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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Electron beam characterization via quantum coherent electric field imaging

We demonstrate an all-optical, minimally invasive electron beam (𝑒−beam) characterization using Rydberg electrometry. An 𝑒-beam passes through a localized detector volume containing thermal Rb atoms that are optically excited in a quantum superposition of ground and Rydberg states. The 𝑒-beam's electric field perturbs atomic coherence and modifies resonance fluorescence in a narrow spectral region near the two-photon optical transition. Imaging Rb fluorescence provides a map of the electric field from the 𝑒-beam via Rydberg state Stark shifts and allows us to reconstruct the 𝑒-beam width, centroid position, and current. For an 𝑒-beam of 20 keV and electron currents of 20–40 µ⁢A, we measured the centroid position with an accuracy of ≤ 8 µ⁢m and width to within 100 µ⁢m, limited by the experimental sensitivity of electric field reconstruction of ∼0.02 V/cm. This method is suitable for a wide range of electron energies and currents, and can be adopted for nuclear and high-energy experiments for minimally invasive real-time diagnostics and profiling of charged particle beams.

Behary, Rob [College of William and Mary, Williams↗
DOE OSTI2018

Photoionization of the iodine 3d, 4s, and 4p orbitals in methyl iodide

Ionization of the I 3d, 4s, and 4p orbitals in methyl iodide (CH 3 I) has been studied by using synchrotron radiation to measure the total ion yield and by recording photoelectron spectra with linearly polarized radiation in two polarization orientations. The complete photoelectron spectrum of CH 3 I has been recorded at several photon energies, and bands due to the C 1s, I 3d, 4s, 4p, and 4d atomic-like orbitals, as well as the molecular orbitals, have been observed and assigned. In the vicinity of the I 3d 5/2 and 3d 3/2 ionization thresholds at 626.8 and 638.3 eV, respectively, the ion yield displays weak structure in the pre-edge region due to transitions into valence or Rydberg states, and, at higher energies, a shoulder and a broad maximum attributed to the I 3d 5/2 → εf and the I 3d 3/2 → εf shape resonances, respectively. The absorption spectrum calculated using time-dependent density functional theory, within the Tamm-Dancoff approximation, has allowed assignments to be proposed for the valence and Rydberg states. The Stieltjes imaging technique has been used to simulate the absorption spectrum above the ionization threshold and indicates that transitions into the f(l = 3) continuum channel dominate. This conclusion has been corroborated by a Continuum Multiple Scattering–Xα (CMS–Xα) calculation. The asymmetric broadening of the photoelectron bands associated with the I 3d orbital, due to post collision interaction, is taken into account in our experimental analysis. Experimentally derived photoelectron anisotropy parameters for the I 3d orbital are in good agreement with the theoretical predictions obtained with the CMS–Xα approach. The I 3d shake-up/shake-off photoelectron spectrum has been recorded, and assignments have been proposed for several of the satellites. The M 4 N 45 N 45 and M 5 N 45 N 45 Auger electron yields have been measured, and that for the M 5 N 45 N 45 decay exhibits a maximum due to interchannel coupling between the 3d5/2 and 3d3/2 continua. The photoelectron band associated with the I 4p orbital has an unusual appearance. Based upon previous theoretical work for the analogous Xe 4p orbital, it appears that the initial I 4p -1 hole state decays rapidly through Coster-Kronig and super-Coster-Kronig transitions. This leads to a redistribution of the spectral intensity associated with the I 4p orbital and results in a photoelectron spectrum containing a single structured band together with an extended continuum. Another continuum is observed on the high binding energy side of the peak due to the 4s orbital, and we assign this to super-Coster-Kronig transitions into the 4p -1 4d -1 continuum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Valence and lowest Rydberg electronic states of phenol investigated by synchrotron radiation and theoretical methods

We present the experimental high-resolution vacuum ultraviolet (VUV) photoabsorption spectra of phenol covering for the first time the full 4.3–10.8 eV energy-range, with absolute cross sections determined. Theoretical calculations on the vertical excitation energies and oscillator strengths were performed using time-dependent density functional theory and the equation-of-motion coupled cluster method restricted to single and double excitations level. These have been used in the assignment of valence and Rydberg transitions of the phenol molecule. The VUV spectrum reveals several new features not previously reported in the literature, with particular reference to the 6.401 eV transition, which is here assigned to the 3sσ/σ{sup ∗}(OH)←3π(3a″) transition. The measured absolute photoabsorption cross sections have been used to calculate the photolysis lifetime of phenol in the earth’s atmosphere (0–50 km).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Chirped-pulse millimeter-wave spectroscopy: Spectrum, dynamics, and manipulation of Rydberg-Rydberg transitions

