Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “RYDBERG STATES”

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.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor

In this paper, we report 65 T magnetoabsorption spectroscopy of exciton Rydberg states in the archetypal monolayer semiconductor WSe 2 . The strongly field-dependent and distinct energy shifts of the 2 s , 3 s , and 4 s excited neutral excitons permits their unambiguous identification and allows for quantitative comparison with leading theoretical models. Both the sizes (via low-field diamagnetic shifts) and the energies of the n s exciton states agree remarkably well with detailed numerical simulations using the nonhydrogenic screened Keldysh potential for 2D semiconductors. Finally and moreover, at the highest magnetic fields, the nearly linear diamagnetic shifts of the weakly bound 3 s and 4 s excitons provide a direct experimental measure of the exciton’s reduced mass m r = 0.20 ± 0.01 m 0 .

2-dimensional systems↗
DOE OSTI2013

Atomic orientation following predissociation of the C {sup 3}{Pi}{sub g} Rydberg state of molecular oxygen

(2 + 1) resonance enhanced multiphoton ionization in combination with time-of-flight mass spectroscopy (TOF-MS) has been used to detect both the O({sup 3}P) and O({sup 1}D) fragments produced as a result of predissociation of the C {sup 3}{Pi}{sub g} (v= 0) and (v= 1) Rydberg states of O{sub 2}, accessed via two-photon absorption from the ground X {sup 3}{Sigma}{sub g}{sup -} state. In particular, TOF profiles have been recorded at various fixed two-photon absorption wavelengths within the two bands, with circular polarized probe laser light used to probe the angular momentum orientation of these photofragments. All photofragments are found to display coherent orientation resulting from interference between two possible two-photon absorption pathways. The measured orientation is affected by rotational depolarization due to the long lifetime of the excited C state; once this effect is accounted for the orientation is found to be nearly constant over all dissociation wavelengths. The origin of the coherent orientation is attributed to two-photon absorption to different spin-orbit components of the C state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1988

Rydberg states of helium - A new recoil term

It is shown that the mass-polarization shift in the energy levels of 1sNL Rydberg states of helium contains a term of second order, in the ratio of the electron mass to that of the nucleus, that is independent of L. The derivation of this new recoil term, based on the method of Drachman (1986), is very simple. It yields a correction of significance for the calculation of absolute ionization energies.

Drachman, Richard J.↗
DOE OSTI2017

Forced field ionization of Rydberg states for the production of monochromatic beams

In this work, we study Rydberg ionization in an electric field in order to produce monochromatic ion and electron beams. We present an experimental study of the photoexcitation and ionization of high quantum-defect states, using excitation from the 7s state in cesium to Rydberg states in the presence of a uniform electric field. Such states can exhibit complex ionization behavior, for instance, highly localized growth in the ionization rate due to interference effects. The data are well reproduced by the WKB quantum-defect and frame transformation methods with no adjustable parameters. This indicates that large changes in the Rydberg ionization rate from small changes in electric field are possible when a nearly stable state crosses a more unstable state. A fast variation of the ionization rate with electric field allows for the production of beams with very low energy dispersion. We develop a simple two-level model to predict the voltage and spatial resolution that would occur when atoms are prepared in a state with such sharp ionization in electric field. This confirms that Rydberg forced ionization in an electric field presents a pathway for the production of high-brightness, highly monochromatic ion and electron beams.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Photodissociation of Methyl Iodide via Selected Vibrational Levels of the $\tilde{B}$ ( 2 E 3/2 )6s Rydberg State

We have determined the I 2P3/2 and 2P1/2 branching fractions following the photodissociation of methyl iodide (CH3I) via a number of vibronic bands associated with the $\tilde{B}$ (2E3/2)6s Rydberg state at excitation wavelengths between 201.2 and 192.7 nm. Vacuum ultraviolet light at 118.2 nm was used to ionize both the product iodine atoms and the methyl radical cofragments, and velocity map ion imaging was used to determine the product translational energy distributions and angular distributions. The known relative photoionization cross sections for I 2P3/2 and 2P1/2 at 118.2 nm were used to determine the corresponding branching fractions. The results extend our earlier work at 193 nm by Xu et al. (J. Chem. Phys. 2013, 139, 214310), and complement the closely related work of González et al. (J. Chem. Phys. 2011, 135, 021102). We find that for most of the excited vibronic levels of the $\tilde{B}$ state studied, the I 2P3/2 branching ratio is small, but nonzero, and that this channel is associated with internally excited CH3 radicals. The results are discussed in relation to the recent theoretical results of Alekseyev et al. (J. Chem. Phys. 2011, 134, 044303).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Furthermore we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The nearly ~1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ~13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.

