. Finally, the electronic-vibrational quantum mixtures do not necessarily play a significant role in electronic energy transfer dynamics despite contributing to the enhancement of long-lived quantum beating in the 2D spectra.

2D electronic spectra↗

DOE OSTI2017

Light weakly coupled axial forces: models, constraints, and projections

Here, we investigate the landscape of constraints on MeV-GeV scale, hidden U(1) forces with nonzero axial-vector couplings to Standard Model fermions. While the purely vector-coupled dark photon, which may arise from kinetic mixing, is a well-motivated scenario, several MeV-scale anomalies motivate a theory with axial couplings which can be UV-completed consistent with Standard Model gauge invariance. Moreover, existing constraints on dark photons depend on products of various combinations of axial and vector couplings, making it difficult to isolate the e ects of axial couplings for particular flavors of SM fermions. We present a representative renormalizable, UV-complete model of a dark photon with adjustable axial and vector couplings, discuss its general features, and show how some UV constraints may be relaxed in a model with nonrenormalizable Yukawa couplings at the expense of fine-tuning. We survey the existing parameter space and the projected reach of planned experiments, brie y commenting on the relevance of the allowed parameter space to low-energy anomalies in π 0 and 8 Be* decay.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2019

Thick branes in extra dimensions and suppressed dark couplings

The nature of dark matter (DM) and how it may interact with the various fields of the Standard Model (SM) remains a mystery. In this paper we show that the interaction between new light dark matter mediators and the SM particles can be naturally suppressed if one employs a single, flat extra dimension (ED). In this setup, the SM fields are localized in a finite width ‘fat’ brane, similar to models of Universal Extra Dimensions (UED), while DM, in turn, is confined to a thin brane at the opposite end of the ED interval. Including brane localized kinetic terms on the fat brane for the mediator fields, the resulting coupling between the SM and these light mediators can be several orders of magnitude smaller than the corresponding ones between the mediators and DM which we assume to be a typical gauge coupling. We investigate the implications of this scenario for both vector (i.e, dark photon, DP) and scalar mediator fields in the 5-D bulk. In this setup kinetic mixing, which is usually employed to suppress light mediator couplings, is not required. Here we assume that the SM particles couple to the DP via their B - L charges while the DP couples to the DM via a dark charge. Both the vector DP couplings and the corresponding Higgs portal couplings with the SM are shown to be natural small in magnitude with a size dependent on ratio of the 5-D compactification radius, R -1 ~ 0.1-1 GeV, and the SM brane thickness, L -1 ~ 2-10 TeV, a range chosen to avoid LHC and other experimental constraints. In this framework one can obtain the observed value of the DM relic abundance for a wide range of parameter choices, while the constrains due to direct DM detection and the invisible width of the Higgs do not impose significant challenges to the model. Finally, this mechanism can lead to distinct signatures in both present and upcoming experiments as it combines some common features of UED and DP models in a single ED setup.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

A coupling approach for linear elasticity problems with spatially non-coincident discretized interfaces

Here we present a new method for coupled linear elasticity problems whose finite element discretization may lead to spatially non-coincident discretized interfaces. Our approach combines the classical Dirichlet–Neumann coupling formulation with a new set of discretized interface conditions obtained through Taylor series expansions. We show that these conditions ensure linear consistency of the coupled finite element solution. We then formulate an iterative solution method for the coupled discrete system and apply the new coupling approach to two representative settings for which we also provide several numerical illustrations. The first setting is a mesh-tying problem in which both coupled structures have the same Lamé parameters whereas the second setting is an interface problem for which the Lamé parameters in the two coupled structures are different.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2020

Heat flow enhancement in a nanoscale plasmonic junction induced by Kondo resonances and electron-phonon coupling

Here recently, we showed that plasmon-exciton coupling can increase entropy current through a bridge coupled to plasmonic metal nanoparticles. Here we show that electron-phonon coupling can also be used to control the entropy current in similar systems. Entropy current tends to decrease due to electron-phonon coupling and to exhibit a monotonous decrease upon temperature ramping. However, an anomaly affecting the current where it is enhanced by electron-phonon coupling is indicated at around 42 times the system's Kondo temperature. We therefore report means to control heat flow by tuning the Kondo resonance through the electron-phonon coupling. We analyze the conditions that bring about these trends due to electron-phonon coupling by employing non-equilibrium Green's function formulation addressing the entropy current and the derived heat flow.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Comparison of Computational Strategies for the Calculation of the Electronic Coupling in Intermolecular Energy and Electron Transport Processes