We apply the chirped-pulse millimeter-wave (CPmmW) technique to transitions between Rydberg states in calcium atoms. The unique feature of Rydberg-Rydberg transitions is that they have enormous electric dipole transition moments ({approx}5 kiloDebye at n*{approx} 40, where n* is the effective principal quantum number), so they interact strongly with the mm-wave radiation. After polarization by a mm-wave pulse in the 70-84 GHz frequency region, the excited transitions re-radiate free induction decay (FID) at their resonant frequencies, and the FID is heterodyne-detected by the CPmmW spectrometer. Data collection and averaging are performed in the time domain. The spectral resolution is {approx}100 kHz. Because of the large transition dipole moments, the available mm-wave power is sufficient to polarize the entire bandwidth of the spectrometer (12 GHz) in each pulse, and high-resolution survey spectra may be collected. Both absorptive and emissive transitions are observed, and they are distinguished by the phase of their FID relative to that of the excitation pulse. With the combination of the large transition dipole moments and direct monitoring of transitions, we observe dynamics, such as transient nutations from the interference of the excitation pulse with the polarization that it induces in the sample. Since the waveform produced by the mm-wave source may be precisely controlled, we can populate states with high angular momentum by a sequence of pulses while recording the results of these manipulations in the time domain. We also probe the superradiant decay of the Rydberg sample using photon echoes. The application of the CPmmW technique to transitions between Rydberg states of molecules is discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Self-energy correction to the hyperfine splitting for excited states

The self-energy corrections to the hyperfine splitting is evaluated for higher excited states in hydrogenlike ions using an expansion in the binding parameter Z{alpha}, where Z is the nuclear-charge number and {alpha} is the fine-structure constant. We present analytic results for D, F, and G states, and for a number of highly excited Rydberg states, with principal quantum numbers in the range 13{<=}n{<=}16, and orbital angular momenta l=n-2 and l=n-1. A closed-form analytic expression is derived for the contribution of high-energy photons, valid for any state with l{>=}2 and arbitrary n, l, and total angular momentum j. The low-energy contributions are written in the form of generalized Bethe logarithms and evaluated for selected states.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1975

Dissociation of CH4 and CD4 by electron impact - Production of metastable and high-Rydberg hydrogen and carbon fragments

Production of hydrogen and carbon atoms in metastable and high-lying Rydberg states by electron-impact dissociation of methane and deuterated methane is investigated for incident electron energies ranging from threshold values to 300 eV. Threshold energies for five different processes resulting in metastable hydrogen and carbon atoms are determined in the energy range from 20 to 70 eV, and it is shown that metastable hydrogen atoms are produced in four of these collisional processes while metastable carbon atoms are produced in the other. The nature of each collisional process is described, differential cross sections are derived for the dissociative excitation of both types of atoms to metastable and high-Rydberg states at 100 eV, and the onset energy for UV photon production is measured. Much of the data is interpreted in terms of the ion core model suggested by Kupriyanov (1968) and developed by Freund (1971).

Finn, T. G.↗
DOE OSTI2018

Determining Orientations of Optical Transition Dipole Moments Using Ultrafast X-ray Scattering

Here, identification of the initially prepared, optically active state remains a challenging problem in many studies of ultrafast photoinduced processes. We show that the initially excited electronic state can be determined using the anisotropic component of ultrafast time-resolved X-ray scattering signals. The concept is demonstrated using the time-dependent X-ray scattering of N -methyl morpholine in the gas phase upon excitation by a 200 nm linearly polarized optical pulse. Analysis of the angular dependence of the scattering signal near time zero renders the orientation of the transition dipole moment in the molecular frame and identifies the initially excited state as the 3pz Rydberg state, thus bypassing the need for further experimental studies to determine the starting point of the photoinduced dynamics and clarifying inconsistent computational results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Observation of a dipole-bound excited state in 4-ethynylphenoxide and comparison with the quadrupole-bound excited state in the isoelectronic 4-cyanophenoxide

