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Sample records for helium rydberg states

  1. STIRAP on helium: Excitation to Rydberg states

    NASA Astrophysics Data System (ADS)

    Yuan, Deqian

    Research in optically induced transitions between dierent atomic levels has a long history. For transitions between states driven by a coherent optical eld, the theoretical eciency could be ideally high as 100% but there could be many factors preventing this. In the three state helium atom excitation process, i.e. 23S→33P→nL , the stimulated emission from intermediate state makes it hard to achieve ecient population transfer to the nal state through an intuitive excitation order. One technique to achieve a higher eciency is Stimulated Raman Adiabatic Passage (STIRAP) which is being studied and under research in our lab. Unlike traditional three level excitation processes, STIRAP actually uses a counter intuitive pulsed laser beams timing arrangement. The excitation objects are metastable helium atoms traveling in a vacuum system with a longitudinal velocity of ~ 1070 m/s. We are using a 389 nm UV laser to connect the 23S and the 33P state and a frequency tunable ~790 nm IR laser to connect the 33P state and the dierent Rydberg states. A third 1083 nm wavelength laser beam drives the 23S → 23P transition to transversely separate the residual metastable atoms and the Rydberg atoms for eciency measurements. The data is taken by a stainless steel detector in the vacuum system. As the Rydberg atoms will get ionized by blackbody radiation under room temperature, we can utilize this for their detection. An ion detector sitting on the eld plate is capable to collect the ion signals of the Rydberg atoms for detection. So far the whole system has not been ready for data collection and measurement, so here we are using data and results from previous theses for discussions. The highest transition frequency that has ever been achieved in our lab is around 70% after corrections.

  2. Rydberg States of rb and cs Atoms on Helium Nanodroplets: a Rydberg-Ritz Analysis

    NASA Astrophysics Data System (ADS)

    Lackner, Florian; Krois, Gunter; Ernst, Wolfgang E.

    2013-06-01

    Rydberg series of Rb and Cs atoms on the surface of helium nanodroplets (He_{N}) have been studied by resonance enhanced multi-photon ionization spectroscopy and laser induced fluorescence spectroscopy. The recorded excitation spectra are analyzed by using a Rydberg-Ritz approach. The dependence of the quantum defects on the principal quantum number within a Rydberg series gives insight into the interaction between the alkali atom's valence electron and the superfluid helium droplet. For higher excited states a screening of the valence electron from the alkali atom core by the helium droplet is observed. For lower states the strength of the screening effect decreases and the quantum defects are found to lie closer to free atom values. In addition, the large spin-orbit (SO) constant of the Cs-He_{N} nP(^{2}Π) states allows a detailed study of the influence of the helium droplet on the SO splitting as function of the principal quantum number. Within the pseudo-diatomic picture the alkali-He_{N} system represents a diatomic molecule. The coupling of the Cs valence electrons spin and the orbital angular momentum with the intermolecular axis, which is defined by the connection between the droplet center and the alkali nucleus, depends on the strength of the atomic SO interaction. While the splitting of the 6^{2}P_{1/2}(^{2}Π_{1/2}) and 6^{2}P_{3/2}(^{2}Π_{3/2}) components has an atom-like character (Hund's case (c) coupling), the SO splitting of higher n states is lower than the atomic value (Hund's case (a) coupling). C. Callegari and W. E. Ernst, Helium Droplets as Nanocryostats for Molecular Spectroscopy - from the Vacuum Ultraviolet to the Microwave Regime, in: Handbook of High-Resolution Spectroscopy, eds. M. Quack and F. Merkt, John Wiley & Sons, Chichester, (2011) F. Lackner, G. Krois, M. Theisen, M. Koch, and W.E. Ernst, Phys. Chem. Chem. Phys., 13, 18781-18788 (2011) F. Lackner, G. Krois, and W.E. Ernst, J. Phys. Chem. Lett., 3, 1404-1408 (2012)

  3. Asymptotic Energies and QED Shifts for Rydberg States of Helium

    NASA Technical Reports Server (NTRS)

    Drake, G.W.F.

    2007-01-01

    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.

  4. Rydberg states of helium in electric and magnetic fields of arbitrary relative orientation

    NASA Astrophysics Data System (ADS)

    Tkáč, Ondřej; Žeško, Matija; Agner, Josef A.; Schmutz, Hansjürg; Merkt, Frédéric

    2016-05-01

    A spectroscopic study of Rydberg states of helium (n = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear (n = 30, B ≤ 120 mT and F = 0–78 V cm‑1), and (ii) the diamagnetic term is dominant and the Stark effect is linear (n = 45, B = 277 mT and F = 0–8 V cm‑1). Both cases correspond to regimes where the interactions induced by the electric and magnetic fields are much weaker than the Coulomb interaction, but much stronger than the spin–orbit interaction. The experimental spectra are compared to spectra calculated by determining the eigenvalues of the Hamiltonian matrix describing helium Rydberg states in the external fields. The spectra and the calculated energy-level diagrams in external fields reveal avoided crossings between levels of different m l values and pronounced m l -mixing effects at all angles between the electric- and magnetic-field vectors other than 0. These observations are discussed in the context of the development of a method to generate dense samples of cold atoms and molecules in a magnetic trap following Rydberg–Stark deceleration.

  5. Blackbody-induced decay, excitation and ionization rates for Rydberg states in hydrogen and helium atoms

    NASA Astrophysics Data System (ADS)

    Glukhov, I. L.; Nekipelov, E. A.; Ovsiannikov, V. D.

    2010-06-01

    New features of the blackbody-induced radiation processes on Rydberg atoms were discovered on the basis of numerical data for the blackbody-induced decay Pdnl(T), excitation Penl(T) and ionization Pionnl(T) rates of nS, nP and nD Rydberg states calculated together with the spontaneous decay rates Pspnl in neutral hydrogen, and singlet and triplet helium atoms for some values of the principal quantum number n from 10 to 500 at temperatures from T = 100 K to 2000 K. The fractional rates Rd(e, ion)nl(T) = Pnld(e, ion)(T)/Pspnl equal to the ratio of the induced decay (excitation, ionization) rates to the rate of spontaneous decay were determined as functions of T and n in every series of states with a given angular momentum l = 0, 1, 2. The calculated data reveal an essential difference between the asymptotic dependence of the ionization rate Pionnl(T) and the rates of decay and excitation Pd(e)nl(T)~T/n2. The departures appear in each Rydberg series for n > 100 and introduce appreciable corrections to the formula of Cooke and Gallagher. Two different approximation formulae are proposed on the basis of the numerical data, one for Rd(e)nl(T) and another one for Rionnl(T), which reproduce the calculated values in wide ranges of principal quantum number from n = 10 to 1000 and temperatures between T = 100 K and T = 2000 K with an accuracy of 2% or better. Modified Fues' model potential approach was used for calculating matrix elements of bound-bound and bound-free radiation transitions in helium.

  6. Photoelectron angular distributions in infrared one-photon and two-photon ionization of FEL-pumped Rydberg states of helium

    NASA Astrophysics Data System (ADS)

    Mondal, S.; Fukuzawa, H.; Motomura, K.; Tachibana, T.; Nagaya, K.; Sakai, T.; Matsunami, K.; Yase, S.; Yao, M.; Wada, S.; Hayashita, H.; Saito, N.; Callegari, C.; Prince, K. C.; O'Keeffe, P.; Bolognesi, P.; Avaldi, L.; Miron, C.; Nagasono, M.; Togashi, T.; Yabashi, M.; Ishikawa, K. L.; Sazhina, I. P.; Kazansky, A. K.; Kabachnik, N. M.; Ueda, K.

    2013-10-01

    The photoelectron angular distributions (PADs) have been investigated for infrared (IR) ionization of He atoms excited to Rydberg states by extreme ultraviolet free-electron laser pulses. The experiment was carried out with two pulses which do not overlap in time. Depending on the intensity of the IR pulses, one IR photon ionization or additionally two-photon above-threshold ionization is observed. For low IR intensity, the PAD is well described by a contribution of s and d partial waves in accordance with early experiments. At high IR intensity, the PAD for two IR photon ionization clearly shows the contribution of higher partial waves. The experimental data are compared with the results of theoretical calculations based on solving the time-dependent Schrödinger equation.

  7. Fractional quantum Hall states of Rydberg polaritons

    NASA Astrophysics Data System (ADS)

    Maghrebi, Mohammad F.; Yao, Norman Y.; Hafezi, Mohammad; Pohl, Thomas; Firstenberg, Ofer; Gorshkov, Alexey V.

    2015-03-01

    We propose a scheme for realizing fractional quantum Hall states of light. In our scheme, photons of two polarizations are coupled to different atomic Rydberg states to form two flavors of Rydberg polaritons that behave as an effective spin. An array of optical cavity modes overlapping with the atomic cloud enables the realization of an effective spin-1 /2 lattice. We show that the dipolar interaction between such polaritons, inherited from the Rydberg states, can be exploited to create a flat, topological band for a single spin-flip excitation. At half filling, this gives rise to a photonic (or polaritonic) fractional Chern insulator—a lattice-based, fractional quantum Hall state of light.

  8. Rydberg states via CPmmW spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhou, Yan; Grimes, David; Field, Robert

    2014-05-01

    Rydberg-Rydberg transitions of Ca atoms are directly observed by chirped-pulse millimeter-wave spectroscopy, which is a form of broadband, high-resolution, free induction decay (FID) spectroscopy with accurate relative intensities. At moderate to high number densities (~106 cm-3), interactions between many Rydberg atoms are mediated by an AC electric field, absorbing and radiating cooperatively. A semiclassical model describes several significant time-domain and frequency-domain cooperative effects in two-level systems and Λ-type three-level systems. Experimental evidence that supports this model will be discussed. A new experiment, employing the buffer gas cooling technique has been constructed and I expect to present preliminary results. In partically, the >100-fold increase in number density will permit study of ``pure electronic'' spectra of Rydberg molecules, such as BaF. We expect to produce 108 state selected core-nonpenetrating Rydberg molecules in a single pulse of a laser-laser-mm-wave excitation sequence.

  9. Excitation of helium Rydberg states and doubly excited resonances in strong extreme ultraviolet fields: Full-dimensional quantum dynamics using exponentially tempered Gaussian basis sets

    SciTech Connect

    Kaprálová-Žďánská, Petra Ruth; Šmydke, Jan; Department of Radiation and Chemical Physics, Institute of Physics, Academy of Sciences of the Czech Republic, Na Slovance 2, 182 21 Prague 8 ; Civiš, Svatopluk

    2013-09-14

    Recently optimized exponentially tempered Gaussian basis sets [P. R. Kapralova-Zdanska and J. Smydke, J. Chem. Phys. 138, 024105 (2013)] are employed in quantitative simulations of helium absorption cross-sections and two-photon excitation yields of doubly excited resonances. Linearly polarized half-infinite and Gaussian laser pulses at wavelengths 38–58 nm and large intensities up to 100 TW/cm{sup 2} are considered. The emphasis is laid on convergence of the results with respect to the quality of the Gaussian basis sets (typically limited by a number of partial waves, density, and spatial extent of the basis functions) as well as to the quality of the basis set of field-free states (typically limited by the maximum rotational quantum number and maximum excitation of the lower electron). Particular attention is paid to stability of the results with respect to varying complex scaling parameter. Moreover, the study of the dynamics is preceded by a thorough check of helium energies and oscillator strengths as they are obtained with the exponentially tempered Gaussian basis sets, being also compared with yet unpublished emission wavelengths measured in electric discharge experiments.

  10. Thermal ionization of Cs Rydberg states

    NASA Astrophysics Data System (ADS)

    Glukhov, I. L.; Ovsiannikov, V. D.

    2009-01-01

    Rates Pnl of photoionization from Rydberg ns-, np-, nd-states of a valence electron in Cs, induced by black-body radiation, were calculated on the basis of the modified Fues model potential method. The numerical data were approximated with a three-term expression which reproduces in a simple analytical form the dependence of Pnl on the ambient temperature T and on the principal quantum number n. The comparison between approximate and exactly calculated values of the thermal ionization rate demonstrates the applicability of the proposed approximation for highly excited states with n from 20 to 100 in a wide temperature range of T from 100 to 10,000 K. We present coefficients of this approximation for the s-, p- and d-series of Rydberg states.

  11. Rydberg States of Atoms and Molecules

    NASA Astrophysics Data System (ADS)

    Stebbings, R. F.; Dunning, F. B.

    2011-03-01

    List of contributors; Preface; 1. Rydberg atoms in astrophysics A. Dalgarno; 2. Theoretical studies of hydrogen Rydberg atoms in electric fields R. J. Damburg and V. V. Kolosov; 3. Rydberg atoms in strong fields D. Kleppner, Michael G. Littman and Myron L. Zimmerman; 4. Spectroscopy of one- and two-electron Rydberg atoms C. Fabre and S. Haroche; 5. Interaction of Rydberg atoms with blackbody radiation T. F. Gallagher; 6. Theoretical approaches to low-energy collisions of Rydberg atoms with atoms and ions A. P. Hickman, R. E. Olson and J. Pascale; 7. Experimental studies of the interaction of Rydberg atoms with atomic species at thermal energies F. Gounand and J. Berlande; 8. Theoretical studies of collisions of Rydberg atoms with molecules Michio Matsuzawa; 9. Experimental studies of thermal-energy collisions of Rydberg atoms with molecules F. B. Dunning and R. F. Stebbings; 10. High-Rydberg molecules Robert S. Freund; 11. Theory of Rydberg collisions with electrons, ions and neutrals M. R. Flannery; 12. Experimental studies of the interactions of Rydberg atoms with charged particles J. -F. Delpech; 13. Rydberg studies using fast beams Peter M. Koch; Index.

  12. Cold Rydberg atoms in circular states

    NASA Astrophysics Data System (ADS)

    Anderson, David; Schwarzkopf, Andrew; Raithel, Georg

    2012-06-01

    Circular-state Rydberg atoms are interesting in that they exhibit a unique combination of extraordinary properties; long lifetimes (˜n^5), large magnetic moments (l=|m|=n-1) and no first order Stark shift. Circular states have found applications in cavity quantum electrodynamics and precision measurements [1,2], among other studies. In this work we present the production of circular states in an atom trapping apparatus using an adiabatic state-switching method (the crossed-field method [3]). To date, we have observed lifetimes of adiabatically prepared states of several milliseconds. Their relatively large ionization electric fields have been verified by time-of-flight signatures of ion trajectories. We intend to explore the magnetic trapping of circular state Rydberg atoms, as well as their production and interaction properties in ultra-cold and degenerate samples.[4pt] [1] P. Bertet et al., Phys. Rev. Lett., 88, 14 (2002)[0pt] [2] M. Brune et al., Phys. Rev. Lett., 72, 21 (1994)[0pt] [3] D. Delande and J.C. Gay, Europhys. Lett., 5, 303-308 (1988).

  13. Rydberg Spectroscopy of Zeeman-Decelerated Beams of Metastable Helium Molecules

    NASA Astrophysics Data System (ADS)

    Jansen, Paul; Motsch, Michael; Sprecher, Daniel; Merkt, Frederic

    2014-06-01

    Having three and four electrons, respectively, He_2^+ and He_2 represent systems for which highly accurate ab-initio calculations might become feasible in the near future. With the goal of performing accurate measurements of the rovibrational energy-level structure of He_2^+ by Rydberg spectroscopy of He_2 and multichannel quantum-defect theory extrapolation techniques, we have produced samples of helium molecules in the a ^3Σu^+ state in supersonic beams with velocities tunable down to 100 m/s by combining a cryogenic supersonic-beam source with a multistage Zeeman decelerator. The molecules are formed at an initial velocity of 500 m/s by striking a discharge in the pulsed expansion of helium gas from a reservoir kept at a cryogenic temperature of 10 K. Using rotationally-resolved PFI-ZEKE (pulsed-field-ionization zero-kinetic-energy) photoelectron spectroscopy, we have probed the rotational-state distribution of the molecules produced in the discharge and found vibrational levels up to ν" = 2 and rotational levels up to N"=21 to be populated. The molecular beam is coupled to a multistage Zeeman decelerator that employs pulsed inhomogeneous magnetic fields to further reduce the beam velocity. By measuring the quantum-state distribution of the decelerated sample using photoelectron and photoionization spectroscopy we observed no rotational or vibrational state-selectivity of the deceleration process, but found that one of the three spin-rotation components of the He_2 a ^3Σu^+ rotational levels is eliminated. W.-C. Tung, M. Pavanello, L. Adamowicz, J. Chem. Phys. 136, 104309 (2012). D. Sprecher, J. Liu, T. Krähenmann, M. Schäfer, and F. Merkt, J. Chem. Phys. 140, 064304 (2014). M. Motsch, P. Jansen, J. A. Agner, H. Schmutz, and F. Merkt, arXiv:1401.7774. N. Vanhaecke, U. Meier, M. Andrist, B. H. Meier, and F. Merkt, Phys. Rev. A 75, 031402(R) (2007).

  14. Formation of heavy-Rydberg ion-pair states in Rydberg atom collisions with attaching targets

    NASA Astrophysics Data System (ADS)

    Wang, Changhao; Kelley, Michael; Buathong, Sitti; Dunning, F. Barry

    2014-05-01

    Electron transfer in collisions between K(np)Rydberg atoms and electron attaching molecules can lead to formation of heavy-Rydberg ion-pair states comprising a weakly-bound positive-negative ion pair orbiting at large internuclear separations. In the present work ion-pair states are created in a small collision cell and allowed to exit into an analysis region where their binding energy and velocity distributions are determined with the aid of electric-field-induced dissociation and a position sensitive detector. Ion pair production is analyzed using a Monte Carlo collision code that models both the initial Rydberg electron capture and the subsequent behavior of the product ion pair. The data demonstrate that collisions with SF6 and CCl4 lead to formation of long-lived ion pair states with a broad distribution of binding energies whose velocity distribution is strongly peaked in the forward direction. Research supported by the Robert A. Welch Foundation.

  15. Direct excitation of butterfly states in Rydberg molecules

    NASA Astrophysics Data System (ADS)

    Lippe, Carsten; Niederpruem, Thomas; Thomas, Oliver; Eichert, Tanita; Ott, Herwig

    2016-05-01

    Since their first theoretical prediction Rydberg molecules have become an increasing field of research. These exotic states originate from the binding of a ground state atom in the electronic wave function of a highly-excited Rydberg atom mediated by a Fermi contact type interaction. A special class of long-range molecular states, the butterfly states, were first proposed by Greene et al.. These states arise from a shape resonance in the p-wave scattering channel of a ground state atom and a Rydberg electron and are characterized by an electron wavefunction whose density distribution resembles the shape of a butterfly. We report on the direct observation of deeply bound butterfly states of Rydberg molecules of 87 Rb. The butterfly states are studied by high resolution spectroscopy of UV-excited Rydberg molecules. We find states bound up to - 50 GHz from the 25 P1/2 , F = 1 state, corresponding to binding lengths of 50a0 to 500a0 and with permanent electric dipole moments of up to 500 Debye. This distinguishes the observed butterfly states from the previously observed long range Rydberg molecules in rubidium.

  16. Coherent control of Rydberg states in silicon.

    PubMed

    Greenland, P T; Lynch, S A; van der Meer, A F G; Murdin, B N; Pidgeon, C R; Redlich, B; Vinh, N Q; Aeppli, G

    2010-06-24

    Laser cooling and electromagnetic traps have led to a revolution in atomic physics, yielding dramatic discoveries ranging from Bose-Einstein condensation to the quantum control of single atoms. Of particular interest, because they can be used in the quantum control of one atom by another, are excited Rydberg states, where wavefunctions are expanded from their ground-state extents of less than 0.1 nm to several nanometres and even beyond; this allows atoms far enough apart to be non-interacting in their ground states to strongly interact in their excited states. For eventual application of such states, a solid-state implementation is very desirable. Here we demonstrate the coherent control of impurity wavefunctions in the most ubiquitous donor in a semiconductor, namely phosphorus-doped silicon. In our experiments, we use a free-electron laser to stimulate and observe photon echoes, the orbital analogue of the Hahn spin echo, and Rabi oscillations familiar from magnetic resonance spectroscopy. As well as extending atomic physicists' explorations of quantum phenomena to the solid state, our work adds coherent terahertz radiation, as a particularly precise regulator of orbitals in solids, to the list of controls, such as pressure and chemical composition, already familiar to materials scientists. PMID:20577211

  17. State dependence of Rydberg interaction-induced collisional loss

    NASA Astrophysics Data System (ADS)

    Feng, Zhigang; Zhao, Kejia; Miao, Jingyuan; Li, Difei; Yang, Zhijun; Wu, Zhaochun; He, Zhao; Zhao, Jianming; Jia, Suotang

    2016-09-01

    We present a simple analytical formula from an existing theoretical model and theoretically investigate in detail the state dependence of interaction-induced collisional loss rate coefficients, and the various parameter effects on collisional loss rate. We also investigate the different mechanisms and corresponding effects on collisional loss by analyzing our previous experimental results using the present formula, and even investigate the time evolution of Rydberg atom number for different Rydberg states.

  18. Retardation (Casimir) energy shifts for Rydberg helium-like low-Z ions: An exploratory study

    NASA Astrophysics Data System (ADS)

    Babb, James F.; Habs, Dietrich; Spruch, Larry; Wolf, Andreas

    1992-09-01

    The development of storage rings and electromagnetic traps for heavy charged particles is opening up new regimes of atomic physics, including, in particular, spectroscopic studies of Rydberg helium-like ions — with nuclear charge Z, one electron in the 1 s state, and one electron in a near-hydrogenic state of high n and l < n, with n and l the principal and orbital quantum numbers, respectively. We consider the possibility of detecting energy shifts due to retardation, Δ E ret ( n, l), Casimir-like effects. These are quantum electrodynamic (QED) retardation effects associated with the finite speed of light. (As opposed to basically kinematic and dynamic QED effects for small quantum numbers n and l, the appropriate expansion parameter for n and l large for retardation QED corrections is not Z( e 2/ħ c) but [( Z - 1)/ n 2 Z 2](ħ c/e 2).) We wish to provide some orientation to those planning experiments in the area, with regard to the choices of n, l, and Z most likely to be able to generate a high-precision confirmation of a retarded interaction. To do so, we provide extensive tables of estimates, for 1 s, nl states, of Δ E ret( n, l), of radiative widths, and of E, the spin-independent (“electric” fine structure) energy in the absence of retardation shifts, for (nuclear spin zero) ions with Z=2, 6, 8, 16 and 20. These ions might be experimentally accessible in storage rings, and the Z's are low enough that virtual pair production effects may not yet be significant. There is also a brief survey of possible experimental techniques.

  19. Radio-frequency-modulated Rydberg states in a vapor cell

    NASA Astrophysics Data System (ADS)

    Miller, S. A.; Anderson, D. A.; Raithel, G.

    2016-05-01

    We measure strong radio-frequency (RF) electric fields using rubidium Rydberg atoms prepared in a room-temperature vapor cell as field sensors. Electromagnetically induced transparency is employed as an optical readout. We RF-modulate the 60{{{S}}}1/2 and 58{{{D}}}5/2 Rydberg states with 50 and 100 MHz fields, respectively. For weak to moderate RF fields, the Rydberg levels become Stark-shifted, and sidebands appear at even multiples of the driving frequency. In high fields, the adjacent hydrogenic manifold begins to intersect the shifted levels, providing rich spectroscopic structure suitable for precision field measurements. A quantitative description of strong-field level modulation and mixing of S and D states with hydrogenic states is provided by Floquet theory. Additionally, we estimate the shielding of DC electric fields in the interior of the glass vapor cell.

  20. Coherent excitation of a single atom to a Rydberg state

    SciTech Connect

    Miroshnychenko, Y.; Gaeetan, A.; Evellin, C.; Grangier, P.; Wilk, T.; Browaeys, A.; Comparat, D.; Pillet, P.

    2010-07-15

    We present the coherent excitation of a single Rubidium atom to the Rydberg state 58d{sub 3/2} using a two-photon transition. The experimental setup is described in detail, as are experimental techniques and procedures. The coherence of the excitation is revealed by observing Rabi oscillations between ground and Rydberg states of the atom. We analyze the observed oscillations in detail and compare them to numerical simulations which include imperfections of our experimental system. Strategies for future improvements on the coherent manipulation of a single atom in our settings are given.

  1. Photoionization dynamics of the C2+ ion in Rydberg states

    NASA Astrophysics Data System (ADS)

    Stancalie, Viorica

    2014-11-01

    The goal of this work is to examine in detail the ionization dynamics of Be-like C ion in Rydberg states. An initial calculation has been done to output the lifetime due to spontaneous decay for unperturbed 1s22sns (1Se) Rydberg states using the multi-configuration Dirac-Fock (MCDF) method with configuration interaction option implemented in the general-purpose relativistic atomic structure package (GRASP). Both the C2+ ground state and the C3+ target state energies have been carefully calculated. We report results from a detailed and systematic study of the behaviour of complex photoionization amplitudes, the lifetime due to spontaneous decay for unperturbed 1s22sns (1Se) Rydberg states, the `resonant' phase shift and the rapidly increasing of this shift from well below to well above the resonance position. The sum-over-state method is used to calculate the static dipole polarizability, while the frequency-dependent polarizability values of C2+ ion in these Rydberg states are obtained from two-state model calculation results. Contribution to the Topical Issue "Elementary Processes with Atoms and Molecules in Isolated and Aggregated States", edited by Friedrich Aumayr, Bratislav Marinkovic, Stefan Matejcik, John Tanis and Kurt H. Becker.

  2. Static and dynamic polarizability for C2+ in Rydberg states

    NASA Astrophysics Data System (ADS)

    Stancalie, V.

    2015-07-01

    This work presents results from a non-perturbative calculation of dynamic polarizability of C III ions in 1s22sns (1Se) Rydberg states. We employ a two-state model for dressed atomic states to investigate the effect of the frequency-dependent polarizability of optically dressed 1s22sns(1Se) states (n = 5 - 12) on transitions to nearby states (1s22pns(1P1o)). Our model calculation results indicate that the resonance structure of the polarizabilities is entirely captured by the transition terms whereas the free electron polarizability only provides a smooth background. The resonance structure is evident in the plots and the widths increase with increasing principal quantum number. This work refers to highly excited 1s22sns (1S) Rydberg states, embedded in the electric dipole field of the 2s - 2p core transition in Li-like C3+ ion. The contributions of the individual transitions to the static polarizabilities of these Rydberg states are obtained from the use of the sum-over-state method. To this aim, both the C2+ ground state and the C3+ target state energies have been carefully calculated based on the configuration interactions method implemented in the General-purpose Relativistic Atomic Structure Package. Agreement is reasonably good with existing data wherever available. These results are believed to be the first such values for this system and will be important for ionic spectroscopy and plasma diagnostics.

  3. Resonant quenching of Rydberg atomic states by highly polar molecules

    NASA Astrophysics Data System (ADS)

    Narits, A. A.; Mironchuk, E. S.; Lebedev, V. S.

    2016-06-01

    The results of theoretical studies of the resonant quenching and ion-pair formation processes induced by collisions of Rydberg atoms with highly polar molecules possessing small electron affinities are reported. We elaborate an approach for describing collisional dynamics of both processes and demonstrate the predominant role of resonant quenching channel of reaction for the destruction of Rydberg states by electron-attaching molecules. The approach is based on the solution of the coupled differential equations for the transition amplitudes between the ionic and Rydberg covalent terms of a quasimolecule formed during a collision of particles. It takes into account the possibility of the dipole-bound anion decay in the Coulomb field of the positive ionic core and generalizes previous models of charge-transfer processes involving Rydberg atoms to the cases, when the multistate Landau–Zener approaches become inapplicable. Our calculations for {{Rb}}({nl}) atom perturbed by {{{C}}}2{{{H}}}4{{SO}}3, {{CH}}2{CHCN}, {{CH}}3{{NO}}2, {{CH}}3{CN}, {{{C}}}3{{{H}}}2{{{O}}}3, and {{{C}}}3{{{H}}}4{{{O}}}3 molecules show that the curves representing the dependence of the resonant quenching cross sections on the principal quantum number n are bell-shaped with the positions of maxima being shifted towards lower values of n and the peak values, {σ }{max}({{q})}, several times higher than those for the ion-pair formation, {σ }{max}({{i})}. We obtain a simple power relation between the energy of electron affinity of a molecule and the position of maximum in n-dependence of the resonant quenching cross section. It can be used as an additional means for determining small binding energies of dipole-bound anions from the experimental data on resonant quenching of Rydberg states by highly polar molecules.

  4. Lifetimes of Heavy-Rydberg Ion-Pair States Formed through Rydberg Electron Transfer

    SciTech Connect

    Cannon, M.; Wang, C. H.; Dunning, F. B.; Reinhold, Carlos O

    2010-01-01

    The lifetimes of K{sup +}-Cl{sup -}, K{sup +}-CN{sup -}, and K{sup +}-SF{sub 6}{sup -} heavy-Rydberg ion-pair states produced through Rydberg electron transfer reactions are measured directly as a function of binding energy using electric field induced detachment and the ion-pair decay channels discussed. The data are interpreted using a Monte Carlo collision code that models the detailed kinematics of electron transfer reactions. The lifetimes of K{sup +}-Cl{sup -} ion-pair states are observed to be very long, >100 {micro}s, and independent of binding energy. The lifetimes of strongly bound (>30 meV) K{sup +}-CN{sup -} ion pairs are found to be similarly long but begin to decrease markedly as the binding energy is reduced below this value. This behavior is attributed to conversion of rotational energy in the CN{sup -} ion into translational energy of the ion pair. No long-lived K{sup +}-SF{sub 6}{sup -} ion pairs are observed, their lifetimes decreasing with increasing binding energy. This behavior suggests that ion-pair loss is associated with mutual neutralization as a result of charge transfer.

  5. Three-photon coherence of Rydberg atomic states

    NASA Astrophysics Data System (ADS)

    Kwak, Hyo Min; Jeong, Taek; Lee, Yoon-Seok; Moon, Han Seb

    2016-05-01

    We investigated three-photon coherence effects of the Rydberg state in a four-level ladder-type atomic system for the 5 S1/2 (F = 3) - 5 P3/2 (F' = 4) - 50 D5/2 - 51 P3/2 transition of 85 Rb atoms. By adding a resonant electric field of microwave (MW) at electromagnetically induced transparency (EIT) in Rydberg state scheme, we observed experimentally that splitting of EIT signal appears under the condition of three-photon resonance in the Doppler-broadened atomic system. Discriminating the two- and three-photon coherence terms from the calculated spectrum in a simple four-level ladder-type Doppler-broadened atomic system, we found that the physical origin of splitting of EIT was three-photon coherence effect, but not three-photon quantum interference phenomena such as three-photon electromagnetically induced absorption (TPEIA).

  6. Progress towards Generating Rydberg State, One Electron Ions

    NASA Astrophysics Data System (ADS)

    Dreiling, Joan; Fogwell Hoogerheide, Shannon; Naing, Aung; Tan, Joseph

    2016-05-01

    We report on progress towards producing hydrogen-like ions in Rydberg states from bare nuclei. Fully stripped neon atoms (Ne10+) are produced by the electron beam ion trap (EBIT) at NIST. These ions are extracted via a beamline from the EBIT into a second apparatus where they are captured at low energy in a unitary Penning trap. The second apparatus has a cross-beam configuration, with a perpendicular beam of laser excited Rb atoms intersecting the ion beam at the Penning trap. While stored in the trap, the ions can interact with the Rb and, through charge exchange interactions, the bare nuclei can capture one or more electrons from the Rb. The ions are then analyzed by dumping the trap to a time-of-flight detector, which allows determination of the ion charge state evolution. This work builds towards laser spectroscopy on hydrogen-like ions in circular Rydberg states to obtain a value for the Rydberg constant independent of nuclear size effects. Such a measurement could shed some light on the proton radius puzzle.

  7. Transfer of entangled state, entanglement swapping and quantum information processing via the Rydberg blockade

    NASA Astrophysics Data System (ADS)

    Deng, Li; Chen, Ai-Xi; Zhang, Jian-Song

    2011-11-01

    We provide a scheme with which the transfer of the entangled state and the entanglement swapping can be realized in a system of neutral atoms via the Rydberg blockade. Our idea can be extended to teleport an unknown atomic state. According to the latest theoretical research of the Rydberg excitation and experimental reports of the Rydberg blockade effect in quantum information processing, we discuss the experimental feasibility of our scheme.

  8. Control of multiple excited Rydberg states around segmented carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Schmelcher, Peter; Sadeghpour, Hossein; Knoerzer, Johannes; Fey, Christian

    2016-05-01

    Electronic image Rydberg states around segmented carbon nanotubes can be confined and shaped along the nanotube axis by engineering the image potential. We show how several such image states can be prepared simultaneously along the same nanotube. The inter-electronic distance can be controlled a priori by engineering tubes of specific geometries. High sensitivity to external electric and magnetic fields can be exploited to manipulate these states and their mutual long-range interactions. These building blocks provide access to a new kind of tailored long-range interacting quantum systems.

  9. On the dynamics of high Rydberg states of large molecules

    NASA Astrophysics Data System (ADS)

    Jortner, Joshua; Bixon, M.

    1995-04-01

    In this paper we explore the level structure, the optical excitation modes and the dynamics of a mixed Stark manifold of very high Rydberg states (with principal quantum numbers n=80-250) of large molecules, e.g., 1,4 diaza bicyclo [2,2,2] octane (DABCO) and bis (benzene) chromium (BBC) [U. Even, R. D. Levine, and R. Bersohn, J. Phys. Chem. 98, 3472 (1994)] and of autoionizing Rydbergs of atoms [F. Merkt, J. Chem. Phys. 100, 2623 (1994)], interrogated by time-resolved zero-electron kinetic energy (ZEKE) spectroscopy. We pursue the formal analogy between the level structure, accessibility and decay of very high Rydbergs in an external weak (F≂0.1-1 V cm-1) electric field and intramolecular (interstate and intrastate) relaxation in a bound molecular level structure. The onset n=nM of the strong mixing (in an external field F and in the field exerted by static ions) of a doorway state, which is characterized by a low azimuthal quantum number l, a finite quantum defect δ, and a total nonradiative width Γs≂Γ0/n3, with the inactive high l manifold is specified by nM≂80.6δ1/5(F/V cm-1)-1/5. At n≥nM the level structure and dynamics are characterized by the product γρ, where ρ is the density of states and γ=ΓsD(n) is the average decay width of the eigenstates, with the dilution factor D(n)≊n-2 for (lml) mixing and D(n)≂n-1 for (l) mixing, whereupon γρ=(Γ0/4δR)(nM/n)5, being independent of D(n). The sparse level structure is realized for γρ≪1, while the dense level structure prevails for γρ≳1, resulting in two limiting situations; (a) a dense limit for n≥nM and a sparse limit for n≫nM, and (b) a sparse limit for all n≥nM. The experimental information currently available on the decay dynamics of molecular (DABCO and BBC) and atomic (Ar) Rydbergs for n≥nM corresponds to case (b). The time-resolved dynamics was characterized in terms of the excited state total population probability P(t) and the population probability I(t) of the doorway

  10. Excitation of Ultracold Molecules to ``TRILOBITE-LIKE" Long-Range Molecular Rydberg States

    NASA Astrophysics Data System (ADS)

    Bellos, M. A.; Carollo, R.; Banerjee, J.; Eyler, E. E.; Gould, P. L.; Stwalley, W. C.

