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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

On the Two-Phonon Relaxation of Excited States of Boron Acceptors in Diamond

The relaxation of holes from excited states of boron acceptors in diamond with the emission of two optical phonons is studied theoretically. To describe the wave function of acceptor states, an electron-like Hamiltonian with an isotropic effective mass is used. The wave function of the ground state is determined by the quantum-defect method. The probability of the transition is calculated in the adiabatic approximation. It is assumed that the phonon dispersion law is isotropic and the phonon frequency is quadratically dependent on the wave-vector modulus, with the maximum and minimum frequencies ω{sub max} and ω{sub min} at the center and boundary of the Brillouin zone, respectively. A high sensitivity of the probability of the transition to the characteristic of phonon dispersion ω{sub max} – ω{sub min} is revealed, especially for the transition with the energy E{sub T} in the range 2ℏω{sub min} ≤ E{sub T} < ℏω{sub min} + ℏω{sub max}. Depending on the energy of the transition and on the phonon dispersion, the two-phonon relaxation rate at the low-temperature limit varies from extremely small values (<10{sup 8} s{sup –1}) near the threshold E{sub T} = 2ℏω{sub min} to extremely large values (>10{sup 12} s{sup –1}) in the “resonance” range ℏω{sub min} + ℏω{sub max} ≤ E{sub T} ≤ 2ℏω{sub max}.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Spontaneous Exciton Collapse in a Strongly Flattened Ellipsoidal InSb Quantum Dot

Abstract Electronic and excitonic states in an InSb strongly flattened ellipsoidal quantum dot (QD) with complicated dispersion law are theoretically investigated within the framework of the geometric adiabatic approximation in the strong, intermediate, and weak quantum confinement regimes. For the lower levels of the spectrum, the square root dependence of energy on QD sizes is revealed in the case of Kane’s dispersion law. The obtained results are compared to the case of a parabolic (standard) dispersion law of charge carriers. The possibility of the accidental exciton instability is revealed for the intermediate quantum confinement regime. For the weak quantum confinement regime, the motion of the exciton's center-of-gravity is quantized, which leads to the appearance of additional Coulomb-like sub-levels. It is revealed that in the case of the Kane dispersion law, the Coulomb levels shift into the depth of the forbidden band gap, moving away from the quantum confined level, whereas in the case of the parabolic dispersion law, the opposite picture is observed. The corresponding selection rules of quantum transitions for the interband absorption of light are obtained. New selection rules of quantum transitions between levels conditioned by 2D exciton center of mass vertical motion quantization in a QD are revealed. The absorption threshold behavior characteristics depending on the QDs geometrical sizes are also revealed.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

WE-FG-206-06: Dual-Input Tracer Kinetic Modeling and Its Analog Implementation for Dynamic Contrast-Enhanced (DCE-) MRI of Malignant Mesothelioma (MPM)

Purpose: To use dual-input tracer kinetic modeling of the lung for mapping spatial heterogeneity of various kinetic parameters in malignant MPM Methods: Six MPM patients received DCE-MRI as part of their radiation therapy simulation scan. 5 patients had the epitheloid subtype of MPM, while one was biphasic. A 3D fast-field echo sequence with TR/TE/Flip angle of 3.62ms/1.69ms/15° was used for DCE-MRI acquisition. The scan was collected for 5 minutes with a temporal resolution of 5-9 seconds depending on the spatial extent of the tumor. A principal component analysis-based groupwise deformable registration was used to co-register all the DCE-MRI series for motion compensation. All the images were analyzed using five different dual-input tracer kinetic models implemented in analog continuous-time formalism: the Tofts-Kety (TK), extended TK (ETK), two compartment exchange (2CX), adiabatic approximation to the tissue homogeneity (AATH), and distributed parameter (DP) models. The following parameters were computed for each model: total blood flow (BF), pulmonary flow fraction (γ), pulmonary blood flow (BF-pa), systemic blood flow (BF-a), blood volume (BV), mean transit time (MTT), permeability-surface area product (PS), fractional interstitial volume (vi), extraction fraction (E), volume transfer constant (Ktrans) and efflux rate constant (kep). Results: Although the majority of patients had epitheloid histologies, kinetic parameter values varied across different models. One patient showed a higher total BF value in all models among the epitheloid histologies, although the γ value was varying among these different models. In one tumor with a large area of necrosis, the TK and ETK models showed higher E, Ktrans, and kep values and lower interstitial volume as compared to AATH and DP and 2CX models. Kinetic parameters such as BF-pa, BF-a, PS, Ktrans values were higher in surviving group compared to non-surviving group across most models. Conclusion: Dual-input tracer kinetic modeling is feasible in determining micro-vascular characteristics of MPM. This project was supported from Cycle for Survival and MSK Imaging and radiation science (IMRAS) grants.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

