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Sample records for adiabatic bond charge

  1. Lattice Thermal Conductivity of Superlattices from an Adiabatic Bond Charge Model

    NASA Astrophysics Data System (ADS)

    Ward, Alistair; Broido, David

    2007-03-01

    The adiabatic bond charge model (ABCM) has successfully rendered phonon dispersions of a host of bulk semiconductors [1,2] and has also been used to calculate the phonon dispersions in quantum well superlattices [3]. We have developed an ABCM for superlattices and combined it with a symmetry-based representation of the anharmonic interatomic forces to calculate the lattice thermal conductivity of short-period superlattices, using an iterative solution to the Boltzmann-Peierls equation [4]. We compare our ABCM results with those obtained from some commonly used models for the interatomic forces in semiconductors to assess the importance of accurate descriptions of the phonon dispersions in thermal conductivity calculations. [1] W. Weber, Physical Review B 15, 4789 (1977). [2] K. C. Rustagi and W. Weber, Solid State Communications 18, 673 (1976). [3] S. K. Yip and Y. C. Chang, Physical Review B 30 7037 (1984). [4] D. A. Broido, A. Ward, and N. Mingo, Physical Review B 72, 014308 (2005).

  2. [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].

  3. 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.

  4. 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.

  5. Canonical-ensemble state-averaged complete active space self-consistent field (SA-CASSCF) strategy for problems with more diabatic than adiabatic states: Charge-bond resonance in monomethine cyanines

    SciTech Connect

    Olsen, Seth

    2015-01-28

    valence-bond (CASVB) analysis of the charge/bond resonance electronic structure of a monomethine cyanine: Michler’s hydrol blue. The diabatic CASVB representation is shown to vary weakly for “temperatures” corresponding to visible photon energies. Canonical-ensemble SA-CASSCF enables the resolution of energies and couplings for all covalent and ionic CASVB structures contributing to the SA-CASSCF ensemble. The CASVB solution describes resonance of charge- and bond-localized electronic structures interacting via bridge resonance superexchange. The resonance couplings can be separated into channels associated with either covalent charge delocalization or chemical bonding interactions, with the latter significantly stronger than the former.

  6. 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.

  7. The adiabatic motion of charged dust grains in rotating magnetospheres

    NASA Astrophysics Data System (ADS)

    Northrop, T. G.; Hill, J. R.

    1983-01-01

    Adiabatic equations of motion are derived for the micrometer-sized dust grains detected in the Jovian and Saturn magnetospheres by the Pioneer 10 and 11 spacecraft. The adiabatic theory of charged particle motion is extended to the case of variable grain charge. Attention is focused on the innermost and outermost limits to the grain orbit evolution, with all orbits tending to become circular with time. The parameters such as the center equation of motion, the drift velocity, and the parallel equation of motion are obtained for grains in a rotating magnetosphere. Consideration is given to the effects of periodic grain charge-discharge, which are affected by the ambient plasma properties and the grain plasma velocity. The charge-discharge process at the gyrofrequency is determined to eliminate the invariance of the magnetic moment and cause the grain to exhibit radial movement. The magnetic moment increases or decreases as a function of the gyrophase of the charge variation.

  8. Quantum Lattice Fluctuations in the Charge Density Wave State beyond the Adiabatic Approximation

    NASA Astrophysics Data System (ADS)

    Shida, Keisuke; Watanabe, Yuko; Gomi, Hiroki; Takahashi, Akira; Tomita, Norikazu

    2015-12-01

    We have developed a tractable numerical method in which large-amplitude quantum lattice fluctuations can be described beyond the adiabatic approximation using the coherent state representation of phonons. A many-body wave function is constructed by the superposition of direct products of non-orthogonal Slater determinants for electrons and coherent states of phonons. Both orbitals in all the Slater determinants and the amplitudes of all the coherent states are simultaneously optimized. We apply the method to the one-dimensional Su-Schrieffer-Heeger model with the on-site and nearest-neighbor-site Coulomb interactions. It is shown the lattice fluctuations in doped charge density wave (CDW) systems are described by the translational and vibrational motion of lattice solitons. Such lattice solitons induce bond alternation in the doped CDW system while the lattice becomes equidistant in the half-filled CDW system.

  9. [Bond selective chemistry beyond the adiabatic approximation]. Technical progress report, September 15, 1992--June 14, 1993

    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}.

  10. Asymmetry and non-adiabaticity in fragmentation of disulfide bonds upon electron capture.

    PubMed

    Gámez, José A; Serrano-Andrés, Luis; Yáñez, Manuel

    2010-08-23

    Although it has been generally assumed that electron attachment to disulfide derivatives leads to a systematic and significant activation of the S-S bond, we show, by using [CH(3)SSX] (X = CH(3), NH(2), OH, F) derivatives as model compounds, that this is the case only when the X substituents have low electronegativity. Through the use of MP2, QCI and CASPT2 molecular orbital (MO) methods, we elucidate, for the first time, the mechanisms that lead to unimolecular fragmentation of disulfide derivatives after electron attachment. Our theoretical scrutiny indicates that these mechanisms are more intricate than assumed in previous studies. The most stable products, from a thermodynamic viewpoint, correspond to the release of neutral molecules; CH(4), NH(3), H(2)O, and HF. However, the barriers to reach these products depend strongly on the electronegativity of the X substituents. Only for very electronegative substituents, such as OH or F, the loss of H(2)O or HF is the most favorable process, and likely the only one observed. This is possible because of two concomitant factors, 1) the extra electron for [CH(3)SSX](-) (X = OH, F) occupies a sigma*(S-X) MO, which favors the cleavage of the S-X bond, and 2) the activation barriers associated with the hydrogen transfer process to produce H(2)O and HF are rather low. Only when the substituents are less electronegative (X = H, CH(3), NH(2)) the extra electron is located in a sigma*(S-S) orbital and the cleavage of the disulfide bridge becomes the most favorable process. The intimate mechanism associated with the S-S bond dissociation process also depends strongly on the nature of the substituent. For X = H or CH(3) the process is strictly adiabatic, while for X = NH(2) it proceeds through a conical intersection (CI) associated with the charge reorganization necessary to obtain, from a molecular anion with the extra electron delocalized in a sigma*(S-S) antibonding orbital, two fragments with the proper charge localization

  11. 19 CFR 10.39 - Cancellation of bond charges.

    Code of Federal Regulations, 2010 CFR

    2010-04-01

    ... 19 Customs Duties 1 2010-04-01 2010-04-01 false Cancellation of bond charges. 10.39 Section 10.39... Importations Under Bond § 10.39 Cancellation of bond charges. (a) Charges against bonds taken pursuant to... destroyed because of their use for the purposes of importation, the bond charge shall not be canceled...

  12. 19 CFR 10.39 - Cancellation of bond charges.

    Code of Federal Regulations, 2013 CFR

    2013-04-01

    ... 19 Customs Duties 1 2013-04-01 2013-04-01 false Cancellation of bond charges. 10.39 Section 10.39... Importations Under Bond § 10.39 Cancellation of bond charges. (a) Charges against bonds taken pursuant to... destroyed because of their use for the purposes of importation, the bond charge shall not be canceled...

  13. 19 CFR 10.39 - Cancellation of bond charges.

    Code of Federal Regulations, 2012 CFR

    2012-04-01

    ... 19 Customs Duties 1 2012-04-01 2012-04-01 false Cancellation of bond charges. 10.39 Section 10.39... Importations Under Bond § 10.39 Cancellation of bond charges. (a) Charges against bonds taken pursuant to... destroyed because of their use for the purposes of importation, the bond charge shall not be canceled...

  14. Charge-Assisted Hydrogen-Bonded Networks

    NASA Astrophysics Data System (ADS)

    Ward, Michael D.

    The importance of hydrogen bonds is widely recognized because of their role in defining the structure and properties of many compounds, including water, proteins, DNA, and polymers. Hydrogen bonding also has emerged as a critical tool in solid-state chemistry, in which the versatility of organic synthesis has been combined with the structure-directing properties of hydrogen-bond donor-acceptor pairs to steer molecular assembly into networks that reflect the symmetries of their molecular constituents. Although these efforts have been largely empirical, the dominance of hydrogen bonding among the multitude of intermolecular forces often leads to predictable control of crystal structure. Although charge-assisted hydrogen bonds (donors and acceptors with ionic character that reinforce the electrostatic character of the hydrogen bond) have been recognized for decades, their use in network design, particularly for “crystal engineering,” has grown substantially in the past decade. The evidence suggests that charge-assisted hydrogen bonds introduce extraordinary robustness to molecular networks that reflects a combination of strong intermolecular forces and structural compliance, thus facilitating design of organic solid-state materials.

  15. Design and fabrication of adiabatic vertical couplers for hybrid integration by flip-chip bonding

    NASA Astrophysics Data System (ADS)

    Mu, Jinfeng; Sefunc, Mustafa A.; Xu, Bojian; Dijkstra, Meindert; García-Blanco, Sonia M.

    2016-02-01

    Rare-earth ion doped crystalline potassium double tungstates, such as KY(WO4)2, KLu(WO4)2 and KY(WO4)2, exhibit many properties that make them promising candidates for the realization of lasers and amplifiers in integrated photonics. One of the key challenges for the hybrid integration of different photonic platforms remains the design and fabrication of low-loss and fabrication tolerant couplers for transferring light between different waveguides. In this paper, adiabatic vertical couplers realized by flip-chip bonding of polymer waveguides to Si3N4 devices are designed, fabricated and tested. An efficient design flow combining 2D and 3D simulations was proposed and its validity was demonstrated. The vertical couplers will ultimately be used for the integration of erbium doped KY(WO4)2 waveguides with passive platforms. The designed couplers exhibit less than 0.5 dB losses at adiabatic angles and below 1 dB loss for ±0.5 μm lateral misalignment. The fabricated vertical couplers show less than 1dB losses in average for different adiabatic angles of Si3N4 tapers, which is in good quantitative agreement with the simulations.

  16. 19 CFR 10.39 - Cancellation of bond charges.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... Note: For Federal Register citations affecting § 10.39, see the List of CFR Sections Affected, which... 19 Customs Duties 1 2011-04-01 2011-04-01 false Cancellation of bond charges. 10.39 Section 10.39... Importations Under Bond § 10.39 Cancellation of bond charges. (a) Charges against bonds taken pursuant...

  17. CLASSICAL TRAJECTORY MODELS FOR ELECTRONICALLY NON-ADIABATIC COLLISION PROCESSES: A CLASSICAL VALENCE BOND MODEL FOR ELECTRONIC DEGREES OF FREEDOM

    SciTech Connect

    Miller, William H.; Orel, Ann E.

    1980-11-01

    A classical interpretation of the Dirac-Van Vleck spin version of valence bond theory is used to obtain a classical model for electronic degrees of freedom within the valence bond framework. The approach is illustrated by deriving the explicit forms of the classical Hamiltonians, involving electronic and heavy particle degrees of freedom, for the H-H{sub 2}, F-H{sub 2} , and O-H{sub 2} systems. It is also shown how the initial conditions for both electronic and heavy particle degrees of freedom are chosen to carry out a classical trajectory simulation of collision processes. The attractive feature of this model is that it is as eaaily applicable to electronically non-adiabatic processes as it is to adiabatic ones.

  18. Vibrational coherences in charge-transfer dyes: A non-adiabatic picture

    SciTech Connect

    Sissa, Cristina; Delchiaro, Francesca; Di Maiolo, Francesco

    2014-10-28

    Essential-state models efficiently describe linear and nonlinear spectral properties of different families of charge-transfer chromophores. Here, the essential-state machinery is applied to the calculation of the early-stage dynamics after ultrafast (coherent) excitation of polar and quadrupolar chromophores. The fully non-adiabatic treatment of coupled electronic and vibrational motion allows for a reliable description of the dynamics of these intriguing systems. In particular, the proposed approach is reliable even when the adiabatic and harmonic approximations do not apply, such as for quadrupolar dyes that show a multistable, broken-symmetry excited state. Our approach quite naturally leads to a clear picture for a dynamical Jahn-Teller effect in these systems. The recovery of symmetry due to dynamical effects is however disrupted in polar solvents where a static symmetry lowering is observed. More generally, thermal disorder in polar solvents is responsible for dephasing phenomena, damping the coherent oscillations with particularly important effects in the case of polar dyes.

  19. Vibrational coherences in charge-transfer dyes: A non-adiabatic picture

    NASA Astrophysics Data System (ADS)

    Sissa, Cristina; Delchiaro, Francesca; Di Maiolo, Francesco; Terenziani, Francesca; Painelli, Anna

    2014-10-01

    Essential-state models efficiently describe linear and nonlinear spectral properties of different families of charge-transfer chromophores. Here, the essential-state machinery is applied to the calculation of the early-stage dynamics after ultrafast (coherent) excitation of polar and quadrupolar chromophores. The fully non-adiabatic treatment of coupled electronic and vibrational motion allows for a reliable description of the dynamics of these intriguing systems. In particular, the proposed approach is reliable even when the adiabatic and harmonic approximations do not apply, such as for quadrupolar dyes that show a multistable, broken-symmetry excited state. Our approach quite naturally leads to a clear picture for a dynamical Jahn-Teller effect in these systems. The recovery of symmetry due to dynamical effects is however disrupted in polar solvents where a static symmetry lowering is observed. More generally, thermal disorder in polar solvents is responsible for dephasing phenomena, damping the coherent oscillations with particularly important effects in the case of polar dyes.

  20. 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

  1. The exact forces on classical nuclei in non-adiabatic charge transfer.

    PubMed

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

    2015-02-28

    The decomposition of electronic and nuclear motion presented in Abedi et al. [Phys. Rev. Lett. 105, 123002 (2010)] yields a time-dependent potential that drives the nuclear motion and fully accounts for the coupling to the electronic subsystem. Here, we show that propagation of an ensemble of independent classical nuclear trajectories on this exact potential yields dynamics that are essentially indistinguishable from the exact quantum dynamics for a model non-adiabatic charge transfer problem. We point out the importance of step and bump features in the exact potential that are critical in obtaining the correct splitting of the quasiclassical nuclear wave packet in space after it passes through an avoided crossing between two Born-Oppenheimer surfaces and analyze their structure. Finally, an analysis of the exact potentials in the context of trajectory surface hopping is presented, including preliminary investigations of velocity-adjustment and the force-induced decoherence effect. PMID:25725727

  2. The exact forces on classical nuclei in non-adiabatic charge transfer

    SciTech Connect

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

    2015-02-28

    The decomposition of electronic and nuclear motion presented in Abedi et al. [Phys. Rev. Lett. 105, 123002 (2010)] yields a time-dependent potential that drives the nuclear motion and fully accounts for the coupling to the electronic subsystem. Here, we show that propagation of an ensemble of independent classical nuclear trajectories on this exact potential yields dynamics that are essentially indistinguishable from the exact quantum dynamics for a model non-adiabatic charge transfer problem. We point out the importance of step and bump features in the exact potential that are critical in obtaining the correct splitting of the quasiclassical nuclear wave packet in space after it passes through an avoided crossing between two Born-Oppenheimer surfaces and analyze their structure. Finally, an analysis of the exact potentials in the context of trajectory surface hopping is presented, including preliminary investigations of velocity-adjustment and the force-induced decoherence effect.

  3. The exact forces on classical nuclei in non-adiabatic charge transfer

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

    The decomposition of electronic and nuclear motion presented in Abedi et al. [Phys. Rev. Lett. 105, 123002 (2010)] yields a time-dependent potential that drives the nuclear motion and fully accounts for the coupling to the electronic subsystem. Here, we show that propagation of an ensemble of independent classical nuclear trajectories on this exact potential yields dynamics that are essentially indistinguishable from the exact quantum dynamics for a model non-adiabatic charge transfer problem. We point out the importance of step and bump features in the exact potential that are critical in obtaining the correct splitting of the quasiclassical nuclear wave packet in space after it passes through an avoided crossing between two Born-Oppenheimer surfaces and analyze their structure. Finally, an analysis of the exact potentials in the context of trajectory surface hopping is presented, including preliminary investigations of velocity-adjustment and the force-induced decoherence effect.

  4. The effect of adiabatic focusing upon charged particle propagation in random magnetic fields

    NASA Technical Reports Server (NTRS)

    Earl, J. A.

    1975-01-01

    Charged particles propagating along the diverging lines of force of a spatially inhomogeneous guiding field were considered as they are scattered by random fields. Their longitudinal transport is described in terms of the eigenfunctions of a Sturm-Liouville operator incorporating the effect of adiabatic focussing along with that of scattering. The relaxation times and characteristic velocities are graphed and tabulated. The particle density is evaluated as a function of space and time for two different regimes. In the first regime (relatively weak focussing), a diffusive mode of propagation is dominant but coherent modes are also dominant. In the second regime (strong focussing), diffusion does not occur and the propagation is purely coherent. This supercoherent mode corresponds exactly to the so-called scatter-free propagation of kilovolt solar flare electrons. On a larger scale, focussed transport provides an interpretation of many observed characteristics of extragalactic radio sources.

  5. Characterization of intramolecular hydrogen bonds by atomic charges and charge fluxes.

    PubMed

    Baranović, Goran; Biliškov, Nikola; Vojta, Danijela

    2012-08-16

    The electronic charge redistribution and the infrared intensities of the two types of intramolecular hydrogen bonds, O-H···O and O-H···π, of o-hydroxy- and o-ethynylphenol, respectively, together with a set of related intermolecular hydrogen bond complexes are described in terms of atomic charges and charge fluxes derived from atomic polar tensors calculated at the B3LYP/cc-pVTZ level of theory. The polarizable continuum model shows that both the atomic charges and charge fluxes are strongly dependent on solvent. It is shown that their values for the OH bond in an intramolecular hydrogen bond are not much different from those for the "free" OH bond, but the changes are toward the values found for an intermolecular hydrogen bond. The intermolecular hydrogen bond is characterized not only by the decreased atomic charge but also by the enlarged charge flux term of the same sign producing thus an enormous increase in IR intensity. The overall behavior of the charges and fluxes of the hydrogen atom in OH and ≡CH bonds agree well with the observed spectroscopic characteristics of inter- and intramolecular hydrogen bonding. The main reason for the differences between the two types of the hydrogen bond lies in the molecular structure because favorable linear proton donor-acceptor arrangement is not possible to achieve within a small molecule. The calculated intensities (in vacuo and in polarizable continuum) are only in qualitative agreement with the measured data. PMID:22809455

  6. Modern ab initio valence bond theory calculations reveal charge shift bonding in protic ionic liquids.

    PubMed

    Patil, Amol Baliram; Bhanage, Bhalchandra Mahadeo

    2016-06-21

    The nature of bonding interactions between the cation and the anion of an ionic liquid is at the heart of understanding ionic liquid properties. A particularly interesting case is a special class of ionic liquids known as protic ionic liquids. The extent of proton transfer in protic ionic liquids has been observed to vary according to the interacting species. Back proton transfer renders protic ionic liquids volatile and to be considered as inferior ionic liquids. We try to address this issue by employing modern ab initio valence bond theory calculations. The results indicate that the bonding in the cation and the anion of a prototypical ionic liquid, ethylammonium nitrate, is fundamentally different. It is neither characteristic of covalent/polar covalent bonding nor ionic bonding but rather charge shift bonding as a resonance hybrid of two competing ionic molecular electronic structure configurations. An investigation of other analogous protic ionic liquids reveals that this charge shift bonding seems to be a typical characteristic of protic ionic liquids while the ionic solid analogue compound ammonium nitrate has less charge shift bonding character as compared to protic ionic liquids. Further the extent of charge shift bonding character has been found to be congruent with the trends in many physicochemical properties such as melting point, conductivity, viscosity, and ionicity of the studied ionic liquids indicating that percentage charge shift character may serve as a key descriptor for large scale computational screening of ionic liquids with desired properties. PMID:27229870

  7. The anomalous Floquet-Anderson insulator as a non-adiabatic quantized charge pump

    NASA Astrophysics Data System (ADS)

    Titum, Paraj; Berg, Erez; Rudner, Mark S.; Refael, Gil; Lindner, Netanel H.

    Periodically driven quantum systems provide a novel and versatile platform for realizing topological phenomena. Among these are analogs of topological insulators and superconductors, attainable in static systems; however, some of these phenomena are unique to the periodically driven case. Here, we show that disordered, periodically driven systems admit an ``anomalous'' two dimensional phase, whose quasi-energy spectrum consists of chiral edge modes that coexist with a fully localized bulk - an impossibility for static Hamiltonians. This unique situation serves as the basis for a new topologically-protected non-equilibrium transport phenomenon: quantized non-adiabatic charge pumping. We identify the bulk topological invariant that characterizes the new phase (which we call the ``anomalous Floquet Anderson Insulator'', or AFAI). We provide explicit models which constitute a proof of principle for the existence of the new phase. Finally, we present evidence that the disorder-driven transition from the AFAI to a trivial, fully localized phase is in the same universality class as the quantum Hall plateau transition.

  8. Multidirectional Angular Electronic Flux during Adiabatic Attosecond Charge Migration in Excited Benzene.

    PubMed

    Hermann, Gunter; Liu, ChunMei; Manz, Jörn; Paulus, Beate; Pérez-Torres, Jhon Fredy; Pohl, Vincent; Tremblay, Jean Christophe

    2016-07-14

    Recently, adiabatic attosecond charge migration (AACM) has been monitored and simulated for the first time, with application to the oriented iodoacetylene cation where AACM starts from the initial superposition of the ground state (φ0) and an electronic excited state (φ1). Here, we develop the theory for electronic fluxes during AACM in ring-shaped molecules, with application to oriented benzene prepared in the superposition of the ground and first excited singlet states. The initial state and its time evolution are analogous to coherent tunneling where φ0 and φ1 have different meanings; however, they denote the wave functions of the lowest tunneling doublet. This analogy suggests to transfer the theory of electronic fluxes during coherent tunneling to AACM, with suitable modifications which account for (i) the different time scales and (ii) the different electronic states, and which make use of (iii) the preparation of the initial state for AACM by a linearly polarized laser pulse. Application to benzene yields the multidirectional angular electronic flux with a pincer-motion type pattern during AACM: this unequivocal result confirms a previous working hypothesis. Moreover, the theory of AACM allows quantification of the electronic flux; that is, the maximum number of electrons (out of 42) which flow concertedly during AACM in benzene is 6 × 0.08 = 0.48. PMID:27046151

  9. 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

  10. Infrared intensities and charge mobility in hydrogen bonded complexes

    NASA Astrophysics Data System (ADS)

    Galimberti, Daria; Milani, Alberto; Castiglioni, Chiara

    2013-08-01

    The analytical model for the study of charge mobility in the molecules presented by Galimberti et al. [J. Chem. Phys. 138, 164115 (2013)] is applied to hydrogen bonded planar dimers. Atomic charges and charge fluxes are obtained from density functional theory computed atomic polar tensors and related first derivatives, thus providing an interpretation of the IR intensity enhancement of the X-H stretching band observed upon aggregation. Our results show that both principal and non-principal charge fluxes have an important role for the rationalization of the spectral behavior; moreover, they demonstrate that the modulation of the charge distribution during vibrational motions of the -XH⋯Y- fragment is not localized exclusively on the atoms directly involved in hydrogen bonding. With these premises we made some correlations between IR intensities, interaction energies, and charge fluxes. The model was tested on small dimers and subsequently to the bigger one cytosine-guanine. Thus, the model can be applied to complex systems.

  11. Charge exchange transition probability for collisions between unlike ions and atoms within the adiabatic approximation

    NASA Technical Reports Server (NTRS)

    Xu, Y. J.; Khandelwal, G. S.; Wilson, John W.

    1989-01-01

    A simple formula for the transition probability for electron exchange between unlike ions and atoms is established within the adiabatic approximation by employing the Linear Combination of Atomic Orbitals (LCAO) method. The formula also involves an adiabatic parameter, introduced by Massey, and thus the difficulties arising from the internal energy defect and the adiabatic approximation are avoided. Specific reactions Li(+++) + H to Li(++) + H(+) and Be(4+) + H to Be(3+) + H(+) are considered as examples. The calculated capture cross section results of the present work are compared with the experimental data and with the calculation of other authors over the velocity range of 10(7) cm/sec to 10(8) cm/sec.

  12. Non-adiabatic quantized charge pumping with tunable-barrier quantum dots: a review of current progress.

    PubMed

    Kaestner, Bernd; Kashcheyevs, Vyacheslavs

    2015-10-01

    Precise manipulation of individual charge carriers in nanoelectronic circuits underpins practical applications of their most basic quantum property--the universality and invariance of the elementary charge. A charge pump generates a net current from periodic external modulation of parameters controlling a nanostructure connected to source and drain leads; in the regime of quantized pumping the current varies in steps of [Formula: see text] as function of control parameters, where [Formula: see text] is the electron charge and f is the frequency of modulation. In recent years, robust and accurate quantized charge pumps have been developed based on semiconductor quantum dots with tunable tunnel barriers. These devices allow modulation of charge exchange rates between the dot and the leads over many orders of magnitude and enable trapping of a precise number of electrons far away from equilibrium with the leads. The corresponding non-adiabatic pumping protocols focus on understanding of separate parts of the pumping cycle associated with charge loading, capture and release. In this report we review realizations, models and metrology applications of quantized charge pumps based on tunable-barrier quantum dots. PMID:26394066

  13. Non-adiabatic quantized charge pumping with tunable-barrier quantum dots: a review of current progress

    NASA Astrophysics Data System (ADS)

    Kaestner, Bernd; Kashcheyevs, Vyacheslavs

    2015-10-01

    Precise manipulation of individual charge carriers in nanoelectronic circuits underpins practical applications of their most basic quantum property—the universality and invariance of the elementary charge. A charge pump generates a net current from periodic external modulation of parameters controlling a nanostructure connected to source and drain leads; in the regime of quantized pumping the current varies in steps of {{q}\\text{e}} f as function of control parameters, where {{q}\\text{e}} is the electron charge and f is the frequency of modulation. In recent years, robust and accurate quantized charge pumps have been developed based on semiconductor quantum dots with tunable tunnel barriers. These devices allow modulation of charge exchange rates between the dot and the leads over many orders of magnitude and enable trapping of a precise number of electrons far away from equilibrium with the leads. The corresponding non-adiabatic pumping protocols focus on understanding of separate parts of the pumping cycle associated with charge loading, capture and release. In this report we review realizations, models and metrology applications of quantized charge pumps based on tunable-barrier quantum dots.

  14. Non-adiabatic processes in the charge transfer reaction of O2 molecules with potassium surfaces without dissociation

    NASA Astrophysics Data System (ADS)

    Krix, David; Nienhaus, Hermann

    2014-08-01

    Thin potassium films grown on Si(001) substrates are used to measure internal chemicurrents and the external emission of exoelectrons simultaneously during adsorption of molecular oxygen on K surfaces at 120 K. The experiments clarify the dynamics of electronic excitations at a simple metal with a narrow valence band. X-ray photoemission reveals that for exposures below 5 L almost exclusively peroxide K2O2 is formed, i.e., no dissociation of the molecule occurs during interaction. Still a significant chemicurrent and a delayed exoelectron emission are detected due to a rapid injection of unoccupied molecular levels below the Fermi level. Since the valence band width of potassium is approximately equal to the potassium work function (2.4 eV) the underlying mechanism of exoemission is an Auger relaxation whereas chemicurrents are detected after resonant charge transfer from the metal valence band into the injected level. The change of the chemicurrent and exoemission efficiencies with oxygen coverage can be deduced from the kinetics of the reaction and the recorded internal and external emission currents traces. It is shown that the non-adiabaticity of the reaction increases with coverage due to a reduction of the electronic density of states at the surface while the work function does not vary significantly. Therefore, the peroxide formation is one of the first reaction systems which exhibits varying non-adiabaticity and efficiencies during the reaction. Non-adiabatic calculations based on model Hamiltonians and density functional theory support the picture of chemicurrent generation and explain the rapid injection of hot hole states by an intramolecular motion, i.e., the expansion of the oxygen molecule on the timescale of a quarter of a vibrational period.

  15. Non-adiabatic processes in the charge transfer reaction of O2 molecules with potassium surfaces without dissociation.

    PubMed

    Krix, David; Nienhaus, Hermann

    2014-08-21

    Thin potassium films grown on Si(001) substrates are used to measure internal chemicurrents and the external emission of exoelectrons simultaneously during adsorption of molecular oxygen on K surfaces at 120 K. The experiments clarify the dynamics of electronic excitations at a simple metal with a narrow valence band. X-ray photoemission reveals that for exposures below 5 L almost exclusively peroxide K2O2 is formed, i.e., no dissociation of the molecule occurs during interaction. Still a significant chemicurrent and a delayed exoelectron emission are detected due to a rapid injection of unoccupied molecular levels below the Fermi level. Since the valence band width of potassium is approximately equal to the potassium work function (2.4 eV) the underlying mechanism of exoemission is an Auger relaxation whereas chemicurrents are detected after resonant charge transfer from the metal valence band into the injected level. The change of the chemicurrent and exoemission efficiencies with oxygen coverage can be deduced from the kinetics of the reaction and the recorded internal and external emission currents traces. It is shown that the non-adiabaticity of the reaction increases with coverage due to a reduction of the electronic density of states at the surface while the work function does not vary significantly. Therefore, the peroxide formation is one of the first reaction systems which exhibits varying non-adiabaticity and efficiencies during the reaction. Non-adiabatic calculations based on model Hamiltonians and density functional theory support the picture of chemicurrent generation and explain the rapid injection of hot hole states by an intramolecular motion, i.e., the expansion of the oxygen molecule on the timescale of a quarter of a vibrational period. PMID:25149810

  16. Non-adiabatic processes in the charge transfer reaction of O{sub 2} molecules with potassium surfaces without dissociation

    SciTech Connect

    Krix, David; Nienhaus, Hermann

    2014-08-21

    Thin potassium films grown on Si(001) substrates are used to measure internal chemicurrents and the external emission of exoelectrons simultaneously during adsorption of molecular oxygen on K surfaces at 120 K. The experiments clarify the dynamics of electronic excitations at a simple metal with a narrow valence band. X-ray photoemission reveals that for exposures below 5 L almost exclusively peroxide K{sub 2}O{sub 2} is formed, i.e., no dissociation of the molecule occurs during interaction. Still a significant chemicurrent and a delayed exoelectron emission are detected due to a rapid injection of unoccupied molecular levels below the Fermi level. Since the valence band width of potassium is approximately equal to the potassium work function (2.4 eV) the underlying mechanism of exoemission is an Auger relaxation whereas chemicurrents are detected after resonant charge transfer from the metal valence band into the injected level. The change of the chemicurrent and exoemission efficiencies with oxygen coverage can be deduced from the kinetics of the reaction and the recorded internal and external emission currents traces. It is shown that the non-adiabaticity of the reaction increases with coverage due to a reduction of the electronic density of states at the surface while the work function does not vary significantly. Therefore, the peroxide formation is one of the first reaction systems which exhibits varying non-adiabaticity and efficiencies during the reaction. Non-adiabatic calculations based on model Hamiltonians and density functional theory support the picture of chemicurrent generation and explain the rapid injection of hot hole states by an intramolecular motion, i.e., the expansion of the oxygen molecule on the timescale of a quarter of a vibrational period.

  17. Breaking of the first adiabatic invariants of charged particles in time-dependent magnetic fields - Computer simulations and theory

    NASA Technical Reports Server (NTRS)

    Borovsky, Joseph E.; Hansen, Paul J.

    1991-01-01

    The mechanics of the first adiabatic invariant mu of nonrelativistic charged particles in time-dependent magnetic inductions B (t) are studied by means of computer simulations and analytic theory. Linear-ramp magnetic-induction profiles are utilized, as well as hyperbolic-tangent ramps and sine half-wave ramps. The change in mu that results from an induction change Delta B that occurs over a time Delta t is quantified for all values of Delta B and Delta t, as well as for all values of the particle position. It is found that the cases fall into two categories with very different mu behavior: cases in which the change in the magnetic induction occurs over a time Delta t that is exactly equal to an integer number of gyroperiods (textbook case) or cases in which the change in the induction occurs over a time Delta t that is not equal to an integer number of gyroperiods (more general case). In both categories mu is an adiabatic invariant, although the conservation of mu is much poorer in the latter category.

  18. Effect of charge density of bonding agent containing a new quaternary ammonium methacrylate on antibacterial and bonding properties

    PubMed Central

    Li, Fang; Weir, Michael D.; Chen, Jihua; Xu, Hockin H. K.

    2014-01-01

    Objectives Quaternary amine charge density is important because when the negatively-charged bacteria contact the positive quaternary amine charge, the electric balance is disturbed and the bacterium could be disrupted. There has been no report on the effects of charge density on the antibacterial efficacy of dental bonding agents. The objective of this study was to synthesize a new quaternary ammonium methacrylate, and investigate the effects of charge density of bonding agent on bacteria early-attachment, biofilm colony-forming units (CFU) and dentin bond strength. Methods Dimethylaminododecyl methacrylate (DMAHDM) with an alkyl chain length of 16 was synthesized and mixed into Scotchbond Multi-Purpose adhesive and primer (SBMP) at mass fractions of 0%, 2.5%, 5%, 7.5%, and 10%. A microtensile dentin bond test was performed. The density of quaternary ammonium groups was measured using a fluorescein dye method. Streptococcus mutans (S. mutans) early-attachment was examined at 4 hours, and biofilm colony-forming units (CFU) were measured at 2 days. Results All groups had similar microtensile bonding strengths (mean ± sd; n = 40) of about 60 MPa (p > 0.1). Quaternary amine charge density of bonding agents monotonically increased with increasing DMAHDM mass fraction. Bacteria early-attachment coverage greatly decreased with increasing DMAHDM content in the resin. Biofilm CFU at 10% DMAHDM was reduced by almost 5 log, compared to SBMP control. Charge density of bonding agent was inversely proportional to bacteria early-attachment coverage and biofilm CFU. Significance Increasing the quaternary amine charge density of dentin bonding agent resin was shown to greatly reduce S. mutans attachment and decrease biofilm CFU by four orders of magnitude, without compromising the dentin bond strength. The new DMAHDM is promising for use in bonding agents and other antibacterial restorative materials to inhibit caries. PMID:24534376

  19. Fission fragment charge and mass distributions in 239Pu(n ,f ) in the adiabatic nuclear energy density functional theory

    NASA Astrophysics Data System (ADS)

    Regnier, D.; Dubray, N.; Schunck, N.; Verrière, M.

    2016-05-01

    Background: Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics. Purpose: In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear density functional theory (DFT). Methods: Our theoretical framework is the nuclear energy density functional (EDF) method, where large-amplitude collective motion is treated adiabatically by using the time-dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). In practice, the TDGCM is implemented in two steps. First, a series of constrained EDF calculations map the configuration and potential-energy landscape of the fissioning system for a small set of collective variables (in this work, the axial quadrupole and octupole moments of the nucleus). Then, nuclear dynamics is modeled by propagating a collective wave packet on the potential-energy surface. Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. Results: We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in two-dimensional collective spaces. Theory and experiment agree typically within two mass units for the position of the asymmetric peak. As expected, calculations are sensitive to the structure of the initial state and the prescription for the collective inertia. We emphasize that results are also sensitive to the continuity of the collective landscape near scission. Conclusions: Our analysis confirms

  20. Intramolecular Charge-Assisted Hydrogen Bond Strength in Pseudochair Carboxyphosphate

    PubMed Central

    2015-01-01

    Carboxyphosphate, a suspected intermediate in ATP-dependent carboxylases, has not been isolated nor observed directly by experiment. Consequently, little is known concerning its structure, stability, and ionization state. Recently, carboxyphosphate as either a monoanion or dianion has been shown computationally to adopt a novel pseudochair conformation featuring an intramolecular charge-assisted hydrogen bond (CAHB). In this work, additive and subtractive correction schemes to the commonly employed open–closed method are used to estimate the strength of the CAHB. Truhlar’s Minnesota M06-2X functional with Dunning’s aug-cc-pVTZ basis set has been used for geometry optimization, energy evaluation, and frequency analysis. The CHARMM force field has been used to approximate the Pauli repulsive terms in the closed and open forms of carboxyphosphate. From our additive correction scheme, differential Pauli repulsion contributions between the pseudochair (closed) and open conformations of carboxyphosphate are found to be significant in determining the CAHB strength. The additive correction modifies the CAHB prediction (ΔEclosed–open) of −14 kcal/mol for the monoanion and −12 kcal/mol for the dianion to −22.9 and −18.4 kcal/mol, respectively. Results from the subtractive technique reinforce those from our additive procedure, where the predicted CAHB strength ranges from −17.8 to −25.4 kcal/mol for the monoanion and from −15.7 to −20.9 kcal/mol for the dianion. Ultimately, we find that the CAHB in carboxyphosphate meets the criteria for short-strong hydrogen bonds. However, carboxyphosphate has a unique energy profile that does not result in the symmetric double-well behavior of low-barrier hydrogen bonds. These findings provide deeper insight into the pseudochair conformation of carboxyphosphate, and lead to an improved mechanistic understanding of this intermediate in ATP-dependent carboxylases. PMID:25405523

  1. Adiabatic description of capture into resonance and surfatron acceleration of charged particles by electromagnetic waves.

    PubMed

    Artemyev, A V; Neishtadt, A I; Zelenyi, L M; Vainchtein, D L

    2010-12-01

    We present an analytical and numerical study of the surfatron acceleration of nonrelativistic charged particles by electromagnetic waves. The acceleration is caused by capture of particles into resonance with one of the waves. We investigate capture for systems with one or two waves and provide conditions under which the obtained results can be applied to systems with more than two waves. In the case of a single wave, the once captured particles never leave the resonance and their velocity grows linearly with time. However, if there are two waves in the system, the upper bound of the energy gain may exist and we find the analytical value of that bound. We discuss several generalizations including the relativistic limit, different wave amplitudes, and a wide range of the waves' wavenumbers. The obtained results are used for qualitative description of some phenomena observed in the Earth's magnetosphere. PMID:21198098

  2. Intramolecular resonance-assisted hydrogen bonds: A theoretical description by means of atomic charges and charge fluxes

    NASA Astrophysics Data System (ADS)

    Baranović, Goran

    2014-01-01

    The characterization of intramolecular H-bonds in terms of atomic charges and charge fluxes (at the B3LYP/cc-pVTZ level of theory) has been extended to the case of the so called resonance-assisted (RA) H-bonds. A quadratic correlation between the charge fluxes ϕH and the molecular IR absorption coefficients E that includes the entire family of the studied systems (31 of them) containing both intra- and intermolecular hydrogen bonds (O-H⋯O/N) confirmed the critical importance of the charge fluxes on the IR intensity enhancements. Since they reflect changing of the atomic charge distribution during the normal modes of vibrations, the dynamic nature of hydrogen bonding properties has been re-emphasized. The changes of the charge flux of the hydroxyl hydrogen in an RA intramolecular H-bond are between those for “free” OH bonds and the values calculated for intermolecular H-bonds. The transition “free” → intramolecular → intermolecular is gradual and therefore the hydrogen charge flux can be considered as practically sufficient to give quantitative measure to the intuitively obvious statement that “intramolecular H-bonding is somehow in between no H-bonding situation and intermolecular H-bonding” and thus provide a quantitative and yet simple parameterization of H-bond strength. In strictly planar molecules, the difference of the sums of charges of atoms participating in the 6-membered H-bond ring ΔΣ can serve as a measure of the charge delocalization after the H-bond is formed. The electronic charge is withdrawn from the group of six atoms when the H-bond is formed in nitrophenol (ΔΣ = -0.07), while the opposite is true (ΔΣ = +0.03) for 2-hydroxy benzylidene amine. The corresponding values of the geometrical resonance parameter Δ are 0.39 and 0.37, respectively, similar to those found for 2-hydroxy acetophenone and 2-hydroxy benzaldehyde. The extent of the π-electron delocalization as measured by the resonance parameter Δ does not follow

  3. Adiabatic calorimetry test of the reaction kinetics and self-heating model for 18650 Li-ion cells in various states of charge

    NASA Astrophysics Data System (ADS)

    Chen, Wei-Chun; Wang, Yih-Wen; Shu, Chi-Min

    2016-06-01

    Use of adiabatic calorimetry to characterise thermal runaway of Li-ion cells is a crucial technique in battery safety testing. Various states of charge (SoC) of Li-ion cells were investigated to ascertain their thermal runaway features using a Vent Sizing Package 2 (VSP2) adiabatic calorimeter. To evaluate the thermal runaway characteristics, the temperature-pressure-time trajectories of commercial cylindrical cells were tested, and it was found that cells at a SoC of greater than 50% were subject to thermal explosion at elevated temperatures. Calorimetry data from various 18650 Li-ion cells with different SoC were used to calculate the thermal explosion energies and chemical kinetics; furthermore, a novel self-heating model based on a pseudo-zero-order reaction that follows the Arrhenius equation was found to be applicable for studying the exothermic reaction of a charged cell.

  4. Connecting a new non-adiabatic vibrational mass to the bonding mechanism of LiH: A quantum superposition of ionic and covalent states

    NASA Astrophysics Data System (ADS)

    Diniz, Leonardo G.; Alijah, Alexander; Adamowicz, Ludwik; Mohallem, José R.

    2015-07-01

    Non-adiabatic vibrational calculations performed with the accuracy of 0.2 cm-1 spanning the whole energy spectrum up to the dissociation limit for 7LiH are reported. A so far unknown v = 23 energy level is predicted. The key feature of the approach used in the calculations is a valence-bond (VB) based procedure for determining the effective masses of the two vibrating atoms, which depend on the internuclear distance, R. It is found that all LiH electrons participate in the vibrational motion. The R-dependent masses are obtained from the analysis of the simple VB two-configuration ionic-covalent representation of the electronic wave function. These findings are consistent with an interpretation of the chemical bond in LiH as a quantum mechanical superposition of one-electron ionic and covalent states.

  5. Topological properties of hydrogen bonds and covalent bonds from charge densities obtained by the maximum entropy method (MEM)

    PubMed Central

    Netzel, Jeanette; van Smaalen, Sander

    2009-01-01

    Charge densities have been determined by the Maximum Entropy Method (MEM) from the high-resolution, low-temperature (T ≃ 20 K) X-ray diffraction data of six different crystals of amino acids and peptides. A comparison of dynamic deformation densities of the MEM with static and dynamic deformation densities of multipole models shows that the MEM may lead to a better description of the electron density in hydrogen bonds in cases where the multipole model has been restricted to isotropic displacement parameters and low-order multipoles (l max = 1) for the H atoms. Topological properties at bond critical points (BCPs) are found to depend systematically on the bond length, but with different functions for covalent C—C, C—N and C—O bonds, and for hydrogen bonds together with covalent C—H and N—H bonds. Similar dependencies are known for AIM properties derived from static multipole densities. The ratio of potential and kinetic energy densities |V(BCP)|/G(BCP) is successfully used for a classification of hydrogen bonds according to their distance d(H⋯O) between the H atom and the acceptor atom. The classification based on MEM densities coincides with the usual classification of hydrogen bonds as strong, intermediate and weak [Jeffrey (1997) ▶. An Introduction to Hydrogen Bonding. Oxford University Press]. MEM and procrystal densities lead to similar values of the densities at the BCPs of hydrogen bonds, but differences are shown to prevail, such that it is found that only the true charge density, represented by MEM densities, the multipole model or some other method can lead to the correct characterization of chemical bonding. Our results do not confirm suggestions in the literature that the promolecule density might be sufficient for a characterization of hydrogen bonds. PMID:19767685

  6. Comments on valence-bond structures and charge-shift + recoupled-pair bonding for symmetrical 4-electron 3-centre bonding units

    NASA Astrophysics Data System (ADS)

    Harcourt, Richard D.

