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DOE OSTI2019

Atomic and Molecular Physics in Strong Fields

In this project, we have investigated a broad range of atomic, molecular, and optical (AMO) processes of current significance in strong-field and ultrafast science and technology. The main goals are to develop new theoretical formalisms and accurate computational methods for ab initio and in-depth non-perturbative study of time-resolved multiphoton quantum dynamics and spectroscopy, very-high-order harmonic generation, optimal control of ultrafast attosecond pulse generation, and resonance-enhanced below threshold harmonics in intense ultrashort laser fields. We have worked on the following projects and we have published 20 top 15 % SCI journal articles during the last 3.5 years (Jan. 1, 2016 to June 30, 2019), including one article in top raking Physical Review Letters, and 3 articles in top ranking (Nature) Scientific Reports, and one Physical Review A article was chosen as Editors’ suggestion paper, etc. (a) Development of new time-dependent methods for accurate and efficient solution of multi-dimensional time-dependent Schrödinger equation and time-dependent density functional theory. (b) Non-perturbative treatment of very-high order (1000th – 5000th order) harmonic generation and broadband supercontinuum spectra from XUV to soft x-ray regime. (c) Development of synchrosqueezing transform (SST) for precision time-frequency analysis of electron multi-rescattering dynamics. (d) Exploration of the dynamical origin of resonance-enhanced near- and below-threshold harmonics. (e) Probing the high-order harmonics generation in disordered semiconductor. (f) Multiphoton ionization of one-electron relativistic diatomic quasi-molecules in strong laser fields. and, (g) New development of non-adiabatic density functional theory. The theoretical and simulation projects we have pursued are closely related to the ongoing experimental researches in several leading laboratories in the US and Europe, etc. It is expected that the outcome of this project will provide timely and significant new information and insight for the advancement of strong-field atomic and molecular physics and ultrafast science and technology.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Predicting Excitation Energies of Twisted Intramolecular Charge-Transfer States with the Time-Dependent Density Functional Theory: Comparison with Experimental Measurements in the Gas Phase and Solvents Ranging from Hexanes to Acetonitrile

Electronically excited states characterized by intramolecular charge transfer play an essential role in many biological processes and optical devices. The ability to make quantitative ab initio predictions of the relative energetics involved is a challenging yet desirable goal, especially for large molecules in solution. In this work, we present a data set of 61 experimental measurements of absorption and emission processes, both in the gas phase and in solvents representing a broad range of polarities, which involve intramolecular charge transfer mediated by a nonzero, "twisted" dihedral angle between one or more donor and acceptor subunits. Among a variety of density functionals investigated within the framework of linear-response theory, the "optimally tuned" LRC-ωPBE functional, which utilizes a system-specific yet nonempirical procedure to specify the range-separation parameter, emerges as the preferred choice. For the entire set of excitation energies, involving changes in dipole moment ranging from 4 to >20 Debye, the mean signed and absolute errors are 0.02 and 0.18 eV, respectively (compared, e.g., to -0.30 and 0.30 for PBE0, 0.44 and 0.47 for LRC-ωPBEh, 0.83 and 0.83 for ωB97X-V). We analyze the performance of polarizable continuum solvation models available in Q-Chem that partition the solvent response into fast and slow time scales, and clear trends emerge when measurements corresponding to the four small 4-(dimethylamino)benzonitrile (DMABN)-like molecules and a charged species are excluded. We make the case that the large errors found only for small molecules in the gas phase and weak solvents cannot be expected to improve via the optimal tuning procedure, which enforces a condition that is exact only in the well-separated donor-acceptor limit, and present empirical evidence implicating the outsized importance for small donor-acceptor systems of relaxation effects that cannot be accounted for by the linear-response time-dependent density functional theory within the adiabatic approximation. Finally, we demonstrate the utility of the optimally tuned density functional approach by targeting the charge-transfer states of a large biomimetic model system for light-harvesting structures in Photosystem II.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Validity of the Born-Oppenheimer approximation in the indirect-dissociative-recombination process