Simple expressions of the nuclear relaxation rate enhancement due to quadrupole nuclei in slowly tumbling molecules

For slowly tumbling entities or quasi-rigid lattices, we derive very simple analytical expressions of the quadrupole relaxation enhancement (QRE) of the longitudinal relaxation rate R{sub 1} of nuclear spins I due to their intramolecular magnetic dipolar coupling with quadrupole nuclei of arbitrary spins S ≥ 1. These expressions are obtained by using the adiabatic approximation for evaluating the time evolution operator of the quantum states of the quadrupole nuclei S. They are valid when the gyromagnetic ratio of the spin S is much smaller than that of the spin I. The theory predicts quadrupole resonant peaks in the dispersion curve of R{sub 1} vs magnetic field. The number, positions, relative intensities, Lorentzian shapes, and widths of these peaks are explained in terms of the following properties: the magnitude of the quadrupole Hamiltonian and the asymmetry parameter of the electric field gradient (EFG) acting on the spin S, the S-I inter-spin orientation with respect to the EFG principal axes, the rotational correlation time of the entity carrying the S–I pair, and/or the proper relaxation time of the spin S. The theory is first applied to protein amide protons undergoing dipolar coupling with fast-relaxing quadrupole {sup 14}N nuclei and mediating the QRE to the observed bulk water protons. The theoretical QRE agrees well with its experimental counterpart for various systems such as bovine pancreatic trypsin inhibitor and cartilages. The anomalous behaviour of the relaxation rate of protons in synthetic aluminium silicate imogolite nano-tubes due to the QRE of {sup 27}Al (S = 5/2) nuclei is also explained.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Communication: Vibrational and vibronic coherences in the two dimensional spectroscopy of coupled electron-nuclear motion

We theoretically investigate the photon-echo spectroscopy of coupled electron-nuclear quantum dynamics. Two situations are treated. In the first case, the Born-Oppenheimer (adiabatic) approximation holds. It is then possible to interpret the two-dimensional (2D) spectra in terms of vibrational motion taking place in different electronic states. In particular, pure vibrational coherences which are related to oscillations in the time-dependent third-order polarization can be identified. This concept fails in the second case, where strong non-adiabatic coupling leads to the breakdown of the Born-Oppenheimer-approximation. Then, the 2D-spectra reveal a complicated vibronic structure and vibrational coherences cannot be disentangled from the electronic motion.

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

Electron-Affinity Time-Dependent Density Functional Theory: Formalism and Applications to Core-Excited States

The lack of particle-hole attraction and orbital relaxation within time-dependent density functional theory (TDDFT) lead to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that uses optimized orbitals of the n - 1-electron system as the reference, building orbital relaxation and a proper hole into the initial density. Here, our approach is an exact generalization of the static-exchange approximation that ameliorates the particle-hole interaction error associated with the adiabatic approximation and reduces errors in TDDFT XAS by orders of magnitude. With a statistical performance of just 0.5 eV root-mean-square error and the same computational scaling as TDDFT under the core-valence separation approximation, we anticipate that this approach will be of great utility in XAS calculations of large systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Multiphonon Intracenter Relaxation of Boron Acceptor States in Diamond