    2013-06-01

    A class of long-range Rydberg molecules, sometimes called ``trilobite states", occurs when a ground-state atom is embedded in the electronic cloud of a Rydberg atom. The bond between the Rydberg atom and the ground-state atom originates from the low-energy scattering of the Rydberg electron from the ground-state atom. We produce trilobite-like states of ultracold Rb_2 at low principal quantum numbers and at internuclear separations less than 40 bohr. We populate these states through single-photon ultraviolet transitions starting from molecules in high-lying vibrational levels of the lowest triplet state. This demonstrates that long-range Rydberg molecules can also be excited through bound-bound transitions, in addition to previous studies that used free-bound transitions. We also discuss the advantages of a bound-bound pathway. C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000).

  11. Multichannel quantum defect theory of strontium bound Rydberg states

    NASA Astrophysics Data System (ADS)

    Vaillant, C. L.; Jones, M. P. A.; Potvliege, R. M.

    2014-08-01

    Using the reactance matrix approach, we systematically develop new multichannel quantum defect theory (MQDT) models for the singlet and triplet S, P, D and F states of strontium below the first ionization limit, based on improved energy level measurements. The new models reveal additional insights into the character of doubly excited perturber states, and the improved energy level measurements for certain series allow fine structure to be resolved for those series’ perturbers. Comparison between the predictions of the new models and those of previous empirical and ab initio studies reveals good agreement with most series; however, some discrepancies are highlighted. Using the MQDT wave functions derived from our models we calculate other observables such as Landé {{g}J}-factors and radiative lifetimes. The analysis reveals the impact of perturbers on the Rydberg state properties of divalent atoms, highlighting the importance of including two-electron effects in the calculations of these properties. The work enables future investigations of properties such as Stark maps and long-range interactions of Rydberg states of strontium.

  12. Rydberg states of chloroform studied by VUV photoabsorption spectroscopy

    NASA Astrophysics Data System (ADS)

    Singh, Param Jeet; Shastri, Aparna; D'Souza, R.; Jagatap, B. N.

    2013-11-01

    The VUV photoabsorption spectra of CHCl3 and CDCl3 in the energy region 6.2-11.8 eV (50,000-95,000 cm-1) have been investigated using synchrotron radiation from the Indus-1 source. Rydberg series converging to the first four ionization limits at 11.48, 11.91, 12.01 and 12.85 eV corresponding to excitation from the 1a2, 4a1, 4e, 3e, orbitals of CHCl3 respectively are identified and analyzed. Quantum defect values are observed to be consistent with excitation from the chlorine lone pair orbitals. Vibrational progressions observed in the region of 72,500-76,500 cm-1 have been reassigned to ν3 and combination modes of ν3+ν6 belonging to the 1a2→4p transition in contrast to earlier studies where they were assigned to a ν3 progression superimposed on the 3e→4p Rydberg transition. The assignments are further confirmed based on isotopic substitution studies on CDCl3 whose VUV photoabsorption spectrum is reported here for the first time. The frequencies of the ν3 and ν6 modes in the 4p Rydberg state of CHCl3 (CDCl3) are proposed to be ~454 (409) cm-1 and~130 (129) cm-1 respectively based on the vibronic analysis. DFT calculations of neutral and ionic ground state vibrational frequencies support the vibronic analysis. Experimental spectrum is found to be in good agreement with that predicted by TDDFT calculations. This work presents a consolidated analysis of the VUV photoabsorption spectrum of chloroform.

  13. The dynamics of high autoionizing Rydberg states of Ar

    NASA Astrophysics Data System (ADS)

    Bixon, M.; Jortner, Joshua

    1995-09-01

    In this paper we present a theoretical study of the autoionization dynamics of high 2P1/2np'[3/2]1 Rydbergs (with the principal quantum numbers n=100-280) of Ar in weak homogeneous electric fields (F=0.01-1.0 V/cm), which were experimentally interrogated by time-resolved zero-electron kinetic energy (ZEKE) spectroscopy [M. Mühlpfordt and U. Even, J. Chem. Phys. 103, 4427 (1995)], and which exhibit a marked dilution (i.e., ˜2 orders of magnitude lengthening) of the lifetimes relative to those inferred on the basis of the n3 scaling law for the spectral linewidths of the np' (n=12-24) Rydbergs. The multichannel effective Hamiltonian (Heff) with several doorway state(s) (for excitation and decay) and pure escape states (for decay) was advanced and utilized to treat the dynamics of the mixed Stark manifold of the ZEKE Rydbergs. Heff of dimension 2n-1 is then constructed for a n Rydberg manifold using independent experimental information on the (l dependent) quantum defects δ(l) and the (l, K, J dependent) decay widths, which are of the form Γ0(lKJ)/(n-δ(l))3, with Γ0(lKJ) being the decay widths constants. Here, l, K, and J are the azimuthal, the electronic and the total electronic angular momentum quantum numbers, respectively. Two coupling ranges are distinguished according to the strength of the reduced electric field F¯(n,p')=(F/V cm-1)n5/ 3.4×109[δ(p')(mod1)]. Range (A); The onset of the effective coupling of the doorway and escape states, i.e., 0.7≤F¯(n,p')≤2. Range (B); The strong mixing domain F¯(n,p')≥3. The lifetimes in range (B) can be well represented by a nearly democratic mixing of all the doorway and escape states (lKJ), with the average value <τ(n)>≂<τSM(n)>= 2n4ℏ/[J(lJK)Γ0(lJK)]. In range (B) <τ(n)> increases with increasing n and is only weakly F dependent. Range (A) is characterized by a hierarchy of two time scales for the decay, with a short decay component, which manifests the residue of the doorway state, and a

  14. Dissociative ionization of sodium molecules via repulsive Rydberg states

    NASA Astrophysics Data System (ADS)

    Chen, Hong

    In this thesis, an investigation of two color resonance multiphoton ionization (REMPI) and fragmentation processes in Na2 has been performed in combination with Linear Time-of-Flight Mass Spectrometry technique. The ionization and dissociative ionizations channels in the energy range up to 2500cm -1 above the dissociative ionization threshold into Na(3s)+Na ++e have been studied. After a mild supersonic expansion from the beam source, neutral sodium dimers in the ground state have been produced. Two tunable, pulsed lasers excite Na2 molecules via the intermediate A1S+u state to a single ro-vibrational level of the second intermediate 21pig state. Following absorption of a third photon, the total energy is above the dissociation limit into Na(3s) + Na+ + e. Typically, a small portion of atomic ions is produced under our experimental conditions. By varying the total available energy below and through the doubly excited states correlating with the Na(3p)+Na(4s) atom pair, there is no evidence that the doubly excited states positioned in the ionic continuum get involved. By calculation of the expected transition probabilities for all possible channels which can decay directly and indirectly into atomic ions, I find that direct dissociative ionization via 12S+u is impossible. The transition probabilities for dissociative ionization via the repulsive Rydberg states with principal quantum numbers n from 5˜12 converging toward the 12S+u state are three to four orders of magnitude larger than those for direct ionization into the continuum of the X2S+g ground state. These repulsive Rydberg states are much more likely to play a role in the photo-ionization through the intermediate 21Pg state. A semi-classical model which was originally developed for negative ion dissociative attachment (O'MAL'67) describes how dissociative ionization occurs along the repulsive Rydberg states. Its prediction concerning the ratio of atomic to molecular ion production as a function of initial

  15. Rydberg States of Lithium and Other Systems

    NASA Technical Reports Server (NTRS)

    Drachman, Richard J.

    1999-01-01

    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.

  16. Stark beats of Ar Rydberg states

    NASA Astrophysics Data System (ADS)

    Morioka, Y.; Aoto, T.; Yoshii, H.

    2001-11-01

    Vacuum ultraviolet fluorescence decay spectra of Ar atom resonance lines excited by pulsed vacuum ultraviolet light in a synchrotron single bunch operation were obtained under a static electric field. When an atom under the static electric field was excited simultaneously to both the magnetic sublevels M=0 and \\|M\\|=1 by polarized light and the observation area was asymmetric, Stark beats were observed in the fluorescent decay spectra. All observed beat frequencies varied proportionally to the square of the external electric field. The results for 8d and 9d doublet lines were compared with those obtained by the usual second order perturbation theory, assuming mixing ratios between three jl coupling scheme d-type states. The beat frequencies were also measured for other resonance lines.

  17. High Rydberg states of DABCO: Spectroscopy, ionization potential, and comparison with mass analyzed threshold ionization

    NASA Astrophysics Data System (ADS)

    Boogaarts, Maarten G. H.; Holleman, Iwan; Jongma, Rienk T.; Parker, David H.; Meijer, Gerard; Even, Uzi

    1996-03-01

    Doubly-resonant excitation/vibrational autoionization is used to accurately determine the ionization potential (IP) of the highly symmetric caged amine 1,4 diazabicyclo[2,2,2]octane (DABCO). The IP of DABCO excited with one quantum of the ν24(e') vibration lies at (59 048.62±0.03) cm-1, based on fitting 56 components of the npxy Rydberg series (δ=0.406±0.002) to the Rydberg formula. Rydberg state transition energies and linewidths are determined using standard calibration and linefitting techniques. The IP determined from Rydberg state extrapolation is compared with that determined by mass analyzed threshold ionization (MATI). Effects of static electric fields on MATI signals measured for the high Rydberg states are discussed.

  18. Deexcitation of high-Rydberg-state atoms with a chirped train of half-cycle pulses

    SciTech Connect

    Kopyciuk, T.; Parzynski, R.

    2007-05-15

    Encouraged by the experiments on production of antihydrogen atoms in high Rydberg states we have calculated the effect of deexcitation towards lower states by a chirped train of identical unidirectional half-cycle pulses. The calculations exploit both the one-dimensional and impulse approximations providing convenient analytical formulas for the Rydberg-to-Rydberg transition amplitudes. The calculated deexcitation is shown in terms of the mean value of localization of the Rydberg wave packet in the coordinate space, the Rydberg-state population distribution, the Husimi phase-space distribution function, and the probability density distribution, each of these measures vs the length of the applied train of half-cycle pulses. The results for chirped trains are compared with those for periodic trains and examples of higher deexcitation efficiency of the chirped trains are given.

  19. Measurement of the electronic momentum distributions of Rydberg Stark states

    SciTech Connect

    Murray-Krezan, J.; Jones, R. R.

    2007-06-15

    Approximate momentum distributions of Rydberg electrons in static electric fields have been obtained using an improved impulsive momentum retrieval (IMR) technique. An imaging detector enables the measurement of half-cycle pulse (HCP) ionization probability across the spatial profile of a focused half-cycle pulse beam. By modulating the HCP amplitude we directly measure the derivative of the ionization vs HCP impulse curve, enabling the recovery of momentum distributions with better resolution than previously demonstrated with IMR. For example, for Stark states with small dipole moments, we observe predicted fine-structure in the projection of the momentum distribution along the Stark field axis. We use a semiclassical model to simulate the effect that the nonzero HCP duration has on our measurements. Good agreement between simulated and measured momentum distributions is obtained.

  20. Lensing effect of electromagnetically induced transparency involving a Rydberg state

    NASA Astrophysics Data System (ADS)

    Han, Jingshan; Vogt, Thibault; Manjappa, Manukumara; Guo, Ruixiang; Kiffner, Martin; Li, Wenhui

    2015-12-01

    We study the lensing effect experienced by a weak probe field under conditions of electromagnetically induced transparency (EIT) involving a Rydberg state. A Gaussian coupling beam tightly focused on a laser-cooled atomic cloud produces an inhomogeneity in the coupling Rabi frequency along the transverse direction and makes the EIT area acting like a gradient-index medium. We image the probe beam at the position where it exits the atomic cloud and observe that a red-detuned probe light is strongly focused with a greatly enhanced intensity whereas a blue-detuned one is defocused with a reduced intensity. Our experimental results agree very well with the numerical solutions of Maxwell-Bloch equations.

  1. State-Mixing of nS Rydberg Atoms in an External Electric Field

    NASA Astrophysics Data System (ADS)

    Jiao, Yuechun; Wang, Limei; Zhang, Hao; Zhang, Linjie; Zhao, Jianming; Jia, Suotang

    2015-09-01

    State-mixing effect of ultracold nS cesium Rydberg atoms in an external electric field is investigated in a magneto-optical trap. Populated high-l Rydberg atoms due to the state-mixing through avoided crossings are measured with a state-selective field ionization technique. The measured transfer rates of high-l states increase with the electric field and get to the maximum at the field of about 3.0 V/cm for 49S1/2 Rydberg state, and show decrease behavior when the electric field increases further. The decrease behavior of the transfer rate is explained with the slower m-mixing effect caused by decreasing dipole-dipole interactions between high-l Rydberg atoms. During the m-mixing process the ultracold plasma is formed by the Penning ionization.

  2. A model for charge transfer in ultracold Rydberg ground-state atomic collisions

    NASA Astrophysics Data System (ADS)

    Markson, Samuel; Sadeghpour, H. R.

    2016-06-01

    In excited molecules, the interaction between the covalent Rydberg and ion-pair channels forms a unique class of excited states, in which the infinite manifold of vibrational levels are the equivalent of atomic Rydberg states with a heavy electron mass. Production of the ion-pair states usually requires excitation through one or several interacting Rydberg states; these interacting channels lead to loss of flux, diminishing the rate of ion-pair production. Here, we develop an analytical, asymptotic charge-transfer model for the interaction between ultracold Rydberg molecular states, and employ this method to demonstrate the utility of off-resonant field control over the ion-pair formation, with near unity efficiency.

  3. Electro-optic control of atom-light interactions using Rydberg dark-state polaritons

    NASA Astrophysics Data System (ADS)

    Bason, M. G.; Mohapatra, A. K.; Weatherill, K. J.; Adams, C. S.

    2008-03-01

    We demonstrate a multiphoton Rydberg dark resonance where a Λ system is coupled to a Rydberg state. This N -type level scheme combines the ability to slow and store light pulses associated with long-lived ground-state superpositions with the strongly interacting character of Rydberg states. For the nd5/2 Rydberg state in R87b (with n=26 or 44) and a beam size of 1 mm, we observe a resonance linewidth of less than 100 kHz in a room-temperature atomic ensemble limited by transit-time broadening. The resonance is switchable with an electric field of order 1Vcm-1 . Applications in electro-optic switching and photonic phase gates are discussed.

  4. Self-interaction corrected density functional calculations of molecular Rydberg states

    SciTech Connect

    Gudmundsdóttir, Hildur; Zhang, Yao; Weber, Peter M.; Jónsson, Hannes

    2013-11-21

    A method is presented for calculating the wave function and energy of Rydberg excited states of molecules. A good estimate of the Rydberg state orbital is obtained using ground state density functional theory including Perdew-Zunger self-interaction correction and an optimized effective potential. The total energy of the excited molecule is obtained using the Delta Self-Consistent Field method where an electron is removed from the highest occupied orbital and placed in the Rydberg orbital. Results are presented for the first few Rydberg states of NH{sub 3}, H{sub 2}O, H{sub 2}CO, C{sub 2}H{sub 4}, and N(CH{sub 3}){sub 3}. The mean absolute error in the energy of the 33 molecular Rydberg states presented here is 0.18 eV. The orbitals are represented on a real space grid, avoiding the dependence on diffuse atomic basis sets. As in standard density functional theory calculations, the computational effort scales as NM{sup 2} where N is the number of orbitals and M is the number of grid points included in the calculation. Due to the slow scaling of the computational effort with system size and the high level of parallelism in the real space grid approach, the method presented here makes it possible to estimate Rydberg electron binding energy in large molecules.

  5. Collective state synthesis in an optical cavity using Rydberg atom dipole blockade

    NASA Astrophysics Data System (ADS)

    Kumar, Santosh; Sheng, Jiteng; Sedlacek, Jonathon A.; Fan, Haoquan; Shaffer, James P.

    2016-03-01

    We investigate the coherent manipulation of interacting Rydberg atoms placed inside a high-finesse optical cavity for the deterministic preparation of strongly coupled light-matter systems. We consider a four-level diamond scheme with one common Rydberg level for N interacting atoms. One side of the diamond is used to excite the atoms into a collective ‘superatom’ Rydberg state using either π-pulses or stimulated Raman adiabatic passage (STIRAP) pulses. The upper transition on the other side of the diamond is used to transfer the collective state to one that is coupled to a field mode of an optical cavity. Due to the strong interaction between the atoms in the Rydberg level, the Rydberg blockade mechanism plays a key role in the deterministic quantum state synthesis of the atoms in the cavity. We use numerical simulation to show that non-classical states of light can be generated and that the state that is coupled to the cavity field is a collective one. We also investigate how different decay mechanisms affect this interacting many-body system. We also analyze our system in the case of two Rydberg excitations within the blockade volume. The simulations are carried out with parameters corresponding to realizable high-finesse optical cavities and alkali atoms like rubidium.

  6. Sub-Poissonian statistics of Rydberg-interacting dark-state polaritons.

    PubMed

    Hofmann, C S; Günter, G; Schempp, H; Robert-de-Saint-Vincent, M; Gärttner, M; Evers, J; Whitlock, S; Weidemüller, M

    2013-05-17

    We observe individual dark-state polaritons as they propagate through an ultracold atomic gas involving Rydberg states coupled via an electromagnetically induced transparency resonance. Strong long-range interactions between Rydberg excitations give rise to a blockade between polaritons, resulting in large optical nonlinearities and modified polariton number statistics. By combining optical imaging and high-fidelity detection of the Rydberg polaritons we investigate both aspects of this coupled atom-light system. We map out the full nonlinear optical response as a function of atomic density and follow the temporal evolution of polaritons through the atomic cloud. In the blockade regime, the statistical fluctuations of the polariton number drop well below the quantum noise limit. The low level of fluctuations indicates that photon correlations modified by the strong interactions have a significant backaction on the Rydberg atom statistics. PMID:25167407

  7. Polarization Measurements of the Resonant Multiphoton Ionization Spectrum of the 3 s Rydberg States of Monomethylpyridines

    NASA Astrophysics Data System (ADS)

    Kosmidis, C.; Bolovinos, A.; Tsekeris, P.

    1993-07-01

    The circular to linear polarization ratio for the two-photon excitation of the 3 s Rydberg states of monomethylpyridines has been measured by 2 + 1 resonant MPI spectroscopy in a static cell. The symmetry of the Rydberg vibrational bands is deduced and the results from the 0-0 transition suggest that the highest occupied MO of 4-methylpyridine is an n MO, while that for 2- and 3-methylpyridines is a π-type one.

  8. Predissociation of high-lying Rydberg states of molecular iodine via ion-pair states

    SciTech Connect

    Bogomolov, Alexandr S.; Grüner, Barbara; Mudrich, Marcel; Kochubei, Sergei A.; Baklanov, Alexey V.

    2014-03-28

    Velocity map imaging of the photofragments arising from two-photon photoexcitation of molecular iodine in the energy range 73 500–74 500 cm{sup −1} covering the bands of high-lying gerade Rydberg states [{sup 2}Π{sub 1/2}]{sub c}6d;0{sub g}{sup +} and [{sup 2}Π{sub 1/2}]{sub c}6d;2{sub g} has been applied. The ion signal was dominated by the atomic fragment ion I{sup +}. Up to 5 dissociation channels yielding I{sup +} ions with different kinetic energies were observed when the I{sub 2} molecule was excited within discrete peaks of Rydberg states and their satellites in this region. One of these channels gives rise to images of I{sup +} and I{sup −} ions with equal kinetic energy indicating predissociation of I{sub 2} via ion-pair states. The contribution of this channel was up to about 50% of the total I{sup +} signal. The four other channels correspond to predissociation via lower lying Rydberg states giving rise to excited iodine atoms providing I{sup +} ions by subsequent one-photon ionization by the same laser pulse. The ratio of these channels varied from peak to peak in the spectrum but their total ionic signal was always much higher than the signal of (2 + 1) resonance enhanced multi-photon ionization of I{sub 2}, which was previously considered to be the origin of ionic signal in this spectral range. The first-tier E0{sub g}{sup +} and D{sup ′}2{sub g} ion-pair states are concluded to be responsible for predissociation of Rydberg states [{sup 2}Π{sub 1/2}]{sub c}6d;0{sub g}{sup +} and [{sup 2}Π{sub 1/2}]{sub c}6d;2{sub g}, respectively. Further predissociation of these ion-pair states via lower lying Rydberg states gives rise to excited I(5s{sup 2}5p{sup 4}6s{sup 1}) atoms responsible for major part of ion signal. The isotropic angular distribution of the photofragment recoil directions observed for all channels indicates that the studied Rydberg states are long-lived compared with the rotational period of the I{sub 2} molecule.

  9. Role of ion-pair states in the predissociation dynamics of Rydberg states of molecular iodine.

    PubMed

    von Vangerow, J; Bogomolov, A S; Dozmorov, N V; Schomas, D; Stienkemeier, F; Baklanov, A V; Mudrich, M

    2016-07-28

    Using femtosecond pump-probe ion imaging spectroscopy, we establish the key role of I(+) + I(-) ion-pair (IP) states in the predissociation dynamics of molecular iodine I2 excited to Rydberg states. Two-photon excitation of Rydberg states lying above the lowest IP state dissociation threshold (1st tier) is found to be followed by direct parallel transitions into IP states of the 1st tier asymptotically correlating to a pair of I ions in their lowest states I(+)((3)P2) + I(-)((1)S0), of the 2nd tier correlating to I(+)((3)P0) + I(-)((1)S0), and of the 3rd tier correlating to I(+)((1)D2) + I(-)((1)S0). Predissociation via the 1st tier proceeds presumably with a delay of 1.6-1.7 ps which is close to the vibrational period in the 3rd tier state (3rd tier-mediated process). The 2nd tier IP state is concluded to be the main precursor for predissociation via lower lying Rydberg states proceeding with a characteristic time of 7-8 ps and giving rise to Rydberg atoms I(5s(2)5p(4)6s(1)). The channel generating I((2)P3/2) + I((2)P1/2) atoms with total kinetic energy corresponding to one-photon excitation is found to proceed via a pump - dump mechanism with dramatic change of angular anisotropy of this channel as compared with earlier nanosecond experiments. PMID:27353150

  10. Generation of tunable coherent far-infrared radiation using atomic Rydberg states

    SciTech Connect

    Bookless, W.

    1980-12-01

    A source of tunable far-infrared radiation has been constructed. The system has been operated at 91.6 cm/sup -1/ with a demonstrated tunability of .63 cm/sup -1/. The system is based on a Rydberg state transition in optically pumped potassium vapor. The transition energy is tuned by the application of an electric field to the excited vapor. The transition wavelength and the shifted wavelength were detected and measured by the use of a Michelson interferometer and a liquid helium cooled Ga:Ge bolometer and the data was reduced using Fast Fourier transform techniques. Extensive spectroscopy was done on the potassium vapor to elucidate the depopulation paths and rates of the excited levels. Both theoretical and experimental results are presented to support the conclusions of the research effort. Additionally, possible alternative approaches to the population of the excited state are explored and recommendations are made for the future development of this source as well as the potential uses of it in molecular spectroscopy.

  11. Observation of g/u-symmetry mixing in the high-n Rydberg states of HD

    NASA Astrophysics Data System (ADS)

    Sprecher, Daniel; Merkt, Frédéric

    2014-03-01

    The structure and dynamics of high-n Rydberg states belonging to series converging to the (v+ = 0, N+ = 0-2) levels of the X^+ ^2Σ _g^+ electronic ground state of HD+ were studied by high-resolution spectroscopy from the GK ^1Σ _g^+ (v = 1, N = 1) state under field-free conditions. Three effects of g/u-symmetry breaking were detected: (i) Single-photon transitions from the GK (v = 1, N = 1) state of gerade symmetry to the 30d21 and 31g22 Rydberg states of gerade symmetry were observed after careful compensation of the stray electric fields. (ii) The singlet 61p12 Rydberg state of ungerade symmetry was found to autoionize to the N+ = 0, ℓ = 2 ionization continuum of gerade symmetry with a lifetime of 77(10) ns. (iii) Shifts of up to 20 MHz induced by g/u-symmetry mixing were measured for members of the np11 Rydberg series which lie close to nd21 Rydberg states. These observations were analyzed in the framework of multichannel quantum-defect theory. From the observed level shifts, the off-diagonal eigenquantum-defect element μ _pd of singlet-π symmetry was determined to be 0.0023(3) and the corresponding autoionization dynamics could be characterized. The ionization energy of the GK (v = 1, N = 1) state of HD was determined to be 12 710.544 23(10) cm-1.

  12. Time Evolution of High-l Stark States in Cold Rydberg Atoms

    NASA Astrophysics Data System (ADS)

    Wang, Limei; Zhang, Hao; Zhang, Linjie; Wang, Yong; Bao, Shanxia; Li, Changyong; Zhao, Jianming; Jia, Suotang

    2014-11-01

    The high-l Rydberg Stark states are populated by the state transfer from initial prepared nS Rydberg state via avoided crossings induced by a weak electric-field pulse, and investigated by the state selective field ionization method in a cesium standard magneto-optical trap. The dependences of the transfer rate, given by the ratio of the number of high-l Stark states to all atoms, on the strength and holding time of electric-field pulse are investigated and compared with those with additional ions. The results show that the time evolution of high-l Stark states strongly depends on the electric-field strength, and is affected by the additional ions at relatively weaker field (1.51 V/cm here). The density of Rydberg atoms has a minor effect on the characteristic time of evolution process.

  13. Millimeter Wave Spectroscopy of Rydberg States of Molecules in the Region of 260-295 GHz

    NASA Astrophysics Data System (ADS)

    Grimes, David; Zhou, Yan; Barnum, Timothy J.; Field, Robert W.

    2015-06-01

    Free induction decay detected chirped pulse millimeter wave spectroscopy of Rydberg-Rydberg transitions in atoms and molecules is a powerful and flexible method for characterizing the electronic structure of Rydberg states and determining the structure and dynamics of the ion-core. Complicating the use of this technique are the difficulties in reliably and repeatedly accessing not just the most information rich core-nonpenetrating states, but also the low-ℓ core-penetrating Rydberg states in the area of principal quantum number n* >35. Small transition moments and narrow linewidths for transitions between valence electronic states and high Rydberg states are the primary limiting factor. We demonstrate a simple method to avoid the problem entirely by using chirped pulse technology operating in the frequency range of 260-295 GHz, which allows us to sample a lower range of n* values than before with comparable frequency resolution and accuracy as our previous W-band experiments. Further improvements to our experiment in order to accurately capture details of Stark demolition, a technique that provides rapid differentiation between core-penetrating and core-nonpenetrating states, will also be discussed.

  14. Two-color photoexcitation of Rydberg states via an electric quadrupole transition

    SciTech Connect

    Li Leping; Gu Quanli; Knee, J. L.; Wright, J. D.; DiSciacca, J. M.; Morgan, T. J.

    2008-03-15

    We report the observation of an electric quadrupole transition between the 4s{sup '}[1/2]{sub 0}{sup o} and 3d[3/2]{sub 2}{sup o} states in the spectrum of argon and use it in the first step of a scheme to excite Rydberg states. The initial identification of the transition is based on one-color, two-photon photoionization. A different experiment utilizing two-color, two-photon photoexcitation to Rydberg states confirms the identification. Despite the unavoidable background of one-color, two-photon photoionization, the latter experimental technique makes possible two-photon spectroscopy of Rydberg states using a resonant intermediate state populated by an electric quadrupole transition.

  15. UV + V UV double-resonance studies of autoionizing Rydberg states of the hydroxyl radical

    NASA Astrophysics Data System (ADS)

    Green, Amy M.; Liu, Fang; Lester, Marsha I.

    2016-05-01

    The hydroxyl radical (OH) is a key oxidant in atmospheric and combustion chemistry. Recently, a sensitive and state-selective ionization method has been developed for detection of the OH radical that utilizes UV excitation on the A2Σ+-X2Π transition followed by fixed 118 nm vacuum ultraviolet (VUV) radiation to access autoionizing Rydberg states [J. M. Beames et al., J. Chem. Phys. 134, 241102 (2011)]. The present study uses tunable VUV radiation generated by four-wave mixing to examine the origin of the enhanced ionization efficiency observed for OH radicals prepared in specific A2Σ+ intermediate levels. The enhancement is shown to arise from resonant excitation to distinct rotational and fine structure levels of two newly identified 2Π Rydberg states with an A3Π cationic core and a 3d electron followed by ionization. Spectroscopic constants are derived and effects due to uncoupling of the Rydberg electron are revealed for the OH 2Π Rydberg states. The linewidths indicate a Rydberg state lifetime due to autoionization on the order of a picosecond.

  16. UV + V UV double-resonance studies of autoionizing Rydberg states of the hydroxyl radical.

    PubMed

    Green, Amy M; Liu, Fang; Lester, Marsha I

    2016-05-14

    The hydroxyl radical (OH) is a key oxidant in atmospheric and combustion chemistry. Recently, a sensitive and state-selective ionization method has been developed for detection of the OH radical that utilizes UV excitation on the A(2)Σ(+)-X(2)Π transition followed by fixed 118 nm vacuum ultraviolet (VUV) radiation to access autoionizing Rydberg states [J. M. Beames et al., J. Chem. Phys. 134, 241102 (2011)]. The present study uses tunable VUV radiation generated by four-wave mixing to examine the origin of the enhanced ionization efficiency observed for OH radicals prepared in specific A(2)Σ(+) intermediate levels. The enhancement is shown to arise from resonant excitation to distinct rotational and fine structure levels of two newly identified (2)Π Rydberg states with an A(3)Π cationic core and a 3d electron followed by ionization. Spectroscopic constants are derived and effects due to uncoupling of the Rydberg electron are revealed for the OH (2)Π Rydberg states. The linewidths indicate a Rydberg state lifetime due to autoionization on the order of a picosecond. PMID:27179488

  17. The interaction potential of NO-H2 in ground and A Rydberg state

    NASA Astrophysics Data System (ADS)

    Pajón-Suárez, Pedro; Valentín-Rodríguez, Mónica; Hernández-Lamoneda, Ramón

    2016-08-01

    The interaction potential for the ground and A Rydberg state of NO-H2 has been calculated using high level ab initio methods. The complex is very floppy in nature and large amplitude motions are expected to characterize its dynamics. The ground state is characterized by two very close-lying states which exhibit crossings. By analogy with other complexes the Rydberg state is characterized by much smaller well depth and larger intermolecular distance. We compare with model potentials used in previous molecular dynamics simulations of photoexcitation and relaxation and conclude on the importance of performing new studies.

  18. Interacting Rydberg atoms in an optical cavity to synthesize coherent collective states using dipole blockade

    NASA Astrophysics Data System (ADS)

    Kumar, Santosh; Sheng, Jiteng; Sedlacek, Jonathon; Ewel, Charlie; Fan, Haoquan; Shaffer, James

    2015-05-01

    We investigate the coherent manipulation of interacting Rydberg atoms placed inside a high-finesse optical cavity for the preparation of strongly coupled light-matter systems. We consider a four-level diamond scheme with one common Rydberg level. One side of the diamond is used to collectively excite the atoms to the Rydberg level using a pair of pulses. The other side of the diamond is used to produce a collective state that is close to resonance with a field mode of a high-finesse optical cavity. The interaction between Rydberg atoms creates a blockade which is useful for synthesizing the coherent collective state. We use numerical simulation to generate non-classical states of light and also investigate different decay mechanisms affecting this system. We also analyze our system in the case of two Rydberg excitations within the blockade volume. In this case, we show that more elaborate few excitation quantum states can be prepared in the cavity to observe interesting dynamics and analyze the correlation of the two-photon emission. This work is supported by the DARPA Quasar program by a grant through ARO, AFOSR and NSF.

  19. Possibility of triple magic trapping of clock and Rydberg states of divalent atoms in optical lattices

    NASA Astrophysics Data System (ADS)

    Topcu, T.; Derevianko, A.

    2016-07-01

    We predict the possibility of ‘triply magic’ optical lattice trapping of neutral divalent atoms. In such a lattice, the {}1{{{S}}}0 and {}3{{{P}}}0 clock states and an additional Rydberg state experience identical optical potentials, fully mitigating detrimental effects of the motional decoherence. In particular, we show that this triply magic trapping condition can be satisfied for Yb atom at optical wavelengths and for various other divalent systems (Ca, Mg, Hg and Sr) in the UV region. We assess the quality of triple magic trapping conditions by estimating the probability of excitation out of the motional ground state as a result of the excitations between the clock and the Rydberg states. We also calculate trapping laser-induced photoionization rates of divalent Rydberg atoms at magic frequencies. We find that such rates are below the radiative spontaneous-emission rates, due to the presence of Cooper minima in photoionization cross-sections.

  20. Vibrational Autoionization and Predissociation in High Rydberg States of Nitric Oxide

    NASA Astrophysics Data System (ADS)

    Pratt, S. T.

    1998-05-01

    New results on the competition between autoionization and predissociation in the high Rydberg states of NO are presented. These results provide insight into the earlier work of H. Park et al. [Phys. Rev. Lett. 76, 1591 (1996)] that show evidence for substantial mixing between Rydberg series and ionization continua with even and odd orbital angular momenta. New data based on fluorescence-dip spectroscopy, detection of neutral predissociation products, and photoelectron spectroscopy suggest that the A' ^2Σ ^+ and I ^2Σ ^+ dissociative valence states play an important role in this mixing. As an example, the ionization and dissociation efficiencies of the nf levels are found to depend strongly on whether the total angular momentum minus spin, N, is even or odd, indicating predissociation via a ^2Σ ^+ state. Zeeman splittings observed in a magnetic bottle electron spectrometer also result in an improvement in the assignment of these high Rydberg states.

