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At least 1,099 records · Page 61
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Transient Symmetry Controls Photo Dynamics near Conical Intersections

Excited-state chemistry lacks generalised symmetry rules. With many femtochemistry studies focused on individual cases, it is hard to build up the same level of chemical intuition for excited-states as exists for ground states. Here, we unravel the degrees of freedom involved in ultrafast internal conversion (IC) by mapping the vibrational coherence of the initial wavepacket, and the dependence on molecular symmetry in various cyclic tertiary amines. Molecular symmetry plays an important role in the preservation of vibrational coherence in the transit from one electronic state to another. We show here that it is sufficient for the molecule to simply have the possibility of a more symmetric structure to achieve the preservation of vibrational coherence. It can be transient and still lead to preservation. Furthermore, this finding provides an additional angle on how symmetry influences electronic transitions and an additional piece to the puzzle of establishing symmetry-based selection rules for excited-state processes.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Single-Molecule Charge Transport through Positively Charged Electrostatic Anchors

The charge transport in single-molecule junctions depends critically on the chemical identity of the anchor groups that are used to connect the molecular wires to the electrodes. In this research, we report a new anchoring strategy — called the electrostatic anchor here — formed through the efficient Coulombic interaction between the gold electrodes and the positively charged pyridinium terminal groups. Our results show that these pyridinium groups serve as efficient electrostatic anchors forming robust gold–molecule–gold junctions. Here, we have also observed binary switching in dicationic viologen molecular junctions, demonstrating an electron injection-induced redox switching in single-molecule junctions. We attribute the difference in low- and high conductance states to a dicationic ground state and a radical cationic metastable state, respectively. Overall, this anchoring strategy and redox switching mechanism could constitute the basis for a new class of redox-activated single-molecule switches.

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

Charge Delocalization and Vibronic Couplings in Quadrupolar Squaraine Dyes

Squaraines are prototypical quadrupolar charge-transfer chromophores that have recently attracted much attention as building blocks for solution-processed photovoltaics, fluorescent probes with large two-photon absorption cross sections, and aggregates with large circular dichroism. Their optical properties are often rationalized in terms of phenomenological essential state models, considering the coupling of two zwitterionic excited states to a neutral ground state. As a result, optical transitions to the lowest S 1 excited state are one-photon allowed, whereas the next higher S 2 state can only be accessed by two-photon transitions. A further implication of these models is a substantial reduction of vibronic coupling to the ubiquitous high-frequency vinyl-stretching modes of organic materials. Here, in this study, we combine time-resolved vibrational spectroscopy, two-dimensional electronic spectroscopy, and quantum-chemical simulations to test and rationalize these predictions for nonaggregated molecules. We find small Huang–Rhys factors below 0.01 for the high-frequency, 1500 cm –1 modes in particular, as well as a noticeable reduction for those of lower frequency modes in general for the electronic S 0 → S 1 transition. The two-photon allowed state S 2 is well separated energetically from S 1 and has weak vibronic signatures as well. Thus, the resulting pronounced concentration of the oscillator strength in a narrow region relevant to the lowest electronic transition makes squaraines and their aggregates exceptionally interesting for strong and ultrastrong coupling of excitons to localized light modes in external resonators with chiral properties that can largely be controlled by the molecular architecture.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Prominent radiative contributions from multiply-excited states in laser-produced tin plasma for nanolithography

Extreme ultraviolet (EUV) lithography is currently entering high-volume manufacturing to enable the continued miniaturization of semiconductor devices. The required EUV light, at 13.5 nm wavelength, is produced in a hot and dense laser-driven tin plasma. The atomic origins of this light are demonstrably poorly understood. Here we calculate detailed tin opacity spectra using the Los Alamos atomic physics suite ATOMIC and validate these calculations with experimental comparisons. Our key finding is that EUV light largely originates from transitions between multiply-excited states, and not from the singly-excited states decaying to the ground state as is the current paradigm. Moreover, we find that transitions between these multiply-excited states also contribute in the same narrow window around 13.5 nm as those originating from singly-excited states, and this striking property holds over a wide range of charge states. We thus reveal the doubly magic behavior of tin and the origins of the EUV light.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Collective excitations of a bound-in-the-continuum condensate