The relaxation rates are calculated in the adiabatic approximation, in which the steady-state impurity states are taken to be electronic-vibrational (vibronic) states. The probabilities of transitions between these states with the emission (or absorption) of one or several phonons are calculated in first-order perturbation theory on the assumption that the transitions are a result of the violation of adiabaticity. The electron part of the wave function of the vibronic state is described by a simple Hamiltonian with an isotropic effective mass. The wave function of the ground state is determined by the quantum defect method. According to the calculations, a hole relaxes from the excited boron acceptor state, whose energy is 304 meV higher than the energy of the ground state, to the ground state with the emission of two optical phonons with a rate of ~10{sup 11} s{sup –1}. This value is an estimate from above, since the model of nondispersive optical phonons used in the study overestimates the number of phonon modes, whose participation in relaxation is allowed by the energy conservation law. However, despite the rough approximation, it can be concluded that the multiphonon relaxation of boron acceptor states in diamond is a fast process.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Thresholded quantum sensing with a frustrated Kitaev trimer

We investigate the response of a Ramsey interferometric quantum sensor based on a frustrated, three-spin system (a Kitaev trimer) to a classical time-dependent field (signal). The system eigenspectrum is symmetric about a critical point, |𝒃| = 0, with four of the spectral components varying approximately linearly with the magnetic field and four exhibiting a nonlinear dependence. Under the adiabatic approximation and for appropriate initial states, we show that the sensor's response to a zero-mean signal is such that below a threshold, |𝒃| <⁢ 𝑏 th , the sensor does not respond to the signal, whereas above the threshold, the sensor acts as a detector that the signal has occurred. This thresholded response is approximately omnidirectional. Moreover, when deployed in an entangled multisensor configuration, the sensor achieves sensitivity at the Heisenberg limit. Such detectors could be useful both as stand-alone units for signal detection above a noise threshold and in two- or three-dimensional arrays, analogous to a quantum bubble chamber, for applications such as particle track detection and long-baseline telescopy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Water dissociation on Ni(100), Ni(110), and Ni(111) surfaces: Reaction path approach to mode selectivity

We performed a comparative study of mode-selectivity of water dissociation on Ni(100), Ni(110), and Ni(111) surfaces at the same level of theory using a fully quantum approach based on the reaction path Hamiltonian. Calculations show that the barrier to water dissociation on the Ni(110) surface is significantly lower compared to its close-packed counterparts. Transition states for this reaction on all three surfaces involve the elongation of one of the O–H bonds. Furthermore, a significant decrease in the symmetric stretching and bending mode frequencies near the transition state is observed in all three cases and in the vibrational adiabatic approximation, excitation of these softened modes results in a significant enhancement in reactivity. Inclusion of non-adiabatic couplings between modes results in the asymmetric stretching mode showing a similar enhancement of reactivity as the symmetric stretching mode. Dissociation probabilities calculated at a surface temperature of 300 K showed higher reactivity at lower collision energies compared to that of the static surface case, underlining the importance of lattice motion in enhancing reactivity. Mode selective behavior is similar on all the surfaces. Molecules with one-quantum of vibrational excitation in the symmetric stretch, at lower energies (up to 0.45 eV), are more reactive on Ni(110) than the Ni(100) and Ni(111) surfaces. But, the dissociation probabilities approach saturation on all the surfaces at higher incident energy values. Ultimately, Ni(110) is found to be highly reactive toward water dissociation among the low-index nickel surfaces owing to a low reaction barrier resulting from the openness and corrugation of the surface. These results show that the mode-selective behavior does not vary with different crystal facets of Ni qualitatively, but there is a significant quantitative effect.