    2016-07-01

    Consideration is given to two charge-shift bonding schemes for a symmetrical 4-electron 3-centre hyperbonding unit with three overlapping atomic orbitals. One of these schemes includes the other scheme and the Hach-Rundle-Pimentel 3-centre molecular orbital model as special cases. SF4 and [Cu(H2O)6]2+ are used to illustrate aspects of charge-shift bonding and recoupled-pair bonding theory by generating the increased-valence structures that are associated with the preferred scheme.

  7. 19 CFR 10.39 - Cancellation of bond charges.

    Code of Federal Regulations, 2014 CFR

    2014-04-01

    ... Note: For Federal Register citations affecting § 10.40, see the List of CFR Sections Affected, which... TREASURY ARTICLES CONDITIONALLY FREE, SUBJECT TO A REDUCED RATE, ETC. General Provisions Temporary... entered temporarily free of duty under bond are destroyed within the bond period by death, accidental...

  8. Cation-cation clusters in ionic liquids: Cooperative hydrogen bonding overcomes like-charge repulsion

    PubMed Central

    Knorr, Anne; Ludwig, Ralf

    2015-01-01

    Direct spectroscopic evidence for H-bonding between like-charged ions is reported for the ionic liquid, 1-(2-hydroxyethyl)-3-methylimidazolium tetrafluoroborate. New infrared bands in the OH frequency range appear at low temperatures indicating the formation of H-bonded cation-cation clusters similar to those known for water and alcohols. Supported by DFT calculations, these vibrational bands can be assigned to attractive interaction between the hydroxyl groups of the cations. The repulsive Coulomb interaction is overcome by cooperative hydrogen bonding between ions of like charge. The transition energy from purely cation-anion interacting configurations to those including cation-cation H-bonds is determined to be 3–4 kJmol−1. The experimental findings and DFT calculations strongly support the concept of anti-electrostatic hydrogen bonds (AEHBs) as recently suggested by Weinhold and Klein. The like-charge configurations are kinetically stabilized with decreasing temperatures. PMID:26626928

  9. How Do Distance and Solvent Affect Halogen Bonding Involving Negatively Charged Donors?

    PubMed

    Chen, Zhaoqiang; Wang, Guimin; Xu, Zhijian; Wang, Jinan; Yu, Yuqi; Cai, Tingting; Shao, Qiang; Shi, Jiye; Zhu, Weiliang

    2016-09-01

    It was reported that negatively charged donors can form halogen bonding, which is stable, especially, in a polar environment. On the basis of a survey of the Protein Data Bank, we noticed that the distance between the negative charge center and the halogen atom of an organohalogen may vary greatly. Therefore, a series of model systems, composed of 4-halophenyl-conjugated polyene acids and ammonia, were designed to explore the potential effect of distance on halogen bonding in different solvents. Quantum mechanics (QM) calculations demonstrated that the longer the distance, the stronger the bonding. The energy decomposition analysis on all of the model systems demonstrated that electrostatic interaction contributes the most (44-56%) to the overall binding, followed by orbital interaction (42-36%). Natural bond orbital calculations showed that electron transfer takes place from the acceptor to the donor, whereas the halogen atom becomes more positive during the bonding, which is in agreement with the result of neutral halogen bonding. QM/molecular mechanics calculations demonstrated that the polarity of binding pockets makes all of the interactions attractive in a protein system. Hence, the strength of halogen bonding involving negatively charged donors could be adjusted by changing the distance between the negative charge center and halogen atom and the environment in which the bonding exists, which may be applied in material and drug design for tuning their function and activity. PMID:27504672

  10. 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

  11. 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.

  12. Charged versus Neutral Hydrogen-Bonded Complexes: Is There a Difference in the Nature of the Hydrogen Bonds?

    PubMed

    Alkorta, Ibon; Mata, Ignasi; Molins, Elies; Espinosa, Enrique

    2016-06-27

    A theoretical study on some carboxylic acid dimers formed by positively or negatively charged molecules has been carried out by using DFT methods. The resulting dimers possess either a charge of +2 or -2. In addition, the corresponding neutral complexes have also been considered. The electron density distribution described by the atoms in molecules and the natural bond orbital methods, as well as the electric field maps of the systems, have been analyzed and compared without finding significant differences between the neutral and ionic complexes. The interaction energy along the dissociation path of the charged dimers shows both a local minimum and a local maximum, defining a stability region between them. When this energetic profile is recalculated by removing the repulsion between the charged groups, it resembles to those of the neutral molecules. Hence, the characteristics of the charged dimers are similar to those of the neutral ones: the addition of a repulsion term for the charged groups permits to retrieve the energetic profiles dependence with the distance in the charged system. The interacting quantum atom (IQA) method has been used to calculate the interaction energy terms, including the classic Coulombic term between the whole molecules and the corresponding of the carboxylic acid groups. The IQA results show repulsive electrostatic interactions when the whole molecules are considered in the ionic complexes, but attractive ones between the carboxylic groups in both neutral and ionic complexes. PMID:27225820

  13. On the ultrafast charge migration dynamics in isolated ionized halogen, chalcogen, pnicogen, and tetrel bonded clusters

    NASA Astrophysics Data System (ADS)

    Chandra, Sankhabrata; Rana, Bhaskar; Periyasamy, Ganga; Bhattacharya, Atanu

    2016-06-01

    Here we demonstrate, compare and contrast relaxation- and correlation-driven charge migration dynamics in halogen, chalcogen, pnicogen and tetrel bonded clusters, following their vertical ionization. For this work, we have selected different isolated A-X:NH3 clusters, where A represents F, Cl, CN and NH2 substituents and X features Cl, SH, PH2 and SiH3 to exhibit specific noncovalent bonding interaction. The charge migration dynamics in these clusters is studied using the density functional theory (DFT) with the wB97XD functional and the 6-31+G(d,p) basis set. Approximately 400-600 attosecond time scale is predicted for charge migration in (1:1) AX:NH3 complexes. Effects of basis set and intermolecular distance on the ultrafast charge migration dynamics through the halogen, chalcogen, pnicogen, and tetrel bonded clusters are also discussed. This is the first report on pure relaxation- and correlation-driven charge migration dynamics in chalcogen, pnicogen and tetrel bonded clusters.

  14. Photophysical studies of metal to ligand charge transfer involving quadruply bonded complexes of molybdenum and tungsten.

    PubMed

    Chisholm, Malcolm H; Brown-Xu, Samantha E; Spilker, Thomas F

    2015-03-17

    Photoinduced metal-to-ligand charge transfer transitions afford numerous applications in terms of photon energy harvesting. The majority of metal complexes studied to date involve diamagnetic systems of d(6), d(8), and d(10) transition metals. These typically have very short-lived, ∼100 fs, singlet metal to ligand charge transfer ((1)MLCT) states that undergo intersystem crossing to triplet metal to ligand charge transfer ((3)MLCT) states that are longer lived and are responsible for much of the photophysical studies. In contrast, the metal-metal quadruply bonded complexes of molybdenum and tungsten supported by carboxylate, O2CR, and related amidinate ligands (RN)2C(R') have relatively long-lived (1)MLCT states arising from M2δ to Lπ* transitions. These have lifetimes in the range 1-20 ps prior to intersystem crossing to T1 states that may be (3)MLCT or (3)MMδδ* with lifetimes of 1-100 ns and 1-100 μs, respectively. The M2 quadruply bonded complexes take the form M2L4 or M2L4-nL'n where n = 1-3. Thus, in their photoexcited MLCT states, these compounds pose the question of how the charge resides on the ligands. This Account reviews the current knowledge of how charge is positioned with time in S1 and T1 states with the aid of active IR reported groups located on the ligands, for example, C≡X multiple bonds (X = C, N, or O). Several examples of localized and delocalized charge distributions are noted along with kinetic barriers to the interconversion of MLCT and δδ* states. On the 50th anniversary of the recognition of the MM quadruple bond, these complexes are revealing some remarkable features in the study of the photophysical properties of metal-ligand charge transfer states. PMID:25695495

  15. Three component assemblies by orthogonal H-bonding and donor-acceptor charge-transfer interaction.

    PubMed

    Kar, Haridas; Ghosh, Suhrit

    2014-02-01

    Three component supramolecular assemblies from a mixture of an aromatic donor (D), acceptor (A) and external structure directing agent (ESDA) are achieved by orthogonal noncovalent interactions involving two different types of H-bonding and alternate D-A stacking. An ESDA containing amide or urea produces a charge-transfer gel and sol, respectively, owing to their contrasting morphology. PMID:24309620

  16. Constructing diabatic states from adiabatic states: Extending generalized Mulliken-Hush to multiple charge centers with Boys localization

    NASA Astrophysics Data System (ADS)

    Subotnik, Joseph E.; Yeganeh, Sina; Cave, Robert J.; Ratner, Mark A.

    2008-12-01

    This article shows that, although Boys localization is usually applied to single-electron orbitals, the Boys method itself can be applied to many electron molecular states. For the two-state charge-transfer problem, we show analytically that Boys localization yields the same charge-localized diabatic states as those found by generalized Mulliken-Hush theory. We suggest that for future work in electron transfer, where systems have more than two charge centers, one may benefit by using a variant of Boys localization to construct diabatic potential energy surfaces and extract electronic coupling matrix elements. We discuss two chemical examples of Boys localization and propose a generalization of the Boys algorithm for creating diabatic states with localized spin density that should be useful for Dexter triplet-triplet energy transfer.

  17. Note: Charge transfer in a hydrated peptide group is determined mainly by its intrinsic hydrogen-bond energetics

    SciTech Connect

    Mirkin, Noemi G.; Krimm, Samuel

    2014-01-28

    Charge transfer in a hydrogen-bonded N-methylacetamide(H{sub 2}O){sub 3} system is obtained from ωB97X-D/6-31++G** and CHelpG atomic charge calculations of individual peptide-water interactions as well as that of the entire complex. In the latter, the electron transfer to water is 0.19 e, influenced primarily by the hydrogen bonds to the C=O group. The values of such charge transfer are paralleled by the corresponding intrinsic hydrogen-bond energies. These results support the desirability of incorporating charge transfer in molecular mechanics energy functions.

  18. On the ultrafast charge migration and subsequent charge directed reactivity in Cl⋯N halogen-bonded clusters following vertical ionization.

    PubMed

    Chandra, Sankhabrata; Periyasamy, Ganga; Bhattacharya, Atanu

    2015-06-28

    In this article, we have presented ultrafast charge transfer dynamics through halogen bonds following vertical ionization of representative halogen bonded clusters. Subsequent hole directed reactivity of the radical cations of halogen bonded clusters is also discussed. Furthermore, we have examined effect of the halogen bond strength on the electron-electron correlation- and relaxation-driven charge migration in halogen bonded complexes. For this study, we have selected A-Cl (A represents F, OH, CN, NH2, CF3, and COOH substituents) molecules paired with NH3 (referred as ACl:NH3 complex): these complexes exhibit halogen bonds. To the best of our knowledge, this is the first report on purely electron correlation- and relaxation-driven ultrafast (attosecond) charge migration dynamics through halogen bonds. Both density functional theory and complete active space self-consistent field theory with 6-31 + G(d, p) basis set are employed for this work. Upon vertical ionization of NCCl⋯NH3 complex, the hole is predicted to migrate from the NH3-end to the ClCN-end of the NCCl⋯NH3 complex in approximately 0.5 fs on the D0 cationic surface. This hole migration leads to structural rearrangement of the halogen bonded complex, yielding hydrogen bonding interaction stronger than the halogen bonding interaction on the same cationic surface. Other halogen bonded complexes, such as H2NCl:NH3, F3CCl:NH3, and HOOCCl:NH3, exhibit similar charge migration following vertical ionization. On the contrary, FCl:NH3 and HOCl:NH3 complexes do not exhibit any charge migration following vertical ionization to the D0 cation state, pointing to interesting halogen bond strength-dependent charge migration. PMID:26133430

  19. On the ultrafast charge migration and subsequent charge directed reactivity in Cl⋯N halogen-bonded clusters following vertical ionization

    NASA Astrophysics Data System (ADS)

    Chandra, Sankhabrata; Periyasamy, Ganga; Bhattacharya, Atanu

    2015-06-01

    In this article, we have presented ultrafast charge transfer dynamics through halogen bonds following vertical ionization of representative halogen bonded clusters. Subsequent hole directed reactivity of the radical cations of halogen bonded clusters is also discussed. Furthermore, we have examined effect of the halogen bond strength on the electron-electron correlation- and relaxation-driven charge migration in halogen bonded complexes. For this study, we have selected A-Cl (A represents F, OH, CN, NH2, CF3, and COOH substituents) molecules paired with NH3 (referred as ACl:NH3 complex): these complexes exhibit halogen bonds. To the best of our knowledge, this is the first report on purely electron correlation- and relaxation-driven ultrafast (attosecond) charge migration dynamics through halogen bonds. Both density functional theory and complete active space self-consistent field theory with 6-31 + G(d, p) basis set are employed for this work. Upon vertical ionization of NCCl⋯NH3 complex, the hole is predicted to migrate from the NH3-end to the ClCN-end of the NCCl⋯NH3 complex in approximately 0.5 fs on the D0 cationic surface. This hole migration leads to structural rearrangement of the halogen bonded complex, yielding hydrogen bonding interaction stronger than the halogen bonding interaction on the same cationic surface. Other halogen bonded complexes, such as H2NCl:NH3, F3CCl:NH3, and HOOCCl:NH3, exhibit similar charge migration following vertical ionization. On the contrary, FCl:NH3 and HOCl:NH3 complexes do not exhibit any charge migration following vertical ionization to the D0 cation state, pointing to interesting halogen bond strength-dependent charge migration.

  20. On the ultrafast charge migration and subsequent charge directed reactivity in Cl⋯N halogen-bonded clusters following vertical ionization

    SciTech Connect

    Chandra, Sankhabrata; Bhattacharya, Atanu; Periyasamy, Ganga

    2015-06-28

    In this article, we have presented ultrafast charge transfer dynamics through halogen bonds following vertical ionization of representative halogen bonded clusters. Subsequent hole directed reactivity of the radical cations of halogen bonded clusters is also discussed. Furthermore, we have examined effect of the halogen bond strength on the electron-electron correlation- and relaxation-driven charge migration in halogen bonded complexes. For this study, we have selected A-Cl (A represents F, OH, CN, NH{sub 2}, CF{sub 3}, and COOH substituents) molecules paired with NH{sub 3} (referred as ACl:NH{sub 3} complex): these complexes exhibit halogen bonds. To the best of our knowledge, this is the first report on purely electron correlation- and relaxation-driven ultrafast (attosecond) charge migration dynamics through halogen bonds. Both density functional theory and complete active space self-consistent field theory with 6-31 + G(d, p) basis set are employed for this work. Upon vertical ionization of NCCl⋯NH{sub 3} complex, the hole is predicted to migrate from the NH{sub 3}-end to the ClCN-end of the NCCl⋯NH{sub 3} complex in approximately 0.5 fs on the D{sub 0} cationic surface. This hole migration leads to structural rearrangement of the halogen bonded complex, yielding hydrogen bonding interaction stronger than the halogen bonding interaction on the same cationic surface. Other halogen bonded complexes, such as H{sub 2}NCl:NH{sub 3}, F{sub 3}CCl:NH{sub 3}, and HOOCCl:NH{sub 3}, exhibit similar charge migration following vertical ionization. On the contrary, FCl:NH{sub 3} and HOCl:NH{sub 3} complexes do not exhibit any charge migration following vertical ionization to the D{sub 0} cation state, pointing to interesting halogen bond strength-dependent charge migration.

  1. Bond-forming reactions of small triply charged cations with neutral molecules.

    PubMed

    Fletcher, James D; Parkes, Michael A; Price, Stephen D

    2013-08-12

    Time-of-flight mass spectrometry reveals that atomic and small molecular triply charged cations exhibit extensive bond-forming chemistry, following gas-phase collisions with neutral molecules. These experiments show that at collision energies of a few eV, I(3+) reacts with a variety of small molecules to generate molecular monocations and molecular dications containing iodine. Xe(3+) and CS2(3+) react in a similar manner to I(3+), undergoing bond-forming reactions with neutrals. A simple model, involving relative product energetics and electrostatic interaction potentials, is used to account for the observed reactivity. PMID:23843367

  2. Electronic structure, stacking energy, partial charge, and hydrogen bonding in four periodic B-DNA models

    NASA Astrophysics Data System (ADS)

    Poudel, Lokendra; Rulis, Paul; Liang, Lei; Ching, W. Y.

    2014-08-01

    We present a theoretical study of the electronic structure of four periodic B-DNA models labeled (AT)10,(GC)10, (AT)5(GC)5, and (AT-GC)5 where A denotes adenine, T denotes thymine, G denotes guanine, and C denotes cytosine. Each model has ten base pairs with Na counterions to neutralize the negative phosphate group in the backbone. The (AT)5(GC)5 and (AT-GC)5 models contain two and five AT-GC bilayers, respectively. When compared against the average of the two pure models, we estimate the AT-GC bilayer interaction energy to be 19.015 Kcal/mol, which is comparable to the hydrogen bonding energy between base pairs obtained from the literature. Our investigation shows that the stacking of base pairs plays a vital role in the electronic structure, relative stability, bonding, and distribution of partial charges in the DNA models. All four models show a highest occupied molecular orbital (HOMO) to lowest unoccupied molecular orbital (LUMO) gap ranging from 2.14 to 3.12 eV with HOMO states residing on the PO4 + Na functional group and LUMO states originating from the bases. Our calculation implies that the electrical conductance of a DNA molecule should increase with increased base-pair mixing. Interatomic bonding effects in these models are investigated in detail by analyzing the distributions of the calculated bond order values for every pair of atoms in the four models including hydrogen bonding. The counterions significantly affect the gap width, the conductivity, and the distribution of partial charge on the DNA backbone. We also evaluate quantitatively the surface partial charge density on each functional group of the DNA models.

  3. Charge transfer mobility of naphthodithiophenediimide derivative: Normal-mode and bond length relaxation analysis

    NASA Astrophysics Data System (ADS)

    Liu, Xiaoyan; Liu, Yujuan; Zheng, Yujun

    2016-02-01

    In this letter, the charge transfer mobility of naphthalenediimide (NDTI) derivative is investigated. By employing the normal-mode analysis and bond length relaxation analysis, the influences of chemical elements on reorganization energies and intermolecular electronic couplings are investigated in NDTI derivative. The results show that the introduction of atom O would decrease reorganization energy in hole-hopping process and increase electronic coupling. This analysis encourages the molecular and material design in organic semiconductors.

  4. Quantum size effects in competing charge and spin orderings of dangling bond wires on Si(001)

    SciTech Connect

    Lee, Ji Young; Cho, Jun-Hyung; Zhang, Zhenyu

    2009-01-01

    Using spin-polarized density-functional theory calculations, we investigate the competition between charge and spin orderings in dangling-bond DB wires of increasing lengths fabricated on an H-terminated Si 001 surface. For wires containing less than ten DBs as studied in recent experiments, we find antiferromagnetic AF ordering to be energetically much more favorable than charge ordering. The energy preference of AF ordering shrinks in an oscillatory way as the wire length increases and preserves its sign even for DB wires of infinite length. The oscillatory behavior can be attributed to quantum size effects as the DB electrons fill discrete quantum levels. The predicted AF ordering is in startling contrast with the prevailing picture of charge ordering due to Jahn-Teller distortion or Peierls instability for wires of finite or infinite lengths, respectively.

  5. X-ray charge density study of chemical bonding in skutterudite CoSb{sub 3}

    SciTech Connect

    Ohno, Atsuko; Sasaki, Satoshi; Nishibori, Eiji; Aoyagi, Shinobu; Sakata, Makoto; Iversen, Bo Brummerstedt

    2007-08-01

    The experimental charge density of nondoped CoSb{sub 3} has been determined by the maximum entropy method (MEM) using low temperature (10 K), short wavelength (0.42 A), and high-resolution (d{sub min}=0.33 A) synchrotron x-ray powder diffraction data measured at SPring-8, Japan. The MEM charge density clearly reveals three types of charge density overlap between atoms in CoSb{sub 3}. The four Sb atoms form an Sb{sub 4} ring, and the MEM charge densities at two types of Sb-Sb midpoints are 0.35 and 0.50 e A{sup -3}. The charge density overlap between the Co and Sb atoms at the midpoint is 0.52 e A{sup -3}, which is larger than the values observed at the Sb-Sb midpoints. The nature of the chemical bonding observed in the present MEM charge density is consistent with a previous theoretical study by Lefebvre-Devos et al. [Phys. Rev. B 63, 125110 (2001)].

  6. 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.

  7. Hydrogen Bonding and Binding of Polybasic Residues with Negatively Charged Mixed Lipid Monolayers

    SciTech Connect

    Lorenz, C.; Feraudo, J.; Travesset, A.

    2008-01-23

    Phosphoinositides, phosphorylated products of phosphatidylinositol, are a family of phospholipids present in tiny amounts (1% or less) in the cytosolic surface of cell membranes, yet they play an astonishingly rich regulatory role, particularly in signaling processes. In this letter, we use molecular dynamics simulations on a model system of mixed lipid monolayers to investigate the interaction of phosphatidylinositol 4,5-bisphosphate (PIP{sub 2}), the most common of the phosphoinositides, with a polybasic peptide consisting of 13 lysines. Our results show that the polybasic peptide sequesters three PIP{sub 2} molecules, forming a complex stabilized by the formation of multiple hydrogen bonds between PIP{sub 2} and the Lys residues. We also show that the polybasic peptide does not sequester other charged phospholipids such as phosphatidylserine because of the inability to form long-lived stable hydrogen bonds.

  8. Photoinduced charge-transfer dynamics simulations in noncovalently bonded molecular aggregates.

    PubMed

    Medrano, Carlos R; Oviedo, M Belén; Sánchez, Cristián G

    2016-06-01

    The rational design of new materials as prototype systems for organic solar cells remains challenging. Perylene diimide has emerged as a promising material to replace fullerene derivatives because of its synthetic flexibility, leading to the manipulation of their optical properties. As a result of their fused aromatic core that favors π-π stacking interactions, the aggregation of these molecules can reach highly ordered nanostructures as one-dimensional nanofibers, with a fast photoinduced charge transfer mechanism. In this article, we present an atomistic description of the photoexcited exciton dynamics in noncovalently bonded perylene diimides by time integration of the electron density in the presence of external time varying electric fields. We show that our approach is able to capture and explain the physics that underlies the charge transport mechanism through perylene diimide aggregates. PMID:27189740

  9. Utilizing Metal to Ligand Charge Transfer States of MM Quadruply Bonded Complexes for Photovoltaic Applications

    NASA Astrophysics Data System (ADS)

    Lewis, Sharlene A.; Brown-Xu, Samantha E.; Chisholm, Malcolm H.; Epstein, Arthur J.

    2013-06-01

    In this contribution, we report two examples of our efforts to develop MM quadruply bonded complexes for photovoltaic applications. In the first example, evidence, based on femtosecond transient absorption and time resolved infrared spectroscopy, is presented for photoinduced charge transfer from the Mo_{2}δ orbital of the quadruply bonded molecule trans-Mo_{2}(TiPB)_{2}BTh)_{2}, where TiPB = 2,4,6-triisopropyl benzoate and BTh = 2,2'-bithienylcarboxylate, to di-n-octyl perylene diimide and di-n-hexylheptyl perylene diimide in thin films and solutions of the mixtures. In the second example, the structural and photophysical properties of the new compounds trans-M_{2}(TiPB)_{2}(L)_{2} and trans-M_{2}(TiPB)_{2}(L')_{2}, where M=Mo or W and L and L' are triphenylamine-cyanoacrylate ligands are presented. These ligands promote intense metal to ligand charge transfer transitions that span the range 550 to 1100 nm. The excited states have been studied by transient absorption and time resolved infrared spectroscopy

  10. Simulation of intramolecular hydrogen bond dynamics in manzamine A as a sensitive test for charge distribution quality.

    PubMed

    Shulga, Dmitry A; Osolodkin, Dmitry I; Palyulin, Vladimir A; Zefirov, Nikolay S

    2012-03-01

    Subtle balance of inter- and intramolecular hydrogen bond strength in aqueous solutions often governs the structure and dynamics of molecular species used as potential drugs and in supramolecular applications. In silico molecular dynamics study of water solution of manzamine A has been performed with different atomic charges in order to investigate the influence of charge distribution choice on predicting qualitative and quantitative features of the simulated systems. Various well known charge schemes (MK-ESP, RESP, Mulliken, AMI-BCC, Gasteiger-Hückel, Gasteiger-Marsili, MMFF94, and Dynamic Electronegativity Relaxation - DENR) led to qualitatively different pictures of dynamic behavior of the intramolecular hydrogen bond. The reported calculation framework represents a relatively rare case where differences in charge distributions lead to noticeable differences in simulated properties, thus providing a useful test case for force field and charge distribution development, provided high quality experiments are conducted to use as references. PMID:22545399

  11. Automation of the CHARMM General Force Field (CGenFF) II: assignment of bonded parameters and partial atomic charges.

    PubMed

    Vanommeslaeghe, K; Raman, E Prabhu; MacKerell, A D

    2012-12-21

    Molecular mechanics force fields are widely used in computer-aided drug design for the study of drug candidates interacting with biological systems. In these simulations, the biological part is typically represented by a specialized biomolecular force field, while the drug is represented by a matching general (organic) force field. In order to apply these general force fields to an arbitrary drug-like molecule, functionality for assignment of atom types, parameters, and partial atomic charges is required. In the present article, algorithms for the assignment of parameters and charges for the CHARMM General Force Field (CGenFF) are presented. These algorithms rely on the existing parameters and charges that were determined as part of the parametrization of the force field. Bonded parameters are assigned based on the similarity between the atom types that define said parameters, while charges are determined using an extended bond-charge increment scheme. Charge increments were optimized to reproduce the charges on model compounds that were part of the parametrization of the force field. A "penalty score" is returned for every bonded parameter and charge, allowing the user to quickly and conveniently assess the quality of the force field representation of different parts of the compound of interest. Case studies are presented to clarify the functioning of the algorithms and the significance of their output data. PMID:23145473

  12. Spectroscopic Evidence for Clusters of Like-Charged Ions in Ionic Liquids Stabilized by Cooperative Hydrogen Bonding.

    PubMed

    Knorr, Anne; Stange, Peter; Fumino, Koichi; Weinhold, Frank; Ludwig, Ralf

    2016-02-01

    Direct spectroscopic evidence for hydrogen-bonded clusters of like-charged ions is reported for ionic liquids. The measured infrared O-H vibrational bands of the hydroxyethyl groups in the cations can be assigned to the dispersion-corrected DFT calculated frequencies of linear and cyclic clusters. Compensating the like-charge Coulomb repulsion, these cationic clusters can range up to cyclic tetramers resembling molecular clusters of water and alcohols. These ionic clusters are mainly present at low temperature and show strong cooperative effects in hydrogen bonding. DFT-D3 calculations of the pure multiply charged clusters suggest that the attractive hydrogen bonds can compete with repulsive Coulomb forces. PMID:26670942

  13. Bonding and charge transfer in nitrogen-donor uranyl complexes: insights from NEXAFS spectra.

    PubMed

    Pemmaraju, C D; Copping, Roy; Wang, Shuao; Janousch, Markus; Teat, Simon J; Tyliszcak, Tolek; Canning, Andrew; Shuh, David K; Prendergast, David

    2014-11-01

    We investigate the electronic structure of three newly synthesized nitrogen-donor uranyl complexes [(UO2)(H2bbp)Cl2], [(UO)2(Hbbp)(Py)Cl], and [(UO2)(bbp)(Py)2] using a combination of near-edge X-ray absorption fine structure (NEXAFS) spectroscopy experiments and simulations. The complexes studied feature derivatives of the tunable tridentate N-donor ligand 2,6-bis(2-benzimidazyl)pyridine (bbp) and exhibit discrete chemical differences in uranyl coordination. The sensitivity of the N K-edge X-ray absorption spectrum to local bonding and charge transfer is exploited to systematically investigate the evolution of structural as well as electronic properties across the three complexes. A thorough interpretation of the measured experimental spectra is achieved via ab initio NEXAFS simulations based on the eXcited electron and Core-Hole (XCH) approach and enables the assignment of spectral features to electronic transitions on specific absorbing sites. We find that ligand-uranyl bonding leads to a signature blue shift in the N K-edge absorption onset, resulting from charge displacement toward the uranyl, while changes in the equatorial coordination shell of the uranyl lead to more subtle modulations in the spectral features. Theoretical simulations show that the flexible local chemistry at the nonbinding imidazole-N sites of the bbp ligand is also reflected in the NEXAFS spectra and highlights potential synthesis strategies to improve selectivity. In particular, we find that interactions of the bbp ligand with solvent molecules can lead to changes in ligand-uranyl binding geometry while also modulating the K-edge absorption. Our results suggest that NEXAFS spectroscopy combined with first-principles interpretation can offer insights into the coordination chemistry of analogous functionalized conjugated ligands. PMID:25330350

  14. Simulations of the THz spectrum of liquid water incorporating the effects of intermolecular charge fluxes through hydrogen bonds

    SciTech Connect

    Torii, Hajime

    2015-12-31

    The intensity of the band at ∼200 cm{sup −1} (∼6 THz) in the Terahertz spectrum of liquid water mainly arises from the modulations of the extent of intermolecular charge transfer through hydrogen bonds, called intermolecular charge fluxes, occurring upon molecular translations along the O…H hydrogen bonds. To obtain reasonable spectral profiles from simulations, it is necessary to effectively incorporate the effects of those intermolecular charge fluxes, but apparently it is not possible by simple classical molecular dynamics simulations with fixed atomic partial charges even if they are amended by molecular induced dipoles due to intermolecular electrostatic interactions. The present paper shows how we can do reasonably correct spectral simulations, without resorting to fully ab initio molecular dynamics.

  15. 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.

  16. Introducing constricted variational density functional theory in its relaxed self-consistent formulation (RSCF-CV-DFT) as an alternative to adiabatic time dependent density functional theory for studies of charge transfer transitions

    SciTech Connect

    Krykunov, Mykhaylo; Seth, Mike; Ziegler, Tom

    2014-05-14

    We have applied the relaxed and self-consistent extension of constricted variational density functional theory (RSCF-CV-DFT) for the calculation of the lowest charge transfer transitions in the molecular complex X-TCNE between X = benzene and TCNE = tetracyanoethylene. Use was made of functionals with a fixed fraction (α) of Hartree-Fock exchange ranging from α = 0 to α = 0.5 as well as functionals with a long range correction (LC) that introduces Hartree-Fock exchange for longer inter-electronic distances. A detailed comparison and analysis is given for each functional between the performance of RSCF-CV-DFT and adiabatic time-dependent density functional theory (TDDFT) within the Tamm-Dancoff approximation. It is shown that in this particular case, all functionals afford the same reasonable agreement with experiment for RSCF-CV-DFT whereas only the LC-functionals afford a fair agreement with experiment using TDDFT. We have in addition calculated the CT transition energy for X-TCNE with X = toluene, o-xylene, and naphthalene employing the same functionals as for X = benzene. It is shown that the calculated charge transfer excitation energies are in as good agreement with experiment as those obtained from highly optimized LC-functionals using adiabatic TDDFT. We finally discuss the relation between the optimization of length separation parameters and orbital relaxation in the RSCF-CV-DFT scheme.

  17. Spectroscopic evidence for medium controlled hydrogen bond inhibition of resonance delocalization of charge in complexes of tetrabutylammonium fluoride with phenols

    NASA Astrophysics Data System (ADS)

    Clark, James H.; Cork, David G.; Tinsdale, Julie A.

    Infrared spectra of tetrabutylammonium fluoride complexes of both 4-cyanophenol and methyl-4-hydroxybenzoate but not 3-cyanophenol reveal the presence of two distinct types of hydrogen bond corresponding to charge localized and partially charge delocalized forms. The latter only occur in polar aprotic protophilic solvents at low temperatures. The activation energies for the interconversion of the two forms reflect the relative abilities of the two groups to delocalize charge through resonance. The chemical shifts of the aromatic protons of the complexes are also medium dependent although the precise nature of this medium dependence is less easily understood.

  18. Influence of intermolecular amide hydrogen bonding on the geometry, atomic charges, and spectral modes of acetanilide: An ab initio study

    NASA Astrophysics Data System (ADS)

    Binoy, J.; Prathima, N. B.; Murali Krishna, C.; Santhosh, C.; Hubert Joe, I.; Jayakumar, V. S.

    2006-08-01

    Acetanilide, a compound of pharmaceutical importance possessing pain-relieving properties due to its blocking the pulse dissipating along the nerve fiber, is subjected to vibrational spectral investigation using NIR FT Raman, FT-IR, and SERS. The geometry, Mulliken charges, and vibrational spectrum of acetanilide have been computed using the Hartree-Fock theory and density functional theory employing the 6-31G (d) basis set. To investigate the influence of intermolecular amide hydrogen bonding, the geometry, charge distribution, and vibrational spectrum of the acetanilide dimer have been computed at the HF/6-31G (d) level. The computed geometries reveal that the acetanilide molecule is planar, while twisting of the secondary amide group with respect to the phenyl ring is found upon hydrogen bonding. The trans isomerism and “amido” form of the secondary amide, hyperconjugation of the C=O group with the adjacent C-C bond, and donor-acceptor interaction have been investigated using computed geometry. The carbonyl stretching band position is found to be influenced by the tendency of the phenyl ring to withdraw nitrogen lone pair, intermolecular hydrogen bonding, conjugation, and hyperconjugation. A decrease in the NH and C=O bond orders and increase in the C-N bond orders due to donor-acceptor interaction can be observed in the vibrational spectra. The SERS spectral analysis reveals that the flat orientation of the molecule on the adsorption plane is preferred.

  19. Quantification of Conventional and Nonconventional Charge-Assisted Hydrogen Bonds in the Condensed and Gas Phases.

    PubMed

    Katsyuba, Sergey A; Vener, Mikhail V; Zvereva, Elena E; Fei, Zhaofu; Scopelliti, Rosario; Brandenburg, Jan Gerit; Siankevich, Sviatlana; Dyson, Paul J

    2015-11-01

    Charge-assisted hydrogen bonds (CAHBs) play critical roles in many systems from biology through to materials. In none of these areas has the role and function of CAHBs been explored satisfactorily because of the lack of data on the energy of CAHBs in the condensed phases. We have, for the first time, quantified three types of CAHBs in both the condensed and gas phases for 1-(2'-hydroxylethyl)-3-methylimidazolium acetate ([C2OHmim][OAc]). The energy of conventional OH···[OAc](-) CAHBs is ∼10 kcal·mol(-1), whereas nonconventional C(sp2)H···[OAc](-) and C(sp3)H···[OAc](-) CAHBs are weaker by ∼5-7 kcal·mol(-1). In the gas phase, the strength of the nonconventional CAHBs is doubled, whereas the conventional CAHBs are strengthened by <20%. The influence of cooperativity effects on the ability of the [OAc](-) anion to deprotonate the imidazolium cation is evaluated. The ability to quantify CAHBs in the condensed phase on the basis of easier accessible gas-phase estimates is highlighted. PMID:26496074

  20. Resonating valence bond and {sigma}-charge density wave phases in a benzannulated phenalenyl radical.

    SciTech Connect

    Bag, P.; Itkis, M. E.; .Pal, S. K; Donnadieu, B.; Tham, F. S.; Park, H.; Schlueter, J. A.; Siegrist, T.; Haddon, R. C.; Materials Science Division; Univ. of California of Riverside; Florida State Univ.

    2010-01-01

    We report the preparation of the first benzannulated phenalenyl neutral radical conductor (18), and we show that the compound displays unprecedented solid state behavior: the structure is dominated by two sets of intermolecular interactions: (1) a {pi}-chain structure with superimposed {pi}-overlap of the benzannulated phenalenyls along [0 0 1], and (2) an interchain overlap involving a pair of carbon atoms (C4) along [0 1 0]. The {pi}-chain-type stacking motif is reminiscent of previously reported phenalenyl radicals and the room temperature structure (space group P2/c) together with the conductivity of {sigma}{sub RT} = 0.03 S/cm and the Pauli-like magnetic susceptibility are best described by the resonating valence bond (RVB) model. The interchain interaction is unstable with respect to the formation of a {sigma}-charge density wave ({sigma}-CDW) involving pairs of C4 carbon atoms between adjacent radicals and this phase is characterized by the P2{sub 1}/c space group which involves a doubling of the unit cell along the [0 1 0] direction. The RVB and CDW phases compete for structural occupancy throughout the whole temperature range (15-293 K) with the RVB phase predominating at 15 and 293 K and the {sigma}-CDW phase achieving a maximum structural occupancy of about 60% at 150 K where it produces clearly discernible effects on the magnetism and conductivity.

  1. Hydrogen Bond Acceptors and Additional Cationic Charges in Methylene Blue Derivatives: Photophysics and Antimicrobial Efficiency

    PubMed Central

    Felgenträger, Ariane; Maisch, Tim; Dobler, Daniel; Späth, Andreas

    2013-01-01

    Photodynamic inactivation of bacteria (PIB) by efficient singlet oxygen photosensitizers might be a beneficial alternative to antibiotics in the struggle against multiresistant bacteria. Phenothiazinium dyes belong to the most prominent classes of such sensitizers due to their intense absorption in the red-light region (λabs, max ca. 600–680 nm, ε > 50000 L mol−1 cm−1), their low toxicity, and their attachment/penetration abilities. Except simple substituents like alkyl or hydroxyalkyl residues, nearly no modifications of the phenothiaziniums have been pursued at the auxochromic sites. By this, the properties of methylene blue derivatives and their fields of application are limited; it remains unclear if their potential antimicrobial efficacy may be enhanced, also to compete with porphyrins. We prepared a set of six mainly novel methylene blue derivatives with the ability of additional hydrogen bonding and/or additional cationic charges to study the substituents' effect on their activity/toxicity profiles and photophysical properties. Direct detection of singlet oxygen was performed at 1270 nm and the singlet oxygen quantum yields were determined. In suspensions with both, Gram-positive and Gram-negative bacteria, some derivatives were highly active upon illumination to inactivate S. aureus and E. coli up to 7 log10 steps (99.99999%) without inherent toxicities in the nonirradiated state. PMID:23509728

  2. Do resonance-assisted intramolecular halogen bonds exist without a charge transfer and a σ-hole?

    PubMed

    Vijaya Pandiyan, B; Deepa, P; Kolandaivel, P

    2015-11-01

    To analyze the properties and mechanisms of six types of intramolecular resonance-assisted halogen bonds (Br···O, Cl···O, F···O, Br···O, Cl···S and F···S), we have chosen the five-membered closed ring system X-C1R1=C3R2-C2R3=Y (X = Br, Cl & F; Y = O & S) of unsaturated compounds with the substituents NO2, CH3 and H. A total of 78 structures were investigated by quantum chemical calculations at the MP2/aug-cc-pVTZ level of theory. A molecular electrostatic potential (MESP) map reveals that the cusp point of the σ-hole was not utilized but the belt point was used for all these intramolecular halogen-bonding interactions, indicating that all are electrostatic interactions. The halogen-bonding angle is below 100° with the strongest interactions. The value of the nucleus-independent chemical shift (NICS (1)) reflects the changes and efficiency of resonance in all structures with a long bond. The presence of all interactions was proved by the bond critical point (BCP) and analyzed through its electron density, Laplacian of electron density and ellipticity parameter. The linear-probability correlation between the difference of the sum of the van der Waals radius and the non-covalent bond length (∑vdW-L) and the electron density of the BCP was reported. 2D and 3D-NCI (non covalent interactions) plots show that halogen-bonding interactions are a mixed type of interactions with an attractive term. Natural bond orbital (NBO) analysis clearly indicates that the halogen bond lacks charge transfer and orbital overlapping through non-interacting lobes. PMID:26426450

  3. Bond dissociation energies from the topology of the charge density using gradient bundle analysis

    NASA Astrophysics Data System (ADS)

    Morgenstern, Amanda; Eberhart, Mark

    2016-02-01

    New and more robust models of chemical bonding are necessary to further our understanding of chemical phenomena. Among these are bond bundle and gradient bundle methods, which analyze bonding interactions in terms of property distributions over geometrically defined volumes. These methods have been shown to provide a systematic framework from which to search for structure-property relationships. In addition to providing a brief review of some of the relationships found using this framework, we present new findings that relate the lowering of kinetic energy in bonding regions to bond dissociation energy.

  4. Intermolecular charge flux as the origin of infrared intensity enhancement upon halogen-bond formation of the peptide group

    NASA Astrophysics Data System (ADS)

    Torii, Hajime

    2010-07-01

    The changes in the vibrational properties of the peptide group upon formation of O⋯X and N⋯X halogen bonds are studied theoretically. Calculations are carried out for complexes of N-methylacetamide (NMA), a well known model molecule of the peptide group, with halogen-containing molecules. For comparison, calculations are also carried out for some NMA-water hydrogen-bonding complexes. It is shown that the infrared (IR) intensity of the amide I mode of the peptide group is enhanced significantly (up to about 520 km mol-1 or 2.6 times) upon CO⋯X halogen-bond formation, in spite of rather modest magnitudes of the intermolecular electric field and of the changes in the CO bond length and in the amide I vibrational frequency as compared with the cases of the CO⋯H(D) hydrogen bonding. From the analysis of the changes in the dipole derivative and in the electronic structure, it is shown that this IR intensity enhancement arises from the intermolecular charge flux. For the N⋯X halogen bonding complexes, some characteristic changes in the vibrational properties are seen, among which the IR intensity enhancement of the ND out-of-plane wagging mode is most notable. The reason why such large IR intensity enhancements are seen for these particular vibrational modes is examined.

  5. 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.

  6. 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.

  7. Chemical bonding in view of electron charge density and kinetic energy density descriptors.

    PubMed

    Jacobsen, Heiko

    2009-05-01

    Stalke's dilemma, stating that different chemical interpretations are obtained when one and the same density is interpreted either by means of natural bond orbital (NBO) and subsequent natural resonance theory (NRT) application or by the quantum theory of atoms in molecules (QTAIM), is reinvestigated. It is shown that within the framework of QTAIM, the question as to whether for a given molecule two atoms are bonded or not is only meaningful in the context of a well-defined reference geometry. The localized-orbital-locator (LOL) is applied to map out patterns in covalent bonding interaction, and produces results that are consistent for a variety of reference geometries. Furthermore, LOL interpretations are in accord with NBO/NRT, and assist in an interpretation in terms of covalent bonding. PMID:19090572

  8. 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

  9. Deep localized distortion of alternating bonds and reduced transport of charged carriers in conjugated polymers under photoexcitation

    NASA Astrophysics Data System (ADS)

    Wang, Cong; Jiang, De-Yao; Chen, Ren-Ai; Li, Sheng; George, Thomas F.

    2014-12-01

    In a real bulk heterojunction polymer solar cell, after exciton separation in the heterojunction, the resulting negatively-charged carrier, a polaron, moves along the polymer chain of the acceptor, which is believed to be of significance for the charged carrier transport properties in a polymer solar cell. During the negative polaron transport, due to the external light field, the polaron, which is re-excited and induces deep localization, also forms a new local distortion of the alternating bonds. It is revealed that the excited polaron moves more slowly than the ground-state polaron. Furthermore, the velocity of the polaron moving along the polymer chain is crucially dependent on the photoexcitation. With an increase in the intensity of the optical field, the localization of the excited polaron will be deepened, with a decrease of the polaron's velocity. It is discovered that, for a charged carrier, photoexcitation is a significant factor in reducing the efficiency during the charged carrier transport in polymer solar cells. Mostly, the deep trapping effect of charged carrier in composite conjugated polymer solar cell presents an opportunity for the future application in nanoscale memory and imaging devices.

