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Sample records for adiabatic ionization potentials

  1. Double-resonant photoionization efficiency spectroscopy: A precise determination of the adiabatic ionization potential of DCO

    NASA Astrophysics Data System (ADS)

    Foltynowicz, Robert J.; Robinson, Jason D.; Grant, Edward R.

    2001-03-01

    We report the first high-resolution measurement of the adiabatic ionization potential of DCO and the fundamental bending frequency of DCO+. Fixing a first-laser frequency on selected ultraviolet transitions to individual rotational levels in the (000) band of the 3pπ 2Π intermediate Rydberg state of DCO, we scan a second visible laser over the range from 20 000 to 20 300 cm-1 to record double resonance photoionization efficiency (DR/PIE) spectra. Intermediate resonance with this Rydberg state facilitates transitions to the threshold for producing ground-state cations by bridging the Franck-Condon gap between the bent neutral radical and linear cation. By selecting a single rotational state for ionization, double-resonant excitation eliminates thermal congestion. Spectroscopic features for first-photon resonance are identified by reference to a complete assignment of the 3pπ 2Π(000)-X 2A'(000) band system of DCO. Calibration with HCO, for which the adiabatic ionization threshold is accurately known, establishes an experimental instrument function that accounts for collisional effects on the shape of the photoionization efficiency spectrum near threshold. Analysis of the DR/PIE threshold for DCO yields an adiabatic ionization threshold of 65 616±3 cm-1. By extrapolation of vibrationally autoionizing Rydberg series accessed from the Σ+ component of the 3pπ 2Π(010) intermediate state, we determine an accurate rotationally state-resolved threshold for producing DCO+(010). This energy, together with the threshold determined for the vibrational ground state of the cation provides a first estimate of the bending frequency for DCO+ as 666±3 cm-1. Assignment of the (010) autoionization spectrum further yields a measurement of an energy of 4.83±0.01 cm-1 for the (2-1) rotational transition in the 1Σ+(0110) state of DCO+.

  2. Band gaps, ionization potentials, and electron affinities of periodic electron systems via the adiabatic-connection fluctuation-dissipation theorem

    NASA Astrophysics Data System (ADS)

    Trushin, Egor; Betzinger, Markus; Blügel, Stefan; Görling, Andreas

    2016-08-01

    An approach to calculate fundamental band gaps, ionization energies, and electron affinities of periodic electron systems is explored. Starting from total energies obtained with the help of the adiabatic-connection fluctuation-dissipation (ACFD) theorem, these physical observables are calculated according to their basic definition by differences of the total energies of the N -, (N -1 ) -, and (N +1 ) -electron system. The response functions entering the ACFD theorem are approximated here by the direct random phase approximation (dRPA). For a set of prototypical semiconductors and insulators it is shown that even with this quite drastic approximation the resulting band gaps are very close to experiment and of a similar quality to those from the computationally more involved G W approximation. By going beyond the dRPA in the future the accuracy of the calculated band gaps may be significantly improved further.

  3. Density functional theory calculations on rhodamine B and pinacyanol chloride. Optimized ground state, dipole moment, vertical ionization potential, adiabatic electron affinity and lowest excited triplet state.

    PubMed

    Delgado, Juan C; Selsby, Ronald G

    2013-01-01

    The ground state configuration of the gas phase cationic dyes pinacyanol chloride and rhodamine B are optimized with HF/6-311 + G(2d,2p) method and basis set. B3PW91/6-311 + G(2df,2p) functional and basis set is used to calculate the Mulliken atom charge distribution, total molecular energy, the dipole moment, the vertical ionization potential, the adiabatic electron affinity and the lowest excited triplet state, the last three as an energy difference between separately calculated open shell and ground states. The triplet and extra electron states are optimized to find the relaxation energy. In the ground state optimization of both dyes the chloride anion migrates to a position near the center of the chromophore. For rhodamine B the benzoidal group turns perpendicular to the chromophore plane. For both dyes, the LUMO is mostly of π character associated with the aromatic part of the molecule containing the chromophore. The highest occupied MOs consist of three almost degenerate eigenvectors involving the chloride anion coordinated with σ electrons in the molecular framework. The fourth highest MO is of π character. For both molecules in the gas phase ionization process the chloride anion loses the significant fraction of electric charge. In electron capture, the excess charge goes mainly on the dye cation. PMID:22891949

  4. Adiabatic Approximation of the Correlation Function in the Density-Functional Treatment of Ionization Processes

    SciTech Connect

    Wilken, F.; Bauer, D.

    2006-11-17

    The ionization of a one-dimensional model helium atom in short laser pulses using time-dependent density-functional theory is investigated. We calculate ionization probabilities as a function of laser intensity by approximating the correlation function of the system adiabatically with an explicit dependence on the fractional number of bound electrons. For the correlation potential we take the derivative discontinuity at integer numbers of bound electrons explicitly into account. This approach reproduces ionization probabilities from the solution of the time-dependent Schroedinger equation, in particular, the so-called knee due to nonsequential ionization.

  5. Adiabatic Hyperspherical Analysis of Realistic Nuclear Potentials

    NASA Astrophysics Data System (ADS)

    Daily, K. M.; Kievsky, Alejandro; Greene, Chris H.

    2015-12-01

    Using the hyperspherical adiabatic method with the realistic nuclear potentials Argonne V14, Argonne V18, and Argonne V18 with the Urbana IX three-body potential, we calculate the adiabatic potentials and the triton bound state energies. We find that a discrete variable representation with the slow variable discretization method along the hyperradial degree of freedom results in energies consistent with the literature. However, using a Laguerre basis results in missing energy, even when extrapolated to an infinite number of basis functions and channels. We do not include the isospin T = 3/2 contribution in our analysis.

  6. Ionization potentials of seaborgium

    SciTech Connect

    Johnson, E.; Pershina, V.; Fricke, B.

    1999-10-21

    Multiconfiguration relativistic Dirac-Fock values were calculated for the first six ionization potentials of seaborgium and of the other group 6 elements. No experimental ionization potentials are available for seaborgium. Accurate experimental values are not available for all of the other ionization potentials. Ionic radii for the 4+ through 6+ ions of seaborgium are also presented. The ionization potentials and ionic radii obtained will be used to predict some physiochemical properties of seaborgium and its compounds.

  7. Theoretical determinations of ionization potentials of dopamine

    NASA Astrophysics Data System (ADS)

    Lu, J. F.; Yu, Z. Y.

    2013-04-01

    Adiabatic and vertical ionization potentials (IPs) of nine conformers of dopamine in the gas phase are determined using density functional theory (DFT) B3LYP, B3P86, B3PW91 methods and high level ab initio HF method with 6-311++G** basis set, respectively. And the nine stable cationic states have been found in the ionization process of dopamine. Vertical ionization potentials of nine conformers of dopamine are calculated using the older outer-valence Green's function (OVGF) calculations at 6-311++G** basis set. Vibrational frequencies and infrared spectrum intensities of G1b and G1b+ at B3LYP/6-311++G** level are discussed.

  8. Non-adiabatic imprints on the electron wave packet in strong field ionization with circular polarization

    NASA Astrophysics Data System (ADS)

    Hofmann, C.; Zimmermann, T.; Zielinski, A.; Landsman, A. S.

    2016-04-01

    The validity of the adiabatic approximation in strong field ionization under typical experimental conditions has recently become a topic of great interest. Experimental results have been inconclusive, in part, due to the uncertainty in experimental calibration of intensity. Here we turn to the time-dependent Schrödinger equation, where all the laser parameters are known exactly. We find that the centre of the electron momentum distribution (typically used for calibration of elliptically and circularly polarized light) is sensitive to non-adiabatic effects, leading to intensity shifts in experimental data that can significantly affect the interpretation of results. On the other hand, the transverse momentum spread in the plane of polarization is relatively insensitive to such effects, even in the Keldysh parameter regime approaching γ ≈ 3. This suggests the transverse momentum spread in the plane of polarization as a good alternative to the usual calibration method, particularly for experimental investigation of non-adiabatic effects using circularly polarized light.

  9. The lowest ionization potentials of Al2

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W., Jr.; Barnes, Leslie A.; Taylor, Peter R.

    1988-01-01

    Potential curves for the lowest two electronic states (X 2 sigma g + and A 2 pi u) of Al2(+) were computed using complete active space SCF/multireference CI wave functions and large Gaussian basis sets. The lowest observable vertical ionization potential (to Al2(+) X 2 sigma g +) of the Al2 X 3 pi u ground state is calculated to occur around 6.1 eV, in excellent agreement with the experimental range of 6.0 to 6.42 eV obtained in recent cluster ionization studies by Cox and co-workers. The second vertical ionization potential (to Al2(+) A 2 pi u) occurs near 6.4 eV, also within the experimental range. The adiabatic IP of 5.90 eV is in good agreement with the value of 5.8 to 6.1 eV deduced by Hanley and co-workers from the difference in thresholds between collision induced dissociation processes of Al3(+). The computed IP values are somewhat larger than those deduced from branching ratios in cluster fragmentation experiments by Jarrold and co-workers. The observation of an ionization threshold below 6.42 eV is shown to be incompatible with an Al2 ground electronic state assignment of 3 sigma g -, but the separation between the two lowest states of Al2 is so small that it is likely that both are populated in the experiments, so that this does not provide unambiguous support for the recent theoretical assignment of the ground state as 3 pi u.

  10. Trapping ultracold atoms in a time-averaged adiabatic potential

    SciTech Connect

    Gildemeister, M.; Nugent, E.; Sherlock, B. E.; Kubasik, M.; Sheard, B. T.; Foot, C. J.

    2010-03-15

    We report an experimental realization of ultracold atoms confined in a time-averaged, adiabatic potential (TAAP). This trapping technique involves using a slowly oscillating ({approx}kHz) bias field to time-average the instantaneous potential given by dressing a bare magnetic potential with a high-frequency ({approx}MHz) magnetic field. The resultant potentials provide a convenient route to a variety of trapping geometries with tunable parameters. We demonstrate the TAAP trap in a standard time-averaged orbiting potential trap with additional Helmholtz coils for the introduction of the radio frequency dressing field. We have evaporatively cooled 5x10{sup 4} atoms of {sup 87}Rb to quantum degeneracy and observed condensate lifetimes of longer than 3 s.

  11. Ionization Potentials for Isoelectronic Series.

    ERIC Educational Resources Information Center

    Agmon, Noam

    1988-01-01

    Presents a quantitative treatment of ionization potentials of isoelectronic atoms. By looking at the single-electron view of calculating the total energy of an atom, trends in the screening and effective quantum number parameters are examined. Approaches the question of determining electron affinities. (CW)

  12. On the ionization potential of molecular oxygen

    NASA Technical Reports Server (NTRS)

    Samson, J. A. R.; Gardner, J. L.

    1974-01-01

    The ionization potential of O2 was measured by the technique of high resolution photoelectron spectroscopy taking into account the influence of rotational structure on the shape of the vibrational bands. A value of 12.071 + or - .001 eV (1027.1 + or - 0.1 A) was found for the ionization potential. A lowering of the ionization potential caused by a branch-head when delta N = -2 gave an appearance potential for ionization of 12.068 + or - .001 eV (1027.4 + or - 0.1 A).

  13. Thermochromic behaviors and ionization potentials of organopolysilanes

    NASA Astrophysics Data System (ADS)

    Yokoyama, Kenji; Yokoyama, Masaaki

    1989-04-01

    Ionization potentials of organopolysilanes with different kinds of substituents were evaluated from the low energy photo-electron emission measurements in air. An aryl-substituted organopolysilane capable of σ - π mixing between Si backbone σ and side-group π electrons gave smaller ionization potential by about 0.1˜0.15 eV compared with alkyl-substituted organopolysilanes. The value of ionization potentials in some alkyl-substituted organopolysilanes which showed thermochromic behaviors was found to vary substantially with thermally induced reversible changes in polymer backbone conformation, indicating that the effective conjugation length of σ electrons decreases above the thermochromic transition temperature.

  14. Geometric phase of an atom inside an adiabatic radio-frequency potential

    SciTech Connect

    Zhang, P.; You, L.

    2007-09-15

    We investigate the geometric phase of an atom inside an adiabatic radio-frequency (rf) potential created from a static magnetic field (B field) and a time-dependent rf field. The spatial motion of the atomic center of mass is shown to give rise to a geometric phase, or Berry's phase, in the adiabatically evolving atomic hyperfine spin along the local B field. This phase is found to depend on both the static B field along the semiclassical trajectory of the atomic center of mass and an effective magnetic field consisting of the total B field, including the oscillating rf field. Specific calculations are provided for several recent atom interferometry experiments and proposals utilizing adiabatic rf potentials.

  15. Classical nuclear dynamics on a single time-dependent potential in electronic non-adiabatic processes

    NASA Astrophysics Data System (ADS)

    Agostini, Federica; Abedi, Ali; Suzuki, Yasumitsu; Min, Seung Kyu; Maitra, Neepa T.; Gross, E. K. U.

    2015-03-01

    The Born-Oppenheimer (BO) approximation allows to visualize the coupled electron-nuclear dynamics in molecular systems as a set of nuclei moving on a single potential energy surface representing the effect of the electrons in a given eigenstate. Many interesting phenomena, however, such as vision or charge separation in organic photovoltaic materials, take place in conditions beyond its range of validity. Nevertheless, the basic construct of the adiabatic treatment, the BO potential energy surfaces, is employed to describe non-adiabatic processes and the full problem is represented in terms of adiabatic states and transitions among them in regions of strong non-adiabatic coupling. But the concept of single potential energy is lost. The alternative point of view arising in the framework of the exact factorization of the electron-nuclear wave function will be presented. A single, time-dependent, potential energy provides the force driving the nuclear motion and is adopted as starting point for the development of quantum-classical approximations to the full quantum mechanical problem.

  16. Ionization of the hydrogen atom in strong magnetic fields. Beyond the adiabatic approximation.

    NASA Astrophysics Data System (ADS)

    Potekhin, A. Y.; Pavlov, G. G.; Ventura, J.

    1997-01-01

    High magnetic fields in neutron stars, B~10^11^-10^13^G, substantially modify the properties of atoms and their interaction with radiation. In particular, the photoionization cross section becomes anisotropic and polarization dependent, being strongly reduced when the radiation is polarized perpendicular to the field. In a number of previous works based on the adiabatic approximation the conclusion was drawn that this transverse cross section vanishes for frequencies ω smaller than the electron cyclotron frequency ω_c_=eB/(m_e_c). In other works (which employed a different form of the interaction operator) appreciable finite values were obtained, ~σ_0gamma^-1^ near the photoionization threshold, where σ_0_ is the cross section without magnetic field, and γ=B/(2.35x10^9^G). Since it is the transverse cross section which determines the properties of radiation emitted from neutron star atmospheres, an adequate interpretation of the neutron star thermal-like radiation requires a resolution of this controversy. In the present work we calculate the atomic wave functions for both discrete and continuum states by solving the coupled channel equations allowing the admixture between different Landau levels, which provides much higher accuracy than the adiabatic approximation. This enables us to resolve the above contradiction in favour of the finite transverse cross sections at ω<ω_c_. Moreover, for any form of the interaction operator the non-adiabatic corrections appear to be substantial for frequencies ω> 0.3ω_c_. The non-adiabatic treatment of the continuum includes coupling between closed and open channels, which leads to the autoionization of quasi-bound energy levels associated with the electron cyclotron (Landau) excitations and gives rise to Beutler-Fano resonances of the photoionization cross section. We calculate the autoionization widths of these quasi-bound levels and compare them with the radiative widths. The correlation of the open channels is

  17. Dressed adiabatic and diabatic potentials to study conical intersections for F + H2

    NASA Astrophysics Data System (ADS)

    Das, Anita; Sahoo, Tapas; Mukhopadhyay, Debasis; Adhikari, Satrajit; Baer, Michael

    2012-02-01

    We follow a suggestion by Lipoff and Herschbach [Mol. Phys. 108, 1133 (2010), 10.1080/00268971003662912] and compare dressed and bare adiabatic potentials to get insight regarding the low-energy dynamics (e.g., cold reaction) taking place in molecular systems. In this particular case, we are interested to study the effect of conical intersections (ci) on the interacting atoms. For this purpose, we consider vibrational dressed adiabatic and vibrational dressed diabatic potentials in the entrance channel of reactive systems. According to our study, the most one should expect, in case of F + H2, is a mild effect of the (1, 2) ci on its reactive/exchange process-an outcome also supported by experiment. This happens although the corresponding dressed and bare potential barriers (and the corresponding van der Waals potential wells) differ significantly from each other.

  18. Femtosecond Laser Ionization of Organic Amines with Very Low Ionization Potential.

    NASA Astrophysics Data System (ADS)

    Yatsuhashi, Tomoyuki; Obayashi, Takashi; Tanaka, Michinori; Murakami, Masanao; Nakashima, Nobuaki

    2006-03-01

    The interaction between high intensity femtosecond laser and molecules is one of the most attractive areas in laser chemistry and ionization is the most fundamental subject. Theoretical consideration successfully reproduced the ionization behavior of rare gases. However, the understanding of ionization mechanisms of large molecules is difficult more than those of rare gases due to their complexity. Generally speaking, molecules are harder to ionize than rare gases even if they have the same ionization potential. The suppressed ionization phenomena are one of the important features of molecular ionization. Hankin et al. examined 23 organic molecules with ionization potentials between 8.25 and 11.52 eV. We have examined ionization and/ or fragmentation of many organic molecules, including aromatic compounds, halogenated compounds, methane derivatives etc. at various wavelengths below 10^16 Wcm-2. In order to investigate the nature of molecular ionization, it is interesting to examine a variety of molecule in a wide range of ionization potential. In this study, we examined several organic amines because we can explore the uninvestigated ionization potential range down to 5.95 eV. In addition to the significant suppression of the ionization rates, stepwise ionization behavior, which was not observed in rare gases, was observed.

  19. CVRQD ab initio ground-state adiabatic potential energy surfaces for the water molecule.

    PubMed

    Barletta, Paolo; Shirin, Sergei V; Zobov, Nikolai F; Polyansky, Oleg L; Tennyson, Jonathan; Valeev, Edward F; Császár, Attila G

    2006-11-28

    The high accuracy ab initio adiabatic potential energy surfaces (PESs) of the ground electronic state of the water molecule, determined originally by Polyansky et al. [Science 299, 539 (2003)] and called CVRQD, are extended and carefully characterized and analyzed. The CVRQD potential energy surfaces are obtained from extrapolation to the complete basis set of nearly full configuration interaction valence-only electronic structure computations, augmented by core, relativistic, quantum electrodynamics, and diagonal Born-Oppenheimer corrections. We also report ab initio calculations of several quantities characterizing the CVRQD PESs, including equilibrium and vibrationally averaged (0 K) structures, harmonic and anharmonic force fields, harmonic vibrational frequencies, vibrational fundamentals, and zero-point energies. They can be considered as the best ab initio estimates of these quantities available today. Results of first-principles computations on the rovibrational energy levels of several isotopologues of the water molecule are also presented, based on the CVRQD PESs and the use of variational nuclear motion calculations employing an exact kinetic energy operator given in orthogonal internal coordinates. The variational nuclear motion calculations also include a simplified treatment of nonadiabatic effects. This sophisticated procedure to compute rovibrational energy levels reproduces all the known rovibrational levels of the water isotopologues considered, H(2) (16)O, H(2) (17)O, H(2) (18)O, and D(2) (16)O, to better than 1 cm(-1) on average. Finally, prospects for further improvement of the ground-state adiabatic ab initio PESs of water are discussed. PMID:17144700

  20. Explicitly correlated potential energy surface of H3+, including relativistic and adiabatic corrections.

    PubMed

    Kutzelnigg, Werner; Jaquet, Ralph

    2006-11-15

    After a short historical account of the theory of the H3+ ion, two ab initio methods are reviewed that allow the computation of the ground-state potential energy surface (PES) of H3+ in the Born-Oppenheimer (BO) approximation, with microhartree or even sub-microhartree accuracy, namely the R12 method and the method of explicitly correlated Gaussians. The BO-PES is improved by the inclusion of relativistic effects and adiabatic corrections. It is discussed how non-adiabatic effects on rotation and vibration can be simulated by corrections to the moving nuclear masses. The importance of the appropriate analytic fit to the computed points of the PES for the subsequent computation of the rovibronic spectrum is addressed. Some recent extensions of the computed PES in the energy region above the barrier to linearity are reviewed. This involves a large set of input geometries and the correct treatment of the dissociation asymptotics, including the coupling with the first excited singlet state. Some comments on this state as well as on the lowest triplet state of H3+ are made. The paper ends with a few remarks on the ion H5+. PMID:17015373

  1. Time-Averaged Adiabatic Potentials: Versatile Matter-Wave Guides and Atom Traps

    NASA Astrophysics Data System (ADS)

    Lesanovsky, Igor; von Klitzing, Wolf

    2007-08-01

    We demonstrate a novel class of trapping potentials, time-averaged adiabatic potentials (TAAP), which allows the generation of a large variety of traps for quantum gases and matter-wave guides for atom interferometers. Examples include stacks of pancakes, rows of cigars, and multiple rings or sickles. The traps can be coupled through controllable tunneling barriers or merged altogether. We present analytical expressions for pancake-, cigar-, and ring-shaped traps. The ring geometry is of particular interest for guided matter-wave interferometry as it provides a perfectly smooth waveguide of widely tunable diameter and thus adjustable sensitivity of the interferometer. The flexibility of the TAAP would make possible the use of Bose-Einstein condensates as coherent matter waves in large-area atom interferometers.

  2. Time-averaged adiabatic potentials: versatile matter-wave guides and atom traps.

    PubMed

    Lesanovsky, Igor; von Klitzing, Wolf

    2007-08-24

    We demonstrate a novel class of trapping potentials, time-averaged adiabatic potentials (TAAP), which allows the generation of a large variety of traps for quantum gases and matter-wave guides for atom interferometers. Examples include stacks of pancakes, rows of cigars, and multiple rings or sickles. The traps can be coupled through controllable tunneling barriers or merged altogether. We present analytical expressions for pancake-, cigar-, and ring-shaped traps. The ring geometry is of particular interest for guided matter-wave interferometry as it provides a perfectly smooth waveguide of widely tunable diameter and thus adjustable sensitivity of the interferometer. The flexibility of the TAAP would make possible the use of Bose-Einstein condensates as coherent matter waves in large-area atom interferometers. PMID:17930945

  3. Time-Averaged Adiabatic Potentials: Versatile Matter-Wave Guides and Atom Traps

    SciTech Connect

    Lesanovsky, Igor; Klitzing, Wolf von

    2007-08-24

    We demonstrate a novel class of trapping potentials, time-averaged adiabatic potentials (TAAP), which allows the generation of a large variety of traps for quantum gases and matter-wave guides for atom interferometers. Examples include stacks of pancakes, rows of cigars, and multiple rings or sickles. The traps can be coupled through controllable tunneling barriers or merged altogether. We present analytical expressions for pancake-, cigar-, and ring-shaped traps. The ring geometry is of particular interest for guided matter-wave interferometry as it provides a perfectly smooth waveguide of widely tunable diameter and thus adjustable sensitivity of the interferometer. The flexibility of the TAAP would make possible the use of Bose-Einstein condensates as coherent matter waves in large-area atom interferometers.

  4. Ab initio adiabatic and diabatic potential-energy curves of the LiH molecule

    NASA Astrophysics Data System (ADS)

    Boutalib, A.; Gadéa, F. X.

    1992-07-01

    For nearly all states below the ionic limit [i.e., Li(2s, 2p, 3s, 3p, 3d, 4s, and 4p)+H] we perform the first adiabatic and diabatic studies. This treatment involves a nonempirical pseudopotential for Li and a full configuration-interaction treatment of the valence-electron system. Core-valence correlation is taken into account according to a core-polarization-potential method. We present an analysis of the diabatic curves and introduce appropriate small corrections accounting for basis-set limitations. For the low-lying states, our vibrational level spacings and spectroscopic constants are in excellent agreement with the available experimental data and with the best all-electron results. Experimental suggestions are given for the higher states.

  5. Diffusion of a massive particle in a periodic potential: Application to adiabatic ratchets

    NASA Astrophysics Data System (ADS)

    Rozenbaum, Viktor M.; Makhnovskii, Yurii A.; Shapochkina, Irina V.; Sheu, Sheh-Yi; Yang, Dah-Yen; Lin, Sheng Hsien

    2015-12-01

    We generalize a theory of diffusion of a massive particle by the way in which transport characteristics are described by analytical expressions that formally coincide with those for the overdamped massless case but contain a factor comprising the particle mass which can be calculated in terms of Risken's matrix continued fraction method (MCFM). Using this generalization, we aim to elucidate how large gradients of a periodic potential affect the current in a tilted periodic potential and the average current of adiabatically driven on-off flashing ratchets. For this reason, we perform calculations for a sawtooth potential of the period L with an arbitrary sawtooth length (l potentials typically considered in MCFM-solvable problems. We find nonanalytic behavior of the transport characteristics calculated for the sharp extremely asymmetric sawtooth potential at l →0 which appears due to the inertial effect. Analysis of the temperature dependences of the quantities under study reveals the dominant role of inertia in the high-temperature region. In particular, we show, by the analytical strong-inertia approach developed for this region, that the temperature-dependent contribution to the mobility at zero force and to the related effective diffusion coefficient are proportional to T-3 /2 and T-1 /2, respectively, and have a logarithmic singularity at l →0 .

  6. Diffusion of a massive particle in a periodic potential: Application to adiabatic ratchets.

    PubMed

    Rozenbaum, Viktor M; Makhnovskii, Yurii A; Shapochkina, Irina V; Sheu, Sheh-Yi; Yang, Dah-Yen; Lin, Sheng Hsien

    2015-12-01

    We generalize a theory of diffusion of a massive particle by the way in which transport characteristics are described by analytical expressions that formally coincide with those for the overdamped massless case but contain a factor comprising the particle mass which can be calculated in terms of Risken's matrix continued fraction method (MCFM). Using this generalization, we aim to elucidate how large gradients of a periodic potential affect the current in a tilted periodic potential and the average current of adiabatically driven on-off flashing ratchets. For this reason, we perform calculations for a sawtooth potential of the period L with an arbitrary sawtooth length (lpotentials typically considered in MCFM-solvable problems. We find nonanalytic behavior of the transport characteristics calculated for the sharp extremely asymmetric sawtooth potential at l→0 which appears due to the inertial effect. Analysis of the temperature dependences of the quantities under study reveals the dominant role of inertia in the high-temperature region. In particular, we show, by the analytical strong-inertia approach developed for this region, that the temperature-dependent contribution to the mobility at zero force and to the related effective diffusion coefficient are proportional to T(-3/2) and T(-1/2), respectively, and have a logarithmic singularity at l→0. PMID:26764657

  7. Photoionization of HOCO revisited : a new upper limit to the adiabatic ionization energy and lower limit to the enthalpy of formation.

    SciTech Connect

    Ruscic, B.; Litorja, M.; Chemistry

    2000-01-07

    A new upper limit to the adiabatic ionization energy of trans-hydroxyoxomethyl, EI(t-HOCO){<=}8.195{+-}0.022 eV, is provided, producing a lower limit to the enthalpy of formation, {Delta}H{sub f 0}{sup o}(t-HOCO){>=}-45.8{+-}0.7 kcal/mol ({>=}-46.5{+-}0.7 kcal/mol at 298 K). The spectrum shows progressions in C{double_bond}O and C-O stretches of HOCO{sup +} and provides evidence for the excitation of OCO bend. In addition, the data tentatively suggest an ionization onset as low as 8.06{+-}0.03 eV. While it is not clear whether the latter corresponds to cis or trans isomer, it may indicate that {Delta}H{sub f 0}{sup o}(HOCO) is even higher.

  8. Rotational excitation of H2O by para-H2 from an adiabatically reduced dimensional potential

    NASA Astrophysics Data System (ADS)

    Scribano, Yohann; Faure, Alexandre; Lauvergnat, David

    2012-03-01

    Cross sections and rate coefficients for low lying rotational transitions in H2O colliding with para-hydrogen pH2 are computed using an adiabatic approximation which reduces the dimensional dynamics from a 5D to a 3D problem. Calculations have been performed at the close-coupling level using the recent potential of Valiron et al. [J. Chem. Phys. 129, 134306 (2008), 10.1063/1.2988314]. A good agreement is found between the reduced adiabatic calculations and the 5D exact calculations, with an impressive time saving and memory gain. This adiabatic reduction of dimensionality seems very promising for scattering studies involving the excitation of a heavy target molecule by a light molecular projectile.

  9. Adiabatic corrections to the potential energy curves of the X 1∑ + state of the isotopic lithium hydrides

    NASA Astrophysics Data System (ADS)

    Hadinger, G.; Tergiman, Y. S.

    1986-12-01

    From isotopic spectroscopic data, the internuclear distance dependence of the adiabatic corrections to the potential energy curve has been determined for the ∑ state of a diatomic molecule. Starting from an analytic inversion procedure previously described, the adiabatic corrections can be found in a straightforward way, provided that they can be considered as perturbing terms of the vibration-rotation wave equation. Application to the case of the X 1∑+ state of the lithium hydrides 6LiH, 7LiH, 6LiD, and 7LiD is carried out. The adiabatic corrections ΔUH(R) and ΔULi(R) are obtained and compared with recent results.

  10. Self-consistent calculation of hyperfine fields and adiabatic potential of impurities in iron

    NASA Astrophysics Data System (ADS)

    Kanamori, Junjiro; Akai, Hisazumi; Akai, Masako

    1984-01-01

    Hyperfine fields of impurities of the atomic number Z=1 56 at the substitutional site and those of light impurities of Z=1 9 at the interstitial sites in ferromagnetic iron are calculated by the KKR method adapted to the system containing a single impurity atom. The potential of the impurity atom is determined self-consistently by use of the local spin density functional formalism. The results for nonmagnetic sp valence impurities agree with those of the previous nonself-consistent calculation by Katayama-Yoshida, Terakura and Kanamori except for a few cases, confirming their theory of the systematic variation of hyperfine fields. The calculation for magnetic impurities of transition elements is presented for the first time in this paper. The calculations mentioned so far assume that impurities are situated at the center of each site. For the purpose of discussing the stability of the impurity positions, the change of the adiabatic potential due to displacements from the center is calculated by carrying out similar self-consistent calculations for off-center impurity positions. It is concluded that positive muon and some light impurities including boron will be displaced from the center when trapped in a vacancy.

  11. Measurement of the first ionization potential of astatine by laser ionization spectroscopy

    NASA Astrophysics Data System (ADS)

    Rothe, S.; Andreyev, A. N.; Antalic, S.; Borschevsky, A.; Capponi, L.; Cocolios, T. E.; de Witte, H.; Eliav, E.; Fedorov, D. V.; Fedosseev, V. N.; Fink, D. A.; Fritzsche, S.; Ghys, L.; Huyse, M.; Imai, N.; Kaldor, U.; Kudryavtsev, Yuri; Köster, U.; Lane, J. F. W.; Lassen, J.; Liberati, V.; Lynch, K. M.; Marsh, B. A.; Nishio, K.; Pauwels, D.; Pershina, V.; Popescu, L.; Procter, T. J.; Radulov, D.; Raeder, S.; Rajabali, M. M.; Rapisarda, E.; Rossel, R. E.; Sandhu, K.; Seliverstov, M. D.; Sjödin, A. M.; van den Bergh, P.; van Duppen, P.; Venhart, M.; Wakabayashi, Y.; Wendt, K. D. A.

    2013-05-01

    The radioactive element astatine exists only in trace amounts in nature. Its properties can therefore only be explored by study of the minute quantities of artificially produced isotopes or by performing theoretical calculations. One of the most important properties influencing the chemical behaviour is the energy required to remove one electron from the valence shell, referred to as the ionization potential. Here we use laser spectroscopy to probe the optical spectrum of astatine near the ionization threshold. The observed series of Rydberg states enabled the first determination of the ionization potential of the astatine atom, 9.31751(8) eV. New ab initio calculations are performed to support the experimental result. The measured value serves as a benchmark for quantum chemistry calculations of the properties of astatine as well as for the theoretical prediction of the ionization potential of superheavy element 117, the heaviest homologue of astatine.

  12. Measurement of the first ionization potential of astatine by laser ionization spectroscopy

    PubMed Central

    Rothe, S.; Andreyev, A. N.; Antalic, S.; Borschevsky, A.; Capponi, L.; Cocolios, T. E.; De Witte, H.; Eliav, E.; Fedorov, D. V.; Fedosseev, V. N.; Fink, D. A.; Fritzsche, S.; Ghys, L.; Huyse, M.; Imai, N.; Kaldor, U.; Kudryavtsev, Yuri; Köster, U.; Lane, J. F. W.; Lassen, J.; Liberati, V.; Lynch, K. M.; Marsh, B. A.; Nishio, K.; Pauwels, D.; Pershina, V.; Popescu, L.; Procter, T. J.; Radulov, D.; Raeder, S.; Rajabali, M. M.; Rapisarda, E.; Rossel, R. E.; Sandhu, K.; Seliverstov, M. D.; Sjödin, A. M.; Van den Bergh, P.; Van Duppen, P.; Venhart, M.; Wakabayashi, Y.; Wendt, K. D. A.

    2013-01-01

    The radioactive element astatine exists only in trace amounts in nature. Its properties can therefore only be explored by study of the minute quantities of artificially produced isotopes or by performing theoretical calculations. One of the most important properties influencing the chemical behaviour is the energy required to remove one electron from the valence shell, referred to as the ionization potential. Here we use laser spectroscopy to probe the optical spectrum of astatine near the ionization threshold. The observed series of Rydberg states enabled the first determination of the ionization potential of the astatine atom, 9.31751(8) eV. New ab initio calculations are performed to support the experimental result. The measured value serves as a benchmark for quantum chemistry calculations of the properties of astatine as well as for the theoretical prediction of the ionization potential of superheavy element 117, the heaviest homologue of astatine. PMID:23673620

  13. Measurement of the first ionization potential of astatine by laser ionization spectroscopy.

    PubMed

    Rothe, S; Andreyev, A N; Antalic, S; Borschevsky, A; Capponi, L; Cocolios, T E; De Witte, H; Eliav, E; Fedorov, D V; Fedosseev, V N; Fink, D A; Fritzsche, S; Ghys, L; Huyse, M; Imai, N; Kaldor, U; Kudryavtsev, Yuri; Köster, U; Lane, J F W; Lassen, J; Liberati, V; Lynch, K M; Marsh, B A; Nishio, K; Pauwels, D; Pershina, V; Popescu, L; Procter, T J; Radulov, D; Raeder, S; Rajabali, M M; Rapisarda, E; Rossel, R E; Sandhu, K; Seliverstov, M D; Sjödin, A M; Van den Bergh, P; Van Duppen, P; Venhart, M; Wakabayashi, Y; Wendt, K D A

    2013-01-01

    The radioactive element astatine exists only in trace amounts in nature. Its properties can therefore only be explored by study of the minute quantities of artificially produced isotopes or by performing theoretical calculations. One of the most important properties influencing the chemical behaviour is the energy required to remove one electron from the valence shell, referred to as the ionization potential. Here we use laser spectroscopy to probe the optical spectrum of astatine near the ionization threshold. The observed series of Rydberg states enabled the first determination of the ionization potential of the astatine atom, 9.31751(8) eV. New ab initio calculations are performed to support the experimental result. The measured value serves as a benchmark for quantum chemistry calculations of the properties of astatine as well as for the theoretical prediction of the ionization potential of superheavy element 117, the heaviest homologue of astatine. PMID:23673620

  14. Determination of the first ionization potential of actinium

    NASA Astrophysics Data System (ADS)

    Roßnagel, J.; Raeder, S.; Hakimi, A.; Ferrer, R.; Trautmann, N.; Wendt, K.

    2012-01-01

    Using resonance ionization spectroscopy the first-ionization potential of actinium has been determined by analyzing different Rydberg series in two-color resonant laser excitation. Three individual Rydberg series were investigated, converging toward the ionic ground state and toward the first- and second-excited state of the actinium ion, respectively. A combined analysis of the convergence limits leads to a consistent value for the first-ionization potential of Ac of 43394.45(19)cm-1, equivalent to 5.380226(24) eV.

  15. Ionizing potential waves and high-voltage breakdown streamers.

    NASA Technical Reports Server (NTRS)

    Albright, N. W.; Tidman, D. A.

    1972-01-01

    The structure of ionizing potential waves driven by a strong electric field in a dense gas is discussed. Negative breakdown waves are found to propagate with a velocity proportional to the electric field normal to the wavefront. This causes a curved ionizing potential wavefront to focus down into a filamentary structure, and may provide the reason why breakdown in dense gases propagates in the form of a narrow leader streamer instead of a broad wavefront.

  16. Determination of the first ionization potential of technetium

    SciTech Connect

    Mattolat, C.; Gottwald, T.; Raeder, S.; Rothe, S.; Schwellnus, F.; Wendt, K.; Thoerle-Pospiech, P.; Trautmann, N.

    2010-05-15

    The first ionization potential (IP) of technetium (Tc) has been determined by evaluating Rydberg convergences toward the first ionization potential as well as toward two low-lying excited states of the singly charged Tc ion. The Rydberg states were excited and detected by applying multiphoton resonance ionization mass spectrometry (RIMS) on the long-lived isotope {sup 99g}Tc using a three-color excitation scheme. The observed Rydberg convergences yield a result for the first ionization potential of Tc V{sub IP}(Tc)=7.119380(32) eV. This precise value for V{sub IP}(Tc) is somewhat lower than the so far published data of 7.23 eV or 7.28 eV, dating back to the 1950s.

  17. Molecular wave function and effective adiabatic potentials calculated by extended multi-configuration time-dependent Hartree-Fock method

    NASA Astrophysics Data System (ADS)

    Kato, Tsuyoshi; Ide, Yoshihiro; Yamanouchi, Kaoru

    2015-12-01

    We first calculate the ground-state molecular wave function of 1D model H2 molecule by solving the coupled equations of motion formulated in the extended multi-configuration time-dependent Hartree-Fock (MCTDHF) method by the imaginary time propagation. From the comparisons with the results obtained by the Born-Huang (BH) expansion method as well as with the exact wave function, we observe that the memory size required in the extended MCTDHF method is about two orders of magnitude smaller than in the BH expansion method to achieve the same accuracy for the total energy. Second, in order to provide a theoretical means to understand dynamical behavior of the wave function, we propose to define effective adiabatic potential functions and compare them with the conventional adiabatic electronic potentials, although the notion of the adiabatic potentials is not used in the extended MCTDHF approach. From the comparison, we conclude that by calculating the effective potentials we may be able to predict the energy differences among electronic states even for a time-dependent system, e.g., time-dependent excitation energies, which would be difficult to be estimated within the BH expansion approach.

  18. Molecular wave function and effective adiabatic potentials calculated by extended multi-configuration time-dependent Hartree-Fock method

    SciTech Connect

    Kato, Tsuyoshi; Ide, Yoshihiro; Yamanouchi, Kaoru

    2015-12-31

    We first calculate the ground-state molecular wave function of 1D model H{sub 2} molecule by solving the coupled equations of motion formulated in the extended multi-configuration time-dependent Hartree-Fock (MCTDHF) method by the imaginary time propagation. From the comparisons with the results obtained by the Born-Huang (BH) expansion method as well as with the exact wave function, we observe that the memory size required in the extended MCTDHF method is about two orders of magnitude smaller than in the BH expansion method to achieve the same accuracy for the total energy. Second, in order to provide a theoretical means to understand dynamical behavior of the wave function, we propose to define effective adiabatic potential functions and compare them with the conventional adiabatic electronic potentials, although the notion of the adiabatic potentials is not used in the extended MCTDHF approach. From the comparison, we conclude that by calculating the effective potentials we may be able to predict the energy differences among electronic states even for a time-dependent system, e.g., time-dependent excitation energies, which would be difficult to be estimated within the BH expansion approach.

  19. Slowly changing potential problems in Quantum Mechanics: Adiabatic theorems, ergodic theorems, and scattering

    NASA Astrophysics Data System (ADS)

    Fishman, S.; Soffer, A.

    2016-07-01

    We employ the recently developed multi-time scale averaging method to study the large time behavior of slowly changing (in time) Hamiltonians. We treat some known cases in a new way, such as the Zener problem, and we give another proof of the adiabatic theorem in the gapless case. We prove a new uniform ergodic theorem for slowly changing unitary operators. This theorem is then used to derive the adiabatic theorem, do the scattering theory for such Hamiltonians, and prove some classical propagation estimates and asymptotic completeness.

  20. Representing Adiabatic Potential Energy Surfaces Coupled by Conical Intersections in their Full Dimensionality Using Coupled Quasi-Diabatic States

    NASA Astrophysics Data System (ADS)

    Yarkony, David

    2015-03-01

    The construction of fit single state potential energy surfaces (PESs), analytic representations of ab initio electronic energies and energy gradients, is now well established. These single state PESs, which are essential for accurate quantum dynamics and have found wide application in more approximate quasi-classical treatments, have revolutionized adiabatic dynamics. The situation for nonadiabatic processes involving dissociative and large amplitude motion is less sanguine. In these cases, compared to single electronic state dynamics, both the electronic structure data and the representation are more challenging to determine. We describe the recent development and applications of algorithms that enable description of multiple adiabatic electronic potential energy surfaces coupled by conical intersections in their full dimensionality using coupled quasi-diabatic states. These representations are demonstrably quasi-diabatic, provide accurate representations of conical intersection seams and can smooth out the discontinuities in electronic structure energies due to changing active orbital spaces that routinely afflict global multistate representations.

  1. A Study of H2O2 with Threshold Photoelectron Spectroscopy (TPES) and Electronic Structure Calculations: Redetermination of the First Adiabatic Ionization Energy (AIE).

    PubMed

    Schio, Luca; Alagia, Michele; Dias, Antonio A; Falcinelli, Stefano; Zhaunerchyk, Vitali; Lee, Edmond P F; Mok, Daniel K W; Dyke, John M; Stranges, Stefano

    2016-07-14

    In this work, hydrogen peroxide has been studied with threshold photoelectron (TPE) spectroscopy and photoelectron (PE) spectroscopy. The TPE spectrum has been recorded in the 10.0-21.0 eV ionization energy region, and the PE spectrum has been recorded at 21.22 eV photon energy. Five bands have been observed which have been assigned on the basis of UCCSD(T)-F12/VQZ-F12 and IP-EOM CCSD calculations. Vibrational structure has only been resolved in the TPE spectrum of the first band, associated with the X̃(2)Bg H2O2(+) ← X̃(1)A H2O2 ionization, on its low energy side. This structure is assigned with the help of harmonic Franck-Condon factor calculations that use the UCCSD(T)-F12a/VQZ-F12 computed adiabatic ionization energy (AIE), and UCCSD(T)-F12a/VQZ-F12 computed equilibrium geometric parameters and harmonic vibrational frequencies for the H2O2 X̃(1)A state and the H2O2(+) X̃(2)Bg state. These calculations show that the main vibrational structure on the leading edge of the first TPE band is in the O-O stretching mode (ω3) and the HOOH deformation mode (ω4), and comparison of the simulated spectrum to the experimental spectrum gives the first AIE of H2O2 as (10.685 ± 0.005) eV and ω4 = (850 ± 30) and ω3 = (1340 ± 30) cm(-1) in the X̃(2)Bg state of H2O2(+). Contributions from ionization of vibrationally excited levels in the torsion mode have been identified in the TPE spectrum of the first band and the need for a vibrationally resolved TPE spectrum from vibrationally cooled molecules, as well as higher level Franck-Condon factors than performed in this work, is emphasized. PMID:27045948

  2. Inner-shell and double ionization potentials of aminophenol isomers.

    SciTech Connect

    Kryzhevoi, N. V.; Santra, R.; Cederbaum, L. S.

    2011-01-01

    A comprehensive study of single and double core ionization potentials of the aminophenol molecule is reported. The role of relaxation, correlation, relativistic, and basis set effects in these potentials is clarified. Special attention is paid to the isomer dependence of the single and double core ionization potentials. Some of them are also compared with the respective values of the phenol and aniline molecules. It is shown that the core level single ionization potentials of the para-, meta-, and ortho-aminophenol molecules differ only slightly from each other, rendering these structural isomers challenging to distinguish for conventional x-ray photoelectron spectroscopy. In contrast, the energy needed to remove two core electrons from different atoms depends noticeably on the mutual arrangement and even on the relative orientations of the hydroxyl and amine groups. Together with the electrostatic repulsion between the two core holes, relaxation effects accompanying double core ionization play a crucial role here. The pronounced sensitivity of the double ionization potentials, therefore, enables a spectroscopic characterization of the electronic structure of aminophenol isomers by means of x-ray two-photon photoelectron spectroscopy.

  3. Direct computation of general chemical energy differences: Application to ionization potentials, excitation, and bond energies

    SciTech Connect

    Beste, Ariana; Harrison, Robert J; Yanai, Takeshi

    2006-01-01

    Chemists are mainly interested in energy differences. In contrast, most quantum chemical methods yield the total energy which is a large number compared to the difference and has therefore to be computed to a higher relative precision than would be necessary for the difference alone. Hence, it is desirable to compute energy differences directly, thereby avoiding the precision problem. Whenever it is possible to find a parameter which transforms smoothly from an initial to a final state, the energy difference can be obtained by integrating the energy derivative with respect to that parameter (c.f., thermodynamic integration or adiabatic connection methods). If the dependence on the parameter is predominantly linear, accurate results can be obtained by single-point integration. In density functional theory (DFT) and Hartree-Fock, we applied the formalism to ionization potentials, excitation energies, and chemical bond breaking. Example calculations for ionization potentials and excitation energies showed that accurate results could be obtained with a linear estimate. For breaking bonds, we introduce a non-geometrical parameter which gradually turns the interaction between two fragments of a molecule on. The interaction changes the potentials used to determine the orbitals as well as constraining the orbitals to be orthogonal.

  4. Direct computation of general chemical energy differences: Application to ionization potentials, excitation, and bond energies

    NASA Astrophysics Data System (ADS)

    Beste, A.; Harrison, R. J.; Yanai, T.

    2006-08-01

    Chemists are mainly interested in energy differences. In contrast, most quantum chemical methods yield the total energy which is a large number compared to the difference and has therefore to be computed to a higher relative precision than would be necessary for the difference alone. Hence, it is desirable to compute energy differences directly, thereby avoiding the precision problem. Whenever it is possible to find a parameter which transforms smoothly from an initial to a final state, the energy difference can be obtained by integrating the energy derivative with respect to that parameter (cf. thermodynamic integration or adiabatic connection methods). If the dependence on the parameter is predominantly linear, accurate results can be obtained by single-point integration. In density functional theory and Hartree-Fock, we applied the formalism to ionization potentials, excitation energies, and chemical bond breaking. Example calculations for ionization potentials and excitation energies showed that accurate results could be obtained with a linear estimate. For breaking bonds, we introduce a nongeometrical parameter which gradually turns the interaction between two fragments of a molecule on. The interaction changes the potentials used to determine the orbitals as well as the constraint on the orbitals to be orthogonal.

  5. Ab initio ground and the first excited adiabatic and quasidiabatic potential energy surfaces of H + + CO system

    NASA Astrophysics Data System (ADS)

    George, D. X. F.; Kumar, Sanjay

    2010-08-01

    Ab initio global adiabatic as well as quasidiabatic potential energy surfaces for the ground and the first excited electronic states of the H + + CO system have been computed as a function of the Jacobi coordinates ( R, r, γ) using Dunning's cc-pVTZ basis set at the internally contracted multi-reference (single and double) configuration interaction level of accuracy. In addition, nonadiabatic coupling matrix elements arising from radial motion, mixing angle and coupling potential have been computed using the ab initio procedure [Simah et al. (1999) [66

  6. Determination of Ionization Potential of Calcium by High-Resolution Resonance Ionization Spectroscopy

    NASA Astrophysics Data System (ADS)

    Miyabe, Masabumi; Geppert, Christopher; Kato, Masaaki; Oba, Masaki; Wakaida, Ikuo; Watanabe, Kazuo; Wendt, Klaus D. A.

    2006-03-01

    High-resolution resonance ionization spectroscopy has been utilized to determine a precise ionization potential of Ca. Three-step resonance excitation with single-mode extended-cavity diode lasers populates long and unperturbed Rydberg series of 4snp (1P1) and 4snf (1F3) states in the range of n=20--150. Using an extended Ritz formula for quantum defects, the series convergence limit has been determined to be 49305.9240(20) cm-1 with the accuracy improved one order of magnitude higher than previously reported ones.

  7. Excited-state nuclear forces on adiabatic potential-energy surfaces by time-dependent density-functional theory

    NASA Astrophysics Data System (ADS)

    Haruyama, Jun; Suzuki, Takahiro; Hu, Chunping; Watanabe, Kazuyuki

    2012-01-01

    We present a simple and computationally efficient method to calculate excited-state nuclear forces on adiabatic potential-energy surfaces (APES) from linear-response time-dependent density-functional theory within a real-space framework. The Casida ansatz, which has been validated for computing first-order nonadiabatic couplings in previous studies, was applied to the calculation of the excited-state forces. Our method is validated by the consistency of results in the lower excited states, which reproduce well those obtained by the numerical derivative of each APES. We emphasize the usefulness of this technique by demonstrating the excited-state molecular-dynamics simulation.

  8. Ab initio adiabatic and quasidiabatic potential energy surfaces of lowest four electronic states of the H++O2 system

    NASA Astrophysics Data System (ADS)

    Xavier, F. George D.; Kumar, Sanjay

    2010-10-01

    Ab initio global adiabatic and quasidiabatic potential energy surfaces of lowest four electronic (1-4 A3″) states of the H++O2 system have been computed in the Jacobi coordinates (R,r,γ) using Dunning's cc-pVTZ basis set at the internally contracted multireference (single and double) configuration interaction level of accuracy, which are relevant to the dynamics studies of inelastic vibrational and charge transfer processes observed in the scattering experiments. The computed equilibrium geometry parameters of the bound [HO2]+ ion in the ground electronic state and other parameters for the transition state for the isomerization process, HOO+⇌OOH+ are in good quantitative agreement with those available from the high level ab initio calculations, thus lending credence to the accuracy of the potential energy surfaces. The nonadiabatic couplings between the electronic states have been analyzed in both the adiabatic and quasidiabatic frameworks by computing the nonadiabatic coupling matrix elements and the coupling potentials, respectively. It is inferred that the dynamics of energy transfer processes in the scattering experiments carried out in the range of 9.5-23 eV would involve all the four electronic states.

  9. 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.

  10. Ionization potentials of small lithium clusters (Lin) and hydrogenated lithium clusters (LinH)

    NASA Astrophysics Data System (ADS)

    Wheeler, Steven E.; Schaefer, Henry F.

    2005-05-01

    We present accurate ionization potentials (IPs) for small lithium clusters and hydrogenated lithium clusters (n=1-4), computed using coupled-cluster singles and doubles theory augmented with a perturbative correction for connected triple excitations [CCSD(T)] with the correlation-consistent weighted core-valence quadruple-ζ basis set (cc-pwCVQZ). In some cases the full CCSDT method has been used. Comparison of computed binding energies with experiment for the pure cationic lithium clusters reveals excellent agreement, demonstrating that previous discrepancies between computed and experimentally derived atomization energies for the corresponding neutral clusters are due to the use of an inaccurate experimental IP for Li4. The experimental IP for Li4 falls 0.43eV below our theoretical adiabatic value of 4.74eV, which should be a lower bound to the measured IP. Our recommended zero-point corrected adiabatic IPs for Li, Li2, Li3, Li4, LiH, Li2H, Li3H, and Li4H are 5.39, 5.14, 4.11, 4.74, 7.69, 3.98, 4.69, and 4.05eV, respectively. Zero-point vibrationally corrected CCSD(T) atomization energies per atom for Li2+, Li3+, Li4+, LiH+, Li2H+, Li3H+, and Li4H+ are 0.64, 0.96, 0.90, 0.056, 1.62, 1.40, and 1.40eV, respectively.

  11. Adiabatically driven Brownian pumps.

    PubMed

    Rozenbaum, Viktor M; Makhnovskii, Yurii A; Shapochkina, Irina V; Sheu, Sheh-Yi; Yang, Dah-Yen; Lin, Sheng Hsien

    2013-07-01

    We investigate a Brownian pump which, being powered by a flashing ratchet mechanism, produces net particle transport through a membrane. The extension of the Parrondo's approach developed for reversible Brownian motors [Parrondo, Phys. Rev. E 57, 7297 (1998)] to adiabatically driven pumps is given. We demonstrate that the pumping mechanism becomes especially efficient when the time variation of the potential occurs adiabatically fast or adiabatically slow, in perfect analogy with adiabatically driven Brownian motors which exhibit high efficiency [Rozenbaum et al., Phys. Rev. E 85, 041116 (2012)]. At the same time, the efficiency of the pumping mechanism is shown to be less than that of Brownian motors due to fluctuations of the number of particles in the membrane. PMID:23944411

  12. Theoretical elucidation of conflicting experimental data on vertical ionization potentials of microhydrated thymine.

    PubMed

    Close, David M; Crespo-Hernández, Carlos E; Gorb, Leonid; Leszczynski, Jerzy

    2008-05-15

    In a recent article we reported calculations of the ionization energy thresholds (IET) of microhydrated thymine (Close; et al. J. Phys. Chem. A, 2006, 110, 7485). Calculations showed a distinct effect of microhydration on the IET's of thymine. The first water molecule was seen to decrease the IET by about 0.1 eV, and the second and third water molecules caused a further decrease of less than 0.1 eV each. These changes in IET calculated for the canonical form of thymine with 1-3 waters of hydration are smaller than the experimental values determined by Kim et al. (J. Phys. Chem. C 1996, 100, 7933). In the present study it has been shown that there is considerable reorientation of the water molecules in microhydrated thymine upon ionization. This leads to the expectation that the experimental ionization energies may therefore represent an adiabatic process. The results presented here show that the changes in experimental ionization energies determined by Kim et al. for microhydrated thymine are in good agreement with the calculated adiabatic ionization energies. PMID:18402430

  13. Ionization potential for excited S states of the lithium atom

    SciTech Connect

    Puchalski, M.; KePdziera, D.; Pachucki, K.

    2010-12-15

    Nonrelativistic, relativistic, quantum electrodynamic, and finite nuclear mass corrections to the energy levels are obtained for the nS{sub 1/2},n=3,...,9 states of the lithium atom. Computational approach is based on the explicitly correlated Hylleraas functions with the analytic integration and recursion relations. Theoretical predictions for the ionization potential of nS{sub 1/2} states and transition energies nS{sub 1/2{yields}}2S{sub 1/2} are compared to known experimental values for {sup 6,7}Li isotopes.

  14. Ionization potential depression for non equilibrated aluminum plasmas

    NASA Astrophysics Data System (ADS)

    Calisti, A.; Ferri, S.; Talin, B.

    2015-11-01

    A classical molecular dynamics simulation model, designed to simulate neutral plasmas with various charge states of a given atom together with electrons, is used to investigate the ionization potential depression (IPD) in dense plasmas. The IPD is discussed for aluminum plasma at and out of equilibrium. The simulation results are compared with those of earlier theoretical models and with experimental data obtained in the framework of x-ray free-electron laser experiments. The model proposed in this work appears as an important tool to provide data for further discussion on IPD models.

  15. Nonsequential double ionization of molecules

    SciTech Connect

    Prauzner-Bechcicki, Jakub S.; Sacha, Krzysztof; Zakrzewski, Jakub; Eckhardt, Bruno

    2005-03-01

    Double ionization of diatomic molecules by short linearly polarized laser pulses is analyzed. We consider the final stage of the ionization process, that is the decay of a highly excited two electron molecule, which is formed after rescattering. The saddles of the effective adiabatic potential energy close to which simultaneous escape of electrons takes place are identified. Numerical simulations of the ionization of molecules show that the process can be dominated by either sequential or nonsequential events. In order to increase the ratio of nonsequential to sequential ionizations very short laser pulses should be applied.

  16. Magnetohydrodynamic Turbulence and the First Ionization Potential (FIP) Effect

    NASA Astrophysics Data System (ADS)

    Laming, J. Martin

    2010-05-01

    The FIP Effect is the elemental abundance anomaly observed in the solar corona and slow speed solar wind, whereby elements with First Ionization Potential (FIP) less than about 10 eV (e.g. Mg, Si, Fe) are enhanced in Elements with FIP higher than 10 eV (e.g. C, N, O) are essentially unchanged. This fractionation is assumed to occur in the solar chromosphere, since the low FIP elements are predominantly ionized here, while the high FIP elements are neutral. The abundance enhancement is currently explained by the upward action of the ponderomotive force on chromospheric ions, but not neutrals, as Alfven waves generated in the corona reflect from the steep chromospheric density gradients at each footpoint. The fractionation so produced is almost independent of ion mass as observed, and is stronger for closed coronal loops than for open field lines, also as observed. I will describe some recent results from models of the FIP effect, including the role of slow mode waves generated by the ponderomotive force of coherent Alfven waves in saturating the abundance enhancement. Work supported by NASA Contract NNGH05HL39I, and by basic research funds of the Office of Naval Research.

  17. A plea for a reexamination of ionization potential depression measurements

    NASA Astrophysics Data System (ADS)

    Iglesias, Carlos A.

    2014-09-01

    Experiments at the Linac Coherent Light Source determined the ionization potential depression (IPD) in dense plasmas by measuring the Kα fluorescence associated with K-shell holes created by the X-ray free-electron laser. The analysis of the experimental spectrum found a significantly larger IPD than predicted by the widely used Stewart-Pyatt model. It is shown, however, that a more accurate treatment of atomic levels than used in the analysis has additional channels reducing the threshold laser energy for creating Kα photons without invoking an increase in the IPD. Thus, it is argued that a simulation of the Kα fluorescence using improved atomic data could impact the interpretation of the experimental results.

  18. Assemblage of Superalkali Complexes with Ever Low-Ionization Potentials.

    PubMed

    Paduani, C; Rappe, Andrew M

    2016-08-18

    A simple recipe is proposed for the obtention of new molecules with even lower vertical ionization potential (VIP): to decorate an atom of an electronegative element with superalkali species in number that exceeds its formal valence by one. For instance, density functional theory calculations show that by using the superalkali Li3O cluster (VIP = 3.83 eV) as building blocks decorating the O atom one obtains VIP = 3.33 eV for the Li9O4 cluster, which is lower than the calculated VIP for Cs (3.89 eV) and Li (5.39 eV). This feature is systematic, as confirmed by calculated results on Li-F and Li-S clusters as well. The calculated binding energy per atom of the large-sized species exceeds by far that of LiF (134.7 kcal/mol). PMID:27463269

  19. Imaging cellular membrane potential through ionization of quantum dots

    NASA Astrophysics Data System (ADS)

    Rowland, Clare E.; Susumu, Kimihiro; Stewart, Michael H.; Oh, Eunkeu; Mäkinen, Antti J.; O'Shaughnessy, Thomas J.; Kushto, Gary; Wolak, Mason A.; Erickson, Jeffrey S.; Efros, Alexander L.; Huston, Alan L.; Delehanty, James B.

    2016-03-01

    Recent interest in quantum dots (QDs) stems from the plethora of potential applications that arises from their tunable absorption and emission profiles, high absorption cross sections, resistance to photobleaching, functionalizable surfaces, and physical robustness. The emergent use of QDs in biological imaging exploits these and other intrinsic properties. For example, quantum confined Stark effect (QCSE), which describes changes in the photoluminescence (PL) of QDs driven by the application of an electric field, provides an inherent means of detecting changes in electric fields by monitoring QD emission and thus points to a ready mean of imaging membrane potential (and action potentials) in electrically active cells. Here we examine the changing PL of various QDs subjected to electric fields comparable to those found across a cellular membrane. By pairing static and timeresolved PL measurements, we attempt to understand the mechanism driving electric-field-induced PL quenching and ultimately conclude that ionization plays a substantial role in initiating PL changes in systems where QCSE has traditionally been credited. Expanding on these findings, we explore the rapidity of response of the QD PL to applied electric fields and demonstrate changes amply able to capture the millisecond timescale of cellular action potentials.

  20. The /A 1 Sigma +/ - /X 1 Sigma +/ system of the isotopic lithium hydrides - The molecular constants, potential energy curves, and their adiabatic corrections

    NASA Technical Reports Server (NTRS)

    Vidal, C. R.; Stwalley, W. C.

    1982-01-01

    The molecular constants and their adiabatic corrections have been determined for the (A 1 Sigma +) - (X 1 Sigma +) system of the isotopic lithium hydrides: (Li-6)H, (Li-7)H, (Li-6)D, and (Li-7)D. Using a fully quantum mechanical variational method, the potential energy curves (IPA potentials) are determined. Extending the variational method, we have obtained for the first time adiabatic corrections of potential energy curves from isotopic spectroscopic data. A significant difference between the potential energy curves of the lithium hydrides and the lithium deuterides has been observed. When Li-6 was replaced by Li-7, a significant difference was only observed for the (A 1 Sigma +) state, but not for the (X 1 Sigma +) state.

  1. Topology of the Adiabatic Potential Energy Surfaces for theResonance States of the Water Anion

    SciTech Connect

    Haxton, Daniel J.; Rescigno, Thomas N.; McCurdy, C. William

    2005-04-15

    The potential energy surfaces corresponding to the long-lived fixed-nuclei electron scattering resonances of H{sub 2}O relevant to the dissociative electron attachment process are examined using a combination of ab initio scattering and bound-state calculations. These surfaces have a rich topology, characterized by three main features: a conical intersection between the {sup 2}A{sub 1} and {sup 2}B{sub 2} Feshbach resonance states; charge-transfer behavior in the OH ({sup 2}{Pi}) + H{sup -} asymptote of the {sup 2}B{sub 1} and {sup 2}A{sub 1} resonances; and an inherent double-valuedness of the surface for the {sup 2}B{sub 2} state the C{sub 2v} geometry, arising from a branch-point degeneracy with a {sup 2}B{sub 2} shape resonance. In total, eight individual seams of degeneracy among these resonances are located.

  2. Monte Carlo simulations of ionization potential depression in dense plasmas

    NASA Astrophysics Data System (ADS)

    Stransky, M.

    2016-01-01

    A particle-particle grand canonical Monte Carlo model with Coulomb pair potential interaction was used to simulate modification of ionization potentials by electrostatic microfields. The Barnes-Hut tree algorithm [J. Barnes and P. Hut, Nature 324, 446 (1986)] was used to speed up calculations of electric potential. Atomic levels were approximated to be independent of the microfields as was assumed in the original paper by Ecker and Kröll [Phys. Fluids 6, 62 (1963)]; however, the available levels were limited by the corresponding mean inter-particle distance. The code was tested on hydrogen and dense aluminum plasmas. The amount of depression was up to 50% higher in the Debye-Hückel regime for hydrogen plasmas, in the high density limit, reasonable agreement was found with the Ecker-Kröll model for hydrogen plasmas and with the Stewart-Pyatt model [J. Stewart and K. Pyatt, Jr., Astrophys. J. 144, 1203 (1966)] for aluminum plasmas. Our 3D code is an improvement over the spherically symmetric simplifications of the Ecker-Kröll and Stewart-Pyatt models and is also not limited to high atomic numbers as is the underlying Thomas-Fermi model used in the Stewart-Pyatt model.

  3. Ab initio calculations on the excited states of Na3 cluster to explore beyond Born-Oppenheimer theories: adiabatic to diabatic potential energy surfaces and nuclear dynamics.

    PubMed

    Paul, Amit Kumar; Ray, Somrita; Mukhopadhyay, Debasis; Adhikari, Satrajit

    2011-07-21

    We perform ab initio calculation using quantum chemistry package (MOLPRO) on the excited states of Na(3) cluster and present the adiabatic PESs for the electronic states 2(2)E' and 1(2)A(1)', and the non-adiabatic coupling (NAC) terms among those states. Since the ab initio calculated NAC elements for the states 2(2)E' and 1(2)A(1)' demonstrate the numerical validity of so called "Curl Condition," such states closely form a sub-Hilbert space. For this subspace, we employ the NAC terms to solve the "adiabatic-diabatic transformation (ADT)" equations to obtain the functional form of the transformation angles and pave the way to construct the continuous and single valued diabatic potential energy surface matrix by exploiting the existing first principle based theoretical means on beyond Born-Oppenheimer treatment. Nuclear dynamics has been carried out on those diabatic surfaces to reproduce the experimental spectrum for system B of Na(3) cluster and thereby, to explore the numerical validity of the theoretical development on beyond Born-Oppenheimer approach for adiabatic to diabatic transformation. PMID:21786987

  4. Accurate ionization potential of semiconductors from efficient density functional calculations

    NASA Astrophysics Data System (ADS)

    Ye, Lin-Hui

    2016-07-01

    Despite its huge successes in total-energy-related applications, the Kohn-Sham scheme of density functional theory cannot get reliable single-particle excitation energies for solids. In particular, it has not been able to calculate the ionization potential (IP), one of the most important material parameters, for semiconductors. We illustrate that an approximate exact-exchange optimized effective potential (EXX-OEP), the Becke-Johnson exchange, can be used to largely solve this long-standing problem. For a group of 17 semiconductors, we have obtained the IPs to an accuracy similar to that of the much more sophisticated G W approximation (GWA), with the computational cost of only local-density approximation/generalized gradient approximation. The EXX-OEP, therefore, is likely as useful for solids as for finite systems. For solid surfaces, the asymptotic behavior of the vx c has effects similar to those of finite systems which, when neglected, typically cause the semiconductor IPs to be underestimated. This may partially explain why standard GWA systematically underestimates the IPs and why using the same GWA procedures has not been able to get an accurate IP and band gap at the same time.