  1. Collisional and electric-field ionization of laser-prepared Rydberg states in an ion trap mass spectrometer

    SciTech Connect

    Ramsey, J.M.; Whitten, W.B.; Goeringer, D.E.; Buckley, B.T.

    1990-01-01

    Rydberg states of rubidium are selectively generated by one and two photon laser excitation in a quadrupole ion trap mass spectrometer. Collisional and electric-field ionization is investigated in trapping device. CCl{sub 4} is studied as a target for ionization of Rydberg states through electron attachment.

  2. Long-range quantum gate via Rydberg states of atoms in a thermal microwave cavity

    NASA Astrophysics Data System (ADS)

    Sárkány, Lőrinc; Fortágh, József; Petrosyan, David

    2015-09-01

    We propose an implementation of a universal quantum gate between pairs of spatially separated atoms in a microwave cavity at finite temperature. The gate results from reversible laser excitation of Rydberg states of atoms interacting with each other via exchange of virtual photons through a common cavity mode. Quantum interference of different transition paths between the two-atom ground and double-excited Rydberg states makes both the transition amplitude and resonance largely insensitive to the excitations in the microwave cavity quantum bus which can therefore be in any superposition or mixture of photon number states. Our scheme for attaining ultra-long-range interactions and entanglement also applies to mesoscopic atomic ensembles in the Rydberg blockade regime and is scalable to many ensembles trapped within a centimeter-sized microwave resonator.

  3. Vibrational autoionization and predissociation in high Rydberg states of nitric oxide

    NASA Astrophysics Data System (ADS)

    Pratt, S. T.

    1998-05-01

    New results on the competition between autoionization and predissociation in the high Rydberg states of nitric oxide are presented. These results provide insight into the earlier work of Park et al. [Phys. Rev. Lett. 76, 1591 (1996)] that shows evidence for substantial mixing between Rydberg series and ionization continua with even and odd orbital angular momenta (l). New data based on fluorescence-dip spectroscopy, detection of neutral predissociation products, and photoelectron spectroscopy suggest that the A' 2Σ+ and I 2Σ+ dissociative valence states play an important role in this l mixing. Zeeman splittings observed in a magnetic bottle electron spectrometer also result in an improvement in the assignment of these high Rydberg states.

  4. Vibrational autoionization and predissociation in high Rydberg states of nitric oxide

    SciTech Connect

    Pratt, S.T.

    1998-05-01

    New results on the competition between autoionization and predissociation in the high Rydberg states of nitric oxide are presented. These results provide insight into the earlier work of Park {ital et al.} [Phys. Rev. Lett. {bold 76}, 1591 (1996)] that shows evidence for substantial mixing between Rydberg series and ionization continua with even and odd orbital angular momenta (l). New data based on fluorescence-dip spectroscopy, detection of neutral predissociation products, and photoelectron spectroscopy suggest that the A{sup {prime}}{sup 2}{Sigma}{sup +} and I{sup 2}{Sigma}{sup +} dissociative valence states play an important role in this l mixing. Zeeman splittings observed in a magnetic bottle electron spectrometer also result in an improvement in the assignment of these high Rydberg states. {copyright} {ital 1998 American Institute of Physics.}

  5. Van der Waals interactions among alkali Rydberg atoms with excitonic states

    NASA Astrophysics Data System (ADS)

    Zoubi, Hashem

    2015-09-01

    We investigate the influence of the appearance of excitonic states on van der Waals interactions among two Rydberg atoms. The atoms are assumed to be in different Rydberg states, e.g., in the | {ns}> and | {np}> states. The resonant dipole-dipole interactions yield symmetric and antisymmetric excitons, with energy splitting that give rise to new resonances as the atoms approach each other. Only away from these resonances can the van der Waals coefficients, C6sp, be defined. We calculate the C6 coefficients for alkali atoms and present the results for lithium by applying perturbation theory. At short interatomic distances of several μ {{m}}, we show that the widely used simple model of two-level systems for excitons in Rydberg atoms breaks down, and the correct representation implies multi-level atoms. Even though, at larger distances one can keep the two-level systems but in including van der Waals interactions among the atoms .

  6. Photodissociation Efficiency Spectroscopy Study of the Rydberg Excited Ion-Pair States of Carbon Dioxide

    NASA Astrophysics Data System (ADS)

    Feng, Qiang; Xu, Yun-Feng; Sun, Jin-Da; Tian, Shan-Xi; Shan, Xiao-Bin; Liu, Fu-Yi; Sheng, Liu-Si

    2009-10-01

    Photodissociation efficiency spectrum of anionic oxygen atom produced via ion-pair dissociations of carbon dioxide is recorded by means of the synchrotron radiation excitation (XUV photon energy 17.40-20.00 eV). The present spectrum is assigned as the Rydberg-like excited ion-pair states, i.e., Tanaka-Ogawa and Henning series, tilde C2Σg+ (CO+2) vibrational ground-state and excitation series. Three Rydberg series, npσu, npπu, and nfu, converging to tilde C2Σg+ (0, 0, 0), show the higher cross sections.

  7. GHz Rabi Flopping to Rydberg States in Hot Atomic Vapor Cells

    SciTech Connect

    Huber, B.; Baluktsian, T.; Schlagmueller, M.; Koelle, A.; Kuebler, H.; Loew, R.; Pfau, T.

    2011-12-09

    We report on the observation of Rabi oscillations to a Rydberg state on a time scale below 1 ns in thermal rubidium vapor. We use a bandwidth-limited pulsed excitation and observe up to 6 full Rabi cycles within a pulse duration of {approx}4 ns. We find good agreement between the experiment and numerical simulations based on a surprisingly simple model. This result shows that fully coherent dynamics with Rydberg states can be achieved even in thermal atomic vapor, thus suggesting small vapor cells as a platform for room-temperature quantum devices. Furthermore, the result implies that previous coherent dynamics in single-atom Rydberg gates can be accelerated by 3 orders of magnitude.

  8. Doppler- and recoil-free laser excitation of Rydberg states via three-photon transitions

    SciTech Connect

    Ryabtsev, I. I.; Beterov, I. I.; Tretyakov, D. B.; Entin, V. M.; Yakshina, E. A.

    2011-11-15

    Three-photon laser excitation of Rydberg states by three different laser beams can be arranged in a starlike geometry that simultaneously eliminates the recoil effect and Doppler broadening. Our analytical and numerical calculations for a particular laser excitation scheme 5S{sub 1/2}{yields}5P{sub 3/2}{yields}6S{sub 1/2}{yields}nP in Rb atoms have shown that, compared to the one- and two-photon laser excitation, this approach provides much narrower linewidth and longer coherence time for both cold atom samples and hot vapors, if the intermediate one-photon resonances of the three-photon transition are detuned by more than respective single-photon Doppler widths. This method can be used to improve fidelity of Rydberg quantum gates and precision of spectroscopic measurements in Rydberg atoms.

  9. Many-body physics of Rydberg dark-state polaritons in the strongly interacting regime

    NASA Astrophysics Data System (ADS)

    Moos, Matthias; Höning, Michael; Unanyan, Razmik; Fleischhauer, Michael

    2015-11-01

    Coupling light to Rydberg states of atoms under conditions of electromagnetically induced transparency (EIT) leads to the formation of interacting quasiparticles, termed Rydberg polaritons. We derive a one-dimensional model describing the time evolution of these polaritons under paraxial propagation conditions. Specifically, we obtain a master equation governing the dynamics of Rydberg polaritons and identify conditions when it can essentially be described by an effective Hamiltonian of a single-species polariton. We verify this Hamiltonian by numerical two-excitation simulations. Under typical stationary EIT conditions it is impossible to reach the strongly interacting regime where long-range density-density correlations emerge. In contrast, by employing the time dependence of the control field the regime of strong interactions can be reached where the polaritons attain quasicrystalline order. We provide a physical explanation for the differences between stationary and time-dependent schemes.

  10. Multiphoton Ionization Dynamics of Strontium Rydberg States in Intense Femtosecond Pulses

    NASA Astrophysics Data System (ADS)

    Tate, D. A.; Gallagher, T. F.

    1997-04-01

    We are investigating multiphoton ionization of Sr 5snl Rydberg states by intense 150 fs pulses. Specifically, we excite the 5snd 20 < n < ∞ states using two ns lasers at 460.9 nm and 420 - 412 nm. These states are then irradiated with the fs pulses which are produced by a mode-locked, regeneratively amplified Ti:Sapphire laser. The laser is tunable between 790 nm and 844 nm, and the pulses are frequency doubled to produce light from 395 - 422 nm. In contrast with a previous experiment, which used ps laser pulses,(H. Stapelfeldt, D.G. Papaioannou, L.D. Noordam, and T.F. Gallagher, Phys. Rev. A, 67, 3223 (1991).) our preliminary results indicate that excitation of Sr^+ Rydberg states and Sr^2+ photoions is relatively insensitive to the fs laser wavelength. We detect both species when the fs pulses are tuned to the 5s arrow 8p (398 nm) and 5s arrow 5f (422 nm) three photon resonances in Sr^+. In addition, we have generated Sr^+ Rydberg states and Sr^2+ using the laser fundamental at 796 nm, though when the laser is tuned to 844nm, the Sr^+ Rydberg states are no longer excited. We will present a systematic experimental study of the ionization process and discuss our results in terms of Floquet theory.

  11. Spin-charge separation of dark-state polaritons in a Rydberg medium

    NASA Astrophysics Data System (ADS)

    Shi, Xiao-Feng; Svetlichnyy, P.; Kennedy, T. A. B.

    2016-04-01

    The propagation of light fields through a quasi one-dimensional cold atomic gas, exciting atomic Rydberg levels of large principal quantum number under conditions of electromagnetically induced transparency, can lead to a stable two-mode Luttinger liquid system. Atomic van der Waals interactions induce a coupling of bosonic field modes that display both photonic and atomic character, the Rydberg dark-state polaritons (RDPs). It is shown that by tunable control of the van der Waals coupling, the RDP may decouple into independent ‘spin’ and ‘charge’ fields which propagate at different speeds, analogous to spin-charge separation of electrons in a one-dimensional metal.

  12. Vibrational modes in excited Rydberg states of acetone: A computational study

    NASA Astrophysics Data System (ADS)

    Shastri, Aparna; Singh, Param Jeet

    2016-04-01

    Computational studies of electronically excited states of the acetone molecule [(CH3)2CO] and its fully deuterated isotopologue [(CD3)2CO] are performed using the time dependent density functional (TDDFT) methodology. In addition to vertical excitation energies for singlet and triplet states, equilibrium geometries and vibrational frequencies of the n=3 Rydberg states (3s, 3p and 3d) are obtained. This is the first report of geometry optimization and frequency calculations for the 3px, 3pz, 3dyz, 3dxy, 3dxz, 3dx2-y2 and 3dz2 Rydberg states. Results of the geometry optimization indicate that the molecule retains approximate C2V geometry in most of these excited Rydberg states, with the most significant structural change seen in the CCO bond angle which is found to be reduced from the ground state value. Detailed comparison of the computationally predicted vibrational wavenumbers with experimental studies helps to confirm several of the earlier vibronic assignments while leading to revised/new assignments for some of the bands. The important role of hot bands in analysis of the room temperature photoabsorption spectra of acetone is corroborated by this study. While the vibrational frequencies in excited Rydberg states are overall found to be close to those of the ionic ground state, geometry optimization and vibrational frequency computation for each excited state proves to be very useful to arrive at a consistent set of vibronic assignments. Isotopic substitution helps in consolidating and confirming assignments. An offshoot of this study is the interpretation of the band at ~8.47 eV as the π-3s Rydberg transition converging to the second ionization potential.

  13. Photoionization indicators of optical mixing of different-parity degenerate Rydberg states

    NASA Astrophysics Data System (ADS)

    Parzyński, R.; Sobczak, M.; Wójcik, A.

    2000-02-01

    We discuss a photoionization version of the photoexcitation model of Corless and Stroud [Phys. Rev. Lett. 79, 637 (1997)]. In the photoexcitation model, a np hydrogenic state of n>>1 was excited from the ground 1s state and the excited population was allowed to migrate to other angular momentum states within the one n only due to strongly nonresonant electric-dipole \\|Δn\\|=0, \\|Δl\\|=1 Rydberg-to-Rydberg couplings. When, as is the essence of the photoexcitation model, the same one n-manifold approximation is made in the model of high-n Rydberg-state photoionization, a number of interesting photoionization effects are obtained. Among them, the most spectacular seems to be the emission of photoelectrons in the ``forbidden'' directions and the suppression of ionization when compared to the Fermi golden rule predictions. However, we show on the basis of an approximate analysis that these photoionization effects can be strongly diminished when additional n manifolds around the selected one are included in the model. Thus, we conclude that the one n-manifold approximation overestimates results when applied to the problem of high-n Rydberg-state photoionization.

  14. Observation of g/u-symmetry mixing in the high-n Rydberg states of HD

    SciTech Connect

    Sprecher, Daniel; Merkt, Frédéric

    2014-03-28

    The structure and dynamics of high-n Rydberg states belonging to series converging to the (v{sup +} = 0, N{sup +} = 0–2) levels of the X{sup +2}Σ{sub g}{sup +} electronic ground state of HD{sup +} were studied by high-resolution spectroscopy from the GK{sup 1}Σ{sub g}{sup +} (v= 1, N = 1) state under field-free conditions. Three effects of g/u-symmetry breaking were detected: (i) Single-photon transitions from the GK (v = 1, N = 1) state of gerade symmetry to the 30d2{sub 1} and 31g2{sub 2} Rydberg states of gerade symmetry were observed after careful compensation of the stray electric fields. (ii) The singlet 61p1{sub 2} Rydberg state of ungerade symmetry was found to autoionize to the N{sup +} = 0, ℓ = 2 ionization continuum of gerade symmetry with a lifetime of 77(10) ns. (iii) Shifts of up to 20 MHz induced by g/u-symmetry mixing were measured for members of the np1{sub 1} Rydberg series which lie close to nd2{sub 1} Rydberg states. These observations were analyzed in the framework of multichannel quantum-defect theory. From the observed level shifts, the off-diagonal eigenquantum-defect element μ{sub pd} of singlet-π symmetry was determined to be 0.0023(3) and the corresponding autoionization dynamics could be characterized. The ionization energy of the GK (v = 1, N = 1) state of HD was determined to be 12 710.544 23(10) cm{sup −1}.

  15. Field ionization process of Eu 4f76snp Rydberg states

    NASA Astrophysics Data System (ADS)

    Zhang, Jing; Shen, Li; Dai, Chang-Jian

    2015-11-01

    The field ionization process of the Eu 4f76snp Rydberg states, converging to the first ionization limit, 4f76s 9S4, is systematically investigated. The spectra of the Eu 4f76snp Rydberg states are populated with three-step laser excitation, and detected by electric field ionization (EFI) method. Two different kinds of the EFI pulses are applied after laser excitation to observe the possible impacts on the EFI process. The exact EFI ionization thresholds for the 4f76snp Rydberg states can be determined by observing the corresponding EFI spectra. In particular, some structures above the EFI threshold are found in the EFI spectra, which may be interpreted as the effect from black body radiation (BBR). Finally, the scaling law of the EFI threshold for the Eu 4f76snp Rydberg states with the effective quantum number is built. Project supported by the National Natural Science Foundation of China (Grant Nos. 11004151 and 11174218).

  16. Solvent interaction with the (2p3s) Rydberg state of hexamethylenetetramine: Energetics and relaxation dynamics

    NASA Astrophysics Data System (ADS)

    Shang, Q. Y.; Dion, C.; Bernstein, E. R.

    1994-07-01

    The (1+1) mass resolved excitation spectra are reported for the (2p3s)←(2p)2 Rydberg transition of the tricyclic, high symmetry molecule hexamethylenetetramine [HMT (C6H12N4)] and its van der Waals clusters. The solvent molecules employed include both nonpolar (Ar, CH4) and polar (NH3, CH3OCH3) species. HMT and its clusters are generated and cooled in a supersonic expansion. The observed electronic transition is assigned as T2←A1 within the Td print group. A transition blue shift of 52 cm-1 for each Ar atom and 65 cm-1 for each methane molecule in the HMT van der Waals cluster is characterized. These shifts are caused by an excited state repulsive interaction between the excited Rydberg electron and the closed shell solvent which reduces the attractive dispersion interaction between the HMT and nonpolar solvent species in the van der Waals cluster. A transition red shift of more than 600 cm-1 for NH3 and CH3OCH3 solvent/HMT clusters is observed; this large increase in interaction energy for the excited Rydberg state of HMT with respect to the ground state of HMT is associated with the delocalization of the excited electron into available (virtual) Rydberg orbitals of the solvent molecules. The interaction is characterized as an electron transfer interaction. These results and assignments are consistent with previously reported ones for DABCO/solvent clusters. Relaxation dynamics of excited HMT and its clusters are investigated via a pump/probe (ionization) technique. Relaxation of the clusters is dominated by an intersystem crossing mechanism resulting in an excited state singlet lifetime of ˜5 ns compared to a bare molecule HMT excited state lifetime of ˜1.0 μs. A triplet state of HMT lies 255 cm-1 below the first excited singlet Rydberg state as determined by two-color threshold ionization studies.

  17. Equation of state of metallic helium

    SciTech Connect

    Shvets, V. T.

    2013-01-15

    The effective ion-ion interaction, free energy, pressure, and electric resistance of metallic liquid helium have been calculated in wide density and temperature ranges using perturbation theory in the electron-ion interaction potential. In the case of conduction electrons, the exchange interaction has been taken into account in the random-phase approximation and correlations have been taken into account in the local-field approximation. The solid-sphere model has been used for the nuclear subsystem. The diameter of these spheres is the only parameter of this theory. The diameter and density of the system at which the transition of helium from the singly ionized to doubly ionized state occurs have been estimated by analyzing the pair effective interaction between helium atoms. The case of doubly ionized helium atoms has been considered. Terms up to the third order of perturbation theory have been taken into account in the numerical calculations. The contribution of the third-order term is significant in all cases. The electric resistance and its temperature dependence for metallic helium are characteristic of simple divalent metals in the liquid state. The thermodynamic parameters-temperature and pressure densities-are within the ranges characteristic of the central regions of giant planets. This makes it possible to assume the existence of helium in the metallic state within the solar system.

  18. Photofragmentation, state interaction, and energetics of Rydberg and ion-pair states: Resonance enhanced multiphoton ionization of HI

    SciTech Connect

    Hróðmarsson, Helgi Rafn; Wang, Huasheng; Kvaran, Ágúst

    2014-06-28

    Mass resolved resonance enhanced multiphoton ionization data for hydrogen iodide (HI), for two-photon resonance excitation to Rydberg and ion-pair states in the 69 600–72 400 cm{sup −1} region were recorded and analyzed. Spectral perturbations due to homogeneous and heterogeneous interactions between Rydberg and ion-pair states, showing as deformations in line-positions, line-intensities, and line-widths, were focused on. Parameters relevant to photodissociation processes, state interaction strengths and spectroscopic parameters for deperturbed states were derived. Overall interaction and dynamical schemes to describe the observations are proposed.

  19. Comparative study on atomic and molecular Rydberg-state excitation in strong infrared laser fields

    NASA Astrophysics Data System (ADS)

    Lv, Hang; Zuo, Wanlong; Zhao, Lei; Xu, Haifeng; Jin, Mingxing; Ding, Dajun; Hu, Shilin; Chen, Jing

    2016-03-01

    Rydberg-state excitation of atoms in strong infrared laser fields provides a new complementary aspect of the perspective of atom-strong field interactions. In this article, we perform an experimental and theoretical study on the corresponding process of diatomic molecules, N2 and O2. We show that neutral molecules can also survive strong 800-nm laser fields in high Rydberg states, while their behavior is remarkably different in comparison with their companion atoms, Ar and Xe. The Rydberg excitation of N2 generally behaves similarly to Ar, while that of O2 is more significantly suppressed than the ionization compared to Xe in a high intensity region, which can be understood in the frame of a semiclassical picture, together with their different structures of molecular orbitals. However, distinct quantum features in the Rydberg excitation processes that are apparently beyond the semiclassical picture have been identified, i.e., the less suppressed probability of O2 at low intensity and the oscillation behavior of the ratio between N2 and Ar, indicating that our understanding of the relevant physics is still far from complete.

  20. Experimental efforts at NIST towards one-electron ions in circular Rydberg states

    NASA Astrophysics Data System (ADS)

    Tan, Joseph N.; Brewer, Samuel M.; Guise, Nicholas D.

    2011-06-01

    Experimental effort is underway at NIST to enable tests of theory with one-electron ions synthesized in circular Rydberg states from captured bare nuclei. Problematic effects that limit the accuracy of predicted energy levels for low-lying states are vanishingly small for high-angular-momentum (high-L) states; in particular, the nuclear size correction for high-L states is completely negligible for any foreseeable improvement of measurement precision. As an initial step towards realizing such states, highly charged ions are extracted from the NIST electron beam ion trap (EBIT) and steered through the electrodes of a Penning trap. The goal is to capture bare nuclei in the Penning trap for experiments to make one-electron atoms in circular Rydberg states with dipole (E1) transitions in the optical domain accessible to a frequency comb.

  1. Observation of interference effects via four-photon excitation of highly excited Rydberg states in thermal cesium vapor

    NASA Astrophysics Data System (ADS)

    Kondo, Jorge M.; Šibalić, Nikola; Guttridge, Alexander; Wade, Christopher G.; De Melo, Natalia R.; Adams, Charles S.; Weatherill, Kevin J.

    2015-12-01

    We report on the observation of electromagnetically induced transparency (EIT) and absorption (EIA) of highly excited Rydberg states in thermal Cs vapor using a four-step excitation scheme. The advantage of this four-step scheme is that the final transition to the Rydberg state has a large dipole moment and one can achieve similar Rabi frequencies to two- or three-step excitation schemes using two orders of magnitude less laser power. This scheme enables new applications such as dephasing free Rydberg excitation. The observed lineshapes are in good agreement with simulations based on multilevel optical Bloch equations.

  2. Collisional destruction of circular Rydberg states by atoms with small electron affinities

    NASA Astrophysics Data System (ADS)

    Mironchuk, Elena S.; Narits, Alexander A.; Lebedev, Vladimir S.

    2014-12-01

    The results of theoretical studies of interaction between neutral targets with small electron affinities and Rydberg atoms in circular states are reported. The cross sections of collisional destruction of such states due to the resonant quenching mechanism are calculated on the basis of the semiclassical theory of nonadiabatic transitions between the ionic and Rydberg covalent terms of a quasimolecule combined with recently developed technique for exact evaluation of matrix elements. We obtain the basic formula for the square of the coupling parameter involving Rydberg nlm-state with the given values of the principal, orbital, and magnetic quantum numbers. It is employed for the derivation of explicit expressions for transitions from circular states applicable in cases of s- and p-states of negative ion temporarily formed during a collision of atoms. Numerical calculations are carried out for thermal collisions of Li∗ and Na∗ atoms with Ca(4s2) and Sr(5s2). We explore n-, l-, m-, and velocity-dependences of the cross sections and analyze orientation effects in such collisions. Cross sections of resonant quenching for circular states (l = | m | = n - 1) are shown to be much smaller than those for states with small l values and typically two times lower than for nearly-circular states (l = n - 1) averaged over m.

  3. Quadratic Zeeman effect in hydrogen Rydberg states: Rigorous bound-state error estimates in the weak-field regime

    SciTech Connect

    Falsaperla, P.; Fonte, G. Istituto Nazionale di Fisica Nucleare, Sezione di Catania, Corso Italia 57, I-95129 Catania )

    1993-05-01

    Applying a method based on some results due to Kato [Proc. Phys. Soc. Jpn. 4, 334 (1949)], we show that series of Rydberg eigenvalues and Rydberg eigenfunctions of hydrogen in a uniform magnetic field can be calculated with a rigorous error estimate. The efficiency of the method decreases as the eigenvalue density increases and as [gamma][ital n][sup 3][r arrow]1, where [gamma] is the magnetic-field strength in units of 2.35[times]10[sup 9] G and [ital n] is the principal quantum number of the unperturbed hydrogenic manifold from which the diamagnetic Rydberg states evolve. Fixing [gamma] at the laboratory value 2[times]10[sup [minus]5] and confining our calculations to the region [gamma][ital n][sup 3][lt]1 (weak-field regime), we obtain extremely accurate results up to states corresponding to the [ital n]=32 manifold.

  4. Formation of positron-atom bound states in collisions between Rydberg Ps and neutral atoms

    NASA Astrophysics Data System (ADS)

    Swann, A. R.; Cassidy, D. B.; Deller, A.; Gribakin, G. F.

    2016-05-01

    Predicted 20 years ago, positron binding to neutral atoms has not yet been observed experimentally. A scheme is proposed to detect positron-atom bound states by colliding Rydberg positronium (Ps) with neutral atoms. Estimates of the charge-transfer reaction cross section are obtained using the first Born approximation for a selection of neutral atom targets and a wide range of incident Ps energies and principal quantum numbers. We also estimate the corresponding Ps ionization cross section. The accuracy of the calculations is tested by comparison with earlier predictions for charge transfer in Ps collisions with hydrogen and antihydrogen. We describe an existing Rydberg Ps beam suitable for producing positron-atom bound states and estimate signal rates based on the calculated cross sections and realistic experimental parameters. We conclude that the proposed methodology is capable of producing such states and of testing theoretical predictions of their binding energies.

  5. Photoionization from excited states of helium

    NASA Technical Reports Server (NTRS)

    Jacobs, V. L.

    1973-01-01

    The cross sections for photoionization from the 2 1S, 2 3S, 2 1P and 2 3P excited states of helium are calculated for photoelectron energies below the n = 2 threshold of He(+) using Hylleraas bound state wave functions and 1s-2s-2p close coupling final state wave functions. The resonant structures associated with the lowest-lying 1S, 1P, 3P, and 1D autoionizing states of helium are found to be characterized by large values of the line profile parameter q. The cross sections and the photoelectron angular distribution asymmetry parameters for the P-states are calculated for various polarization states of the target atom and the incident photon. Experiments which would lead to the separate determinations of the S- and D- wave partial photoionization cross sections are discussed.

  6. Spectroscopy of acetylene Rydberg states studied by VUV absorption and (3+1)-Resonantly Enhanced Multiphoton Ionisation

    NASA Astrophysics Data System (ADS)

    Boyé, Séverine; Campos, Andrea; Fillion, Jean-Hugues; Douin, Stéphane; Shafizadeh, Niloufar; Gauyacq, Dolores

    2004-03-01

    The ungerade ns+ nd Rydberg states of C 2H 2 converging to the ground state of the C 2H 2+ cation have been investigated in the energy range 74 000- 88 000 cm-1 by (3+1)-multiphoton ionisation (REMPI) and by VUV absorption spectroscopy at the Super-ACO synchrotron radiation facility. Both methods have allowed the selective analysis of the Rydberg transitions with rotational resolution. Mulliken's semi-united atom model, in which predissociation has been taken into account, was used to understand the relative three-photon intensities among the different electronic transitions within the same Rydberg supercomplex. Lifetimes have been evaluated and illustrate very different behaviours towards predissociation for the observed Rydberg states. To cite this article: S. Boyé et al., C. R. Physique 5 (2004).

  7. Classical Monte-Carlo simulation for Rydberg states ionization in strong field

    NASA Astrophysics Data System (ADS)

    Carrat, Vincent; Magnuson, Eric; Gallagher, Thomas

    2016-05-01

    The resilience of Rydberg states against ionization has fascinated physicists for a long time. One might expect that the loosely bound electron would be ionized by modest electromagnetic field. However, experiments show that a notable fraction of neutral atoms survive in Rydberg states when exposed to strong microwave or laser fields. Energy transfer between the field and the photoelectron occurs when the electron is close to the ionic core and depends on the phase of the field. Since those states have orbital times that can be larger than the field pulse duration, these energy exchanges will only occur a few times. While we can experimentally control the initial time when we create the Rydberg states and as a consequence the initial energy transfer from the field, our classical calculation suggests that the phase when the electron is returning to the ionic core on the next orbit is chaotic. Statistically the electron only has a 50% chance to gain energy which may lead to ionization. Additionally the population tends to accumulate in very high n states where ionization is less likely due to fewer rescattering events. Though incomplete, this classical Monte­-Carlo simulation provides useful insights for understanding the experimental observations. This work has been entirely performed at University of Virginia and is supported by the U. S. Department of Energy, Office of Basic energy Sciences.

  8. Long-lived Electronic Coherence of Rydberg States in the Strong-Field Ionization of a Polyatomic Molecule

    NASA Astrophysics Data System (ADS)

    Konar, Arkaprabha; Shu, Yinan; Levine, Benjamin; Lozovoy, Vadim; Dantus, Marcos

    2015-05-01

    Here, we report on quantum coherent control of a large (>20 atoms) polyatomic molecule. In particular, we explore the time resolved dynamics of dicyclopentadiene when excited by a pair of phase-locked intense 800nm femtosecond pulses by monitoring changes in ion yield of the parent and fragments. Long-lived oscillations are observed for ~ 500 fs in the parent ion yield indicating the presence of long lived-electronic states. We take advantage of the long-lived electronic coherence to control the yield of different fragment ions. The presence of Rydberg states is further supported by ab initio calculations at the EOM-CCSD/6-31 +G** level of theory which identified five low-lying electronic states of neutral DCPD in the regions between 6.4 and 7.0 eV in vertical excitation energy. States of both pure Rydberg and mixed π --> π */Rydberg character are observed in this low energy region and are known to originate from ethylene. The multiphoton excitation of two or more Rydberg states, separated by the photon energy is the key to the observed long-lived electronic coherence in DCPD with a quantum beat at the difference frequency. Rydberg states are expected to have very similar potential energy surfaces and the Rydberg electron is relatively uncoupled to the nuclear dynamics, therefore supporting long electronic coherence time.

  9. Transport of charge and atomic particles in Rydberg state-rich plasmas

    NASA Astrophysics Data System (ADS)

    Hagström, Magnus; Davidsson, Jan; Holmlid, Leif

    1998-02-01

    New methods make it possible to form considerable flux densities of Rydberg atoms of alkali metals. It is now possible to study the transport processes in regions where the density of Rydberg atoms is large. Examples of such studies have been given by Svensson and coworkers. In the present study, 0022-3727/31/4/013/img1 ions and Rydberg states 0022-3727/31/4/013/img2 are formed by desorption at 1300-1800 K from an Ir surface covered by a thin graphite layer. Due to the very large cross sections for collision processes involving Rydberg species, the Rydberg state-rich plasma between the Ir emitter and a cold grid electrode is not collision free, even at a pressure of 0022-3727/31/4/013/img3 mbar. Electron or 0022-3727/31/4/013/img4 emission takes place from the grid at a rate controlled by the flux of 0022-3727/31/4/013/img1 and 0022-3727/31/4/013/img2. The transition to penetration of 0022-3727/31/4/013/img1 and 0022-3727/31/4/013/img2 through the cloud of excited species between the emitter and grid is observed directly by molecular beam and ion sampling to detectors in a separate chamber. There is a space-charge limited behaviour for the positive current through the plasma as well as, in some modes, a clear positive saturation current, which shows that little gas phase ionization takes place. A current larger than expected from the saturation current as well as maxima in the voltage dependences are observed at high Rydberg densities. These effects are probably caused by space charge compensation due to a dielectric phase of condensed excited species, which means, for example, that the effective distance between the emitter and grid is decreased, as observed. The temperature variation of the space charge limited behaviour gives an activation energy of 0022-3727/31/4/013/img9, while the saturation current gives an activation energy of 0022-3727/31/4/013/img10. This agrees well with the electronic excitations 0022-3727/31/4/013/img11 at 0.90 eV and 0022

  10. Studying dissociative electron attachment through formation of heavy-Rydberg ion-pair states

    NASA Astrophysics Data System (ADS)

    Kelley, Michael; Buathong, Sitti; Dunning, F. Barry

    2016-05-01

    Following dissociative electron transfer in collisions between Rydberg atoms and electron-attaching targets, it is possible for the resulting pair of ions to remain electrostatically bound, forming heavy-Rydberg ion-pair states. Precise measurement of the velocity distributions of such ion-pair states provides information concerning the dissociation dynamics of the excited intermediates initially created by electron transfer. Here, electric-field-induced dissociation is used to detect the product ion pairs and observe their velocity distributions. These distributions are analyzed with the aid of a Monte Carlo collision code that models the electron transfer. Measurements with a number of different target species show that through this analysis, dissociation energetics, the branching ratios into different dissociation products, and the lifetimes of the excited intermediates can be examined. Research supported by the Robert A. Welch Foundation.

  11. MPI spectroscopy in the region of the 3p Rydberg state of some cycloketones

    NASA Astrophysics Data System (ADS)

    Kosmidis, C.; Boulakis, G.; Bolovinos, A.; Tsekeris, P.; Brint, P.

    1992-03-01

    The two-photon resonance three photon ionization spectra of cyclopentanone, cyclohexanone and cycloheptanone in the region of the 3p Rydberg state have been recorded, analysed and compared with the one-photon absorption spectra. A new 3p origin is identified for cyclopentanone. The absence from the MPI spectra of a sharp spectral feature that is observed in the absorption spectra is discussed. Photochemical generation of acetaldehyde is observed at high laser intensities and possible mechanisms for this are considered.

  12. Heavy Rydberg behaviour in high vibrational levels of some ion-pair states of the halogens and inter-halogens

    SciTech Connect

    Donovan, Robert J. E-mail: tr01@staffmail.ed.ac.uk; Lawley, Kenneth P. Ridley, Trevor E-mail: tr01@staffmail.ed.ac.uk

    2015-05-28

    We report the identification of heavy Rydberg resonances in the ion-pair spectra of I{sub 2}, Cl{sub 2}, ICl, and IBr. Extensive vibrational progressions are analysed in terms of the energy dependence of the quantum defect δ(E{sub b}) rather than as Dunham expansions. This is shown to define the heavy Rydberg region, providing a more revealing fit to the data with fewer coefficients and leads just as easily to numbering data sets separated by gaps in the observed vibrational progressions. Interaction of heavy Rydberg states with electronic Rydberg states at avoided crossings on the inner wall of the ion-pair potential is shown to produce distinctive changes in the energy dependence of δ(E{sub b}), with weak and strong interactions readily distinguished. Heavy Rydberg behaviour is found to extend well below near-dissociation states, down to vibrational levels ∼18 000-20 000 cm{sup −1} below dissociation. The rapid semi-classical calculation of δ(E{sub b}) for heavy Rydberg states is emphasised and shows their absolute magnitude to be essentially the volume of phase space excluded from the vibrational motion by avoiding core-core penetration of the ions.