An alternative method is introduced to solve a simple two-dimensional model describing vibrational excitation and dissociation processes during the electron-molecule collisions. The model works with one electronic and one nuclear degree of freedom. The two-dimensional R matrix can be constructed simultaneously on the electronic and nuclear surfaces using all three forms developed previously for electron-atom and electron-molecule collisions. These are the eigenchannel R-matrix form, inversion technique of Nesbet and Robicheaux, and the Wigner-Eisenbud-type form using expansion over the poles of the symmetrized Hamiltonian. The 2D R-matrix method is employed to solve a simple model tailored to describe the dissociative recombination and the vibrational excitation of H 2 + cation in the singlet ungerade symmetry 1 Σ u . These results then serve as a (near-exact) benchmark for the following calculation in which the R-matrix states are replaced by their Born-Oppenheimer approximations. Furthermore, the accuracy of this approach and its correction with the first-order nonadiabatic couplings are discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Potassium carbonate decomposition modeling within rotating detonation engines for direct power extraction applications

We report that recently, there has been a significant interest in detonation-based combustion systems, such as rotating detonation engines (RDE), due to potential performance advantages in propulsion and energy applications. This includes improvements in thermodynamic efficiency, inherently high gas velocities, and the possibility of achieving an increase in total pressure (i.e. pressure gain) through the combustion process. Due to approximating a constant volume combustion process, these devices also tend to exhibit extremely high local gas temperatures relative to a comparable constant pressure combustor. These advantages overlap well with desirable performance characteristics of direct power extraction (DPE) technologies, such as a magnetohydrodynamic (MHD) generator. Typically, in DPE systems hot combustion products are seeded with an easily ionizable material such as potassium carbonate (K 2 CO 3 ) in order to boost the electrical conductivity. However, due to the short gas residence times within an RDE, it was unclear whether forming an electrically conductive combustion plasma would be feasible for integration with a downstream MHD generator. A model is presented which describes the heating, decomposition, and ionization of solid K 2 CO 3 particles and aqueous solutions of K 2 CO 3 in water, for a given initial particle diameter. This model was combined with available computational fluid dynamics (CFD) data for an oxygen-methane RDE in a one-way coupled Eulerian-Lagrangian framework to predict particle trajectories and the corresponding heating, decomposition, and ionization histories. Electrical conductivities were computed using a previously developed model, and a method was proposed to determine an equivalent average electrical conductivity. Results show that particle sizes below ~30 µm are able to fully decompose before reaching the exit of the RDE. While the one-way coupled nature of the simulations precluded rigorous evaluation of the effects of seed material on detonability, a substantial temperature reduction is expected at the detonation wave front due to heating and decomposition. A preliminary comparison is presented between the RDE and an equivalent constant pressure adiabatic combustor, showing a potential performance advantage for the RDE.

42 ENGINEERING↗

DOE OSTI2024

Cloud response to co-condensation of water and organic vapors over the boreal forest

Abstract. Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation-driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct chemical ionization mass spectrometer (I-CIMS), is utilized to construct volatility distributions of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of temperature, relative humidity, updraft velocity, aerosol size distribution, organic vapor concentration, and the volatility distribution. The predicted median enhancements in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics fall on average between 16 % and 22 %. This corresponds to activating particles 10–16 nm smaller in dry diameter that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ∼ 40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30 %–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest. To evaluate the frequencies with which such distributions are experienced by an Earth system model over the whole boreal biome, 5 years of UK Earth System Model (UKESM1) simulations are further used. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time), and the positive values, peaking in spring, are modeled only over Fennoscandia and the western parts of Siberia. Overall, the similarities in the size distributions between observed and modeled (UKESM1) are limited, which would limit the ability of this model, or any model with a similar aerosol representation, to project the climate relevance of co-condensation over the boreal forest. For the critical aerosol size distribution regime, ΔCDNC is shown to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs), especially when the overall particle surface area is low. The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low- and low-volatility organic compounds (ELVOCs and LVOCs). The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below the cloud base, and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce the critical supersaturations enough for droplet activation to occur. A reduction in the critical supersaturation caused by organic condensation emerges as the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, also in larger-scale models, an accurate representation of the aerosol size distribution is critical. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Planck 2018 results