Negative ions do not possess Rydberg states, but can have Rydberg-like nonvalence excited states near the electron detachment threshold, including dipole-bound states (DBSs) and quadrupole-bound states (QBSs). While DBSs have been studied extensively, quadrupole-bound excited states have been more rarely observed. 4-cyanophenoxide (4CP – ) was the first anion observed to possess a quadrupole-bound exited state 20 cm-1 below its detachment threshold. Here we report the observation of a DBS in the isoelectronic 4-ethynylphenoxide anion (4EP – ), providing a rare opportunity to compare the behaviors of a dipole-bound and a quadrupole-bound excited state in a pair of very similar anions. Photodetachment spectroscopy (PDS) of cryogenically-cooled 4EP – reveals a DBS 76 cm -1 below its detachment threshold. Photoelectron spectroscopy (PES) at 266 nm shows that the electronic structure of 4EP – and 4CP – are nearly identical. The observed vibrational features in both the PDS and PES, as well as autodetachment from the nonvalence excited states, are also found to be similar for both anions. However, resonant two-photon detachment (R2PD) from the bound vibrational ground state is observed to be very different for the DBS in 4EP – and the QBS in 4CP – . The R2PD spectra reveal that decays take place from both the DBS and QBS to the respective anion ground electronic states within the 5 ns detachment laser pulse due to internal conversion followed by intramolecular vibrational redistribution (IVR), but the decay mechanisms appear to be very different. In the R2PD spectrum of 4EP – , we observe strong threshold electron signals, which are due to detachment, by the second photon, of highly rotationally excited anions resulted from the decay of the DBS. On the other hand, in the R2PD spectrum of 4CP – we observe well-resolved vibrational peaks due to the three lowest-frequency vibrational modes of 4CP – , which are populated from the decay of the QBS. Here, the different behaviors of the R2PD spectra suggest unexpected differences between the relaxation mechanisms of the dipole-bound and quadrupole-bound excited states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Rydberg Excitation of Single Atoms for Applications in Quantum Information and Metrology

With the advent of laser cooling and trapping, neutral atoms have become a foundational source of accuracy for applications in metrology and are showing great potential for their use as qubits in quantum information. In metrology, neutral atoms provide the most accurate references for the measurement of time and acceleration. The unsurpassed stability provided by these systems make neutral atoms an attractive avenue to explore applications in quantum information and computing. However, to fully investigate the eld of quantum information, we require a method to generate entangling interactions between neutral-atom qubits. Recent progress in the use of highly-excited Rydberg states for strong dipolar interactions has shown great promise for controlled entanglement using the Rydberg blockade phenomenon. I report the use of singly-trapped 133 Cs atoms as qubits for applications in metrology and quantum information. Each atom provides a physical basis for a single qubit by encoding the required information into the ground-state hyper ne structure of 133 Cs. Through the manipulation of these qubits with microwave and optical frequency sources, we demonstrate the capacity for arbitrary single-qubit control by driving qubit rotations in three orthogonal directions on the Bloch sphere. With this control, we develop an atom interferometer that far surpasses the force sensitivity of other approaches by applying the well-established technique of lightpulsed atom-matterwave interferometry to single atoms. Following this, we focus on two-qubit interactions using highly-excited Rydberg states. Through the development of a unique single-photon approach to Rydberg excitation using an ultraviolet laser at 319 nm, we observe the Rydberg blockade interaction between atoms separated by 6.6(3) m. Motivated by the observation of Rydberg blockade, we study the application of Rydberg-dressed states for a quantum controlled-phase gate. Using a realistic simulation of the dressed-state dynamics, we calculate a controlled-phase gate delity of 94% that is primarily limited by Doppler frequency shifts. Finally, we employ our single-photon excitation laser to measure the Rydberg-dressed interaction, thus demonstrating the viability of this approach.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2011

Evidence of the 2s2p({sup 1}P) doubly excited state in the harmonic generation spectrum of helium

By solving the two-active-electron time-dependent Schroedinger equation in an intense, ultrashort laser field, we investigate evidence of electron correlations in the high-order harmonic generation spectrum of helium. As the frequency of the driving laser pulse varies from 4.6 to 6.6 eV, the 13th, 11th, and 9th harmonics sequentially become resonant with the transition between the ground state and the isolated 2s2p({sup 1}P) autoionizing state of helium, which dramatically enhances these harmonics and changes their profiles. When each of the 9th and 13th harmonics are in resonance with this autoionizing state, there is also a low-order multiphoton resonance with a Rydberg state, resulting in a particularly large enhancement of these harmonics relative to neighboring harmonics. When the 11th harmonic is in resonance with the 2s2p({sup 1}P) autoionizing state, the 13th harmonic is simultaneously in resonance with numerous higher-energy autoionizing states, resulting in a competition between these two harmonics for intensity. These results demonstrate that even electron correlations occurring over a narrow energy interval can have a significant effect on strong-field processes such as harmonic generation.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1990