  13. Strong field radio-frequency measurements using Rydberg states in a vapor cell

    NASA Astrophysics Data System (ADS)

    Miller, Stephanie; Anderson, David; Raithel, Georg

    2016-05-01

    There has been a growing interest in using electromagnetically induced transparency with Rydberg atoms in a room-temperature vapor cell as an all-optical readout method for measuring microwave electric fields. We present results from RF-modulating the 60S1 / 2 and 58D5 / 2 Rydberg states of rubidium with 50 MHz and 100 MHz fields, respectively. Weak RF fields AC Stark-shifts the Rydberg states. As the field strength is increased, sidebands appear at even multiples of the driving frequency. When strong fields are applied, the nearby hydrogenic manifold begins to intersect with the shifted levels. Similar investigations have been performed in cesium. Due to the significant amount of state mixing and level structure, Floquet theory is required to describe the level shifts and mixing. By comparing the calculation with the experimental data, we obtain an absolute determination of the RF electric field reaching a maximum field of 296 V/m to within +/- 0 . 35 % . Additionally, we estimate the shielding of DC fields within the vapor cell.

  14. Tests of Theory in Rydberg States of One-Electron Ions

    NASA Astrophysics Data System (ADS)

    Tan, Joseph N.; Mohr, Peter J.

    Comparison of optical frequency measurements to predictions of quantum electrodynamics (QED) for Rydberg states of one-electron ions can test theory and allow new determinations of constants of nature to be made. Simplifications in the QED theory of high-angular-momentum states reduces the uncertainty in the prediction of transition frequencies to a level where a new value of the Rydberg constant which is independent of the proton radius can be determined. Since the energy-level spacing between neighbouring Rydberg states grows as the square of the nuclear charge number, it is possible to study transitions with optical frequencies that are accessible to femtosecond laser frequency combs. Recently at the US National Institute of Standards and Technology (NIST), highly charged ions (including bare nuclei) created in an Electron Beam Ion Trap (EBIT) were extracted and captured in a novel compact Penning trap. An ongoing experiment aims to produce one-electron ions isolated in an ion trap designed for laser spectroscopy. Tests of theory in a regime free of nuclear effects would be valuable in shedding light on the puzzle surrounding the large discrepancy in the value of the proton radius inferred from the observed Lamb shift in muonic hydrogen as compared to the value deduced from hydrogen and deuterium spectroscopy and electron scattering measurements.

  15. Quantum defects of nonpenetrating Rydberg states of the SO molecule in adiabatic and nonadiabatic regions of the spectrum

    NASA Astrophysics Data System (ADS)

    Dorofeev, Dmitry L.; Elfimov, Sergei V.; Zon, Boris A.

    2012-02-01

    This paper is dedicated to the implementation of a generalized approach for calculating quantum defects in high Rydberg states of polar molecules with an account for the dipole moment of the molecular core and l uncoupling of the Rydberg electron. Adiabatic (Born-Oppenheimer) and nonadiabatic (inverse Born-Oppenheimer) regions of the spectrum are considered. The nonadiabatic case with a nonzero projection of the core momentum on the core axis is considered and is illustrated by the example of the SO molecule.

  16. Electron capture into large-l Rydberg states of multiply charged ions escaping from solid surfaces

    NASA Astrophysics Data System (ADS)

    Nedeljković, N.; Nedeljković, Lj.; Mirković, M.

    2003-07-01

    We have investigated the electron capture into large-l Rydberg states of multiply charged ionic projectiles (e.g., the core charges Z=6, 7, and 8) escaping solid surfaces with intermediate velocities (v≈1 a.u.) in the normal emergence geometry. A model of the nonresonant electron capture from the solid conduction band into the moving large angular-momentum Rydberg states of the ions is developed through a generalization of our results obtained previously for the low-l cases (l=0, 1, and 2). The model is based on the two-wave-function dynamics of the Demkov-Ostrovskii type. The electron exchange process is described by a mixed flux through a moving plane (“Firsov plane”), placed between the solid surface and the ionic projectile. Due to low eccentricities of the large-l Rydberg systems, the mixed flux must be evaluated through the whole Firsov plane. It is for this purpose that a suitable asymptotic method is developed. For intermediate ionic velocities and for all relevant values of the principal quantum number n≈Z, the population probability Pnl is obtained as a nonlinear l distribution. The theoretical predictions concerning the ions S VI, Cl VII, and Ar VIII are compared with the available results of the beam-foil experiments.

  17. Solvation effects on the molecular 3s Rydberg state: AZAB/CYCLO octanes clustered with argon

    NASA Astrophysics Data System (ADS)

    Shang, Q. Y.; Moreno, P. O.; Li, S.; Bernstein, E. R.

    1993-02-01

    Two color, 1+1, mass resolved excitation spectroscopy (MRES) is used to obtain molecular Rydberg (3s←n) spectra of azabicyclo[2.2.2]octane (ABCO) and diazabicyclo[2.2.2]octane (DABCO) clustered with argon. Nozzle/laser timing delay studies are employed together with time-of-flight mass spectroscopy to identify cluster composition. Population depletion techniques are used to differentiate between clusters with the same mass, but different geometries. A Lennard-Jones 6-12 potential is used to model the intermolecular interactions and predict minimum energy cluster geometries and cluster binding energies. The experimental results are combined with the cluster geometry calculations to assign spectral features to specific cluster geometries. Three different excited state interactions are required to model the experimentally observed line shapes, spectral shifts, and cluster dissociation. The relationship between these model potentials and the cluster binding sites suggests that the form of the cluster intermolecular potential in the Rydberg excited state is dictated by the distance between the argon and chromophore atoms. A comparison of results for ABCO(Ar)1 and DABCO(Ar)1 leads to the conclusion that the nitrogen 3s Rydberg orbital in clusters of DABCO is delocalized.

  18. Theoretical description of electronically excited vinylidene up to 10 eV: first high level ab initio study of singlet valence and Rydberg states.

    PubMed

    Boyé-Péronne, Séverine; Gauyacq, Dolores; Liévin, Jacques

    2014-11-01

    The first quantitative description of the Rydberg and valence singlet electronic states of vinylidene lying in the 0-10 eV region is performed by using large scale ab initio calculations. A deep analysis of Rydberg-valence interactions has been achieved thanks to the comprehensive information contained in the accurate Multi-Reference Configuration Interaction wavefunctions and an original population analysis highlighting the respective role played by orbital and state mixing in such interactions. The present theoretical approach is thus adequate for dealing with larger than diatomic Rydberg systems. The nine lowest singlet valence states have been optimized. Among them, some are involved in strong Rydberg-valence interactions in the region of the Rydberg state equilibrium geometry. The Rydberg states of vinylidene present a great similarity with the acetylene isomer, concerning their quantum defects and Rydberg molecular orbital character. As in acetylene, strong s-d mixing is revealed in the n = 3 s-d supercomplex. Nevertheless, unlike in acetylene, the close-energy of the two vinylidene ionic cores (2)A1 and (2)B1 results into two overlapped Rydberg series. These Rydberg series exhibit local perturbations when an accidental degeneracy occurs between them and results in avoided crossings. In addition, some Δl = 1 (s-p and p-d) mixings arise for some Rydberg states and are rationalized in term of electrostatic interaction from the electric dipole moment of the ionic core. The strongest dipole moment of the (2)B1 cationic state also stabilizes the lowest members of the n = 3 Rydberg series converging to this excited state, as compared to the adjacent series converging toward the (2)A1 ionic ground state. The overall energies of vinylidene Rydberg states lie above their acetylene counterpart. Finally, predictions for optical transitions in singlet vinylidene are suggested for further experimental spectroscopic characterization of vinylidene. PMID:25381524

  19. Theoretical description of electronically excited vinylidene up to 10 eV: First high level ab initio study of singlet valence and Rydberg states

    NASA Astrophysics Data System (ADS)

    Boyé-Péronne, Séverine; Gauyacq, Dolores; Liévin, Jacques

    2014-11-01

    The first quantitative description of the Rydberg and valence singlet electronic states of vinylidene lying in the 0-10 eV region is performed by using large scale ab initio calculations. A deep analysis of Rydberg-valence interactions has been achieved thanks to the comprehensive information contained in the accurate Multi-Reference Configuration Interaction wavefunctions and an original population analysis highlighting the respective role played by orbital and state mixing in such interactions. The present theoretical approach is thus adequate for dealing with larger than diatomic Rydberg systems. The nine lowest singlet valence states have been optimized. Among them, some are involved in strong Rydberg-valence interactions in the region of the Rydberg state equilibrium geometry. The Rydberg states of vinylidene present a great similarity with the acetylene isomer, concerning their quantum defects and Rydberg molecular orbital character. As in acetylene, strong s-d mixing is revealed in the n = 3 s-d supercomplex. Nevertheless, unlike in acetylene, the close-energy of the two vinylidene ionic cores 2A1 and 2B1 results into two overlapped Rydberg series. These Rydberg series exhibit local perturbations when an accidental degeneracy occurs between them and results in avoided crossings. In addition, some Δl = 1 (s-p and p-d) mixings arise for some Rydberg states and are rationalized in term of electrostatic interaction from the electric dipole moment of the ionic core. The strongest dipole moment of the 2B1 cationic state also stabilizes the lowest members of the n = 3 Rydberg series converging to this excited state, as compared to the adjacent series converging toward the 2A1 ionic ground state. The overall energies of vinylidene Rydberg states lie above their acetylene counterpart. Finally, predictions for optical transitions in singlet vinylidene are suggested for further experimental spectroscopic characterization of vinylidene.

  20. Theoretical description of electronically excited vinylidene up to 10 eV: First high level ab initio study of singlet valence and Rydberg states

    SciTech Connect

    Boyé-Péronne, Séverine; Gauyacq, Dolores; Liévin, Jacques

    2014-11-07

    The first quantitative description of the Rydberg and valence singlet electronic states of vinylidene lying in the 0–10 eV region is performed by using large scale ab initio calculations. A deep analysis of Rydberg-valence interactions has been achieved thanks to the comprehensive information contained in the accurate Multi-Reference Configuration Interaction wavefunctions and an original population analysis highlighting the respective role played by orbital and state mixing in such interactions. The present theoretical approach is thus adequate for dealing with larger than diatomic Rydberg systems. The nine lowest singlet valence states have been optimized. Among them, some are involved in strong Rydberg-valence interactions in the region of the Rydberg state equilibrium geometry. The Rydberg states of vinylidene present a great similarity with the acetylene isomer, concerning their quantum defects and Rydberg molecular orbital character. As in acetylene, strong s-d mixing is revealed in the n = 3 s-d supercomplex. Nevertheless, unlike in acetylene, the close-energy of the two vinylidene ionic cores {sup 2}A{sub 1} and {sup 2}B{sub 1} results into two overlapped Rydberg series. These Rydberg series exhibit local perturbations when an accidental degeneracy occurs between them and results in avoided crossings. In addition, some Δl = 1 (s-p and p-d) mixings arise for some Rydberg states and are rationalized in term of electrostatic interaction from the electric dipole moment of the ionic core. The strongest dipole moment of the {sup 2}B{sub 1} cationic state also stabilizes the lowest members of the n = 3 Rydberg series converging to this excited state, as compared to the adjacent series converging toward the {sup 2}A{sub 1} ionic ground state. The overall energies of vinylidene Rydberg states lie above their acetylene counterpart. Finally, predictions for optical transitions in singlet vinylidene are suggested for further experimental spectroscopic

  1. Static and dynamic polarizability for C{sup 2+} in Rydberg states

    SciTech Connect

    Stancalie, V.

    2015-07-15

    This work presents results from a non-perturbative calculation of dynamic polarizability of C III ions in 1s{sup 2}2sns ({sup 1}S{sup e}) Rydberg states. We employ a two-state model for dressed atomic states to investigate the effect of the frequency-dependent polarizability of optically dressed 1s{sup 2}2sns({sup 1}S{sup e}) states (n = 5 − 12) on transitions to nearby states (1s{sup 2}2pns({sup 1}P{sub 1}{sup o})). Our model calculation results indicate that the resonance structure of the polarizabilities is entirely captured by the transition terms whereas the free electron polarizability only provides a smooth background. The resonance structure is evident in the plots and the widths increase with increasing principal quantum number. This work refers to highly excited 1s{sup 2}2sns ({sup 1}S) Rydberg states, embedded in the electric dipole field of the 2s – 2p core transition in Li-like C{sup 3+} ion. The contributions of the individual transitions to the static polarizabilities of these Rydberg states are obtained from the use of the sum-over-state method. To this aim, both the C{sup 2+} ground state and the C{sup 3+} target state energies have been carefully calculated based on the configuration interactions method implemented in the General-purpose Relativistic Atomic Structure Package. Agreement is reasonably good with existing data wherever available. These results are believed to be the first such values for this system and will be important for ionic spectroscopy and plasma diagnostics.

  2. Vacuum ultraviolet studies of electron impact of helium: Excitation of He n P Rydberg series and ionization-excitation of He nl Rydberg series

    SciTech Connect

    Shemansky, D.E.; Hall, D.T.; Ajello, J.M.; Franklin, B.

    1985-09-15

    Laboratory measurements of the electron excitation cross sections of emission in the He Rydberg series (1sS S-1snp P) for n = 2,3,4 have been obtained. The cross sections were estimated by two methods: (1) analysis of calibrated laboratory spectra placed on an absolute scale using the H Ly dissociative excitation standard and (2) analysis of relative cross section data using a modified Born approximation. A new method has been developed for the application of the Bethe-Born approximation using experimental relative excitation functions that does not require extrapolation in a Fano plot in the determination of the absolute cross section. The two methods agree to within 3% for the 58.4 nm line when allowance is made for cascade transitions. We find the direct excitation cross sections at 200 eV for the n = 2,3,4 members of the published electron impact experimental measurements of the two electron process of ionization-excitation impact are generally in agreement, especially on the energy dependence of excitation functions, but show significant differences with theoretical calculations.

  3. Vibronic structure and ion core interactions in Rydberg states of diazomethane: an experimental and theoretical investigation.

    PubMed

    Fedorov, Igor; Koziol, Lucas; Li, Guosheng; Reisler, Hanna; Krylov, Anna I

    2007-12-27

    Vibronic transitions to the 21A2(3py <-- pi) Rydberg state of CH2N2, CD2N2, and CHDN2 were recorded by 2 + 1 REMPI spectroscopy, and kinetic energy distributions (eKE) of photoelectrons from ionization of selected vibronic levels were determined by velocity map imaging. Normal-mode frequencies were obtained for the 21A2(3py) Rydberg state and for the cation. Mixed levels of the 21A2(3py) and 21B1(3pz) of the three isotopologs were identified by photoelectron imaging and analyzed. The equilibrium geometries and harmonic vibrational frequencies of the electronic states of neutral diazomethane were calculated by CCSD(T)/cc-pVTZ, and B3LYP/6-311G(2df,p). The latter method was also used to calculate isotope shifts for the ground-state neutral and cation. Geometry and frequencies of the ground state of the cation were calculated by CCSD(T)/cc-pVTZ, using the unrestricted (UHF) reference. The equilibrium structures, frequencies, and isotope shifts of the 21A2(3py) and 21B1(3pz) Rydberg states were calculated by EOM-EE-CCSD/6-311(3+,+)G(2df). In all cases where comparisons with experimental results were available, the agreement between theory and experiment was very good allowing a full analysis of trends in structure and vibrational frequencies in going from the neutral species to the excited Rydberg states, 21A2(3py) and 21B1(3pz), and the cation. Although the 21A2(3py) and 21B1(3pz) states have planar C2v symmetry like the ion, they exhibit differences in geometry due to the specific interactions of the electron in the 3py and 3pz orbitals with the nuclei charge distributions of the ion core. Moreover, trends in normal-mode frequencies in the ground states of the neutral and ion and the 21A2(3py) and 21B1(3pz) Rydberg states are consistent with removing an electron from the bonding piCN-orbital, which also has an antibonding character with respect to NN. To explain the observed trends, the vibrational modes are divided into two groups that involve displacements mainly

  4. Probing the Dynamics of Rydberg and Valence States of Molecular Nitrogen with Attosecond Transient Absorption Spectroscopy.

    PubMed

    Warrick, Erika R; Cao, Wei; Neumark, Daniel M; Leone, Stephen R

    2016-05-19

    An attosecond pulse is used to create a wavepacket in molecular nitrogen composed of multiple bound and autoionizing electronic states of Rydberg and valence character between 12 and 16.7 eV. A time-delayed, few-femtosecond, near-infrared (NIR) laser pulse is used to couple individual states in the wavepacket to multiple neighboring states, resulting in time-dependent modification of the absorption spectrum and revealing both individual quantum beats of the wavepacket and the energy shifts of the excited states in the presence of the strong NIR field. The broad bandwidth of the attosecond pulse and high energy resolution of the extreme ultraviolet spectrometer allow the simultaneous observation of time-dependent dynamics for many individual vibrational levels in each electronic state. Quantum beating with periods from 1.3 to 12 fs and transient line shape changes are observed among vibrational levels of a progression of electronically autoionizing Rydberg states leading to the excited A (2)Πu N2(+) ion core. Vibrational levels in the valence b (1)Πu state exhibit 50 fs oscillation periods, revealing superpositions between individual vibrational levels within this state. Comparisons are made to previous studies of electronic wavepackets in atoms that highlight similarities to atomic behavior yet illustrate unique contributions of the diatomic molecular structure to the wavepacket, including the influence of different electronic potentials and vibrational-level-specific electronic dynamics. PMID:26862883

  5. Spectra and Autoionization Lifetimes of Long-Range Rydberg Molecular States of 85 Rb2

    NASA Astrophysics Data System (ADS)

    Carollo, Ryan; Eyler, Edward; Gould, Phillip; Stwalley, William

    2016-05-01

    We present high-resolution autoionization data and modeling of the 7 p long-range Rydberg molecular states in 85 Rb2. Our process excites a photoassociation resonance in the 1 (0g-) state which decays to v'' = 35 and 36 long-range levels of the a3Σu+ state and to the continuum. These bound molecules are then excited via a single UV photon to target states below the 5 s + 7 p asymptote by a frequency-doubled pulse-amplified CW laser with narrow linewidth, ~ 150 MHz. The long-range portion of the bonding potential is formed by the scattering interaction of the Rydberg electron of a perturbed 7 p atom scattering from a nearby ground-state atom. We use time-of-flight to selectively measure molecular ions, which are formed via autoionization. Using a hyperfine model of the a3Σu+ and its coupling to the X1Σg+ state, we are able to place an upper limit on the autoionization linewidth of 450 MHz, corresponding to a lifetime >= 3 . 5 ×10-10 s. Excited-state hyperfine structure suggests a still-lower linewidth (and thus longer lifetime), but its contribution is not yet fully understood. This work is supported by NSF and AFOSR.

  6. A sensitive electrometer based on a Rydberg atom in a Schrödinger-cat state

    NASA Astrophysics Data System (ADS)

    Facon, Adrien; Dietsche, Eva-Katharina; Grosso, Dorian; Haroche, Serge; Raimond, Jean-Michel; Brune, Michel; Gleyzes, Sébastien

    2016-07-01

    Fundamental quantum fluctuations caused by the Heisenberg principle limit measurement precision. If the uncertainty is distributed equally between conjugate variables of the meter system, the measurement precision cannot exceed the standard quantum limit. When the meter is a large angular momentum, going beyond the standard quantum limit requires non-classical states such as squeezed states or Schrödinger-cat-like states. However, the metrological use of the latter has been so far restricted to meters with a relatively small total angular momentum because the experimental preparation of these non-classical states is very challenging. Here we report a measurement of an electric field based on an electrometer consisting of a large angular momentum (quantum number J ≈ 25) carried by a single atom in a high-energy Rydberg state. We show that the fundamental Heisenberg limit can be approached when the Rydberg atom undergoes a non-classical evolution through Schrödinger-cat states. Using this method, we reach a single-shot sensitivity of 1.2 millivolts per centimetre for a 100-nanosecond interaction time, corresponding to 30 microvolts per centimetre per square root hertz at our 3 kilohertz repetition rate. This highly sensitive, non-invasive space- and time-resolved field measurement extends the realm of electrometric techniques and could have important practical applications: detection of individual electrons in mesoscopic devices at a distance of about 100 micrometres with a megahertz bandwidth is within reach.

  7. Generation of Rydberg states of hydrogen atoms with intense laser pulses: The roles of Coulomb force and initial lateral momentum

    NASA Astrophysics Data System (ADS)

    Zhang, Bin; Chen, Wenbo; Zhao, Zengxiu

    2014-08-01

    We investigate the generation of Rydberg states of hydrogen atoms with intense laser pulses by solving the time-dependent Schrödinger equation and by means of classical-trajectory Monte Carlo simulations. Both linearly polarized multicycle pulses and pairs of optical half-cycle pulses are used. Comparisons between these methods show that both the Coulomb force and initial lateral momentum, which have effects on the n distribution and l distribution of the population of excited states, are important in the generation of Rydberg states.

  8. Hydrogenic Rydberg States of Molecular van der Waals Complexes: Resolved Rydberg Spectroscopy of DABCO-N2

    NASA Astrophysics Data System (ADS)

    Cockett, Martin C.; Watkins, Mark J.

    2004-01-01

    The complementary threshold ionization techniques of MATI and ZEKE spectroscopy have been used to reveal well-resolved, long-lived (>10 μs) hydrogenic Rydberg series (50≤n≤98) in a van der Waals complex formed between a polyatomic molecule and a diatomic molecule for the first time. The series are observed within 50 cm-1 of the adiabatic ionization threshold as well as two core-excited thresholds corresponding to excitation of up to two quanta in the van der Waals vibra­tional mode.

  9. Multiphoton ionization/dissociation of cyclopentanone at the lower Rydberg states

    NASA Astrophysics Data System (ADS)

    Philis, John G.; Kosmidis, Constantine; Tzallas, Paraskevas

    1998-12-01

    The 2-photon excitation of the 3p and 3d Rydberg states in jet-cooled cyclopentanone has been investigated by resonance enhanced multiphoton ionization (REMPI) in a time of flight mass spectrometer. The three 3px,y,z components are clearly resolved while the case for the 3di excitations is obscure due to the S1 one-photon resonance. The ns laser induced mass spectra are characteristic of hard ionization while the fs laser induced mass spectrum is very similar to the Electron Impact one.

  10. Coherent states of the driven Rydberg atom: Quantum-classical correspondence of periodically driven systems

    NASA Astrophysics Data System (ADS)

    Vela-Arevalo, Luz V.; Fox, Ronald F.

    2005-06-01

    A methodology to calculate generalized coherent states for a periodically driven system is presented. We study wave packets constructed as a linear combination of suitable Floquet states of the three-dimensional Rydberg atom in a microwave field. The driven coherent states show classical space localization, spreading, and revivals and remain localized along the classical trajectory. The microwave strength and frequency have a great effect in the localization of Floquet states, since quasienergy avoided crossings produce delocalization of the Floquet states, showing that tuning of the parameters is very important. Using wavelet-based time-frequency analysis, the classical phase-space structure is determined, which allows us to show that the driven coherent state is located in a large regular region in which the z coordinate is in resonance with the external field. The expectation values of the wave packet show that the driven coherent state evolves along the classical trajectory.

  11. Coherent states of the driven Rydberg atom: Quantum-classical correspondence of periodically driven systems

    SciTech Connect

    Vela-Arevalo, Luz V.; Fox, Ronald F.

    2005-06-15

    A methodology to calculate generalized coherent states for a periodically driven system is presented. We study wave packets constructed as a linear combination of suitable Floquet states of the three-dimensional Rydberg atom in a microwave field. The driven coherent states show classical space localization, spreading, and revivals and remain localized along the classical trajectory. The microwave strength and frequency have a great effect in the localization of Floquet states, since quasienergy avoided crossings produce delocalization of the Floquet states, showing that tuning of the parameters is very important. Using wavelet-based time-frequency analysis, the classical phase-space structure is determined, which allows us to show that the driven coherent state is located in a large regular region in which the z coordinate is in resonance with the external field. The expectation values of the wave packet show that the driven coherent state evolves along the classical trajectory.

  12. Observation of Cavity Rydberg Polaritons

    NASA Astrophysics Data System (ADS)

    Georgakopoulos, Alexandros; Jia, Ningyuan; Ryou, Albert; Schine, Nathan; Sommer, Ariel; Simon, Jonathan

    2016-05-01

    We demonstrate hybridization of optical cavity photons with atomic Rydberg excitations using electromagnetically induced transparency (EIT). The resulting dark state Rydberg polaritons exhibit a compressed frequency spectrum and enhanced lifetime indicating strong light-matter mixing. We study the coherence properties of cavity Rydberg polaritons and identify the generalized EIT linewidth for optical cavities. Strong collective coupling suppresses polariton losses due to inhomogeneous broadening, which we demonstrate by using different Rydberg levels with a range of polarizabilities. Our results point the way towards using cavity Rydberg polaritons as a platform for creating photonic quantum materials.

  13. Energy shift and state mixing of Rydberg atoms in ponderomotive optical traps

    NASA Astrophysics Data System (ADS)

    Wang, Xiao; Robicheaux, F.

    2016-08-01

    We present a degenerate perturbation analysis in the spin–orbit coupled basis for Rydberg atoms in an optical trap. The perturbation matrix is found to be nearly the same for two states with the same total angular momentum j, and orbital angular momentum number l differing by 1, The same perturbation matrices result in the same state-mixing and energy shift. We also study the dependence of state mixing and energy shift on the periodicity and symmetry of the ponderomotive potentials induced by different optical traps. State mixing in a one-dimensional lattice formed with two counterpropagating Gaussian beams is studied and yields a state-dependent trap depth. We also calculate the state-mixing in an optical trap formed by four parallel, separated and highly focused Gaussian beams.

  14. Trilobites and other molecular animals: How Rydberg-electrons catch ground state atoms

    NASA Astrophysics Data System (ADS)

    Pfau, Tilman

    2012-06-01

    We report on laser spectroscopy results obtained in a dense and frozen Rydberg gas. Novel molecular bonds resulting in ultralong-range Rydberg dimers were predicted [1] and dimers as well as trimers in different vibrational states were found [2]. Some of these states are predicted to be bound by quantum reflection. Lifetime measurements confirm this prediction. Coherent superposition between free and bound states have been investigated [3]. Recently we have also confirmed that in an electric field these homonuclear molecules develop a permanent dipole moment [4]. [4pt] [1] C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000). [0pt] [2] V. Bendkowsky, B. Butscher, J. Nipper, J. P. Shaffer, R. L"ow, T. Pfau, Nature 458, 1005 (2009), V. Bendkowsky, B. Butscher, J. Nipper, J. Balewski, J. P. Shaffer, R. L"ow, T. Pfau, W. Li, J. Stanojevic, T. Pohl, and J. M. Rost, Phys. Rev. Lett. 105, 163201 (2010). [0pt] [3] B. Butscher, J. Nipper, J. B. Balewski, L. Kukota, V. Bendkowsky, R. L"ow, and T. Pfau Nature Physics 6, 970--974 (2010). [0pt] [4] W. Li, T. Pohl, J. M. Rost, Seth T. Rittenhouse, H. R. Sadeghpour, J. Nipper, B. Butscher, J. B. Balewski, V. Bendkowsky, R. L"ow, T. Pfau, Science 334, 1110 (2011).

  15. Molecular detection using Rydberg, autoionizing, and cluster states. Progress report

    SciTech Connect

    Wessel, J.

    1989-08-17

    Continuing investigations of multiphoton ionization processes in naphthalene have established the geometry and spectroscopy of trimer and tetramer cluster states. A new, highly efficient ionization mechanism has been identified in the trimer. It is closely related to autoionization of 2-electron atoms by resonant 2-photon excitation and to exciton fusion in larger clusters.

  16. Combined theoretical and experimental study of the valence, Rydberg, and ionic states of chlorobenzene

    NASA Astrophysics Data System (ADS)

    Palmer, Michael H.; Ridley, Trevor; Vrønning Hoffmann, Søren; Jones, Nykola C.; Coreno, Marcello; de Simone, Monica; Grazioli, Cesare; Zhang, Teng; Biczysko, Malgorzata; Baiardi, Alberto; Peterson, Kirk A.

    2016-03-01

    New photoelectron (PE) and ultra violet (UV) and vacuum UV (VUV) spectra have been obtained for chlorobenzene by synchrotron study with higher sensitivity and resolution than previous work and are subjected to detailed analysis. In addition, we report on the mass-resolved (2 + 1) resonance enhanced multiphoton ionization (REMPI) spectra of a jet-cooled sample. Both the VUV and REMPI spectra have enabled identification of a considerable number of Rydberg states for the first time. The use of ab initio calculations, which include both multi-reference multi-root doubles and singles configuration interaction (MRD-CI) and time dependent density functional theoretical (TDDFT) methods, has led to major advances in interpretation of the vibrational structure of the ionic and electronically excited states. Franck-Condon (FC) analyses of the PE spectra, including both hot and cold bands, indicate much more complex envelopes than previously thought. The sequence of ionic states can be best interpreted by our multi-configuration self-consistent field computations and also by comparison of the calculated vibrational structure of the B and C ionic states with experiment; these conclusions suggest that the leading sequence is the same as that of iodobenzene and bromobenzene, namely: X2B1(3b1-1) < A2A2(1a2-1) < B2B2(6b2-1) < C2B1(2b1-1). The absorption onset near 4.6 eV has been investigated using MRD-CI and TDDFT calculations; the principal component of this band is 1B2 and an interpretation based on the superposition of FC and Herzberg-Teller contributions has been performed. The other low-lying absorption band near 5.8 eV is dominated by a 1A1 state, but an underlying weak 1B1 state (πσ∗) is also found. The strongest band in the VUV spectrum near 6.7 eV is poorly resolved and is analyzed in terms of two ππ∗ states of 1A1 (higher oscillator strength) and 1B2 (lower oscillator strength) symmetries, respectively. The calculated vertical excitation energies of these two

  17. Combined theoretical and experimental study of the valence, Rydberg, and ionic states of chlorobenzene.

    PubMed

    Palmer, Michael H; Ridley, Trevor; Vrønning Hoffmann, Søren; Jones, Nykola C; Coreno, Marcello; de Simone, Monica; Grazioli, Cesare; Zhang, Teng; Biczysko, Malgorzata; Baiardi, Alberto; Peterson, Kirk A

    2016-03-28

    New photoelectron (PE) and ultra violet (UV) and vacuum UV (VUV) spectra have been obtained for chlorobenzene by synchrotron study with higher sensitivity and resolution than previous work and are subjected to detailed analysis. In addition, we report on the mass-resolved (2 + 1) resonance enhanced multiphoton ionization (REMPI) spectra of a jet-cooled sample. Both the VUV and REMPI spectra have enabled identification of a considerable number of Rydberg states for the first time. The use of ab initio calculations, which include both multi-reference multi-root doubles and singles configuration interaction (MRD-CI) and time dependent density functional theoretical (TDDFT) methods, has led to major advances in interpretation of the vibrational structure of the ionic and electronically excited states. Franck-Condon (FC) analyses of the PE spectra, including both hot and cold bands, indicate much more complex envelopes than previously thought. The sequence of ionic states can be best interpreted by our multi-configuration self-consistent field computations and also by comparison of the calculated vibrational structure of the B and C ionic states with experiment; these conclusions suggest that the leading sequence is the same as that of iodobenzene and bromobenzene, namely: X(2)B1(3b1 (-1)) < A(2)A2(1a2 (-1)) < B(2)B2(6b2 (-1)) < C(2)B1(2b1 (-1)). The absorption onset near 4.6 eV has been investigated using MRD-CI and TDDFT calculations; the principal component of this band is (1)B2 and an interpretation based on the superposition of FC and Herzberg-Teller contributions has been performed. The other low-lying absorption band near 5.8 eV is dominated by a (1)A1 state, but an underlying weak (1)B1 state (πσ(∗)) is also found. The strongest band in the VUV spectrum near 6.7 eV is poorly resolved and is analyzed in terms of two ππ(∗) states of (1)A1 (higher oscillator strength) and (1)B2 (lower oscillator strength) symmetries, respectively. The calculated vertical

  18. Tailoring Rydberg interactions via Förster resonances: state combinations, hopping and angular dependence

    NASA Astrophysics Data System (ADS)

    Paris-Mandoki, Asaf; Gorniaczyk, Hannes; Tresp, Christoph; Mirgorodskiy, Ivan; Hofferberth, Sebastian

    2016-08-01

    Förster resonances provide a highly flexible tool to tune both the strength and the angular shape of interactions between two Rydberg atoms. We give a detailed explanation about how Förster resonances can be found by searching through a large range of possible quantum number combinations. We apply our search method to SS, SD and DD pair states of 87Rb with principal quantum numbers from 30 to 100, taking into account the fine structure splitting of the Rydberg states. We find various strong resonances between atoms with a large difference in principal quantum numbers. We quantify the strength of these resonances by introducing a figure of merit {\\tilde{C}}3 which is independent of the magnetic quantum numbers and geometry to classify the resonances by interaction strength. We further predict to what extent excitation exchange is possible on different resonances and point out limitations of the coherent hopping process. Finally, we discuss the angular dependence of the dipole–dipole interaction and its tunability near resonances.

  19. Scaled Energy Spectroscopy of Collisionally Perturbed Potassium Rydberg States

    NASA Astrophysics Data System (ADS)

    Keeler, Matthew Len; Setzer, William

    2010-03-01

    We will present preliminary results on the recurrence spectroscopy (or scaled energy spectroscopy) of highly-excited potassium in the presence of collisional perturbations. Recurrence spectroscopy, with the aid of closed orbit theory, has produced useful insights into the semi-classical description of non-hydrogenic spectral features of excited atoms in external fields. We demonstrate how to apply recurrence spectroscopy to the Stark spectrum of potassium subject to collisional line-shift and line-broadening. When krypton gas is added to the system the absorption spectrum experiences line broadening, differential line shifts, and state mixing. With an appropriately modified energy scale, perturbations of the absorption spectrum become meaningful features within the scaled-energy spectrum. New features found within the recurrence spectra can then, with semi-classical closed orbit theory, be interpreted in terms of classical decoherence, elastic and inelastic collisions.

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

    NASA Astrophysics Data System (ADS)

    Palmer, Michael H.; Ridley, Trevor; Vrønning Hoffmann, Søren; Jones, Nykola C.; Coreno, Marcello; de Simone, Monica; Grazioli, Cesare; Zhang, Teng; Biczysko, Malgorzata; Baiardi, Alberto; Peterson, Kirk A.