We analyse the Planck full-mission cosmic microwave background (CMB) temperature and E -mode polarization maps to obtain constraints on primordial non-Gaussianity (NG). We compare estimates obtained from separable template-fitting, binned, and optimal modal bispectrum estimators, finding consistent values for the local, equilateral, and orthogonal bispectrum amplitudes. Our combined temperature and polarization analysis produces the following final results: f NL local = -0.9 ± 5.1; f NL equil = -26 ± 47; and f NL ortho = -38 ± 24 (68% CL, statistical). These results include low-multipole (4 ≤ ℓ < 40) polarization data that are not included in our previous analysis. The results also pass an extensive battery of tests (with additional tests regarding foreground residuals compared to 2015), and they are stable with respect to our 2015 measurements (with small fluctuations, at the level of a fraction of a standard deviation, which is consistent with changes in data processing). Polarization-only bispectra display a significant improvement in robustness; they can now be used independently to set primordial NG constraints with a sensitivity comparable to WMAP temperature-based results and they give excellent agreement. In addition to the analysis of the standard local, equilateral, and orthogonal bispectrum shapes, we consider a large number of additional cases, such as scale-dependent feature and resonance bispectra, isocurvature primordial NG, and parity-breaking models, where we also place tight constraints but do not detect any signal. The non-primordial lensing bispectrum is, however, detected with an improved significance compared to 2015, excluding the null hypothesis at 3.5 σ . Beyond estimates of individual shape amplitudes, we also present model-independent reconstructions and analyses of the Planck CMB bispectrum. Our final constraint on the local primordial trispectrum shape is g NL local = (-5.8 ± 6.5) × 10 4 (68% CL, statistical), while constraints for other trispectrum shapes are also determined. Exploiting the tight limits on various bispectrum and trispectrum shapes, we constrain the parameter space of different early-Universe scenarios that generate primordial NG, including general single-field models of inflation, multi-field models (e.g. curvaton models), models of inflation with axion fields producing parity-violation bispectra in the tensor sector, and inflationary models involving vector-like fields with directionally-dependent bispectra. Our results provide a high-precision test for structure-formation scenarios, showing complete agreement with the basic picture of the ΛCDM cosmology regarding the statistics of the initial conditions, with cosmic structures arising from adiabatic, passive, Gaussian, and primordial seed perturbations.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

