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Sample records for adiabatic potential surface

  1. A classical determination of vibrationally adiabatic barriers and wells of a collinear potential energy surface

    NASA Astrophysics Data System (ADS)

    Pollak, Eli

    1981-05-01

    A necessary and sufficient condition for the existence of a classical vibrationally adiabatic barrier or well in collinear systems is the existence of periodic orbit dividing surfaces. Knowledge of all pods immediately provides all adiabatic barriers and wells. Furthermore, the classical equation connecting the barriers and wells to the masses and potential energy surface of the system is shown, under mild conditions, to be identical in form to the corresponding quantal equation. The only difference is in the determination of the vibrational state which is obtained by WKB quantization classically. The classical barriers and wells can therefore be used to analyze quantal computations. Such analysis is provided for the hydrogen exchange reaction and the F+HH system. A novel result is the existence of vibrationally adiabatic barriers even where no saddle point exists on the static potential energy surface. These barriers are an outcome of competition between the increase of potential energy and decrease of vibrational force constant along the reaction coordinate. Their existence is therefore of general nature — not limited to the specific structure of a given potential energy surface. The experimental significance of these barriers is discussed. The implications on the use of forward or reverse quasiclassical computations is analyzed. A definite conclusion is that one should not average over initial vibrational action in such calculations.

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

    NASA Astrophysics Data System (ADS)

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

    2012-01-01

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

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

    SciTech Connect

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

    2005-04-15

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

  4. Ab - initio non-adiabatic couplings among three lowest singlet states of H3 +: Construction of multisheeted diabatic potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Mukherjee, Bijit; Mukherjee, Saikat; Adhikari, Satrajit

    2016-10-01

    We calculate the adiabatic potential energy surfaces and non-adiabatic interactions among the three lowest singlet states (11 A', 21 A' and 31 A') of H3 + in hyperspherical coordinates for a fixed hyperradius, ρ = 9 bohr as functions of hyperangles, θ (0 < θ < 90°) and ϕ (0 < ϕ < 360°). All ab initio calculations are performed using MRCI level of methodology implemented in quantum chemistry package, MOLPRO. The ground (11 A') and the first excited (21 A') states exhibit several conical intersections as functions of ϕ for θ > 70°. Subsequently, we carry out adiabatic to diabatic transformation (ADT) to obtain ADT angles for constructing single-valued, continuous, smooth and symmetric 3 × 3 diabatic potential energy matrix to perform accurate scattering calculations.

  5. Coupled wave-packets for non-adiabatic molecular dynamics: a generalization of Gaussian wave-packet dynamics to multiple potential energy surfaces

    SciTech Connect

    White, Alexander James; Tretiak, Sergei; Mozyrsky, Dima V.

    2016-04-25

    Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as efficient as the commonly used mean field Ehrenfest or ad hoc surface hopping methods and properly accounts for interference and decoherence effects. This novel method is an extension of Heller's thawed Gaussian wave-packet dynamics that includes coupling between potential energy surfaces. By studying several standard test problems we demonstrate that the accuracy of the method can be systematically improved while maintaining high efficiency. The method is suitable for investigating the role of quantum coherence in the non-adiabatic dynamics of many-atom molecules.

  6. Coupled wave-packets for non-adiabatic molecular dynamics: a generalization of Gaussian wave-packet dynamics to multiple potential energy surfaces

    DOE PAGES

    White, Alexander James; Tretiak, Sergei; Mozyrsky, Dima V.

    2016-04-25

    Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as efficient as the commonly used mean field Ehrenfest or ad hoc surface hopping methods and properly accounts for interference and decoherence effects. This novel method is an extension of Heller's thawed Gaussian wave-packet dynamics that includes coupling between potential energy surfaces. By studying several standard test problems we demonstrate that the accuracy of the method can be systematically improved while maintaining high efficiency. The method is suitablemore » for investigating the role of quantum coherence in the non-adiabatic dynamics of many-atom molecules.« less

  7. 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.

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

    NASA Astrophysics Data System (ADS)

    Cremers, C.; Degen, J.

    1998-11-01

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

  9. Probing mechanistic photochemistry of glyoxal in the gas phase by ab initio calculations of potential-energy surfaces and adiabatic and nonadiabatic rates.

    PubMed

    Li, Quan-Song; Zhang, Feng; Fang, Wei-Hai; Yu, Jian-Guo

    2006-02-07

    In the present work, the wavelength-dependent mechanistic photochemistry of glyoxal in the gas phase has been explored by ab initio calculations of potential-energy surfaces, surface crossing points, and adiabatic and nonadiabatic rates. The CHOCHO molecules in S1 by photoexcitation at 393-440 nm mainly decay to the ground state via internal conversion, which is followed by molecular eliminations to form CO, H2CO,H2, and HCOH. Upon photodissociation of CHOCHO at 350-390 nm, intersystem crossing to T1 followed by the C-C bond cleavage is the dominant process in this wavelength range, which is responsible for the formation of the CHO radicals. The C-C and C-H bond cleavages along the S1 pathway are energetically accessible upon photodissociation of CHOCHO at 290-310 nm, which can compete with the S1-->T1 intersystem crossing process. The present study predicts that the C-H bond cleavage on the S1 surface is probably a new photolysis pathway at high excitation energy, which has not been observed experimentally. In addition, the trans-cis isomerization is predicted to occur more easily in the ground state than in the excited states.

  10. A quantum equation of motion for chemical reaction systems on an adiabatic double-well potential surface in solution based on the framework of mixed quantum-classical molecular dynamics.

    PubMed

    Yamada, Atsushi; Okazaki, Susumu

    2008-01-28

    We present a quantum equation of motion for chemical reaction systems on an adiabatic double-well potential surface in solution in the framework of mixed quantum-classical molecular dynamics, where the reactant and product states are explicitly defined by dividing the double-well potential into the reactant and product wells. The equation can describe quantum reaction processes such as tunneling and thermal excitation and relaxation assisted by the solvent. Fluctuations of the zero-point energy level, the height of the barrier, and the curvature of the well are all included in the equation. Here, the equation was combined with the surface hopping technique in order to describe the motion of the classical solvent. Applying the present method to model systems, we show two numerical examples in order to demonstrate the potential power of the present method. The first example is a proton transfer by tunneling where the high-energy product state was stabilized very rapidly by solvation. The second example shows a thermal activation mechanism, i.e., the initial vibrational excitation in the reactant well followed by the reacting transition above the barrier and the final vibrational relaxation in the product well.

  11. The best of both Reps—Diabatized Gaussians on adiabatic surfaces

    NASA Astrophysics Data System (ADS)

    Meek, Garrett A.; Levine, Benjamin G.

    2016-11-01

    When simulating nonadiabatic molecular dynamics, choosing an electronic representation requires consideration of well-known trade-offs. The uniqueness and spatially local couplings of the adiabatic representation come at the expense of an electronic wave function that changes discontinuously with nuclear motion and associated singularities in the nonadiabatic coupling matrix elements. The quasi-diabatic representation offers a smoothly varying wave function and finite couplings, but identification of a globally well-behaved quasi-diabatic representation is a system-specific challenge. In this work, we introduce the diabatized Gaussians on adiabatic surfaces (DGAS) approximation, a variant of the ab initio multiple spawning (AIMS) method that preserves the advantages of both electronic representations while avoiding their respective pitfalls. The DGAS wave function is expanded in a basis of vibronic functions that are continuous in both electronic and nuclear coordinates, but potentially discontinuous in time. Because the time-dependent Schrödinger equation contains only first-order derivatives with respect to time, singularities in the second-derivative nonadiabatic coupling terms (i.e., diagonal Born-Oppenheimer correction; DBOC) at conical intersections are rigorously absent, though singular time-derivative couplings remain. Interpolation of the electronic wave function allows the accurate prediction of population transfer probabilities even in the presence of the remaining singularities. We compare DGAS calculations of the dynamics of photoexcited ethene to AIMS calculations performed in the adiabatic representation, including the DBOC. The 28 fs excited state lifetime observed in DGAS simulations is considerably shorter than the 50 fs lifetime observed in the adiabatic simulations. The slower decay in the adiabatic representation is attributable to the large, repulsive DBOC in the neighborhood of conical intersections. These repulsive DBOC terms are artifacts

  12. Recent developments in trapping and manipulation of atoms with adiabatic potentials

    NASA Astrophysics Data System (ADS)

    Garraway, Barry M.; Perrin, Hélène

    2016-09-01

    A combination of static and oscillating magnetic fields can be used to ‘dress’ atoms with radio-frequency (RF), or microwave, radiation. The spatial variation of these fields can be used to create an enormous variety of traps for ultra-cold atoms and quantum gases. This article reviews the type and character of these adiabatic traps and the applications which include atom interferometry and the study of low-dimensional quantum systems. We introduce the main concepts of magnetic traps leading to adiabatic dressed traps. The concept of adiabaticity is discussed in the context of the Landau-Zener model. The first bubble trap experiment is reviewed together with the method used for loading it. Experiments based on atom chips show the production of double wells and ring traps. Dressed atom traps can be evaporatively cooled with an additional RF field, and a weak RF field can be used to probe the spectroscopy of the adiabatic potentials. Several approaches to ring traps formed from adiabatic potentials are discussed, including those based on atom chips, time-averaged adiabatic potentials and induction methods. Several proposals for adiabatic lattices with dressed atoms are also reviewed.

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

    SciTech Connect

    Zhang, P.; You, L.

    2007-09-15

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

  14. Temperature-Driven and Electrochemical-Potential-Driven Adiabatic Pumping via a Quantum Dot

    NASA Astrophysics Data System (ADS)

    Hasegawa, Masahiro; Kato, Takeo

    2017-02-01

    We investigate adiabatic pumping via a single level quantum dot induced by periodic modulation of thermodynamic variables of reservoirs, i.e., temperatures and electrochemical potentials. We consider the impurity Anderson model and derive analytical formulas for coherent adiabatic charge pumping applicable to the strong dot-reservoir coupling within the first-order perturbation with respect to Coulomb interaction. We show that charge pumping is induced by rectification effect due to delayed response of the quantum dot to time-dependent reservoir parameters. The presence of interaction is necessary because this delayed response rectifies charge current via Coulomb interaction. For temperature-driven charge pumping, one-way pumping is realized regardless of reservoir temperatures when an energy level of the quantum dot locates near the Fermi level. We clarify that this new feature of adiabatic pumping is caused by level broadening effect of the quantum dot due to strong dot-reservoir coupling.

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

    NASA Astrophysics Data System (ADS)

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

    2012-02-01

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

  16. Accurate ab initio-based adiabatic global potential energy surface for the 2{sup 2}A″ state of NH{sub 2} by extrapolation to the complete basis set limit

    SciTech Connect

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

    2013-10-21

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

  17. Idealized numerical simulation study of the potential vorticity banners over a mesoscale mountain: Dry adiabatic process

    NASA Astrophysics Data System (ADS)

    Wang, Qiwei; Tan, Zhemin

    2009-09-01

    Topography-induced potential vorticity (PV) banners over a mesoscale topography (Dabie Mountain, hereafter DM) in eastern China, under an idealized dry adiabatic flow, are studied with a mesoscale numerical model, ARPS. PV banners generate over the leeside of the DM with a maximal intensity of ˜1.5 PVU, and extend more than 100 km downstream, while the width varies from several to tens of kilometers, which contrasts with the half-width of the peaks along the ridge of the DM. Wave breaking occurs near the leeside surface of the DM, and leads to a strong PV generation. Combining with the PV generation, due to the friction and the flow splitting upstream, the PV is advected downstream, and then forms the PV banners over the DM. The PV banners are sensitive to the model resolution, Coriolis force, friction, subgrid turbulent mixing, stratification, the upstream wind speed and wind direction. The negative PV banners have a more compact connection with the low level turbulent kinetic energy. The PV banners are built up by the baroclinic and barotropic components. The barotropic-associated PV can identify the distribution of the PV banners, while the baroclinic one only has important contributions on the flanks and on the leeside near the topography. PV fluxes are diagnosed to investigate the influence of friction on the PV banners. Similar patterns are found between the total PV flux and the advective PV flux, except near the surface and inside the dipole of the PV banners, where the nonadvective PV flux associated with the friction has a net negative contribution.

  18. Practical approximation of the non-adiabatic coupling terms for same-symmetry interstate crossings by using adiabatic potential energies only

    NASA Astrophysics Data System (ADS)

    Baeck, Kyoung Koo; An, Heesun

    2017-02-01

    A very simple equation, Fij A p p=[(∂2(Via-Vja ) /∂Q2 ) /(Via-Vja ) ] 1 /2/2 , giving a reliable magnitude of non-adiabatic coupling terms (NACTs, Fij's) based on adiabatic potential energies only (Via and Vja) was discovered, and its reliability was tested for several prototypes of same-symmetry interstate crossings in LiF, C2, NH3Cl, and C6H5SH molecules. Our theoretical derivation starts from the analysis of the relationship between the Lorentzian dependence of NACTs along a diabatization coordinate and the well-established linear vibronic coupling scheme. This analysis results in a very simple equation, α =2 κ /Δc , enabling the evaluation of the Lorentz function α parameter in terms of the coupling constant κ and the energy gap Δc (Δc=|Via-Vja| Q c ) between adiabatic states at the crossing point QC. Subsequently, it was shown that QC corresponds to the point where Fij A p p exhibit maximum values if we set the coupling parameter as κ =[(Via-Vja ) ṡ(∂2(Via-Vja ) /∂Q2 ) ] Qc1 /2 /2 . Finally, we conjectured that this relation could give reasonable values of NACTs not only at the crossing point but also at other geometries near QC. In this final approximation, the pre-defined crossing point QC is not required. The results of our test demonstrate that the approximation works much better than initially expected. The present new method does not depend on the selection of an ab initio method for adiabatic electronic states but is currently limited to local non-adiabatic regions where only two electronic states are dominantly involved within a nuclear degree of freedom.

  19. Non-adiabatic dynamics close to conical intersections and the surface hopping perspective.

    PubMed

    Malhado, João Pedro; Bearpark, Michael J; Hynes, James T

    2014-01-01

    Conical intersections play a major role in the current understanding of electronic de-excitation in polyatomic molecules, and thus in the description of photochemistry and photophysics of molecular systems. This article reviews aspects of the basic theory underlying the description of non-adiabatic transitions at conical intersections, with particular emphasis on the important case when the dynamics of the nuclei are treated classically. Within this classical nuclear motion framework, the main aspects of the surface hopping methodology in the conical intersection context are presented. The emerging picture from this treatment is that of electronic transitions around conical intersections dominated by the interplay of the nuclear velocity and the derivative non-adiabatic coupling vector field.

  20. Non-adiabatic dynamics close to conical intersections and the surface hopping perspective

    PubMed Central

    Malhado, João Pedro; Bearpark, Michael J.; Hynes, James T.

    2014-01-01

    Conical intersections play a major role in the current understanding of electronic de-excitation in polyatomic molecules, and thus in the description of photochemistry and photophysics of molecular systems. This article reviews aspects of the basic theory underlying the description of non-adiabatic transitions at conical intersections, with particular emphasis on the important case when the dynamics of the nuclei are treated classically. Within this classical nuclear motion framework, the main aspects of the surface hopping methodology in the conical intersection context are presented. The emerging picture from this treatment is that of electronic transitions around conical intersections dominated by the interplay of the nuclear velocity and the derivative non-adiabatic coupling vector field. PMID:25485263

  1. A theoretical study of non-adiabatic surface effects for a model in the NTF cryogenic wind tunnel

    NASA Technical Reports Server (NTRS)

    Macha, J. M.; Pare, L. A.; Landrum, D. B.

    1985-01-01

    A theoretical analysis was made of the severity and effect of nonadiabatic surface conditions for a model in the NTF cryogenic wind tunnel. The nonadiabatic condition arises from heaters that are used to maintain a constant thermal environment for instrumentation internal to the model. The analysis was made for several axi-symmetric representations of a fuselage cavity, using a finite element heat conduction code. Potential flow and boundary layer codes were used to calculate the convection condition for the exterior surface of the model. The results of the steady state analysis show that it is possible to maintain the surface temperature very near the adiabatic value, with the judicious use of insulating material. Even for the most severe nonadiabatic condition studied, the effects on skin friction drag and displacement thickness were only marginally significant. The thermal analysis also provided an estimate of the power required to maintain a specified cavity temperature.

  2. Efficient and direct generation of multidimensional free energy surfaces via adiabatic dynamics without coordinate transformations.

    PubMed

    Abrams, Jerry B; Tuckerman, Mark E

    2008-12-11

    Adiabatic free energy dynamics (AFED) was introduced by Rosso et al. [J. Chem. Phys. 2002, 116, 4389] for computing free energy profiles quickly and accurately using a dynamical adiabatic separation between a set of collective variables or reaction coordinates and the remaining degrees of freedom of a system. This approach has been shown to lead to a significant gain in efficiency versus traditional methods such as umbrella sampling, thermodynamic integration, and free energy perturbation for generating one-dimensional free energy profiles. More importantly, AFED is able to generate multidimensional free energy surfaces efficiently via full sweeps of the surface that rapidly map out the locations of the free energy minima. The most significant drawback to the AFED approach is the need to transform the coordinates into a generalized coordinate system that explicitly contains the collective variables of interest. Recently, Maragliano and Vanden-Eijnden built upon the AFED approach by introducing a set of extended phase-space variables, to which the adiabatic decoupling and high temperature are applied [Chem. Phys. Lett. 2006, 426, 168]. In this scheme, which the authors termed "temperature accelerated molecular dynamics" or TAMD, the need for explicit coordinate transformations is circumvented. The ability of AFED and TAMD to generate free energy surfaces efficiently depends on the thermostatting mechanism employed, since both approaches are inherently nonequilibrium due to the adiabatic decoupling. Indeed, Maragliano and Vanden-Eijnden did not report any direct generation of free energy surfaces within the overdamped Langevin dynamics employed by these authors. Here, we show that by formulating TAMD in a manner that is closer to the original AFED approach, including the generalized Gaussian moment thermostat (GGMT) and multiple time-scale integration, multidimensional free energy surfaces for complex systems can be generated directly from the probability

  3. Theoretical study of the CsNa molecule: adiabatic and diabatic potential energy and dipole moment.

    PubMed

    Mabrouk, N; Berriche, H

    2014-09-25

    The adiabatic and diabatic potential energy curves of the low-lying electronic states of the NaCs molecule dissociating into Na (3s, 3p) + Cs (6s, 6p, 5d, 7s, 7p, 6d, 8s, 4f) have been investigated. The molecular calculations are performed using an ab initio approach based on nonempirical pseudopotential, parametrized l-dependent polarization potentials and full configuration interaction calculations through the CIPCI quantum chemistry package. The derived spectroscopic constants (Re, De, Te, ωe, ωexe, and Be) of the ground state and lower excited states are compared with the available theoretical and experimental works. Moreover, accurate permanent and transition dipole moment have been determined as a function of the internuclear distance. The adiabatic permanent dipole moment for the first nine (1)Σ(+) electronic states have shown both ionic characters associated with electron transfer related to Cs(+)Na(-) and Cs(-)Na(+) arrangements. By a simple rotation, the diabatic permanent dipole moment is determined and has revealed a linear behavior, particularly at intermediate and large distances. Many peaks around the avoided crossing locations have been observed for the transition dipole moment between neighbor electronic states.