Electronic couplings in intermolecular electron and energy transfer processes calculated by six different existing computational techniques are compared to nonorthogonal configuration interaction for fragments (NOCI-F) results. The paper addresses the calculation of the electronic coupling in diketopyrrolopyrol, tetracene, 5,5'-difluoroindigo, and benzene–Cl for hole and electron transport, as well as the local exciton and singlet fission coupling. NOCI-F provides a rigorous computational scheme to calculate these couplings, but its computational cost is rather elevated. The here-considered ab initio Frenkel–Davydov (AIFD), Dimer projection (DIPRO), transition dipole moment coupling, Michl–Smith, effective Hamiltonian, and Mulliken–Hush approaches are computationally less demanding, and the comparison with the NOCI-F results shows that the NOCI-F results in the couplings for hole and electron transport are rather accurately predicted by the more approximate schemes but that the NOCI-F exciton transfer and singlet fission couplings are more difficult to reproduce.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Low-Temperature Reductive Coupling of Formaldehyde on Rutile TiO2(110)

The formation and the coupling of methylene upon dissociation of formaldehyde on reduced TiO2(110) are studied using variable temperature scanning tunneling microscope (STM). In agreement with prior studies, formaldehyde preferably adsorbs to bridging-bonded oxygen vacancy (VO) defect site. VO-bound formaldehyde couples with Ti-bound CH2O forming a diolate species, which appears as the majority visible product on the surface at 300 K. Here, STM images directly visualize another low-temperature coupling reaction channel. Two VO-bound formaldehyde molecules can couple and form Ti-bound species, which desorbs above ~215 K. This coupling reaction heals both the VO sites indicating the formation and the desorption of ethylene. We also directly observed the diffusion of methylene groups to nearby empty VO sites upon dissociation of the C-O bond in VO-bound formaldehyde, which suggests that the ethylene formation is via coupling of the methylene groups. Statistical analysis shows that the total visible reaction products observed on the surfaces can only account for a half of the consumption of the initial VO coverage, which further supports the desorption of the coupling reaction product, ethylene, after formaldehyde exposures at 215 K and 300 K.

Zhu, Ke↗

DOE OSTI2022

Formation of the N≡N Triple Bond from Reductive Coupling of a Paramagnetic Diruthenium Nitrido Compound

Construction of nitrogen–nitrogen triple bonds via homocoupling of metal nitrides is an important fundamental reaction relevant to a potential Nitrogen Economy. Here, we report that room temperature photolysis of Ru 2 (chp) 4 N 3 (chp– = 2-chloro-6-hydroxypyridinate) in CH 2 Cl 2 produces N 2 via reductive coupling of Ru2(chp)4N nitrido species. Computational analysis reveals that the nitride coupling transition state (TS) features an out-of-plane “zigzag” geometry instead of the anticipated planar zigzag TS. However, with intentional exclusion of dispersion correction, the planar zigzag TS geometry can also be found. Both the out-of-plane and planar zigzag TS geometries feature two important types of orbital interactions: (1) donor–acceptor interactions involving intermolecular donation of a nitride lone pair into an empty Ru–N π* orbital and (2) Ru–N π to Ru–N π* interactions derived from coupling of nitridyl radicals. The relative importance of these two interactions is quantified both at and after the TS. Our analysis shows that both interactions are important for the formation of the N–N σ bond, while radical coupling interactions dominate the formation of N–N π bonds. Comparison is made to isoelectronic Ru 2 -oxo compounds. Formation of an O–O bond via bimolecular oxo coupling is not observed experimentally and is calculated to have a much higher TS energy. As a result, the major difference between the nitrido and oxo systems stems from an extremely large driving force, ~–500 kJ/mol, for N–N coupling vs a more modest driving force for O–O coupling, –40 to –140 kJ/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Development of Land‐River Two‐Way Hydrologic Coupling for Floodplain Inundation in the Energy Exascale Earth System Model