  5. Multi-minimum adiabatic potential in the single crystal normal spinel ZnAl(2)O(4), doped by Cu(2+) ions.

    PubMed

    Shapovalov, V A; Zhitlukhina, E S; Lamonova, K V; Shapovalov, V V; Rafailovich, M; Schwarz, S A; Jahoda, R; Reidy, V J; Orel, S M; Pashkevich, Yu G

    2010-06-23

    Spectroscopic investigations of a ZnAl(2)O(4) spinel doped with bivalent copper ions of 0.05% concentration have been carried out in the temperature range 4.2-290 K using a 3 cm(-1) range electron paramagnetic resonance (EPR) spectrometer having an operational frequency f = (9.241 ± 0.001) GHz. The spectrum can be represented as a superposition of two components: a low-temperature (LT) and a high-temperature (HT) one. Redistribution of integrated intensity between HT and LT components of the spectra occurs with temperature change that is typical of systems with multi-minimum adiabatic potential. Spectra observed are explained within the modified theory of crystalline field (MTCF). The electron levels of a Cu(2+) ion placed in an octahedral coordination center with trigonal distortion [CuO(6)](10-) have been calculated. The influence of possible types of oxygen octahedron distortions and possible displacement of copper ions from the symmetry center on the electron spectrum, as well as the shape of the adiabatic potential, has been analyzed. It is shown that in the low-temperature phase the multiple minima of the adiabatic potential occur due to tetragonal distortions while the depth of a minimum is determined by the degree of trigonal octahedron distortions. Tetragonal distortion values and multi-minimum potential barrier heights have been determined. PMID:21393785

  6. Ionization potentials of large sodium doped ammonia clusters.

    PubMed

    Steinbach, C; Buck, U

    2005-04-01

    In a continuous neat supersonic expansion ammonia clusters are generated and doped with sodium atoms in a pickup cell. Thus clusters of the form Na(NH(3))(n) are produced that are photoionized by a tunable dye laser system. The ions are mass analyzed in a reflectron time-of-flight mass spectrometer, and the wavelength dependent ion signals serve for the determination of the ionization potentials (IP) of the different clusters in the size range 10< or =n< or =1500. Aside from a plateau for 10< or =n< or =17 and smaller steps at n=24, 35, and 59 on the average a continuous decrease of the IP with cluster size is observed. The IPs in this size range are linear with (n+1)(-13) and extrapolate to IP(n=infinity)=1.66+/-0.01 eV. The slope is consistent with a dielectric continuum model of the solvated electron and the dielectric constant of the solid. The extrapolated IPs are compared with results obtained for negative ammonia cluster ions and metallic solutions in liquid ammonia. Differences are explained by the presence of counterions and their various distances from the solvated electron. PMID:15847459

  7. Ionization potentials of large sodium doped ammonia clusters

    NASA Astrophysics Data System (ADS)

    Steinbach, C.; Buck, U.

    2005-04-01

    In a continuous neat supersonic expansion ammonia clusters are generated and doped with sodium atoms in a pickup cell. Thus clusters of the form Na(NH3)n are produced that are photoionized by a tunable dye laser system. The ions are mass analyzed in a reflectron time-of-flight mass spectrometer, and the wavelength dependent ion signals serve for the determination of the ionization potentials (IP) of the different clusters in the size range 10⩽n ⩽1500. Aside from a plateau for 10⩽n⩽17 and smaller steps at n =24, 35, and 59 on the average a continuous decrease of the IP with cluster size is observed. The IPs in this size range are linear with (n+1)-1/3 and extrapolate to IP (n=∞)=1.66±0.01eV. The slope is consistent with a dielectric continuum model of the solvated electron and the dielectric constant of the solid. The extrapolated IPs are compared with results obtained for negative ammonia cluster ions and metallic solutions in liquid ammonia. Differences are explained by the presence of counterions and their various distances from the solvated electron.

  8. Strong field ionization rates simulated with time-dependent configuration interaction and an absorbing potential

    SciTech Connect

    Krause, Pascal; Sonk, Jason A.; Schlegel, H. Bernhard

    2014-05-07

    Ionization rates of molecules have been modeled with time-dependent configuration interaction simulations using atom centered basis sets and a complex absorbing potential. The simulations agree with accurate grid-based calculations for the ionization of hydrogen atom as a function of field strength and for charge resonance enhanced ionization of H{sub 2}{sup +} as the bond is elongated. Unlike grid-based methods, the present approach can be applied to simulate electron dynamics and ionization in multi-electron polyatomic molecules. Calculations on HCl{sup +} and HCO{sup +} demonstrate that these systems also show charge resonance enhanced ionization as the bonds are stretched.

  9. Accurate potential energy functions, non-adiabatic and spin-orbit couplings in the ZnH+ system

    NASA Astrophysics Data System (ADS)

    Liang, Guiying; Liu, Xiaoting; Zhang, Xiaomei; Xu, Haifeng; Yan, Bing

    2016-03-01

    A high-level ab initio calculation on the ZnH+ cation has been carried out with the multi-reference configuration interaction method plus Davison correction (MRCI + Q). The scalar relativistic effect is included by using the Douglas-Kroll-Hess (DKH) method. The calculated potential energy curves (PECs) of the 7 Λ-S states are associated with the dissociation limits of Zn+(2Sg) + H(2Sg), Zn(1Sg) + H+(1Sg), and Zn+(2Pu) + H(2Sg), respectively (The Λ-S state is labeled as 2S + 1Λ, in which Λ is the quantum number for the projection along the internuclear axis of the total electronic orbital angular momentum and S is the total electron spin). The spectroscopic constants of the bound states are determined and in good agreement with the available theoretical and experimental results. The permanent dipole moments (PDMs) of Λ-S states and the spin-orbit (SO) matrix elements between Λ-S states are also computed. The results show that the abrupt changes of the PDMs and SO matrix elements come into being for the reason of the avoided crossing between the states with the same symmetry. In addition, the non-adiabatic couplings matrix elements between Λ-S states are also evaluated. Finally, the spin-orbit couplings (SOCs) for the low-lying states are considered with Breit-Pauli operator. The SOC effect makes the 7 Λ-S states of the ZnH+ cation split into 12 Ω states (Ω = Λ + Sz, in which Sz is projection of the total electron spin S along the internuclear Z-axis). For the (3)0+ state, the two energy minima exhibit in the potential, which could be attributed to the formation of the new avoided crossing point. The transition dipole moments (TDMs), Franck-Condon factors, and the radiative lifetimes of the selected transitions (2)0+-X0+, (3)0+-X0+, (2)1-X0+ and (3)1-X0+ have been reported.

  10. Accurate potential energy functions, non-adiabatic and spin-orbit couplings in the ZnH(+) system.

    PubMed

    Liang, Guiying; Liu, Xiaoting; Zhang, Xiaomei; Xu, Haifeng; Yan, Bing

    2016-03-01

    A high-level ab initio calculation on the ZnH(+) cation has been carried out with the multi-reference configuration interaction method plus Davison correction (MRCI+Q). The scalar relativistic effect is included by using the Douglas-Kroll-Hess (DKH) method. The calculated potential energy curves (PECs) of the 7 Λ-S states are associated with the dissociation limits of Zn(+)((2)Sg)+H((2)Sg), Zn((1)Sg)+H(+)((1)Sg), and Zn(+)((2)Pu)+H((2)Sg), respectively (The Λ-S state is labeled as (2S+1)Λ, in which Λ is the quantum number for the projection along the internuclear axis of the total electronic orbital angular momentum and S is the total electron spin). The spectroscopic constants of the bound states are determined and in good agreement with the available theoretical and experimental results. The permanent dipole moments (PDMs) of Λ-S states and the spin-orbit (SO) matrix elements between Λ-S states are also computed. The results show that the abrupt changes of the PDMs and SO matrix elements come into being for the reason of the avoided crossing between the states with the same symmetry. In addition, the non-adiabatic couplings matrix elements between Λ-S states are also evaluated. Finally, the spin-orbit couplings (SOCs) for the low-lying states are considered with Breit-Pauli operator. The SOC effect makes the 7 Λ-S states of the ZnH(+) cation split into 12 Ω states (Ω=Λ+Sz, in which Sz is projection of the total electron spin S along the internuclear Z-axis). For the (3)0(+) state, the two energy minima exhibit in the potential, which could be attributed to the formation of the new avoided crossing point. The transition dipole moments (TDMs), Franck-Condon factors, and the radiative lifetimes of the selected transitions (2)0(+)-X0(+), (3)0(+)-X0(+), (2)1-X0(+) and (3)1-X0(+) have been reported. PMID:26637984

  11. Separation of low first ionization potential ions from high first ionization potential neutrals in the low chromosphere

    NASA Astrophysics Data System (ADS)

    Athay, R. Grant

    1994-03-01

    Spectroscopic data from two flights of the Naval Research Laboratory's High Resolution Telescope and Spectrograph (HRTS) are analyzed for evidence of variations in relative abundances in the low chromosphere. Comparisons of sunspot, active region, and quiet-Sun data from HRTS II reveal decreases of intensities of sunspot lines from the first ionization stages of elements with low first ionization potential relative to both the active region and the quiet Sun. C I lines, however, are more intense in the sunspot than either the active region or the quiet Sun. Within a sunspot in Spacelab II data, the C I line at 156.1 nm is near its average intensity, whereas the Fe II line at 156.3 is much weaker than average. Both spots suggest a relative high value for the C I/Fe II abundance ratio. Within the zone of the same magnetic polarity as the sunspot (leading polarity) in the Spacelab II data, the brightest plages in C I show large C I/Fe II intensity ratios similar to those found in the sunspot. By contrast, the zones of following polarity on either side of the leading polarity show several well-defined areas of unusually low C I/Fe II intensity ratios associated with dark features in C I. The plages within these same zones have near normal or somewhat enhanced values for the C I/Fe II intensity ratios. It is noteworthy, also, that many of the brightest areas in C I do not coincide spatially with the brightest regions in Fe II. Neither do the darkest areas in C I align well with the darkest areas in Fe II. The association of high C I/Fe II intensity ratios with the zone of leading polarity and low-intensity ratios with zones of following polarity suggests that the iron abundance is dependent on the field polarity and is relatively low in the sunspot and the brighter plages in the zone of leading polarity and relatively high in C I dark flocculi in zones of following polarity. Failure of the brightest and darkest features in C I to align with the brightest and darkest

  12. Measurement of the first ionization potential of lawrencium, element 103

    NASA Astrophysics Data System (ADS)

    Sato, T. K.; Asai, M.; Borschevsky, A.; Stora, T.; Sato, N.; Kaneya, Y.; Tsukada, K.; Düllmann, Ch. E.; Eberhardt, K.; Eliav, E.; Ichikawa, S.; Kaldor, U.; Kratz, J. V.; Miyashita, S.; Nagame, Y.; Ooe, K.; Osa, A.; Renisch, D.; Runke, J.; Schädel, M.; Thörle-Pospiech, P.; Toyoshima, A.; Trautmann, N.

    2015-04-01

    The chemical properties of an element are primarily governed by the configuration of electrons in the valence shell. Relativistic effects influence the electronic structure of heavy elements in the sixth row of the periodic table, and these effects increase dramatically in the seventh row--including the actinides--even affecting ground-state configurations. Atomic s and p1/2 orbitals are stabilized by relativistic effects, whereas p3/2, d and f orbitals are destabilized, so that ground-state configurations of heavy elements may differ from those of lighter elements in the same group. The first ionization potential (IP1) is a measure of the energy required to remove one valence electron from a neutral atom, and is an atomic property that reflects the outermost electronic configuration. Precise and accurate experimental determination of IP1 gives information on the binding energy of valence electrons, and also, therefore, on the degree of relativistic stabilization. However, such measurements are hampered by the difficulty in obtaining the heaviest elements on scales of more than one atom at a time. Here we report that the experimentally obtained IP1 of the heaviest actinide, lawrencium (Lr, atomic number 103), is electronvolts. The IP1 of Lr was measured with 256Lr (half-life 27 seconds) using an efficient surface ion-source and a radioisotope detection system coupled to a mass separator. The measured IP1 is in excellent agreement with the value of 4.963(15) electronvolts predicted here by state-of-the-art relativistic calculations. The present work provides a reliable benchmark for theoretical calculations and also opens the way for IP1 measurements of superheavy elements (that is, transactinides) on an atom-at-a-time scale.

  13. Measurement of the first ionization potential of lawrencium, element 103.

    PubMed

    Sato, T K; Asai, M; Borschevsky, A; Stora, T; Sato, N; Kaneya, Y; Tsukada, K; Düllmann, Ch E; Eberhardt, K; Eliav, E; Ichikawa, S; Kaldor, U; Kratz, J V; Miyashita, S; Nagame, Y; Ooe, K; Osa, A; Renisch, D; Runke, J; Schädel, M; Thörle-Pospiech, P; Toyoshima, A; Trautmann, N

    2015-04-01

    The chemical properties of an element are primarily governed by the configuration of electrons in the valence shell. Relativistic effects influence the electronic structure of heavy elements in the sixth row of the periodic table, and these effects increase dramatically in the seventh row--including the actinides--even affecting ground-state configurations. Atomic s and p1/2 orbitals are stabilized by relativistic effects, whereas p3/2, d and f orbitals are destabilized, so that ground-state configurations of heavy elements may differ from those of lighter elements in the same group. The first ionization potential (IP1) is a measure of the energy required to remove one valence electron from a neutral atom, and is an atomic property that reflects the outermost electronic configuration. Precise and accurate experimental determination of IP1 gives information on the binding energy of valence electrons, and also, therefore, on the degree of relativistic stabilization. However, such measurements are hampered by the difficulty in obtaining the heaviest elements on scales of more than one atom at a time. Here we report that the experimentally obtained IP1 of the heaviest actinide, lawrencium (Lr, atomic number 103), is 4.96(+0.08)(-0.07) electronvolts. The IP1 of Lr was measured with (256)Lr (half-life 27 seconds) using an efficient surface ion-source and a radioisotope detection system coupled to a mass separator. The measured IP1 is in excellent agreement with the value of 4.963(15) electronvolts predicted here by state-of-the-art relativistic calculations. The present work provides a reliable benchmark for theoretical calculations and also opens the way for IP1 measurements of superheavy elements (that is, transactinides) on an atom-at-a-time scale. PMID:25855457

  14. Ab initio molecular orbital calculations of DNA radical ions. 5. Scaling of calculated electron affinities and ionization potentials to experimental values

    SciTech Connect

    Sevilla, M.D.; Colson, A.O. ); Besler, B. )

    1995-01-19

    Ab initio molecular orbital calculations of the electron affinities (EAs) and ionization potentials (IPs) of the DNA bases are presented in this work. Comparisons of calculated and experimental values are made for a series of compounds of size and/or structure similar to the DNA bases. Excellent correlations between calculated and experimental values are found for both Koopmans EAs at the 6-31G[sup *] and D95v levels and calculated vertical EAs of the model compounds. Several basis sets are considered: 6-31G[sup *], 6-31+G(d), and D95v. Calculations at 6-31G[sup *] and 6-31+G(d) using both ROHF and ROMP2 theories show a consistent difference between calculated vertical and adiabatic EAs. This allows for a good estimate of DNA base adiabatic EAs. i.e., -0.7, -0.3, 0.2, 0.3, and 0.4 eV; from the vertical EAs -1.23, -0.74, -0.40, -0.32, and -0.19 eV for G, A, C, T, and U respectively. While EAs must be scaled, we find that Koopmans IPs calculated at the simple 3-21G level predict vertical IPs of the DNA bases with only a 0.15 eV average absolute deviation from the experimentally reported values and calculations at MP2/6-31+G(d)//6-31G[sup *] for the adiabatic ionization potentials of the DNA bases are all within 0.1 eV of experiment. 41 refs., 2 figs., 5 tabs.

  15. On the Construction of Diabatic and Adiabatic Potential Energy Surfaces Based on Ab Initio Valence Bond Theory‡

    PubMed Central

    Song, Lingchun; Gao, Jiali

    2009-01-01

    A theoretical model is presented for deriving effective diabatic states based on ab initio self-consistent field valence bond (VBSCF) theory by reducing the multi-configurational VB Hamiltonian into an effective two-state model. We describe two computational approaches for the optimization of the effective diabatic configurations, resulting in two ways of interpreting such effective diabatic states. In the variational diabatic configuration (VDC) method, the energies of the individual diabatic states are variationally minimized. In the consistent diabatic configuration (CDC) method, both the configuration coefficients and orbital coefficients are simultaneously optimized to minimize the adiabatic ground-state energy in VBSCF calculations. In addition, we describe a mixed molecular orbital and valence bond (MOVB) approach to construct the CDC diabatic and adiabatic states for a chemical reaction, whereas the VDC-MOVB method has been described previously. Employing the symmetric SN2 reaction between NH3 and CH3NH3+ as a test system, we found that the results from ab initio VBSCF and from MOVB calculations are in good agreement, suggesting that the computationally efficient MOVB method is a reasonable model for VB simulations of condensed phase reactions. The results indicate that CDC and VDC diabatic states converge, respectively, to covalent and ionic states as the molecular geometries are distorted from the minimum of the respective diabatic state along the reaction coordinate. Furthermore, the resonance energy that stabilizes the energy of crossing between the two diabatic states, resulting in the transition state of the adiabatic ground-state reaction, has a strong dependence on the overlap integral between the two diabatic states and is a function of both the exchange integral and the total diabatic ground-state energy. PMID:18828577

  16. Ab initio adiabatic and quasidiabatic potential energy surfaces of H+ + CO system: A study of the ground and the first three excited electronic states

    NASA Astrophysics Data System (ADS)

    Saheer, V. C.; Kumar, Sanjay

    2016-01-01

    The global ground and first three excited electronic state adiabatic as well as the corresponding quasidiabatic potential energy surfaces is reported as a function of nuclear geometries in the Jacobi coordinates ( R → , r → , γ ) using Dunning's cc-pVTZ basis set at the internally contracted multi-reference (single and double) configuration interaction level of accuracy. Nonadiabatic couplings, arising out of relative motion of proton and the vibrational motion of CO, are also reported in terms of coupling potentials. The quasidiabatic potential energy surfaces and the coupling potentials have been obtained using the ab initio procedure [Simah et al., J. Chem. Phys. 111, 4523 (1999)] for the purpose of dynamics studies.

  17. The ionization potentials of atomic ions in laser-irradiated Ar, Kr and Xe clusters

    NASA Astrophysics Data System (ADS)

    Gets, A. V.; Krainov, V. P.

    2006-04-01

    The ionization potentials of atomic ions in laser-irradiated Ar, Kr and Xe clusters are derived as functions of electron temperature. These potentials decrease significantly compared to the case of the isolated atomic ions because of the screening effect by the atomic ions and electrons inside the cluster. The results can be used for derivations of inner ionization by impact collisions of hot electrons with atomic ions and by the static Coulomb field of the ionized cluster. The broadening of atomic states by the quasistatic Holtsmark field of atomic ions is also considered.

  18. Polycyclic aromatic hydrocarbon reaction rates with peroxy-acid treatment: prediction of reactivity using local ionization potential.

    PubMed

    Shoulder, J M; Alderman, N S; Breneman, C M; Nyman, M C

    2013-08-01

    Property-Encoded Surface Translator (PEST) descriptors were found to be correlated with the degradation rates of polycyclic aromatic hydrocarbons (PAHs) by the peroxy-acid process. Reaction rate constants (k) in hr(-1) for nine PAHs (acenaphthene, anthracene, benzo[a]pyrene, benzo[k]fluoranthene, fluoranthene, fluorene, naphthalene, phenanthrene, and pyrene) were determined by a peroxy-acid treatment method that utilized acetic acid, hydrogen peroxide, and a sulphuric acid catalyst to degrade the polyaromatic structures. Molecular properties of the selected nine PAHs were derived from structures optimized at B3LYP/6-31G(d) and HF/6-31G(d) levels of theory. Properties of adiabatic and vertical ionization potential (IP), highest occupied molecular orbitals (HOMO), HOMO/lowest unoccupied molecular orbital (LUMO) gap energies and HOMO/singly occupied molecular orbital (SOMO) gap energies were not correlated with rates of peroxy-acid reaction. PEST descriptors were calculated from B3LYP/6-31G(d) optimized structures and found to have significant levels of correlation with k. PIP Min described the minimum local IP on the surface of the molecule and was found to be related to k. PEST technology appears to be an accurate method in predicting reactivity and could prove to be a valuable asset in building treatment models and in remediation design for PAHs and other organic contaminants in the environment. PMID:23734862

  19. Two-color multiphoton ionization of diazabicyclooctane in a supersonic free jet

    NASA Astrophysics Data System (ADS)

    Fujii, Masaaki; Ebata, Takayuki; Mikami, Naohiko; Ito, Mitsuo

    1983-11-01

    Two-color multiphoton ionization (MPI) spectroscopy has been applied for diazabicyclooctane (DABCO) in a supersonic free jet. The MPI spectra due to transitions from the various vibronic levels of the S 1 (3s Rydberg) state which were excited by the first laser revealed the high Rydberg states above the adiabatic ionization potential. The ionization process and the vibrational potential of the ion are discussed.

  20. Ionization potentials of cobalt and nickel ions in the local-spin-density approximation

    SciTech Connect

    Dhar, S. ); Kestner, N.R. )

    1990-06-15

    In this article we report on the ionization potentials of all configurations of the Co{sup {ital n}+} and Ni{sup {ital n}+} ions obtained via transition-state calculations using local-spin-density (LSD) potentials. The calculations were performed numerically with and without modifications of the local exchange potential for fractional occupation numbers. When the exchange potential is corrected for noninteger occupation numbers, a more consistent picture of the ionization process is obtained than that given by the LSD Kohn-Sham exchange. The agreement with experimental results is also significantly improved.

  1. Ionization Potential Depression in Hot Dense Plasmas Through a Pure Classical Model

    NASA Astrophysics Data System (ADS)

    Calisti, A.; Ferri, S.; Talin, B.

    2015-05-01

    The ionization potential of an ion embedded in a plasma, lowered due to the whole of the charged particles (ions and electrons) interacting with this ion, is the so-called plasma effect. A numerical plasma model based on classical molecular dynamics has been developed recently. It is capable to describe a neutral plasma at equilibrium involving ions of various charge states of the same atom together with electrons. This code is used here to investigate the ionization potential depression (IPD). The study of the IPD is illustrated and discussed for aluminum plasmas at mid and solid density and electron temperatures varying from 50eV to 190eV. The method relies on a sampling of the total potential energy of the electron located at an ion being ionized. The potential energy of such electron results from all of the interacting charged particles interacting with it.

  2. Radioprotective Potential of Plants and Herbs against the Effects of Ionizing Radiation

    PubMed Central

    C. Jagetia, Ganesh

    2007-01-01

    Ionizing radiations produce deleterious effects in the living organisms and the rapid technological advancement has increased human exposure to ionizing radiations enormously. There is a need to protect humans against such effects of ionizing radiation. Attempts to protect against the deleterious effects of ionizing radiations by pharmacological intervention were made as early as 1949 and efforts are continued to search radioprotectors, which may be of great help for human application. This review mainly dwells on the radioprotective potential of plant and herbal extracts. The results obtained from in vitro and in vivo studies indicate that several botanicals such as Gingko biloba, Centella asiatica, Hippophae rhamnoides, Ocimum sanctum, Panax ginseng, Podophyllum hexandrum, Amaranthus paniculatus, Emblica officinalis, Phyllanthus amarus, Piper longum, Tinospora cordifoila, Mentha arvensis, Mentha piperita, Syzygium cumini, Zingiber officinale, Ageratum conyzoides, Aegle marmelos and Aphanamixis polystachya protect against radiation-induced lethality, lipid peroxidation and DNA damage. The fractionation-guided evaluation may help to develop new radioprotectors of desired activities. PMID:18188408

  3. Laser-induced resonance states as dynamic suppressors of ionization in high-frequency short pulses

    SciTech Connect

    Barash, Danny; Orel, Ann E.; Baer, Roi

    2000-01-01

    An adiabatic-Floquet formalism is used to study the suppression of ionization in short laser pulses. In the high-frequency limit the adiabatic equations involve only the pulse envelope where transitions are purely ramp effects. For a short-ranged potential having a single-bound state we show that ionization suppression is caused by the appearance of a laser-induced resonance state, which is coupled by the pulse ramp to the ground state and acts to trap ionizing flux. (c) 1999 The American Physical Society.

  4. Spectroscopic evidence for the coexistence of tetragonal and trigonal minima within the exited state adiabatic potential energy surfaces of hexachlorotellurate and -selenate complexes

    NASA Astrophysics Data System (ADS)

    Cremers, C.; Degen, J.

    1998-11-01

    Coexistence of Jahn-Teller minima resulting from the coupling to different accepting modes within the adiabatic potential energy surface (APES) is not possible within the framework of linear vibronic coupling theory. For the lowest exited triplet state 3T1u of inorganic complexes with s2 electronic ground-state configuration, such a coexistence, due to quadratic coupling effects, is discussed. As a direct experimental evidence two vibronic progressions with different accepting modes in the emission spectra resulting from a single electronic state are observed in the emission spectra of the title compounds. The observation of vibronic finestructure in the emission spectra of [TeCl6]2- is reported for the first time.

  5. Exact Potential Driving the Electron Dynamics in Enhanced Ionization of H2+

    NASA Astrophysics Data System (ADS)

    Khosravi, Elham; Abedi, Ali; Maitra, Neepa T.

    2015-12-01

    It was recently shown that the exact factorization of the electron-nuclear wave function allows the construction of a Schrödinger equation for the electronic system, in which the potential contains exactly the effect of coupling to the nuclear degrees of freedom and any external fields. Here we study the exact potential acting on the electron in charge-resonance enhanced ionization in a model one-dimensional H2+ molecule. We show there can be significant differences between the exact potential and that used in the traditional quasistatic analyses, arising from nonadiabatic coupling to the nuclear system, and that these are crucial to include for accurate simulations of time-resolved ionization dynamics and predictions of the ionization yield.

  6. Density-functional errors in ionization potential with increasing system size

    NASA Astrophysics Data System (ADS)

    Whittleton, Sarah R.; Sosa Vazquez, Xochitl A.; Isborn, Christine M.; Johnson, Erin R.

    2015-05-01

    This work investigates the effects of molecular size on the accuracy of density-functional ionization potentials for a set of 28 hydrocarbons, including series of alkanes, alkenes, and oligoacenes. As the system size increases, delocalization error introduces a systematic underestimation of the ionization potential, which is rationalized by considering the fractional-charge behavior of the electronic energies. The computation of the ionization potential with many density-functional approximations is not size-extensive due to excessive delocalization of the incipient positive charge. While inclusion of exact exchange reduces the observed errors, system-specific tuning of long-range corrected functionals does not generally improve accuracy. These results emphasize that good performance of a functional for small molecules is not necessarily transferable to larger systems.

  7. Density-functional errors in ionization potential with increasing system size

    SciTech Connect

    Whittleton, Sarah R.; Sosa Vazquez, Xochitl A.; Isborn, Christine M.; Johnson, Erin R.

    2015-05-14

    This work investigates the effects of molecular size on the accuracy of density-functional ionization potentials for a set of 28 hydrocarbons, including series of alkanes, alkenes, and oligoacenes. As the system size increases, delocalization error introduces a systematic underestimation of the ionization potential, which is rationalized by considering the fractional-charge behavior of the electronic energies. The computation of the ionization potential with many density-functional approximations is not size-extensive due to excessive delocalization of the incipient positive charge. While inclusion of exact exchange reduces the observed errors, system-specific tuning of long-range corrected functionals does not generally improve accuracy. These results emphasize that good performance of a functional for small molecules is not necessarily transferable to larger systems.

  8. Determination of the ionization potentials of security-relevant substances with single photon ionization mass spectrometry using synchrotron radiation.

    PubMed

    Schramm, E; Mühlberger, F; Mitschke, S; Reichardt, G; Schulte-Ladbeck, R; Pütz, M; Zimmermann, R

    2008-02-01

    Several ionization potentials (IPs) of security relevant substances were determined with single photon ionization time of flight mass spectrometry (SPI-TOFMS) using monochromatized synchrotron radiation from the "Berliner Elektronenspeicherring-Gesellschaft für Synchrotronstrahlung" (BESSY). In detail, the IPs of nine explosives and related compounds, seven narcotics and narcotics precursors, and one chemical warfare agent (CWA) precursor were determined, whereas six IPs already known from the literature were verified correctly. From seven other substances, including one CWA precursor, the IP could not be determined as the molecule ion peak could not be detected. For these substances the appearance energy (AE) of a main fragment was determined. The analyzed security-relevant substances showed IPs significantly below the IPs of common matrix compounds such as nitrogen and oxygen. Therefore, it is possible to find photon energies in between, whereby the molecules of interest can be detected with SPI in very low concentrations due to the shielding of the matrix. All determined IPs except the one of the explosive EGDN were below 10.5 eV. Hence, laser-generated 118 nm photons can be applied for detecting almost all security-relevant substances by, e.g., SPI-TOFMS. PMID:18284801

  9. The Diagnostic Potential of Transition Region Lines Undergoing Transient Ionization in Dynamic Events

    NASA Astrophysics Data System (ADS)

    Doyle, J. G.; Giunta, A.; Singh, A.; Madjarska, M. S.; Summers, H.; Kellett, B. J.; O'Mullane, M.

    2012-09-01

    We discuss the diagnostic potential of high cadence UV spectral data when transient ionization is considered. For this we use high cadence UV spectra taken during the impulsive phase of a solar flare (observed with instruments on-board the Solar Maximum Mission) which showed excellent correspondence with hard X-ray pulses. The ionization fraction of the transition region ion O v and, in particular, the contribution function for the O v 1371 Å line are computed within the Atomic Data and Analysis Structure, which is a collection of fundamental and derived atomic data and codes to manipulate them. Due to transient ionization, the O v 1371 Å line is enhanced in the first fraction of a second with the peak in the line contribution function occurring initially at a higher electron temperature than in ionization equilibrium. The rise time and enhancement factor depend mostly on the electron density. The fractional increase in the O v 1371 Å emissivity due to transient ionization can reach a factor of two-four and can explain the fast response in the line flux of transition regions ions during the impulsive phase of flares solely as a result of transient ionization. This technique can be used to diagnose the electron temperature and density of solar flares observed with the forthcoming Interface Region Imaging Spectrograph.

  10. Ionization potentials and radii of neutral and ionized species of elements 107 (bohrium) and 108 (hassium) from extended multiconfiguration Dirac-Fock calculations

    NASA Astrophysics Data System (ADS)

    Johnson, E.; Fricke, B.; Jacob, T.; Dong, C. Z.; Fritzsche, S.; Pershina, V.

    2002-02-01

    Large multiconfiguration Dirac-Fock calculations were performed for all neutral and up to 7 and 8 times ionized species of elements 107 and 108, respectively, as well as all the homologous elements Mn, Tc, Re, Fe, Ru, and Os for a number of different total angular momenta. Comparison of the resulting ionization potentials to the known values of the homologues allow an extrapolation and thus a prediction of the chemically important seven or eight ionization potentials of elements 107 or 108 as well as a prediction of some ionic radii.

  11. The adiabatic energy change of plasma electrons and the frame dependence of the cross-shock potential at collisionless magnetosonic shock waves

    NASA Technical Reports Server (NTRS)

    Goodrich, C. C.; Scudder, J. D.

    1984-01-01

    The adiabatic energy gain of electrons in the stationary electric and magnetic field structure of collisionless shock waves was examined analytically in reference to conditions of the earth's bow shock. The study was performed to characterize the behavior of electrons interacting with the cross-shock potential. A normal incidence frame (NIF) was adopted in order to calculate the reversible energy change across a time stationary shock, and comparisons were made with predictions made by the de Hoffman-Teller (HT) model (1950). The electron energy gain, about 20-50 eV, is demonstrated to be consistent with a 200-500 eV potential jump in the bow shock quasi-perpendicular geometry. The electrons lose energy working against the solar wind motional electric field. The reversible energy process is close to that modeled by HT, which predicts that the motional electric field vanishes and the electron energy gain from the electric potential is equated to the ion energy loss to the potential.

  12. Ultrafast ionization and fragmentation of molecular silane

    SciTech Connect

    Sayres, Scott G.; Ross, Matt W.; Castleman, A. W. Jr.

    2010-09-15

    The ionization and fragmentation of molecular silane is examined here with laser intensities ranging between 7x10{sup 12} and 1x10{sup 15} W/cm{sup 2} at 624 nm. The ionization potential of silane determined using both multiphoton ionization (MPI) and tunneling ionization (TI) models agrees with the vertical ionization potential of the molecule. In addition, the application of the tunneling ionization model is extended here to the fragments of silane to determine their appearance potentials. MPI values for SiH{sub 3}{sup +}, SiH{sub 2}{sup +}, SiH{sup +}, Si{sup +}, as well as H{sub 2}{sup +} and H{sup +} are consistent with vertical potentials, whereas the TI measurements are found to be in accord with adiabatic potentials. The tunneling appearance potentials observed for the fragments H{sub 2}{sup +} and H{sup +} are lower than reported for other techniques. In fact, the appearance potential measurements for these species resulting from silane are lower than their ionization potentials. The fragmentation rate of silane is determined to be nearly 20 times larger than the ionization rate. The main precursor for producing amorphous silicon (a-Si:H) thin films, SiH{sub 3}{sup +} is the dominant fragmentation product making up roughly a third of the total ion yield, a substantial increase from other techniques.

  13. Size-dependent error of the density functional theory ionization potential in vacuum and solution

    SciTech Connect

    Sosa Vazquez, Xochitl A.; Isborn, Christine M.

    2015-12-28

    Density functional theory is often the method of choice for modeling the energetics of large molecules and including explicit solvation effects. It is preferable to use a method that treats systems of different sizes and with different amounts of explicit solvent on equal footing. However, recent work suggests that approximate density functional theory has a size-dependent error in the computation of the ionization potential. We here investigate the lack of size-intensivity of the ionization potential computed with approximate density functionals in vacuum and solution. We show that local and semi-local approximations to exchange do not yield a constant ionization potential for an increasing number of identical isolated molecules in vacuum. Instead, as the number of molecules increases, the total energy required to ionize the system decreases. Rather surprisingly, we find that this is still the case in solution, whether using a polarizable continuum model or with explicit solvent that breaks the degeneracy of each solute, and we find that explicit solvent in the calculation can exacerbate the size-dependent delocalization error. We demonstrate that increasing the amount of exact exchange changes the character of the polarization of the solvent molecules; for small amounts of exact exchange the solvent molecules contribute a fraction of their electron density to the ionized electron, but for larger amounts of exact exchange they properly polarize in response to the cationic solute. In vacuum and explicit solvent, the ionization potential can be made size-intensive by optimally tuning a long-range corrected hybrid functional.

  14. Size-dependent error of the density functional theory ionization potential in vacuum and solution

    SciTech Connect

    Sosa Vazquez, Xochitl A.; Isborn, Christine M.

    2015-12-22

    Density functional theory is often the method of choice for modeling the energetics of large molecules and including explicit solvation effects. It is preferable to use a method that treats systems of different sizes and with different amounts of explicit solvent on equal footing. However, recent work suggests that approximate density functional theory has a size-dependent error in the computation of the ionization potential. We here investigate the lack of size-intensivity of the ionization potential computed with approximate density functionals in vacuum and solution. We show that local and semi-local approximations to exchange do not yield a constant ionization potential for an increasing number of identical isolated molecules in vacuum. Instead, as the number of molecules increases, the total energy required to ionize the system decreases. Rather surprisingly, we find that this is still the case in solution, whether using a polarizable continuum model or with explicit solvent that breaks the degeneracy of each solute, and we find that explicit solvent in the calculation can exacerbate the size-dependent delocalization error. We demonstrate that increasing the amount of exact exchange changes the character of the polarization of the solvent molecules; for small amounts of exact exchange the solvent molecules contribute a fraction of their electron density to the ionized electron, but for larger amounts of exact exchange they properly polarize in response to the cationic solute. As a result, in vacuum and explicit solvent, the ionization potential can be made size-intensive by optimally tuning a long-range corrected hybrid functional.

  15. Rydberg levels and ionization potential of francium measured by laser-resonance ionization in a hot cavity

    SciTech Connect

    Andreev, S.V.; Mishin, V.I.; Letokhov, V.S.

    1988-10-01

    A highly sensitive method of detecting atoms in samples has been used for spectral investigations of the rare radioactive element Fr. The method is based on laser-resonance photoionization of Fr atoms in a hot quasi-enclosed cavity. The investigations have been carried out with samples in which short-lived radioactive /sup 221/Fr atoms formed at a rate of approximately 10/sup 3/ atoms/sec. The data obtained, to our knowledge for the first time, on the energies of the high-lying Rydberg levels of the /sup 2/S/sub 1/2/ and /sup 2/D series have made it possible to determine the electron binding energy of the 7p /sup 2/P/sub 3/2/ state and to establish the ionization potential of Fr accurately.

  16. Use of Relativistic Effective Core Potentials in the Calculation of Electron-Impact Ionization Cross Sections

    NASA Technical Reports Server (NTRS)

    Huo, Winifred M.; Kim, Yong-Ki

    1999-01-01

    Based on the Binary-Encounter-Bethe (BEB) model, the advantage of using relativistic effective core potentials (RECP) in the calculation of total ionization cross sections of heavy atoms or molecules containing heavy atoms is discussed. Numerical examples for Ar, Kr, Xe, and WF6 are presented.

  17. Size-dependent error of the density functional theory ionization potential in vacuum and solution

    DOE PAGESBeta

    Sosa Vazquez, Xochitl A.; Isborn, Christine M.

    2015-12-22

    Density functional theory is often the method of choice for modeling the energetics of large molecules and including explicit solvation effects. It is preferable to use a method that treats systems of different sizes and with different amounts of explicit solvent on equal footing. However, recent work suggests that approximate density functional theory has a size-dependent error in the computation of the ionization potential. We here investigate the lack of size-intensivity of the ionization potential computed with approximate density functionals in vacuum and solution. We show that local and semi-local approximations to exchange do not yield a constant ionization potentialmore » for an increasing number of identical isolated molecules in vacuum. Instead, as the number of molecules increases, the total energy required to ionize the system decreases. Rather surprisingly, we find that this is still the case in solution, whether using a polarizable continuum model or with explicit solvent that breaks the degeneracy of each solute, and we find that explicit solvent in the calculation can exacerbate the size-dependent delocalization error. We demonstrate that increasing the amount of exact exchange changes the character of the polarization of the solvent molecules; for small amounts of exact exchange the solvent molecules contribute a fraction of their electron density to the ionized electron, but for larger amounts of exact exchange they properly polarize in response to the cationic solute. As a result, in vacuum and explicit solvent, the ionization potential can be made size-intensive by optimally tuning a long-range corrected hybrid functional.« less

  18. HF echoes from ionization potentially produced by high-altitude discharges

    SciTech Connect

    Roussel-Dupre, R.; Fitzgerald, T.J.; Symbalisty, E.

    1997-04-01

    In this paper the authors report on recent radar measurements taken during the month of October 1994 with the LDG HF radar in the Ivory Coast, Africa as part of the International Equatorial Electrojet Year. The purpose of this experimental effort in part was to study the effects of thunderstorms on the ionosphere. At the same time, the authors decided to carry out a set of experiments of an exploratory nature to look for echoes that could potentially arise from ionization produced in the mesosphere. The two leading candidates for producing transient ionization in the mesosphere are meteors and high-altitude discharges. Each is discussed in the context of these measurements.

  19. POTHMF: A program for computing potential curves and matrix elements of the coupled adiabatic radial equations for a hydrogen-like atom in a homogeneous magnetic field

    NASA Astrophysics Data System (ADS)

    Chuluunbaatar, O.; Gusev, A. A.; Gerdt, V. P.; Rostovtsev, V. A.; Vinitsky, S. I.; Abrashkevich, A. G.; Kaschiev, M. S.; Serov, V. V.

    2008-02-01

    A FORTRAN 77 program is presented which calculates with the relative machine precision potential curves and matrix elements of the coupled adiabatic radial equations for a hydrogen-like atom in a homogeneous magnetic field. The potential curves are eigenvalues corresponding to the angular oblate spheroidal functions that compose adiabatic basis which depends on the radial variable as a parameter. The matrix elements of radial coupling are integrals in angular variables of the following two types: product of angular functions and the first derivative of angular functions in parameter, and product of the first derivatives of angular functions in parameter, respectively. The program calculates also the angular part of the dipole transition matrix elements (in the length form) expressed as integrals in angular variables involving product of a dipole operator and angular functions. Moreover, the program calculates asymptotic regular and irregular matrix solutions of the coupled adiabatic radial equations at the end of interval in radial variable needed for solving a multi-channel scattering problem by the generalized R-matrix method. Potential curves and radial matrix elements computed by the POTHMF program can be used for solving the bound state and multi-channel scattering problems. As a test desk, the program is applied to the calculation of the energy values, a short-range reaction matrix and corresponding wave functions with the help of the KANTBP program. Benchmark calculations for the known photoionization cross-sections are presented. Program summaryProgram title:POTHMF Catalogue identifier:AEAA_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEAA_v1_0.html Program obtainable from:CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions:Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.:8123 No. of bytes in distributed program, including test data

  20. Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography.

    PubMed

    Song, Xiaohong; Lin, Cheng; Sheng, Zhihao; Liu, Peng; Chen, Zhangjin; Yang, Weifeng; Hu, Shilin; Lin, C D; Chen, Jing

    2016-01-01

    Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules. PMID:27329071

  1. Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography

    PubMed Central

    Song, Xiaohong; Lin, Cheng; Sheng, Zhihao; Liu, Peng; Chen, Zhangjin; Yang, Weifeng; Hu, Shilin; Lin, C. D.; Chen, Jing

    2016-01-01

    Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules. PMID:27329071

  2. Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography

    NASA Astrophysics Data System (ADS)

    Song, Xiaohong; Lin, Cheng; Sheng, Zhihao; Liu, Peng; Chen, Zhangjin; Yang, Weifeng; Hu, Shilin; Lin, C. D.; Chen, Jing

    2016-06-01

    Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.

  3. Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography

    DOE PAGESBeta

    Song, Xiaohong; Lin, Cheng; Sheng, Zhihao; Liu, Peng; Chen, Zhangjin; Yang, Weifeng; Hu, Shilin; Lin, C. D.; Chen, Jing

    2016-06-22

    Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. Inmore » addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. Here, we showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.« less

  4. Electron wavepacket dynamics in highly quasi-degenerate coupled electronic states: A theory for chemistry where the notion of adiabatic potential energy surface loses the sense

    NASA Astrophysics Data System (ADS)

    Yonehara, Takehiro; Takatsuka, Kazuo

    2012-12-01

    We develop a theory and the method of its application for chemical dynamics in systems, in which the adiabatic potential energy hyper-surfaces (PES) are densely quasi-degenerate to each other in a wide range of molecular geometry. Such adiabatic electronic states tend to couple each other through strong nonadiabatic interactions. Technically, therefore, it is often extremely hard to accurately single out the individual PES in those systems. Moreover, due to the mutual nonadiabatic couplings that may spread wide in space and due to the energy-time uncertainty relation, the notion of the isolated and well-defined potential energy surface should lose the sense. On the other hand, such dense electronic states should offer a very interesting molecular field in which chemical reactions to proceed in characteristic manners. However, to treat these systems, the standard theoretical framework of chemical reaction dynamics, which starts from the Born-Oppenheimer approximation and ends up with quantum nuclear wavepacket dynamics, is not very useful. We here explore this problem with our developed nonadiabatic electron wavepacket theory, which we call the phase-space averaging and natural branching (PSANB) method [T. Yonehara and K. Takatsuka, J. Chem. Phys. 129, 134109 (2008)], 10.1063/1.2987302, or branching-path representation, in which the packets are propagated in time along the non-Born-Oppenheimer branching paths. In this paper, after outlining the basic theory, we examine using a one-dimensional model how well the PSANB method works with such densely quasi-degenerate nonadiabatic systems. To do so, we compare the performance of PSANB with the full quantum mechanical results and those given by the fewest switches surface hopping (FSSH) method, which is known to be one of the most reliable and flexible methods to date. It turns out that the PSANB electron wavepacket approach actually yields very good results with far fewer initial sampling paths. Then we apply the

  5. Adiabatic potential-energy curves of long-range Rydberg molecules: Two-electron R -matrix approach

    NASA Astrophysics Data System (ADS)

    Tarana, Michal; Čurík, Roman

    2016-01-01

    We introduce a computational method developed for study of long-range molecular Rydberg states of such systems that can be approximated by two electrons in a model potential of the atomic cores. Only diatomic molecules are considered. The method is based on a two-electron R -matrix approach inside a sphere centered on one of the atoms. The wave function is then connected to a Coulomb region outside the sphere via a multichannel version of the Coulomb Green's function. This approach is put into a test by its application to a study of Rydberg states of the hydrogen molecule for internuclear distances R from 20 to 400 bohrs and energies corresponding to n from 3 to 22. The results are compared with previous quantum chemical calculations (lower quantum numbers n ) and computations based on contact-potential models (higher quantum numbers n ).

  6. Boiling point determination using adiabatic Gibbs ensemble Monte Carlo simulations: Application to metals described by embedded-atom potentials

    NASA Astrophysics Data System (ADS)

    Gelb, Lev D.; Chakraborty, Somendra Nath

    2011-12-01

    The normal boiling points are obtained for a series of metals as described by the "quantum-corrected Sutton Chen" (qSC) potentials [S.-N. Luo, T. J. Ahrens, T. Çağın, A. Strachan, W. A. Goddard III, and D. C. Swift, Phys. Rev. B 68, 134206 (2003)]. Instead of conventional Monte Carlo simulations in an isothermal or expanded ensemble, simulations were done in the constant-NPH adabatic variant of the Gibbs ensemble technique as proposed by Kristóf and Liszi [Chem. Phys. Lett. 261, 620 (1996)]. This simulation technique is shown to be a precise tool for direct calculation of boiling temperatures in high-boiling fluids, with results that are almost completely insensitive to system size or other arbitrary parameters as long as the potential truncation is handled correctly. Results obtained were validated using conventional NVT-Gibbs ensemble Monte Carlo simulations. The qSC predictions for boiling temperatures are found to be reasonably accurate, but substantially underestimate the enthalpies of vaporization in all cases. This appears to be largely due to the systematic overestimation of dimer binding energies by this family of potentials, which leads to an unsatisfactory description of the vapor phase.

  7. Boiling point determination using adiabatic Gibbs ensemble Monte Carlo simulations: application to metals described by embedded-atom potentials.

    PubMed

    Gelb, Lev D; Chakraborty, Somendra Nath

    2011-12-14

    The normal boiling points are obtained for a series of metals as described by the "quantum-corrected Sutton Chen" (qSC) potentials [S.-N. Luo, T. J. Ahrens, T. Çağın, A. Strachan, W. A. Goddard III, and D. C. Swift, Phys. Rev. B 68, 134206 (2003)]. Instead of conventional Monte Carlo simulations in an isothermal or expanded ensemble, simulations were done in the constant-NPH adabatic variant of the Gibbs ensemble technique as proposed by Kristóf and Liszi [Chem. Phys. Lett. 261, 620 (1996)]. This simulation technique is shown to be a precise tool for direct calculation of boiling temperatures in high-boiling fluids, with results that are almost completely insensitive to system size or other arbitrary parameters as long as the potential truncation is handled correctly. Results obtained were validated using conventional NVT-Gibbs ensemble Monte Carlo simulations. The qSC predictions for boiling temperatures are found to be reasonably accurate, but substantially underestimate the enthalpies of vaporization in all cases. This appears to be largely due to the systematic overestimation of dimer binding energies by this family of potentials, which leads to an unsatisfactory description of the vapor phase. PMID:22168686

  8. Effect of Coulomb Collisions on the Gravitational Settling of Low and High First Ionization Potential Elements

    NASA Astrophysics Data System (ADS)

    Bø, Iselin M. Th.; Esser, Ruth; Lie-Svendsen, Øystein

    2013-05-01

    We model the effect of gravitational settling in the upper chromosphere on O, Fe, Si, and Ne, studying whether Coulomb collisions between ionized low First Ionization Potential (FIP) elements and protons is sufficient to cause abundance enhancements relative to oxygen. We find that low-FIP abundance enhancements comparable to observed values can be obtained provided the hydrogen ionization degree lies in the approximate range 10%-30%, which agrees with chromospheric models. Lower or higher hydrogen ionization causes the FIP-effect to become smaller or absent (depletion of all heavy elements). Iron must be almost fully ionized in order to become enriched relative to high-FIP elements, and this requires a high iron photoionization rate. The time scale necessary to produce the enrichment increases rapidly with increasing H ionization. For iron in a background from a semiempirical chromospheric model, with an H ion fraction of the order of 30%-40% in the upper chromosphere, 1-2 hr of settling is required to produce enhancements comparable to observations. The absolute abundance (relative to H), which monotonically decreases with time during settling, has by that time decreased by less than 50% in the same altitude region. With the same background conditions, the silicon abundance is more strongly enhanced by the settling than the iron abundance. The high-FIP element neon is depleted, relative to O and low-FIP elements, in the same background and altitude region where iron is enhanced, typically by 50% or more relative to O after 1-2 hr of settling.

  9. EFFECT OF COULOMB COLLISIONS ON THE GRAVITATIONAL SETTLING OF LOW AND HIGH FIRST IONIZATION POTENTIAL ELEMENTS

    SciTech Connect

    Bo, Iselin M. Th.; Esser, Ruth; Lie-Svendsen, Oystein E-mail: ruth.esser@uit.no

    2013-05-20

    We model the effect of gravitational settling in the upper chromosphere on O, Fe, Si, and Ne, studying whether Coulomb collisions between ionized low First Ionization Potential (FIP) elements and protons is sufficient to cause abundance enhancements relative to oxygen. We find that low-FIP abundance enhancements comparable to observed values can be obtained provided the hydrogen ionization degree lies in the approximate range 10%-30%, which agrees with chromospheric models. Lower or higher hydrogen ionization causes the FIP-effect to become smaller or absent (depletion of all heavy elements). Iron must be almost fully ionized in order to become enriched relative to high-FIP elements, and this requires a high iron photoionization rate. The time scale necessary to produce the enrichment increases rapidly with increasing H ionization. For iron in a background from a semiempirical chromospheric model, with an H ion fraction of the order of 30%-40% in the upper chromosphere, 1-2 hr of settling is required to produce enhancements comparable to observations. The absolute abundance (relative to H), which monotonically decreases with time during settling, has by that time decreased by less than 50% in the same altitude region. With the same background conditions, the silicon abundance is more strongly enhanced by the settling than the iron abundance. The high-FIP element neon is depleted, relative to O and low-FIP elements, in the same background and altitude region where iron is enhanced, typically by 50% or more relative to O after 1-2 hr of settling.

  10. Radical ions with nearly degenerate ground state: correlation between the rate of spin-lattice relaxation and the structure of adiabatic potential energy surface.

    PubMed

    Borovkov, V I; Beregovaya, I V; Shchegoleva, L N; Potashov, P A; Bagryansky, V A; Molin, Y N

    2012-09-14

    Paramagnetic spin-lattice relaxation (SLR) in radical cations (RCs) of the cycloalkane series in liquid solution was studied and analyzed from the point of view of the correlation between the relaxation rate and the structure of the adiabatic potential energy surface (PES) of the RCs. SLR rates in the RCs formed in x-ray irradiated n-hexane solutions of the cycloalkanes studied were measured with the method of time-resolved magnetic field effect in the recombination fluorescence of spin-correlated radical ion pairs. Temperature and, for some cycloalkanes, magnetic field dependences of the relaxation rate were determined. It was found that the conventional Redfield theory of the paramagnetic relaxation as applied to the results on cyclohexane RC, gave a value of about 0.2 ps for the correlation time of the perturbation together with an unrealistically high value of 0.1 T in field units for the matrix element of the relaxation transition. The PES structure was obtained with the DFT quantum-chemical calculations. It was found that for all of the cycloalkanes RCs considered, including low symmetric alkyl-substituted ones, the adiabatic PESes were surfaces of pseudorotation due to avoided crossing. In the RCs studied, a correlation between the SLR rate and the calculated barrier height to the pseudorotation was revealed. For RCs with a higher relaxation rate, the apparent activation energies for the SLR were similar to the calculated heights of the barrier. To rationalize the data obtained it was assumed that the vibronic states degeneracy, which is specific for Jahn-Teller active cyclohexane RC, was approximately kept in the RCs of substituted cycloalkanes for the vibronic states with the energies above and close to the barrier height to the pseudorotation. It was proposed that the effective spin-lattice relaxation in a radical with nearly degenerate low-lying vibronic states originated from stochastic crossings of the vibronic levels that occur due to fluctuations of

  11. Non-adiabatic effects within a single thermally averaged potential energy surface: thermal expansion and reaction rates of small molecules.

    PubMed

    Alonso, J L; Castro, A; Clemente-Gallardo, J; Echenique, P; Mazo, J J; Polo, V; Rubio, A; Zueco, D

    2012-12-14

    At non-zero temperature and when a system has low-lying excited electronic states, the ground-state Born-Oppenheimer approximation breaks down and the low-lying electronic states are involved in any chemical process. In this work, we use a temperature-dependent effective potential for the nuclei which can accommodate the influence of an arbitrary number of electronic states in a simple way, while at the same time producing the correct Boltzmann equilibrium distribution for the electronic part. With the help of this effective potential, we show that thermally activated low-lying electronic states can have a significant effect in molecular properties for which electronic excitations are oftentimes ignored. We study the thermal expansion of the Manganese dimer, Mn(2), where we find that the average bond length experiences a change larger than the present experimental accuracy upon the inclusion of the excited states into the picture. We also show that, when these states are taken into account, reaction-rate constants are modified. In particular, we study the opening of the ozone molecule, O(3), and show that in this case the rate is modified as much as a 20% with respect to the ground-state Born-Oppenheimer prediction. PMID:23249070

  12. Adiabatic invariance of oscillons/I -balls

    NASA Astrophysics Data System (ADS)

    Kawasaki, Masahiro; Takahashi, Fuminobu; Takeda, Naoyuki

    2015-11-01

    Real scalar fields are known to fragment into spatially localized and long-lived solitons called oscillons or I -balls. We prove the adiabatic invariance of the oscillons/I -balls for a potential that allows periodic motion even in the presence of non-negligible spatial gradient energy. We show that such a potential is uniquely determined to be the quadratic one with a logarithmic correction, for which the oscillons/I -balls are absolutely stable. For slightly different forms of the scalar potential dominated by the quadratic one, the oscillons/I -balls are only quasistable, because the adiabatic charge is only approximately conserved. We check the conservation of the adiabatic charge of the I -balls in numerical simulation by slowly varying the coefficient of logarithmic corrections. This unambiguously shows that the longevity of oscillons/I -balls is due to the adiabatic invariance.

  13. An improved quasi-diabatic representation of the 1, 2, 3(1)A coupled adiabatic potential energy surfaces of phenol in the full 33 internal coordinates.

    PubMed

    Zhu, Xiaolei; Malbon, Christopher L; Yarkony, David R

    2016-03-28

    In a recent work we constructed a quasi-diabatic representation, H(d), of the 1, 2, 3(1)A adiabatic states of phenol from high level multireference single and double excitation configuration interaction electronic structure data, energies, energy gradients, and derivative couplings. That H(d) accurately describes surface minima, saddle points, and also regions of strong nonadiabatic interactions, reproducing the locus of conical intersection seams and the coordinate dependence of the derivative couplings. The present work determines the accuracy of H(d) for describing phenol photodissociation. Additionally, we demonstrate that a modest energetic shift of two diabats yields a quantifiably more accurate H(d) compared with experimental energetics. The analysis shows that in favorable circumstances it is possible to use single point energies obtained from the most reliable electronic structure methods available, including methods for which the energy gradients and derivative couplings are not available, to improve the quality of a global representation of several coupled potential energy surfaces. Our data suggest an alternative interpretation of kinetic energy release measurements near λphot ∼ 248 nm. PMID:27036453

  14. An improved quasi-diabatic representation of the 1, 2, 31A coupled adiabatic potential energy surfaces of phenol in the full 33 internal coordinates

    NASA Astrophysics Data System (ADS)

    Zhu, Xiaolei; Malbon, Christopher L.; Yarkony, David R.

    2016-03-01

    In a recent work we constructed a quasi-diabatic representation, Hd, of the 1, 2, 31A adiabatic states of phenol from high level multireference single and double excitation configuration interaction electronic structure data, energies, energy gradients, and derivative couplings. That Hd accurately describes surface minima, saddle points, and also regions of strong nonadiabatic interactions, reproducing the locus of conical intersection seams and the coordinate dependence of the derivative couplings. The present work determines the accuracy of Hd for describing phenol photodissociation. Additionally, we demonstrate that a modest energetic shift of two diabats yields a quantifiably more accurate Hd compared with experimental energetics. The analysis shows that in favorable circumstances it is possible to use single point energies obtained from the most reliable electronic structure methods available, including methods for which the energy gradients and derivative couplings are not available, to improve the quality of a global representation of several coupled potential energy surfaces. Our data suggest an alternative interpretation of kinetic energy release measurements near λphot ˜ 248 nm.

  15. Equation of motion coupled cluster methods for electron attachment and ionization potential in polyacenes

    SciTech Connect

    Bhaskaran-Nair, Kiran; Kowalski, Karol; Jarrell, Mark; Moreno, Juana; Shelton, William A.

    2015-11-05

    Polyacenes have attracted considerable attention due to their use in organic based optoelectronic materials. Polyacenes are polycyclic aromatic hydrocarbons composed of fused benzene rings. Key to understanding and design of new functional materials is an understanding of their excited state properties starting with their electron affinity (EA) and ionization potential (IP). We have developed a highly accurate and com- putationally e*fficient EA/IP equation of motion coupled cluster singles and doubles (EA/IP-EOMCCSD) method that is capable of treating large systems and large basis set. In this study we employ the EA/IP-EOMCCSD method to calculate the electron affinity and ionization potential of naphthalene, anthracene, tetracene, pentacene, hex- acene and heptacene. We have compared our results with other previous theoretical studies and experimental data. Our EA/IP results are in very good agreement with experiment and when compared with the other theoretical investigations our results represent the most accurate calculations as compared to experiment.

  16. Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules IV: Electron-Propagator Methods.

    PubMed

    Dolgounitcheva, O; Díaz-Tinoco, Manuel; Zakrzewski, V G; Richard, Ryan M; Marom, Noa; Sherrill, C David; Ortiz, J V

    2016-02-01

    Comparison of ab initio electron-propagator predictions of vertical ionization potentials and electron affinities of organic, acceptor molecules with benchmark calculations based on the basis set-extrapolated, coupled cluster single, double, and perturbative triple substitution method has enabled identification of self-energy approximations with mean, unsigned errors between 0.1 and 0.2 eV. Among the self-energy approximations that neglect off-diagonal elements in the canonical, Hartree-Fock orbital basis, the P3 method for electron affinities, and the P3+ method for ionization potentials provide the best combination of accuracy and computational efficiency. For approximations that consider the full self-energy matrix, the NR2 methods offer the best performance. The P3+ and NR2 methods successfully identify the correct symmetry label of the lowest cationic state in two cases, naphthalenedione and benzoquinone, where some other methods fail. PMID:26730459

  17. The ionization potential of aqueous hydroxide computed using many-body perturbation theory

    SciTech Connect

    Opalka, Daniel Sprik, Michiel; Pham, Tuan Anh; Galli, Giulia

    2014-07-21

    The ionization potentials of electrolyte solutions provide important information about the electronic structure of liquids and solute-solvent interactions. We analyzed the positions of solute and solvent bands of aqueous hydroxide and the influence of the solvent environment on the ionization potential of hydroxide ions. We used the concept of a computational hydrogen electrode to define absolute band positions with respect to vacuum. We found that many-body perturbation theory in the G{sub 0} W{sub 0} approximation substantially improves the relative and absolute positions of the band edges of solute and solvent with respect to those obtained within Density Functional Theory, using semi-local functionals, yielding results in satisfactory agreement with recent experiments.

  18. Multireference configuration interaction calculations of the first six ionization potentials of the uranium atom

    SciTech Connect

    Bross, David H.; Parmar, Payal; Peterson, Kirk A.

    2015-11-14

    The first 6 ionization potentials (IPs) of the uranium atom have been calculated using multireference configuration interaction (MRCI+Q) with extrapolations to the complete basis set limit using new all-electron correlation consistent basis sets. The latter was carried out with the third-order Douglas-Kroll-Hess Hamiltonian. Correlation down through the 5s5p5d electrons has been taken into account, as well as contributions to the IPs due to the Lamb shift. Spin-orbit coupling contributions calculated at the 4-component Kramers restricted configuration interaction level, as well as the Gaunt term computed at the Dirac-Hartree-Fock level, were added to the best scalar relativistic results. The final ionization potentials are expected to be accurate to at least 5 kcal/mol (0.2 eV) and thus more reliable than the current experimental values of IP{sub 3} through IP{sub 6}.

  19. Wireless adiabatic power transfer

    SciTech Connect

    Rangelov, A.A.; Suchowski, H.; Silberberg, Y.; Vitanov, N.V.

    2011-03-15

    Research Highlights: > Efficient and robust mid-range wireless energy transfer between two coils. > The adiabatic energy transfer is analogous to adiabatic passage in quantum optics. > Wireless energy transfer is insensitive to any resonant constraints. > Wireless energy transfer is insensitive to noise in the neighborhood of the coils. - Abstract: We propose a technique for efficient mid-range wireless power transfer between two coils, by adapting the process of adiabatic passage for a coherently driven two-state quantum system to the realm of wireless energy transfer. The proposed technique is shown to be robust to noise, resonant constraints, and other interferences that exist in the neighborhood of the coils.

  20. Increasing the applicability of density functional theory. IV. Consequences of ionization-potential improved exchange-correlation potentials

    SciTech Connect

    Verma, Prakash; Bartlett, Rodney J.

    2014-05-14

    This paper's objective is to create a “consistent” mean-field based Kohn-Sham (KS) density functional theory (DFT) meaning the functional should not only provide good total energy properties, but also the corresponding KS eigenvalues should be accurate approximations to the vertical ionization potentials (VIPs) of the molecule, as the latter condition attests to the viability of the exchange-correlation potential (V{sub XC}). None of the prominently used DFT approaches show these properties: the optimized effective potential V{sub XC} based ab initio dft does. A local, range-separated hybrid potential cam-QTP-00 is introduced as the basis for a “consistent” KS DFT approach. The computed VIPs as the negative of KS eigenvalue have a mean absolute error of 0.8 eV for an extensive set of molecule's electron ionizations, including the core. Barrier heights, equilibrium geometries, and magnetic properties obtained from the potential are in good agreement with experiment. A similar accuracy with less computational efforts can be achieved by using a non-variational global hybrid variant of the QTP-00 approach.

