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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Leveraging Intramolecular π-Stacking to Access an Exceptionally Long-Lived 3 MC Excited State in an Fe(II) Carbene Complex

The ability to manipulate excited-state decay cascades using molecular structure is essential to the application of abundant-metal photosensitizers and chromophores. Ligand design has yielded some spectacular results elongating charge-transfer excited state lifetimes of Fe(II) coordination complexes, but triplet metal-centered ( 3 MC) excited states - recently demonstrated to be critical to the photoactivity of isoelectronic Co(III) polypyridyls - have to date remained elusive, with temporally isolable examples limited to the picosecond regime. Here, with this report, we show how strong-field donors and intramolecular π-stacking can conspire to stabilize a long-lived 3 MC excited state for a remarkable 4.1 ± 0.3 ns in fluid solution at ambient temperature. Analysis of variable-temperature time-resolved absorption data using theoretical models ranging from Arrhenius to semiclassical Marcus theory, combined with computational modeling and X-ray crystallography, reveal a Jahn−Teller stabilized excited state with a high activation barrier for ground-state recovery. The net result is a chromophore with a 3 MC excited-state lifetime that is orders of magnitude longer than anything yet observed for an Fe(II) complex.

carbene compounds↗
DOE OSTI2024

Picosecond volume expansion drives a later-time insulator–metal transition in a nano-textured Mott insulator

There is significant technological interest in developing ever faster switching between different electronic and magnetic states of matter. Manipulating properties at terahertz rates requires accessing the intrinsic timescales of both electrons and associated phonons, which is possible with short-pulse photoexcitation. However, in many Mott insulators, the electronic transition is accompanied by the nucleation and growth of percolating domains of the changed lattice structure, leading to empirical timescales dominated by slowly coarsening dynamics. Here, in this study, we use time-resolved X-ray diffraction and reflectivity measurements to show that the photoinduced insulator-to-metal transition in an epitaxially strained Mott insulating thin film occurs without observable domain formation and coarsening effects, allowing the study of the intrinsic electronic and lattice dynamics. Above a fluence threshold, the initial electronic excitation drives a fast lattice rearrangement, which is followed by a slower electronic evolution into a metastable nonequilibrium state. Microscopic model calculations based on time-dependent dynamical mean-field theory and semiclassical lattice dynamics explain the threshold behaviour and elucidate the delayed onset of the electronic phase transition. This work highlights the importance of combined electronic and structural studies in unravelling the physics of dynamic transitions and the timescales of photoinduced processes. During a photoinduced phase transition, electronic rearrangements are usually faster than lattice ones. Time-resolved measurements now show that the insulator-to-metal transition in a thin-film Mott insulator is preceded by lattice reconfiguration.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Stress inside the pion in holographic light-front QCD

In this work, we propose a method to compute the gravitational form factor D ( Q 2 ) in holographic QCD by exploiting the remarkable correspondence between semiclassical light-front QCD and semiclassical field theories in wrapped spacetime in five dimensions. The use of light-front holography bridges physics at large Q 2 as attained in light-front QCD and physics at small Q 2 where the coupling to scalar and tensor fields, e.g. glueballs, are dominant. As an application, we compute the D -term for the pion and compare the results with recent lattice simulations. Published by the American Physical Society 2024

Astronomy & Astrophysics↗
DOE OSTI2022

Path Integrals for Nonadiabatic Dynamics: Multistate Ring Polymer Molecular Dynamics

This review focuses on a recent class of path-integral-based methods for the simulation of nonadiabatic dynamics in the condensed phase using only classical molecular dynamics trajectories in an extended phase space. Specifically, a semiclassical mapping protocol is used to derive an exact, continuous, Cartesian variable path-integral representation for the canonical partition function of a system in which multiple electronic states are coupled to nuclear degrees of freedom. Building on this exact statistical foundation, multistate ring polymer molecular dynamics methods are developed for the approximate calculation of real-time thermal correlation functions. As a result, the remarkable promise of these multistate ring polymer methods, their successful applications, and their limitations are discussed in detail.