    2016-05-01

    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 X2B1 and A2A2 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 B2B2states forces reconsideration of the nature of the PIRI spectrum. The coupling between these two states is induced by the a2 modes, ν12 and ν14 and we propose that the 141 band is observed in the B2B2 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 ν12 and ν14. The relative intensities of the various Rydberg state peaks in the VUV absorption and REMPI spectra of fluorobenzene are very similar to

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

    PubMed

    Palmer, Michael H; Ridley, Trevor; Vrønning Hoffmann, Søren; Jones, Nykola C; Coreno, Marcello; de Simone, Monica; Grazioli, Cesare; Zhang, Teng; Biczysko, Malgorzata; Baiardi, Alberto; Peterson, Kirk A

    2016-05-28

    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(2)B1 and A(2)A2 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(2)B2states forces reconsideration of the nature of the PIRI spectrum. The coupling between these two states is induced by the a2 modes, ν12 and ν14 and we propose that the 14(1) band is observed in the B(2)B2 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 ν12 and ν14. The relative intensities of the various Rydberg state peaks in the VUV absorption and REMPI spectra of fluorobenzene are

  2. Electric-Field-Induced Dissociation of Heavy Rydberg Ion-Pair States

    SciTech Connect

    Reinhold, Carlos O; Yoshida, S.; Dunning, F. B.

    2011-01-01

    A classical trajectory Monte Carlo approach is used to simulate the dissociation of H+..F and K+..Cl heavy Rydberg ion pairs induced by a ramped electric-field, a technique used experimentally to detect and probe ion-pair states. The simulations include the effects of the strong short-range repulsive interaction associated with ion-pair scattering and provide results in good agreement with experimental data for Stark wavepackets probed by a ramped field, demonstrating that many of the characteristics of field-induced dissociation can be well described using a purely classical model. The data also show that states with a given value of principal quantum number (i.e., binding energy) can dissociate over a broad range of applied fields, the exact field being governed by the initial orbital angular momentum and orientation of the state.

  3. A sensitive electrometer based on a Rydberg atom in a Schrödinger-cat state.

    PubMed

    Facon, Adrien; Dietsche, Eva-Katharina; Grosso, Dorian; Haroche, Serge; Raimond, Jean-Michel; Brune, Michel; Gleyzes, Sébastien

    2016-07-14

    Fundamental quantum fluctuations caused by the Heisenberg principle limit measurement precision. If the uncertainty is distributed equally between conjugate variables of the meter system, the measurement precision cannot exceed the standard quantum limit. When the meter is a large angular momentum, going beyond the standard quantum limit requires non-classical states such as squeezed states or Schrödinger-cat-like states. However, the metrological use of the latter has been so far restricted to meters with a relatively small total angular momentum because the experimental preparation of these non-classical states is very challenging. Here we report a measurement of an electric field based on an electrometer consisting of a large angular momentum (quantum number J ≈ 25) carried by a single atom in a high-energy Rydberg state. We show that the fundamental Heisenberg limit can be approached when the Rydberg atom undergoes a non-classical evolution through Schrödinger-cat states. Using this method, we reach a single-shot sensitivity of 1.2 millivolts per centimetre for a 100-nanosecond interaction time, corresponding to 30 microvolts per centimetre per square root hertz at our 3 kilohertz repetition rate. This highly sensitive, non-invasive space- and time-resolved field measurement extends the realm of electrometric techniques and could have important practical applications: detection of individual electrons in mesoscopic devices at a distance of about 100 micrometres with a megahertz bandwidth is within reach. PMID:27411632

  4. Excitation of high orbital angular momentum Rydberg states with Laguerre-Gauss beams

    NASA Astrophysics Data System (ADS)

    Rodrigues, J. D.; Marcassa, L. G.; Mendonça, J. T.

    2016-04-01

    We consider the excitation of Rydberg states through photons carrying an intrinsic orbital angular momentum degree of freedom. Laguerre-Gauss modes, with a helical wave-front structure, correspond to such a set of laser beams, which carry {{\\ell }}0 units of orbital angular momentum in their propagation direction, with ℓ 0 the winding number. We demonstrate that, in a proper geometry setting, this orbital angular momentum can be transferred to the internal degrees of freedom of the atoms, thus violating the standard dipole selection rules. Higher orbital angular momentum states become accessible through a single photon excitation process. We investigate how the spacial structure of the Laguerre-Gauss beam affects the radial coupling strength, assuming the simplest case of hydrogen-like wavefunctions. Finally we discuss a generalization of the angular momentum coupling, in order to include the effects of the fine and hyperfine splitting, in the context of the Wigner-Eckart theorem.

  5. Femtosecond predissociation dynamics of the methyl radical from the 3p(z) Rydberg state.

    PubMed

    Balerdi, Garikoitz; Woodhouse, Joanne; Zanchet, Alexander; de Nalda, Rebeca; Senent, María L; García-Vela, Alberto; Bañares, Luis

    2016-01-01

    The real time dynamics of electronic predissociation of the CH3 radical (and its deuterated variant CD3) from selected vibrational states of the 3pz Rydberg state have been measured for the first time using a novel methodology based on a femtosecond three-color experiment to generate, two-photon excite and ionize methyl radicals as a function of time in combination with velocity map imaging detection. Subpicosecond lifetimes have been measured, showing a decreasing trend as vibrational excitation in the symmetric stretch and bending umbrella modes increases for both species. High-level ab initio calculations have been carried out in order to elucidate the CH3 3pz predissociation mechanism and support the lifetime measurements. The observed lifetimes are relevant for the understanding of the resonance enhanced multiphoton ionization spectroscopy of this radical. PMID:26473180

  6. Self-interaction corrected density functional calculations of Rydberg states of molecular clusters: N,N-dimethylisopropylamine.

    PubMed

    Gudmundsdóttir, Hildur; Zhang, Yao; Weber, Peter M; Jónsson, Hannes

    2014-12-21

    Theoretical calculations of Rydberg excited states of molecular clusters consisting of N,N-dimethylisopropylamine molecules using a Perdew-Zunger self-interaction corrected energy functional are presented and compared with results of resonant multiphoton ionization measurements. The binding energy of the Rydberg electron in the monomer is calculated to be 2.79 eV and 2.27 eV in the 3s and 3p state, respectively, which compares well with measured values of 2.88 eV and 2.21 eV. Three different stable configurations of the dimer in the ground state were found using an energy functional that includes van der Waals interaction. The lowest ground state energy conformation has the two N-atoms widely separated, by 6.2 Å, while the Rydberg state energy is lowest for a configuration where the N-atoms of the two molecules come close together, separated by 3.7 Å. This conformational change is found to lower the Rydberg electron binding energy by 0.2 eV. The self-interaction corrected functional gives a highly localized hole on one of the two molecules, unlike results obtained using the PBE functional or the hybrid B3LYP functional which give a delocalized hole. For the trimer, the self-interaction corrected calculation gives a Rydberg electron binding energy lowered further by 0.13 eV as compared with the dimer. The calculated results compare well with trends observed in experimental measurements. The reduction of the Rydberg electron binding energy with cluster size can be ascribed to an effective delocalization of the positive charge of the hole by the induced and permanent dipole moments of the neighboring molecules. A further decrease observed to occur on a time scale of tens of ps can be ascribed to a structural rearrangement of the clusters in the Rydberg state where molecules rotate to orient their dipoles in response to the formation of the localized hole. PMID:25527936

  7. Self-interaction corrected density functional calculations of Rydberg states of molecular clusters: N,N-dimethylisopropylamine

    SciTech Connect

    Gudmundsdóttir, Hildur; Zhang, Yao; Weber, Peter M.; Jónsson, Hannes

    2014-12-21

    Theoretical calculations of Rydberg excited states of molecular clusters consisting of N,N-dimethylisopropylamine molecules using a Perdew-Zunger self-interaction corrected energy functional are presented and compared with results of resonant multiphoton ionization measurements. The binding energy of the Rydberg electron in the monomer is calculated to be 2.79 eV and 2.27 eV in the 3s and 3p state, respectively, which compares well with measured values of 2.88 eV and 2.21 eV. Three different stable configurations of the dimer in the ground state were found using an energy functional that includes van der Waals interaction. The lowest ground state energy conformation has the two N-atoms widely separated, by 6.2 Å, while the Rydberg state energy is lowest for a configuration where the N-atoms of the two molecules come close together, separated by 3.7 Å. This conformational change is found to lower the Rydberg electron binding energy by 0.2 eV. The self-interaction corrected functional gives a highly localized hole on one of the two molecules, unlike results obtained using the PBE functional or the hybrid B3LYP functional which give a delocalized hole. For the trimer, the self-interaction corrected calculation gives a Rydberg electron binding energy lowered further by 0.13 eV as compared with the dimer. The calculated results compare well with trends observed in experimental measurements. The reduction of the Rydberg electron binding energy with cluster size can be ascribed to an effective delocalization of the positive charge of the hole by the induced and permanent dipole moments of the neighboring molecules. A further decrease observed to occur on a time scale of tens of ps can be ascribed to a structural rearrangement of the clusters in the Rydberg state where molecules rotate to orient their dipoles in response to the formation of the localized hole.

  8. Formation rate for Rb 2 + molecular ions created in collisions of Rb Rydberg and ground-state atoms

    NASA Astrophysics Data System (ADS)

    Stanojevic, Jovica; Côté, Robin

    2016-05-01

    We calculate the formation rate of the molecular Rb2+ion in its various bound states produced in the associative ionization of a Rydberg and a ground-state atom. Before the formation takes place, the colliding atoms are accelerated by an attractive force between the collision partners. In this way the ground-state atom is first captured by the Rydberg electron and then guided towards the positive ion-core where a molecular ion is subsequently formed. As recently demonstrated, this process results in giant collisional cross sections for the molecular ion formation, with the cross sections essentially determined by the size of the Rydberg atom. For sufficient high principal quantum numbers and atomic densities, many ground-state atoms are already located inside the Rydberg atom and ready to participate in the associative ionization. The same process can occur between a Rydberg and a ground-state atom that form a long-range Rydberg molecule, possibly contributing to the shortening of the lifetimes of Rydberg atoms and molecules. Partial support from the US Army Research Office (ARO-MURI W911NF-14-1-0378), and from NSF (Grant No. PHY-1415560).

  9. The effect of nonpolar solvents on Rydberg states: van der Waals complexes of azabicyclooctanes

    NASA Astrophysics Data System (ADS)

    Shang, Q. Y.; Moreno, P. O.; Dion, C.; Bernstein, E. R.

    1993-05-01

    The effect of solvation by nonpolar solvents on the (n,3s) Rydberg states of 1,4-diazabicyclo[2.2.2]octane (DABCO) and azabicyclo[2.2.2]octane (ABCO) is investigated through mass resolved excitation spectroscopy of their van der Waals complexes. The solute/solvent clusters formed in a supersonic expansion include DABCO and ABCO with Ar, n-CmH2m+2 (m=1-7), and CF4 and C2F6. The resulting spectra are analyzed with the help of empirical potential energy calculations of the cluster binding energies, minimum energy structures, van der Waals modes, and potential barriers between the various cluster minimum energy structures. Good agreement is found between the calculated and experimental results for DABCO and ABCO clustered with argon and methane. The spectra of clusters with all other hydrocarbons can be ascribed to only one major geometry for each cluster stoichiometry, despite the fact that calculations yield many stable geometries for each cluster. This apparent lack of agreement between calculations and experiments can be rationalized based on cluster binding energy, zero point energy, and the potential energy barriers between the cluster minima. The observed blue shift of the cluster 000 transition energy as a function of the n-alkane chain length can be qualitatively modeled by a Lennard-Jones potential for the solute-solvent interaction for both the ground and excited states. The model reveals a strong repulsive interaction between the Rydberg state electronic distribution and the solvent molecule. This repulsion depends on the distance between the solvent molecule and the solute molecule nitrogen atom.

  10. Fractional Quantum Hall Effect of lossy Rydberg Dark-State Polaritons

    NASA Astrophysics Data System (ADS)

    Grusdt, Fabian; Fleischhauer, Michael; Höning, Michael; Otterbach, Johannes

    2012-06-01

    Dark-state-polaritons (DSP) are bosonic quasiparticles arising in the interaction of light with 3-level atoms under conditions of electromagnetically induced transparency (EIT). When exposed to a strong artificial magnetic field, they can enter the lowest Landau level regime. With additional long range interactions, as realized e.g. when the 3-level atom contains a Rydberg-excited state, DSPs are natural candidates for a realization of the bosonic fractional quantum Hall effect. Besides their high controllability, they offer the possibility to examine open quantum Hall systems. We show how highly-correlated quantum Hall states of DSPs can be prepared, making use of nonlinear polariton losses. The possibility of realizing these states as stationary states of open systems is investigated. We propose a realistic quantum-optical setup, and show that different fractional quantum Hall states can be prepared, manipulated and observed. Numerical and analytical results for the excitation gaps of the ν=1/2p Laughlin states are presented.

  11. Rydberg, Valence and Ion-Pair Quintet States of O_2

    NASA Astrophysics Data System (ADS)

    Vazquez, Gabriel J.; Liebermann, Hans P.; Lefebvre-Brion, H.

    2015-06-01

    We carried out a relatively comprehensive ab--initio study of the electronic structure of O_2 and O_2^+. We employed the MRD--CI package together with the cc--pV4Z basis set augmented with seven diffuse functions of s, p and d character on each atom. In this contribution we focus on the quintet states. Potential energy curves of about 50 quintet states were computed. The spectroscopic constants of the six valence quintet states (^5σ^+_g, ^5σ^-_g, ^5σ^-_u, ^5Π_u, ^5Π_g, ^5Δ_g) dissociating to the first dissociation limit O(^3P)+O(^3P) are reported. The four ion--pair quintet states (^5σ^-_g, ^5σ^-_u, ^5Π_g, ^5Π_u) dissociating into O^+(^4S)+O^-(^2P) at 17.28 eV were also computed and their spectroscopic constants will be presented. A number of bound quintet Rydberg states belonging to series converging to the a^4Π_u, b^4σ^-_g, f^4Π_g and ^6σ^+_u states of the O_2^+ cation were identified and attributed. Long--range interactions involving the ion--pair states as they slowly approach their dissociation limit will be shown.

  12. Microwave Transitions Between Pair States Composed of Two rb Rydberg Atoms

    NASA Astrophysics Data System (ADS)

    Lee, Jeonghun; Gallagher, Tom

    2015-06-01

    Microwave transitions between pair states composed of two Rb Rydberg atoms in a magneto-optical trap are investigated. Our current interest is the transition from ndnd to (n+1)d(n-2)f states. This transition is allowed because the dipole-dipole induced configuration interaction between the ndnd state and the energetically close (n+2)p(n-2)f state admixes some of the latter state into the former. The resonance frequencies of the ndnd-(n+1)d(n-2)f transitions for n=35 to 42 have been measured and found to agree well with the calculated values. In addition, the power shifts of the resonance frequencies have been measured for n=35 to 42. The dependence of the fractional population transfer from the ndnd to (n+1)d(n-2)f states on the microwave field strength and atomic density has been measured and can be compared to a simple theoretical model. This work has been supported by the Air Force Office of Scientific Research.

  13. Microwave transitions between pair states composed of two Rb Rydberg atoms

    NASA Astrophysics Data System (ADS)

    Lee, Jeonghun; Gallagher, Tom

    2015-05-01

    Microwave transitions between pair states composed of two Rb Rydberg atoms in a magneto-optical trap are investigated. Our current interest is the transition from ndnd to (n+1)d(n-2)f states. This transition is allowed because the dipole-dipole induced configuration interaction between the ndnd state and the energetically close (n+2)p(n-2)f state admixes some of the latter state into the former. The resonance frequencies of the ndnd-(n+1)d(n-2)f transitions for n = 35 to 42 have been measured and found to agree well with the calculated values. In addition, the power shifts of the resonance frequencies have been measured for n = 35 to 42. The dependence of the fractional population transfer from the ndnd to (n+1)d(n-2)f states on the microwave field strength and atomic density has been measured and can be compared to a simple theoretical model. This work has been supported by the Air Force Office of Scientific Research.

  14. Calculating helium atomic excited states in coordinate space

    NASA Astrophysics Data System (ADS)

    Hall, Shane; Siegel, P. B.

    2015-12-01

    Two coupled Schrödinger equations are used to calculate excited states of atomic helium. Using product state functions for the two-electron state, the shooting method is used to numerically determine the energies of the allowed singlet and triplet levels. The calculations agree well with the data, and the coordinate-space basis yields Schrödinger equations for helium that are familiar to students who have used similar methods for the hydrogen atom.

  15. Corrigendum to "New REMPI observations and analyses for Rydberg and ion-pair states of HI" [J. Mol. Spectrosc. 290 (2013) 5-12

    NASA Astrophysics Data System (ADS)

    Hróðmarsson, Helgi Rafn; Wang, Huasheng; Kvaran, Ágúst

    2016-06-01

    This article presents a comprehensive overview of Rydberg and ion-pair states for HI in the two-photon excitation region of 69,600-72,300 cm-1. There are two errors in the paper that need to be addressed. These are associated with (i) the wavelength calibration and (ii) the assignment of the d3Π0(1) Rydberg state spectrum.

  16. Properties of Th3+ from Optical Spectroscopy of High-L Rydberg states of Th2+

    NASA Astrophysics Data System (ADS)

    Keele, Julie; Woods, Shannon; Lundeen, Stephen; Fehrenbach, Charles

    2011-05-01

    The Fr-like Thorium ion, Th3+, has one valence electron outside a Rn-like closed shell, but its ground electronic state is 2F5/2 instead of 2S1/2 due to the high nuclear charge. The positions of the lowest seven levels of this ion have been established by optical spectroscopy, but no other properties have been measured previously. We measure the properties of the Th3+ ground state that control its long-range interactions, such as polarizabilities and permanent moments, by attaching a single electron in a non-penetrating Rydberg state and measuring the details of its binding energy using the Resonant Excitation Stark Ionization Spectroscopy (RESIS) technique. A typical transition is n = 29 to n ' = 72. The laser excitation partially resolves the complex fine structure pattern in the lower state caused by the long-range interactions, and this leads to measurements of the core ion properties controlling those interactions. Supported by the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Science, U.S. Dept. of Energy.

  17. Spin Exchange in Rydberg EIT

    NASA Astrophysics Data System (ADS)

    Nicholson, Travis; Thompson, Jeff; Liang, Qiyu; Cantu, Sergio; Venkatramani, Aditya; Pohl, Thomas; Choi, Soonwon; Lukin, Mikhail; Vuletic, Vladan

    2016-05-01

    The realization of strong optical nonlinearities between two photons has been a longstanding goal in quantum science. We achieve large single-photon-level nonlinearities with Rydberg EIT, which combines slow light techniques with strongly interacting Rydberg states. For two Rydberg atoms in the same state, a Van der Waals interaction is the dominant coupling mechanism. Inherently stronger dipole-dipole interactions are also possible between atoms in different Rydberg states. Using light storage and microwave resonances, we study the effect of dipole-dipole interactions in Rydberg EIT. We observe a coherent spin exchange effect for pairs of states dominated by dipole-dipole interactions. Spin exchange manifests as an increase in optical transmission through a cold Rubidium gas that is highly dissipative in the presence of Van der Waals interactions. We also observe a controlled π / 2 phase shift due to this effect, which paves the way for robust, universal all-optical quantum gates.

  18. Long lifetimes of high molecular Rydberg states in crossed magnetic and electric fields: An experimental and classical computational study

    NASA Astrophysics Data System (ADS)

    Mühlpfordt, Annette; Even, U.; Rabani, Eran; Levine, R. D.

    1995-05-01

    Crossed magnetic and electric fields are observed to extend the lifetime of high molecular Rydberg states of DABCO (1,4-Diazabicyclo[2.2.2]octane) well into the microsecond range. The experimental and computational (using classical mechanics and for a diatomic polar core) results agree both on the magnitude of the effect and on its decrease with increasing electrical field. Theoretical considerations suggest that this time-stretching effect is only present for high Rydberg states and/or for not too weak fields. The computed lifetime increases as the magnetic-field strength is decreased but it requires a finite magnetic field for the onset of the effect. The experimental technique of detection of the surviving Rydberg states via their ionization in a delayed field pulse (known as ZEKE spectroscopy) is most easily implemented for high (say, n>100) but not too high (n<400) Rydberg states. In this regime, the magnetic field required for the additional time stretching is larger than that due to the earth but can be significantly weaker than that required to induce extensive chaotic behavior. The results of the numerically exact classical simulations are interpreted using equations of motion, cast in the form of a mapping, which retain terms up to second order in the fields. (The first-order terms are qualitatively and quantitatively not, by themselves, sufficient.) As is to be expected on physical grounds, the origin of the effect is the slow, periodic modulation of the magnitude of the magnetic quantum number ml of the electron due to terms second order in the magnetic field. Since the angular momentum l of the electron is bounded from below by ml, and since it requires a low l for the electron to couple effectively to the molecular core, the presence of the magnetic field provides for an elongation of the time scale which is over and above that made possible due to the periodic motion of l due to the dc electric field.

  19. Velocity-selective electromagnetically-induced-transparency measurements of potassium Rydberg states

    NASA Astrophysics Data System (ADS)

    Xu, Wenchao; DeMarco, Brian

    2016-01-01

    We demonstrate a velocity selection scheme that mitigates suppression of electromagnetically induced transparency (EIT) by Doppler shifts for coupling wavelengths larger than the probe wavelength. An optical pumping beam counterpropagating with the EIT probe beam transfers atoms between hyperfine states in a velocity-selective fashion. Measurement of the transmitted probe beam synchronous with chopping of the optical pumping beam enables a Doppler-free EIT signal to be detected. Transition frequencies between 5 P1 /2 and n S1 /2 states for n =26 , 27, and 28 in 39K are obtained via EIT spectroscopy in a heated vapor cell with a probe beam stabilized to the 4 S1 /2→5 P1 /2 transition. Using previous high-resolution measurements of the 4 S1 /2→n S1 /2 transitions, we make a determination of the absolute frequency of the 4 S1 /2→5 P1 /2 transition. Our measurement is shifted by 560 MHz from the currently accepted value with a twofold improvement in uncertainty. These measurements will enable novel experiments with Rydberg-dressed ultracold Fermi gases composed of 40K atoms.

  20. Exploring the high-order harmonic generation from Rydberg states with a fixed Keldysh parameter

    NASA Astrophysics Data System (ADS)

    Ata Bleda, Erdi; Yavuz, Ilhan; Altun, Zikri; Topcu, Turker

    2012-06-01

    The commonly adopted viewpoint that the Keldysh parameter γ determines the dynamical regime of ionization in strong field physics has long been demonstrated to be a misleading one. One can then ask what happens in strong field ionization as relevant parameters, such as laser intensity and frequency, are varied while keeping γ fixed. We present results from our simulations of high-order harmonic generation (HHG) from Rydberg states of a hydrogen atom. We calculate high harmonic spectra from various initial states with n up to 42, where the laser intensities and the frequencies are scaled from those for n=1 in order to maintain a fixed Keldysh parameter γ<1. We find that as we go up in n for a fixed γ, the position of the cut-off scales as ˜1/n^2 in terms of the cut-off law predicted by the three-step model for n=1. However, a secondary cut-off structure forms below this, which moves to lower harmonics as n is increased. This second cut-off splits the plateau into two regions, one higher in yield and below the second cut-off, and the second with lower yield following it. We further investigate the final n-distributions for some of the interesting cases to elucidate the physical mechanism leading to this structure

  1. Dynamics of Bloch State Positronium Emission from MOF Targets Studied via Rydberg TOF Spectroscopy

    NASA Astrophysics Data System (ADS)

    Piñeiro Escalera, Alina; Jones, Adric; Mills, Allen

    2016-05-01

    Recent advances in the efficient production and detection of Rydberg positronium (Ps) have made it possible to perform energy- and angle- resolved time-of-flight (TOF) spectroscopy with Ps. We report here TOF measurements of Ps emission from the metal-oxide framework (MOF) targets, MOF-5 and ZIF-8. MOFs are a recently synthesized class of chemical structures, characterized by high long-range order and large surface area to volume ratios (i.e., they are highly porous and uniform, crystalline materials). Ps is found to be emitted predominantly in a series of monoenergetic peaks, providing clear evidence of Ps Bloch states. Measuring the relative populations of the monoenergetic peaks, as a function of implantation energy and target temperature, provides insight into the target-dependent dynamics of Bloch state Ps. Work supported by the U.S. National Science Foundation Grants No. PHY 1206100 and No. PHY 1040590 and the National Science Foundation Graduate Research Fellowship Progam (NSF-GRFP). DOE BES DE-FG02-13ER46972 (MOF-5 synthesis and characterization).

  2. Far infrared stimulated emission from the ns and nf Rydberg states of NO

    SciTech Connect

    Furukawa, Hiroki; Araki, Mitsunori; Umeki, Hiroya; Tsukiyama, Koichi

    2013-06-28

    We report directional far-infrared emission from the {upsilon}= 0 vibrational levels of the 9s{sigma}, 10s{sigma}, 11s{sigma}, 9f, and 10f Rydberg states of NO in the gas phase. The emission around 28 and 19 {mu}m from the 9f state was identified as the downward 9f{yields} 8g and subsequent 8g{yields} 7f cascade transitions, respectively. The emission around 38 and 40 {mu}m from the 10f state was identified as the 10f{yields} 9g and 10f{yields} 9d{sigma}{pi} transition, respectively. Following the excitation of the 9s{sigma}, 10s{sigma}, and 11s{sigma} states, the emission around 40, 60, and 83 {mu}m was assigned as the 9s{sigma}{yields} 8p{sigma}, 10s{sigma}{yields} 9p{sigma}, and 11s{sigma}{yields} 10p{sigma} transitions, respectively. In addition to these emission systems originated from the laser-prepared levels, we found the emission bands from the 8f, 9f, and 10f states which are located energetically above the 9s{sigma}, 10s{sigma}, and 11s{sigma} states, respectively. This observation suggests that the upward 8f Leftwards-Arrow 9s{sigma}, 9f Leftwards-Arrow 10s{sigma}, and 10f Leftwards-Arrow 11s{sigma} optical excitation occurs. Since the energy differences between nf and (n+ 1)s{sigma} states correspond to the wavelength longer than 100 {mu}m, the absorption of blackbody radiation is supposed to be essential for these upward transitions.

  3. Ultralong-range polyatomic Rydberg molecules

    NASA Astrophysics Data System (ADS)

    Gonzalez-Ferez, Rosario

    2016-05-01

    Ultralong-range polyatomic Rydberg molecules are formed when a ground-state atom is bound to a Rydberg atom. The binding mechanism of these Rydberg molecules is based on the low-energy collisions between a Rydberg electron and a ground-state atom and leads to the unusual oscillatory behavior of the adiabatic potential energy curves. If the ground-state atom immersed into the Rydberg wave function is replaced by a heteronuclear diatomic molecule another type of polyatomic Rydberg molecules can form. In this case, the Rydberg electron is coupled to the internal states of the polar ground-state molecule. In this talk, we will explore the electronic structure and rovibrational properties of these ultralong-range polyatomic Rydberg molecule. For the second type of Rydberg molecules, the polar dimer is allowed to rotate in the electric fields generated by the Rydberg electron and Rydberg core as well as an additional external field. We will investigate the metamorphosis of the Born-Oppenheimer potential curves, essential for the binding mechanism, with varying electric field and analyze the resulting properties such as the vibrational structure and the alignment and orientation of the polar dimer.

  4. Detection of precise quantum defects of the 6snd, 6sng and 6sni Rydberg states of Ytterbium

    NASA Astrophysics Data System (ADS)

    Niyaz, Fathima; Nunkaew, Jirakan; Gallagher, Thomas

    2016-05-01

    We use a selective field ionization technique to observe the microwave transitions of Ytterbium Rydberg states, from the 6s(n + 3)d states to the 6sng and 6snh states for 27 <= n <= 33. We also observe the microwave transitions from 6snd to 6s(n + 1)d for states 33 <= n <= 38. Our measurements and previous 6snd to 6s(n + 1)d measurements give precise values for the 6snd quantum defects which indicate the presence of a previously undetected perturbation in the series. This work has been supported by the U. S. Department of Energy, Office of Basic Energy Sciences.

  5. Formation of Triplet Positron-helium Bound State by Stripping of Positronium Atoms in Collision with Ground State Helium

    NASA Technical Reports Server (NTRS)

    Drachman, Richard J.

    2006-01-01

    Formation of triplet positron-helium bound state by stripping of positronium atoms in collision with ground state helium JOSEPH DI RlENZI, College of Notre Dame of Maryland, RICHARD J. DRACHMAN, NASA/Goddard Space Flight Center - The system consisting of a positron and a helium atom in the triplet state e(+)He(S-3)(sup e) was conjectured long ago to be stable [1]. Its stability has recently been established rigorously [2], and the values of the energies of dissociation into the ground states of Ps and He(+) have also been reported [3] and [4]. We have evaluated the cross-section for this system formed by radiative attachment of a positron in triplet He state and found it to be small [5]. The mechanism of production suggested here should result in a larger cross-section (of atomic size) which we are determining using the Born approximation with simplified initial and final wave functions.

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

    SciTech Connect

    Zelener, B. B. Saakyan, S. A.; Sautenkov, V. A.; Manykin, E. A.; Zelener, B. V.; Fortov, V. E.

    2015-12-15

    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.

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

    NASA Astrophysics Data System (ADS)

    Zelener, B. B.; Saakyan, S. A.; Sautenkov, V. A.; Manykin, E. A.; Zelener, B. V.; Fortov, V. E.

    2015-12-01

    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.

  8. Fano resonances observed in helium nanodroplets

    NASA Astrophysics Data System (ADS)

    LaForge, A. C.; Regina, D.; Jabbari, G.; Gokhberg, K.; Kryzhevoi, N. V.; Krishnan, S. R.; Hess, M.; O'Keeffe, P.; Ciavardini, A.; Prince, K. C.; Richter, R.; Stienkemeier, F.; Cederbaum, L. S.; Pfeifer, T.; Moshammer, R.; Mudrich, M.

    2016-05-01

    Doubly excited Rydberg states of helium (He) have been studied in nanodroplets using synchrotron radiation. Although qualitatively similar to their atomic counterparts, the Fano resonances in droplets are broader and exhibit blueshifts which increase for the higher excited states. However, varying the droplet size hardly affects the shapes of the resonances. Furthermore, additional dipole-forbidden resonances appear which are not seen in the He atom. We discuss these features in terms of localized atomic states perturbed by the surrounding He atoms.

  9. Ionization yield and absorption spectra reveal superexcited Rydberg state relaxation processes in H2O and D2O

    NASA Astrophysics Data System (ADS)

    Fillion, J.-H.; Dulieu, F.; Baouche, S.; Lemaire, J.-L.; Jochims, H. W.; Leach, S.

    2003-07-01

    The absorption cross section and the ionization quantum yield of H2O have been measured using a synchrotron radiation source between 9 and 22 eV. Comparison between the two curves highlights competition between relaxation processes for Rydberg states converging to the first tilde A 2A 1 and to the second tilde B 2B 2 excited states of H2O+. Comparison with D2O absorption and ionization yields, derived from Katayama et al (1973 J. Chem. Phys. 59 4309), reveals specific energy-dependent deuteration effects on competitive predissociation and autoionization relaxation channels. Direct ionization was found to be only slightly affected by deuteration.

  10. Rydberg and valence state excitation dynamics: a velocity map imaging study involving the E-V state interaction in HBr.

    PubMed

    Zaouris, Dimitris; Kartakoullis, Andreas; Glodic, Pavle; Samartzis, Peter C; Rafn Hróðmarsson, Helgi; Kvaran, Ágúst

    2015-04-28

    Photoexcitation dynamics of the E((1)Σ(+)) (v' = 0) Rydberg state and the V((1)Σ(+)) (v') ion-pair vibrational states of HBr are investigated by velocity map imaging (VMI). H(+) photoions, produced through a number of vibrational and rotational levels of the two states were imaged and kinetic energy release (KER) and angular distributions were extracted from the data. In agreement with previous work, we found the photodissociation channels forming H*(n = 2) + Br((2)P3/2)/Br*((2)P1/2) to be dominant. Autoionization pathways leading to H(+) + Br((2)P3/2)/Br*((2)P1/2) via either HBr(+)((2)Π3/2) or HBr(+)*((2)Π1/2) formation were also present. The analysis of KER and angular distributions and comparison with rotationally and mass resolved resonance enhanced multiphoton ionization (REMPI) spectra revealed the excitation transition mechanisms and characteristics of states involved as well as the involvement of the E-V state interactions and their v' and J' dependence. PMID:25801122

  11. Ab initio potential energy curves of the valence, Rydberg, and ion-pair states of iodine monochloride, ICl

    SciTech Connect

    Kalemos, Apostolos; Prosmiti, Rita

    2014-09-14

    We present for the first time a coherent ab initio study of 39 states of valence, Rydberg, and ion-pair character of the diatomic interhalogen ICl species through large scale multireference variational methods including spin-orbit effects coupled with quantitative basis sets. Various avoided crossings are responsible for a non-adiabatic behaviour creating a wonderful vista for its theoretical description. Our molecular constants are compared with all available experimental data with the aim to assist experimentalists especially in the high energy regime of up to ∼95 000 cm{sup −1}.

  12. Rotationally Resolved Vacuum Ultraviolet Resonance-Enhanced Multiphoton Ionization (VUV REMPI) of Acetylene via the G̃ Rydberg State.

    PubMed

    Schmidt-May, Alice F; Grütter, Monika; Neugebohren, Jannis; Kitsopoulos, T N; Wodtke, Alec M; Harding, Dan J

    2016-07-14

    We present a 1 + 1' resonance-enhanced multiphoton ionization (REMPI) scheme for acetylene via the linear G̃ 4sσ (1)Πu Rydberg state, offering partial rotational resolution and the possibility to detect excitation in both the cis- and trans-bending modes. The resonant transition to the G̃ state is driven by a vacuum ultraviolet (VUV) photon, generated by resonant four-wave mixing (FWM) in krypton. Ionization from the short-lived G̃ state then occurs quickly, driven by the high intensity of the residual light from the FWM process. We have observed nine bands in the region between 79 200 cm(-1) and 80 500 cm(-1) in C2H2 and C2D2. We compare our results with published spectra in this region and suggest alternative assignments for some of the Renner-Teller split bands. Similar REMPI schemes should be applicable to other small molecules with picosecond lifetime Rydberg states. PMID:27073931

  13. Detection of excited-state electron bubbles in superfluid helium.

    PubMed

    Konstantinov, Denis; Maris, Humphrey J

    2003-01-17

    We report on experiments in which the pressure oscillation associated with a sound wave is used to explode electron bubbles in liquid helium. Using this technique, we are able to detect the presence of electron bubbles in excited states. PMID:12570553

  14. Direct Electron Impact Excitation of Rydberg-Valence States of Molecular Nitrogen

    NASA Astrophysics Data System (ADS)

    Malone, C. P.; Johnson, P. V.; Liu, X.; Ajdari, B.; Muleady, S.; Kanik, I.; Khakoo, M. A.

