SEARCH · Engineering Papers
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
No abstract prepared.
X-ray diffraction combined with conventional spectroscopy could provide a powerful means to characterize electronically excited atoms and molecules. We demonstrate theoretically how x-ray diffraction from laser excited atoms can be used to determine electronic structure, including angular momentum composition, principal quantum numbers, and channel populations. A theoretical formalism appropriate for highly excited atoms, and easily extended to molecules, is presented together with numerical results for Xe and H atoms.
Accurate non-relativistic variational calculations are performed for the seven lowest members of the {sup 2}D Rydberg series (1s{sup 2}2s2p{sup 2}, and 1s{sup 2}2s{sup 2}nd, n= 3, Horizontal-Ellipsis , 8) of the boron atom. The wave functions of the states are expanded in terms of all-electron explicitly correlated Gaussian basis functions and the effect of the finite nuclear mass is directly included in the calculations allowing for determining the isotopic shifts of the energy levels. The Gaussian basis is optimized independently for each state with the aid of the analytic energy gradient with respect to the Gaussian parameters. The calculations represent the highest accuracy level currently achievable for the considered states. The computed energies are compared with the available experimental data.
The nonadiabatic predissociation dynamics of the hydroxymethyl radical (CH 2 OH) in its 3 2 A(3p x ) state is investigated using a nine-dimensional quantum mechanical model based on an ab initio three coupled diabatic state potential energy matrix. The calculated absorption spectrum, which is dominated by predissociative resonances, is in excellent agreement with experiment. The predissociation is facilitated by two conical intersection seams formed between the 3 2 A(3p x ) and 2 2 A(3s) states near the Franck–Condon region. The h and g vectors of energy minimized points on these seams are analyzed using the normal modes of the 3 2 A equilibrium structure. The low-lying predissociative resonances have been assigned and their lifetimes are less than 100 fs and moderately mode specific. Finally, the absorption spectrum is dominated by a CO vibrational progression, due apparently to the promotion of an electron from the ground state antibonding $π$ CO * orbital to the carbon Rydberg orbital, which effectively increases the C–O bond order.
Measurements of high-lying even-parity 6sns 1 S 0 and 6snd 1,3 D 2 levels of neutral 174 Yb are presented in this paper. Spectroscopy is performed with a two-step laser excitation from the ground state 4f 14 6s 21 S 0 , and the Rydberg levels are detected by using the field ionization method. Additional two-photon microwave spectroscopy is used to improve the relative energy accuracy where possible. The spectroscopic measurements are complemented by a multichannel-quantum-defect-theory (MQDT) analysis for the J = 0 and the two-coupled J = 2 even-parity series. Here, we compare our results with the previous analysis of Aymar, Débarre, and Robaux and analyze the observed differences. From the MQDT models, a revised value for the first ionization limit I 6s = 50443.07041 (25) cm –1 is proposed for 174 Yb.
The paper emphasizes the necessity of high energy resolution (resolving powers greater than 100,000) in VUV spectroscopic determinations of atomic and molecular Rydberg electronic structures. Attention is given to spectral observations of Rydberg levels in Ge I near the 4p 2P(0)1/2 limit, in Sr I near the 4d 2D3/2 limit, and in diatomic hydrogen halides (especially H I) below the X2Pi3/2 limit.
The choice of the active degrees of freedom (DOFs) is a pivotal issue in a reduced-dimensional model of quantum dynamics when a full-dimensional one is not feasible. Here, several five-dimensional (5D) models are used to investigate the nonadiabatic photodissociation dynamics of the hydroxymethyl (CH 2 OH) radical, which possesses nine internal DOFs, in its lowest absorption band. A normal-mode based scheme is used to identify the active and spectator modes, and its predictions are confirmed by 5D quantum dynamical calculations. Furthermore our results underscore the important role of the CO stretching mode in the photodissociation dynamics of CH 2 OH, originating from the photo-induced promotion of an electron from the half-occupied π* CO antibonding orbital to a carbon Rydberg orbital.
Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe 2 ) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ~[Formula: see text] which is ~4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.
Abstract not provided
Explore the source record for details and available documents.
