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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Efficient simulation of open quantum systems coupled to a reservoir through multiple channels

It is challenging to simulate open quantum systems that are connected to a reservoir through multiple channels. For example, vibrations may induce fluctuations in both energy gaps and electronic couplings, which represent two independent channels of system–bath couplings. Systems of this kind are ubiquitous in the processes of excited state radiationless decay. Combined with density matrix renormalization group (DMRG) and matrix product states (MPS) methods, we develop an interaction-picture chain mapping strategy for vibrational reservoirs to simulate the dynamics of these open systems, resulting in time-dependent spatially local system–bath couplings in the chain-mapped Hamiltonian. This transformation causes the entanglement generated by the system–bath interactions to be restricted within a narrow frequency window of vibrational modes, enabling efficient DMRG/MPS dynamical simulations. We demonstrate the utility of this approach by simulating singlet fission dynamics using a generalized spin-boson Hamiltonian with both diagonal and off-diagonal system–bath couplings. This approach generalizes an earlier interaction-picture chain mapping scheme, allowing for efficient and exact simulation of systems with multi-channel system–bath couplings using matrix product states, which may further our understanding of nonlocal exciton–phonon couplings in exciton transport and the non-Condon effect in energy and electron transfer.

Chemistry↗
NASA NTRS1987

Full CI benchmark calculations for several states of the same symmetry

Full CI (FCI) wave functions are used to compute energies for several electronic states of the same symmetry for SiH2, CH2, and CH2(+). It is found that CASSCF/multireference CI wave functions yield results very similar to FCI, irrespective of whether the CASSCF MOs are optimized independently for each state or using an average of the CASSCF energies for all desired states. The ionization potentials and excitation energies obtained from the FCI calculations should help calibrate methods (such as Green's function approaches, equations of motion and propagator methods, and cluster expansions) in which energy differences are computed directly.

Bauschlicher, Charles W., Jr.↗
NASA NTRS1988

Nonlinear modeling, identification and estimation of slew induced structural deformation

This proposal discusses a new nonlinear, nonparametric method for off-line modeling and on-line estimation of the deformation of a flexible structure undergoing rapid retargeting maneuvers. In these circumstances, the structural stiffness and damping coefficients depend on the angular acceleration omega(dot), the angular rate omega, and the square of the angular rate omega. In the single axis case, the excitation of the structure is represented by the vector u(exp T) = (omega(dot), omega(exp 2), 2(omega)), to which the structural dynamics responds as a 'bilinear' (i.e., parametrically excited) system. A similar technique for multiaxial rotations yields a bilinear model with respect to matrix valued excitations. Three methods of estimation and modeling are described in this proposal to achieve deformation state determination: (1) a method based on a feedback linearized procedure which gives an estimate of the state by means of observers installed in the deformable body; (2) off-line modeling of the deformation state of the structure by means of topological interpolators; and (3) an on-line structural state estimation method based on a combination of the two previous techniques.

Dwyer, Thomas A., III↗
DOE OSTI2025

Design of facilitated dissociation enables timing of cytokine signalling

Protein design has focused on the design of ground states, ensuring that they are sufficiently low energy to be highly populated. Designing the kinetics and dynamics of a system requires, in addition, the design of excited states that are traversed in transitions from one low-lying state to another. This is a challenging task because such states must be sufficiently strained to be poorly populated, but not so strained that they are not populated at all, and because protein design methods have focused on generating near-ideal structures. Here we describe a general approach for designing systems that use an induced-fit power stroke to generate a structurally frustrated and strained excited state, allosterically driving protein complex dissociation. X-ray crystallography, double electron–electron resonance spectroscopy and kinetic binding measurements show that incorporating excited states enables the design of effector-induced increases in dissociation rates as high as 5,700-fold. We highlight the power of this approach by designing rapid biosensors, kinetically controlled circuits and cytokine mimics that can be dissociated from their receptors within seconds, enabling dissection of the temporal dynamics of interleukin-2 signalling.

deformation dynamics↗
DOE OSTI2025

Control of wakefield in sub-THz dielectric-lined waveguides using multiple-bunch excitation

Beam-driven wakefield accelerators offer the potential to achieve accelerating fields approaching the sub-GV/m range, paving the way for compact and cost-effective next-generation high-energy colliders. This method typically employs a two-bunch system: a drive bunch that excites an electromagnetic wakefield in a solid-state or plasma medium, and a witness bunch that extracts energy from the wake for acceleration. Our research focuses on two key challenges in wakefield acceleration using structures. First, we investigate strategies to suppress transverse instabilities by employing non-cylindrical geometries that damp dipole modes. Second, we explore methods to precisely terminate the wakefield after the interaction region, thereby improving the efficiency of energy transfer. This paper presents detailed simulation results and the corresponding experimental design developed to validate these concepts. Furthermore, the proposed experiment will be carried out at the Argonne Wakefield Accelerator (AWA) facility, focusing on controlling wakefield duration through tailored drive and witness bunch configurations and evaluating dielectric-lined structures with non-cylindrical cross sections.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