    2012-12-01

    Collisions between electrons and neutral N2 molecules result in emissions that provide an important diagnostic probe for understanding the ionospheric energy balance and the effects of space weather in upper atmospheres. Also, transitions to singlet ungerade states cause N2 to be a strong absorber of solar radiation in the EUV spectral range where many ro-vibrational levels of these Rydberg-valence (RV) states are predissociative. Thus, their respective excitation and emission cross sections are important parameters for understanding the [N]/[N2] ratio in the thermosphere of nitrogen dominated atmospheres. The following work provides improved constraints on absolute and relative excitation cross sections of numerous RV states of N2, enabling more physically accurate atmospheric modeling. Here, we present recent integral cross sections (ICSs) for electron impact excitation of RV states of N2 [6], which were based on the differential cross sections (DCSs) derived from electron energy-loss (EEL) spectra of [5]. This work resulted in electronic excitation cross sections over the following measured vibrational levels: b 1Πu (v‧=0-14), c3 1Πu (v‧=0-3), o3 1Πu (v‧=0-3), b‧ 1Σu+ (v‧=0-10), c‧4 1Σu+ (v‧=0-3), G 3Πu (v‧=0-3), and F 3Πu (v‧=0-3). We further adjusted the cross sections of the RV states by extending the vibronic contributions to unmeasured v‧-levels via the relative excitation probabilities (REPs) as discussed in [6]. This resulted in REP-scaled ICSs over the following vibrational levels for the singlet ungerade states: b(0-19), c3(0-4), o3(0-4), b‧(0-16), and c‧4(0-8). Comparison of the ICSs of [6] with available EEL based measurements, theoretical calculations, and emission based work generally shows good agreement within error estimations, except with the recent reevaluation provided by [1]. Further, we have extended these results, using the recent EEL data of [3], to include the unfolding of better resolved features above ~13

  15. A quantum defect analysis of heavy Rydberg behaviour in the B(u+1Σ) and B″ B ‾ (u+1Σ) states of H2 and the B(u+1Σ) state of D2

    NASA Astrophysics Data System (ADS)

    Lawley, Kenneth P.; Donovan, Robert J.

    2016-08-01

    Heavy Rydberg behaviour in the B(u+1Σ) and B″ B ‾ (u+1Σ) ion-pair states of H2 and the B(u+1Σ) state of D2, is analysed in terms of the absolute quantum defects of the vibronic levels. The influence of the inner repulsive wall of ion-pair potentials on heavy Rydberg behaviour is considered and shown to determine the size of both absolute quantum defects and their energy dependence.

  16. Applicability of equations of state for modeling helium systems

    NASA Astrophysics Data System (ADS)

    Thomas, Rijo Jacob; Dutta, Rohan; Ghosh, Parthasarathi; Chowdhury, Kanchan

    2012-07-01

    Proper design of helium systems with large number of components and involved configurations such as helium liquefiers/refrigerators requires the use of tools like process simulators. The accuracy of the simulation results, to a great extent, depends on the accuracy of property data. For computation of thermodynamic properties of helium, the 32-parameter MBWR equation of state proposed by McCarty and Arp [1] is widely used. However, it is computationally involved, makes the simulation process more time-consuming and sometimes leads to computational difficulties such as numerical oscillations, divergence in solution especially, when the process operates over a wide thermodynamic region and is constituted of many components. Substituting MBWR EOS by simpler equations of state (EOS(s)) at selected thermodynamic planes, where the simpler EOS(s) have the similar accuracy as that of MBWR EOS may enhance ease of computation. In the present paper, the methodology to implement this concept has been elucidated with examples of steady state and dynamic simulation of helium liquefier/refrigerator based on Collins cycle. The above concept can be applied to thermodynamic analysis of other process cycles where computation of fluid property is involved.

  17. Using Uncertainty Principle to Find the Ground-State Energy of the Helium and a Helium-like Hookean Atom

    ERIC Educational Resources Information Center

    Harbola, Varun

    2011-01-01

    In this paper, we accurately estimate the ground-state energy and the atomic radius of the helium atom and a helium-like Hookean atom by employing the uncertainty principle in conjunction with the variational approach. We show that with the use of the uncertainty principle, electrons are found to be spread over a radial region, giving an electron…

  18. Observation of intracluster Coulombic decay of Rydberg-like states triggered by intense near-infrared pulses

    NASA Astrophysics Data System (ADS)

    Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Gokhberg, Kirill; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, Arnaud

    2015-05-01

    Interatomic Coulombic decay (ICD) describes a process, where an excited atom relaxes by transferring its energy to an atom in the environment that gets ionized. So far, ICD has been observed following XUV ionization or excitation of clusters. Here we present novel results of an intracluster Coulombic decay mechanism induced by intense NIR pulses and following Rydberg atom formation in the generated nanoplasma. When a highly-excited Rydberg atom relaxes to its ground state by transferring its excess energy to a weakly bound electron in the environment, electrons with kinetic energies close to the atomic ionization potential are emitted. We show evidence for such an intracluster Coulombic decay process that leaves clear signatures in the electron kinetic energy spectra. ICD is time-resolved in a pump-probe experiment, where a weak probe pulse depopulates the excited states, leading to a quenching of the ICD signal. We find a decay time of 87 ps, which is siginificantly longer than for previous ICD observations, where inner-shell holes were created by XUV pulses. Intracluster Coulombic decay is found to be a generic process that takes places in atomic and molecular clusters and at different wavelengths. It may play an important role in biological systems and in astronomical plasmas. Previous affiliation: Max-Born-Institut, Berlin, Germany.

  19. Isotope Shifts and Hyperfine Structure in Calcium 4snp1P1 and 4snf F Rydberg States

    SciTech Connect

    Muller, P.; Bushaw, Bruce A.; Nortershauser, Wilfried; Wendt, K.

    2000-06-01

    Isotope shifts and hyperfine structure have been measured in 4snp 1P1 and 4snf F Rydberg states for all stable calcium isotopes and the radioisotope 41Ca using high-resolution laser spectroscopy. Triple-resonance excitation via 4s2 1S0 --- 4s4p 1P1 --- 4s4d 1D2 --- Rydberg State was followed by photoionization with a CO2 laser and mass selective ion detection. Isotope shifts for the even-mass isotopes have been analyzed to derive specific mass shift and field shift factors. The apparent isotope shifts for 41Ca and 43Ca exhibit anomalous values that are n-dependent. This is interpreted in terms of hyperfine-induced fine structure mixing, which becomes very pronounced when singlet-triplet fine structure splitting is comparable to the hyperfine interaction energy. Measurements of fine structure splittings for the predominant isotope 40Ca have been used as input parameters for theoretical calculation of the perturbed hyperfine structure. Results obtained by diagonalizing the second-order hyperfine interaction matrices agree very well with experimentally observed spectra.

  20. Core-Penetrating Rydberg Series of BaF: New Electronic States in the n* ≈ 4 Region

    NASA Astrophysics Data System (ADS)

    Jakubek, Zygmunt J.; Field, Robert W.

    1996-09-01

    We report results of our studies of the electronic spectrum of the BaF molecule in the energy region of T0= 31 460-32 400 cm -1(3.88 < n* < 4.16). We have observed four new electronic states (all constants in cm -1): K2Π 1/2( T0= 31 996), 4.08 2Σ +( T0= 32 166.293(2), B0= 0.2333892(17)), 3.94 2Δ ( T1= 32 252.426(2), B1= 0.2294684(16), A1= 0.879(13)), and J2Π ( T0= 32 297.918(2), B0= 0.22952165(51), A0= 57.196(1)). In addition, the previously observed G2Σ +( T0= 30 969.715(2), B0= 0.2297411(13)) and H2Σ +( T0= 31 606.238(2), B0= 0.23031573(85)) states were rotationally analyzed for the first time. We verified by isotope analysis that the G2Σ +state, previously reported by J. Singh and H. Mohan [ Indian J. Pure Appl. Phys.11,918-922 (1973)], had been incorrectly assigned vibrationally. The I2Σ +state, which Singh and Mohan observed at low resolution, was absent from our spectra and we suspect that this state belongs to a species other than BaF. Electronic term values for the remaining seven not yet observed BaF core-penetrating Rydberg states below n* = 6 were predicted by interpolation of well-characterized Rydberg series. We suggest that the E″ state, assigned by Effantin et al.as a 2Π 1/2state [C. Effantin, A. Bernard, J. D'Incan, E. Andrianavalona, and R. F. Barrow, J. Mol. Spectrosc.145,456-457 (1991)] must be reassigned as a 2Δ state.

  1. The Jahn-Teller effect in the 3pe' Rydberg state of H3: review of experimental and ab initio determinations.

    PubMed

    Jungen, Ch; Jungen, M; Pratt, S T

    2012-11-13

    The dissociative recombination (DR) of H(3)(+) ions with electrons, producing neutral atomic and molecular fragments, is driven primarily by the vibronic Jahn-Teller (JT) interaction between the electronic components of the pe' e(-)-H(3)(+) collision (Rydberg) channel. The JT parameters characterizing this interaction are therefore of great interest as they are required for the theoretical predictions of the DR cross section. In this contribution, we review various determinations of these quantities that have been made previously, based both on spectroscopic studies of 3pe' Rydberg-excited H(3) states, and on the analysis of the corresponding ab initio H(3) Rydberg potential surfaces near the conical intersection (D(3h) symmetry) for n=3-5. The highly correlated theoretical 3pe' potential surfaces of Mistrík et al. are used for a new determination of both the linear and quadratic JT terms. PMID:23028155

  2. Method for laser spectroscopy of metastable pionic helium atoms

    NASA Astrophysics Data System (ADS)

    Hori, M.; Sótér, A.; Aghai-Khozani, H.; Barna, D.; Dax, A.; Hayano, R. S.; Murakami, Y.; Yamada, H.

    2015-08-01

    The PiHe collaboration is currently attempting to carry out laser spectroscopy of metastable pionic helium atoms using the high-intensity π - beam of the ring cyclotron facility of the Paul Scherrer Institute. These atoms are heretofore hypothetical three-body Coulomb systems each composed of a helium nucleus, a π - occupying a Rydberg state, and an electron occupying the 1s ground state. We briefly review the proposed method by which we intend to detect the laser spectroscopic signal. This complements our experiments on metastable antiprotonic helium atoms at CERN.

  3. Rydberg series of 1Σu+ and 1Δu states of the Li2 molecule studied by the promotion model

    NASA Astrophysics Data System (ADS)

    Kim, Hyun-Jin; Lee, Chun-Woo

    2015-01-01

    We studied the Rydberg series for the 12 1Σu+, 7 1Δu, and 1 1Γu states. This set consists of the seventeen states derivable from the Li(2s) + Li(nl) (n = 2, 3, 4, 5) configuration, one 1Σu+ state and one 1Δu state derivable from Li(2s) + Li(6p) and Li(2s) + Li(6d), respectively, plus one ionic state. We used the multireference configuration interaction method, combined with the Stuttgart/Köln group’s effective core potential/core polarization potential method, to calculate their potential energy curves (PECs). Four Rydberg series, σuns (n = 3, 4, 5, 6), σunp (n = 2, 3, 4, 5), δund (n = 3, 4, 5, 6), and δunf (n = 4, 5), are identified near the potential energy minima (referred to as the ‘Rydberg region’). The promotion model is used to examine the behaviour of PECs and quantum defect curves (QDCs) by constructing diabatic PECs and QDCs. Besides QDCs, effective n and promotion curves are also used to directly examine the promotion. This reveals that the promotion model can be successfully applied to the singlet ungerade states of Li2, indicating that the Rydberg region has the same characteristics as the united atom (UA) limit. Thus, the Rydberg region in Li2 is much closer to the UA limit than the separated atoms (SA) limit. Correlation diagrams based on the promotion model show a big difference in the number of avoided crossings for the 1Σu+ and 1Δu states. The larger number of avoided crossings for 1Σu+ states produces features in the PECs of the 1Σu+ states such as shoulders, flattening, and grouping. The promotion model not only helps to identify Rydberg series, but also to explain all the major and minor aspects and subtle phenomena observed in the PECs and spectroscopic constants of the singlet ungerade Rydberg states of Li2.

  4. Density of states of helium droplets

    NASA Astrophysics Data System (ADS)

    Hansen, Klavs; Johnson, Michael D.; Kresin, Vitaly V.

    2007-12-01

    Accurate analytical expressions for the state densities of liquid He4 droplets are derived, incorporating the ripplon and phonon degrees of freedom. The microcanonical temperature and the ripplon angular momentum level density are also evaluated. The approach is based on inversions and systematic expansions of canonical thermodynamic properties.

  5. Interaction of Rydberg atoms in circular states with the alkaline-earth Ca(4s{sup 2}) and Sr(5s{sup 2}) atoms

    SciTech Connect

    Mironchuk, E. S.; Narits, A. A.; Lebedev, V. S.

    2015-11-15

    The resonant mechanism of interaction of alkaline-earth atoms having a low electron affinity to Rydberg atoms in circular (l = vertical bar m vertical bar = n–1) and near-circular states has been studied. To describe the dynamics of resonant processes accompanied by nonadiabatic transitions between ionic and Rydberg covalent terms of a quasimolecule, an approach based on the integration of coupled equations for the probability amplitudes has been developed taking into account the possibility of the decay of an anion in the Coulomb field of the positive ionic core of a highly excited atom. The approach involves the specific features of the problem associated with the structure of the wavefunction of a Rydberg electron in states with high orbital angular momenta l ∼ n–1. This approach provides a much more accurate description of the dynamics of electronic transitions at collisions between atoms than that within the modified semiclassical Landau–Zener model. In addition, this approach makes it possible to effectively take into account many channels of the problem. The cross sections for resonant quenching of Rydberg states of the Li(nlm) atom with given principal n, orbital l = n–1, and magnetic m quantum numbers at thermal collisions with the Ca(4s{sup 2}) and Sr(5s{sup 2}) atoms have been calculated. The dependences of the results on n, m, and angle α between the relative velocity of the atoms and the normal to the plane of the orbit of the Rydberg electron have been obtained. The influence of orientational effects on the efficiency of the collisional destruction of circular and near-circular states has been studied. The results indicate a higher stability of such states to their perturbations by neutral particles as compared to usually studied nl states with low values of l (l ≪ n)

  6. Interaction of Rydberg atoms in circular states with the alkaline-earth Ca(4 s 2) and Sr(5 s 2) atoms

    NASA Astrophysics Data System (ADS)

    Mironchuk, E. S.; Narits, A. A.; Lebedev, V. S.

    2015-11-01

    The resonant mechanism of interaction of alkaline-earth atoms having a low electron affinity to Rydberg atoms in circular ( l = | m| = n-1) and near-circular states has been studied. To describe the dynamics of resonant processes accompanied by nonadiabatic transitions between ionic and Rydberg covalent terms of a quasimolecule, an approach based on the integration of coupled equations for the probability amplitudes has been developed taking into account the possibility of the decay of an anion in the Coulomb field of the positive ionic core of a highly excited atom. The approach involves the specific features of the problem associated with the structure of the wavefunction of a Rydberg electron in states with high orbital angular momenta l ~ n-1. This approach provides a much more accurate description of the dynamics of electronic transitions at collisions between atoms than that within the modified semiclassical Landau-Zener model. In addition, this approach makes it possible to effectively take into account many channels of the problem. The cross sections for resonant quenching of Rydberg states of the Li( nlm) atom with given principal n, orbital l = n-1, and magnetic m quantum numbers at thermal collisions with the Ca(4 s 2) and Sr(5 s 2) atoms have been calculated. The dependences of the results on n, m, and angle α between the relative velocity of the atoms and the normal to the plane of the orbit of the Rydberg electron have been obtained. The influence of orientational effects on the efficiency of the collisional destruction of circular and near-circular states has been studied. The results indicate a higher stability of such states to their perturbations by neutral particles as compared to usually studied nl states with low values of l ( l ≪ n).

  7. Selective-field-ionization dynamics of a lithium m=2 Rydberg state: Landau-Zener model versus quantal approach

    SciTech Connect

    Foerre, M.; Hansen, J.P.

    2003-05-01

    The selective-field-ionization (SFI) dynamics of a Rydberg state of lithium with magnetic quantum number m=2 is studied in detail based on two different theoretical models: (1) a close coupling integration of the Schroedinger equation and (2) the multichannel (incoherent) Landau-Zener (MLZ) model. The m=2 states are particularly interesting, since they define a border zone between fully adiabatic (m=0,1) and fully diabatic (m>2) ionization dynamics. Both sets of calculations are performed up to, and above, the classical ionization limit. It is found that the MLZ model is excellent in the description of the fully diabatic dynamics while certain discrepancies between the time dependent quantal amplitudes appear when the dynamics become involved. Thus, in this region, the analysis of experimental SFI spectra should be performed with care.

  8. Tunable cw UV laser with <35 kHz absolute frequency instability for precision spectroscopy of Sr Rydberg states.

    PubMed

    Bridge, Elizabeth M; Keegan, Niamh C; Bounds, Alistair D; Boddy, Danielle; Sadler, Daniel P; Jones, Matthew P A

    2016-02-01

    We present a solid-state laser system that generates over 200 mW of continuous-wave, narrowband light, tunable from 316.3 nm - 317.7 nm and 318.0 nm - 319.3 nm. The laser is based on commercially available fiber amplifiers and optical frequency doubling technology, along with sum frequency generation in a periodically poled stoichiometric lithium tantalate crystal. The laser frequency is stabilized to an atomic-referenced high finesse optical transfer cavity. Using a GPS-referenced optical frequency comb we measure a long term frequency instability of < 35 kHz for timescales between 10(-3) s and 10(3) s. As an application we perform spectroscopy of Sr Rydberg states from n = 37 - 81, demonstrating mode-hop-free scans of 24 GHz. In a cold atomic sample we measure Doppler-limited linewidths of 350 kHz. PMID:26906804

  9. Rydberg phases of Hydrogen and low energy nuclear reactions

    NASA Astrophysics Data System (ADS)

    Olafsson, Sveinn; Holmlid, Leif

    2016-03-01

    For over the last 26 years the science of cold fusion/LENR has been researched around the world with slow pace of progress. Modest quantity of excess heat and signatures of nuclear transmutation and helium production have been confirmed in experiments and theoretical work has only resulted in a large flora of inadequate theoretical scenarios. Here we review current state of research in Rydberg matter of Hydrogen that is showing strong signature of nuclear processes. In the presentation experimental behavior of Rydberg matter of hydrogen is described. An extensive collaboration effort of surface physics, catalysis, atomic physics, solid state physics, nuclear physics and quantum information is need to tackle the surprising experimental results that have so far been obtained. Rydberg matter of Hydrogen is the only known state of matter that is able to bring huge collection of protons to so short distances and for so long time that tunneling becomes a reasonable process for making low energy nuclear reactions. Nuclear quantum entanglement can also become realistic process at theses conditions.

  10. Auger width of metastable states in antiprotonic helium

    SciTech Connect

    Revai, J.; Kruppa, A.T.

    1998-01-01

    Auger decay probabilities of metastable states in antiprotonic helium are derived using a minimal extension of the existing bound-state wave functions to account for the electron continuum. Calculations were performed for the Born-Oppenheimer wave functions of Shimamura [Phys. Rev. A {bold 46}, 3776 (1992)] and the variational wave functions of Korobov [Phys. Rev. A {bold 54}, 1749 (1996)]. Our results suggest that the overall accuracy of the Auger widths calculated from the presently available bound-state wave functions is not sufficient. {copyright} {ital 1998} {ital The American Physical Society}

  11. Ultrafast spectroscopy of wavelength-dependent coherent photoionization cross sections of Li2 wave packets in the E1Σg+ state: The role of Rydberg states

    NASA Astrophysics Data System (ADS)

    Uberna, Radoslaw; Amitay, Zohar; Qian, Charles X. W.; Leone, Stephen R.

    2001-06-01

    The significance of Rydberg states in the probing (via ionization) of Li2 wave packets has been studied through quantitative measurements of the relative coherent ionization cross sections in a two-color pump-probe femtosecond experiment. Following the preparation of a single intermediate rovibronic state with a cw laser, a femtosecond pump pulse (around 800 nm) creates a single two-state rotational wave packet by coherent excitation of the E1Σg+ (ν=9; J=27 and 29) states. The wave packet is then probed through ionization using time-delayed, wavelength tunable pulses (in the region 508-690 nm) while the total energy of the system is kept below the dissociation limit of Li2+. The background-free coherent ionization yield (for each probe wavelength) is measured as the relative oscillation amplitude of the single quantum beat time-dependent signal. The experimental results closely follow a relatively simple theoretical model, which is based on the assumption that the coherent ionization predominantly takes place via the excitation of high-n bound singly excited Rydberg states in the ionization continuum converging to the X 2Σg+ ground electronic state of Li2+. The best interpretation is that the high-n Rydberg states (above n˜25) undergo collisional ionization or autoionization and contribute to the measured coherent ionization signal, while the low-n Rydberg states undergo predissociation and do not contribute to the measured signal. An implication of the results is that the final states of the Li2 system, accessed by the above probe pulses, can be better approximated by a corresponding set of isolated discrete levels rather than by a continuum. This conclusion is important to experimental, as well as theoretical, coherent control and wave packet dynamics studies, in particular, when phase- and amplitude-shaped pump and probe pulses are employed. This study is also the first to investigate ionization of lithium dimer slightly below the E 1Σg+ shelf region with

  12. Quantification of Entanglement Entropies for Doubly Excited States in Helium

    NASA Astrophysics Data System (ADS)

    Lin, Chien-Hao; Ho, Yew Kam

    2015-05-01

    In this work, we study the quantum entanglement for doubly excited resonance states in helium by using highly correlated Hylleraas type functions to represent such states of the two-electron system. The doubly-excited resonance states are determined by calculation of density of resonance states under the framework of the stabilization method. The spatial (electron-electron orbital) entanglement measures for the low-lying doubly excited 2 s 2, 2 s3 s, and 2 p 2 1 S e states are carried out. Once a resonance state wave function is obtained, the linear entropy and von Neumann entropy for such a state are quantified using the Schmidt-Slater decomposition method. To check the consistence, linear entropy is also determined by solving analytically the needed four-electron (12-dimensional) integrals.

  13. Quadratic Zeeman effect in hydrogen Rydberg states: Rigorous error estimates for energy eigenvalues, energy eigenfunctions, and oscillator strengths

    SciTech Connect

    Falsaperla, P.; Fonte, G. Istituto Nazionale di Fisica Nucleare, Sezione di Catania, Corso Italia 57, I-95129 Catania )

    1994-10-01

    A variational method, based on some results due to T. Kato [Proc. Phys. Soc. Jpn. 4, 334 (1949)], and previously discussed is here applied to the hydrogen atom in uniform magnetic fields of tesla in order to calculate, with a rigorous error estimate, energy eigenvalues, energy eigenfunctions, and oscillator strengths relative to Rydberg states up to just below the field-free ionization threshold. Making use of a basis (parabolic Sturmian basis) with a size varying from 990 up to 5050, we obtain, over the energy range of [minus]190 to [minus]24 cm[sup [minus]1], all of the eigenvalues and a good part of the oscillator strengths with a remarkable accuracy. This, however, decreases with increasing excitation energy and, thus, above [similar to][minus]24 cm[sup [minus]1], we obtain results of good accuracy only for eigenvalues ranging up to [similar to][minus]12 cm[sup [minus]1].

  14. Large numbers of cold positronium atoms created in laser-selected Rydberg states using resonant charge exchange

    NASA Astrophysics Data System (ADS)

    McConnell, R.; Gabrielse, G.; Kolthammer, W. S.; Richerme, P.; Müllers, A.; Walz, J.; Grzonka, D.; Zielinski, M.; Fitzakerley, D.; George, M. C.; Hessels, E. A.; Storry, C. H.; Weel, M.; ATRAP Collaboration

    2016-03-01

    Lasers are used to control the production of highly excited positronium atoms (Ps*). The laser light excites Cs atoms to Rydberg states that have a large cross section for resonant charge-exchange collisions with cold trapped positrons. For each trial with 30 million trapped positrons, more than 700 000 of the created Ps* have trajectories near the axis of the apparatus, and are detected using Stark ionization. This number of Ps* is 500 times higher than realized in an earlier proof-of-principle demonstration (2004 Phys. Lett. B 597 257). A second charge exchange of these near-axis Ps* with trapped antiprotons could be used to produce cold antihydrogen, and this antihydrogen production is expected to be increased by a similar factor.

  15. Rydberg atoms in ultracold plasmas

    NASA Astrophysics Data System (ADS)

    Rolston, Steven

    2009-05-01

    Ultracold plasmas are formed through the photoionization of laser-cooled atoms, or spontaneous ionization of a dense cloud of Rydberg atoms or now molecules[1]. Ultracold plasmas are inherently metastable, as the ions and electrons would be in a lower energy state bound together as atoms. The dominant process of atom formation in these plasmas is three-body recombination, a collision between two electrons and an ion that leads to the formation of a Rydberg atom. This collisional process is not only important in determining the lifetime and density of the plasma, but is also critical in determining the time evolution of the temperature. The formation of the Rydberg atoms is accompanied by an increase in electron energy for the extra electron in the collision, and is a source of heating in these plasmas. Classical three-body recombination theory scales as T-9/2, and thus as a plasma cools due to a process such as adiabatic expansion, recombination-induced heating turns on, limiting the temperature [2]. The Rydberg atoms formed live in the plasma and contribute to the temperature dynamics, as collisions with plasma electrons can change the principal quantum number of the Rydberg atom, driving it to more tightly bound states (a source of plasma heating) or to higher states (a source of plasma cooling). If the plasma is cold and dense enough to be strongly coupled, classical three-body recombination theory breaks down. Recent theoretical work [3] suggests that the rate limits as the plasma gets strongly coupled. I will review the role of Rydberg atoms in ultracold plasmas and prospects for probing Rydberg collisions in the strongly coupled environment. [4pt] [1] J. P. Morrison, et al., Phys. Rev. Lett. 101, 205005 (2008 [0pt] [2] R. S. Fletcher, X. Zhang, and S. L. Rolston, Phys. Rev. Lett. 99, 145001 (2007 [0pt] [3] T. Pohl, private communication.

  16. An Experimental Apparatus for Studying Rydberg-Rydberg Interactions in Quantum Degenerate Gases of Strontium

    NASA Astrophysics Data System (ADS)

    Camargo, Francisco; Ding, Roger; Aman, James; Zhang, Xinyue; Whalen, Joseph; Fields, Robert; Dunning, F. Barry; Killian, Thomas

    2014-05-01

    We discuss the design and construction of a new apparatus for creating and studying long-range interactions in ultracold gases of strontium by exploiting Rydberg states, either through their direct excitation or through laser-induced Rydberg dressing. Strontium features one fermionic (87Sr) and three bosonic (84Sr, 86Sr, 88Sr) isotopes, all of which have been brought to quantum degeneracy. It also possesses singlet and triplet Rydberg states that furnish a wide variety of attractive and repulsive interactions. Furthermore, strontium Rydberg atoms feature an optically active core electron which can be used to manipulate and detect Rydberg atoms. These features make strontium a promising system for studying interactions in ultracold Rydberg gases. Research supported by Rice University, the NSF, the AFOSR, Shell, and the Robert A. Welch Foundation.

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

    NASA Astrophysics Data System (ADS)

    Limão-Vieira, P.; Duflot, D.; Ferreira da Silva, F.; Lange, E.; Jones, N. C.; Hoffmann, S. V.; Śmiałek, M. A.; Jones, D. B.; Brunger, M. J.

    2016-07-01

    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∗(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).

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

    PubMed

    Limão-Vieira, P; Duflot, D; Ferreira da Silva, F; Lange, E; Jones, N C; Hoffmann, S V; Śmiałek, M A; Jones, D B; Brunger, M J

    2016-07-21

    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(∗)(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). PMID:27448882

  19. Measurement of absolute transition frequencies of {sup 87}Rb to nS and nD Rydberg states by means of electromagnetically induced transparency

    SciTech Connect

    Mack, Markus; Karlewski, Florian; Hattermann, Helge; Hoeckh, Simone; Jessen, Florian; Cano, Daniel; Fortagh, Jozsef

    2011-05-15

    We report the measurement of absolute excitation frequencies of {sup 87}Rb to nS and nD Rydberg states. The Rydberg transition frequencies are obtained by observing electromagnetically induced transparency on a rubidium vapor cell. The accuracy of the measurement of each state is < or approx. 1 MHz, which is achieved by frequency stabilizing the two diode lasers employed for the spectroscopy to a frequency comb and a frequency comb calibrated wavelength meter, respectively. Based on the spectroscopic data we determine the quantum defects of {sup 87}Rb, and compare it with previous measurements on {sup 85}Rb. We determine the ionization frequency from the 5S{sub 1/2}(F=1) ground state of {sup 87}Rb to 1010.029 164 6(3)THz, providing the binding energy of the ground state with an accuracy improved by two orders of magnitude.

  20. Influence of inelastic Rydberg atom-atom collisional process on kinetic and optical properties of low-temperature laboratory and astrophysical plasmas

    NASA Astrophysics Data System (ADS)

    Klyucharev, A. N.; Bezuglov, N. N.; Mihajlov, A. A.; Ignjatović, Lj M.

    2010-11-01

    Elementary processes in plasma phenomena traditionally attract physicist's attention. The channel of charged-particle formation in Rydberg atom-atom thermal and sub-thermal collisions (the low temperature plasmas conditions) leads to creation of the molecular ions - associative ionization (AI). atomic ions - Penning-like ionization (PI) and the pair of the negative and positive ions. In our universe the chemical composition of the primordial gas consists mainly of Hydrogen and Helium (H, H-, H+, H2, He,He+). Hydrogen-like alkali-metal Lithium (Li, Li+,Li-) and combinations (HeH+, LiH-, LiH+). There is a wide range of plasma parameters in which the Rydberg atoms of the elements mentioned above make the dominant contribution to ionization and that process may be regarded as a prototype of the elementary process of light excitation energy transformation into electric one. The latest stochastic version of chemi-ionisation (AI+PI) on Rydberg atom-atom collisions extends the treatment of the "dipole resonant" model by taking into account redistribution of population over a range of Rydberg states prior to ionization. This redistribution is modelled as diffusion within the frame of stochastic dynamic of the Rydberg electron in the Rydberg energy spectrum. This may lead to anomalies of Rydberg atom spectra. Another result obtained in recent time is understanding that experimental results on chemi-ionization relate to the group of mixed Rydberg atom closed to the primary selected one. The Rydberg atoms ionisation theory today makes a valuable contribution in the deterministic and stochastic approaches correlation in atomic physic.

  1. Large energy superpositions via Rydberg dressing

    NASA Astrophysics Data System (ADS)

    Khazali, Mohammadsadegh; Lau, Hon Wai; Humeniuk, Adam; Simon, Christoph

    2016-08-01

    We propose to create superposition states of over 100 strontium atoms in a ground state or metastable optical clock state using the Kerr-type interaction due to Rydberg state dressing in an optical lattice. The two components of the superposition can differ by an order of 300 eV in energy, allowing tests of energy decoherence models with greatly improved sensitivity. We take into account the effects of higher-order nonlinearities, spatial inhomogeneity of the interaction, decay from the Rydberg state, collective many-body decoherence, atomic motion, molecular formation, and diminishing Rydberg level separation for increasing principal number.

  2. Retardation (Casimir) effect for a multielectron core system and a Rydberg electron

    NASA Astrophysics Data System (ADS)

    Babb, James F.; Spruch, Larry

    1989-09-01

    Theoretical predictions for the expected Casimir or retardation energy shift ΔEret(n,l) arising from retarded two-photon exchange in a Rydberg helium atom or in Rydberg low-Z heliumlike ions have been available for some time; n and l pertain to the Rydberg electron. These systems consist of a one-electron core [nucleus and 1s electron (e-)] and a Rydberg e-. Recent experiments on the n=10 states of singly excited helium have given a weak confirmation for the presence of Casimir shifts ΔEret(n,l). High-precision confirmation is likely to come from measurements on helium, as experiments improve. Nevertheless, though probably not suitable for high-precision confirmation, a retardation effect could be very large for a system with a many-e- core, and it might then be important to be able to at least estimate that effect. It is shown that the same formalism that was previously developed for the evaluation of ΔEret(n,l) for a one-electron (He-like) core can often be used for the many-electron core. In particular, with the core property characterized by a function F(k) (where k is the wave number of a virtual photon) related to the electric dipole polarizability, if the multi-e- core is in an S state, we obtain essentially the same result as for helium; formally, one need merely replace the F(k) of He+ by the F(k) of the ion under consideration. The extension described is largely notational. Furthermore, we show that as long as the core electrons have a spherically symmetric charge density, for a given core state or for an average over a set of core states which differ only in their angular momentum projections, the result for ΔEret(n,l) is very similar to the heliumlike result. Thus, we give several methods to estimate core properties and ΔEret(n,l) for a variety of systems and use these methods to obtain rough estimates of ΔEret(n,l) for some representative Rydberg levels of Li and Na. We note that storage rings may soon make possible high-precision experiments to

  3. Efficient Multiparticle Entanglement via Asymmetric Rydberg Blockade

    SciTech Connect

    Saffman, M.; Moelmer, K.

    2009-06-19

    We present an efficient method for producing N particle entangled states using Rydberg blockade interactions. Optical excitation of Rydberg states that interact weakly, yet have a strong coupling to a second control state is used to achieve state dependent qubit rotations in small ensembles. On the basis of quantitative calculations, we predict that an entangled quantum superposition state of eight atoms can be produced with a fidelity of 84% in cold Rb atoms.