  1. Low-adiabat rugby hohlraum experiments on the National Ignition Facility: Comparison with high-flux modeling and the potential for gas-wall interpenetration

    NASA Astrophysics Data System (ADS)

    Amendt, Peter; Ross, J. Steven; Milovich, Jose L.; Schneider, Marilyn; Storm, Erik; Callahan, Debra A.; Hinkel, Denise; Lasinski, Barbara; Meeker, Don; Michel, Pierre; Moody, John; Strozzi, David

    2014-11-01

    Rugby-shaped gold hohlraums driven by a nominal low-adiabat laser pulse shape have been tested on the National Ignition Facility. The rugby affords a higher coupling efficiency than a comparably sized cylinder hohlraum or, alternatively, improved drive symmetry and laser beam clearances for a larger hohlraum with similar cylinder wall area and laser energy. A first (large rugby hohlraum) shot at low energy (0.75 MJ) to test laser backscatter resulted in a moderately oblate CH capsule implosion, followed by a high energy shot (1.3 MJ) that gave a highly oblate compressed core according to both time-integrated and -resolved x-ray images. These implosions used low wavelength separation (1.0 Å) between the outer and inner cones to provide an alternative platform free of significant cross-beam energy transfer for simplified hohlraum dynamics. Post-shot 2- and 3-D radiation-hydrodynamic simulations using the high-flux model [M. D. Rosen et al., High Energy Density Phys. 7, 180 (2011)], however, give nearly round implosions for both shots, in striking contrast with observations. An analytic assessment of Rayleigh-Taylor hydrodynamic instability growth on the gold-helium gas-fill interface shows the potential for significant linear growth, saturation and transition to a highly nonlinear state. Candidate seeds for instability growth include laser speckle during the early-time laser picket episode in the presence of only partial temporal beam smoothing (1-D smoothing by spectral dispersion and polarization smoothing) and intensity modulations from quad-to-quad and beam overlap. Radiation-hydrodynamic 2-D simulations adapted to include a dynamic fall-line mix model across the unstable Au-He interface show good agreement with the observed implosion symmetry for both shots using an interface-to-fall-line penetration fraction of 100%. Physically, the potential development of an instability layer in a rugby hohlraum is tantamount to an enhanced wall motion leading to hindered

  2. Low-adiabat rugby hohlraum experiments on the National Ignition Facility: Comparison with high-flux modeling and the potential for gas-wall interpenetration

    SciTech Connect

    Amendt, Peter Ross, J. Steven; Milovich, Jose L.; Schneider, Marilyn; Storm, Erik; Callahan, Debra A.; Hinkel, Denise; Lasinski, Barbara; Meeker, Don; Michel, Pierre; Moody, John; Strozzi, David

    2014-11-15

    Rugby-shaped gold hohlraums driven by a nominal low-adiabat laser pulse shape have been tested on the National Ignition Facility. The rugby affords a higher coupling efficiency than a comparably sized cylinder hohlraum or, alternatively, improved drive symmetry and laser beam clearances for a larger hohlraum with similar cylinder wall area and laser energy. A first (large rugby hohlraum) shot at low energy (0.75 MJ) to test laser backscatter resulted in a moderately oblate CH capsule implosion, followed by a high energy shot (1.3 MJ) that gave a highly oblate compressed core according to both time-integrated and –resolved x-ray images. These implosions used low wavelength separation (1.0 Å) between the outer and inner cones to provide an alternative platform free of significant cross-beam energy transfer for simplified hohlraum dynamics. Post-shot 2- and 3-D radiation-hydrodynamic simulations using the high-flux model [M. D. Rosen et al., High Energy Density Phys. 7, 180 (2011)], however, give nearly round implosions for both shots, in striking contrast with observations. An analytic assessment of Rayleigh-Taylor hydrodynamic instability growth on the gold–helium gas-fill interface shows the potential for significant linear growth, saturation and transition to a highly nonlinear state. Candidate seeds for instability growth include laser speckle during the early-time laser picket episode in the presence of only partial temporal beam smoothing (1-D smoothing by spectral dispersion and polarization smoothing) and intensity modulations from quad-to-quad and beam overlap. Radiation-hydrodynamic 2-D simulations adapted to include a dynamic fall-line mix model across the unstable Au-He interface show good agreement with the observed implosion symmetry for both shots using an interface-to-fall-line penetration fraction of 100%. Physically, the potential development of an instability layer in a rugby hohlraum is tantamount to an enhanced wall motion leading to

  3. Potential Energy Curves and Collisions Integrals of Air Components. 2; Interactions Involving Ionized Atoms

    NASA Technical Reports Server (NTRS)

    Stallcop, James R.; Partridge, Harry; Levin, Eugene; Langhoff, Stephen R. (Technical Monitor)

    1995-01-01

    Collision integrals are fundamental quantities required to determine the transport properties of the environment surrounding aerospace vehicles in the upper atmosphere. These collision integrals can be determined as a function of temperature from the potential energy curves describing the atomic and molecular collisions. Ab initio calculations provide a practical method of computing the required interaction potentials. In this work we will discuss recent advances in scattering calculations with an emphasis on the accuracy that is obtainable. Results for interactions of the atoms and ionized atoms of nitrogen and oxygen will be reviewed and their application to the determination of transport properties, such as diffusion and viscosity coefficients, will be examined.

  4. Communication: Physical origins of ionization potential shifts in mixed carboxylic acids and water complexes

    NASA Astrophysics Data System (ADS)

    Gu, Quanli; Tang, Zhen; Su, Peifeng; Wu, Wei; Yang, Zhijun; Trindle, Carl O.; Knee, Joseph L.

    2016-08-01

    The ionization potential (IP) of the aromatic alpha hydroxy carboxylic acid, 9-hydroxy-9-fluorene carboxylic acid (9HFCA), is shifted by complexation with hydrogen bonding ligands such as water and formic acid. Generalized Kohn-Sham energy decomposition analysis decomposes the intermolecular binding energies into a frozen energy term, polarization, correlation, and/or dispersion energy terms, as well as terms of geometric relaxation and zero point energy. We observe that in each dimer the attractive polarization always increases upon ionization, enhancing binding in the cation and shifting the IP toward the red. For 9HFCA—H2O, a substantial decrease of the repulsive frozen energy in cation further shifts the IP toward red. For 9HFCA—HCOOH, the increase of the frozen energy actually occurs in the cation and shifts the IP toward blue. Consistent with the experimental measurements, our analysis provides new, non-intuitive perspectives on multiple hydrogen bonds interactions in carboxylic acids and water complexes.

  5. Parallelizable adiabatic gate teleportation

    NASA Astrophysics Data System (ADS)

    Nakago, Kosuke; Hajdušek, Michal; Nakayama, Shojun; Murao, Mio

    2015-12-01

    To investigate how a temporally ordered gate sequence can be parallelized in adiabatic implementations of quantum computation, we modify adiabatic gate teleportation, a model of quantum computation proposed by Bacon and Flammia [Phys. Rev. Lett. 103, 120504 (2009), 10.1103/PhysRevLett.103.120504], to a form deterministically simulating parallelized gate teleportation, which is achievable only by postselection. We introduce a twisted Heisenberg-type interaction Hamiltonian, a Heisenberg-type spin interaction where the coordinates of the second qubit are twisted according to a unitary gate. We develop parallelizable adiabatic gate teleportation (PAGT) where a sequence of unitary gates is performed in a single step of the adiabatic process. In PAGT, numeric calculations suggest the necessary time for the adiabatic evolution implementing a sequence of L unitary gates increases at most as O (L5) . However, we show that it has the interesting property that it can map the temporal order of gates to the spatial order of interactions specified by the final Hamiltonian. Using this property, we present a controlled-PAGT scheme to manipulate the order of gates by a control qubit. In the controlled-PAGT scheme, two differently ordered sequential unitary gates F G and G F are coherently performed depending on the state of a control qubit by simultaneously applying the twisted Heisenberg-type interaction Hamiltonians implementing unitary gates F and G . We investigate why the twisted Heisenberg-type interaction Hamiltonian allows PAGT. We show that the twisted Heisenberg-type interaction Hamiltonian has an ability to perform a transposed unitary gate by just modifying the space ordering of the final Hamiltonian implementing a unitary gate in adiabatic gate teleportation. The dynamics generated by the time-reversed Hamiltonian represented by the transposed unitary gate enables deterministic simulation of a postselected event of parallelized gate teleportation in adiabatic

  6. Equation of motion coupled cluster methods for electron attachment and ionization potential in polyacenes

    NASA Astrophysics Data System (ADS)

    Bhaskaran-Nair, Kiran; Kowalski, Karol; Jarrell, Mark; Moreno, Juana; Shelton, William A.

    2015-11-01

    Polyacenes have attracted considerable attention due to their various applications in organic optoelectronic materials. This study focuses on linear polyacenes and their electron affinity (EA) and ionization potential (IP) properties. We have employed our recent implementation of EA/IP equation of motion coupled cluster singles and doubles (EA/IP-EOMCCSD) methods which are accurate, computationally efficient and are capable of treating large systems employing reasonable basis sets size. The EA/IP results obtained for naphthalene, anthracene, tetracene, pentacene, hexacene and heptacene are in a good agreement with experiment. Comparison between quality of excitation energies obtained from IP-EOMCCSD and EE-EOMCCSD formalisms were also studied.

  7. Optical potential approach to the electron-atom impact ionization threshold problem

    NASA Technical Reports Server (NTRS)

    Temkin, A.; Hahn, Y.

    1973-01-01

    The problem of the threshold law for electron-atom impact ionization is reconsidered as an extrapolation of inelastic cross sections through the ionization threshold. The cross sections are evaluated from a distorted wave matrix element, the final state of which describes the scattering from the Nth excited state of the target atom. The actual calculation is carried for the e-H system, and a model is introduced which is shown to preserve the essential properties of the problem while at the same time reducing the dimensionability of the Schrodinger equation. Nevertheless, the scattering equation is still very complex. It is dominated by the optical potential which is expanded in terms of eigen-spectrum of QHQ. It is shown by actual calculation that the lower eigenvalues of this spectrum descend below the relevant inelastic thresholds; it follows rigorously that the optical potential contains repulsive terms. Analytical solutions of the final state wave function are obtained with several approximations of the optical potential.

  8. Potential human study populations for non-ionizing (radio frequency) radiation health effects

    SciTech Connect

    Novotney, L.C.; Gravitis, I.

    1982-12-01

    This research project was initiated to identify potential human populations for future epidemiological studies of the health effects of radio frequency radiation. Through a literature search and contacts with various groups and organizations, numerous occupations and applications of radio frequency radiation (RFR) were identified and evaluated for their suitability for further study. Many populations were eliminated early because their potential exposure to RFR was too limited or data necessary for epidemiological research were unavailable. Eight populations were evaluated in detail and appear to satisfy many of the criteria for epidemiological research and could be useful study groups in an investigation of the health effects of non-ionizing radiation. The eight potential study populations are: RF heat sealer operators, HF (high frequency) tube welder operators, medical diathermy operators in Veterans Administration hospitals, medical diathermy operators in rehabilitation facilities, school children located near broadcasting towers, state policemen, security guards, and radar technicians.

  9. Accurate Kohn-Sham ionization potentials from scaled-opposite-spin second-order optimized effective potential methods.

    PubMed

    Śmiga, Szymon; Della Sala, Fabio; Buksztel, Adam; Grabowski, Ireneusz; Fabiano, Eduardo

    2016-08-15

    One important property of Kohn-Sham (KS) density functional theory is the exact equality of the energy of the highest occupied KS orbital (HOMO) with the negative ionization potential of the system. This exact feature is out of reach for standard density-dependent semilocal functionals. Conversely, accurate results can be obtained using orbital-dependent functionals in the optimized effective potential (OEP) approach. In this article, we investigate the performance, in this context, of some advanced OEP methods, with special emphasis on the recently proposed scaled-opposite-spin OEP functional. Moreover, we analyze the impact of the so-called HOMO condition on the final quality of the HOMO energy. Results are compared to reference data obtained at the CCSD(T) level of theory. © 2016 Wiley Periodicals, Inc. PMID:27357413

  10. Numerical adiabatic potentials of orthorhombic Jahn-Teller effects retrieved from ultrasound attenuation experiments. Application to the SrF2:Cr crystal

    NASA Astrophysics Data System (ADS)

    Zhevstovskikh, I. V.; Bersuker, I. B.; Gudkov, V. V.; Averkiev, N. S.; Sarychev, M. N.; Zherlitsyn, S.; Yasin, S.; Shakurov, G. S.; Ulanov, V. A.; Surikov, V. T.

    2016-06-01

    A methodology is worked out to retrieve the numerical values of all the main parameters of the six-dimensional adiabatic potential energy surface (APES) of a polyatomic system with a quadratic T-term Jahn-Teller effect (JTE) from the ultrasound experiments. The method is based on a verified assumption that ultrasound attenuation and speed encounter anomalies when the direction of propagation and polarization of its wave of strain coincides with the characteristic directions of symmetry breaking in the JTE. For the SrF2:Cr crystal, employed as a basic example, we observed anomaly peaks in the temperature dependence of attenuation of ultrasound at frequencies of 50-160 MHz in the temperature interval of 40-60 K for the wave propagating along the [110] direction, for both the longitudinal and the shear modes, the latter with two polarizations along the [001] and [1 1 ¯ 0 ] axes, respectively. We show that these anomalies are due to the ultrasound relaxation by the system of non-interacting Cr2+ JT centers with orthorhombic local distortions. The interpretation of the experimental findings is based on the T2 g⊗(eg+t2 g) JTE problem including the linear and the quadratic terms of vibronic interactions in the Hamiltonian and the same-symmetry modes reduced to one interaction mode. Combining the experimental results with a theoretical analysis, we show that on the complicated six-dimensional APES of this system with three tetragonal, four trigonal, and six orthorhombic extrema points, the latter are global minima, while the former are saddle points, and we estimate numerically all the main parameters of this surface, including the linear and quadratic vibronic coupling constants, the primary force constants, the coordinates of all the extrema points and their energies, the energy barrier between the orthorhombic minima, and the tunneling splitting of the ground vibrational states. To our knowledge, such a based-on-experimental-data numerical reconstruction of the APES

  11. Adiabatic cooling of antiprotons.

    PubMed

    Gabrielse, G; Kolthammer, W S; McConnell, R; Richerme, P; Kalra, R; Novitski, E; Grzonka, D; Oelert, W; Sefzick, T; Zielinski, M; Fitzakerley, D; George, M C; Hessels, E A; Storry, C H; Weel, M; Müllers, A; Walz, J

    2011-02-18

    Adiabatic cooling is shown to be a simple and effective method to cool many charged particles in a trap to very low temperatures. Up to 3×10(6) p are cooled to 3.5 K-10(3) times more cold p and a 3 times lower p temperature than previously reported. A second cooling method cools p plasmas via the synchrotron radiation of embedded e(-) (with many fewer e(-) than p in preparation for adiabatic cooling. No p are lost during either process-a significant advantage for rare particles. PMID:21405511

  12. Adiabatic Cooling of Antiprotons

    SciTech Connect

    Gabrielse, G.; Kolthammer, W. S.; McConnell, R.; Richerme, P.; Kalra, R.; Novitski, E.; Oelert, W.; Grzonka, D.; Sefzick, T.; Zielinski, M.; Fitzakerley, D.; George, M. C.; Hessels, E. A.; Storry, C. H.; Weel, M.; Muellers, A.; Walz, J.

    2011-02-18

    Adiabatic cooling is shown to be a simple and effective method to cool many charged particles in a trap to very low temperatures. Up to 3x10{sup 6} p are cooled to 3.5 K--10{sup 3} times more cold p and a 3 times lower p temperature than previously reported. A second cooling method cools p plasmas via the synchrotron radiation of embedded e{sup -} (with many fewer e{sup -} than p) in preparation for adiabatic cooling. No p are lost during either process--a significant advantage for rare particles.

  13. A hierarchy of local coupled cluster singles and doubles response methods for ionization potentials

    NASA Astrophysics Data System (ADS)

    Wälz, Gero; Usvyat, Denis; Korona, Tatiana; Schütz, Martin

    2016-02-01

    We present a hierarchy of local coupled cluster (CC) linear response (LR) methods to calculate ionization potentials (IPs), i.e., excited states with one electron annihilated relative to a ground state reference. The time-dependent perturbation operator V(t), as well as the operators related to the first-order (with respect to V(t)) amplitudes and multipliers, thus are not number conserving and have half-integer particle rank m. Apart from calculating IPs of neutral molecules, the method offers also the possibility to study ground and excited states of neutral radicals as ionized states of closed-shell anions. It turns out that for comparable accuracy IPs require a higher-order treatment than excitation energies; an IP-CC LR method corresponding to CC2 LR or the algebraic diagrammatic construction scheme through second order performs rather poorly. We therefore systematically extended the order with respect to the fluctuation potential of the IP-CC2 LR Jacobian up to IP-CCSD LR, keeping the excitation space of the first-order (with respect to V(t)) cluster operator restricted to the m = /1 2 ⊕ /3 2 subspace and the accuracy of the zero-order (ground-state) amplitudes at the level of CC2 or MP2. For the more expensive diagrams beyond the IP-CC2 LR Jacobian, we employ local approximations. The implemented methods are capable of treating large molecular systems with hundred atoms or more.

  14. Multireference configuration interaction calculations of the first six ionization potentials of the uranium atom

    SciTech Connect

    Bross, David H.; Parmar, Payal; Peterson, Kirk A.

    2015-11-12

    The first 6 ionization potentials (IPs) of the uranium atom have been calculated using multireference configuration interaction (MRCI+Q) with extrapolations to the complete basis set (CBS) limit using new all-electron correlation consistent basis sets. The latter were carried out with the third-order Douglas-Kroll-Hess Hamiltonian. Correlation down through the 5s5p5d electrons have been taken into account, as well as contributions to the IPs due to the Lamb shift. Spin-orbit coupling contributions calculated at the 4-component Kramers restricted configuration interaction level, as well as the Gaunt term computed at the Dirac-Hartree-Fock level, were added to the best scalar relativistic results. As a result, the final ionization potentials are expected to be accurate to at least 5 kcal/mol (0.2 eV), and thus more reliable than the current experimental values of IP3 through IP6.

  15. Multireference configuration interaction calculations of the first six ionization potentials of the uranium atom

    DOE PAGESBeta

    Bross, David H.; Parmar, Payal; Peterson, Kirk A.

    2015-11-12

    The first 6 ionization potentials (IPs) of the uranium atom have been calculated using multireference configuration interaction (MRCI+Q) with extrapolations to the complete basis set (CBS) limit using new all-electron correlation consistent basis sets. The latter were carried out with the third-order Douglas-Kroll-Hess Hamiltonian. Correlation down through the 5s5p5d electrons have been taken into account, as well as contributions to the IPs due to the Lamb shift. Spin-orbit coupling contributions calculated at the 4-component Kramers restricted configuration interaction level, as well as the Gaunt term computed at the Dirac-Hartree-Fock level, were added to the best scalar relativistic results. As amore » result, the final ionization potentials are expected to be accurate to at least 5 kcal/mol (0.2 eV), and thus more reliable than the current experimental values of IP3 through IP6.« less

  16. Preventive or Potential Therapeutic Value of Nutraceuticals against Ionizing Radiation-Induced Oxidative Stress in Exposed Subjects and Frequent Fliers

    PubMed Central

    Giardi, Maria Teresa; Touloupakis, Eleftherios; Bertolotto, Delfina; Mascetti, Gabriele

    2013-01-01

    Humans are constantly exposed to ionizing radiation deriving from outer space sources or activities related to medical care. Absorption of ionizing radiation doses over a prolonged period of time can result in oxidative damage and cellular dysfunction inducing several diseases, especially in ageing subjects. In this report, we analyze the effects of ionizing radiation, particularly at low doses, in relation to a variety of human pathologies, including cancer, and cardiovascular and retinal diseases. We discuss scientific data in support of protection strategies by safe antioxidant formulations that can provide preventive or potential therapeutic value in response to long-term diseases that may develop following exposure. PMID:23965979

  17. Adiabatically implementing quantum gates

    SciTech Connect

    Sun, Jie; Lu, Songfeng Liu, Fang

    2014-06-14

    We show that, through the approach of quantum adiabatic evolution, all of the usual quantum gates can be implemented efficiently, yielding running time of order O(1). This may be considered as a useful alternative to the standard quantum computing approach, which involves quantum gates transforming quantum states during the computing process.

  18. Entanglement and adiabatic quantum computation

    NASA Astrophysics Data System (ADS)

    Ahrensmeier, D.

    2006-06-01

    Adiabatic quantum computation provides an alternative approach to quantum computation using a time-dependent Hamiltonian. The time evolution of entanglement during the adiabatic quantum search algorithm is studied, and its relevance as a resource is discussed.

  19. High-field plasma acceleration in a high-ionization-potential gas

    NASA Astrophysics Data System (ADS)

    Corde, S.; Adli, E.; Allen, J. M.; An, W.; Clarke, C. I.; Clausse, B.; Clayton, C. E.; Delahaye, J. P.; Frederico, J.; Gessner, S.; Green, S. Z.; Hogan, M. J.; Joshi, C.; Litos, M.; Lu, W.; Marsh, K. A.; Mori, W. B.; Vafaei-Najafabadi, N.; Walz, D.; Yakimenko, V.

    2016-06-01

    Plasma accelerators driven by particle beams are a very promising future accelerator technology as they can sustain high accelerating fields over long distances with high energy efficiency. They rely on the excitation of a plasma wave in the wake of a drive beam. To generate the plasma, a neutral gas can be field-ionized by the head of the drive beam, in which case the distance of acceleration and energy gain can be strongly limited by head erosion. Here we overcome this limit and demonstrate that electrons in the tail of a drive beam can be accelerated by up to 27 GeV in a high-ionization-potential gas (argon), boosting their initial 20.35 GeV energy by 130%. Particle-in-cell simulations show that the argon plasma is sustaining very high electric fields, of ~150 GV m-1, over ~20 cm. The results open new possibilities for the design of particle beam drivers and plasma sources.

  20. High-field plasma acceleration in a high-ionization-potential gas

    PubMed Central

    Corde, S.; Adli, E.; Allen, J. M.; An, W.; Clarke, C. I.; Clausse, B.; Clayton, C. E.; Delahaye, J. P.; Frederico, J.; Gessner, S.; Green, S. Z.; Hogan, M. J.; Joshi, C.; Litos, M.; Lu, W.; Marsh, K. A.; Mori, W. B.; Vafaei-Najafabadi, N.; Walz, D.; Yakimenko, V.

    2016-01-01

    Plasma accelerators driven by particle beams are a very promising future accelerator technology as they can sustain high accelerating fields over long distances with high energy efficiency. They rely on the excitation of a plasma wave in the wake of a drive beam. To generate the plasma, a neutral gas can be field-ionized by the head of the drive beam, in which case the distance of acceleration and energy gain can be strongly limited by head erosion. Here we overcome this limit and demonstrate that electrons in the tail of a drive beam can be accelerated by up to 27 GeV in a high-ionization-potential gas (argon), boosting their initial 20.35 GeV energy by 130%. Particle-in-cell simulations show that the argon plasma is sustaining very high electric fields, of ∼150 GV m−1, over ∼20 cm. The results open new possibilities for the design of particle beam drivers and plasma sources. PMID:27312720

  1. High-field plasma acceleration in a high-ionization-potential gas.

    PubMed

    Corde, S; Adli, E; Allen, J M; An, W; Clarke, C I; Clausse, B; Clayton, C E; Delahaye, J P; Frederico, J; Gessner, S; Green, S Z; Hogan, M J; Joshi, C; Litos, M; Lu, W; Marsh, K A; Mori, W B; Vafaei-Najafabadi, N; Walz, D; Yakimenko, V

    2016-01-01

    Plasma accelerators driven by particle beams are a very promising future accelerator technology as they can sustain high accelerating fields over long distances with high energy efficiency. They rely on the excitation of a plasma wave in the wake of a drive beam. To generate the plasma, a neutral gas can be field-ionized by the head of the drive beam, in which case the distance of acceleration and energy gain can be strongly limited by head erosion. Here we overcome this limit and demonstrate that electrons in the tail of a drive beam can be accelerated by up to 27 GeV in a high-ionization-potential gas (argon), boosting their initial 20.35 GeV energy by 130%. Particle-in-cell simulations show that the argon plasma is sustaining very high electric fields, of ∼150 GV m(-1), over ∼20 cm. The results open new possibilities for the design of particle beam drivers and plasma sources. PMID:27312720

  2. High-field plasma acceleration in a high-ionization-potential gas

    DOE PAGESBeta

    Corde, S.; Adli, E.; Allen, J. M.; An, W.; Clarke, C. I.; Clausse, B.; Clayton, C. E.; Delahaye, J. P.; Frederico, J.; Gessner, S.; et al

    2016-06-17

    Plasma accelerators driven by particle beams are a very promising future accelerator technology as they can sustain high accelerating fields over long distances with high energy efficiency. They rely on the excitation of a plasma wave in the wake of a drive beam. To generate the plasma, a neutral gas can be field-ionized by the head of the drive beam, in which case the distance of acceleration and energy gain can be strongly limited by head erosion. In our research, we overcome this limit and demonstrate that electrons in the tail of a drive beam can be accelerated by upmore » to 27 GeV in a high-ionization-potential gas (argon), boosting their initial 20.35 GeV energy by 130%. Particle-in-cell simulations show that the argon plasma is sustaining very high electric fields, of ~150 GV m-1, over ~20 cm. Lastly, the results open new possibilities for the design of particle beam drivers and plasma sources.« less

  3. Stellar coronal abundances. 3: The solar first ionization potential effect determined from full-disk observation

    NASA Technical Reports Server (NTRS)

    Laming, J. Martin; Drake, J. J.; Widing, Kenneth G.

    1995-01-01

    In this paper we reanalayze the full-disk quiet-sun spectrum of Mallinovsky & Heroux (1973) with modern atomic data. The purposes of this are to check our atomic data and methods in other investigations using data from nearby stars obtained with the NASA Extreme Ultraviolet Explorer (EUVE) satellite, and to confirm that the solar first ionization potential (FIP) effect investigated by previous authors studying discrete solar regions is the same as that found in full-disk spectra. We recover the usual solar FIP effect of a coronal abundance enhancement of elements with a low FIP of a factor approximately 3-4 for lines formed at temperatures greater than approximately 10(exp 6) K. For lower temperatures, the FIP effect seems to be substantially smaller, in qualitative agreement with other data. Comparing our full-disk result with those from discrete solar structures suggest that the FIP effect is a function of altitude, with the lower temperature full-disk emission being dominated by the super-granulation network. We also compare the recent ionization balance of Arnaud & Raymond (1992) with that of Arnaud & Rothenflug (1985).

  4. Communication: Physical origins of ionization potential shifts in mixed carboxylic acids and water complexes.

    PubMed

    Gu, Quanli; Tang, Zhen; Su, Peifeng; Wu, Wei; Yang, Zhijun; Trindle, Carl O; Knee, Joseph L

    2016-08-01

    The ionization potential (IP) of the aromatic alpha hydroxy carboxylic acid, 9-hydroxy-9-fluorene carboxylic acid (9HFCA), is shifted by complexation with hydrogen bonding ligands such as water and formic acid. Generalized Kohn-Sham energy decomposition analysis decomposes the intermolecular binding energies into a frozen energy term, polarization, correlation, and/or dispersion energy terms, as well as terms of geometric relaxation and zero point energy. We observe that in each dimer the attractive polarization always increases upon ionization, enhancing binding in the cation and shifting the IP toward the red. For 9HFCA-H2O, a substantial decrease of the repulsive frozen energy in cation further shifts the IP toward red. For 9HFCA-HCOOH, the increase of the frozen energy actually occurs in the cation and shifts the IP toward blue. Consistent with the experimental measurements, our analysis provides new, non-intuitive perspectives on multiple hydrogen bonds interactions in carboxylic acids and water complexes. PMID:27497532

  5. NON-WKB MODELS OF THE FIRST IONIZATION POTENTIAL EFFECT: THE ROLE OF SLOW MODE WAVES

    SciTech Connect

    Laming, J. Martin

    2012-01-10

    A model for element abundance fractionation between the solar chromosphere and corona is further developed. The ponderomotive force due to Alfven waves propagating through or reflecting from the chromosphere in solar conditions generally accelerates chromospheric ions, but not neutrals, into the corona. This gives rise to what has become known as the first ionization potential effect. We incorporate new physical processes into the model. The chromospheric ionization balance is improved and the effect of different approximations is discussed. We also treat the parametric generation of slow mode waves by the parallel propagating Alfven waves. This is also an effect of the ponderomotive force, arising from the periodic variation of the magnetic pressure driving an acoustic mode, which adds to the background longitudinal pressure. This can have subtle effects on the fractionation, rendering it quasi-mass independent in the lower regions of the chromosphere. We also briefly discuss the change in the fractionation with Alfven wave frequency, relative to the frequency of the overlying coronal loop resonance.

  6. The computation of ionization potentials for second-row elements by ab initio and density functional theory methods

    SciTech Connect

    Jursic, B.S.

    1996-12-31

    Up to four ionization potentials of elements from the second-row of the periodic table were computed using the ab initio (HF, MP2, MP3, MP4, QCISD, GI, G2, and G2MP2) and DFT (B3LY, B3P86, B3PW91, XALPHA, HFS, HFB, BLYP, BP86, BPW91, BVWN, XAPLY, XAP86, XAPW91, XAVWN, SLYR SP86, SPW91 and SVWN) methods. In all of the calculations, the large 6-311++G(3df,3pd) gaussian type of basis set was used. The computed values were compared with the experimental results and suitability of the ab initio and DFF methods were discussed, in regard to reproducing the experimental data. From the computed ionization potentials of the second-row elements, it can be concluded that the HF ab initio computation is not capable of reproducing the experimental results. The computed ionization potentials are too low. However, by using the ab initio methods that include electron correlation, the computed IPs are becoming much closer to the experimental values. In all cases, with the exception of the first ionization potential for oxygen, the G2 computation result produces ionization potentials that are indistinguishable from the experimental results.

  7. Ionization potential of {sup 9}Be calculated including nuclear motion and relativistic corrections

    SciTech Connect

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

    2007-05-15

    Variational calculations employing explicitly correlated Gaussian functions have been performed for the ground states of {sup 9}Be and {sup 9}Be{sup +} including the nuclear motion [i.e., without assuming the Born-Oppenheimer (BO) approximation]. An approach based on the analytical energy gradient calculated with respect to the Gaussian exponential parameters was employed, leading to energies of the two systems noticeably improved over those found in the recent paper of Pachucki and Komasa [Phys. Rev. A 73, 052502 (2006)]. The non-BO wave functions were used to calculate the {alpha}{sup 2} relativistic corrections ({alpha}=e{sup 2}/({Dirac_h}/2{pi})c). With those corrections and the {alpha}{sup 3} and {alpha}{sup 4} corrections taken from Pachucki and Komasa, a new value of the ionization potential (IP) of {sup 9}Be was determined. It agrees very well with the most recent experimental IP.

  8. Ab initio calculation of ionization potential and electron affinity in solid-state organic semiconductors

    NASA Astrophysics Data System (ADS)

    Kang, Youngho; Jeon, Sang Ho; Cho, Youngmi; Han, Seungwu

    2016-01-01

    We investigate the vertical ionization potential (IP) and electron affinity (EA) of organic semiconductors in the solid state that govern the optoelectrical property of organic devices using a fully ab initio way. The present method combines the density functional theory and many-body perturbation theory based on G W approximations. To demonstrate the accuracy of this approach, we carry out calculations on several prototypical organic molecules. Since IP and EA depend on the molecular orientation at the surface, the molecular geometry of the surface is explicitly considered through the slab model. The computed IP and EA are in reasonable and consistent agreements with spectroscopic data on organic surfaces with various molecular arrangements. However, the transport gaps are slightly underestimated in calculations, which can be explained by different screening effects between surface and bulk regions.

  9. Role of the ionization potential in nonequilibrium metals driven to absorption saturation

    NASA Astrophysics Data System (ADS)

    Mincigrucci, R.; Bencivenga, F.; Capotondi, F.; Principi, E.; Giangrisostomi, E.; Battistoni, A.; Caputo, M.; Casolari, F.; Gessini, A.; Manfredda, M.; Pedersoli, E.; Masciovecchio, C.

    2015-07-01

    A composite metallic foil (Al/Mg/Al) has been exposed to intense sub-100 fs free electron laser (FEL) pulses and driven to ultrafast massive photoionization. The resulting nonequilibrium state of matter has been monitored through absorption spectroscopy across the L2 ,3 edge of Mg as a function of the FEL fluence. The raw spectroscopic data indicate that at about 100 J /cm2 the main absorption channels of the sample, i.e., Mg (2 p →free ) and oxidized Al (valence→free ), are almost saturated. The spectral behavior of the induced transparency has been interpreted with an analytical approach based on an effective ionization potential of the generated solid-density plasma.

  10. Solar radiation pressure as a mechanism of acceleration of atoms and first ions with low ionization potentials

    NASA Astrophysics Data System (ADS)

    Shestakova, L. I.

    2015-04-01

    Calculated results are presented for solar radiation pressure acting on atoms and first ions. For some of these particles, radiation pressure exceeds the gravitational attraction and can accelerate them to large velocities. A comparison of the results with ionization potentials shows that the maxima of radiation pressure on neutral atoms coincide with the minima of the first ionization potentials (FIPs). This relationship is even more apparent for first ions. The minima of the second ionization potentials (SIPs) coincide with the radiation pressure maxima for a number of ions such as Be II, Mg II, Ca II, and the neighboring elements. Thus, radiation pressure may serve as a possible mechanism of acceleration of pickup ions and energetic neutral atoms (ENA) coming from an inner source (zodiacal dust and sungrazing comets). These atoms and ions, which are not typical of the solar wind, are formed as a result of the disintegration of comets or meteor showers near the Sun and can accelerate and reach the Earth's orbit as part of the solar wind. Doubly ionized atoms have resonance lines in the UV range, where solar radiation pressure has no apparent impact on the particle dynamics; thus, the proposed acceleration mechanism can only be applied to neutral atoms and first ions with low potentials of the subsequent ionization.

  11. Adiabatic topological quantum computing

    NASA Astrophysics Data System (ADS)

    Cesare, Chris; Landahl, Andrew J.; Bacon, Dave; Flammia, Steven T.; Neels, Alice

    2015-07-01

    Topological quantum computing promises error-resistant quantum computation without active error correction. However, there is a worry that during the process of executing quantum gates by braiding anyons around each other, extra anyonic excitations will be created that will disorder the encoded quantum information. Here, we explore this question in detail by studying adiabatic code deformations on Hamiltonians based on topological codes, notably Kitaev's surface codes and the more recently discovered color codes. We develop protocols that enable universal quantum computing by adiabatic evolution in a way that keeps the energy gap of the system constant with respect to the computation size and introduces only simple local Hamiltonian interactions. This allows one to perform holonomic quantum computing with these topological quantum computing systems. The tools we develop allow one to go beyond numerical simulations and understand these processes analytically.

  12. Accurate adiabatic correction in the hydrogen molecule

    SciTech Connect

    Pachucki, Krzysztof; Komasa, Jacek

    2014-12-14

    A new formalism for the accurate treatment of adiabatic effects in the hydrogen molecule is presented, in which the electronic wave function is expanded in the James-Coolidge basis functions. Systematic increase in the size of the basis set permits estimation of the accuracy. Numerical results for the adiabatic correction to the Born-Oppenheimer interaction energy reveal a relative precision of 10{sup −12} at an arbitrary internuclear distance. Such calculations have been performed for 88 internuclear distances in the range of 0 < R ⩽ 12 bohrs to construct the adiabatic correction potential and to solve the nuclear Schrödinger equation. Finally, the adiabatic correction to the dissociation energies of all rovibrational levels in H{sub 2}, HD, HT, D{sub 2}, DT, and T{sub 2} has been determined. For the ground state of H{sub 2} the estimated precision is 3 × 10{sup −7} cm{sup −1}, which is almost three orders of magnitude higher than that of the best previous result. The achieved accuracy removes the adiabatic contribution from the overall error budget of the present day theoretical predictions for the rovibrational levels.

  13. Accurate adiabatic correction in the hydrogen molecule

    NASA Astrophysics Data System (ADS)

    Pachucki, Krzysztof; Komasa, Jacek

    2014-12-01

    A new formalism for the accurate treatment of adiabatic effects in the hydrogen molecule is presented, in which the electronic wave function is expanded in the James-Coolidge basis functions. Systematic increase in the size of the basis set permits estimation of the accuracy. Numerical results for the adiabatic correction to the Born-Oppenheimer interaction energy reveal a relative precision of 10-12 at an arbitrary internuclear distance. Such calculations have been performed for 88 internuclear distances in the range of 0 < R ⩽ 12 bohrs to construct the adiabatic correction potential and to solve the nuclear Schrödinger equation. Finally, the adiabatic correction to the dissociation energies of all rovibrational levels in H2, HD, HT, D2, DT, and T2 has been determined. For the ground state of H2 the estimated precision is 3 × 10-7 cm-1, which is almost three orders of magnitude higher than that of the best previous result. The achieved accuracy removes the adiabatic contribution from the overall error budget of the present day theoretical predictions for the rovibrational levels.

  14. Anomalous abundances of solar energetic particles and coronal gas: Coulomb effects and First Ionization Potential (FIP) ordering

    NASA Technical Reports Server (NTRS)

    Mullan, D. J.

    1985-01-01

    The first ionization potential (FIP) ordering of elemental abundances in solar energetic particles and in the corona which can both be explained Coulomb effects is discussed. Solar energetic particles (SEP) and coronal gas have anomalous abundances relative to the photosphere. The anomalies are similar in both cases: which led to the conclusion that SEP acceleration is not selective, but merely preserves the source abundances. It is argued that SEP acceleration can be selective, because identical selectivity operates to determine the coronal abundances. The abundance anomalies are ordered by first ionization potential (FIP).

  15. Drifting potential humps in ionization zones: The “propeller blades” of high power impulse magnetron sputtering

    SciTech Connect

    Anders, André; Ni, Pavel; Panjan, Matjaž; Franz, Robert; Andersson, Joakim

    2013-09-30

    Ion energy distribution functions measured for high power impulse magnetron sputtering show features, such as a broad peak at several 10 eV with an extended tail, as well as asymmetry with respect to E×B, where E and B are the local electric and magnetic field vectors, respectively. Here it is proposed that those features are due to the formation of a potential hump of several 10 V in each of the traveling ionization zones. Potential hump formation is associated with a negative-positive-negative space charge that naturally forms in ionization zones driven by energetic drifting electrons.

  16. Three-step resonant photoionization spectroscopy of Ni and Ge: ionization potential and odd-parity Rydberg levels

    NASA Astrophysics Data System (ADS)

    Kessler, T.; Brück, K.; Baktash, C.; Beene, J. R.; Geppert, Ch; Havener, C. C.; Krause, H. F.; Liu, Y.; Schultz, D. R.; Stracener, D. W.; Vane, C. R.; Wendt, K.

    2007-12-01

    In preparation of a laser ion source, we have investigated multi-step laser ionization via Rydberg and autoionizing states for atomic Ni and Ge using a mass separator with an ion beam energy of 20 keV. For both elements resonant three-step excitation schemes suitable for modern Ti:sapphire laser systems were developed. Rydberg series in the range of principal quantum numbers 20 <= n <= 80 were localized, assigned and quantum numbers were allocated to the individual resonances. Ionization potentials (IP) were extracted from fits of the individual series and quantum defects of individual levels were analysed for confirmation of series assignment. For Ni the ionization potential could be extracted with significantly increased precision compared to literature with a value of EIP (Ni) = 61 619.77(14) cm-1. Also, at least one notable autoionizing state above the first IP was discovered for both elements, and the different ionization schemes via Rydberg or autoionizing states were compared with respect to line shape, ionization efficiency and selectivity.

  17. Vertical Ionization Potentials of Nucleobases in a Fully Solvated DNA Environment

    SciTech Connect

    Cauet, Emilie L.; Valiev, Marat; Weare, John H.

    2010-05-06

    Calculations of the direct ionization potentials (DIP) of DNA nucleobases in the fully solvated DNA helix are reported. The results show an unexpected large shift of roughly 3.2-3.3 eV compared to the corresponding gas-phase IP values. The DIP shift is nearly the same for all the four DNA bases and appears to vary slowly with the stacking and H-bonding interactions of the nucleobases. We demonstrate that the large shift in the DIP of bases is due to the electric potential around the DNA resulting from the long range solvent structure created by the negative phosphate groups and positive counterions of the DNA helical structure. Thermal fluctuations in the fluid can result in DIP changes of roughly 1ev on a picosecond time scale. The model used in this work is based on a QM/MM approach in which the base (or clusters of bases) are chosen as the QM system and calculated using a high-level quantum chemistry method. The remaining DNA fragment and the species in solution are included in an exact molecular mechanics (MM) model. The expected high accuracy of the QM/MM model is defended in terms of the essentially Columbic nature of the interactions of the solvent (the MM region) with isolated base in the quantum region. For the test anion, Cl-, the QM/MM approach yields the 3.4 eV (gas-phase) to 9.3 eV (aqueous solution) shift of the ionization energy in agreement with experimental values (3.6 and 9.6 eV). The localization of the electronic excitation inside the QM region is supported by current experimental and theoretical evidence indicating that the HOMO of the nucleotide is localized on the base rather than the sugar or the phosphate backbone. Our calculations performed in the native DNA environment support this localization. The QM/MM model presented in this work provides an important simplification to the difficult problem of incorporating a detailed structural model of the physiological conditions into investigations of the electronic processes in DNA.

  18. Methemoglobinemia hemotoxicity of some antimalarial 8-aminoquinoline analogues and their hydroxylated derivatives: density functional theory computation of ionization potentials

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The administration of primaquine (PQ), an essential drug for treatment and radical cure of malaria, can lead to methemoglobin formation and life-threatening hemolysis for glucose-6-phosphate dehydrogenase deficient patients. The ionization potential (IP, a quantitative measure of the ability to lose...

  19. Adiabatic Halo Formation

    SciTech Connect

    Bazzani, A.; Turchetti, G.; Benedetti, C.; Rambaldi, S.; Servizi, G.

    2005-06-08

    In a high intensity circular accelerator the synchrotron dynamics introduces a slow modulation in the betatronic tune due to the space-charge tune depression. When the transverse motion is non-linear due to the presence of multipolar effects, resonance islands move in the phase space and change their amplitude. This effect introduces the trapping and detrapping phenomenon and a slow diffusion in the phase space. We apply the neo-adiabatic theory to describe this diffusion mechanism that can contribute to halo formation.

  20. Effects of dust-charge fluctuations on the potential of an array of projectiles in a partially ionized dusty plasma

    NASA Astrophysics Data System (ADS)

    Ali, S.; Nasim, M. H.; Murtaza, G.

    2003-11-01

    The expressions for the Debye and the wake potential are derived by incorporating dust-charge fluctuations of a single projectile, as well as of an array of dust grain projectiles, propagating through a partially ionized dusty plasma with a constant velocity. Numerically, the effects of the dust-charge fluctuations and the dust-neutral collisions on the electrostatic potential for a single, three, six and ten projectiles are examined. The dust-charge relaxation rate modifies the shape of the Debye as well as the wake potential. For smaller values of the relaxation rates a potential well is formed instead of Debye potential.

  1. Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules III: A Benchmark of GW Methods.

    PubMed

    Knight, Joseph W; Wang, Xiaopeng; Gallandi, Lukas; Dolgounitcheva, Olga; Ren, Xinguo; Ortiz, J Vincent; Rinke, Patrick; Körzdörfer, Thomas; Marom, Noa

    2016-02-01

    The performance of different GW methods is assessed for a set of 24 organic acceptors. Errors are evaluated with respect to coupled cluster singles, doubles, and perturbative triples [CCSD(T)] reference data for the vertical ionization potentials (IPs) and electron affinities (EAs), extrapolated to the complete basis set limit. Additional comparisons are made to experimental data, where available. We consider fully self-consistent GW (scGW), partial self-consistency in the Green's function (scGW0), non-self-consistent G0W0 based on several mean-field starting points, and a "beyond GW" second-order screened exchange (SOSEX) correction to G0W0. We also describe the implementation of the self-consistent Coulomb hole with screened exchange method (COHSEX), which serves as one of the mean-field starting points. The best performers overall are G0W0+SOSEX and G0W0 based on an IP-tuned long-range corrected hybrid functional with the former being more accurate for EAs and the latter for IPs. Both provide a balanced treatment of localized vs delocalized states and valence spectra in good agreement with photoemission spectroscopy (PES) experiments. PMID:26731609

  2. Quantum-Mechanical Calculation of Ionization-Potential Lowering in Dense Plasmas

    NASA Astrophysics Data System (ADS)

    Son, Sang-Kil; Thiele, Robert; Jurek, Zoltan; Ziaja, Beata; Santra, Robin

    2014-07-01

    The charged environment within a dense plasma leads to the phenomenon of ionization-potential depression (IPD) for ions embedded in the plasma. Accurate predictions of the IPD effect are of crucial importance for modeling atomic processes occurring within dense plasmas. Several theoretical models have been developed to describe the IPD effect, with frequently discrepant predictions. Only recently, first experiments on IPD in Al plasma have been performed with an x-ray free-electron laser, where their results were found to be in disagreement with the widely used IPD model by Stewart and Pyatt. Another experiment on Al, at the Orion laser, showed disagreement with the model by Ecker and Kröll. This controversy shows a strong need for a rigorous and consistent theoretical approach to calculate the IPD effect. Here, we propose such an approach: a two-step Hartree-Fock-Slater model. With this parameter-free model, we can accurately and efficiently describe the experimental Al data and validate the accuracy of standard IPD models. Our model can be a useful tool for calculating atomic properties within dense plasmas with wide-ranging applications to studies on warm dense matter, shock experiments, planetary science, inertial confinement fusion, and nonequilibrium plasmas created with x-ray free-electron lasers.

  3. Density functional theory study on the ionization potentials and electron affinities of thymine-formamide complexes

    NASA Astrophysics Data System (ADS)

    Sun, Haitao; Tang, Ke; Li, Yanmin; Su, Chunfang; Zhou, Zhengyu; Wang, Zhizhong

    The effect of hydrogen bond interactions on ionization potentials (IPs) and electron affinities (EAs) of thymine-formamide complexes (T-F) have been investigated employing the density functional theory B3LYP at 6-311++G(d, p) basis set level. All complexes experience a geometrical change on either electron detachment or attachment, and the change might be facilitated or hindered according to the strength of the hydrogen-bonding interaction involved. The strength of hydrogen bonds presents an opposite changing trend on the two processes. A more important role that H-bonding interaction plays in the process of electron attachment than in the process of electron detachment can be seen by a comparison of the IPs and EAs of complexes with that of isolated thymine. Futhermore, the EAs of isolated thymine are in good agreement with the experimental values (AEA is 0.79 eV, VEA is -0.29 eV [Wetmore et al., Chem Phys Lett 2000, 322, 129]). The calculated total NPA charge distributions reveal that nearly all the negative charges locate on thymine monomer in the anions and even in the cationic states, there are a few negative charges on thymine monomer. An analysis of dissociation energies predicts the processes T-F+→ T++ F and T-F- → T- + F to be the most energetically favorable for T-F+ and T-F-, respectively. Content:text/plain; charset="UTF-8"

  4. An integrated programming and development environment for adiabatic quantum optimization

    NASA Astrophysics Data System (ADS)

    Humble, T. S.; McCaskey, A. J.; Bennink, R. S.; Billings, J. J.; DʼAzevedo, E. F.; Sullivan, B. D.; Klymko, C. F.; Seddiqi, H.

    2014-01-01

    Adiabatic quantum computing is a promising route to the computational power afforded by quantum information processing. The recent availability of adiabatic hardware has raised challenging questions about how to evaluate adiabatic quantum optimization (AQO) programs. Processor behavior depends on multiple steps to synthesize an adiabatic quantum program, which are each highly tunable. We present an integrated programming and development environment for AQO called Jade Adiabatic Development Environment (JADE) that provides control over all the steps taken during program synthesis. JADE captures the workflow needed to rigorously specify the AQO algorithm while allowing a variety of problem types, programming techniques, and processor configurations. We have also integrated JADE with a quantum simulation engine that enables program profiling using numerical calculation. The computational engine supports plug-ins for simulation methodologies tailored to various metrics and computing resources. We present the design, integration, and deployment of JADE and discuss its potential use for benchmarking AQO programs by the quantum computer science community.

  5. Adiabatic Quantum Computing

    NASA Astrophysics Data System (ADS)

    Landahl, Andrew

    2012-10-01

    Quantum computers promise to exploit counterintuitive quantum physics principles like superposition, entanglement, and uncertainty to solve problems using fundamentally fewer steps than any conventional computer ever could. The mere possibility of such a device has sharpened our understanding of quantum coherent information, just as lasers did for our understanding of coherent light. The chief obstacle to developing quantum computer technology is decoherence--one of the fastest phenomena in all of physics. In principle, decoherence can be overcome by using clever entangled redundancies in a process called fault-tolerant quantum error correction. However, the quality and scale of technology required to realize this solution appears distant. An exciting alternative is a proposal called ``adiabatic'' quantum computing (AQC), in which adiabatic quantum physics keeps the computer in its lowest-energy configuration throughout its operation, rendering it immune to many decoherence sources. The Adiabatic Quantum Architectures In Ultracold Systems (AQUARIUS) Grand Challenge Project at Sandia seeks to demonstrate this robustness in the laboratory and point a path forward for future hardware development. We are building devices in AQUARIUS that realize the AQC architecture on up to three quantum bits (``qubits'') in two platforms: Cs atoms laser-cooled to below 5 microkelvin and Si quantum dots cryo-cooled to below 100 millikelvin. We are also expanding theoretical frontiers by developing methods for scalable universal AQC in these platforms. We have successfully demonstrated operational qubits in both platforms and have even run modest one-qubit calculations using our Cs device. In the course of reaching our primary proof-of-principle demonstrations, we have developed multiple spinoff technologies including nanofabricated diffractive optical elements that define optical-tweezer trap arrays and atomic-scale Si lithography commensurate with placing individual donor atoms with

  6. Geometry of the Adiabatic Theorem

    ERIC Educational Resources Information Center

    Lobo, Augusto Cesar; Ribeiro, Rafael Antunes; Ribeiro, Clyffe de Assis; Dieguez, Pedro Ruas

    2012-01-01

    We present a simple and pedagogical derivation of the quantum adiabatic theorem for two-level systems (a single qubit) based on geometrical structures of quantum mechanics developed by Anandan and Aharonov, among others. We have chosen to use only the minimum geometric structure needed for the understanding of the adiabatic theorem for this case.…

  7. The effects of ionization potential depression on the spectra emitted by hot dense aluminium plasmas

    NASA Astrophysics Data System (ADS)

    Preston, Thomas R.; Vinko, Sam M.; Ciricosta, Orlando; Chung, Hyun-Kyung; Lee, Richard W.; Wark, Justin S.

    2013-06-01

    Recent experiments at the Linac Coherent Light Source (LCLS) X-ray Free-Electron-Laser (FEL) have demonstrated that the standard model used for simulating ionization potential depression (IPD) in a plasma (the Stewart-Pyatt (SP) model, J.C. Stewart and K.D. Pyatt Jr., Astrophysical Journal 144 (1966) 1203) considerably underestimates the degree of IPD in a solid density aluminium plasma at temperatures up to 200 eV. In contrast, good agreement with the experimental data was found by use of a modified Ecker-Kröll (mEK) model (G. Ecker and W. Kröll, Physics of Fluids 6 (1963) 62-69). We present here detailed simulations, using the FLYCHK code, of the predicted spectra from hot dense, hydrogenic and helium-like aluminium plasmas ranging in densities from 0.1 to 4 times solid density, and at temperatures up to 1000 eV. Importantly, we find that the greater IPDs predicted by the mEK model result in the loss of the n = 3 states for the hydrogenic ions for all densities above ≈0.8 times solid density, and for the helium-like ions above ≈0.65 solid density. Therefore, we posit that if the mEK model holds at these higher temperatures, the temperature of solid density highly-charged aluminium plasmas cannot be determined by using spectral features associated with the n = 3 principal quantum number, and propose a re-evaluation of previous experimental data where high densities have been inferred from the spectra, and the SP model has been used.

  8. No first ionization potential fractionation in the active stars AR Piscium and AY Ceti

    NASA Astrophysics Data System (ADS)

    Sanz-Forcada, J.; Affer, L.; Micela, G.

    2009-10-01

    Context: The comparison of coronal and photospheric abundances in cool stars is an essential question to resolve. In the Sun an enhancement of the elements with low first ionization potential (FIP) is observed in the corona with respect to the photosphere. Stars with high levels of activity seem to show a depletion of elements with low FIP when compared to solar standard values; however, the few cases of active stars in which photospheric values are available for comparison lead to confusing results, and an enlargement of the sample is mandatory for solving this longstanding problem. Aims: We calculate in this paper the photospheric and coronal abundances of two well known active binary systems, AR Psc and AY Cet, to get further insight into the complications of coronal abundances. Methods: Coronal abundances of 9 elements were calculated by means of the reconstruction of a detailed emission measure distribution, using a line-based method that considers the lines from different elements separately. Photospheric abundances of 8 elements were calculated using high-resolution optical spectra of the stars. Results: The results once again show a lack of any FIP-related effect in the coronal abundances of the stars. The presence of metal abundance depletion (MAD) or inverse FIP effects in some stars could stem from a mistaken comparison to solar photospheric values or from a deficient calculation of photospheric abundances in fast-rotating stars. Conclusions: The lack of FIP fractionation seems to confirm that Alfvén waves combined with pondermotive forces are dominant in the corona of active stars. Tables 2 and 3 are only available in electronic form at http://www.aanda.org

  9. New ab initio adiabatic potential energy surfaces and bound state calculations for the singlet ground X˜ 1A1 and excited C˜ 1B2(21A') states of SO2

    NASA Astrophysics Data System (ADS)

    Kłos, Jacek; Alexander, Millard H.; Kumar, Praveen; Poirier, Bill; Jiang, Bin; Guo, Hua

    2016-05-01

    We report new and more accurate adiabatic potential energy surfaces (PESs) for the ground X˜ 1A1 and electronically excited C˜ 1B2(21A') states of the SO2 molecule. Ab initio points are calculated using the explicitly correlated internally contracted multi-reference configuration interaction (icMRCI-F12) method. A second less accurate PES for the ground X ˜ state is also calculated using an explicitly correlated single-reference coupled-cluster method with single, double, and non-iterative triple excitations [CCSD(T)-F12]. With these new three-dimensional PESs, we determine energies of the vibrational bound states and compare these values to existing literature data and experiment.

  10. Influence of magnetic field strength on potential well in the ionization stage of a double stage Hall thruster

    SciTech Connect

    Yu Daren; Song Maojiang; Liu Hui; Zhang Xu; Li Hong

    2012-07-15

    Similar to a single stage Hall thruster, the magnetic field, which controls electron trajectory and electric field distribution, is the most important factor determining the performance of a double stage Hall thruster. Especially, a potential well, which is helpful to reduce the ion loss on the thruster walls, is shaped in the ionization stage due to the existence of an annular magnetic field topology there. In this paper, the influence of magnetic field strength in the ionization stage on the potential well is researched with both experiments and particle-in-cell simulations. It is found that the depth of potential well increases with the magnetic field strength as a result of enhanced magnetic confinement and lowered electron conductivity. Consequently, the plasma density as well as the ion current entering the acceleration stage increases. However, an excessive magnetic field strength leads to an excess of ion loss on the walls of the acceleration stage. Therefore, there is an appropriate magnetic field strength in the ionization stage that results in a proper potential well and consequently an optimal performance of a double stage Hall thruster.

  11. Increasing the applicability of density functional theory. V. X-ray absorption spectra with ionization potential corrected exchange and correlation potentials

    NASA Astrophysics Data System (ADS)

    Verma, Prakash; Bartlett, Rodney J.

    2016-07-01

    Core excitation energies are computed with time-dependent density functional theory (TD-DFT) using the ionization energy corrected exchange and correlation potential QTP(0,0). QTP(0,0) provides C, N, and O K-edge spectra to about an electron volt. A mean absolute error (MAE) of 0.77 and a maximum error of 2.6 eV is observed for QTP(0,0) for many small molecules. TD-DFT based on QTP (0,0) is then used to describe the core-excitation spectra of the 22 amino acids. TD-DFT with conventional functionals greatly underestimates core excitation energies, largely due to the significant error in the Kohn-Sham occupied eigenvalues. To the contrary, the ionization energy corrected potential, QTP(0,0), provides excellent approximations (MAE of 0.53 eV) for core ionization energies as eigenvalues of the Kohn-Sham equations. As a consequence, core excitation energies are accurately described with QTP(0,0), as are the core ionization energies important in X-ray photoionization spectra or electron spectroscopy for chemical analysis.

  12. Increasing the applicability of density functional theory. V. X-ray absorption spectra with ionization potential corrected exchange and correlation potentials.

    PubMed

    Verma, Prakash; Bartlett, Rodney J

    2016-07-21

    Core excitation energies are computed with time-dependent density functional theory (TD-DFT) using the ionization energy corrected exchange and correlation potential QTP(0,0). QTP(0,0) provides C, N, and O K-edge spectra to about an electron volt. A mean absolute error (MAE) of 0.77 and a maximum error of 2.6 eV is observed for QTP(0,0) for many small molecules. TD-DFT based on QTP (0,0) is then used to describe the core-excitation spectra of the 22 amino acids. TD-DFT with conventional functionals greatly underestimates core excitation energies, largely due to the significant error in the Kohn-Sham occupied eigenvalues. To the contrary, the ionization energy corrected potential, QTP(0,0), provides excellent approximations (MAE of 0.53 eV) for core ionization energies as eigenvalues of the Kohn-Sham equations. As a consequence, core excitation energies are accurately described with QTP(0,0), as are the core ionization energies important in X-ray photoionization spectra or electron spectroscopy for chemical analysis. PMID:27448875

  13. HF echoes from ionization potentially produced by high-altitude discharges

    SciTech Connect

    Roussel-Dupre, R.A.; Blanc, E.

    1997-03-01

    The presence of ionization associated with high-altitude discharges has been detected using an HF radar operating at 2.2, 2.5, and 2.8 MHz. On several occasions, oblique echoes lasting several hundred ms at night and 1{r_arrow}10s during the day were observed. The echoes turned on in several interpulse times of 70 ms and were generally correlated with strong lightning activity prior to onset. The angles of arrival of sferics detected at three goniometer stations were used to determine the distance to thunderstorms. The data are consistent with specular reflections from columns of ionization produced at 55{endash}65 km altitude and having minimum electron densities of 6{times}10{sup 4}{endash}10{sup 5}cm{sup {minus}3}. The source of the ionization is believed to be high-altitude discharges.{copyright} 1997 American Geophysical Union

  14. Measurements of Ionization Cross Sections by Molecular Beam Experiments: Information Content on the Imaginary Part of the Optical Potential.

    PubMed

    Falcinelli, Stefano; Rosi, Marzio; Pirani, Fernando; Stranges, Domenico; Vecchiocattivi, Franco

    2016-07-14

    In this work, we present and analyze in detail new and recent ionization cross section and mass spectrum determinations, collected in the case of He*, Ne*-H2O, -H2S, and -NH3 ionizing collisions. These sets of data, obtained under the same experimental conditions, are relevant to identify differences in the autoionization stereodynamics of the three hydrogenated molecules and on the selective role of the imaginary part of the optical potential. We demonstrate that in these autoionization processes hydrogen and halogen bonds are competing because they are controlling both real and imaginary components of the optical potential that drives the complete reaction dynamics. In particular, we found that both components critically depend on the angular and radial approach between the reagent partners in determining the collision dynamics. PMID:26938026

  15. Strong-field ionization rates of linear polyenes simulated with time-dependent configuration interaction with an absorbing potential

    SciTech Connect

    Krause, Pascal; Schlegel, H. Bernhard

    2014-11-07

    The strong field ionization rates for ethylene, trans 1,3-butadiene, and trans,trans 1,3,5-hexatriene have been calculated using time-dependent configuration interaction with single excitations and a complex absorbing potential (TDCIS-CAP). The calculations used the aug-cc-pVTZ basis set with a large set of diffuse functions (3 s, 2 p, 3 d, and 1 f) on each atom. The absorbing boundary was placed 3.5 times the van der Waals radius from each atom. The simulations employed a seven-cycle cosine squared pulse with a wavelength of 800 nm. Ionization rates were calculated for intensities ranging from 0.3 × 10{sup 14} W/cm{sup 2} to 3.5 × 10{sup 14} W/cm{sup 2}. Ionization rates along the molecular axis increased markedly with increasing conjugation length. By contrast, ionization rates perpendicular to the molecular axis were almost independent of the conjugation length.

  16. Strong-field ionization rates of linear polyenes simulated with time-dependent configuration interaction with an absorbing potential.

    PubMed

    Krause, Pascal; Schlegel, H Bernhard

    2014-11-01

    The strong field ionization rates for ethylene, trans 1,3-butadiene, and trans,trans 1,3,5-hexatriene have been calculated using time-dependent configuration interaction with single excitations and a complex absorbing potential (TDCIS-CAP). The calculations used the aug-cc-pVTZ basis set with a large set of diffuse functions (3 s, 2 p, 3 d, and 1 f) on each atom. The absorbing boundary was placed 3.5 times the van der Waals radius from each atom. The simulations employed a seven-cycle cosine squared pulse with a wavelength of 800 nm. Ionization rates were calculated for intensities ranging from 0.3 × 10(14) W/cm(2) to 3.5 × 10(14) W/cm(2). Ionization rates along the molecular axis increased markedly with increasing conjugation length. By contrast, ionization rates perpendicular to the molecular axis were almost independent of the conjugation length. PMID:25381499

  17. Complete population inversion of Bose particles by an adiabatic cycle

    NASA Astrophysics Data System (ADS)

    Tanaka, Atushi; Cheon, Taksu

    2016-04-01

    We show that an adiabatic cycle excites Bose particles confined in a one-dimensional box. During the adiabatic cycle, a wall described by a δ-shaped potential is applied and its strength and position are slowly varied. When the system is initially prepared in the ground state, namely, in the zero-temperature equilibrium state, the adiabatic cycle brings all Bosons into the first excited one-particle state, leaving the system in a nonequilibrium state. The absorbed energy during the cycle is proportional to the number of Bosons.

  18. The Effect of the Residual Ion Potential on the Fully Differential Cross Section of Helium for Ionization by Electron Impact

    SciTech Connect

    Toth, A.; Nagy, L.

    2011-10-03

    We have carried out calculations for the fully differential cross section of the ionization of helium by electron projectiles. In order to study the effect of the residual ion potential, we employed three models, and tested them for the coplanar and perpendicular plane geometry. In spite of the simplicity of our models, the results for the coplanar case are in fair agreement with the available experimental data. The results for the perpendicular geometry need more improvement.

  19. The importance of accurate adiabatic interaction potentials for the correct description of electronically nonadiabatic vibrational energy transfer: A combined experimental and theoretical study of NO(v = 3) collisions with a Au(111) surface

    SciTech Connect

    Golibrzuch, Kai; Shirhatti, Pranav R.; Kandratsenka, Alexander; Wodtke, Alec M.; Bartels, Christof; Max Planck Institute for Biophysical Chemistry, Göttingen 37077 ; Rahinov, Igor; Auerbach, Daniel J.; Max Planck Institute for Biophysical Chemistry, Göttingen 37077; Department of Chemistry and Biochemistry, University of California Santa Barbara, Santa Barbara, California 93106

    2014-01-28

    We present a combined experimental and theoretical study of NO(v = 3 → 3, 2, 1) scattering from a Au(111) surface at incidence translational energies ranging from 0.1 to 1.2 eV. Experimentally, molecular beam–surface scattering is combined with vibrational overtone pumping and quantum-state selective detection of the recoiling molecules. Theoretically, we employ a recently developed first-principles approach, which employs an Independent Electron Surface Hopping (IESH) algorithm to model the nonadiabatic dynamics on a Newns-Anderson Hamiltonian derived from density functional theory. This approach has been successful when compared to previously reported NO/Au scattering data. The experiments presented here show that vibrational relaxation probabilities increase with incidence energy of translation. The theoretical simulations incorrectly predict high relaxation probabilities at low incidence translational energy. We show that this behavior originates from trajectories exhibiting multiple bounces at the surface, associated with deeper penetration and favored (N-down) molecular orientation, resulting in a higher average number of electronic hops and thus stronger vibrational relaxation. The experimentally observed narrow angular distributions suggest that mainly single-bounce collisions are important. Restricting the simulations by selecting only single-bounce trajectories improves agreement with experiment. The multiple bounce artifacts discovered in this work are also present in simulations employing electronic friction and even for electronically adiabatic simulations, meaning they are not a direct result of the IESH algorithm. This work demonstrates how even subtle errors in the adiabatic interaction potential, especially those that influence the interaction time of the molecule with the surface, can lead to an incorrect description of electronically nonadiabatic vibrational energy transfer in molecule-surface collisions.

  20. Adiabatic theory for anisotropic cold molecule collisions

    SciTech Connect

    Pawlak, Mariusz; Shagam, Yuval; Narevicius, Edvardas; Moiseyev, Nimrod

    2015-08-21

    We developed an adiabatic theory for cold anisotropic collisions between slow atoms and cold molecules. It enables us to investigate the importance of the couplings between the projection states of the rotational motion of the atom about the molecular axis of the diatom. We tested our theory using the recent results from the Penning ionization reaction experiment {sup 4}He(1s2s {sup 3}S) + HD(1s{sup 2}) → {sup 4}He(1s{sup 2}) + HD{sup +}(1s) + e{sup −} [Lavert-Ofir et al., Nat. Chem. 6, 332 (2014)] and demonstrated that the couplings have strong effect on positions of shape resonances. The theory we derived provides cross sections which are in a very good agreement with the experimental findings.