Spectra of low-lying elementary excitations are critical to characterize properties of bosonic quantum fluids. Usually these spectra are difficult to observe, due to low occupation of non-condensate states compared to the ground state. Recently, low-threshold Bose-Einstein condensation was realised in a symmetry-protected bound state in the continuum, at a saddle point, thanks to coupling of this electromagnetic resonance to semiconductor excitons. While it has opened the door to long-living polariton condensates, their intrinsic collective properties are still unexplored. Here we unveil the peculiar features of the Bogoliubov spectrum of excitations in this system. Thanks to the dark nature of the bound-in-the-continuum state, collective excitations lying directly above the condensate become observable in enhanced detail. We reveal interesting aspects, such as energy-flat parts of the dispersion characterized by two parallel stripes in photoluminescence pattern, pronounced linearization at non-zero momenta in one of the directions, and a strongly anisotropic velocity of sound.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Electronic properties of ThC − and ThC

The present study investigates the properties of low-lying states of ThC − and ThC using correlated wave function theories. To this end, we employed multireference calculations and various coupled-cluster approaches in combination with large correlation-consistent basis sets. These methods were applied to examine potential energy curves (PECs), electron configurations, energetics, spectroscopic constants, and spin–orbit coupling effects for 9 states of ThC − and 18 states of ThC. The ground states of ThC − and ThC were identified as single-reference 2 Σ + 1/2 (I) and $^3Σ^+_{0^-} (\textrm{I})$, respectively. Electron detachment from the 7s orbital of the Th center in ThC − [ 2 Σ + (I); 1σ 2 2σ1 3 σ2 1 π 4 ] yields ThC [ 3 Σ + (I); 1σ 2 2σ 1 3σ 1 1π 4 ]. The calculated adiabatic detachment energy (ADE) and vertical detachment energy (VDE) for this process are 1.591 and 1.604 eV, respectively. Furthermore, the dissociation energy (D 0 ) of ThC [$^3Σ^+_{0^-} (\textrm{I})$] is predicted to be 5.099 eV. The standard enthalpy of formation, $ΔH^{°}_{\textrm{f}}$ (298 K), of ThC is estimated to be 822.52 ± 6 kJ mol −1 .

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

First principles free energy model with dynamic magnetism for δ -plutonium

We present an ab initio free energy model derived from a fully relativistic density functional theory (DFT) electronic structure with dynamic magnetism for δ -plutonium (face-centered cubic, fcc). The DFT model is extended with orbital-orbital interaction in a parameter free orbital polarization (OP) mechanism consistent with previous modeling of plutonium. Gibbs free energy is built from components associated with the temperature dependence of the electronic structure and the corresponding electronic entropy, lattice vibrations within an anharmonic lattice dynamics model, and dynamical fluctuations of the magnetization density, i.e. magnetic fluctuations. The fluctuation model consists of transverse and longitudinal modes driven by temperature induced excitations of the DFT + OP electronic structure. The ab initio model thus incorporates fluctuating states beyond the electronic ground state. Thanks to the dynamic magnetism, the theory predicts excellent thermodynamic properties and a Gibbs free energy in accord with CALPHAD and semi-empirical modeling developed from the thermodynamic observables. The magnetic fluctuations further explain anomalous behaviors of the thermal expansion in plutonium. Specifically, a thermal expansion for the δ -plutonium system turning from positive to negative at temperatures above room temperature, a tendency for gallium to reduce and remove the negative thermal expansion depending on composition, and a positive thermal expansion for the high temperature ϵ phase.