Thermal Analysis for SRS Saltstone Disposal Unit Facility

Saltstone Disposal Units (SDU) are long term disposal units for low activity grout produced from the solidification of decontaminated non-hazardous salt waste at SRS. The unit is a cylindrical disposal vault of 150 ft. in diameter and 23 ft. in height. The total volume the SDU can hold is 3 million gallons of grout. The hydration process of the grout material produces heat from an exothermic chemical reaction. If the grout reaches temperatures higher than the maximum safety temperature of 95 deg. C, cracks can start forming leading to contamination of the environment. The purpose of this study is to develop the optimal baseline domain boundary conditions and to perform a sensitivity analysis with respect to the baseline modeling conditions. The following assumptions were made for the modeling calculations: - The system geometry is axisymmetric; - The system was at steady state; - Ambient temperature was set to 100 deg. F; - Air was assumed to be an incompressible ideal gas; - Radiation was neglected for a conservative estimation; - Natural convection for the SDU vapor space is assumed to be turbulent because Rayleigh number based on typical operating conditions is higher than 10{sup 8}; - Water tables were not taken into consideration. The following sensitivity analyses were performed to find the optimal domain boundary: - Mesh size sensitivity; - Soil depth sensitivity - Soil depth varied from 30 ft to 250 ft with a soil thickness of 90 ft; - Soil thickness sensitivity - Soil thickness varied from 30 ft to 270 ft with a soil depth of 180 ft; - Soil conductivity sensitivity - Soil thermal conductivity varied from 0.25 W/m-K to 1 W/m-K; - Ambient Temperature Sensitivity - Ambient temperature varied from 70 deg. F to 110 deg. F. For the thermal calculations, the temperature of the bottom of the soil was set to 17.4 deg. C. The heat flux on the roof of the building and surface of the earth is 163.2 W/m{sup 2}. The soil sides are set to be adiabatic. The sensitivity analysis shows that the mesh size has no effect on the numerical results. This is mainly due to a small convection zone and large conduction zones in the modeling domain. The optimal domain boundary was found to be a soil thickness of 90 ft and a soil depth of 150 ft. The different sensitivity analysis performed here shows the optimal boundary domain to be used for thermal calculations is a soil depth of 150 ft beneath the SDU and a soil thickness of 90 ft. Anything larger would produce similar solutions but at a longer computational time to solve. The maximum temperature was more sensitive to soil properties as shown here. While the ambient temperature affected the max temperature linearly. Most of the heat transfer takes place downward vertically between the SDU and the soil beneath it. Using the optimal domain boundary determined by the sensitivity analyses, the maximum thermal loading to keep the maximum grout temperature below 95 deg. C is 1.646 W/m{sup 3}.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2013

Transforming the representation of the boundary layer and low clouds for high-resolution regional climate modeling: Final report

Stratocumulus and shallow cumulus clouds in subtropical oceanic regions (e.g., Southeast Pacific) cover thousands of square kilometers and play a key role in regulating global climate (e.g., Klein and Hartmann, 1993). Numerical modeling is an essential tool to study these clouds in regional and global systems, but the current generation of climate and weather models has difficulties in representing them in a realistic way (e.g., Siebesma et al., 2004; Stevens et al., 2007; Teixeira et al., 2011). While numerical models resolve the large-scale flow, subgrid-scale parameterizations are needed to estimate small-scale properties (e.g. boundary layer turbulence and convection, clouds, radiation), which have significant influence on the resolved scale due to the complex nonlinear nature of the atmosphere. To represent the contribution of these fine-scale processes to the resolved scale, climate models use various parameterizations, which are the main pieces in the model that contribute to the low clouds dynamics and therefore are the major sources of errors or approximations in their representation. In this project, we aim to 1) improve our understanding of the physical processes in thermal circulation and cloud formation, 2) examine the performance and sensitivity of various parameterizations in the regional weather model (Weather Research and Forecasting model; WRF), and 3) develop, implement, and evaluate the advanced boundary layer parameterization in the regional model to better represent stratocumulus, shallow cumulus, and their transition. Thus, this project includes three major corresponding studies. We find that the mean diurnal cycle is sensitive to model domain in ways that reveal the existence of different contributions originating from the Southeast Pacific land-masses. The experiments suggest that diurnal variations in circulations and thermal structures over this region are influenced by convection over the Peruvian sector of the Andes cordillera, while the mostly dry mountain-breeze circulations force an additional component that results in semi-diurnal variations near the coast. A series of numerical tests, however, reveal sensitivity of the simulations to the choice of vertical grid, limiting the possibility of solid quantitative statements on the amplitudes and phases of the diurnal and semidiurnal components across the domain. According to our experiments, the Mellor-Yamada-Nakanishi-Niino (MYNN) boundary layer scheme and the WSM6 microphysics scheme is the combination of schemes that performs best. For that combination, mean cloud cover, liquid water path, and cloud depth are fairly wellsimulated, while mean cloud top height remains too low in comparison to observations. Both microphysics and boundary layer schemes contribute to the spread in liquid water path and cloud depth, although the microphysics contribution is slightly more prominent. Boundary layer schemes are the primary contributors to cloud top height, degree of adiabaticity, and cloud cover. Cloud top height is closely related to surface fluxes and boundary layer structure. Thus, our study infers that an appropriate tuning of cloud top height would likely improve the low-cloud representation in the model. Finally, we show that entrainment governs the degree of adiabaticity, while boundary layer decoupling is a control on cloud cover. In the intercomparison study using WRF single-column model experiments, most parameterizations show a poor agreement of the vertical boundary layer structure when compared with large-eddy simulation models. We also implement a new Total-Energy/Mass- Flux boundary layer scheme into the WRF model and evaluate its ability to simulate both stratocumulus and shallow cumulus clouds. Result comparisons against large-eddy simulation show that this advanced parameterization based on the new Eddy-Diffusivity/Mass-Flux approach provides a better performance than other boundary layer parameterizations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Entropy generation from hydrodynamic mixing in inertial confinement fusion indirect-drive targets