  4. Evidence for strong van der Waals type Rydberg-Rydberg interaction in a thermal vapor.

    PubMed

    Baluktsian, T; Huber, B; Löw, R; Pfau, T

    2013-03-22

    We present evidence for Rydberg-Rydberg interaction in a gas of rubidium atoms above room temperature. Rabi oscillations on the nanosecond time scale to different Rydberg states are investigated in a vapor cell experiment. Analyzing the atomic time evolution and comparing to a dephasing model, we find a scaling with the Rydberg quantum number n that is consistent with van der Waals interaction. Our results show that the interaction strength can be larger than the kinetic energy scale (Doppler width), which is the requirement for realization of thermal quantum devices in the GHz regime. PMID:25166800

  5. The Helium Field Effect Transistor (I): Storing Surface State Electrons on Helium Films

    NASA Astrophysics Data System (ADS)

    Ashari, M.; Rees, D. G.; Kono, K.; Scheer, E.; Leiderer, P.

    2012-04-01

    We present investigations of surface state electrons on liquid helium films in confined geometry, using a suitable substrate structure microfabricated on a silicon wafer, similar to a Field Effect Transistor (FET). The sample has a source and drain region, separated by a gate structure, which consists of two gold electrodes with a narrow gap (channel) through which the transport of the surface state electrons takes place. The sample is illuminated to provide a sufficient number of free carriers in the silicon substrate, such that a well-defined potential distribution is achieved. The eventual goal of these experiments is to study the electron transport through a narrow channel in the various states of the phase diagram of the 2D electron system. In the present work we focus on storing the electrons in the source area of the FET, and investigate the spatial distribution of these electrons. It is shown that under the influence of a potential gradient in the silicon substrate the electrons accumulate in front of the potential barrier of the gate. The electron distribution, governed by Coulomb repulsion and by the substrate potential, is determined experimentally. The result is found to be in good agreement with a parallel-plate capacitor model of the system, developed with the aid of a finite element calculation of the surface potential profile of the device.

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

    SciTech Connect

    Gilchrist, A. J.; Ritchie, G. A. D.

    2013-06-07

    (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.

  7. High-lying bound Rydberg states of excited Hg(6s6p {sup 3}P{sub 1}) atoms from two-color resonance ionization mass spectroscopy

    SciTech Connect

    Bisling, Peter; Dederichs, Jan; Neidhart, Bernd; Weitkamp, Claus

    1998-12-16

    Mercury isotopes are investigated with two-color resonance ionization mass spectroscopy (RIMS). Isotope shifts, hyperfine structure splittings, and the lifetime of the intermediate 6s6p {sup 3}P{sub 1} state are determined by RIMS. Ion yields at the threshold region in various static electric fields are measured in order to determine an extrapolated ionization energy value at zero field strength. New energy values for high-lying bound 6s nd {sup 3}D (21Rydberg states of Hg isotopes are found under field-free conditions and with delayed, pulsed electric field ionization. To the author's knowledge this is the first time that isotopic effects on the ionization energy are deduced from the convergence limit of the Rydberg series.

  8. Rydberg polaritons in a thermal vapor

    NASA Astrophysics Data System (ADS)

    Ripka, Fabian; Chen, Yi-Hsin; Löw, Robert; Pfau, Tilman

    2016-05-01

    We present a pulsed four-wave mixing scheme via a Rydberg state to create, store, and retrieve collective Rydberg polaritons. The storage medium consists of a gas of thermal Rb atoms confined in a 220 -μ m -thick cell, which is heated above room temperature. The experimental sequence consists of a pulsed excitation of Rydberg polaritons via the D1 line, a variable delay or storage time, and a final retrieval pulse via the D2 line. The lifetime of the Rydberg polaritons is around 1.2 ns, almost entirely limited by the excitation bandwidth and the corresponding motional dephasing of the atoms. The presented scheme combined with a tightly confined atomic ensemble is a good candidate for a deterministic single-photon source, as soon as strong interactions in terms of a Rydberg blockade are added.

  9. Three-body physics of Rydberg polaritons

    NASA Astrophysics Data System (ADS)

    Wang, Yidan; Gorshkov, Alexey; Qi, Ran; Gullans, Michael; Maghrebi, Mohammad

    2016-05-01

    Under the conditions electromagnetically induced transparency in Rydberg media, slow-light polaritons interact strongly via Rydberg states. While two such polaritons can interact attractively and form two-body bound states, three polariton physics remains largely unexplored. We show that while exact three-polariton bound states do not exist, metastable ones do. The understanding of three-polariton physics will allow for the construction of more precise low energy many-body theories of Rydberg polaritons and may enable the realization of novel exotic equilibrium and out-of equilibrium phenomena with interacting light.

  10. Dynamics of the Rydberg state population of slow highly charged ions impinging a solid surface at arbitrary collision geometry

    NASA Astrophysics Data System (ADS)

    Nedeljković, N. N.; Majkić, M. D.; Božanić, D. K.; Dojčilović, R. J.

    2016-06-01

    We consider the population dynamics of the intermediate Rydberg states of highly charged ions (core charge Z\\gg 1, principal quantum number {n}{{A}}\\gg 1) interacting with solid surfaces at arbitrary collision geometry. The recently developed resonant two-state vector model for the grazing incidence (2012 J. Phys. B: At. Mol. Opt. Phys. 45 215202) is extended to the quasi-resonant case and arbitrary angle of incidence. According to the model, the population probabilities depend both on the projectile parallel and perpendicular velocity components, in a complementary way. A cascade neutralization process for {{{Xe}}}Z+ ions, for Z=15{--}45, interacting with a conductive-surface is considered by taking into account the population dynamics. For an arbitrary collision geometry and given range of ionic velocities, a micro-staircase model for the simultaneous calculation of the kinetic energy gain and the charge state of the ion in front of the surface is proposed. The relevance of the obtained results for the explanation of the formation of nanostructures on solid surfaces by slow highly charged ions for normal incidence geometry is briefly discussed.

  11. Rydberg excitation assisted light shift blockade in Rb atoms for realizing a collective state quantum bit and quantum memory

    NASA Astrophysics Data System (ADS)

    Tu, Yanfei; Kim, May E.; Shahriar, Selim M.

    2014-10-01

    Previously, we had proposed the technique of light shift imbalance induced blockade which leads to a condition where a collection of non-interacting atoms under laser excitation remains combined to a superposition of the ground and the fist excited states, thus realizing a collective state quantum bit which in turn can be used to realize a quantum computer. In this paper, we show first that the light shift imbalance by itself is actually not enough to produce such a blockade, and explain the reason by the limitation of our previous analysis had reached this constraint. We then show that by introducing Rydberg interaction, it is possible to achieve such a blockade for a wide range of parameters. Analytic arguments used to establish these results are confirmed by numerical simulations. The fidelity of coupled quantum gates based on such collective state qubits is highly insensitive to the exact number of atoms in the ensemble. As such, this approach may prove be viable for scalable quantum computing based on neutral atoms.

  12. Observation of Rydberg blockade effects at very high n, n ~ 300 , using strontium n1F3 states

    NASA Astrophysics Data System (ADS)

    Zhang, Xinyue; Dunning, F. B.; Yoshida, Shuhei; Burgdörfer, Joachim

    2015-05-01

    Rydberg blockade at very high n, n ~ 300 , is examined using strontium n1F3 Rydberg atoms excited in a small volume defined by two tightly-focused crossed laser beams. Measurements of the number distribution of Rydberg atoms created show deviations from a Poisson distribution revealing sizeable blockade effects. The statistics of the number distribution are studied using a Monte Carlo method in which the interaction between strontium Rydberg atoms is evaluated by solving the Schrödinger equation within a two-active-electron model. The strength of blockade is analyzed in detail with respect to the alignment of two atoms relative to the laser polarizations. With careful control of the experimental parameters the probability for creating one, and only one, Rydberg atom, P(1) , in the excitation volume can be sufficiently large, P(1) > 0 . 6 , as to enable detailed studies of strongly-coupled Rydberg atom pairs. Research supported by the NSF, the Robert A. Welch Foundation, and the FWF (Austria).

  13. Diagrams of the state of a steady-state arc discharge in hydrogen and helium

    NASA Astrophysics Data System (ADS)

    Vasil'ev, E. N.

    2014-12-01

    The temperature, electric field strength, and specific and integrated powers of energy mechanisms of an axisymmetric steady-state equilibrium arc discharge in hydrogen and helium under atmospheric pressure are calculated for various values of the current and radius. The results of calculations are presented in the form of state diagrams intended for estimating the main energy characteristics of electric arcs.

  14. Measurement of Rydberg positronium fluorescence lifetimes

    NASA Astrophysics Data System (ADS)

    Deller, A.; Alonso, A. M.; Cooper, B. S.; Hogan, S. D.; Cassidy, D. B.

    2016-06-01

    We report measurements of the fluorescence lifetimes of positronium (Ps) atoms with principal quantum numbers n =10 -19 . Ps atoms in Rydberg-Stark states were produced via a two-color two-step 1 3S→2 3P→n 3S/n Rydberg levels, yielding values ranging from 3 μ s to 26 μ s . Our data are in accord with the expected radiative lifetimes of Rydberg-Stark states of Ps.

  15. Phase Modulation in Rydberg Dressed Multi-Wave Mixing processes.

    PubMed

    Zhang, Zhaoyang; Zheng, Huaibin; Yao, Xin; Tian, Yaling; Che, Junling; Wang, Xiuxiu; Zhu, Dayu; Zhang, Yanpeng; Xiao, Min

    2015-01-01

    We study the enhancement and suppression of different multi-waving mixing (MWM) processes in a Rydberg-EIT rubidium vapor system both theoretically and experimentally. The nonlinear dispersion property of hot rubidium atoms is modulated by the Rydberg-Rydberg interaction, which can result in a nonlinear phase shift of the relative phase between dark and bright states. Such Rydberg-induced nonlinear phase shift can be quantitatively estimated by the lineshape asymmetry in the enhancedand suppressed MWM processes, which can also demonstrate the cooperative atom-light interaction caused by Rydberg blockaded regime. Current study on phase shift is applicable to phase-sensitive detection and the study of strong Rydberg-Rydberg interaction. PMID:26053438

  16. Phase Modulation in Rydberg Dressed Multi-Wave Mixing processes

    PubMed Central

    Zhang, Zhaoyang; Zheng, Huaibin; Yao, Xin; Tian, Yaling; Che, Junling; Wang, Xiuxiu; Zhu, Dayu; Zhang, Yanpeng; Xiao, Min

    2015-01-01

    We study the enhancement and suppression of different multi-waving mixing (MWM) processes in a Rydberg-EIT rubidium vapor system both theoretically and experimentally. The nonlinear dispersion property of hot rubidium atoms is modulated by the Rydberg-Rydberg interaction, which can result in a nonlinear phase shift of the relative phase between dark and bright states. Such Rydberg-induced nonlinear phase shift can be quantitatively estimated by the lineshape asymmetry in the enhancedand suppressed MWM processes, which can also demonstrate the cooperative atom-light interaction caused by Rydberg blockaded regime. Current study on phase shift is applicable to phase-sensitive detection and the study of strong Rydberg-Rydberg interaction. PMID:26053438

  17. Rydberg state photochemistry of 1,4-diazabicyclo(2. 2. 2)octane excited by 193- and 248-nm lasers

    SciTech Connect

    Lin, C.T.

    1987-05-21

    Linear and nonlinear photochemistries of 1,4-diazabicyclo(2.2.2)octane (DABCO) are investigated at room temperature by using ArF (193 nm) and KrF (248 nm) lasers. With an unfocused beam geometry, DABCO vapor displays a strong fluorescence when excited at 248 nm, but it shows no detectable emission with 193-nm excitation. The linear photochemistry quantum yield for DABCO is determined as phi/sub p/(248nm) approx. 0.1 and phi/sub p/(193 nm) approx. 0.3. The main stable photochemical products are analyzed as C/sub 2/H/sub 4/ and C/sub 2/H/sub 2/ for 248- and 193-nm excitation, respectively. When focused beam excitation is used, both ArF and KrF lasers dissociate DABCO molecules and give three strong radical emissions of CN*(B vector /sup 2/..sigma.. ..-->.. X vector /sup 2/ ..sigma../sup +/), CH*(A vector /sup 2/..delta.. ..-->.. X vector /sup 2/II), and C/sub 2/*(D vector /sup 3/II/sub g/ ..-->.. a vector /sup 3/II/sub u/). The time behavior, the laser power dependence, and the sample pressure dependence of these emissive radicals are examined. The possible mechanisms for the Rydberg state photochemistry of DABCO are discussed.

  18. Stability of Surface State Electrons on Helium Films

    NASA Astrophysics Data System (ADS)

    Leiderer, P.; Scheer, E.; Kono, K.; Lin, J.-J.; Rees, D. G.

    2016-05-01

    Electrons on helium substrates form a model Coulomb system in which the transition from classical electron liquid to Wigner crystal is readily observed. However, attempts to increase the electron density in order to observe the `quantum melting' of the system to a Fermi degenerate gas are hindered by an instability of the helium surface. Here we describe experimental efforts to reach the degenerate regime on thin helium films and microstructured substrates, for which the surface instability is suppressed. We demonstrate that, although the electron densities obtained exceed those for bulk helium substrates, observation of quantum melting remains challenging. We discuss possible solutions to the technical challenges involved.

  19. Polarization control of absorption of virtual dressed states in helium

    NASA Astrophysics Data System (ADS)

    Reduzzi, Maurizio; Hummert, Johan; Dubrouil, Antoine; Calegari, Francesca; Nisoli, Mauro; Frassetto, Fabio; Poletto, Luca; Chen, Shaohao; Wu, Mengxi; Gaarde, Mette B.; Schafer, Kenneth; Sansone, Giuseppe

    2015-09-01

    The extreme ultraviolet absorption spectrum of an atom is strongly modified in the presence of a synchronized intense infrared field. In this work we demonstrate control of the absorption properties of helium atoms dressed by an infrared pulse by changing the relative polarization of the infrared and extreme ultraviolet fields. Light-induced features associated with the dressed 1 s 2 s , 1 s 3 s , and 1 s 3 d states, referred to as 2 s+ , 3 s± , and 3 d± light-induced states, are shown to be strongly modified or even eliminated when the relative polarization is rotated. The experimental results agree well with calculations based on the solution of the time-dependent Schrödinger equation using a restricted excitation model that allows efficient treatment of the three-dimensional problem. We also present an analysis of the light-induced states based on Floquet theory, which allows for a simple explanation of their properties. Our results open a new route to creating controllable superpositions of dipole allowed and nondipole allowed states in atoms and molecules.

  20. Rotationally resolved photoelectron spectra in resonance enhanced multiphoton ionization of HCl via the F 1Δ2 Rydberg state

    NASA Astrophysics Data System (ADS)

    Wang, Kwanghsi; McKoy, V.

    1991-12-01

    Results of studies of rotational ion distributions in the X 2Π3/2 and X 2Π1/2 spin-orbit states of HCl+ resulting from (2+1') resonance enhanced multiphoton ionization (REMPI) via the S(0) branch of the F 1Δ2 Rydberg state are reported and compared with measured threshold-field-ionization zero-kinetic-energy spectra reported recently [K. S. Haber, Y. Jiang, G. Bryant, H. Lefebvre-Brion, and E. R. Grant, Phys. Rev. A (in press)]. These results show comparable intensities for J+=3/2 of the X 2Π3/2 ion and J+=1/2 of the X 2Π1/2 ion. Both transitions require an angular momentum change of ΔN=-1 upon photoionization. To provide further insight into the near-threshold dynamics of this process, we also show rotationally resolved photoelectron angular distributions, alignment of the ion rotational levels, and rotational distributions for the parity components of the ion rotational levels. About 18% population is predicted to occur in the (+) parity component, which would arise from odd partial-wave contributions to the photoelectron matrix element. This behavior is similar to that in (2+1) REMPI via the S(2) branch of the F 1Δ2 state of HBr and was shown to arise from significant l mixing in the electronic continuum due to the nonspherical molecular ion potential. Rotational ion distributions resulting from (2+1) REMPI via the S(10) branch of the F 1Δ2 state are also shown.

  1. Ultracold Long-Range Rydberg Molecules with Complex Multichannel Spectra

    NASA Astrophysics Data System (ADS)

    Eiles, Matthew; Greene, Chris

    2016-05-01

    A generalized class of exotic long-range Rydberg molecules consisting of a multichannel Rydberg atom bound to a distant ground state atom by the Rydberg electron is predicted. These molecules are characterized by the rich physics provided by the strongly perturbed multichannel Rydberg spectra of divalent atoms, in contrast to the regular Rydberg series of the alkali atoms used to form Rydberg molecules to date. These multichannel Rydberg molecules exhibit favorable properties for laser excitation, because states exist where the quantum defect varies strongly with the principal quantum number n. In particular, the nd Rydberg state of calcium becomes nearly degenerate with states of high orbital angular momentum over the range 17 < n < 22 , promoting its admixture into the high l deeply bound ``trilobite'' molecule states and thereby circumventing the usual difficulty posed by electric dipole selection rules. Further novel molecular states are predicted to occur in the low- J states of silicon, which are strongly perturbed due to channel interactions between Rydberg series leading to the spin-orbit split ionization thresholds. These interactions manifest themselves in potential curves exhibiting two distinct length scales, providing novel opportunities for quantum manipulation. Supported in part by the National Science Foundation under Grant No. PHY-1306905.

  2. Quantum-classical lifetimes of Rydberg molecules

    NASA Astrophysics Data System (ADS)

    Junginger, Andrej; Main, Jörg; Wunner, Günter

    2013-04-01

    A remarkable property of Rydberg atoms is the possibility of creating molecules formed by one highly excited atom and another atom in the ground state. The first realization of such a Rydberg molecule has opened an active field of physical investigations, and showed that its basic properties can be described within a simple model regarding the ground state atom as a small perturber that is bound by a low-energy scattering process with the Rydberg electron (Greene et al 2000 Phys. Rev. Lett. 85 2458). Besides the good agreement between theory and the experiment concerning the vibrational states of the molecule, the experimental observations yield the astonishing feature that the lifetime of the molecule is clearly reduced as compared to the bare Rydberg atom (Butscher et al 2011 J. Phys. B: At. Mol. Opt. Phys. 44 184004). With focus on this yet unexplained observation, we investigate in this paper the vibrational ground state of the molecule in a quantum-classical framework. We show that the Rydberg wavefunction is continuously detuned by the presence of the moving ground state atom and that the timescale on which the detuning significantly exceeds the natural linewidth is in good agreement with the observed reduced lifetimes of the Rydberg molecule.

  3. Observations and analysis with the spline-based Rydberg-Klein-Rees approach for the 3(1)Σg(+) state of Rb2.

    PubMed

    Yang, Jinxin; Guan, Yafei; Zhao, Wei; Zhou, Zhaoyu; Han, Xiaomin; Ma, Jie; Sovkov, Vladimir B; Ivanov, Valery S; Ahmed, Ergin H; Lyyra, A Marjatta; Dai, Xingcan

    2016-01-14

    Ro-vibrational term values of the 3(1)Σg (+) state of (85,85)Rb2 and (85,87)Rb2 and resolved fluorescence spectra to the A(1)Σu (+) state are recorded following optical-optical double resonance excitation. The experimental data are heavily perturbed, and as a result, the standard analysis based on Dunham series representation of the energy levels fails. The analysis is done via modeling the adiabatic potential function with the Rydberg-Klein-Rees potential constructed from the generalized smoothing spline interpolation of the vibrational energies Gv and rotational constants Bv. PMID:26772572

  4. Determination of the binding energies of the np Rydberg states of H{sub 2}, HD, and D{sub 2} from high-resolution spectroscopic data by multichannel quantum-defect theory

    SciTech Connect

    Sprecher, Daniel; Merkt, Frédéric; Jungen, Christian

    2014-03-14

    Multichannel quantum-defect theory (MQDT) is used to calculate the electron binding energies of np Rydberg states of H{sub 2}, HD, and D{sub 2} around n = 60 at an accuracy of better than 0.5 MHz. The theory includes the effects of rovibronic channel interactions and the hyperfine structure, and has been extended to the calculation of the asymmetric hyperfine structure of Rydberg states of a heteronuclear diatomic molecule (HD). Starting values for the eigenquantum-defect parameters of MQDT were extracted from ab initio potential-energy functions for the low-lying p Rydberg states of molecular hydrogen and subsequently refined in a global weighted fit to available experimental data on the singlet and triplet Rydberg states of H{sub 2} and D{sub 2}. The electron binding energies of high-np Rydberg states derived in this work represent important quantities for future determinations of the adiabatic ionization energies of H{sub 2}, HD, and D{sub 2} at sub-MHz accuracy.

  5. Multiphoton Microwave Ionization of Rydberg Atoms

    NASA Astrophysics Data System (ADS)

    Gurian, Joshua Houston

    This thesis describes a series of multiphoton microwave experiments on Rydberg atoms when the microwave frequency is much greater than the classical Kepler frequency of the excited atoms. A new kHz pulse repetition frequency dye laser system was constructed for Rydberg lithium excitation with a linewidth as narrow as 3 GHz. This new laser system is used for first experiments of multiphoton microwave ionization of Rydberg lithium approaching the photoionization limit using 17 and 36 GHz microwave pulses. A multi-channel quantum defect model is presented that well describes the experimental results, indicating that these results are due to the coherent coupling of many atomic levels both above and below the classical ionization limit. Finally, preliminary results of measuring the final-state distributions of high lying Rydberg states after 17 GHz microwave pulses are presented.

  6. Electrostatically Guided Rydberg Positronium.

    PubMed

    Deller, A; Alonso, A M; Cooper, B S; Hogan, S D; Cassidy, D B

    2016-08-12

    We report experiments in which positronium (Ps) atoms were guided using inhomogeneous electric fields. Ps atoms in Rydberg-Stark states with principal quantum number n=10 and electric dipole moments up to 610 D were prepared via two-color two-photon optical excitation in the presence of a 670  V cm^{-1} electric field. The Ps atoms were created at the entrance of a 0.4 m long electrostatic quadrupole guide, and were detected at the end of the guide via annihilation gamma radiation. When the lasers were tuned to excite low-field-seeking Stark states, a fivefold increase in the number of atoms reaching the end of the guide was observed, whereas no signal was detected when high-field-seeking states were produced. The data are consistent with the calculated geometrical guide acceptance. PMID:27563960

  7. Electrostatically Guided Rydberg Positronium

    NASA Astrophysics Data System (ADS)

    Deller, A.; Alonso, A. M.; Cooper, B. S.; Hogan, S. D.; Cassidy, D. B.

    2016-08-01

    We report experiments in which positronium (Ps) atoms were guided using inhomogeneous electric fields. Ps atoms in Rydberg-Stark states with principal quantum number n =10 and electric dipole moments up to 610 D were prepared via two-color two-photon optical excitation in the presence of a 670 V cm-1 electric field. The Ps atoms were created at the entrance of a 0.4 m long electrostatic quadrupole guide, and were detected at the end of the guide via annihilation gamma radiation. When the lasers were tuned to excite low-field-seeking Stark states, a fivefold increase in the number of atoms reaching the end of the guide was observed, whereas no signal was detected when high-field-seeking states were produced. The data are consistent with the calculated geometrical guide acceptance.

  8. Bond angle variations in XH3 [X = N, P, As, Sb, Bi]: the critical role of Rydberg orbitals exposed using a diabatic state model.

    PubMed

    Reimers, Jeffrey R; McKemmish, Laura K; McKenzie, Ross H; Hush, Noel S

    2015-10-14

    Ammonia adopts sp(3) hybridization (HNH bond angle 108°) whereas the other members of the XH3 series PH3, AsH3, SbH3, and BiH3 instead prefer octahedral bond angles of 90-93°. We use a recently developed general diabatic description for closed-shell chemical reactions, expanded to include Rydberg states, to understand the geometry, spectroscopy and inversion reaction profile of these molecules, fitting its parameters to results from Equation of Motion Coupled-Cluster Singles and Doubles (EOM-CCSD) calculations using large basis sets. Bands observed in the one-photon absorption spectrum of NH3 at 18.3 eV, 30 eV, and 33 eV are reassigned from Rydberg (formally forbidden) double excitations to valence single-excitation resonances. Critical to the analysis is the inclusion of all three electronic states in which two electrons are placed in the lone-pair orbital n and/or the symmetric valence σ* antibonding orbital. An illustrative effective two-state diabatic model is also developed containing just three parameters: the resonance energy driving the high-symmetry planar structure, the reorganization energy opposing it, and HXH bond angle in the absence of resonance. The diabatic orbitals are identified as sp hybrids on X; for the radical cations XH3(+) for which only 2 electronic states and one conical intersection are involved, the principle of orbital following dictates that the bond angle in the absence of resonance is acos(-1/5) = 101.5°. The multiple states and associated multiple conical intersection seams controlling the ground-state structure of XH3 renormalize this to acos[3 sin(2)(2(1/2)atan(1/2))/2 - 1/2] = 86.7°. Depending on the ratio of the resonance energy to the reorganization energy, equilibrium angles can vary from these limiting values up to 120°, and the anomalously large bond angle in NH3 arises because the resonance energy is unexpectedly large. This occurs as the ordering of the lowest Rydberg orbital and the σ* orbital swap, allowing

  9. Millimeter-wave spectroscopy and multichannel quantum-defect-theory analysis of high Rydberg states of xenon: The hyperfine structure of {sup 129}Xe{sup +} and {sup 131}Xe{sup +}

    SciTech Connect

    Schaefer, Martin; Raunhardt, Matthias; Merkt, Frederic

    2010-03-15

    Millimeter-wave transitions between high-n Rydberg states of several isotopes of xenon have been recorded at sub-megahertz resolution. The fine and, for {sup 129}Xe and {sup 131}Xe, hyperfine structures of s, p, d, and f Rydberg states with principal quantum number in the range 52{<=}n{<=}64 have been determined from combination differences and analyzed using multichannel quantum defect theory. Improved eigenquantum defects and channel interaction parameters for the odd- and even-parity Rydberg states of xenon and the hyperfine structure of the {sup 2}P{sub 3/2} ground state of {sup 129}Xe{sup +} and {sup 131}Xe{sup +} have been obtained. Nearly degenerate p and d fine or hyperfine levels are very easily mixed by even weak stray electric fields.

  10. Ground-state energetics of helium and deuterium fermion fluids

    NASA Astrophysics Data System (ADS)

    Krotscheck, E.; Smith, R. A.; Clark, J. W.; Panoff, R. M.

    1981-12-01

    description of the ground-state energetics of liquid 3He. Bulk atomic deuterium with all electronic spins aligned is treated at the same level of approximation as applied to helium. Three choices of nuclear-spin distribution are examined, with a single spin state present, or two or three equally populated nuclear spin states. The finite-density energy minimum is found to lie very close to zero energy in all three examples; a very precise many-body calculation will thus be needed to decide their liquid or gaseous nature at zero temperature under zero external pressure.

  11. Spectrum, radial wave functions, and hyperfine splittings of the Rydberg states in heavy alkali-metal atoms

    NASA Astrophysics Data System (ADS)

    Sanayei, Ali; Schopohl, Nils

    2016-07-01

    We present numerically accurate calculations of the bound-state spectrum of the highly excited valence electron in the heavy alkali-metal atoms solving the radial Schrödinger eigenvalue problem with a modern spectral collocation method that applies also for a large principal quantum number n ≫1 . As an effective single-particle potential we favor the reputable potential of Marinescu et al. [Phys. Rev. A 49, 982 (1994)], 10.1103/PhysRevA.49.982. Recent quasiclassical calculations of the quantum defect of the valence electron agree for orbital angular momentum l =0 ,1 ,2 ,... overall remarkably well with the results of the numerical calculations, but for the Rydberg states of rubidium and also cesium with l =3 this agreement is less fair. The reason for this anomaly is that in rubidium and cesium the potential acquires for l =3 deep inside the ionic core a second classical region, thus invalidating a standard Wentzel-Kramers-Brillouin (WKB) calculation with two widely spaced turning points. Comparing then our numerical solutions of the radial Schrödinger eigenvalue problem with the uniform analytic WKB approximation of Langer constructed around the remote turning point rn,j ,l (" close=")n -δ0)">+ we observe everywhere a remarkable agreement, apart from a tiny region around the inner turning point rn,j ,l (-). For s states the centrifugal barrier is absent and no inner turning point exists: rn,j ,0 (-)=0 . With the help of an ansatz proposed by Fock we obtain for the s states a second uniform analytic approximation to the radial wave function complementary to the WKB approximation of Langer, which is exact for r →0+ . From the patching condition, that is, for l =0 the Langer and Fock solutions should agree in the intermediate region 0

  12. Double-resonance spectroscopy of the high Rydberg states of HCO. III. Multiple pathways in the vibrational autoionization of the bending overtone

    NASA Astrophysics Data System (ADS)

    Mayer, Eric E.; Hedderich, Hartmut G.; Grant, Edward R.

    1998-05-01

    Ultraviolet first-photon absorption selects individual rotational levels in the Renner-Teller split (020) vibronic band system in the 3pπ 2Π Rydberg state of HCO. These gateway states serve as originating levels for vertical second-photon transitions to vibrationally autoionizing Rydberg series converging to individual rotational levels associated with the (0200) and (0220) states of HCO+. Linewidths of assigned series convey information on autoionization dynamics. Resonances throughout the (020) autoionization spectrum match sharp profiles seen earlier for series converging to HCO+(010). Linewidths for autoionization via relaxation both of the bending fundamental and its overtone are measurably narrower than resonances built on CO stretch, (001), which indicates that mode-selectivity inhibiting bending autoionization relative to stretch extends to the bending overtone. Features in the (020) spectrum that fall below the threshold energy for decay by autoionization to the (010) continuum appear with diminished intensity and yet narrower linewidth. This provides evidence that vibrational autoionization in HCO conforms with a Δv=1 propensity rule that favors relaxation of (020) states to the (010) continuum over the two-quantum decay to produce HCO+(000). Analysis of detailed line shapes and intensities associated with individual vibrational angular momentum components of the relaxing-core overtone point to the way in which vibrational and orbital-electronic symmetries factor in the bound molecule and cation plus free electron, and fix the order in vibrational coordinates of necessary coupling terms.

  13. Spin-dependent localized Hartree-Fock density-functional calculation of singly, doubly, and triply excited and Rydberg states of He- and Li-like ions

    SciTech Connect

    Zhou Zhongyuan; Chu, Shih-I

    2005-02-01

    A spin-dependent density-functional approach for the calculation of highly and multiply excited state of atomic system is proposed based on the localized Hartree-Fock density-functional method and Slater's diagonal sum rule. In this approach, electron spin orbitals in an electronic configuration are obtained first by solving the Kohn-Sham equation with an exact nonvariational spin-dependent localized Hartree-Fock exchange potential. Then a single-Slater-determinant energy of the electronic configuration is calculated by using these electron spin orbitals. Finally, a multiplet energy of an excited state is evaluated from the single-Slater-determinant energies of the electronic configurations involved in terms of Slater's diagonal sum rule. This approach has been applied to the calculation of singly, doubly, and especially triply excited Rydberg states of He- and Li-like ions. The total energies obtained from the calculation with an exchange-only (X-only) potential are surprisingly close to those of Hartree-Fock method and the total energies from the calculation with exchange-correlation potential are in overall agreement with available theoretical and experimental data. The presented procedure provides a simple and computationally efficient scheme for the accurate calculation of highly and multiply excited Rydberg states of an atomic system within density-functional theory.

  14. Experimental study of bound and autoionizing Rydberg states of the europium atom

    NASA Astrophysics Data System (ADS)

    Xiao, Ying; Dai, Chang-Jian; Qin, Wen-Jie

    2010-06-01

    An isolated-core-excitation (ICE) scheme and stepwise excitation are employed to study the highly excited states of the europium atom. The bound europium spectrum with odd parity in a region of 42400-43500 cm-1 is measured, from which spectral information on 38 transitions, such as level position and relative intensity, can be deduced. Combined with information about excitation calibration and the error estimation process, the selection rules enable us to determine the possible values of total angular momentum J for the observed states. The autoionization spectra of atomic europium, belonging to the 4f76pnl (l = 0, 2) configurations, are systematically investigated by using the three-step laser resonance ionization spectroscopy (RIS) approach. With the ICE scheme, all the experimental spectra of the autoionizing states have nearly symmetric profiles whose peak positions and widths can be easily obtained. A comparison between our results and those from the relevant literature shows that our work not only confirms many reported states, but also discovers 14 bound states and 16 autoionizing states.

  15. Optical Mixing of Rydberg Angular Momenta

    SciTech Connect

    Corless, J.D.; Stroud, C.R., Jr.

    1997-07-01

    When optical frequency fields are used to couple a ground state to a Rydberg state, the resonant dipole coupling is to a low angular momentum state. Higher angular momentum states are typically thought not to play a role in the excitation. The extremely large dipole matrix elements coupling Rydberg states of the same n but differing l , however, allow optical fields of modest strengths to produce Rabi frequencies larger than optical frequencies. We demonstrate that these optical fields can therefore readily excite the higher angular momentum states, and we examine the consequences of this coupling. {copyright} {ital 1997} {ital The American Physical Society}

  16. Ultralong-range triatomic Rydberg molecules in an electric field

    NASA Astrophysics Data System (ADS)

    Aguilera Fernández, Javier; Schmelcher, Peter; González-Férez, Rosario

    2016-06-01

    We investigate the electronic structure of a triatomic Rydberg molecule formed by a Rydberg atom and two neutral ground-state atoms. Taking into account the s-wave and p-wave interactions, we perform electronic structure calculations and analyze the adiabatic electronic potentials evolving from the Rb (n=35,l≥slant 3) Rydberg degenerate manifold. We hereby focus on three different classes of geometries of the Rydberg molecules, including symmetric, asymmetric and planar configurations. The metamorphosis of these potential energy surfaces in the presence of an external electric field is explored.

  17. Heavy-Rydberg ion-pair formation in collisions of Rydberg atoms with attaching targets

    NASA Astrophysics Data System (ADS)

    Wang, Changhao; Kelley, Michael; Dunning, F. Barry

    2012-06-01

    Collisions between K(np) Rydberg atoms and electron attaching targets can lead to the creation of heavy-Rydberg ion-pair states comprising a weakly-bound positive-negative ion pair orbiting at large internuclear separations. The lifetimes of such states and their correlation with binding energy and the channels available for decay, which can be controlled by varying n, the Rydberg atom velocity, and the target species, are being investigated. The ion-pair states are produced in a small collision cell and allowed to exit to form a beam that passes between a pair of electrodes where their number and binding energy distribution is determined by electric field induced dissociation. Ion-pair production is analyzed with the aid of a Monte Carlo collision code that models both initial Rydberg electron capture and the subsequent evolution of the product ion pair. Research supported by the Robert A Welch Foundation.