  10. High charge mobility in two-dimensional percolative networks of PbSe quantum dots connected by atomic bonds

    PubMed Central

    Evers, Wiel H.; Schins, Juleon M.; Aerts, Michiel; Kulkarni, Aditya; Capiod, Pierre; Berthe, Maxime; Grandidier, Bruno; Delerue, Christophe; van der Zant, Herre S. J.; van Overbeek, Carlo; Peters, Joep L.; Vanmaekelbergh, Daniel; Siebbeles, Laurens D. A.

    2015-01-01

    Two-dimensional networks of quantum dots connected by atomic bonds have an electronic structure that is distinct from that of arrays of quantum dots coupled by ligand molecules. We prepared atomically coherent two-dimensional percolative networks of PbSe quantum dots connected via atomic bonds. Here, we show that photoexcitation leads to generation of free charges that eventually decay via trapping. The charge mobility probed with an AC electric field increases with frequency from 150±15 cm2 V−1 s−1 at 0.2 terahertz to 260±15 cm2 V−1 s−1 at 0.6 terahertz. Gated four-probe measurements yield a DC electron mobility of 13±2 cm2 V−1 s−1. The terahertz mobilities are much higher than for arrays of quantum dots coupled via surface ligands and are similar to the highest DC mobilities reported for PbSe nanowires. The terahertz mobility increases only slightly with temperature in the range of 15–290 K. The extent of straight segments in the two-dimensional percolative networks limits the mobility, rather than charge scattering by phonons. PMID:26400049

  11. NUCLEOPHILIC ADDITION TO ACTIVATED DOUBLE BONDS: PREDICTION OF REACTIVITY FROM THE LAPLACIAN OF CHARGE DENSITY

    EPA Science Inventory

    The reactivities of a series of molecules in a Michael addition reaction are analyzed on the basis of properties expressed in the Laplacian of the charge density distribution. he charge densities of structurally optimized acrylic acid (AA), methacrylic acid (MAA), acrylonitrile (...

  12. Charge-dependent non-bonded interaction methods for use in quantum mechanical modeling of condensed phase reactions

    NASA Astrophysics Data System (ADS)

    Kuechler, Erich R.

    Molecular modeling and computer simulation techniques can provide detailed insight into biochemical phenomena. This dissertation describes the development, implementation and parameterization of two methods for the accurate modeling of chemical reactions in aqueous environments, with a concerted scientific effort towards the inclusion of charge-dependent non-bonded non-electrostatic interactions into currently used computational frameworks. The first of these models, QXD, modifies interactions in a hybrid quantum mechanical/molecular (QM/MM) mechanical framework to overcome the current limitations of 'atom typing' QM atoms; an inaccurate and non-intuitive practice for chemically active species as these static atom types are dictated by the local bonding and electrostatic environment of the atoms they represent, which will change over the course of the simulation. The efficacy QXD model is demonstrated using a specific reaction parameterization (SRP) of the Austin Model 1 (AM1) Hamiltonian by simultaneously capturing the reaction barrier for chloride ion attack on methylchloride in solution and the solvation free energies of a series of compounds including the reagents of the reaction. The second, VRSCOSMO, is an implicit solvation model for use with the DFTB3/3OB Hamiltonian for biochemical reactions; allowing for accurate modeling of ionic compound solvation properties while overcoming the discontinuous nature of conventional PCM models when chemical reaction coordinates. The VRSCOSMO model is shown to accurately model the solvation properties of over 200 chemical compounds while also providing smooth, continuous reaction surfaces for a series of biologically motivated phosphoryl transesterification reactions. Both of these methods incorporate charge-dependent behavior into the non-bonded interactions variationally, allowing the 'size' of atoms to change in meaningful ways with respect to changes in local charge state, as to provide an accurate, predictive and

  13. 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

  14. Intermolecular hydrogen bond complexes by in situ charge transfer complexation of o-tolidine with picric and chloranilic acids

    NASA Astrophysics Data System (ADS)

    Refat, Moamen S.; Saad, Hosam A.; Adam, Abdel Majid A.

    2011-08-01

    A two new charge transfer complexes formed from the interactions between o-tolidine (o-TOL) and picric (PA) or chloranilic (CA) acids, with the compositions, [(o-TOL)(PA) 2] and [(o-TOL)(CA) 2] have been prepared. The 13C NMR, 1H NMR, 1H-Cosy, and IR show that the charge-transfer chelation occurs via the formation of chain structures O-H⋯N intermolecular hydrogen bond between 2NH 2 groups of o-TOL molecule and OH group in each PA or CA units. Photometric titration measurements concerning the two reactions in methanol were performed and the measurements show that the donor-acceptor molar ratio was found to be 1:2 using the modified Benesi-Hildebrand equation. The spectroscopic data were discussed in terms of formation constant, molar extinction coefficient, oscillator strength, dipole moment, standard free energy, and ionization potential. Thermal behavior of both charge transfer complexes showed that the complexes were more stable than their parents. The thermodynamic parameters were estimated from the differential thermogravimetric curves. The results indicated that the formation of molecular charge transfer complexes is spontaneous and endothermic.

  15. Putative Hydrogen Bond to Tyrosine M208 in Photosynthetic Reaction Centers from Rhodobacter capsulatus Significantly Slows Primary Charge Separation

    PubMed Central

    2015-01-01

    Slow, ∼50 ps, P* → P+HA– electron transfer is observed in Rhodobacter capsulatus reaction centers (RCs) bearing the native Tyr residue at M208 and the single amino acid change of isoleucine at M204 to glutamic acid. The P* decay kinetics are unusually homogeneous (single exponential) at room temperature. Comparative solid-state NMR of [4′-13C]Tyr labeled wild-type and M204E RCs show that the chemical shift of Tyr M208 is significantly altered in the M204E mutant and in a manner consistent with formation of a hydrogen bond to the Tyr M208 hydroxyl group. Models based on RC crystal structure coordinates indicate that if such a hydrogen bond is formed between the Glu at M204 and the M208 Tyr hydroxyl group, the −OH would be oriented in a fashion expected (based on the calculations by Alden et al., J. Phys. Chem.1996, 100, 16761–16770) to destabilize P+BA– in free energy. Alteration of the environment of Tyr M208 and BA by Glu M204 via this putative hydrogen bond has a powerful influence on primary charge separation. PMID:24902471

  16. Effect of Polar Environments on the Aluminum Oxide Shell Surrounding Aluminum Particles: Simulations of Surface Hydroxyl Bonding and Charge.

    PubMed

    Padhye, Richa; Aquino, Adelia J A; Tunega, Daniel; Pantoya, Michelle L

    2016-06-01

    Density functional theory (DFT) calculations were performed to understand molecular variations on an alumina surface due to exposure to a polar environment. The analysis has strong implications for the reactivity of aluminum (Al) particles passivated by an alumina shell. Recent studies have shown a link between the carrier fluid used for Al powder intermixing and the reactivity of Al with fluorine containing reactive mixtures. Specifically, flame speeds show a threefold increase when polar liquids are used to intermix aluminum and fluoropolymer powder mixtures. It was hypothesized that the alumina lattice structure could be transformed due to hydrogen bonding forces exerted by the environment that induce modified bond distances and charges and influence reactivity. In this study, the alumina surface was analyzed using DFT calculations and model clusters as isolated systems embedded in polar environments (acetone and water). The conductor-like screening model (COSMO) was used to mimic environmental effects on the alumina surface. Five defect models for specific active -OH sites were investigated in terms of structures and vibrational -OH stretching frequencies. The observed changes of the surface OH sites invoked by the polar environment were compared to the bare surface. The calculations revealed a strong connection between the impact of carrier fluid polarity on the hydrogen bonding forces between the surface OH sites and surrounding species. Changes were observed in the OH characteristic properties such as OH distances (increase), atomic charges (increase), and OH stretching frequencies (decrease); these consequently improve OH surface reactivity. The difference between medium (acetone) and strong (water) polar environments was minimal in the COSMO approximation. PMID:27175545

  17. Electron-flux infrared response to varying π-bond topology in charged aromatic monomers.

    PubMed

    Álvaro Galué, Héctor; Oomens, Jos; Buma, Wybren Jan; Redlich, Britta

    2016-01-01

    The interaction of delocalized π-electrons with molecular vibrations is key to charge transport processes in π-conjugated organic materials based on aromatic monomers. Yet the role that specific aromatic motifs play on charge transfer is poorly understood. Here we show that the molecular edge topology in charged catacondensed aromatic hydrocarbons influences the Herzberg-Teller coupling of π-electrons with molecular vibrations. To this end, we probe the radical cations of picene and pentacene with benchmark armchair- and zigzag-edges using infrared multiple-photon dissociation action spectroscopy and interpret the recorded spectra via quantum-chemical calculations. We demonstrate that infrared bands preserve information on the dipolar π-electron-flux mode enhancement, which is governed by the dynamical evolution of vibronically mixed and correlated one-electron configuration states. Our results reveal that in picene a stronger charge π-flux is generated than in pentacene, which could justify the differences of electronic properties of armchair- versus zigzag-type families of technologically relevant organic molecules. PMID:27577323

  18. Demystifying Introductory Chemistry. Part 3: Ionization Energies, Electronegativity, Polar Bonds, and Partial Charges.

    ERIC Educational Resources Information Center

    Spencer, James; And Others

    1996-01-01

    Shows how ionization energies provide a convenient method for obtaining electronegativity values that is simpler than the conventional methods. Demonstrates how approximate atomic charges can be calculated for polar molecules and how this method of determining electronegativities may lead to deeper insights than are typically possible for the…

  19. Computational evaluations of charge coupling and hydrogen bonding in the active site of a family 7 cellobiohydrolase.

    PubMed

    Granum, David M; Vyas, Shubham; Sambasivarao, Somisetti V; Maupin, C Mark

    2014-01-16

    Solution pH and the pKa values of ionizable residues are critical factors known to influence enzyme catalysis, structural stability, and dynamical fluctuations. Presented here is an exhaustive computational study utilizing long time constant pH molecular dynamics, pH replica exchange simulations, and kinetic modeling to evaluate pH-dependent conformations, charge dynamics, residue pKa values, and the catalytic activity-pH profile for cellobiohydrolase Cel7B from Melanocarpus albomyces . The predicted pKa values support the role of Glu212 as the catalytic nucleophile and Glu217 as the acid-base residue. The presence of a charge-correlated active site and an extensive hydrogen bonding network is found to be critical in enabling favorable residue orientations for catalysis and shuttling excess protons around the active site. Clusters of amino acids are identified that act in concert to effectively modulate the optimal pH for catalysis while elevating the overall catalytic rate with respect to a noncoupled system. The work presented here demonstrates the complex and critical role of coupled ionizable residues to the proper functioning of cellobiohydrolase Cel7B, functionally related glycosyl hydrolases, and enzymes in general. The simulations also support the use of the CpHMD for the accurate prediction of residue pKa values and to evaluate the impact of pH on protein structure and charge dynamics. PMID:24359013

  20. Raman Spectra of Liquid Water from Ab Initio Molecular Dynamics: Vibrational Signatures of Charge Fluctuations in the Hydrogen Bond Network.

    PubMed

    Wan, Quan; Spanu, Leonardo; Galli, Giulia A; Gygi, François

    2013-09-10

    We report the first ab initio simulations of the Raman spectra of liquid water, obtained by combining first principles molecular dynamics and density functional perturbation theory. Our computed spectra are in good agreement with experiments, especially in the low frequency region. We also describe a systematic strategy to analyze the Raman intensities, which is of general applicability to molecular solids and liquids, and it is based on maximally localized Wannier functions and effective molecular polarizabilities. Our analysis revealed the presence of intermolecular charge fluctuations accompanying the hydrogen bond (HB) stretching modes at 270 cm(-1), in spite of the absence of any Raman activity in the isotropic spectrum. We also found that charge fluctuations partly contribute to the 200 cm(-1) peak in the anisotropic spectrum, thus providing insight into the controversial origin of such peak. Our results highlighted the importance of taking into account electronic effects in interpreting the Raman spectra of liquid water and the key role of charge fluctuations within the HB network; they also pointed at the inaccuracies of models using constant molecular polarizabilities to describe the Raman response of liquid water. PMID:26592405

  1. Transient luminescence induced by electrical refilling of charge carrier traps of dislocation network at hydrophilically bonded Si wafers interface

    SciTech Connect

    Bondarenko, Anton; Vyvenko, Oleg

    2014-02-21

    Dislocation network (DN) at hydrophilically bonded Si wafers interface is placed in space charge region (SCR) of a Schottky diode at a depth of about 150 nm from Schottky electrode for simultaneous investigation of its electrical and luminescent properties. Our recently proposed pulsed traps refilling enhanced luminescence (Pulsed-TREL) technique based on the effect of transient luminescence induced by refilling of charge carrier traps with electrical pulses is further developed and used as a tool to establish DN energy levels responsible for D1 band of dislocation-related luminescence in Si (DRL). In present work we do theoretical analysis and simulation of traps refilling kinetics dependence on refilling pulse magnitude (Vp) in two levels model: shallow and deep. The influence of initial charge state of deep level on shallow level occupation-Vp dependence is discussed. Characteristic features predicted by simulations are used for Pulsed-TREL experimental results interpretation. We conclude that only shallow (∼0.1 eV from conduction and valence band) energetic levels in the band gap participate in D1 DRL.

  2. 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.

  3. 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.

  4. S···O chalcogen bonding in sulfa drugs: insights from multipole charge density and X-ray wavefunction of acetazolamide.

    PubMed

    Thomas, Sajesh P; Jayatilaka, Dylan; Guru Row, T N

    2015-10-14

    Experimental charge density analysis combined with the quantum crystallographic technique of X-ray wavefunction refinement (XWR) provides quantitative insights into the intra- and intermolecular interactions formed by acetazolamide, a diuretic drug. Firstly, the analysis of charge density topology at the intermolecular level shows the presence of exceptionally strong interaction motifs such as a DDAA-AADD (D-donor, A-acceptor) type quadruple hydrogen bond motif and a sulfonamide dimer synthon. The nature and strength of intra-molecular S···O chalcogen bonding have been characterized using descriptors from the multipole model (MM) and XWR. Although pure geometrical criteria suggest the possibility of two intra-molecular S···O chalcogen bonded ring motifs, only one of them satisfies the "orbital geometry" so as to exhibit an interaction in terms of an electron density bond path and a bond critical point. The presence of 'σ-holes' on the sulfur atom leading to the S···O chalcogen bond has been visualized on the electrostatic potential surface and Laplacian isosurfaces close to the 'reactive surface'. The electron localizability indicator (ELI) and Roby bond orders derived from the 'experimental wave function' provide insights into the nature of S···O chalcogen bonding. PMID:26365207

  5. Bond Dissociation Energies of the Tungsten Fluorides and Their Singly-Charged Ions: A Density Functional Survey

    NASA Technical Reports Server (NTRS)

    Dyall, Kenneth G.; Arnold, James (Technical Monitor)

    1999-01-01

    The dissociation of WF6 and the related singly-charged cations and anions into the lower fluorides and fluorine atoms has been investigated theoretically using density functional theory (B3LYP) and relativistic effective core potentials, with estimates of spin-orbit effects included using a simple model. The inclusion of spin-orbit is essential for a correct description of the thermochemistry. The total atomization energy of the neutral and anionic WF6 is reproduced to within 25 kcal/mol, but comparison of individual bond dissociation energies with available experimental data shows discrepancies of up to 10 kcal/mol. The results are nevertheless useful to help resolve discrepancies in experimental data and provide estimates of missing data.

  6. Adsorption of charged and neutral polymer chains on silica surfaces: The role of electrostatics, volume exclusion, and hydrogen bonding

    NASA Astrophysics Data System (ADS)

    Spruijt, Evan; Biesheuvel, P. M.; de Vos, Wiebe M.

    2015-01-01

    We develop an off-lattice (continuum) model to describe the adsorption of neutral polymer chains and polyelectrolytes to surfaces. Our continuum description allows taking excluded volume interactions between polymer chains and ions directly into account. To implement those interactions, we use a modified hard-sphere equation of state, adapted for mixtures of connected beads. Our model is applicable to neutral, charged, and ionizable surfaces and polymer chains alike and accounts for polarizability effects of the adsorbed layer and chemical interactions between polymer chains and the surface. We compare our model predictions to data of a classical system for polymer adsorption: neutral poly(N -vinylpyrrolidone) (PVP) on silica surfaces. The model shows that PVP adsorption on silica is driven by surface hydrogen bonding with an effective maximum binding energy of about 1.3 kBT per PVP segment at low p H . As the p H increases, the Si-OH groups become increasingly dissociated, leading to a lower capacity for H bonding and simultaneous counterion accumulation and volume exclusion close to the surface. Together these effects result in a characteristic adsorption isotherm, with the adsorbed amount dropping sharply at a critical p H . Using this model for adsorption data on silica surfaces cleaned by either a piranha solution or an O2 plasma, we find that the former have a significantly higher density of silanol groups.

  7. Chemical bonding and charge redistribution - Valence band and core level correlations for the Ni/Si, Pd/Si, and Pt/Si systems

    NASA Technical Reports Server (NTRS)

    Grunthaner, P. J.; Grunthaner, F. J.; Madhukar, A.

    1982-01-01

    Via a systematic study of the correlation between the core and valence level X-ray photoemission spectra, the nature of the chemical bonding and charge redistribution for bulk transition metal silicides has been examined. Particular emphasis is placed on Pt2Si and PtSi. It is observed that the strength of the metal (d)-silicon (p) interaction increases in the order Ni2Si, Pd2Si, Pt2Si. It is also observed that both the metal and silicon core lines shift to higher binding energy as the silicides are formed. The notion of charge redistribution for metallic bonds is invoked to explain these data.

  8. 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.

  9. Femtosecond Hydrogen Bond Dynamics of Bulk-like and Bound Water at Positively and Negatively Charged Lipid Interfaces Revealed by 2D HD-VSFG Spectroscopy.

    PubMed

    Singh, Prashant Chandra; Inoue, Ken-Ichi; Nihonyanagi, Satoshi; Yamaguchi, Shoichi; Tahara, Tahei

    2016-08-26

    Interfacial water in the vicinity of lipids plays an important role in many biological processes, such as drug delivery, ion transportation, and lipid fusion. Hence, molecular-level elucidation of the properties of water at lipid interfaces is of the utmost importance. We report the two-dimensional heterodyne-detected vibrational sum frequency generation (2D HD-VSFG) study of the OH stretch of HOD at charged lipid interfaces, which shows that the hydrogen bond dynamics of interfacial water differ drastically, depending on the lipids. The data indicate that the spectral diffusion of the OH stretch at a positively charged lipid interface is dominated by the ultrafast (<∼100 fs) component, followed by the minor sub-picosecond slow dynamics, while the dynamics at a negatively charged lipid interface exhibit sub-picosecond dynamics almost exclusively, implying that fast hydrogen bond fluctuation is prohibited. These results reveal that the ultrafast hydrogen bond dynamics at the positively charged lipid-water interface are attributable to the bulk-like property of interfacial water, whereas the slow dynamics at the negatively charged lipid interface are due to bound water, which is hydrogen-bonded to the hydrophilic head group. PMID:27482947

  10. Molecular geometry, vibrational frequencies, infrared intensities and CN effective bond charges in a series of simple nitrile compounds: HF/6-31+G(d,p) molecular orbital study

    NASA Astrophysics Data System (ADS)

    Dudev, Todor; Bobadova-Parvanova, Petia; Pencheva, Daniela; Galabov, Boris

    1997-12-01

    The structural and vibrational spectroscopic parameters of a series of simple nitrile compounds were evaluated by HF/6-31+G(d,p) ab initio quantum mechanical calculations. The series includes HCN, FCN, CICN, CH 2FCN, CH 2CICN, CH 3CN, CF 3CN, CCl 3CN, HOCN, HSCN and NH 2CN. The theoretical infrared intensities were transformed into quantities associated with the charge distribution and dynamics in the molecules following the formalism of the effective bond charge method. Satisfactory linear relations were found between the effective bond charges and bond lengths, as well as between the bond charges and the molecular electrostatic potential at the nitrogen atom.

  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. Trioxorhenium and trioxotechnetium as strong acceptor groups. 3. Charge transfer and bonding energetics in O{sub 3}M-M(CO){sub 5} (M = Re, Tc)

    SciTech Connect

    Costas, M.; Poblet, J.M.; Rohmer, M.M.; Benard, M.

    1995-01-04

    The bonding in O{sub 3}M-M(CO){sub 5} has been studied by ab initio SCF, two-configuration SCF, and CI methods for M = Re and Tc. Calculations indicate that these complexes are highly polar. The nature of the charge transfer in these complexes is considered.

  13. Quantum theory of atoms in molecules/charge-charge flux-dipole flux models for fundamental vibrational intensity changes on H-bond formation of water and hydrogen fluoride

    SciTech Connect

    Silva, Arnaldo F.; Richter, Wagner E.; Bruns, Roy E.; Terrabuio, Luiz A.; Haiduke, Roberto L. A.

    2014-02-28

    The Quantum Theory of Atoms In Molecules/Charge-Charge Flux-Dipole Flux (QTAIM/CCFDF) model has been used to investigate the electronic structure variations associated with intensity changes on dimerization for the vibrations of the water and hydrogen fluoride dimers as well as in the water-hydrogen fluoride complex. QCISD/cc-pVTZ wave functions applied in the QTAIM/CCFDF model accurately provide the fundamental band intensities of water and its dimer predicting symmetric and antisymmetric stretching intensity increases for the donor unit of 159 and 47 km mol{sup −1} on H-bond formation compared with the experimental values of 141 and 53 km mol{sup −1}. The symmetric stretching of the proton donor water in the dimer has intensity contributions parallel and perpendicular to its C{sub 2v} axis. The largest calculated increase of 107 km mol{sup −1} is perpendicular to this axis and owes to equilibrium atomic charge displacements on vibration. Charge flux decreases occurring parallel and perpendicular to this axis result in 42 and 40 km mol{sup −1} total intensity increases for the symmetric and antisymmetric stretches, respectively. These decreases in charge flux result in intensity enhancements because of the interaction contributions to the intensities between charge flux and the other quantities. Even though dipole flux contributions are much smaller than the charge and charge flux ones in both monomer and dimer water they are important for calculating the total intensity values for their stretching vibrations since the charge-charge flux interaction term cancels the charge and charge flux contributions. The QTAIM/CCFDF hydrogen-bonded stretching intensity strengthening of 321 km mol{sup −1} on HF dimerization and 592 km mol{sup −1} on HF:H{sub 2}O complexation can essentially be explained by charge, charge flux and their interaction cross term. Atomic contributions to the intensities are also calculated. The bridge hydrogen atomic contributions alone

  14. 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.

  15. 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

  16. 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.…

  17. Spectroscopic investigation and computational analysis of charge transfer hydrogen bonded reaction between 3-aminoquinoline with chloranilic acid in 1:1 stoichiometric ratio

    NASA Astrophysics Data System (ADS)

    Al-Ahmary, Khairia M.; Alenezi, Maha S.; Habeeb, Moustafa M.

    2015-10-01

    Charge transfer hydrogen bonded reaction between the electron donor (proton acceptor) 3-aminoquinoline with the electron acceptor (proton donor) chloranilic acid (H2CA) has been investigated experimentally and theoretically. The experimental work included the application of UV-vis spectroscopy to identify the charge transfer band of the formed complex, its molecular composition as well as estimating its formation constants in different solvent included acetonitrile (AN), methanol (MeOH), ethanol (EtOH) and chloroform (CHL). It has been recorded the presence of new absorption bands in the range 500-550 nm attributing to the formed complex. The molecular composition of the HBCT complex was found to be 1:1 (donor:acceptor) in all studied solvents based on continuous variation and photometric titration methods. In addition, the calculated formation constants from Benesi-Hildebrand equation recorded high values, especially in chloroform referring to the formation of stable HBCT complex. Infrared spectroscopy has been applied for the solid complex where formation of charge and proton transfer was proven in it. Moreover, 1H and 13C NMR spectroscopies were used to characterize the formed complex where charge and proton transfers were reconfirmed. Computational analysis included the use of GAMESS computations as a package of ChemBio3D Ultr12 program were applied for energy minimization and estimation of the stabilization energy for the produced complex. Also, geometrical parameters (bond lengths and bond angles) of the formed HBCT complex were computed and analyzed. Furthermore, Mullikan atomic charges, molecular potential energy surface, HOMO and LUMO molecular orbitals as well as assignment of the electronic spectra of the formed complex were presented. A full agreement between experimental and computational analysis has been found especially in the existence of the charge and proton transfers and the assignment of HOMO and LUMO molecular orbitals in the formed complex as

  18. Catching the role of anisotropic electronic distribution and charge transfer in halogen bonded complexes of noble gases.

    PubMed

    Bartocci, Alessio; Belpassi, Leonardo; Cappelletti, David; Falcinelli, Stefano; Grandinetti, Felice; Tarantelli, Francesco; Pirani, Fernando

    2015-05-14

    The systems studied in this work are gas-phase weakly bound adducts of the noble-gas (Ng) atoms with CCl4 and CF4. Their investigation was motivated by the widespread current interest for the intermolecular halogen bonding (XB), a structural motif recognized to play a role in fields ranging from elementary processes to biochemistry. The simulation of the static and dynamic behaviors of complex systems featuring XB requires the formulation of reliable and accurate model potentials, whose development relies on the detailed characterization of strength and nature of the interactions occurring in simple exemplary halogenated systems. We thus selected the prototypical Ng-CCl4 and Ng-CF4 and performed high-resolution molecular beam scattering experiments to measure the absolute scale of their intermolecular potentials, with high sensitivity. In general, we expected to probe typical van der Waals interactions, consisting of a combination of size (exchange) repulsion with dispersion/induction attraction. For the He/Ne-CF4, the analysis of the glory quantum interference pattern, observable in the velocity dependence of the integral cross section, confirmed indeed this expectation. On the other hand, for the He/Ne/Ar-CCl4, the scattering data unravelled much deeper potential wells, particularly for certain configurations of the interacting partners. The experimental data can be properly reproduced only including a shifting of the repulsive wall at shorter distances, accompanied by an increased role of the dispersion attraction, and an additional short-range stabilization component. To put these findings on a firmer ground, we performed, for selected geometries of the interacting complexes, accurate theoretical calculations aimed to evaluate the intermolecular interaction and the effects of the complex formation on the electron charge density of the constituting moieties. It was thus ascertained that the adjustments of the potential suggested by the analysis of the

  19. Catching the role of anisotropic electronic distribution and charge transfer in halogen bonded complexes of noble gases

    SciTech Connect

    Bartocci, Alessio; Cappelletti, David; Pirani, Fernando; Belpassi, Leonardo; Falcinelli, Stefano; Grandinetti, Felice; Tarantelli, Francesco

    2015-05-14

    The systems studied in this work are gas-phase weakly bound adducts of the noble-gas (Ng) atoms with CCl{sub 4} and CF{sub 4}. Their investigation was motivated by the widespread current interest for the intermolecular halogen bonding (XB), a structural motif recognized to play a role in fields ranging from elementary processes to biochemistry. The simulation of the static and dynamic behaviors of complex systems featuring XB requires the formulation of reliable and accurate model potentials, whose development relies on the detailed characterization of strength and nature of the interactions occurring in simple exemplary halogenated systems. We thus selected the prototypical Ng-CCl{sub 4} and Ng-CF{sub 4} and performed high-resolution molecular beam scattering experiments to measure the absolute scale of their intermolecular potentials, with high sensitivity. In general, we expected to probe typical van der Waals interactions, consisting of a combination of size (exchange) repulsion with dispersion/induction attraction. For the He/Ne-CF{sub 4}, the analysis of the glory quantum interference pattern, observable in the velocity dependence of the integral cross section, confirmed indeed this expectation. On the other hand, for the He/Ne/Ar-CCl{sub 4}, the scattering data unravelled much deeper potential wells, particularly for certain configurations of the interacting partners. The experimental data can be properly reproduced only including a shifting of the repulsive wall at shorter distances, accompanied by an increased role of the dispersion attraction, and an additional short-range stabilization component. To put these findings on a firmer ground, we performed, for selected geometries of the interacting complexes, accurate theoretical calculations aimed to evaluate the intermolecular interaction and the effects of the complex formation on the electron charge density of the constituting moieties. It was thus ascertained that the adjustments of the potential

  20. Catching the role of anisotropic electronic distribution and charge transfer in halogen bonded complexes of noble gases

    NASA Astrophysics Data System (ADS)

    Bartocci, Alessio; Belpassi, Leonardo; Cappelletti, David; Falcinelli, Stefano; Grandinetti, Felice; Tarantelli, Francesco; Pirani, Fernando

    2015-05-01

    The systems studied in this work are gas-phase weakly bound adducts of the noble-gas (Ng) atoms with CCl4 and CF4. Their investigation was motivated by the widespread current interest for the intermolecular halogen bonding (XB), a structural motif recognized to play a role in fields ranging from elementary processes to biochemistry. The simulation of the static and dynamic behaviors of complex systems featuring XB requires the formulation of reliable and accurate model potentials, whose development relies on the detailed characterization of strength and nature of the interactions occurring in simple exemplary halogenated systems. We thus selected the prototypical Ng-CCl4 and Ng-CF4 and performed high-resolution molecular beam scattering experiments to measure the absolute scale of their intermolecular potentials, with high sensitivity. In general, we expected to probe typical van der Waals interactions, consisting of a combination of size (exchange) repulsion with dispersion/induction attraction. For the He/Ne-CF4, the analysis of the glory quantum interference pattern, observable in the velocity dependence of the integral cross section, confirmed indeed this expectation. On the other hand, for the He/Ne/Ar-CCl4, the scattering data unravelled much deeper potential wells, particularly for certain configurations of the interacting partners. The experimental data can be properly reproduced only including a shifting of the repulsive wall at shorter distances, accompanied by an increased role of the dispersion attraction, and an additional short-range stabilization component. To put these findings on a firmer ground, we performed, for selected geometries of the interacting complexes, accurate theoretical calculations aimed to evaluate the intermolecular interaction and the effects of the complex formation on the electron charge density of the constituting moieties. It was thus ascertained that the adjustments of the potential suggested by the analysis of the

  1. The polar 2e/12c bond in phenalenyl-azaphenalenyl hetero-dimers: Stronger stacking interaction and fascinating interlayer charge transfer

    NASA Astrophysics Data System (ADS)

    Zhong, Rong-Lin; Xu, Hong-Liang; Li, Zhi-Ru

    2016-08-01

    An increasing number of chemists have focused on the two-electron/multicenter bond (2e/mc) that was first introduced to interpret the bonding mechanism of radical dimers. Herein, we report the polar two-electron/twelve center (2e/12c) bonding character in a series of phenalenyl-azaphenalenyl radical hetero-dimers. Interestingly, the bonding energy of weaker polar hetero-dimer (P-TAP) is dominated by the overlap of the two different singly occupied molecular orbital of radicals, while that of stronger polar hetero-dimer (P-HAP) is dominated by the electrostatic attraction. Results show that the difference between the electronegativity of the monomers plays a prominent role in the essential attribution of the polar 2e/12c bond. Correspondingly, a stronger stacking interaction in the hetero-dimer could be effectively achieved by increasing the difference of nitrogen atoms number between the monomers. It is worthy of note that an interesting interlayer charge transfer character is induced in the polar hetero-dimers, which is dependent on the difference between the electronegativity of the monomers. It is our expectation that the new knowledge about the bonding nature of radical hetero-dimers might provide important information for designing radical based functional materials with various applications.

  2. Adiabatic Betatron deceleration of ionospheric charged particles: a new explanation for (i) the rapid outflow of ionospheric O ions, and for (ii) the increase of plasma mass density observed in magnetospheric flux tubes during main phases of geomagnetic s

    NASA Astrophysics Data System (ADS)

    Lemaire, Joseph; Pierrard, Viviane; Darrouzet, Fabien

    2013-04-01

    Using European arrays of magnetometers and the cross-phase analysis to determine magnetic field line resonance frequencies, it has been found by Kale et al. (2009) that the plasma mass density within plasmaspheric flux tubes increased rapidly after the SSC of the Hallowe'en 2003 geomagnetic storms. These observations tend to confirm other independent experimental results, suggesting that heavy ion up-flow from the ionosphere is responsible for the observed plasma density increases during main phases of geomagnetic storms. The aim of our contribution is to point out that, during main phases, reversible Betatron effect induced by the increase of the southward Dst-magnetic field component (|Δ Bz|), diminishes slightly the perpendicular kinetic energy (W?) of charged particles spiraling along field lines. Furthermore, due to the conservation of the first adiabatic invariant (μ = Wm/ Bm) the mirror points of all ionospheric ions and electrons are lifted up to higher altitudes i.e. where the mirror point magnetic field (Bm) is slightly smaller. Note that the change of the mirror point altitude is given by: Δ hm = -1/3 (RE + hm) Δ Bm / Bm. It is independent of the ion species and it does not depend of their kinetic energy. The change of kinetic energy is determined by: Δ Wm = Wm Δ Bm / Bm. Both of these equations have been verified numerically by Lemaire et al. (2005; doi: 10.1016/S0273-1177(03)00099-1) using trajectory calculations in a simple time-dependant B-field model: i.e. the Earth's magnetic dipole, plus an increasing southward B-field component: i.e. the Dst magnetic field whose intensity becomes more and more negative during the main phase of magnetic storms. They showed that a variation of Bz (or Dst) by more than - 50 nT significantly increases the mirror point altitudes by more than 100 km which is about equal to scale height of the plasma density in the topside ionosphere where particles are almost collisionless (see Fig. 2 in Lemaire et al., 2005

  3. Charge redistribution and a shortening of the Fe--As bond at the quantum critical point of SmO1-xFxFeAs.

    PubMed

    Cheng, Jie; Dong, Peng; Xu, Wei; Liu, Shengli; Chu, Wangsheng; Chen, Xianhui; Wu, Ziyu

    2015-07-01

    Many researchers have pointed out that there is a quantum critical point (QCP) in the F-doped SmOFeAs system. In this paper, the electronic structure and local structure of the superconductive FeAs layer in SmO(1-x)FxFeAs as a function of the F-doping concentration have been investigated using Fe and As K-edge X-ray absorption spectroscopy. Experiments performed on the X-ray absorption near-edge structure showed that in the vicinity of the QCP the intensity of the pre-edge feature at the Fe-edge decreases continuously, while there is a striking rise of the shoulder-peak at the As edge, suggesting the occurrence of charge redistribution near the QCP. Further analysis on the As K-edge extended X-ray absorption fine structure demonstrated that the charge redistribution originates mostly from a shortening of the Fe-As bond at the QCP. An evident relationship between the mysterious QCP and the fundamental Fe-As bond was established, providing new insights on the interplay between QCP, charge dynamics and the local structural Fe-As bond in Fe-based superconductors. PMID:26134807

  4. 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.

  5. Classical nuclear motion coupled to electronic non-adiabatic transitions

    SciTech Connect

    Agostini, Federica; Abedi, Ali; Gross, E. K. U.

    2014-12-07

    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.

  6. A new analysis of charge transfer and polarization for ligand-metal bonding - Model studies of Al4CO and Al4NH3

    NASA Technical Reports Server (NTRS)

    Bagus, P. S.; Hermann, K.; Bauschlicher, C. W., Jr.

    1984-01-01

    The nature of the bonding of CO and NH3 ligands to Al is analyzed, and the intra-unit charge polarization and inter-unit donation for the interaction of ligands with metals are studied. The consequences of metal-to-ligand and ligand-to-metal charge transfer are separately considered by performing a constrained space orbital variation (CSOV) with the electrons of the metal member of the complex in the field of frozen ligand. The electrons of the metal atoms are then frozen in the relaxed distribution given by the CSOV SCF wave function and the ligand electrons are allowed to relax. Quantitative measures of the importance of inter-unit charge transfers and intra-unit polarization are obtained using results of SCF studies of Al4CO and Al4NH3 clusters chosen to simulate the adsorption of the ligands at an on-top side of the Al(111) surface. The electrostatic attraction of the effective dipole moments of the metal and ligand units makes an important contribution to the bond.

  7. Collision-Induced Dissociation of Fatty Acid [M - 2H + Na]- Ions: Charge-Directed Fragmentation and Assignment of Double Bond Position

    NASA Astrophysics Data System (ADS)

    Thomas, Michael C.; Altvater, Jens; Gallagher, Thomas J.; Nette, Geoffrey W.

    2014-08-01

    The collision-induced dissociation (CID) of cationic fatty acid-metal ion complexes has been extensively studied and, in general, provides rich structural information. In particular, charge-remote fragmentation processes are commonly observed allowing the assignment of double bond position. In a previous manuscript, we presented two methods to doubly deprotonate polyunsaturated fatty acids to form anionic fatty acid-sodium ion complexes, referred to as [M - 2H + Na] - ions. In the current manuscript, the CID behavior of these [M - 2H + Na] - ions is investigated for the first time. Significantly, we also present a deuterium-labeling experiment, which excludes the possibility that deprotonation occurs predominately at the α-carbon in the formation of fatty acid [M - H + NaF]- ions. This supports our original proposal where deprotonation occurs at the bis-allylic positions of polyunsaturated fatty acids. CID spectra of polyunsaturated fatty acid [M - 2H + Na]- ions display abundant product ions arising from acyl chain cleavages. Through the examination of fatty acid isomers, it is demonstrated that double bond position may be unequivocally determined for methylene-interrupted polyunsaturated fatty acids with three or more carbon-carbon double bonds. In addition, CID of [M - 2H + Na]- ions was applied to 18:3 isomers of Nannochloropsis oculata and three isomers were tentatively identified: ∆9,12,1518:3, ∆6,9,1218:3, and ∆5,8,1118:3. We propose that structurally-informative product ions are formed via charge-driven fragmentation processes at the site of the resonance-stabilized carbanion as opposed to charge-remote fragmentation processes, which could be inferred if deprotonation occurred predominately at the α-carbon.

  8. Molecular structure, natural bond analysis, vibrational and electronic spectra, surface enhanced Raman scattering and Mulliken atomic charges of the normal modes of [Mn(DDTC)2] complex.

    PubMed

    Téllez S, Claudio A; Costa, Anilton C; Mondragón, M A; Ferreira, Glaucio B; Versiane, O; Rangel, J L; Lima, G Müller; Martin, A A

    2016-12-01

    Theoretical and experimental bands have been assigned for the Fourier Transform Infrared and Raman spectra of the bis(diethyldithiocarbamate)Mn(II) complex, [Mn(DDTC)2]. The calculations have been based on the DFT/B3LYP method, second derivative spectra and band deconvolution analysis. The UV-vis experimental spectra were measured in acetonitrile solution, and the calculated electronic spectrum was obtained using the TD/B3LYP method with 6-311G(d, p) basis set for all atoms. Charge transfer bands and those d-d spin forbidden were assigned in the UV-vis spectrum. The natural bond orbital analysis was carried out using the DFT/B3LYP method and the Mn(II) hybridization leading to the planar geometry of the framework was discussed. Surface enhanced Raman scattering (SERS) was also performed. Mulliken charges of the normal modes were obtained and related to the SERS enhanced bands. PMID:27344520

  9. Effects of the surface concentration of fixed charges in C18-bonded stationary phases on the adsorption process and on the preparative chromatography of small ionizable compounds.

    PubMed

    Gritti, Fabrice; Guiochon, Georges

    2014-11-01

    The effects of the surface concentration of positive charges attached to the surface of research BEH-C18 hybrid particles on the overloaded band profiles and the adsorption isotherms of a neutral (caffeine) and a positively charged (nortryptilinium hydrochloride) compounds were measured and investigated. The inverse method (IM) of chromatography was used to determine the isotherm parameters. Three columns were packed with endcapped BEH-C18 particles doped with three different charge densities on their surfaces (LOW, MEDIUM and HIGH). Two other columns packed with unbonded, non-endcapped, and endcapped BEH-C18 particles served as standard reference materials. Minor disturbance method (MDM) experiments were conducted with acetonitrile/water mixtures in order to assess qualitatively the surface densities of the fixed positive charges. A more quantitative approach based on the solution of the linearized Poisson-Boltzmann equation and the decrease of the experimental Henry constant was also applied. The results show that the surface concentrations of the fixed charges in the LOW, MEDIUM and HIGH columns were 0.029, 0.050, and 0.064μmol/m(2), e.g., close to two orders of magnitude smaller than the surface density of bonded C18 chains (2.1μmol/m(2)). The adsorption isotherm of the ionizable compound nortryptilinium onto the BEH-C18 columns is consistent with a two-sites adsorption model. The density of the high energy sites correlates directly to the total amount of the fixed charges and isolated silanols amidst the C18-bonded chains. The amount of low energy sites reflects the specific surface area of the adsorbent. The binding constants on the high- and low-energy adsorption sites are respectively ten and two times lower on the HIGH column than on the reference endcapped column. The active sites are closer to the adsorbent surface than the weak adsorption sites. Finally, a higher production rate of ionizable compounds can be achieved in preparative chromatography with

  10. Hydrogen-Bond Networks: Strengths of Different Types of Hydrogen Bonds and An Alternative to the Low Barrier Hydrogen-Bond Proposal

    SciTech Connect

    Shokri, Alireza; Wang, Yanping; O'Doherty, George A.; Wang, Xue B.; Kass, Steven R.

    2013-11-27

    We report quantifying the strengths of different types of hydrogen bonds in hydrogen bond networks (HBNs) via measurement of the adiabatic electron detachment energy of the conjugate base of a small covalent polyol model compound (i.e., (HOCH2CH2CH(OH)CH2)2CHOH) in the gas phase and the pKa of the corresponding acid in DMSO. The latter result reveals that the hydrogen bonds to the charged center and those that are one solvation shell further away (i.e., primary and secondary) provide 5.3 and 2.5 pKa units of stabilization per hydrogen bond in DMSO. Computations indicate that these energies increase to 8.4 and 3.9 pKa units in benzene and that the total stabilizations are 16 (DMSO) and 25 (benzene) pKa units. Calculations on a larger linear heptaol (i.e., (HOCH2CH2CH(OH)CH2CH(OH)CH2)2CHOH) reveal that the terminal hydroxyl groups each contribute 0.6 pKa units of stabilization in DMSO and 1.1 pKa units in benzene. All of these results taken together indicate that the presence of a charged center can provide a powerful energetic driving force for enzyme catalysis and conformational changes such as in protein folding due to multiple hydrogen bonds in a HBN.

  11. 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

  12. 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…

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. 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).

  18. Ligand K-edge x-ray absorption spectroscopy as a probe of ligand-metal bonding: Charge donation and covalency in copper-chloride systems

    SciTech Connect

    Shadle, S.E.; Hedman, B.; Solomon, E.I.; Hodgson, K.O.