  1. Adiabatic theory for anisotropic cold molecule collisions.

    PubMed

    Pawlak, Mariusz; Shagam, Yuval; Narevicius, Edvardas; Moiseyev, Nimrod

    2015-08-21

    We developed an adiabatic theory for cold anisotropic collisions between slow atoms and cold molecules. It enables us to investigate the importance of the couplings between the projection states of the rotational motion of the atom about the molecular axis of the diatom. We tested our theory using the recent results from the Penning ionization reaction experiment (4)He(1s2s (3)S) + HD(1s(2)) → (4)He(1s(2)) + HD(+)(1s) + e(-) [Lavert-Ofir et al., Nat. Chem. 6, 332 (2014)] and demonstrated that the couplings have strong effect on positions of shape resonances. The theory we derived provides cross sections which are in a very good agreement with the experimental findings. PMID:26298122

  2. Multisurface Adiabatic Reactive Molecular Dynamics.

    PubMed

    Nagy, Tibor; Yosa Reyes, Juvenal; Meuwly, Markus

    2014-04-01

    Adiabatic reactive molecular dynamics (ARMD) simulation method is a surface-crossing algorithm for modeling chemical reactions in classical molecular dynamics simulations using empirical force fields. As the ARMD Hamiltonian is time dependent during crossing, it allows only approximate energy conservation. In the current work, the range of applicability of conventional ARMD is explored, and a new multisurface ARMD (MS-ARMD) method is presented, implemented in CHARMM and applied to the vibrationally induced photodissociation of sulfuric acid (H2SO4) in the gas phase. For this, an accurate global potential energy surface (PES) involving 12 H2SO4 and 4 H2O + SO3 force fields fitted to MP2/6-311G++(2d,2p) reference energies is employed. The MS-ARMD simulations conserve total energy and feature both intramolecular H-transfer reactions and water elimination. An analytical treatment of the dynamics in the crossing region finds that conventional ARMD can approximately conserve total energy for limiting cases. In one of them, the reduced mass of the system is large, which often occurs for simulations of solvated biomolecular systems. On the other hand, MS-ARMD is a general approach for modeling chemical reactions including gas-phase, homogeneous, heterogeneous, and enzymatic catalytic reactions while conserving total energy in atomistic simulations. PMID:26580356

  3. Acceleration of adiabatic quantum dynamics in electromagnetic fields

    SciTech Connect

    Masuda, Shumpei; Nakamura, Katsuhiro

    2011-10-15

    We show a method to accelerate quantum adiabatic dynamics of wave functions under electromagnetic field (EMF) by developing the preceding theory [Masuda and Nakamura, Proc. R. Soc. London Ser. A 466, 1135 (2010)]. Treating the orbital dynamics of a charged particle in EMF, we derive the driving field which accelerates quantum adiabatic dynamics in order to obtain the final adiabatic states in any desired short time. The scheme is consolidated by describing a way to overcome possible singularities in both the additional phase and driving potential due to nodes proper to wave functions under EMF. As explicit examples, we exhibit the fast forward of adiabatic squeezing and transport of excited Landau states with nonzero angular momentum, obtaining the result consistent with the transitionless quantum driving applied to the orbital dynamics in EMF.

  4. Adiabatic and isocurvature perturbation projections in multi-field inflation

    NASA Astrophysics Data System (ADS)

    Gordon, Chris; Saffin, Paul M.

    2013-08-01

    Current data are in good agreement with the predictions of single field inflation. However, the hemispherical asymmetry, seen in the cosmic microwave background data, may hint at a potential problem. Generalizing to multi-field models may provide one possible explanation. A useful way of modeling perturbations in multi-field inflation is to investigate the projection of the perturbation along and perpendicular to the background fields' trajectory. These correspond to the adiabatic and isocurvature perturbations. However, it is important to note that in general there are no corresponding adiabatic and isocurvature fields. The purpose of this article is to highlight the distinction between a field redefinition and a perturbation projection. We provide a detailed derivation of the evolution of the isocurvature perturbation to show that no assumption of an adiabatic or isocurvature field is needed. We also show how this evolution equation is consistent with the field covariant evolution equations for the adiabatic perturbation in the flat field space limit.

  5. Quantum Monte Carlo simulations of tunneling in quantum adiabatic optimization

    NASA Astrophysics Data System (ADS)

    Brady, Lucas T.; van Dam, Wim

    2016-03-01

    We explore to what extent path-integral quantum Monte Carlo methods can efficiently simulate quantum adiabatic optimization algorithms during a quantum tunneling process. Specifically we look at symmetric cost functions defined over n bits with a single potential barrier that a successful quantum adiabatic optimization algorithm will have to tunnel through. The height and width of this barrier depend on n , and by tuning these dependencies, we can make the optimization algorithm succeed or fail in polynomial time. In this article we compare the strength of quantum adiabatic tunneling with that of path-integral quantum Monte Carlo methods. We find numerical evidence that quantum Monte Carlo algorithms will succeed in the same regimes where quantum adiabatic optimization succeeds.

  6. Microwave ionization of Rydberg atoms

    SciTech Connect

    Gallagher, T.F.

    1996-12-31

    An atom can be ionized by a static field if the field depresses the potential below the binding energy W, leading to the requirement E = W{sup 2}/4 in atomic units. The atomic units of field and energy are 5.14 {times} 10{sup 9} V/cm and 27.2 eV. The ionization field is often expressed in terms of the principal quantum number n of the state in question as E = 1/16n{sup 4}. In a microwave field with frequency far less than the separation {Delta}W = 1/n{sup 3} between adjacent n states, atoms other than H ionize at the much lower microwave field amplitude of E = 1/3n{sup 5}. This field corresponds to the Inglis-Teller limit, where it is impossible to resolve spectrally adjacent n states due to Stark broadening in a plasma. In H ionization occurs as it does in a static field. The difference exists because the finite sized ionic core of a non hydrogenic atom breaks one of the symmetries found in H. In non hydrogenic atoms the microwave field drives a series of transitions through successively higher n states culminating in ionization. These transitions can be understood in terms of a Landau-Zener picture based on the variation of the energies of the atoms produced by the time varying field or as the resonant multiphoton absorption of the microwave photons. In either case, the atoms make transitions through real intermediate states en route to ionization. With short, four cycle, microwave pulses complete ionization does not occur with fields of E = 1/3n{sup 5}, and population is left in intermediate states. The transition from ionization at fields near E = 1/3n{sup 5} to fields of E = 1/16n{sup 4} occurs when the frequency becomes low enough that the energies of the states vary adiabatically in the temporally varying field.

  7. Accurate adiabatic potential energy surface for 12A' state of FH2 based on ab initio data extrapolated to the complete basis set limit

    NASA Astrophysics Data System (ADS)

    Li, Yong-Qing; Song, Yu-Zhi; Joaquim de Campos Varandas, António

    2015-01-01

    An accurate single-sheeted double many-body expansion potential energy surface is reported for the title system. It is obtained by using the aug-cc-pVTZ and aug-cc-pVQZ basis sets with extrapolation of the electron correlation energy to the complete basis set limit, plus extrapolation to the complete basis set limit of the complete-active-space self-consistent field energy. The collinear and bending barrier heights of the new global potential energy surface is 2.301 and 1.768 kcal mol-1, in very good agreement with the values of 2.222 and 1.770 kcal mol-1 from the current best potential energy surface. In particular, the new potential energy surface describes well the important van der Waals interactions which is very useful for investigating the dynamics of the title system. Thus, the new potential energy surface can both be recommended for dynamics studies of the F + H2 reaction and as building block for constructing the potential energy surfaces of larger fluorine/hydrogen containing systems. Based on the new potential energy surface, a preliminary theoretical study of the reaction F(2P) + H2 (X1 Σg+) → FH(X1Σ+) + H(2S) has been carried out with the methods of quasi-classical trajectory and quantum mechanical. The results have shown that the new PES is suitable for any kind of dynamics studies. Supplementary material in the form of one pdf file available from the Journal web page at http://dx.doi.org/10.1140/epjd/e2014-50445-3

  8. Polynucleotide kinase as a potential target for enhancing cytotoxicity by ionizing radiation and topoisomerase I inhibitors

    PubMed Central

    Bernstein, N. K.; Karimi-Busheri, F.; Rasouli-Nia, A.; Mani, R.; Dianov, G.; Glover, J. N. M.; Weinfeld, M.

    2010-01-01

    The cytotoxicity of many antineoplastic agents is due to their capacity to damage DNA and there is evidence indicating that DNA repair contributes to the cellular resistance to such agents. DNA strand breaks constitute a significant proportion of the lesions generated by a broad range of genotoxic agents, either directly, or during the course of DNA repair. Strand breaks that are caused by many agents including ionizing radiation, topoisomerase I inhibitors, and DNA repair glycosylases such as NEIL1 and NEIL2, often contain 5’-hydroxyl and/or 3’-phosphate termini. These ends must be converted to 5’-phosphate and 3’-hydroxyl termini in order to allow DNA polymerases and ligases to catalyze repair synthesis and strand rejoining. A key enzyme involved in this end-processing is polynucleotide kinase (PNK), which possesses two enzyme activities, a DNA 5’-kinase activity and a 3’-phosphatase activity. PNK participates in the single-strand break repair pathway and the non-homologous end joining pathway for double-strand break repair. RNAi-mediated down-regulation of PNK renders cells more sensitive to ionizing radiation and camptothecin, a topoisomerase I inhibitor. Structural analysis of PNK revealed the protein is composed of three domains, the kinase domain at the C-terminus, the phosphatase domain in the centre and a forkhead associated (FHA) domain at the N-terminus. The FHA domain plays a critical role in the binding of PNK to other DNA repair proteins. Thus each PNK domain may be a suitable target for small molecule inhibition to effectively reduce resistance to ionizing radiation and topoisomerase I inhibitors. PMID:18473721

  9. Neutral resonant ionization in a H- plasma source: Potential of doubly excited **H-

    NASA Astrophysics Data System (ADS)

    Vogel, J. S.

    2016-02-01

    Hydrogen plasmas are optically dense to Lyman-α radiation, maintaining *H(n = 2) neutral atoms that may undergo neutral resonant ionization to **H-. One state, **H-(2p2 3Pe), is thought bound at 9.7 meV with a several nanosecond lifetime while all others are unbound resonances. Collision dynamics of two *H(2s) shows that an ionic pair of (p, **H-) resolves at least three long-standing collision experiments. The doubly excited anion also has a path to the unexcited ion pair whose only physical distinction is that both (p, H-) have energy of 3.7 eV.

  10. Calculations of the ionization potentials of the halogens by the relativistic Hartree-Rock-Dirac method taking account of superposition of configurations

    SciTech Connect

    Tupitsyn, I.I.

    1988-03-01

    The ionization potentials of the halogen group have been calculated. The calculations were carried out using the relativistic Hartree-Fock method taking into account correlation effects. Comparison of theoretical results with experimental data for the elements F, Cl, Br, and I allows an estimation of the accuracy and reliability of the method. The theoretical values of the ionization potential of astatine obtained here may be of definite interest for the chemistry of astatine.

  11. Equation of motion coupled cluster methods for electron attachment and ionization potential in fullerenes C60 and C70

    SciTech Connect

    Bhaskaran-Nair, Kiran; Kowalski, Karol; Moreno, Juana; Jarrell, Mark; Shelton, William A.

    2014-08-21

    Discovery of fullerenes has opened a entirely new chapter in chemistry due to their wide range of properties which holds exciting applications in numerous disciplines of science. The Nobel Prize in Chemistry 1996 was awarded jointly to Robert F. Curl Jr., Sir Harold W. Kroto and Richard E. Smalley in recoginition for their discovery of this new carbon allotrope. In this letter we are reporting ionization potential and electron attachment studies on fullerenes (C60 and C70) obtained with novel parallel implementation of the EA-EOM-CCSD and IP-EOM-CCSD methods in NWChem program package.

  12. Ionization potentials, electron affinities, resonance excitation energies, oscillator strengths, and ionic radii of element Uus (Z = 117) and astatine.

    PubMed

    Chang, Zhiwei; Li, Jiguang; Dong, Chenzhong

    2010-12-30

    Multiconfiguration Dirac-Fock (MCDF) method was employed to calculate the first five ionization potentials, electron affinities, resonance excitation energies, oscillator strengths, and radii for the element Uus and its homologue At. Main valence correlation effects were taken into account. The Breit interaction and QED effects were also estimated. The uncertainties of calculated IPs, EAs, and IR for Uus and At were reduced through an extrapolation procedure. The good consistency with available experimental and other theoretical values demonstrates the validity of the present results. These theoretical data therefore can be used to predict some unknown physicochemical properties of element Uus, Astatine, and their compounds. PMID:21141866

  13. Using the charge-stabilization technique in the double ionization potential equation-of-motion calculations with dianion references.

    PubMed

    Kuś, Tomasz; Krylov, Anna I

    2011-08-28

    The charge-stabilization method is applied to double ionization potential equation-of-motion (EOM-DIP) calculations to stabilize unstable dianion reference functions. The auto-ionizing character of the dianionic reference states spoils the numeric performance of EOM-DIP limiting applications of this method. We demonstrate that reliable excitation energies can be computed by EOM-DIP using a stabilized resonance wave function instead of the lowest energy solution corresponding to the neutral + free electron(s) state of the system. The details of charge-stabilization procedure are discussed and illustrated by examples. The choice of optimal stabilizing Coulomb potential, which is strong enough to stabilize the dianion reference, yet, minimally perturbs the target states of the neutral, is the crux of the approach. Two algorithms of choosing optimal parameters of the stabilization potential are presented. One is based on the orbital energies, and another--on the basis set dependence of the total Hartree-Fock energy of the reference. Our benchmark calculations of the singlet-triplet energy gaps in several diradicals show a remarkable improvement of the EOM-DIP accuracy in problematic cases. Overall, the excitation energies in diradicals computed using the stabilized EOM-DIP are within 0.2 eV from the reference EOM spin-flip values. PMID:21895161

  14. Inertial effects in adiabatically driven flashing ratchets

    NASA Astrophysics Data System (ADS)

    Rozenbaum, Viktor M.; Makhnovskii, Yurii A.; Shapochkina, Irina V.; Sheu, Sheh-Yi; Yang, Dah-Yen; Lin, Sheng Hsien

    2014-05-01

    We study analytically the effect of a small inertial correction on the properties of adiabatically driven flashing ratchets. Parrondo's lemma [J. M. R. Parrondo, Phys. Rev. E 57, 7297 (1998), 10.1103/PhysRevE.57.7297] is generalized to include the inertial term so as to establish the symmetry conditions allowing directed motion (other than in the overdamped massless case) and to obtain a high-temperature expansion of the motion velocity for arbitrary potential profiles. The inertial correction is thus shown to enhance the ratchet effect at all temperatures for sawtooth potentials and at high temperatures for simple potentials described by the first two harmonics. With the special choice of potentials represented by at least the first three harmonics, the correction gives rise to the motion reversal in the high-temperature region. In the low-temperature region, inertia weakens the ratchet effect, with the exception of the on-off model, where diffusion is important. The directed motion adiabatically driven by potential sign fluctuations, though forbidden in the overdamped limit, becomes possible due to purely inertial effects in neither symmetric nor antisymmetric potentials, i.e., not for commonly used sawtooth and two-sinusoid profiles.

  15. Accurate ab initio-based adiabatic global potential energy surface for the 2(2)A" state of NH2 by extrapolation to the complete basis set limit.

    PubMed

    Li, Y Q; Ma, F C; Sun, M T

    2013-10-21

    A full three-dimensional global potential energy surface is reported first time for the title system, which is important for the photodissociation processes. It is obtained using double many-body expansion theory and an extensive set of accurate ab initio energies extrapolated to the complete basis set limit. Such a work can be recommended for dynamics studies of the N((2)D) + H2 reaction, a reliable theoretical treatment of the photodissociation dynamics and as building blocks for constructing the double many-body expansion potential energy surface of larger nitrogen/hydrogen containing systems. In turn, a preliminary theoretical study of the reaction N((2)D)+H2(X(1)Σg (+))(ν=0,j=0)→NH(a(1)Δ)+H((2)S) has been carried out with the method of quasi-classical trajectory on the new potential energy surface. Integral cross sections and thermal rate constants have been calculated, providing perhaps the most reliable estimate of the integral cross sections and the rate constants known thus far for such a reaction. PMID:24160511

  16. Accurate ab initio-based adiabatic global potential energy surface for the 22A″ state of NH2 by extrapolation to the complete basis set limit

    NASA Astrophysics Data System (ADS)

    Li, Y. Q.; Ma, F. C.; Sun, M. T.

    2013-10-01

    A full three-dimensional global potential energy surface is reported first time for the title system, which is important for the photodissociation processes. It is obtained using double many-body expansion theory and an extensive set of accurate ab initio energies extrapolated to the complete basis set limit. Such a work can be recommended for dynamics studies of the N(2D) + H2 reaction, a reliable theoretical treatment of the photodissociation dynamics and as building blocks for constructing the double many-body expansion potential energy surface of larger nitrogen/hydrogen containing systems. In turn, a preliminary theoretical study of the reaction N(^2D)+H_2(X^1Σ _g^+)(ν =0,j=0)rArr NH(a^1Δ )+H(^2S) has been carried out with the method of quasi-classical trajectory on the new potential energy surface. Integral cross sections and thermal rate constants have been calculated, providing perhaps the most reliable estimate of the integral cross sections and the rate constants known thus far for such a reaction.

  17. Grain in weakly ionized plasma in the presence of an external magnetic field: Charging by plasma currents and effective potential

    SciTech Connect

    Momot, A. I.; M.M. Bogolubov Institute for Theoretical Physics, Nat. Acad. Sci. of Ukraine, 14b, Metrologichna Str., Kyiv, 03680

    2013-07-15

    The problem of grain screening is solved numerically for the case of weakly ionized plasma in the presence of an external magnetic field. The plasma dynamics is described within the drift-diffusion approximation under the assumption that the grain absorbs all encountered electrons and ions. We also assume that the plasma current through the grain surface is equal to zero in the stationary state. This condition is used to perform self-consistent calculations of the grain charge. The spatial distribution of the screened grain potential is studied and compared with the analytical estimates. It is shown that at the distances larger than the Debye length such potential has the Coulomb-like asymptotics with the effective charge dependent on the angle between the radius vector and the external magnetic field direction. The numerical solutions show that in the direction parallel to the external magnetic field the effective potential can have nonmonotonic behavior.

  18. Inverted perturbation approach (IPA) potentials and adiabatic corrections of the X 1Sigma + state of the lithium hydrides near the dissociation limits

    NASA Astrophysics Data System (ADS)

    Chan, Y. C.; Harding, D. R.; Stwalley, W. C.; Vidal, C. R.

    1986-09-01

    Laser-induced fluorescence (LIF) spectra of the A-X system of the LiH isotopes, excited by the UV lines of an argon and a krypton ion laser, were observed and analyzed. Three long LIF series of different LiH isotopes were taken with a 3.4 m high resolution spectrograph. The results were combined with previous experimental data to study the breakdown of the Born-Oppenheimer approximation in the X 1Σ+ electronic ground state of the isotopic LiH molecules. Using a quantum mechanical variational method, potential energy curves of the four LiH isotopes were extended almost up to the dissociation limits.

  19. Theory of warm ionized gases: equation of state and kinetic Schottky anomaly.

    PubMed

    Capolupo, A; Giampaolo, S M; Illuminati, F

    2013-10-01

    Based on accurate Lennard-Jones-type interaction potentials, we derive a closed set of state equations for the description of warm atomic gases in the presence of ionization processes. The specific heat is predicted to exhibit peaks in correspondence to single and multiple ionizations. Such kinetic analog in atomic gases of the Schottky anomaly in solids is enhanced at intermediate and low atomic densities. The case of adiabatic compression of noble gases is analyzed in detail and the implications on sonoluminescence are discussed. In particular, the predicted plasma electron density in a sonoluminescent bubble turns out to be in good agreement with the value measured in recent experiments. PMID:24229140

  20. Functional representation for the born-oppenheimer diagonal correction and born-huang adiabatic potential energy surfaces for isotopomers of H3.

    PubMed

    Mielke, Steven L; Schwenke, David W; Schatz, George C; Garrett, Bruce C; Peterson, Kirk A

    2009-04-23

    Multireference configuration interaction (MRCI) calculations of the Born-Oppenheimer diagonal correction (BODC) for H(3) were performed at 1397 symmetry-unique configurations using the Handy-Yamaguchi-Schaefer approach; isotopic substitution leads to 4041 symmetry-unique configurations for the DH(2) mass combination. These results were then fit to a functional form that permits calculation of the BODC for any combination of isotopes. Mean unsigned fitting errors on a test grid of configurations not included in the fitting process were 0.14, 0.12, and 0.65 cm(-1) for the H(3), DH(2), and MuH(2) isotopomers, respectively. This representation can be combined with any Born-Oppenheimer potential energy surface (PES) to yield Born-Huang (BH) PESs; herein, we choose the CCI potential energy surface, the uncertainties of which ( approximately 0.01 kcal/mol) are much smaller than the magnitude of the BODC. Fortran routines to evaluate these BH surfaces are provided. Variational transition state theory calculations are presented comparing thermal rate constants for reactions on the BO and BH surfaces to provide an initial estimate of the significance of the diagonal correction for the dynamics. PMID:19290604

  1. Revisiting The Brightest RV Tauri Star: First Ionization Potential (FIP) Effect in R Sct

    NASA Astrophysics Data System (ADS)

    Yolalan, Gizay; Sahin, Timur

    2016-07-01

    We have derived elemental abundances of the brightest RV Tauri star, R Sct. The abundance analysis of the star is based on high resolution and high quality (S/N>300) echelle spectra, mainly obtained for radial velocity study of a large sample of IRAS like RV Tau sample stars, from the McDonald Observatory (R~48,000). Our analysis is based on optical spectra obtained at only one phase of the variation. The standard 1D LTE analysis provided a fresh determination of the atmospheric parameters: Teff=5000 K, logg=1.05 cgs, and a microturbulence velocity ξ=3.4 km/s and [Fe/H] = -0.33. We report on chemical abundances of 10 neutral and ionized species identified over 4800 - 5600 A wavelength region. In an effort to explain observed deficiency in abundances, possible scenarios including FIP is investigated.

  2. Adiabatic evolution of plasma equilibrium

    PubMed Central

    Grad, H.; Hu, P. N.; Stevens, D. C.

    1975-01-01

    A new theory of plasma equilibrium is introduced in which adiabatic constraints are specified. This leads to a mathematically nonstandard structure, as compared to the usual equilibrium theory, in which prescription of pressure and current profiles leads to an elliptic partial differential equation. Topologically complex configurations require further generalization of the concept of adiabaticity to allow irreversible mixing of plasma and magnetic flux among islands. Matching conditions across a boundary layer at the separatrix are obtained from appropriate conservation laws. Applications are made to configurations with planned islands (as in Doublet) and accidental islands (as in Tokamaks). Two-dimensional, axially symmetric, helically symmetric, and closed line equilibria are included. PMID:16578729

  3. Calculations of the ionization potentials and electron affinities of bacteriochlorophyll and bacteriopheophytin via ab initio quantum chemistry

    SciTech Connect

    Crystal, J.; Friesner, R.A.

    2000-03-23

    Ionization potentials (IP) and electron affinities (EA) are calculated for bacteriopheophytin (BPh) and bacteriochlorophyll (BChl) in the photosynthetic reaction center utilizing density functional methods implemented in a parallel version of the JAGUAR electronic structure code. These quantities are studied as a function of basis set size and molecular geometry. The results indicate the necessity of using large basis sets with diffuse functions in order to obtain reliable IP and EA in the gas phase. The relative reduction potentials of BChl and BPh in dimethylformamide solution are also calculated and compared with experimental results. Excellent agreement between theory and experiment is obtained when ligand binding of solvent molecules to the central Mg atom of BNhl is incorporated in the calculations.

  4. Shortcuts to adiabaticity in a time-dependent box

    PubMed Central

    Campo, A. del; Boshier, M. G.

    2012-01-01

    A method is proposed to drive an ultrafast non-adiabatic dynamics of an ultracold gas trapped in a time-dependent box potential. The resulting state is free from spurious excitations associated with the breakdown of adiabaticity, and preserves the quantum correlations of the initial state up to a scaling factor. The process relies on the existence of an adiabatic invariant and the inversion of the dynamical self-similar scaling law dictated by it. Its physical implementation generally requires the use of an auxiliary expulsive potential. The method is extended to a broad family of interacting many-body systems. As illustrative examples we consider the ultrafast expansion of a Tonks-Girardeau gas and of Bose-Einstein condensates in different dimensions, where the method exhibits an excellent robustness against different regimes of interactions and the features of an experimentally realizable box potential. PMID:22970340

  5. Experimental breaking of an adiabatic invariant

    NASA Astrophysics Data System (ADS)

    Notte, J.; Fajans, J.; Chu, R.; Wurtele, J. S.

    1993-06-01

    When a cylindrical pure electron plasma is displaced from the center of the trap, it performs a bulk circular orbital motion known as the l=1 diocotron mode. The slow application of a perturbing potential to a patch on the trap wall distorts the orbit into a noncircular closed path. Experiments and a simple theoretical model indicate that the area by the loop is an adiabatic invariant. Detailed studies are made of the breaking of the invariant when perturbations are rapidly applied. When the perturbation is applied with discontinuous time derivatives, the invariant breaking greatly exceeds the predictions of the standard theory for smooth perturbations.

  6. [Bond selective chemistry beyond the adiabatic approximation

    SciTech Connect

    Butler, L.J.

    1993-02-28

    The adiabatic Born-Oppenheimer potential energy surface approximation is not valid for reaction of a wide variety of energetic materials and organic fuels; coupling between electronic states of reacting species plays a key role in determining the selectivity of the chemical reactions induced. This research program initially studies this coupling in (1) selective C-Br bond fission in 1,3- bromoiodopropane, (2) C-S:S-H bond fission branching in CH[sub 3]SH, and (3) competition between bond fission channels and H[sub 2] elimination in CH[sub 3]NH[sub 2].

  7. Local entanglement generation in the adiabatic regime

    SciTech Connect

    Cliche, M.; Veitia, Andrzej

    2010-09-15

    We study entanglement generation in a pair of qubits interacting with an initially correlated system. Using time-independent perturbation theory and the adiabatic theorem, we show conditions under which the qubits become entangled as the joint system evolves into the ground state of the interacting theory. We then apply these results to the case of qubits interacting with a scalar quantum field. We study three different variations of this setup; a quantum field subject to Dirichlet boundary conditions, a quantum field interacting with a classical potential, and a quantum field that starts in a thermal state.

  8. Oxidation-reduction potentials and ionization states of extracellular peroxidases from the lignin-degrading fungus Phanerochaete chrysosporium.

    PubMed

    Millis, C D; Cai, D Y; Stankovich, M T; Tien, M

    1989-10-17

    The oxidation-reduction potentials of lignin peroxidase isozymes H1, H2, H8, and H10 as well as the Mn-dependent peroxidase isozymes H3 and H4 are reported. The potentiometric titrations involving the ferrous and ferric states of the enzyme had Nernst plots indicating single-electron transfer. The Em7 values of lignin peroxidase isozymes H1, H2, H8, and H10 are -142, -135, -137, and -127 mV versus standard hydrogen electrode, respectively. The Em7 values for the Mn-dependent peroxidase isozymes H3 and H4 are -88 and -93 mV versus standard hydrogen electrode, respectively. The midpoint potential of H1, H8, and H4 remained unchanged in the presence of their respective substrates, veratryl alcohol and Mn(II). The midpoint potential between the ferric and ferrous forms of isozymes H1 and H4 exhibited a pH-dependent change between pH 3.5 and pH 6.5. These results indicate that the reductive half-reaction of the enzymes is the following: ferric peroxidase + le- + H+----ferrous peroxidase. Above pH 6.5, the effect of pH on the midpoint potential is diminished and indicates that an ionization with an apparent pKa equal to approximately 6.6-6.7 occurs in the reduced form of the enzymes. A heme-linked ionization group in the ferrous form of the enzymes was confirmed by studying the effect of pH on the absorption spectra of isozymes H1 and H4. These spectrophotometric pH titration experiments confirmed the electrochemical results indicating pKa values of 6.59 and 6.69 for reduced isozymes H1 and H4, respectively. These results indicate the presence of a heme-linked ionization of an amino acid in the reduced form of the lignin peroxidase isozymes similar to that of other plant peroxidases. PMID:2605198

  9. Potential treatment of inflammatory and proliferative diseases by ultra-low doses of ionizing radiations.

    PubMed

    Sanders, Charles L

    2012-12-01

    Ultra-low doses and dose- rates of ionizing radiation are effective in preventing disease which suggests that they also may be effective in treating disease. Limited experimental and anecdotal evidence indicates that low radiation doses from radon in mines and spas, thorium-bearing monazite sands and enhanced radioactive uranium ore obtained from a natural geological reactor may be useful in treating many inflammatory conditions and proliferative disorders, including cancer. Optimal therapeutic applications were identified via a literature survey as dose-rates ranging from 7 to 11μGy/hr or 28 to 44 times world average background rates. Rocks from an abandoned uranium mine in Utah were considered for therapeutic application and were examined by γ-ray and laser-induced breakdown fluorescence spectroscopy. The rocks showed the presence of transuranics and fission products with a γ-ray energy profile similar to aged spent uranium nuclear fuel (93% dose due to β particles and 7% due to γ rays). Mud packs of pulverized uranium ore rock dust in sealed plastic bags delivering bag surface β,γ dose-rates of 10-450 μGy/h were used with apparent success to treat several inflammatory and proliferative conditions in humans. PMID:23304108

  10. Potential Treatment of Inflammatory and Proliferative Diseases by Ultra-Low Doses of Ionizing Radiations

    PubMed Central

    Sanders, Charles L.

    2012-01-01

    Ultra-low doses and dose- rates of ionizing radiation are effective in preventing disease which suggests that they also may be effective in treating disease. Limited experimental and anecdotal evidence indicates that low radiation doses from radon in mines and spas, thorium-bearing monazite sands and enhanced radioactive uranium ore obtained from a natural geological reactor may be useful in treating many inflammatory conditions and proliferative disorders, including cancer. Optimal therapeutic applications were identified via a literature survey as dose-rates ranging from 7 to 11μGy/hr or 28 to 44 times world average background rates. Rocks from an abandoned uranium mine in Utah were considered for therapeutic application and were examined by γ-ray and laser-induced breakdown fluorescence spectroscopy. The rocks showed the presence of transuranics and fission products with a γ-ray energy profile similar to aged spent uranium nuclear fuel (93% dose due to β particles and 7% due to γ rays). Mud packs of pulverized uranium ore rock dust in sealed plastic bags delivering bag surface β,γ dose-rates of 10–450 μGy/h were used with apparent success to treat several inflammatory and proliferative conditions in humans. PMID:23304108

  11. Pressure Oscillations in Adiabatic Compression

    ERIC Educational Resources Information Center

    Stout, Roland

    2011-01-01

    After finding Moloney and McGarvey's modified adiabatic compression apparatus, I decided to insert this experiment into my physical chemistry laboratory at the last minute, replacing a problematic experiment. With insufficient time to build the apparatus, we placed a bottle between two thick textbooks and compressed it with a third textbook forced…

  12. Adiabatic dynamics of magnetic vortices

    NASA Astrophysics Data System (ADS)

    Papanicolaou, N.

    1994-03-01

    We formulate a reasonably detailed adiabatic conjecture concerning the dynamics of skew deflection of magnetic vortices in a field gradient, which is expected to be valid at sufficiently large values of the winding number. The conjecture is consistent with the golden rule used to describe the dynamics of realistic magnetic bubbles and is verified here numerically within the 2-D isotropic Heisenberg model.

  13. Transitionless driving on adiabatic search algorithm

    SciTech Connect

    Oh, Sangchul; Kais, Sabre

    2014-12-14

    We study quantum dynamics of the adiabatic search algorithm with the equivalent two-level system. Its adiabatic and non-adiabatic evolution is studied and visualized as trajectories of Bloch vectors on a Bloch sphere. We find the change in the non-adiabatic transition probability from exponential decay for the short running time to inverse-square decay in asymptotic running time. The scaling of the critical running time is expressed in terms of the Lambert W function. We derive the transitionless driving Hamiltonian for the adiabatic search algorithm, which makes a quantum state follow the adiabatic path. We demonstrate that a uniform transitionless driving Hamiltonian, approximate to the exact time-dependent driving Hamiltonian, can alter the non-adiabatic transition probability from the inverse square decay to the inverse fourth power decay with the running time. This may open up a new but simple way of speeding up adiabatic quantum dynamics.

  14. Transitionless driving on adiabatic search algorithm

    NASA Astrophysics Data System (ADS)

    Oh, Sangchul; Kais, Sabre

    2014-12-01

    We study quantum dynamics of the adiabatic search algorithm with the equivalent two-level system. Its adiabatic and non-adiabatic evolution is studied and visualized as trajectories of Bloch vectors on a Bloch sphere. We find the change in the non-adiabatic transition probability from exponential decay for the short running time to inverse-square decay in asymptotic running time. The scaling of the critical running time is expressed in terms of the Lambert W function. We derive the transitionless driving Hamiltonian for the adiabatic search algorithm, which makes a quantum state follow the adiabatic path. We demonstrate that a uniform transitionless driving Hamiltonian, approximate to the exact time-dependent driving Hamiltonian, can alter the non-adiabatic transition probability from the inverse square decay to the inverse fourth power decay with the running time. This may open up a new but simple way of speeding up adiabatic quantum dynamics.

  15. Transitionless driving on adiabatic search algorithm.

    PubMed

    Oh, Sangchul; Kais, Sabre

    2014-12-14

    We study quantum dynamics of the adiabatic search algorithm with the equivalent two-level system. Its adiabatic and non-adiabatic evolution is studied and visualized as trajectories of Bloch vectors on a Bloch sphere. We find the change in the non-adiabatic transition probability from exponential decay for the short running time to inverse-square decay in asymptotic running time. The scaling of the critical running time is expressed in terms of the Lambert W function. We derive the transitionless driving Hamiltonian for the adiabatic search algorithm, which makes a quantum state follow the adiabatic path. We demonstrate that a uniform transitionless driving Hamiltonian, approximate to the exact time-dependent driving Hamiltonian, can alter the non-adiabatic transition probability from the inverse square decay to the inverse fourth power decay with the running time. This may open up a new but simple way of speeding up adiabatic quantum dynamics. PMID:25494733

  16. Electronic structure and spectroscopy of nucleic acid bases: Ionization energies, ionization-induced structural changes, and photoelectron spectra

    SciTech Connect

    Bravaya, Ksenia B.; Kostko, Oleg; Dolgikh, Stanislav; Landau, Arie; Ahmed, Musahid; Krylov, Anna I.

    2010-08-02

    We report high-level ab initio calculations and single-photon ionization mass spectrometry study of ionization of adenine (A), thymine (T), cytosine (C) and guanine (G). For thymine and adenine, only the lowest-energy tautomers were considered, whereas for cytosine and guanine we characterized five lowest-energy tautomeric forms. The first adiabatic and several vertical ionization energies were computed using equation-of-motion coupled-cluster method for ionization potentials with single and double substitutions. Equilibrium structures of the cationic ground states were characterized by DFT with the {omega}B97X-D functional. The ionization-induced geometry changes of the bases are consistent with the shapes of the corresponding molecular orbitals. For the lowest-energy tautomers, the magnitude of the structural relaxation decreases in the following series G > C > A > T, the respective relaxation energies being 0.41, 0.32, 0.25 and 0.20 eV. The computed adiabatic ionization energies (8.13, 8.89, 8.51-8.67 and 7.75-7.87 eV for A,T,C and G, respectively) agree well with the onsets of the photoionization efficiency (PIE) curves (8.20 {+-} 0.05, 8.95 {+-} 0.05, 8.60 {+-} 0.05 and 7.75 {+-} 0.05 eV). Vibrational progressions for the S{sub 0}-D{sub 0} vibronic bands computed within double-harmonic approximation with Duschinsky rotations are compared with previously reported experimental photoelectron spectra.

  17. Bond selective chemistry beyond the adiabatic approximation

    SciTech Connect

    Butler, L.J.

    1993-12-01

    One of the most important challenges in chemistry is to develop predictive ability for the branching between energetically allowed chemical reaction pathways. Such predictive capability, coupled with a fundamental understanding of the important molecular interactions, is essential to the development and utilization of new fuels and the design of efficient combustion processes. Existing transition state and exact quantum theories successfully predict the branching between available product channels for systems in which each reaction coordinate can be adequately described by different paths along a single adiabatic potential energy surface. In particular, unimolecular dissociation following thermal, infrared multiphoton, or overtone excitation in the ground state yields a branching between energetically allowed product channels which can be successfully predicted by the application of statistical theories, i.e. the weakest bond breaks. (The predictions are particularly good for competing reactions in which when there is no saddle point along the reaction coordinates, as in simple bond fission reactions.) The predicted lack of bond selectivity results from the assumption of rapid internal vibrational energy redistribution and the implicit use of a single adiabatic Born-Oppenheimer potential energy surface for the reaction. However, the adiabatic approximation is not valid for the reaction of a wide variety of energetic materials and organic fuels; coupling between the electronic states of the reacting species play a a key role in determining the selectivity of the chemical reactions induced. The work described below investigated the central role played by coupling between electronic states in polyatomic molecules in determining the selective branching between energetically allowed fragmentation pathways in two key systems.

  18. Studies in Chaotic adiabatic dynamics

    SciTech Connect

    Jarzynski, C.

    1994-01-01

    Chaotic adiabatic dynamics refers to the study of systems exhibiting chaotic evolution under slowly time-dependent equations of motion. In this dissertation the author restricts his attention to Hamiltonian chaotic adiabatic systems. The results presented are organized around a central theme, namely, that the energies of such systems evolve diffusively. He begins with a general analysis, in which he motivates and derives a Fokker-Planck equation governing this process of energy diffusion. He applies this equation to study the {open_quotes}goodness{close_quotes} of an adiabatic invariant associated with chaotic motion. This formalism is then applied to two specific examples. The first is that of a gas of noninteracting point particles inside a hard container that deforms slowly with time. Both the two- and three-dimensional cases are considered. The results are discussed in the context of the Wall Formula for one-body dissipation in nuclear physics, and it is shown that such a gas approaches, asymptotically with time, an exponential velocity distribution. The second example involves the Fermi mechanism for the acceleration of cosmic rays. Explicit evolution equations are obtained for the distribution of cosmic ray energies within this model, and the steady-state energy distribution that arises when this equation is modified to account for the injection and removal of cosmic rays is discussed. Finally, the author re-examines the multiple-time-scale approach as applied to the study of phase space evolution under a chaotic adiabatic Hamiltonian. This leads to a more rigorous derivation of the above-mentioned Fokker-Planck equation, and also to a new term which has relevance to the problem of chaotic adiabatic reaction forces (the forces acting on slow, heavy degrees of freedom due to their coupling to light, fast chaotic degrees).

  19. POTENTIAL HUMAN STUDY POPULATIONS FOR NON-IONIZING (RADIO FREQUENCY) RADIATION HEALTH EFFECTS

    EPA Science Inventory

    This research project was initiated to identify potential human populations for future epidemiological studies of the health effects of radio frequency radiation. Through a literature search and contacts with various groups and organizations, numerous occupations and applications...

  20. Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules II: Non-Empirically Tuned Long-Range Corrected Hybrid Functionals.

    PubMed

    Gallandi, Lukas; Marom, Noa; Rinke, Patrick; Körzdörfer, Thomas

    2016-02-01

    The performance of non-empirically tuned long-range corrected hybrid functionals for the prediction of vertical ionization potentials (IPs) and electron affinities (EAs) is assessed for a set of 24 organic acceptor molecules. Basis set-extrapolated coupled cluster singles, doubles, and perturbative triples [CCSD(T)] calculations serve as a reference for this study. Compared to standard exchange-correlation functionals, tuned long-range corrected hybrid functionals produce highly reliable results for vertical IPs and EAs, yielding mean absolute errors on par with computationally more demanding GW calculations. In particular, it is demonstrated that long-range corrected hybrid functionals serve as ideal starting points for non-self-consistent GW calculations. PMID:26731340

  1. Increasing the efficiency of CO/sub 2/ transverse electric atmospheric lasers by use of low ionization potential additives

    SciTech Connect

    Cruz, C.H.B.; Fragnito, H.L.

    1981-02-01

    A method for increasing the efficiency of conventional CO/sub 2/ transverse electric atmospheric lasers is presented. We take advantage of the fact that by strongly doping the usual CO/sub 2/:N/sub 2/:He gas mixture with a low ionization potential additive, the plasma sustaining field can be suitably reduced to attain a value optimum for the excitation of the upper laser level of CO/sub 2/. We observed field reductions to as little as 20% of the reported value for the nondoped mixture. This permitted us to increase the CO/sub 2/ excitation efficiency by a factor of 2. We also observed that the laser operating efficiency was increased by reducing the helium concentration in the gas mixture.

  2. Non-Targeted Effects Induced by Ionizing Radiation: Mechanisms and Potential Impact on Radiation Induced Health Effects

    SciTech Connect

    Morgan, William F.; Sowa, Marianne B.

    2015-01-01

    Not-targeted effects represent a paradigm shift from the "DNA centric" view that ionizing radiation only elicits biological effects and subsequent health consequences as a result of an energy deposition event in the cell nucleus. While this is likely true at higher radiation doses (> 1Gy), at low doses (< 100mGy) non-targeted effects associated with radiation exposure might play a significant role. Here definitions of non-targeted effects are presented, the potential mechanisms for the communication of signals and signaling networks from irradiated cells/tissues are proposed, and the various effects of this intra- and intercellular signaling are described. We conclude with speculation on how these observations might lead to and impact long-term human health outcomes.

  3. Second-Order Perturbation Theory for Fractional Occupation Systems: Applications to Ionization Potential and Electron Affinity Calculations.

    PubMed

    Su, Neil Qiang; Xu, Xin

    2016-05-10

    Recently, we have developed an integration approach for the calculations of ionization potentials (IPs) and electron affinities (EAs) of molecular systems at the level of second-order Møller-Plesset (MP2) (Su, N. Q.; Xu, X. J. Chem. Theory Comput. 11, 4677, 2015), where the full MP2 energy gradient with respect to the orbital occupation numbers was derived but only at integer occupations. The theory is completed here to cover the fractional occupation systems, such that Slater's transition state concept can be used to have accurate predictions of IPs and EAs. Antisymmetrized Goldstone diagrams have been employed for interpretations and better understanding of the derived equations, where two additional rules were introduced in the present work specifically for hole or particle lines with fractional occupation numbers. PMID:27010405

  4. An ab initio study of the ionization potentials and f-f spectroscopy of europium atoms and ions.

    SciTech Connect

    Naleway, C.; Seth, M.; Shepard, R.; Wagner, A. F.; Tilson, J. L.; Ermler, W. C.; Brozell, S. R.; Stevens Inst. of Tech.; Ohio State Univ.

    2002-04-01

    The first three ionization potentials of europium and the f-f spectroscopy of the two lowest multiplets of Eu+3 have been calculated using ab initio spin-orbit configuration interaction techniques. To accomplish this, a new averaged relativistic effective core potential has been developed which leaves only the 5s, 5p, and 4f in the valence space. A series of configuration interaction calculations were carried out up through single and partial double excitations with a double-zeta quality basis set. The computed ionization values have an absolute error of about 0.1 eV from the experimental values. The computed f-f spectroscopy for the lowest {sup 7}F multiplet of Eu{sup +3} has a RMS error with experiment of about 100 cm-1. The computed f-f spectroscopy for the first excited {sup 5}D multiplet has a higher RMS error of about 350 cm{sup -1}. The computed center of gravity separation between the {sup 5}D-{sup 7}F multiplet is underestimated by 750 cm{sup -1}. Comparisons between non-spin-orbit and spin-orbit configuration interaction calculations for the separations of the centers of gravity of multiplets are very favorable up through single and double excitations with differences of a tenth of an eV or less. The spin-orbit configuration interaction calculations are among the largest ever performed for lanthanides, with expansion lengths in excess of 1.9 million double-group-adapted functions. The calculations were achieved by application of a new parallel spin-orbit configuration interaction component in the COLUMBUS Program System.

  5. Direct Delta-MBPT(2) method for ionization potentials, electron affinities, and excitation energies using fractional occupation numbers

    SciTech Connect

    Beste, Ariana; Vazquez-Mayagoitia, Alvaro; Ortiz, J. Vincent

    2013-01-01

    A direct method (D-Delta-MBPT(2)) to calculate second-order ionization potentials (IPs), electron affinities (EAs), and excitation energies is developed. The Delta-MBPT(2) method is defined as the correlated extension of the Delta-HF method. Energy differences are obtained by integrating the energy derivative with respect to occupation numbers over the appropriate parameter range. This is made possible by writing the second-order energy as a function of the occupation numbers. Relaxation effects are fully included at the SCF level. This is in contrast to linear response theory, which makes the D-Delta-MBPT(2) applicable not only to single excited but also higher excited states. We show the relationship of the D-Delta-MBPT(2) method for IPs and EAs to a second-order approximation of the effective Fock-space coupled-cluster Hamiltonian and a second-order electron propagator method. We also discuss the connection between the D-Delta-MBPT(2) method for excitation energies and the CIS-MP2 method. Finally, as a proof of principle, we apply our method to calculate ionization potentials and excitation energies of some small molecules. For IPs, the Delta-MBPT(2) results compare well to the second-order solution of the Dyson equation. For excitation energies, the deviation from EOM-CCSD increases when correlation becomes more important. When using the numerical integration technique, we encounter difficulties that prevented us from reaching the Delta-MBPT(2) values. Most importantly, relaxation beyond the Hartree Fock level is significant and needs to be included in future research.

  6. The excited states of K3 cluster: The molecular symmetry adapted non-adiabatic coupling terms and diabatic Hamiltonian matrix

    NASA Astrophysics Data System (ADS)

    Mukherjee, Saikat; Adhikari, Satrajit

    2014-08-01

    We calculate the adiabatic potential energy surfaces (PESs) and the non-adiabatic coupling terms (NACTs) for the excited electronic states of K3 cluster by MRCI approach using MOLPRO. The NACTs are adapted with molecular symmetry to assign appropriate IREPs so that the elements of the Hamiltonian matrix are totally symmetric. We incorporate those NACTs into three-state adiabatic-to-diabatic transformation (ADT) equations to obtain ADT angles for constructing continuous, single-valued, smooth and symmetric diabatic Hamiltonian matrix, where its elements are fitted with analytic functions. Finally, we demonstrate that the dressed diabatic and adiabatic-via-dressed diabatic PECs show prominent topological effect over dressed adiabatic curves.

  7. Methemoglobinemia Hemotoxicity of Some Antimalarial 8-Aminoquinoline Analogues and Their Hydroxylated Derivatives: Density Functional Theory Computation of Ionization Potentials.

    PubMed

    Ding, Yuanqing; Liu, Haining; Tekwani, Babu L; Nanayakkara, N P Dhammika; Khan, Ikhlas A; Walker, Larry A; Doerksen, Robert J

    2016-07-18

    The administration of primaquine (PQ), an essential drug for the treatment and radical cure of malaria, can lead to methemoglobin formation and life-threatening hemolysis for glucose-6-phosphate dehydrogenase deficient patients. The ionization potential (IP, a quantitative measure of the ability to lose an electron) of the metabolites generated by antimalarial 8-aminoquinoline (8-AQ) drugs like PQ has been believed to be correlated in part to this methemoglobinemia hemotoxicity: the lower the IP of an 8-AQ derivative, the higher the concentration of methemoglobin generated. In this work, demethoxylated primaquine (AQ02) was employed as a model, by intensive computation at the B3LYP-SCRF(PCM)/6-311++G**//B3LYP/6-31G** level in water, to study the effects of hydroxylation at various positions on the ionization potential. Compared to the parent AQ02, the IPs of AQ02's metabolites hydroxylated at N1', C5, and C7 were lower by 61, 30, and 19 kJ/mol, respectively, while differences in the IP relative to PQ were small for hydroxylation at all other positions. The C6 position, at which the IP of the hydroxylated metabolite was greater than that of AQ02, by 2 kJ/mol, was found to be unique. Several literature and proposed 8-AQ analogues were studied to evaluate substituent effects on their potential to generate methemoglobin, with the finding that hydroxylations at N1' and C5 contribute the most to the potential hemotoxicity of PQ-based antimalarials, whereas hydroxylation at C7 has little effect. Phenoxylation at C5 in PQ-based 8-AQs can block the hydroxylation at C5 and reduce the potential for methemoglobin generation, while -CF3 and chlorines attached to the phenolic ring can further reduce the risk. The H-shift at N1' during the cationization of hydroxylated metabolites of 8-AQs sharply decreased their IPs, but this effect can be significantly reduced by the introduction of an electron-withdrawing group to the quinoline core. The results and this approach may be

  8. Ionization potentials of transparent conductive indium tin oxide films covered with a single layer of fluorine-doped tin oxide nanoparticles grown by spray pyrolysis deposition

    SciTech Connect

    Fukano, Tatsuo; Motohiro, Tomoyoshi; Ida, Takashi; Hashizume, Hiroo

    2005-04-15

    Indium tin oxide (ITO) films deposited with single layers of monodispersive fluorine-doped tin oxide (FTO) nanoparticles of several nanometers in size were grown on glass substrates by intermittent spray pyrolysis deposition using conventional atomizers. These films have significantly higher ionization potentials than the bare ITO and FTO films grown using the same technique. The ITO films covered with FTO particles of 7 nm in average size show an ionization potential of 5.01 eV, as compared with {approx}4.76 and {approx}4.64 eV in ITO and FTO films, respectively, which decreases as the FTO particle size increases. The ionization potentials are practically invariant against oxidation and reduction treatments, promising a wide application of the films to transparent conducting oxide electrodes in organic electroluminescent devices and light-emitting devices of high efficiencies.

  9. Ionization potentials of transparent conductive indium tin oxide films covered with a single layer of fluorine-doped tin oxide nanoparticles grown by spray pyrolysis deposition

    NASA Astrophysics Data System (ADS)

    Fukano, Tatsuo; Motohiro, Tomoyoshi; Ida, Takashi; Hashizume, Hiroo

    2005-04-01

    Indium tin oxide (ITO) films deposited with single layers of monodispersive fluorine-doped tin oxide (FTO) nanoparticles of several nanometers in size were grown on glass substrates by intermittent spray pyrolysis deposition using conventional atomizers. These films have significantly higher ionization potentials than the bare ITO and FTO films grown using the same technique. The ITO films covered with FTO particles of 7nm in average size show an ionization potential of 5.01eV, as compared with ˜4.76 and ˜4.64eV in ITO and FTO films, respectively, which decreases as the FTO particle size increases. The ionization potentials are practically invariant against oxidation and reduction treatments, promising a wide application of the films to transparent conducting oxide electrodes in organic electroluminescent devices and light-emitting devices of high efficiencies.

  10. Robust adiabatic sum frequency conversion.

    PubMed

    Suchowski, Haim; Prabhudesai, Vaibhav; Oron, Dan; Arie, Ady; Silberberg, Yaron

    2009-07-20

    We discuss theoretically and demonstrate experimentally the robustness of the adiabatic sum frequency conversion method. This technique, borrowed from an analogous scheme of robust population transfer in atomic physics and nuclear magnetic resonance, enables the achievement of nearly full frequency conversion in a sum frequency generation process for a bandwidth up to two orders of magnitude wider than in conventional conversion schemes. We show that this scheme is robust to variations in the parameters of both the nonlinear crystal and of the incoming light. These include the crystal temperature, the frequency of the incoming field, the pump intensity, the crystal length and the angle of incidence. Also, we show that this extremely broad bandwidth can be tuned to higher or lower central wavelengths by changing either the pump frequency or the crystal temperature. The detailed study of the properties of this converter is done using the Landau-Zener theory dealing with the adiabatic transitions in two level systems. PMID:19654679

  11. Adiabaticity in open quantum systems

    NASA Astrophysics Data System (ADS)

    Venuti, Lorenzo Campos; Albash, Tameem; Lidar, Daniel A.; Zanardi, Paolo

    2016-03-01

    We provide a rigorous generalization of the quantum adiabatic theorem for open systems described by a Markovian master equation with time-dependent Liouvillian L (t ) . We focus on the finite system case relevant for adiabatic quantum computing and quantum annealing. Adiabaticity is defined in terms of closeness to the instantaneous steady state. While the general result is conceptually similar to the closed-system case, there are important differences. Namely, a system initialized in the zero-eigenvalue eigenspace of L (t ) will remain in this eigenspace with a deviation that is inversely proportional to the total evolution time T . In the case of a finite number of level crossings, the scaling becomes T-η with an exponent η that we relate to the rate of the gap closing. For master equations that describe relaxation to thermal equilibrium, we show that the evolution time T should be long compared to the corresponding minimum inverse gap squared of L (t ) . Our results are illustrated with several examples.

  12. Quantum dynamics by the constrained adiabatic trajectory method

    SciTech Connect

    Leclerc, A.; Jolicard, G.; Guerin, S.; Killingbeck, J. P.

    2011-03-15

    We develop the constrained adiabatic trajectory method (CATM), which allows one to solve the time-dependent Schroedinger equation constraining the dynamics to a single Floquet eigenstate, as if it were adiabatic. This constrained Floquet state (CFS) is determined from the Hamiltonian modified by an artificial time-dependent absorbing potential whose forms are derived according to the initial conditions. The main advantage of this technique for practical implementation is that the CFS is easy to determine even for large systems since its corresponding eigenvalue is well isolated from the others through its imaginary part. The properties and limitations of the CATM are explored through simple examples.

  13. Spatial adiabatic passage: a review of recent progress

    NASA Astrophysics Data System (ADS)

    Menchon-Enrich, R.; Benseny, A.; Ahufinger, V.; Greentree, A. D.; Busch, Th; Mompart, J.

    2016-07-01

    Adiabatic techniques are known to allow for engineering quantum states with high fidelity. This requirement is currently of large interest, as applications in quantum information require the preparation and manipulation of quantum states with minimal errors. Here we review recent progress on developing techniques for the preparation of spatial states through adiabatic passage, particularly focusing on three state systems. These techniques can be applied to matter waves in external potentials, such as cold atoms or electrons, and to classical waves in waveguides, such as light or sound.

  14. Spatial adiabatic passage: a review of recent progress.

    PubMed

    Menchon-Enrich, R; Benseny, A; Ahufinger, V; Greentree, A D; Busch, Th; Mompart, J

    2016-07-01

    Adiabatic techniques are known to allow for engineering quantum states with high fidelity. This requirement is currently of large interest, as applications in quantum information require the preparation and manipulation of quantum states with minimal errors. Here we review recent progress on developing techniques for the preparation of spatial states through adiabatic passage, particularly focusing on three state systems. These techniques can be applied to matter waves in external potentials, such as cold atoms or electrons, and to classical waves in waveguides, such as light or sound. PMID:27245462

  15. Interaction-induced adiabatic cooling for antiferromagnetism in optical lattices

    SciTech Connect

    Dare, A.-M.; Raymond, L.; Albinet, G.; Tremblay, A.-M. S.

    2007-08-01

    In the experimental context of cold-fermion optical lattices, we discuss the possibilities to approach the pseudogap or ordered phases by manipulating the scattering length or the strength of the laser-induced lattice potential. Using the two-particle self-consistent approach, as well as quantum Monte Carlo simulations, we provide isentropic curves for the two- and three-dimensional Hubbard models at half-filling. These quantitative results are important for practical attempts to reach the ordered antiferromagnetic phase in experiments on optical lattices of two-component fermions. We find that adiabatically turning on the interaction in two dimensions to cool the system is not very effective. In three dimensions, adiabatic cooling to the antiferromagnetic phase can be achieved in such a manner, although the cooling efficiency is not as high as initially suggested by dynamical mean-field theory. Adiabatic cooling by turning off the repulsion beginning at strong coupling is possible in certain cases.

  16. The density temperature and the dry and wet virtual adiabats

    NASA Technical Reports Server (NTRS)

    Bartlo, J.; Betts, Alan K.

    1991-01-01

    A density temperature is introduced to represent virtual temperature and potential temperature on thermodynamic diagrams. This study reviews how the dry and wet virtual adiabats can be used to represent stability and air parcel density for unsaturated and cloudy air, and present formula and tabulations.

  17. Effect of the Heat Pipe Adiabatic Region.

    PubMed

    Brahim, Taoufik; Jemni, Abdelmajid

    2014-04-01

    The main motivation of conducting this work is to present a rigorous analysis and investigation of the potential effect of the heat pipe adiabatic region on the flow and heat transfer performance of a heat pipe under varying evaporator and condenser conditions. A two-dimensional steady-state model for a cylindrical heat pipe coupling, for both regions, is presented, where the flow of the fluid in the porous structure is described by Darcy-Brinkman-Forchheimer model which accounts for the boundary and inertial effects. The model is solved numerically by using the finite volumes method, and a fortran code was developed to solve the system of equations obtained. The results show that a phase change can occur in the adiabatic region due to temperature gradient created in the porous structure as the heat input increases and the heat pipe boundary conditions change. A recirculation zone may be created at the condenser end section. The effect of the heat transfer rate on the vapor radial velocities and the performance of the heat pipe are discussed. PMID:24895467

  18. Invalidity of the quantitative adiabatic condition and general conditions for adiabatic approximations

    NASA Astrophysics Data System (ADS)

    Li, Dafa

    2016-05-01

    The adiabatic theorem was proposed about 90 years ago and has played an important role in quantum physics. The quantitative adiabatic condition constructed from eigenstates and eigenvalues of a Hamiltonian is a traditional tool to estimate adiabaticity and has proven to be the necessary and sufficient condition for adiabaticity. However, recently the condition has become a controversial subject. In this paper, we list some expressions to estimate the validity of the adiabatic approximation. We show that the quantitative adiabatic condition is invalid for the adiabatic approximation via the Euclidean distance between the adiabatic state and the evolution state. Furthermore, we deduce general necessary and sufficient conditions for the validity of the adiabatic approximation by different definitions.

  19. Spatially Resolved Plant Metabolomics: Some Potentials and Limitations of Laser-Ablation Electrospray Ionization Mass Spectrometry Metabolite Imaging1[OPEN

    PubMed Central

    Etalo, Desalegn W.; De Vos, Ric C.H.; Joosten, Matthieu H.A.J.; Hall, Robert D.

    2015-01-01

    Laser-ablation electrospray ionization (LAESI)-mass spectrometry imaging has been applied to contrasting plant organs to assess its potential as a procedure for performing in vivo metabolomics in plants. In a proof-of-concept experiment, purple/white segmented Phalaenopsis spp. petals were first analyzed using standard liquid chromatography-mass spectrometry analyses of separate extracts made specifically from the purple and white regions. Discriminatory compounds were defined and putatively annotated. LAESI analyses were then performed on living tissues, and these metabolites were then relocalized within the LAESI-generated data sets of similar tissues. Maps were made to illustrate their locations across the petals. Results revealed that, as expected, anthocyanins always mapped to the purple regions. Certain other (nonvisible) polyphenols were observed to colocalize with the anthocyanins, whereas others were found specifically within the white tissues. In a contrasting example, control and Cladosporium fulvum-infected tomato (Solanum lycopersicum) leaves were subjected to the same procedures, and it could be observed that the alkaloid tomatine has clear heterogeneous distribution across the tomato leaf lamina. Furthermore, LAESI analyses revealed perturbations in alkaloid content following pathogen infection. These results show the clear potential of LAESI-based imaging approaches as a convenient and rapid way to perform metabolomics analyses on living tissues. However, a range of limitations and factors have also been identified that must be taken into consideration when interpreting LAESI-derived data. Such aspects deserve further evaluation before this approach can be applied in a routine manner. PMID:26392264

  20. Continuum ionization transition probabilities of atomic oxygen

    NASA Technical Reports Server (NTRS)

    Samson, J. R.; Petrosky, V. E.

    1973-01-01

    The technique of photoelectron spectroscopy was used to obtain the relative continuum transition probabilities of atomic oxygen at 584 A for transitions from 3P ground state into the 4S, D2, and P2 states of the ion. Transition probability ratios for the D2 and P2 states relative to the S4 state of the ion are 1.57 + or - 0.14 and 0.82 + or - 0.07, respectively. In addition, transitions from excited O2(a 1 Delta g) state into the O2(+)(2 Phi u and 2 Delta g) were observed. The adiabatic ionization potential of O2(+)(2 Delta g) was measured as 18.803 + or - 0.006 eV.

  1. Adiabatic Wankel type rotary engine

    NASA Technical Reports Server (NTRS)

    Kamo, R.; Badgley, P.; Doup, D.

    1988-01-01

    This SBIR Phase program accomplished the objective of advancing the technology of the Wankel type rotary engine for aircraft applications through the use of adiabatic engine technology. Based on the results of this program, technology is in place to provide a rotor and side and intermediate housings with thermal barrier coatings. A detailed cycle analysis of the NASA 1007R Direct Injection Stratified Charge (DISC) rotary engine was performed which concluded that applying thermal barrier coatings to the rotor should be successful and that it was unlikely that the rotor housing could be successfully run with thermal barrier coatings as the thermal stresses were extensive.

  2. Adiabatic Mass Loss Model in Binary Stars

    NASA Astrophysics Data System (ADS)

    Ge, H. W.

    2012-07-01

    onset of dynamical time scale mass transfer; if the ratio of donor to accretor masses exceeds this critical value, the dynamical time scale mass transfer ensues. The grid of criterion for all stars can be used to be the basic input as the binary population synthetic method, which will be improved absolutely. In common envelope evolution, the dissipation of orbital energy of the binary provides the energy to eject the common envelope; the energy budget for this process essentially consists of the initial orbital energy of the binary and the initial binding energies of the binary components. We emphasize that, because stellar core and envelope contribute mutually to each other's gravitational potential energy, proper evaluation of the total energy of a star requires integration over the entire stellar interior, not the ejected envelope alone as commonly assumed. We show that the change in total energy of the donor star, as a function of its remaining mass along an adiabatic mass-loss sequence, can be calculated. This change in total energy of the donor star, combined with the requirement that both remnant donor and its companion star fit within their respective Roche lobes, then circumscribes energetically possible survivors of common envelope evolution. It is the first time that we can calculate the accurate total energy of the donor star in common envelope evolution, while the results with the old method are inconsistent with observations.

  3. Relativistic equation-of-motion coupled-cluster method using open-shell reference wavefunction: Application to ionization potential.

    PubMed

    Pathak, Himadri; Sasmal, Sudip; Nayak, Malaya K; Vaval, Nayana; Pal, Sourav

    2016-08-21

    The open-shell reference relativistic equation-of-motion coupled-cluster method within its four-component description is successfully implemented with the consideration of single- and double- excitation approximations using the Dirac-Coulomb Hamiltonian. At the first attempt, the implemented method is employed to calculate ionization potential value of heavy atomic (Ag, Cs, Au, Fr, and Lr) and molecular (HgH and PbF) systems, where the effect of relativity does really matter to obtain highly accurate results. Not only the relativistic effect but also the effect of electron correlation is crucial in these heavy atomic and molecular systems. To justify the fact, we have taken two further approximations in the four-component relativistic equation-of-motion framework to quantify how the effect of electron correlation plays a role in the calculated values at different levels of theory. All these calculated results are compared with the available experimental data as well as with other theoretically calculated values to judge the extent of accuracy obtained in our calculations. PMID:27544090

  4. Sequence and conformation effects on ionization potential and charge distribution of homo-nucleobase stacks using M06-2X hybrid density functional theory calculations.

    PubMed

    Rooman, Marianne; Wintjens, René

    2014-04-01

    DNA is subject to oxidative damage due to radiation or by-products of cellular metabolism, thereby creating electron holes that migrate along the DNA stacks. A systematic computational analysis of the dependence of the electronic properties of nucleobase stacks on sequence and conformation was performed here, on the basis of single- and double-stranded homo-nucleobase stacks of 1-10 bases or 1-8 base pairs in standard A-, B-, and Z-conformation. First, several levels of theory were tested for calculating the vertical ionization potentials of individual nucleobases; the M06-2X/6-31G* hybrid density functional theory method was selected by comparison with experimental data. Next, the vertical ionization potential, and the Mulliken charge and spin density distributions were calculated and considered on all nucleobase stacks. We found that (1) the ionization potential decreases with the number of bases, the lowest being reached by Gua≡Cyt tracts; (2) the association of two single strands into a double-stranded tract lowers the ionization potential significantly (3) differences in ionization potential due to sequence variation are roughly three times larger than those due to conformational modifications. The charge and spin density distributions were found (1) to be located toward the 5'-end for single-stranded Gua-stacks and toward the 3'-end for Cyt-stacks and basically delocalized over all bases for Ade- and Thy-stacks; (2) the association into double-stranded tracts empties the Cyt- and Thy-strands of most of the charge and all the spin density and concentrates them on the Gua- and Ade-strands. The possible biological implications of these results for transcription are discussed. PMID:23582046

  5. Sequence and conformation effects on ionization potential and charge distribution of homo-nucleobase stacks using M06-2X hybrid density functional theory calculations

    PubMed Central

    Rooman, Marianne; Wintjens, René

    2013-01-01

    DNA is subject to oxidative damage due to radiation or by-products of cellular metabolism, thereby creating electron holes that migrate along the DNA stacks. A systematic computational analysis of the dependence of the electronic properties of nucleobase stacks on sequence and conformation was performed here, on the basis of single- and double-stranded homo-nucleobase stacks of 1–10 bases or 1–8 base pairs in standard A-, B-, and Z-conformation. First, several levels of theory were tested for calculating the vertical ionization potentials of individual nucleobases; the M06-2X/6-31G* hybrid density functional theory method was selected by comparison with experimental data. Next, the vertical ionization potential, and the Mulliken charge and spin density distributions were calculated and considered on all nucleobase stacks. We found that (1) the ionization potential decreases with the number of bases, the lowest being reached by Gua≡Cyt tracts; (2) the association of two single strands into a double-stranded tract lowers the ionization potential significantly (3) differences in ionization potential due to sequence variation are roughly three times larger than those due to conformational modifications. The charge and spin density distributions were found (1) to be located toward the 5′-end for single-stranded Gua-stacks and toward the 3′-end for Cyt-stacks and basically delocalized over all bases for Ade- and Thy-stacks; (2) the association into double-stranded tracts empties the Cyt- and Thy-strands of most of the charge and all the spin density and concentrates them on the Gua- and Ade-strands. The possible biological implications of these results for transcription are discussed. PMID:23582046

  6. Failure of geometric electromagnetism in the adiabatic vector Kepler problem

    SciTech Connect

    Anglin, J.R.; Schmiedmayer, J.