  18. Progress towards deterministic generation of entangled W-states of neutral atoms using Rydberg blockade

    NASA Astrophysics Data System (ADS)

    Gill, Alexander T.

    Every day, millions of cubic feet of natural gas is transported through interstate pipelines and consumed by customers all over the United States of America. Gas distributors, responsible for sending natural gas to individual customers, are eager for an estimate of how much natural gas will be used in the near future. GasHour(TM) software, a reliable forecasting tool from the Marquette University GasDay(TM) lab, has been providing highly accurate hourly forecasts over the past few years. Our goal is to improve current GasHour forecasts, and my thesis presents an approach to achieve that using a blending technique. This thesis includes detailed explanations of the multi-horizon forecasting technique employed by GasHour models. Several graphs are displayed to reveal the structure of hourly forecasts from GasHour. We present SMHF (Smoothing Multi-horizon Forecasts), a step-by-step method showing how a polynomial smoothing technique is applied to current GasHour predications. A slightly different approach of smoothing has also been introduced. We compare RMSEs of both GasHour forecasts and smoothed ones. Different comparisons resulting from different situations have been demonstrated as well. Several conclusions have been reached. Based on the results, blending techniques can improve current GasHour forecasts. We look forward to applying this blending technique to other fields of forecasting.

  19. Trapping Rydberg Atoms in an Optical Lattice

    NASA Astrophysics Data System (ADS)

    Anderson, Sarah E.

    2012-06-01

    Optical lattice traps for Rydberg atoms are of interest in advanced science and in practical applications. After a brief discussion of these areas of interest, I will review some basics of optical Rydberg-atom trapping. The trapping potential experienced by a Rydberg atom in an optical lattice is given by the spatial average of the free-electron ponderomotive energy weighted by the Rydberg electron's probability distribution. I will then present experimental results on the trapping of ^85Rb Rydberg atoms in a one-dimensional ponderomotive optical lattice (wavelength 1064 nm). The principal methods employed to study the lattice performance are microwave spectroscopy, which is used to measure the lattice's trapping efficiency, and photo-ionization, which is used to measure the dwell time of the atoms in the lattice. I have achieved a 90% trapping efficiency for ^85Rb 50S atoms by inverting the lattice immediately after laser excitation of ground-state atoms into Rydberg states. I have characterized the dwell time of the atoms in the lattice using photo-ionization of 50D5/2 atoms. In continued work, I have explored the dependence of the Rydberg-atom trapping potential on the angular portion of the atomic wavefunction. Distinct angular states exhibit different trapping behavior in the optical lattice, depending on how their wavefunctions are oriented relative to the lattice planes. Specifically, I have measured the lattice potential depth of sublevels of ^85Rb nD atoms (50<=n<=65) in a one-dimensional optical lattice with a transverse DC electric field. The trapping behavior varies substantially for the various angular sublevels, in agreement with theory. The talk will conclude with an outlook into planned experiments.

  20. Transfer of a weakly bound electron in collisions of Rydberg atoms with neutral particles. II. Ion-pair formation and resonant quenching of the Rb(nl) and Ne(nl) States by Ca, Sr, and Ba atoms

    SciTech Connect

    Narits, A. A.; Mironchuk, E. S.; Lebedev, V. S.

    2013-10-15

    Electron-transfer processes are studied in thermal collisions of Rydberg atoms with alkaline-earth Ca(4s{sup 2}), Sr(5s{sup 2}), and Ba(6s{sup 2}) atoms capable of forming negative ions with a weakly bound outermost p-electron. We consider the ion-pair formation and resonant quenching of highly excited atomic states caused by transitions between Rydberg covalent and ionic terms of a quasi-molecule produced in collisions of particles. The contributions of these reaction channels to the total depopulation cross section of Rydberg states of Rb(nl) and Ne(nl) atoms as functions of the principal quantum number n are compared for selectively excited nl-levels with l Much-Less-Than n and for states with large orbital quantum numbers l = n - 1, n - 2. It is shown that the contribution from resonant quenching dominates at small values of n, and the ion-pair formation process begins to dominate with increasing n. The values and positions of the maxima of cross sections for both processes strongly depend on the electron affinity of an alkaline-earth atom and on the orbital angular momentum l of a highly excited atom. It is shown that in the case of Rydberg atoms in states with large l {approx} n - 1, the rate constants of ion-pair formation and collisional quenching are considerably lower than those for nl-levels with l Much-Less-Than n.

  1. Storage enhanced non-linearities in a cold Rydberg ensemble

    NASA Astrophysics Data System (ADS)

    Distante, Emanuele; Padron-Brito, Auxiliadora; Cristiani, Matteo; Paredes-Barato, David; de Riedmatten, Hugues

    2016-05-01

    The possibility to control the interaction between photons provided by highly nonlinear media is a key ingredient to the goal of quantum information processing using photons and a unique tool to study the dynamics of the many-body correlated system. To mediate this interaction, one can exploit electromagnetically induced transparency (EIT) to map the state of the photons into atomic coherence in the form of Rydberg dark-state polaritons. The combination of EIT with the nonlinear interaction between Rydberg atoms provides and effective interaction between photons. By measuring the dynamics of stored Rydberg polaritons, we experimentally demonstrate that storing a probe pulse as Rydberg polaritons strongly enhances the Rydberg mediated interaction compared to the slow-propagation case. We show that the process is characterized by two time scales. We measure a strong enhancement of the interaction at short time scales. By measuring the time-dependent coherence of the stored polariton, we also show that the long time scale dynamics is dominated by Rydberg induced dephasing of the multiparticle components of the state. Our results have a direct consequence in Rydberg quantum optics and enable the test of new theories of strongly interacting Rydberg systems. This work has been funded by: ERC starting Grant QuLIMA, MINECO, Severo Ochoa Grant, AUGAUR and the Europea Union's Horizon 2020.

  2. Dynamics and kinetics of molecular high Rydberg states in the presence of an electrical field: An experimental and classical computational study

    NASA Astrophysics Data System (ADS)

    Rabani, Eran; Levine, R. D.; Mühlpfordt, Annette; Even, U.

    1995-01-01

    The effect of an electrical field on the dynamics and decay kinetics of a high Rydberg electron coupled to a core is discussed with special reference to simulations using classical dynamics and to experiment. The emphasis is on the evolution of the system within the range of Rydberg states that can be detected by delayed pulsed ionization spectroscopy (which is n≳90 for both the experiment and the computations). The Hamiltonian used in the computations is that of a diatomic ionic core about which the electron revolves. The primary coupling is due to the anisotropic part of the potential which can induce energy and angular momentum exchange between the orbital motion of the electron and the rotation of the ion. The role of the field is to modulate this coupling due to the oscillation of the orbital angular momentum l of the electron. In the region of interest, this oscillation reduces the frequency with which the electron gets near to the core and thereby slows down the decay caused by the coupling to the core. In the kinetic decay curves this is seen as a stretching of the time axis. For lower Rydberg states, where the oscillation of l is slower, the precession of the orbit, due to the central but not Coulombic part of the potential of the core, prevents the oscillation of l and the decay is not slowed down. Examination of individual trajectories demonstrates that the stretching of the time axis due to the oscillatory motion of the electron angular momentum in the presence of the field is as expected on the basis of theoretical considerations. The relation of this time stretch to the concept of the dilution effect is discussed, with special reference to the coherence width of our laser and to other details of the excitation process. A limit on the principal quantum number below which the time stretch effect will be absent is demonstrated by the computations. The trajectories show both up and down processes in which the electron escapes from the detection window

  3. Role of the helium ground state in (e,3e) processes

    SciTech Connect

    Ancarani, L.U.; Montagnese, T.; Dal Cappello, C.

    2004-07-01

    Absolute (e,3e) measurements on helium, at high incident energy, have been recently reproduced by a calculation in the first Born approximation [Phys. Rev. Lett. 91, 73201 (2003)]. The theoretical model is based on the product of three Coulomb waves for the final state and the use of Pluvinage wave function for the initial helium ground state. The authors suggest that the good agreement obtained is strongly related to the quality of the initial state, in particular to the fact that it is diagonal in all Coulomb interactions. In this paper, we show that this conclusion is not correct. We construct three other helium ground states to demonstrate that diagonalizing the Hamiltonian is not the deciding factor in obtaining agreement with the absolute experimental data.

  4. Direct detection of Rydberg-Rydberg millimeter-wave transitions in a buffer gas cooled molecular beam

    NASA Astrophysics Data System (ADS)

    Zhou, Yan; Grimes, David D.; Barnum, Timothy J.; Patterson, David; Coy, Stephen L.; Klein, Ethan; Muenter, John S.; Field, Robert W.

    2015-11-01

    Millimeter-wave transitions between molecular Rydberg states (n ∼ 35) of barium monofluoride are directly detected via Free Induction Decay (FID). Two powerful technologies are used in combination: Chirped-Pulse millimeter-Wave (CPmmW) spectroscopy and a buffer gas cooled molecular beam photoablation source. Hundreds of Rydberg-Rydberg transitions are recorded in 1 h with >10:1 signal:noise ratio and ∼150 kHz resolution. This high resolution, high spectral velocity experiment promises new strategies for rapid measurements of structural and dynamical information, such as the electric structure (multipole moments and polarizabilities) of the molecular ion-core and the strengths and mechanisms of resonances between Rydberg electron and ion-core motions. Direct measurements of Rydberg-Rydberg transitions with kilo-Debye dipole moments support efficient and definitive spectral analysis techniques, such as the Stark demolition and polarization diagnostics, which enable semi-automatic assignments of core-nonpenetrating Rydberg states. In addition, extremely strong radiation-mediated collective effects (superradiance) in a dense Rydberg gas of barium atoms are observed.

  5. A Deeper Look into the Thermodynamic Perfection of the Debye Equation of State for Helium-3

    NASA Astrophysics Data System (ADS)

    Huang, Yonghua

    A new form of a state equation for helium-3 in wide range of temperature and pressure, based on a conceptual extrapolation from the Debye equation for specific heat of solid materials was previously developed. A deeper look into the performance of the state equation was recently considered necessary and valuable, due to some feedback from cryogenic applications. The evaluation of has been conducted with the Grüneisen parameter along isobar and isotherms, cubic sound velocity - pressure linearity, enthalpy and entropy at low pressures, and the virial coefficients as the benchmarks. Some similar analysis was applied to helium-4 for the sake of analogizing the common behavior of these isotopes, particularly in the critical region. The results confirmed the good thermodynamic perfection of the Debye state equation for helium-3 in most areas on the phase diagram as declared before.

  6. Spin squeezing in a Rydberg lattice clock.

    PubMed

    Gil, L I R; Mukherjee, R; Bridge, E M; Jones, M P A; Pohl, T

    2014-03-14

    We theoretically demonstrate a viable approach to spin squeezing in optical lattice clocks via optical dressing of one clock state to a highly excited Rydberg state, generating switchable atomic interactions. For realistic experimental parameters, these interactions are shown to generate over 10 dB of squeezing in large ensembles within a few microseconds and without degrading the subsequent clock interrogation. PMID:24679291

  7. Analysis of 1s(2s2p {sup 3}P)nl Rydberg states in the K-shell photoionization of the Be atom

    SciTech Connect

    Yoshida, Fumiko; Matsuoka, Leo; Takashima, Ryuta; Hasegawa, Shuichi; Nagata, Tetsuo; Azuma, Yoshiro; Obara, Satoshi; Koike, Fumihiro

    2006-06-15

    We have observed inner-shell photoionization of Be using synchrotron radiation in the energy region of the 1s(2s2p {sup 3}P)nl Rydberg states. We used a time-of-flight method to distinguish singly and doubly charged photoions and obtained the Be{sup +} [ns; n=5-12 ({sup 1}P)3s] and Be{sup 2+} [ns; n=5-8, nd=5,6 ({sup 1}P)3s] ion spectra with high resolution corresponding to an instrumental bandpass of 13 meV. Detailed analysis enabled the autoionization parameters, resonance energy position E{sub 0}, resonance width {gamma}, and Fano parameter q, to be obtained. From the resonance positions of the {sup 3}Pnl series members, the series limit was determined to be 127.97 eV, which is in good agreement with previous experiments.

  8. Simulated quantum process tomography of quantum gates with Rydberg superatoms

    NASA Astrophysics Data System (ADS)

    Beterov, I. I.; Saffman, M.; Yakshina, E. A.; Tretyakov, D. B.; Entin, V. M.; Hamzina, G. N.; Ryabtsev, I. I.

    2016-06-01

    We have numerically simulated quantum tomography of single-qubit and two-qubit quantum gates with qubits represented by mesoscopic ensembles containing random numbers of atoms. Such ensembles of strongly interacting atoms in the regime of Rydberg blockade are known as Rydberg superatoms. The stimulated Raman adiabatic passage (STIRAP) in the regime of Rydberg blockade is used for determining Rydberg excitation in the ensemble, required for the storage of quantum information in the collective state of the atomic ensemble and implementation of two-qubit gates. The optimized shapes of the STIRAP pulses are used to achieve high fidelity of the population transfer. Our simulations confirm the validity and high fidelity of single-qubit and two-qubit gates with Rydberg superatoms.

  9. Classical description of charge exchange involving He-like or Li-like ions in Rydberg states in plasmas

    NASA Astrophysics Data System (ADS)

    Kryukov, N.; Oks, E.

    2016-02-01

    A purely classical description of energy terms of one-electron Rydberg quasimolecules (hereafter, RQ1) consisting of one electron and two fully stripped ions of charges Z and Z‧, where Z‧ ≠ Z, had been previously published by one of us. The analysis of the crossings of the energy terms led to a classical description of charge exchange either between a hydrogen-like ion of the nuclear charge Z with a fully stripped ion of the charge Z‧ or between a hydrogen-like ion of the nuclear charge Z‧ with a fully stripped ion of the charge Z. Later applications included, e.g., the influence of electric and magnetic fields, as well as of the screening by plasma electrons. In the present paper we extend the classical description of energy terms to two-electron Rydberg quasimolecules (RQ2), consisting of two electrons and two fully stripped ions of charges Z and Z‧, and to three-electron Rydberg quasimolecules (RQ3), consisting of three electrons and two fully stripped ions of charges Z and Z‧. We show that classical energy terms of RQ2 and RQ3 also exhibit crossings like the energy terms of RQ1. The crossing of terms of RQ2 occurs at a larger internuclear distance compared to the crossing of the corresponding terms of RQ1, so that the cross-section of the charge exchange for RQ2 is larger than the corresponding cross-section for RQ1. The crossing of terms of RQ3 occurs at an even larger internuclear distance compared to the crossing of the corresponding terms of RQ2, so that the cross-section of the charge exchange for RQ3 is even larger than the corresponding cross-section for RQ2. Thus, the classical roots of charge exchange are revealed not only by the example of RQ1 systems, but also by the examples of RQ2 and RQ3 systems. Our results contribute to advance the understanding of the quantum-classical correspondence and can be used in applications where charge exchange plays the key role.

  10. Filtering single atoms from Rydberg-blockaded mesoscopic ensembles

    NASA Astrophysics Data System (ADS)

    Petrosyan, David; Rao, D. D. Bhaktavatsala; Mølmer, Klaus

    2015-04-01

    We propose an efficient method to filter out single atoms from trapped ensembles with unknown numbers of atoms. The method employs stimulated adiabatic passage to reversibly transfer a single atom to the Rydberg state which blocks subsequent Rydberg excitation of all the other atoms within the ensemble. This triggers the excitation of Rydberg-blockaded atoms to short-lived intermediate states and their subsequent decay to untrapped states. Using an auxiliary microwave field to carefully engineer the dissipation, we obtain a nearly deterministic single-atom source. Our method is applicable to small atomic ensembles in individual microtraps and in lattice arrays.

  11. Quasi-One-Dimensional Electronic States Inside and Outside Helium-Plated Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Motta, M.; Galli, D. E.; Liebrecht, M.; Del Maestro, A.; Cole, M. W.

    2016-06-01

    About one-half a century ago, it was realized that electrons experience a repulsive barrier when approaching the surface of condensed phases of helium, hydrogen, and neon. This led to the proposal and subsequent observation of image-potential surface-bound electronic states, which exhibit intriguing quasi-two-dimensional behavior. In the present work, we report similar quasi-one-dimensional electronic states by exploring single-wall carbon nanotubes coated both inside and outside by thin helium films. Electrons near such structures are localized in the radial direction, but free to move along the nanotube axis. The many-body aspects of the system are discussed qualitatively.

  12. Coherence in Rydberg Atoms: Measurement and Control

    NASA Astrophysics Data System (ADS)

    Kutteruf, Mary

    We demonstrate a variety of techniques for measuring and controlling dephasing and decoherence in alkali metal Rydberg atom systems. Specifically, we investigate the coherence of the spin-orbit interaction in individual atoms and of dipole-dipole resonant energy exchange between pairs of atoms. Rydberg atoms are a good model system for exploring decoherence because they are sensitive to noise in their environments. The phase coherence of wave packets encoded on the fine-structure Rydberg states of lithium atoms is measured using a population echo and preserved using pulsed and continuous dynamic decoupling techniques. Pulsed electric fields toggle the spin-orbit coupling, repeatedly flipping the state vector, and preventing the slow acquisition of phase noise in a bang-bang scheme. Continuous dynamic decoupling is implemented by driving population between the relevant electronic states with a resonant rf field. The energy spacing between the levels is locked to the rf frequency as long as the Rabi rate is much greater than the dephasing rate. We demonstrate a technique which reduces the average relative velocity between interacting potassium Rydberg atoms, extending the atom transit time and allowing us to control when all resonant energy exchange interactions in the ensemble begin and end. Velocity reduction is achieved without the use of a chopper wheel by exciting a small cylinder of atoms and allowing them to thermally expand prior to tuning them into resonance. Resonant energy transfer is explored further in a nearly frozen rubidium Rydberg gas. We observe enhancement in the transition signal when the probability amplitudes acquired on opposite sides of the resonance interfere constructively compared to the population transferred when remaining on either side of the resonance. This enhancement reflects the coherence of the energy exchange interaction and decays over 10 us microseconds. The observed coherence time is much longer than previously measured

  13. Progress towards a precision measurement of the n=2 triplet P fine structure of atomic helium

    NASA Astrophysics Data System (ADS)

    Kato, K.; Fitzakerley, D. W.; George, M. C.; Vutha, A. C.; Storry, C. H.; Hessels, E. A.

    2016-05-01

    We report progress on the measurement of the J = 1 to J = 2 23 P fine-structure interval of atomic helium. The measurement uses a liquid-nitrogen-cooled DC discharge source of metastable helium and the atomic beam is laser cooled in the transverse directions. The atoms are excited to 23 P by a 1083-nm diode laser, and the fine-structure transition is driven by microwaves using the frequency-offset separated oscillatory fields technique. The transition is detected by further laser excitation to a Rydberg state, followed by Stark ionization. This work is supported by NSERC, CRC.

  14. Relativistic corrections to the non-Born-Oppenheimer energies of the lowest singlet Rydberg states of 3He and 4He.

    PubMed

    Stanke, Monika; Kedziera, Dariusz; Bubin, Sergiy; Adamowicz, Ludwik

    2007-05-21

    In this work the authors present an approach to calculate the leading-order relativistic corrections for ground and excited states of helium isotopomers. In the calculations they used variational wave functions expanded in terms of explicitly correlated Gaussians obtained without assuming the Born-Oppenheimer approximation. PMID:17523809

  15. Steady-state bistability and long-range order in optically driven Rydberg gases in the anti-blockade regime

    NASA Astrophysics Data System (ADS)

    Letscher, Fabian; Linzner, Dominik; Fleischhauer, Michael

    2016-05-01

    Motivated by recent experiments, we study spatial and temporal correlations of Rydberg excitations of optically driven ultra-cold atoms in the anti-blockade regime. In particular, we discuss the influence of dissipation on the excitation dynamics of a linear chain of atoms, described by the dissipative, transverse-field Ising model. Using t-DMRG simulations of the density matrix we identify parameter regimes with diverging correlation lengths in the coherent regime of weak dissipation. Correlation lengths remain short-ranged in the incoherent regime of strong dissipation, where classical rate equations can be employed. We discuss the different physical mechanisms determining the many-body dynamics in the two regimes and compare theoretical predictions with recent experimental results. In particular we discuss the formation of excitation cluster in the incoherent regime and explain the observed slow-down of the relaxation process due to cluster formation.

  16. Exotic Self-trapped States of an Electron in Superfluid Helium

    NASA Astrophysics Data System (ADS)

    Elser, Veit

    2015-09-01

    We explore the possibility that the fast and exotic negative ions in superfluid helium are electrons bound to quantized vortex structures, the simplest being a ring. In the states we consider, the electron energy is only slightly below the conduction band minimum of bulk helium. To support our proposal, we present two calculations. In the first, we show that the electron pressure on the vortex core is insufficient to cavitate the helium and form an electron bubble. In the second, we estimate the equilibrium radius of the vortex ring that would bind an electron and find it is much smaller than the electron bubble, about 7 Å. The many exotic ions reported in experiments might be bound states of an electron with more complex vortex structures.

  17. Transition rates for a Rydberg atom surrounded by a plasma

    NASA Astrophysics Data System (ADS)

    Lin, Chengliang; Gocke, Christian; Röpke, Gerd; Reinholz, Heidi

    2016-04-01

    We derive a quantum master equation for an atom coupled to a heat bath represented by a charged particle many-body environment. In the Born-Markov approximation, the influence of the plasma environment on the reduced system is described by the dynamical structure factor. Expressions for the profiles of spectral lines are obtained. Wave packets are introduced as robust states allowing for a quasiclassical description of Rydberg electrons. Transition rates for highly excited Rydberg levels are investigated. A circular-orbit wave-packet approach has been applied in order to describe the localization of electrons within Rydberg states. The calculated transition rates are in a good agreement with experimental data.

  18. Rydberg states of the ArCO2 and KrCO2 van der Waals molecules

    SciTech Connect

    Dehmer, Patricia M.

    1985-01-01

    Relative photoionization cross sections were determined for ArCO2 at a wavelength resolution of 0.24 A in the regions of both the Ar*+CO2 and the Ar+CO2* dissociation limits (690--920 Â) and for KrCO2 at a wavelength resolution of 0.4 Â in the region of the Kr+CO2* dissociation limits (690--780 Â). The dimer ionization potentials are 13.59±0.04 eV (912.5±2.5 Â) for ArCO2 and 13.33±0.04 eV (930.0±3.0 Â) for KrCO2. Combining these values with the known value of the CO2 ionization potential and the known (or estimated) values of the ArCO2 and KrCO2 dissociation energies yields values for the dimer ion ground state dissociation energies of 0.20±0.04 eV for ArCO2⁺ and 0.47±0.05 eV for KrCO2⁺. Rydberg structure is observed in the photoionization cross section of ArCO2 corresponding to dissociation limits of the type Ar*(nd,ns)+CO2; however, discrete structure is observed only near the Ar*(3d,5s)+CO2 dissociation limits. Van der Waals structure corresponding to the higher Ar*+CO2 limits is diffuse and red degraded. Molecular Rydberg structure also is observed in the photoionization cross sections of both ArCO2 and KrCO2 corresponding to dissociation limits of the type Ar+CO2*. Prominent van der Waals structure is observed corresponding to dissociation limits based on members of the CO2 Henning sharp and diffuse Rydberg series, which converge to CO2B ²Σu⁺ ; however, no van der Waals structure is observed corresponding to dissociation limits based on members of the CO2 Tanaka–Ogawa Rydberg series, which converge to CO2⁺ A ²Πu . Various experimental evidence indicates that neither vibrational predissociation of the excited van der Waals dimer nor vibrational

  19. From molecular spectra to a density shift in dense Rydberg gases

    PubMed Central

    Gaj, A.; Krupp, A. T.; Balewski, J. B.; Löw, R.; Hofferberth, S.; Pfau, T.

    2014-01-01

    In Rydberg atoms, at least one electron is excited to a state with a high principal quantum number. In an ultracold environment, this low-energy electron can scatter off a ground state atom allowing for the formation of a Rydberg molecule consisting of one Rydberg atom and several ground state atoms. Here we investigate those Rydberg molecules created by photoassociation for the spherically symmetric S-states. A step by step increase of the principal quantum number up to n=111 enables us to go beyond the previously observed dimer and trimer states up to a molecule, where four ground state atoms are bound by one Rydberg atom. The increase of bound atoms and the decreasing binding potential per atom with principal quantum number results finally in an overlap of spectral lines. The associated density-dependent line broadening sets a fundamental limit, for example, for the optical thickness per blockade volume in Rydberg quantum optics experiments. PMID:25082599

  20. Equation of state and transport properties of warm dense helium via quantum molecular dynamics simulations

    NASA Astrophysics Data System (ADS)

    Li, Zhi-Guo; Cheng, Yan; Chen, Qi-Feng; Chen, Xiang-Rong

    2016-05-01

    The equation of state, self-diffusion, and viscosity coefficients of helium have been investigated by quantum molecular dynamics (QMD) simulations in the warm dense matter regime. Our simulations are validated through the comparison with the reliable experimental data. The calculated principal and reshock Hugoniots of liquid helium are in good agreement with the gas-gun data. On this basis, we revisit the issue for helium, i.e., the possibility of the instabilities predicted by chemical models at around 2000 GPa and 10 g/cm3 along the pressure isotherms of 6309, 15 849, and 31 623 K. Our calculations show no indications of instability in this pressure-temperature region, which reconfirm the predictions of previous QMD simulations. The self-diffusion and viscosity coefficients of warm dense helium have been systematically investigated by the QMD simulations. We carefully test the finite-size effects and convergences of statistics, and obtain numerically converged self-diffusion and viscosity coefficients by using the Kubo-Green formulas. The present results have been used to evaluate the existing one component plasma models. Finally, the validation of the Stokes-Einstein relationship for helium in the warm dense regime is discussed.

  1. State-to-State Inelastic Scattering of O2 with Helium.

    PubMed

    Bishwakarma, Chandan Kumar; van Oevelen, George; Scheidsbach, Roy; Parker, David H; Kalugina, Yulia; Lique, François

    2016-02-18

    Molecular oxygen (O2) is extremely important for a wide variety of processes on and outside Earth. Indeed, O2–He collisions are crucial to model O2 abundance in space or to create ultracold O2 molecules. A crossed molecular beam experiment to probe rotational excitation of O2 due to helium collisions at energies of 660 cm–1 is reported. Velocity map imaging was combined with state-selective detection of O2(X3Σg–) by (2+1) resonance-enhanced multiphoton ionization. The obtained raw O2+ images were corrected from density to flux and the differential cross sections (DCS) were then extracted for six O2 final states. Exact quantum mechanical calculations were also performed. A very good agreement between experimental and theoretical DCSs was found by using an initial O2 beam population ratio of 80% for the first rotational state and 20% for the first excited state. The agreement demonstrates our ability to model inelastic processes between O2 molecules and rare gas both theoretically and experimentally. PMID:26829188

  2. Dislocation-mediated melting of one-dimensional Rydberg crystals

    SciTech Connect

    Sela, Eran; Garst, Markus; Punk, Matthias

    2011-08-15

    We consider cold Rydberg atoms in a one-dimensional optical lattice in the Mott regime with a single atom per site at zero temperature. An external laser drive with Rabi frequency {Omega} and laser detuning {Delta} creates Rydberg excitations whose dynamics is governed by an effective spin-chain model with (quasi) long-range interactions. This system possesses intrinsically a large degree of frustration resulting in a ground-state phase diagram in the ({Delta},{Omega}) plane with a rich topology. As a function of {Delta}, the Rydberg blockade effect gives rise to a series of crystalline phases commensurate with the optical lattice that form a so-called devil's staircase. The Rabi frequency {Omega}, on the other hand, creates quantum fluctuations that eventually lead to a quantum melting of the crystalline states. Upon increasing {Omega}, we find that generically a commensurate-incommensurate transition to a floating Rydberg crystal that supports gapless phonon excitations occurs first. For even larger {Omega}, dislocations within the floating Rydberg crystal start to proliferate and a second, Kosterlitz-Thouless-Nelson-Halperin-Young dislocation-mediated melting transition finally destroys the crystalline arrangement of Rydberg excitations. This latter melting transition is generic for one-dimensional Rydberg crystals and persists even in the absence of an optical lattice. The floating phase and the concomitant transitions can, in principle, be detected by Bragg scattering of light.

  3. Cavity quantum electrodynamics with a Rydberg-blocked atomic ensemble

    SciTech Connect

    Guerlin, Christine; Brion, Etienne; Esslinger, Tilman; Moelmer, Klaus

    2010-11-15

    The realization of a Jaynes-Cummings model in the optical domain is proposed for an atomic ensemble. The scheme exploits the collective coupling of the atoms to a quantized cavity mode and the nonlinearity introduced by coupling to high-lying Rydberg states. A two-photon transition resonantly couples the single-atom ground state |g> to a Rydberg state |e> via a nonresonant intermediate state |i>, but due to the interaction between Rydberg atoms only a single atom can be resonantly excited in the ensemble. This restricts the state space of the ensemble to the collective ground state |G> and the collectively excited state |E> with a single Rydberg excitation distributed evenly on all atoms. The collectively enhanced coupling of all atoms to the cavity field with coherent coupling strengths which are much larger than the decay rates in the system leads to the strong coupling regime of the resulting effective Jaynes-Cummings model. We use numerical simulations to show that the cavity transmission can be used to reveal detailed properties of the Jaynes-Cummings ladder of excited states and that the atomic nonlinearity gives rise to highly nontrivial photon emission from the cavity. Finally, we suggest that the absence of interactions between remote Rydberg atoms may, due to a combinatorial effect, induce a cavity-assisted excitation blockade whose range is larger than the typical Rydberg dipole-dipole interaction length.

  4. Rydberg Impurity Probes in Ultracold Gases

    NASA Astrophysics Data System (ADS)

    Mitchison, Mark; Johnson, Tomi; Plenio, Martin; Jaksch, Dieter

    2015-03-01

    Impurities immersed in ultracold gases can act as highly sensitive, tunable and potentially non-destructive probes of their environment. In this setting, we propose the use of an atomic impurity in a Rydberg state to measure density fluctuations via Ramsey interferometry. The rapid collisional dynamics of the light Rydberg electron interacting with the heavy gas particles, combined with the capability to quickly change the state of the impurity with optical pulses, make such a probe ideal for measuring local properties of ultracold gases. Our proposed device promises angle-resolved density measurements with sub-micron spatial resolution, and with no need to integrate over the line of sight. We outline how Rydberg impurity probes could be applied to study various interesting quantum states of current experimental relevance. We also discuss the possibility of using multiple Rydberg atoms to extract the spatial pair distribution function g (2) (r). Our work is placed in the context of other recently proposed impurity-based probes.

  5. Rydberg Spectroscopy in an Optical Lattice: Blackbody Thermometry for Atomic Clocks

    SciTech Connect

    Ovsiannikov, Vitali D.; Derevianko, Andrei; Gibble, Kurt

    2011-08-26

    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}.

  6. Imaging Spatial Correlations of Rydberg Excitations in Cold Atom Clouds

    SciTech Connect

    Schwarzkopf, A.; Sapiro, R. E.; Raithel, G.

    2011-09-02

    We use direct spatial imaging of cold {sup 85}Rb Rydberg atom clouds to measure the Rydberg-Rydberg correlation function. The results are in qualitative agreement with theoretical predictions [F. Robicheaux and J. V. Hernandez, Phys. Rev. A 72, 063403 (2005)]. We determine the blockade radius for states 44D{sub 5/2}, 60D{sub 5/2}, and 70D{sub 5/2} and investigate the dependence of the correlation behavior on excitation conditions and detection delay. Experimental data hint at the existence of long-range order.

  7. Addressing single trapped ions for Rydberg quantum logic

    NASA Astrophysics Data System (ADS)

    Bachor, P.; Feldker, T.; Walz, J.; Schmidt-Kaler, F.

    2016-08-01

    We demonstrate the excitation of ions to the Rydberg state 22F by vacuum ultraviolet radiation at a wavelength of 123 nm combined with the coherent manipulation of the optical qubit transition in {}40{{Ca}}+. With a tightly focused beam at 729 nm wavelength we coherently excite a single ion from a linear string into the metastable 3{D}5/2 state before a VUV pulse excites it to the Rydberg state. In combination with ion shuttling in the trap, we extend this approach to the addressed excitation of multiple ions. The coherent initialization as well as the addressed Rydberg excitation are key prerequisites for more complex applications of Rydberg ions in quantum simulation or quantum information processing.

  8. Variational calculation of energy levels for metastable states of antiprotonic helium

    NASA Astrophysics Data System (ADS)

    Hu, Mu-Hong; Yao, Si-Meng; Wang, Yi; Li, Wang; Gu, Ying-Ying; Zhong, Zhen-Xiang

    2016-06-01

    We apply the variational method in Hylleraas coordinates to solve the energy eigenvalue problem for antiprotonic helium molecular systems including p bar 3 He+ and p bar 4 He+. The numerical accuracy on the nonrelativistic energies is shown to reach 10-17, thus the precision of our results is only limited by the width of the metastable states. Expectation values of the Dirac delta operators for these states are also calculated.

  9. Measurement of the lifetime of excited-state electron bubbles in superfluid helium

    SciTech Connect

    Ghosh, Ambarish; Maris, Humphrey J.

    2005-08-01

    We report on the measurement of the lifetime of bubbles in superfluid helium that contain an electron in the 1P state. The 1P bubbles are produced by laser excitation of ground-state bubbles, and are detected by ultrasonic cavitation. Our measurements show that the lifetime of these excited bubbles is much less than the calculated lifetime for radiative decay and, hence, is determined by a nonradiative mechanism.

  10. Standoff detection of large organic molecules using Rydberg fingerprint spectroscopy and microwave Rayleigh scattering

    SciTech Connect

    Rudakov, Fedor M; Zhang, Zhili

    2012-01-01

    We present a technique for nonintrusive and standoff detection of large organic molecules using coherent microwave Rayleigh scattering from plasma produced by structure sensitive photoionization through Rydberg states. We test the method on 1,4-diazobicyclooctane. Transitions between the 3s Rydberg state and higher lying Rydberg states are probed using two-color photoionization with 266?nm photons and photons in the range of 460-2400 nm. Photoionization is detected using microwave radiation, which is scattered by the unbounded electrons. Highly resolved Rydberg spectra are acquired in vacuum and in air.