    1994-09-14

    X-ray absorption spectra (XAS) have been measured at the chloride K-edge for a series of complexes containing chloride ligands bound to open shell d{sup 9} copper ions in order to probe ligand-metal bonding. The intensity of the pre-edge feature in these spectra reflects the covalency in the half-occupied d{sub x}{sup 2-}{sub y}{sup 2-} derived molecular orbital (HOMO) of the complex. The energy of the pre-edge feature as well as the energy of the rising absorption edge provides quantitative information about the covalency of the ligand-metal interaction, the charge donated by the chloride, and the energy of the copper d-manifold. The results demonstrate that ligand K-edge XAS features can be used to obtain information about ligand-metal bonding. The results also identify the chemical basis for trends in the XAS data for the following complexes: D{sub 4h} CuCl{sub 4}{sup 2-}, D{sub 2d} CuCl{sub 4}{sup 2-}, planar trans-CuCl{sub 2-} (pdmp){sub 2} (pdmp = N-phenyl-3,5-dimethylpyrazole), square pyramidal CuCl{sub 5}{sup 3-}, the planar dimer KCuCl{sub 3}, the distorted tetrahedral dimer (Ph{sub 4}P)CuCl{sub 3}, and two dimers with mixed ligation, one containing a bridging chloride, and the other, containing terminally bound chloride. Several of these results are supported by independent spectral data or by basic ligand field concepts. A geometric distortion from square planar to distorted tetrahedral results in a decrease in the chloride-copper HOMO covalency but an increase in the total charge donation by the chlorides. While the geometry can maximize the overlap for a highly covalent HOMO, this does not necessarily reflect the overall charge donation.

  19. Adiabatic Berry phase in an atom-molecule conversion system

    SciTech Connect

    Fu Libin; Liu Jie

    2010-11-15

    We investigate the Berry phase of adiabatic quantum evolution in the atom-molecule conversion system that is governed by a nonlinear Schroedinger equation. We find that the Berry phase consists of two parts: the usual Berry connection term and a novel term from the nonlinearity brought forth by the atom-molecule coupling. The total geometric phase can be still viewed as the flux of the magnetic field of a monopole through the surface enclosed by a closed path in parameter space. The charge of the monopole, however, is found to be one third of the elementary charge of the usual quantized monopole. We also derive the classical Hannay angle of a geometric nature associated with the adiabatic evolution. It exactly equals minus Berry phase, indicating a novel connection between Berry phase and Hannay angle in contrast to the usual derivative form.

  20. The concerted action of a positive charge and hydrogen bonds dynamically regulates the pKa of the nucleophilic cysteine in the NrdH-redoxin family.

    PubMed

    Van Laer, Koen; Oliveira, Margarida; Wahni, Khadija; Messens, Joris

    2014-02-01

    NrdH-redoxins shuffle electrons from the NADPH pool in the cell to Class Ib ribonucleotide reductases, which in turn provide the precursors for DNA replication and repair. NrdH-redoxins have a CVQC active site motif and belong to the thioredoxin-fold protein family. As for other thioredoxin-fold proteins, the pK(a) of the nucleophilic cysteine of NrdH-redoxins is of particular interest since it affects the catalytic reaction rate of the enzymes. Recently, the pK(a) value of this cysteine in Corynebacterium glutamicum and Mycobacterium tuberculosis NrdH-redoxins were determined, but structural insights explaining the relatively low pK(a) remained elusive. We subjected C. glutamicum NrdH-redoxin to an extensive molecular dynamics simulation to expose the factors regulating the pK(a) of the nucleophilic cysteine. We found that the nucleophilic cysteine receives three hydrogen bonds from residues within the CVQC active site motif. Additionally, a fourth hydrogen bond with a lysine located N-terminal of the active site further lowers the cysteine pK(a). However, site-directed mutagenesis data show that the major contribution to the lowering of the cysteine pK(a) comes from the positive charge of the lysine and not from the additional Lys-Cys hydrogen bond. In 12% of the NrdH-redoxin family, this lysine is replaced by an arginine that also lowers the cysteine pK(a). All together, the four hydrogen bonds and the electrostatic effect of a lysine or an arginine located N-terminally of the active site dynamically regulate the pK(a) of the nucleophilic cysteine in NrdH-redoxins. PMID:24243781

  1. Electronic structure, bonding, charge distribution, and x-ray absorption spectra of the (001) surfaces of fluorapatite and hydroxyapatite from first principles

    NASA Astrophysics Data System (ADS)

    Rulis, Paul; Yao, Hongzhi; Ouyang, Lizhi; Ching, W. Y.

    2007-12-01

    Fluorapatite (FAP) and hydroxyapatite (HAP) are two very important bioceramic crystals. The (001) surfaces of FAP and HAP crystals are studied by ab initio density functional calculations using a supercell slab geometry. It is shown that in both crystals, the O-terminated (001) surface is more stable with calculated surface energies of 0.865 and 0.871J/m2 for FAP and HAP, respectively. In FAP, the two surfaces are symmetric. In HAP, the orientation of the OH group along the c axis reduces the symmetry such that the top and bottom surfaces are no longer symmetric. It is revealed that the atoms near the surface and subsurface are significantly relaxed especially in the case of HAP. The largest relaxations occurred via the lateral movements of the O ions at the subsurface level. The electronic structures of the surface models in the form of layer-by-layer resolved partial density of states for all the atoms show systematic variation from the surface region toward the bulk region. The calculated Mulliken effective charge on each type of atom and the bond order values between cations (Ca, P) and anions (O, F) show different charge transfers and bond strength variations from the bulk crystal values. Electron charge density calculations show that the surfaces of both FAP and HAP crystals are mostly positively charged due to the presence of Ca ions at the surface. The positively charged surfaces have implications for the absorption on apatite surfaces of water and other organic molecules in an aqueous environment which are an important part of its bioactivity. The x-ray absorption near-edge structure (XANES) spectra ( Ca-K , O-K , F-K , P-K , and P-L3 edges) of both the surface models and the bulk crystals are calculated and compared. The calculations use a supercell approach which takes into account the electron-core-hole interaction. It is shown that the site-specific XANES spectra show significant differences between atoms near the surface and in the bulk and are very

  2. Dynamic in situ fourier transform infrared measurements of chemical bonds of electrolyte solvents during the initial charging process in a Li ion battery

    NASA Astrophysics Data System (ADS)

    Hongyou, Kenichi; Hattori, Takashi; Nagai, Youko; Tanaka, Toshihiro; Nii, Hiroyuki; Shoda, Kaoru

    2013-12-01

    Solvation/desolvation and the solid electrolyte interphase (SEI) formation at a graphite electrode during the initial charging process were investigated using in situ Fourier transform infrared spectroscopy (FTIR) measurements. These measurements were developed by applying a diamond attenuated total reflectance (ATR) crystal, which probed the electrolyte solvents at the surface of the graphite electrode and provided successive FTIR spectra with high signal-to-noise ratio. The charging process was performed in the Li(reference)/electrolyte/graphite(working)/Cu cell at a voltage ranging from 3.2 to 0.0001 V vs. Li/Li+. The measurement elucidated the change in the chemical bond of the electrolyte solvents. In an early stage, the amounts of solvated and desolvated solvents changed, providing evidence that the Li+ ions were intercalated into the graphite layer. The formation of the Li alkyl carbonate that forms the SEI layer was facilitated toward the end of the charging process. Measurements were also obtained of the electrolyte with a vinylene carbonate additive, and the contribution of the additive to the electrolyte solvent reduction was investigated.

  3. Charge accumulation in the buried oxide of SOI structures with the bonded Si/SiO2 interface under γ-irradiation: effect of preliminary ion implantation

    NASA Astrophysics Data System (ADS)

    Naumova, O. V.; Fomin, B. I.; Ilnitsky, M. A.; Popov, V. P.

    2012-06-01

    In this study, we examined the effect of preliminary boron or phosphorous implantation on charge accumulation in the buried oxide of SOI-MOSFETs irradiated with γ-rays in the total dose range (D) of 105-5 × 107 rad. The buried oxide was obtained by high-temperature thermal oxidation of Si, and it was not subjected to any implantation during the fabrication process of SOI structures. It was found that implantation with boron or phosphorous ions, used in fabrication technologies of SOI-MOSFETs, increases the concentration of precursor traps in the buried oxide of SOI structures. Unlike in the case of boron implantation, phosphorous implantation leads to an increased density of states at the Si/buried SiO2 interface during subsequent γ-irradiation. In the γ-irradiated SOI-MOSFETs, the accumulated charge density and the density of surface states in the Si/buried oxide layer systems both vary in proportion to kiln D. The coefficients ki for as-fabricated and ion-implanted Si/buried SiO2 systems were evaluated. From the data obtained, it was concluded that a low density of precursor hole traps was a factor limiting the positive charge accumulation in the buried oxide of as-fabricated (non-implanted) SOI structures with the bonded Si/buried SiO2 interface.

  4. Surface enhanced Raman scattering, natural bond orbitals and Mulliken atomic charge distribution in the normal modes of diethyldithiocarbamate cadmium (II) complex, [Cd(DDTC)2

    NASA Astrophysics Data System (ADS)

    Téllez Soto, C. A.; Costa, A. C.; Versiane, O.; Lemma, T.; Machado, N. C. F.; Mondragón, M. A.; Martin, A. A.

    2015-07-01

    Theoretical and experimental bands have been assigned to the Fourier Transform Infrared (FT-IR) and FT-Raman spectra of the bis(diethyldithiocarbamate)Cd(II) complex, abbreviated as ([Cd(DDTC)2]). The calculations and spectral interpretation have been based on the DFT/B3LYP method, infrared and Raman second derivative spectra, and band deconvolution analysis to assist in the assignment of observed fundamentals. This study validated the unusual pseudo tetrahedral molecular structure formed around the Cd(II) cation. Surface-enhanced Raman scattering (SERS) was used to determine the interactions of the normal-modes of the diethyldithiocarbamate cadmium (II) complex on nano-structured silver surfaces. Natural bond orbital (NBO) analysis was also carried out to study the Cd(II) hybridization causing the pseudo tetrahedral geometry of the framework of the [Cd(DDTC)2] complex, and to confirm the charge transfer mechanisms through second order perturbation theory analysis of the Fox Matrix. In order to find out the electronic dispersion of the Mulliken atomic charges (MAC) in the normal modes, we calculated the MAC for each normal mode and correlated these values with the SERS effect. Experimental UV-Vis spectra were obtained and charge transfer bands were assigned. Good agreement between the calculated and experimental values for the vibrational and UV-Vis spectra was obtained.

  5. Surface enhanced Raman scattering, electronic spectrum, natural bond orbital, and Mulliken charge distribution in the normal modes of diethyldithiocarbamate copper (II) complex, [Cu(DDTC)2].

    PubMed

    Téllez Soto, C A; Costa, A C; Ramos, J M; Vieira, L S; Rost, N C V; Versiane, O; Rangel, J L; Mondragón, M A; Raniero, L; Martin, A A

    2013-12-01

    Surface-enhanced Raman scattering (SERS) was used to study the interactions of the normal modes of the diethyldithiocarbamate copper (II) complex, [Cu(DDTC)2] on nano-structured mixture silver-gold surfaces and on silver surfaces. The electronic spectrum of this complex was measured and the charge transfer bands were assigned through the TD-PBE1PBE procedure. Natural bond orbital (NBO) were also carried out to study the Cu(II) hybridation leading to the square planar geometry of the framework of the [Cu(DDTC)2] complex, and to study which are the donor NBO and the acceptor NBO in meaningful charge transfer through the Second Order Perturbation Theory Analysis of the Fox Matrix in NBO basis. To see the electronic dispersion, the Mulliken electronic charges (MAC) were calculated for each normal mode and correlated with the SERS effect. Full assignment of the SERS spectra was also supported by carefully analysis of the distorted geometries generated by the normal modes. PMID:23978740

  6. Surface enhanced Raman scattering, natural bond orbitals and Mulliken atomic charge distribution in the normal modes of diethyldithiocarbamate cadmium (II) complex, [Cd(DDTC)₂].

    PubMed

    Soto, C A Téllez; Costa, A C; Versiane, O; Lemma, T; Machado, N C F; Mondragón, M A; Martin, A A

    2015-07-01

    Theoretical and experimental bands have been assigned to the Fourier Transform Infrared (FT-IR) and FT-Raman spectra of the bis(diethyldithiocarbamate)Cd(II) complex, abbreviated as ([Cd(DDTC)2]). The calculations and spectral interpretation have been based on the DFT/B3LYP method, infrared and Raman second derivative spectra, and band deconvolution analysis to assist in the assignment of observed fundamentals. This study validated the unusual pseudo tetrahedral molecular structure formed around the Cd(II) cation. Surface-enhanced Raman scattering (SERS) was used to determine the interactions of the normal-modes of the diethyldithiocarbamate cadmium (II) complex on nano-structured silver surfaces. Natural bond orbital (NBO) analysis was also carried out to study the Cd(II) hybridization causing the pseudo tetrahedral geometry of the framework of the [Cd(DDTC)2] complex, and to confirm the charge transfer mechanisms through second order perturbation theory analysis of the Fox Matrix. In order to find out the electronic dispersion of the Mulliken atomic charges (MAC) in the normal modes, we calculated the MAC for each normal mode and correlated these values with the SERS effect. Experimental UV-Vis spectra were obtained and charge transfer bands were assigned. Good agreement between the calculated and experimental values for the vibrational and UV-Vis spectra was obtained. PMID:25813176

  7. A study of vibrational spectra and investigations of charge transfer and chemical bonding features of 2-chloro benzimidazole based on DFT computations

    NASA Astrophysics Data System (ADS)

    Muthunatesan, S.; Ragavendran, V.

    2015-01-01

    Benzimidazoles are bicyclic heteroatomic molecules. Polycyclic heteroatomic molecules have extensive coupling of different modes leading to strong coupling of force constants associated with the various chemical bonds of the molecules. To carry out a detailed vibrational spectroscopic analysis of such a bicyclic heteroatomic molecule, FT-IR and FT-Raman spectra of 2-chloro benzimidazole (CBZ) have been recorded in the condensed phase. Density Functional Theory calculations in the B3LYP/6-31G* level have been carried out to determine the optimized geometry and vibrational frequencies. In order to obtain a close agreement between theoretical and observed frequencies and hence to perform a reliable assignment, the theoretical DFT force field was transformed from Cartesian to local symmetry co-ordinates and then scaled empirically using SQM methodology. The SQM treatment resulted in a RMS deviation of 9.4 cm-1. For visual comparison, the observed and calculated spectra are presented on a common wavenumber scale. From the NBO analysis, the electron density (ED) charge transfers in the σ* and π* antibonding orbitals and second order delocalization energies E(2) confirms the occurrence of intramolecular charge transfer (ICT) within the molecule. The calculated Homo and Lumo energies show that charge transfer occurs within the molecule. The results obtained from the vibrational, NBO and HOMO-LUMO analyses have been properly tabulated.

  8. Host-Guest Chemistry: Oxoanion Recognition Based on Combined Charge-Assisted C-H or Halogen-Bonding Interactions and Anion⋅⋅⋅Anion Interactions Mediated by Hydrogen Bonds.

    PubMed

    González, Lidia; Zapata, Fabiola; Caballero, Antonio; Molina, Pedro; Ramírez de Arellano, Carmen; Alkorta, Ibon; Elguero, José

    2016-05-23

    Several bis-triazolium-based receptors have been synthesized and their anion-recognition capabilities have been studied. The central chiral 1,1'-bi-2-naphthol (BINOL) core features either two aryl or ferrocenyl end-capped side arms with central halogen- or hydrogen-bonding triazolium receptors. NMR spectroscopic data indicate the simultaneous occurrence of several charge-assisted aliphatic and heteroaromatic C-H noncovalent interactions and combinations of C-H hydrogen and halogen bonding. The receptors are able to selectively interact with HP2 O7 (3-) , H2 PO4 (-) , and SO4 (2-) anions, and the value of the association constant follows the sequence: HP2 O7 (3-) >SO4 (2-) >H2 PO4 (-) . The ferrocenyl end-capped 7(2+) ⋅2 BF4 (-) receptor allows recognition and differentiation of H2 PO4 (-) and HP2 O7 (3-) anions by using different channels: H2 PO4 (-) is selectively detected through absorption and emission methods and HP2 O7 (3-) by using electrochemical techniques. Significant structural results are the observation of an anion⋅⋅⋅anion interaction in the solid state (2:2 complex, 6(2+) ⋅[H2 P2 O7 ](2-) ), and a short C-I⋅⋅⋅O contact is observed in the structure of the complex [8(2+) ][SO4 ]0.5 [BF4 ]. PMID:27061729

  9. Charged particle dynamics in turbulent current sheets

    NASA Astrophysics Data System (ADS)

    Artemyev, A. V.; Vainchtein, D. L.; Neishtadt, A. I.; Zelenyi, L. M.

    2016-05-01

    We study dynamics of charged particle in current sheets with magnetic fluctuations. We use the adiabatic theory to describe the nonperturbed charged particle motion and show that magnetic field fluctuations destroy the adiabatic invariant. We demonstrate that the evolution of particle adiabatic invariant's distribution is described by a diffusion equation and derive analytical estimates of the rate of adiabatic invariant's diffusion. This rate is proportional to power density of magnetic field fluctuations. We compare analytical estimates with numerical simulations. We show that adiabatic invariant diffusion results in transient particles trapping in the current sheet. For magnetic field fluctuation amplitude a few times larger than a normal magnetic field component, more than 50% of transient particles become trapped. We discuss the possible consequences of destruction of adiabaticity of the charged particle motion on the state of the current sheets.

  10. Nature of halogen bonding. A study based on the topological analysis of the Laplacian of the electron charge density and an energy decomposition analysis.

    PubMed

    Duarte, Darío J R; Sosa, Gladis L; Peruchena, Nélida M

    2013-05-01

    In this work we investigate the nature of the Cl···N interactions in complexes formed between substituted ammonium [NHn(X3-n) (with n = 0, 1, 2, 3 and X = -CH3, -F] as Lewis bases and F-Cl molecule as Lewis acid. They have been chosen as a study case due to the wide range of variation of their binding energies, BEs. Møller-Plesset [MP2/6-311++G(2d,2p)] calculations show that the BEs for this set of complexes lie in the range from 1.27 kcal/mol (in F-Cl···NF3) to 27.62 kcal/mol [in F-Cl···N(CH3)3]. The intermolecular distribution of the electronic charge density and their L(r) = -¼∇(2)ρ(r) function have been investigated within the framework of the atoms in molecules (AIM) theory. The intermolecular interaction energy decomposition has also been analyzed using the reduced variational space (RVS) method. The topological analysis of the L(r) function reveals that the local topological properties measured at the (3,+1) critical point [in L(r) topology] are good descriptors of the strength of the halogen bonding interactions. The results obtained from energy decomposition analysis indicate that electrostatic interactions play a key role in these halogen bonding interactions. These results allow us to establish that, when the halogen atom is bonded to a group with high electron-withdrawing capacity, the electrostatic interaction between the electron cloud of the Lewis base and the halogen atom unprotected nucleus of the Lewis acid produces the formation and determines the geometry of the halogen bonded complexes. In addition, a good linear relationship has been established between: the natural logarithm of the BEs and the electrostatic interaction energy between electron charge distribution of N atom and nucleus of Cl atom, denoted as V e-n(N,Cl) within the AIM theory. PMID:23076553

  11. Stochasticity, superadiabaticity, and the theory of adiabatic invariants and guiding center motion

    SciTech Connect

    Dubin, D.H.E.; Krommes, J.A.

    1981-07-01

    The theory of adiabatic invariants is discussed within the modern framework of symplectic Hamiltonian dynamics. The distinctions between exact, adiabatic, and superadiabatic invariants are clarified. The intimate connection between adiabatic (as opposed to exact) invariance and resonant interactions between motions on disparate time scales is elucidated. For the important case of charged particle motion in a strong magnetic field, resonances between gyration, bounce motion, and an external sinusoidal perturbation are described explicitly by introducing a time-dependent symplectic formulation of the guiding center motion. Destruction of invariance is discussed for quite general situations of physical interest, including the case of a trapped particle in a tokamak.

  12. 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

  13. A theoretical study of charge-transport parameters for a hydrogen-bonded organic semiconductor: the indigo and s-indaceno [1,2-b:5,6-b‧] dithiophene-4,9-dione derivatives

    NASA Astrophysics Data System (ADS)

    Wei, Hui-Ling; Shi, Ya-Rui; Liu, Yu-Fang

    2016-06-01

    The properties of synthesized ambipolar organic semiconductor (OSC) materials, containing hydrogen bonding, i.e. the 6,6‧-dibromoindigo and the three s-indaceno [1, 2-b:5, 6-b‧] dithiophene-4,9-dione derivatives, have been systematically studied using a density functional theory. The hydrogen bonding formed between the interlayer molecules, though it does not affect the charge mobility in the same layer, influences the interorbital overlapping of HOMO and LUMO states between the layers, and influences the charge mobility directly. In addition, the hydrogen bonding between the layers may reinforce the π-π stacking and make the center-to-center distance closer, which indirectly enhances charge mobility, and can turn a monopole OSC into an ambipolar one.

  14. 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.

  15. Synthesis, spectral and thermal studies of the newly hydrogen bonded charge transfer complex of o-phenylenediamine with π acceptor picric acid

    NASA Astrophysics Data System (ADS)

    Khan, Ishaat M.; Ahmad, Afaq

    2010-10-01

    Newly proton or charge transfer complex [(OPDH) +(PA) -] was synthesized by the reaction of the donor, o-phenylenediamine (OPD) with acceptor, 2,4,6-trinitrophenol (PAH). The chemical reaction has occurred via strong hydrogen bonding followed by migration of proton from acceptor to donor. UV-vis, 1H NMR and FTIR spectra, in addition to the thermal and elemental analysis were used to confirm the proposed occurrence of the chemical reaction and to investigate the newly synthesized solid CT complex. The stoichiometry of the CT complex was found to be 1:1. The formation constant and molar extinction coefficient of the CT complex were evaluated by the Benesi-Hildebrand equation.

  16. Imaging ion-molecule reactions: Charge transfer and C-N bond formation in the C{sup +}+ NH{sub 3} system

    SciTech Connect

    Pei, Linsen; Farrar, James M.

    2012-05-28

    The velocity mapping ion imaging method is applied to the ion-molecule reactions occurring between C{sup +} and NH{sub 3}. The velocity space images are collected over the relative collision energy range from 1.5 to 3.3 eV, allowing both product kinetic energy distributions and angular distributions to be obtained from the data. The charge transfer process appears to be direct, dominated by long-range electron transfer that results in minimal deflection of the products. The product kinetic energy distributions are consistent with a process dominated by energy resonance. The kinetic energy distributions for C-N bond formation appear to scale with the total available energy, providing strong evidence that energy in the [CNH{sub 3}]{sup +} precursor to products is distributed statistically. The angular distributions for C-N bond formation show pronounced forward-backward symmetry, as expected for a complex that resembles a prolate symmetric top decaying along its symmetry axis.

  17. Photochemistry of (E)-1-(9-anthryl)-2-(4-nitrophenyl)ethene in the presence of aliphatic amines: H-bonding and charge-transfer effects.

    PubMed

    Bortolus, Pietro; Galiazzo, Guido; Gennari, Giorgio; Monti, Sandra E

    2002-06-01

    Polysubstituted aliphatic and aromatic amines and alcohols quench the fluorescence of (E)-1-(9-anthryl)-2-(4-nitrophenyl)ethene (NA). The quenching occurs without modification of the NA emission characteristics, follows a Stern-Volmer (SV) relationship and correlates with the decrease of the photoisomerization and intersystem crossing (ISC) yields. The dependence of the quenching rate constants (k(q)) on the ionization potentials suggests a charge-transfer interaction for the amines. The dependence of the k(q) values on alcohol acidity indicates the intervention of H-bonding phenomena. The interaction of primary aliphatic amines and NA in low-polarity solvents results in a broadening and a quenching of the NA emission. The quenching does not follow the SV relationship, has no effect on the E --> Z photoisomerization nor on the population of the triplet state, and increases the yield of the photobleaching reaction, especially in more polar solvents (chlorobenzene). This peculiar behaviour of primary aliphatic amines is attributed to H-bonded complexes in both the ground and the lowest excited singlet state. PMID:12856709

  18. Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid.

    PubMed

    Rury, Aaron S; Sorenson, Shayne; Dawlaty, Jahan M

    2016-03-14

    Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone, we find sub-cm(-1) oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology. PMID:26979698

  19. Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

    NASA Astrophysics Data System (ADS)

    Rury, Aaron S.; Sorenson, Shayne; Dawlaty, Jahan M.

    2016-03-01

    Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone, we find sub-cm-1 oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.

  20. Interlayer bonding in IIb chlorite

    SciTech Connect

    Bish, D.L.; Giese, R.F. Jr.

    1981-01-01

    The interlayer bond energy of a IIb-4 chlorite has been calculated as a function of layer charge, the site of the charge and the selective replacement of hydroxyl groups by fluoride ions. Long hydrogen bonds between the hydroxide sheet and the adjacent oxygens are strong and by themselves sufficient to create a stable structure. Coupled substitutions giving the 2:1 layer a negative charge and the hydroxide sheet a positive charge increase substantially the interlayer bond energy. 3 figures.

  1. 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.

  2. 8 CFR 103.6 - Surety bonds.

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... acceptable surety. (c) Cancellation—(1) Public charge bonds. A public charge bond posted for an immigrant..., provided the immigrant did not become a public charge prior to death, departure, or naturalization. The district director may cancel a public charge bond at any time if he/she finds that the immigrant is...

  3. Tetrapeptide-coumarin conjugate 3D networks based on hydrogen-bonded charge transfer complexes: gel formation and dye release.

    PubMed

    Guo, Zongxia; Gong, Ruiying; Jiang, Yi; Wan, Xiaobo

    2015-08-14

    Oligopeptide-based derivatives are important synthons for bio-based functional materials. In this article, a Gly-(L-Val)-Gly-(L-Val)-coumarin (GVGV-Cou) conjugate was synthesized, which forms 3D networks in ethanol. The gel nanostructures were characterized by UV-vis spectroscopy, FT-IR spectroscopy, X-ray diffraction (XRD), SEM and TEM. It is suggested that the formation of charge transfer (CT) complexes between the coumarin moieties is the main driving force for the gel formation. The capability of the gel to encapsulate and release dyes was explored. Both Congo Red (CR) and Methylene Blue (MB) can be trapped in the CT gel matrix and released over time. The present gel might be used as a functional soft material for guest encapsulation and release. PMID:26138931

  4. Coulombic Models in Chemical Bonding.

    ERIC Educational Resources Information Center

    Sacks, Lawrence J.

    1986-01-01

    Compares the coulumbic point charge model for hydrogen chloride with the valence bond model. It is not possible to assign either a nonpolar or ionic canonical form of the valence bond model, while the covalent-ionic bond distribution does conform to the point charge model. (JM)

  5. Photoinduced melting of charge order in a quarter-filled electron system coupled with different types of phonons

    NASA Astrophysics Data System (ADS)

    Yonemitsu, Kenji; Maeshima, Nobuya

    2007-08-01

    Photoinduced melting of charge order is calculated by using the exact many-electron wave function coupled with classically treated phonons in the one-dimensional quarter-filled Hubbard model with Peierls and Holstein types of electron-phonon couplings. The model parameters are taken from recent experiments on (EDO-TTF)2PF6 (EDO-TTF=ethylenedioxy-tetrathiafulvalene) with a (0110) charge order, where transfer integrals are modulated by molecular displacements (bond-coupled phonons) and site energies by molecular deformations (charge-coupled phonons). The charge-transfer photoexcitation from (0110) to (0200) configurations and that from (0110) to (1010) configurations have different energies. The corresponding excited states have different shapes of adiabatic potentials as a function of these two phonon amplitudes. The adiabatic potentials are shown to be useful in understanding differences in the photoinduced charge dynamics and the efficiency of melting, which depend not only on the excitation energy but also on the relative phonon frequency of the bond- and charge-coupled phonons.

  6. Which Method of Assigning Bond Orders in Lewis Structures Best Reflects Experimental Data? An Analysis of the Octet Rule and Formal Charge Systems for Period 2 and 3 Nonmetallic Compounds

    ERIC Educational Resources Information Center

    See, Ronald F.

    2009-01-01

    Two systems were evaluated for drawing Lewis structures of period 2 and 3 non-metallic compounds: the octet rule and minimization of formal charge. The test set of molecules consisted of the oxides, halides, oxohalides, oxoanions, and oxoacids of B, N, O, F, Al, P, S, and Cl. Bond orders were quantified using experimental data, including bond…

  7. Distinguishing Bonds.

    PubMed

    Rahm, Martin; Hoffmann, Roald

    2016-03-23

    The energy change per electron in a chemical or physical transformation, ΔE/n, may be expressed as Δχ̅ + Δ(VNN + ω)/n, where Δχ̅ is the average electron binding energy, a generalized electronegativity, ΔVNN is the change in nuclear repulsions, and Δω is the change in multielectron interactions in the process considered. The last term can be obtained by the difference from experimental or theoretical estimates of the first terms. Previously obtained consequences of this energy partitioning are extended here to a different analysis of bonding in a great variety of diatomics, including more or less polar ones. Arguments are presented for associating the average change in electron binding energy with covalence, and the change in multielectron interactions with electron transfer, either to, out, or within a molecule. A new descriptor Q, essentially the scaled difference between the Δχ̅ and Δ(VNN + ω)/n terms, when plotted versus the bond energy, separates nicely a wide variety of bonding types, covalent, covalent but more correlated, polar and increasingly ionic, metallogenic, electrostatic, charge-shift bonds, and dispersion interactions. Also, Q itself shows a set of interesting relations with the correlation energy of a bond. PMID:26910496

  8. Piezoelectric control of the mobility of a domain wall driven by adiabatic and non-adiabatic torques

    NASA Astrophysics Data System (ADS)

    de Ranieri, E.; Roy, P. E.; Fang, D.; Vehsthedt, E. K.; Irvine, A. C.; Heiss, D.; Casiraghi, A.; Campion, R. P.; Gallagher, B. L.; Jungwirth, T.; Wunderlich, J.

    2013-09-01

    The rich internal degrees of freedom of magnetic domain walls make them an attractive complement to electron charge for exploring new concepts of storage, transport and processing of information. Here we use the tunable internal structure of a domain wall in a perpendicularly magnetized GaMnAsP/GaAs ferromagnetic semiconductor and demonstrate devices in which piezoelectrically controlled magnetic anisotropy yields up to 500% mobility variations for an electrical-current-driven domain wall. We observe current-induced domain wall motion over a wide range of current-pulse amplitudes and report a direct observation and the piezoelectric control of the Walker breakdown separating two regimes with different mobilities. Our work demonstrates that in spin-orbit-coupled ferromagnets with weak extrinsic domain wall pinning, the piezoelectric control allows one to experimentally assess the upper and lower boundaries of the characteristic ratio of adiabatic and non-adiabatic spin-transfer torques in the current-driven domain wall motion.

  9. Velocity Map Imaging Study of Ion-Radical Chemistry: Charge Transfer and Carbon-Carbon Bond Formation in the Reactions of Allyl Radicals with C(.).

    PubMed

    Pei, Linsen; Farrar, James M

    2016-08-11

    We present an experimental and computational study of the dynamics of collisions of ground state carbon cations with allyl radicals, C3H5, at a collision energy of 2.2 eV. Charge transfer to produce the allyl cation, C3H5(+), is exoergic by 3.08 eV and proceeds via energy resonance such that the electron transfer occurs without a significant change in nuclear velocities. The products have sufficient energy to undergo the dissociation process C3H5(+) → C3H4(+) + H. Approximately 80% of the reaction products are ascribed to charge transfer, with ∼40% of those products decaying via loss of a hydrogen atom. We also observe products arising from the formation of new carbon-carbon bonds. The experimental velocity space flux distributions for the four-carbon products are symmetric about the centroid of the reactants, providing direct evidence that the products are mediated by formation of a C4H5(+) complex living at least a few rotational periods. The primary four-carbon reaction products are formed by elimination of molecular hydrogen from the C4H5(+) complex. More than 75% of the nascent C4H3(+) products decay by C-H bond cleavage to yield a C4H2(+) species. Quantum chemical calculations at the MP2/6-311+g(d,p) level of theory support the formation of a nonplanar cyclic C4H5(+) adduct that is produced when the p-orbital containing the unpaired electron on C(+) overlaps with the unpaired spin density on the terminal carbon atoms in allyl. Product formation then occurs by 1,2-elimination of molecular hydrogen from the cyclic intermediate to form a planar cyclic C4H3(+) product. The large rearrangement in geometry as the C4H3(+) products are formed is consistent with high vibrational excitation in that product and supports the observation that the majority of those products decay to form the C4H2(+) species. PMID:27434380

  10. Electronegativity Equalization and Partial Charge

    ERIC Educational Resources Information Center

    Sanderson, R. T.

    1974-01-01

    This article elaborates the relationship between covalent radius, homonuclear bond energy, and electronegativity, and sets the background for bond energy calculation by discussing the nature of heteronuclear covalent bonding on the basis of electronegativity equalization and particle charge. (DT)

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. Steam bottoming cycle for an adiabatic diesel engine

    SciTech Connect

    Poulin, E.; Demler, R.; Krepchin, I.; Walker, D.

    1984-03-01

    A study of steam bottoming cycles using adiabatic diesel engine exhaust heat projected substantial performance and economic benefits for long haul trucks. A parametric analysis of steam cycle and system component variables, system cost, size and performance was conducted. An 811 K/6.90 MPa state-of-the-art reciprocating expander steam system with a monotube boiler and radiator core condenser was selected for preliminary design. When applied to a NASA specified turbo-charged adiabatic diesel the bottoming system increased the diesel output by almost 18%. In a comparison of the costs of the diesel with bottoming system (TC/B) and a NASA specified turbocompound adiabatic diesel with after-cooling with the same total output, the annual fuel savings less the added maintenance cost was determined to cover the increased initial cost of the TC/B system in a payback period of 2.3 years. Also during this program steam bottoming system freeze protection strategies were developed, technological advances required for improved system reliability were considered and the cost and performance of advanced systems were evaluated.

  16. 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

  17. Optical characterization of 2 kF bond-charge-density wave in quasi-one-dimensional 3 /4 -filled (EDO-TTF)2 X ( X= PF6 and AsF6 )

    NASA Astrophysics Data System (ADS)

    Drozdova, Olga; Yakushi, Kyuya; Yamamoto, Kaoru; Ota, Akira; Yamochi, Hideki; Saito, Gunzi; Tashiro, Hidenori; Tanner, David B.

    2004-08-01

    We present the electronic and vibrational spectra of quasi-one-dimensional (3)/(4) -filled (EDO-TTF)2X ( EDO-TTF=ethylenedioxy-tetrathiafulvalene , X=PF6 and AsF6 ) above and below the metal-insulator phase transition ( TMI=280K for the PF6 salt and 268K for the AsF6 salt). For the low-temperature insulating phase, the pattern of both bond and charge order was identified. Almost all charge density is localized on the strongly bound central pair of 0110 tetramer giving rise to a characteristic spectrum of electronic excitations. Infrared spectra along the stacking axis show evidence of strong electron-molecular vibration coupling between the charge transfer band within the pair and some specific intramolecular vibrations. This charge order is assisted by a molecular deformation.

  18. 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.

  19. 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.

  20. 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

  1. 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

  2. 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

  3. 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

  4. Adiabatic Mach-Zehnder Interferometry on a Quantized Bose-Josephson Junction

    SciTech Connect

    Lee, Chaohong

    2006-10-13

    We propose a scheme to achieve Mach-Zehnder interferometry using a quantized Bose-Josephson junction with a negative charging energy. The quantum adiabatic evolution through a dynamical bifurcation is used to accomplish the beam splitting and recombination. The negative charging energy ensures the existence of a path-entangled state which enhances the phase measurement precision to the Heisenberg limit. A feasible detection procedure is also presented. The scheme should be realizable with current technology.

  5. 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.

  6. 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.

  7. 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.

  8. 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)

  9. 8 CFR 103.6 - Surety bonds.

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... a public charge. A bond may also be cancelled in order to allow substitution of another bond. A... surety bonds posted in immigration cases shall be executed on Form I-352, Immigration Bond, a copy of... to approve a bond, a formal agreement to extension of liability of surety, a request for delivery...

  10. 8 CFR 103.6 - Surety bonds.

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... a public charge. A bond may also be cancelled in order to allow substitution of another bond. A... surety bonds posted in immigration cases shall be executed on Form I-352, Immigration Bond, a copy of... to approve a bond, a formal agreement to extension of liability of surety, a request for delivery...

  11. 8 CFR 103.6 - Surety bonds.

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... a public charge. A bond may also be cancelled in order to allow substitution of another bond. A... surety bonds posted in immigration cases shall be executed on Form I-352, Immigration Bond, a copy of... to approve a bond, a formal agreement to extension of liability of surety, a request for delivery...

  12. 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…

  13. 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.

  14. Bond and charge-density waves in (DI-DCNQI)2Ag (DI-DCNQI=2,5-diiodo-N,N'-dicyanoquinediimine) studied by single-crystal infrared and Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Yamamoto, Kaoru; Yamamoto, Takashi; Yakushi, Kyuya; Pecile, Cesare; Meneghetti, Moreno

    2005-01-01

    The charge distribution and molecular arrangement of a quarter-filled quasi-one-dimensional system (DI-DCNQI)2Ag (DI-DCNQI=2,5-diiodo-dicyanoquinediimine) has been studied by IR and Raman spectroscopy. The charge localization of this material was believed to be a one-dimensional generalization of a Wigner crystal driven by intersite Coulomb repulsion. While charge disproportionation is confirmed via the splitting of bu modes in the infrared spectrum, the appearance of intense IR vibronic bands of ag modes strongly suggests the presence of the dimerization that is not expected by the proposed 1010 charge ordering model. In addition, the selection rules for the IR and Raman signals cannot be explained without a further symmetry reduction of the unit cell. To explain the vibrational behavior observed for a single crystal, we show that a more appropriate model for the charge ordering is 0110 ( 2kF charge-density wave and 4kF bond-order wave).

  15. 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.

  16. Dust-acoustic solitary waves in a four-component adiabatic magnetized dusty plasma

    SciTech Connect

    Akhter, T. Mannan, A.; Mamun, A. A.

    2013-07-15

    Theoretical investigation has been made on obliquely propagating dust-acoustic (DA) solitary waves (SWs) in a magnetized dusty plasma which consists of non-inertial adiabatic electron and ion fluids, and inertial negatively as well as positively charged adiabatic dust fluids. The reductive perturbation method has been employed to derive the Korteweg-de Vries equation which admits a solitary wave solution for small but finite amplitude limit. It has been shown that the basic features (speed, height, thickness, etc.) of such DA solitary structures are significantly modified by adiabaticity of plasma fluids, opposite polarity dust components, and the obliqueness of external magnetic field. The SWs have been changed from compressive to rarefactive depending on the value of {mu} (a parameter determining the number of positive dust present in this plasma model). The present investigation can be of relevance to the electrostatic solitary structures observed in various dusty plasma environments (viz. cometary tails, upper mesosphere, Jupiter's magnetosphere, etc.)

  17. Simple Bond Cleavage

    SciTech Connect

    Gary S. Groenewold

    2005-08-01

    Simple bond cleavage is a class of fragmentation reactions in which a single bond is broken, without formation of new bonds between previously unconnected atoms. Because no bond making is involved, simple bond cleavages are endothermic, and activation energies are generally higher than for rearrangement eliminations. The rate of simple bond cleavage reactions is a strong function of the internal energy of the molecular ion, which reflects a loose transition state that resembles reaction products, and has a high density of accessible states. For this reason, simple bond cleavages tend to dominate fragmentation reactions for highly energized molecular ions. Simple bond cleavages have negligible reverse activation energy, and hence they are used as valuable probes of ion thermochemistry, since the energy dependence of the reactions can be related to the bond energy. In organic mass spectrometry, simple bond cleavages of odd electron ions can be either homolytic or heterolytic, depending on whether the fragmentation is driven by the radical site or the charge site. Simple bond cleavages of even electron ions tend to be heterolytic, producing even electron product ions and neutrals.

  18. Bent Bonds and Multiple Bonds.

    ERIC Educational Resources Information Center

    Robinson, Edward A.; Gillespie, Ronald J.

    1980-01-01

    Considers carbon-carbon multiple bonds in terms of Pauling's bent bond model, which allows direct calculation of double and triple bonds from the length of a CC single bond. Lengths of these multiple bonds are estimated from direct measurements on "bent-bond" models constructed of plastic tubing and standard kits. (CS)

  19. 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.

  20. 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.

  1. 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.

  2. A Model for the Chemical Bond

    ERIC Educational Resources Information Center

    Magnasco, Valerio

    2004-01-01

    Bond stereochemistry in polyatomic hydrides is explained in terms of the principle of bond energies maximization, which yields X-H straight bonds and suggests the formation of appropriate sp hybrids on the central atom. An introduction to the electron charge distribution in molecules is given, and atomic, overlap, gross and formal charges are…

  3. 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.

  4. 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.

  5. 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.

  6. 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

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. Piezoelectric control of the mobility of a domain wall driven by adiabatic and non-adiabatic torques.

    PubMed

    De Ranieri, E; Roy, P E; Fang, D; Vehsthedt, E K; Irvine, A C; Heiss, D; Casiraghi, A; Campion, R P; Gallagher, B L; Jungwirth, T; Wunderlich, J

    2013-09-01

    The rich internal degrees of freedom of magnetic domain walls make them an attractive complement to electron charge for exploring new concepts of storage, transport and processing of information. Here we use the tunable internal structure of a domain wall in a perpendicularly magnetized GaMnAsP/GaAs ferromagnetic semiconductor and demonstrate devices in which piezoelectrically controlled magnetic anisotropy yields up to 500% mobility variations for an electrical-current-driven domain wall. We observe current-induced domain wall motion over a wide range of current-pulse amplitudes and report a direct observation and the piezoelectric control of the Walker breakdown separating two regimes with different mobilities. Our work demonstrates that in spin-orbit-coupled ferromagnets with weak extrinsic domain wall pinning, the piezoelectric control allows one to experimentally assess the upper and lower boundaries of the characteristic ratio of adiabatic and non-adiabatic spin-transfer torques in the current-driven domain wall motion. PMID:23749266

  13. Pitch-angle scattering of energetic particles with adiabatic focusing

    SciTech Connect

    Tautz, R. C.; Shalchi, A.; Dosch, A. E-mail: andreasm4@yahoo.com

    2014-10-20

    Understanding turbulent transport of charged particles in magnetized plasmas often requires a model for the description of random variations in the particle's pitch angle. The Fokker-Planck coefficient of pitch-angle scattering, which is used to describe scattering parallel to the mean magnetic field, is therefore of central importance. Whereas quasi-linear theory assumes a homogeneous mean magnetic field, such a condition is often not fulfilled, especially for high-energy particles. Here, a new derivation of the quasi-linear approach is given that is based on the unperturbed orbit found for an adiabatically focused mean magnetic field. The results show that, depending on the ratio of the focusing length and the particle's Larmor radius, the Fokker-Planck coefficient is significantly modified but agrees with the classical expression in the limit of a homogeneous mean magnetic field.

  14. 27 CFR 19.516 - Bond account.

    Code of Federal Regulations, 2010 CFR

    2010-04-01

    ... maximum penal sum, he shall maintain an account of his bond and he shall charge the bond with the amount... 27 Alcohol, Tobacco Products and Firearms 1 2010-04-01 2010-04-01 false Bond account. 19.516... Determination and Payment of Tax § 19.516 Bond account. Where the proprietor has furnished a withdrawal or...

  15. 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)

  16. 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…

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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

  3. 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.