    2004-02-01

    The magnetic moment of a particle orbiting a straight current-carrying wire may precess rapidly enough in the wire's magnetic field to justify an adiabatic approximation, eliminating the rapid time dependence of the magnetic moment and leaving only the particle position as a slow degree of freedom. To zeroth order in the adiabatic expansion, the orbits of the particle in the plane perpendicular to the wire are Keplerian ellipses. Higher-order postadiabatic corrections make the orbits precess, but recent analysis of this 'vector Kepler problem' has shown that the effective Hamiltonian incorporating a postadiabatic scalar potential ('geometric electromagnetism') fails to predict the precession correctly, while a heuristic alternative succeeds. In this paper we resolve the apparent failure of the postadiabatic approximation, by pointing out that the correct second-order analysis produces a third Hamiltonian, in which geometric electromagnetism is supplemented by a tensor potential. The heuristic Hamiltonian of Schmiedmayer and Scrinzi is then shown to be a canonical transformation of the correct adiabatic Hamiltonian, to second order. The transformation has the important advantage of removing a 1/r{sup 3} singularity which is an artifact of the adiabatic approximation.

  7. Entropy in Adiabatic Regions of Convection Simulations

    NASA Astrophysics Data System (ADS)

    Tanner, Joel D.; Basu, Sarbani; Demarque, Pierre

    2016-05-01

    One of the largest sources of uncertainty in stellar models is caused by the treatment of convection in stellar envelopes. One-dimensional stellar models often make use of the mixing length or equivalent approximations to describe convection, all of which depend on various free parameters. There have been attempts to rectify this by using 3D radiative-hydrodynamic simulations of stellar convection, and in trying to extract an equivalent mixing length from the simulations. In this Letter, we show that the entropy of the deeper, adiabatic layers in these simulations can be expressed as a simple function of {log}g and {log}{T}{{eff}}, which holds potential for calibrating stellar models in a simple and more general manner.

  8. Sliding seal materials for adiabatic engines

    NASA Technical Reports Server (NTRS)

    Lankford, J.

    1985-01-01

    The sliding friction coefficients and wear rates of promising carbide, oxide, and nitride materials were measured under temperature, environmental, velocity, loading conditions that are representative of the adiabatic engine environment. In order to provide guidance needed to improve materials for this application, the program stressed fundamental understanding of the mechanisms involved in friction and wear. Microhardness tests were performed on the candidate materials at elevated temperatures, and in atmospheres relevant to the piston seal application, and optical and electron microscopy were used to elucidate the micromechanisms of wear following wear testing. X-ray spectroscopy was used to evaluate interface/environment interactions which seemed to be important in the friction and wear process. Electrical effects in the friction and wear processes were explored in order to evaluate the potential usefulness of such effects in modifying the friction and wear rates in service. However, this factor was found to be of negligible significance in controlling friction and wear.

  9. Trace element mass balance in hydrous adiabatic mantle melting: The Hydrous Adiabatic Mantle Melting Simulator version 1 (HAMMS1)

    NASA Astrophysics Data System (ADS)

    Kimura, Jun-Ichi; Kawabata, Hiroshi

    2014-06-01

    numerical mass balance calculation model for the adiabatic melting of a dry to hydrous peridotite has been programmed in order to simulate the trace element compositions of basalts from mid-ocean ridges, back-arc basins, ocean islands, and large igneous provinces. The Excel spreadsheet-based calculator, Hydrous Adiabatic Mantle Melting Simulator version 1 (HAMMS1) uses (1) a thermodynamic model of fractional adiabatic melting of mantle peridotite, with (2) the parameterized experimental melting relationships of primitive to depleted mantle sources in terms of pressure, temperature, water content, and degree of partial melting. The trace element composition of the model basalt is calculated from the accumulated incremental melts within the adiabatic melting regime, with consideration for source depletion. The mineralogic mode in the primitive to depleted source mantle in adiabat is calculated using parameterized experimental results. Partition coefficients of the trace elements of mantle minerals are parameterized to melt temperature mostly from a lattice strain model and are tested using the latest compilations of experimental results. The parameters that control the composition of trace elements in the model are as follows: (1) mantle potential temperature, (2) water content in the source mantle, (3) depth of termination of adiabatic melting, and (4) source mantle depletion. HAMMS1 enables us to obtain the above controlling parameters using Monte Carlo fitting calculations and by comparing the calculated basalt compositions to primary basalt compositions. Additionally, HAMMS1 compares melting parameters with a major element model, which uses petrogenetic grids formulated from experimental results, thus providing better constraints on the source conditions.

  10. Ionization Thresholds of Small Carbon Clusters: Tunable VUVExperiments and Theory

    SciTech Connect

    Belau, Leonid; Wheeler, Steven E.; Ticknor, Brian W.; Ahmed,Musahid; Leone, Stephen R.; Allen, Wesley D.; Schaefer III, Henry F.; Duncan, Michael A.

    2007-07-31

    Small carbon clusters (Cn, n = 2-15) are produced in amolecular beam by pulsed laser vaporization and studied with vacuumultraviolet (VUV) photoionization mass spectrometry. The required VUVradiation in the 8-12 eV range is provided by the Advanced Light Source(ALS) at the Lawrence Berkeley National Laboratory. Mass spectra atvarious ionization energies reveal the qualitative relative abundances ofthe neutral carbon clusters produced. By far the most abundant species isC3. Using the tunability of the ALS, ionization threshold spectra arerecorded for the clusters up to 15 atoms in size. The ionizationthresholds are compared to those measured previously with charge-transferbracketing methods. To interpret the ionization thresholds for differentcluster sizes, new ab initio calculations are carried out on the clustersfor n = 4-10. Geometric structures are optimized at the CCSD(T) levelwith cc-pVTZ (or cc-pVDZ) basis sets, and focal point extrapolations areapplied to both neutral and cation species to determine adiabatic andvertical ionization potentials. The comparison of computed and measuredionization potentials makes it possible to investigate the isomericstructures of the neutral clusters produced in this experiment. Themeasurements are inconclusive for the n = 4-6 species because ofunquenched excited electronic states. However, the data provide evidencefor the prominence of linear structures for the n = 7, 9, 11, 13 speciesand the presence of cyclic C10.

  11. Adiabatic trapping in coupled kinetic Alfven-acoustic waves

    SciTech Connect

    Shah, H. A.; Ali, Z.; Masood, W.

    2013-03-15

    In the present work, we have discussed the effects of adiabatic trapping of electrons on obliquely propagating Alfven waves in a low {beta} plasma. Using the two potential theory and employing the Sagdeev potential approach, we have investigated the existence of arbitrary amplitude coupled kinetic Alfven-acoustic solitary waves in both the sub and super Alfvenic cases. The results obtained have been analyzed and presented graphically and can be applied to regions of space where the low {beta} assumption holds true.

  12. Investigations of the potential functions of weakly bound diatomic molecules and laser-assisted excitive Penning ionization

    SciTech Connect

    Goble, J.H. Jr.

    1982-05-01

    Three variations on the Dunham series expansion function of the potential of a diatomic molecule are compared. The differences among these expansions lie in the choice of the expansion variable, lambda. The functional form of these variables are lambda/sub s/ = l-r/sub e//r for the Simon-Parr-Finlan version, lambda/sub T/ - 1-(r/sub e//r)/sup p/ for that of Thakkar, and lambda/sub H/ = 1-exp(-rho(r/r/sub e/-1) for that of Huffaker. A wide selection of molecular systems are examined. It is found that, for potentials in excess of thirty kcal/mole, the Huffaker expansion provides the best description of the three, extrapolating at large internuclear separation to a value within 10% of the true dissociation energy. For potentials that result from the interaction of excited states, all series expansions show poor behavior away from the equilibrium internuclear separation of the molecule. The series representation of the potentials of weakly bound molecules are examined in more detail. The ground states of BeAr/sup +/, HeNe/sup +/, NaAr, and Ar/sub 2/ and the excited states of HeNe+, NaNe, and NaAr are best described by the Thakkar expansion. Finally, the observation of laser-assisted excitive Penning ionization in a flowing afterglow is reported. The reaction Ar(/sup 3/P/sub 2/) + Ca + h nu ..-->.. Ar + Ca/sup +/(5p /sup 2/P/sub J/) + e/sup -/ occurs when the photon energy, h nu, is approximately equal to the energy difference between the metastable argon and one of the fine structure levels of the ion's doublet. By monitoring the cascade fluorescence of the above reaction and comparing it to the flourescence from the field-free process Ar(/sup 3/P/sub 2/) + Ca ..-->.. Ar + Ca/sup +/(4p /sup 2/P/sub J/) + e/sup -/ a surprisingly large cross section of 6.7 x 10/sup 3/ A/sup 2/ is estimated.

  13. Degenerate adiabatic perturbation theory: Foundations and applications

    NASA Astrophysics Data System (ADS)

    Rigolin, Gustavo; Ortiz, Gerardo

    2014-08-01

    We present details and expand on the framework leading to the recently introduced degenerate adiabatic perturbation theory [Phys. Rev. Lett. 104, 170406 (2010), 10.1103/PhysRevLett.104.170406], and on the formulation of the degenerate adiabatic theorem, along with its necessary and sufficient conditions [given in Phys. Rev. A 85, 062111 (2012), 10.1103/PhysRevA.85.062111]. We start with the adiabatic approximation for degenerate Hamiltonians that paves the way to a clear and rigorous statement of the associated degenerate adiabatic theorem, where the non-Abelian geometric phase (Wilczek-Zee phase) plays a central role to its quantitative formulation. We then describe the degenerate adiabatic perturbation theory, whose zeroth-order term is the degenerate adiabatic approximation, in its full generality. The parameter in the perturbative power-series expansion of the time-dependent wave function is directly associated to the inverse of the time it takes to drive the system from its initial to its final state. With the aid of the degenerate adiabatic perturbation theory we obtain rigorous necessary and sufficient conditions for the validity of the adiabatic theorem of quantum mechanics. Finally, to illustrate the power and wide scope of the methodology, we apply the framework to a degenerate Hamiltonian, whose closed-form time-dependent wave function is derived exactly, and also to other nonexactly solvable Hamiltonians whose solutions are numerically computed.

  14. Metronomic Small Molecule Inhibitor of Bcl-2 (TW-37) Is Antiangiogenic and Potentiates the Antitumor Effect of Ionizing Radiation

    SciTech Connect

    Zeitlin, Benjamin D.; Spalding, Aaron C.; Campos, Marcia S.; Ashimori, Naoki; Dong Zhihong; Wang Shaomeng; Lawrence, Theodore S.; Noer, Jacques E.

    2010-11-01

    Purpose: To investigate the effect of a metronomic (low-dose, high-frequency) small-molecule inhibitor of Bcl-2 (TW-37) in combination with radiotherapy on microvascular endothelial cells in vitro and in tumor angiogenesis in vivo. Methods and Materials: Primary human dermal microvascular endothelial cells were exposed to ionizing radiation and/or TW-37 and colony formation, as well as capillary sprouting in three-dimensional collagen matrices, was evaluated. Xenografts vascularized with human blood vessels were engineered by cotransplantation of human squamous cell carcinoma cells (OSCC3) and human dermal microvascular endothelial cells seeded in highly porous biodegradable scaffolds into the subcutaneous space of immunodeficient mice. Mice were treated with metronomic TW-37 and/or radiation, and tumor growth was evaluated. Results: Low-dose TW-37 sensitized primary endothelial cells to radiation-induced inhibition of colony formation. Low-dose TW-37 or radiation partially inhibited endothelial cell sprout formation, and in combination, these therapies abrogated new sprouting. Combination of metronomic TW-37 and low-dose radiation inhibited tumor growth and resulted in significant increase in time to failure compared with controls, whereas single agents did not. Notably, histopathologic analysis revealed that tumors treated with TW-37 (with or without radiation) are more differentiated and showed more cohesive invasive fronts, which is consistent with less aggressive phenotype. Conclusions: These results demonstrate that metronomic TW-37 potentiates the antitumor effects of radiotherapy and suggest that patients with head and neck cancer might benefit from the combination of small molecule inhibitor of Bcl-2 and radiation therapy.

  15. Shortcut to adiabatic gate teleportation

    NASA Astrophysics Data System (ADS)

    Santos, Alan C.; Silva, Raphael D.; Sarandy, Marcelo S.

    2016-01-01

    We introduce a shortcut to the adiabatic gate teleportation model of quantum computation. More specifically, we determine fast local counterdiabatic Hamiltonians able to implement teleportation as a universal computational primitive. In this scenario, we provide the counterdiabatic driving for arbitrary n -qubit gates, which allows to achieve universality through a variety of gate sets. Remarkably, our approach maps the superadiabatic Hamiltonian HSA for an arbitrary n -qubit gate teleportation into the implementation of a rotated superadiabatic dynamics of an n -qubit state teleportation. This result is rather general, with the speed of the evolution only dictated by the quantum speed limit. In particular, we analyze the energetic cost for different Hamiltonian interpolations in the context of the energy-time complementarity.

  16. Quantum gates with controlled adiabatic evolutions

    NASA Astrophysics Data System (ADS)

    Hen, Itay

    2015-02-01

    We introduce a class of quantum adiabatic evolutions that we claim may be interpreted as the equivalents of the unitary gates of the quantum gate model. We argue that these gates form a universal set and may therefore be used as building blocks in the construction of arbitrary "adiabatic circuits," analogously to the manner in which gates are used in the circuit model. One implication of the above construction is that arbitrary classical boolean circuits as well as gate model circuits may be directly translated to adiabatic algorithms with no additional resources or complexities. We show that while these adiabatic algorithms fail to exhibit certain aspects of the inherent fault tolerance of traditional quantum adiabatic algorithms, they may have certain other experimental advantages acting as quantum gates.

  17. On a Nonlinear Model in Adiabatic Evolutions

    NASA Astrophysics Data System (ADS)

    Sun, Jie; Lu, Song-Feng

    2016-08-01

    In this paper, we study a kind of nonlinear model of adiabatic evolution in quantum search problem. As will be seen here, for this problem, there always exists a possibility that this nonlinear model can successfully solve the problem, while the linear model can not. Also in the same setting, when the overlap between the initial state and the final stare is sufficiently large, a simple linear adiabatic evolution can achieve O(1) time efficiency, but infinite time complexity for the nonlinear model of adiabatic evolution is needed. This tells us, it is not always a wise choice to use nonlinear interpolations in adiabatic algorithms. Sometimes, simple linear adiabatic evolutions may be sufficient for using. Supported by the National Natural Science Foundation of China under Grant Nos. 61402188 and 61173050. The first author also gratefully acknowledges the support from the China Postdoctoral Science Foundation under Grant No. 2014M552041

  18. Competitive bond rupture in the photodissociation of bromoacetyl chloride and 2- and 3-bromopropionyl chloride: adiabatic versus diabatic dissociation.

    PubMed

    Hsu, Ming-Yi; Tsai, Po-Yu; Wei, Zheng-Rong; Chao, Meng-Hsuan; Zhang, Bing; Kasai, Toshio; Lin, King-Chuen

    2013-04-01

    Competitive bond dissociation mechanisms for bromoacetyl chloride and 2- and 3-bromopropionyl chloride following the (1) [n(O)→π*(C=O)] transition at 234-235 nm are investigated. Branching ratios for C−Br/C−Cl bond fission are found by using the (2+1) resonance-enhanced multiphoton ionization (REMPI) technique coupled with velocity ion imaging. The fragment branching ratios depend mainly on the dissociation pathways and the distances between the orbitals of Br and the C=O chromophore. C−Cl bond fission is anticipated to follow an adiabatic potential surface for a strong diabatic coupling between the n(O)π*(C=O) and np (Cl)σ*(C−Cl) bands. In contrast, C−Br bond fission is subject to much weaker coupling between n(O)π*(C=O) and np (Br)σ*(C−Br). Thus, a diabatic pathway is preferred for bromoacetyl chloride and 2-bromopropionyl chloride, which leads to excited-state products. For 3-bromopropionyl chloride, the available energy is not high enough to reach the excited-state products such that C−Br bond fission must proceed through an adiabatic pathway with severe suppression by nonadiabatic coupling. The fragment translational energies and anisotropy parameters for the three molecules are also analyzed and appropriately interpreted. PMID:23400968

  19. Ionization photophysics and spectroscopy of cyanoacetylene.

    PubMed

    Leach, Sydney; Garcia, Gustavo A; Mahjoub, Ahmed; Bénilan, Yves; Fray, Nicolas; Gazeau, Marie-Claire; Gaie-Levrel, François; Champion, Norbert; Schwell, Martin

    2014-05-01

    Photoionization of cyanoacetylene was studied using synchrotron radiation over the non-dissociative ionization excitation range 11-15.6 eV, with photoelectron-photoion coincidence techniques. The absolute ionization cross-section and spectroscopic aspects of the parent ion were recorded. The adiabatic ionization energy of cyanoacetylene was measured as 11.573 ± 0.010 eV. A detailed analysis of photoelectron spectra of HC3N involves new aspects and new assignments of the vibrational components to excitation of the A(2)Σ(+) and B(2)Π states of the cation. Some of the structured autoionization features observed in the 11.94 to 15.5 eV region of the total ion yield (TIY) spectrum were assigned to two Rydberg series converging to the B(2)Π state of HC3N(+). A number of the measured TIY features are suggested to be vibrational components of Rydberg series converging to the C(2)Σ(+) state of HC3N(+) at ≈17.6 eV and others to valence shell transitions of cyanoacetylene in the 11.6-15 eV region. The results of quantum chemical calculations of the cation electronic state geometries, vibrational frequencies and energies, as well as of the C-H dissociation potential energy profiles of the ground and electronic excited states of the ion, are compared with experimental observations. Ionization quantum yields are evaluated and discussed and the problem of adequate calibration of photoionization cross-sections is raised. PMID:24811639

  20. Ionization photophysics and spectroscopy of cyanoacetylene

    SciTech Connect

    Leach, Sydney; Champion, Norbert; Garcia, Gustavo A.; Fray, Nicolas; Gaie-Levrel, François; Mahjoub, Ahmed; Bénilan, Yves; Gazeau, Marie-Claire; Schwell, Martin

    2014-05-07

    Photoionization of cyanoacetylene was studied using synchrotron radiation over the non-dissociative ionization excitation range 11–15.6 eV, with photoelectron-photoion coincidence techniques. The absolute ionization cross-section and spectroscopic aspects of the parent ion were recorded. The adiabatic ionization energy of cyanoacetylene was measured as 11.573 ± 0.010 eV. A detailed analysis of photoelectron spectra of HC{sub 3}N involves new aspects and new assignments of the vibrational components to excitation of the A{sup 2}Σ{sup +} and B{sup 2}Π states of the cation. Some of the structured autoionization features observed in the 11.94 to 15.5 eV region of the total ion yield (TIY) spectrum were assigned to two Rydberg series converging to the B{sup 2}Π state of HC{sub 3}N{sup +}. A number of the measured TIY features are suggested to be vibrational components of Rydberg series converging to the C{sup 2}Σ{sup +} state of HC{sub 3}N{sup +} at ≈17.6 eV and others to valence shell transitions of cyanoacetylene in the 11.6–15 eV region. The results of quantum chemical calculations of the cation electronic state geometries, vibrational frequencies and energies, as well as of the C–H dissociation potential energy profiles of the ground and electronic excited states of the ion, are compared with experimental observations. Ionization quantum yields are evaluated and discussed and the problem of adequate calibration of photoionization cross-sections is raised.

  1. Equation of motion coupled cluster methods for electron attachment and ionization potential in fullerenes C{sub 60} and C{sub 70}

    SciTech Connect

    Bhaskaran-Nair, Kiran; Kowalski, Karol; Moreno, Juana; Jarrell, Mark; Shelton, William A.

    2014-08-21

    In both molecular and periodic solid-state systems there is a need for the accurate determination of the ionization potential and the electron affinity for systems ranging from light harvesting polymers and photocatalytic compounds to semiconductors. The development of a Green's function approach based on the coupled cluster (CC) formalism would be a valuable tool for addressing many properties involving many-body interactions along with their associated correlation functions. As a first step in this direction, we have developed an accurate and parallel efficient approach based on the equation of motion-CC technique. To demonstrate the high degree of accuracy and numerical efficiency of our approach we calculate the ionization potential and electron affinity for C{sub 60} and C{sub 70}. Accurate predictions for these molecules are well beyond traditional molecular scale studies. We compare our results with experiments and both quantum Monte Carlo and GW calculations.

  2. Ionization Energies and Aqueous Redox Potentials of Organic Molecules: Comparison of DFT, Correlated ab Initio Theory and Pair Natural Orbital Approaches.

    PubMed

    Isegawa, Miho; Neese, Frank; Pantazis, Dimitrios A

    2016-05-10

    The calculation of redox potentials involves large energetic terms arising from gas phase ionization energies, thermodynamic contributions, and solvation energies of the reduced and oxidized species. In this work we study the performance of a wide range of wave function and density functional theory methods for the prediction of ionization energies and aqueous one-electron oxidation potentials of a set of 19 organic molecules. Emphasis is placed on evaluating methods that employ the computationally efficient local pair natural orbital (LPNO) approach, as well as several implementations of coupled cluster theory and explicitly correlated F12 methods. The electronic energies are combined with implicit solvation models for the solvation energies. With the exception of MP2 and its variants, which suffer from enormous errors arising at least partially from the poor Hartree-Fock reference, ionization energies can be systematically predicted with average errors below 0.1 eV for most of the correlated wave function based methods studies here, provided basis set extrapolation is performed. LPNO methods are the most efficient way to achieve this type of accuracy. DFT methods show in general larger errors and suffer from inconsistent behavior. The only exception is the M06-2X functional which is found to be competitive with the best LPNO-based approaches for ionization energies. Importantly, the limiting factor for the calculation of accurate redox potentials is the solvation energy. The errors in the predicted solvation energies by all continuum solvation models tested in this work dominate the final computed reduction potential, resulting in average errors typically in excess of 0.3 V and hence obscuring the gains that arise from choosing a more accurate electronic structure method. PMID:27065224

  3. Non-adiabatic dynamics of molecules in optical cavities

    NASA Astrophysics Data System (ADS)

    Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

    2016-02-01

    Strong coupling of molecules to the vacuum field of micro cavities can modify the potential energy surfaces thereby opening new photophysical and photochemical reaction pathways. While the influence of laser fields is usually described in terms of classical field, coupling to the vacuum state of a cavity has to be described in terms of dressed photon-matter states (polaritons) which require quantized fields. We present a derivation of the non-adiabatic couplings for single molecules in the strong coupling regime suitable for the calculation of the dressed state dynamics. The formalism allows to use quantities readily accessible from quantum chemistry codes like the adiabatic potential energy surfaces and dipole moments to carry out wave packet simulations in the dressed basis. The implications for photochemistry are demonstrated for a set of model systems representing typical situations found in molecules.

  4. Adiabatic two-photon quantum gate operations using a long-range photonic bus

    NASA Astrophysics Data System (ADS)

    Hope, Anthony P.; Nguyen, Thach G.; Mitchell, Arnan; Greentree, Andrew D.

    2015-03-01

    Adiabatic techniques have much potential to realize practical and robust optical waveguide devices. Traditionally, photonic elements are limited to coupling schemes that rely on proximity to nearest neighbour elements. We combine adiabatic passage with a continuum based long-range optical bus to break free from such topological restraints and thereby outline a new approach to photonic quantum gate design. We explicitly show designs for adiabatic quantum gates that produce a Hadamard, 50:50 and 1/3:2/3 beam splitter, and non-deterministic controlled NOT gate based on planar thin, shallow ridge waveguides. Our calculations are performed under conditions of one and two-photon inputs.

  5. Arbitrary Amplitude DIA and DA Solitary Waves in Adiabatic Dusty Plasmas

    SciTech Connect

    Mamun, A. A.; Jahan, N.; Shukla, P. K.

    2008-10-15

    The dust-ion-acoustic (DIA) as well as the dust-acoustic (DA) solitary waves (SWs) in an adiabatic dusty plasma are investigated by the pseudo-potential approach which is valid for arbitrary amplitude SWs. The role of the adiabaticity of electrons and ions in modifying the basic features (polarity, speed, amplitude and width) of arbitrary amplitude DIA and DA SWs are explicitly examined. It is found that the effects of the adiabaticity of electrons and ions significantly modify the basic features (polarity, speed, amplitude and width) of the DIA and DA SWs. The implications of our results in space and laboratory dusty plasmas are briefly discussed.

  6. The molecular symmetry adapted non - adiabatic coupling terms and diabatic Hamiltonian matrix

    NASA Astrophysics Data System (ADS)

    Mukherjee, Saikat; Bandyopadhyay, Sudip; Paul, Amit Kumar; Adhikari, Satrajit

    2013-04-01

    We calculate the adiabatic Potential Energy Surfaces (PESs) and the Non - Adiabatic Coupling Terms (NACTs) for the excited electronic states (22 E' and 12 A'1) of Na3 cluster at the MRCI level by using ab initio quantum chemistry package (MOLPRO), where the NACTs are adapted with Molecular Symmetry (MS) by employing appropriate Irreducible Representations (IREPs). Such terms are incorporated into the Adiabatic to Diabatic Transformation (ADT) equations to obtain the ADT angles to construct the continuous, single - valued, symmetric and smooth 3 × 3 diabatic Hamiltonian matrix.

  7. Semiclassical quantization of bound and quasistationary states beyond the adiabatic approximation

    SciTech Connect

    Benderskii, V.A.; Vetoshkin, E.V.; Kats, E.I.

    2004-06-01

    We examine one important (and previously overlooked) aspect of well-known crossing diabatic potentials or Landau-Zener (LZ) problem. We derive the semiclassical quantization rules for the crossing diabatic potentials with localized initial and localized or delocalized final states, in the intermediate energy region, when all four adiabatic states are coupled and should be taken into account. We found all needed connection matrices and present the following analytical results: (i) in the tunneling region, the splittings of vibrational levels are represented as a product of the splitting in the lower adiabatic potential and the nontrivial function depending on the Massey parameter; (ii) in the overbarrier region, we find specific resonances between the levels in the lower and in the upper adiabatic potentials and, in that condition, independent quantizations rules are not correct; (iii) for the delocalized final states (decay lower adiabatic potential), we describe quasistationary states and calculate the decay rate as a function of the adiabatic coupling; and (iv) for the intermediate energy regions, we calculate the energy level quantization, which can be brought into a compact form by using either adiabatic or diabatic basis set (in contrast to the previous results found in the Landau diabatic basis). Applications of the results may concern the various systems; e.g., molecules undergoing conversion of electronic states, radiationless transitions, or isomerization reactions.

  8. Determination of ionization fraction and plasma potential in a dc magnetron sputtering system using a quartz crystal microbalance and a gridded energy analyzer

    SciTech Connect

    Green, K.M.

    1997-01-01

    A diagnostic which combines a quartz crystal microbalance and a gridded energy analyzer has been developed to measure the ion-to- neutral ratio and the plasma potential in a commercial dc magnetron sputtering device. Additional features of this sensor include an externally controlled shutter which protects the diagnostic when it is in the chamber, but it is not in use. The diagnostic is mounted on a linear motion feedthrough and embedded in a slot in the wafer chuck to allow for measuring uniformity in deposition and ionization throughout the plane of the wafer. RF power is introduced to ionize the Al particles. Using the quartz crystal microbalance and the gridded energy analyzer, the ion-to-neutral ratio and other parameters are determined. Comparing the total deposition rate with and without a bias that screens out the ions, but leaves the plasma undisturbed, allows for the determination of the ion-to-neutral ratio. By varying the voltage applied to the grids, the plasma potential is measured. For example, a magnetron configuration having a pressure of 35 mtorr, a dc power of 2 kW, and a net rf power of 310{+-}5 W yielded 78{+-}5% ionization and a plasma potential of 35{+-}1 V.

  9. Modulated voltage metastable ionization detector

    NASA Technical Reports Server (NTRS)

    Carle, G. C.; Kojiro, D. R.; Humphrey, D. E. (Inventor)

    1985-01-01

    The output current from a metastable ionization detector (MID) is applied to a modulation voltage circuit. An adjustment is made to balance out the background current, and an output current, above background, is applied to an input of a strip chart recorder. For low level concentrations, i.e., low detected output current, the ionization potential will be at a maximum and the metastable ionization detector will operate at its most sensitive level. When the detected current from the metastable ionization detector increases above a predetermined threshold level, a voltage control circuit is activated which turns on a high voltage transistor which acts to reduce the ionization potential. The ionization potential applied to the metastable ionization detector is then varied so as to maintain the detected signal level constant. The variation in ionization potential is now related to the concentration of the constituent and a representative amplitude is applied to another input of said strip chart recorder.

  10. Benchmark theoretical study of the ionization threshold of benzene and oligoacenes

    NASA Astrophysics Data System (ADS)

    Deleuze, M. S.; Claes, L.; Kryachko, E. S.; François, J.-P.

    2003-08-01

    In straightforward continuation of Green's function studies of the ultraviolet photoelectron spectra of polycyclic aromatic compounds [Deleuze et al., J. Chem. Phys. 115, 5859 (2001); M. S. Deleuze, ibid. 116, 7012 (2002)], we present a benchmark theoretical determination of the ionization thresholds of benzene, naphthalene, anthracene, naphthacene (tetracene), pentacene, and hexacene, within chemical accuracy [0.02-0.07 eV]. The vertical ionization potentials of these compounds have been obtained from series of single-point calculations at the Hartree-Fock, second-, third-, and partial fourth-order Møller-Plesset (MP2, MP3, MP4SDQ) levels, and from coupled cluster calculations including single and double excitations (CCSD) as well as a perturbative estimate of connected triple excitations [CCSD(T)], using basis sets of improving quality, introducing up to 510, 790, 1070, 1350, 1630, and 1910 basis functions in the computations, respectively. A focal point analysis of the convergence of the calculated ionization potentials has been performed in order to extrapolate the CCSD(T) results to an asymptotically (cc-pV∞Z) complete basis set. The present results confirm the adequacy of the outer-valence Green's function scheme for strongly correlated systems. Adiabatic ionization energies have been further determined by incorporating Beck-three-parameter Lee-Yang-Parr functional corrections for zero-point vibrational energies and for geometrical relaxations. Extension of the analysis to the CCSD(T)/cc-pV∞Z level shows that the energy minimum form of the benzene radical cation is an obtuse structure related to the 2B2g state. Isotopic shifts of the adiabatic ionization potentials, due to deuterium substitution of hydrogens, have also been discussed.

  11. Non-adiabatic Dynamics of Molecules in Optical Cavities

    NASA Astrophysics Data System (ADS)

    Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

    Molecular systems coupled to optical cavities are promising candidates for a novel kind of photo chemistry. Strong coupling to the vacuum field of the cavity can modify the potential energy surfaces opening up new reaction pathways. We present a derivation of the non-adiabatic couplings for single molecules in the strong coupling regime. The possibilities for photo chemistry are demonstrated for a set of model systems representing typical situations found in molecules. Supported by the Alexander von Humboldt Foundation.

  12. Adiabatic Compression of Oxygen: Real Fluid Temperatures

    NASA Technical Reports Server (NTRS)

    Barragan, Michelle; Wilson, D. Bruce; Stoltzfus, Joel M.

    2000-01-01

    The adiabatic compression of oxygen has been identified as an ignition source for systems operating in enriched oxygen atmospheres. Current practice is to evaluate the temperature rise on compression by treating oxygen as an ideal gas with constant heat capacity. This paper establishes the appropriate thermodynamic analysis for the common occurrence of adiabatic compression of oxygen and in the process defines a satisfactory equation of state (EOS) for oxygen. It uses that EOS to model adiabatic compression as isentropic compression and calculates final temperatures for this system using current approaches for comparison.

  13. Heating and cooling in adiabatic mixing process

    NASA Astrophysics Data System (ADS)

    Zhou, Jing; Cai, Zi; Zou, Xu-Bo; Guo, Guang-Can

    2010-12-01

    We study the effect of interaction on the temperature change in the process of adiabatic mixing of two components of Fermi gases using the real-space Bogoliubov-de Gennes method. We find that in the process of adiabatic mixing, the competition between the adiabatic expansion and the attractive interaction makes it possible to cool or heat the system depending on the strength of the interaction and the initial temperature of the system. The changes of the temperature in a bulk system and in a trapped system are investigated.

  14. NON-WKB MODELS OF THE FIRST IONIZATION POTENTIAL EFFECT: IMPLICATIONS FOR SOLAR CORONAL HEATING AND THE CORONAL HELIUM AND NEON ABUNDANCES

    SciTech Connect

    Laming, J. Martin

    2009-04-20

    We revisit in more detail a model for element abundance fractionation in the solar chromosphere that gives rise to the 'first ionization potential (FIP) effect' in the solar corona and wind. Elements with first ionization potential below about 10 eV, i.e., those that are predominantly ionized in the chromosphere, are enriched in the corona by a factor of 3-4. We model the propagation of Alfven waves through the chromosphere using a non-WKB treatment, and evaluate the ponderomotive force associated with these waves. Under solar conditions, this is generally pointed upward in the chromosphere, and enhances the abundance of chromospheric ions in the corona. Our new approach captures the essentials of the solar coronal abundance anomalies, including the depletion of He relative to H, and also the putative depletion of Ne, recently discussed in the literature. We also argue that the FIP effect provides the strongest evidence to date for energy fluxes of Alfven waves sufficient to heat the corona. However, it appears that these waves must also be generated in the corona, in order to preserve the rather regular fractionation pattern without strong variations from loop to loop observed in the solar corona and slow-speed solar wind.

  15. Pathways and dynamics of dissociation of ionized (H{sub 2}O){sub 2}

    SciTech Connect

    Barnett, R.N.; Landman, U.

    1995-11-30

    The energetics, geometrical and electronic structure, ionization processes, dynamics, and dissociation pathways of natural and singly and doubly ionized water dimers are investigated with simulations employing the Born-Oppenheimer local-spin-density functional molecular dynamics (BO-LSD-MD) method. Vertical and adiabatic ionization potentials and dissociation energies and barriers are calculated for various dissociation channels of the singly and doubly ionized dimer. A new bound ground-state, (H{sub 2}O){sub 2} {sup +}(a), with a hydrazine-like configuration, whose energy is lower by 0.22 eV than that of the disproportionated-ion isomer, (OH)(H{sub 3}O){sup +}, is found for the singly charged dimer cation. A state with a similar geometry is found for a bound metastable state of the doubly ionized water dimer, whose dissociation into 2(H{sub 2}O{sup +}) involves a barrier of {approx}0.68 eV. The dissociation pathways of the singly ionized dimer depend on the internal energy of the parent neutral and on the excited energy, with the OH + H{sub 2}O{sup +} channel dominating at low energies. 45 refs., 5 figs., 3 tabs.

  16. A Frontier orbital energy approach to redox potentials

    NASA Astrophysics Data System (ADS)

    Conradie, Jeanet

    2015-09-01

    The prediction of the oxidation and reduction potentials of molecules is important in many research areas. A review of relationships obtained between frontier orbital energies (eV), the calculated ionization potentials (IP in eV), or adiabatic electron affinities (EA in eV) with the experimental oxidation and reduction potentials is presented, for selected series of β- diketones, rhodium-β-diketonato complexes, as well as metal-tris-β-diketonato complexes, with the metal Fe or Mn. The good linear relationships obtained for related series of complexes show that the oxidation and reduction potentials of these complexes can be predicted by their DFT-calculated energies.

  17. Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. I. Propagation of single-active-electron wave packets in chiral pseudo-potentials

    SciTech Connect

    Artemyev, Anton N.; Müller, Anne D.; Demekhin, Philipp V.; Hochstuhl, David

    2015-06-28

    A theoretical method to study the angle-resolved multiphoton ionization of polyatomic molecules is developed. It is based on the time-dependent formulation of the Single Center (TDSC) method and consists in the propagation of single-active-electron wave packets in the effective molecular potentials in the presence of intense laser pulses. For this purpose, the time-dependent Schrödinger equation for one electron, moving in a molecular field and interacting with an arbitrary laser pulse, is solved in spherical coordinates by an efficient numerical approach. As a test, the method is applied to the one- and two-photon ionizations of a model methane-like chiral system by circularly polarized short intense high-frequency laser pulses. Thereby, we analyze the photoelectron circular dichroism (PECD) in the momentum distribution. The considered model application illustrates the capability of the TDSC method to study multiphoton PECD in fixed-in-space and randomly oriented chiral molecules.

  18. Adiabatic limits on Riemannian Heisenberg manifolds

    SciTech Connect

    Yakovlev, A A

    2008-02-28

    An asymptotic formula is obtained for the distribution function of the spectrum of the Laplace operator, in the adiabatic limit for the foliation defined by the orbits of an invariant flow on a compact Riemannian Heisenberg manifold. Bibliography: 21 titles.

  19. Experimental demonstration of composite adiabatic passage

    NASA Astrophysics Data System (ADS)

    Schraft, Daniel; Halfmann, Thomas; Genov, Genko T.; Vitanov, Nikolay V.

    2013-12-01

    We report an experimental demonstration of composite adiabatic passage (CAP) for robust and efficient manipulation of two-level systems. The technique represents a altered version of rapid adiabatic passage (RAP), driven by composite sequences of radiation pulses with appropriately chosen phases. We implement CAP with radio-frequency pulses to invert (i.e., to rephase) optically prepared spin coherences in a Pr3+:Y2SiO5 crystal. We perform systematic investigations of the efficiency of CAP and compare the results with conventional π pulses and RAP. The data clearly demonstrate the superior features of CAP with regard to robustness and efficiency, even under conditions of weakly fulfilled adiabaticity. The experimental demonstration of composite sequences to support adiabatic passage is of significant relevance whenever a high efficiency or robustness of coherent excitation processes need to be maintained, e.g., as required in quantum information technology.

  20. An Adiabatic Architecture for Linear Signal Processing

    NASA Astrophysics Data System (ADS)

    Vollmer, M.; Götze, J.

    2005-05-01

    Using adiabatic CMOS logic instead of the more traditional static CMOS logic can lower the power consumption of a hardware design. However, the characteristic differences between adiabatic and static logic, such as a four-phase clock, have a far reaching influence on the design itself. These influences are investigated in this paper by adapting a systolic array of CORDIC devices to be implemented adiabatically. We present a means to describe adiabatic logic in VHDL and use it to define the systolic array with precise timing and bit-true calculations. The large pipeline bubbles that occur in a naive version of this array are identified and removed to a large degree. As an example, we demonstrate a parameterization of the CORDIC array that carries out adaptive RLS filtering.

  1. General conditions for quantum adiabatic evolution

    SciTech Connect

    Comparat, Daniel

    2009-07-15

    Adiabaticity occurs when, during its evolution, a physical system remains in the instantaneous eigenstate of the Hamiltonian. Unfortunately, existing results, such as the quantum adiabatic theorem based on a slow down evolution [H({epsilon}t),{epsilon}{yields}0], are insufficient to describe an evolution driven by the Hamiltonian H(t) itself. Here we derive general criteria and exact bounds, for the state and its phase, ensuring an adiabatic evolution for any Hamiltonian H(t). As a corollary, we demonstrate that the commonly used condition of a slow Hamiltonian variation rate, compared to the spectral gap, is indeed sufficient to ensure adiabaticity but only when the Hamiltonian is real and nonoscillating (for instance, containing exponential or polynomial but no sinusoidal functions)

  2. Potential of gas chromatography-atmospheric pressure chemical ionization-tandem mass spectrometry for screening and quantification of hexabromocyclododecane.

    PubMed

    Sales, Carlos; Portolés, Tania; Sancho, Juan Vicente; Abad, Esteban; Ábalos, Manuela; Sauló, Jordi; Fiedler, Heidelore; Gómara, Belén; Beltrán, Joaquim

    2016-01-01

    A fast method for the screening and quantification of hexabromocyclododecane (sum of all isomers) by gas chromatography using a triple quadrupole mass spectrometer with atmospheric pressure chemical ionization (GC-APCI-QqQ) is proposed. This novel procedure makes use of the soft atmospheric pressure chemical ionization source, which results in less fragmentation of the analyte than by conventional electron impact (EI) and chemical ionization (CI) sources, favoring the formation of the [M - Br](+) ion and, thus, enhancing sensitivity and selectivity. Detection was based on the consecutive loses of HBr from the [M - Br](+) ion to form the specific [M - H5Br6](+) and [M - H4Br5](+) ions, which were selected as quantitation (Q) and qualification (q) transitions, respectively. Parameters affecting ionization and MS/MS detection were studied. Method performance was also evaluated; calibration curves were found linear from 1 pg/μL to 100 pg/μL for the total HBCD concentration; instrumental detection limit was estimated to be 0.10 pg/μL; repeatability and reproducibility, expressed as relative standard deviation, were better than 7% in both cases. The application to different real samples [polyurethane foam disks (PUFs), food, and marine samples] pointed out a rapid way to identify and allow quantification of this compound together with a number of polybrominated diphenyl ethers (BDE congeners 28, 47, 66, 85, 99, 100, 153, 154, 183, 184, 191, 196, 197, and 209) and two other novel brominated flame retardants [i.e., decabromodiphenyl ethane (DBDPE) and 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE)] because of their presence in the same fraction when performing the usual sample treatment. PMID:26554601

  3. AB INITIO SIMULATIONS FOR MATERIAL PROPERTIES ALONG THE JUPITER ADIABAT

    SciTech Connect

    French, Martin; Becker, Andreas; Lorenzen, Winfried; Nettelmann, Nadine; Bethkenhagen, Mandy; Redmer, Ronald; Wicht, Johannes

    2012-09-15

    We determine basic thermodynamic and transport properties of hydrogen-helium-water mixtures for the extreme conditions along Jupiter's adiabat via ab initio simulations, which are compiled in an accurate and consistent data set. In particular, we calculate the electrical and thermal conductivity, the shear and longitudinal viscosity, and diffusion coefficients of the nuclei. We present results for associated quantities like the magnetic and thermal diffusivity and the kinematic shear viscosity along an adiabat that is taken from a state-of-the-art interior structure model. Furthermore, the heat capacities, the thermal expansion coefficient, the isothermal compressibility, the Grueneisen parameter, and the speed of sound are calculated. We find that the onset of dissociation and ionization of hydrogen at about 0.9 Jupiter radii marks a region where the material properties change drastically. In the deep interior, where the electrons are degenerate, many of the material properties remain relatively constant. Our ab initio data will serve as a robust foundation for applications that require accurate knowledge of the material properties in Jupiter's interior, e.g., models for the dynamo generation.

  4. Surface ionization of terpene hydrocarbons

    SciTech Connect

    Zandberg, E.Y.; Nezdyurov, A.L.; Paleev, V.I.; Ponomarev, D.A.

    1986-09-01

    By means of a surface ionization indicator for traces of materials in the atmosphere it has been established that many natural materials containing terpenes and their derivatives are ionized on the surface of heated molybdenum oxide at atmospheric air pressure. A mass-spectrometer method has been used to explain the mechanism of ionization of individual terpene hydrocarbons and to establish its principles. The ionization of ..cap alpha..-pinene, alloocimene, camphene, and also adamantane on oxidized tungsten under vacuum conditions has been investigated. The ..cap alpha..-pinene and alloocimene are ionized by surface ionization but camphene and adamantane are not ionized under vacuum conditions. The surface ionization mass spectra of ..cap alpha..-pinene and alloocimene are of low line brightness in comparison with electron ionization mass spectra and differ between themselves. The temperature relations for currents of the same compositions of ions during ionization of ..cap alpha..-pinene and alloocimene are also different, which leads to the possibility of surface ionization analysis of mixtures of terpenes being ionized. The ionization coefficients of alloocimene and ..cap alpha..-pinene on oxidized tungsten under temperatures optimum for ionization and the ionization potentials of alloocimene molecules and of radicals (M-H) of both compounds have been evaluated.

  5. Broadband electrically detected magnetic resonance using adiabatic pulses.

    PubMed

    Hrubesch, F M; Braunbeck, G; Voss, A; Stutzmann, M; Brandt, M S

    2015-05-01

    We present a broadband microwave setup for electrically detected magnetic resonance (EDMR) based on microwave antennae with the ability to apply arbitrarily shaped pulses for the excitation of electron spin resonance (ESR) and nuclear magnetic resonance (NMR) of spin ensembles. This setup uses non-resonant stripline structures for on-chip microwave delivery and is demonstrated to work in the frequency range from 4 MHz to 18 GHz. π pulse times of 50 ns and 70 μs for ESR and NMR transitions, respectively, are achieved with as little as 100 mW of microwave or radiofrequency power. The use of adiabatic pulses fully compensates for the microwave magnetic field inhomogeneity of the stripline antennae, as demonstrated with the help of BIR4 unitary rotation pulses driving the ESR transition of neutral phosphorus donors in silicon and the NMR transitions of ionized phosphorus donors as detected by electron nuclear double resonance (ENDOR). PMID:25828243

  6. Symmetry of the Adiabatic Condition in the Piston Problem

    ERIC Educational Resources Information Center

    Anacleto, Joaquim; Ferreira, J. M.

    2011-01-01

    This study addresses a controversial issue in the adiabatic piston problem, namely that of the piston being adiabatic when it is fixed but no longer so when it can move freely. It is shown that this apparent contradiction arises from the usual definition of adiabatic condition. The issue is addressed here by requiring the adiabatic condition to be…

  7. Calcium - ionized

    MedlinePlus

    ... at both ionized calcium and calcium attached to proteins. You may need to have a separate ionized calcium test if you have factors that increase or decrease total calcium levels. These may include abnormal blood levels ...

  8. Analytical instruments, ionization sources, and ionization methods

    DOEpatents

    Atkinson, David A.; Mottishaw, Paul

    2006-04-11

    Methods and apparatus for simultaneous vaporization and ionization of a sample in a spectrometer prior to introducing the sample into the drift tube of the analyzer are disclosed. The apparatus includes a vaporization/ionization source having an electrically conductive conduit configured to receive sample particulate which is conveyed to a discharge end of the conduit. Positioned proximate to the discharge end of the conduit is an electrically conductive reference device. The conduit and the reference device act as electrodes and have an electrical potential maintained between them sufficient to cause a corona effect, which will cause at least partial simultaneous ionization and vaporization of the sample particulate. The electrical potential can be maintained to establish a continuous corona, or can be held slightly below the breakdown potential such that arrival of particulate at the point of proximity of the electrodes disrupts the potential, causing arcing and the corona effect. The electrical potential can also be varied to cause periodic arcing between the electrodes such that particulate passing through the arc is simultaneously vaporized and ionized. The invention further includes a spectrometer containing the source. The invention is particularly useful for ion mobility spectrometers and atmospheric pressure ionization mass spectrometers.

  9. Impact of electron ionization on the generation of high-order harmonics from molecules

    SciTech Connect

    Brener, S.; Moiseyev, N.; Ivanov, M. V.

    2003-08-01

    When the laser frequency is tuned to be equal to the molecular electronic excitation, high-order harmonics are generated due to the electronic dipole transitions between the corresponding two potential-energy surfaces (PES). A natural, often taken, choice is the PES of the field-free molecular system. In this special choice the ionization phenomenon is not considered. Only the effect of the dissociation is considered. The method we developed enables one to remain within the framework of the 2-PES approximation and yet to include also the ionization effect in the calculations of molecular high-order harmonic generation spectra. In this approach the coupling between the electronic and nuclear motions is taken into consideration by using coupled complex adiabatic PES. As an illustrative numerical example, we calculated the high harmonic generation (HHG) spectra of H{sub 2}{sup +} in a 730-nm laser with the intensity of 8.77x10{sup 13} W/cm{sup 2}. The inclusion of the ionization in our approach not only enables the electrons to tunnel through the effective static potential barrier, but also apply an asymmetric force which accelerates the electron before ionization takes place. Therefore, indirectly the inclusion of the ionization by the laser field may lead eventually to an enhanced HHG spectra in comparison with the calculated one when the ''natural'' choice of the field-free 2PES is taken.

  10. A first-principle protocol for calculating ionization energies and redox potentials of solvated molecules and ions: Theory and application to aqueous phenol and phenolate

    PubMed Central

    Ghosh, Debashree; Roy, Anirban; Seidel, Robert; Winter, Bernd; Bradforth, Stephen; Krylov, Anna I.

    2012-01-01

    The effect of hydration on the lowest vertical ionization energy (VIE) of phenol and phenolate solvated in bulk water was characterized using the equation-of-motion ionization potential coupled-cluster (EOM-IP-CCSD) and effective fragment potential (EFP) methods (referred to as EOM/EFP), and determined experimentally by valence photo-emission measurements using microjets and synchrotron radiation. The computed solvent-induced shifts in VIEs (ΔVIE) are −0.66 eV and +5.72 eV for phenol and phenolate, respectively. Our best estimates of the absolute values of VIEs (7.9 and 7.7 eV for phenol and phenolate) agree reasonably well with the respective experimental values (7.8±0.1 eV and 7.1±0.1 eV). The EOM/EFP scheme was benchmarked against full EOM-IP-CCSD using micro-solvated phenol and phenolate clusters. A protocol for calculating redox potentials with EOM/EFP was developed based on linear response approximation (LRA) of free energy determination. The oxidation potentials of phenol and phenolate calculated using LRA and EOM/EFP are 1.32 V and 0.89 V, respectively; they agree well with experimental values. PMID:22497288

  11. Ionized cluster beam deposition

    NASA Technical Reports Server (NTRS)

    Kirkpatrick, A. R.

    1983-01-01

    Ionized Cluster Beam (ICB) deposition, a new technique originated by Takagi of Kyoto University in Japan, offers a number of unique capabilities for thin film metallization as well as for deposition of active semiconductor materials. ICB allows average energy per deposited atom to be controlled and involves impact kinetics which result in high diffusion energies of atoms on the growth surface. To a greater degree than in other techniques, ICB involves quantitative process parameters which can be utilized to strongly control the characteristics of films being deposited. In the ICB deposition process, material to be deposited is vaporized into a vacuum chamber from a confinement crucible at high temperature. Crucible nozzle configuration and operating temperature are such that emerging vapor undergoes supercondensation following adiabatic expansion through the nozzle.

  12. Ionization photophysics and spectroscopy of dicyanoacetylene

    SciTech Connect

    Leach, Sydney E-mail: Martin.Schwell@lisa.u-pec.fr; Champion, Norbert; Schwell, Martin E-mail: Martin.Schwell@lisa.u-pec.fr; Bénilan, Yves; Fray, Nicolas; Gazeau, Marie-Claire; Garcia, Gustavo A.; Gaie-Levrel, François; Guillemin, Jean-Claude

    2013-11-14

    Photoionization of dicyanoacetylene was studied using synchrotron radiation over the excitation range 8–25 eV, with photoelectron-photoion coincidence techniques. The absolute ionization cross-section and detailed spectroscopic aspects of the parent ion were recorded. The adiabatic ionization energy of dicyanoacetylene was measured as 11.80 ± 0.01 eV. A detailed analysis of the cation spectroscopy involves new aspects and new assignments of the vibrational components to excitation of the quasi-degenerate A{sup 2}Π{sub g}, B{sup 2}Σ{sub g}{sup +} states as well as the C{sup 2}Σ{sub u}{sup +} and D{sup 2}Π{sub u} states of the cation. Some of the structured autoionization features observed in the 12.4–15 eV region of the total ion yield spectrum were assigned to vibrational components of valence shell transitions and to two previously unknown Rydberg series converging to the D{sup 2}Π{sub u} state of C{sub 4}N{sub 2}{sup +}. The appearance energies of the fragment ions C{sub 4}N{sup +}, C{sub 3}N{sup +}, C{sub 4}{sup +}, C{sub 2}N{sup +}, and C{sub 2}{sup +} were measured and their heats of formation were determined and compared with existing literature values. Thermochemical calculations of the appearance potentials of these and other weaker ions were used to infer aspects of dissociative ionization pathways.

  13. Graph isomorphism and adiabatic quantum computing

    NASA Astrophysics Data System (ADS)

    Gaitan, Frank; Clark, Lane

    2014-02-01

    In the graph isomorphism (GI) problem two N-vertex graphs G and G' are given and the task is to determine whether there exists a permutation of the vertices of G that preserves adjacency and transforms G →G'. If yes, then G and G' are said to be isomorphic; otherwise they are nonisomorphic. The GI problem is an important problem in computer science and is thought to be of comparable difficulty to integer factorization. In this paper we present a quantum algorithm that solves arbitrary instances of GI and which also provides an approach to determining all automorphisms of a given graph. We show how the GI problem can be converted to a combinatorial optimization problem that can be solved using adiabatic quantum evolution. We numerically simulate the algorithm's quantum dynamics and show that it correctly (i) distinguishes nonisomorphic graphs; (ii) recognizes isomorphic graphs and determines the permutation(s) that connect them; and (iii) finds the automorphism group of a given graph G. We then discuss the GI quantum algorithm's experimental implementation, and close by showing how it can be leveraged to give a quantum algorithm that solves arbitrary instances of the NP-complete subgraph isomorphism problem. The computational complexity of an adiabatic quantum algorithm is largely determined by the minimum energy gap Δ (N) separating the ground and first-excited states in the limit of large problem size N ≫1. Calculating Δ (N) in this limit is a fundamental open problem in adiabatic quantum computing, and so it is not possible to determine the computational complexity of adiabatic quantum algorithms in general, nor consequently, of the specific adiabatic quantum algorithms presented here. Adiabatic quantum computing has been shown to be equivalent to the circuit model of quantum computing, and so development of adiabatic quantum algorithms continues to be of great interest.

  14. Liver metabolomics reveals increased oxidative stress and fibrogenic potential in gfrp transgenic mice in response to ionizing radiation.

    PubMed

    Cheema, Amrita K; Pathak, Rupak; Zandkarimi, Fereshteh; Kaur, Prabhjit; Alkhalil, Lynn; Singh, Rajbir; Zhong, Xiaogang; Ghosh, Sanchita; Aykin-Burns, Nukhet; Hauer-Jensen, Martin

    2014-06-01

    Although radiation-induced tissue-specific injury is well documented, the underlying molecular changes resulting in organ dysfunction and the consequences thereof on overall metabolism and physiology have not been elucidated. We previously reported the generation and characterization of a transgenic mouse strain that ubiquitously overexpresses Gfrp (GTPH-1 feedback regulatory protein) and exhibits higher oxidative stress, which is a possible result of decreased tetrahydrobiopterin (BH4) bioavailability. In this study, we report genotype-dependent changes in the metabolic profiles of liver tissue after exposure to nonlethal doses of ionizing radiation. Using a combination of untargeted and targeted quantitative mass spectrometry, we report significant accumulation of metabolites associated with oxidative stress, as well as the dysregulation of lipid metabolism in transgenic mice after radiation exposure. The radiation stress seems to exacerbate lipid peroxidation and also results in higher expression of genes that facilitate liver fibrosis, in a manner that is dependent on the genetic background and post-irradiation time interval. These findings suggest the significance of Gfrp in regulating redox homeostasis in response to stress induced by ionizing radiation affecting overall physiology. PMID:24824572

  15. Liver Metabolomics Reveals Increased Oxidative Stress and Fibrogenic Potential in Gfrp Transgenic Mice in Response to Ionizing Radiation

    PubMed Central

    2015-01-01

    Although radiation-induced tissue-specific injury is well documented, the underlying molecular changes resulting in organ dysfunction and the consequences thereof on overall metabolism and physiology have not been elucidated. We previously reported the generation and characterization of a transgenic mouse strain that ubiquitously overexpresses Gfrp (GTPH-1 feedback regulatory protein) and exhibits higher oxidative stress, which is a possible result of decreased tetrahydrobiopterin (BH4) bioavailability. In this study, we report genotype-dependent changes in the metabolic profiles of liver tissue after exposure to nonlethal doses of ionizing radiation. Using a combination of untargeted and targeted quantitative mass spectrometry, we report significant accumulation of metabolites associated with oxidative stress, as well as the dysregulation of lipid metabolism in transgenic mice after radiation exposure. The radiation stress seems to exacerbate lipid peroxidation and also results in higher expression of genes that facilitate liver fibrosis, in a manner that is dependent on the genetic background and post-irradiation time interval. These findings suggest the significance of Gfrp in regulating redox homeostasis in response to stress induced by ionizing radiation affecting overall physiology. PMID:24824572

  16. Evaluation of Potential Ionizing Irradiation Protectors and Mitigators Using Clonogenic Survival of Human Umbilical Cord Blood Hematopoietic Progenitor Cells

    PubMed Central

    Goff, Julie P.; Shields, Donna S.; Wang, Hong; Skoda, Erin M.; Sprachman, Melissa M.; Wipf, Peter; Garapati, Venkata Krishna; Atkinson, Jeffrey; London, Barry; Lazo, John S.; Kagan, Valerian; Epperly, Michael W.; Greenberger, Joel S.

    2013-01-01

    We evaluated the use of colony formation (CFU-GM, BFU-E, and CFU-GEMM) by human umbilical cord blood (CB) hematopoietic progenitor cells for testing novel small molecule ionizing irradiation protectors and mitigators. Each of 11 compounds was added before (protection) or after (mitigation) ionizing irradiation including: GS-nitroxides (JP4-039 and XJB-5-131), the bifunctional sulfoxide MMS-350, the phosphoinositol-3-kinase inhibitor (LY294002), TPP-imidazole fatty acid, (TPP-IOA), the nitric oxide synthase inhibitor (MCF-201-89), the p53/mdm2/mdm4 inhibitor (BEB55), methoxamine, isoproterenol, propanolol, and the ATP sensitive potassium channel blocker (glyburide). The drugs XJB-5-131, JP4-039, and MMS-350 were radiation protectors for CFU-GM. JP4-039 was also a radiation protector for CFU-GEMM. The drugs, XJB-5-131, JP4-039, and MMS-350 were radiation mitigators for BFU-E, MMS-350 and JP4-039 were mitigators for CFU-GM, and MMS350 was a mitigator for CFU-GEMM. In contrast, other drugs that were effective in murine assays: TTP-IOA, LY294002, MCF201-89, BEB55, propranolol, isoproterenol, methoxamine, and glyburide showed no significant protection or mitigation in human CB assays. These data support testing of new candidate clinical radiation protectors and mitigators using human CB clonogenic assays early in the drug discovery process, reducing the need for animal experiments. PMID:23933481

  17. Symmetry-Protected Quantum Adiabatic Transistors

    NASA Astrophysics Data System (ADS)

    Williamson, Dominic J.; Bartlett, Stephen D.

    2014-03-01

    An essential development in the history of computing was the invention of the transistor as it allowed logic circuits to be implemented in a robust and modular way. The physical characteristics of semiconductor materials were the key to building these devices. We aim to present an analogous development for quantum computing by showing that quantum adiabatic transistors (as defined by Flammia et al.) are built upon the essential qualities of symmetry-protected (SP) quantum ordered phases in one dimension. Flammia et al. and Renes et al. have demonstrated schemes for universal adiabatic quantum computation using quantum adiabatic transistors described by interacting spin chain models with specifically chosen Hamiltonian terms. We show that these models can be understood as specific examples of the generic situation in which all SP phases lead to quantum computation on encoded edge degrees of freedom by adiabatically traversing a symmetric phase transition into a trivial symmetric phase. This point of view is advantageous as it allows us to readily see that the computational properties of a quantum adiabatic transistor arise from a phase of matter rather than due to carefully tuned interactions.

  18. Boosting the Detection Potential of Liquid Chromatography-Electron Ionization Mass Spectrometry Using a Ceramic Coated Ion Source

    NASA Astrophysics Data System (ADS)

    Magrini, Laura; Famiglini, Giorgio; Palma, Pierangela; Termopoli, Veronica; Cappiello, Achille

    2016-01-01

    Detection of target and non-target substances and their characterization in complex samples is a challenging task. Here we demonstrate that coating the electron ionization (EI) ion source of an LC-MS system with a sol-gel ceramic film can drastically improve the detection of high-molecular weight and high-boiling analytes. A new ion source coated with a ceramic material was developed and tested with a mixture of polycyclic aromatic hydrocarbons (PAH) with an increasing number of rings. Comparison of the results obtained with those for an uncoated stainless steel (SS) ion source shows a dramatic improvement in the MS signals, with a nearly 40-fold increase of the signal-to-noise ratio. We also demonstrate the ability of the new system to produce excellent chromatographic profiles for hard-to-detect hormones.

  19. Boosting the Detection Potential of Liquid Chromatography-Electron Ionization Mass Spectrometry Using a Ceramic Coated Ion Source.

    PubMed

    Magrini, Laura; Famiglini, Giorgio; Palma, Pierangela; Termopoli, Veronica; Cappiello, Achille

    2016-01-01

    Detection of target and non-target substances and their characterization in complex samples is a challenging task. Here we demonstrate that coating the electron ionization (EI) ion source of an LC-MS system with a sol-gel ceramic film can drastically improve the detection of high-molecular weight and high-boiling analytes. A new ion source coated with a ceramic material was developed and tested with a mixture of polycyclic aromatic hydrocarbons (PAH) with an increasing number of rings. Comparison of the results obtained with those for an uncoated stainless steel (SS) ion source shows a dramatic improvement in the MS signals, with a nearly 40-fold increase of the signal-to-noise ratio. We also demonstrate the ability of the new system to produce excellent chromatographic profiles for hard-to-detect hormones. PMID:26350384

  20. Evaluation of potential ionizing irradiation protectors and mitigators using clonogenic survival of human umbilical cord blood hematopoietic progenitor cells.

    PubMed

    Goff, Julie P; Shields, Donna S; Wang, Hong; Skoda, Erin M; Sprachman, Melissa M; Wipf, Peter; Garapati, Venkata Krishna; Atkinson, Jeffrey; London, Barry; Lazo, John S; Kagan, Valerian; Epperly, Michael W; Greenberger, Joel S

    2013-11-01

    We evaluated the use of colony formation (colony-forming unit-granulocyte macrophage [CFU-GM], burst-forming unit erythroid [BFU-E], and colony-forming unit-granulocyte-erythroid-megakaryocyte-monocytes [CFU-GEMM]) by human umbilical cord blood (CB) hematopoietic progenitor cells for testing novel small molecule ionizing irradiation protectors and mitigators. The following compounds were added before (protection) or after (mitigation) ionizing irradiation: GS-nitroxides (JP4-039 and XJB-5-131), the bifunctional sulfoxide MMS-350, the phosphoinositol-3-kinase inhibitor LY29400, triphenylphosphonium-imidazole fatty acid, the nitric oxide synthase inhibitor (MCF-201-89), the p53/mdm2/mdm4 inhibitor (BEB55), methoxamine, isoproterenol, propranolol, and the adenosine triphosphate-sensitive potassium channel blocker (glyburide). The drugs XJB-5-131, JP4-039, and MMS-350 were radiation protectors for CFU-GM. JP4-039 was also a radiation protector for CFU-GEMM. The drugs XJB-5-131, JP4-039, and MMS-350 were radiation mitigators for BFU-E, MMS-350 and JP4-039 were mitigators for CFU-GM, and MMS350 was a mitigator for CFU-GEMM. In contrast, other drugs were effective in murine assays; TTP-IOA, LY294002, MCF201-89, BEB55, propranolol, isoproterenol, methoxamine, and glyburide but showed no significant protection or mitigation in human CB assays. These data support the testing of new candidate clinical radiation protectors and mitigators using human CB clonogenic assays early in the drug discovery process, thus reducing the need for animal experiments. PMID:23933481

  1. Nonadiabatic exchange dynamics during adiabatic frequency sweeps

    NASA Astrophysics Data System (ADS)

    Barbara, Thomas M.

    2016-04-01

    A Bloch equation analysis that includes relaxation and exchange effects during an adiabatic frequency swept pulse is presented. For a large class of sweeps, relaxation can be incorporated using simple first order perturbation theory. For anisochronous exchange, new expressions are derived for exchange augmented rotating frame relaxation. For isochronous exchange between sites with distinct relaxation rate constants outside the extreme narrowing limit, simple criteria for adiabatic exchange are derived and demonstrate that frequency sweeps commonly in use may not be adiabatic with regard to exchange unless the exchange rates are much larger than the relaxation rates. Otherwise, accurate assessment of the sensitivity to exchange dynamics will require numerical integration of the rate equations. Examples of this situation are given for experimentally relevant parameters believed to hold for in-vivo tissue. These results are of significance in the study of exchange induced contrast in magnetic resonance imaging.

  2. Adiabatic approximation for the density matrix

    NASA Astrophysics Data System (ADS)

    Band, Yehuda B.