The increase in entropy from the physical mixing of two adjacent materials in inertial confinement fusion (ICF) implosions and gas-filled hohlraums is analytically assessed. An idealized model of entropy generation from the mixing of identical ideal-gas particles across a material interface in the presence of pressure and temperature gradients is applied. Physically, mix-driven entropy generation refers to the work done by the gases in expanding into a larger common volume from atomic mixing under the condition of no internal energy change, or work needed to restore the initial unmixed state. Furthermore, the effect of a mix-generated entropy increase is analytically shown to lead to less compression of the composite ICF fluid under adiabatic conditions. The amount of entropy generation is estimated to be ~10 J for a Rayleigh–Taylor-induced micrometer-scale annular mixing layer between the solid deuterium–tritium fuel and (undoped) high-density carbon pusher of an imploding capsule at the National Ignition Facility (NIF). This level of entropy generation is consistent with lower-than-expected fuel compressions measured on the NIF [Hurricane et al., Phys. Plasmas 26, 052704 (2019)]. The degree of entropy increase from mixing of high-Z hohlraum wall material and low-Z, moderate- to high-density gas fills is estimated to lead to ~100 kJ of heat generation for NIF-scale experiments [Moody et al., Phys. Plasmas 21, 056317 (2014)]. This value represents a significant fraction of the inferred missing x-ray drive energy based on observed delays in capsule implosion times compared with mainline simulations [Jones et al., Phys. Plasmas 19, 056315 (2012)].

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

General relativistic pulsations of ultra-massive ZZ Ceti stars

ABSTRACT Ultra-massive white dwarf stars are currently being discovered at a considerable rate, thanks to surveys such as the Gaia space mission. These dense and compact stellar remnants likely play a major role in Type Ia supernova explosions. It is possible to probe the interiors of ultra-massive white dwarfs through asteroseismology. In the case of the most massive white dwarfs, general relativity could affect their structure and pulsations substantially. In this work, we present results of relativistic pulsation calculations employing relativistic ultra-massive ONe-core white dwarf models with hydrogen-rich atmospheres and masses ranging from 1.29 to $1.369 \ \mathrm{M}_{\odot }$ with the aim of assessing the impact of general relativity on the adiabatic gravity (g)-mode period spectrum of very high mass ZZ Ceti stars. Employing the relativistic Cowling approximation for the pulsation analysis, we find that the critical buoyancy (Brunt–Väisälä) and acoustic (Lamb) frequencies are larger for the relativistic case, compared to the Newtonian case, due to the relativistic white dwarf models having smaller radii and higher gravities for a fixed stellar mass. In addition, the g-mode periods are shorter in the relativistic case than those in the Newtonian computations, with relative differences of up to ∼$50$ per cent for the highest mass models ($1.369 \ \mathrm{M}_{\odot }$) and for effective temperatures typical of the ZZ Ceti instability strip. Hence, the effects of general relativity on the structure, evolution, and pulsations of white dwarfs with masses larger than ∼$1.29 \ \mathrm{M}_{\odot }$ cannot be ignored in the asteroseismological analysis of ultra-massive ZZ Ceti stars.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2014