  4. Jumps of adiabatic invariant at the separatrix of a degenerate saddle point.

    PubMed

    Artemyev, A V; Neishtadt, A I; Zelenyi, L M

    2011-12-01

    We consider a slow-fast Hamiltonian system with two degrees of freedom. One degree of freedom corresponds to slow variables, and the other one corresponds to fast variables. A characteristic ratio of the rates of change of slow and fast variables is a small parameter κ. For every fixed value of the slow variables, in the phase portrait of the fast variables there are a saddle point and separatrices passing through it. When the slow variables change, phase points may cross the separatrices. The action variable of the fast motion is an adiabatic invariant of the full system as long as a trajectory is far from the separatrices: value of the adiabatic invariant is conserved with an accuracy of order of κ on time intervals of order of 1/κ. A passage through a narrow neighborhood of the separatrices results in a jump of the adiabatic invariant. We consider a case when the saddle point is degenerate. We derive an asymptotic formula for the jump of the adiabatic invariant which turns out to be a value of order of κ(3/4) (in the case of a non-degenarate saddle point a similar jump is known to be a value of order of κ). Accumulation of these jumps after many consecutive separatrix crossings leads to the "diffusion" of the adiabatic invariant and chaotic dynamics. We verify the analytical expression for the jump of the adiabatic invariant by numerical simulations. We discuss application of the obtained results to the description of charged particle dynamics in the Earth magnetosphere. PMID:22225357

  5. Charge separation and covalent bonding in metal oxide surfaces: A local density functional study on the MgO(001) surface

    SciTech Connect

    Birkenheuer, U. ); Boettger, J.C. ); Roesch, N. )

    1994-05-01

    A first principles local density functional investigation on extended, two-dimensional periodic slab models of the MgO(001) surface is performed, using the linear combination of Gaussian-type orbitals (LCGTO) technique as implemented in the FILMS program package. Stimulated by recent theoretical evidence for a reduced charge separation in MgO(001), a detailed analysis of the charge distribution and its influence on the electrical field above the surface is carried out. Two different methods to quantify the charge separation in the ionic substrate are employed, a local one based on the topological atom approach and a global one derived from the Madelung field of the surface near potential adsorbates. Both procedures lead to a charge separation significantly (10%--20%) below the nominal ionic value of [plus minus]2 a.u. A variational atomic orbital analysis is utilized to discuss the origin of the Mg 3[ital s] and 3[ital p] structures discernible in the crystal orbitals of the MgO slab systems. They are identified as covalent magnesium valence orbital admixtures to the oxygen dominated valence bands in consistence with the reduced charge separation. Their influence on the cohesive energy of crystalline MgO, however, is found to be only 5% ([similar to]0.5 eV).

  6. Stimuli-responsive self-assembly of a naphthalene diimide by orthogonal hydrogen bonding and its coassembly with a pyrene derivative by a pseudo-intramolecular charge-transfer interaction.

    PubMed

    Das, Anindita; Ghosh, Suhrit

    2014-01-20

    A naphthalene diimide (NDI) building block containing hydrazide (H1) and hydroxy (H2) groups self-assembled into a reverse-vesicular structure in methylcyclohexane by orthogonal H-bonding and π-stacking. At an elevated temperature (LCST=43 °C), destruction of the assembled structure owing to selective dissociation of H2-H2 H bonding led to macroscopic precipitation. Further heating resulted in homogeneous redispersion of the sample at 70 °C (UCST) and the formation of a reverse-micellar structure. In the presence of a pyridine (H3)-functionalized pyrene (PY) donor, a supramolecular dyad (NDI-PY) was formed by H2-H3 H-bonding. Slow transformation into an alternate NDI-PY stack occurred by a folding process due to the charge-transfer interaction between NDI and PY. The mixed NDI-PY assembly exhibited a morphology transition from a reverse micelle (with a NDI-PY mixed-stack core) below the LCST to another reverse micelle (with a NDI core) above the UCST via a "denatured" intermediate. PMID:24376055

  7. The hydrogen bond network structure within the hydration shell around simple osmolytes: Urea, tetramethylurea, and trimethylamine-N-oxide, investigated using both a fixed charge and a polarizable water model

    NASA Astrophysics Data System (ADS)

    Kuffel, Anna; Zielkiewicz, Jan

    2010-07-01

    Despite numerous experimental and computer simulation studies, a controversy still exists regarding the effect of osmolytes on the structure of surrounding water. There is a question, to what extent some of the contradictory results may arise from differences in potential models used to simulate the system or parameters employed to describe physical properties of the mixture and interpretation of the results. Bearing this in mind, we determine two main aims of this work as follows: description of the water-water hydrogen bond network structure within the solvation layer around solute molecules (urea, trimethylamine-N-oxide, and tetramethylurea), and also comparison of rigid simple point charges (SPC) and polarizable (POL3) models of water. The following quantities have been examined: radial distribution functions of water molecules around the investigated solutes, both local and overall characteristics of the hydrogen bond network structure (using recently elaborated method), along with estimation of the mean energy of a single hydrogen bond, and also the probability distributions which describe the orientation of a single water particle plane relatively to the center of mass of the solute molecule. As an independent method for the evaluation of the degree of changes in local structural ordering, a harmonic approximation has been adopted to estimate the absolute entropy of water. It was found that within the solvation shell of the investigated solutes, the structure of hydrogen bond network changes only slightly comparing to bulk water. Therefore, we conclude that the investigated osmolyte molecules do not disturb significantly the structure of surrounding water. This conclusion was also confirmed by calculations of the absolute entropy of water using a harmonic approximation. In the immediate vicinity of the solutes, we observe that the water-water hydrogen bonds are slightly more stable; they are slightly less distorted and a little shorter than in bulk water

  8. The hydrogen bond network structure within the hydration shell around simple osmolytes: urea, tetramethylurea, and trimethylamine-N-oxide, investigated using both a fixed charge and a polarizable water model.

    PubMed

    Kuffel, Anna; Zielkiewicz, Jan

    2010-07-21

    Despite numerous experimental and computer simulation studies, a controversy still exists regarding the effect of osmolytes on the structure of surrounding water. There is a question, to what extent some of the contradictory results may arise from differences in potential models used to simulate the system or parameters employed to describe physical properties of the mixture and interpretation of the results. Bearing this in mind, we determine two main aims of this work as follows: description of the water-water hydrogen bond network structure within the solvation layer around solute molecules (urea, trimethylamine-N-oxide, and tetramethylurea), and also comparison of rigid simple point charges (SPC) and polarizable (POL3) models of water. The following quantities have been examined: radial distribution functions of water molecules around the investigated solutes, both local and overall characteristics of the hydrogen bond network structure (using recently elaborated method), along with estimation of the mean energy of a single hydrogen bond, and also the probability distributions which describe the orientation of a single water particle plane relatively to the center of mass of the solute molecule. As an independent method for the evaluation of the degree of changes in local structural ordering, a harmonic approximation has been adopted to estimate the absolute entropy of water. It was found that within the solvation shell of the investigated solutes, the structure of hydrogen bond network changes only slightly comparing to bulk water. Therefore, we conclude that the investigated osmolyte molecules do not disturb significantly the structure of surrounding water. This conclusion was also confirmed by calculations of the absolute entropy of water using a harmonic approximation. In the immediate vicinity of the solutes, we observe that the water-water hydrogen bonds are slightly more stable; they are slightly less distorted and a little shorter than in bulk water

  9. Cooperative Roles of Charge Transfer and Dispersion Terms in Hydrogen-Bonded Networks of (H2O)n, n = 6, 11, and 16

    SciTech Connect

    Iwata, Suehiro; Bandyopadhyay, Pradipta; Xantheas, Sotiris S.

    2013-08-01

    The perturbation expansion based on the locally-projected molecular orbital (LPMO PT) was applied to the study of the hydrogenbonded networks of water clusters with up to 16 molecules. Utilizing the local nature of the occupied and excited MOs on each monomer, the chargetransfer and dispersion terms are evaluated for every pair of molecules. The two terms are strongly correlated with each other for the hydrogen-bonded pairs. The strength of the hydrogen bonds in the clusters is further classified by the types of the hydrogen donor and acceptor water molecules. The relative energies evaluated with th LPMO PT among the isomers of (H2O)6, (H2O)11, and (H2O)16 agree very well with those obtained from CCSD(T) calculations with large basis sets. The binding energy of the LPMO PT is approximately free of the basis set superposition errors caused both by the orbital basis inconsistency and by the configuration basis inconsistency.

  10. 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.

  11. 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

  12. 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

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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

  19. 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.

  20. 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.

  1. 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

  2. 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.

  3. 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.

  4. 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

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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).

  14. 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.

  15. 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.

  16. Charge Disproportionation in Tetragonal La2MoO5 , a Small Band Gap Semiconductor Influenced by Direct Mo–Mo Bonding

    DOE PAGESBeta

    Colabello, Diane M.; Camino, Fernando E.; Huq, Ashfia; Hybertsen, Mark; Khalifah, Peter G.

    2014-12-31

    The structure of the novel compound La2MoO5 has been solved from powder X-ray and neutron diffraction data and belongs to the tetragonal space group P4/m (no. 83) with a = 12.6847(3) Å and c = 6.0568(2) Å and with Z = 8. It consists of equal proportions of bioctahedral (Mo2O10) and square prismatic (Mo2O8) dimers, both of which contain direct Mo-Mo bonds and are arranged in 1D chains. The Mo-Mo bond length in the Mo2O10dimers is 2.684(8) Å, while there are two types of Mo2O8 dimers with Mo-Mo bonds lengths of 2.22(2) and 2.28(2) Å. Although the average Mo oxidationmore » state in La2MoO5 is 4+, the very different Mo-Mo distances reflect the fact that the Mo2O10 dimers contain only Mo5+ (d(1)), while the prismatic Mo2O8 dimers only contain Mo3+ (d3), a result directly confirmed by density function theory calculations. This is due to the complete disproportionation of Mo4+, a phenomenon which has not previously been observed in solid-state compounds. La2MoO5 is diamagnetic, behavior which is not expected for a nonmetallic transition-metal oxide whose cation sites have an odd number of d-electrons. The resistivity displays the Arrhenius-type activated behavior expected for a semiconductor with a band gap of 0.5 eV, exhibiting an unusually small transport gap relative to other diamagnetic oxides. Diffuse reflectance studies indicate that La2MoO5 is a rare example of a stable oxide semiconductor with strong infrared absorbance. Lastly, we show that the d-orbital splitting associated with the Mo2O8 and Mo2O10 dimeric units can be rationalized using simple molecular orbital bonding concepts.« less

  17. Charge Disproportionation in Tetragonal La2MoO5 , a Small Band Gap Semiconductor Influenced by Direct Mo–Mo Bonding

    SciTech Connect

    Colabello, Diane M.; Camino, Fernando E.; Huq, Ashfia; Hybertsen, Mark; Khalifah, Peter G.

    2014-12-31

    The structure of the novel compound La2MoO5 has been solved from powder X-ray and neutron diffraction data and belongs to the tetragonal space group P4/m (no. 83) with a = 12.6847(3) Å and c = 6.0568(2) Å and with Z = 8. It consists of equal proportions of bioctahedral (Mo2O10) and square prismatic (Mo2O8) dimers, both of which contain direct Mo-Mo bonds and are arranged in 1D chains. The Mo-Mo bond length in the Mo2O10dimers is 2.684(8) Å, while there are two types of Mo2O8 dimers with Mo-Mo bonds lengths of 2.22(2) and 2.28(2) Å. Although the average Mo oxidation state in La2MoO5 is 4+, the very different Mo-Mo distances reflect the fact that the Mo2O10 dimers contain only Mo5+ (d(1)), while the prismatic Mo2O8 dimers only contain Mo3+ (d3), a result directly confirmed by density function theory calculations. This is due to the complete disproportionation of Mo4+, a phenomenon which has not previously been observed in solid-state compounds. La2MoO5 is diamagnetic, behavior which is not expected for a nonmetallic transition-metal oxide whose cation sites have an odd number of d-electrons. The resistivity displays the Arrhenius-type activated behavior expected for a semiconductor with a band gap of 0.5 eV, exhibiting an unusually small transport gap relative to other diamagnetic oxides. Diffuse reflectance studies indicate that La2MoO5 is a rare example of a stable oxide semiconductor with strong infrared absorbance. Lastly, we show that the d-orbital splitting associated with the Mo2O8 and Mo2O10 dimeric units can be rationalized using simple molecular orbital bonding concepts.

  18. Photoinduced Charge-Transfer State of 4-Carbazolyl-3-(trifluoromethyl)benzoic Acid: Photophysical Property and Application to Reduction of Carbon-Halogen Bonds as a Sensitizer.

    PubMed

    Matsubara, Ryosuke; Shimada, Toshiyuki; Kobori, Yasuhiro; Yabuta, Tatsushi; Osakai, Toshiyuki; Hayashi, Masahiko

    2016-07-20

    The photoinduced persistent intramolecular charge-transfer state of 4-carbazolyl-3-(trifluoromethyl)benzoic acid was confirmed. It showed a higher catalytic activity in terms of yield and selectivity in the photochemical reduction of alkyl halides compared to the parent carbazole. Even unactivated primary alkyl bromides could be reduced by this photocatalyst. The high catalytic activity is rationalized by considering the slower backward single-electron transfer owing to the spatial separation of the donor and acceptor subunits. PMID:27305449

  19. Adiabatic quantum pump in a zigzag graphene nanoribbon junction

    NASA Astrophysics Data System (ADS)

    Zhang, Lin

    2015-11-01

    The adiabatic electron transport is theoretically studied in a zigzag graphene nanoribbon (ZGNR) junction with two time-dependent pumping electric fields. By modeling a ZGNR p-n junction and applying the Keldysh Green’s function method, we find that a pumped charge current is flowing in the device at a zero external bias, which mainly comes from the photon-assisted tunneling process and the valley selection rule in an even-chain ZGNR junction. The pumped charge current and its ON and OFF states can be efficiently modulated by changing the system parameters such as the pumping frequency, the pumping phase difference, and the Fermi level. A ferromagnetic ZGNR device is also studied to generate a pure spin current and a fully polarized spin current due to the combined spin pump effect and the valley valve effect. Our finding might pave the way to manipulate the degree of freedom of electrons in a graphene-based electronic device. Project supported by the National Natural Science Foundation of China (Grant No. 110704033), the Natural Science Foundation of Jiangsu Province, China (Grant No. BK2010416), and the Natural Science Foundation for Colleges and Universities in Jiangsu Province, China (Grant No. 13KJB140005).

  20. Acoustic solitary waves in dusty and/or multi-ion plasmas with cold, adiabatic, and hot constituents

    SciTech Connect

    Verheest, Frank; Hellberg, Manfred A.; Kourakis, Ioannis

    2008-11-15

    Large nonlinear acoustic waves are discussed in a four-component plasma, made up of two superhot isothermal species, and two species with lower thermal velocities, being, respectively, adiabatic and cold. First a model is considered in which the isothermal species are electrons and ions, while the cooler species are positive and/or negative dust. Using a Sagdeev pseudopotential formalism, large dust-acoustic structures have been studied in a systematic way, to delimit the compositional parameter space in which they can be found, without restrictions on the charges and masses of the dust species and their charge signs. Solitary waves can only occur for nonlinear structure velocities smaller than the adiabatic dust thermal velocity, leading to a novel dust-acoustic-like mode based on the interplay between the two dust species. If the cold and adiabatic dust are oppositely charged, only solitary waves exist, having the polarity of the cold dust, their parameter range being limited by infinite compression of the cold dust. However, when the charges of the cold and adiabatic species have the same sign, solitary structures are limited for increasing Mach numbers successively by infinite cold dust compression, by encountering the adiabatic dust sonic point, and by the occurrence of double layers. The latter have, for smaller Mach numbers, the same polarity as the charged dust, but switch at the high Mach number end to the opposite polarity. Typical Sagdeev pseudopotentials and solitary wave profiles have been presented. Finally, the analysis has nowhere used the assumption that the dust would be much more massive than the ions and hence, one or both dust species can easily be replaced by positive and/or negative ions and the conclusions will apply to that plasma model equally well. This would cover a number of different scenarios, such as, for example, very hot electrons and ions, together with a mix of adiabatic ions and dust (of either polarity) or a very hot electron

  1. Bond Issues.

    ERIC Educational Resources Information Center

    Pollack, Rachel H.

    2000-01-01

    Notes trends toward increased borrowing by colleges and universities and offers guidelines for institutions that are considering issuing bonds to raise money for capital projects. Discussion covers advantages of using bond financing, how use of bonds impacts on traditional fund raising, other cautions and concerns, and some troubling aspects of…

  2. Inter-layer charge disproportionation in the dual-layer organic metal (tTTF-I)2ClO4 with unsymmetrical I···O halogen bond interactions.

    PubMed

    Shin, Kyoung-Soon; Jeannin, Olivier; Brezgunova, Mariya; Dahaoui, Slimane; Aubert, Emmanuel; Espinosa, Enrique; Auban-Senzier, Pascale; Świetlik, Roman; Frąckowiak, Arkadiusz; Fourmigué, Marc

    2014-04-14

    A mixed-valence salt of tTTF-I with ClO4(-), formulated as (tTTF-I)2ClO4, is characterized by the presence of two crystallographically independent donor molecules, segregated in different layers and linked together through I···O interactions with the ClO4(-) anion disordered at room temperature. The tTTF-I donor molecule was prepared by metallation of tTTF (trimethylene tetrathiafulvalene) followed by reaction with iodine to afford the mono and diiodo derivatives tTTF-I and tTTFI2, respectively. The crystal structure of the latter neutral tTTFI2 shows the occurrence of strong type II, II halogen bond interactions. Band structure calculations of the dual-layer structure of the 2 : 1 salt (tTTF-I)2ClO4 show co-existence of both 1D open and 2D closed Fermi surfaces. The salt undergoes a metal-insulator phase transition at T(MI) = 90 K, associated with an electronic dimensionality decrease, since already at 100 K, the 2D part of the Fermi surface transforms into 1D corrugated planes. High resolution X-ray investigations performed at 100 K, combined with multipolar refinements, indicate an approximately equivalent +0.5e charge in both donor molecules, as also deduced from the intramolecular bond distances. On the other hand, Raman spectroscopic investigations show that at ambient temperature the charge is actually distributed non-uniformly in conducting layers of tTTF-I molecules, with the identification of molecules with charges +1, +0.5, 0e, while at low temperature the charge distribution becomes essentially uniform (+0.5e), as confirmed from the X-ray high resolution data. These apparently contradictory behaviors are actually a consequence of a partial electron transfer between the two independent slabs to reach a common Fermi level in the metallic phase. PMID:24327264

  3. Charge mobility induced by Brownian fluctuations in π-conjugated polymers in solution.

    PubMed

    Poole, Jessica Ellen; Damry, Djamshid Ahmud; Tozer, Oliver Robert; Barford, William

    2016-01-28

    We study the motion of a doped charge in a π-conjugated polymer chain in solution subject to Brownian fluctuations. Specifically, we take poly(para-phenylene) to be our model system where the Brownian fluctuations cause rotational motion of the phenylene rings. The instantaneous torsional fluctuations cause Anderson localization of the charge wavefunction, with the lower-energy spectrum being composed of local ground states and the higher-energy spectrum being composed of quasi-extended states. At low temperatures, additional charge localization occurs via torsional relaxation. The dynamical torsional fluctuations lead to two distinct modes of motion of the charge: adiabatic and non-adiabatic. Adiabatic motion is a 'crawling' motion of the charge along the polymer chain while the charge remains in its local ground state. Non-adiabatic motion is a rapid 'hopping' motion as the charge is excited into higher energy quasi-extended states and travels ballistically along the chain before relaxing into a local ground state. The adiabatic motion dominates at low temperatures, and exhibits a linear temperature dependence and thus a constant zero-field charge mobility. Non-adiabatic motion begins to dominate as the temperature is increased, as the charge is thermally excited into higher energy states. At high temperatures the diffusion constant becomes almost temperature independent, indicating a decrease in the charge mobility with increasing temperature, which we attribute to the charge localization length being a decreasing function of temperature at high temperatures. PMID:26699806

  4. 27 CFR 26.68a - Bond account.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... 27 Alcohol, Tobacco Products and Firearms 1 2011-04-01 2011-04-01 false Bond account. 26.68a... Liquors and Articles in Puerto Rico Bonds § 26.68a Bond account. Every person who files a bond under this subpart shall keep an account of the charges against and credits to the bond if the penal sum of his...

  5. 27 CFR 26.68a - Bond account.

    Code of Federal Regulations, 2010 CFR

    2010-04-01

    ... 27 Alcohol, Tobacco Products and Firearms 1 2010-04-01 2010-04-01 false Bond account. 26.68a... Liquors and Articles in Puerto Rico Bonds § 26.68a Bond account. Every person who files a bond under this subpart shall keep an account of the charges against and credits to the bond if the penal sum of his...

  6. Reorientational dynamics of charged and neutral solutes in 1-alkyl-3-methylimidazoilum bis(trifluoromethylsulfonyl)imide ionic liquids: Realization of ionic component of hydrogen bond

    NASA Astrophysics Data System (ADS)

    Sahu, Prabhat Kumar; Sarkar, Moloy

    2016-05-01

    Role of electrostatic interaction on rotational relaxation dynamics of two charged solutes, sodium 8-methoxypyrene-1,3,6-trisulfonate (MPTS), 1-pyrenesulfonic acid sodium salt (1-PSA) and neutral perylene has been studied in two structurally similar but chemically distinguishable imidazolium-based ionic liquids (ILs). Analysis of the results reveals that rotational relaxation of MPTS is significantly hindered even in the IL where acidic C2-H of the imidazolium moiety is replaced by the methyl group. Moreover, rotational relaxation of neutral perylene is found to be faster than mononegative 1-PSA which is again observed to be faster than that of tri-negative MPTS in the same ILs.

  7. The bonding, charge distribution, spin ordering, optical, and elastic properties of four MAX phases Cr2AX (A = Al or Ge, X = C or N): From density functional theory study

    NASA Astrophysics Data System (ADS)

    Li, Neng; Mo, Yuxiang; Ching, Wai-Yim

    2013-11-01

    In this work, we assess a full spectrum of properties (chemical bonding, charge distribution, spin ordering, optical, and elastic properties) of Cr2AC (A = Al, Ge) and their hypothetical nitride counterparts Cr2AN (A = Al, Ge) based on density functional theory calculations. The calculated total energy values indicate that a variety of spin ordering of these four compounds depending on interlayer-interactions between M-A and M-X within the sublattice, which is supported by bonding analysis. MAX phase materials are discovered to possess exotic magnetic properties which indicates that these materials could serve as promising candidates for novel layered magnetic materials for various electronic and spintronic applications. Further analysis of optical properties for two polarization vectors of Cr2AX shows that the reflectivity is high in the visible-ultraviolet region up to ˜15 eV suggesting Cr2AX as a promising candidate for use as a coating material. The elastic coefficients (Cij) and bulk mechanical properties [bulk modulus (K), shear modulus (G), Young's modulus (E), Poisson's ratio (η), and Pugh ratio (G/K)] of these four Cr2AX compounds are also calculated and analyzed, which pave the way to predict or design new MAX phases that are less brittle or tougher by having a lower G/K value or higher η.

  8. The bonding, charge distribution, spin ordering, optical, and elastic properties of four MAX phases Cr{sub 2}AX (A = Al or Ge, X = C or N): From density functional theory study

    SciTech Connect

    Li, Neng; Mo, Yuxiang; Ching, Wai-Yim

    2013-11-14

    In this work, we assess a full spectrum of properties (chemical bonding, charge distribution, spin ordering, optical, and elastic properties) of Cr{sub 2}AC (A = Al, Ge) and their hypothetical nitride counterparts Cr{sub 2}AN (A = Al, Ge) based on density functional theory calculations. The calculated total energy values indicate that a variety of spin ordering of these four compounds depending on interlayer-interactions between M-A and M-X within the sublattice, which is supported by bonding analysis. MAX phase materials are discovered to possess exotic magnetic properties which indicates that these materials could serve as promising candidates for novel layered magnetic materials for various electronic and spintronic applications. Further analysis of optical properties for two polarization vectors of Cr{sub 2}AX shows that the reflectivity is high in the visible-ultraviolet region up to ∼15 eV suggesting Cr{sub 2}AX as a promising candidate for use as a coating material. The elastic coefficients (C{sub ij}) and bulk mechanical properties [bulk modulus (K), shear modulus (G), Young's modulus (E), Poisson's ratio (η), and Pugh ratio (G/K)] of these four Cr{sub 2}AX compounds are also calculated and analyzed, which pave the way to predict or design new MAX phases that are less brittle or tougher by having a lower G/K value or higher η.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. Density functional study of electronic, charge density, and chemical bonding properties of 9-methyl-3-Thiophen-2-YI-Thieno [3,2-e] [1, 2, 4] Thriazolo [4,3-c] pyrimidine-8-Carboxylic acid ethyl ester crystals

    NASA Astrophysics Data System (ADS)

    Reshak, A. H.; Kamarudin, H.; Alahmed, Z. A.; Auluck, S.; Chyský, Jan

    2014-06-01

    A comprehensive theoretical density functional investigation of the electronic crystal structure, chemical bonding, and the electron charge densities of 9-Methyl-3-Thiophen-2-YI-Thieno [3, 2-e] [1, 2, 4] Thriazolo [4,3-c] Pyrimidine-8-Carboxylic Acid Ethyl Ester (C15H12N4O2S2) is performed. The density of states at Fermi level equal to 5.50 (3.45) states/Ry cell, and the calculated bare electronic specific heat coefficient is found to be 0.95 (0.59) mJ/mole-K2 for the local density approximation (Engel-Vosko generalized gradient approximation). The electronic charge density space distribution contours in (1 0 0) and (1 1 0) planes were calculated. We find that there are two independent molecules (A and B) in the asymmetric unit exhibit intramolecular C-H…O, C-H…N interactions. This intramolecular interaction is different in molecules A and B, where A molecule show C-H…O interaction while B molecule exhibit C-H…N interaction. We should emphasis that there is π-π interaction between the pyrimidine rings of the two neighbors B molecules gives extra strengths and stabilizations to the superamolecular structure. The calculated distance between the two neighbors pyrimidine rings found to be 3.345 Å, in good agreement with the measured one (3.424(1) Å).

  19. 8 CFR 103.6 - Surety bonds.

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... likely to become a public charge. A bond may also be cancelled in order to allow substitution of another..., Immigration Bond, a copy of which, and any rider attached thereto, shall be furnished the obligor. A district director is authorized to approve a bond, a formal agreement to extension of liability of surety, a...

  20. Thermal explosion hazards on 18650 lithium ion batteries with a VSP2 adiabatic calorimeter.

    PubMed

    Jhu, Can-Yong; Wang, Yih-Wen; Shu, Chi-Min; Chang, Jian-Chuang; Wu, Hung-Chun

    2011-08-15

    Thermal abuse behaviors relating to adiabatic runaway reactions in commercial 18650 lithium ion batteries (LiCoO(2)) are being studied in an adiabatic calorimeter, vent sizing package 2 (VSP2). We select four worldwide battery producers, Sony, Sanyo, Samsung and LG, and tested their Li-ion batteries, which have LiCoO(2) cathodes, to determine their thermal instabilities and adiabatic runaway features. The charged (4.2V) and uncharged (3.7 V) 18650 Li-ion batteries are tested using a VSP2 with a customized stainless steel test can to evaluate their thermal hazard characteristics, such as the initial exothermic temperature (T(0)), the self-heating rate (dT/dt), the pressure rise rate (dP/dt), the pressure-temperature profiles and the maximum temperature (T(max)) and pressure (P(max)). The T(max) and P(max) of the charged Li-ion battery during the runaway reaction reach 903.0°C and 1565.9 psig (pound-force per square inch gauge), respectively. This result leads to a thermal explosion, and the heat of reaction is 26.2 kJ. The thermokinetic parameters of the reaction of LiCoO(2) batteries are also determined using the Arrhenius model. The thermal reaction mechanism of the Li-ion battery (pack) proved to be an important safety concern for energy storage. Additionally, use of the VSP2 to classify the self-reactive ratings of the various Li-ion batteries demonstrates a new application of the adiabatic calorimetric methodology. PMID:21612866

  1. 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.

  2. 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 .

  3. 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.

  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. 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

  7. 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.

  8. 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.

  9. Adiabatic Mass Loss Model in Binary Stars

    NASA Astrophysics Data System (ADS)

    Ge, H. W.

    2012-07-01

    Rapid mass transfer process in the interacting binary systems is very complicated. It relates to two basic problems in the binary star evolution, i.e., the dynamically unstable Roche-lobe overflow and the common envelope evolution. Both of the problems are very important and difficult to be modeled. In this PhD thesis, we focus on the rapid mass loss process of the donor in interacting binary systems. The application to the criterion of dynamically unstable mass transfer and the common envelope evolution are also included. Our results based on the adiabatic mass loss model could be used to improve the binary evolution theory, the binary population synthetic method, and other related aspects. We build up the adiabatic mass loss model. In this model, two approximations are included. The first one is that the energy generation and heat flow through the stellar interior can be neglected, hence the restructuring is adiabatic. The second one is that he stellar interior remains in hydrostatic equilibrium. We model this response by constructing model sequences, beginning with a donor star filling its Roche lobe at an arbitrary point in its evolution, holding its specific entropy and composition profiles fixed. These approximations are validated by the comparison with the time-dependent binary mass transfer calculations and the polytropic model for low mass zero-age main-sequence stars. In the dynamical time scale mass transfer, the adiabatic response of the donor star drives it to expand beyond its Roche lobe, leading to runaway mass transfer and the formation of a common envelope with its companion star. For donor stars with surface convection zones of any significant depth, this runaway condition is encountered early in mass transfer, if at all; but for main sequence stars with radiative envelopes, it may be encountered after a prolonged phase of thermal time scale mass transfer, so-called delayed dynamical instability. We identify the critical binary mass ratio for the

  10. Photoinduced hydrogen-bonding dynamics.

    PubMed

    Chu, Tian-Shu; Xu, Jinmei

    2016-09-01

    Hydrogen bonding dynamics has received extensive research attention in recent years due to the significant advances in femtolaser spectroscopy experiments and quantum chemistry calculations. Usually, photoexcitation would cause changes in the hydrogen bonding formed through the interaction between hydrogen donor and acceptor molecules on their ground electronic states, and such transient strengthening or weakening of hydrogen bonding could be crucial for the photophysical transformations and the subsequent photochemical reactions that occurred on a time scale from tens of femtosecond to a few nanoseconds. In this article, we review the combined experimental and theoretical studies focusing on the ultrafast electronic and vibrational hydrogen bonding dynamics. Through these studies, new mechanisms and proposals and common rules have been put forward to advance our understanding of the hydrogen bondings dynamics in a variety of important photoinduced phenomena like photosynthesis, dual fluorescence emission, rotational reorientation, excited-state proton transfer and charge transfer processes, chemosensor fluorescence sensing, rearrangements of the hydrogen-bond network including forming and breaking hydrogen bond in water. Graphical Abstract We review the recent advances on exploring the photoinduced hydrogen bonding dynamics in solutions through a joint approach of laser spectroscopy and theoretical calculation. The reviewed studies have put forward a new mechanism, new proposal, and new rule for a variety of photoinduced phenomena such as photosynthesis, dual fluorescence emission, rotational reorientation, excited-state proton transfer and charge transfer, chemosensor fluorescence sensing, and rearrangements of the hydrogen-bond network in water. PMID:27491849

  11. Conical Intersections Between Vibrationally Adiabatic Surfaces in Methanol

    NASA Astrophysics Data System (ADS)

    Dawadi, Mahesh B.; Perry, David S.

    2014-06-01

    The discovery of a set of seven conical intersections (CI's) between vibrationally adiabatic surfaces in methanol is reported. The intersecting surfaces represent the energies of the two asymmetric CH stretch vibrations, νb{2} and νb{9}, regarded as adiabatic functions of the torsional angle, γ, and COH bend angle, ρ. One conical intersection, required by symmetry, is located at the C3v geometry where the COH group is linear (ρ = 0°); the other six are in eclipsed conformations with ρ = 62° and 94°. The three CI's at ρ = 62° are close to the equilibrium geometry (ρ = 71.4°), within the zero-point amplitude of the COH bending vibration. CI's between electronic surfaces have long been recognized as crucial conduits for ultrafast relaxation, and recently Hamm, and Stock have shown that vibrational CI's may also provide a mechanism for ultrafast vibrational relaxation. The ab initio data reported here are well described by an extended Zwanziger and Grant model for E ⊗ e Jahn-Teller systems in which Renner-Teller coupling is also active. However, in the present case, the distortion ρ from C3v symmetry is much larger than is typical in the Jahn-Teller coupling of electronic surfaces and accordingly higher-order terms in ρ are required. The present results are also consistent with the two-state model of Xu et al. The cusp-like features, which they found along the internal-rotation path, are explained in the context of the present work in terms of proximity to the CI's. The presence of multiple CI's near the torsional minimum energy path impacts the role of geometric phase in this three-fold internal-rotor system. When the dimensionality of the low-frequency space is extended to include the CO bond length as well as γ and ρ, the individual CI's become seams of CI's. It is shown that the CI's at ρ = 62° and 94° lie along the same seam of CI's in this higher dimensional space. P. Hamm and G. Stock, Phys. Rev. Lett., 109, 173201, (2012) P. Hamm, and G

  12. Calibration of STUD+ parameters to achieve optimally efficient broadband adiabatic decoupling in a single transient

    PubMed

    Bendall; Skinner

    1998-10-01

    To provide the most efficient conditions for spin decoupling with least RF power, master calibration curves are provided for the maximum centerband amplitude, and the minimum amplitude for the largest cycling sideband, resulting from STUD+ adiabatic decoupling applied during a single free induction decay. The principal curve is defined as a function of the four most critical experimental input parameters: the maximum amplitude of the RF field, RFmax, the length of the sech/tanh pulse, Tp, the extent of the frequency sweep, bwdth, and the coupling constant, Jo. Less critical parameters, the effective (or actual) decoupled bandwidth, bweff, and the sech/tanh truncation factor, beta, which become more important as bwdth is decreased, are calibrated in separate curves. The relative importance of nine additional factors in determining optimal decoupling performance in a single transient are considered. Specific parameters for efficient adiabatic decoupling can be determined via a set of four equations which will be most useful for 13C decoupling, covering the range of one-bond 13C1H coupling constants from 125 to 225 Hz, and decoupled bandwidths of 7 to 100 kHz, with a bandwidth of 100 kHz being the requirement for a 2 GHz spectrometer. The four equations are derived from a recent vector model of adiabatic decoupling, and experiment, supported by computer simulations. The vector model predicts an inverse linear relation between the centerband and maximum sideband amplitudes, and it predicts a simple parabolic relationship between maximum sideband amplitude and the product JoTp. The ratio bwdth/(RFmax)2 can be viewed as a characteristic time scale, tauc, affecting sideband levels, with tauc approximately Tp giving the most efficient STUD+ decoupling, as suggested by the adiabatic condition. Functional relationships between bwdth and less critical parameters, bweff and beta, for efficient decoupling can be derived from Bloch-equation calculations of the inversion profile

  13. Kinetic theory of plasma adiabatic major radius compression in tokamaks

    NASA Astrophysics Data System (ADS)

    Gorelenkova, M. V.; Gorelenkov, N. N.; Azizov, E. A.; Romannikov, A. N.; Herrmann, H. W.

    1998-05-01

    In order to understand the individual charged particle behavior as well as plasma macroparameters (temperature, density, etc.) during the adiabatic major radius compression (R-compression) in a tokamak, a kinetic approach is used. The perpendicular electric field from the Ohm's law at zero resistivity is made use of in order to describe particle motion during the R-compression. Expressions for both passing and trapped particle energy and pitch angle change are derived for a plasma with high aspect ratio and circular magnetic surfaces. The particle behavior near the passing trapped boundary during the compression is studied to simulate the compression-induced collisional losses of alpha particles. Qualitative agreement is obtained with the alphas loss measurements in deuterium-tritium (D-T) experiments in the Tokamak Fusion Test Reactor (TFTR) [World Survey of Activities in Controlled Fusion Research [Nucl. Fusion special supplement (1991)] (International Atomic Energy Agency, Vienna, 1991)]. The plasma macroparameters evolution at the R-compression is calculated by solving the gyroaveraged drift kinetic equation.

  14. Decoherence in current induced forces: Application to adiabatic quantum motors

    NASA Astrophysics Data System (ADS)

    Fernández-Alcázar, Lucas J.; Bustos-Marún, Raúl A.; Pastawski, Horacio M.

    2015-08-01

    Current induced forces are not only related with the discrete nature of electrons but also with its quantum character. It is natural then to wonder about the effect of decoherence. Here, we develop the theory of current induced forces including dephasing processes and we apply it to study adiabatic quantum motors (AQMs). The theory is based on Büttiker's fictitious probe model, which here is reformulated for this particular case. We prove that it accomplishes the fluctuation-dissipation theorem. We also show that, in spite of decoherence, the total work performed by the current induced forces remains equal to the pumped charge per cycle times the voltage. We find that decoherence affects not only the current induced forces of the system but also its intrinsic friction and noise, modifying in a nontrivial way the efficiency of AQMs. We apply the theory to study an AQM inspired by a classical peristaltic pump where we surprisingly find that decoherence can play a crucial role by triggering its operation. Our results can help to understand how environmentally induced dephasing affects the quantum behavior of nanomechanical devices.

  15. 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.

  16. Institutional Bonding.

    ERIC Educational Resources Information Center

    Allard, M. June

    Institutional bonding was examined at a public, urban commuter college with exceptionally high attrition and visibly low morale. Changes in bonding and attrition were measured 6 years after a 2-year effort to develop school identity and student feelings of membership. It was found that a simple index of campus morale is provided by level of…

  17. 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.

  18. 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

  19. 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.

  20. 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)

  1. 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…

  2. Intermediate regime of charged particle scattering in the field-reversal configuration

    SciTech Connect

    Shustov, P. I. Yushkov, E. V.; Artemyev, A. V.

    2015-12-15

    In this paper, we investigate the charged particle scattering in the magnetic field configuration with stretched magnetic field lines. This scattering results from the violation of the adiabaticity of charged particle motion in the region with the strong gradient of the magnetic field. We consider the intermediate regime of charged particle dynamics, when the violation of the adiabaticity is significant enough, but particle motion is not chaotic. We demonstrate and describe the significant scattering of particles with large adiabatic invariants (magnetic moment). We discuss a possible application of obtained results for description of the peculiarities of pitch-angle diffusion of relativistic electrons in the Earth radiation belts.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. 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

  14. 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.

  15. 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

  16. 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.

  17. 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

  18. 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.

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. Semiclassical Monte Carlo: A first principles approach to non-adiabatic molecular dynamics

    SciTech Connect

    White, Alexander J.; Gorshkov, Vyacheslav N.; Wang, Ruixi; Tretiak, Sergei; Mozyrsky, Dmitry

    2014-11-14

    Modeling the dynamics of photophysical and (photo)chemical reactions in extended molecular systems is a new frontier for quantum chemistry. Many dynamical phenomena, such as intersystem crossing, non-radiative relaxation, and charge and energy transfer, require a non-adiabatic description which incorporate transitions between electronic states. Additionally, these dynamics are often highly sensitive to quantum coherences and interference effects. Several methods exist to simulate non-adiabatic dynamics; however, they are typically either too expensive to be applied to large molecular systems (10's-100's of atoms), or they are based on ad hoc schemes which may include severe approximations due to inconsistencies in classical and quantum mechanics. We present, in detail, an algorithm based on Monte Carlo sampling of the semiclassical time-dependent wavefunction that involves running simple surface hopping dynamics, followed by a post-processing step which adds little cost. The method requires only a few quantities from quantum chemistry calculations, can systematically be improved, and provides excellent agreement with exact quantum mechanical results. Here we show excellent agreement with exact solutions for scattering results of standard test problems. Additionally, we find that convergence of the wavefunction is controlled by complex valued phase factors, the size of the non-adiabatic coupling region, and the choice of sampling function. These results help in determining the range of applicability of the method, and provide a starting point for further improvement.

  4. Semiclassical Monte Carlo: A first principles approach to non-adiabatic molecular dynamics

    NASA Astrophysics Data System (ADS)

    White, Alexander J.; Gorshkov, Vyacheslav N.; Wang, Ruixi; Tretiak, Sergei; Mozyrsky, Dmitry

    2014-11-01

    Modeling the dynamics of photophysical and (photo)chemical reactions in extended molecular systems is a new frontier for quantum chemistry. Many dynamical phenomena, such as intersystem crossing, non-radiative relaxation, and charge and energy transfer, require a non-adiabatic description which incorporate transitions between electronic states. Additionally, these dynamics are often highly sensitive to quantum coherences and interference effects. Several methods exist to simulate non-adiabatic dynamics; however, they are typically either too expensive to be applied to large molecular systems (10's-100's of atoms), or they are based on ad hoc schemes which may include severe approximations due to inconsistencies in classical and quantum mechanics. We present, in detail, an algorithm based on Monte Carlo sampling of the semiclassical time-dependent wavefunction that involves running simple surface hopping dynamics, followed by a post-processing step which adds little cost. The method requires only a few quantities from quantum chemistry calculations, can systematically be improved, and provides excellent agreement with exact quantum mechanical results. Here we show excellent agreement with exact solutions for scattering results of standard test problems. Additionally, we find that convergence of the wavefunction is controlled by complex valued phase factors, the size of the non-adiabatic coupling region, and the choice of sampling function. These results help in determining the range of applicability of the method, and provide a starting point for further improvement.

  5. Quasi-adiabatic dynamics of ions in a bifurcated current sheet

    SciTech Connect

    Kartsev, Yu. I.; Artemyev, A. V.; Malova, H. V. Zelenyi, L. M.

    2013-04-15

    The study is devoted to ion dynamics in bifurcated current sheets with a two-peak current-density distribution observed in the Earth's magnetotail and solar wind. The ion motion is described by a Hamiltonian system with two degrees of freedom. The presence of a small parameter {kappa} characterizing the ratio between the amplitudes of the normal and tangential magnetic field components allows one to separate variables into fast and slow ones and introduce the quasi-adiabatic invariant of motion I{sub z}. Conservation of this invariant makes it possible to analytically describe the dynamics of charged particles. Deviations of the particle dynamics from the quasi-adiabatic one, which are caused by the nonconservation of the quasi-adiabatic invariant, are investigated. The jump of the invariant {Delta}I{sub z} is shown to depend on the small parameter according to the power-law {Delta}I{sub z} {approx} {kappa}{sup h}, where the exponent h varies between unity and 3/4, depending on the level of current sheet bifurcation. The obtained dependence of {Delta}I{sub z} on {kappa} coincides with analytic expressions in the limiting cases of nonbifurcated and completely bifurcated current sheets.

  6. Asymmetric bifurcated halogen bonds.

    PubMed

    Novák, Martin; Foroutan-Nejad, Cina; Marek, Radek

    2015-03-01

    Halogen bonding (XB) is being extensively explored for its potential use in advanced materials and drug design. Despite significant progress in describing this interaction by theoretical and experimental methods, the chemical nature remains somewhat elusive, and it seems to vary with the selected system. In this work we present a detailed DFT analysis of three-center asymmetric halogen bond (XB) formed between dihalogen molecules and variously 4-substituted 1,2-dimethoxybenzene. The energy decomposition, orbital, and electron density analyses suggest that the contribution of electrostatic stabilization is comparable with that of non-electrostatic factors. Both terms increase parallel with increasing negative charge of the electron donor molecule in our model systems. Depending on the orientation of the dihalogen molecules, this bifurcated interaction may be classified as 'σ-hole - lone pair' or 'σ-hole - π' halogen bonds. Arrangement of the XB investigated here deviates significantly from a recent IUPAC definition of XB and, in analogy to the hydrogen bonding, the term bifurcated halogen bond (BXB) seems to be appropriate for this type of interaction. PMID:25656525

  7. 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.

  8. 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.

  9. 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.