14 SOLAR ENERGY↗
NASA NTRS2010

Polarizabilites and Rydberg States in the Presence of a Debye Potential

Polarizabilities and hyperpolarizabilities, alpha(1), beta(1),gamma(1), alpha(2), beta(2),gamma(2), alpha(3), beta(3),gamma(3), delta and epsilon of hydrogenic systems have been calculated by Drachman. We have now calculated these quantities by using pseudostates for the S. P. D and F states. All of them converge very fast as the number of terms in the pseudostates is increased, and are essentially independent of the nonlinear parameters. All the results are in good agreement with the results obtained by Drachman. except for delta, which is of the third-order in perturbation formalism. We have calculated Rydberg states of He for high N and L. The effective potential is -alpha(sub 1)/x(exp 4)+{6 * Beta(sub 1) -alpha(sub 2)/x(exp6), where x is the distance of the outer electron from the nucleus. The exchange and electron-electron correlations are unimportant because the outer electron is far away from the nucleus. This implies that the conventional variational calculations are not necessary. The results agree well with the results of Drachman. We have generalized this approach in the presence of a Debye potential.

Bhatia, A. K.↗
DOE OSTI2025

Large inverse Faraday effect for Rydberg states of free atoms and isolated donors in semiconductors

We report on the induction of magnetization in Rydberg systems by means of the inverse Faraday effect and propose the appearance of the effect in two such systems: Rydberg atoms proper and shallow dopants in semiconductors. Rydberg atoms are characterized by a large orbital radius. This large radius gives such excited states a large angular moment, which when driven with circularly polarized light translates to a large effective magnetic field $\mathscr{B}$ eff . We calculate this effect to generate effective magnetic fields of O⁡(1⁢ µ⁢T)×($\frac{ω}{1THz}$) -1 ⁢ ($\frac{\mathscr{I}}{10Wcm^{-2}}$)⁢n 4 in the Rydberg states of atoms such as Rb and Cs for off-resonant photon beams with frequency ω and intensity $\mathscr{I}$ expressed in units of the denominators and n the principal quantum number. Additionally, terahertz spectroscopy of phosphorus-doped silicon reveals a large cross section for excitation of shallow dopants to Rydberg-like states, which even for small n have the potential to be driven similarly with circularly polarized light to produce an even larger magnetization. Our theoretical calculations estimate $\mathscr{B}$ eff as O⁡(10 2 T) for Si:P with a beam intensity of 10 8 Wcm -2 .

36 MATERIALS SCIENCE↗
DOE OSTI2017

Resonant ionization spectroscopy of autoionizing Rydberg states in cobalt and redetermination of its ionization potential

We obtained multi-step resonance ionization spectroscopy of cobalt using a hot-cavity laser ion source and three Ti:Sapphire lasers. Furthermore, the photoionization spectra revealed members of five new autoionizing Rydberg series that originate from three different lower levels of 3d 7 4s5s h 4 F 9/2 , 3d 7 4s4d f 4 G 11/2 , and 3d 7 4s4d f 4 H 13/2 and converge to the first four excited states of singly ionized Co. Our analyses of the Rydberg series yield 63564.689 0.036 cm -1 as the first ionization potential of Co, which is an order of magnitude more accurate than the previous estimation. Using a three-step resonance ionization scheme that employs an autoinizing Rydberg state in the last transition, we obtained an overall ionization efficiency of about 18% for Co.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Observation of Excitonic Rydberg States in Monolayer MoS 2 and WS 2 by Photoluminescence Excitation Spectroscopy

Here, we have identified excited exciton states in monolayers of MoS 2 and WS 2 supported on fused silica by means of photoluminescence excitation spectroscopy. In monolayer WS 2 , the positions of the excited A exciton states imply an exciton binding energy of 0.32 eV. In monolayer MoS 2 , excited exciton transitions are observed at energies of 2.24 and 2.34 eV. Assigning these states to the B exciton Rydberg series yields an exciton binding energy of 0.44 eV.