A lumped particle direct simulation Monte-Carlo method combined with the collisional-radiative model for simulations of non-equilibrium laser-induced plasma plumes

Collisional plasma plumes induced by laser irradiation of material targets exhibit large variations in local density as well as ionization and excitation states, making purely hydrodynamic or kinetic simulations inaccurate or infeasible. To address this challenge and capture non-equilibrium effects in laser-induced plasma plumes at arbitrary degrees of ionization, we develop a hybrid computational approach that combines the kinetic direct simulation Monte Carlo (DSMC) method with a collisional-radiative model (CRM). This ℓDSMC-CRM approach utilizes a lumped particle method to represent minor fractions of excited ions in particle-based simulations and a special coarse-graining technique for atomic spectra and photoionization rates, ensuring numerical convergence at reduced computational cost. The hybrid approach is applied to simulate spatially homogeneous relaxation as well as one- and two-dimensional expansions of plasma plumes induced by irradiation of a copper target by a nanosecond laser pulse in a vacuum or background gas. The comparison with an equilibrium model, where local Saha-Boltzmann equilibrium is enforced, shows that the non-equilibrium effects play a dominant role. The equilibrium model can fail to predict the flow structure and strongly underestimate the degree of absorption of laser radiation by the plume. The ℓDSMC-CRM approach is validated against experimental data demonstrating reasonable agreement with the experimental electron density and temperature, while the equilibrium model is found to dramatically underestimate electron density and temperature. The flexibility of the ℓDSMC-CRM approach allows for its seamless integration into existing DSMC frameworks, making it a valuable tool for high-fidelity plasma modeling in laser-material interactions, laser-based manufacturing, and beyond.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Excited electronic states of Na 2 and K 2 : The potential for long-lived “reservoir” states leading to collision induced population inversions

Potential energy curves (PECs) for the spin-free (ΛS) and spin–orbit (Ω) states associated with the four lowest-lying dissociation channels of Na 2 and K 2 were calculated at the SA-CASSCF/SO-CASPT2/aug-cc-pwCVQZ-DK level. The PECs of Na 2 were consistent with the experimental data and with the FS-CCSD (2,0) calculations, reproducing the double-well and the “shelf” character for some of the potentials of the excited states. For K 2 , the PECs behaved in a similar way and the spectroscopic parameters for the ground and the excited states are in good agreement with the available experimental values. The dissociation energy of K 2 was predicted to be D e = 4454 cm −1 , within an agreement of 5 cm −1 with the experiments. For Na 2 , D e = 5789 cm −1 compared to the experimental value of 6022 cm −1 . The inclusion of spin–orbit coupling effects resulted in avoided crossings, which affect the PECs. Spin–orbit changes the predicted curves for some excited Ω states arising from ΛS states that overlap each other, affecting their associated vibrational frequencies and bond distances. Here, the current studies of the low-lying states in K 2 reveal a similar structure to those of Na 2 , which suggests the accessibility of long-lived energy storing reservoir states and possible population inversions in K 2 following prior experimental work on the reaction of halogen atoms with Na 3 to produce excited states of Na 2 .

Ab-initio methods↗
NASA NTRS1975

Douglas Experience in Flight Flutter Testing

Douglas Aircraft Company experience in flight flutter testing is reviewed briefly, with comments on state-of-the-art excitation and instrumentation techniques used up to the present time. The limitations of previous techniques are discussed with emphasis on the problem of: (1) establishing a flutter margin of safety for predicted marginal flutter modes; (2) resolving instances of flutter not predicted by theoretical calculations in advance; and (3) delaying the airplane demonstration by time consumed in acquisition and reduction of flutter data. Current Douglas philosophy in flight flutter testing is presented and a description given of steady-state vane excitation system development, automatic data handling system, and the potential application of automatic computing methods for increasing flutter data yield.

Philbrick, J.↗
NASA NTRS1989

A fully-coupled implicit method for thermo-chemical nonequilibrium air at sub-orbital flight speeds

A CFD technique is described in which the finite-rate chemistry in thermal and chemical nonequilibrium air is fully and implicitly coupled with the fluid motion. Developed for use in the suborbital hypersonic flight speed range, the method accounts for nonequilibrium vibrational and electronic excitation and dissociation, but not ionization. The steady-state solution to the resulting system of equations is obtained by using a lower-upper factorization and symmetric Gauss-Seidel sweeping technique through Newton iteration. Inversion of the left-hand-side matrices is replaced by scalar multiplications through the use of the diagonal dominance algorithm. The code, named CENS2H (Compressible-Euler-Navier-Stokes Two-Dimensional Hypersonic), is fully vectorized and requires about 8.8 x 10 to the -5th sec per node point per iteration using a Cray X-MP computer. Converged solutions are obtained after about 2400 iterations. Sample calculations are made for a circular cylinder and a 10 percent airfoil at 5 deg angle of attack. The calculated cylinder flow field agrees with that obtained experimentally. The code predicts a 10 percent change in lift, drag, and pitching moment for the airfoil due to the thermochemical phenomena.