Novel concepts for the compression of large volumes of carbon dioxide-phase III

In the effort to reduce the release of CO 2 greenhouse gases to the atmosphere, sequestration of CO 2 from Integrated Gasification Combined Cycle (IGCC) and Oxy-Fuel power plants is being pursued. This approach, however, requires significant compression power to boost the pressure to typical pipeline levels. The penalty can be as high as 8-12% on a typical IGCC plant. The goal of this research is to reduce this penalty through novel compression concepts and integration with existing IGCC processes. The primary objective of the study of novel CO 2 compression concepts is to reliably boost the pressure of CO 2 to pipeline pressures with the minimal amount of energy required. Fundamental thermodynamics were studied to explore pressure rise in both liquid and gaseous states. For gaseous compression, the project investigated novel methods to compress CO 2 while removing the heat of compression internal to the compressor. The highpressure ratio, due to the delivery pressure of the CO 2 for enhanced oil recovery, results in significant heat of compression. Since less energy is required to boost the pressure of a cooler gas stream, both upstream and inter-stage cooling is desirable. While isothermal compression has been utilized in some services, it has not been optimized for the IGCC environment. Phase I of this project determined the optimum compressor configuration and developed technology concepts for internal heat removal. Other compression options using liquefied CO 2 and cryogenic pumping were explored as well. Preliminary analysis indicated up to a 35% reduction in power is possible with the new concepts being considered. In the Phase II program, two experimental test rigs were developed to investigate the two concepts further. A new pump loop facility was constructed to qualify a cryogenic turbopump for use on liquid CO 2 . Also, an internally cooled compressor diaphragm was developed and tested in a closed loop compressor facility using CO 2 . Both test programs successfully demonstrated good performance and mechanical behavior. In Phase III, a pilot compression plant consisting of a multi-stage centrifugal compressor with cooled diaphragm technology has been designed, constructed, and tested. Comparative testing of adiabatic and cooled tests at equivalent inlet conditions shows that the cooled diaphragms reduce power consumption by 3-8% when the compressor is operated as a back-to-back unit and by up to 9% when operated as a straight-though compressor with no intercooler. The power savings, heat exchanger effectiveness, and temperature drops for the cooled diaphragm were all slightly higher than predicted values but showed the same trends.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Communication: GAIMS—Generalized Ab Initio Multiple Spawning for both internal conversion and intersystem crossing processes

Full multiple spawning is a formally exact method to describe the excited-state dynamics of molecular systems beyond the Born-Oppenheimer approximation. However, it has been limited until now to the description of radiationless transitions taking place between electronic states with the same spin multiplicity. This Communication presents a generalization of the full and ab initio multiple spawning methods to both internal conversion (mediated by nonadiabatic coupling terms) and intersystem crossing events (triggered by spin-orbit coupling matrix elements) based on a spin-diabatic representation. The results of two numerical applications, a model system and the deactivation of thioformaldehyde, validate the presented formalism and its implementation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Quantum decoherence during inflation from gravitational nonlinearities

We study the inflationary quantum-to-classical transition for the adiabatic curvature perturbation ζ due to quantum decoherence, focusing on the role played by squeezed-limit mode couplings. We evolve the quantum state Ψ in the Schrödinger picture, for a generic cubic coupling to additional environment degrees of freedom. Focusing on the case of minimal gravitational interactions, we find the evolution of the reduced density matrix for a given long-wavelength fluctuation by tracing out the other (mostly shorter-wavelength) modes of ζ as an environment. We show that inflation produces phase oscillations in the wave functional Ψ[ζ(x)], which suppress off-diagonal components of the reduced density matrix, leaving a diagonal mixture of different classical configurations. Gravitational nonlinearities thus provide a minimal mechanism for generating classical stochastic perturbations from inflation. We identify the time when decoherence occurs, which is delayed after horizon crossing due to the weak coupling, and find that Hubble-scale modes act as the decohering environment. We also comment on the observational relevance of decoherence and its relation to the squeezing of the quantum state.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2018