Theoretical studies of important processes in planetary and comet atmospheres

Dissociative recombination (DR) reactions in planetary and comet atmospheres are discussed. A computer program was developed which determines DR cross sections and rates using potential curves and electronic capture widths. It uses Multi-Channel Quantum Defect Theory (MQDT) to include excited Rydberg resonance levels in the DR cross section and rate calculations. Each vibrational level of a molecular ion is the limit for an infinite series of Rydberg states. Above each ion vibrational level are Rydberg vibrational levels having higher ion levels as their series limit. These Rydberg vibrational levels are resonances, i.e., neutral states which are imbedded in the electron-molecular ion continuum. The process in which the Rydberg level causes an abrupt perturbation in the cross section for DR (because of interference between capture into the Rydberg level and capture into the repulsive dissociative state) is referred to as indirect recombination. The process in which the Rydberg levels are excluded and recombination goes from the entrance channel to the repulsive state is called direct recombination. The full DR process, i.e., both direct and indirect recombination, is the process of importance for planetary atmospheres. These ideas are illustrated with the new results for DR from excited ion vibrational levels of O2(+) into the dissociative state which leads to O(1S) + O(1D).

Guberman, Steven L.↗
DOE OSTI2016

Combined theoretical and experimental study of the valence, Rydberg and ionic states of fluorobenzene

New photoelectron spectra (PES) and ultra violet (UV) and vacuum UV (VUV) absorption spectra of fluorobenzene recorded at higher resolution than previously, have been combined with mass-resolved (2 + 1) and (3 + 1) resonance enhanced multiphoton ionization (REMPI) spectra; this has led to the identification of numerous Rydberg states. The PES have been compared with earlier mass-analyzed threshold ionization and photoinduced Rydberg ionization (PIRI) spectra to give an overall picture of the ionic state sequence. The analysis of these spectra using both equations of motion with coupled cluster singles and doubles (EOM-CCSD) configuration interaction and time dependent density functional theory (TDDFT) calculations have been combined with vibrational analysis of both the hot and cold bands of the spectra, in considerable detail. The results extend several earlier studies on the vibronic coupling leading to conical intersections between the X{sup 2}B{sub 1} and A{sup 2}A{sub 2} states, and a further trio (B, C, and D) of states. The conical intersection of the X and A states has been explicitly identified, and its structure and energetics evaluated. The energy sequence of the last group is only acceptable to the present study if given as B{sup 2}B{sub 2}<C{sup 2}B{sub 1}<D{sup 2}A{sub 1}, a conclusion which is in agreement with most previous EOM-CCSD and other calculations. However, this symmetry ordering of the B and C states forces reconsideration of the nature of the PIRI spectrum. The coupling between these two states is induced by the a{sub 2} modes, ν{sub 12} and ν{sub 14} and we propose that the 14{sup 1} band is observed in the B{sup 2}B{sub 2} band in the PES for the first time, because of the improved resolution. This same assignment is given to the lowest energy band in the PIRI spectrum which was previously assigned as the origin band and further conclude that the entire PIRI spectrum is induced by ν{sub 12} and ν{sub 14}. The relative intensities of the various Rydberg state peaks in the VUV absorption and REMPI spectra of fluorobenzene are very similar to those observed in the equivalent spectra of benzene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Electrometry near a dielectric surface using Rydberg electromagnetically induced transparency

Electrometry near a dielectric surface is performed using Rydberg electromagnetically induced transparency. The large polarizability of high-n-state Rydberg atoms gives this method extreme sensitivity. We show that dipoles produced by adsorbates on the dielectric surface produce a significant electric field that responds to an applied field with a time constant of order 1 s. For transient applied fields (with a time scale of less than 1 s) we observe good agreement with calculations based on numerical solutions of Laplace's equation using an effective dielectric constant to simulate the bulk dielectric.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Satellite bands of the RbCs molecule in the range of highly excited states