Abstract Floodplain inundation links river and land systems through significant water, sediment, and nutrient exchanges. However, these two‐way interactions between land and river are currently missing in most Earth System Models. In this study, we introduced the two‐way hydrological coupling between the land component, E3SM Land Model, and the river component, Model for Scale Adaptive River Transport, in Energy Exascale Earth System Model (E3SM) to study the impacts of floodplain inundation on land and river processes. We calibrated the river channel geometry and developed a new data‐driven inundation scheme to improve the simulation of inundation dynamics in E3SM. The new inundation scheme captures 96% of the spatial variation of inundation area in a satellite inundation product at global scale, in contrast with 7% when the default inundation scheme of E3SM was used. Global simulations including the new inundation scheme performed at resolution with and without land‐river two‐way coupling was used to quantify the impact of coupling. Comparisons show that two‐way coupling modifies the water and energy cycle in 20% of the global land cells. Specifically, riverine inundation is reduced by two‐way coupling, but inland inundation is intensified. Wetter periods are more impacted by the two‐way coupling at the global scale, while regions with different climates exhibit different sensitivities. The two‐way exchange of water between the land and river components of E3SM provides the foundation for enabling two‐way coupling of land‐river sediment and biogeochemical fluxes. These capabilities will be used to improve understanding of the interactions between water and biogeochemical cycles and their response to human perturbations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Insights on Simulating Summer Warming of the Great Lakes: Understanding the Behavior of a Newly Developed Coupled Lake-Atmosphere Modeling System

The Laurentian Great Lakes are the world's largest freshwater system and regulate the climate of the Great Lakes region, which has been increasingly experiencing climatic, hydrological, and ecological changes. An accurate mechanistic representation of the Great Lakes thermal structure in Regional Climate Models (RCMs) is paramount to studying the climate of this region. Currently, RCMs have primarily represented the Great Lakes through coupled one-dimensional (1D) column lake models; this approach works well for small inland lakes but is unable to resolve the realistic hydrodynamics of the Great Lakes and leads to inaccurate representations of lake surface temperature (LST) that influence regional climate and weather patterns. This work overcomes this limitation by developing a fully two-way coupled modeling system using the Weather Research and Forecasting model and a three-dimensional (3D) hydrodynamic model. The coupled model system resolves the interactive physical processes between the atmosphere, lake, and surrounding watersheds; and validated against a range of observational data. The model is then used to investigate the potential impacts of lake-atmosphere coupling on the simulated summer LST of Lake Superior. By evaluating the difference between our two-way coupled modeling system and our observation-driven modeling system, we find that coupled-lake atmosphere dynamics can lead to a higher LST during June-September through higher net surface heat flux entering the lake in June and July and a lower net surface heat flux entering the lake in August and September. The unstratified water in June distributes the entering surface heat flux throughout the water column leading to a minor LST increase, while the stratified waters of July create a conducive thermal structure for the water surface to warm rapidly under the higher incoming surface heat flux. This research provides insight into the coupled modeling system behavior, which is critical for enhancing our predictive understanding of the Great Lakes climate system.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Spin–phonon couplings in transition metal complexes with slow magnetic relaxation

Spin–phonon coupling plays an important role in single-molecule magnets and molecular qubits. However, there have been few detailed studies of its nature. Here in this paper, we show for the first time distinct couplings of g phonons of Co II (acac) 2 (H 2 O) 2 (acac = acetylacetonate) and its deuterated analogs with zero-field-split, excited magnetic/spin levels (Kramers doublet (KD)) of the S = 3/2 electronic ground state. The couplings are observed as avoided crossings in magnetic-field-dependent Raman spectra with coupling constants of 1–2 cm -1 . Far-IR spectra reveal the magnetic-dipole-allowed, inter-KD transition, shifting to higher energy with increasing field. Density functional theory calculations are used to rationalize energies and symmetries of the phonons. A vibronic coupling model, supported by electronic structure calculations, is proposed to rationalize the behavior of the coupled Raman peaks. In conclusion, this work spectroscopically reveals and quantitates the spin–phonon couplings in typical transition metal complexes and sheds light on the origin of the spin–phonon entanglement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Parametric longitudinal coupling between a high-impedance superconducting resonator and a semiconductor quantum dot singlet-triplet spin qubit

Coupling qubits to a superconducting resonator provides a mechanism to enable long-distance entangling operations in a quantum computer based on spins in semiconducting materials. Here, we demonstrate a controllable spin-photon coupling based on a longitudinal interaction between a spin qubit and a resonator. We show that coupling a singlet-triplet qubit to a high-impedance superconducting resonator can produce the desired longitudinal coupling when the qubit is driven near the resonator’s frequency. We measure the energy splitting of the qubit as a function of the drive amplitude and frequency of a microwave signal applied near the resonator antinode, revealing pronounced effects close to the resonator frequency due to longitudinal coupling. By tuning the amplitude of the drive, we reach a regime with longitudinal coupling exceeding 1 MHz. This mechanism for qubit-resonator coupling represents a stepping stone towards producing high-fidelity two-qubit gates mediated by a superconducting resonator.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