dynamic↗
DOE OSTI2020

Electric and magnetic dipole strength in 112,114,116,118,120,124 Sn

Background: There is renewed interest in electric dipole strength distributions for a variety of reasons including the extraction of the dipole polarizability related to properties of the symmetry energy and a measure for the neutron skin thickness, understanding the structure of low-energy $\textit{E}$1 strength in nuclei with neutron excess, and establishing the systematics of the isovector giant dipole resonance (IVGDR). Inelastic proton scattering at energies of a few hundred MeV and very forward angles including 0° has been established as a tool for the study of electric and magnetic dipole strength distributions in nuclei. Purpose: The present work aims at a systematic investigation of the electric and magnetic dipole strength distributions in the chain of stable even-mass tin isotopes. Methods: Inelastic proton scattering experiments were performed at the Research Center for Nuclear Physics, Osaka, with a 295-MeV beam covering laboratory angles 0°–6° and excitation energies 6–22 MeV. Cross sections due to $\textit{E}$1 and $\textit{M}$1 excitations were extracted with a multipole decomposition analysis (MDA) and then converted to reduced transition probabilities with the “virtual photon method” for $\textit{E}$1 and the “unit cross section method” for $\textit{M}$1 excitations, respectively. Including a theory-aided correction for the high-excitation-energy region not covered experimentally, the electric dipole polarizability was determined from the $\textit{E}$1 strength distributions. Results: In this work, total photoabsorption cross sections derived from the $\textit{E}$1 and $\textit{M}$1 strength distributions show significant differences compared to those from previous ($\textit{γ, xn}$) experiments in the energy region of the IVGDR. The widths of the IVGDR deduced from the present data with a Lorentz parametrization show an approximately constant value of about 4.5 MeV in contrast to the large variations between isotopes observed in previous work. The IVGDR centroid energies are in good correspondence to expectations from empirical systematics of their mass dependence. Furthermore, a study of the dependence of the IVGDR energies on bulk matter properties is presented. The $\textit{E}$1 strengths below neutron threshold show fair agreement in this work with results from ($\textit{γ, γ'}$) experiments on 112,116,120,124 Sn in the energy region between 6 and 7 MeV, where also isoscalar $\textit{E}$1 strength was found for 124 Sn. At higher excitation energies, large differences are observed, pointing to a different nature of the excited states with small ground-state branching ratios. The isovector spin-$\textit{M}$1 strengths exhibit a broad distribution between 6 and 12 MeV in all studied nuclei. Conclusions: The present results contribute to the solution of a variety of nuclear structure problems including the systematics of the energy and width of the IVGDR, the structure of low-energy $\textit{E}$1 strength in nuclei, new constraints to energy density functionals (EDFs) aiming at a systematic description of the dipole polarizability across the nuclear chart, from which properties of the symmetry energy can be derived, and the systematics of the isovector spin-$\textit{M}$1 strength in heavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Production of $Υ(nS)$ mesons in Pb + Pb and $pp$ collisions at 5.02 TeV

A measurement of the production of vector bottomonium states, $Υ$(1S), $Υ$(2S), and $Υ$(3S), in Pb + Pb and $pp$ collisions at a center-of-mass energy per nucleon pair of 5.02 TeV is presented. The data correspond to integrated luminosities of 1.38 nb –1 of Pb + Pb data collected in 2018, 0.44 nb –1 of Pb + Pb data collected in 2015, and 0.26 fb –1 of $pp$ data collected in 2017 by the ATLAS detector at the Large Hadron Collider. The measurements are performed in the dimuon decay channel for transverse momentum ${p}_{T}^{μμ}$ < 30 GeV, absolute rapidity |$y^{μμ}$| < 1.5, and Pb + Pb event centrality 0–80%. The production rates of the three bottomonium states in Pb + Pb collisions are compared with those in $pp$ collisions to extract the nuclear modification factors as functions of event centrality, ${p}_{T}^{μμ}$, and $|y^{μμ}|$. In addition, the suppression of the excited states relative to the ground state is studied. The results are compared with theoretical model calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Oscillations and random walk of the soliton core in a fuzzy dark matter halo