  4. Development of a general time-dependent absorbing potential for the constrained adiabatic trajectory method.

    PubMed

    Leclerc, Arnaud; Jolicard, Georges; Killingbeck, John P

    2011-05-21

    The constrained adiabatic trajectory method (CATM) allows us to compute solutions of the time-dependent Schrödinger equation using the Floquet formalism and Fourier decomposition, using matrix manipulation within a non-orthogonal basis set, provided that suitable constraints can be applied to the initial conditions for the Floquet eigenstate. A general form is derived for the inherent absorbing potential, which can reproduce any dispersed boundary conditions. This new artificial potential acting over an additional time interval transforms any wavefunction into a desired state, with an error involving exponentially decreasing factors. Thus, a CATM propagation can be separated into several steps to limit the size of the required Fourier basis. This approach is illustrated by some calculations for the H(2)(+) molecular ion illuminated by a laser pulse.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  6. Laser propulsion of nanobullets by adiabatic compression of surface plasmon polaritons

    NASA Astrophysics Data System (ADS)

    Folli, Viola; Ruocco, Giancarlo; Conti, Claudio

    2015-12-01

    Laser propulsion and guide of nanosized objects is fundamental for a wide number of applications. These applications are often limited by the fact that the optical forces acting on nanoparticles are almost negligible even in the favorable case of metallic particles and hence large laser powers are needed to accelerate and guide nanosize devices in practical applications. Furthermore, metallic nanoparticles exhibit strong absorption bands and scattering and this makes more difficult controlling nanopropulsion. Thus, finding some mechanism enhancing the optomechanical interaction at the nanoscale controlled by laser is specifically challenging and pivotal. Here, we demonstrate a novel physical effect where the well-known adiabatic localization of the enhanced plasmonic surface field on the apex of metallic nanocones produces a significant optical pressure employable as a propulsive mechanism. The proposed method gives the possibility to develop new photonics devices to accelerate metallic nanobullets over long distances for a variety of applications.

  7. Atomistic potentials based energy flux integral criterion for dynamic adiabatic shear banding

    NASA Astrophysics Data System (ADS)

    Xu, Yun; Chen, Jun

    2015-02-01

    The energy flux integral criterion based on atomistic potentials within the framework of hyperelasticity-plasticity is proposed for dynamic adiabatic shear banding (ASB). System Helmholtz energy decomposition reveals that the dynamic influence on the integral path dependence is originated from the volumetric strain energy and partial deviatoric strain energy, and the plastic influence only from the rest part of deviatoric strain energy. The concept of critical shear banding energy is suggested for describing the initiation of ASB, which consists of the dynamic recrystallization (DRX) threshold energy and the thermal softening energy. The criterion directly relates energy flux to the basic physical processes that induce shear instability such as dislocation nucleations and multiplications, without introducing ad-hoc parameters in empirical constitutive models. It reduces to the classical path independent J-integral for quasi-static loading and elastic solids. The atomistic-to-continuum multiscale coupling method is used to simulate the initiation of ASB. Atomic configurations indicate that DRX induced microstructural softening may be essential to the dynamic shear localization and hence the initiation of ASB.

  8. Nonintuitive Diabatic Potential Energy Surfaces for Thioanisole.

    PubMed

    Li, Shaohong L; Xu, Xuefei; Hoyer, Chad E; Truhlar, Donald G

    2015-09-03

    Diabatization of potential energy surfaces is a technique that enables convenient molecular dynamics simulations of electronically nonadiabatic processes, but diabatization itself is nonunique and can be inconvenient; the best methods to achieve diabatization are still under study. Here, we present the diabatization of two electronic states of thioanisole in the S-CH3 bond stretching and C-C-S-C torsion two-dimensional nuclear coordinate space containing a conical intersection. We use two systematic methods: the (orbital-dependent) 4-fold way and the (orbital-free) Boys localization diabatization method. These very different methods yield strikingly similar diabatic potential energy surfaces that cross at geometries where the adiabatic surfaces are well separated and do not exhibit avoided crossings, and the contours of the diabatic gap and diabatic coupling are similar for the two methods. The validity of the diabatization is supported by comparing the nonadiabatic couplings calculated from the diabatic matrix elements to those calculated by direct differentiation of the adiabatic states.

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

    SciTech Connect

    Kato, Tsuyoshi; Ide, Yoshihiro; Yamanouchi, Kaoru

    2015-12-31

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

  10. 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.

  11. Double-resonance spectroscopy of the high Rydberg states of HCO. I. A precise determination of the adiabatic ionization potential

    NASA Astrophysics Data System (ADS)

    Mayer, Eric; Grant, Edward R.

    1995-12-01

    We report the first spectroscopic observation of the high Rydberg states of HCO. Individual lines in a system of vibrationally autoionizing Rydberg series converging to the (010) state of HCO+ are rotationally labeled in a double-resonance excitation scheme that uses resolved levels in the (010) A' vibronic component of the 3pπ 2Π Rydberg state as intermediates. Observed high-Rydberg structure extends from the adiabatic ionization threshold—which falls just below the principal quantum number of 12 in the vibrationally excited series—to the (010) vertical threshold. Elements of a single series extending from n=12 to 50, for which the total angular momentumless spin can be assigned as N=1, are extrapolated to obtain a vertical convergence limit with respect to the 3pπ 2Π(010)A' N'=0 intermediate state of 20 296.9±0.3 cm-1. Referring this transition energy to the ground state, and subtracting the precisely known fundamental bending frequency of the cation, establishes the adiabatic ionization potential corresponding to the transition from HCO 2A'(000) J″=0, K″=0 to HCO+ J+=0 1Σ+(000). The result is 65 735.9±0.5 cm-1 or 8.150 22±0.000 06 eV.

  12. Effect of adiabatic wall on the natural convection heat transfer from a wavy surface created by attached horizontal cylinders

    SciTech Connect

    Harsini, I.; Ashjaee, M.

    2010-09-15

    The effect of a vertical adiabatic wall on the natural convection heat transfer from vertical array of attached cylinders, which can be considered as wavy surface, was investigated experimentally and numerically. The experiments were carried out using Mach-Zehnder interferometer and the commercial FLUENT code was used for numerical study. This paper focuses on the effect of wall-wavy surface spacing and Rayleigh number variation on the local and average free convection heat transfer coefficients from the each cylinder and the wavy surface. Rayleigh number ranges from 2400 to 10,000 and from 300,000 to 1,250,000 based on cylinder diameter and wavy surface height respectively. The local and average Nusselt numbers were determined for the different Rayleigh numbers, and the ratio of wall- wavy surface spacing to cylinder diameter 0.75, 1, 1.5, 2, 3, 4, 5, and {infinity}. Results are indicated with a single correlation which gives the average Nusselt number as a function of the ratio of the wall-wavy surface spacing to cylinder diameter and the Rayleigh numbers. There is an optimum distance between the wall and wavy surface in which the Nusselt number attain its maximum value. This optimum distance depends on the Rayleigh number. (author)

  13. Modelling non-adiabatic effects in H{sub 3}{sup +}: Solution of the rovibrational Schrödinger equation with motion-dependent masses and mass surfaces

    SciTech Connect

    Mátyus, Edit; Szidarovszky, Tamás

    2014-10-21

    Introducing different rotational and vibrational masses in the nuclear-motion Hamiltonian is a simple phenomenological way to model rovibrational non-adiabaticity. It is shown on the example of the molecular ion H{sub 3}{sup +}, for which a global adiabatic potential energy surface accurate to better than 0.1 cm{sup −1} exists [M. Pavanello, L. Adamowicz, A. Alijah, N. F. Zobov, I. I. Mizus, O. L. Polyansky, J. Tennyson, T. Szidarovszky, A. G. Császár, M. Berg et al., Phys. Rev. Lett. 108, 023002 (2012)], that the motion-dependent mass concept yields much more accurate rovibrational energy levels but, unusually, the results are dependent upon the choice of the embedding of the molecule-fixed frame. Correct degeneracies and an improved agreement with experimental data are obtained if an Eckart embedding corresponding to a reference structure of D{sub 3h} point-group symmetry is employed. The vibrational mass of the proton in H{sub 3}{sup +} is optimized by minimizing the root-mean-square (rms) deviation between the computed and recent high-accuracy experimental transitions. The best vibrational mass obtained is larger than the nuclear mass of the proton by approximately one third of an electron mass, m{sub opt,p}{sup (v)}=m{sub nuc,p}+0.31224 m{sub e}. This optimized vibrational mass, along with a nuclear rotational mass, reduces the rms deviation of the experimental and computed rovibrational transitions by an order of magnitude. Finally, it is shown that an extension of the algorithm allowing the use of motion-dependent masses can deal with coordinate-dependent mass surfaces in the rovibrational Hamiltonian, as well.

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

    NASA Technical Reports Server (NTRS)

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

    1982-01-01

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

  15. Digital waveguide adiabatic passage part 1: theory

    NASA Astrophysics Data System (ADS)

    Vaitkus, Jesse A.; Steel, M. J.; Greentree, Andrew D.

    2017-03-01

    Spatial adiabatic passage represents a new way to design integrated photonic devices. In conventional adiabatic passage designs require smoothly varying waveguide separations. Here we show modelling of adiabatic passage devices where the waveguide separation is varied digitally. Despite digitisation, our designs show robustness against variations in the input wavelength and refractive index contrast of the waveguides relative to the cladding. This approach to spatial adiabatic passage opens new design strategies and hence the potential for new photonics devices.

  16. Effects of adiabatic, relativistic, and quantum electrodynamics interactions on the pair potential and thermophysical properties of helium.

    PubMed

    Cencek, Wojciech; Przybytek, Michał; Komasa, Jacek; Mehl, James B; Jeziorski, Bogumił; Szalewicz, Krzysztof

    2012-06-14

    The adiabatic, relativistic, and quantum electrodynamics (QED) contributions to the pair potential of helium were computed, fitted separately, and applied, together with the nonrelativistic Born-Oppenheimer (BO) potential, in calculations of thermophysical properties of helium and of the properties of the helium dimer. An analysis of the convergence patterns of the calculations with increasing basis set sizes allowed us to estimate the uncertainties of the total interaction energy to be below 50 ppm for interatomic separations R smaller than 4 bohrs and for the distance R = 5.6 bohrs. For other separations, the relative uncertainties are up to an order of magnitude larger (and obviously still larger near R = 4.8 bohrs where the potential crosses zero) and are dominated by the uncertainties of the nonrelativistic BO component. These estimates also include the contributions from the neglected relativistic and QED terms proportional to the fourth and higher powers of the fine-structure constant α. To obtain such high accuracy, it was necessary to employ explicitly correlated Gaussian expansions containing up to 2400 terms for smaller R (all R in the case of a QED component) and optimized orbital bases up to the cardinal number X = 7 for larger R. Near-exact asymptotic constants were used to describe the large-R behavior of all components. The fitted potential, exhibiting the minimum of -10.996 ± 0.004 K at R = 5.608 0 ± 0.000 1 bohr, was used to determine properties of the very weakly bound (4)He(2) dimer and thermophysical properties of gaseous helium. It is shown that the Casimir-Polder retardation effect, increasing the dimer size by about 2 Å relative to the nonrelativistic BO value, is almost completely accounted for by the inclusion of the Breit-interaction and the Araki-Sucher contributions to the potential, of the order α(2) and α(3), respectively. The remaining retardation effect, of the order of α(4) and higher, is practically negligible for the bound

  17. Surface-effect corrections for solar-like oscillations using 3D hydrodynamical simulations. I. Adiabatic oscillations

    NASA Astrophysics Data System (ADS)

    Sonoi, T.; Samadi, R.; Belkacem, K.; Ludwig, H.-G.; Caffau, E.; Mosser, B.

    2015-11-01

    Context. The CoRoT and Kepler space-borne missions have provided us with a wealth of high-quality observational data that allows for seismic inferences of stellar interiors. This requires the computation of precise and accurate theoretical frequencies, but imperfect modeling of the uppermost stellar layers introduces systematic errors. To overcome this problem, an empirical correction has been introduced by Kjeldsen et al. (2008, ApJ, 683, L175) and is now commonly used for seismic inferences. Nevertheless, we still lack a physical justification allowing for the quantification of the surface-effect corrections. Aims: Our aim is to constrain the surface-effect corrections across the Hertzsprung-Russell (HR) diagram using a set of 3D hydrodynamical simulations. Methods: We used a grid of these simulations computed with the CO5BOLD code to model the outer layers of solar-like stars. Upper layers of the corresponding 1D standard models were then replaced by the layers obtained from the horizontally averaged 3D models. The frequency differences between these patched models and the 1D standard models were then calculated using the adiabatic approximation and allowed us to constrain the Kjeldsen et al. power law, as well as a Lorentzian formulation. Results: We find that the surface effects on modal frequencies depend significantly on both the effective temperature and the surface gravity. We further provide the variation in the parameters related to the surface-effect corrections using their power law as well as a Lorentzian formulation. Scaling relations between these parameters and the elevation (related to the Mach number) is also provided. The Lorentzian formulation is shown to be more robust for the whole frequency spectrum, while the power law is not suitable for the frequency shifts in the frequency range above νmax. Finally, we show that, owing to turbulent pressure, the elevation of the uppermost layers modifies the location of the hydrogen ionization zone and

  18. On the accuracy of surface hopping dynamics in condensed phase non-adiabatic problems

    NASA Astrophysics Data System (ADS)

    Chen, Hsing-Ta; Reichman, David R.

    2016-03-01

    We perform extensive benchmark comparisons of surface hopping dynamics with numerically exact calculations for the spin-boson model over a wide range of energetic and coupling parameters as well as temperature. We find that deviations from golden-rule scaling in the Marcus regime are generally small and depend sensitively on the energetic bias between electronic states. Fewest switches surface hopping (FSSH) is found to be surprisingly accurate over a large swath of parameter space. The inclusion of decoherence corrections via the augmented FSSH algorithm improves the accuracy of dynamical behavior compared to exact simulations, but the effects are generally not dramatic, at least for the case of an environment modeled with the commonly used Debye spectral density.

  19. Analysis of Potential Energy Surfaces.

    ERIC Educational Resources Information Center

    Fernandez, G. M.; And Others

    1988-01-01

    Introduces different methodological strategies in analyzing potential energy surfaces (PES) used in chemical reactivity studies. Discusses the theory of PES and gives examples to be used for student work. Provides procedures for calculating normal coordinates and vibrational properties of an activated complex. (ML)

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

    PubMed

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

    2016-03-05

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  2. Corrected body surface potential mapping.

    PubMed

    Krenzke, Gerhard; Kindt, Carsten; Hetzer, Roland

    2007-02-01

    In the method for body surface potential mapping described here, the influence of thorax shape on measured ECG values is corrected. The distances of the ECG electrodes from the electrical heart midpoint are determined using a special device for ECG recording. These distances are used to correct the ECG values as if they had been measured on the surface of a sphere with a radius of 10 cm with its midpoint localized at the electrical heart midpoint. The equipotential lines of the electrical heart field are represented on the virtual surface of such a sphere. It is demonstrated that the character of a dipole field is better represented if the influence of the thorax shape is reduced. The site of the virtual reference electrode is also important for the dipole character of the representation of the electrical heart field.

  3. On Adiabatic Pair Creation

    NASA Astrophysics Data System (ADS)

    Pickl, Peter; Dürr, Detlef

    2008-08-01

    We give here a rigorous proof of the well known prediction of pair creation as it arises from the Dirac equation with an external time dependent potential. Pair creation happens with probability one if the potential changes adiabatically in time and becomes overcritical, which means that an eigenvalue curve (as a function of time) bridges the gap between the negative and positive spectral continuum. The potential can be thought of as being zero at large negative and large positive times. The rigorous treatment of this effect has been lacking since the pioneering work of Beck, Steinwedel and Süßmann [1] in 1963 and Gershtein and Zeldovich [8] in 1970.

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

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

  6. Potential energy surface of cyclooctatetraene

    NASA Astrophysics Data System (ADS)

    Andrés, José L.; Castaño, Obis; Morreale, Antonio; Palmeiro, Raul; Gomperts, Roberto

    1998-01-01

    We present a theoretical study of the cyclooctatetraene (COT) molecule. Seven COT structures are located on the singlet ground state potential energy surface. Four of them, which present D2d (tub), Cs (bicyclo[4.2.0]octa-2,4,7-triene or BOT), C2h (chair) and D4 (crown) symmetries are stable species, and the other three are transition state structures showing Cs, D4h, and D8h symmetry. We discuss the symmetry of wave functions for these stationary points. Geometries, energies, and harmonic vibrational frequencies of these structures, and energy gaps between singlet-triplet states and low-lying singlets are presented. For the planar D4h and D8h structures, Jahn-Teller and tunneling effects have also been discussed. Ring inversion, bond shifting and valence isomerization reactive channels from the tub COT conformer are discussed from the point of view of the corresponding transition state structures. Where possible, in order to lend support to this theoretical information comparisons with recent transition state spectroscopy data are made.