Park, Chul↗
NASA NTRS1992

Numerical simulations of non-equilibrium shock layers with efficient implicit schemes

Current and future calculations of nonequilibrium shock layers require the use of a very large number of equations, due to a multiplicity of chemical species, excited states, and internal energy modes. The computational cost associated with the use of standard implicit methods becomes prohibitive; it is therefore desirable to examine the potential of several methods and determine if any can be projected to be more efficient and accurate for large systems of equations. Here, the performance of several implicit schemes on several simple practical examples of reacting flows is examined. The Euler equations are solved by three different implicit methods, and two methods of coupling between the fluid dynamics and the chemistry are studied. Several cases of stiffness are considered and both 1D and 2D examples are computed.

Cambier, Jean-Luc↗
NASA NTRS1994

Theoretical Study of the Low-Lying States of MgN+2

The structure and binding energies of the low-lying states of MgN2+ have been computed at the multireference configuration interaction level of theory. The effect of Mg inner-shell correlation have been included using the core-polarization potential method. The charge-quadrupole interaction results in a linear 2Sigma+ ground state as expected. The excited states can arise from either the interaction of the 2-P state of Mg+ with N2 or from charge transfer states with Mg(sup 2+)N2- bonding character. The lowest lying excited state, 2-B2, is mixture of these two mechanisms, which results in a C2v, geometry with Mg atoms sitting at the N2 bond midpoint. The small barrier in the bending potential exists between this state and the 2-II State which is the lowest lying linear excited state.

Maitre, Philippe↗
NASA NTRS2006

Adjoint-Based Algorithms for Adaptation and Design Optimizations on Unstructured Grids

Schemes based on discrete adjoint algorithms present several exciting opportunities for significantly advancing the current state of the art in computational fluid dynamics. Such methods provide an extremely efficient means for obtaining discretely consistent sensitivity information for hundreds of design variables, opening the door to rigorous, automated design optimization of complex aerospace configuration using the Navier-Stokes equation. Moreover, the discrete adjoint formulation provides a mathematically rigorous foundation for mesh adaptation and systematic reduction of spatial discretization error. Error estimates are also an inherent by-product of an adjoint-based approach, valuable information that is virtually non-existent in today's large-scale CFD simulations. An overview of the adjoint-based algorithm work at NASA Langley Research Center is presented, with examples demonstrating the potential impact on complex computational problems related to design optimization as well as mesh adaptation.

Nielsen, Eric J.↗
DOE OSTI2024

Excited state electronic structure of dimethyl disulfide involved in photodissociation at ∼200 nm

Dimethyl disulfide (DMDS), one of the smallest organic molecules with an S–S bond, serves as a model system for understanding photofragmentation in polypeptides and proteins. Prior studies of DMDS photodissociation excited at ∼266 nm and ∼248 nm have elucidated the mechanisms of S–S and C–S bond cleavage, which involve the lowest excited electronic states S 1 and S 2 . Far less is known about the dissociation mechanisms and electronic structure of relevant excited states of DMDS excited at ∼200 nm. Herein we present calculations of the electronic structure and properties of electronic states S 1 –S 6 accessed when DMDS is excited at ∼200 nm. Our analysis includes a comparison of theoretical and experimental UV spectra, as well as theoretically predicted one-dimensional cuts through the singlet and triplet potential energy surfaces along the S–S and C–S bond dissociation coordinates. Finally, we present calculations of spin–orbit coupling constants at the Franck–Condon geometry to assess the likelihood of ultrafast intersystem crossing. We show that choosing an accurate yet computationally efficient electronic structure method for calculating the S 0 –S 6 potential energy surfaces along relevant dissociation coordinates is challenging due to excited states with doubly excited character and/or mixed Rydberg-valence character. Our findings demonstrate that the extended multi-state complete active space second-order perturbation theory (XMS-CASPT2) balances this computational efficiency and accuracy, as it captures both the Rydberg character of states in the Franck–Condon region and multiconfigurational character toward the bond-dissociation limits. In conclusion, we compare the performance of XMS-CASPT2 to a new variant of equation of motion coupled cluster theory with single, double, and perturbative triple corrections, EOM-CCSD(T)(a)*, finding that EOM-CCSD(T)(a)* significantly improves the treatment of doubly excited states compared to EOM-CCSD, but struggles to quantitatively capture asymptotic energies along bond dissociation coordinates for these states.