36 MATERIALS SCIENCE↗
NASA NTRS1973

On the improper neglect of certain terms in random function theory

This paper presents some exact solutions of problems in random function theory for the purpose of testing the validity of an approximate method known variously in the many different fields of its application as first order smoothing theory, first order cumulant discard, quasilinear theory, or the adiabatic approximation. The hydromagnetic dynamo equations are used here, as particularly appropriate for such an investigation. The calculations show that in one case the exact and approximate solutions agree. In the other case the approximate solution is wrong. Hence, in the absence of a general criterion for validity, a result based on first order smoothing theory is a conjecture rather than a fact. This impacts strongly on much of the recent work on hydromagnetic dynamos.

Lerche, I.↗
DOE OSTI2026

On the role of symmetry in quenching OH tunneling in 2,6-dimethylphenol

Here, we model the spectroscopy of the two methyl torsional degrees of freedom coupled to the OH torsional motion in 2,6-dimethylphenol. Recent gas-phase rotational transitions [Welsh et al ., J. Phys. Chem. Lett. 17 , 3749–3758 (2026)] have been interpreted to be the result of certain symmetry states of the methyl groups leading to the quenching of the OH torsional motion. Both a three-dimensional model and an adiabatic model, in which the OH torsion is treated as the slow mode, are developed to test these conjectures. Good agreement is found between the exact and approximate adiabatic models. The adiabatic model is developed to interpret and elucidate the key couplings leading to the quenching of the tunneling splitting.

Sibert, III, Edwin L. [Univ. of Wisconsin, Madison↗
DOE OSTI2017

Exact Time-Dependent Exchange-Correlation Potential in Electron Scattering Processes

We identify peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory that are crucial for time-resolved electron scattering in a model one-dimensional system. These structures are completely missed by adiabatic approximations that, consequently, significantly underestimate the scattering probability. A recently proposed nonadiabatic approximation is shown to correctly capture the approach of the electron to the target when the initial Kohn-Sham state is chosen judiciously, and it is more accurate than standard adiabatic functionals but ultimately fails to accurately capture reflection. These results may explain the underestimation of scattering probabilities in some recent studies on molecules and surfaces.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Changes in polarization dictate necessary approximations for modeling electronic deexcitation intensity: Application to x-ray emission

Accurate simulation of electronic excitations and deexcitations are critical for complementing complex spectroscopic experiments and can provide validation to theoretical approaches. Here, using a generalized framework, we contrast the accuracy and validity of orbital-constrained and linear-response approaches that build upon Kohn-Sham density functional theory (DFT) to simulate emission spectra of electronic origin and propose an efficient approximation, named many-body x-ray emission spectroscopy or MBXES, for simulating such processes. We show analytically as well as with computed examples that for electronic (de)excitation leading to an appreciable change in polarization (i.e., density rearrangement), the adiabatic approximation in a response-based formalism will be inadequate for the calculation of oscillator strength. Thus, such a change (e.g., in the net electrostatic dipole moment of a finite system) can be used as a metric for evaluating the applicability of the adiabatic response-based approach and can be particularly valuable in x-ray emission spectroscopy. On the other hand, MBXES, the flexible method introduced in this paper, can compute oscillator strengths accurately at a much lower computational expense on the basis of two DFT-based self-consistent field calculations. Using illustrative examples of emission spectra, the efficacy of the MBXES method is demonstrated by comparison with its parent theory, orbital-optimized DFT, and with experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Predominance of non-adiabatic effects in zero-point renormalization of the electronic band gap

Electronic and optical properties of materials are affected by atomic motion through the electron–phonon interaction: not only band gaps change with temperature, but even at absolute zero temperature, zero-point motion causes band-gap renormalization. We present a large-scale first-principles evaluation of the zero-point renormalization of band edges beyond the adiabatic approximation. For materials with light elements, the band gap renormalization is often larger than 0.3 eV, and up to 0.7 eV. This effect cannot be ignored if accurate band gaps are sought. For infrared-active materials, global agreement with available experimental data is obtained only when non-adiabatic effects are taken into account. They even dominate zero-point renormalization for many materials, as shown by a generalized Fröhlich model that includes multiple phonon branches, anisotropic and degenerate electronic extrema, whose range of validity is established by comparison with first-principles results.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Current-Induced Forces for Nonadiabatic Molecular Dynamics