    1992-05-01

    An adiabatic approximation for the Liouville density-matrix equation which includes decay terms is developed. The adiabatic approximation employs the eigenvectors of the non-normal Liouville operator. The approximation is valid when there exists a complete set of eigenvectors of the non-normal Liouville operator (i.e., the eigenvectors span the density-matrix space), the time rate of change of the Liouville operator is small, and an auxiliary matrix is nonsingular. Numerical examples are presented involving efficient population transfer in a molecule by stimulated Raman scattering, with the intermediate level of the molecule decaying on a time scale that is fast compared with the pulse durations of the pump and Stokes fields. The adiabatic density-matrix approximation can be simply used to determine the density matrix for atomic or molecular systems interacting with cw electromagnetic fields when spontaneous emission or other decay mechanisms prevail.

  3. Extensive Adiabatic Invariants for Nonlinear Chains

    NASA Astrophysics Data System (ADS)

    Giorgilli, Antonio; Paleari, Simone; Penati, Tiziano

    2012-09-01

    We look for extensive adiabatic invariants in nonlinear chains in the thermodynamic limit. Considering the quadratic part of the Klein-Gordon Hamiltonian, by a linear change of variables we transform it into a sum of two parts in involution. At variance with the usual method of introducing normal modes, our constructive procedure allows us to exploit the complete resonance, while keeping the extensive nature of the system. Next we construct a nonlinear approximation of an extensive adiabatic invariant for a perturbation of the discrete nonlinear Schrödinger model. The fluctuations of this quantity are controlled via Gibbs measure estimates independent of the system size, for a large set of initial data at low specific energy. Finally, by numerical calculations we show that our adiabatic invariant is well conserved for times much longer than predicted by our first order theory, with fluctuation much smaller than expected according to standard statistical estimates.

  4. Anderson localization makes adiabatic quantum optimization fail

    PubMed Central

    Altshuler, Boris; Krovi, Hari; Roland, Jérémie

    2010-01-01

    Understanding NP-complete problems is a central topic in computer science (NP stands for nondeterministic polynomial time). This is why adiabatic quantum optimization has attracted so much attention, as it provided a new approach to tackle NP-complete problems using a quantum computer. The efficiency of this approach is limited by small spectral gaps between the ground and excited states of the quantum computer’s Hamiltonian. We show that the statistics of the gaps can be analyzed in a novel way, borrowed from the study of quantum disordered systems in statistical mechanics. It turns out that due to a phenomenon similar to Anderson localization, exponentially small gaps appear close to the end of the adiabatic algorithm for large random instances of NP-complete problems. This implies that unfortunately, adiabatic quantum optimization fails: The system gets trapped in one of the numerous local minima. PMID:20616043

  5. Identification of four rotamers of m-methoxystyrene by resonant two-photon ionization and mass analyzed threshold ionization spectroscopy

    SciTech Connect

    Xu, Yanqi; Tzeng, Sheng Yuan; Takahashi, Kaito; Shivatare, Vidya; Zhang, Bing; Tzeng, Wen Bih

    2015-03-28

    We report the vibronic and cation spectra of four rotamers of m-methoxystyrene, recorded by using the two-color resonant two-photon ionization and mass-analyzed threshold ionization techniques. The excitation energies of the S{sub 1}← S{sub 0} electronic transition are found to be 32 767, 32 907, 33 222, and 33 281 cm{sup −1}, and the corresponding adiabatic ionization energies are 65 391, 64 977, 65 114, and 64 525 cm{sup −1} for these isomeric species. Most of the observed active vibrations in the electronically excited S{sub 1} and cationic ground D{sub 0} states involve in-plane ring deformation and substituent-sensitive bending motions. It is found that the relative orientation of the methoxyl with respect to the vinyl group does not influence the vibrational frequencies of the ring-substituent bending modes. The two dimensional potential energy surface calculations support our experimental finding that the isomerization is restricted in the S{sub 1} and D{sub 0} states.

  6. Spontaneous emission in stimulated Raman adiabatic passage

    SciTech Connect

    Ivanov, P. A.; Vitanov, N. V.; Bergmann, K.

    2005-11-15

    This work explores the effect of spontaneous emission on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The approach uses adiabatic elimination of weakly coupled density matrix elements in the Liouville equation, from which a very accurate analytic approximation is derived. The loss of population transfer efficiency is found to decrease exponentially with the factor {omega}{sub 0}{sup 2}/{gamma}, where {gamma} is the spontaneous emission rate and {omega}{sub 0} is the peak Rabi frequency. The transfer efficiency increases with the pulse delay and reaches a steady value. For large pulse delay and large spontaneous emission rate STIRAP degenerates into optical pumping.

  7. On black hole spectroscopy via adiabatic invariance

    NASA Astrophysics Data System (ADS)

    Jiang, Qing-Quan; Han, Yan

    2012-12-01

    In this Letter, we obtain the black hole spectroscopy by combining the black hole property of adiabaticity and the oscillating velocity of the black hole horizon. This velocity is obtained in the tunneling framework. In particular, we declare, if requiring canonical invariance, the adiabatic invariant quantity should be of the covariant form Iadia = ∮pi dqi. Using it, the horizon area of a Schwarzschild black hole is quantized independently of the choice of coordinates, with an equally spaced spectroscopy always given by ΔA = 8 π lp2 in the Schwarzschild and Painlevé coordinates.

  8. Complexity of the Quantum Adiabatic Algorithm

    NASA Technical Reports Server (NTRS)

    Hen, Itay

    2013-01-01

    The Quantum Adiabatic Algorithm (QAA) has been proposed as a mechanism for efficiently solving optimization problems on a quantum computer. Since adiabatic computation is analog in nature and does not require the design and use of quantum gates, it can be thought of as a simpler and perhaps more profound method for performing quantum computations that might also be easier to implement experimentally. While these features have generated substantial research in QAA, to date there is still a lack of solid evidence that the algorithm can outperform classical optimization algorithms.

  9. Adiabatic approximation for nucleus-nucleus scattering

    SciTech Connect

    Johnson, R.C.

    2005-10-14

    Adiabatic approximations to few-body models of nuclear scattering are described with emphasis on reactions with deuterons and halo nuclei (frozen halo approximation) as projectiles. The different ways the approximation should be implemented in a consistent theory of elastic scattering, stripping and break-up are explained and the conditions for the theory's validity are briefly discussed. A formalism which links few-body models and the underlying many-body system is outlined and the connection between the adiabatic and CDCC methods is reviewed.

  10. Novel developments and applications of the classical adiabatic dynamics technique

    NASA Astrophysics Data System (ADS)

    Rosso, Lula

    The present work aims to apply and develop modern molecular dynamics techniques based on a novel analysis of the classical adiabatic dynamics approach. In the first part of this thesis, Car-Parrinello ab-initio molecular dynamics, a successful technique based on adiabatic dynamics, is used to study the charge transport mechanism in solid ammonium perchlorate (AP) crystal exposed to an ammonia-rich environment. AP is a solid-state proton conductor composed of NH+4 and ClO-4 units that can undergo a decomposition process at high temperature, leading to its use such as rocket fuel. After computing IR spectra and carefully analysing the dynamics at different temperatures, we found that the charge transport mechanism in the pure crystal is dominated by diffusion of the ammonium ions and that the translational diffusion is strongly coupled to rotational diffusion of the two types of ions present. When the pure ammonium-perchlorate crystal is doped with neutral ammonia, another mechanism comes into play, namely, the Grotthuss proton hopping mechanism via short-lived N2H+7 complexes. In the second part of this thesis, adiabatic dynamics will be used to develop an alternative approach to the calculation of free energy profiles along reaction paths. The new method (AFED) is based on the creation of an adiabatic separation between the reaction coordinate subspace and the remaining degrees of freedom within a molecular dynamics run. This is achieved by associating with the reaction coordinate(s) a high temperature and large mass. These conditions allow the activated process to occur while permitting the remaining degrees of freedom to respond adiabatically. In this limit, by applying a formal multiple time scale Liouville operator factorization, it can be rigorously shown that the free energy profile is obtained directly from the probability distribution of the reaction coordinate subspace and, therefore, no postprocessing of the output data is required. The new method is

  11. From Classical Nonlinear Integrable Systems to Quantum Shortcuts to Adiabaticity

    NASA Astrophysics Data System (ADS)

    Okuyama, Manaka; Takahashi, Kazutaka

    2016-08-01

    Using shortcuts to adiabaticity, we solve the time-dependent Schrödinger equation that is reduced to a classical nonlinear integrable equation. For a given time-dependent Hamiltonian, the counterdiabatic term is introduced to prevent nonadiabatic transitions. Using the fact that the equation for the dynamical invariant is equivalent to the Lax equation in nonlinear integrable systems, we obtain the counterdiabatic term exactly. The counterdiabatic term is available when the corresponding Lax pair exists and the solvable systems are classified in a unified and systematic way. Multisoliton potentials obtained from the Korteweg-de Vries equation and isotropic X Y spin chains from the Toda equations are studied in detail.

  12. Resonance Ionization of Heavy Noble Gases: The Potential of KR and Xe Measurements from Single Pre-Solar Grains

    NASA Astrophysics Data System (ADS)

    Thonnard, N.

    1995-09-01

    measure noble gases from fourteen individual "X" SiC grains, previously identified by ion microprobe analysis, was unsuccessful with the 2,000 132Xe atom detection limit of the mass spectrometer [12,13]. From the Kr concentration measurements of SiC particles KJF by Lewis et al. [6], a 2 micrometer diameter particle will on average contain 134 Kr atoms. If only 4% of the SiC grains contain the majority of the noble gas atoms, then a single gas rich grain will contain 3,350 Kr atoms, or 12, 75, 385, 398, 1910, and 580 atoms for 78Kr through 86Kr, respectively. The Xe single-grain abundances would be similar. Resonance ionization, an emerging laser-based element analysis technique, is being harnessed to a wide variety of problems in which minute quantities of a particular element need to be measured efficiently in the presence of an overwhelmingly larger background of other materials [14]. By utilizing lasers tuned to specific atomic energy levels of the analyte element, ions are produced selectively in a mass spectrometer with much higher efficiency than possible using conventional methods, such as electron bombardment, thermal ionization, or ion sputtering. In a static resonance ionization system for noble gases, the combination of high ionization efficiency and sample concentrator results in an extremely fast (~3 min. detection half-life vs. ~60 min. for conventional systems) analyzer with a detection limit of ~100 85Kr atoms [15]. In addition to the almost complete absence of interferences, the short analysis time significantly reduces the background contribution of outgassing in the mass spectrometer. Although using a less efficient laser scheme resulting in slightly slower analyses, a similar system has recently been completed and dedicated to extraterrestrial Xe measurements [16]. At the newly formed Institute for Rare Isotope Measurements [17], the noble gas equipment that had previously been at Atom Sciences [14,15] is being re-installed and upgraded to provide

  13. Assessment of the "6-31+G** + LANL2DZ" Mixed Basis Set Coupled with Density Functional Theory Methods and the Effective Core Potential: Prediction of Heats of Formation and Ionization Potentials for First-Row-Transition-Metal Complexes

    NASA Astrophysics Data System (ADS)

    Yang, Yue; Weaver, Michael N.; Merz, Kenneth M.

    2009-08-01

    Computational chemists have long demonstrated great interest in finding ways to reliably and accurately predict the molecular properties for transition-metal-containing complexes. This study is a continuation of our validation efforts of density functional theory (DFT) methods when applied to transition-metal-containing systems (Riley, K.E.; Merz, K. M., Jr. J. Phys. Chem. 2007, 111, 6044-6053). In our previous work we examined DFT using all-electron basis sets, but approaches incorporating effective core potentials (ECPs) are effective in reducing computational expense. With this in mind, our efforts were expanded to include evaluation of the performance of the basis set derived to approximate such an approach as well on the same set of density functionals. Indeed, employing an ECP basis such as LANL2DZ (Los Alamos National Laboratory 2 double ζ) for transition metals, while using all-electron basis sets for all other non-transition-metal atoms, has become more and more popular in computations on transition-metal-containing systems. In this study, we assess the performance of 12 different DFT functionals, from the GGA (generalized gradient approximation), hybrid-GGA, meta-GGA, and hybrid-meta-GGA classes, respectively, along with the 6-31+G** + LANL2DZ (on the transition metal) mixed basis set in predicting two important molecular properties, heats of formation and ionization potentials, for 94 and 58 systems containing first-row transition metals from Ti to Zn, which are all in the third row of the periodic table. An interesting note is that the inclusion of the exact exchange term in density functional methods generally increases the accuracy of ionization potential prediction for the hybrid-GGA methods but decreases the reliability of determining the heats of formation for transition-metal-containing complexes for all hybrid density functional methods. The hybrid-GGA functional B3LYP gives the best performance in predicting the ionization potentials, while the

  14. Adiabatic Compression in a Fire Syringe.

    ERIC Educational Resources Information Center

    Hayn, Carl H.; Baird, Scott C.

    1985-01-01

    Suggests using better materials in fire syringes to obtain more effective results during demonstrations which show the elevation in temperature upon a very rapid (adiabatic) compression of air. Also describes an experiment (using ignition temperatures) which introduces students to the use of thermocouples for high temperature measurements. (DH)

  15. Apparatus to Measure Adiabatic and Isothermal Processes.

    ERIC Educational Resources Information Center

    Lamb, D. W.; White, G. M.

    1996-01-01

    Describes a simple manual apparatus designed to serve as an effective demonstration of the differences between isothermal and adiabatic processes for the general or elementary physics student. Enables students to verify Boyle's law for slow processes and identify the departure from this law for rapid processes and can also be used to give a clear…

  16. Ionizing radiation

    Technology Transfer Automated Retrieval System (TEKTRAN)

    This chapter gives a comprehensive review on ionizing irradiation of fresh fruits and vegetables. Topics include principles of ionizing radiation, its effects on pathogenic and spoilage microorganisms, shelf-life, sensory quality, nutritional and phytochemical composition, as well as physiologic and...

  17. Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. I. Propagation of single-active-electron wave packets in chiral pseudo-potentials.

    PubMed

    Artemyev, Anton N; Müller, Anne D; Hochstuhl, David; Demekhin, Philipp V

    2015-06-28

    A theoretical method to study the angle-resolved multiphoton ionization of polyatomic molecules is developed. It is based on the time-dependent formulation of the Single Center (TDSC) method and consists in the propagation of single-active-electron wave packets in the effective molecular potentials in the presence of intense laser pulses. For this purpose, the time-dependent Schrödinger equation for one electron, moving in a molecular field and interacting with an arbitrary laser pulse, is solved in spherical coordinates by an efficient numerical approach. As a test, the method is applied to the one- and two-photon ionizations of a model methane-like chiral system by circularly polarized short intense high-frequency laser pulses. Thereby, we analyze the photoelectron circular dichroism (PECD) in the momentum distribution. The considered model application illustrates the capability of the TDSC method to study multiphoton PECD in fixed-in-space and randomly oriented chiral molecules. PMID:26133408

  18. Ionization Time and Exit Momentum in Strong-Field Tunnel Ionization.

    PubMed

    Teeny, Nicolas; Yakaboylu, Enderalp; Bauke, Heiko; Keitel, Christoph H

    2016-02-12

    Tunnel ionization belongs to the fundamental processes of atomic physics. The so-called two-step model, which describes the ionization as instantaneous tunneling at the electric field maximum and classical motion afterwards with zero exit momentum, is commonly employed to describe tunnel ionization in adiabatic regimes. In this contribution, we show by solving numerically the time-dependent Schrödinger equation in one dimension and employing a virtual detector at the tunnel exit that there is a nonvanishing positive time delay between the electric field maximum and the instant of ionization. Moreover, we find a nonzero exit momentum in the direction of the electric field. To extract proper tunneling times from asymptotic momentum distributions of ionized electrons, it is essential to incorporate the electron's initial momentum in the direction of the external electric field. PMID:26918986

  19. Ionization Time and Exit Momentum in Strong-Field Tunnel Ionization

    NASA Astrophysics Data System (ADS)

    Teeny, Nicolas; Yakaboylu, Enderalp; Bauke, Heiko; Keitel, Christoph H.

    2016-02-01

    Tunnel ionization belongs to the fundamental processes of atomic physics. The so-called two-step model, which describes the ionization as instantaneous tunneling at the electric field maximum and classical motion afterwards with zero exit momentum, is commonly employed to describe tunnel ionization in adiabatic regimes. In this contribution, we show by solving numerically the time-dependent Schrödinger equation in one dimension and employing a virtual detector at the tunnel exit that there is a nonvanishing positive time delay between the electric field maximum and the instant of ionization. Moreover, we find a nonzero exit momentum in the direction of the electric field. To extract proper tunneling times from asymptotic momentum distributions of ionized electrons, it is essential to incorporate the electron's initial momentum in the direction of the external electric field.

  20. Transient Particle Energies in Shortcuts to Adiabatic Expansions of Harmonic Traps.

    PubMed

    Cui, Yang-Yang; Chen, Xi; Muga, J G

    2016-05-19

    The expansion of a harmonic potential that holds a quantum particle may be realized without any final particle excitation but much faster than adiabatically via "shortcuts to adiabaticity" (STA). While ideally the process time can be reduced to zero, practical limitations and constraints impose minimal finite times for the externally controlled time-dependent frequency protocols. We examine the role of different time-averaged energies (total, kinetic, potential, nonadiabatic) and of the instantaneous power in characterizing or selecting different protocols. Specifically, we prove a virial theorem for STA processes, set minimal energies (or times) for given times (or energies), and discuss their realizability by means of Dirac impulses or otherwise. PMID:26237328

  1. Vibrational states of the triplet electronic state of H3+. The role of non-adiabatic Jahn-Teller coupling

    NASA Astrophysics Data System (ADS)

    Alijah, Alexander; Kokoouline, Viatcheslav

    2015-10-01

    Vibrational energies and wave functions of the triplet state of the H3+ ion have been determined. In the calculations, the ground and first excited triplet electronic states are included as well as the most important part of the non-Born-Oppenheimer coupling between them. The diabatization procedure proposed by Longuet-Higgins is then applied to transform the two adiabatic ab initio potential energy surfaces of the triplet-H3+ state into a 2 × 2 diabatic matrix. The diabatization takes into account the effect of the geometrical phase due to the conical intersection between the two adiabatic potential surfaces. The results are compared to the calculation involving only the lowest adiabatic potential energy surface of the triplet-H3+ ion and neglecting the geometrical phase. The energy difference between results with and without the non-adiabatic coupling and the geometrical phase is about one wave number for the lowest vibrational levels.

  2. Communication: Adiabatic and non-adiabatic electron-nuclear motion: Quantum and classical dynamics

    NASA Astrophysics Data System (ADS)

    Albert, Julian; Kaiser, Dustin; Engel, Volker

    2016-05-01

    Using a model for coupled electronic-nuclear motion we investigate the range from negligible to strong non-adiabatic coupling. In the adiabatic case, the quantum dynamics proceeds in a single electronic state, whereas for strong coupling a complete transition between two adiabatic electronic states takes place. It is shown that in all coupling regimes the short-time wave-packet dynamics can be described using ensembles of classical trajectories in the phase space spanned by electronic and nuclear degrees of freedom. We thus provide an example which documents that the quantum concept of non-adiabatic transitions is not necessarily needed if electronic and nuclear motion is treated on the same footing.

  3. The dynamic instability of adiabatic blast waves

    NASA Technical Reports Server (NTRS)

    Ryu, Dongsu; Vishniac, Ethan T.

    1991-01-01

    Adiabatic blastwaves, which have a total energy injected from the center E varies as t(sup q) and propagate through a preshock medium with a density rho(sub E) varies as r(sup -omega) are described by a family of similarity solutions. Previous work has shown that adiabatic blastwaves with increasing or constant postshock entropy behind the shock front are susceptible to an oscillatory instability, caused by the difference between the nature of the forces on the two sides of the dense shell behind the shock front. This instability sets in if the dense postshock layer is sufficiently thin. The stability of adiabatic blastwaves with a decreasing postshock entropy is considered. Such blastwaves, if they are decelerating, always have a region behind the shock front which is subject to convection. Some accelerating blastwaves also have such region, depending on the values of q, omega, and gamma where gamma is the adiabatic index. However, since the shock interface stabilizes dynamically induced perturbations, blastwaves become convectively unstable only if the convective zone is localized around the origin or a contact discontinuity far from the shock front. On the other hand, the contact discontinuity of accelerating blastwaves is subject to a strong Rayleigh-Taylor instability. The frequency spectra of the nonradial, normal modes of adiabatic blastwaves have been calculated. The results have been applied to the shocks propagating through supernovae envelopes. It is shown that the metal/He and He/H interfaces are strongly unstable against the Rayleigh-Taylor instability. This instability will induce mixing in supernovae envelopes. In addition the implications of this work for the evolution of planetary nebulae is discussed.

  4. Adiabatic circuits: converter for static CMOS signals

    NASA Astrophysics Data System (ADS)

    Fischer, J.; Amirante, E.; Bargagli-Stoffi, A.; Schmitt-Landsiedel, D.

    2003-05-01

    Ultra low power applications can take great advantages from adiabatic circuitry. In this technique a multiphase system is used which consists ideally of trapezoidal voltage signals. The input signals to be processed will often come from a function block realized in static CMOS. The static rectangular signals must be converted for the oscillating multiphase system of the adiabatic circuitry. This work shows how to convert the input signals to the proposed pulse form which is synchronized to the appropriate supply voltage. By means of adder structures designed for a 0.13µm technology in a 4-phase system there will be demonstrated, which additional circuits are necessary for the conversion. It must be taken into account whether the data arrive in parallel or serial form. Parallel data are all in one phase and therefore it is advantageous to use an adder structure with a proper input stage, e.g. a Carry Lookahead Adder (CLA). With a serial input stage it is possible to read and to process four signals during one cycle due to the adiabatic 4-phase system. Therefore input signals with a frequency four times higher than the adiabatic clock frequency can be used. This reduces the disadvantage of the slow clock period typical for adiabatic circuits. By means of an 8 bit Ripple Carry Adder (8 bit RCA) the serial reading will be introduced. If the word width is larger than 4 bits the word can be divided in 4 bit words which are processed in parallel. This is the most efficient way to minimize the number of input lines and pads. At the same time a high throughput is achieved.

  5. The dynamic instability of adiabatic blast waves

    NASA Astrophysics Data System (ADS)

    Ryu, Dongsu; Vishniac, Ethan T.

    1991-02-01

    Adiabatic blastwaves, which have a total energy injected from the center E varies as tq and propagate through a preshock medium with a density rhoE varies as r-omega are described by a family of similarity solutions. Previous work has shown that adiabatic blastwaves with increasing or constant postshock entropy behind the shock front are susceptible to an oscillatory instability, caused by the difference between the nature of the forces on the two sides of the dense shell behind the shock front. This instability sets in if the dense postshock layer is sufficiently thin. The stability of adiabatic blastwaves with a decreasing postshock entropy is considered. Such blastwaves, if they are decelerating, always have a region behind the shock front which is subject to convection. Some accelerating blastwaves also have such region, depending on the values of q, omega, and gamma where gamma is the adiabatic index. However, since the shock interface stabilizes dynamically induced perturbations, blastwaves become convectively unstable only if the convective zone is localized around the origin or a contact discontinuity far from the shock front. On the other hand, the contact discontinuity of accelerating blastwaves is subject to a strong Rayleigh-Taylor instability. The frequency spectra of the nonradial, normal modes of adiabatic blastwaves have been calculated. The results have been applied to the shocks propagating through supernovae envelopes. It is shown that the metal/He and He/H interfaces are strongly unstable against the Rayleigh-Taylor instability. This instability will induce mixing in supernovae envelopes. In addition the implications of this work for the evolution of planetary nebulae is discussed.

  6. The dynamic instability of adiabatic blastwaves

    NASA Astrophysics Data System (ADS)

    Ryu, Dongsu; Vishniac, Ethan T.

    1990-05-01

    Adiabatic blastwaves, which have a total energy injected from the center E varies as t(sup q) and propagate through a preshock medium with a density rho(sub E) varies as r(sup -omega) are described by a family of similarity solutions. Previous work has shown that adiabatic blastwaves with increasing or constant postshock entropy behind the shock front are susceptible to an oscillatory instability, caused by the difference between the nature of the forces on the two sides of the dense shell behind the shock front. This instability sets in if the dense postshock layer is sufficiently thin. The stability of adiabatic blastwaves with a decreasing postshock entropy is considered. Such blastwaves, if they are decelerating, always have a region behind the shock front which is subject to convection. Some accelerating blastwaves also have such region, depending on the values of q, omega, and gamma where gamma is the adiabatic index. However, since the shock interface stabilizes dynamically induced perturbations, blastwaves become convectively unstable only if the convective zone is localized around the origin or a contact discontinuity far from the shock front. On the other hand, the contact discontinuity of accelerating blastwaves is subject to a strong Rayleigh-Taylor instability. The frequency spectra of the nonradial, normal modes of adiabatic blastwaves have been calculated. The results have been applied to the shocks propagating through supernovae envelopes. It is shown that the metal/He and He/H interfaces are strongly unstable against the Rayleigh-Taylor instability. This instability will induce mixing in supernovae envelopes. In addition the implications of this work for the evolution of planetary nebulae is discussed.

  7. Adiabatic burst evaporation from bicontinuous nanoporous membranes

    PubMed Central

    Ichilmann, Sachar; Rücker, Kerstin; Haase, Markus; Enke, Dirk

    2015-01-01

    Evaporation of volatile liquids from nanoporous media with bicontinuous morphology and pore diameters of a few 10 nm is an ubiquitous process. For example, such drying processes occur during syntheses of nanoporous materials by sol–gel chemistry or by spinodal decomposition in the presence of solvents as well as during solution impregnation of nanoporous hosts with functional guests. It is commonly assumed that drying is endothermic and driven by non-equilibrium partial pressures of the evaporating species in the gas phase. We show that nearly half of the liquid evaporates in an adiabatic mode involving burst-like liquid-to-gas conversions. During single adiabatic burst evaporation events liquid volumes of up to 107 μm3 are converted to gas. The adiabatic liquid-to-gas conversions occur if air invasion fronts get unstable because of the built-up of high capillary pressures. Adiabatic evaporation bursts propagate avalanche-like through the nanopore systems until the air invasion fronts have reached new stable configurations. Adiabatic cavitation bursts thus compete with Haines jumps involving air invasion front relaxation by local liquid flow without enhanced mass transport out of the nanoporous medium and prevail if the mean pore diameter is in the range of a few 10 nm. The results reported here may help optimize membrane preparation via solvent-based approaches, solution-loading of nanopore systems with guest materials as well as routine use of nanoporous membranes with bicontinuous morphology and may contribute to better understanding of adsorption/desorption processes in nanoporous media. PMID:25926406

  8. Multielectron dynamics in the tunneling ionization of correlated quantum systems

    NASA Astrophysics Data System (ADS)

    Hollstein, Maximilian; Pfannkuche, Daniela

    2015-11-01

    The importance of multielectron dynamics during the tunneling ionization of a correlated quantum system is investigated. By comparison of the solution of the time-dependent Schrödinger equation with the time-dependent configuration-interaction singles approach, we demonstrate the importance of a multielectron description of the tunneling ionization process especially for weakly confined quantum systems. Within this context, we observe that adiabatic driving by an intense light field can even enhance the correlations between still trapped electrons.

  9. Adiabatic evolution of an irreversible two level system

    SciTech Connect

    Kvitsinsky, A.; Putterman, S. )

    1991-05-01

    The adiabatic dynamics of a two level atom with spontaneous decay is studied. The existence of a complex adiabatic phase shift is established: The real part being the usual Berry's phase. A closed-form expression for this phase and the adiabatic transition amplitudes is obtained. Incorporation of a finite preparation time for the initial state yields a new asymptotic form for the adiabatic transition amplitudes which is significantly different from the standard Landau--Zener--Dykhne formula.

  10. Adiabatic expansion of cosmic ray sources and the consequences for secondary antiprotons

    NASA Technical Reports Server (NTRS)

    Mauger, B. G.; Stephens, S. A.

    1983-01-01

    The low-energy antiproton flux measurement of Buffinton et al. (1981) is more than an order of magnitude higher than can be explained by interstellar production. It has been suggested that the excess antiprotons may be created by supernovae in very dense regions of ISM. These sources would provide the additional target material necessary to produce the excess cosmic ray antiprotons; in addition, adiabatic energy losses due to supernova expansion will increase the flux of low-energy antiprotons. The antiproton flux from such sources is examined here, with attention given to the energy loss effects of the adiabatic and collisional losses of both the primary and secondary cosmic ray fluxes. Ionization losses of the antiprotons are also considered.

  11. Transport of ultracold atoms between concentric traps via spatial adiabatic passage

    NASA Astrophysics Data System (ADS)

    Polo, J.; Benseny, A.; Busch, Th; Ahufinger, V.; Mompart, J.

    2016-01-01

    Spatial adiabatic passage processes for ultracold atoms trapped in tunnel-coupled cylindrically symmetric concentric potentials are investigated. Specifically, we discuss the matter-wave analog of the rapid adiabatic passage (RAP) technique for a high fidelity and robust loading of a single atom into a harmonic ring potential from a harmonic trap, and for its transport between two concentric rings. We also consider a system of three concentric rings and investigate the transport of a single atom between the innermost and the outermost rings making use of the matter-wave analog of the stimulated Raman adiabatic passage (STIRAP) technique. We describe the RAP-like and STIRAP-like dynamics by means of a two- and a three-state model, respectively, obtaining good agreement with the numerical simulations of the corresponding two-dimensional Schrödinger equation.

  12. Geometry- and diffraction-independent ionization probabilities in intense laser fields: Probing atomic ionization mechanisms with effective intensity matching

    SciTech Connect

    Bryan, W. A.; Stebbings, S. L.; English, E. M. L.; Goodworth, T. R. J.; Newell, W. R.; McKenna, J.; Suresh, M.; Srigengan, B.; Williams, I. D.; Turcu, I. C. E.; Smith, J. M.; Divall, E. J.; Hooker, C. J.; Langley, A. J.

    2006-01-15

    We report an experimental technique for the comparison of ionization processes in ultrafast laser pulses irrespective of pulse ellipticity. Multiple ionization of xenon by 50 fs 790 nm, linearly and circularly polarized laser pulses is observed over the intensity range 10 TW/cm{sup 2} to 10 PW/cm{sup 2} using effective intensity matching (EIM), which is coupled with intensity selective scanning (ISS) to recover the geometry-independent probability of ionization. Such measurements, made possible by quantifying diffraction effects in the laser focus, are compared directly to theoretical predictions of multiphoton, tunnel and field ionization, and a remarkable agreement demonstrated. EIM-ISS allows the straightforward quantification of the probability of recollision ionization in a linearly polarized laser pulse. Furthermore, the probability of ionization is discussed in terms of the Keldysh adiabaticity parameter {gamma}, and the influence of the precursor ionic states present in recollision ionization is observed.

  13. Vibrational analysis and ionization potentials of XCH 3 (X=Be,Mg,Ca) calculated by hybrid density functional theory and high order ab initio methods

    NASA Astrophysics Data System (ADS)

    Jalbout, Abraham F.

    2001-06-01

    The amount of attention dedicated to the theoretical and experimental investigation of small cationic organometallic systems in the literature is very limited. In this Letter we use the B3LYP method with a variety of basis sets as well as the very advanced CBS-Q, CBS-QB3, G1, G2MP2, G2, G3, and G3B3 ab initio methods in order to analyze the vibrational spectra as well as ionization potentials of BeCH 3,MgCH 3 and CaCH 3. The need for further addition of experimental data to the archives for these systems is discussed, as well as recommendations for which theoretical methods are optimum for a particular result.

  14. Acanthocephalan fish parasites (Rhadinorhynchidae Lühe, 1912) as potential biomarkers: Molecular-chemical screening by pyrolysis-field ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

    Kleinertz, S.; Eckhardt, K.-U.; Theisen, S.; Palm, H. W.; Leinweber, P.

    2016-07-01

    The present study represents the first molecular-chemical screening by pyrolysis-field ionization mass spectrometry applied on fish parasites. A total of 71 fishes from Balinese fish markets, 36 Auxis rochei (Risso, 1810) and 35 A. thazard (Lacepède, 1800), were studied for their acanthocephalan parasites. This is the first record of Rhadinorhynchus zhukovi in Balinese waters, Indonesia, and we describe for the first time A. rochei and A. thazard as R. zhukovi hosts. Using this method, small scale variations within the chemical compounds of acanthocephalans could be detected. Using this methodology it will be possible to generate additional, pollutant specific information from aquatic habitats in future with the potential of a new bioindicator application for parasite/host origin and/or environmental pollution.

  15. Effect of Ionization Potential of Hole Transport Layer on Device Characteristics of Organic Light Emitting Diode with Oxygen Plasma Treated Indium Tin Oxide

    NASA Astrophysics Data System (ADS)

    Hashimoto, Yuichi; Hamagaki, Manabu; Sakakibara, Takeshi

    2001-07-01

    We have investigated the contribution of the oxygen ions and electrons, and of the kinetic energy of these species on oxygen plasma treatment of indium tin oxide (ITO) electrode. In the case of the treatment by positive oxygen ions with kinetic energy of 50 eV, the luminance increased markedly with a lowering of the operating voltage in the organic light emitting diode (OLED). The change in the device characteristics was attributed to an effective removal of organic contaminants from the ITO surface, leading to enhanced hole injection from ITO to a hole transport layer (HTL) due to an increase in work function of the ITO@. Moreover, the highest luminance and luminous efficiency were obtained in the OLED having HTL with ionization potential of 5.4 eV@. These results have suggested that OLEDs fabricated using the oxygen plasma treated ITO can give the best device performance by the selection of an optimum HTL.

  16. Deep proton tunneling in the electronically adiabatic and non-adiabatic limits: Comparison of the quantum and classical treatment of donor-acceptor motion in a protein environment

    SciTech Connect

    Benabbas, Abdelkrim; Salna, Bridget; Sage, J. Timothy; Champion, Paul M.

    2015-03-21

    Analytical models describing the temperature dependence of the deep tunneling rate, useful for proton, hydrogen, or hydride transfer in proteins, are developed and compared. Electronically adiabatic and non-adiabatic expressions are presented where the donor-acceptor (D-A) motion is treated either as a quantized vibration or as a classical “gating” distribution. We stress the importance of fitting experimental data on an absolute scale in the electronically adiabatic limit, which normally applies to these reactions, and find that vibrationally enhanced deep tunneling takes place on sub-ns timescales at room temperature for typical H-bonding distances. As noted previously, a small room temperature kinetic isotope effect (KIE) does not eliminate deep tunneling as a major transport channel. The quantum approach focuses on the vibrational sub-space composed of the D-A and hydrogen atom motions, where hydrogen bonding and protein restoring forces quantize the D-A vibration. A Duschinsky rotation is mandated between the normal modes of the reactant and product states and the rotation angle depends on the tunneling particle mass. This tunnel-mass dependent rotation contributes substantially to the KIE and its temperature dependence. The effect of the Duschinsky rotation is solved exactly to find the rate in the electronically non-adiabatic limit and compared to the Born-Oppenheimer (B-O) approximation approach. The B-O approximation is employed to find the rate in the electronically adiabatic limit, where we explore both harmonic and quartic double-well potentials for the hydrogen atom bound states. Both the electronically adiabatic and non-adiabatic rates are found to diverge at high temperature unless the proton coupling includes the often neglected quadratic term in the D-A displacement from equilibrium. A new expression is presented for the electronically adiabatic tunnel rate in the classical limit for D-A motion that should be useful to experimentalists working

  17. Deep proton tunneling in the electronically adiabatic and non-adiabatic limits: comparison of the quantum and classical treatment of donor-acceptor motion in a protein environment.

    PubMed

    Benabbas, Abdelkrim; Salna, Bridget; Sage, J Timothy; Champion, Paul M

    2015-03-21

    Analytical models describing the temperature dependence of the deep tunneling rate, useful for proton, hydrogen, or hydride transfer in proteins, are developed and compared. Electronically adiabatic and non-adiabatic expressions are presented where the donor-acceptor (D-A) motion is treated either as a quantized vibration or as a classical "gating" distribution. We stress the importance of fitting experimental data on an absolute scale in the electronically adiabatic limit, which normally applies to these reactions, and find that vibrationally enhanced deep tunneling takes place on sub-ns timescales at room temperature for typical H-bonding distances. As noted previously, a small room temperature kinetic isotope effect (KIE) does not eliminate deep tunneling as a major transport channel. The quantum approach focuses on the vibrational sub-space composed of the D-A and hydrogen atom motions, where hydrogen bonding and protein restoring forces quantize the D-A vibration. A Duschinsky rotation is mandated between the normal modes of the reactant and product states and the rotation angle depends on the tunneling particle mass. This tunnel-mass dependent rotation contributes substantially to the KIE and its temperature dependence. The effect of the Duschinsky rotation is solved exactly to find the rate in the electronically non-adiabatic limit and compared to the Born-Oppenheimer (B-O) approximation approach. The B-O approximation is employed to find the rate in the electronically adiabatic limit, where we explore both harmonic and quartic double-well potentials for the hydrogen atom bound states. Both the electronically adiabatic and non-adiabatic rates are found to diverge at high temperature unless the proton coupling includes the often neglected quadratic term in the D-A displacement from equilibrium. A new expression is presented for the electronically adiabatic tunnel rate in the classical limit for D-A motion that should be useful to experimentalists working near

  18. Deep proton tunneling in the electronically adiabatic and non-adiabatic limits: Comparison of the quantum and classical treatment of donor-acceptor motion in a protein environment

    NASA Astrophysics Data System (ADS)

    Benabbas, Abdelkrim; Salna, Bridget; Sage, J. Timothy; Champion, Paul M.

    2015-03-01

    Analytical models describing the temperature dependence of the deep tunneling rate, useful for proton, hydrogen, or hydride transfer in proteins, are developed and compared. Electronically adiabatic and non-adiabatic expressions are presented where the donor-acceptor (D-A) motion is treated either as a quantized vibration or as a classical "gating" distribution. We stress the importance of fitting experimental data on an absolute scale in the electronically adiabatic limit, which normally applies to these reactions, and find that vibrationally enhanced deep tunneling takes place on sub-ns timescales at room temperature for typical H-bonding distances. As noted previously, a small room temperature kinetic isotope effect (KIE) does not eliminate deep tunneling as a major transport channel. The quantum approach focuses on the vibrational sub-space composed of the D-A and hydrogen atom motions, where hydrogen bonding and protein restoring forces quantize the D-A vibration. A Duschinsky rotation is mandated between the normal modes of the reactant and product states and the rotation angle depends on the tunneling particle mass. This tunnel-mass dependent rotation contributes substantially to the KIE and its temperature dependence. The effect of the Duschinsky rotation is solved exactly to find the rate in the electronically non-adiabatic limit and compared to the Born-Oppenheimer (B-O) approximation approach. The B-O approximation is employed to find the rate in the electronically adiabatic limit, where we explore both harmonic and quartic double-well potentials for the hydrogen atom bound states. Both the electronically adiabatic and non-adiabatic rates are found to diverge at high temperature unless the proton coupling includes the often neglected quadratic term in the D-A displacement from equilibrium. A new expression is presented for the electronically adiabatic tunnel rate in the classical limit for D-A motion that should be useful to experimentalists working near

  19. Non-adiabatic perturbations in multi-component perfect fluids

    SciTech Connect

    Koshelev, N.A.

    2011-04-01

    The evolution of non-adiabatic perturbations in models with multiple coupled perfect fluids with non-adiabatic sound speed is considered. Instead of splitting the entropy perturbation into relative and intrinsic parts, we introduce a set of symmetric quantities, which also govern the non-adiabatic pressure perturbation in models with energy transfer. We write the gauge invariant equations for the variables that determine on a large scale the non-adiabatic pressure perturbation and the rate of changes of the comoving curvature perturbation. The analysis of evolution of the non-adiabatic pressure perturbation has been made for several particular models.

  20. Adiabatic Far Field Sub-Diffraction Imaging

    PubMed Central

    Cang, Hu; Salandrino, Alessandro; Wang, Yuan; Zhang, Xiang

    2015-01-01

    The limited resolution of a conventional optical imaging system stems from the fact that the fine feature information of an object is carried by evanescent waves, which exponentially decay in space thus cannot reach the imaging plane. We introduce here a new concept of adiabatic lens, which utilizes a geometrically conformal surface to mediate the interference of slowly decompressed electromagnetic waves at far field to form images. The decompression is satisfying an adiabatic condition, and by bridging the gap between far field and near field, it allows far field optical systems to project an image of the near field features directly. Using these designs, we demonstrated the magnification can be up to 20 times and it is possible to achieve sub-50nm imaging resolution in visible. Our approach provides a means to extend the domain of geometrical optics to a deep sub-wavelength scale. PMID:26258769

  1. Shortcuts to adiabaticity from linear response theory.

    PubMed

    Acconcia, Thiago V; Bonança, Marcus V S; Deffner, Sebastian

    2015-10-01

    A shortcut to adiabaticity is a finite-time process that produces the same final state as would result from infinitely slow driving. We show that such shortcuts can be found for weak perturbations from linear response theory. With the help of phenomenological response functions, a simple expression for the excess work is found-quantifying the nonequilibrium excitations. For two specific examples, i.e., the quantum parametric oscillator and the spin 1/2 in a time-dependent magnetic field, we show that finite-time zeros of the excess work indicate the existence of shortcuts. Finally, we propose a degenerate family of protocols, which facilitates shortcuts to adiabaticity for specific and very short driving times. PMID:26565209

  2. Arbitrary qudit gates by adiabatic passage

    NASA Astrophysics Data System (ADS)

    Rousseaux, B.; Guérin, S.; Vitanov, N. V.

    2013-03-01

    We derive an adiabatic technique that implements the most general SU(d) transformation in a quantum system of d degenerate states, featuring a qudit. This technique is based on the factorization of the SU(d) transformation into d generalized quantum Householder reflections, each of which is implemented by a two-shot stimulated Raman adiabatic passage with appropriate static phases. The energy of the lasers needed to synthesize a single Householder reflection is shown to be remarkably constant as a function of d. This technique is directly applicable to a linear trapped ion system with d+1 ions. We implement the quantum Fourier transform numerically in a qudit with d=4 (defined as a quartit) as an example.

  3. Trapped Ion Quantum Computation by Adiabatic Passage

    SciTech Connect

    Feng Xuni; Wu Chunfeng; Lai, C. H.; Oh, C. H.

    2008-11-07

    We propose a new universal quantum computation scheme for trapped ions in thermal motion via the technique of adiabatic passage, which incorporates the advantages of both the adiabatic passage and the model of trapped ions in thermal motion. Our scheme is immune from the decoherence due to spontaneous emission from excited states as the system in our scheme evolves along a dark state. In our scheme the vibrational degrees of freedom are not required to be cooled to their ground states because they are only virtually excited. It is shown that the fidelity of the resultant gate operation is still high even when the magnitude of the effective Rabi frequency moderately deviates from the desired value.

  4. Adiabatic Quantum Optimization for Associative Memory Recall

    NASA Astrophysics Data System (ADS)

    Seddiqi, Hadayat; Humble, Travis

    2014-12-01

    Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are stored in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.

  5. Quantum adiabatic evolution with energy degeneracy levels

    NASA Astrophysics Data System (ADS)

    Zhang, Qi

    2016-01-01

    A classical-kind phase-space formalism is developed to address the tiny intrinsic dynamical deviation from what is predicted by Wilczek-Zee theorem during quantum adiabatic evolution on degeneracy levels. In this formalism, the Hilbert space and the aggregate of degenerate eigenstates become the classical-kind phase space and a high-dimensional subspace in the phase space, respectively. Compared with the previous analogous study by a different method, the current result is qualitatively different in that the first-order deviation derived here is always perpendicular to the degeneracy subspace. A tripod-scheme Hamiltonian with two degenerate dark states is employed to illustrate the adiabatic deviation with degeneracy levels.

  6. Shortcuts to adiabaticity from linear response theory

    NASA Astrophysics Data System (ADS)

    Acconcia, Thiago V.; Bonança, Marcus V. S.; Deffner, Sebastian

    2015-10-01

    A shortcut to adiabaticity is a finite-time process that produces the same final state as would result from infinitely slow driving. We show that such shortcuts can be found for weak perturbations from linear response theory. With the help of phenomenological response functions, a simple expression for the excess work is found—quantifying the nonequilibrium excitations. For two specific examples, i.e., the quantum parametric oscillator and the spin 1/2 in a time-dependent magnetic field, we show that finite-time zeros of the excess work indicate the existence of shortcuts. Finally, we propose a degenerate family of protocols, which facilitates shortcuts to adiabaticity for specific and very short driving times.

  7. Adiabatic quantum optimization for associative memory recall

    DOE PAGESBeta

    Seddiqi, Hadayat; Humble, Travis S.

    2014-12-22

    Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are storedmore » in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.« less

  8. Adiabatic quantum optimization for associative memory recall

    SciTech Connect

    Seddiqi, Hadayat; Humble, Travis S.

    2014-12-22

    Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are stored in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.

  9. Shortcuts to adiabaticity from linear response theory

    SciTech Connect

    Acconcia, Thiago V.; Bonança, Marcus V. S.; Deffner, Sebastian

    2015-10-23

    A shortcut to adiabaticity is a finite-time process that produces the same final state as would result from infinitely slow driving. We show that such shortcuts can be found for weak perturbations from linear response theory. Moreover, with the help of phenomenological response functions, a simple expression for the excess work is found—quantifying the nonequilibrium excitations. For two specific examples, i.e., the quantum parametric oscillator and the spin 1/2 in a time-dependent magnetic field, we show that finite-time zeros of the excess work indicate the existence of shortcuts. We finally propose a degenerate family of protocols, which facilitates shortcuts to adiabaticity for specific and very short driving times.

  10. Shortcuts to adiabaticity from linear response theory

    DOE PAGESBeta

    Acconcia, Thiago V.; Bonança, Marcus V. S.; Deffner, Sebastian

    2015-10-23

    A shortcut to adiabaticity is a finite-time process that produces the same final state as would result from infinitely slow driving. We show that such shortcuts can be found for weak perturbations from linear response theory. Moreover, with the help of phenomenological response functions, a simple expression for the excess work is found—quantifying the nonequilibrium excitations. For two specific examples, i.e., the quantum parametric oscillator and the spin 1/2 in a time-dependent magnetic field, we show that finite-time zeros of the excess work indicate the existence of shortcuts. We finally propose a degenerate family of protocols, which facilitates shortcuts tomore » adiabaticity for specific and very short driving times.« less

  11. Adiabatic Quantization of Andreev Quantum Billiard Levels

    NASA Astrophysics Data System (ADS)

    Silvestrov, P. G.; Goorden, M. C.; Beenakker, C. W.

    2003-03-01

    We identify the time T between Andreev reflections as a classical adiabatic invariant in a ballistic chaotic cavity (Lyapunov exponent λ), coupled to a superconductor by an N-mode constriction. Quantization of the adiabatically invariant torus in phase space gives a discrete set of periods Tn, which in turn generate a ladder of excited states ɛnm=(m+1/2)πℏ/Tn. The largest quantized period is the Ehrenfest time T0=λ-1ln(N. Projection of the invariant torus onto the coordinate plane shows that the wave functions inside the cavity are squeezed to a transverse dimension W/(N), much below the width W of the constriction.

  12. Adiabatic state preparation study of methylene

    SciTech Connect

    Veis, Libor Pittner, Jiří

    2014-06-07

    Quantum computers attract much attention as they promise to outperform their classical counterparts in solving certain type of problems. One of them with practical applications in quantum chemistry is simulation of complex quantum systems. An essential ingredient of efficient quantum simulation algorithms are initial guesses of the exact wave functions with high enough fidelity. As was proposed in Aspuru-Guzik et al. [Science 309, 1704 (2005)], the exact ground states can in principle be prepared by the adiabatic state preparation method. Here, we apply this approach to preparation of the lowest lying multireference singlet electronic state of methylene and numerically investigate preparation of this state at different molecular geometries. We then propose modifications that lead to speeding up the preparation process. Finally, we decompose the minimal adiabatic state preparation employing the direct mapping in terms of two-qubit interactions.

  13. Adiabatic Quantum Simulation of Quantum Chemistry

    PubMed Central

    Babbush, Ryan; Love, Peter J.; Aspuru-Guzik, Alán

    2014-01-01

    We show how to apply the quantum adiabatic algorithm directly to the quantum computation of molecular properties. We describe a procedure to map electronic structure Hamiltonians to 2-body qubit Hamiltonians with a small set of physically realizable couplings. By combining the Bravyi-Kitaev construction to map fermions to qubits with perturbative gadgets to reduce the Hamiltonian to 2-body, we obtain precision requirements on the coupling strengths and a number of ancilla qubits that scale polynomially in the problem size. Hence our mapping is efficient. The required set of controllable interactions includes only two types of interaction beyond the Ising interactions required to apply the quantum adiabatic algorithm to combinatorial optimization problems. Our mapping may also be of interest to chemists directly as it defines a dictionary from electronic structure to spin Hamiltonians with physical interactions. PMID:25308187

  14. Pulse sequences in photoassociation via adiabatic passage

    NASA Astrophysics Data System (ADS)

    Li, Xuan; Dupre, William; Parker, Gregory A.

    2012-07-01

    We perform a detailed study of pulse sequences in a photoassociation via adiabatic passage (PAP) process to transfer population from an ensemble of ultracold atomic clouds to a vibrationally cold molecular state. We show that an appreciable final population of ultracold NaCs molecules can be achieved with optimized pulses in either the ‘counter-intuitive’ (tP > tS) or ‘intuitive’ (tP < tS) PAP pulse sequences, with tP and tS denoting the temporal centers of the pump and Stokes pulses, respectively. By investigating the dependence of the reactive yield on pulse sequences, in a wide range of tP-tS, we show that there is not a fundamental preference to either pulse sequence in a PAP process. We explain this no-sequence-preference phenomenon by analyzing a multi-bound model so that an analogy can be drawn to the conventional stimulated Raman adiabatic passage.

  15. ADIABATIC MASS LOSS IN BINARY STARS. I. COMPUTATIONAL METHOD

    SciTech Connect

    Ge Hongwei; Chen Xuefei; Han Zhanwen; Webbink, Ronald F. E-mail: mshjell@gmail.co

    2010-07-10

    binary provides the energy to eject the common envelope; the energy budget for this process consists essentially of the initial orbital energy of the binary and the initial self-energies of the binary components. We emphasize that, because the stellar core and envelope contribute mutually to each other's gravitational potential energy, proper evaluation of the total energy of a star requires integration over the entire stellar interior, and not just over the ejected envelope alone as commonly assumed. We show that the change in total energy of the donor star, as a function of its remaining mass along an adiabatic mass-loss sequence, can be calculated either by integration over initial and final models, or by a path integral along the mass-loss sequence. That change in total energy of the donor star, combined with the requirement that both remnant donor and its companion star fit within their respective Roche lobes, then circumscribes energetically possible survivors of common envelope evolution.

  16. Adiabatic charging of nickel-hydrogen batteries

    NASA Technical Reports Server (NTRS)

    Lurie, Chuck; Foroozan, S.; Brewer, Jeff; Jackson, Lorna

    1995-01-01

    Battery management during prelaunch activities has always required special attention and careful planning. The transition from nickel-cadium to nickel-hydrogen batteries, with their high self discharge rate and lower charge efficiency, as well as longer prelaunch scenarios, has made this aspect of spacecraft battery management even more challenging. The AXAF-I Program requires high battery state of charge at launch. The use of active cooling, to ensure efficient charging, was considered and proved to be difficult and expensive. Alternative approaches were evaluated. Optimized charging, in the absence of cooling, appeared promising and was investigated. Initial testing was conducted to demonstrate the feasibility of the 'Adiabatic Charging' approach. Feasibility was demonstrated and additional testing performed to provide a quantitative, parametric data base. The assumption that the battery is in an adiabatic environment during prelaunch charging is a conservative approximation because the battery will transfer some heat to its surroundings by convective air cooling. The amount is small compared to the heat dissipated during battery overcharge. Because the battery has a large thermal mass, substantial overcharge can occur before the cells get too hot to charge efficiently. The testing presented here simulates a true adiabatic environment. Accordingly the data base may be slightly conservative. The adiabatic charge methodology used in this investigation begins with stabilizing the cell at a given starting temperature. The cell is then fully insulated on all sides. Battery temperature is carefully monitored and the charge terminated when the cell temperature reaches 85 F. Charging has been evaluated with starting temperatures from 55 to 75 F.

  17. Advanced Adiabatic Demagnetization Refrigerators for Continuous Cooling

    NASA Technical Reports Server (NTRS)

    Chu, Paul C. W.

    2004-01-01

    The research at Houston was focused on optimizing the design of superconducting magnets for advanced adiabatic demagnetization refrigerators (ADRs), assessing the feasibility of using high temperature superconducting (HTS) magnets in ADRs in the future, and developing techniques to deposit HTS thin and thick films on high strength, low thermal conductivity substrates for HTS magnet leads. Several approaches have been tested for the suggested superconducting magnets.

  18. Computer Code For Turbocompounded Adiabatic Diesel Engine

    NASA Technical Reports Server (NTRS)

    Assanis, D. N.; Heywood, J. B.

    1988-01-01

    Computer simulation developed to study advantages of increased exhaust enthalpy in adiabatic turbocompounded diesel engine. Subsytems of conceptual engine include compressor, reciprocator, turbocharger turbine, compounded turbine, ducting, and heat exchangers. Focus of simulation of total system is to define transfers of mass and energy, including release and transfer of heat and transfer of work in each subsystem, and relationship among subsystems. Written in FORTRAN IV.

  19. Siphon flows in isolated magnetic flux tubes. II - Adiabatic flows

    NASA Technical Reports Server (NTRS)

    Montesinos, Benjamin; Thomas, John H.

    1989-01-01

    This paper extends the study of steady siphon flows in isolated magnetic flux tubes surrounded by field-free gas to the case of adiabatic flows. The basic equations governing steady adiabatic siphon flows in a thin, isolated magnetic flux tube are summarized, and qualitative features of adiabatic flows in elevated, arched flux tubes are discussed. The equations are then cast in nondimensional form and the results of numerical computations of adiabatic siphon flows in arched flux tubes are presented along with comparisons between isothermal and adiabatic flows. The effects of making the interior of the flux tube hotter or colder than the surrounding atmosphere at the upstream footpoint of the arch is considered. In this case, is it found that the adiabatic flows are qualitatively similar to the isothermal flows, with adiabatic cooling producing quantitative differences. Critical flows can produce a bulge point in the rising part of the arch and a concentration of magnetic flux above the bulge point.

  20. Random matrix model of adiabatic quantum computing

    SciTech Connect

    Mitchell, David R.; Adami, Christoph; Lue, Waynn; Williams, Colin P.

    2005-05-15

    We present an analysis of the quantum adiabatic algorithm for solving hard instances of 3-SAT (an NP-complete problem) in terms of random matrix theory (RMT). We determine the global regularity of the spectral fluctuations of the instantaneous Hamiltonians encountered during the interpolation between the starting Hamiltonians and the ones whose ground states encode the solutions to the computational problems of interest. At each interpolation point, we quantify the degree of regularity of the average spectral distribution via its Brody parameter, a measure that distinguishes regular (i.e., Poissonian) from chaotic (i.e., Wigner-type) distributions of normalized nearest-neighbor spacings. We find that for hard problem instances - i.e., those having a critical ratio of clauses to variables - the spectral fluctuations typically become irregular across a contiguous region of the interpolation parameter, while the spectrum is regular for easy instances. Within the hard region, RMT may be applied to obtain a mathematical model of the probability of avoided level crossings and concomitant failure rate of the adiabatic algorithm due to nonadiabatic Landau-Zener-type transitions. Our model predicts that if the interpolation is performed at a uniform rate, the average failure rate of the quantum adiabatic algorithm, when averaged over hard problem instances, scales exponentially with increasing problem size.

  1. Adiabatic heating in impulsive solar flares

    NASA Technical Reports Server (NTRS)

    Maetzler, C.; Bai, T.; Crannell, C. J.; Frost, K. J.

    1978-01-01

    A study is made of adiabatic heating in two impulsive solar flares on the basis of dynamic X-ray spectra in the 28-254 keV range, H-alpha, microwave, and meter-wave radio observations. It is found that the X-ray spectra of the events are like those of thermal bremsstrahlung from single-temperature plasmas in the 10-60 keV range if photospheric albedo is taken into account. The temperature-emission correlation indicates adiabatic compression followed by adiabatic expansion and that the electron distribution remains isotropic. H-alpha data suggest compressive energy transfer. The projected areas and volumes of the flares are estimated assuming that X-ray and microwave emissions are produced in a single thermal plasma. Electron densities of about 10 to the 9th/cu cm are found for homogeneous, spherically symmetric sources. It is noted that the strong self-absorption of hot-plasma gyrosynchrotron radiation reveals low magnetic field strengths.

  2. Aspects of adiabatic population transfer and control

    NASA Astrophysics Data System (ADS)

    Demirplak, Mustafa

    This thesis explores two different questions. The first question we answer is how to restore a given population transfer scenario given that it works efficiently in the adiabatic limit but fails because of lack of intensity and/or short duration. We derive a very simple algorithm to do this and apply it to both toy and realistic models. Two results emerge from this study. While the mathematical existence of the programme is certain it might not always be physically desirable. The restoration of adiabaticity is phase sensitive. The second question that is answered in this thesis is not how to invent new control paradigms, but rather what would happen to them in the presence of stochastic perturbers. We first use a phenomenological model to study the effect of stochastic dephasing on population transfer by stimulated Raman adiabatic passage. The results of this Monte Carlo calculation are qualitatively explained with a perturbation theoretical result in the dressed state basis. The reliability of our phenomenological model is questioned through a more rigorous hybrid quantal-classical simulation of controlled population transfer in HCl in Ar.

  3. Non-adiabatic effect on quantum pumping

    NASA Astrophysics Data System (ADS)

    Uchiyama, Chikako

    2014-03-01

    We study quantum pumping for an anharmonic junction model which interacts with two kinds of bosonic environments. We provide an expression for the quantum pumping under a piecewise modulation of environmental temperatures with including non-adiabatic effect under Markovian approximation. The obtained formula is an extension of the one expressed with the geometrical phase(Phys. Rev. Lett. 104,170601 (2010)). This extension shows that the quantum pumping depends on the initial condition of the anharmonic junction just before the modulation, as well as the characteristic environmental parameters such as interaction strength and cut-off frequencies of spectral density other than the conditions of modulation. We clarify that the pumping current including non-adiabatic effect can be larger than that under the adiabatic condition. This means that we can find the optimal condition of the current by adjusting these parameters. (The article has been submitted as http://arxiv.org/submit/848201 and will be appeared soon.) This work is supported by a Grant-in-Aid for Scientific Research (B) (KAKENHI 25287098).

  4. An adiabatic approximation for grain alignment theory

    NASA Astrophysics Data System (ADS)

    Roberge, W. G.

    1997-10-01

    The alignment of interstellar dust grains is described by the joint distribution function for certain `internal' and `external' variables, where the former describe the orientation of the axes of a grain with respect to its angular momentum, J, and the latter describe the orientation of J relative to the interstellar magnetic field. I show how the large disparity between the dynamical time-scales of the internal and external variables - which is typically 2-3 orders of magnitude - can be exploited to simplify calculations of the required distribution greatly. The method is based on an `adiabatic approximation' which closely resembles the Born-Oppenheimer approximation in quantum mechanics. The adiabatic approximation prescribes an analytic distribution function for the `fast' dynamical variables and a simplified Fokker-Planck equation for the `slow' variables which can be solved straightforwardly using various techniques. These solutions are accurate to O(epsilon), where epsilon is the ratio of the fast and slow dynamical time-scales. As a simple illustration of the method, I derive an analytic solution for the joint distribution established when Barnett relaxation acts in concert with gas damping. The statistics of the analytic solution agree with the results of laborious numerical calculations which do not exploit the adiabatic approximation.

  5. An Adiabatic Approximation for Grain Alignment Theory

    NASA Astrophysics Data System (ADS)

    Roberge, W. G.

    1997-12-01

    The alignment of interstellar dust grains is described by the joint distribution function for certain ``internal'' and ``external'' variables, where the former describe the orientation of a grain's axes with respect to its angular momentum, J, and the latter describe the orientation of J relative to the interstellar magnetic field. I show how the large disparity between the dynamical timescales of the internal and external variables--- which is typically 2--3 orders of magnitude--- can be exploited to greatly simplify calculations of the required distribution. The method is based on an ``adiabatic approximation'' which closely resembles the Born-Oppenheimer approximation in quantum mechanics. The adiabatic approximation prescribes an analytic distribution function for the ``fast'' dynamical variables and a simplified Fokker-Planck equation for the ``slow'' variables which can be solved straightforwardly using various techniques. These solutions are accurate to cal {O}(epsilon ), where epsilon is the ratio of the fast and slow dynamical timescales. As a simple illustration of the method, I derive an analytic solution for the joint distribution established when Barnett relaxation acts in concert with gas damping. The statistics of the analytic solution agree with the results of laborious numerical calculations which do not exploit the adiabatic approximation.

  6. Non-equilibrium scale invariance and shortcuts to adiabaticity in a one-dimensional Bose gas

    PubMed Central

    Rohringer, W.; Fischer, D.; Steiner, F.; Mazets, I. E.; Schmiedmayer, J.; Trupke, M.

    2015-01-01

    We present experimental evidence for scale invariant behaviour of the excitation spectrum in phase-fluctuating quasi-1d Bose gases after a rapid change of the external trapping potential. Probing density correlations in free expansion, we find that the temperature of an initial thermal state scales with the spatial extension of the cloud as predicted by a model based on adiabatic rescaling of initial eigenmodes with conserved quasiparticle occupation numbers. Based on this result, we demonstrate that shortcuts to adiabaticity for the rapid expansion or compression of the gas do not induce additional heating. PMID:25867640

  7. Protecting and accelerating adiabatic passage with time-delayed pulse sequences.

    PubMed

    Sampedro, Pablo; Chang, Bo Y; Sola, Ignacio R

    2016-05-21

    Using numerical simulations of two-photon electronic absorption with femtosecond pulses in Na2 we show that: (i) it is possible to avoid the characteristic saturation or dumped Rabi oscillations in the yield of absorption by time-delaying the laser pulses; (ii) it is possible to accelerate the onset of adiabatic passage by using the vibrational coherence starting in a wave packet; and (iii) it is possible to prepare the initial wave packet in order to achieve full state-selective transitions with broadband pulses. The findings can be used, for instance, to achieve ultrafast adiabatic passage by light-induced potentials and understand its intrinsic robustness. PMID:27125342

  8. Creation and Transfer of Coherence via Technique of Stimulated Raman Adiabatic Passage in Triple Quantum Dots

    NASA Astrophysics Data System (ADS)

    Tian, Si-Cong; Wan, Ren-Gang; Wang, Chun-Liang; Shu, Shi-Li; Wang, Li-Jie; Tong, Chun-Zhu

    2016-04-01

    We propose a scheme for creation and transfer of coherence among ground state and indirect exciton states of triple quantum dots via the technique of stimulated Raman adiabatic passage. Compared with the traditional stimulated Raman adiabatic passage, the Stokes laser pulse is replaced by the tunneling pulse, which can be controlled by the externally applied voltages. By varying the amplitudes and sequences of the pump and tunneling pulses, a complete coherence transfer or an equal coherence distribution among multiple states can be obtained. The investigations can provide further insight for the experimental development of controllable coherence transfer in semiconductor structure and may have potential applications in quantum information processing.

  9. Adiabatic response and quantum thermoelectrics for ac-driven quantum systems

    NASA Astrophysics Data System (ADS)

    Ludovico, María Florencia; Battista, Francesca; von Oppen, Felix; Arrachea, Liliana

    2016-02-01

    We generalize the theory of thermoelectrics to include coherent electron systems under adiabatic ac driving, accounting for quantum pumping of charge and heat, as well as for the work exchanged between the electron system and driving potentials. We derive the relevant response coefficients in the adiabatic regime and show that they obey generalized Onsager reciprocity relations. We analyze the consequences of our generalized thermoelectric framework for quantum motors, generators, heat engines, and heat pumps, characterizing them in terms of efficiencies and figures of merit. We illustrate these concepts in a model for a quantum pump.