Not Available
An experimental investigation was undertaken to identify as many transitions as possible in the 7-10 eV region of the electron impact energy-loss spectrum of 02 at low impact energies and high scattering angles. A number of new transitions were found which do not appear in optical spectra: bands at 8.595, 8.826, 9.045, and 9.27 eV have been assigned to the 3 s sigma g 1Pi(nu prime equals 0, 1, 2, and 3) excitations, respectively, and the identification of the corresponding 3Pi-g bands have been reconfirmed.
Consequences of the nonrelativistic Coulomb Hamiltonian with a fixed proton are considered for positronium hydride (PsH). An optical-potential method and certain simplifying assumptions are used to compute the lowest s-wave resonance parameters on the basis of the /e(+)H(-)/ configuration. Resonance parameters corresponding to a Ps scattering energy of 4.0190 eV and a width of 0.0303 eV are obtained. These results are shown to be in very close agreement with those of previous studies.
A general expression is derived for the Born amplitude for electron capture into high principal, and arbitrary angular momentum, quantum numbers, n and l, by bare nuclei from hydrogenic atom targets. Cross sections for capture into high n and l = 0,1 are given in analytic forms. The limiting values of the ratios of the Born over OBK cross sections for n >> 1 and l = 0,1 are found, and shown that they confirm the empirical law of Jackson and Schiff only approximately. For high angular momenta, it is shown that the Born cross section approaches the OBK cross section. An error in a previous publication by the author has been corrected.
The interesting calculation of retardation corrections to excited atomic state energies is facilitated by the existence of good calculations of the nonrelativistic and nonretarded energies, to which retardation corrections can be added. Here I describe a perturbation method, applicable when the angular momentum is high enough which generates an asymptotic series for the energy. It makes use of generalized polarizabilities of the atomic or ionic core (numerically obtained) but otherwise is completely analytic. It is applied here to the lithium atom in detail, and its application to hydrogen molecular ions is outlined.
This paper reviews progress that has been made in obtaining essentially exact solutions to the nonrelativistic three-body problem for helium by a combination of variational and asymptotic expansion methods. The calculation of relativistic and quantum electrodynamic corrections by perturbation theory is discussed, and in particular, methods for the accurate calculation of the Bethe logarithm part of the electron self energy are presented. As an example, the results are applied to the calculation of isotope shifts for the short-lived 'halo' nucleus He-6 relative to He-4 in order to determine the nuclear charge radius of He-6 from high precision spectroscopic measurements carried out at the Argonne National Laboratory. The results demonstrate that the high precision that is now available from atomic theory is creating new opportunities to create novel measurement tools, and helium, along with hydrogen, can be regarded as a fundamental atomic system whose spectrum is well understood for all practical purposes.
The photoionization and photofragmentation dynamics of I 2 in intense femtosecond near-infrared laser fields were studied using velocity-map imaging of cations, electrons, and anions. A series of photofragmentation pathways originating from different cationic electronic states were observed following single ionization, leading to I + fragments with distinct kinetic energies, which could not be resolved in previous studies. Photoelectron spectra indicate that these high-lying dissociative states are primarily produced through nonresonant ionization from several molecular orbitals (MO) of the neutral. The photoelectron spectra also show clear signatures of resonant ionization pathways (Freeman resonances) to low-lying bound ionic states via Rydberg states of the neutral moiety. To investigate the role of these Rydberg states further, we imaged anionic products (I – ) formed through ion-pair dissociations of neutral molecules excited to these Rydberg states by the intense femtosecond laser pulse. Collectively, these results shed significant new light on the complex dynamics of I 2 molecules in intense laser fields and on the important role of neutral Rydberg states in a full description of strong-field phenomena in molecules.
We show that optical spectroscopy of Rydberg states can provide accurate in situ thermometry at room temperature. Transitions from a metastable state to Rydberg states with principal quantum numbers of 25-30 have 200 times larger fractional frequency sensitivities to blackbody radiation than the strontium clock transition. We demonstrate that magic-wavelength lattices exist for both strontium and ytterbium transitions between the metastable and Rydberg states. Frequency measurements of Rydberg transitions with 10{sup -16} accuracy provide 10 mK resolution and yield a blackbody uncertainty for the clock transition of 10{sup -18}.