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

First-Principles Calculations of Thermoelectric Transport Properties of Quaternary and Ternary Bulk Chalcogenide Crystals

Chalcogenide crystals have a wide range of applications, especially as thermoelectric materials for energy conversion. Thermoelectric materials can be used to generate an electric current from a temperature gradient based on the Seebeck effect and based on the Peltier effect, and they can be used in cooling applications. Using first-principles calculations and semiclassical Boltzmann theory, we have computed the Seebeck coefficient, electrical conductivity, electronic thermal conductivity, power factor, and figure of merit of 30 chalcogenide crystals. A Quantum Espresso package is used to calculate the electronic properties and locate the Fermi level. The transport properties are then calculated using the BoltzTraP code. The 30 crystals are divided into two groups. The first group has four crystals with quaternary composition (A 2 BCQ 4 ) (A = Tl; B = Cd, Hg; C = Si, Ge, Sn; Q = S, Se, Te). The second group contains 26 crystals with the ternary composition (A’B’Q 2 ) (A’ = Ag, Cu, Au, Na; B’ = B, Al, Ga, In; Q = S, Se, Te). Among these 30 chalcogenide crystals, the results for 11 crystals: Tl 2 CdGeSe 4 , Tl 2 CdSnSe 4 , Tl 2 HgSiSe 4 , Tl 2 HgSnS 4 , AuBSe 2 , AuBTe 2 , AuAlTe 2 , AuGaTe 2 , AuInTe 2 , AgAlSe 2 , and AgAlTe 2 are revealed for the first time. In addition, temperature-dependent transport properties of pure and doped AgSbSe 2 and AgSbTe 2 crystals with dopant compositions of AgSb 0.94 Cd 0.06 Te 2 and AgSbTe 1.85 Se 0.15 were explored. These results provide an excellent database for bulk chalcogenides crucial for a wide range of potential applications in renewable energy fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

Simplified Formulae System for Resonant Inverse Compton Scattering of a Fast Electron in an Intense Magnetic Field

We present simple analytical formulae for the emission spectrum and total power of a special kind of resonant inverse Compton scattering (RICS) of a relativistic electron in an intense magnetic field. In contrast with the available formulae system, we obtain a markedly simplified one based on the semiclassical quantum theory, which is more understandable for people who are unfamiliar with quantum electrodynamics. We show that the RICS process, under an appropriate 'accommodation condition' derived in this paper, is predominantly much more efficient than the coexistent ordinary inverse Compton scattering, and produces highly beamed high-frequency radiation with moderately good monochromaticity. Our formulae are simple to use - thus offering a lucid physical intuition for the theory - and may find wide applications in hard X-ray and gamma-ray astrophysics.

You, J. H.↗
NASA NTRS2015

Line Mixing in Parallel and Perpendicular Bands of CO2: A Further Test of the Refined Robert-Bonamy Formalism

Starting from the refined Robert-Bonamy formalism [Q. Ma, C. Boulet, and R. H. Tipping, J. Chem. Phys. 139, 034305 (2013)], we propose here an extension of line mixing studies to infrared absorptions of linear polyatomic molecules having stretching and bending modes. The present formalism does not neglect the internal degrees of freedom of the perturbing molecules, contrary to the energy corrected sudden (ECS) modeling, and enables one to calculate the whole relaxation matrix starting from the potential energy surface. Meanwhile, similar to the ECS modeling, the present formalism properly accounts for roles played by all the internal angular momenta in the coupling process, including the vibrational angular momentum. The formalism has been applied to the important case of CO2 broadened by N2. Applications to two kinds of vibrational bands (sigma yields sigma and sigma yields pi) have shown that the present results are in good agreement with both experimental data and results derived from the ECS model.

Semiclassical theories↗
NASA NTRS2017

Relaxation Matrix for Symmetric Tops with Inversion Symmetry: Line Coupling and Line Mixing Effects on NH3 Lines in the V4 Band

Line shape parameters including the half-widths and the off-diagonal elements of the relaxation matrix have been calculated for self-broadened NH3 lines in the perpendicular v4 band. As in the pure rotational and the parallel v1 bands, the small inversion splitting in this band causes a complete failure of the isolated line approximation. As a result, one has to use formalisms not relying on this approximation. However, due to differences between parallel and perpendicular bands of NH3, the applicability of the formalism used in our previous studies of the v1 band and other parallel bands must be carefully verified. We have found that, as long as potential models only contain components with K1 equals K2 equals 0, whose matrix elements require the selection rule delta k equals 0, the formalism is applicable for the v4 band with some minor adjustments. Based on both theoretical considerations and results from numerical calculations, the non-diagonality of the relaxation matrices in all the PP, RP, PQ, RQ, PR, and RR branches is discussed. Theoretically calculated self-broadened half-widths are compared with measurements and the values listed in HITRAN 2012. With respect to line coupling effects, we have compared our calculated intra-doublet off-diagonal elements of the relaxation matrix with reliable measurements carried out in the PP branch where the spectral environment is favorable. The agreement is rather good since our results do well reproduce the observed k and j dependences of these elements, thus validating our formalism.