  10. Modulating the strength of tetrel bonding through beryllium bonding.

    PubMed

    Liu, Mingxiu; Yang, Li; Li, Qingzhong; Li, Wenzuo; Cheng, Jianbo; Xiao, Bo; Yu, Xuefang

    2016-08-01

    Quantum chemical calculations were performed to investigate the stability of the ternary complexes BeH2···XMH3···NH3 (X = F, Cl, and Br; M = C, Si, and Ge) and the corresponding binary complexes at the atomic level. Our results reveal that the stability of the XMH3···BeH2 complexes is mainly due to both a strong beryllium bond and a weak tetrel-hydride interaction, while the XMH3···NH3 complexes are stabilized by a tetrel bond. The beryllium bond with a halogen atom as the electron donor has many features in common with a beryllium bond with an O or N atom as the electron donor, although they do exhibit some different characteristics. The stability of the XMH3···NH3 complex is dominated by the electrostatic interaction, while the orbital interaction also makes an important contribution. Interestingly, as the identities of the X and M atoms are varied, the strength of the tetrel bond fluctuates in an irregular manner, which can explained by changes in electrostatic potentials and orbital interactions. In the ternary systems, both the beryllium bond and the tetrel bond are enhanced, which is mainly ascribed to increased electrostatic potentials on the corresponding atoms and charge transfer. In particular, when compared to the strengths of the tetrel and beryllium bonds in the binary systems, in the ternary systems the tetrel bond is enhanced to a greater degree than the beryllium bond. Graphical Abstract A tetrel bond can be strengthened greatly by a beryllium bond. PMID:27464738

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. σ-Hole Bond vs π-Hole Bond: A Comparison Based on Halogen Bond.

    PubMed

    Wang, Hui; Wang, Weizhou; Jin, Wei Jun

    2016-05-11

    The σ-hole and π-hole are the regions with positive surface electrostatic potential on the molecule entity; the former specifically refers to the positive region of a molecular entity along extension of the Y-Ge/P/Se/X covalent σ-bond (Y = electron-rich group; Ge/P/Se/X = Groups IV-VII), while the latter refers to the positive region in the direction perpendicular to the σ-framework of the molecular entity. The directional noncovalent interactions between the σ-hole or π-hole and the negative or electron-rich sites are named σ-hole bond or π-hole bond, respectively. The contributions from electrostatic, charge transfer, and other terms or Coulombic interaction to the σ-hole bond and π-hole bond were reviewed first followed by a brief discussion on the interplay between the σ-hole bond and the π-hole bond as well as application of the two types of noncovalent interactions in the field of anion recognition. It is expected that this review could stimulate further development of the σ-hole bond and π-hole bond in theoretical exploration and practical application in the future. PMID:26886515

  17. A DIRECT METHOD TO DETERMINE THE PARALLEL MEAN FREE PATH OF SOLAR ENERGETIC PARTICLES WITH ADIABATIC FOCUSING

    SciTech Connect

    He, H.-Q.; Wan, W. E-mail: wanw@mail.iggcas.ac.cn

    2012-03-01

    The parallel mean free path of solar energetic particles (SEPs), which is determined by physical properties of SEPs as well as those of solar wind, is a very important parameter in space physics to study the transport of charged energetic particles in the heliosphere, especially for space weather forecasting. In space weather practice, it is necessary to find a quick approach to obtain the parallel mean free path of SEPs for a solar event. In addition, the adiabatic focusing effect caused by a spatially varying mean magnetic field in the solar system is important to the transport processes of SEPs. Recently, Shalchi presented an analytical description of the parallel diffusion coefficient with adiabatic focusing. Based on Shalchi's results, in this paper we provide a direct analytical formula as a function of parameters concerning the physical properties of SEPs and solar wind to directly and quickly determine the parallel mean free path of SEPs with adiabatic focusing. Since all of the quantities in the analytical formula can be directly observed by spacecraft, this direct method would be a very useful tool in space weather research. As applications of the direct method, we investigate the inherent relations between the parallel mean free path and various parameters concerning physical properties of SEPs and solar wind. Comparisons of parallel mean free paths with and without adiabatic focusing are also presented.

  18. 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

  19. 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.

  20. 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.

  1. 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.

  2. 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.

  3. 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.

  4. Non-adiabatic ab initio molecular dynamics of supersonic beam epitaxy of silicon carbide at room temperature

    SciTech Connect

    Taioli, Simone; Garberoglio, Giovanni; Simonucci, Stefano; Beccara, Silvio a; Aversa, Lucrezia; Nardi, Marco; Verucchi, Roberto; Iannotta, Salvatore; Dapor, Maurizio; and others

    2013-01-28

    In this work, we investigate the processes leading to the room-temperature growth of silicon carbide thin films by supersonic molecular beam epitaxy technique. We present experimental data showing that the collision of fullerene on a silicon surface induces strong chemical-physical perturbations and, for sufficient velocity, disruption of molecular bonds, and cage breaking with formation of nanostructures with different stoichiometric character. We show that in these out-of-equilibrium conditions, it is necessary to go beyond the standard implementations of density functional theory, as ab initio methods based on the Born-Oppenheimer approximation fail to capture the excited-state dynamics. In particular, we analyse the Si-C{sub 60} collision within the non-adiabatic nuclear dynamics framework, where stochastic hops occur between adiabatic surfaces calculated with time-dependent density functional theory. This theoretical description of the C{sub 60} impact on the Si surface is in good agreement with our experimental findings.

  5. 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.

  6. 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.

  7. 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.

  8. Yankee bonds

    SciTech Connect

    Delaney, P. )

    1993-10-01

    Yankee and Euromarket bonds may soon find their way into the financing of power projects in Latin America. For developers seeking long-term commitments under build, own, operate, and transfer (BOOT) power projects in Latin America, the benefits are substantial.

  9. On The Nature of the Halogen Bond.

    PubMed

    Wang, Changwei; Danovich, David; Mo, Yirong; Shaik, Sason

    2014-09-01

    The wide-ranging applications of the halogen bond (X-bond), notably in self-assembling materials and medicinal chemistry, have placed this weak intermolecular interaction in a center of great deal of attention. There is a need to elucidate the physical nature of the halogen bond for better understanding of its similarity and differences vis-à-vis other weak intermolecular interactions, for example, hydrogen bond, as well as for developing improved force-fields to simulate nano- and biomaterials involving X-bonds. This understanding is the focus of the present study that combines the insights of a bottom-up approach based on ab initio valence bond (VB) theory and the block-localized wave function (BLW) theory that uses monomers to reconstruct the wave function of a complex. To this end and with an aim of unification, we studied the nature of X-bonds in 55 complexes using the combination of VB and BLW theories. Our conclusion is clear-cut; most of the X-bonds are held by charge transfer interactions (i.e., intermolecular hyperconjugation) as envisioned more than 60 years ago by Mulliken. This is consistent with the experimental and computational findings that X-bonds are more directional than H-bonds. Furthermore, the good linear correlation between charge transfer energies and total interaction energies partially accounts for the success of simple force fields in the simulation of large systems involving X-bonds. PMID:26588518

  10. The method of Gaussian weighted trajectories. III. An adiabaticity correction proposal

    SciTech Connect

    Bonnet, L.

    2008-01-28

    The addition of an adiabaticity correction (AC) to the Gaussian weighted trajectory (GWT) method and its normalized version (GWT-N) is suggested. This correction simply consists in omitting vibrationally adiabatic nonreactive trajectories in the calculations of final attributes. For triatomic exchange reactions, these trajectories satisfy the criterion {omega} not much larger than ({Dirac_h}/2{pi}), where {omega} is a vibrational action defined by {omega}={integral}{sup []}-[]dt(pr-p{sub 0}r{sub 0}), r being the reagent diatom bond length, p its conjugate momentum, and r{sub 0} and p{sub 0} the corresponding variables for the unperturbed diatom ({omega}/({Dirac_h}/2{pi}) bears some analogy with the semiclassical elastic scattering phase shift). The resulting GWT-AC and GWT-ACN methods are applied to the recently studied H{sup +}+H{sub 2} and H{sup +}+D{sub 2} reactions and the agreement between their predictions and those of exact quantum scattering calculations is found to be much better than for the initial GWT and GWT-N methods. The GWT-AC method, however, appears to be the most accurate one for the processes considered, in particular, the H{sup +}+D{sub 2} reaction.

  11. Reduction of thioredoxin significantly decreases its partial specific volume and adiabatic compressibility.

    PubMed Central

    Kaminsky, S. M.; Richards, F. M.

    1992-01-01

    The partial specific volume and adiabatic compressibility were determined at several temperatures for oxidized and reduced Escherichia coli thioredoxin. Oxidized thioredoxin had a partial specific volume of 0.785-0.809 mL/g at the observed upper limit for all proteins whereas the partial specific volume of reduced thioredoxin was 0.745-0.755 mL/g, a value in the range found for a majority of proteins. The adiabatic compressibility of oxidized thioredoxin was also much larger (9.8-18 x 10(-12) cm2 dyne-1) than that of the reduced protein (3.8-7.3 x 10(-12)). Apart from the region immediately around the small disulfide loop, the structures of the oxidized (X-ray, crystal) and reduced protein (nuclear magnetic resonance, solution) are reported to be very similar. It would appear that alterations in the solvent layer in contact with the protein surface must play a major role in producing these large changes in the apparent specific volumes and compressibilities in this system. Some activities of thioredoxin require the reduced structure but are not electron transfer reactions. The large changes in physical parameters reported here suggest the possibility of a reversible metabolic control function for the SS bond. PMID:1304879

  12. Diffusion bonding

    DOEpatents

    Anderson, Robert C.

    1976-06-22

    1. A method for joining beryllium to beryllium by diffusion bonding, comprising the steps of coating at least one surface portion of at least two beryllium pieces with nickel, positioning a coated surface portion in a contiguous relationship with an other surface portion, subjecting the contiguously disposed surface portions to an environment having an atmosphere at a pressure lower than ambient pressure, applying a force upon the beryllium pieces for causing the contiguous surface portions to abut against each other, heating the contiguous surface portions to a maximum temperature less than the melting temperature of the beryllium, substantially uniformly decreasing the applied force while increasing the temperature after attaining a temperature substantially above room temperature, and maintaining a portion of the applied force at a temperature corresponding to about maximum temperature for a duration sufficient to effect the diffusion bond between the contiguous surface portions.

  13. Adiabatic-Nonadiabatic Transition in Warm Long-Range Interacting Systems: The Transport of Intense Inhomogeneous Beams

    NASA Astrophysics Data System (ADS)

    Souza, Everton G.; Endler, Antonio; Rizzato, Felipe B.; Pakter, Renato

    2012-08-01

    We investigate the role of the temperature in the onset of singularities and the consequent breakdown in a macroscopic fluid model for long-range interacting systems. In particular, we consider an adiabatic fluid description for the transport of intense inhomogeneous charged particle beams. We find that there exists a critical temperature below which the fluid model always develops a singularity and breaks down as the system evolves. As the critical temperature is approached, however, the time for the occurrence of the singularity diverges. Therefore, the critical temperature separates two distinct dynamical phases: a nonadiabatic transport at lower temperatures and a completely adiabatic evolution at higher temperatures. These findings are verified with the aid of self-consistent N-particle simulations.

  14. Advances in Charge Displacement Analysis.

    PubMed

    Bistoni, Giovanni; Belpassi, Leonardo; Tarantelli, Francesco

    2016-03-01

    We define new general density-based descriptors for the quantification of charge transfer and polarization effects associated with the interaction between two fragments and the formation of a chemical bond. Our aim is to provide a simple yet accurate picture of a chemical interaction by condensing the information on the charge rearrangement accompanying it into a few chemically meaningful parameters. These charge displacement (CD) parameters quantify the total charge displaced upon bond formation and decompose it into a charge transfer component between the fragments and charge rearrangements taking place within the fragments. We then show how the new parameters can be easily calculated using the well-known CD function, which describes the charge flow along a chosen axis accompanying the formation of a bond. The approach presented here can be useful in a wide variety of contexts, ranging from weak interactions to electronic excitations to coordination chemistry. In particular, we discuss here how the scheme can be used for the characterization of the donation and back-donation components of metal-ligand bonds, in combination with the natural orbitals for chemical valence (NOCV) theory. In doing so, we discuss the interesting relationship between the proposed parameters and the corresponding NOCV eigenvalues, commonly used as a measure of the electron charge displacement associated with a given bonding contribution. As a prototype case study, we investigate the bond between a N-heterocyclic carbene and different metallic fragments. Finally, we show that our approach can be used in combination with the energy decomposition of the extended transition state method, providing an estimate of both charge transfer and polarization contributions to the interaction energy. PMID:26824715

  15. 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.

  16. Theory and X-ray Absorption Spectroscopy for Aluminum Coordination Complexes – Al K-Edge Studies of Charge and Bonding in (BDI)Al, (BDI)AlR2, and (BDI)AlX2 Complexes.

    PubMed

    Altman, Alison B; Pemmaraju, C D; Camp, Clément; Arnold, John; Minasian, Stefan G; Prendergast, David; Shuh, David K; Tyliszczak, Tolek

    2015-08-19

    Polarized aluminum K-edge X-ray absorption near edge structure (XANES) spectroscopy and first-principles calculations were used to probe electronic structure in a series of (BDI)Al, (BDI)AlX2, and (BDI)AlR2 coordination compounds (X = F, Cl, I; R = H, Me; BDI = 2,6-diisopropylphenyl-β-diketiminate). Spectral interpretations were guided by examination of the calculated transition energies and polarization-dependent oscillator strengths, which agreed well with the XANES spectroscopy measurements. Pre-edge features were assigned to transitions associated with the Al 3p orbitals involved in metal-ligand bonding. Qualitative trends in Al 1s core energy and valence orbital occupation were established through a systematic comparison of excited states derived from Al 3p orbitals with similar symmetries in a molecular orbital framework. These trends suggested that the higher transition energies observed for (BDI)AlX2 systems with more electronegative X(1-) ligands could be ascribed to a decrease in electron density around the aluminum atom, which causes an increase in the attractive potential of the Al nucleus and concomitant increase in the binding energy of the Al 1s core orbitals. For (BDI)Al and (BDI)AlH2 the experimental Al K-edge XANES spectra and spectra calculated using the eXcited electron and Core-Hole (XCH) approach had nearly identical energies for transitions to final state orbitals of similar composition and symmetry. These results implied that the charge distributions about the aluminum atoms in (BDI)Al and (BDI)AlH2 are similar relative to the (BDI)AlX2 and (BDI)AlMe2 compounds, despite having different formal oxidation states of +1 and +3, respectively. However, (BDI)Al was unique in that it exhibited a low-energy feature that was attributed to transitions into a low-lying p-orbital of b1 symmetry that is localized on Al and orthogonal to the (BDI)Al plane. The presence of this low-energy unoccupied molecular orbital on electron-rich (BDI)Al distinguishes

  17. Pi Bond Orders and Bond Lengths

    ERIC Educational Resources Information Center

    Herndon, William C.; Parkanyi, Cyril

    1976-01-01

    Discusses three methods of correlating bond orders and bond lengths in unsaturated hydrocarbons: the Pauling theory, the Huckel molecular orbital technique, and self-consistent-field techniques. (MLH)

  18. 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

  19. 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

  20. 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)

  1. 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.

  2. 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.

  3. 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

  4. 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.

  5. 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.

  6. 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

  7. Experimental aspects of the adiabatic approach in estimating the effect of electron screening on alpha decay

    SciTech Connect

    Karpeshin, F. F.; Trzhaskovskaya, M. B.

    2015-12-15

    Special features of the effect of the electron shell on alpha decay that have important experimental implications are studied within the adiabatic approach. The magnitude of the effect is about several tenths of a percent or smaller, depending on the transition energy and on the atomic number. A dominant role of inner shells is shown: more than 80% of the effect is saturated by 1s electrons. This circumstance plays a crucial role for experiments, making it possible to measure this small effect by a difference method in the same storage rings via a comparison of, for example, decay probabilities in bare nuclei and heliumlike ions. The reasons behind the relative success and the applicability limits of the frozen-shell model, which has been used to calculate the effect in question for more than half a century, are analyzed. An interesting experiment aimed at studying charged alpha-particle states is proposed. This experiment will furnish unique information for testing our ideas of the interplay of nonadiabatic and adiabatic processes.

  8. 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).

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  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. 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.

  16. Bonded Lubricants

    NASA Technical Reports Server (NTRS)

    1977-01-01

    Another spinoff to the food processing industry involves a dry lubricant developed by General Magnaplate Corp. of Linden, N.J. Used in such spacecraft as Apollo, Skylab and Viking, the lubricant is a coating bonded to metal surfaces providing permanent lubrication and corrosion resistance. The coating lengthens equipment life and permits machinery to be operated at greater speed, thus increasing productivity and reducing costs. Bonded lubricants are used in scores of commercia1 applications. They have proved particularly valuable to food processing firms because, while increasing production efficiency, they also help meet the stringent USDA sanitation codes for food-handling equipment. For example, a cookie manufacturer plagued production interruptions because sticky batter was clogging the cookie molds had the brass molds coated to solve the problem. Similarly, a pasta producer faced USDA action on a sanitation violation because dough was clinging to an automatic ravioli-forming machine; use of the anti-stick coating on the steel forming plates solved the dual problem of sanitation deficiency and production line downtime.

  17. 27 CFR 19.231 - Accounting for bond coverage.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... 27 Alcohol, Tobacco Products and Firearms 1 2011-04-01 2011-04-01 false Accounting for bond... Deferred Payment and Prepayment of Taxes § 19.231 Accounting for bond coverage. When a proprietor furnishes... charge the bond for the amount of liability incurred on each withdrawal on determination of tax...

  18. Non-adiabatic and adiabatic transitions at level crossing with decay: two- and three-level systems

    NASA Astrophysics Data System (ADS)

    Kenmoe, M. B.; Mkam Tchouobiap, S. E.; Kenfack Sadem, C.; Tchapda, A. B.; Fai, L. C.

    2015-03-01

    We investigate the Landau-Zener (LZ) like dynamics of decaying two- and three-level systems with decay rates {{Γ }1} and {{Γ }2} for levels with minimum and maximum spin projection. Non-adiabatic and adiabatic transition probabilities are calculated from diabatic and adiabatic bases for two- and three-level systems. We extend the familiar two-level model of atoms with decay from the excited state out of the system into the hierarchy of three-level models which can be solved analytically or computationally in a non-perturbative manner. Exact analytical solutions are obtained within the framework of an extended form of the proposed procedure which enables to take into account all possible initial moments rather than large negative time {{t}0}=-∞ as in standard LZ problems. We elucidate the applications of our results from a unified theoretical basis that numerically analyzes the dynamics of a system as probed by experiments.

  19. Basics of Fidelity Bonding.

    ERIC Educational Resources Information Center

    Kahn, Steven P.

    Fidelity bonds are important for an agency to hold to protect itself against any financial loss that can result from dishonest acts by its employees. Three types of fidelity bonds are available to an agency: (1) public official bonds; (2) dishonesty bonds; and (3) faithful performance bonds. Public official bonds are required by state law to be…

  20. 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.

  1. Probing the electronic structure and metal-metal bond of Re{sub 2}Cl{sub 8}{sup 2{minus}} in the gas phase

    SciTech Connect

    Wang, X.B.; Wang, L.S.

    2000-03-08

    Re{sub 2}Cl{sub 8}{sup 2{minus}}, the classical metal complex with a metal-metal multiple bond, was observed in the gas phase for the first time using electrospray. Photodetachment photoelectron spectroscopy (PES) was used to probe its electronic structure, metal-metal bonding, and gas-phase molecular properties. The PES spectra provide a unique and direct picture about the occupied molecular orbitals (Mos) of Re{sub 2}Cl{sub 8}{sup 2{minus}}. Detachments from the metal-metal and metal-ligand bonding Mos were clearly observed and distinguished. The authors found that the metal-metal bonding Mos from the d orbitals ({delta}, {pi}, and {sigma}) have low electron binding energies and yielded three well-resolved detachment bands. The metal-ligand or pure ligand Mos all have higher binding energies and give congested PES features. The ground state of Re{sub 2}Cl{sub 8}{sup 2{minus}} with a configuration of {hor{underscore}ellipsis}{sigma}{sup 2}{pi}{sup 4}{delta}{sup 2} and a formal quadruple Re-Re bond is unequivocally confirmed. The PES spectra yielded a 1.00 eV adiabatic binding energy for the second excess electron in the doubly charged anion. The magnitude of the intramolecular Coulomb repulsion was estimated to be {approximately}2.3 eV using photo-energy-dependent PES spectra. Despite its electronic stability, Re{sub 2}Cl{sub 8}{sup 2{minus}} was found to be metastable against the loss of a Cl{sup {minus}} in the gas phase, suggesting that the Re-Cl bond strength is less than 2.3 eV.

  2. Red and blue shifted hydridic bonds.

    PubMed

    Jabłoński, Mirosław

    2014-09-15

    By performing MP2/aug-cc-pVTZ ab initio calculations for a large set of dimer systems possessing a R-H hydridic bond involved in diverse types of intermolecular interactions (dihydrogen bonds, hydride halogen bonds, hydride hydrogen bonds, and charge-assisted hydride hydrogen bonds), we show that this is rather an elongation than a shortening that a hydride bond undergoes on interaction. Contrary to what might have been expected on the basis of studies in uniform electric field, this elongation is accompanied by a blue instead of red shift of the R-H stretching vibration frequency. We propose that the "additional" elongation of the R-H hydridic bond results from the significant charge outflow from the sigma bonding orbital of R-H that weakens this bond. The more standard red shift obtained for stronger complexes is explained by means of the Hermansson's formula and the particularly strong electric field produced by the H-acceptor molecule. PMID:25043253

  3. Adiabatic transport, Kubo formula and Anderson localization in some lattice and continuum models

    NASA Astrophysics Data System (ADS)

    Elgart, A.

    2006-03-01

    The different explanations of the Quantum Hall Effect rely on the validity of the linear response theory for a system that has infinite extent. We will present recent results on the adiabatic charge transport in this context for two dimensional lattice (joint work with M. Aizenman and J. Schenker) and continuum (joint work with B. Schlein) models of a non-interacting electron gas. It is proved that if the Fermi energy falls in the localization regime then the Hall transport is correctly described by the linear response Kubo formula. The localization condition is set forth by the fractional moment method, which is by now extended also to continuum models (joint work with M. Aizenman, S. Naboko, J. Schenker and G. Stoltz). In the present talk, besides localization criteria, we will discuss some ideas -- Nenciu's asymptotic expansion, generalized space-momentum inequalities, and finite speed of propagation estimates -- which enter the proof.

  4. Nanomagnet coupled to quantum spin Hall edge: An adiabatic quantum motor

    NASA Astrophysics Data System (ADS)

    Arrachea, Liliana; von Oppen, Felix

    2015-11-01

    The precessing magnetization of a magnetic islands coupled to a quantum spin Hall edge pumps charge along the edge. Conversely, a bias voltage applied to the edge makes the magnetization precess. We point out that this device realizes an adiabatic quantum motor and discuss the efficiency of its operation based on a scattering matrix approach akin to Landauer-Büttiker theory. Scattering theory provides a microscopic derivation of the Landau-Lifshitz-Gilbert equation for the magnetization dynamics of the device, including spin-transfer torque, Gilbert damping, and Langevin torque. We find that the device can be viewed as a Thouless motor, attaining unit efficiency when the chemical potential of the edge states falls into the magnetization-induced gap. For more general parameters, we characterize the device by means of a figure of merit analogous to the ZT value in thermoelectrics.

  5. Reprint of : Nanomagnet coupled to quantum spin Hall edge: An adiabatic quantum motor

    NASA Astrophysics Data System (ADS)

    Arrachea, Liliana; von Oppen, Felix

    2016-08-01

    The precessing magnetization of a magnetic islands coupled to a quantum spin Hall edge pumps charge along the edge. Conversely, a bias voltage applied to the edge makes the magnetization precess. We point out that this device realizes an adiabatic quantum motor and discuss the efficiency of its operation based on a scattering matrix approach akin to Landauer-Büttiker theory. Scattering theory provides a microscopic derivation of the Landau-Lifshitz-Gilbert equation for the magnetization dynamics of the device, including spin-transfer torque, Gilbert damping, and Langevin torque. We find that the device can be viewed as a Thouless motor, attaining unit efficiency when the chemical potential of the edge states falls into the magnetization-induced gap. For more general parameters, we characterize the device by means of a figure of merit analogous to the ZT value in thermoelectrics.

  6. Adiabatic quantum computing with phase modulated laser pulses

    PubMed Central

    Goswami, Debabrata

    2005-01-01

    Implementation of quantum logical gates for multilevel systems is demonstrated through decoherence control under the quantum adiabatic method using simple phase modulated laser pulses. We make use of selective population inversion and Hamiltonian evolution with time to achieve such goals robustly instead of the standard unitary transformation language. PMID:17195865

  7. Does temperature increase or decrease in adiabatic decompression of magma?

    NASA Astrophysics Data System (ADS)

    Kilinc, A. I.; Ghiorso, M. S.; Khan, T.

    2011-12-01

    We have modeled adiabatic decompression of an andesitic and a basaltic magma as an isentropic process using the Melts algorithm. Our modeling shows that during adiabatic decompression temperature of andesitic magma increases but temperature of basaltic magma decreases. In an isentropic process entropy is constant so change of temperature with pressure can be written as dT/dP=T (dV/dT)/Cp where T (dV/dT)/Cp is generally positive. If delta P is negative so is delta T. In general, in the absence of phase change, we expect the temperature to decrease with adiabatic decompression. The effect of crystallization is to turn a more entropic phase (liquid) into a less entropic phase (solid), which must be compensated by raising the temperature. If during adiabatic decompression there is small amount or no crystallization, T (dV/dT)/Cp effect which lowers the temperature overwhelms the small amount of crystallization, which raises the temperature, and overall system temperature decreases.

  8. A Kinetic Study of the Adiabatic Polymerization of Acrylamide.

    ERIC Educational Resources Information Center

    Thomson, R. A. M.

    1986-01-01

    Discusses theory, procedures, and results for an experiment which demonstrates the application of basic physics to chemical problems. The experiment involves the adiabatic process, in which polymerization carried out in a vacuum flask is compared to the theoretical prediction of the model with the temperature-time curve obtained in practice. (JN)

  9. The flat Grothendieck-Riemann-Roch theorem without adiabatic techniques

    NASA Astrophysics Data System (ADS)

    Ho, Man-Ho

    2016-09-01

    In this paper we give a simplified proof of the flat Grothendieck-Riemann-Roch theorem. The proof makes use of the local family index theorem and basic computations of the Chern-Simons form. In particular, it does not involve any adiabatic limit computation of the reduced eta-invariant.

  10. Fast Quasi-Adiabatic Gas Cooling: An Experiment Revisited

    ERIC Educational Resources Information Center

    Oss, S.; Gratton, L. M.; Calza, G.; Lopez-Arias, T.

    2012-01-01

    The well-known experiment of the rapid expansion and cooling of the air contained in a bottle is performed with a rapidly responsive, yet very cheap thermometer. The adiabatic, low temperature limit is approached quite closely and measured with our apparatus. A straightforward theoretical model for this process is also presented and discussed.…

  11. 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.

  12. When an Adiabatic Irreversible Expansion or Compression Becomes Reversible

    ERIC Educational Resources Information Center

    Anacleto, Joaquim; Ferreira, J. M.; Soares, A. A.

    2009-01-01

    This paper aims to contribute to a better understanding of the concepts of a "reversible process" and "entropy". For this purpose, an adiabatic irreversible expansion or compression is analysed, by considering that an ideal gas is expanded (compressed), from an initial pressure P[subscript i] to a final pressure P[subscript f], by being placed in…

  13. Digitized adiabatic quantum computing with a superconducting circuit.

    PubMed

    Barends, R; Shabani, A; Lamata, L; Kelly, J; Mezzacapo, A; Las Heras, U; Babbush, R; Fowler, A G; Campbell, B; Chen, Yu; Chen, Z; Chiaro, B; Dunsworth, A; Jeffrey, E; Lucero, E; Megrant, A; Mutus, J Y; Neeley, M; Neill, C; O'Malley, P J J; Quintana, C; Roushan, P; Sank, D; Vainsencher, A; Wenner, J; White, T C; Solano, E; Neven, H; Martinis, John M

    2016-06-01

    Quantum mechanics can help to solve complex problems in physics and chemistry, provided they can be programmed in a physical device. In adiabatic quantum computing, a system is slowly evolved from the ground state of a simple initial Hamiltonian to a final Hamiltonian that encodes a computational problem. The appeal of this approach lies in the combination of simplicity and generality; in principle, any problem can be encoded. In practice, applications are restricted by limited connectivity, available interactions and noise. A complementary approach is digital quantum computing, which enables the construction of arbitrary interactions and is compatible with error correction, but uses quantum circuit algorithms that are problem-specific. Here we combine the advantages of both approaches by implementing digitized adiabatic quantum computing in a superconducting system. We tomographically probe the system during the digitized evolution and explore the scaling of errors with system size. We then let the full system find the solution to random instances of the one-dimensional Ising problem as well as problem Hamiltonians that involve more complex interactions. This digital quantum simulation of the adiabatic algorithm consists of up to nine qubits and up to 1,000 quantum logic gates. The demonstration of digitized adiabatic quantum computing in the solid state opens a path to synthesizing long-range correlations and solving complex computational problems. When combined with fault-tolerance, our approach becomes a general-purpose algorithm that is scalable. PMID:27279216

  14. Digitized adiabatic quantum computing with a superconducting circuit

    NASA Astrophysics Data System (ADS)

    Barends, R.; Shabani, A.; Lamata, L.; Kelly, J.; Mezzacapo, A.; Heras, U. Las; Babbush, R.; Fowler, A. G.; Campbell, B.; Chen, Yu; Chen, Z.; Chiaro, B.; Dunsworth, A.; Jeffrey, E.; Lucero, E.; Megrant, A.; Mutus, J. Y.; Neeley, M.; Neill, C.; O’Malley, P. J. J.; Quintana, C.; Roushan, P.; Sank, D.; Vainsencher, A.; Wenner, J.; White, T. C.; Solano, E.; Neven, H.; Martinis, John M.

    2016-06-01

    Quantum mechanics can help to solve complex problems in physics and chemistry, provided they can be programmed in a physical device. In adiabatic quantum computing, a system is slowly evolved from the ground state of a simple initial Hamiltonian to a final Hamiltonian that encodes a computational problem. The appeal of this approach lies in the combination of simplicity and generality; in principle, any problem can be encoded. In practice, applications are restricted by limited connectivity, available interactions and noise. A complementary approach is digital quantum computing, which enables the construction of arbitrary interactions and is compatible with error correction, but uses quantum circuit algorithms that are problem-specific. Here we combine the advantages of both approaches by implementing digitized adiabatic quantum computing in a superconducting system. We tomographically probe the system during the digitized evolution and explore the scaling of errors with system size. We then let the full system find the solution to random instances of the one-dimensional Ising problem as well as problem Hamiltonians that involve more complex interactions. This digital quantum simulation of the adiabatic algorithm consists of up to nine qubits and up to 1,000 quantum logic gates. The demonstration of digitized adiabatic quantum computing in the solid state opens a path to synthesizing long-range correlations and solving complex computational problems. When combined with fault-tolerance, our approach becomes a general-purpose algorithm that is scalable.

  15. Nonadiabatic quantum Liouville and master equations in the adiabatic basis

    SciTech Connect

    Jang, Seogjoo

    2012-12-14

    A compact form of nonadiabatic molecular Hamiltonian in the basis of adiabatic electronic states and nuclear position states is presented. The Hamiltonian, which includes both the first and the second derivative couplings, is Hermitian and thus leads to a standard expression for the quantum Liouville equation for the density operator. With the application of a projection operator technique, a quantum master equation for the diagonal components of the density operator is derived. Under the assumption that nuclear states are much more short ranged compared to electronic states and assuming no singularity, a semi-adiabatic approximation is invoked, which results in expressions for the nonadiabatic molecular Hamiltonian and the quantum Liouville equation that are much more amenable to advanced quantum dynamics calculation. The semi-adiabatic approximation is also applied to a resonance energy transfer system consisting of a donor and an acceptor interacting via Coulomb terms, and explicit detailed expressions for exciton-bath Hamiltonian including all the non-adiabatic terms are derived.

  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. Adiabatic single scan two-dimensional NMR spectrocopy.

    PubMed

    Pelupessy, Philippe

    2003-10-01

    New excitation schemes, based on the use adiabatic pulses, for single scan two-dimensional NMR experiments (Frydman et al., Proc. Nat. Acad. Sci. 2002, 99, 15 858-15 862) are introduced. The advantages are discussed. Applications in homo- and heteronuclear experiments are presented. PMID:14519020

  18. SIMULATION OF CONTINUOUS-CONTACT SEPARATION PROCESSES: MULTICOMPONENT, ADIABATIC ABSORPTION

    EPA Science Inventory

    A new algorithm has been developed for the steady-state simulation of multicomponent, adiabatic absorption in packed columns. The system of differential model equations that describe the physical absorption process is reduced to algebraic equations by using a finite difference me...

  19. Equations for Adiabatic but Rotational Steady Gas Flows without Friction

    NASA Technical Reports Server (NTRS)

    Schaefer, Manfred

    1947-01-01

    This paper makes the following assumptions: 1) The flowing gases are assumed to have uniform energy distribution. ("Isoenergetic gas flows," that is valid with the same constants for the the energy equation entire flow.) This is correct, for example, for gas flows issuing from a region of constant pressure, density, temperature, end velocity. This property is not destroyed by compression shocks because of the universal validity of the energy law. 2) The gas behaves adiabatically, not during the compression shock itself but both before and after the shock. However, the adiabatic equation (p/rho(sup kappa) = C) is not valid for the entire gas flow with the same constant C but rather with an appropriate individual constant for each portion of the gas. For steady flows, this means that the constant C of the adiabatic equation is a function of the stream function. Consequently, a gas that has been flowing "isentropically",that is, with the same constant C of the adiabatic equation throughout (for example, in origination from a region of constant density, temperature, and velocity) no longer remains isentropic after a compression shock if the compression shock is not extremely simple (wedge shaped in a two-dimensional flow or cone shaped in a rotationally symmetrical flow). The solution of nonisentropic flows is therefore an urgent necessity.

  20. Non-adiabatic response of relativistic radiation belt electrons to GEM magnetic storms

    NASA Astrophysics Data System (ADS)

    McAdams, K. L.; Reeves, G. D.

    The importance of fully adiabatic effects in the relativistic radiation belt electron response to magnetic storms is poorly characterized due to many difficulties in calculating adiabatic flux response. Using the adiabatic flux model of Kim and Chan [1997a] and Los Alamos National Laboratory geosynchronous satellite data, we examine the relative timing of the adiabatic and non-adiabatic flux responses. In the three storms identified by the GEM community for in depth study, the non-adiabatic energization occurs hours earlier than the adiabatic re-energization. The adiabatic energization can account for only 10-20% of the flux increases in the first recovery stages, and only 1% of the flux increase if there is continuing activity.

  1. A non-adiabatic dynamics study of octatetraene: the radiationless conversion from S2 to S1.

    PubMed

    Qu, Zexing; Liu, Chungen

    2013-12-28

    Simulation of the excited state dynamics of all-trans-1,3,5,7-octatetraene has been performed to investigate the ultrafast radiationless S2 → S1 internal conversion process. Multireference configuration interaction with single excitation method has been employed to optimize the equilibrium structure of the excited states, as well as the S2/S1 conical intersection, and to investigate the non-adiabatic molecular dynamics of the S2/S1 state transition. At the conical intersection, the molecule is found to be distorted from the original planar trans structure to a nearly perpendicular conformation around C3-C4 bond, with the torsion angle being about 107°. Such structural change can result in mutual approaching of states S2 and S1 in energy, and drastically increase the nonadiabatic coupling between the two states by destroying the inter-state symmetry prohibition in the electronic wavefunctions. Surface-hopping molecular dynamics simulations are performed to describe the non-adiabatic process. Upon the Franck-Condon excitation to the S2 state, the molecule quickly twists its C3-C4 bond and approaches the conical intersection region, where it can undergo efficient internal conversion to S1. The decay time constant (τ) of S2 state is estimated to be around 251 fs by fitting the occupation number of average fraction of trajectories using an exponential damping function. This value is reasonably consistent with previous experimental measurements of around 300-400 fs. PMID:24387367

  2. A Preorganized Hydrogen Bond Network and Its Effect on Anion Stability

    SciTech Connect

    Samet, Masoud; Wang, Xue B.; Kass, Steven R.

    2014-08-07

    Rigid tricyclic locked in all axial 1,3,5-cyclohexanetriol derivatives with 0–3 trifluoromethyl groups were synthesized and photoelectron spectra of their conjugate bases and chloride anion clusters are reported along with density functional computations. The resulting vertical and adiabatic detachment energies provide measures of the anion stabilization due to the hydrogen bond network and inductive effects. The latter mechanism is found to be transmitted through space via hydrogen bonds

  3. Non-adiabatic resonant conversion of solar neutrinos in three generations

    NASA Astrophysics Data System (ADS)

    Kim, C. W.; Nussinov, S.; Sze, W. K.

    1987-02-01

    The survival probability of solar electron neutrinos after non-adiabatic passage through the resonance-oscillation region in the Sun is discussed for the case of three generations. A method to calculate three-generation Landau-Zener transition probabilities between adiabatic states is described. We also discuss how the Landua-Zener probability is modified in the extreme non-adiabatic case.

  4. Thermodynamic model for bouncing charged particles inside a capacitor

    NASA Astrophysics Data System (ADS)

    Rezaeizadeh, Amin; Mameghani, Pooya

    2013-08-01

    We introduce an equation of state for a conducting particle inside a charged parallel-plate capacitor and show that it is similar to the equation of state for an ideal gas undergoing an adiabatic process. We describe a simple experiment that shows reasonable agreement with the theoretical model.

  5. Ultra-Flexible Thermal Bus for Use in the Astro-H Adiabatic Demagnetization Refrigerator

    NASA Technical Reports Server (NTRS)

    Kimball, Mark O.; Shirron, Peter J.

    2015-01-01

    The adiabatic demagnetization refrigerator (ADR) developed for the Astro-H Soft-X-ray Spectrometer (SXS) is a multi-stage solid-state cooler. It is capable of holding the SXS detector array at 0.050 K for greater than 24 hours with a recycle time of less than one hour. This quick recycle time relies upon high-conductivity thermal straps to couple the individual stages to a pair of heat switches without imposing a lateral load on the paramagnetic salt pills. To accomplish this we construct thermal straps using a technique of diffusion bonding together the ends of high-purity copper straps leaving the length between as individual foils. A thermal bus created this way has a thermal conductivity comparable to a solid strap of the equivalent thickness but with much-increased flexibility. The technique for selecting the base material, machining, cleaning, forming into final shape, and finally bonding together individual foils will be discussed along with examples of complete straps in various geometries.

  6. The Influence of the Terminal Phosphorothioate Diester Bond on the DNA Oxidation Process. An Experimental and Theoretical Approach.

    PubMed

    Karwowski, Boleslaw T

    2015-01-01

    In this study, the influence of the terminal phosphorothioate (PT) internucleotide bond in ds-DNA on the oxidation process was taken into consideration. The interaction of UV with the targeted oligonucleotide leads to an electron ejection and radical cation "hole" migration through the ds-DNA until it is trapped irreversibly in a suitable place. Phosphorothiate internucleotide bonds were detected in the bacterial genome; however, their role is still unclear. In this study a PAGE analysis of irradiated ds-DNA showed that the degradation rea ction was slowed down by the presence PT next to the anthraquinone moiety. Further, theoretical study shows that [RP] AQ-PS-dG can adopt a slightly lower ionisation potential energy and triplet excited state with a subsequent slightly higher adiabatic electron affinity value in comparison with [SP] AQ-PS-dG and AQ-PO-dG. Moreover, the energy gap between HOMO and LUMO, indicated the radical stabilisation properties of [RP] AQ-PS-dG, which can hinder the charge transfer through ds-DNA. PMID:26184129

  7. The effect of pi-stacking, h-bonding, and electrostatic interactions on the ionization energies of nucleic acid bases: adenine-adenine, thymine-thymine and adenine-thymine dimers

    SciTech Connect

    Bravaya, Ksenia B.; Kostko, Oleg; Ahmed, Musahid; Krylov, Anna I.

    2009-09-02

    A combined theoretical and experimental study of the ionized dimers of thymine and adenine, TT, AA, and AT, is presented. Adiabatic and vertical ionization energies(IEs) for monomers and dimers as well as thresholds for the appearance of the protonated species are reported and analyzed. Non-covalent interactions stronglyaffect the observed IEs. The magnitude and the nature of the effect is different for different isomers of the dimers. The computations reveal that for TT, the largestchanges in vertical IEs (0.4 eV) occur in asymmetric h-bonded and symmetric pi- stacked isomers, whereas in the lowest-energy symmetric h-bonded dimer the shiftin IEs is much smaller (0.1 eV). The origin of the shift and the character of the ionized states is different in asymmetric h-bonded and symmetric stacked isomers. Inthe former, the initial hole is localized on one of the fragments, and the shift is due to the electrostatic stabilization of the positive charge of the ionized fragment by thedipole moment of the neutral fragment. In the latter, the hole is delocalized, and the change in IE is proportional to the overlap of the fragments' MOs. The shifts in AAare much smaller due to a less effcient overlap and a smaller dipole moment. The ionization of the h-bonded dimers results in barrierless (or nearly barrierless) protontransfer, whereas the pi-stacked dimers relax to structures with the hole stabilized by the delocalization or electrostatic interactions.

  8. Folding without charges

    PubMed Central

    Kurnik, Martin; Hedberg, Linda; Danielsson, Jens; Oliveberg, Mikael

    2012-01-01

    Surface charges of proteins have in several cases been found to function as “structural gatekeepers,” which avoid unwanted interactions by negative design, for example, in the control of protein aggregation and binding. The question is then if side-chain charges, due to their desolvation penalties, play a corresponding role in protein folding by avoiding competing, misfolded traps? To find out, we removed all 32 side-chain charges from the 101-residue protein S6 from Thermus thermophilus. The results show that the charge-depleted S6 variant not only retains its native structure and cooperative folding transition, but folds also faster than the wild-type protein. In addition, charge removal unleashes pronounced aggregation on longer timescales. S6 provides thus an example where the bias toward native contacts of a naturally evolved protein sequence is independent of charges, and point at a fundamental difference in the codes for folding and intermolecular interaction: specificity in folding is governed primarily by hydrophobic packing and hydrogen bonding, whereas solubility and binding relies critically on the interplay of side-chain charges. PMID:22454493

  9. The gravito-electrodynamics of charged dust in planetary ring systems

    NASA Technical Reports Server (NTRS)

    Mendis, D. A.; Hill, J. R.; Northrop, T. G.

    1982-01-01

    The dynamics of micron and submicron sized dust grains moving under the combined influence of planetary gravitation and the electromagnetic forces within the corotating regions of planetary magnetospheres are discussed. Magnetogravitational capture of charged grains in planetary rings is outlined. The adiabatic motion of charged dust is reviewed.

  10. A Series of Diamagnetic Pyridine Monoimine Rhenium Complexes with Different Degrees of Metal-to-Ligand Charge Transfer: Correlating (13) C NMR Chemical Shifts with Bond Lengths in Redox-Active Ligands.