Rishi, Varun↗
NASA NTRS1987

Full CI studies of the collinear transition state for the reaction F + H2 yields HF + H

Full CI calculations on the collinear transition state for the reaction F + H2 yields HF + H are reported. The full CI results are compared with those obtained from single-reference and multireference CI calculations and from single-reference CPF calculations. In general, only those methods which attempt to account for the effects of higher excitations, such as CPF or CI plus the Davidson correction, yield a transition-state location and barrier height in good agreement with the full CI. In an extended basis, the effect of higher excitations is estimated to lower the barrier by as much as 1.5 kcal/mol; such an effect would essentially eliminate the present discrepancy between theory and experiment.

Bauschlicher, Charles W., Jr.↗
DOE OSTI2024

Core-excited states in 105 Cd

105 Cd was produced in the 96 Mo+ 12 C fusion/evaporation reaction, performed at NIPNE, Bucharest-Magurele, Romania. Various excited states of positive- and negative-parities were populated. Picosecond half-lives were measured by using the Differential Decay Curve Method (DDCM) method, allowing to control the side feeding of the states of interest. Further, new data were obtained for the half-lives of the 11/2 + , 15/2 - and 19/2 -105 Cd states. Reduced electric quadrupole transition strengths were calculated and compared to the neighboring odd-A and even-A cadmium nuclei. The particle-core weak coupling approach was used to interpret excited states of 105 Cd in the light of the new data.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1997

Collision Strengths for Electron Collisional Excitation of S II

Electron collisional excitation strengths for inelastic transitions in S II are calculated using the R-matrix method in a 19-state (3s(sup 2)3p(sup 3)(sup 4)S(sup o), (sup 2)D(sup o), (sup 2)p(sup o), 3s3p(sup 4)(sup 4)P, (sup 2)D, (sup 2)S, 3S(sup 2)3p(sup 2)3d(sup 2)P, (sup 4)F, (sup 4)D, (sup 2)F, (sup 4)P, 3s(sup 2)3p(sup 2)4s(sup 4)P, (sup 2)P, 3s(sup 2)3p(sup 2)4p(sup 2)S(s o), (sup 4)D(sup o), (sup 4)P(sup o), (sup 2)D(sup o), (sup 4)S(sup o), (sup 2)P(sup o)) close-coupling approximation. These target states are represented by extensive configuration-interaction wave functions that give excitation energies and oscillator strengths that are usually in good agreement with the experimental values and the available accurate calculations. The present results for collision strengths are in very good agreement with the recent merged beams energy loss measurement of Liao et al. and agree reasonably well with the 18-state R-matrix calculation of Ramsbottom, Bell, & Stafford, but show significant differences from the 12-state R-matrix calculation of Cai & Pradhan.

Tayal, S. S.↗
NASA NTRS1977

Spatially resolved excitation temperature measurements in a hypersonic flow using the hook method

Following an analysis of the hook equations for variation of refractivity along a spectrograph slit a series of experiments is reported, in which CO2 was used as the test gas, and the flow variations were spatially resolved. The hooked spectra were used to measure the ground state number densities of the impurity atom of CrI present in the flow. The excitation temperature of the CrI 1-eV level was obtained from the separation of the hooks of the CrI 425.4-nm transition resonance line and simultaneously the 434.4-nm CrI eV lower level line, from the shock to the body of the hypersonic shock tunnel flow. This excitation temperature is compared with theoretical calculations of the CO2 gas temperature. Some further applications of the hook type methods to gas diagnostics are discussed.

Sandeman, R. J.↗
DOE OSTI2024

Predissociation-based measurements of bond dissociation energies: US 2 , OUS, and USe

The uranium-containing molecules US 2 , OUS, and USe have been investigated using a pulsed laser ablation supersonic beam molecular source with time-of-flight mass spectrometric detection. Spectra have been recorded using the resonant two-photon ionization method over the spectroscopic range from 277 to 238 nm. These species have a myriad of excited electronic states in this spectroscopic region, leading to spectra that are highly congested and appear quasicontinuous. Sharp predissociation thresholds are observed, allowing precise bond dissociation energies to be measured. In the case of the triatomic molecules, it was necessary to use one laser for excitation and a delayed laser for ionization in order to observe a sharp predissociation threshold that allowed a precise bond dissociation energy to be measured. The resulting thermochemical values are D 0 (SU-S) = 4.910 ± 0.003 eV, D 0 (OU-S) = 5.035 ± 0.004 eV, and D 0 (USe) = 4.609 ± 0.009 eV. These results provide the first measurement of D 0 (USe) and reduce the error limits in the previous values of D 0 (SU-S) and D 0 (OU-S) by a factor of more than 70.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