Three-Dimensional, Space-Dependent Mesoscale Diffusivity: Derivation and Implications

Recently, we presented a parameterization of an arbitrary tracer 3D mesoscale flux that describes both diabatic and adiabatic regimes without using arbitrary tapering functions. However, we did not parameterize the mesoscale diffusivity, which is the subject of this work. A key difference between the present and previous diffusivity parameterizations is that in the latter, the two main ingredients, mesoscale drift velocity and eddy kinetic energy, were not parameterized but determined using present data, which deprives the models of predictive power. Since winds, stratification, etc., are predicted to change in the future, use of these parameterizations to study future climate scenarios becomes questionable. In this work, we parameterize drift velocity and eddy kinetic energy (vertical–horizontal components), which we first assess with data [WOCE, TOPEX/Poseidon (T/P), and North Atlantic Tracer Release Experiment (NATRE)] and then use in a coarse-resolution stand-alone ocean code under Coordinated Ocean-Ice Reference Experiment I (CORE-I) forcing. We present results for the global ocean temperature and salinity, Atlantic overturning circulation, meridional heat transport, and Drake Passage transport, which we compare with several previous studies. The temperature drift is less than that of five of seven previous OGCMs, and the salinity drift is among the smallest in those studies. The predicted winter Antarctic Circumpolar Current mixed layer depths (MLDs) are in good agreement with the data. Predicting the correct MLD is important in climate studies since models that predict very deep mixed layers transfer more of the radiative perturbation to the deep ocean, reducing surface warming (and vice versa).

Eddies; Mesoscale processes; Mixing; Ocean models;↗

DOE OSTI2022

Properties of the Prompt Optical Counterpart Arising from the Cooling of Electrons in Gamma-Ray Bursts

This work extends a contemporaneous effort to study the properties of the lower-energy counterpart synchrotron emission produced by the cooling of relativistic gamma-ray burst (GRB) electrons through radiation (synchrotron and self-Compton) emission and adiabatic losses. We derive the major characteristics (pulse duration, lag time after burst, and brightness relative to the burst) of the prompt optical counterpart (POC) occurring during or after the GRB. Depending on the magnetic field lifetime, duration of electron injection, and electron transit time Δt o from hard X-ray (GRB) to optical-emitting energies, a POC may appear during the GRB pulse (of duration δt γ ) or after (delayed OC). The signature of counterparts arising from the cooling of GRB electrons is that POC pulses (Δto < δtγ) last as long as the corresponding GRB pulse (δt o ≃ δt γ ), while delayed OC pulses (Δt o > δt γ ) last as long as the transit time (δt o ≃ Δt o ). If OC variability can be measured, then another signature for this OC mechanism is that the GRB variability is passed on to POCs but not to delayed OCs. Within the GRB electron cooling model for counterparts, POCs should be on average dimmer than delayed ones (consistent with the data), and harder GRB low-energy slopes β LE should be associated more often with the dimmer POCs. The latter sets an observational bias against detecting POCs from (the cooling of electrons in) GRBs with a hard slope β LE , making it more likely that the detected POCs of such bursts arise from another mechanism.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

All-electron molecular tunnel ionization based on the weak-field asymptotic theory in the integral representation