We report that a fuzzy dark matter halo consists of a soliton core close to the center and a Navarro-Frenk-White–like density profile in the outer region. Previous investigations found that the soliton core exhibits temporal oscillations and random walk excursions around the halo center. Analyzing a set of numerical simulations, we show that both phenomena can be understood as the results of wave interference - a suitable superposition of the ground (solitonic) state and excited states in a fixed potential suffices to account for the main features of these phenomena. Such an eigenmode analysis can shed light on the evolution of a satellite halo undergoing tidal disruption. As the outer halo is stripped away, reducing the amplitudes of the excited states, the ground state evolves adiabatically. This suggests diminished soliton oscillations and random walk excursions, an effect to consider in deducing constraints from stellar heating.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Constant-Depth Preparation of Matrix Product States with Adaptive Quantum Circuits

Adaptive quantum circuits, which combine local unitary gates, midcircuit measurements, and feedforward operations, have recently emerged as a promising avenue for efficient state preparation, particularly on near-term quantum devices limited to shallow-depth circuits. Matrix product states (MPS) comprise a significant class of many-body entangled states, efficiently describing the ground states of one-dimensional gapped local Hamiltonians and finding applications in a number of recent quantum algorithms. Recently, it has been shown that the Affleck-Kennedy-Lieb-Tasaki state—a paradigmatic example of an MPS—can be exactly prepared with an adaptive quantum circuit of constant depth, an impossible feat with local unitary gates alone due to its nonzero correlation length [Smith , PRX Quantum 4, 020315 (2023)]. In this work, we broaden the scope of this approach and demonstrate that a diverse class of MPS can be exactly prepared using constant-depth adaptive quantum circuits, outperforming theoretically optimal preparation with unitary circuits. We show that this class includes short- and long-ranged entangled MPS, symmetry-protected topological (SPT) and symmetry-broken states, MPS with finite Abelian, non-Abelian, and continuous symmetries, resource states for MBQC, and families of states with tunable correlation length. Moreover, we illustrate the utility of our framework for designing constant-depth sampling protocols, such as for random MPS or for generating MPS in a particular SPT phase. We present sufficient conditions for particular MPS to be preparable in constant time, with global on-site symmetry playing a pivotal role. Altogether, this work demonstrates the immense promise of adaptive quantum circuits for efficiently preparing many-body entangled states and provides explicit algorithms that outperform known protocols to prepare an essential class of states. Published by the American Physical Society 2024

Smith, Kevin C. (ORCID:0000000223971518)↗
DOE OSTI2026

Loop series expansions for tensor networks

Belief propagation (BP) can be a useful tool to approximately contract a tensor network, provided that the contributions from any closed loops in the network are sufficiently weak. In this article, we describe how a loop series expansion can be applied to systematically improve the accuracy of a BP approximation to a tensor network contraction, in principle converging arbitrarily close to the exact result. More generally, our result provides a framework for expanding a tensor network as a sum of component networks in a hierarchy of increasing complexity. We benchmark this proposal for the contraction of infinite projected entangled pair states, either representing the ground state of an Affleck-Kennedy-Lieb-Tasaki (AKLT) model or with randomly defined tensors, where it is shown to improve in accuracy over standard BP by several orders of magnitude while incurring only a minor increase in computational cost. These results indicate that the proposed series expansions could be a useful tool to accurately evaluate tensor networks in cases that otherwise exceed the limits of established contraction routines.