  7. Optimizing Adiabaticity in NMR

    NASA Astrophysics Data System (ADS)

    Vandermause, Jonathan; Ramanathan, Chandrasekhar

    We demonstrate the utility of Berry's superadiabatic formalism for numerically finding control sequences that implement quasi-adiabatic unitary transformations. Using an iterative interaction picture, we design a shortcut to adiabaticity that reduces the time required to perform an adiabatic inversion pulse in liquid state NMR. We also show that it is possible to extend our scheme to two or more qubits to find adiabatic quantum transformations that are allowed by the control algebra, and demonstrate a two-qubit entangling operation in liquid state NMR. We examine the pulse lengths at which the fidelity of these adiabatic transitions break down and compare with the quantum speed limit.

  8. Theoretical studies of the potential surface for the F + H2 - HF + H reaction

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W., Jr.; Walch, Stephen P.; Langhoff, Stephen R.; Taylor, Peter R.; Jaffe, Richard L.

    1988-01-01

    Several aspects of the F + H2 - HF + H potential energy hypersurface are considered. The classical barrier height is studied as a function of improvements to both the one-particle and n-particle treatments, approaching the one-particle basis set limit. The externally contracted CI (CCI) method is used to compute bending potentials in the collinear saddle point region. The calculated CCI surface is used to locate the bottleneck on the vibrationally adiabatic potential curve, and the reaction threshold is deduced from a one-dimensinal tunneling calculation. The true classical barrier height is estimated by adjusting the CCI barrier height for the difference in the calculated and experimental thresholds.

  9. 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.

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

    NASA Technical Reports Server (NTRS)

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

    1984-01-01

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

  11. Accurate ab initio determination of the adiabatic potential energy function and the Born-Oppenheimer breakdown corrections for the electronic ground state of LiH isotopologues

    NASA Astrophysics Data System (ADS)

    Holka, Filip; Szalay, Péter G.; Fremont, Julien; Rey, Michael; Peterson, Kirk A.; Tyuterev, Vladimir G.

    2011-03-01

    High level ab initio potential energy functions have been constructed for LiH in order to predict vibrational levels up to dissociation. After careful tests of the parameters of the calculation, the final adiabatic potential energy function has been composed from: (a) an ab initio nonrelativistic potential obtained at the multireference configuration interaction with singles and doubles level including a size-extensivity correction and quintuple-sextuple ζ extrapolations of the basis, (b) a mass-velocity-Darwin relativistic correction, and (c) a diagonal Born-Oppenheimer (BO) correction. Finally, nonadiabatic effects have also been considered by including a nonadiabatic correction to the kinetic energy operator of the nuclei. This correction is calculated from nonadiabatic matrix elements between the ground and excited electronic states. The calculated vibrational levels have been compared with those obtained from the experimental data [J. A. Coxon and C. S. Dickinson, J. Chem. Phys. 134, 9378 (2004)]. It was found that the calculated BO potential results in vibrational levels which have root mean square (rms) deviations of about 6-7 cm-1 for LiH and ˜3 cm-1 for LiD. With all the above mentioned corrections accounted for, the rms deviation falls down to ˜1 cm-1. These results represent a drastic improvement over previous theoretical predictions of vibrational levels for all isotopologues of LiH.

  12. Accurate ab initio determination of the adiabatic potential energy function and the Born-Oppenheimer breakdown corrections for the electronic ground state of LiH isotopologues.

    PubMed

    Holka, Filip; Szalay, Péter G; Fremont, Julien; Rey, Michael; Peterson, Kirk A; Tyuterev, Vladimir G

    2011-03-07

    High level ab initio potential energy functions have been constructed for LiH in order to predict vibrational levels up to dissociation. After careful tests of the parameters of the calculation, the final adiabatic potential energy function has been composed from: (a) an ab initio nonrelativistic potential obtained at the multireference configuration interaction with singles and doubles level including a size-extensivity correction and quintuple-sextuple ζ extrapolations of the basis, (b) a mass-velocity-Darwin relativistic correction, and (c) a diagonal Born-Oppenheimer (BO) correction. Finally, nonadiabatic effects have also been considered by including a nonadiabatic correction to the kinetic energy operator of the nuclei. This correction is calculated from nonadiabatic matrix elements between the ground and excited electronic states. The calculated vibrational levels have been compared with those obtained from the experimental data [J. A. Coxon and C. S. Dickinson, J. Chem. Phys. 134, 9378 (2004)]. It was found that the calculated BO potential results in vibrational levels which have root mean square (rms) deviations of about 6-7 cm(-1) for LiH and ∼3 cm(-1) for LiD. With all the above mentioned corrections accounted for, the rms deviation falls down to ∼1 cm(-1). These results represent a drastic improvement over previous theoretical predictions of vibrational levels for all isotopologues of LiH.

  13. Sudden transition from a stable to an unstable harmonic trap as the adiabatic potential parameter is varied in a time-periodic harmonic trap

    NASA Astrophysics Data System (ADS)

    Moiseyev, Nimrod

    2013-09-01

    It has been shown already that when the harmonic trap is opened (or closed) as a function of time while keeping the adiabatic parameter μ=[dω(t)/dt]/ω2(t) fixed, a sharp transition from an oscillatory to a monotonic exponential dynamics occurs at μ=2 [Uzdin, Dalla Torre, Kosloff, and Moiseyev, Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.88.022505 88, 022505 (2013)]. Here we show that by using time-dependent linear coordinate transformation the time-dependent Schrödinger equation with Hermitian time-dependent Hamiltonian is transformed into a time-dependent Schrödinger equation with a time-independent harmonic oscillator with the dimensionless frequency of 1-(μ/2)2. At μ=2 a transition to a non-Hermitian Hamiltonian is obtained as the potential well is transformed to a parabolic potential barrier. While in a harmonic trap noninteracting particles have classical periodic motions, they are pushed apart exponentially in time as the potential well is suddenly transformed into a parabolic potential barrier in the new variable representation.

  14. 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.

  15. Non-adiabatic dynamics of molecules in optical cavities

    SciTech Connect

    Kowalewski, Markus Bennett, Kochise; Mukamel, Shaul

    2016-02-07

    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.

  16. Adiabatic Pseudospectral Technique: Applications to Four Atom Molecules

    NASA Astrophysics Data System (ADS)

    Antikainen, Jyrki Tapio

    1995-01-01

    After the introduction, in chapter 2 we review some of the well established techniques used to solve the Schrodinger equation. The following methods are discussed: the Finite Basis Representation, the Discrete Variable Representation, the Basic Light basis set truncation, and the Lanczos tridiagonalization. After reviewing the previous techniques we present the main features of our Adiabatic Pseudospectral (APS) technique. The Adiabatic Pseudospectral technique is a synthesis of several powerful computational methods such as the sequential adiabatic basis set reduction, the iterative Lanczos diagonalization, the collocation techniques, and a careful implementation of the matrix -vector product for the Hamiltonian in the reduced adiabatic representation. In chapter 3 we use our adiabatic pseudospectral method (APS) to calculate energy levels of the H _2O_2 molecule up to 5000 cm ^{-1}. Reasonably high accuracy (a few wavenumbers) is achieved for a fully six dimensional calculation in a few hours of CPU time on an IBM 580 workstation. These results are a great improvement over previous calculations on the same system which required 50-100 times more computational effort for a similar level of accuracy. The method presented here is both general and robust. It will allow for routine studies of six dimensional potential surfaces and the associated spectroscopy, while making calculations on still larger systems feasible. In chapter 4 the adiabatic pseudospectral method is used to study the high energy vibrational levels of the H_2C_2 molecule. We calculate stimulated emission pumping spectra initialized by the excited electronic state vibrational trans-bent state ~ A_sp{u}{1 }3_{nu}_3 . The calculations show that with the APS-method we can easily investigate energy regions in the excess of 15,000 cm^{-1}; these high energy regions have been previously unattainable by computational techniques.

  17. Techniques for Measuring Surface Potentials in Space

    NASA Technical Reports Server (NTRS)

    Minow, Joseph I.; Parker, Linda Neergaard

    2015-01-01

    Materials exposed to the space plasma environment charge to a net potential relative to the ambient plasma. The charging process is due to differential currents to the material surface that results in a net surface charge density. While this process is termed "spacecraft surface charging" when applied to aerospace hardware, it also applies to the surfaces of astronomical objects in direct contact with the space plasma environment including a number of planetary bodies, asteroids, and dust particles. The ability to measure surface potentials is important to many techniques used in conducting fundamental heliospheric science, spacecraft engineering operations, and space technology development activities. This presentation provides a survey of current technologies used to measure surface potentials of spacecraft and planetary bodies with examples of their application to space science and technology programs.

  18. Jahn-Teller effect for short-lived states: Study of the complex potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Feuerbacher, Sven; Cederbaum, Lorenz S.

    2004-07-01

    The Jahn-Teller effect for bound electronic states has been investigated for many decades. In contrast, nothing is known regarding its occurrence for short-lived electronic states. Here we investigate the linear and the quadratic E⊗e Jahn-Teller effect for degenerate resonance states with special regard to the complex potential energy surfaces. We find many new phenomena for both the real and imaginary parts of the potential energy surfaces including additional minima and intersections. Possible simplifications of the equations describing the adiabatic potential energy surfaces are discussed. We also briefly investigate other Jahn-Teller effects in linear approximation. The theoretical concepts are exemplified by calculating ab initio data for the degenerate Π*-type resonance states of the tris(boramethyl)amin anion along two different doubly degenerate vibrational modes.

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

    PubMed

    Gelb, Lev D; Chakraborty, Somendra Nath

    2011-12-14

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

  20. Scanning Surface Potential Microscopy of Spore Adhesion on Surfaces

    SciTech Connect

    Lee, Ida; Chung, Eunhyea; Kweon, Hyojin; Yiacoumi, Sotira; Tsouris, Costas

    2012-01-01

    The adhesion of spores of Bacillus anthracis - the cause of anthrax and a likely biological threat - to solid surfaces is an important consideration in cleanup after an accidental or deliberate release. However, because of safety concerns, directly studying B. anthracis spores with advanced instrumentation is problematic. As a first step, we are examining the electrostatic potential of Bacillus thuringiensis (Bt), which is a closely related species that is often used as a simulant to study B. anthracis. Scanning surface potential microscopy (SSPM), also known as Kelvin probe force microscopy (KPFM), was used to investigate the influence of relative humidity (RH) on the surface electrostatic potential of Bt that had adhered to silica, mica, or gold substrates. AFM/SSPM side-by-side images were obtained separately in air, at various values of RH, after an aqueous droplet with spores was applied on each surface and allowed to dry before measurements. In the SSPM images, a negative potential on the surface of the spores was observed compared with that of the substrates. The surface potential decreased as the humidity increased. Spores were unable to adhere to a surface with an extremely negative potential, such as mica.

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

    PubMed

    Delgado, Juan C; Selsby, Ronald G

    2013-01-01

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

  2. Adiabatic molecular-dynamics-simulation-method studies of kinetic friction

    NASA Astrophysics Data System (ADS)

    Zhang, J.; Sokoloff, J. B.

    2005-06-01

    An adiabatic molecular-dynamics method is developed and used to study the Muser-Robbins model for dry friction (i.e., nonzero kinetic friction in the slow sliding speed limit). In this model, dry friction between two crystalline surfaces rotated with respect to each other is due to mobile molecules (i.e., dirt particles) adsorbed at the interface. Our adiabatic method allows us to quickly locate interface potential-well minima, which become unstable during sliding of the surfaces. Since dissipation due to friction in the slow sliding speed limit results from mobile molecules dropping out of such unstable wells, our method provides a way to calculate dry friction, which agrees extremely well with results found by conventional molecular dynamics for the same system, but our method is more than a factor of 10 faster.

  3. 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.

  4. Adiabatic states derived from a spin-coupled diabatic transformation: semiclassical trajectory study of photodissociation of HBr and the construction of potential curves for LiBr+.

    PubMed

    Valero, Rosendo; Truhlar, Donald G; Jasper, Ahren W

    2008-06-26

    The development of spin-coupled diabatic representations for theoretical semiclassical treatments of photodissociation dynamics is an important practical goal, and some of the assumptions required to carry this out may be validated by applications to simple systems. With this objective, we report here a study of the photodissociation dynamics of the prototypical HBr system using semiclassical trajectory methods. The valence (spin-free) potential energy curves and the permanent and transition dipole moments were computed using high-level ab initio methods and were transformed to a spin-coupled diabatic representation. The spin-orbit coupling used in the transformation was taken as that of atomic bromine at all internuclear distances. Adiabatic potential energy curves, nonadiabatic couplings and transition dipole moments were then obtained from the diabatic ones and were used in all the dynamics calculations. Nonadiabatic photodissociation probabilities were computed using three semiclassical trajectory methods, namely, coherent switching with decay of mixing (CSDM), fewest switches with time uncertainty (FSTU), and its recently developed variant with stochastic decoherence (FTSU/SD), each combined with semiclassical sampling of the initial vibrational state. The calculated branching fraction to the higher fine-structure level of the bromine atom is in good agreement with experiment and with more complete theoretical treatments. The present study, by comparing our new calculations to wave packet calculations with distance-dependent ab initio spin-orbit coupling, validates the semiclassical trajectory methods, the semiclassical initial state sample scheme, and the use of a distance-independent spin-orbit coupling for future applications to polyatomic photodissociation. Finally, using LiBr(+) as a model system, it is shown that accurate spin-coupled potential curves can also be constructed for odd-electron systems using the same strategy as for HBr.

  5. Computed potential energy surfaces for chemical reactions

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.; Levin, Eugene

    1993-01-01

    A new global potential energy surface (PES) is being generated for O(P-3) + H2 yields OH + H. This surface is being fit using the rotated Morse oscillator method, which was used to fit the previous POL-CI surface. The new surface is expected to be more accurate and also includes a much more complete sampling of bent geometries. A new study has been undertaken of the reaction N + O2 yields NO + O. The new studies have focused on the region of the surface near a possible minimum corresponding to the peroxy form of NOO. A large portion of the PES for this second reaction has been mapped out. Since state to state cross sections for the reaction are important in the chemistry of high temperature air, these studies will probably be extended to permit generation of a new global potential for reaction.

  6. A new approach for the development of diabatic potential energy surfaces: Hybrid block-diagonalization and diabatization by ansatz

    NASA Astrophysics Data System (ADS)

    Wittenbrink, Nils; Venghaus, Florian; Williams, David; Eisfeld, Wolfgang

    2016-11-01

    A new diabatization method is presented, which is suitable for the development of accurate high-dimensional coupled potential energy surfaces for use in quantum dynamics studies. The method is based on the simultaneous use of adiabatic wave function and energy data, respectively, and combines block-diagonalization and diabatization by ansatz approaches. It thus is called hybrid diabatization. The adiabatic wave functions of suitable ab initio calculations are projected onto a diabatic state space and the resulting vectors are orthonormalized like in standard block-diagonalization. A parametrized diabatic model Hamiltonian is set up as an ansatz for which the block-diagonalization data can be utilized to find the optimal model. Finally, the parameters are optimized with respect to the ab initio reference data such that the deviations between adiabatic energies and eigenvalues of the model as well as projected state vectors and eigenvectors of the model are minimized. This approach is particularly advantageous for problems with a complicated electronic structure where the diabatic state space must be of higher dimension than the number of calculated adiabatic states. This is an efficient way to handle problems with intruder states, which are very common for reactive systems. The use of wave function information also increases the information content for each data point without additional cost, which is beneficial in handling the undersampling problem for high-dimensional systems. The new method and its performance are demonstrated by application to three prototypical systems, ozone (O3), methyl iodide (CH3I), and propargyl (H2CCCH).

  7. 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

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

    NASA Astrophysics Data System (ADS)

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

    2008-02-01

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

  9. Interpolation of multi-sheeted multi-dimensional potential-energy surfaces via a linear optimization procedure.

    PubMed

    Opalka, Daniel; Domcke, Wolfgang

    2013-06-14

    Significant progress has been achieved in recent years with the development of high-dimensional permutationally invariant analytic Born-Oppenheimer potential-energy surfaces, making use of polynomial invariant theory. In this work, we have developed a generalization of this approach which is suitable for the construction of multi-sheeted multi-dimensional potential-energy surfaces exhibiting seams of conical intersections. The method avoids the nonlinear optimization problem which is encountered in the construction of multi-sheeted diabatic potential-energy surfaces from ab initio electronic-structure data. The key of the method is the expansion of the coefficients of the characteristic polynomial in polynomials which are invariant with respect to the point group of the molecule or the permutation group of like atoms. The multi-sheeted adiabatic potential-energy surface is obtained from the Frobenius companion matrix which contains the fitted coefficients. A three-sheeted nine-dimensional adiabatic potential-energy surface of the (2)T2 electronic ground state of the methane cation has been constructed as an example of the application of this method.

  10. Quantum adiabatic machine learning

    NASA Astrophysics Data System (ADS)

    Pudenz, Kristen L.; Lidar, Daniel A.

    2013-05-01

    We develop an approach to machine learning and anomaly detection via quantum adiabatic evolution. This approach consists of two quantum phases, with some amount of classical preprocessing to set up the quantum problems. In the training phase we identify an optimal set of weak classifiers, to form a single strong classifier. In the testing phase we adiabatically evolve one or more strong classifiers on a superposition of inputs in order to find certain anomalous elements in the classification space. Both the training and testing phases are executed via quantum adiabatic evolution. All quantum processing is strictly limited to two-qubit interactions so as to ensure physical feasibility. We apply and illustrate this approach in detail to the problem of software verification and validation, with a specific example of the learning phase applied to a problem of interest in flight control systems. Beyond this example, the algorithm can be used to attack a broad class of anomaly detection problems.