2D materials↗
DOE OSTI2019

Ultrafast Rydberg-state dissociation in oxygen: Identifying the role of multielectron excitations

We investigated the fragmentation dynamics of highly excited states of molecular oxygen using femtosecond transient photoelectron spectroscopy. An extreme ultraviolet (XUV) pulse populates the autoionizing Rydberg series converging to O$_2^+$c 4 Σ$_u^-$, and a femtosecond near-infrared (IR) pulse was used to photoionize these states as they dissociate. Monitoring the differential photoelectron spectra as a function of time delay allowed us to obtain the relaxation lifetimes of these Rydberg states. We observed a photoelectron signal corresponding to the formation of a 4 p excited atomic oxygen fragment, which is not an expected dissociation product of the (O$_2^+$c 4 Σ$_u^-$) nl σ g Rydberg series. Analysis of the time-dependent photoelectron spectra and photoionization calculations indicate that this fragment results from a previously unexplored (O$_2^+$ 4 II$_g$)4 p repulsive state and that, contrary to expectations, this multielectron excitation pathway presents a substantial cross section. Here, our study demonstrates that two-color time-resolved differential photoelectron spectroscopy is an excellent tool to study the fragmentation dynamics of such multielectron excited states, which are not easily probed by other means.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Refinement of the experimental energy levels of higher {sup 2}D Rydberg states of the lithium atom with very accurate quantum mechanical calculations

Very accurate variational non-relativistic calculations are performed for four higher Rydberg {sup 2}D states (1s{sup 2}nd{sup 1}, n= 8, ..., 11) of the lithium atom ({sup 7}Li). The wave functions of the states are expanded in terms of all-electron explicitly correlated Gaussian functions and finite nuclear mass is used. The exponential parameters of the Gaussians are optimized using the variational method with the aid of the analytical energy gradient determined with respect to those parameters. The results of the calculations allow for refining the experimental energy levels determined with respect to the {sup 2}S 1s{sup 2}2s{sup 1} ground state.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Laser diagnostics of the energy spectrum of Rydberg states of the lithium-7 atom

The spectra of excited lithium-7 atoms prepared in a magneto-optical trap are studied using a UV laser. The laser diagnostics of the energy of Rydberg atoms is developed based on measurements of the change in resonance fluorescence intensity of ultracold atoms as the exciting UV radiation frequency passes through the Rydberg transition frequency. The energies of various nS configurations are obtained in a broad range of the principal quantum number n from 38 to 165. The values of the quantum defect and ionization energy obtained in experiments and predicted theoretically are discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Atomic-Orbital Close-Coupling Calculations Of Electron Capture From Hydrogen Atoms Into Highly Excited Rydberg States Of Multiply Charged Ions

Collisions of neutral hydrogen atoms with multiply charged ions have been studied in the past using the semi-classical atomic-orbital close-coupling method. We present total and state-resolved cross sections for charge exchange as well as ionization. The advent of supercomputers and parallel programming facilities now allow treatment of collision systems that have been out of reach before, because much larger basis sets involving high quantum numbers are now feasible.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Nonadiabatic photodissociation dynamics of the hydroxymethyl radical via the 2 2 A (3 s ) Rydberg state: A four-dimensional quantum study

Here, the quantum mechanical nonadiabatic photodissociation dynamics of the hydroxymethyl (CH 2 OH) radical in its lowest absorption band is investigated for the first time on a set of coupled diabatic potential energy surfaces determined by accurately fitting a large set of ab initio data. In this two-state approximation, only the ground and first excited states of CH 2 OH, which are coupled by conical intersections, are included. The reduced-dimensional dynamical model includes the CO stretch, the COH bend, the HCOH torsion, and the O–H dissociation coordinate. The experimentally measured hydrogen atom kinetic energy distribution is satisfactorily reproduced. The calculated product state distribution of the H 2 CO( X ) fragment indicates strong vibrational excitation in the CO stretching mode, resulting from the relatively large difference in the C–O bond length between the ground and excited electronic states of CH 2 OH due to the photo-induced promotion of an electron from the half-occupied π* CO antibonding orbital to a Rydberg orbital. In addition, the bimodal kinetic energy distribution is confirmed to originate from nonadiabatic transitions near the conical intersection along the O–H dissociation coordinate

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