Absorption coefficient↗
DOE OSTI2025

Quantum Aspects of Natural Top Quark Condensation

In top quark condensation the Brout-Englert-Higgs (BEH) boson is a $\bar{t}t$ bound state. With a UV completion of a single coloron exchange interaction, a recent semiclassical treatment gave a novel theory of the BEH boson as an extended object with composite scale $M_0\sim 6$ TeV. Presently we obtain the semiclassical theory as an effective action, using the source/Legendre transformation techniques of Jackiw, \etal, and fermion loop effects in the large-$N_c$ limit by deploying an auxiliary field to implement the sum of leading fermion loop diagrams. The theory remains natural at the loop level, with fine tuning at the level of a few %, and the effective coupling of the 4-fermion interaction, $\bar{g}_0^2$, is significantly enhanced by quantum loops over the fundamental coloron coupling, $g_0^2$. Hence a relatively weaker ``topcolor'' theory can produce critical coupling in the effective BEH bound state theory.

Hill, Christopher T. [Fermilab; Wisconsin U., Madi↗
NASA NTRS1977

Transformation theory and translation factors in inelastic atomic collisions

It is shown through the use of transformation theory that unique semiclassical atomic scattering states which obey the asymptotic conditions of formal scattering theory can be derived by transforming 'nontraveling' atomic states, ie., states whose coordinate variables are referred to a stationary origin, to frames at rest with respect to the incoming or outgoing particles. An overview of the problem of properly defining such scattering states is presented. The operator which carries out the necessary transformation from inertial to noninertial frames is derived and its properties are discussed. The relation of this transformation operator to the 'translation factor' discussed in the literature is presented. The application of this operator to transform the time-dependent Schroedinger equation from an inertial to a noninertial frame is presented and shown to introduce new terms in the resulting equation. The implications of these new terms to scattering problems are discussed.

Schmid, G. B.↗
DOE OSTI2025

First-Principles Studies on Sc 2 RuZ (Z = Si, Ge, Sn) Inverse Heusler Alloys: Structural, Electronic, and Transport Properties

The continuous demand for efficient, nontoxic, and thermally stable materials for room-temperature energy conversion motivates the exploration of novel thermoelectric systems beyond the traditional magnetic Heusler alloys. While full and half-Heusler compounds, especially Co-, Ni-, and Mn-based systems, have demonstrated promising thermoelectric properties, their typically high operating temperatures and magnetic complexities limit their applicability in ambient thermal management. In this context, we investigate whether Sc-based inverse Heusler alloys can offer a viable nonmagnetic alternative with competitive thermoelectric performance. In this work, we perform a systematic first-principles study of the inverse Heusler compounds Sc 2 RuZ (Z = Si, Ge, Sn), focusing on their structural, electronic, mechanical, and thermodynamic-thermoelectric properties. Density Functional Theory (DFT) was employed to compute optimized lattice structures and band dispersion, while dynamical stability was assessed via phonon calculations. Thermoelectric transport coefficients, including Seebeck coefficient, electrical conductivity, and thermal conductivity, were estimated using the semiclassical Boltzmann transport theory within the constant relaxation time approximation. Our results show that all Sc 2 RuZ compounds are thermodynamically stable semiconductors with indirect band gaps of 0.12–0.16 eV and exhibit high elastic moduli, especially Sc 2 RuSn, which demonstrates superior stiffness and incompressibility. Importantly, all compounds display promising room-temperature thermoelectric characteristics, including high Seebeck coefficients and power factors. These findings reveal that Sc 2 RuZ alloys represent a rare class of stable, nonmagnetic inverse Heusler semiconductors with intrinsic thermoelectric potential at room temperature, unlike many existing Heusler systems optimized for spintronics or high-temperature operation. This work expands the known design space for Heusler-based thermoelectrics and offers a theoretical basis for experimental realization of efficient, low-temperature, nonmagnetic thermoelectric materials.

alloys↗
DOE OSTI2024

Chiral kinematic theory and converse vortical effects

Response theories in condensed matter typically describe the response of an electron fluid to external electromagnetic fields, while perturbations on neutral particles are often designed to mimic such fields. Here, we study the response of fermions to a space-time-dependent velocity field, thereby sidestepping the issue of gauge charge. First, we use a semiclassical chiral kinematic theory to obtain the local density of current and extract the orbital magnetization. The theory immediately predicts a "converse vortical effect," defined as an orbital magnetization driven by linear velocity. It receives contributions from magnetic moments on the Fermi surface and the Berry curvature of the occupied bands. Then, transcending semiclassics via a complementary Kubo formalism reveals that the uniform limit of a clean system receives only the Berry curvature contribution while other limits sense the Fermi surface magnetic moments too. We propose CoSi as a candidate material and suggest magnetometry of a sample under a thermal gradient to detect the effect. Overall, our study sheds light on the effects of a space-time-dependent velocity field on electron fluids and paves the way for exploring quantum materials using new probes and perturbations.