  11. Effect of RANS-Type Turbulence Models on Adiabatic Film Cooling Effectiveness over a Scaled Up Gas Turbine Blade Leading Edge Surface

    NASA Astrophysics Data System (ADS)

    Yepuri, Giridhara Babu; Talanki Puttarangasetty, Ashok Babu; Kolke, Deepak Kumar; Jesuraj, Felix

    2016-06-01

    Increasing the gas turbine inlet temperature is one of the key technologies in raising gas turbine engine power output. Film cooling is one of the efficient cooling techniques to cool the hot section components of a gas turbine engines in turn the turbine inlet temperature can be increased. This study aims at investigating the effect of RANS-type turbulence models on adiabatic film cooling effectiveness over a scaled up gas turbine blade leading edge surfaces. For the evaluation, five different two equation RANS-type turbulent models have been taken in consideration, which are available in the ANSYS-Fluent. For this analysis, the gas turbine blade leading edge configuration is generated using Solid Works. The meshing is done using ANSYS-Workbench Mesh and ANSYS-Fluent is used as a solver to solve the flow field. The considered gas turbine blade leading edge model is having five rows of film cooling circular holes, one at stagnation line and the two each on either side of stagnation line at 30° and 60° respectively. Each row has the five holes with the hole diameter of 4 mm, pitch of 21 mm arranged in staggered manner and has the hole injection angle of 30° in span wise direction. The experiments are carried in a subsonic cascade tunnel facility at heat transfer lab of CSIR-National Aerospace Laboratory with a Reynolds number of 1,00,000 based on leading edge diameter. From the Computational Fluid Dynamics (CFD) evaluation it is found that K-ɛ Realizable model gives more acceptable results with the experimental values, compared to the other considered turbulence models for this type of geometries. Further the CFD evaluated results, using K-ɛ Realizable model at different blowing ratios are compared with the experimental results.

  12. Theory of Adiabatic Fountain Resonance

    NASA Astrophysics Data System (ADS)

    Williams, Gary A.

    2017-01-01

    The theory of "Adiabatic Fountain Resonance" with superfluid ^4{He} is clarified. In this geometry a film region between two silicon wafers bonded at their outer edge opens up to a central region with a free surface. We find that the resonance in this system is not a Helmholtz resonance as claimed by Gasparini et al., but in fact is a fourth sound resonance. We postulate that it occurs at relatively low frequency because the thin silicon wafers flex appreciably from the pressure oscillations of the sound wave.

  13. Adiabatic capture and debunching

    SciTech Connect

    Ng, K.Y.; /Fermilab

    2012-03-01

    In the study of beam preparation for the g-2 experiment, adiabatic debunching and adiabatic capture are revisited. The voltage programs for these adiabbatic processes are derived and their properties discussed. Comparison is made with some other form of adiabatic capture program. The muon g-2 experiment at Fermilab calls for intense proton bunches for the creation of muons. A booster batch of 84 bunches is injected into the Recycler Ring, where it is debunched and captured into 4 intense bunches with the 2.5-MHz rf. The experiment requires short bunches with total width less than 100 ns. The transport line from the Recycler to the muon-production target has a low momentum aperture of {approx} {+-}22 MeV. Thus each of the 4 intense proton bunches required to have an emittance less than {approx} 3.46 eVs. The incoming booster bunches have total emittance {approx} 8.4 eVs, or each one with an emittance {approx} 0.1 eVs. However, there is always emittance increase when the 84 booster bunches are debunched. There will be even larger emittance increase during adiabatic capture into the buckets of the 2.5-MHz rf. In addition, the incoming booster bunches may have emittances larger than 0.1 eVs. In this article, we will concentrate on the analysis of the adiabatic capture process with the intention of preserving the beam emittance as much as possible. At this moment, beam preparation experiment is being performed at the Main Injector. Since the Main Injector and the Recycler Ring have roughly the same lattice properties, we are referring to adiabatic capture in the Main Injector instead in our discussions.

  14. Adiabatic gate teleportation.

    PubMed

    Bacon, Dave; Flammia, Steven T

    2009-09-18

    The difficulty in producing precisely timed and controlled quantum gates is a significant source of error in many physical implementations of quantum computers. Here we introduce a simple universal primitive, adiabatic gate teleportation, which is robust to timing errors and many control errors and maintains a constant energy gap throughout the computation above a degenerate ground state space. This construction allows for geometric robustness based upon the control of two independent qubit interactions. Further, our piecewise adiabatic evolution easily relates to the quantum circuit model, enabling the use of standard methods from fault-tolerance theory for establishing thresholds.

  15. Generating shortcuts to adiabaticity in quantum and classical dynamics

    NASA Astrophysics Data System (ADS)

    Jarzynski, Christopher

    2013-10-01

    Transitionless quantum driving achieves adiabatic evolution in a hurry, using a counterdiabatic Hamiltonian to stifle nonadiabatic transitions. Here this shortcut to adiabaticity is cast in terms of a generator of adiabatic transport. This yields a classical analog of transitionless driving, and provides a strategy for constructing quantal counterdiabatic Hamiltonians. As an application of this framework, exact classical and quantal counterdiabatic terms are obtained for a particle in a box and for even-power-law potentials in one degree of freedom.

  16. Constructing polyatomic potential energy surfaces by interpolating diabatic Hamiltonian matrices with demonstration on green fluorescent protein chromophore

    SciTech Connect

    Park, Jae Woo; Rhee, Young Min

    2014-04-28

    Simulating molecular dynamics directly on quantum chemically obtained potential energy surfaces is generally time consuming. The cost becomes overwhelming especially when excited state dynamics is aimed with multiple electronic states. The interpolated potential has been suggested as a remedy for the cost issue in various simulation settings ranging from fast gas phase reactions of small molecules to relatively slow condensed phase dynamics with complex surrounding. Here, we present a scheme for interpolating multiple electronic surfaces of a relatively large molecule, with an intention of applying it to studying nonadiabatic behaviors. The scheme starts with adiabatic potential information and its diabatic transformation, both of which can be readily obtained, in principle, with quantum chemical calculations. The adiabatic energies and their derivatives on each interpolation center are combined with the derivative coupling vectors to generate the corresponding diabatic Hamiltonian and its derivatives, and they are subsequently adopted in producing a globally defined diabatic Hamiltonian function. As a demonstration, we employ the scheme to build an interpolated Hamiltonian of a relatively large chromophore, para-hydroxybenzylidene imidazolinone, in reference to its all-atom analytical surface model. We show that the interpolation is indeed reliable enough to reproduce important features of the reference surface model, such as its adiabatic energies and derivative couplings. In addition, nonadiabatic surface hopping simulations with interpolation yield population transfer dynamics that is well in accord with the result generated with the reference analytic surface. With these, we conclude by suggesting that the interpolation of diabatic Hamiltonians will be applicable for studying nonadiabatic behaviors of sizeable molecules.

  17. Constructing polyatomic potential energy surfaces by interpolating diabatic Hamiltonian matrices with demonstration on green fluorescent protein chromophore

    NASA Astrophysics Data System (ADS)

    Park, Jae Woo; Rhee, Young Min

    2014-04-01

    Simulating molecular dynamics directly on quantum chemically obtained potential energy surfaces is generally time consuming. The cost becomes overwhelming especially when excited state dynamics is aimed with multiple electronic states. The interpolated potential has been suggested as a remedy for the cost issue in various simulation settings ranging from fast gas phase reactions of small molecules to relatively slow condensed phase dynamics with complex surrounding. Here, we present a scheme for interpolating multiple electronic surfaces of a relatively large molecule, with an intention of applying it to studying nonadiabatic behaviors. The scheme starts with adiabatic potential information and its diabatic transformation, both of which can be readily obtained, in principle, with quantum chemical calculations. The adiabatic energies and their derivatives on each interpolation center are combined with the derivative coupling vectors to generate the corresponding diabatic Hamiltonian and its derivatives, and they are subsequently adopted in producing a globally defined diabatic Hamiltonian function. As a demonstration, we employ the scheme to build an interpolated Hamiltonian of a relatively large chromophore, para-hydroxybenzylidene imidazolinone, in reference to its all-atom analytical surface model. We show that the interpolation is indeed reliable enough to reproduce important features of the reference surface model, such as its adiabatic energies and derivative couplings. In addition, nonadiabatic surface hopping simulations with interpolation yield population transfer dynamics that is well in accord with the result generated with the reference analytic surface. With these, we conclude by suggesting that the interpolation of diabatic Hamiltonians will be applicable for studying nonadiabatic behaviors of sizeable molecules.

  18. 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.

  19. Potential energy surfaces for cluster emitting nuclei

    SciTech Connect

    Poenaru, Dorin N.; Gherghescu, Radu A.; Greiner, Walter

    2006-01-15

    Potential energy surfaces are calculated by use of the most advanced asymmetric two-center shell model that allows us to obtain shell-and-pairing corrections that are added to the Yukawa-plus-exponential model deformation energy. Shell effects are of crucial importance for the experimental observation of spontaneous disintegration by heavy-ion emission. Results for {sup 222}Ra, {sup 232}U, {sup 236}Pu, and {sup 242}Cm illustrate the main ideas and show for the first time, for a cluster emitter, a potential barrier obtained by use of the macroscopic-microscopic method.

  20. Computed potential energy surfaces for chemical reactions

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.

    1994-01-01

    Quantum mechanical methods have been used to compute potential energy surfaces for chemical reactions. The reactions studied were among those believed to be important to the NASP and HSR programs and included the recombination of two H atoms with several different third bodies; the reactions in the thermal Zeldovich mechanism; the reactions of H atom with O2, N2, and NO; reactions involved in the thermal De-NO(x) process; and the reaction of CH(squared Pi) with N2 (leading to 'prompt NO'). These potential energy surfaces have been used to compute reaction rate constants and rates of unimolecular decomposition. An additional application was the calculation of transport properties of gases using a semiclassical approximation (and in the case of interactions involving hydrogen inclusion of quantum mechanical effects).

  1. Computed potential energy surfaces for chemical reactions

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.

    1990-01-01

    The objective was to obtain accurate potential energy surfaces (PES's) for a number of reactions which are important in the H/N/O combustion process. The interest in this is centered around the design of the SCRAM jet engine for the National Aerospace Plane (NASP), which was envisioned as an air-breathing hydrogen-burning vehicle capable of reaching velocities as large as Mach 25. Preliminary studies indicated that the supersonic flow in the combustor region of the scram jet engine required accurate reaction rate data for reactions in the H/N/O system, some of which was not readily available from experiment. The most important class of combustion reactions from the standpoint of the NASP project are radical recombinaton reactions, since these reactions result in most of the heat release in the combustion process. Theoretical characterizations of the potential energy surfaces for these reactions are presented and discussed.

  2. Assessment of total efficiency in adiabatic engines

    NASA Astrophysics Data System (ADS)

    Mitianiec, W.

    2016-09-01

    The paper presents influence of ceramic coating in all surfaces of the combustion chamber of SI four-stroke engine on working parameters mainly on heat balance and total efficiency. Three cases of engine were considered: standard without ceramic coating, fully adiabatic combustion chamber and engine with different thickness of ceramic coating. Consideration of adiabatic or semi-adiabatic engine was connected with mathematical modelling of heat transfer from the cylinder gas to the cooling medium. This model takes into account changeable convection coefficient based on the experimental formulas of Woschni, heat conductivity of multi-layer walls and also small effect of radiation in SI engines. The simulation model was elaborated with full heat transfer to the cooling medium and unsteady gas flow in the engine intake and exhaust systems. The computer program taking into account 0D model of engine processes in the cylinder and 1D model of gas flow was elaborated for determination of many basic engine thermodynamic parameters for Suzuki DR-Z400S 400 cc SI engine. The paper presents calculation results of influence of the ceramic coating thickness on indicated pressure, specific fuel consumption, cooling and exhaust heat losses. Next it were presented comparisons of effective power, heat losses in the cooling and exhaust systems, total efficiency in function of engine rotational speed and also comparison of temperature inside the cylinder for standard, semi-adiabatic and full adiabatic engine. On the basis of the achieved results it was found higher total efficiency of adiabatic engines at 2500 rpm from 27% for standard engine to 37% for full adiabatic engine.

  3. Conical intersections and diabatic potential energy surfaces for the three lowest electronic singlet states of H3 (+).

    PubMed

    Mukherjee, Saikat; Mukhopadhyay, Debasis; Adhikari, Satrajit

    2014-11-28

    We calculate the adiabatic Potential Energy Surfaces (PESs) and the Non-Adiabatic Coupling Terms (NACTs) for the three lowest singlet states of H3 (+) in hyperspherical coordinates as functions of hyperangles (θ and ϕ) for a grid of fixed values of hyperradius (1.5 ⩽ ρ ⩽ 20 bohrs) using the MRCI level of methodology employing ab initio quantum chemistry package (MOLPRO). The NACT between the ground and the first excited state translates along the seams on the θ - ϕ space, i.e., there are six Conical Intersections (CIs) at each θ (60° ⩽ θ ⩽ 90°) within the domain, 0 ⩽ ϕ ⩽ 2π. While transforming the adiabatic PESs to the diabatic ones, such surfaces show up six crossings along those seams. Our beyond Born-Oppenheimer approach could incorporate the effect of NACTs accurately and construct single-valued, continuous, smooth, and symmetric diabatic PESs. Since the location of CIs and the spatial amplitudes of NACTs are most prominent around ρ = 10 bohrs, generally only those results are depicted.

  4. An interacting adiabatic quantum motor

    NASA Astrophysics Data System (ADS)

    Viola Kusminskiy, Silvia; Bruch, Anton; von Oppen, Felix

    We consider the effect of electron-electron interactions on the performance of an adiabatic quantum motor based on a Thouless pump operating in reverse. We model such a device by electrons in a 1d wire coupled to a slowly moving periodic potential associated with the classical mechanical degree of freedom of the motor. This periodic degree of freedom is set into motion by a bias voltage applied to the 1d electron channel. We investigate the Thouless motor with interacting leads modeled as Luttinger liquids. We show that interactions enhance the energy gap opened by the periodic potential and thus the robustness of the Thouless motor against variations in the chemical potential. We show that the motor degree of freedom can be described as a mobile impurity in a Luttinger liquid obeying Langevin dynamics with renormalized coefficients due to interactions, for which we give explicit expressions.

  5. Semiconductor adiabatic qubits

    DOEpatents

    Carroll, Malcolm S.; Witzel, Wayne; Jacobson, Noah Tobias; Ganti, Anand; Landahl, Andrew J.; Lilly, Michael; Nguyen, Khoi Thi; Bishop, Nathaniel; Carr, Stephen M.; Bussmann, Ezra; Nielsen, Erik; Levy, James Ewers; Blume-Kohout, Robin J.; Rahman, Rajib

    2016-12-27

    A quantum computing device that includes a plurality of semiconductor adiabatic qubits is described herein. The qubits are programmed with local biases and coupling terms between qubits that represent a problem of interest. The qubits are initialized by way of a tuneable parameter, a local tunnel coupling within each qubit, such that the qubits remain in a ground energy state, and that initial state is represented by the qubits being in a superposition of |0> and |1> states. The parameter is altered over time adiabatically or such that relaxation mechanisms maintain a large fraction of ground state occupation through decreasing the tunnel coupling barrier within each qubit with the appropriate schedule. The final state when tunnel coupling is effectively zero represents the solution state to the problem represented in the |0> and |1> basis, which can be accurately read at each qubit location.

  6. Theoretical studies of potential energy surfaces

    SciTech Connect

    Harding, L.B.

    1993-12-01

    The goal of this program is to calculate accurate potential energy surfaces (PES) for both reactive and nonreactive systems. To do this the electronic Schrodinger equation must be solved. Our approach to this problem starts with multiconfiguration self-consistent field (MCSCF) reference wavefunctions. These reference wavefunctions are designed to be sufficiently flexible to accurately describe changes in electronic structure over a broad range of geometries. Electron correlation effects are included via multireference, singles and doubles configuration interaction (MRSDCI) calculations. With this approach, the authors are able to provide useful predictions of the energetics for a broad range of systems.

  7. Energy decomposition analysis in an adiabatic picture.

    PubMed

    Mao, Yuezhi; Horn, Paul R; Head-Gordon, Martin

    2017-02-22

    Energy decomposition analysis (EDA) of electronic structure calculations has facilitated quantitative understanding of diverse intermolecular interactions. Nevertheless, such analyses are usually performed at a single geometry and thus decompose a "single-point" interaction energy. As a result, the influence of the physically meaningful EDA components on the molecular structure and other properties are not directly obtained. To address this gap, the absolutely localized molecular orbital (ALMO)-EDA is reformulated in an adiabatic picture, where the frozen, polarization, and charge transfer energy contributions are defined as energy differences between the stationary points on different potential energy surfaces (PESs), which are accessed by geometry optimizations at the frozen, polarized and fully relaxed levels of density functional theory (DFT). Other molecular properties such as vibrational frequencies can thus be obtained at the stationary points on each PES. We apply the adiabatic ALMO-EDA to different configurations of the water dimer, the water-Cl(-) and water-Mg(2+)/Ca(2+) complexes, metallocenes (Fe(2+), Ni(2+), Cu(2+), Zn(2+)), and the ammonia-borane complex. This method appears to be very useful for unraveling how physical effects such as polarization and charge transfer modulate changes in molecular properties induced by intermolecular interactions. As an example of the insight obtained, we find that a linear hydrogen bond geometry for the water dimer is preferred even without the presence of polarization and charge transfer, while the red shift in the OH stretch frequency is primarily a charge transfer effect; by contrast, a near-linear geometry for the water-chloride hydrogen bond is achieved only when charge transfer is allowed.