  10. Non-equilibrium scale invariance and shortcuts to adiabaticity in a one-dimensional Bose gas.

    PubMed

    Rohringer, W; Fischer, D; Steiner, F; Mazets, I E; Schmiedmayer, J; Trupke, M

    2015-01-01

    We present experimental evidence for scale invariant behaviour of the excitation spectrum in phase-fluctuating quasi-1d Bose gases after a rapid change of the external trapping potential. Probing density correlations in free expansion, we find that the temperature of an initial thermal state scales with the spatial extension of the cloud as predicted by a model based on adiabatic rescaling of initial eigenmodes with conserved quasiparticle occupation numbers. Based on this result, we demonstrate that shortcuts to adiabaticity for the rapid expansion or compression of the gas do not induce additional heating. PMID:25867640

  11. Creation and Transfer of Coherence via Technique of Stimulated Raman Adiabatic Passage in Triple Quantum Dots.

    PubMed

    Tian, Si-Cong; Wan, Ren-Gang; Wang, Chun-Liang; Shu, Shi-Li; Wang, Li-Jie; Tong, Chun-Zhu

    2016-12-01

    We propose a scheme for creation and transfer of coherence among ground state and indirect exciton states of triple quantum dots via the technique of stimulated Raman adiabatic passage. Compared with the traditional stimulated Raman adiabatic passage, the Stokes laser pulse is replaced by the tunneling pulse, which can be controlled by the externally applied voltages. By varying the amplitudes and sequences of the pump and tunneling pulses, a complete coherence transfer or an equal coherence distribution among multiple states can be obtained. The investigations can provide further insight for the experimental development of controllable coherence transfer in semiconductor structure and may have potential applications in quantum information processing. PMID:27107772

  12. Shortcut to adiabaticity in full-wave optics for ultra-compact waveguide junctions

    NASA Astrophysics Data System (ADS)

    Della Valle, Giuseppe; Perozziello, Gerardo; Longhi, Stefano

    2016-09-01

    We extend the concept of shortcuts to adiabaticity to full-wave optics and provide an application to the design of an ultra-compact waveguide junction. In particular, we introduce a procedure allowing one to synthesize a purely dielectric optical potential that precisely compensates for non-adiabatic losses of the transverse electric fundamental mode in any (sufficiently regular) two-dimensional waveguide junction. Our results are corroborated by finite-element method numerical simulations in a Pöschl–Teller waveguide mode expander.

  13. Alkali metal ionization detector

    DOEpatents

    Bauerle, James E.; Reed, William H.; Berkey, Edgar

    1978-01-01

    Variations in the conventional filament and collector electrodes of an alkali metal ionization detector, including the substitution of helical electrode configurations for either the conventional wire filament or flat plate collector; or, the substitution of a plurality of discrete filament electrodes providing an in situ capability for transferring from an operationally defective filament electrode to a previously unused filament electrode without removing the alkali metal ionization detector from the monitored environment. In particular, the helical collector arrangement which is coaxially disposed about the filament electrode, i.e. the thermal ionizer, provides an improved collection of positive ions developed by the filament electrode. The helical filament design, on the other hand, provides the advantage of an increased surface area for ionization of alkali metal-bearing species in a monitored gas environment as well as providing a relatively strong electric field for collecting the ions at the collector electrode about which the helical filament electrode is coaxially positioned. Alternatively, both the filament and collector electrodes can be helical. Furthermore, the operation of the conventional alkali metal ionization detector as a leak detector can be simplified as to cost and complexity, by operating the detector at a reduced collector potential while maintaining the sensitivity of the alkali metal ionization detector adequate for the relatively low concentration of alkali vapor and aerosol typically encountered in leak detection applications.

  14. Collisional and Radiative Processes in Adiabatic Deceleration, Deflection, and Off-Axis Trapping of a Rydberg Atom Beam

    SciTech Connect

    Seiler, Ch.; Hogan, S. D.; Schmutz, H.; Agner, J. A.; Merkt, F.

    2011-02-18

    A supersonic beam of Rydberg hydrogen atoms has been adiabatically deflected by 90 deg., decelerated to zero velocity in less than 25 {mu}s, and loaded into an electric trap. The deflection has allowed the suppression of collisions with atoms in the trailing part of the gas pulse. The processes leading to trap losses, i.e., fluorescence to the ground state, and transitions and ionization induced by blackbody radiation have been monitored over several milliseconds and quantitatively analyzed.

  15. Electronic non-adiabatic states: towards a density functional theory beyond the Born–Oppenheimer approximation

    PubMed Central

    Gidopoulos, Nikitas I.; Gross, E. K. U.

    2014-01-01

    A novel treatment of non-adiabatic couplings is proposed. The derivation is based on a theorem by Hunter stating that the wave function of the complete system of electrons and nuclei can be written, without approximation, as a Born–Oppenheimer (BO)-type product of a nuclear wave function, X(R), and an electronic one, ΦR(r), which depends parametrically on the nuclear configuration R. From the variational principle, we deduce formally exact equations for ΦR(r) and X(R). The algebraic structure of the exact nuclear equation coincides with the corresponding one in the adiabatic approximation. The electronic equation, however, contains terms not appearing in the adiabatic case, which couple the electronic and the nuclear wave functions and account for the electron–nuclear correlation beyond the BO level. It is proposed that these terms can be incorporated using an optimized local effective potential. PMID:24516183

  16. Determination of caloric values of agricultural crops and crop waste by Adiabatic Bomb Calorimetry

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Calorific values of agricultural crops and their waste were measured by adiabatic bomb calorimetry. Sustainable farming techniques require that all potential sources of revenue be utilized. A wide variety of biomass is beginning to be used as alternative fuels all over the world. The energy potentia...

  17. Precision measurements of ionization and dissociation energies by extrapolation of Rydberg series: from H2 to larger molecules.

    PubMed

    Sprecher, D; Beyer, M; Merkt, F

    2013-01-01

    Recent experiments are reviewed which have led to the determination of the ionization and dissociation energies of molecular hydrogen with a precision of 0.0007 cm(-)1 (8 mJ/mol or 20 MHz) using a procedure based on high-resolution spectroscopic measurements of high Rydberg states and the extrapolation of the Rydberg series to the ionization thresholds. Molecular hydrogen, with only two protons and two electrons, is the simplest molecule with which all aspects of a chemical bond, including electron correlation effects, can be studied. Highly precise values of its ionization and dissociation energies provide stringent tests of the precision of molecular quantum mechanics and of quantum-electrodynamics calculations in molecules. The comparison of experimental and theoretical values for these quantities enable one to quantify the contributions to a chemical bond that are neglected when making the Born-Oppenheimer approximation, i.e. adiabatic, nonadiabatic, relativistic, and radiative corrections. Ionization energies of a broad range of molecules can now be determined experimentally with high accuracy (i.e. about 0.01 cm(-1)). Calculations at similar accuracies are extremely challenging for systems containing more than two electrons. The combination of precision measurements of molecular ionization energies with highly accurateab initio calculations has the potential to provide, in future, fully reliable sets of thermochemical quantities for gas-phase reactions. PMID:23967701

  18. Accurate ab initio-based adiabatic global potential energy surface for the 2{sup 2}A″ state of NH{sub 2} by extrapolation to the complete basis set limit

    SciTech Connect

    Li, Y. Q.; Ma, F. C.; Sun, M. T.

    2013-10-21

    A full three-dimensional global potential energy surface is reported first time for the title system, which is important for the photodissociation processes. It is obtained using double many-body expansion theory and an extensive set of accurate ab initio energies extrapolated to the complete basis set limit. Such a work can be recommended for dynamics studies of the N({sup 2}D) + H{sub 2} reaction, a reliable theoretical treatment of the photodissociation dynamics and as building blocks for constructing the double many-body expansion potential energy surface of larger nitrogen/hydrogen containing systems. In turn, a preliminary theoretical study of the reaction N({sup 2}D)+H{sub 2}(X{sup 1}Σ{sub g}{sup +})(ν=0,j=0)→NH(a{sup 1}Δ)+H({sup 2}S) has been carried out with the method of quasi-classical trajectory on the new potential energy surface. Integral cross sections and thermal rate constants have been calculated, providing perhaps the most reliable estimate of the integral cross sections and the rate constants known thus far for such a reaction.

  19. Adiabatic passage in photon-echo quantum memories

    NASA Astrophysics Data System (ADS)

    Demeter, Gabor

    2013-11-01

    Photon-echo-based quantum memories use inhomogeneously broadened, optically thick ensembles of absorbers to store a weak optical signal and employ various protocols to rephase the atomic coherences for information retrieval. We study the application of two consecutive, frequency-chirped control pulses for coherence rephasing in an ensemble with a “natural” inhomogeneous broadening. Although propagation effects distort the two control pulses differently, chirped pulses that drive adiabatic passage can rephase atomic coherences in an optically thick storage medium. Combined with spatial phase-mismatching techniques to prevent primary echo emission, coherences can be rephased around the ground state to achieve secondary echo emission with close to unit efficiency. Potential advantages over similar schemes working with π pulses include greater potential signal fidelity, reduced noise due to spontaneous emission, and better capability for the storage of multiple memory channels.

  20. Non-Gaussianities in multifield inflation: Superhorizon evolution, adiabaticity, and the fate of f{sub NL}

    SciTech Connect

    Meyers, Joel; Sivanandam, Navin

    2011-05-15

    We explore the superhorizon generation of large f{sub NL} of the local form in two-field inflation. We calculate the two- and three-point observables in a general class of potentials which allow for an analytic treatment using the {delta}N formalism. Motivated by the conservation of the curvature perturbation outside the horizon in the adiabatic mode and also by the observed adiabaticity of the power spectrum, we follow the evolution of f{sub NL}{sup local} until it is driven into the adiabatic solution by passing through a phase of effectively single-field inflation. We find that, although large f{sub NL}{sup local} may be generated during inflation, such nongaussianities are transitory and will be exponentially damped as the cosmological fluctuations approach adiabaticity.

  1. Ionization chamber

    DOEpatents

    Walenta, Albert H.

    1981-01-01

    An ionization chamber has separate drift and detection regions electrically isolated from each other by a fine wire grid. A relatively weak electric field can be maintained in the drift region when the grid and another electrode in the chamber are connected to a high voltage source. A much stronger electric field can be provided in the detection region by connecting wire electrodes therein to another high voltage source. The detection region can thus be operated in a proportional mode when a suitable gas is contained in the chamber. High resolution output pulse waveforms are provided across a resistor connected to the detection region anode, after ionizing radiation enters the drift region and ionize the gas.

  2. Ionization chamber

    DOEpatents

    Walenta, A.H.

    An ionization chamber is described which has separate drift and detection regions electrically isolated from each other by a fine wire grid. A relatively weak electric field can be maintained in the drift region when the grid and another electrode in the chamber are connected to a high voltage source. A much stronger electric field can be provided in the detection region by connecting wire electrodes therein to another high voltage source. The detection region can thus be operated in a proportional mode when a suitable gas is contained in the chamber. High resolution output pulse waveforms are provided across a resistor connected to the detection region anode, after ionizing radiation enters the drift region and ionizes the gas.

  3. IONIZATION CHAMBER

    DOEpatents

    Redman, W.C.; Shonka, F.R.

    1958-02-18

    This patent describes a novel ionization chamber which is well suited to measuring the radioactivity of the various portions of a wire as the wire is moved at a uniform speed, in order to produce the neutron flux traverse pattern of a reactor in which the wire was previously exposed to neutron radiation. The ionization chamber of the present invention is characterized by the construction wherein the wire is passed through a tubular, straight electrode and radiation shielding material is disposed along the wire except at an intermediate, narrow area where the second electrode of the chamber is located.

  4. Phase avalanches in near-adiabatic evolutions

    SciTech Connect

    Vertesi, T.; Englman, R.

    2006-02-15

    In the course of slow, nearly adiabatic motion of a system, relative changes in the slowness can cause abrupt and high magnitude phase changes, ''phase avalanches,'' superimposed on the ordinary geometric phases. The generality of this effect is examined for arbitrary Hamiltonians and multicomponent (>2) wave packets and is found to be connected (through the Blaschke term in the theory of analytic signals) to amplitude zeros in the lower half of the complex time plane. Motion on a nonmaximal circle on the Poincare-sphere suppresses the effect. A spectroscopic transition experiment can independently verify the phase-avalanche magnitudes.

  5. Adiabatic chaos in the spin orbit problem

    NASA Astrophysics Data System (ADS)

    Benettin, Giancarlo; Guzzo, Massimiliano; Marini, Valerio

    2008-05-01

    We provide evidences that the angular momentum of a symmetric rigid body in a spin orbit resonance can perform large scale chaotic motions on time scales which increase polynomially with the inverse of the oblateness of the body. This kind of irregular precession appears as soon as the orbit of the center of mass is non-circular and the angular momentum of the body is far from the principal directions with minimum (maximum) moment of inertia. We also provide a quantitative explanation of these facts by using the theory of adiabatic invariants, and we provide numerical applications to the cases of the 1:1 and 1:2 spin orbit resonances.

  6. Adiabatic passage in the presence of noise

    NASA Astrophysics Data System (ADS)

    Noel, T.; Dietrich, M. R.; Kurz, N.; Shu, G.; Wright, J.; Blinov, B. B.

    2012-02-01

    We report on an experimental investigation of rapid adiabatic passage (RAP) in a trapped barium ion system. RAP is implemented on the transition from the 6S1/2 ground state to the metastable 5D5/2 level by applying a laser at 1.76 μm. We focus on the interplay of laser frequency noise and laser power in shaping the effectiveness of RAP, which is commonly assumed to be a robust tool for high-efficiency population transfer. However, we note that reaching high state transfer fidelity requires a combination of small laser linewidth and large Rabi frequency.

  7. Adiabatic demagnetization refrigerator for space use

    NASA Technical Reports Server (NTRS)

    Serlemitsos, A. T.; Warner, B. A.; Castles, S.; Breon, S. R.; San Sebastian, M.; Hait, T.

    1990-01-01

    An Adiabatic Demagnetization Refrigerator (ADR) for space use is under development at NASA's Goddard Space Flight Center (GSFC). The breadboard ADR operated at 100 mK for 400 minutes. Some significant changes to that ADR, designed to eliminate shortcomings revealed during tests, are reported. To increase thermal contact, the ferric ammonium sulfate crystals were grown directly on gold-plated copper wires which serve as the thermal bus. The thermal link to the X-ray sensors was also markedly improved. To speed up the testing required to determine the best design parameters for the gas gap heat switch, the new heat switch has a modular design and is easy to disassemble.

  8. An adiabatic demagnetization refrigerator for infrared bolometers

    NASA Technical Reports Server (NTRS)

    Britt, R. D.; Richards, P. L.

    1981-01-01

    Adiabatic demagnetization refrigerators have been built and installed in small portable liquid helium cryostats to test the feasibility of this method of cooling infrared bolometric detectors to temperatures below 0.3 K. Performance has been achieved which suggests that bolometer temperatures of 0.2 K can be maintained for periods of approximately 60 hours. Applications to sensitive infrared detection from ground-based telescopes and space satellites are discussed. Design data are given which permit the evaluation of refrigerator performance for a variety of design parameters.

  9. Generalized Ramsey numbers through adiabatic quantum optimization

    NASA Astrophysics Data System (ADS)

    Ranjbar, Mani; Macready, William G.; Clark, Lane; Gaitan, Frank

    2016-06-01

    Ramsey theory is an active research area in combinatorics whose central theme is the emergence of order in large disordered structures, with Ramsey numbers marking the threshold at which this order first appears. For generalized Ramsey numbers r(G, H), the emergent order is characterized by graphs G and H. In this paper we: (i) present a quantum algorithm for computing generalized Ramsey numbers by reformulating the computation as a combinatorial optimization problem which is solved using adiabatic quantum optimization; and (ii) determine the Ramsey numbers r({{T}}m,{{T}}n) for trees of order m,n = 6,7,8 , most of which were previously unknown.

  10. Decoherence in a scalable adiabatic quantum computer

    SciTech Connect

    Ashhab, S.; Johansson, J. R.; Nori, Franco

    2006-11-15

    We consider the effects of decoherence on Landau-Zener crossings encountered in a large-scale adiabatic-quantum-computing setup. We analyze the dependence of the success probability--i.e., the probability for the system to end up in its new ground state--on the noise amplitude and correlation time. We determine the optimal sweep rate that is required to maximize the success probability. We then discuss the scaling of decoherence effects with increasing system size. We find that those effects can be important for large systems, even if they are small for each of the small building blocks.

  11. Transition energy and potential energy curves for ionized inner-shell states of CO, O2 and N 2 calculated by several inner-shell multiconfigurational approaches.

    PubMed

    Moura, Carlos E V de; Oliveira, Ricardo R; Rocha, Alexandre B

    2013-05-01

    Potential energy curves and inner-shell ionization energies of carbon monoxide, oxygen and nitrogen molecules were calculated using several forms of the inner-shell multiconfigurational self-consistent field (IS-MCSCF) method-a recently proposed protocol to obtain specifically converged inner-shell states at this level. The particular forms of the IS-MCSCF method designated IS-GVB-PP, IS-FVBL and IS-CASSCF stand for perfect pairing generalized valence bond, full valence bond-like MCSCF and complete active space self consistent field, respectively. A comparison of these different versions of the IS-MCSCF method was carried out for the first time. The results indicate that inner-shell states are described accurately even for the simplest version of the method (IS-GVB-PP). Dynamic correlation was recovered by multireference configuration interaction or multireference perturbation theory. For molecules not having equivalent atoms, all methods led to comparable and accurate transition energies. For molecules with equivalent atoms, the most accurate results were obtained by multireference perturbation theory. Scalar relativistic effects were accounted for using the Douglas-Kroll-Hess Hamiltonian. PMID:23070335

  12. Is near-``spectroscopic accuracy'' possible for heavy atoms and coupled cluster theory? An investigation of the first ionization potentials of the atoms Ga-Kr

    NASA Astrophysics Data System (ADS)

    DeYonker, Nathan J.; Peterson, Kirk A.

    2013-04-01

    Recent developments in ab initio coupled cluster (CC) theory and correlation consistent basis sets have ushered in an era of unprecedented accuracy when studying the spectroscopy and thermodynamics of molecules containing main group elements. These same developments have recently seen application to heavier inorganic or transition metal-containing species. The present work benchmarks conventional single reference coupled cluster theory (up to full configuration interaction for valence electron correlation and coupled cluster with up to full pentuple excitations (CCSDTQP) for core-valence correlation) and explicitly correlated coupled cluster methods [CC with single, double, and perturbative triple substitutions (CCSD(T)-F12)] for the atomic ionization potentials of the six 4p elements (Ga-Kr), a property with experimental error bars no greater than a few cm-1. When second-order spin orbit coupling effects are included, a composite methodology based on CCSD(T) calculations yielded a mean signed error of just -0.039 kcal mol-1 and a mean unsigned error of 0.043 kcal mol-1. Inclusion of post-CCSD(T) correlation corrections reduced both of these values to -0.008 kcal mol-1 and 0.025 kcal mol-1, respectively, with the latter corresponding to an average error of just 9 cm-1. The maximum signed error in the latter scheme was just -0.043 kcal mol-1 (15 cm-1).

  13. Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules I. Reference Data at the CCSD(T) Complete Basis Set Limit.

    PubMed

    Richard, Ryan M; Marshall, Michael S; Dolgounitcheva, O; Ortiz, J V; Brédas, Jean-Luc; Marom, Noa; Sherrill, C David

    2016-02-01

    In designing organic materials for electronics applications, particularly for organic photovoltaics (OPV), the ionization potential (IP) of the donor and the electron affinity (EA) of the acceptor play key roles. This makes OPV design an appealing application for computational chemistry since IPs and EAs are readily calculable from most electronic structure methods. Unfortunately reliable, high-accuracy wave function methods, such as coupled cluster theory with single, double, and perturbative triples [CCSD(T)] in the complete basis set (CBS) limit are too expensive for routine applications to this problem for any but the smallest of systems. One solution is to calibrate approximate, less computationally expensive methods against a database of high-accuracy IP/EA values; however, to our knowledge, no such database exists for systems related to OPV design. The present work is the first of a multipart study whose overarching goal is to determine which computational methods can be used to reliably compute IPs and EAs of electron acceptors. This part introduces a database of 24 known organic electron acceptors and provides high-accuracy vertical IP and EA values expected to be within ±0.03 eV of the true non-relativistic, vertical CCSD(T)/CBS limit. Convergence of IP and EA values toward the CBS limit is studied systematically for the Hartree-Fock, MP2 correlation, and beyond-MP2 coupled cluster contributions to the focal point estimates. PMID:26731487

  14. Study of gas-phase O-H bond dissociation enthalpies and ionization potentials of substituted phenols - Applicability of ab initio and DFT/B3LYP methods

    NASA Astrophysics Data System (ADS)

    Klein, Erik; Lukeš, Vladimír

    2006-11-01

    In this paper, the study of phenol and 37 compounds representing various ortho-, para-, and meta-substituted phenols is presented. Molecules and their radical structures were studied using ab initio methods with inclusion of correlation energy and DFT in order to calculate the O-H bond dissociation enthalpies (BDEs) and vertical ionization potentials (IPs). Calculated BDEs and IPs were compared with available experimental values to ascertain the suitability of used methods, especially for the description of the substituent induced changes in BDE and IP. MP2, MP3, and MP4 methods do not give reliable results, since they significantly underestimate substituent induced changes in BDE and do not reflect distinct effect of substituents related to para and meta position correctly. DFT/B3LYP method reflects the effect of substituents on BDE satisfactorily, though ΔBDEs are in narrower range than experimental values. BDE of phenol was calculated also using CCSD(T) method in various basis sets. Both, DFT and HF methods describe the effect of substituents on IP identically. However, DFT considerably underestimates individual values. HF method gives IPs in very good agreement with experimental data. Obtained results show that dependences of BDEs and IPs on Hammett constants of the substituents are linear. Linearity of DFT BDE vs. IP dependence is even better than the dependences on Hammett constants and obtained equations allow estimating of O-H BDEs of meta- and para-substituted phenols from calculated IPs.

  15. Photoreduction of benzophenone by acetonitrile: correlation of rates of hydrogen abstraction from RH with the ionization potentials of the radicals R

    SciTech Connect

    Naguib, Y.M.A.; Steel, C.; Cohen, S.G.; Young, M.A.

    1987-05-21

    Triplet benzophenone (/sup 4/K) abstracts a hydrogen from acetonitrile with a rate constant of 130 +/- 30 M/sup -1/ s/sup -1/. Despite this low rate constant acetonitrile is not really an inert solvent and at low light fluxes, where T-T annihilation is not a major fate of the triplet, a major decay path for /sup 4/K is hydrogen abstraction with resulting pinacol (K/sub 2/H/sub 2/) formation (phi/sub K/sub 2/H/sub 2/ approx. = 0.1 at t = 0). Both K/sub 2/H/sub 2/ formation and /sup 3/K lifetime rapidly decrease with irradiation due to the light absorbing transients (LAT's) which are formed along with K/sub 7/H/sub 2/ from ketyl radicals (KH). The rate constants per hydrogen (k/sub H/) for abstraction from R-H by the electrophilic /sup 3/K correlate well with the ionization potentials (IP) of the corresponding radicals (R).

  16. Basis set limit electronic excitation energies, ionization potentials, and electron affinities for the 3d transition metal atoms: Coupled cluster and multireference methods

    NASA Astrophysics Data System (ADS)

    Balabanov, Nikolai B.; Peterson, Kirk A.

    2006-08-01

    Recently developed correlation consistent basis sets for the first row transition metal elements Sc-Zn have been utilized to determine complete basis set (CBS) scalar relativistic electron affinities, ionization potentials, and 4s23dn -2-4s1dn -1 electronic excitation energies with single reference coupled cluster methods [CCSD(T), CCSDT, and CCSDTQ] and multireference configuration interaction with three reference spaces: 3d4s, 3d4s4p, and 3d4s4p3d'. The theoretical values calculated with the highest order coupled cluster techniques at the CBS limit, including extrapolations to full configuration interaction, are well within 1kcal/mol of the corresponding experimental data. For the early transition metal elements (Sc-Mn) the internally contracted multireference averaged coupled pair functional method yielded excellent agreement with experiment; however, the atomic properties for the late transition metals (Mn-Zn) proved to be much more difficult to describe with this level of theory, even with the largest reference function of the present work.

  17. Atmospheric Ionization Measurements

    NASA Astrophysics Data System (ADS)

    Slack, Thomas; Mayes, Riley

    2015-04-01

    The measurement of atmospheric ionization is a largely unexplored science that potentially holds the key to better understanding many different geophysical phenomena through this new and valuable source of data. Through the LaACES program, which is funded by NASA through the Louisiana Space Consortium, students at Loyola University New Orleans have pursued the goal of measuring high altitude ionization for nearly three years, and were the first to successfully collect ionization data at altitudes over 30,000 feet using a scientific weather balloon flown from the NASA Columbia Scientific Ballooning Facility in Palestine, TX. In order to measure atmospheric ionization, the science team uses a lightweight and highly customized sensor known as a Gerdien condenser. Among other branches of science the data is already being used for, such as the study of aerosol pollution levels in the atmosphere, the data may also be useful in meteorology and seismology. Ionization data might provide another variable with which to predict weather or seismic activity more accurately and further in advance. Thomas Slack and Riley Mayes have served as project managers for the experiment, and have extensive knowledge of the experiment from the ground up. LaSPACE Louisiana Space Consortium.

  18. Nucleon-deuteron scattering using the adiabatic projection method

    NASA Astrophysics Data System (ADS)

    Elhatisari, Serdar; Lee, Dean; Meißner, Ulf-G.; Rupak, Gautam

    2016-06-01

    In this paper we discuss the adiabatic projection method, a general framework for scattering and reaction calculations on the lattice. We also introduce several new techniques developed to study nucleus-nucleus scattering and reactions on the lattice. We present technical details of the method for large-scale problems. To estimate the systematic errors of the calculations we consider simple two-particle scattering on the lattice. Then we benchmark the accuracy and efficiency of the numerical methods by applying these to calculate fermion-dimer scattering in lattice effective field theory with and without a long-range Coulomb potential. The fermion-dimer calculations correspond to neutron-deuteron and proton-deuteron scattering in the spin-quartet channel at leading order in the pionless effective field theory.

  19. Do biomolecular ion-motive ATPase work as adiabatic pumps

    NASA Astrophysics Data System (ADS)

    Astumian, Raymond Dean

    2001-03-01

    Biomolecular ion pumps use chemical energy to pump ions from low to high chemical potential across a biological membrane. Experiments show that the chemical energy can be substituted by an external oscillating or stochastically fluctuating electric field. This result can be interpreted analogously to a mechanism for an adiabatic electron pump originally suggested by Thouless (PRB 27: 6083 (1983)) in which two system parameters are modulated out of phase with one another. In our model, internal relaxations of the protein (at least two with different time scales) provide a mechanism for transforming a single ac or stochastically fluctuating external signal into a two phase shifted outputs. For a sinusoidally oscillating electric field, the frequency response for the Sodium-Potassium ATPase for both sodium and rubidium (an analog of potassium) can be fit using a very simple expression with only one fit parameter. These results show how biomolecular pumps can be modelled at the mesoscopic level of detail.

  20. Geometry of an adiabatic passage at a level crossing

    SciTech Connect

    Cholascinski, Mateusz

    2005-06-15

    We discuss adiabatic quantum phenomena at a level crossing. Given a path in the parameter space which passes through a degeneracy point, we find a criterion which determines whether the adiabaticity condition can be satisfied. For paths that can be traversed adiabatically we also derive a differential equation which specifies the time dependence of the system parameters, for which transitions between distinct energy levels can be neglected. We also generalize the well-known geometric connections to the case of adiabatic paths containing arbitrarily many level-crossing points and degenerate levels.

  1. Geometrical representation of sum frequency generation and adiabatic frequency conversion

    NASA Astrophysics Data System (ADS)

    Suchowski, Haim; Oron, Dan; Arie, Ady; Silberberg, Yaron

    2008-12-01

    We present a geometrical representation of the process of sum frequency generation in the undepleted pump approximation, in analogy with the known optical Bloch equations. We use this analogy to propose a technique for achieving both high efficiency and large bandwidth in sum frequency conversion using the adiabatic inversion scheme. The process is analogous with rapid adiabatic passage in NMR, and adiabatic constraints are derived in this context. This adiabatic frequency conversion scheme is realized experimentally using an aperiodically poled potassium titanyl phosphate (KTP) device, where we achieved high efficiency signal-to-idler conversion over a bandwidth of 140nm .

  2. On the Role of Prior Probability in Adiabatic Quantum Algorithms

    NASA Astrophysics Data System (ADS)

    Sun, Jie; Lu, Songfeng; Yang, Liping

    2016-03-01

    In this paper, we study the role of prior probability on the efficiency of quantum local adiabatic search algorithm. The following aspects for prior probability are found here: firstly, only the probabilities of marked states affect the running time of the adiabatic evolution; secondly, the prior probability can be used for improving the efficiency of the adiabatic algorithm; thirdly, like the usual quantum adiabatic evolution, the running time for the case of multiple solution states where the number of marked elements are smaller enough than the size of the set assigned that contains them can be significantly bigger than that of the case where the assigned set only contains all the marked states.

  3. Identification of phosphorylated peptides from complex mixtures using negative-ion orifice-potential stepping and capillary liquid chromatography/electrospray ionization mass spectrometry.

    PubMed

    Ding, J; Burkhart, W; Kassel, D B

    1994-01-01

    A rapid method for identifying and characterizing sites of phosphorylation of peptides and proteins is described. High-performance capillary liquid chromatography (HPLC) coupled with electrospray ionization mass spectrometry (ESI-MS) is used to distinguish non-phosphorylated and phosphorylated peptides originating from mixtures as complex as enzyme digests. The method relies on the ability to produce a fragment ion characteristic and unique to phosphopeptides (m/z 79, PO3) by stepping the orifice potential of the mass spectrometer as a function of mass. At low m/z values, a high orifice potential is applied to induce extensive fragmentation of the peptide, leading to the formation of the m/z 79 phosphate-derived ion. This method is analogous to that described by Carr et al. for the identification of glycopeptides from enzymatic digestion of glycoproteins (S.A. Carr, M.J. Huddleston, M.F. Bean, Protein Science 2, 183 (1993)). The method was first evaluated and validated for a mixture of non-, mono- and di-phosphorylated synthetic peptides. Both mono- and di-phosphorylated peptides were found to generate fragment ions characteristic of PO3 whereas the non-phosphorylated peptide did not. Application of the method was extended to identifying phosphopeptides generated from an endoprotease Lys-C digestion of beta-casein. Both the expected mono- and tetra-phosphorylated Lys-C peptides were observed and identified rapidly in the LC/SEI-MS analysis. The procedure was used additionally to identify the site(s) of phosphorylation of the cytosolic non-receptor tyrosine kinase, pp60(c-src). PMID:8118063

  4. Quantum Adiabatic Algorithms and Large Spin Tunnelling

    NASA Technical Reports Server (NTRS)

    Boulatov, A.; Smelyanskiy, V. N.

    2003-01-01

    We provide a theoretical study of the quantum adiabatic evolution algorithm with different evolution paths proposed in this paper. The algorithm is applied to a random binary optimization problem (a version of the 3-Satisfiability problem) where the n-bit cost function is symmetric with respect to the permutation of individual bits. The evolution paths are produced, using the generic control Hamiltonians H (r) that preserve the bit symmetry of the underlying optimization problem. In the case where the ground state of H(0) coincides with the totally-symmetric state of an n-qubit system the algorithm dynamics is completely described in terms of the motion of a spin-n/2. We show that different control Hamiltonians can be parameterized by a set of independent parameters that are expansion coefficients of H (r) in a certain universal set of operators. Only one of these operators can be responsible for avoiding the tunnelling in the spin-n/2 system during the quantum adiabatic algorithm. We show that it is possible to select a coefficient for this operator that guarantees a polynomial complexity of the algorithm for all problem instances. We show that a successful evolution path of the algorithm always corresponds to the trajectory of a classical spin-n/2 and provide a complete characterization of such paths.

  5. Nonadiabatic Transitions in Adiabatic Rapid Passage

    NASA Astrophysics Data System (ADS)

    Lu, T.; Miao, X.; Metcalf, H.

    2006-05-01

    Optical forces much larger than the ordinary radiative force can be achieved on a two-level atom by multiple repetitions of adiabatic rapid passage sweeps with counterpropagating light beams. Chirped light pulses drive the atom-laser system up a ladder of dressed state energy sheets on sequential trajectories, thereby decreasing the atomic kinetic energy. Nonadiabatic transitions between the energy sheets must be avoided for this process to be effective. We have calculated the nonadiabatic transition probability for various chirped light pulses numerically. These results were compared to the first Demkov-Kunike model and the well-known Landau-Zener model. In addition, an analytical form of the nonadiabatic transition probability has been found for linearly chirped pulses and an approximate form for generic symmetric finite-time pulses has been found for the entire parameter space using the technique of unitary integration. From this, the asymptotic transition probability in the adiabatic limit was derived. T. Lu, X. Miao, and H. Metcalf, Phys., Rev. A 71 061405(R) (2005). Yu. Demkov and M. Kunike, Vestn. Leningr. Univ. Fis. Khim., 16, 39 (1969); K.-A. Suominen and B. Garraway, Phys. Rev. A45, 374 (1992)

  6. Adiabatic cooling of solar wind electrons

    NASA Technical Reports Server (NTRS)

    Sandbaek, Ornulf; Leer, Egil

    1992-01-01

    In thermally driven winds emanating from regions in the solar corona with base electron densities of n0 not less than 10 exp 8/cu cm, a substantial fraction of the heat conductive flux from the base is transfered into flow energy by the pressure gradient force. The adiabatic cooling of the electrons causes the electron temperature profile to fall off more rapidly than in heat conduction dominated flows. Alfven waves of solar origin, accelerating the basically thermally driven solar wind, lead to an increased mass flux and enhanced adiabatic cooling. The reduction in electron temperature may be significant also in the subsonic region of the flow and lead to a moderate increase of solar wind mass flux with increasing Alfven wave amplitude. In the solar wind model presented here the Alfven wave energy flux per unit mass is larger than that in models where the temperature in the subsonic flow is not reduced by the wave, and consequently the asymptotic flow speed is higher.

  7. An empirical dependence of frequency in the oscillatory sorption of H2 and D2 in Pd on the first ionization potential of noble gases.

    PubMed

    Lalik, Erwin

    2011-08-14

    Oscillatory heat evolution in sorption of H(2) and D(2) in Pd can be induced by an admixture of ~10 vol.% of an inert gas (He, Ne, Ar, Kr, or N(2)) to either isotope prior to its contact with palladium powder. The oscillations are represented in the form of a calorimetric time series, recorded using a gas flow-through microcalorimeter at the temperatures of 75 °C for D(2) and 106 °C for H(2). For both D(2) and H(2), the oscillation parameters change as a function of the kind of inert gas used: the amplitude increases and the frequency decreases in passing from He to Kr. An empirical dependence of the oscillation frequencies observed for various admixtures and normalized with respect to Kr has been found. Accordingly, the frequency is a function of a product of the first ionization potential and the square root of atomic mass of the inert gas (He, Ne, Ar, Kr, or N(2)). On the other hand, invariance of the thermal effects of sorption is evident from the integrated areas under the calorimetric time series yielding the molar heats of sorption conserved, irrespective of the inert gas admixture. A novel calibration procedure has been devised in order to deal with an instability of calibration factor arising in desorption of H(2) and D(2) from Pd. A method of dynamic calibration factor made it possible to obtain a good agreement between the heats of sorption and desorption of both H(2) and D(2) within individual sorption-desorption cycles for all inert gas admixtures. PMID:21842944

  8. Ionizing Irradiation Not Only Inactivates Clonogenic Potential in Primary Normal Human Diploid Lens Epithelial Cells but Also Stimulates Cell Proliferation in a Subset of This Population

    PubMed Central

    Fujimichi, Yuki; Hamada, Nobuyuki

    2014-01-01

    Over the past century, ionizing radiation has been known to induce cataracts in the crystalline lens of the eye, but its mechanistic underpinnings remain incompletely understood. This study is the first to report the clonogenic survival of irradiated primary normal human lens epithelial cells and stimulation of its proliferation. Here we used two primary normal human cell strains: HLEC1 lens epithelial cells and WI-38 lung fibroblasts. Both strains were diploid, and a replicative lifespan was shorter in HLEC1 cells. The colony formation assay demonstrated that the clonogenic survival of both strains decreases similarly with increasing doses of X-rays. A difference in the survival between two strains was actually insignificant, although HLEC1 cells had the lower plating efficiency. This indicates that the same dose inactivates the same fraction of clonogenic cells in both strains. Intriguingly, irradiation enlarged the size of clonogenic colonies arising from HLEC1 cells in marked contrast to those from WI-38 cells. Such enhanced proliferation of clonogenic HLEC1 cells was significant at ≥2 Gy, and manifested as increments of ≤2.6 population doublings besides sham-irradiated controls. These results suggest that irradiation of HLEC1 cells not only inactivates clonogenic potential but also stimulates proliferation of surviving uniactivated clonogenic cells. Given that the lens is a closed system, the stimulated proliferation of lens epithelial cells may not be a homeostatic mechanism to compensate for their cell loss, but rather should be regarded as abnormal. This is because these findings are consistent with the early in vivo evidence documenting that irradiation induces excessive proliferation of rabbit lens epithelial cells and that suppression of lens epithelial cell divisions inhibits radiation cataractogenesis in frogs and rats. Thus, our in vitro model will be useful to evaluate the excessive proliferation of primary normal human lens epithelial cells that

  9. Immune potentiation after fractionated exposure to very low doses of ionizing radiation and/or caloric restriction in autoimmune-prone and normal C57Bl/6 mice

    SciTech Connect

    James, S.J.; Enger, S.M.; Peterson, W.J.; Makinodan, T. )

    1990-06-01

    Very low doses of ionizing radiation can enhance immune responsiveness and extend life span in normal mice. Total lymphoid irradiation at relatively high doses of radiation can retard autoimmune disease in genetically susceptible mice, but may impair immune function. In order to determine whether fractionated low dose exposure would enhance immune response and retard lymphadenopathy in autoimmune-prone mice, groups of C57B1/6 lpr/lpr mice were sham irradiated, exposed 5 days/week for 4 weeks to 0.04 Gy/day, or to 0.1 Gy/day. After the radiation protocol, the mice were evaluated for splenic T cell proliferative capacity, T cell subset distribution, and total spleen cell numbers. The independent and additive effect of caloric restriction was additionally assessed since this intervention has been shown to increase immune responsiveness and retard disease progression in autoimmune-prone mice. The congenic C57B1/6 +/+ immunologically normal strain was evaluated in parallel as congenic control. The results indicated that mitogen-stimulated proliferation was up-regulated in both strains of mice after exposure to 0.04 Gy/day. The proliferative capacity was additively enhanced when radiation at this dose level was combined with caloric restriction. Exposure to 0.1 Gy/day resulted in further augmentation of proliferative response in the lpr/lpr mice, but was depressive in the +/+ mice. Although the proportions of the various T cell subpopulations were altered in both strains after exposure to LDR, the specific subset alterations were different within each strain. Additional experiments were subsequently performed to assess whether the thymus is required for LDR-induced immune potentiation. Thymectomy completely abrogated the LDR effect in the +/+ mice, suggesting that thymic processing and/or trafficking is adaptively altered with LDR in this strain.

  10. Phospholipidomic identification of potential serum biomarkers in dengue fever, hepatitis B and hepatitis C using liquid chromatography-electrospray ionization-tandem mass spectrometry.

    PubMed

    Khedr, Alaa; Hegazy, Maha A; Kammoun, Ahmed K; Shehata, Mostafa A

    2016-01-15

    The serum phospholipid (PL) profiles of healthy volunteers (HE) and patients with recently diagnosed dengue fever (DF), hepatitis B (HBV), and hepatitis C (HCV) were investigated using liquid chromatography-ion trap-mass spectrometry (LC-IT-MS) and liquid chromatography-triple quad-mass spectrometry (LC-TQ-MS). Major PLs, including lyso-phosphatidylcholins (LPCs), phosphatidylcholins (PCs), phosphatidylinositols (PIs), phosphatidylethanolamines (PEs) and phosphatidylserines (PSs), were characterized in human serum using LC-IT-MS. Thirty-five PLs were quantified using seven non-endogenous odd-carbon PL standards. An MS search protocol for the identification of PLs is described. The analytical method was optimized to achieve maximum recovery and detection. PLs were detected with minimal ionization suppression. The PLs species were characterized on the basis of (i) MS(2) peaks due to polar head, (ii) precursor ion or neutral loss scans, (iii) identification of fatty acid, (iv) identification of sn-1 and sn-2 fatty acid. The quantitation data were subjected to principal component analysis (PCA), and a significant difference was observed between the PL profiles of the investigated diseases and those of HE subjects. The significance of the changes in each lipid among the four groups was statistically assessed using one-way analysis of variance (ANOVA) followed by Bonferroni post hoc multiple comparison. The serum profiles of 28 PLs were determined to be significantly different and enabled the discrimination between HE individuals and the studied patients. Potentially dysregulated PLs were considered as differentiating biomarkers to diagnose DF, HBV, and HCV. PMID:26708624

  11. Comparative anti-inflammatory activities of curcumin and tetrahydrocurcumin based on the phenolic O-H bond dissociation enthalpy, ionization potential and quantum chemical descriptor.

    PubMed

    Murakami, Yukio; Ishii, Hiroaki; Takada, Naoki; Tanaka, Shoji; Machino, Mamoru; Ito, Shigeru; Fujisawa, Seiichiro

    2008-01-01

    Curcumin and its reduced derivative tetrahydrocurcumin have been shown to exhibit chemopreventive activity. Cyclooxygenase-2 (COX-2) inhibition in lipopolysaccharide (LPS)- or Porphyromonas gingivalis fimbria-stimulated RAW 264.7 cells was investigated using Northern blot analysis. The fimbria-stimulated expression of the COX-2 gene was inhibited by curcumin but not by tetrahydrocurcumin. LPS-stimulated COX-2 gene expression was completely inhibited by curcumin, but an increase in the concentration of tetrahydrocurcumin did not cause complete inhibition of COX-2 expression. The inhibitory effect of curcumin on nuclear factor kappa B (NF-kappaB) activation in the cells was clearly observed, but that of tetrahydrocurcumin was incomplete even at a concentration of 20 microM. To explain the difference in effect between the two compounds, analysis of the frontier orbital was performed using ab initio 6-31G* wave function. The calculated chemical hardness (eta) for curcumin was clearly smaller, whereas its electronegativity (chi) and electrophilicity (omega) were clearly greater than the corresponding values for the curcumin-related compounds tetrahydrocurcumin, isoeugenol and eugenol. This suggested that the anti-inflammatory activities of curcumin may be related to eta-, chi- and/or omega-controlled enzymes. In addition, the bond dissociation enthalpy (BDE) of the phenolic OH was calculated using the density function theory (DFT)/B3LY. The total BDE values of curcumin and tetrahydrocurcumin were almost identical, but the BDE of one-electron oxidation and ionization potential (IP) for curcumin were lower than those for tetrahydrocurcumin, suggesting the highly pro-oxidative activity of curcumin. Curcumin has both oxidant and antioxidant properties. A causal link between the anti-inflammatory activities and molecular properties of phenolic antioxidants is suggested. PMID:18507010

  12. O(6) algebraic approach to three bound identical particles in the hyperspherical adiabatic representation

    NASA Astrophysics Data System (ADS)

    Salom, Igor; Dmitrašinović, V.

    2016-05-01

    We construct the three-body permutation symmetric O (6) hyperspherical harmonics and use them to solve the non-relativistic three-body Schrödinger equation in three spatial dimensions. We label the states with eigenvalues of the U (1) ⊗ SO(3)rot ⊂ U (3) ⊂ O (6) chain of algebras, and we present the K ≤ 4 harmonics and tables of their matrix elements. That leads to closed algebraic form of low-K energy spectra in the adiabatic approximation for factorizable potentials with square-integrable hyper-angular parts. This includes homogeneous pairwise potentials of degree α ≥ - 1. More generally, a simplification is achieved in numerical calculations of non-adiabatic approximations to non-factorizable potentials by using our harmonics.

  13. Adiabatic quantum optimization in the presence of discrete noise: Reducing the problem dimensionality

    NASA Astrophysics Data System (ADS)

    Mandrà, Salvatore; Guerreschi, Gian Giacomo; Aspuru-Guzik, Alán

    2015-12-01

    Adiabatic quantum optimization is a procedure to solve a vast class of optimization problems by slowly changing the Hamiltonian of a quantum system. The evolution time necessary for the algorithm to be successful scales inversely with the minimum energy gap encountered during the dynamics. Unfortunately, the direct calculation of the gap is strongly limited by the exponential growth in the dimensionality of the Hilbert space associated to the quantum system. Although many special-purpose methods have been devised to reduce the effective dimensionality, they are strongly limited to particular classes of problems with evident symmetries. Moreover, little is known about the computational power of adiabatic quantum optimizers in real-world conditions. Here we propose and implement a general purposes reduction method that does not rely on any explicit symmetry and which requires, under certain general conditions, only a polynomial amount of classical resources. Thanks to this method, we are able to analyze the performance of "nonideal" quantum adiabatic optimizers to solve the well-known Grover problem, namely the search of target entries in an unsorted database, in the presence of discrete local defects. In this case, we show that adiabatic quantum optimization, even if affected by random noise, is still potentially faster than any classical algorithm.

  14. Rotation-vibrational states of H3+ and the adiabatic approximation.

    PubMed

    Alijah, Alexander; Hinze, Juergen

    2006-11-15

    We discuss recent progress in the calculation and identification of rotation-vibrational states of H3+ at intermediate energies up to 13,000 cm(-1). Our calculations are based on the potential energy surface of Cencek et al. which is of sub-microhartree accuracy. As this surface includes diagonal adiabatic and relativistic corrections to the fixed nuclei electronic energies, the remaining discrepancies between our calculated and experimental data should be due to the neglect of non-adiabatic coupling to excited electronic states in the calculations. To account for this, our calculated energy values were adjusted empirically by a simple correction formula. Based on our understanding of the adiabatic approximation, we suggest two new approaches to account for the off-diagonal adiabatic correction, which should work; however, they have not been tested yet for H3+. Theoretical predictions made for the above-barrier energy region of recent experimental interest are accurate to 0.35 cm(-1) or better. PMID:17015396

  15. Adiabat-shaping in indirect drive inertial confinement fusion

    NASA Astrophysics Data System (ADS)

    Baker, K. L.; Robey, H. F.; Milovich, J. L.; Jones, O. S.; Smalyuk, V. A.; Casey, D. T.; MacPhee, A. G.; Pak, A.; Celliers, P. M.; Clark, D. S.; Landen, O. L.; Peterson, J. L.; Berzak-Hopkins, L. F.; Weber, C. R.; Haan, S. W.; Döppner, T. D.; Dixit, S.; Giraldez, E.; Hamza, A. V.; Jancaitis, K. S.; Kroll, J. J.; Lafortune, K. N.; MacGowan, B. J.; Moody, J. D.; Nikroo, A.; Widmayer, C. C.

    2015-05-01

    Adiabat-shaping techniques were investigated in indirect drive inertial confinement fusion experiments on the National Ignition Facility as a means to improve implosion stability, while still maintaining a low adiabat in the fuel. Adiabat-shaping was accomplished in these indirect drive experiments by altering the ratio of the picket and trough energies in the laser pulse shape, thus driving a decaying first shock in the ablator. This decaying first shock is designed to place the ablation front on a high adiabat while keeping the fuel on a low adiabat. These experiments were conducted using the keyhole experimental platform for both three and four shock laser pulses. This platform enabled direct measurement of the shock velocities driven in the glow-discharge polymer capsule and in the liquid deuterium, the surrogate fuel for a DT ignition target. The measured shock velocities and radiation drive histories are compared to previous three and four shock laser pulses. This comparison indicates that in the case of adiabat shaping the ablation front initially drives a high shock velocity, and therefore, a high shock pressure and adiabat. The shock then decays as it travels through the ablator to pressures similar to the original low-adiabat pulses when it reaches the fuel. This approach takes advantage of initial high ablation velocity, which favors stability, and high-compression, which favors high stagnation pressures.

  16. Quantum adiabatic algorithm for factorization and its experimental implementation.

    PubMed

    Peng, Xinhua; Liao, Zeyang; Xu, Nanyang; Qin, Gan; Zhou, Xianyi; Suter, Dieter; Du, Jiangfeng

    2008-11-28

    We propose an adiabatic quantum algorithm capable of factorizing numbers, using fewer qubits than Shor's algorithm. We implement the algorithm in a NMR quantum information processor and experimentally factorize the number 21. In the range that our classical computer could simulate, the quantum adiabatic algorithm works well, providing evidence that the running time of this algorithm scales polynomially with the problem size. PMID:19113467

  17. Adiabat-shaping in indirect drive inertial confinement fusion

    SciTech Connect

    Baker, K. L.; Robey, H. F.; Milovich, J. L.; Jones, O. S.; Smalyuk, V. A.; Casey, D. T.; MacPhee, A. G.; Pak, A.; Celliers, P. M.; Clark, D. S.; Landen, O. L.; Peterson, J. L.; Berzak-Hopkins, L. F.; Weber, C. R.; Haan, S. W.; Döppner, T. D.; Dixit, S.; Hamza, A. V.; Jancaitis, K. S.; Kroll, J. J.; and others

    2015-05-15

    Adiabat-shaping techniques were investigated in indirect drive inertial confinement fusion experiments on the National Ignition Facility as a means to improve implosion stability, while still maintaining a low adiabat in the fuel. Adiabat-shaping was accomplished in these indirect drive experiments by altering the ratio of the picket and trough energies in the laser pulse shape, thus driving a decaying first shock in the ablator. This decaying first shock is designed to place the ablation front on a high adiabat while keeping the fuel on a low adiabat. These experiments were conducted using the keyhole experimental platform for both three and four shock laser pulses. This platform enabled direct measurement of the shock velocities driven in the glow-discharge polymer capsule and in the liquid deuterium, the surrogate fuel for a DT ignition target. The measured shock velocities and radiation drive histories are compared to previous three and four shock laser pulses. This comparison indicates that in the case of adiabat shaping the ablation front initially drives a high shock velocity, and therefore, a high shock pressure and adiabat. The shock then decays as it travels through the ablator to pressures similar to the original low-adiabat pulses when it reaches the fuel. This approach takes advantage of initial high ablation velocity, which favors stability, and high-compression, which favors high stagnation pressures.

  18. Kinetic Theory Derivation of the Adiabatic Law for Ideal Gases.

    ERIC Educational Resources Information Center

    Sobel, Michael I.

    1980-01-01

    Discusses how the adiabatic law for ideal gases can be derived from the assumption of a Maxwell-Boltzmann (or any other) distribution of velocities--in contrast to the usual derivations from thermodynamics alone, and the higher-order effect that leads to one-body viscosity. An elementary derivation of the adiabatic law is given. (Author/DS)

  19. The Adiabatic Invariance of the Action Variable in Classical Dynamics

    ERIC Educational Resources Information Center

    Wells, Clive G.; Siklos, Stephen T. C.

    2007-01-01

    We consider one-dimensional classical time-dependent Hamiltonian systems with quasi-periodic orbits. It is well known that such systems possess an adiabatic invariant which coincides with the action variable of the Hamiltonian formalism. We present a new proof of the adiabatic invariance of this quantity and illustrate our arguments by means of…

  20. Adiabatic principles in atom-diatom collisional energy transfer

    SciTech Connect

    Hovingh, W.J.

    1993-01-01

    This work describes the application of numerical methods to the solution of the time dependent Schroedinger equation for non-reactive atom-diatom collisions in which only one of the degrees of freedom has been removed. The basic method involves expanding the wave function in a basis set in two of the diatomic coordinates in a body-fixed frame (with respect to the triatomic complex) and defining the coefficients in that expansion as functions on a grid in the collision coordinate. The wave function is then propagated in time using a split operator method. The bulk of this work is devoted to the application of this formalism to the study of internal rotational predissociation in NeHF, in which quasibound states of the triatom predissociate through the transfer of energy from rotation of the diatom into translational energy in the atom-diatom separation coordinate. The author analyzes the computed time dependent wave functions to calculate the lifetimes for several quasibound states; these are in agreement with time independent quantum calculations using the same potential. Moreover, the time dependent behavior of the wave functions themselves sheds light on the dynamics of the predissociation processes. Finally, the partial cross sections of the products in those processes is determined with multiple exit channels. These show strong selectivity in the orbital angular momentum of the outgoing fragments, which the author explains with an adiabatic channel interpretation of the wave function's dynamics. The author also suggests that the same formalism might profitably be used to investigate the quantum dynamics of [open quotes]quasiresonant vibration-rotation transfer[close quotes], in which remarkably strong propensity rules in certain inelastic atom-diatom collision arise from classical adiabatic invariance theory.

  1. Quantum Adiabatic Optimization and Combinatorial Landscapes

    NASA Technical Reports Server (NTRS)

    Smelyanskiy, V. N.; Knysh, S.; Morris, R. D.

    2003-01-01

    In this paper we analyze the performance of the Quantum Adiabatic Evolution (QAE) algorithm on a variant of Satisfiability problem for an ensemble of random graphs parametrized by the ratio of clauses to variables, gamma = M / N. We introduce a set of macroscopic parameters (landscapes) and put forward an ansatz of universality for random bit flips. We then formulate the problem of finding the smallest eigenvalue and the excitation gap as a statistical mechanics problem. We use the so-called annealing approximation with a refinement that a finite set of macroscopic variables (verses only energy) is used, and are able to show the existence of a dynamic threshold gamma = gammad, beyond which QAE should take an exponentially long time to find a solution. We compare the results for extended and simplified sets of landscapes and provide numerical evidence in support of our universality ansatz.

  2. An adiabatic demagnetization refrigerator for SIRTF

    NASA Technical Reports Server (NTRS)

    Timbie, P. T.; Bernstein, G. M.; Richards, P. L.

    1989-01-01

    An adiabatic demagnetization refrigerator (ADR) has been proposed to cool bolometric infrared detectors on the multiband imaging photometer of the Space Infrared Telescope Facility (SIRTF). One such refrigerator has been built which uses a ferric ammonium alum salt pill suspended by nylon threads in a 3-T solenoid. The resonant modes of this suspension are above 100 Hz. The heat leak to the salt pill is less than 0.5 microW. The system has a hold time at 0.1K of more than 12 h. The cold stage temperature is regulated with a feedback loop that controls the magnetic field. A second, similar refrigerator is being built at a SIRTF prototype to fly on a ballon-borne telescope. It will use a ferromagnetic shield. The possibility of using a high-Tc solenoid-actuated heat switch is also discussed.

  3. Design of a spaceworthy adiabatic demagnetization refrigerator

    NASA Technical Reports Server (NTRS)

    Serlemitsos, A. T.; Kunes, E.; Sansebastian, M.

    1992-01-01

    A spaceworthy adiabatic demagnetization refrigerator (ADR) under development at NASA-Goddard is presented. A baseline model heat switch was tested extensively with an on/off ratio of about 10,000 and a parasitic heat leak of 10 micro-W. Data obtained from the breadboard models were used to design an ADR with improved structural integrity. The core of the ADR is the salt pill which consists of the paramagnetic salt crystal and the thermal bus. When a magnetic field is applied to the salt it forces the alignment of the magnetic moments, thereby decreasing the entropy of the salt. Preliminary tests results showed a net crystal mass of 680 g instead of the expected 740 g, which indicate that there are gaps in the salt pill. A partial fix was accomplished by sealing helium gas in the salt pill at a pressure of 2 bar, which improved the thermal contact during salt magnetization, at about 2 K.

  4. Differential topology of adiabatically controlled quantum processes

    NASA Astrophysics Data System (ADS)

    Jonckheere, Edmond A.; Rezakhani, Ali T.; Ahmad, Farooq

    2013-03-01

    It is shown that in a controlled adiabatic homotopy between two Hamiltonians, H 0 and H 1, the gap or "anti-crossing" phenomenon can be viewed as the development of cusps and swallow tails in the region of the complex plane where two critical value curves of the quadratic map associated with the numerical range of H 0 + i H 1 come close. The "near crossing" in the energy level plots happens to be a generic situation, in the sense that a crossing is a manifestation of the quadratic numerical range map being unstable in the sense of differential topology. The stable singularities that can develop are identified and it is shown that they could occur near the gap, making those singularities of paramount importance. Various applications, including the quantum random walk, are provided to illustrate this theory.

  5. Reversible logic gate using adiabatic superconducting devices

    PubMed Central

    Takeuchi, N.; Yamanashi, Y.; Yoshikawa, N.

    2014-01-01

    Reversible computing has been studied since Rolf Landauer advanced the argument that has come to be known as Landauer's principle. This principle states that there is no minimum energy dissipation for logic operations in reversible computing, because it is not accompanied by reductions in information entropy. However, until now, no practical reversible logic gates have been demonstrated. One of the problems is that reversible logic gates must be built by using extremely energy-efficient logic devices. Another difficulty is that reversible logic gates must be both logically and physically reversible. Here we propose the first practical reversible logic gate using adiabatic superconducting devices and experimentally demonstrate the logical and physical reversibility of the gate. Additionally, we estimate the energy dissipation of the gate, and discuss the minimum energy dissipation required for reversible logic operations. It is expected that the results of this study will enable reversible computing to move from the theoretical stage into practical usage. PMID:25220698

  6. Symmetry-protected adiabatic quantum transistors

    NASA Astrophysics Data System (ADS)

    Williamson, Dominic J.; Bartlett, Stephen D.

    2015-05-01

    Adiabatic quantum transistors (AQT) allow quantum logic gates to be performed by applying a large field to a quantum many-body system prepared in its ground state, without the need for local control. The basic operation of such a device can be viewed as driving a spin chain from a symmetry-protected (SP) phase to a trivial phase. This perspective offers an avenue to generalize the AQT and to design several improvements. The performance of quantum logic gates is shown to depend only on universal symmetry properties of a SP phase rather than any fine tuning of the Hamiltonian, and it is possible to implement a universal set of logic gates in this way by combining several different types of SP matter. Such SP AQTs are argued to be robust to a range of relevant noise processes.

  7. Number Partitioning via Quantum Adiabatic Computation

    NASA Technical Reports Server (NTRS)

    Smelyanskiy, Vadim N.; Toussaint, Udo; Clancy, Daniel (Technical Monitor)

    2002-01-01

    We study both analytically and numerically the complexity of the adiabatic quantum evolution algorithm applied to random instances of combinatorial optimization problems. We use as an example the NP-complete set partition problem and obtain an asymptotic expression for the minimal gap separating the ground and exited states of a system during the execution of the algorithm. We show that for computationally hard problem instances the size of the minimal gap scales exponentially with the problem size. This result is in qualitative agreement with the direct numerical simulation of the algorithm for small instances of the set partition problem. We describe the statistical properties of the optimization problem that are responsible for the exponential behavior of the algorithm.

  8. Geometric Adiabatic Transport in Quantum Hall States

    NASA Astrophysics Data System (ADS)

    Klevtsov, S.; Wiegmann, P.

    2015-08-01

    We argue that in addition to the Hall conductance and the nondissipative component of the viscous tensor, there exists a third independent transport coefficient, which is precisely quantized. It takes constant values along quantum Hall plateaus. We show that the new coefficient is the Chern number of a vector bundle over moduli space of surfaces of genus 2 or higher and therefore cannot change continuously along the plateau. As such, it does not transpire on a sphere or a torus. In the linear response theory, this coefficient determines intensive forces exerted on electronic fluid by adiabatic deformations of geometry and represents the effect of the gravitational anomaly. We also present the method of computing the transport coefficients for quantum Hall states.

  9. Geometric Adiabatic Transport in Quantum Hall States.

    PubMed

    Klevtsov, S; Wiegmann, P

    2015-08-21

    We argue that in addition to the Hall conductance and the nondissipative component of the viscous tensor, there exists a third independent transport coefficient, which is precisely quantized. It takes constant values along quantum Hall plateaus. We show that the new coefficient is the Chern number of a vector bundle over moduli space of surfaces of genus 2 or higher and therefore cannot change continuously along the plateau. As such, it does not transpire on a sphere or a torus. In the linear response theory, this coefficient determines intensive forces exerted on electronic fluid by adiabatic deformations of geometry and represents the effect of the gravitational anomaly. We also present the method of computing the transport coefficients for quantum Hall states. PMID:26340197

  10. Adiabatic connection at negative coupling strengths

    SciTech Connect

    Seidl, Michael; Gori-Giorgi, Paola

    2010-01-15

    The adiabatic connection of density functional theory (DFT) for electronic systems is generalized here to negative values of the coupling strength alpha (with attractive electrons). In the extreme limit alpha->-infinity a simple physical solution is presented and its implications for DFT (as well as its limitations) are discussed. For two-electron systems (a case in which the present solution can be calculated exactly), we find that an interpolation between the limit alpha->-infinity and the opposite limit of infinitely strong repulsion (alpha->+infinity) yields a rather accurate estimate of the second-order correlation energy E{sub c}{sup GL2}[rho] for several different densities rho, without using virtual orbitals. The same procedure is also applied to the Be isoelectronic series, analyzing the effects of near degeneracy.

  11. Adiabatically-tapered fiber mode multiplexers.

    PubMed

    Yerolatsitis, S; Gris-Sánchez, I; Birks, T A

    2014-01-13

    Simple all-fiber three-mode multiplexers were made by adiabatically merging three dissimilar single-mode cores into one multimode core. This was achieved by collapsing air holes in a photonic crystal fiber and (in a separate device) by fusing and tapering separate telecom fibers in a fluorine-doped silica capillary. In each case the LP01 mode and both LP11 modes were individually excited from three separate input cores, with losses below 0.3 and 0.7 dB respectively and mode purities exceeding 10 dB. Scaling to more modes is challenging, but would be assisted by using single-mode fibers with a smaller ratio of cladding to core diameter. PMID:24515021

  12. The HAWC and SAFIRE Adiabatic Demagnetization Refrigerators

    NASA Technical Reports Server (NTRS)

    Tuttle, Jim; Shirron, Peter; DiPirro, Michael; Jackson, Michael; Behr, Jason; Kunes, Evan; Hait, Tom; Krebs, Carolyn (Technical Monitor)

    2001-01-01

    The High-Resolution Airborne Wide-band Camera (HAWC) and Submillimeter and Far Infrared Experiment (SAFIRE) are far-infrared experiments which will fly on the Stratospheric Observatory for Infrared Astronomy (SOFIA) aircraft. HAWC's detectors will operate at 0.2 Kelvin, while those of SAFIRE will be at 0.1 Kelvin. Each instrument will include an adiabatic demagnetization refrigerator (ADR) to cool its detector stage from the liquid helium bath temperature (HAWC's at 4.2 Kelvin and SAFIRE's pumped to about 1.3 Kelvin) to its operating temperature. Except for the magnets used to achieve the cooling and a slight difference in the heat switch design, the two ADRs are nearly identical. We describe the ADR design and present the results of performance testing.

  13. An Integrated Development Environment for Adiabatic Quantum Programming

    SciTech Connect

    Humble, Travis S; McCaskey, Alex; Bennink, Ryan S; Billings, Jay Jay; D'Azevedo, Eduardo; Sullivan, Blair D; Klymko, Christine F; Seddiqi, Hadayat

    2014-01-01

    Adiabatic quantum computing is a promising route to the computational power afforded by quantum information processing. The recent availability of adiabatic hardware raises the question of how well quantum programs perform. Benchmarking behavior is challenging since the multiple steps to synthesize an adiabatic quantum program are highly tunable. We present an adiabatic quantum programming environment called JADE that provides control over all the steps taken during program development. JADE captures the workflow needed to rigorously benchmark performance while also allowing a variety of problem types, programming techniques, and processor configurations. We have also integrated JADE with a quantum simulation engine that enables program profiling using numerical calculation. The computational engine supports plug-ins for simulation methodologies tailored to various metrics and computing resources. We present the design, integration, and deployment of JADE and discuss its use for benchmarking adiabatic quantum programs.

  14. Non-adiabatic molecular dynamics with complex quantum trajectories. II. The adiabatic representation

    NASA Astrophysics Data System (ADS)

    Zamstein, Noa; Tannor, David J.

    2012-12-01

    We present a complex quantum trajectory method for treating non-adiabatic dynamics. Each trajectory evolves classically on a single electronic surface but with complex position and momentum. The equations of motion are derived directly from the time-dependent Schrödinger equation, and the population exchange arises naturally from amplitude-transfer terms. In this paper the equations of motion are derived in the adiabatic representation to complement our work in the diabatic representation [N. Zamstein and D. J. Tannor, J. Chem. Phys. 137, 22A517 (2012)], 10.1063/1.4739845. We apply our method to two benchmark models introduced by John Tully [J. Chem. Phys. 93, 1061 (1990)], 10.1063/1.459170, and get very good agreement with converged quantum-mechanical calculations. Specifically, we show that decoherence (spatial separation of wavepackets on different surfaces) is already contained in the equations of motion and does not require ad hoc augmentation.

  15. Non-adiabatic molecular dynamics with complex quantum trajectories. II. The adiabatic representation

    SciTech Connect

    Zamstein, Noa; Tannor, David J.

    2012-12-14

    We present a complex quantum trajectory method for treating non-adiabatic dynamics. Each trajectory evolves classically on a single electronic surface but with complex position and momentum. The equations of motion are derived directly from the time-dependent Schroedinger equation, and the population exchange arises naturally from amplitude-transfer terms. In this paper the equations of motion are derived in the adiabatic representation to complement our work in the diabatic representation [N. Zamstein and D. J. Tannor, J. Chem. Phys. 137, 22A517 (2012)]. We apply our method to two benchmark models introduced by John Tully [J. Chem. Phys. 93, 1061 (1990)], and get very good agreement with converged quantum-mechanical calculations. Specifically, we show that decoherence (spatial separation of wavepackets on different surfaces) is already contained in the equations of motion and does not require ad hoc augmentation.