Evenbly, Glen [AWS Center for Quantum Computing, P↗
DOE OSTI2025

Study of alpha-resonances in ¹¹B via the ⁷Li(⁷Li, t ) reaction

The near-threshold proton resonance in ¹¹B, recently identified and characterized through independent experi-ments, plays a crucial role in understanding the unexpectedly high decay branch observed in the β-delayed proton emission (β− p) from the neutron halo nucleus ¹¹Be. Critical to interpreting this process is the determination of whether or not this state has any significant α-decay width (rα). A coincidence measurement was conducted to study the alpha-transfer reaction ⁷Li(⁷Li, t ) ¹¹B∗ → ⁷Li +α employing the Super-Enge Split Pole Spectrograph coupled with a silicon detector at Florida State University. This experiment aimed to investigate the structure of α resonances in ¹¹B in the Eₑₓ = 9.0 MeV–14 MeV energy region. In particular, to explore and constrain the α-decay branch of the near-threshold proton resonance at Eₑₓ = 11.44 MeV. No significant α-decay strength was observed from this state. Additionally, the experimental results provided insights into the state at Eₑₓ = 12.55 MeV, previously proposed as the T = 3/2 isobaric analog state of the ¹¹Be ground state. The observed decay pattern, dominated by α + ⁷Li, suggests a strong T = 1/2 component, indicating the need for further experimental measurements.

Lopez-Saavedra, E.↗
NASA NTRS1978

Transport properties of monatomic carbon

Transport collision integrals for each of the 18 molecular C2 states that dissociate into ground state carbon atoms are presented. The integrals are obtained by fitting two-body semiempirical interaction potentials, for which the collision integrals are tabulated, to experimental and/or accurate theoretical calculations for each of these states. The collision integrals are applied to calculate the diffusion coefficient, viscosity, and translational contribution to the thermal conductivity of monatomic carbon at 1-atm pressure from 1000 K to 25,000 K. Because of ablation injection, monatomic carbon is an important flow field constituent of ablative flow during planetary entry, and knowledge of the transport properties for carbon species is required for calculating the flow field properties and surface heating.

Biolsi, L.↗
NASA NTRS1983

Monodeuterated methane in the outer solar system. I Spectroscopic analysis of the bands at 1.55 and 1.95 microns

The analysis of the near-infrared spectrum of monodeuterated methane (CH3D) near 6400/cm and 5100/cm is presented. Three new parallel bands which have locally perturbed upper states connecting with the ground state are identified, and approximate rotational constants are derived. The band centered near 6425/cm and the 9613 A band previously analyzed by Lutz, Danehy, and Ramsay (1978) are found to form an apparent vibrational progression with the nu2 fundamental at 2200/cm, and vibrational assignments of 3nu2 and 5nu2, respectively, are proposed. Detailed comparison of the rotational constants of the states involved is shown to support these assignments.

Lutz, B. L.↗
NASA NTRS1985

The internal state distribution of CN radicals produced in the photolysis of HC2CN and CH3CN

The energy partitioning in CN radicals produced by the vacuum ultraviolet photodissociation of HC2CN and CH3CN is studied by means of laser-induced fluorescence of the B-X transition. Experiments are performed in two collision regimes: (1) in the low-collision number regime, the energy partitioning in CN(X) is measured; (2) in the high-collision number regime, the formation of CN(A) is monitored. It is shown that photodissociation of HC2CN in its linear predissociative 1Sigma(+) state produces predominantly ground-state CN in rotationally and vibrationally excited states. The vibrational population ratios and the temperatures computed from a Boltzmann fit of the rotational levels are given in a table. The excitation of CH3CN produces CN radicals almost entirely in the first excited A-state with vibrational excitation.

Cody, R. J.↗
NASA NTRS1988

The computed spectrum of AlC

The low-lying (up to about 40,000/cm) doublet and quartet states of AlC have been studied at the CASSCF and MRCI levels of theory. The bonding in the X4Sigma(-) state is shown to involve three one-electron bonds. The first excited state, a 2Pi, lies about 8700/cm higher and like the X4Sigma(-) state is derived from ground state Al and C, but has a two-electron pi bond leading to a much shorter bond length.

Bauschlicher, Charles W., Jr.↗
NASA NTRS1988

The OI 989 and 1173 A multiplets in the dayglow

Sounding rocket measurements of the O-I 989-A dayglow obtained in 1978, 1980, and 1985 are discussed. The 989-A intensity and multiplet ratios are consistent with total branching losses (to atomic states other than the ground state) of 1.5-4 x 10 to the -4th. It is found that the 1173/989 intensity ratio is dependent only on the 1173/989 branching ratio and the atomic oxygen concentration when viewing upward from rocket altitudes.

Morrison, M. D.↗