  8. Mechanical Surface Waves Accompany Action Potential Propagation

    NASA Astrophysics Data System (ADS)

    Machta, Benjamin; El Hady, Ahmed

    2015-03-01

    The action potential (AP) is the basic mechanism by which information is transmitted along neuronal axons. Although the excitable nature of axons is understood to be primarily electrical, many experimental studies have shown that a mechanical displacement of the axonal membrane co-propagates with the electrical signal. While the experimental evidence for co-propagating mechanical waves is diverse and compelling, there is no consensus for their physical underpinnings. We present a model in which these mechanical displacements arise from the driving of mechanical surface waves, in which potential energy is stored in elastic deformations of the neuronal membrane and cytoskeleton while kinetic energy is stored in the movement of the axoplasmic fluid. In our model these surface waves are driven by the traveling wave of electrical depolarization that characterizes the AP, altering the electrostatic forces across the membrane as it passes. Our model allows us to predict the shape of the displacement that should accompany any traveling wave of voltage, including the well-characterized AP. We expect our model to serve as a framework for understanding the physical origins and possible functional roles of these AWs in neurobiology. See Arxiv/1407.7600

  9. Potential energy surfaces of superheavy nuclei

    SciTech Connect

    Bender, M.; Rutz, K.; Maruhn, J.A.; Greiner, W.; Reinhard, P.-G. Rutz, K.; Maruhn, J.A.; Greiner, W.

    1998-10-01

    We investigate the structure of the potential energy surfaces of the superheavy nuclei {sub 158}{sup 258}Fm{sub 100}, {sub 156}{sup 264}Hs{sub 108}, {sub 166}{sup 278}112, {sub 184}{sup 298}114, and {sub 172}{sup 292}120 within the framework of self-consistent nuclear models, i.e., the Skyrme-Hartree-Fock approach and the relativistic mean-field model. We compare results obtained with one representative parametrization of each model which is successful in describing superheavy nuclei. We find systematic changes as compared to the potential energy surfaces of heavy nuclei in the uranium region: there is no sufficiently stable fission isomer any more, the importance of triaxial configurations to lower the first barrier fades away, and asymmetric fission paths compete down to rather small deformation. Comparing the two models, it turns out that the relativistic mean-field model gives generally smaller fission barriers. {copyright} {ital 1998} {ital The American Physical Society}

  10. Diabatic-At-Construction Method for Diabatic and Adiabatic Ground and Excited States Based on Multistate Density Functional Theory.

    PubMed

    Grofe, Adam; Qu, Zexing; Truhlar, Donald G; Li, Hui; Gao, Jiali

    2017-03-14

    We describe a diabatic-at-construction (DAC) strategy for defining diabatic states to determine the adiabatic ground and excited electronic states and their potential energy surfaces using the multistate density functional theory (MSDFT). The DAC approach differs in two fundamental ways from the adiabatic-to-diabatic (ATD) procedures that transform a set of preselected adiabatic electronic states to a new representation. (1) The DAC states are defined in the first computation step to form an active space, whose configuration interaction produces the adiabatic ground and excited states in the second step of MSDFT. Thus, they do not result from a similarity transformation of the adiabatic states as in the ATD procedure; they are the basis for producing the adiabatic states. The appropriateness and completeness of the DAC active space can be validated by comparison with experimental observables of the ground and excited states. (2) The DAC diabatic states are defined using the valence bond characters of the asymptotic dissociation limits of the adiabatic states of interest, and they are strictly maintained at all molecular geometries. Consequently, DAC diabatic states have specific and well-defined physical and chemical meanings that can be used for understanding the nature of the adiabatic states and their energetic components. Here we present results for the four lowest singlet states of LiH and compare them to a well-tested ATD diabatization method, namely the 3-fold way; the comparison reveals both similarities and differences between the ATD diabatic states and the orthogonalized DAC diabatic states. Furthermore, MSDFT can provide a quantitative description of the ground and excited states for LiH with multiple strongly and weakly avoided curve crossings spanning over 10 Å of interatomic separation.

  11. A finite-element visualization of quantum reactive scattering. II. Nonadiabaticity on coupled potential energy surfaces

    SciTech Connect

    Warehime, Mick; Kłos, Jacek; Alexander, Millard H.

    2015-01-21

    This is the second in a series of papers detailing a MATLAB based implementation of the finite element method applied to collinear triatomic reactions. Here, we extend our previous work to reactions on coupled potential energy surfaces. The divergence of the probability current density field associated with the two electronically adiabatic states allows us to visualize in a novel way where and how nonadiabaticity occurs. A two-dimensional investigation gives additional insight into nonadiabaticity beyond standard one-dimensional models. We study the F({sup 2}P) + HCl and F({sup 2}P) + H{sub 2} reactions as model applications. Our publicly available code (http://www2.chem.umd.edu/groups/alexander/FEM) is general and easy to use.

  12. Ab initio potential energy surface and vibration-rotation energy levels of sulfur dioxide.

    PubMed

    Koput, Jacek

    2017-05-05

    An accurate potential energy surface of sulfur dioxide, SO2 , in its ground electronic state X∼ 1A1 has been determined from ab initio calculations using the coupled-cluster approach in conjunction with the correlation-consistent basis sets up to septuple-zeta quality. The results obtained with the conventional and explicitly correlated coupled-cluster methods are compared. The role of the core-electron correlation, higher-order valence-electron correlation, scalar relativistic, and adiabatic effects in determining the structure and dynamics of the SO2 molecule is discussed. The vibration-rotation energy levels of the (32) SO2 and (34) SO2 isotopologues were predicted using a variational approach. It was shown that the inclusion of the aforementioned effects was mandatory to attain the "spectroscopic" accuracy. © 2017 Wiley Periodicals, Inc.

  13. Ab initio potential energy surface and vibration-rotation energy levels of beryllium monohydroxide.

    PubMed

    Koput, Jacek

    2017-01-05

    The accurate potential energy surface of beryllium monohydroxide, BeOH, in its ground electronic state X 2A' has been determined from ab initio calculations using the coupled-cluster approach in conjunction with the correlation-consistent core-valence basis sets up to septuple-zeta quality. The higher-order electron correlation, scalar relativistic, and adiabatic effects were taken into account. The BeOH molecule was confirmed to be bent at equilibrium, with the BeOH angle of 141.2° and the barrier to linearity of 129 cm(-1) . The vibration-rotation energy levels of the BeOH and BeOD isotopologues were predicted using a variational approach and compared with recent experimental data. The results can be useful in a further analysis of high-resolution vibration-rotation spectra of these interesting species. © 2016 Wiley Periodicals, Inc.

  14. 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.

  15. Energy conservation potential of surface modification technologies

    SciTech Connect

    Le, H.K.; Horne, D.M.; Silberglitt, R.S.

    1985-09-01

    This report assesses the energy conservation impact of surface modification technologies on the metalworking industries. The energy conservation impact of surface modification technologies on the metalworking industries is assessed by estimating their friction and wear tribological sinks and the subsequent reduction in these sinks when surface modified tools are used. Ion implantation, coatings, and laser and electron beam surface modifications are considered.

  16. Computed potential energy surfaces for chemical reactions

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.

    1988-01-01

    The minimum energy path for the addition of a hydrogen atom to N2 is characterized in CASSCF/CCI calculations using the (4s3p2d1f/3s2p1d) basis set, with additional single point calculations at the stationary points of the potential energy surface using the (5s4p3d2f/4s3p2d) basis set. These calculations represent the most extensive set of ab initio calculations completed to date, yielding a zero point corrected barrier for HN2 dissociation of approx. 8.5 kcal mol/1. The lifetime of the HN2 species is estimated from the calculated geometries and energetics using both conventional Transition State Theory and a method which utilizes an Eckart barrier to compute one dimensional quantum mechanical tunneling effects. It is concluded that the lifetime of the HN2 species is very short, greatly limiting its role in both termolecular recombination reactions and combustion processes.

  17. 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.…

  18. Vibrational dynamics of the bifluoride ion. II. Adiabatic separation and proton dynamics

    NASA Astrophysics Data System (ADS)

    Epa, V. C.; Thorson, W. R.

    1990-01-01

    Vibrational dynamics of the bifluoride ion FHF-, which exhibits strongly anharmonic and nonseparable vibrations, is studied using the extended ab initio model potential surface described in the first paper of this series. Adiabatic separation of the proton motion from the F-F (ν1) motion forms a zero-order basis for description, although strong coupling of adiabatic states by the ν1 motion is important in higher vibrational levels and must be considered to understand the spectrum. The adiabatic protonic eigenstates at F-F separations R from 3.75 to 6.40 a.u. have been determined using the self-consistent field approximation in prolate spheroidal coordinates to provide a basis set for configuration interaction expansion of the exact eigenstates. 78 SCF eigenstates (21 σg, 21 σu, 21 πu, and 15 πg) were computed by ``exact'' numerical solution of the SCF equations. The adiabatic CI eigenstates are shown to be converged in energy to better than 1.0 cm-1 for the ground state of each symmetry type and usually better than 10 cm-1 for the lowest three to five states, and pass critical tests of accuracy such as the Hellmann-Feynman theorem. The resulting CI potential energy curves closely resemble corresponding SCF energy curves and justify the concept of mode separation even in this very anharmonic system. The adiabatic CI potential energy curves explain most aspects of the dynamics relevant to the IR and Raman spectra of FHF- (e.g., in KHF2), and calculations of ν1 dynamics within the adiabatic approximation suffice to assign most of the observed IR spectrum of KHF2(s) (to about 6000 cm-1). States corresponding qualitatively to modal overtone and combination levels such as 3ν2 and (ν2+2ν3) however exhibit avoided crossings in the neighborhood of the equilibrium configuration and ``Fermi resonance'' involving interactions of two or more such adiabatic states via the ν1 motion must be treated by close-coupling to predict both frequencies and intensities in the

  19. Urban Surfaces and Heat Island Mitigation Potentials

    SciTech Connect

    Akbari, Hashem; Akbari, Hashem; Shea Rose, Leanna

    2007-06-14

    Data on materials and surface types that comprise a city, i.e. urban fabric, are needed in order to estimate the effects of light-colored surfaces (roofs and pavements) and urban vegetation (trees, grass, shrubs) on the meteorology and air quality of a city. We discuss the results of a semi-automatic statistical approach used to develop data on surface-type distribution and urban-fabric makeup using aerial color orthophotography, for four metropolitan areas of Chicago, IL, Houston, TX, Sacramento, CA, and Salt Lake City, UT. The digital high resolution (0.3 to 0.5-m) aerial photographs for each of these metropolitan areas covers representative urban areas ranging from 30 km{sup 2} to 52 km{sup 2}. Major land-use types examined included: commercial, residential, industrial, educational, and transportation. On average, for the metropolitan areas studied, vegetation covers about 29-41% of the area, roofs 19-25%, and paved surfaces 29-39%. For the most part, trees shade streets, parking lots, grass, and sidewalks. At ground level, i.e., view from below the tree canopies, vegetation covers about 20-37% of the area, roofs 20-25%, and paved surfaces 29-36%.

  20. Fast forward to the classical adiabatic invariant

    NASA Astrophysics Data System (ADS)

    Jarzynski, Christopher; Deffner, Sebastian; Patra, Ayoti; Subaşı, Yiǧit

    2017-03-01

    We show how the classical action, an adiabatic invariant, can be preserved under nonadiabatic conditions. Specifically, for a time-dependent Hamiltonian H =p2/2 m +U (q ,t ) in one degree of freedom, and for an arbitrary choice of action I0, we construct a so-called fast-forward potential energy function VFF(q ,t ) that, when added to H , guides all trajectories with initial action I0 to end with the same value of action. We use this result to construct a local dynamical invariant J (q ,p ,t ) whose value remains constant along these trajectories. We illustrate our results with numerical simulations. Finally, we sketch how our classical results may be used to design approximate quantum shortcuts to adiabaticity.

  1. Adiabatic invariance with first integrals of motion.

    PubMed

    Adib, Artur B

    2002-10-01

    The construction of a microthermodynamic formalism for isolated systems based on the concept of adiabatic invariance is an old but seldom appreciated effort in the literature, dating back at least to P. Hertz [Ann. Phys. (Leipzig) 33, 225 (1910)]. An apparently independent extension of such formalism for systems bearing additional first integrals of motion was recently proposed by Hans H. Rugh [Phys. Rev. E 64, 055101 (2001)], establishing the concept of adiabatic invariance even in such singular cases. After some remarks in connection with the formalism pioneered by Hertz, it will be suggested that such an extension can incidentally explain the success of a dynamical method for computing the entropy of classical interacting fluids, at least in some potential applications where the presence of additional first integrals cannot be ignored.

  2. A harmonic adiabatic approximation to calculate highly excited vibrational levels of ``floppy molecules''

    NASA Astrophysics Data System (ADS)

    Lauvergnat, David; Nauts, André; Justum, Yves; Chapuisat, Xavier

    2001-04-01

    The harmonic adiabatic approximation (HADA), an efficient and accurate quantum method to calculate highly excited vibrational levels of molecular systems, is presented. It is well-suited to applications to "floppy molecules" with a rather large number of atoms (N>3). A clever choice of internal coordinates naturally suggests their separation into active, slow, or large amplitude coordinates q', and inactive, fast, or small amplitude coordinates q″, which leads to an adiabatic (or Born-Oppenheimer-type) approximation (ADA), i.e., the total wave function is expressed as a product of active and inactive total wave functions. However, within the framework of the ADA, potential energy data concerning the inactive coordinates q″ are required. To reduce this need, a minimum energy domain (MED) is defined by minimizing the potential energy surface (PES) for each value of the active variables q', and a quadratic or harmonic expansion of the PES, based on the MED, is used (MED harmonic potential). In other words, the overall picture is that of a harmonic valley about the MED. In the case of only one active variable, we have a minimum energy path (MEP) and a MEP harmonic potential. The combination of the MED harmonic potential and the adiabatic approximation (harmonic adiabatic approximation: HADA) greatly reduces the size of the numerical computations, so that rather large molecules can be studied. In the present article however, the HADA is applied to our benchmark molecule HCN/CNH, to test the validity of the method. Thus, the HADA vibrational energy levels are compared and are in excellent agreement with the ADA calculations (adiabatic approximation with the full PES) of Light and Bačić [J. Chem. Phys. 87, 4008 (1987)]. Furthermore, the exact harmonic results (exact calculations without the adiabatic approximation but with the MEP harmonic potential) are compared to the exact calculations (without any sort of approximation). In addition, we compare the densities of

  3. Montgomery Potential and Wind Fields on Isentropic Surfaces from GPS Radio Occultation

    NASA Astrophysics Data System (ADS)

    Scherllin-Pirscher, Barbara; Steiner, Andrea; Kirchengast, Gottfried; Leroy, Stephen

    2015-04-01

    Atmospheric profiles from Global Positioning System (GPS) radio occultation (RO) measurements provide precise and accurate information on the thermal structure of the troposphere and lower stratosphere. Since altitude (and also geopotential height) is based on accurate knowledge of the position and velocity vectors of the transmitter and receiver satellites involved, it is possible to obtain highly resolved and accurate vertical information from RO. In this study we use observational data from 2007 to 2013 from the RO missions CHAMP, SAC-C, GRACE-A, and Formosat-3/COSMIC. Using potential temperature as the vertical coordinate we calculate monthly means of the Montgomery potential on isentropic surfaces from 300 K to 600 K (approximately 12 km to 24 km in altitude) with a horizontal resolution of 5° in latitude and 5° in longitude. Contours of the Montgomery potential on isentropic surfaces correspond to a stream-function for adiabatic, geostrophic flow. Subsequently we derive monthly mean geostrophic wind fields (outside the tropics) from sampling error-corrected fields of the Montgomery potential on isentropic surfaces. We find that these climatological RO wind fields clearly capture all of the main wind features with departures from analysis winds being, in general, smaller than 2 m s-1. Larger biases close to the subtropical jet and at high latitudes'biases rarely exceed 10 %'are caused by the geostrophic approximation. We present monthly mean wind fields, their annual cycle as well as inter-annual variability related to the El Niño-Southern Oscillation. This three-dimensional information of high quality from RO data can subsequently be utilized to investigate atmospheric dynamics close to the tropopause.

  4. Adiabatic fission barriers in superheavy nuclei

    NASA Astrophysics Data System (ADS)

    Jachimowicz, P.; Kowal, M.; Skalski, J.

    2017-01-01

    Using the microscopic-macroscopic model based on the deformed Woods-Saxon single-particle potential and the Yukawa-plus-exponential macroscopic energy, we calculated static fission barriers Bf for 1305 heavy and superheavy nuclei 98 ≤Z ≤126 , including even-even, odd-even, even-odd and odd-odd systems. For odd and odd-odd nuclei, adiabatic potential-energy surfaces were calculated by a minimization over configurations with one blocked neutron or/and proton on a level from the 10th below to the 10th above the Fermi level. The parameters of the model that have been fixed previously by a fit to masses of even-even heavy nuclei were kept unchanged. A search for saddle points has been performed by the "imaginary water flow" method on a basic five-dimensional deformation grid, including triaxiality. Two auxiliary grids were used for checking the effects of the mass asymmetry and hexadecapole nonaxiality. The ground states (g.s.) were found by energy minimization over configurations and deformations. We find that the nonaxiality significantly changes first and second fission saddle in many nuclei. The effect of the mass asymmetry, known to lower the second, very deformed saddles in actinides, in the heaviest nuclei appears at the less deformed saddles in more than 100 nuclei. It happens for those saddles in which the triaxiality does not play any role, which suggests a decoupling between effects of the mass asymmetry and triaxiality. We studied also the influence of the pairing interaction strength on the staggering of Bf for odd- and even-particle numbers. Finally, we provide a comparison of our results with other theoretical fission barrier evaluations and with available experimental estimates.

  5. 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.

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

    SciTech Connect

    Gordon, Chris; Saffin, Paul M. E-mail: Paul.Saffin@nottingham.ac.uk

    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.

  7. Use of scaled external correlation, a double many-body expansion, and variational transition state theory to calibrate a potential energy surface for FH2

    NASA Technical Reports Server (NTRS)

    Lynch, Gillian C.; Steckler, Rozeanne; Varandas, Antonio J. C.; Truhlar, Donald G.; Schwenke, David W.

    1991-01-01

    New ab initio results and a double many-body expansion formalism have been used to parameterize a new FH2 potential energy surface with improved properties near the saddle point and in the region of long-range attraction. The functional form of the new surface includes dispersion forces by a double many-body expansion. Stationary point properties for the new surface are calculated along with the product-valley barrier maxima of vibrationally adiabatic potential curves for F + H2 - HF(nu-prime = 3) + H, F + HD - HF(nu-prime = 3) + D, and F + D2 - DF(nu-prime = 4) + D. The new surface should prove useful for studying the effect on dynamics of a low, early barrier with a wide, flat bend potential.