Chen, Kai↗
NASA NTRS1985

Calculation of pressure-broadened linewidths for CO in Ar

Calculations of the pressure-broadening cross sections of CO in Ar have been made within the infinite-order sudden (IOS) and coupled states (CS) quantum scattering approximations. Two intermolecular potentials were used, a pairwise additive atom-atom potential which has been employed previously in semiclassical (modified Anderson theory) studies of this system and one calculated ab initio within an electron gas formalism. Predictions from the two potentials generally agree within about 25 percent and bracket experimental values (except for some recent high temperature data obtained in shock tube experiments). The CS approximation appears to be quite accurate although computationally expensive. The much cheaper IOS approximation is accurate for the J = 0-1 line but does not properly predict the dependence on line number. The quantum results are also compared with earlier semiclassical values.

Green, S.↗
DOE OSTI2024

Null states and time evolution in a toy model of black hole dynamics

Abstract Spacetime wormholes can provide non-perturbative contributions to the gravitational path integral that make the actual number of statese S in a gravitational system much smaller than the number of states$$ {e}^{S_{\textrm{p}}} $$ e S p predicted by perturbative semiclassical effective field theory. The effects on the physics of the system are naturally profound in contexts in which the perturbative description actively involvesN=O(e S ) of the possible$$ {e}^{S_{\textrm{p}}} $$ e S p perturbative states; e.g., in late stages of black hole evaporation. Such contexts are typically associated with the existence of non-trivial quantum extremal surfaces. However, by forcing a simple topological gravity model to evolve in time, we find that such effects can also have large impact forN≪e S (in which case no quantum extremal surfaces can arise). In particular, even for smallN, the insertion of generic operators into the path integral can cause the non-perturbative time evolution to differ dramatically from perturbative expectations. On the other hand, this discrepancy is small for the special case where the inserted operators are non-trivial only in a subspace of dimensionD≪e S . We thus study this latter case in detail. We also discuss potential implications for more realistic gravitational systems.

Physics↗
DOE OSTI2022

Level density within a micro-macroscopic approach

Statistical level density $ρ$($E, A$) is derived for nucleonic system with a given energy $E$, particle number $A$ and other integrals of motion in the micro-macroscopic approximation beyond the standard saddle-point method of the Fermi gas model. This level density reaches the two limits; the well-known Fermi gas grand-canonical ensemble limit for a large entropy $S$ related to large excitation energies, and the finite micro-canonical limit for a small combinatorical entropy $S$ at low excitation energies. In conclusion, the inverse level density parameter $K$ as function of the particle number $A$ in the semiclassical periodic orbit theory, taking into account the extended Thomas-Fermi and Strutinsky shell corrections, is calculated and compared with experimental data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Microscopic-macroscopic level densities for low excitation energies

Level density ρ(E,Q) is derived within the micro-macroscopic approximation (MMA) for a system of strongly interacting Fermi particles with the energy E and additional integrals of motion Q , in line with several topics of the universal and fruitful activity of A. S. Davydov. Within the extended Thomas Fermi and semiclassical periodic orbit theory beyond the Fermi-gas saddle-point method, we obtain ρ ∝ I ν (S)/S ν , where I ν (S) is the modified Bessel function of the entropy S . For small shell-structure contribution, one finds ν = κ/2 + 1, where κ is the number of additional integrals of motion. This integer number is a dimension of Q, Q = { N, Z , …} for the case of two-component atomic nuclei, where N and Z are the numbers of neutrons and protons, respectively. For much larger shell structure contributions, one obtains ν = κ /2 + 2. The MMA level density ρ reaches the well-known Fermi gas asymptote for large excitation energies and the finite micro-canonical combinatoric limit for low excitation energies. Further, the additional integrals of motion can also be the projection of the angular momentum of a nuclear system for nuclear rotations of deformed nuclei, number of excitons for collective dynamics, and so on. Fitting the MMA total level density ρ( E , Q) for a set of the integrals of motion Q = { N, Z }, to experimental data on a long nuclear isotope chain for low excitation energies, one obtains the results for the inverse level-density parameter K , which differs significantly from those of neutron resonances due to shell, isotopic asymmetry, and pairing effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS1973

Proton collisional excitation in the ground configuration of Fe/+12/.

Using semiclassical Coulomb excitation theory, proton collisional excitation and deexcitation cross sections are calculated for all transitions between the Fe(+12) ground configuration levels. Rate constants pertaining to these processes are then derived for coronal temperatures. These rates are shown to be comparable in all cases to the corresponding electron rate constants.

Landman, D. A.↗