    PubMed

    Sieh, Daniel; Kubiak, Clifford P

    2016-07-18

    A set of pyridine monoimine (PMI) rhenium(I) tricarbonyl chlorido complexes with substituents of different steric and electronic properties was synthesized and fully characterized. Spectroscopic (NMR and IR) and single-crystal X-ray diffraction analyses of these complexes showed that the redox-active PMI ligands are neutral and that the overall electronic structure is little affected by the choices of the substituent at the ligand backbone. One- and two-electron reduction products were prepared from selected starting compounds and could also be characterized by multiple spectroscopic methods and X-ray diffraction. The final product of a one-electron reduction in THF is a diamagnetic metal-metal-bonded dimer after loss of the chlorido ligand. Bond lengths in and NMR chemical shifts of the PMI ligand backbone indicate partial electron transfer to the ligand. Two-electron reduction in THF also leads to the loss of the chlorido ligand and a pentacoordinate complex is obtained. The comparison with reported bond lengths and (13) C NMR chemical shifts of doubly reduced free pyridine monoaldimine ligands indicates that both redox equivalents in the doubly reduced rhenium complex investigated here are located in the PMI ligand. With diamagnetic complexes varying over three formal reduction stages at the PMI ligand we were, for the first time, able to establish correlations of the (13) C NMR chemical shifts with the relevant bond lengths in redox-active ligands over a full redox series. PMID:27319753

  11. Necessary and sufficient condition for quantum adiabatic evolution by unitary control fields

    NASA Astrophysics Data System (ADS)

    Wang, Zhen-Yu; Plenio, Martin B.

    2016-05-01

    We decompose the quantum adiabatic evolution as the products of gauge invariant unitary operators and obtain the exact nonadiabatic correction in the adiabatic approximation. A necessary and sufficient condition that leads to adiabatic evolution with geometric phases is provided, and we determine that in the adiabatic evolution, while the eigenstates are slowly varying, the eigenenergies and degeneracy of the Hamiltonian can change rapidly. We exemplify this result by the example of the adiabatic evolution driven by parametrized pulse sequences. For driving fields that are rotating slowly with the same average energy and evolution path, fast modulation fields can have smaller nonadiabatic errors than obtained under the traditional approach with a constant amplitude.

  12. Chemical Bonds II

    ERIC Educational Resources Information Center

    Sanderson, R. T.

    1972-01-01

    The continuation of a paper discussing chemical bonding from a bond energy viewpoint, with a number of examples of single and multiple bonds. (Part I appeared in volume 1 number 3, pages 16-23, February 1972.) (AL)

  13. What Determines Bond Costs. Municipal Bonds Series.

    ERIC Educational Resources Information Center

    Young, Douglas; And Others

    Public officials in small towns who participate infrequently in the bond market need information about bond financing. This publication, one in a series of booklets published by the Western Rural Development Center using research gathered between 1967-77, discusses factors influencing the marketability and cost of bond financing for towns and…

  14. Experimental implementation of adiabatic passage between different topological orders.

    PubMed

    Peng, Xinhua; Luo, Zhihuang; Zheng, Wenqiang; Kou, Supeng; Suter, Dieter; Du, Jiangfeng

    2014-08-22

    Topological orders are exotic phases of matter existing in strongly correlated quantum systems, which are beyond the usual symmetry description and cannot be distinguished by local order parameters. Here we report an experimental quantum simulation of the Wen-plaquette spin model with different topological orders in a nuclear magnetic resonance system, and observe the adiabatic transition between two Z(2) topological orders through a spin-polarized phase by measuring the nonlocal closed-string (Wilson loop) operator. Moreover, we also measure the entanglement properties of the topological orders. This work confirms the adiabatic method for preparing topologically ordered states and provides an experimental tool for further studies of complex quantum systems. PMID:25192080

  15. Adiabatic and diabatic process of sum frequency conversion.

    PubMed

    Liqing, Ren; Yongfang, Li; Baihong, Li; Lei, Wang; Zhaohua, Wang

    2010-09-13

    Based on the dressed state formalism, we obtain the adiabatic criterion of the sum frequency conversion. We show that this constraint restricts the energy conversion between the two dressed fields, which are superpositions of the signal field and the sum frequency field. We also show that the evolution of the populations of the dressed fields, which in turn describes the conversion of light photons from the seed frequency to the sum frequency during propagation through the nonlinear crystal. Take the quasiphased matched (QPM) scheme as an example, we calculate the expected bandwidth of the frequency conversion process, and its dependence on the length of the crystal. We demonstrate that the evolutionary patterns of the sum frequency field's energy are similar to the Fresnel diffraction of a light field. We finally show that the expected bandwidth can be also deduced from the evolution of the adiabaticity of the dressed fileds. PMID:20940935

  16. On the off-stoichiometric peaking of adiabatic flame temperature

    SciTech Connect

    Law, C.K.; Lu, T.F.; Makino, A.

    2006-06-15

    The characteristic rich shifting of the maximum adiabatic flame temperature from the stoichiometric value for mixtures of hydrocarbon and air is demonstrated to be caused by product dissociation and hence reduced amount of heat release. Since the extent of dissociation is greater on the lean side as a result of the stoichiometry of dissociated products, the peaking occurs on the rich side. The specific heat per unit mass of the mixture is shown to increase monotonically with increasing fuel concentration, and as such tends to shift the peak toward the lean side. It is further shown that this is the cause for the lean shifting of the adiabatic flame temperature of oxidizer-enriched mixtures of N{sub m}H{sub n} and F{sub 2} and of NH{sub 3} and O{sub 2}, with various amounts of inert dilution, even though their maximum heat release still peaks on the rich side. (author)

  17. Microscopic expression for heat in the adiabatic basis.

    PubMed

    Polkovnikov, Anatoli

    2008-11-28

    We derive a microscopic expression for the instantaneous diagonal elements of the density matrix rho(nn)(t) in the adiabatic basis for an arbitrary time-dependent process in a closed Hamiltonian system. If the initial density matrix is stationary (diagonal) then this expression contains only squares of absolute values of matrix elements of the evolution operator, which can be interpreted as transition probabilities. We then derive the microscopic expression for the heat defined as the energy generated due to transitions between instantaneous energy levels. If the initial density matrix is passive [diagonal with rho(nn)(0) monotonically decreasing with energy] then the heat is non-negative in agreement with basic expectations of thermodynamics. Our findings also can be used for systematic expansion of various observables around the adiabatic limit. PMID:19113464

  18. 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.

  19. Fastest Effectively Adiabatic Transitions for a Collection of Harmonic Oscillators.

    PubMed

    Boldt, Frank; Salamon, Peter; Hoffmann, Karl Heinz

    2016-05-19

    We discuss fastest effectively adiabatic transitions (FEATs) for a collection of noninteracting harmonic oscillators with shared controllable real frequencies. The construction of such transitions is presented for given initial and final equilibrium states, and the dependence of the minimum time control on the interval of achievable frequencies is discussed. While the FEAT times and associated FEAT processes are important in their own right as optimal controls, the FEAT time is an added feature which provides a measure of the quality of a shortcut to adiabaticity (STA). The FEAT time is evaluated for a previously reported experiment, wherein a cloud of Rb atoms is cooled following a STA recipe that took about twice as long as the FEAT speed limit, a time efficiency of 50%. PMID:26811863

  20. Ultrafast adiabatic manipulation of slow light in a photonic crystal

    SciTech Connect

    Kampfrath, T.; Kuipers, L.; Beggs, D. M.; White, T. P.; Krauss, T. F.; Melloni, A.

    2010-04-15

    We demonstrate by experiment and theory that a light pulse propagating through a Si-based photonic-crystal waveguide is adiabatically blueshifted when the refractive index of the Si is reduced on a femtosecond time scale. Thanks to the use of slow-light modes, we are able to shift a 1.3-ps pulse at telecom frequencies by 0.3 THz with an efficiency as high as 80% in a waveguide as short as 19{mu}m. An analytic theory reproduces the experimental data excellently, which shows that adiabatic dynamics are possible even on the femtosecond time scale as long as the external stimulus conserves the spatial symmetry of the system.

  1. Adiabatic tapered optical fiber fabrication in two step etching

    NASA Astrophysics Data System (ADS)

    Chenari, Z.; Latifi, H.; Ghamari, S.; Hashemi, R. S.; Doroodmand, F.

    2016-01-01

    A two-step etching method using HF acid and Buffered HF is proposed to fabricate adiabatic biconical optical fiber tapers. Due to the fact that the etching rate in second step is almost 3 times slower than the previous droplet etching method, terminating the fabrication process is controllable enough to achieve a desirable fiber diameter. By monitoring transmitted spectrum, final diameter and adiabaticity of tapers are deduced. Tapers with losses about 0.3 dB in air and 4.2 dB in water are produced. The biconical fiber taper fabricated using this method is used to excite whispering gallery modes (WGMs) on a microsphere surface in an aquatic environment. So that they are suitable to be used in applications like WGM biosensors.

  2. Fluctuations of work in nearly adiabatically driven open quantum systems.

    PubMed

    Suomela, S; Salmilehto, J; Savenko, I G; Ala-Nissila, T; Möttönen, M

    2015-02-01

    We extend the quantum jump method to nearly adiabatically driven open quantum systems in a way that allows for an accurate account of the external driving in the system-environment interaction. Using this framework, we construct the corresponding trajectory-dependent work performed on the system and derive the integral fluctuation theorem and the Jarzynski equality for nearly adiabatic driving. We show that such identities hold as long as the stochastic dynamics and work variable are consistently defined. We numerically study the emerging work statistics for a two-level quantum system and find that the conventional diabatic approximation is unable to capture some prominent features arising from driving, such as the continuity of the probability density of work. Our results reveal the necessity of using accurate expressions for the drive-dressed heat exchange in future experiments probing jump time distributions. PMID:25768477

  3. Adiabatic creation of atomic squeezing in dark states versus decoherences

    SciTech Connect

    Gong, Z. R.; Sun, C. P.; Wang Xiaoguang

    2010-07-15

    We study the multipartite correlations of the multiatom dark states, which are characterized by the atomic squeezing beyond the pairwise entanglement. It is shown that, in the photon storage process with atomic ensemble via the electromagnetically induced transparency (EIT) mechanism, the atomic squeezing and the pairwise entanglement can be created by adiabatically manipulating the Rabi frequency of the classical light field on the atomic ensemble. We also consider the sudden death for the atomic squeezing and the pairwise entanglement under various decoherence channels. An optimal time for generating the greatest atomic squeezing and pairwise entanglement is obtained by studying in detail the competition between the adiabatic creation of quantum correlation in the atomic ensemble and the decoherence that we describe with three typical decoherence channels.

  4. Steam bottoming cycle for an adiabatic diesel engine

    NASA Technical Reports Server (NTRS)

    Poulin, E.; Demier, R.; Krepchin, I.; Walker, D.

    1984-01-01

    Steam bottoming cycles using adiabatic diesel engine exhaust heat which projected substantial performance and economic benefits for long haul trucks were studied. Steam cycle and system component variables, system cost, size and performance were analyzed. An 811 K/6.90 MPa state of the art reciprocating expander steam system with a monotube boiler and radiator core condenser was selected for preliminary design. The costs of the diesel with bottoming system (TC/B) and a NASA specified turbocompound adiabatic diesel with aftercooling with the same total output were compared, the annual fuel savings less the added maintenance cost was determined to cover the increase initial cost of the TC/B system in a payback period of 2.3 years. Steam bottoming system freeze protection strategies were developed, technological advances required for improved system reliability are considered and the cost and performance of advanced systes are evaluated.

  5. Engineering adiabaticity at an avoided crossing with optimal control

    NASA Astrophysics Data System (ADS)

    Chasseur, T.; Theis, L. S.; Sanders, Y. R.; Egger, D. J.; Wilhelm, F. K.

    2015-04-01

    We investigate ways to optimize adiabaticity and diabaticity in the Landau-Zener model with nonuniform sweeps. We show how diabaticity can be engineered with a pulse consisting of a linear sweep augmented by an oscillating term. We show that the oscillation leads to jumps in populations whose value can be accurately modeled using a model of multiple, photon-assisted Landau-Zener transitions, which generalizes work by Wubs et al. [New J. Phys. 7, 218 (2005)], 10.1088/1367-2630/7/1/218. We extend the study on diabaticity using methods derived from optimal control. We also show how to preserve adiabaticity with optimal pulses at limited time, finding a nonuniform quantum speed limit.

  6. Adiabatic Tip-Plasmon Focusing for Nano-Raman Spectroscopy

    SciTech Connect

    Berweger, Samuel; Atkin, Joanna M.; Olmon, Robert L.; Raschke, Markus Bernd

    2010-12-16

    True nanoscale optical spectroscopy requires the efficient delivery of light for a spatially nanoconfined excitation. We utilize adiabatic plasmon focusing to concentrate an optical field into the apex of a scanning probe tip of {approx}10 nm in radius. The conical tips with the ability for two-stage optical mode matching of the surface plasmon polariton (SPP) grating-coupling and the adiabatic propagating SPP conversion into a localized SPP at the tip apex represent a special optical antenna concept for far-field transduction into nanoscale excitation. The resulting high nanofocusing efficiency and the spatial separation of the plasmonic grating coupling element on the tip shaft from the near-field apex probe region allows for true background-free nanospectroscopy. As an application, we demonstrate tip-enhanced Raman spectroscopy (TERS) of surface molecules with enhanced contrast and its extension into the near-IR with 800 nm excitation.

  7. Adiabatic far-field sub-diffraction imaging

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

    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 decays in space and thus cannot reach the imaging plane. We introduce here an 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-50 nm imaging resolution in visible. Our approach provides a means to extend the domain of geometrical optics to a deep sub-wavelength scale.

  8. Adiabatic nonlinear waves with trapped particles. II. Wave dispersion

    SciTech Connect

    Dodin, I. Y.; Fisch, N. J.

    2012-01-15

    A general nonlinear dispersion relation is derived in a nondifferential form for an adiabatic sinusoidal Langmuir wave in collisionless plasma, allowing for an arbitrary distribution of trapped electrons. The linear dielectric function is generalized, and the nonlinear kinetic frequency shift {omega}{sub NL} is found analytically as a function of the wave amplitude a. Smooth distributions yield {omega}{sub NL}{proportional_to}{radical}(a), as usual. However, beam-like distributions of trapped electrons result in different power laws, or even a logarithmic nonlinearity, which are derived as asymptotic limits of the same dispersion relation. Such beams are formed whenever the phase velocity changes, because the trapped distribution is in autoresonance and thus evolves differently from the passing distribution. Hence, even adiabatic {omega}{sub NL}(a) is generally nonlocal.

  9. Charge density waves and local states in quasi-one-dimensional mixed valence inorganic complexes

    NASA Astrophysics Data System (ADS)

    Conradson, S. D.; Stroud, M. A.; Zietlow, M. H.; Swanson, B. I.; Baeriswyl, D.; Bishop, A. R.

    1988-02-01

    The ground state structures and local states associated with chemical defects in quasi-one-dimensional halogen ( X) bridged transition metal ( M) mixed valence solids of MX and MMX type have been studied. An adiabatic Hartree-Fock theoretical framework is presented and representative members are classified. The MX materials provide a class whose strong electron-phonon coupling usually favors a charge-density-wave (CDW) ground state. However, the coupling strength can be chemically tuned (e.g., by extension to MMX systems) or altered by pressure, driving the ground state structures towards, e.g., a bond-order-wave (BOW) phase. Electron-phonon driven self-trapped states are expected in both the CDW or BOW regimes. Resonance Raman spectra of the MMX solid K 4[Pt 2(P 2O 5H 2) 4Cl]·H 2O show, in addition to the homogeneous ground state modes, sharp new features with excitation profiles shifted to the red of the intervalence-charge-transfer (IVCT) band. We attribute these new bands to a local polaron state formed by oxidation of the Pt 2Cl chain by a chemical defect. The observed spectral characteristics of this local state are in good agreement with theoretical predictions.

  10. Photoinduced Charge Transfer from Titania to Surface Doping Site

    PubMed Central

    Inerbaev, Talgat; Hoefelmeyer, James D.; Kilin, Dmitri S.

    2013-01-01

    We evaluate a theoretical model in which Ru is substituting for Ti at the (100) surface of anatase TiO2. Charge transfer from the photo-excited TiO2 substrate to the catalytic site triggers the photo-catalytic event (such as water oxidation or reduction half-reaction). We perform ab-initio computational modeling of the charge transfer dynamics on the interface of TiO2 nanorod and catalytic site. A slab of TiO2 represents a fragment of TiO2 nanorod in the anatase phase. Titanium to ruthenium replacement is performed in a way to match the symmetry of TiO2 substrate. One molecular layer of adsorbed water is taken into consideration to mimic the experimental conditions. It is found that these adsorbed water molecules saturate dangling surface bonds and drastically affect the electronic properties of systems investigated. The modeling is performed by reduced density matrix method in the basis of Kohn-Sham orbitals. A nano-catalyst modeled through replacement defect contributes energy levels near the bottom of the conduction band of TiO2 nano-structure. An exciton in the nano-rod is dissipating due to interaction with lattice vibrations, treated through non-adiabatic coupling. The electron relaxes to conduction band edge and then to the Ru cite with faster rate than hole relaxes to the Ru cite. These results are of the importance for an optimal design of nano-materials for photo-catalytic water splitting and solar energy harvesting. PMID:23795229

  11. Photoinduced Charge Transfer from Titania to Surface Doping Site.

    PubMed

    Inerbaev, Talgat; Hoefelmeyer, James D; Kilin, Dmitri S

    2013-05-16

    We evaluate a theoretical model in which Ru is substituting for Ti at the (100) surface of anatase TiO2. Charge transfer from the photo-excited TiO2 substrate to the catalytic site triggers the photo-catalytic event (such as water oxidation or reduction half-reaction). We perform ab-initio computational modeling of the charge transfer dynamics on the interface of TiO2 nanorod and catalytic site. A slab of TiO2 represents a fragment of TiO2 nanorod in the anatase phase. Titanium to ruthenium replacement is performed in a way to match the symmetry of TiO2 substrate. One molecular layer of adsorbed water is taken into consideration to mimic the experimental conditions. It is found that these adsorbed water molecules saturate dangling surface bonds and drastically affect the electronic properties of systems investigated. The modeling is performed by reduced density matrix method in the basis of Kohn-Sham orbitals. A nano-catalyst modeled through replacement defect contributes energy levels near the bottom of the conduction band of TiO2 nano-structure. An exciton in the nano-rod is dissipating due to interaction with lattice vibrations, treated through non-adiabatic coupling. The electron relaxes to conduction band edge and then to the Ru cite with faster rate than hole relaxes to the Ru cite. These results are of the importance for an optimal design of nano-materials for photo-catalytic water splitting and solar energy harvesting. PMID:23795229

  12. 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.

  13. Adiabaticity and gravity theory independent conservation laws for cosmological perturbations

    NASA Astrophysics Data System (ADS)

    Romano, Antonio Enea; Mooij, Sander; Sasaki, Misao

    2016-04-01

    We carefully study the implications of adiabaticity for the behavior of cosmological perturbations. There are essentially three similar but different definitions of non-adiabaticity: one is appropriate for a thermodynamic fluid δPnad, another is for a general matter field δPc,nad, and the last one is valid only on superhorizon scales. The first two definitions coincide if cs2 = cw2 where cs is the propagation speed of the perturbation, while cw2 = P ˙ / ρ ˙ . Assuming the adiabaticity in the general sense, δPc,nad = 0, we derive a relation between the lapse function in the comoving slicing Ac and δPnad valid for arbitrary matter field in any theory of gravity, by using only momentum conservation. The relation implies that as long as cs ≠cw, the uniform density, comoving and the proper-time slicings coincide approximately for any gravity theory and for any matter field if δPnad = 0 approximately. In the case of general relativity this gives the equivalence between the comoving curvature perturbation Rc and the uniform density curvature perturbation ζ on superhorizon scales, and their conservation. This is realized on superhorizon scales in standard slow-roll inflation. We then consider an example in which cw =cs, where δPnad = δPc,nad = 0 exactly, but the equivalence between Rc and ζ no longer holds. Namely we consider the so-called ultra slow-roll inflation. In this case both Rc and ζ are not conserved. In particular, as for ζ, we find that it is crucial to take into account the next-to-leading order term in ζ's spatial gradient expansion to show its non-conservation, even on superhorizon scales. This is an example of the fact that adiabaticity (in the thermodynamic sense) is not always enough to ensure the conservation of Rc or ζ.

  14. Geometric Phase for Adiabatic Evolutions of General Quantum States

    SciTech Connect

    Wu, Biao; Liu, Jie; Niu, Qian; Singh, David J

    2005-01-01

    The concept of a geometric phase (Berry's phase) is generalized to the case of noneigenstates, which is applicable to both linear and nonlinear quantum systems. This is particularly important to nonlinear quantum systems, where, due to the lack of the superposition principle, the adiabatic evolution of a general state cannot be described in terms of eigenstates. For linear quantum systems, our new geometric phase reduces to a statistical average of Berry's phases. Our results are demonstrated with a nonlinear two-level model.

  15. Breakdown of adiabaticity when loading ultracold atoms in optical lattices

    NASA Astrophysics Data System (ADS)

    Zakrzewski, Jakub; Delande, Dominique

    2009-07-01

    Realistic simulations of current ultracold atom experiments in optical lattices show that the ramping up of the optical lattice is significantly nonadiabatic, implying that experimentally prepared Mott insulators are not really in the ground state of the atomic system. The nonadiabaticity is even larger in the presence of a secondary quasiperiodic lattice simulating “disorder.” Alternative ramping schemes are suggested that improve the adiabaticity when the disorder is not too large.

  16. Complete Cycle Experiments Using the Adiabatic Gas Law Apparatus

    NASA Astrophysics Data System (ADS)

    Kutzner, Mickey D.; Plantak, Mateja

    2014-10-01

    The ability of our society to make informed energy-usage decisions in the future depends partly on current science and engineering students retaining a deep understanding of the thermodynamics of heat engines. Teacher imaginations and equipment budgets can both be taxed in the effort to engage students in hands-on heat engine activities. The experiments described in this paper, carried out using the Adiabatic Gas Law Apparatus1 (AGLA), quantitatively explore popular complete cycle heat engine processes.

  17. 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.

  18. Numerical Investigation of the effect of adiabatic section location on thermal performance of a heat pipe network with the application in thermal energy storage systems

    NASA Astrophysics Data System (ADS)

    Mahdavi, Mahboobe; Tiari, Saeed; Qiu, Songgang

    2015-11-01

    Latent heat thermal energy storage systems benefits from high energy density and isothermal storing process. However, the low thermal conductivity of the phase change material leads to prolong the melting or solidification time. Using a passive device such as heat pipes is required to enhance the heat transfer and to improve the efficiency of the system. In the present work, the performance of a heat pipe network specifically designed for a thermal energy storage system is studied numerically. The network includes a primary heat pipe, which transfers heat received from solar receiver to the heat engine. The excess heat is simultaneously delivered to charge the phase change material via secondary heat pipes. The primary heat pipe composed of a disk shape evaporator, an adiabatic section and a disk shape condenser. The adiabatic section can be either located at the center or positioned outward to the surrounding of the container. Here, the effect of adiabatic section position on thermal performance of the system is investigated. It was concluded that displacing the adiabatic section outwards dramatically increases the average temperatures of the condensers and reduces the thermal resistance of heat pipes.

  19. Non-adiabatic molecular dynamics by accelerated semiclassical Monte Carlo

    DOE PAGESBeta

    White, Alexander J.; Gorshkov, Vyacheslav N.; Tretiak, Sergei; Mozyrsky, Dmitry

    2015-07-07

    Non-adiabatic dynamics, where systems non-radiatively transition between electronic states, plays a crucial role in many photo-physical processes, such as fluorescence, phosphorescence, and photoisomerization. Methods for the simulation of non-adiabatic dynamics are typically either numerically impractical, highly complex, or based on approximations which can result in failure for even simple systems. Recently, the Semiclassical Monte Carlo (SCMC) approach was developed in an attempt to combine the accuracy of rigorous semiclassical methods with the efficiency and simplicity of widely used surface hopping methods. However, while SCMC was found to be more efficient than other semiclassical methods, it is not yet as efficientmore » as is needed to be used for large molecular systems. Here, we have developed two new methods: the accelerated-SCMC and the accelerated-SCMC with re-Gaussianization, which reduce the cost of the SCMC algorithm up to two orders of magnitude for certain systems. In many cases shown here, the new procedures are nearly as efficient as the commonly used surface hopping schemes, with little to no loss of accuracy. This implies that these modified SCMC algorithms will be of practical numerical solutions for simulating non-adiabatic dynamics in realistic molecular systems.« less

  20. Adiabatic shear mechanisms for the hard cutting process

    NASA Astrophysics Data System (ADS)

    Yue, Caixu; Wang, Bo; Liu, Xianli; Feng, Huize; Cai, Chunbin

    2015-05-01

    The most important consequence of adiabatic shear phenomenon is formation of sawtooth chip. Lots of scholars focused on the formation mechanism of sawtooth, and the research often depended on experimental approach. For the present, the mechanism of sawtooth chip formation still remains some ambiguous aspects. This study develops a combined numerical and experimental approach to get deeper understanding of sawtooth chip formation mechanism for Polycrystalline Cubic Boron Nitride (PCBN) tools orthogonal cutting hard steel GCr15. By adopting the Johnson-Cook material constitutive equations, the FEM simulation model established in this research effectively overcomes serious element distortions and cell singularity in high strain domain caused by large material deformation, and the adiabatic shear phenomenon is simulated successfully. Both the formation mechanism and process of sawtooth are simulated. Also, the change features regarding the cutting force as well as its effects on temperature are studied. More specifically, the contact of sawtooth formation frequency with cutting force fluctuation frequency is established. The cutting force and effect of cutting temperature on mechanism of adiabatic shear are investigated. Furthermore, the effects of the cutting condition on sawtooth chip formation are researched. The researching results show that cutting feed has the most important effect on sawtooth chip formation compared with cutting depth and speed. This research contributes a better understanding of mechanism, feature of chip formation in hard turning process, and supplies theoretical basis for the optimization of hard cutting process parameters.

  1. Dynamics of Quantum Adiabatic Evolution Algorithm for Number Partitioning

    NASA Technical Reports Server (NTRS)

    Smelyanskiy, V. N.; Toussaint, U. V.; Timucin, D. A.

    2002-01-01

    We have developed a general technique to study the dynamics of the quantum adiabatic evolution algorithm applied to random combinatorial optimization problems in the asymptotic limit of large problem size n. We use as an example the NP-complete Number Partitioning problem and map the algorithm dynamics to that of an auxiliary quantum spin glass system with the slowly varying Hamiltonian. We use a Green function method to obtain the adiabatic eigenstates and the minimum excitation gap. g min, = O(n 2(exp -n/2), corresponding to the exponential complexity of the algorithm for Number Partitioning. The key element of the analysis is the conditional energy distribution computed for the set of all spin configurations generated from a given (ancestor) configuration by simultaneous flipping of a fixed number of spins. For the problem in question this distribution is shown to depend on the ancestor spin configuration only via a certain parameter related to 'the energy of the configuration. As the result, the algorithm dynamics can be described in terms of one-dimensional quantum diffusion in the energy space. This effect provides a general limitation of a quantum adiabatic computation in random optimization problems. Analytical results are in agreement with the numerical simulation of the algorithm.

  2. Non-adiabatic molecular dynamics by accelerated semiclassical Monte Carlo

    SciTech Connect

    White, Alexander J.; Gorshkov, Vyacheslav N.; Tretiak, Sergei; Mozyrsky, Dmitry

    2015-07-07

    Non-adiabatic dynamics, where systems non-radiatively transition between electronic states, plays a crucial role in many photo-physical processes, such as fluorescence, phosphorescence, and photoisomerization. Methods for the simulation of non-adiabatic dynamics are typically either numerically impractical, highly complex, or based on approximations which can result in failure for even simple systems. Recently, the Semiclassical Monte Carlo (SCMC) approach was developed in an attempt to combine the accuracy of rigorous semiclassical methods with the efficiency and simplicity of widely used surface hopping methods. However, while SCMC was found to be more efficient than other semiclassical methods, it is not yet as efficient as is needed to be used for large molecular systems. Here, we have developed two new methods: the accelerated-SCMC and the accelerated-SCMC with re-Gaussianization, which reduce the cost of the SCMC algorithm up to two orders of magnitude for certain systems. In many cases shown here, the new procedures are nearly as efficient as the commonly used surface hopping schemes, with little to no loss of accuracy. This implies that these modified SCMC algorithms will be of practical numerical solutions for simulating non-adiabatic dynamics in realistic molecular systems.

  3. Irreconcilable difference between quantum walks and adiabatic quantum computing

    NASA Astrophysics Data System (ADS)

    Wong, Thomas G.; Meyer, David A.

    2016-06-01

    Continuous-time quantum walks and adiabatic quantum evolution are two general techniques for quantum computing, both of which are described by Hamiltonians that govern their evolutions by Schrödinger's equation. In the former, the Hamiltonian is fixed, while in the latter, the Hamiltonian varies with time. As a result, their formulations of Grover's algorithm evolve differently through Hilbert space. We show that this difference is fundamental; they cannot be made to evolve along each other's path without introducing structure more powerful than the standard oracle for unstructured search. For an adiabatic quantum evolution to evolve like the quantum walk search algorithm, it must interpolate between three fixed Hamiltonians, one of which is complex and introduces structure that is stronger than the oracle for unstructured search. Conversely, for a quantum walk to evolve along the path of the adiabatic search algorithm, it must be a chiral quantum walk on a weighted, directed star graph with structure that is also stronger than the oracle for unstructured search. Thus, the two techniques, although similar in being described by Hamiltonians that govern their evolution, compute by fundamentally irreconcilable means.

  4. Conditions for super-adiabatic droplet growth after entrainment mixing

    NASA Astrophysics Data System (ADS)

    Yang, Fan; Shaw, Raymond; Xue, Huiwen

    2016-07-01

    Cloud droplet response to entrainment and mixing between a cloud and its environment is considered, accounting for subsequent droplet growth during adiabatic ascent following a mixing event. The vertical profile for liquid water mixing ratio after a mixing event is derived analytically, allowing the reduction to be predicted from the mixing fraction and from the temperature and humidity for both the cloud and environment. It is derived for the limit of homogeneous mixing. The expression leads to a critical height above the mixing level: at the critical height the cloud droplet radius is the same for both mixed and unmixed parcels, and the critical height is independent of the updraft velocity and mixing fraction. Cloud droplets in a mixed parcel are larger than in an unmixed parcel above the critical height, which we refer to as the "super-adiabatic" growth region. Analytical results are confirmed with a bin microphysics cloud model. Using the model, we explore the effects of updraft velocity, aerosol source in the environmental air, and polydisperse cloud droplets. Results show that the mixed parcel is more likely to reach the super-adiabatic growth region when the environmental air is humid and clean. It is also confirmed that the analytical predictions are matched by the volume-mean cloud droplet radius for polydisperse size distributions. The findings have implications for the origin of large cloud droplets that may contribute to onset of collision-coalescence in warm clouds.

  5. Non-adiabatic molecular dynamics by accelerated semiclassical Monte Carlo

    SciTech Connect

    White, Alexander J.; Gorshkov, Vyacheslav N.; Tretiak, Sergei; Mozyrsky, Dmitry

    2015-07-07

    Non-adiabatic dynamics, where systems non-radiatively transition between electronic states, plays a crucial role in many photo-physical processes, such as fluorescence, phosphorescence, and photoisomerization. Methods for the simulation of non-adiabatic dynamics are typically either numerically impractical, highly complex, or based on approximations which can result in failure for even simple systems. Recently, the Semiclassical Monte Carlo (SCMC) approach was developed in an attempt to combine the accuracy of rigorous semiclassical methods with the efficiency and simplicity of widely used surface hopping methods. However, while SCMC was found to be more efficient than other semiclassical methods, it is not yet as efficient as is needed to be used for large molecular systems. Here, we have developed two new methods: the accelerated-SCMC and the accelerated-SCMC with re-Gaussianization, which reduce the cost of the SCMC algorithm up to two orders of magnitude for certain systems. In most cases shown here, the new procedures are nearly as efficient as the commonly used surface hopping schemes, with little to no loss of accuracy. This implies that these modified SCMC algorithms will be of practical numerical solutions for simulating non-adiabatic dynamics in realistic molecular systems.

  6. Dynamics of Quantum Adiabatic Evolution Algorithm for Number Partitioning

    NASA Technical Reports Server (NTRS)

    Smelyanskiy, Vadius; vonToussaint, Udo V.; Timucin, Dogan A.; Clancy, Daniel (Technical Monitor)

    2002-01-01

    We have developed a general technique to study the dynamics of the quantum adiabatic evolution algorithm applied to random combinatorial optimization problems in the asymptotic limit of large problem size n. We use as an example the NP-complete Number Partitioning problem and map the algorithm dynamics to that of an auxiliary quantum spin glass system with the slowly varying Hamiltonian. We use a Green function method to obtain the adiabatic eigenstates and the minimum exitation gap, gmin = O(n2(sup -n/2)), corresponding to the exponential complexity of the algorithm for Number Partitioning. The key element of the analysis is the conditional energy distribution computed for the set of all spin configurations generated from a given (ancestor) configuration by simultaneous flipping of a fixed number of spins. For the problem in question this distribution is shown to depend on the ancestor spin configuration only via a certain parameter related to the energy of the configuration. As the result, the algorithm dynamics can be described in terms of one-dimensional quantum diffusion in the energy space. This effect provides a general limitation of a quantum adiabatic computation in random optimization problems. Analytical results are in agreement with the numerical simulation of the algorithm.

  7. NMR implementation of adiabatic SAT algorithm using strongly modulated pulses.

    PubMed

    Mitra, Avik; Mahesh, T S; Kumar, Anil

    2008-03-28

    NMR implementation of adiabatic algorithms face severe problems in homonuclear spin systems since the qubit selective pulses are long and during this period, evolution under the Hamiltonian and decoherence cause errors. The decoherence destroys the answer as it causes the final state to evolve to mixed state and in homonuclear systems, evolution under the internal Hamiltonian causes phase errors preventing the initial state to converge to the solution state. The resolution of these issues is necessary before one can proceed to implement an adiabatic algorithm in a large system where homonuclear coupled spins will become a necessity. In the present work, we demonstrate that by using "strongly modulated pulses" (SMPs) for the creation of interpolating Hamiltonian, one can circumvent both the problems and successfully implement the adiabatic SAT algorithm in a homonuclear three qubit system. This work also demonstrates that the SMPs tremendously reduce the time taken for the implementation of the algorithm, can overcome problems associated with decoherence, and will be the modality in future implementation of quantum information processing by NMR. PMID:18376911

  8. NMR implementation of adiabatic SAT algorithm using strongly modulated pulses

    NASA Astrophysics Data System (ADS)

    Mitra, Avik; Mahesh, T. S.; Kumar, Anil

    2008-03-01

    NMR implementation of adiabatic algorithms face severe problems in homonuclear spin systems since the qubit selective pulses are long and during this period, evolution under the Hamiltonian and decoherence cause errors. The decoherence destroys the answer as it causes the final state to evolve to mixed state and in homonuclear systems, evolution under the internal Hamiltonian causes phase errors preventing the initial state to converge to the solution state. The resolution of these issues is necessary before one can proceed to implement an adiabatic algorithm in a large system where homonuclear coupled spins will become a necessity. In the present work, we demonstrate that by using "strongly modulated pulses" (SMPs) for the creation of interpolating Hamiltonian, one can circumvent both the problems and successfully implement the adiabatic SAT algorithm in a homonuclear three qubit system. This work also demonstrates that the SMPs tremendously reduce the time taken for the implementation of the algorithm, can overcome problems associated with decoherence, and will be the modality in future implementation of quantum information processing by NMR.

  9. Adiabatic corrections to density functional theory energies and wave functions.

    PubMed

    Mohallem, José R; Coura, Thiago de O; Diniz, Leonardo G; de Castro, Gustavo; Assafrão, Denise; Heine, Thomas

    2008-09-25

    The adiabatic finite-nuclear-mass-correction (FNMC) to the electronic energies and wave functions of atoms and molecules is formulated for density-functional theory and implemented in the deMon code. The approach is tested for a series of local and gradient corrected density functionals, using MP2 results and diagonal-Born-Oppenheimer corrections from the literature for comparison. In the evaluation of absolute energy corrections of nonorganic molecules the LDA PZ81 functional works surprisingly better than the others. For organic molecules the GGA BLYP functional has the best performance. FNMC with GGA functionals, mainly BLYP, show a good performance in the evaluation of relative corrections, except for nonorganic molecules containing H atoms. The PW86 functional stands out with the best evaluation of the barrier of linearity of H2O and the isotopic dipole moment of HDO. In general, DFT functionals display an accuracy superior than the common belief and because the corrections are based on a change of the electronic kinetic energy they are here ranked in a new appropriate way. The approach is applied to obtain the adiabatic correction for full atomization of alcanes C(n)H(2n+2), n = 4-10. The barrier of 1 mHartree is approached for adiabatic corrections, justifying its insertion into DFT. PMID:18537228

  10. Does fluorine participate in halogen bonding?

    PubMed

    Eskandari, Kiamars; Lesani, Mina

    2015-03-16

    When R is sufficiently electron withdrawing, the fluorine in the R-F molecules could interact with electron donors (e.g., ammonia) and form a noncovalent bond (F⋅⋅⋅N). Although these interactions are usually categorized as halogen bonding, our studies show that there are fundamental differences between these interactions and halogen bonds. Although the anisotropic distribution of electronic charge around a halogen is responsible for halogen bond formations, the electronic charge around the fluorine in these molecules is spherical. According to source function analysis, F is the sink of electron density at the F⋅⋅⋅N BCP, whereas other halogens are the source. In contrast to halogen bonds, the F⋅⋅⋅N interactions cannot be regarded as lump-hole interactions; there is no hole in the valence shell charge concentration (VSCC) of fluorine. Although the quadruple moment of Cl and Br is mainly responsible for the existence of σ-holes, it is negligibly small in the fluorine. Here, the atomic dipole moment of F plays a stabilizing role in the formation of F⋅⋅⋅N bonds. Interacting quantum atoms (IQA) analysis indicates that the interaction between halogen and nitrogen in the halogen bonds is attractive, whereas it is repulsive in the F⋅⋅⋅N interactions. Virial-based atomic energies show that the fluorine, in contrast to Cl and Br, stabilize upon complex formation. According to these differences, it seems that the F⋅⋅⋅N interactions should be referred to as "fluorine bond" instead of halogen bond. PMID:25652256

  11. Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells

    DOE PAGESBeta

    Xin, Xukai; Li, Bo; Jung, Jaehan; Yoon, Young Jun; Biswas, Rana; Lin, Zhiqun

    2014-07-24

    Quantum dot-sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next-generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO2 acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. In order to understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO2 substrate are simulated using a rigorous ab initio density functional method. Our method capitalizes on localized orbitalmore » basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO2 occurring via the strong bonding between the conduction bands of QDs and TiO2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO2 systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO2 acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size.« less

  12. Halogen bonding origin properties and applications

    SciTech Connect

    Hobza, Pavel

    2015-12-31

    σ-hole bonding represents an unusual and novel type of noncovalent interactions in which atom with σ- hole interacts with Lewis base such as an electronegative atom (oxygen, nitrogen, …) or aromatic systems. This bonding is of electrostatic nature since the σ-hole bears a positive charge. Dispersion energy forms equally important energy term what is due to the fact that two heavy atoms (e.g. halogen and oxygen) having high polarizability lie close together (the respective distance is typically shorter than the sum of van der Waals radii). Among different types of σ-hole bondings the halogen bonding is by far the most known but chalcogen and pnictogen bondings are important as well.

  13. Non-adiabatic effects in thermochemistry, spectroscopy and kinetics: the general importance of all three Born-Oppenheimer breakdown corrections.

    PubMed

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

    2015-10-14

    Using a simple model Hamiltonian, the three correction terms for Born-Oppenheimer (BO) breakdown, the adiabatic diagonal correction (DC), the first-derivative momentum non-adiabatic correction (FD), and the second-derivative kinetic-energy non-adiabatic correction (SD), are shown to all contribute to thermodynamic and spectroscopic properties as well as to thermal non-diabatic chemical reaction rates. While DC often accounts for >80% of thermodynamic and spectroscopic property changes, the commonly used practice of including only the FD correction in kinetics calculations is rarely found to be adequate. For electron-transfer reactions not in the inverted region, the common physical picture that diabatic processes occur because of surface hopping at the transition state is proven inadequate as the DC acts first to block access, increasing the transition state energy by (ℏω)(2)λ/16J(2) (where λ is the reorganization energy, J the electronic coupling and ω the vibration frequency). However, the rate constant in the weakly-coupled Golden-Rule limit is identified as being only inversely proportional to this change rather than exponentially damped, owing to the effects of tunneling and surface hopping. Such weakly-coupled long-range electron-transfer processes should therefore not be described as "non-adiabatic" processes as they are easily described by Born-Huang ground-state adiabatic surfaces made by adding the DC to the BO surfaces; instead, they should be called just "non-Born-Oppenheimer" processes. The model system studied consists of two diabatic harmonic potential-energy surfaces coupled linearly through a single vibration, the "two-site Holstein model". Analytical expressions are derived for the BO breakdown terms, and the model is solved over a large parameter space focusing on both the lowest-energy spectroscopic transitions and the quantum dynamics of coherent-state wavepackets. BO breakdown is investigated pertinent to: ammonia inversion, aromaticity

  14. Towards an understanding of the bonding in polyoxometalates through bond order and bond energy analysis.

    PubMed

    Bridgeman, Adam J; Cavigliasso, Germán

    2003-01-01

    The molecular and electronic structures of transition metal complexes, [MOCl5]n- (n = 2 for M = V,Nb,Ta and n = 1 for Mo,W) and mixed-metal polyoxometalates, [M'M5O19]3-V,Nb,Ta, M = Mo,W) containing a single terminal oxo group on each metal, and of complexes of the uranyl ion [UO2]2+, [UO2(H2O)5]2+ and [UO2Cl4]2-, have been calculated using density functional methods. The calculated structures of the complexes are in good agreement with available experimental parameters. For the mixed-metal hexametalates, for which no crystallographic data is available, the calculations predict a small tetragonal compression of the clusters with only minor structural changes compared to the parent molybdate and tungstate. The metal oxygen bonding in these anions has been probed using Mayer-Mulliken, bond energy and atoms in molecule analyses (AIM). These methods provide a consistent description of the bonding in polyoxometalates. The terminal bonds between transition metal or uranium and oxygen atoms have large sigma and pi components with the pi contributions exceeding the sigma bonding. The transition metals utilize their d orbitals almost exclusively to bond to oxygen whilst uranium uses both its 5f and 6d orbitals. Oxygen atom charges increase and covalency indexes decrease with coordination number, with a marked separation of these terms according to the oxygen atom type. The total valency and AIM energies of the oxygen atoms are predicted to be almost constant for all types of oxygen site. The constancy of the bonding power of the oxygen atoms appears to be an important factor in determining the gross structures and details of the bonding in polyoxometalates. The Mayer Mulliken approach provides direct characterization of the bonding power of atoms and the extent of the interaction between pairs of atoms that is consistent with the results of the considerably more computationally demanding bond energy and AIM approaches. PMID:14527219

  15. Charge distribution and transport properties in reduced ceria phases: A review

    NASA Astrophysics Data System (ADS)

    Shoko, E.; Smith, M. F.; McKenzie, Ross H.