  8. Computed potential energy surfaces for chemical reactions

    NASA Technical Reports Server (NTRS)

    Heinemann, K.; Walch, Stephen P.

    1992-01-01

    The work on the NH + NO system which was described in the last progress report was written up and a draft of the manuscript is included in the appendix. The appendix also contains a draft of a manuscript on an Ar + H + H surface. New work which was completed in the last six months includes the following: (1) calculations on the (1)CH2 + H2O, H2 + HCOH, and H2 + H2CO product channels in the CH3 + OH reaction; (2) calculations for the NH2 + O reaction; (3) calculations for the CH3 + O2 reaction; and (4) calculations for CH3O and the two decomposition channels--CH2OH and H + H2CO. Detailed descriptions of this work will be given in manuscripts; however, brief descriptions of the CH3 + OH and CH3 + O2 projects are given.

  9. A new potential energy surface for OH(A 2Σ+)-Kr: the van der Waals complex and inelastic scattering.

    PubMed

    Chadwick, H; Brouard, M; Chang, Y-P; Eyles, C J; Perkins, T; Seamons, S A; Kłos, J; Alexander, M H; Aoiz, F J

    2012-10-21

    New ab initio studies of the OH(A(2)Σ(+))-Kr system reveal significantly deeper potential energy wells than previously believed, particularly for the linear configuration in which Kr is bound to the oxygen atom side of OH(A(2)Σ(+)). In spite of this difference with previous work, bound state calculations based on a new RCCSD(T) potential energy surface yield an energy level structure in reasonable accord with previous studies. However, the new calculations suggest the need for a reassignment of the vibrational levels of the electronically excited complex. Quantum mechanical and quasi-classical trajectory scattering calculations are also performed on the new potential energy surface. New experimental measurements of rotational inelastic scattering cross sections are reported, obtained using Zeeman quantum beat spectroscopy. The values of the rotational energy transfer cross sections measured experimentally are in good agreement with those derived from the dynamical calculations on the new adiabatic potential energy surface.

  10. 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.

  11. Potential energy surfaces of Polonium isotopes

    NASA Astrophysics Data System (ADS)

    Nerlo-Pomorska, B.; Pomorski, K.; Schmitt, C.; Bartel, J.

    2015-11-01

    The evolution of the potential energy landscape is analysed in detail for ten even-even polonium isotopes in the mass range 188\\lt A\\lt 220 as obtained within the macroscopic-microscopic approach, relying on the Lublin-Strasbourg drop model and the Yukawa-folded single-particle energies for calculating the microscopic shell and pairing corrections. A variant of the modified Funny-Hills nuclear shape parametrization is used to efficiently map possible fission paths. The approach explains the main features of the fragment partition as measured in low-energy fission along the polonium chain. The latter lies in a transitional region of the nuclear chart, and will be essential to consistently understand the evolution of fission properties from neutron-deficient mercury to heavy actinides. The ability of our method to predict fission observables over such an extended region looks promising.

  12. Theoretical studies of the potential surface for the F - H2 greater than HF + H reaction

    NASA Technical Reports Server (NTRS)

    Bauschlicher, Charles W., Jr.; Walch, Stephen, P.; Langhoff, Stephen R.; Taylor, Peter R.; Jaffe, Richard L.

    1987-01-01

    The F + H2 yields HF + H potential energy hypersurface was studied in the saddle point and entrance channel regions. Using a large (5s 5p 3d 2f 1g/4s 3p 2d) atomic natural orbital basis set, a classical barrier height of 1.86 kcal/mole was obtained at the CASSCF/multireference CI level (MRCI) after correcting for basis set superposition error and including a Davidson correction (+Q) for higher excitations. Based upon an analysis of the computed results, the true classical barrier is estimated to be about 1.4 kcal/mole. The location of the bottleneck on the lowest vibrationally adiabatic potential curve was also computed and the translational energy threshold determined from a one-dimensional tunneling calculation. Using the difference between the calculated and experimental threshold to adjust the classical barrier height on the computed surface yields a classical barrier in the range of 1.0 to 1.5 kcal/mole. Combining the results of the direct estimates of the classical barrier height with the empirical values obtained from the approximation calculations of the dynamical threshold, it is predicted that the true classical barrier height is 1.4 + or - 0.4 kcal/mole. Arguments are presented in favor of including the relatively large +Q correction obtained when nine electrons are correlated at the CASSCF/MRCI level.

  13. Dynamics of the reactions of muonium and deuterium atoms with vibrationally excited hydrogen molecules: tunneling and vibrational adiabaticity.

    PubMed

    Jambrina, P G; García, E; Herrero, V J; Sáez-Rábanos, V; Aoiz, F J

    2012-11-14

    Quantum mechanical (QM) and quasiclassical trajectory (QCT) calculations have been carried out for the exchange reactions of D and Mu (Mu = muonium) with hydrogen molecules in their ground and first vibrational states. In all the cases considered, the QM rate coefficients, k(T), are in very good agreement with the available experimental results. In particular, QM calculations on the most accurate potential energy surfaces (PESs) predict a rate coefficient for the Mu + H(2) (ν = 1) reaction which is very close to the preliminary estimate of its experimental value at 300 K. In contrast to the D + H(2) (ν = 0,1) and the Mu + H(2) (ν = 0) reactions, the QCT calculations for Mu + H(2) (ν = 1) predict a much smaller k(T) than that obtained with the accurate QM method. This behaviour is indicative of tunneling. The QM reaction probabilities and total reactive cross sections show that the total energy thresholds for the reactions of Mu with H(2) in ν = 0 and ν = 1 are very similar, whereas for the corresponding reaction with D the ν = 0 total energy threshold is about 0.3 eV lower than that for ν = 1. The results just mentioned can be explained by considering the vibrational adiabatic potentials along the minimum energy path. The threshold for the reaction of Mu with H(2) in both ν = 0 and ν = 1 states is the same and is given by the height of the ground vibrational adiabatic collinear potential, whereas for the D + H(2) reaction the adiabaticity is preserved and the threshold for the reaction in ν = 1 is very close to the height of the ν = 1 adiabatic collinear barrier. For Mu + H(2) (ν = 1) the reaction takes place by crossing from the ν = 1 to the ν = 0 adiabat, since the exit channel leading to MuH (ν = 1) is not energetically accessible. At the lowest possible energies, the non-adiabatic vibrational crossing implies a strong tunneling effect through the ν = 1 adiabatic barrier. Absence of tunneling in the classical calculations results in a threshold

  14. Adiabatic channel capture theory applied to cold atom-molecule reactions: Li + CaH \\to LiH + Ca at 1K

    NASA Astrophysics Data System (ADS)

    Tscherbul, Timur V.; Buchachenko, Alexei A.

    2015-03-01

    We use quantum and classical adiabatic capture theories to study the chemical reaction Li + CaH \\to LiH + Ca. Using a recently developed ab initio potential energy surface, which provides an accurate representation of long-range interactions in the entrance reaction channel, we calculate the adiabatic channel potentials by diagonalizing the Li-CaH Hamiltonian as a function of the atom-molecule separation. The resulting adiabatic channel potentials are used to calculate both the classical and quantum capture probabilities as a function of collision energy, as well as the temperature dependencies of the partial and total reaction rates. The calculated reaction rate agrees well with the measured value at 1 K (V Singh et al 2012 Phys. Rev. Lett. 108 203201), suggesting that the title reaction proceeds without an activation barrier. The calculated classical adiabatic capture rate agrees well with the quantum result in the multiple-partial-wave regime of relevance to the experiment. Significant differences are found only in the ultracold limit (T\\lt 1 mK), demonstrating that adiabatic capture theories can predict the reaction rates with nearly quantitative accuracy in the multiple-partial-wave regime.

  15. A fast solver for the gyrokinetic field equation with adiabatic electrons

    SciTech Connect

    Borchardt, M.; Kleiber, R.; Hackbusch, W.

    2012-07-15

    Describing turbulence and microinstabilities in fusion devices is often modelled with the gyrokinetic equation. During the time evolution of the distribution function a field equation for the electrostatic potential needs to be solved. In the case of adiabatic electrons it contains a flux-surface-average term resulting in an integro-differential equation. Its numerical solution is time and memory intensive for three-dimensional configurations. Here a new algorithm is presented which only requires the numerical inversion of a simpler differential operator and a subsequent addition of a correction term. This new procedure is as fast as solving the equation without the surface average.

  16. Potential-Energy Surfaces, the Born-Oppenheimer Approximations, and the Franck-Condon Principle: Back to the Roots.

    PubMed

    Mustroph, Heinz

    2016-09-05

    The concept of a potential-energy surface (PES) is central to our understanding of spectroscopy, photochemistry, and chemical kinetics. However, the terminology used in connection with the basic approximations is variously, and somewhat confusingly, represented with such phrases as "adiabatic", "Born-Oppenheimer", or "Born-Oppenheimer adiabatic" approximation. Concerning the closely relevant and important Franck-Condon principle (FCP), the IUPAC definition differentiates between a classical and quantum mechanical formulation. Consequently, in many publications we find terms such as "Franck-Condon (excited) state", or a vertical transition to the "Franck-Condon point" with the "Franck-Condon geometry" that relaxes to the excited-state equilibrium geometry. The Born-Oppenheimer approximation and the "classical" model of the Franck-Condon principle are typical examples of misused terms and lax interpretations of the original theories. In this essay, we revisit the original publications of pioneers of the PES concept and the FCP to help stimulate a lively discussion and clearer thinking around these important concepts.

  17. The Floquet Adiabatic Theorem revisited

    NASA Astrophysics Data System (ADS)

    Weinberg, Phillip; Bukov, Marin; D'Alessio, Luca; Kolodrubetz, Michael; Davidson, Shainen; Polkovnikov, Anatoli

    2015-03-01

    The existance of the adiabatic theorem for Floquet systems has been the subject of an active debate with different articles reaching opposite conclusions over the years. In this talk we clarify the situation by deriving a systematic expansion in the time-derivatives of a slow parameter for the occupation probabilities of the Floque states. Our analysis shows that the in a certain limit the transition between Floquet eigenstates are suppressed and it is possible to define an adiabatic theorem for Floquet systems. Crucially we observe however that the conditions for adiabaticity in ordinary and Floquet systems are different and that this difference can become important when the amplitude of the periodic driving is large. We illustrate our results with specific examples of a periodically driven harmonic oscillator and cold atoms in optical lattices which are relevant in current experiments.

  18. Adiabatic losses in Stirling refrigerators

    SciTech Connect

    Bauwens, L.

    1996-06-01

    The Stirling cycle has been used very effectively in cryocoolers; but efficiencies relative to the Carnot limit are typically observed to peak for absolute temperature ratios of about two, which makes it less suitable for low-life refrigeration. The adiabatic loss appears to be responsible for poor performance at small temperature differences. In this paper, adiabatic losses are evaluated, for a temperature ratio of 2/3, taking into account the effect of phase angle between pistons, of volume ratio, of the distribution of the dead volume necessary to reduce the volume ratio, and of the distribution of displacement between expansion and compression spaces. The study is carried out numerically, using an adiabatic Stirling engine model in which cylinder flow is assumed to be stratified. Results show that the best location for the cylinder dead volume is on the compression side. Otherwise, all strategies used to trade off refrigeration for coefficient of performance are found to be roughly equivalent.

  19. Surface Potential of DPPC Monolayers on Concentrated Aqueous Salt Solutions.

    PubMed

    Casper, Clayton B; Verreault, Dominique; Adams, Ellen M; Hua, Wei; Allen, Heather C

    2016-03-03

    The presence and exchange of electrical charges on the surfaces of marine aerosols influence their ability to act as cloud condensation nuclei and play a role in thundercloud electrification. Although interactions exist between surface-active inorganic ions and organic compounds, their role in surface charging of marine aerosols is not well understood. In this study, the surface potential of dipalmitoylphosphatidylcholine (DPPC) monolayers, a zwitterionic phospholipid found in the sea surface microlayer, is measured on concentrated (0.3-2.0 M) chloride salt solutions containing marine-relevant cations (Na(+), K(+), Mg(2+), Ca(2+)) to model and elucidate the electrical properties of organic-covered marine aerosols. Monovalent cations show only a weak effect on the surface potential of DPPC monolayers in the condensed phase compared to water. In contrast, Mg(2+) and Ca(2+) increase the surface potential, indicating different cation binding modes and affinities for the PC headgroup. Moreover, it is found that for divalent chloride salt solutions, the PC headgroup and interfacial water molecules make the largest dipolar contribution to the surface potential. This study shows that for equal charge concentrations, divalent cations impact surface potential of DPPC monolayers more strongly than monovalents likely through changes in the PC headgroup orientation induced by their complexation along with the lesser ordering of interfacial water molecules caused by phosphate group charge screening.

  20. 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

  1. 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

  2. Strongly Emitting Surfaces Unable to Float below Plasma Potential

    DOE PAGES

    Campanell, M. D.; Umansky, M. V.

    2016-02-25

    One important unresolved question in plasma physics concerns the effect of strong electron emission on plasma-surface interactions. Previous papers reported solutions with negative and positive floating potentials relative to the plasma edge. For these two models a very different predictions for particle and energy balance is given. Here we show that the positive potential state is the only possible equilibrium in general. Even if a negative floating potential existed at t=0, the ionization collisions near the surface will force a transition to the positive floating potential state. Moreover, this transition is demonstrated with a new simulation code.

  3. An analytic mapping of oligomer potential energy surfaces to an effective Frenkel model.

    PubMed

    Binder, Robert; Römer, Sarah; Wahl, Jan; Burghardt, Irene

    2014-07-07

    While the use of Frenkel-type models for semiconducting polymer assemblies and related molecular aggregates is well established, the direct parametrization of such models based on electronic structure data is attempted less frequently. In this work, we develop a systematic mapping procedure which is adapted to J-type and H-type homo-aggregate systems. The procedure is based upon the analytic solution of an inverse eigenvalue problem for an effective Frenkel Hamiltonian with nearest-neighbor couplings. Vibronic interactions are included for both site-local and site-correlated modes. For illustration, an application is presented to the excited-state ab initio potential energy surfaces (PESs) of an oligothiophene octamer. The procedure performs a pointwise mapping of the PESs of oligomers of arbitrary chain length n, provided that the electronic ground state and any two of the n lowest adiabatic states of the excitonic manifold of interest are known. These three states are reproduced exactly by the procedure while the remaining n - 2 states of the excitonic manifold can be predicted. Explicit conditions are derived permitting to verify whether a given data set is compatible with the effective Frenkel model under study.

  4. An analytic mapping of oligomer potential energy surfaces to an effective Frenkel model

    SciTech Connect

    Binder, Robert; Römer, Sarah E-mail: burghardt@chemie.uni-frankfurt.de; Wahl, Jan; Burghardt, Irene E-mail: burghardt@chemie.uni-frankfurt.de

    2014-07-07

    While the use of Frenkel-type models for semiconducting polymer assemblies and related molecular aggregates is well established, the direct parametrization of such models based on electronic structure data is attempted less frequently. In this work, we develop a systematic mapping procedure which is adapted to J-type and H-type homo-aggregate systems. The procedure is based upon the analytic solution of an inverse eigenvalue problem for an effective Frenkel Hamiltonian with nearest-neighbor couplings. Vibronic interactions are included for both site-local and site-correlated modes. For illustration, an application is presented to the excited-state ab initio potential energy surfaces (PESs) of an oligothiophene octamer. The procedure performs a pointwise mapping of the PESs of oligomers of arbitrary chain length n, provided that the electronic ground state and any two of the n lowest adiabatic states of the excitonic manifold of interest are known. These three states are reproduced exactly by the procedure while the remaining n − 2 states of the excitonic manifold can be predicted. Explicit conditions are derived permitting to verify whether a given data set is compatible with the effective Frenkel model under study.

  5. 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…

  6. Representing Global Reactive Potential Energy Surfaces Using Gaussian Processes.

    PubMed

    Kolb, Brian; Marshall, Paul; Zhao, Bin; Jiang, Bin; Guo, Hua

    2017-03-23

    Representation of multidimensional global potential energy surfaces suitable for spectral and dynamical calculations from high-level ab initio calculations remains a challenge. Here, we present a detailed study on constructing potential energy surfaces using a machine learning method, namely, Gaussian process regression. Tests for the (3)A″ state of SH2, which facilitates the SH + H ↔ S((3)P) + H2 abstraction reaction and the SH + H' ↔ SH' + H exchange reaction, suggest that the Gaussian process is capable of providing a reasonable potential energy surface with a small number (∼1 × 10(2)) of ab initio points, but it needs substantially more points (∼1 × 10(3)) to converge reaction probabilities. The implications of these observations for construction of potential energy surfaces are discussed.

  7. 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.

  8. 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.

  9. 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.

  10. On the turbulence generated by the potential surface waves

    NASA Astrophysics Data System (ADS)

    Benilov, A. Y.

    2012-11-01

    The turbulence (the random vortex motions) of the upper ocean is nourished by the energy and momentum of the surface waves (the potential motion). The statistical characteristics of the turbulence (turbulent kinetic energy, dissipation rate, and Reynolds stresses) depend on the state of the ocean surface waves. This paper discusses the possibilities of generating this turbulence using the vortex instability of the potential surface waves. The vortex component of fluctuations of velocity field and possibly the interaction between both the vortex and potential motions cause the vertical transport of the momentum. The Reynolds tensor is a linear function of the correlation tensor of vortex field. The initial small vortex perturbations always exist in the upper ocean because of the molecular viscosity influences, especially near the free surface, and the fluctuations of the seawater density. The horizontal inhomogeneities of the seawater density produce the vortex field even if the initial vorticity was zero and the initial flow was the potential flow. The evolution of the small initial vortex disturbances in the velocity field of potential linear surface waves is reduced to a coupled set of linear ordinary differential equations of the first order with periodic coefficients. The solution of this problem shows that the small initial vortex perturbations of potential linear surface waves always grow. The initial small vortex perturbations interacting with the potential surface wave produce the small-scale turbulence (Novikov's turbulence) that finally causes the viscous dissipation of the potential surface wave. The wave-induced turbulence can be considered as developed turbulence with a well distinguishable range of the turbulent wave numberskwhere turbulence obeys the Kolmogorov's self-similarity law.