  16. Effect of noncovalent interactions on conformers of the n-butylbenzene monomer studied by mass analyzed threshold ionization spectroscopy and basis-set convergent ab initio computations.

    PubMed

    Tong, Xin; Cerný, Jirí; Müller-Dethlefs, Klaus; Dessent, Caroline E H

    2008-07-01

    Two conformational isomers of the aromatic hydrocarbon n-butylbenzene have been studied using two-color MATI (mass analyzed threshold ionization) spectroscopy to explore the effect of conformation on ionization dynamics. Cationic states of g auche-conformer III and anti- conformers IV were selectively produced by two-color excitation via the respective S 1 origins. Adiabatic ionization potentials of the gauche- and anti-conformations were determined to be 70146 and 69872 +/- 5 cm (-1) respectively. Spectral features and vibrational modes are interpreted with the aid of MP2/cc-pVDZ ab initio calculations, and ionization-induced changes in the molecular conformations are discussed. Complete basis set (CBS) ab initio studies at MP2 level reveal reliable energetics for all four n-butylbenzene conformers observed in earlier two-color REMPI (resonance enhanced multiphoton ionization) spectra. For the S 0 state, the energies of conformer III, IV and V are above conformer I by 130, 289, 73 cm (-1), respectively. Furthermore, the combination of the CBS calculations with the measured REMPI, MATI spectra allowed the determination of the energetics of all four conformers in the S 1 and D 0 states. PMID:18533642

  17. Semiclassical analysis of the electron-nuclear coupling in electronic non-adiabatic processes

    NASA Astrophysics Data System (ADS)

    Agostini, Federica; Min, Seung Kyu; Gross, E. K. U.

    2015-10-01

    In the context of the exact factorization of the electron-nuclear wave function, the coupling between electrons and nuclei beyond the adiabatic regime is encoded (i) in the time-dependent vector and scalar potentials and (ii) in the electron-nuclear coupling operator. The former appear in the Schroedinger-like equation that drives the evolution of the nuclear degrees of freedom, whereas the latter is responsible for inducing non-adiabatic effects in the electronic evolution equation. As we have devoted previous studies to the analysis of the vector and scalar potentials, in this paper we focus on the properties of the electron-nuclear coupling operator, with the aim of describing a numerical procedure to approximate it within a semiclassical treatment of the nuclear dynamics.

  18. Adiabatic path to fractional quantum Hall states of a few bosonic atoms

    SciTech Connect

    Popp, M.; Paredes, B.; Cirac, J.I.

    2004-11-01

    We propose a realistic scheme to create motionally entangled states of a few bosonic atoms. It can experimentally be realized with a gas of ultracold bosonic atoms trapped in a deep optical lattice potential. By simultaneously deforming and rotating the trapping potential on each lattice site it is feasible to adiabatically create a variety of entangled states on each lattice well. We fully address the case of N=2 and 4 atoms per well and identify a sequence of fractional quantum Hall states: the Pfaffian state, the 1/2-Laughlin quasiparticle, and the 1/2-Laughlin state. Exact knowledge of the spectrum has allowed us to design adiabatic paths to these states, with all times and parameters well within the reach of current experimental setups. We further discuss the detection of these states by measuring different properties as their density profile, angular momentum, or correlation functions.

  19. Non-adiabatic perturbations in Ricci dark energy model

    SciTech Connect

    Karwan, Khamphee; Thitapura, Thiti E-mail: nanodsci2523@hotmail.com

    2012-01-01

    We show that the non-adiabatic perturbations between Ricci dark energy and matter can grow both on superhorizon and subhorizon scales, and these non-adiabatic perturbations on subhorizon scales can lead to instability in this dark energy model. The rapidly growing non-adiabatic modes on subhorizon scales always occur when the equation of state parameter of dark energy starts to drop towards -1 near the end of matter era, except that the parameter α of Ricci dark energy equals to 1/2. In the case where α = 1/2, the rapidly growing non-adiabatic modes disappear when the perturbations in dark energy and matter are adiabatic initially. However, an adiabaticity between dark energy and matter perturbations at early time implies a non-adiabaticity between matter and radiation, this can influence the ordinary Sachs-Wolfe (OSW) effect. Since the amount of Ricci dark energy is not small during matter domination, the integrated Sachs-Wolfe (ISW) effect is greatly modified by density perturbations of dark energy, leading to a wrong shape of CMB power spectrum. The instability in Ricci dark energy is difficult to be alleviated if the effects of coupling between baryon and photon on dark energy perturbations are included.

  20. Microwave remote sensing of ionized air.

    SciTech Connect

    Liao, S.; Gopalsami, N.; Heifetz, A.; Elmer, T.; Fiflis, P.; Koehl, E. R.; Chien, H. T.; Raptis, A. C.

    2011-07-01

    We present observations of microwave scattering from ambient room air ionized with a negative ion generator. The frequency dependence of the radar cross section of ionized air was measured from 26.5 to 40 GHz (Ka-band) in a bistatic mode with an Agilent PNA-X series (model N5245A) vector network analyzer. A detailed calibration scheme is provided to minimize the effect of the stray background field and system frequency response on the target reflection. The feasibility of detecting the microwave reflection from ionized air portends many potential applications such as remote sensing of atmospheric ionization and remote detection of radioactive ionization of air.

  1. Ultraviolet femtosecond laser ionization mass spectrometry.

    PubMed

    Imasaka, Totaro

    2008-01-01

    For this study, multiphoton ionization/mass spectrometry using an ultraviolet (UV) femtosecond laser was employed for the trace analysis of organic compounds. Some of the molecules, such as dioxins, contain several chlorine atoms and have short excited-state lifetimes due to a "heavy atom" effect. A UV femtosecond laser is, then, useful for efficient resonance excitation and subsequent ionization. A technique of multiphoton ionization using an extremely short laser pulse (e.g., <10 fs), referred to as "impulsive ionization," may have a potential for use in fragmentation-free ionization, thus providing information on molecular weight in mass spectrometry. PMID:18302290

  2. NOVAE EJECTA AS DISCRETE ADIABATICALLY EXPANDING GLOBULES

    SciTech Connect

    Williams, Robert

    2013-09-15

    Available data for novae show that the X-ray and visible spectral regions correlate with each other as they evolve. Large differences in ionization exist simultaneously in the two wavelength regimes, and a straightforward model is proposed that explains the characteristics observed in both spectral regimes. Its key features are (1) ejected blobs of very high density gas from the white dwarf (WD) that expand to create within each clump a wide range of emitting density, ionization, and velocity, and (2) a more homogeneous circumbinary envelope of gas that is produced by secondary star mass loss. The relative mass loss rates from the two stars determine whether the He/N or the Fe II visible spectrum predominates during decline, when hard X-rays are detected, and when the WD can be detected as a super soft X-ray source.

  3. Dynamics of Charged Particles in an Adiabatic Thermal Beam Equilibrium

    NASA Astrophysics Data System (ADS)

    Chen, Chiping; Wei, Haofei

    2010-11-01

    Charged-particle motion is studied in the self-electric and self-magnetic fields of a well-matched, intense charged-particle beam and an applied periodic solenoidal magnetic focusing field. The beam is assumed to be in a state of adiabatic thermal equilibrium. The phase space is analyzed and compared with that of the well-known Kapchinskij-Vladimirskij (KV)-type beam equilibrium. It is found that the widths of nonlinear resonances in the adiabatic thermal beam equilibrium are narrower than those in the KV-type beam equilibrium. Numerical evidence is presented, indicating almost complete elimination of chaotic particle motion in the adiabatic thermal beam equilibrium.

  4. Dephasing effects on stimulated Raman adiabatic passage in tripod configurations

    SciTech Connect

    Lazarou, C.; Vitanov, N. V.

    2010-09-15

    We present an analytic description of the effects of dephasing processes on stimulated Raman adiabatic passage in a tripod quantum system. To this end, we develop an effective two-level model. Our analysis makes use of the adiabatic approximation in the weak dephasing regime. An effective master equation for a two-level system formed by two dark states is derived, where analytic solutions are obtained by utilizing the Demkov-Kunike model. From these, it is found that the fidelity for the final coherent superposition state decreases exponentially for increasing dephasing rates. Depending on the pulse ordering and for adiabatic evolution, the pulse delay can have an inverse effect.

  5. Adiabatic theory in regions of strong field gradients. [in magnetosphere

    NASA Technical Reports Server (NTRS)

    Whipple, E. C.; Northrop, T. G.; Birmingham, T. J.

    1986-01-01

    The theory for the generalized first invariant for adiabatic motion of charged particles in regions where there are large gradients in magnetic or electric fields is developed. The general condition for an invariant to exist in such regions is that the potential well in which the particle oscillates change its shape slowly as the particle drifts. It is shown how the Kruskal (1962) procedure can be applied to obtain expressions for the invariant and for drift velocities that are asymptotic in a smallness parameter epsilon. The procedure is illustrated by obtaining the invariant and drift velocities for particles traversing a perpendicular shock, and the generalized invariant is compared with the magnetic moment, and the drift orbits with the actual orbits, for a particular case. In contrast to the magnetic moment, the generalized first invariant is better for large gyroradii (large kinetic energies) than for small gyroradii. Expressions for the invariant when an electrostatic potential jump is imposed across the perpendicular shock, and when the particle traverses a rotational shear layer with a small normal component of the magnetic field are given.

  6. Design of the PIXIE Adiabatic Demagnetization Refrigerators

    NASA Technical Reports Server (NTRS)

    Shirron, Peter J.; Kimball, Mark Oliver; Fixsen, Dale J.; Kogut, Alan J.; Li, Xiaoyi; DiPirro, Michael

    2012-01-01

    The Primordial Inflation Explorer (PIXIE) is a proposed mission to densely map the polarization of the cosmic microwave background. It will operate in a scanning mode from a sun-synchronous orbit, using low temperature detectors (at 0.1 K) and located inside a teslescope that is cooled to approximately 2.73 K - to match the background temperature. A mechanical cryocooler operating at 4.5 K establishes a low base temperature from which two adiabatic demagnetization refrigerator (ADR) assemblies will cool the telescope and detectors. To achieve continuous scanning capability, the ADRs must operate continuously. Complicating the design are two factors: 1) the need to systematically vary the temperature of various telescope components in order to separate the small polarization signal variations from those that may arise from temperature drifts and changing gradients within the telescope, and 2) the orbital and monthly variations in lunar irradiance into the telescope barrels. These factors require the telescope ADR to reject quasi-continuous heat loads of 2-3 millwatts, while maintaining a peak heat reject rate of less than 12 milliwatts. The detector heat load at 0.1 K is comparatively small at 1-2 microwatts. This paper will describe the 3-stage and 2-stage continuous ADRs that will be used to meet the cooling power and temperature stability requirements of the PIXIE detectors and telescope.

  7. Design of the PIXIE adiabatic demagnetization refrigerators

    NASA Astrophysics Data System (ADS)

    Shirron, Peter J.; Kimball, Mark O.; Fixsen, Dale J.; Kogut, Alan J.; Li, Xiaoyi; DiPirro, Michael J.

    2012-04-01

    The Primordial Inflation Explorer (PIXIE) is a proposed mission to densely map the polarization of the cosmic microwave background. It will operate in a scanning mode from a sun-synchronous orbit, using low temperature detectors (at 0.1 K) and located inside a telescope that is cooled to approximately 2.73 K - to match the background temperature. A mechanical cryocooler operating at 4.5 K establishes a low base temperature from which two adiabatic demagnetization refrigerator (ADR) assemblies will cool the telescope and detectors. To achieve continuous scanning capability, the ADRs must operate continuously. Complicating the design are two factors: (1) the need to systematically vary the temperature of various telescope components in order to separate the small polarization signal variations from those that may arise from temperature drifts and changing gradients within the telescope, and (2) the orbital and monthly variations in lunar irradiance into the telescope barrels. These factors require the telescope ADR to reject quasi-continuous heat loads of 2-3 mW, while maintaining a peak heat reject rate of less than 12 mW. The detector heat load at 0.1 K is comparatively small at 1-2 μW. This paper will describe the 3-stage and 2-stage continuous ADRs that will be used to meet the cooling power and temperature stability requirements of the PIXIE detectors and telescope.

  8. Graph isomorphism and adiabatic quantum computing

    NASA Astrophysics Data System (ADS)

    Gaitan, Frank; Clark, Lane

    2014-03-01

    In the Graph Isomorphism (GI) problem two N-vertex graphs G and G' are given and the task is to determine whether there exists a permutation of the vertices of G that preserves adjacency and maps G --> G'. If yes (no), then G and G' are said to be isomorphic (non-isomorphic). The GI problem is an important problem in computer science and is thought to be of comparable difficulty to integer factorization. We present a quantum algorithm that solves arbitrary instances of GI, and which provides a novel approach to determining all automorphisms of a graph. The algorithm converts a GI instance to a combinatorial optimization problem that can be solved using adiabatic quantum evolution. Numerical simulation of the algorithm's quantum dynamics shows that it correctly distinguishes non-isomorphic graphs; recognizes isomorphic graphs; and finds the automorphism group of a graph. We also discuss the algorithm's experimental implementation and show how it can be leveraged to solve arbitrary instances of the NP-Complete Sub-Graph Isomorphism problem.

  9. Adiabatic Quantum Computation with Neutral Atoms

    NASA Astrophysics Data System (ADS)

    Biedermann, Grant

    2013-03-01

    We are implementing a new platform for adiabatic quantum computation (AQC)[2] based on trapped neutral atoms whose coupling is mediated by the dipole-dipole interactions of Rydberg states. Ground state cesium atoms are dressed by laser fields in a manner conditional on the Rydberg blockade mechanism,[3,4] thereby providing the requisite entangling interactions. As a benchmark we study a Quadratic Unconstrained Binary Optimization (QUBO) problem whose solution is found in the ground state spin configuration of an Ising-like model. In collaboration with Lambert Parazzoli, Sandia National Laboratories; Aaron Hankin, Center for Quantum Information and Control (CQuIC), University of New Mexico; James Chin-Wen Chou, Yuan-Yu Jau, Peter Schwindt, Cort Johnson, and George Burns, Sandia National Laboratories; Tyler Keating, Krittika Goyal, and Ivan Deutsch, Center for Quantum Information and Control (CQuIC), University of New Mexico; and Andrew Landahl, Sandia National Laboratories. This work was supported by the Laboratory Directed Research and Development program at Sandia National Laboratories

  10. Adiabatic Quantum Algorithm for Search Engine Ranking

    NASA Astrophysics Data System (ADS)

    Garnerone, Silvano; Zanardi, Paolo; Lidar, Daniel A.

    2012-06-01

    We propose an adiabatic quantum algorithm for generating a quantum pure state encoding of the PageRank vector, the most widely used tool in ranking the relative importance of internet pages. We present extensive numerical simulations which provide evidence that this algorithm can prepare the quantum PageRank state in a time which, on average, scales polylogarithmically in the number of web pages. We argue that the main topological feature of the underlying web graph allowing for such a scaling is the out-degree distribution. The top-ranked log⁡(n) entries of the quantum PageRank state can then be estimated with a polynomial quantum speed-up. Moreover, the quantum PageRank state can be used in “q-sampling” protocols for testing properties of distributions, which require exponentially fewer measurements than all classical schemes designed for the same task. This can be used to decide whether to run a classical update of the PageRank.

  11. Adiabaticity and spectral splits in collective neutrino transformations

    SciTech Connect

    Raffelt, Georg G.; Smirnov, Alexei Yu.

    2007-12-15

    Neutrinos streaming off a supernova core transform collectively by neutrino-neutrino interactions, leading to 'spectral splits' where an energy E{sub split} divides the transformed spectrum sharply into parts of almost pure but different flavors. We present a detailed description of the spectral-split phenomenon which is conceptually and quantitatively understood in an adiabatic treatment of neutrino-neutrino effects. Central to this theory is a self-consistency condition in the form of two sum rules (integrals over the neutrino spectra that must equal certain conserved quantities). We provide explicit analytic and numerical solutions for various neutrino spectra. We introduce the concept of the adiabatic reference frame and elaborate on the relative adiabatic evolution. Violating adiabaticity leads to the spectral split being 'washed out'. The sharpness of the split appears to be represented by a surprisingly universal function.

  12. Startup of the RFP in a quasi-adiabatic mode

    SciTech Connect

    Caramana, E.J.

    1980-01-01

    The equations describing the purely adiabatic formation of the reversed-field pinch are solved. This method of formation in principle remedies the problem of flux consumption during the startup phase of this device.

  13. Ultrafast stimulated Raman parallel adiabatic passage by shaped pulses

    SciTech Connect

    Dridi, G.; Guerin, S.; Hakobyan, V.; Jauslin, H. R.; Eleuch, H.

    2009-10-15

    We present a general and versatile technique of population transfer based on parallel adiabatic passage by femtosecond shaped pulses. Their amplitude and phase are specifically designed to optimize the adiabatic passage corresponding to parallel eigenvalues at all times. We show that this technique allows the robust adiabatic population transfer in a Raman system with the total pulse area as low as 3{pi}, corresponding to a fluence of one order of magnitude below the conventional stimulated Raman adiabatic passage process. This process of short duration, typically picosecond and subpicosecond, is easily implementable with the modern pulse shaper technology and opens the possibility of ultrafast robust population transfer with interesting applications in quantum information processing.

  14. Understanding the Performance of Low-Adiabat Cryogenic Implosions on OMEGA

    NASA Astrophysics Data System (ADS)

    Goncharov, V. N.; Sangster, T. C.; Epstein, R.; Hu, S. X.; Igumenshchev, I. V.; Forrest, C. J.; Froula, D. H.; Marshall, F. J.; Michel, D. T.; Radha, P. B.; Seka, W.; Stoeckl, C.; Frenje, J. A.; Gatu Johnson, M.

    2014-10-01

    While the moderate-adiabat (α > 3.5) cryogenic implosions on OMEGA are well understood using multidimensional hydrocode simulations, the performance of lower-adiabat implosions is degraded relative to code predictions. The potential degradation mechanisms (not fully accounted for in simulations) include target-nonuniformity sources (excessive laser imprint, target debris, beam-overlap nonuniformity) and inaccuracies in laser-coupling modeling, especially during the pulse rise. To address the target-stability issues, target designs with thicker ice layers and smaller implosion velocities are considered. These targets have smaller in-flight aspect ratios, making them less susceptible to hydrodynamic instability growth. To address inaccuracies in laser coupling, a design with a slower main pulse rise is considered. This talk will summarize progress made on these issues. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

  15. General integral relations for the description of scattering states using the hyperspherical adiabatic basis

    SciTech Connect

    Romero-Redondo, C.; Garrido, E.; Barletta, P.; Kievsky, A.; Viviani, M.

    2011-02-15

    In this work we investigate 1+2 reactions within the framework of the hyperspherical adiabatic expansion method. With this aim two integral relations, derived from the Kohn variational principle, are used. A detailed derivation of these relations is shown. The expressions derived are general, not restricted to relative s partial waves, and with applicability in multichannel reactions. The convergence of the K matrix in terms of the adiabatic potentials is investigated. Together with a simple model case used as a test for the method, we show results for the collision of a {sup 4}He atom on a {sup 4}He{sub 2} dimer (only the elastic channel open), and for collisions involving a {sup 6}Li and two {sup 4}He atoms (two channels open).

  16. Adiabaticity and the fate of non-Gaussianities: The trispectrum and beyond

    NASA Astrophysics Data System (ADS)

    Meyers, Joel; Sivanandam, Navin

    2011-09-01

    Extending the analysis of J. Meyers and N. Sivanandam [Phys. Rev. DPRVDAQ1550-7998 83, 103517 (2011)10.1103/PhysRevD.83.103517] beyond the bispectrum, we explore the superhorizon generation of local non-Gaussianities and their subsequent approach to adiabaticity. Working with a class of two field models of inflation with potentials amenable to treatment with the δN formalism, we find that, as is the case for fNLlocal, the local trispectrum parameters τNL and gNL are exponentially driven toward values which are slow-roll suppressed if the fluctuations are driven into an adiabatic mode by a phase of effectively single field inflation. We argue that general considerations should ensure that a similar behavior will hold for the local forms of higher point correlations as well.

  17. Revisiting Adiabatic Switching for Initial Conditions in Quasi-Classical Trajectory Calculations: Application to CH4.

    PubMed

    Qu, Chen; Bowman, Joel M

    2016-07-14

    Semiclassical quantization of vibrational energies, using adiabatic switching (AS), is applied to CH4 using a recent ab initio potential energy surface, for which exact quantum calculations of vibrational energies are available. Details of the present calculations, which employ a harmonic normal-mode zeroth-order Hamiltonian, emphasize the importance of transforming to the Eckart frame during the propagation of the adiabatically switched Hamiltonian. The AS energies for the zero-point, and fundamental excitations of two modes are in good agreement with the quantum ones. The use of AS in the context of quasi-classical trajectory calculations is revisited, following previous work reported in 1995, which did not recommend the procedure. We come to a different conclusion here. PMID:26881845

  18. Nonadiabatic transitions in finite-time adiabatic rapid passage

    NASA Astrophysics Data System (ADS)

    Lu, T.; Miao, X.; Metcalf, H.

    2007-06-01

    To apply the adiabatic rapid passage process repetitively [T. Lu, X. Miao, and H. Metcalf, Phys. Rev. A 71, 061405(R) (2005)], the nonadiabatic transition probability of a two-level atom subject to chirped light pulses over a finite period of time needs to be calculated. Using a unitary first-order perturbation method in the rotating adiabatic frame, an approximate formula has been derived for such transition probabilities in the entire parameter space of the pulses.

  19. Realization of adiabatic Aharonov-Bohm scattering with neutrons

    NASA Astrophysics Data System (ADS)

    Sjöqvist, Erik; Almquist, Martin; Mattsson, Ken; Gürkan, Zeynep Nilhan; Hessmo, Björn

    2015-11-01

    The adiabatic Aharonov-Bohm (AB) effect is a manifestation of the Berry phase acquired when some slow variables take a planar spin around a loop. While the effect has been observed in molecular spectroscopy, direct measurement of the topological phase shift in a scattering experiment has been elusive in the past. Here, we demonstrate an adiabatic AB effect by explicit simulation of the dynamics of unpolarized very slow neutrons that scatter on a long straight current-carrying wire.

  20. Shortcuts to adiabaticity for non-Hermitian systems

    SciTech Connect

    Ibanez, S.; Martinez-Garaot, S.; Torrontegui, E.; Muga, J. G.; Chen Xi

    2011-08-15

    Adiabatic processes driven by non-Hermitian, time-dependent Hamiltonians may be sped up by generalizing inverse engineering techniques based on counter-diabatic (transitionless driving) algorithms or on dynamical invariants. We work out the basic theory and examples described by two-level Hamiltonians: the acceleration of rapid adiabatic passage with a decaying excited level and of the dynamics of a classical particle on an expanding harmonic oscillator.

  1. Collisional and radiative processes in adiabatic deceleration, deflection, and off-axis trapping of a Rydberg atom beam.

    PubMed

    Seiler, Ch; Hogan, S D; Schmutz, H; Agner, J A; Merkt, F

    2011-02-18

    A supersonic beam of Rydberg hydrogen atoms has been adiabatically deflected by 90°, decelerated to zero velocity in less than 25  μs, and loaded into an electric trap. The deflection has allowed the suppression of collisions with atoms in the trailing part of the gas pulse. The processes leading to trap losses, i.e., fluorescence to the ground state, and transitions and ionization induced by blackbody radiation have been monitored over several milliseconds and quantitatively analyzed. PMID:21405512

  2. Extended adiabatic blast waves and a model of the soft X-ray background. [interstellar matter

    NASA Technical Reports Server (NTRS)

    Cox, D. P.; Anderson, P. R.

    1981-01-01

    An analytical approximation is generated which follows the development of an adiabatic spherical blast wave in a homogeneous ambient medium of finite pressure. An analytical approximation is also presented for the electron temperature distribution resulting from coulomb collisional heating. The dynamical, thermal, ionization, and spectral structures are calculated for blast waves of energy E sub 0 = 5 x 10 to the 50th power ergs in a hot low-density interstellar environment. A formula is presented for estimating the luminosity evolution of such explosions. The B and C bands of the soft X-ray background, it is shown, are reproduced by such a model explosion if the ambient density is about .000004 cm, the blast radius is roughly 100 pc, and the solar system is located inside the shocked region. Evolution in a pre-existing cavity with a strong density gradient may, it is suggested, remove both the M band and OVI discrepancies.

  3. Stimulated Raman adiabatic passage for improved performance of a cold-atom electron and ion source

    NASA Astrophysics Data System (ADS)

    Sparkes, B. M.; Murphy, D.; Taylor, R. J.; Speirs, R. W.; McCulloch, A. J.; Scholten, R. E.

    2016-08-01

    We implement high-efficiency coherent excitation to a Rydberg state using stimulated Raman adiabatic passage in a cold-atom electron and ion source. We achieve an efficiency of 60% averaged over the laser excitation volume with a peak efficiency of 82%, a 1.6 times improvement relative to incoherent pulsed-laser excitation. Using pulsed electric field ionization of the Rydberg atoms we create electron bunches with durations of 250 ps. High-efficiency excitation will increase source brightness, crucial for ultrafast electron diffraction experiments, and coherent excitation to high-lying Rydberg states could allow for the reduction of internal bunch heating and the creation of a high-speed single-ion source.

  4. Comparison of the rotationally adiabatic and vibrationally adiabatic distorted wave methods for the H H2(v=0, j=0)→') H chemical reactions

    NASA Astrophysics Data System (ADS)

    Clary, D. C.; Connor, J. N. L.

    Rotationally adiabatic distorted wave (RADW) and vibrationally adiabatic distorted wave (VADW) calculations of total and differential cross sections are reported for the three-dimensional H + H2(v=0, j=0) →H2(v'=0, j') + H and D + H2(v=0, j=0) →DH(v'=0, j') + H chemical reactions. Both the Porter-Karplus (PK) and the Siegbahn-Liu-Truhlar-Horowitz (SLTH) potential energy surfaces are used. The RADW results for D+H2 on the SLTH potential surface agree well with those obtained by Yung et al. In calculations using the PK surface, we obtain poor agreement with the RADW results reported for the H + H2 reaction by Choi and Tang, and for the D + H2 reaction by Tang and Choi. Reasons for these discrepancies are discussed. The absolute total RADW cross sections for the H + H2 reaction using both potential surfaces fall well below those obtained in accurate quantum calculations while the VADW total cross sections are smaller in magnitude than the RADW cross sections. The RADW and VADW results for relative rotational population distributions and for normalized differential cross sections are almost identical, and agree well with accurate quantum calculations for these quantities for the H + H2 reaction using the PK potential surface.

  5. Adiabatic calorimetric decomposition studies of 50 wt.% hydroxylamine/water.

    PubMed

    Cisneros, L O; Rogers, W J; Mannan, M S

    2001-03-19

    Calorimetric data can provide a basis for determining potential hazards in reactions, storage, and transportation of process chemicals. This work provides calorimetric data for the thermal decomposition behavior in air of 50wt.% hydroxylamine/water (HA), both with and without added stabilizers, which was measured in closed cells with an automatic pressure tracking adiabatic calorimeter (APTAC). Among the data provided are onset temperatures, reaction order, activation energies, pressures of noncondensable products, thermal stability at 100 degrees C, and the effect of HA storage time. Discussed also are the catalytic effects of carbon steel, stainless steel, stainless steel with silica coating, inconel, titanium, and titanium with silica coating on the reaction self-heat rates and onset temperatures. In borosilicate glass cells, HA was relatively stable at temperatures up to 133 degrees C, where the HA decomposition self-heat rate reached 0.05 degrees C/min. The added stabilizers appeared to reduce HA decomposition rates in glass cells and at ambient temperatures. The tested metals and metal surfaces coated with silica acted as catalysts to lower the onset temperatures and increase the self-heat rates. PMID:11165058

  6. Shortcuts to Adiabaticity in Transport of a Single Trapped Ion

    NASA Astrophysics Data System (ADS)

    An, Shuoming; Lv, Dingshun; Campo, Adolfo Del; Kim, Kihwan

    2015-05-01

    We report an experimental study on shortcuts to adiabaticity in the transport of a single 171Yb+ ion trapped in a harmonic potential. In these driving schemes, the application of a force induces a nonadiabatic dynamics in which excitations are tailored so as to preserve the ion motional state in the ground state upon completion of the process. We experimentally apply the laser induced force and realize three different protocols: (1) a transitionless driving with a counterdiabatic term out of phase with the displacement force, (2) a classical protocol assisted by counterdiabatic fields in phase with the main force, (3) and an engineered transport protocol based on the Fourier transform of the trap acceleration. We experimentally compare and discuss the robustness of these protocols under given experimental limitations such as trap frequency drifts. This work was supported by the National Basic Research Program of China under Grants No. 2011CBA00300 (No. 2011CBA00301), the National Natural Science Foundation of China 11374178, and the University of Massachusetts Boston (No. P20150000029279).

  7. Evolution of f{sub NL} to the adiabatic limit

    SciTech Connect

    Elliston, Joseph; Mulryne, David J.; Tavakol, Reza; Seery, David E-mail: D.Mulryne@qmul.ac.uk E-mail: R.Tavakol@qmul.ac.uk

    2011-11-01

    We study inflationary perturbations in multiple-field models, for which ζ typically evolves until all isocurvature modes decay — the {sup a}diabatic limit{sup .} We use numerical methods to explore the sensitivity of the local-shape bispectrum to the process by which this limit is achieved, finding an appreciable dependence on model-specific data such as the time at which slow-roll breaks down or the timescale of reheating. In models with a sum-separable potential where the isocurvature modes decay before the end of the slow-roll phase we give an analytic criterion for the asymptotic value of f{sub NL} to be large. Other examples can be constructed using a waterfall field to terminate inflation while f{sub NL} is transiently large, caused by descent from a ridge or convergence into a valley. We show that these two types of evolution are distinguished by the sign of the bispectrum, and give approximate expressions for the peak f{sub NL}.

  8. Weakly ionized cosmic gas: Ionization and characterization

    NASA Technical Reports Server (NTRS)

    Rosenberg, M.; Mendis, D. A.; Chow, V. W.

    1994-01-01

    Since collective plasma behavior may determine important transport processes (e.g., plasma diffusion across a magnetic field) in certain cosmic environments, it is important to delineate the parameter space in which weakly ionized cosmic gases may be characterized as plasmas. In this short note, we do so. First, we use values for the ionization fraction given in the literature, wherein the ionization is generally assumed to be due primarily to ionization by cosmic rays. We also discuss an additional mechanism for ionization in such environments, namely, the photoelectric emission of electrons from cosmic dust grains in an interstellar Far Ultra Violet (FUV) radiation field. Simple estimates suggest that under certain conditions this mechanism may dominate cosmic ray ionization, and possibly also the photoionization of metal atoms by the interstellar FUV field, and thereby lead to an enhanced ionization level.

  9. Adiabatic and diabatic invariants in ion-molecule reactions.

    PubMed

    Lorquet, J C

    2009-12-28

    A point charge interacting with a dipole (either induced or permanent) constitutes a completely integrable dynamical subsystem characterized by three first integrals of the motion (E, p(phi), and either l(2) or a Hamilton-Jacobi separation constant beta). An ion-molecule reaction (capture or fragmentation) can be seen as an interaction between such a subsystem and a bath of oscillators. This interaction is a perturbation that destroys some of the first integrals. However, the perturbation depends on the separation between the fragments and the destruction is gradual. The mathematical simplicity of the long-range electrostatic interaction potential leads to useful simplifications. A first-order perturbation treatment based on the structured and regular nature of the multipole expansion is presented. The separating integrals valid in the asymptotic limit are found to subsist at intermediate distances, although in a weaker form. As the reaction coordinate decreases, i.e., as the fragments approach, the asymptotic range is followed by an outer region where (i) the azimuthal momentum p(phi) remains a constant of the motion; (ii) the square angular momentum l(2) or the separation constant beta transform into a diabatic invariant in regions of phase space characterized by a high value of the translational momentum p(r); (iii) for low values of p(r), it is advantageous to use the action integral contour integral(p(theta)d theta), which is an adiabatic invariant. The conditions under which an effective potential obtained by adding centrifugal repulsion to an electrostatic attractive term can be validly constructed are specified. In short, the dynamics of ion-molecule interactions is still regular in parts of phase space corresponding to a range of the reaction coordinate where the interaction potential deviates from its asymptotic shape. PMID:20059072

  10. Potential of atmospheric pressure chemical ionization source in gas chromatography tandem mass spectrometry for the screening of urinary exogenous androgenic anabolic steroids.

    PubMed

    Raro, M; Portolés, T; Pitarch, E; Sancho, J V; Hernández, F; Garrostas, L; Marcos, J; Ventura, R; Segura, J; Pozo, O J

    2016-02-01

    The atmospheric pressure chemical ionization (APCI) source for gas chromatography-mass spectrometry analysis has been evaluated for the screening of 16 exogenous androgenic anabolic steroids (AAS) in urine. The sample treatment is based on the strategy currently applied in doping control laboratories i.e. enzymatic hydrolysis, liquid-liquid extraction (LLE) and derivatization to form the trimethylsilyl ether-trimethylsilyl enol ether (TMS) derivatives. These TMS derivatives are then analyzed by gas chromatography tandem mass spectrometry using a triple quadrupole instrument (GC-QqQ MS/MS) under selected reaction monitoring (SRM) mode. The APCI promotes soft ionization with very little fragmentation resulting, in most cases, in abundant [M + H](+) or [M + H-2TMSOH](+) ions, which can be chosen as precursor ions for the SRM transitions, improving in this way the selectivity and sensitivity of the method. Specificity of the transitions is also of great relevance, as the presence of endogenous compounds can affect the measurements when using the most abundant ions. The method has been qualitatively validated by spiking six different urine samples at two concentration levels each. Precision was generally satisfactory with RSD values below 25 and 15% at the low and high concentration level, respectively. Most the limits of detection (LOD) were below 0.5 ng mL(-1). Validation results were compared with the commonly used method based on the electron ionization (EI) source. EI analysis was found to be slightly more repeatable whereas lower LODs were found for APCI. In addition, the applicability of the developed method has been tested in samples collected after the administration of 4-chloromethandienone. The highest sensitivity of the APCI method for this compound, allowed to increase the period in which its administration can be detected. PMID:26772132

  11. Statistical mechanics of Roskilde liquids: Configurational adiabats, specific heat contours, and density dependence of the scaling exponent

    SciTech Connect

    Bailey, Nicholas P.; Bøhling, Lasse; Veldhorst, Arno A.; Schrøder, Thomas B.; Dyre, Jeppe C.

    2013-11-14

    We derive exact results for the rate of change of thermodynamic quantities, in particular, the configurational specific heat at constant volume, C{sub V}, along configurational adiabats (curves of constant excess entropy S{sub ex}). Such curves are designated isomorphs for so-called Roskilde liquids, in view of the invariance of various structural and dynamical quantities along them. The slope of the isomorphs in a double logarithmic representation of the density-temperature phase diagram, γ, can be interpreted as one third of an effective inverse power-law potential exponent. We show that in liquids where γ increases (decreases) with density, the contours of C{sub V} have smaller (larger) slope than configurational adiabats. We clarify also the connection between γ and the pair potential. A fluctuation formula for the slope of the C{sub V}-contours is derived. The theoretical results are supported with data from computer simulations of two systems, the Lennard-Jones fluid, and the Girifalco fluid. The sign of dγ/dρ is thus a third key parameter in characterizing Roskilde liquids, after γ and the virial-potential energy correlation coefficient R. To go beyond isomorph theory we compare invariance of a dynamical quantity, the self-diffusion coefficient, along adiabats and C{sub V}-contours, finding it more invariant along adiabats.

  12. Ionized cluster beam technology for material science

    NASA Astrophysics Data System (ADS)

    Takagi, Toshinori

    1997-06-01

    The most suitable kinetic energy range of ionized materials in film formation and epitaxial growth is from a few eV to a few hundreds eV, especially, less than about 100eV, when ions are used as a host. The main roles of ions in film formation are the effects due to their kinetic energy and the electronic charge effects which involve the effect to active film formation and the effect acceleration of chemical reactions. Therefore, it is important to develope the technology to transport large volume of a flux of ionized particles with an extremely low incident energy without any troubles due to the space charge effects and charge up problems on the surface. This is the exact motivation for us to have been developing the Ionized Cluster Beam (ICB) technology since 1972. By ICB technology materials (actually wide varieties of materials such as metal, semiconductor, magnetic material, insulator, organic material, etc.) are vaporized and ejected through a small hole nozzle into a high vacuum, where the vaporized material condenses into clusters with loosely coupled atoms with the sizes about from 100 to a few 1000 atoms (mainly 100-2000 atoms) by supercondensation phenomena due to the adiabatic expansion in this evaporation process through a small hole nozzle. In the ICB technology an atom in each cluster is ionized by irradiated by electron shower, and the ionized clusters are accelerated by electric field onto a substrate. The ionized clusters with neutral clusters impinged onto a substrate are spreaded separately into atoms migrating over the substrate, so that the surface migration energy of the impinged atoms, that is, surface diffusion energy are controlled by an incident energy of a cluster. In this report the theoretical and also experimental results of ICB technology are summarized.

  13. High-energy electron-energy spectra of atoms undergoing tunneling and barrier-suppression ionization by superintense linearly polarized laser radiation

    SciTech Connect

    Krainov, V.P.; Sofronov, A.V.

    2004-01-01

    The high-energy electron-energy spectra of atoms and atomic ions undergoing direct tunneling or barrier-suppression ionization by superintense linearly polarized femtosecond laser pulse are derived. The Landau-Dykhne adiabatic approximation is used. The new result is the simple analytic expression for the electron momentum spectrum along the polarization axis and along the other directions in the case of the relativistic quiver electron energies. The contribution from the direct tunneling ionization exceeds the contribution from the ionization occurring in the rescattering processes. The energy spectrum is independent of the laser frequency and of the nonrelativistic ionization potential of the atom (atomic ion) considered. The conclusions have been made that (1) the drift electron energy along the polarization axis is much greater than in other directions. (2) the energy distribution depends on the sign of the electron drift momentum along the propagation of laser radiation, and (3) the electron drift energy is the nonrelativistic quantity even when the quiver electron energy has high ultrarelativistic values.

  14. Exchange–Correlation Functionals via Local Interpolation along the Adiabatic Connection

    PubMed Central

    2016-01-01

    The construction of density-functional approximations is explored by modeling the adiabatic connection locally, using energy densities defined in terms of the electrostatic potential of the exchange–correlation hole. These local models are more amenable to the construction of size-consistent approximations than their global counterparts. In this work we use accurate input local ingredients to assess the accuracy of a range of local interpolation models against accurate exchange–correlation energy densities. The importance of the strictly correlated electrons (SCE) functional describing the strong coupling limit is emphasized, enabling the corresponding interpolated functionals to treat strong correlation effects. In addition to exploring the performance of such models numerically for the helium and beryllium isoelectronic series and the dissociation of the hydrogen molecule, an approximate analytic model is presented for the initial slope of the local adiabatic connection. Comparisons are made with approaches based on global models, and prospects for future approximations based on the local adiabatic connection are discussed. PMID:27116427

  15. Exchange-Correlation Functionals via Local Interpolation along the Adiabatic Connection.

    PubMed

    Vuckovic, Stefan; Irons, Tom J P; Savin, Andreas; Teale, Andrew M; Gori-Giorgi, Paola

    2016-06-14

    The construction of density-functional approximations is explored by modeling the adiabatic connection locally, using energy densities defined in terms of the electrostatic potential of the exchange-correlation hole. These local models are more amenable to the construction of size-consistent approximations than their global counterparts. In this work we use accurate input local ingredients to assess the accuracy of a range of local interpolation models against accurate exchange-correlation energy densities. The importance of the strictly correlated electrons (SCE) functional describing the strong coupling limit is emphasized, enabling the corresponding interpolated functionals to treat strong correlation effects. In addition to exploring the performance of such models numerically for the helium and beryllium isoelectronic series and the dissociation of the hydrogen molecule, an approximate analytic model is presented for the initial slope of the local adiabatic connection. Comparisons are made with approaches based on global models, and prospects for future approximations based on the local adiabatic connection are discussed. PMID:27116427

  16. Coverage dependent non-adiabaticity of CO on a copper surface

    SciTech Connect

    Omiya, Takuma; Arnolds, Heike

    2014-12-07

    We have studied the coverage-dependent energy transfer dynamics between hot electrons and CO on Cu(110) with femtosecond visible pump, sum frequency probe spectroscopy. We find that transients of the C–O stretch frequency display a red shift, which increases from 3 cm{sup −1} at 0.1 ML to 9 cm{sup −1} at 0.77 ML. Analysis of the transients reveals that the non-adiabatic coupling between the adsorbate vibrational motion and the electrons becomes stronger with increasing coverage. This trend requires the frustrated rotational mode to be the cause of the non-adiabatic behavior, even for relatively weak laser excitation of the adsorbate. We attribute the coverage dependence to both an increase in the adsorbate electronic density of states and an increasingly anharmonic potential energy surface caused by repulsive interactions between neighboring CO adsorbates. This work thus reveals adsorbate-adsorbate interactions as a new way to control adsorbate non-adiabaticity.

  17. Ab initio adiabatic and diabatic energies and dipole moments of the KH molecule

    NASA Astrophysics Data System (ADS)

    Khelifi, Neji; Oujia, Brahim; Gadea, Florent Xavier

    2002-02-01

    An ab initio adiabatic and diabatic study of the KH molecule is performed for all states below the ionic limit [i.e., K (4s, 4p, 5s, 3d, 5p, 4d, 6s, and 4f)+H(1s)] in 1Σ+ and 3Σ+ symmetries. Adiabatic results are also reported for 1Π, 3Π, 1Δ, and 3Δ symmetries. The ab initio calculations rely on pseudopotential, operatorial core valence correlation, and full valence CI approaches, combined to an efficient diabatization procedure. For the low-lying states, our vibrational level spacings and spectroscopic constants are in very good agreement with the available experimental data. Diabatic potentials and dipoles moments are analyzed, revealing the strong imprint of the ionic state in the 1Σ+ adiabatic states while improving the results. The undulations of the diabatic curves and of the triplet-singlet diabatic energy difference which we found positive, as in Hund's rule, are related to the Rydberg functions. As for LiH, the vibrational spacing of the A state is bracketed by our results with and without the improvement taking into account the diabatic representation. Experimental suggestions are also given.

  18. Comment on ``Adiabatic quantum computation with a one-dimensional projector Hamiltonian''

    NASA Astrophysics Data System (ADS)

    Kay, Alastair

    2013-10-01

    The partial adiabatic search algorithm was introduced in Tulsi's paper [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.80.052328 80, 052328 (2009)] as a modification of the usual adiabatic algorithm for a quantum search with the idea that most of the interesting computation only happens over a very short range of the adiabatic path. By focusing on that restricted range, one can potentially gain an advantage by reducing the control requirements on the system, enabling a uniform rate of evolution. In this Comment, we point out an oversight in Tulsi's paper [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.80.052328 80, 052328 (2009)] that invalidates its proof. However, the argument can be corrected, and the calculations in Tulsi's paper [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.80.052328 80, 052328 (2009)] are then sufficient to show that the scheme still works. Nevertheless, subsequent works [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.82.034304 82, 034304 (2010), Chin. Phys. BCPBHAJ1674-105610.1088/1674-1056/20/4/040309 20, 040309 (2011), Chin. Phys. BCPBHAJ1674-105610.1088/1674-1056/21/1/010306 21, 010306 (2012), AASRI Procedia 1, 5862 (2012), and Quantum Inf. Process.10.1007/s11128-013-0557-1 12, 2689 (2013)] cannot all be recovered in the same way.

  19. Waste heat recovery from adiabatic diesel engines by exhaust-driven Brayton cycles

    NASA Technical Reports Server (NTRS)

    Khalifa, H. E.

    1983-01-01

    An evaluation of Bryton Bottoming Systems (BBS) as waste heat recovery devices for future adiabatic diesel engines in heavy duty trucks is presented. Parametric studies were performed to evaluate the influence of external and internal design parameters on BBS performance. Conceptual design and trade-off studies were undertaken to estimate the optimum configuration, size, and cost of major hardware components. The potential annual fuel savings of long-haul trucks equipped with BBS were estimated. The addition of a BBS to a turbocharged, nonaftercooled adiabatic engine would improve fuel economy by as much as 12%. In comparison with an aftercooled, turbocompound engine, the BBS-equipped turbocharged engine would offer a 4.4% fuel economy advantage. If installed in tandem with an aftercooled turbocompound engine, the BBS could effect a 7.2% fuel economy improvement. The cost of a mass-produced 38 Bhp BBS is estimated at about $6460 or 170/Bhp. Technical and economic barriers that hinder the commercial introduction of bottoming systems were identified. Related studies in the area of waste heat recovery from adiabatic diesel engines and NASA-CR-168255 (Steam Rankine) and CR-168256 (Organic Rankine).

  20. Viscous heating, adiabatic heating and energetic consistency in compressible mantle convection

    NASA Astrophysics Data System (ADS)

    Leng, Wei; Zhong, Shijie

    2008-05-01

    Although it has been suggested that the total viscous heating, Qv, should be exactly balanced by the total adiabatic heating, Qa, for compressible mantle convection, previous numerical studies show a significant imbalance of up to several percent between Qv and Qa for simple isoviscous compressible convection. The cause of this imbalance and its potential effects on more complicated convective systems remain largely unknown. In this study, we present an analysis to show that total viscous heating and adiabatic heating for compressible mantle convection with anelastic liquid approximation (ALA) and the Adams-Williamson equation of state are balanced out at any instant in time, and that the previously reported imbalance between Qv and Qa for numerical models with a truncated anelastic liquid approximation (TALA) is caused by neglecting the effect of the pressure on the buoyancy force. Although we only consider the Adams-Williamson equation of state in our analysis, our method can be used to check the energetic consistency for other forms of equation of state. We formulate numerical models of compressible mantle convection under both TALA and ALA formulations by modifying the Uzawa algorithm in Citcom code. Our numerical results confirm our analysis on the balance between total viscous heating and total adiabatic heating.

  1. Adiabatic condition and the quantum hitting time of Markov chains

    SciTech Connect

    Krovi, Hari; Ozols, Maris; Roland, Jeremie

    2010-08-15

    We present an adiabatic quantum algorithm for the abstract problem of searching marked vertices in a graph, or spatial search. Given a random walk (or Markov chain) P on a graph with a set of unknown marked vertices, one can define a related absorbing walk P{sup '} where outgoing transitions from marked vertices are replaced by self-loops. We build a Hamiltonian H(s) from the interpolated Markov chain P(s)=(1-s)P+sP{sup '} and use it in an adiabatic quantum algorithm to drive an initial superposition over all vertices to a superposition over marked vertices. The adiabatic condition implies that, for any reversible Markov chain and any set of marked vertices, the running time of the adiabatic algorithm is given by the square root of the classical hitting time. This algorithm therefore demonstrates a novel connection between the adiabatic condition and the classical notion of hitting time of a random walk. It also significantly extends the scope of previous quantum algorithms for this problem, which could only obtain a full quadratic speedup for state-transitive reversible Markov chains with a unique marked vertex.

  2. Ionization probes of molecular structure and chemistry

    SciTech Connect

    Johnson, P.M.

    1993-12-01

    Various photoionization processes provide very sensitive probes for the detection and understanding of the spectra of molecules relevant to combustion processes. The detection of ionization can be selective by using resonant multiphoton ionization or by exploiting the fact that different molecules have different sets of ionization potentials. Therefore, the structure and dynamics of individual molecules can be studied even in a mixed sample. The authors are continuing to develop methods for the selective spectroscopic detection of molecules by ionization, and to use these methods for the study of some molecules of combustion interest.

  3. Direct Infusion Electrospray Ionization - Ion Mobility - High Resolution Mass Spectrometry (DIESI-IM-HRMS) for Rapid Characterization of Potential Bioprocess Streams

    NASA Astrophysics Data System (ADS)

    Munisamy, Sharon M.; Chambliss, C. Kevin; Becker, Christopher

    2012-07-01

    Direct infusion electrospray ionization - ion mobility - high resolution mass spectrometry (DIESI-IM-HRMS) has been utilized as a rapid technique for the characterization of total molecular composition in "whole-sample" biomass hydrolysates and extracts. IM-HRMS data reveal a broad molecular weight distribution of sample components (up to 1100 m/z) and provide trendline isolation of feedstock components from those introduced "in process." Chemical formulas were obtained from HRMS exact mass measurements (with typical mass error less than 5 ppm) and were consistent with structural carbohydrates and other lignocellulosic degradation products. Analyte assignments are supported via IM-MS collision-cross-section measurements and trendline analysis (e.g., all carbohydrate oligomers identified in a corn stover hydrolysate were found to fall within 6 % of an average trendline). These data represent the first report of collision cross sections for several negatively charged carbohydrates and other acidic species occurring natively in biomass hydrolysates.

  4. The selective Aurora-A kinase inhibitor MLN8237 (alisertib) potently inhibits proliferation of glioblastoma neurosphere tumor stem-like cells and potentiates the effects of temozolomide and ionizing radiation

    PubMed Central

    Hong, Xin; O’Donnell, James P.; Salazar, Clarence R.; Van Brocklyn, James R.; Barnett, Kahlil D.; Pearl, Dennis K.; deCarvalho, Ana C.; Ecsedy, Jeffrey A.; Brown, Stephen L.; Mikkelsen, Tom; Lehman, Norman L.

    2016-01-01

    The selective Aurora-A kinase inhibitor MLN8237 is in clinical trials for hematologic malignancies, ovarian cancer and other solid tumors. We previously showed that MLN8237 is potently antiproliferative toward standard monolayer cultured glioblastoma cells. We have now investigated the effect of MLN8237 with and without temozolomide or ionizing radiation on the proliferation of glioblastoma tumor stem-like cells (neurospheres) using soft agar colony formation assays and normal human astrocytes by MTT assay. Western blotting was utilized to compare MLN8237 IC50s to cellular Aurora-A and phospho-Thr288-Aurora-A levels. MLN8237 was more potently antiproliferative to neurosphere cells than to standard monolayer glioma cells, and was non-toxic to normal human astrocytes. Western blot analysis revealed that MLN8237 treatment inhibits phospho-Thr288-Aurora–A levels providing proof of drug target-hit in glioblastoma cells. Furthermore, phospho-Thr288-Aurora-A levels partially predicted the antiproliferative efficacy of MLN8237. We also found that Aurora-A inhibition by MLN8237 was synergistic with temozolomide and potentiated the effects of ionizing radiation on colony formation in neurosphere glioblastoma tumor stem-like cells. These results further support the potential of Aurora-A inhibitors as primary chemotherapy agents or biological response modifiers in glioblastoma patients. PMID:24627220

  5. Integrated polarization rotator/converter by stimulated Raman adiabatic passage.

    PubMed

    Xiong, Xiao; Zou, Chang-Ling; Ren, Xi-Feng; Guo, Guang-Can

    2013-07-15

    We proposed a polarization rotator inspired by stimulated Raman adiabatic passage model from quantum optics, which is composed of a signal waveguide and an ancillary waveguide. The two orthogonal modes in signal waveguide and the oblique mode in ancillary waveguide form a Λ-type three-level system. By controlling the width of signal waveguide and the gap between two waveguides, adiabatic conversion between two orthogonal modes can be realized in the signal waveguide. With such adiabatic passage, polarization conversion is completed within 150 μm length, with the efficiencies over 99% for both conversions between horizontal polarization and vertical polarization. In addition, such a polarization rotator is quite robust against fabrication error, allowing a wide range of tolerances for the rotator geometric parameters. Our work is not only significative to photonic simulations of coherent quantum phenomena with engineered photonic waveguides, but also enlightens the practical applications of these phenomena in optical device designs. PMID:23938558

  6. Adiabatic compressibility of myoglobin. Effect of axial ligand and denaturation.

    PubMed

    Leung, W P; Cho, K C; Lo, Y M; Choy, C L

    1986-03-01

    An ultrasonic technique has been employed to study the adiabatic compressibility of three metmyoglobin derivatives (aquomet-, fluoromet- and azidometmyoglobin) at neutral pH, and aquometmyoglobin as a function of pH in the frequency range of 1-10 MHz at 20 degrees C. No difference was observed in the adiabatic compressibility of the various derivatives. This indicates that the binding of different axial ligands to myoglobin does not affect significantly the conformational fluctuations of the protein. The finding is consistent with the results of the hydrogen exchange rate experiment, indicating that both types of measurements are useful for the study of protein dynamics. Upon acid-induced denaturation, the adiabatic compressibility of myoglobin drops from 5.3 X 10(-12) cm2/dyn to 0.5 X 10(-12) cm2/dyn. Plausible reasons for such a decrease are discussed. PMID:3947645

  7. Effect of dephasing on stimulated Raman adiabatic passage

    SciTech Connect

    Ivanov, P.A.; Vitanov, N.V.; Bergmann, K.

    2004-12-01

    This work explores the effect of phase relaxation on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The study is based on the Liouville equation, which is solved analytically in the adiabatic limit. The transfer efficiency of STIRAP is found to decrease exponentially with the dephasing rate; this effect is stronger for shorter pulse delays and weaker for larger delays, since the transition time is found to be inversely proportional to the pulse delay. Moreover, it is found that the transfer efficiency of STIRAP in the presence of dephasing does not depend on the peak Rabi frequencies at all, as long as they are sufficiently large to enforce adiabatic evolution; hence increasing the field intensity cannot reduce the dephasing losses. It is shown also that for any dephasing rate, the final populations of the initial state and the intermediate state are equal. For strong dephasing all three populations tend to (1/3)

  8. Adiabatic Quantum Programming: Minor Embedding With Hard Faults

    SciTech Connect

    Klymko, Christine F; Sullivan, Blair D; Humble, Travis S

    2013-01-01

    Adiabatic quantum programming defines the time-dependent mapping of a quantum algorithm into the hardware or logical fabric. An essential programming step is the embedding of problem-specific information into the logical fabric to define the quantum computational transformation. We present algorithms for embedding arbitrary instances of the adiabatic quantum optimization algorithm into a square lattice of specialized unit cells. Our methods are shown to be extensible in fabric growth, linear in time, and quadratic in logical footprint. In addition, we provide methods for accommodating hard faults in the logical fabric without invoking approximations to the original problem. These hard fault-tolerant embedding algorithms are expected to prove useful for benchmarking the adiabatic quantum optimization algorithm on existing quantum logical hardware. We illustrate this versatility through numerical studies of embeddabilty versus hard fault rates in square lattices of complete bipartite unit cells.

  9. Pressure sensitivity of adiabatic shear banding in metals

    NASA Astrophysics Data System (ADS)

    Hanina, E.; Rittel, D.; Rosenberg, Z.

    2007-01-01

    Adiabatic shear banding (ASB) is a dynamic failure mode characterized by large plastic strains in a narrow localized band. ASB occurs at high strain rates (ɛ˙⩾103s-1), under adiabatic conditions leading to a significant temperature rise inside the band [H. Tresca, Annales du Conservatoire des Arts et Métiers 4, (1879); Y. L. Bai and B. Dodd, Adiabatic Shear Localization-Occurrence, Theories, and Applications (Pergamon, Oxford, 1992); M. A. Meyers, Dynamic Behavior of Materials (Wiley, New York, 1994).; and J. J. Lewandowski and L. M. Greer, Nat. Mater. 5, 15 (2006)]. Large hydrostatic pressures are experienced in many dynamic applications involving ASB formation (e.g., ballistic penetration, impact, and machining). The relationship between hydrostatic pressure and ASB development remains an open question, although its importance has been often noted. This letter reports original experimental results indicating a linear relationship between the (normalized) dynamic deformation energy and the (normalized) hydrostatic pressure.

  10. Adiabatic quantum programming: minor embedding with hard faults

    NASA Astrophysics Data System (ADS)

    Klymko, Christine; Sullivan, Blair D.; Humble, Travis S.

    2013-11-01

    Adiabatic quantum programming defines the time-dependent mapping of a quantum algorithm into an underlying hardware or logical fabric. An essential step is embedding problem-specific information into the quantum logical fabric. We present algorithms for embedding arbitrary instances of the adiabatic quantum optimization algorithm into a square lattice of specialized unit cells. These methods extend with fabric growth while scaling linearly in time and quadratically in footprint. We also provide methods for handling hard faults in the logical fabric without invoking approximations to the original problem and illustrate their versatility through numerical studies of embeddability versus fault rates in square lattices of complete bipartite unit cells. The studies show that these algorithms are more resilient to faulty fabrics than naive embedding approaches, a feature which should prove useful in benchmarking the adiabatic quantum optimization algorithm on existing faulty hardware.

  11. Non Adiabatic Evolution of Elliptical Galaxies by Dynamical Friction

    NASA Astrophysics Data System (ADS)

    Arena, S. E.; Bertin, G.; Liseikina, T.; Pegoraro, F.

    2007-05-01

    Many astrophysical problems, ranging from structure formation in cosmology to dynamics of elliptical galaxies, refer to slow processes of evolution of essentially collisionless self-gravitating systems. In order to determine the relevant quasi-equilibrium configuration at time t from given initial conditions, it is often argued that such slow evolution may be approximated in terms of adiabatic evolution, for the calculation of which efficient semi--analytical techniques are available. Here we focus on the slow process of evolution, induced by dynamical friction of a host stellar system on a minority component of "satellites", to determine to what extent an adiabatic description might be applied. The study is realized by means of N--body simulations of the evolution of the total system (the stellar system plus the minority component), in a controlled numerical environment. In particular, we compare the evolution from initial to final configurations of the system subject to dynamical friction with that of the same system evolved adiabatically (in the absence of dynamical friction). We consider two classes of galaxy models characterized by significantly different density and pressure anisotropy profiles. We demonstrate that, for the examined process, the evolution driven by dynamical friction is significantly different from the adiabatic case, not only quantitatively, but also qualitatively. The two classes of galaxy models considered in this investigation exhibit generally similar trends in evolution, with one exception: concentrated models reach a final total density profile, in the internal region, shallower than the initial one, while galaxy models with a broad core show the opposite behaviour. The evolution of elliptical galaxies induced by dynamical friction is a slow process but it is not adiabatic. The results of our investigation should be taken as a warning against the indiscriminate use of adiabatic growth prescriptions in studies of the structure of

  12. Ionization of Atoms by Slow Heavy Particles, Including Dark Matter

    NASA Astrophysics Data System (ADS)

    Roberts, B. M.; Flambaum, V. V.; Gribakin, G. F.

    2016-01-01

    Atoms and molecules can become ionized during the scattering of a slow, heavy particle off a bound electron. Such an interaction involving leptophilic weakly interacting massive particles (WIMPs) is a promising possible explanation for the anomalous 9 σ annual modulation in the DAMA dark matter direct detection experiment [R. Bernabei et al., Eur. Phys. J. C 73, 2648 (2013)]. We demonstrate the applicability of the Born approximation for such an interaction by showing its equivalence to the semiclassical adiabatic treatment of atomic ionization by slow-moving WIMPs. Conventional wisdom has it that the ionization probability for such a process should be exponentially small. We show, however, that due to nonanalytic, cusplike behavior of Coulomb functions close to the nucleus this suppression is removed, leading to an effective atomic structure enhancement. We also show that electron relativistic effects actually give the dominant contribution to such a process, enhancing the differential cross section by up to 1000 times.

  13. Ionization of Atoms by Slow Heavy Particles, Including Dark Matter.

    PubMed

    Roberts, B M; Flambaum, V V; Gribakin, G F

    2016-01-15

    Atoms and molecules can become ionized during the scattering of a slow, heavy particle off a bound electron. Such an interaction involving leptophilic weakly interacting massive particles (WIMPs) is a promising possible explanation for the anomalous 9σ annual modulation in the DAMA dark matter direct detection experiment [R. Bernabei et al., Eur. Phys. J. C 73, 2648 (2013)]. We demonstrate the applicability of the Born approximation for such an interaction by showing its equivalence to the semiclassical adiabatic treatment of atomic ionization by slow-moving WIMPs. Conventional wisdom has it that the ionization probability for such a process should be exponentially small. We show, however, that due to nonanalytic, cusplike behavior of Coulomb functions close to the nucleus this suppression is removed, leading to an effective atomic structure enhancement. We also show that electron relativistic effects actually give the dominant contribution to such a process, enhancing the differential cross section by up to 1000 times. PMID:26824537

  14. Adiabatic invariants, diffusion and acceleration in rigid body dynamics

    NASA Astrophysics Data System (ADS)

    Borisov, Alexey V.; Mamaev, Ivan S.

    2016-03-01

    The onset of adiabatic chaos in rigid body dynamics is considered. A comparison of the analytically calculated diffusion coefficient describing probabilistic effects in the zone of chaos with a numerical experiment is made. An analysis of the splitting of asymptotic surfaces is performed and uncertainty curves are constructed in the Poincaré-Zhukovsky problem. The application of Hamiltonian methods to nonholonomic systems is discussed. New problem statements are given which are related to the destruction of an adiabatic invariant and to the acceleration of the system (Fermi's acceleration).

  15. Adiabatic Rosen-Zener interferometry with ultracold atoms

    SciTech Connect

    Fu Libin; Ye Defa; Lee Chaohong; Zhang Weiping; Liu Jie

    2009-07-15

    We propose a time-domain 'interferometer' based on double-well ultracold atoms through a so-called adiabatic Rosen-Zener process, that is, the barrier between two wells is ramped down slowly, held for a while, and then ramped back. After the adiabatic Rosen-Zener process, we count the particle population in each well. We find that the final occupation probability shows nice interference fringes. The fringe pattern is sensitive to the initial state as well as the intrinsic parameters of the system such as interatomic interaction or energy bias between two wells. The underlying mechanism is revealed and possible applications are discussed.

  16. Speeding up Adiabatic Quantum State Transfer by Using Dressed States

    NASA Astrophysics Data System (ADS)

    Baksic, Alexandre; Ribeiro, Hugo; Clerk, Aashish A.

    2016-06-01

    We develop new pulse schemes to significantly speed up adiabatic state transfer protocols. Our general strategy involves adding corrections to an initial control Hamiltonian that harness nonadiabatic transitions. These corrections define a set of dressed states that the system follows exactly during the state transfer. We apply this approach to stimulated Raman adiabatic passage protocols and show that a suitable choice of dressed states allows one to design fast protocols that do not require additional couplings, while simultaneously minimizing the occupancy of the "intermediate" level.

  17. Gravitational Chern-Simons and the adiabatic limit

    SciTech Connect

    McLellan, Brendan

    2010-12-15

    We compute the gravitational Chern-Simons term explicitly for an adiabatic family of metrics using standard methods in general relativity. We use the fact that our base three-manifold is a quasiregular K-contact manifold heavily in this computation. Our key observation is that this geometric assumption corresponds exactly to a Kaluza-Klein Ansatz for the metric tensor on our three-manifold, which allows us to translate our problem into the language of general relativity. Similar computations have been performed by Guralnik et al.[Ann. Phys. 308, 222 (2008)], although not in the adiabatic context.

  18. Adiabatic fluctuations from cosmic strings in a contracting universe

    SciTech Connect

    Brandenberger, Robert H.; Takahashi, Tomo; Yamaguchi, Masahide E-mail: tomot@cc.saga-u.ac.jp

    2009-07-01

    We show that adiabatic, super-Hubble, and almost scale invariant density fluctuations are produced by cosmic strings in a contracting universe. An essential point is that isocurvature perturbations produced by topological defects such as cosmic strings on super-Hubble scales lead to a source term which seeds the growth of curvature fluctuations on these scales. Once the symmetry has been restored at high temperatures, the isocurvature seeds disappear, and the fluctuations evolve as adiabatic ones in the expanding phase. Thus, cosmic strings may be resurrected as a mechanism for generating the primordial density fluctuations observed today.

  19. Quantum Adiabatic Pumping by Modulating Tunnel Phase in Quantum Dots

    NASA Astrophysics Data System (ADS)

    Taguchi, Masahiko; Nakajima, Satoshi; Kubo, Toshihiro; Tokura, Yasuhiro

    2016-08-01

    In a mesoscopic system, under zero bias voltage, a finite charge is transferred by quantum adiabatic pumping by adiabatically and periodically changing two or more control parameters. We obtained expressions for the pumped charge for a ring of three quantum dots (QDs) by choosing the magnetic flux penetrating the ring as one of the control parameters. We found that the pumped charge shows a steplike behavior with respect to the variance of the flux. The value of the step heights is not universal but depends on the trajectory of the control parameters. We discuss the physical origin of this behavior on the basis of the Fano resonant condition of the ring.

  20. Classical nuclear motion coupled to electronic non-adiabatic transitions

    NASA Astrophysics Data System (ADS)

    Agostini, Federica; Abedi, Ali; Gross, E. K. U.

    2014-12-01

    Based on the exact factorization of the electron-nuclear wave function, we have recently proposed a mixed quantum-classical scheme [A. Abedi, F. Agostini, and E. K. U. Gross, Europhys. Lett. 106, 33001 (2014)] to deal with non-adiabatic processes. Here we present a comprehensive description of the formalism, including the full derivation of the equations of motion. Numerical results are presented for a model system for non-adiabatic charge transfer in order to test the performance of the method and to validate the underlying approximations.