Coupled Langmuir oscillations in 2-dimensional quantum plasmas

In this work, we present a hydrodynamic model to study the coupled quantum electron plasma oscillations (QEPO) for two dimensional (2D) degenerate plasmas, which incorporates all the essential quantum ingredients such as the statistical degeneracy pressure, electron-exchange, and electron quantum diffraction effect. Effects of diverse physical aspects like the electronic band-dispersion effect, the electron exchange-correlations and the quantum Bohm-potential as well as other important plasma parameters such as the coupling parameter (plasma separation) and the plasma electron number-densities on the linear response of the coupled system are investigated. By studying three different 2D plasma coupling types, namely, graphene-graphene, graphene-metalfilm, and metalfilm-metalfilm coupling configurations, it is remarked that the collective quantum effects can influence the coupled modes quite differently, depending on the type of the plasma configuration. It is also found that the slow and fast QEPO frequency modes respond very differently to the change in plasma parameters. Current findings can help in understanding of the coupled density oscillations in multilayer graphene, graphene-based heterojunctions, or nanofabricated integrated circuits.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2015

Anomalous photon-gauge boson coupling contribution to the exclusive vector boson pair production from two photon exchange in pp collisions at 13 TeV

We study the W and Z pair production from two-photon exchange in proton-proton collisions at the LHC in order to evaluate the contributions of anomalous photon-gauge boson couplings, that simulates new particles and couplings predicted in many Standard Model (SM) extensions. The experimental results of W{sup +} W{sup −} exclusive production (pp → pW{sup +}W{sup −} p) at 7 TeV from the CMS collaboration [1] updates the experimental limits on anomalous couplings obtained at the Large Electron-Positron Collider (LEP). This motivates our present analysis hopefully anticipating the expected results using the Precision Proton Spectrometer (PPS) to be installed as part of CMS. In this work, we consider the W{sup +}W{sup −} exclusive production to present the p{sub T} distribution of the lepton pair corresponding to the SM signal with p{sub T} (e, μ) > 10 GeV. Next, we consider the photon-gauge boson anomalous couplings by calculating, from the FPMC and MadGraph event generators, the process γγ → W{sup +}W{sup −} from a model with gauge boson quartic couplings, by considering a 1 TeV scale for new physical effects. We present our results for an integrated luminosity of 5 fb{sup −1} at center-of-mass energy of 7 TeV and for an integrated luminosity of 100 fb{sup −1} at 13 TeV. We present our preliminary results for Z pair exclusive production from two-photon exchange with anomalous couplings, where the ZZγγ quartic coupling is absent in the SM. We calculate the total cross section for the exclusive process and present the four lepton invariant mass distribution. Finally we present an outlook for the present analysis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2015

Interference between Coulombic and CT-mediated couplings in molecular aggregates: H- to J-aggregate transformation in perylene-based π-stacks

The spectroscopic differences between J and H-aggregates are traditionally attributed to the spatial dependence of the Coulombic coupling, as originally proposed by Kasha. However, in tightly packed molecular aggregates wave functions on neighboring molecules overlap, leading to an additional charge transfer (CT) mediated exciton coupling with a vastly different spatial dependence. The latter is governed by the nodal patterns of the molecular LUMOs and HOMOs from which the electron (t{sub e}) and hole (t{sub h}) transfer integrals derive. The sign of the CT-mediated coupling depends on the sign of the product t{sub e}t{sub h} and is therefore highly sensitive to small (sub-Angstrom) transverse displacements or slips. Given that Coulombic and CT-mediated couplings exist simultaneously in tightly packed molecular systems, the interference between the two must be considered when defining J and H-aggregates. Generally, such π-stacked aggregates do not abide by the traditional classification scheme of Kasha: for example, even when the Coulomb coupling is strong the presence of a similarly strong but destructively interfering CT-mediated coupling results in “null-aggregates” which spectroscopically resemble uncoupled molecules. Based on a Frenkel/CT Holstein Hamiltonian that takes into account both sources of electronic coupling as well as intramolecular vibrations, vibronic spectral signatures are developed for integrated Frenkel/CT systems in both the perturbative and resonance regimes. In the perturbative regime, the sign of the lowest exciton band curvature, which rigorously defines J and H-aggregation, is directly tracked by the ratio of the first two vibronic peak intensities. Even in the resonance regime, the vibronic ratio remains a useful tool to evaluate the J or H nature of the system. The theory developed is applied to the reversible H to J-aggregate transformations recently observed in several perylene bisimide systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Near field fluid coupling between internal motion of the organ of Corti and the basilar membrane