  11. Surface properties of a single perfluoroalkyl group on water surfaces studied by surface potential measurements.

    PubMed

    Shimoaka, Takafumi; Tanaka, Yuki; Shioya, Nobutaka; Morita, Kohei; Sonoyama, Masashi; Amii, Hideki; Takagi, Toshiyuki; Kanamori, Toshiyuki; Hasegawa, Takeshi

    2016-12-01

    A discriminative study of a single perfluoroalkyl (Rf) group from a bulk material is recently recognized to be necessary toward the total understanding of Rf compounds based on a primary chemical structure. The single molecule and the bulk matter have an interrelationship via an intrinsic two-dimensional (2D) aggregation property of an Rf group, which is theorized by the stratified dipole-arrays (SDA) theory. Since an Rf group has dipole moments along many C-F bonds, a single Rf group would possess a hydrophilic-like character on the surface. To reveal the hydration character of a single Rf group, in the present study, surface potential (ΔV) measurements are performed for Langmuir monolayers of Rf-containing compounds. From a comparative study with a monolayer of a normal hydrocarbon compound, the hydration/dehydration dynamics of a lying Rf group on water has first been monitored by ΔV measurements, through which a single Rf group has been revealed to have a unique "dipole-interactive" character, which enables the Rf group interacted with the water 'surface.' In addition, the SDA theory proves to be useful to predict the 2D aggregation property across the phase transition temperature of 19°C by use of the ΔV measurements.

  12. Neutral surfaces and potential vorticity in the world's oceans

    NASA Astrophysics Data System (ADS)

    You, Yuzhu; McDougall, Trevor J.

    1990-08-01

    Several neutral surfaces are mapped in this paper and their properties are contrasted with those of potential density surfaces. It is shown that the Pacific is relatively forgiving to the use of potential density, while more care must be taken in the Atlantic and Indian oceans because of the larger compensating lateral gradients of potential temperature and salinity along neutral surfaces in these oceans. The dynamically important tracer, neutral-surface potential vorticity (NSPV), defined to be proportional to f/h (where f is the Coriolis frequency and h is the height between two neutral surfaces), is mapped on several neutral surfaces in each of the world's oceans. At a depth of 1000m in the Atlantic and Indian oceans, the epineutral gradient of NSPV is different to the isopycnal variations of fN2 by as much as a factor of two (here N is the buoyancy frequency). Maps of isopycnal potential vorticity (IPV) resemble those of fN2, but the values of IPV are less by the simple factor μ, defined by μ = c[Rρ-1]/[Rρ-c], where Rρ is the stability ratio of the water column and c is the ratio of the values of α/β at the in situ pressure to that at the reference pressure (α and β being the thermal expansion and saline contraction coefficients, respectively). Layered models of the ocean circulation often take the vertical shear between layers (the thermal wind) to be given by the product of the interface slope and the contrast of potential density across the interface. The true thermal wind equation involves the interfaeial difference of in situ density, which is larger than the corresponding difference of potential density by the factor μ that is mapped in this paper, taking values up to 1.25 at a depth of 1000 m. This implies that the thermal wind is currently underestimated by up to 25% in layered ocean models. The differences between the slopes of neutral surfaces and potential density surfaces can be quantified Using the factory μ. The magnitudes of these

  13. On the uniqueness of the surface sources of evoked potentials.

    PubMed

    Cabo, A; Handy, C; Bessis, D

    2001-10-01

    The uniqueness of a surface density of sources localized inside a spatial region R and producing a given electric potential distribution in its boundary B0 is revisited. The situation in which R is filled with various subregions, each one having a definite constant value for the electric conductivity is considered. It is argued that the knowledge of the potential in all B0 fully determines the surface-located sources for a general class of surfaces supporting them and also a wide type of those sources. The class of surfaces can be defined as a union of an arbitrary but finite number of open or closed surfaces. The only restriction upon them is that no one of the closed surfaces contains inside it another (nesting) of the closed or open ones. The types of sources are surface charge densities and double layer (dipolar) densities for the open surfaces and more restrictively, only surface charge densities for the closed ones. A two-dimensional analytically solvable example illustrating the drastic appearance of uniqueness after arbitrarily small holes are opened in nested surfaces is discussed.

  14. Universal steps in quantum dynamics with time-dependent potential-energy surfaces: Beyond the Born-Oppenheimer picture

    NASA Astrophysics Data System (ADS)

    Albareda, Guillermo; Abedi, Ali; Tavernelli, Ivano; Rubio, Angel

    2016-12-01

    It was recently shown [G. Albareda et al., Phys. Rev. Lett. 113, 083003 (2014)], 10.1103/PhysRevLett.113.083003 that within the conditional decomposition approach to the coupled electron-nuclear dynamics, the electron-nuclear wave function can be exactly decomposed into an ensemble of nuclear wave packets effectively governed by nuclear conditional time-dependent potential-energy surfaces (C-TDPESs). Employing a one-dimensional model system, we show that for strong nonadiabatic couplings the nuclear C-TDPESs exhibit steps that bridge piecewise adiabatic Born-Oppenheimer potential-energy surfaces. The nature of these steps is identified as an effect of electron-nuclear correlation. Furthermore, a direct comparison with similar discontinuities recently reported in the context of the exact factorization framework allows us to draw conclusions about the universality of these discontinuities, viz., they are inherent to all nonadiabatic nuclear dynamics approaches based on (exact) time-dependent potential-energy surfaces.

  15. A new ab initio potential energy surface for the collisional excitation of N{sub 2}H{sup +} by H{sub 2}

    SciTech Connect

    Spielfiedel, Annie; Balança, Christian; Feautrier, Nicole; Senent, Maria Luisa; Kalugina, Yulia; Scribano, Yohann; Lique, François

    2015-07-14

    We compute a new potential energy surface (PES) for the study of the inelastic collisions between N{sub 2}H{sup +} and H{sub 2} molecules. A preliminary study of the reactivity of N{sub 2}H{sup +} with H{sub 2} shows that neglecting reactive channels in collisional excitation studies is certainly valid at low temperatures. The four dimensional (4D) N{sub 2}H{sup +}–H{sub 2} PES is obtained from electronic structure calculations using the coupled cluster with single, double, and perturbative triple excitation level of theory. The atoms are described by the augmented correlation consistent triple zeta basis set. Both molecules were treated as rigid rotors. The potential energy surface exhibits a well depth of ≃2530 cm{sup −1}. Considering this very deep well, it appears that converged scattering calculations that take into account the rotational structure of both N{sub 2}H{sup +} and H{sub 2} should be very difficult to carry out. To overcome this difficulty, the “adiabatic-hindered-rotor” treatment, which allows para-H{sub 2}(j = 0) to be treated as if it were spherical, was used in order to reduce the scattering calculations to a 2D problem. The validity of this approach is checked and we find that cross sections and rate coefficients computed from the adiabatic reduced surface are in very good agreement with the full 4D calculations.

  16. Surface tension, surface energy, and chemical potential due to their difference.

    PubMed

    Hui, C-Y; Jagota, A

    2013-09-10

    It is well-known that surface tension and surface energy are distinct quantities for solids. Each can be regarded as a thermodynamic property related first by Shuttleworth. Mullins and others have suggested that the difference between surface tension and surface energy cannot be sustained and that the two will approach each other over time. In this work we show that in a single-component system where changes in elastic energy can be neglected, the chemical potential difference between the surface and bulk is proportional to the difference between surface tension and surface energy. By further assuming that mass transfer is driven by this chemical potential difference, we establish a model for the kinetics by which mass transfer removes the difference between surface tension and surface energy.

  17. Effects of surface potential fluctuations on DLTS of MOS structure

    NASA Astrophysics Data System (ADS)

    Özder, Serhat; Atilgan, İsmai˙l.; Katircioǧlu, Bayram

    1996-02-01

    Although the conventional large signal deep-level transient spectroscopy (DLTS) technique is immune to surface potential fluctuations resulting from interface charge inhomogeneities in a MOS structure, in energy resolved, small signal DLTS, the eventual surface potential fluctuation should be considered. In this paper, the effect of the potential fluctuation on the temperature-scan DLTS signal for a given gate bias has been carried out. In fact, this effect shifts the DLTS peak position to lower temperatures and decreases the peak amplitude, leading to an apparent energy position and lower Dit values, respectively.

  18. Ab initio Potential Energy Surface for H-H2

    NASA Technical Reports Server (NTRS)

    Partridge, Harry; Bauschlicher, Charles W., Jr.; Stallcop, James R.; Levin, Eugene

    1993-01-01

    Ab initio calculations employing large basis sets are performed to determine an accurate potential energy surface for H-H2 interactions for a broad range of separation distances. At large distances, the spherically averaged potential determined from the calculated energies agrees well with the corresponding results determined from dispersion coefficients; the van der Waals well depth is predicted to be 75 +/- (mu)E(sub h). Large basis sets have also been applied to reexamine the accuracy of theoretical repulsive potential energy surfaces. Multipolar expansions of the computed H-H2 potential energy surface are reported for four internuclear separation distances (1.2, 1.401, 1.449, and 1.7a(sub 0) of the hydrogen molecule. The differential elastic scattering cross section calculated from the present results is compared with the measurements from a crossed beam experiment.

  19. Geometric and potential driving formation and evolution of biomolecular surfaces.

    PubMed

    Bates, P W; Chen, Zhan; Sun, Yuhui; Wei, Guo-Wei; Zhao, Shan

    2009-08-01

    This paper presents new geometrical flow equations for the theoretical modeling of biomolecular surfaces in the context of multiscale implicit solvent models. To account for the local variations near the biomolecular surfaces due to interactions between solvent molecules, and between solvent and solute molecules, we propose potential driven geometric flows, which balance the intrinsic geometric forces that would occur for a surface separating two homogeneous materials with the potential forces induced by the atomic interactions. Stochastic geometric flows are introduced to account for the random fluctuation and dissipation in density and pressure near the solvent-solute interface. Physical properties, such as free energy minimization (area decreasing) and incompressibility (volume preserving), are realized by some of our geometric flow equations. The proposed approach for geometric and potential forces driving the formation and evolution of biological surfaces is illustrated by extensive numerical experiments and compared with established minimal molecular surfaces and molecular surfaces. Local modification of biomolecular surfaces is demonstrated with potential driven geometric flows. High order geometric flows are also considered and tested in the present work for surface generation. Biomolecular surfaces generated by these approaches are typically free of geometric singularities. As the speed of surface generation is crucial to implicit solvent model based molecular dynamics, four numerical algorithms, a semi-implicit scheme, a Crank-Nicolson scheme, and two alternating direction implicit (ADI) schemes, are constructed and tested. Being either stable or conditionally stable but admitting a large critical time step size, these schemes overcome the stability constraint of the earlier forward Euler scheme. Aided with the Thomas algorithm, one of the ADI schemes is found to be very efficient as it balances the speed and accuracy.

  20. 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.

  1. Intermolecular potential energy surface for CS2 dimer.

    PubMed

    Farrokhpour, Hossein; Mombeini, Zainab; Namazian, Mansoor; Coote, Michelle L

    2011-04-15

    A new four-dimensional intermolecular potential energy surface for CS(2) dimer is obtained by ab initio calculation of the interaction energies for a range of configurations and center-of-mass separation distances for the first time. The calculations were performed using the supermolecular approach at the Møller-Plesset second-order perturbation (MP2) level of theory with the augmented correlation consistent basis sets (aug-cc-pVxZ, x = D, T) and corrected for the basis-set superposition error using the full counterpoise correction method. A two-point extrapolation method was used to extrapolate the calculated energy points to the complete basis set limit. The effect of using the higher levels of theory, quadratic configuration interaction containing single, double, and perturbative triple excitations QCISD(T) and coupled cluster singles, doubles and perturbative triples excitations CCSD(T), on the shape of potential energy surface was investigated. It is shown that the MP2 level of theory apparently performs extremely poorly for describing the intermolecular potential energy surface, overestimating the total energy by a factor of nearly 1.73 in comparison with the QCISD(T) and CCSD(T) values. The value of isotropic dipole-dipole dispersion coefficient (C(6) ) of CS(2) fluid was obtained from the extrapolated MP2 potential energy surface. The MP2 extrapolated energy points were fitted to well-known analytical potential functions using two different methods to represent the potential energy surface analytically. The most stable configuration of the dimer was determined at R = 6.23 au, α = 90°, β = 90°, and γ = 90°, with a well depth of 3.980 kcal mol(-1) at the MP2 level of theory. Finally, the calculated second virial coefficients were compared with experimental values to test the quality of the presented potential energy surface.

  2. Zero-point energy, tunneling, and vibrational adiabaticity in the Mu + H2 reaction

    SciTech Connect

    Mielke, Steven L.; Garrett, Bruce C.; Fleming, Donald G.; Truhlar, Donald G.

    2015-01-09

    Abstract: Isotopic substitution of muonium for hydrogen provides an unparalleled opportunity to deepen our understanding of quantum mass effects on chemical reactions. A recent topical review [Aldegunde et al., Mol. Phys. 111, 3169 (2013)] of the thermal and vibrationally-stateselected reaction of Mu with H2 raises a number of issues that are addressed here. We show that some earlier quantum mechanical calculations of the Mu + H2 reaction, which are highlighted in this review and which have been used to benchmark approximate methods, are in error by as much as 19% in the low-temperature limit. We demonstrate that an approximate treatment of the Born–Oppenheimer diagonal correction that was used in some recent studies is not valid for treating the vibrationally-state-selected reaction. We also discuss why vibrationally adiabatic potentials that neglect bend zero-point energy are not a useful analytical tool for understanding reaction rates and why vibrationally nonadiabatic transitions cannot be understood by considering tunneling through vibrationally adiabatic potentials. Finally, we present calculations on a hierarchical family of potential energy surfaces to assess the sensitivity of rate constants to the quality of the potential surface.

  3. 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.

  4. 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.

  5. Applications of chirped Raman adiabatic rapid passage to atom interferometry

    NASA Astrophysics Data System (ADS)

    Kotru, Krish; Butts, David L.; Kinast, Joseph M.; Johnson, David M. S.; Radojevic, Antonije M.; Timmons, Brian P.; Stoner, Richard E.

    2012-02-01

    We present robust atom optics, based on chirped Raman adiabatic rapid passage (ARP), in the context of atom interferometry. Such ARP light pulses drive coherent population transfer between two hyperfine ground states by sweeping the frequency difference of two fixed-intensity optical fields with large single photon detunings. Since adiabatic transfer is less sensitive to atom temperature and non-uniform Raman beam intensity than standard Raman pulses, this approach should improve the stability of atom interferometers operating in dynamic environments. In such applications, chirped Raman ARP may also provide advantages over the previously demonstrated stimulated Raman adiabatic passage (STIRAP) technique, which requires precise modulation of beam intensity and zeroing of the single photon detuning. We demonstrate a clock interferometer with chirped Raman ARP pulses, and compare its stability to that of a conventional Raman pulse interferometer. We also discuss potential improvements to inertially sensitive atom interferometers. Copyright 2011 by The Charles Stark Draper Laboratory, Inc. All rights reserved.

  6. The Contribution of Surface Potential to Diverse Problems in Electrostatics

    NASA Astrophysics Data System (ADS)

    Horenstein, M.

    2015-10-01

    Electrostatics spans many different subject areas. Some comprise “good electrostatics,” where charge is used for desirable purposes. Such areas include industrial manufacturing, electrophotography, surface modification, precipitators, aerosol control, and MEMS. Other areas comprise “bad electrostatics,” where charge is undesirable. Such areas include hazardous discharges, ESD, health effects, nuisance triboelectrification, particle contamination, and lightning. Conference proceedings such as this one inevitably include papers grouped around these topics. One common thread throughout is the surface potential developed when charge resides on an insulator surface. Often, the charged insulator will be in intimate contact with a ground plane. At other times, the charged insulator will be isolated. In either case, the resulting surface potential is important to such processes as propagating brush discharges, charge along a moving web, electrostatic biasing effects in MEMS, non-contacting voltmeters, field-effect transistor sensors, and the maximum possible charge on a woven fabric.

  7. Identifying and tracing potential energy surfaces of electronic excitations with specific character via their transition origins: application to oxirane.

    PubMed

    Li, Jian-Hao; Zuehlsdorff, T J; Payne, M C; Hine, N D M

    2015-05-14

    We show that the transition origins of electronic excitations identified by quantified natural transition orbital (QNTO) analysis can be employed to connect potential energy surfaces (PESs) according to their character across a wide range of molecular geometries. This is achieved by locating the switching of transition origins of adiabatic potential surfaces as the geometry changes. The transition vectors for analysing transition origins are provided by linear response time-dependent density functional theory (TDDFT) calculations under the Tamm-Dancoff approximation. We study the photochemical CO ring opening of oxirane as an example and show that the results corroborate the traditional Gomer-Noyes mechanism derived experimentally. The knowledge of specific states for the reaction also agrees well with that given by previous theoretical work using TDDFT surface-hopping dynamics that was validated by high-quality quantum Monte Carlo calculations. We also show that QNTO can be useful for considerably larger and more complex systems: by projecting the excitations to those of a reference oxirane molecule, the approach is able to identify and analyse specific excitations of a trans-2,3-diphenyloxirane molecule.

  8. Potential energy surfaces of LaH + and LaH + 2

    NASA Astrophysics Data System (ADS)

    Das, Kalyan K.; Balasubramanian, K.