We report on the observation of three RbCs satellite bands in the blue and green ranges of the visible spectrum. Absorption measurements are performed using all-sapphire cell filled with a mixture of Rb and Cs. We compare high resolution absorption spectrum of Rb-Cs vapor mixture with pure Rb and Cs vapor spectra from the literature. After detailed analysis, the new satellite bands of RbCs molecule at 418.3 nm, 468.3, and 527.5 nm are identified. The origin of these bands is discussed by direct comparison with difference potentials derived from quantum chemistry calculations of RbCs potential energy curves. These bands originate from the lower Rydberg states of the RbCs molecule. This study thus provides further insight into photoassociation of lower Rydberg molecular states, approximately between Cs(7s) + Rb(5s) and Cs(6s) + Rb(6p) asymptotes, in ultracold gases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

An experimental and theoretical study of the C 1s ionization satellites in CH 3 I

We report the C 1s ionization spectrum of CH 3 I has been studied both experimentally and theoretically. Synchrotron radiation has been employed to record polarization dependent photoelectron spectra at a photon energy of 614 eV. These spectra encompass the main-line due to the C 1s single-hole state and the peaks associated with the shake-up satellites. Vertical ionization energies and relative photoelectron intensities have been computed using the fourth-order algebraic-diagrammatic construction approximation scheme for the one-particle Green’s function and the 6-311++G** basis set. The theoretical spectrum derived from these calculations agrees qualitatively with the experimental results, thereby allowing the principal spectral features to be assigned. According to our calculations, two 2 A 1 shake-up states of the C 1s -1 σ CI → σ$*\atop{CI}$ type with singlet and triplet intermediate coupling of the electron spins (S' = 0, 1) play an important role in the spectrum and contribute significantly to the overall intensity. Both of these states are expected to have dissociative diabatic potential energy surfaces with respect to the C–I separation. Whereas the upper of these states perturbs the manifold of Rydberg states, the lower state forms a band which is characterized by a strongly increased width. Our results indicate that the lowest shake-up peak with significant spectral intensity is due to the pair (S' = 0, 1) of 2 E (C 1s -1 I 5p → σ$*\atop{CI}$) states. We predict that these 2 E states acquire photoelectron intensity due to spin-orbit interaction. Lastly, such interactions play an important role here due to the involvement of the I 5p orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Multiphoton Rabi oscillations between highly excited Stark states of potassium

We have applied a nonperturbative resonant theory to study the Rabi frequency of microwave multiphoton transitions between two Rydberg states of potassium in a static electric field. The Stark electric dipole moments used to calculate the Rabi frequency are determined by the Stark states' wave functions, which are obtained by the diagonalization method. The frequencies of the Rabi oscillations are in good agreement with either experimental ones or ones calculated by the time-dependent close-coupling method and the Floquet theory. Furthermore, we are able to show that the size of avoided crossings between the (n+2)s and (n,3) states can be predicted from the Stark electric dipole moment and the difference of the two Stark states' energy at a given resonance.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Effects of pulse shape on strongly driven two-level systems

We present an experimental study of the dynamics of a two-level system driven by strong nonresonant electromagnetic pulses as a function of pulse intensity and detuning. We have explored the qualitative and quantitative behavior of the transition probability as a function of pulse area for five different temporal profiles: Lorentzian, Lorentzian squared, hyperbolic secant, hyperbolic secant squared, and Gaussian. The two-level system consists of a fine-structure doublet in sodium Rydberg states coupled by Raman transitions driven through far-off-resonance intermediate states. The pulses are in the microwave regime and have high fidelity and uniform intensity. Experiments show that, despite the similarity in the pulse shapes, the behavior of the population transfer versus intensity depends dramatically on the temporal shape and that the spectral properties and area of the pulse do not adequately describe the response.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Ionization and stabilization of atoms in a high-intensity, low-frequency laser field

The dynamics of a model silver atom in the strong radiation field of a Ti:sapphire laser is studied in the Keldysh parameter regions {gamma} Greater-Than-Or-Slanted-Equal-To 1 and {gamma} Less-Than-Or-Slanted-Equal-To 1. It is found that in the entire range of Keldysh parameter variations, along with ionization, the efficient excitation of Rydberg states of the atom with principal quantum numbers n = 6-14 is observed. A Rydberg wavepacket appearing in this case proved stable with respect to ionization; i.e., the atomic system in strong low-frequency electromagnetic fields becomes stable with respect to ionization. The physical reasons behind the stabilization are discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