Tunnel ionization (TI) underlies many important ultrafast processes, such as high-harmonic generation andstrong-field ionization. Among the existing theories for TI, many-electron weak-field asymptotic theory (ME-WFAT) is by design capable of accurately treating many-electron effects in TI. An earlier version of ME-WFATrelied on an accurate representation of the asymptotic tail of the orbitals, which hindered its implementation inGaussian-basis-set-based quantum chemistry programs. In this work, we reformulate ME-WFAT in the integralrepresentation, which makes the quality of the asymptotic tail much less critical, hence greatly facilitating itsimplementation in standard quantum chemistry packages. The integral reformulation introduced here is thereforemuch more robust when applied to molecules with arbitrary geometry. Here, we present several case studies, amongwhich is the CO molecule where some earlier theories disagree with experiments. Here we find that ME-WFATproduces the largest ionization probability when the field points from C to O, as experiments suggest. Anattractive feature of ME-WFAT is that it can be used with various types of multielectron methods whether ofdensity functional or multiconfiguration types, this inturn facilitates tunnel ionization calculation in systems exhibiting a strong multireference character.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2014

Relaxation dynamics in quantum dissipative systems: The microscopic effect of intramolecular vibrational energy redistribution

We investigate the effect of inter-mode coupling on the vibrational relaxation dynamics of molecules in weak dissipative environments. The simulations are performed within the reduced density matrix formalism in the Markovian regime, assuming a Lindblad form for the system-bath interaction. The prototypical two-dimensional model system representing two CO molecules approaching a Cu(100) surface is adapted from an ab initio potential, while the diatom-diatom vibrational coupling strength is systematically varied. In the weak system-bath coupling limit and at low temperatures, only first order non-adiabatic uni-modal coupling terms contribute to surface-mediated vibrational relaxation. Since dissipative dynamics is non-unitary, the choice of representation will affect the evolution of the reduced density matrix. Two alternative representations for computing the relaxation rates and the associated operators are thus compared: the fully coupled spectral basis, and a factorizable ansatz. The former is well-established and serves as a benchmark for the solution of Liouville-von Neumann equation. In the latter, a contracted grid basis of potential-optimized discrete variable representation is tailored to incorporate most of the inter-mode coupling, while the Lindblad operators are represented as tensor products of one-dimensional operators, for consistency. This procedure results in a marked reduction of the grid size and in a much more advantageous scaling of the computational cost with respect to the increase of the dimensionality of the system. The factorizable method is found to provide an accurate description of the dissipative quantum dynamics of the model system, specifically of the time evolution of the state populations and of the probability density distribution of the molecular wave packet. The influence of intra-molecular vibrational energy redistribution appears to be properly taken into account by the new model on the whole range of coupling strengths. It demontrates that most of the mode mixing during relaxation is due to the potential part of the Hamiltonian and not to the coupling among relaxation operators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Randomized Adiabatic Quantum Linear Solver Algorithm with Optimal Complexity Scaling and Detailed Running Costs

Solving linear systems of equations is a fundamental problem with a wide variety of applications across many fields of science, and there is increasing effort to develop quantum linear solver algorithms. Subaşı et al. [Phys. Rev. Lett. 122, 060504 (2019)] proposed a randomized algorithm inspired by adiabatic quantum computing, based on a sequence of random Hamiltonian simulation steps, with suboptimal scaling in the condition number 𝜅 of the linear system and the target error 𝜖. Here we go beyond these results in several ways. Firstly, using filtering [Lin and Tong, Quantum 4, 361 (2020)] and Poissonization techniques [Cunningham and Roland, ArXiv:2406.03972 (2024)], the algorithm complexity is improved to the optimal scaling 𝑂⁡(𝜅⁢log (1/𝜖))—an exponential improvement in 𝜖, and a shaving of a log 𝜅 scaling factor in 𝜅. Secondly, the algorithm is further modified to achieve constant factor improvements, which are vital as we progress towards hardware implementations on fault-tolerant devices. We introduce a cheaper randomized walk operator method replacing Hamiltonian simulation—which also removes the need for potentially challenging classical precomputations; randomized routines are sampled over optimized random variables; circuit constructions are improved. We obtain a closed formula rigorously upper bounding the expected number of times one needs to apply a block-encoding of the linear system matrix to output a quantum state encoding the solution to the linear system. The upper bound is 837⁢𝜅 at 𝜖 = 10 −10 for Hermitian matrices.

97 MATHEMATICS AND COMPUTING↗