We present general first-principles derivation of the expression for current-induced forces. The expression is applicable in nonequilibrium molecular systems with arbitrary intramolecular interactions and for any electron-nuclei coupling. It provides a controlled consistent way to account for quantum effects of nuclear motion around a classical trajectory, accounts for electronic non-Markov character of the friction tensor, and suggests a method for treatment beyond strictly adiabatic approximation. Lastly, we show the connection of the expression with previous studies and discuss effective ways to evaluate the friction tensor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Dynamics of the Mott to superfluid quantum phase transition in the truncated Wigner approximation

The quantum phase transition from the Mott insulator state to the superfluid in the Bose-Hubbard model is investigated. We research one, two and three dimensional lattices in the truncated Wigner approximation. We compute both kinetic and potential energy and they turn out to have a power law behaviour as a function of the transition rate, with the power equal to 1/3. The same applies to the total energy in a system with a harmonic trap, which is usually present in the experimental set-up. These observations are in agreement with the experiment of, where such scalings were also observed and the power of the decay was numerically close to 1/3. The results confirm the Kibble-Zurek (adiabatic-impulse-adiabatic approximation) scenario for this transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Magic Angles and Fractional Chern Insulators in Twisted Homobilayer Transition Metal Dichalcogenides

We explain the appearance of magic angles and fractional Chern insulators in twisted K-valley homobilayer transition metal dichalcogenides by mapping their continuum model to a Landau level problem. Here, our approach relies on an adiabatic approximation for the quantum mechanics of valence band holes in a layer-pseudospin field that is valid for sufficiently small twist angles and on a lowest Landau level approximation that is valid for sufficiently large twist angles. It provides a simple qualitative explanation for the nearly ideal quantum geometry of the lowest moir´e miniband at particular twist angles, predicts that topological flat bands occur only when the valley-dependent moir´e potential is sufficiently strong compared to the interlayer tunneling amplitude, and provides a convenient starting point for the study of interactions.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Sub-Doppler infrared spectroscopy of CH 2 OH radical in a slit supersonic jet: Vibration-rotation-tunneling dynamics in the symmetric CH stretch manifold

In this paper, the sub-Doppler CH-symmetric stretch (ν 3 ) infrared absorption spectrum of a hydroxymethyl (CH 2 OH) radical is observed and analyzed with the radical formed in a slit-jet supersonic discharge expansion (T rot = 18 K) via Cl atom mediated H atom abstraction from methanol. The high sensitivity of the spectrometer and reduced spectral congestion associated with the cooled expansion enable first infrared spectroscopic observation of hydroxymethyl transitions from both ± symmetry tunneling states resulting from large amplitude COH torsional motion. Nuclear spin statistics due to exchange of the two methyl H-atoms aid in unambiguous rovibrational assignment of two A-type K a = 0 ← 0 and K a = 1 ← 1 bands out of each ± tunneling state, with additional spectral information obtained from spin-rotation splittings in P, Q, and R branch K a = 1 ← 1 transitions that become resolved at low N. A high level ab initio potential surface (CCSD(T)-f12b/cc-pvnzf12 (n = 2,3)/CBS) is calculated in the large amplitude COH torsional and CH 2 wag coordinates, which in the adiabatic approximation and with zero point correction predicts ground state tunneling splittings in good qualitative agreement with experiment. Finally, of particular astrochemical interest, a combined fit of the present infrared ground state combination differences with recently reported millimeter-wave frequencies permits the determination of improved accuracy rotational constants for the ground vibrational state, which will facilitate ongoing millimeter/microwave searches for a hydroxymethyl radical in the interstellar medium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