    2011-12-01

    The question of the charge distribution in reduced ceria phases (CeO2-x) is important for understanding the microscopic physics of oxygen storage capacity, and the electronic and ionic conductivities in these materials. All these are key properties in the application of these materials in catalysis and electrochemical devices. Several approaches have been applied to study this problem, including ab initio methods. Recently [1], we applied the bond valence model (BVM) to discuss the charge distribution in several different crystallographic phases of reduced ceria. Here, we compare the BVM results to those from atomistic simulations to determine if there is consistency in the predictions of the two approaches. Our analysis shows that the two methods give a consistent picture of the charge distribution around oxygen vacancies in bulk reduced ceria phases. We then review the transport theory applicable to reduced ceria phases, providing useful relationships which enable comparison of experimental results obtained by different techniques. In particular, we compare transport parameters obtained from the observed optical absorption spectrum, α(ω), dc electrical conductivity with those predicted by small polaron theory and the Harrison method. The small polaron energy is comparable to that estimated from α(ω). However, we found a discrepancy between the value of the electron hopping matrix element, t, estimated from the Marcus-Hush formula and that obtained by the Harrison method. Part of this discrepancy could be attributed to the system lying in the crossover region between adiabatic and nonadiabatic whereas our calculations assumed the system to be nonadiabatic. Finally, by considering the relationship between the charge distribution and electronic conductivity, we suggest the possibility of low temperature metallic conductivity for intermediate phases, i.e., x˜0.3. This has not yet been experimentally observed.

  16. Bond Energies in Models of the Schrock Metathesis Catalyst

    SciTech Connect

    Vasiliu, Monica; Li, Shenggang; Arduengo, Anthony J.; Dixon, David A.

    2011-06-23

    Heats of formation, adiabatic and diabatic bond dissociation energies (BDEs) of the model Schrock-type metal complexes M(NH)(CRR)(OH)₂ (M = Cr, Mo, W; CRR = CH₂, CHF, CF₂) and MO₂(OH)₂ compounds, and Brønsted acidities and fluoride affinities for the M(NH)(CH₂)(OH) ₂ transition metal complexes are predicted using high level CCSD(T) calculations. The metallacycle intermediates formed by reaction of C₂H4 with M(NH)-(CH₂)(OH)2 and MO₂(OH)₂ are investigated at the same level of theory. Additional corrections were added to the complete basis set limit to obtain near chemical accuracy ((1 kcal/mol). A comparison between adiabatic and diabatic BDEs is made and provides an explanation of trends in the BDEs. Electronegative groups bonded on the carbenic carbon lead to less stable Schrock-type complexes as the adiabatic BDEs ofMdCF₂ andMdCHF bonds are much lower than theMdCH₂ bonds. The Cr compounds have smaller BDEs than theWorMo complexes and should be less stable. Different M(NH)(OH)₂(C₃H₆) and MO(OH)₂(OC₂H4) metallacycle intermediates are investigated, and the lowest-energy metallacycles have a square pyramidal geometry. The results show that consideration of the singlet_triplet splitting in the carbene in the initial catalyst as well as in the metal product formed by the retro [2+2] cycloaddition is a critical component in the design of an effective olefin metathesis catalyst in terms of the parent catalyst and the groups being transferred.

  17. Coherent adiabatic spin control in the presence of charge noise using tailored pulses.

    PubMed

    Ribeiro, Hugo; Burkard, Guido; Petta, J R; Lu, H; Gossard, A C

    2013-02-22

    We study finite-time Landau-Zener transitions at a singlet-triplet level crossing in a GaAs double quantum dot, both experimentally and theoretically. Sweeps across the anticrossing in the high driving speed limit result in oscillations with a small visibility. Here we demonstrate how to increase the oscillation visibility while keeping sweep times shorter than T(2)(*) using a tailored pulse with a detuning dependent level velocity. Our results show an improvement of a factor of ~2.9 for the oscillation visibility. In particular, we were able to obtain a visibility of ~0.5 for Stückelberg oscillations, which demonstrates the creation of an equally weighted superposition of the qubit states. PMID:23473186

  18. Using Multiple Bonding Strategies.

    PubMed

    Larson, Thomas D

    2015-01-01

    There are many ways to bond to tooth structure, some micro-mechanical some chemical, some a combination. Different dentin bonding materials have different bonding strengths to differently prepared surfaces, and because of differences in their nature, different areas of tooth structure present peculiar bonding challenges. This paper will review a variety of material types, elucidating their particular bonding strengths and commenting on improved bonding strategies to increase durability, strength, and favorable pulpal response. In this discussion, resin dentin bonding systems, glass ionomers, Gluma, resin cements, and newer combined products will br reviewed. PMID:26485903

  19. Inducing changes in the bond length of diatomic molecules by time-symmetric chirped pulses

    SciTech Connect

    Chang, Bo Y.; Shin, Seokmin; Sola, Ignacio R.

    2010-12-15

    We show numerically that it is possible to change the structure of a simple molecule, that is, a diatomic molecule, where the bond length is modified at a precise timing with symmetrically chirped laser pulses. In the adiabatic regime, the process is fully time reversible, making it possible to design slow vibrations with large bond elongations. The scheme relies on the preparation of a separable state of both nuclear and electronic degrees of freedom with predominant amplitude on the dissociative (antibonding) electronic wave function. Shorter laser pulses can be used to dynamically induce larger bond elongations, preparing a highly excited vibrational wave packet in the ground potential as the laser is switched off.

  20. 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

    The asymptotic response of donor stars in interacting binary systems to very rapid mass loss is characterized by adiabatic expansion throughout their interiors. In this limit, energy generation and heat flow through the stellar interior can be neglected. We model this response by constructing model sequences, beginning with a donor star filling its Roche lobe at an arbitrary point in its evolution, holding its specific entropy and composition profiles fixed as mass is removed from the surface. The stellar interior remains in hydrostatic equilibrium. Luminosity profiles in these adiabatic models of mass-losing stars can be reconstructed from the specific entropy profiles and their gradients. These approximations are validated by comparison with time-dependent binary mass transfer calculations. We describe how adiabatic mass-loss sequences can be used to quantify threshold conditions for dynamical timescale mass transfer, and to establish the range of post-common envelope binaries that are allowed energetically. In dynamical timescale mass transfer, the adiabatic response of the donor star drives it to expand beyond its Roche lobe, leading to runaway mass transfer and the formation of a common envelope with its companion star. For donor stars with surface convection zones of any significant depth, this runaway condition is encountered early in mass transfer, if at all; but for main-sequence stars with radiative envelopes, it may be encountered after a prolonged phase of thermal timescale mass transfer, a so-called delayed dynamical instability. We identify the critical binary mass ratio for the onset of dynamical timescale mass transfer as that ratio for which the adiabatic response of the donor star radius to mass loss matches that of its Roche lobe at some point during mass transfer; if the ratio of donor to accretor masses exceeds this critical value, dynamical timescale mass transfer ensues. In common envelope evolution, the dissipation of orbital energy of the

  1. CHARGE IMBALANCE

    SciTech Connect

    Clarke, John

    1980-09-01

    The purpose of this article is to review the theory of charge imbalance, and to discuss its relevance to a number of experimental situations. We introduce the concepts of quasiparticle charge and charge imbalance, and discuss the generation and detection of charge imbalance by tunneling. We describe the relaxation of the injected charge imbalance by inelastic scattering processes, and show how the Boltzmann equation can be solved to obtain the steady state quasiparticle distribution and the charge relaxation rate. Details are given of experiments to measure charge imbalance and the charge relaxation rate when inelastic scattering is the predominant relaxation mechanism. Experiments on and theories of other charge relaxation mechanisms are discussed, namely relaxation via elastic scattering in the presence of energy gap anisotropy, or in the presence of a pair breaking mechanism such as magnetic impurities or an applied supercurrent or magnetic field. We describe three other situations in which charge imbalance occurs, namely the resistance of the NS interface, phase slip centers, and the flow of a supercurrent in the presence of a temperature gradient.

  2. Influence of viscosity and the adiabatic index on planetary migration

    NASA Astrophysics Data System (ADS)

    Bitsch, B.; Boley, A.; Kley, W.

    2013-02-01

    Context. The strength and direction of migration of low mass embedded planets depends on the disk's thermodynamic state. It has been shown that in active disks, where the internal dissipation is balanced by radiative transport, migration can be directed outwards, a process which extends the lifetime of growing embryos. Very important parameters determining the structure of disks, and hence the direction of migration, are the viscosity and the adiabatic index. Aims: In this paper we investigate the influence of different viscosity prescriptions (α-type and constant) and adiabatic indices on disk structures. We then determine how this affects the migration rate of planets embedded in such disks. Methods: We perform three-dimensional numerical simulations of accretion disks with embedded planets. We use the explicit/implicit hydrodynamical code NIRVANA that includes full tensor viscosity and radiation transport in the flux-limited diffusion approximation, as well as a proper equation of state for molecular hydrogen. The migration of embedded 20 MEarth planets is studied. Results: Low-viscosity disks have cooler temperatures and the migration rates of embedded planets tend toward the isothermal limit. Hence, in these disks, planets migrate inwards even in the fully radiative case. The effect of outward migration can only be sustained if the viscosity in the disk is large. Overall, the differences between the treatments for the equation of state seem to play a more important role in disks with higher viscosity. A change in the adiabatic index and in the viscosity changes the zero-torque radius that separates inward from outward migration. Conclusions: For larger viscosities, temperatures in the disk become higher and the zero-torque radius moves to larger radii, allowing outward migration of a 20-MEarth planet to persist over an extended radial range. In combination with large disk masses, this may allow for an extended period of the outward migration of growing

  3. Kibble-Zurek mechanism beyond adiabaticity: Finite-time scaling with critical initial slip

    NASA Astrophysics Data System (ADS)

    Huang, Yingyi; Yin, Shuai; Hu, Qijun; Zhong, Fan

    2016-01-01

    The Kibble-Zurek mechanism demands an initial adiabatic stage before an impulse stage to have a frozen correlation length that generates topological defects in a cooling phase transition. Here we study such a driven critical dynamics but with an initial condition that is near the critical point and that is far away from equilibrium. In this case, there is no initial adiabatic stage at all and thus adiabaticity is broken. However, we show that there again exists a finite length scale arising from the driving that divides the evolution into three stages. A relaxation-finite-time-scaling-adiabatic scenario is then proposed in place of the adiabatic-impulse-adiabatic scenario of the original Kibble-Zurek mechanism. A unified scaling theory, which combines finite-time scaling with critical initial slip, is developed to describe the universal behavior and is confirmed with numerical simulations of a two-dimensional classical Ising model.

  4. Optimized sympathetic cooling of atomic mixtures via fast adiabatic strategies

    SciTech Connect

    Choi, Stephen; Sundaram, Bala; Onofrio, Roberto

    2011-11-15

    We discuss fast frictionless cooling techniques in the framework of sympathetic cooling of cold atomic mixtures. It is argued that optimal cooling of an atomic species--in which the deepest quantum degeneracy regime is achieved--may be obtained by means of sympathetic cooling with another species whose trapping frequency is dynamically changed to maintain constancy of the Lewis-Riesenfeld adiabatic invariant. Advantages and limitations of this cooling strategy are discussed, with particular regard to the possibility of cooling Fermi gases to a deeper degenerate regime.

  5. Magnetic shielding for a spaceborne adiabatic demagnetization refrigerator (ADR)

    NASA Technical Reports Server (NTRS)

    Warner, Brent A.; Shirron, Peter J.; Castles, Stephen H.; Serlemitsos, Aristides T.

    1991-01-01

    The Goddard Space Flight Center has studied magnetic shielding for an adiabatic demagnetization refrigerator. Four types of shielding were studied: active coils, passive ferromagnetic shells, passive superconducting coils, and passive superconducting shells. The passive superconducting shells failed by allowing flux penetration. The other three methods were successful, singly or together. Experimental studies of passive ferromagnetic shielding are compared with calculations made using the Poisson Group of programs, distributed by the Los Alamos Accelerator Code Group of the Los Alamos National Laboratory. Agreement between calculation and experiment is good. The ferromagnetic material is a silicon iron alloy.

  6. Modeling of the Adiabatic and Isothermal Methanation Process

    NASA Astrophysics Data System (ADS)

    Porubova, Jekaterina; Bazbauers, Gatis; Markova, Darja

    2011-01-01

    Increased use of biomass offers one of the ways to reduce anthropogenic impact on the environment. Using various biomass conversion processes, it is possible to obtain different types of fuels: • solid, e.g. bio-carbon; • liquid, e.g. biodiesel and ethanol; • gaseous, e.g. biomethane. Biomethane can be used in the transport and energy sector, and the total methane production efficiency can reach 65%. By modeling adiabatic and isothermal methanation processes, the most effective one from the methane production point of view is defined. Influence of the process parameters on the overall efficiency of the methane production is determined.

  7. Relativistic blast waves in two dimensions. I - The adiabatic case

    NASA Technical Reports Server (NTRS)

    Shapiro, P. R.

    1979-01-01

    Approximate solutions are presented for the dynamical evolution of strong adiabatic relativistic blast waves which result from a point explosion in an ambient gas in which the density varies both with distance from the explosion center and with polar angle in axisymmetry. Solutions are analytical or quasi-analytical for the extreme relativistic case and numerical for the arbitrarily relativistic case. Some general properties of nonplanar relativistic shocks are also discussed, including the incoherence of spherical ultrarelativistic blast-wave fronts on angular scales greater than the reciprocal of the shock Lorentz factor, as well as the conditions for producing blast-wave acceleration.

  8. Stimulated Raman adiabatic passage in Tm{sup 3+}:YAG

    SciTech Connect

    Alexander, A. L.; Lauro, R.; Louchet, A.; Chaneliere, T.; Le Goueet, J. L.

    2008-10-01

    We report on the experimental demonstration of stimulated Raman adiabatic passage in a Tm{sup 3+}:YAG crystal. Tm{sup 3+}:YAG is a promising material for use in quantum information processing applications, but as yet there are few experimental investigations of coherent Raman processes in this material. We investigate the effect of inhomogeneous broadening and Rabi frequency on the transfer efficiency and the width of the two-photon spectrum. Simulations of the complete Tm{sup 3+}:YAG system are presented along with the corresponding experimental results.

  9. Nonlinear effects generation in non-adiabatically tapered fibres

    NASA Astrophysics Data System (ADS)

    Palací, Jesús; Mas, Sara; Monzón-Hernández, David; Martí, Javier

    2015-12-01

    Nonlinear effects are observed in a non-adiabatically tapered optical fibre. The designed structure allows for the introduction of self-phase modulation, which is observed through pulse breaking and spectral broadening, in approximately a centimetre of propagation using a commercial telecom laser. These devices are simple to fabricate and suitable to generate and control a variety of nonlinear effects in practical applications because they do not experience short-term degradation as previously reported approaches. Experimental and theoretical results are obtained, showing a good agreement.

  10. Plasma heating via adiabatic magnetic compression-expansion cycle

    NASA Astrophysics Data System (ADS)

    Avinash, K.; Sengupta, M.; Ganesh, R.

    2016-06-01

    Heating of collisionless plasmas in closed adiabatic magnetic cycle comprising of a quasi static compression followed by a non quasi static constrained expansion against a constant external pressure is proposed. Thermodynamic constraints are derived to show that the plasma always gains heat in cycles having at least one non quasi static process. The turbulent relaxation of the plasma to the equilibrium state at the end of the non quasi static expansion is discussed and verified via 1D Particle in Cell (PIC) simulations. Applications of this scheme to heating plasmas in open configurations (mirror machines) and closed configurations (tokamak, reverse field pinche) are discussed.

  11. Ultrasonic velocity and adiabatic compressibility in dioxane-water mixtures

    NASA Technical Reports Server (NTRS)

    Ciupe, A.; Auslaender, D.

    1974-01-01

    Using a method of diffraction of light on an ultrasonic beam, the velocity of ultrasounds and the adiabatic compressibility in dioxane-water mixtures were determined. The dependence of these quantities on the temperature (in the 15-50 C range) and on the concentration (0-100%) were studied. For each temperature there was found a velocity maximum and a compressibility minimum for a given value of the dioxane concentration. The different behavior of these mixtures is due to intense interactions between the molecules of the two liquids composing the mixture.

  12. Quantum corrections during inflation and conservation of adiabatic perturbations

    SciTech Connect

    Campo, David

    2010-02-15

    The possibility that quantum corrections break the conservation of superhorizon adiabatic perturbations in single field inflation is examined. I consider the lowest order corrections from massless matter fields in the Hamiltonian formalism. Particular emphasis is therefore laid on the renormalization. The counterterms are the same as in the Lagrangian formalism. The renormalized value of the tadpole is zero. I find a possible secular dependence of the power spectrum at one loop due to the trace anomaly, but this result depends on the approximation of the modes and is inconclusive. The symmetry (not) violated by the quantum corrections is the invariance by dilatation. Perspectives on the backreaction problem are briefly discussed.

  13. More bang for your buck: Super-adiabatic quantum engines

    PubMed Central

    Campo, A. del; Goold, J.; Paternostro, M.

    2014-01-01

    The practical untenability of the quasi-static assumption makes any realistic engine intrinsically irreversible and its operating time finite, thus implying friction effects at short cycle times. An important technological goal is thus the design of maximally efficient engines working at the maximum possible power. We show that, by utilising shortcuts to adiabaticity in a quantum engine cycle, one can engineer a thermodynamic cycle working at finite power and zero friction. Our findings are illustrated using a harmonic oscillator undergoing a quantum Otto cycle. PMID:25163421

  14. Salt materials testing for a spacecraft adiabatic demagnetization refrigerator

    NASA Technical Reports Server (NTRS)

    Savage, M. L.; Kittel, P.; Roellig, T.

    1990-01-01

    As part of a technology development effort to qualify adiabatic demagnetization refrigerators for use in a NASA spacecraft, such as the Space Infrared Telescope Facility, a study of low temperature characteristics, heat capacity and resistance to dehydration was conducted for different salt materials. This report includes results of testing with cerrous metaphosphate, several synthetic rubies, and chromic potassium alum (CPA). Preliminary results show that CPA may be suitable for long-term spacecraft use, provided that the salt is property encapsulated. Methods of salt pill construction and testing for all materials are discussed, as well as reliability tests. Also, the temperature regulation scheme and the test cryostat design are briefly discussed.

  15. Gravitational radiation reaction and inspiral waveforms in the adiabatic limit.

    PubMed

    Hughes, Scott A; Drasco, Steve; Flanagan, Eanna E; Franklin, Joel

    2005-06-10

    We describe progress evolving an important limit of binaries in general relativity: stellar mass compact objects spiraling into much larger black holes. Such systems are of great observational interest. We have developed tools to compute for the first time the radiation from generic orbits. Using global conservation laws, we find the orbital evolution and waveforms for special cases. For generic orbits, inspirals and waveforms can be found by augmenting our approach with an adiabatic self-force rule due to Mino. Such waveforms should be accurate enough for gravitational-wave searches. PMID:16090377

  16. 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.

  17. More bang for your buck: super-adiabatic quantum engines.

    PubMed

    del Campo, A; Goold, J; Paternostro, M

    2014-01-01

    The practical untenability of the quasi-static assumption makes any realistic engine intrinsically irreversible and its operating time finite, thus implying friction effects at short cycle times. An important technological goal is thus the design of maximally efficient engines working at the maximum possible power. We show that, by utilising shortcuts to adiabaticity in a quantum engine cycle, one can engineer a thermodynamic cycle working at finite power and zero friction. Our findings are illustrated using a harmonic oscillator undergoing a quantum Otto cycle. PMID:25163421

  18. Stimulated Raman adiabatic passage through permanent dipole moment transitions

    SciTech Connect

    Niu Yingyu; Wang Rong; Qiu Minghui

    2010-04-15

    The rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) through permanent dipole moment transitions are investigated theoretically using a time-dependent quantum wave packet method for the ground electronic state of an HF molecule. The two basic STIRAP processes, {Lambda} and ladder systems, are simulated. The calculated results show that nearly 100% of the population can be transferred to the target state. Besides the interested transitions, the pulses can induce other transitions which affect the dynamics of STIRAP. The final populations of the initial and target states depend on delay time.

  19. Local shortcut to adiabaticity for quantum many-body systems

    NASA Astrophysics Data System (ADS)

    Mukherjee, Victor; Montangero, Simone; Fazio, Rosario

    2016-06-01

    We study the environmentally assisted local transitionless dynamics in closed spin systems driven through quantum critical points. In general the shortcut to adaiabaticity (STA) in quantum critical systems requires highly nonlocal control Hamiltonians. In this work we develop an approach to achieve local shortcuts to adiabaticity (LSTA) in spin chains, using local control fields which scale polynomially with the system size, following universal critical exponents. We relate the control fields to reduced fidelity susceptibility and use the transverse Ising model in one dimension to exemplify our generic results. We also extend our analysis to achieve LSTA in central spin models.

  20. Steady-state coherent transfer by adiabatic passage.

    PubMed

    Huneke, Jan; Platero, Gloria; Kohler, Sigmund

    2013-01-18

    We propose steady-state electron transport based on coherent transfer by adiabatic passage (CTAP) in a linearly arranged triple quantum dot with leads attached to the outer dots. Its main feature is repeated steering of single electrons from the first dot to the last dot without relevant occupation of the middle dot. The coupling to leads enables a steady-state current, whose shot noise is significantly suppressed provided that the CTAP protocol performs properly. This represents an indication for the direct transfer between spatially separated dots and, thus, may resolve the problem of finding experimental evidence for the nonoccupation of the middle dot. PMID:23373941

  1. Bifunctional hydrogen bonds in monohydrated cycloether complexes.

    PubMed

    Vallejos, Margarita M; Angelina, Emilio L; Peruchena, Nélida M

    2010-03-01

    In this work, the cooperative effects implicated in bifunctional hydrogen bonds (H-bonds) were studied (in monohydrated six-membered cycloether) within the framework of the atoms in molecules (AIM) theory and of the natural bond orbitals (NBO) analysis. The study was carried out in complexes formed by six-membered cycloether compounds (tetrahydropyrane, 1,4-dioxane, and 1,3-dioxane) and a water molecule. These compounds were used as model systems instead of more complicated molecules of biological importance. All the results were obtained at the second-order Møller-Plesset (MP2) level theory using a 6-311++G(d,p) basis set. Attention was focused on the indicators of the cooperative effects that arise when a water molecule interacts simultaneously with a polar and a nonpolar portion of a six-membered cycloether (via bifunctional hydrogen bonds) and compared with conventional H-bonds where the water molecule only interacts with the polar portion of the cycloether. Different indicators of H-bonds strength, such as structural and spectroscopic data, electron charge density, population analysis, hyperconjugation energy and charge transference, consistently showed significant cooperative effects in bifunctional H-bonds. From the AIM, as well as from the NBO analysis, the obtained results allowed us to state that in the monohydrated six-membered cycloether, where the water molecule plays a dual role, as proton acceptor and proton donor, a mutual reinforcement of the two interactions occurs. Because of this feature, the complexes engaged by bifunctional hydrogen bonds are more stabilized than the complexes linked by conventional hydrogen bonds. PMID:20136161

  2. 29 CFR 2580.412-20 - Use of existing bonds, separate bonds and additional bonding.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 29 Labor 9 2010-07-01 2010-07-01 false Use of existing bonds, separate bonds and additional..., separate bonds and additional bonding. (a) Additional bonding. Section 13 neither prevents additional... or separate bond. (b) Use of existing bonds. Insofar as a bond currently in use is adequate to...

  3. Hydroxide-catalyzed bonding

    NASA Technical Reports Server (NTRS)

    Gwo, Dz-Hung (Inventor)

    2003-01-01

    A method of bonding substrates by hydroxide-catalyzed hydration/dehydration involves applying a bonding material to at least one surface to be bonded, and placing the at least one surface sufficiently close to another surface such that a bonding interface is formed between them. A bonding material of the invention comprises a source of hydroxide ions, and may optionally include a silicate component, a particulate filling material, and a property-modifying component. Bonding methods of the invention reliably and reproducibly provide bonds which are strong and precise, and which may be tailored according to a wide range of possible applications. Possible applications for bonding materials of the invention include: forming composite materials, coating substrates, forming laminate structures, assembly of precision optical components, and preparing objects of defined geometry and composition. Bonding materials and methods of preparing the same are also disclosed.

  4. Between ethylene and polyenes--the non-adiabatic dynamics of cis-dienes.

    PubMed

    Kuhlman, Thomas S; Glover, William J; Mori, Toshifumi; Møller, Klaus B; Martínez, Todd J

    2012-01-01

    Using Ab Initio Multiple Spawning (AIMS) with a Multi-State Multi-Reference Perturbation theory (MS-MR-CASPT2) treatment of the electronic structure, we have simulated the non-adiabatic excited state dynamics of cyclopentadiene (CPD) and 1,2,3,4-tetramethyl-cyclopentadiene (Me4-CPD) following excitation to S1. It is observed that torsion around the carbon-carbon double bonds is essential in reaching a conical intersection seam connecting S1 and S0. We identify two timescales; the induction time from excitation to the onset of population transfer back to S0 (CPD: -25 fs, Me4-CPD: -71 fs) and the half-life of the subsequent population transfer (CPD: -28 fs, Me4-CPD: -48 fs). The longer timescales for Me4-CPD are a kinematic consequence of the inertia of the substituents impeding the essential out-of-plane motion that leads to the conical intersection seam. A bifurcation is observed on S1 leading to population transfer being attributable, in a 5 : 2 ratio for CPD and 7 : 2 ratio for Me4-CPD, to two closely related conical intersections. Calculated time-resolved photoelectron spectra are in excellent agreement with experimental spectra validating the simulation results. PMID:23230770

  5. Shortcut to Adiabatic Passage in Two- and Three-Level Atoms

    SciTech Connect

    Chen Xi; Lizuain, I.; Muga, J. G.; Ruschhaupt, A.; Guery-Odelin, D.

    2010-09-17

    We propose a method to speed up adiabatic passage techniques in two-level and three-level atoms extending to the short-time domain their robustness with respect to parameter variations. It supplements or substitutes the standard laser beam setups with auxiliary pulses that steer the system along the adiabatic path. Compared to other strategies, such as composite pulses or the original adiabatic techniques, it provides a fast and robust approach to population control.

  6. Fractional adiabatic passage in two-level systems: Mirrors and beam splitters for atomic interferometry

    SciTech Connect

    Bateman, James; Freegarde, Tim

    2007-07-15

    Atom interferometers require atom mirrors and beam splitters that can maintain high fidelity even when experimental parameters vary from the ideal. We address the use of chirped laser pulses to provide such elements via rapid adiabatic passage, and present a prescription for practical pulses that offer controlled adiabaticity throughout. Full- and half-adiabatic pulses, providing mirrors and beam splitters, respectively, are derived, and the latter examined for robustness and suitability for experimental implementations.

  7. Tunneling conductance through the half-metal/conical magnet/superconductor junctions in the adiabatic and non-adiabatic regimes: Self-consistent calculations

    NASA Astrophysics Data System (ADS)

    Wójcik, P.; Zegrodnik, M.; Rzeszotarski, B.; Adamowski, J.

    2016-09-01

    The tunneling conductance through the half-metal/conical magnet/superconductor (HM/CM/SC) junctions is investigated with the use of the Bogoliubov-de Gennes equations in the framework of Blonder-Tinkham-Klapwijk formalism. Due to the spin band separation in the HM, the conductance in the subgap region is mainly determined by the anomalous Andreev reflection, the probability of which strongly depends on the spin transmission in the CM layer. We show that the spins of electrons injected from the HM can be transmitted through the CM to the SC either adiabatically or non-adiabatically depending on the period of the spatial modulation of the exchange field. We find that the conductance in the subgap region oscillates as a function of the CM layer thickness wherein the oscillations transform from the irregular pattern in the non-adiabatic regime to the regular one in the adiabatic regime. For both adiabatic and non-adiabatic transport regimes the conductance is studied over a broad range of parameters determining the spiral magnetization in the CM. We find that in the non-adiabatic regime, the decrease of the exchange field amplitude in the CM leads to the emergence of the conductance peak for the particular CM thickness in agreement with recent experiments.

  8. Internal Charging

    NASA Technical Reports Server (NTRS)

    Minow, Joseph I.

    2014-01-01

    (1) High energy (>100keV) electrons penetrate spacecraft walls and accumulate in dielectrics or isolated conductors; (2) Threat environment is energetic electrons with sufficient flux to charge circuit boards, cable insulation, and ungrounded metal faster than charge can dissipate; (3) Accumulating charge density generates electric fields in excess of material breakdown strenght resulting in electrostatic discharge; and (4) System impact is material damage, discharge currents inside of spacecraft Faraday cage on or near critical circuitry, and RF noise.

  9. The Bondons: The Quantum Particles of the Chemical Bond

    PubMed Central

    Putz, Mihai V.

    2010-01-01

    By employing the combined Bohmian quantum formalism with the U(1) and SU(2) gauge transformations of the non-relativistic wave-function and the relativistic spinor, within the Schrödinger and Dirac quantum pictures of electron motions, the existence of the chemical field is revealed along the associate bondon particle B̶ characterized by its mass (mB̶), velocity (vB̶), charge (eB̶), and life-time (tB̶). This is quantized either in ground or excited states of the chemical bond in terms of reduced Planck constant ħ, the bond energy Ebond and length Xbond, respectively. The mass-velocity-charge-time quaternion properties of bondons’ particles were used in discussing various paradigmatic types of chemical bond towards assessing their covalent, multiple bonding, metallic and ionic features. The bondonic picture was completed by discussing the relativistic charge and life-time (the actual zitterbewegung) problem, i.e., showing that the bondon equals the benchmark electronic charge through moving with almost light velocity. It carries negligible, although non-zero, mass in special bonding conditions and towards observable femtosecond life-time as the bonding length increases in the nanosystems and bonding energy decreases according with the bonding length-energy relationship Ebond[kcal/mol]×Xbond[A0]=182019, providing this way the predictive framework in which the B̶ particle may be observed. Finally, its role in establishing the virtual states in Raman scattering was also established. PMID:21151435

  10. Singularity of the time-energy uncertainty in adiabatic perturbation and cycloids on a Bloch sphere.

    PubMed

    Oh, Sangchul; Hu, Xuedong; Nori, Franco; Kais, Sabre

    2016-01-01

    Adiabatic perturbation is shown to be singular from the exact solution of a spin-1/2 particle in a uniformly rotating magnetic field. Due to a non-adiabatic effect, its quantum trajectory on a Bloch sphere is a cycloid traced by a circle rolling along an adiabatic path. As the magnetic field rotates more and more slowly, the time-energy uncertainty, proportional to the length of the quantum trajectory, calculated by the exact solution is entirely different from the one obtained by the adiabatic path traced by the instantaneous eigenstate. However, the non-adiabatic Aharonov-Anandan geometric phase, measured by the area enclosed by the exact path, approaches smoothly the adiabatic Berry phase, proportional to the area enclosed by the adiabatic path. The singular limit of the time-energy uncertainty and the regular limit of the geometric phase are associated with the arc length and arc area of the cycloid on a Bloch sphere, respectively. Prolate and curtate cycloids are also traced by different initial states outside and inside of the rolling circle, respectively. The axis trajectory of the rolling circle, parallel to the adiabatic path, is shown to be an example of transitionless driving. The non-adiabatic resonance is visualized by the number of cycloid arcs. PMID:26916031

  11. Singularity of the time-energy uncertainty in adiabatic perturbation and cycloids on a Bloch sphere

    PubMed Central

    Oh, Sangchul; Hu, Xuedong; Nori, Franco; Kais, Sabre

    2016-01-01

    Adiabatic perturbation is shown to be singular from the exact solution of a spin-1/2 particle in a uniformly rotating magnetic field. Due to a non-adiabatic effect, its quantum trajectory on a Bloch sphere is a cycloid traced by a circle rolling along an adiabatic path. As the magnetic field rotates more and more slowly, the time-energy uncertainty, proportional to the length of the quantum trajectory, calculated by the exact solution is entirely different from the one obtained by the adiabatic path traced by the instantaneous eigenstate. However, the non-adiabatic Aharonov- Anandan geometric phase, measured by the area enclosed by the exact path, approaches smoothly the adiabatic Berry phase, proportional to the area enclosed by the adiabatic path. The singular limit of the time-energy uncertainty and the regular limit of the geometric phase are associated with the arc length and arc area of the cycloid on a Bloch sphere, respectively. Prolate and curtate cycloids are also traced by different initial states outside and inside of the rolling circle, respectively. The axis trajectory of the rolling circle, parallel to the adiabatic path, is shown to be an example of transitionless driving. The non-adiabatic resonance is visualized by the number of cycloid arcs. PMID:26916031

  12. Bond Dissociation Energies in Second-Row Compounds

    SciTech Connect

    Grant, Daniel J.; Matus, Myrna H.; Switzer, Jackson R.; Dixon, David A.; Francisco, Joseph S.; Christe, Karl O.

    2008-04-10

    The research described in this product was performed in part in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. Heats of formation at 0 and 298 K are predicted for PF₃, PF₅, PF₃O, SF₂, SF₄, SF₆, SF₂O, SF₂O₂, and SF₄O as well as a number of radicals derived from these stable compounds on the basis of coupled cluster theory [CCSD(T)] calculations extrapolated to the complete basis set limit. In order to achieve near chemical accuracy (±1 kcal/mol), additional corrections were added to the complete basis set binding energies based on frozen core coupled cluster theory energies: a correction for core-valence effects, a correction for scalar relativistic effects, a correction for first-order atomic spin-orbit effects, and vibrational zero-point energies. The calculated values substantially reduce the error limits for these species. A detailed comparison of adiabatic and diabatic bond dissociation energies (BDEs) is made and used to explain trends in the BDEs. Because the adiabatic BDEs of polyatomic molecules represent not only the energy required for breaking a specific bond but also contain any reorganization energies of the bonds in the resulting products, these BDEs can be quite different for each step in the stepwise loss of ligands in binary compounds. For example, the adiabatic BDE for the removal of one fluorine ligand from the very stable closed-shell SF₆ molecule to give the unstable SF₅ radical is 2.8 times the BDE needed for the removal of one fluorine ligand from the unstable SF₅ radical to give the stable closed-shell SF₄ molecule. Similarly, the BDE for the removal of one fluorine ligand from the stable closed-shell PF₃O molecule to give the unstable PF₂O radical is higher than the BDE needed to remove the oxygen atom to give the stable closed

  13. Schedule path optimization for adiabatic quantum computing and optimization

    NASA Astrophysics Data System (ADS)

    Zeng, Lishan; Zhang, Jun; Sarovar, Mohan

    2016-04-01

    Adiabatic quantum computing and optimization have garnered much attention recently as possible models for achieving a quantum advantage over classical approaches to optimization and other special purpose computations. Both techniques are probabilistic in nature and the minimum gap between the ground state and first excited state of the system during evolution is a major factor in determining the success probability. In this work we investigate a strategy for increasing the minimum gap and success probability by introducing intermediate Hamiltonians that modify the evolution path between initial and final Hamiltonians. We focus on an optimization problem relevant to recent hardware implementations and present numerical evidence for the existence of a purely local intermediate Hamiltonian that achieve the optimum performance in terms of pushing the minimum gap to one of the end points of the evolution. As a part of this study we develop a convex optimization formulation of the search for optimal adiabatic schedules that makes this computation more tractable, and which may be of independent interest. We further study the effectiveness of random intermediate Hamiltonians on the minimum gap and success probability, and empirically find that random Hamiltonians have a significant probability of increasing the success probability, but only by a modest amount.

  14. Sliding Seal Materials for Adiabatic Engines, Phase 2

    NASA Technical Reports Server (NTRS)

    Lankford, J.; Wei, W.

    1986-01-01

    An essential task in the development of the heavy-duty adiabatic diesel engine is identification and improvements of reliable, low-friction piston seal materials. In the present study, the sliding friction coefficients and wear rates of promising carbide, oxide, and nitride materials were measured under temperature, environmental, velocity, and loading conditions that are representative of the adiabatic engine environment. In addition, silicon nitride and partially stabilized zirconia disks were ion implanted with TiNi, Ni, Co, and Cr, and subsequently run against carbide pins, with the objective of producing reduced friction via solid lubrication at elevated temperature. 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. Electron microscopy was used to elucidate the micromechanisms of wear following wear testing, and Auger electron spectroscopy was used to evaluate interface/environment interactions which seemed to be important in the friction and wear process. Unmodified ceramic sliding couples were characterized at all temperatures by friction coefficients of 0.24 and above. The coefficient at 800 C in an oxidizing environment was reduced to below 0.1, for certain material combinations, by the ion implanation of TiNi or Co. This beneficial effect was found to derive from lubricious Ti, Ni, and Co oxides.

  15. Fast Ion Non-adiabaticity in Spherical Tokamaks

    SciTech Connect

    V.A. Yavorskij; D. Darrow; V.Ya. Goloborod'ko; S.N. Reznik; U. Holzmueller-Steinacker; N. Gorelenkov; K. Schoepf

    2002-08-01

    Transport processes of fast ions in axisymmetric low-aspect-ratio spherical torus (ST) plasmas are investigated, which are induced by the non-conservation of the magnetic moment {mu}. The reason for non-conservation of {mu} of fast ions in ST's is the relatively large adiabaticity parameter epsilon typically exceeding the value 0.1 (epsilon = ratio of ion gyroradius to the gradient scale length of the magnetic field). Both analytical and numerical evaluations of the magnitude of nonadiabatic variations of {mu} are performed. Nonadiabaticity effects are shown to be most significant for fast ions for which the bounce oscillations are in resonance with the gyromotion, i.e., for ions with omega(subscript)B - lomega(subscript)b = 0, where omega(subscript)B and omega(subscript)b represent the bounce-averaged gyrofrequency and the bounce frequency, respectively, and l is an integer. The critical threshold of the adiabaticity parameter, epsilon(subscript)cr, to be exceeded for the transition to stochastic behavior of fast ions in axisymmetric ST's is inspected. Nonadiabatic variations of {mu} are shown to lead to collisionless transformation of trapped orbits into circulating ones and vice versa. For the case of strong nonadiabaticity, epsilon > epsilon(subscript)cr, we assess the transport coefficients describing intense collisionless pitch-angle diffusion, whereas, in the case of weak nonadiabaticity, epsilon > epsilon(subscript)cr, the more substantial coefficients of enhanced collisional radial diffusion and convection of fast ions gyrating resonantly with the bounce oscillations are estimated.

  16. Robust quantum logic in neutral atoms via adiabatic Rydberg dressing

    SciTech Connect

    Keating, Tyler; Cook, Robert L.; Hankin, Aaron M.; Jau, Yuan -Yu; Biedermann, Grant W.; Deutsch, Ivan H.

    2015-01-28

    We study a scheme for implementing a controlled-Z (CZ) gate between two neutral-atom qubits based on the Rydberg blockade mechanism in a manner that is robust to errors caused by atomic motion. By employing adiabatic dressing of the ground electronic state, we can protect the gate from decoherence due to random phase errors that typically arise because of atomic thermal motion. In addition, the adiabatic protocol allows for a Doppler-free configuration that involves counterpropagating lasers in a σ+- orthogonal polarization geometry that further reduces motional errors due to Doppler shifts. The residual motional error is dominated by dipole-dipole forces acting on doubly-excited Rydberg atoms when the blockade is imperfect. As a result, for reasonable parameters, with qubits encoded into the clock states of 133Cs, we predict that our protocol could produce a CZ gate in < 10 μs with error probability on the order of 10-3.

  17. Adiabatic cooling of the artificial Porcupine plasma jet

    NASA Astrophysics Data System (ADS)

    Ruizhin, Iu. Ia.; Treumann, R. A.; Bauer, O. H.; Moskalenko, A. M.

    1987-01-01

    Measurements of the plasma density obtained during the interaction of the artificial plasma jet, fired into the ionosphere with the body of the Porcupine main payload, have been analyzed for times when there was a well-developed wake effect. Using wake theory, the maximum temperature of the quasi-neutral xenon ion beam has been determined for an intermediate distance from the ion beam source when the beam has left the diamagnetic region but is still much denser than the ionospheric background plasma. The beam temperature is found to be about 4 times less than the temperature at injection. This observation is very well explained by adiabatic cooling of the beam during its initial diamagnetic and current-buildup phases at distances r smaller than 10 m. Outside this region, the beam conserves the temperature achieved. The observation proves that the artificial plasma jet passes through an initial gas-like diamagnetic phase restricted to the vicinity of the beam source, where it expands adiabatically. Partial cooling also takes place outside the diamagnetic region where the beam current still builds up. The observations also support a recently developed current-closure model of the quasi-neutral ion beam.

  18. The 0.1K bolometers cooled by adiabatic demagnetization

    NASA Technical Reports Server (NTRS)

    Roellig, T.; Lesyna, L.; Kittel, P.; Werner, M.

    1983-01-01

    The most straightforward way of reducing the noise equivalent power of bolometers is to lower their operating temperature. We have been exploring the possibility of using conventionally constructed bolometers at ultra-low temperatures to achieve NEP's suitable to the background environment of cooled space telescopes. We have chosen the technique of adiabatic demagnetization of a paramagnetic salt as a gravity independent, compact, and low power way to achieve temperatures below pumped He-3 (0.3 K). The demagnetization cryostat we used was capable of reaching temperatures below 0.08 K using Chromium Potassium Alum as a salt from a starting temperature of 1.5 K and a starting magnetic field of 30,000 gauss. Computer control of the magnetic field decay allowed a temperature of 0.2 K to be maintained to within 0.5 mK over a time period exceeding 14 hours. The refrigerator duty cycle was over 90 percent at this temperature. The success of these tests has motivated us to construct a more compact portable adiabatic demagnetization cryostat capable of bolometer optical tests and use at the 5m Hale telescope at 1mm wavelengths.

  19. FRW-type cosmologies with adiabatic matter creation

    NASA Astrophysics Data System (ADS)

    Lima, J. A. S.; Germano, A. S. M.; Abramo, L. R. W.

    1996-04-01

    Some properties of cosmological models with matter creation are investigated in the framework of the Friedmann-Robertson-Walker line element. For adiabatic matter creation, as developed by Prigogine and co-workers, we derive a simple expression relating the particle number density n and energy density ρ which holds regardless of the matter creation rate. The conditions to generate inflation are discussed and by considering the natural phenomenological matter creation rate ψ=3βnH, where β is a pure number of the order of unity and H is the Hubble parameter, a minimally modified hot big-bang model is proposed. The dynamic properties of such models can be deduced from the standard ones simply by replacing the adiabatic index γ of the equation of state by an effective parameter γ*=γ(1-β). The thermodynamic behavior is determined and it is also shown that ages large enough to agree with observations are obtained even given the high values of H suggested by recent measurements.

  20. Conditions for super-adiabatic droplet growth after entrainment mixing

    DOE PAGESBeta

    Yang, Fan; Shaw, Raymond; Xue, Huiwen

    2016-07-29

    Cloud droplet response to entrainment and mixing between a cloud and its environment is considered, accounting for subsequent droplet growth during adiabatic ascent following a mixing event. The vertical profile for liquid water mixing ratio after a mixing event is derived analytically, allowing the reduction to be predicted from the mixing fraction and from the temperature and humidity for both the cloud and environment. It is derived for the limit of homogeneous mixing. The expression leads to a critical height above the mixing level: at the critical height the cloud droplet radius is the same for both mixed and unmixedmore » parcels, and the critical height is independent of the updraft velocity and mixing fraction. Cloud droplets in a mixed parcel are larger than in an unmixed parcel above the critical height, which we refer to as the “super-adiabatic” growth region. Analytical results are confirmed with a bin microphysics cloud model. Using the model, we explore the effects of updraft velocity, aerosol source in the environmental air, and polydisperse cloud droplets. Results show that the mixed parcel is more likely to reach the super-adiabatic growth region when the environmental air is humid and clean. It is also confirmed that the analytical predictions are matched by the volume-mean cloud droplet radius for polydisperse size distributions. The findings have implications for the origin of large cloud droplets that may contribute to onset of collision–coalescence in warm clouds.« less