The pressure distribution in each of the fluid chambers of the cochlea can be decomposed into a 1D, or plane wave, component and a near field component, which decays rapidly away from the excitation point. The transverse motion of the basilar membrane, BM, for example, generates both a 1D pressure field, which couples into the slow wave, and a local near field pressure, proportional to the BM acceleration, that generates an added mass on the BM due to the fluid motion. When the organ of Corti, OC, undergoes internal motion, due for example to outer hair cell activity, this motion will not itself generate any 1D pressure if the OC is incompressible and the BM is constrained not to move volumetrically, and so will not directly couple into the slow wave. This motion will, however, generate a near field pressure, proportional to the OC acceleration, which will act on the OC and thus increases its effective mass. The near field pressure due to this OC motion will also act on the BM, generating a force on the BM proportional to the acceleration of the OC, and thus create a “coupling mass” effect. By reciprocity, this coupling mass is the same as that acting on the OC due to the motion of the BM. This near field fluid coupling is initially observed in a finite element model of a slice of the cochlea. These simulations suggest a simple analytical formulation for the fluid coupling, using higher order beam modes across the width of the cochlear partition. It is well known that the added mass due to the near field pressure dominates the overall mass of the BM, and thus significantly affects the micromechanical dynamics. This work not only quantifies the added mass of the OC due its own motion in the fluid, and shows that this is important, but also demonstrates that the coupling mass effect between the BM and OC significantly affects the dynamics of simple micromechanical models.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Inter-phase heat transfer and energy coupling in turbulent dispersed multiphase flows

Here, the present paper addresses important fundamental issues of inter-phase heat transfer and energy coupling in turbulent dispersed multiphase flows through scaling analysis. In typical point-particle or two-fluid approaches, the fluid motion and convective heat transfer at the particle scale are not resolved and the momentum and energy coupling between fluid and particles are provided by proper closure models. By examining the kinetic energy transfer due to the coupling forces from the macroscale to microscale fluid motion, closure models are obtained for the contributions of the coupling forces to the energy coupling. Due to the inviscid origin of the added-mass force, its contribution to the microscale kinetic energy does not contribute to dissipative transfer to fluid internal energy as was done by the quasi-steady force. Time scale analysis shows that when the particle is larger than a critical diameter, the diffusive-unsteady kernel decays at a time scale that is smaller than the Kolmogorov time scale. As a result, the computationally costly Basset-like integral form of diffusive-unsteady heat transfer can be simplified to a non-integral form. Conventionally, the fluid-to-particle volumetric heat capacity ratio is used to evaluate the relative importance of the unsteady heat transfer to the energy balance of the particles. Therefore, for gas-particle flows, where the fluid-to-particle volumetric heat capacity ratio is small, unsteady heat transfer is usually ignored. However, the present scaling analysis shows that for small fluid-to-particle volumetric heat capacity ratio, the importance of the unsteady heat transfer actually depends on the ratio between the particle size and the Kolmogorov scale. Furthermore, the particle mass loading multiplied by the heat capacity ratio is usually used to estimate the importance of the thermal two-way coupling effect. Through scaling argument, improved estimates are established for the energy coupling parameters of each energy exchange mechanism between the phases.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Spatial coupling of gyrokinetic simulations, a generalized scheme based on first-principles

In this paper, we present a scheme that spatially couples two gyrokinetic codes using first-principles. Coupled equations are presented and a necessary and sufficient condition for ensuring accuracy is derived. This new scheme couples both the field and the particle distribution function. The coupling of the distribution function is only performed once every few time-steps, using a five-dimensional (5D) grid to communicate the distribution function between the two codes. This 5D grid interface enables the coupling of different types of codes and models, such as particle and continuum codes, or delta-f and total-f models. Transferring information from the 5D grid to the marker particle weights is achieved using a new resampling technique. Demonstration of the coupling scheme is shown using two XGC gyrokinetic simulations for both the core and edge. We also apply the coupling scheme to two continuum simulations for a one-dimensional advection–diffusion problem.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