    1991-03-01

    Using the complete active space multiconfiguration self-consistent field (CAS-MCSCF) followed by full second-order configuration interaction (SOCI) calculations, 16 electronic states of LaH+ and 8 electronic states of LaH+2 are investigated. The potential energy surface of these electronic states of LaH+2 and LaH+ are computed. These calculations show that the 3F(5d2) ground state of La+ ion forms a weak complex with H2. The La+(1D) excited state inserts into H2 with a small barrier (<8 kcal/mol) to form the 1A1 ground state of LaH+2 (re=2.057 Å, θe=106°). At the SOCI level of theory LaH+2 is found to be 11 kcal/mol more stable than La+(3F)+H2. Our calculations explain the experimental observations on La++H2→LaH++H reaction. The adiabatic ionization potential (IP) of LaH2 and LaH are calculated as 5.23 and 5.33 eV, respectively. The ground state of LaH+ was found to be a 2Δ state. We compute De(LaH+) and De(HLa-H+) as 2.54 eV in excellent agreement with the experimental De(LaH+)=2.57 eV measured by Armentrout and co-workers. The spin-orbit effects of LaH+ were also studied using the relativistic configuration interaction (RCI) method.

  9. Potential energy surfaces for YH + 2 and ZrH + 2

    NASA Astrophysics Data System (ADS)

    Das, Kalyan K.; Balasubramanian, K.

    1989-08-01

    Electronic structures, potential energy surfaces, and one-electron properties of 16 electronic states of two transition metal dihydride ions YH+2 and ZrH+2 are calculated using the complete active space multiconfiguration self-consistent field (MCSCF) followed by a full second-order configuration interaction (SOCI) method. The MCSCF/SOCI method yields 1A1 as the ground state for YH+2 with re=1.833 Å and θe=116° and a 2A1 ground state for ZrH+2 with re=1.75 Å and θe=113.5°. The SOCI atomization energy [YH+2(1A1) →Y+(1S)+2H] is calculated to be 5.22 eV in good agreement with an experimental value of 5.52 eV at 298 K for this process. The De(Y+-H) for YH+ is calculated to be 58.9 kcal/mol in excellent agreement with an experimental value of 58±3 kcal/mol. The first adiabatic ionization potentials of YH2 and ZrH2 are calculated as 6.18 and 6.95 eV, respectively. The excited Zr+(2D) ion inserts spontaneously into H2 leading to the bent ground state of ZrH+2, while the ground state of Zr+ does not insert into H2. The 1S0 ground state of Y+ has to surmount a small barrier of about 10 kcal/mol for insertion into H2. The addition of f type diffuse functions does not change the geometrical parameters much.

  10. 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.

  11. Lunar Surface Potential Increases during Terrestrial Bow Shock Traversals

    NASA Technical Reports Server (NTRS)

    Collier, Michael R.; Stubbs, Timothy J.; Hills, H. Kent; Halekas, Jasper; Farrell, William M.; Delory, Greg T.; Espley, Jared; Freeman, John W.; Vondrak, Richard R.; Kasper, Justin

    2009-01-01

    Since the Apollo era the electric potential of the Moon has been a subject of interest and debate. Deployed by three Apollo missions, Apollo 12, Apollo 14 and Apollo 15, the Suprathermal Ion Detector Experiment (SIDE) determined the sunlit lunar surface potential to be about +10 Volts using the energy spectra of lunar ionospheric thermal ions accelerated toward the Moon. We present an analysis of Apollo 14 SIDE "resonance" events that indicate the lunar surface potential increases when the Moon traverses the dawn bow shock. By analyzing Wind spacecraft crossings of the terrestrial bow shock at approximately this location and employing current balancing models of the lunar surface, we suggest causes for the increasing potential. Determining the origin of this phenomenon will improve our ability to predict the lunar surface potential in support of human exploration as well as provide models for the behavior of other airless bodies when they traverse similar features such as interplanetary shocks, both of which are goals of the NASA Lunar Science Institute's Dynamic Response of the Environment At the Moon (DREAM) team.

  12. Investigation of structural and surface potential studies of CZTS nanorods

    NASA Astrophysics Data System (ADS)

    Kumari, Navnita; Varandani, Deepak; Mehta, Bodh Raj

    2017-04-01

    Copper zinc tin sulphide (Cu2ZnSnS4) known as CZTS is a potential absorber layer due to its non toxicity and earth abundant availability of its constituent elements. CZTS nanorods are successfully synthesized using hydrothermal route and characterized by X-ray powder diffraction, field-emission scanning electron microscopy, high-resolution transmission electron microscopy, raman spectroscopy, and Kelvin probe force microscopy (KPFM) techniques. XRD and Raman it confirm that the synthesized CZTS samples are in keseterite phase without any impurities. From FESEM and EDAX, the elemental ratio is observed to 1.81:0.90:0.85:3.71. Raman study shows the peak position at 287, 339, and 372 cm-1 which corresponds to CZTS pure phase without any impurity peak. Surface potential and work function of CZTS nanorods (NRs) has been derived by KPFM data. KPFM shows that with an increase in diameter of CZTS nanorods surface potential decreases indicating enhancement of p-type conductivity with decrease in NR diameter. The value of surface potential is found to be 496 and 486 mV NRs with diameter 40 and 60 nm, respectively. The results are explained on the basis of Oxygen induced passivation of surface states in NRs diameter. The results of the study are important for potential applications of CZTS NRs in the field of optoelectronic and solar cells.

  13. Ab Initio Potential Energy Surface for H-H2

    NASA Technical Reports Server (NTRS)

    Patridge, Harry; Bauschlicher, Charles W., Jr.; Stallcop, James R.; Levin, Eugene

    1993-01-01

    Ab initio calculations employing large basis sets are performed to determine an accurate potential energy surface for H-H2 interactions for a broad range of separation distances. At large distances, the spherically averaged potential determined from the calculated energies agrees well with the corresponding results determined from dispersion coefficients; the van der Waals well depth is predicted to be 75 +/- 3 micro E(h). Large basis sets have also been applied to reexamine the accuracy of theoretical repulsive potential energy surfaces (25-70 kcal/mol above the H-H2 asymptote) at small interatomic separations; the Boothroyd, Keogh, Martin, and Peterson (BKMP) potential energy surface is found to agree with results of the present calculations within the expected uncertainty (+/- 1 kcal/mol) of the fit. Multipolar expansions of the computed H-H2 potential energy surface are reported for four internuclear separation distances (1.2, 1.401, 1.449, and 1.7a(0)) of the hydrogen molecule. The differential elastic scattering cross section calculated from the present results is compared with the measurements from a crossed beam experiment.

  14. Theory of the photodissociation of ozone in the Hartley continuum: potential energy surfaces, conical intersections, and photodissociation dynamics.

    PubMed

    Baloïtcha, Ezinvi; Balint-Kurti, Gabriel G

    2005-07-01

    Ab initio potential energy and transition dipole moment surfaces are presented for the five lowest singlet even symmetry electronic states of ozone. The surfaces are calculated using the complete active space self consistent field method followed by contracted multireference configuration interaction (MRCI) calculations. A slightly reduced augmented correlation consistent valence triple-zeta orbital basis set is used. The ground and excited state energies of the molecule have been computed at 9282 separate nuclear geometries. Cuts through the potential energy surfaces, which pass through the geometry of the minimum of the ground electronic state, show several closely avoided crossings. Close examination, and higher level calculations, very strongly suggests that some of these seemingly avoided crossings are in fact associated with non-symmetry related conical intersections. Diabatic potential energy and transition dipole moment surfaces are created from the computed ab initio adiabatic MRCI energies and transition dipole moments. The transition dipole moment connecting the ground electronic state to the diabatic B state surface is by far the strongest. Vibrational-rotational wavefunctions and energies are computed using the ground electronic state. The energy level separations compare well with experimentally determined values. The ground vibrational state wavefunction is then used, together with the diabatic B<--X transition dipole moment surface, to form an initial wavepacket. The analysis of the time-dependent quantum dynamics of this wavepacket provides the total and partial photodissociation cross sections for the system. Both the total absorption cross section and the predicted product quantum state distributions compare well with experimental observations. A discussion is also given as to how the observed alternation in product diatom rotational state populations might be explained.

  15. New ab initio potential energy surface for BrH2 and rate constants for the H + HBr → H2 + Br abstraction reaction.

    PubMed

    Jiang, Bin; Xie, Changjian; Xie, Daiqian

    2011-03-21

    A global potential energy surface (PES) for the electronic ground state of the BrH(2) system was constructed based on the multireference configuration interaction (MRCI) method including the Davidson's correction using a large basis set. In addition, the spin-orbit correction were computed using the Breit-Pauli Hamiltonian and the unperturbed MRCI wavefunctions in the Br + H(2) channel and the transition state region. Adding the correction to the ground state potential, the lowest spin-orbit correlated adiabatic potential was obtained. The characters of the new potential are discussed. Accurate initial state specified rate constants for the H + HBr → H(2) + Br abstraction reaction were calculated using a time-dependent wave packet method. The predicted rate constants were found to be in excellent agreement with the available experimental values and much better than those obtained from a previous PES.

  16. Locating potential biosignatures on Europa from surface geology observations.

    PubMed

    Figueredo, Patricio H; Greeley, Ronald; Neuer, Susanne; Irwin, Louis; Schulze-Makuch, Dirk

    2003-01-01

    We evaluated the astrobiological potential of the major classes of geologic units on Europa with respect to possible biosignatures preservation on the basis of surface geology observations. These observations are independent of any formational model and therefore provide an objective, though preliminary, evaluation. The assessment criteria include high mobility of material, surface concentration of non-ice components, relative youth, textural roughness, and environmental stability. Our review determined that, as feature classes, low-albedo smooth plains, smooth bands, and chaos hold the highest potential, primarily because of their relative young age, the emplacement of low-viscosity material, and indications of material exchange with the subsurface. Some lineaments and impact craters may be promising sites for closer study despite the comparatively lower astrobiological potential of their classes. This assessment will be expanded by multidisciplinary examination of the potential for habitability of specific features.

  17. An Exercise in Evaluating the Contamination Potential of Surface Impoundments.

    ERIC Educational Resources Information Center

    Tinker, John R., Jr.

    1982-01-01

    Outlines a laboratory procedure which enables students to evaluate the contamination potential of surface impoundments and apply basic principles of hydrogeology to the land disposal of waste material. Includes a list of materials needed and directions for the instructor. (Author/DC)

  18. Potential Energy Surface Database of Group II Dimer

    National Institute of Standards and Technology Data Gateway

    SRD 143 NIST Potential Energy Surface Database of Group II Dimer (Web, free access)   This database provides critical atomic and molecular data needed in order to evaluate the feasibility of using laser cooled and trapped Group II atomic species (Mg, Ca, Sr, and Ba) for ultra-precise optical clocks or quantum information processing devices.

  19. Communication: Separable potential energy surfaces from multiplicative artificial neural networks

    SciTech Connect

    Koch, Werner Zhang, Dong H.

    2014-07-14

    We present a potential energy surface fitting scheme based on multiplicative artificial neural networks. It has the sum of products form required for efficient computation of the dynamics of multidimensional quantum systems with the multi configuration time dependent Hartree method. Moreover, it results in analytic potential energy matrix elements when combined with quantum dynamics methods using Gaussian basis functions, eliminating the need for a local harmonic approximation. Scaling behavior with respect to the complexity of the potential as well as the requested accuracy is discussed.

  20. Quantum and classical non-adiabatic dynamics of Li_{2}^{+}Ne photodissociation

    NASA Astrophysics Data System (ADS)

    Pouilly, Brigitte; Monnerville, Maurice; Zanuttini, David; Gervais, Benoît

    2015-01-01

    The 3D photodissociation dynamics of Li2+Ne system is investigated by quantum calculations using the multi-configuration time-dependent Hartree (MCTDH) method and by classical simulations with the trajectory surface hopping (TSH) approach. Six electronic states of A’ symmetry and two states of A” symmetry are involved in the process. Couplings in the excitation region and two conical intersections in the vicinity of the Franck-Condon zone control the non-adiabatic nuclear dynamics. A diabatic representation including all the states and the couplings is determined. Diabatic and adiabatic populations calculated for initial excitation to pure diabatic and adiabatic states lead to a clear understanding of the mechanisms governing the non-adiabatic photodissociation process. The classical and quantum photodissociation cross-sections for absorption in two adiabatic states of the A’ symmetry are calculated. A remarkable agreement between quantum and classical results is obtained regarding the populations and the absorption cross-sections.

  1. Communication: Fitting potential energy surfaces with fundamental invariant neural network

    NASA Astrophysics Data System (ADS)

    Shao, Kejie; Chen, Jun; Zhao, Zhiqiang; Zhang, Dong H.

    2016-08-01

    A more flexible neural network (NN) method using the fundamental invariants (FIs) as the input vector is proposed in the construction of potential energy surfaces for molecular systems involving identical atoms. Mathematically, FIs finitely generate the permutation invariant polynomial (PIP) ring. In combination with NN, fundamental invariant neural network (FI-NN) can approximate any function to arbitrary accuracy. Because FI-NN minimizes the size of input permutation invariant polynomials, it can efficiently reduce the evaluation time of potential energy, in particular for polyatomic systems. In this work, we provide the FIs for all possible molecular systems up to five atoms. Potential energy surfaces for OH3 and CH4 were constructed with FI-NN, with the accuracy confirmed by full-dimensional quantum dynamic scattering and bound state calculations.

  2. Apatite nucleation on silica surface: a zeta potential approach.

    PubMed

    Coreño, J; Martínez, A; Bolarín, A; Sánchez, F

    2001-10-01

    Zeta potential measurements on pure silica, prepared by the sol-gel method from tetraethoxysilane under acidic conditions, are reported in different suspensions. Water suspensions and suspensions containing calcium or phosphate ions with and without NaCl were tested. zeta potential measurements were carried out as a function of the pH and ion concentration. Also, calcium and phosphate adsorption on silica was determined experimentally. The results of zeta potential and adsorption measurements suggest that both calcium and phosphate ions can be adsorbed on the silica surface; however, calcium adsorption is stronger than phosphate adsorption. When calcium and sodium ions are present in the suspension, calcium adsorption decreases. It seems that certain sites on the silica surface are specific for calcium adsorption.

  3. An accurate full-dimensional potential energy surface for H–Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption

    SciTech Connect

    Janke, Svenja M.; Auerbach, Daniel J.; Kandratsenka, Alexander; Wodtke, Alec M.

    2015-09-28

    We have constructed a potential energy surface (PES) for H-atoms interacting with fcc Au(111) based on fitting the analytic form of the energy from Effective Medium Theory (EMT) to ab initio energy values calculated with density functional theory. The fit used input from configurations of the H–Au system with Au atoms at their lattice positions as well as configurations with the Au atoms displaced from their lattice positions. It reproduces the energy, in full dimension, not only for the configurations used as input but also for a large number of additional configurations derived from ab initio molecular dynamics (AIMD) trajectories at finite temperature. Adiabatic molecular dynamics simulations on this PES reproduce the energy loss behavior of AIMD. EMT also provides expressions for the embedding electron density, which enabled us to develop a self-consistent approach to simulate nonadiabatic electron-hole pair excitation and their effect on the motion of the incident H-atoms. For H atoms with an energy of 2.7 eV colliding with Au, electron-hole pair excitation is by far the most important energy loss pathway, giving an average energy loss ≈3 times that of the adiabatic case. This increased energy loss enhances the probability of the H-atom remaining on or in the Au slab by a factor of 2. The most likely outcome for H-atoms that are not scattered also depends prodigiously on the energy transfer mechanism; for the nonadiabatic case, more than 50% of the H-atoms which do not scatter are adsorbed on the surface, while for the adiabatic case more than 50% pass entirely through the 4 layer simulation slab.

  4. An accurate full-dimensional potential energy surface for H-Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption.

    PubMed

    Janke, Svenja M; Auerbach, Daniel J; Wodtke, Alec M; Kandratsenka, Alexander

    2015-09-28

    We have constructed a potential energy surface (PES) for H-atoms interacting with fcc Au(111) based on fitting the analytic form of the energy from Effective Medium Theory (EMT) to ab initio energy values calculated with density functional theory. The fit used input from configurations of the H-Au system with Au atoms at their lattice positions as well as configurations with the Au atoms displaced from their lattice positions. It reproduces the energy, in full dimension, not only for the configurations used as input but also for a large number of additional configurations derived from ab initio molecular dynamics (AIMD) trajectories at finite temperature. Adiabatic molecular dynamics simulations on this PES reproduce the energy loss behavior of AIMD. EMT also provides expressions for the embedding electron density, which enabled us to develop a self-consistent approach to simulate nonadiabatic electron-hole pair excitation and their effect on the motion of the incident H-atoms. For H atoms with an energy of 2.7 eV colliding with Au, electron-hole pair excitation is by far the most important energy loss pathway, giving an average energy loss ≈3 times that of the adiabatic case. This increased energy loss enhances the probability of the H-atom remaining on or in the Au slab by a factor of 2. The most likely outcome for H-atoms that are not scattered also depends prodigiously on the energy transfer mechanism; for the nonadiabatic case, more than 50% of the H-atoms which do not scatter are adsorbed on the surface, while for the adiabatic case more than 50% pass entirely through the 4 layer simulation slab.

  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. Potential for carbon adsorption on concrete: surface XPS analyses.

    PubMed

    Haselbach, Liv M; Ma, Shuguo

    2008-07-15

    The concrete industry is a contributor to the global carbon cycle particularly with respect to the contribution of carbon dioxide in the manufacturing of cement (calcination). The reverse reaction of carbonation is known to occur in concrete, but is usually limited to exterior surfaces exposed to carbon dioxide and humidity in the air. As alternate concrete uses expand which have more surface area, such as crushed concrete for recycling, it is important to understand surface adsorption of carbon dioxide and the positive impacts it might have on the carbon cycle. X-ray photoelectron spectroscopy (XPS) is used in this study to evaluate carbon species on hydrated cement mortar surfaces. Initial estimates for carbon absorption in concrete using othertechniques predictthe potential for carbonate species to be a fraction of the calcination stoichiometric equivalent The XPS results indicate that there is a rapid and substantial uptake of carbon dioxide on the surfaces of these mortars, sometimes exceeding the calcination stoichiometric equivalents, indicative of carbon dioxide surface complexation species. On pure calcite, the excess is on the order of 30%. This accelerated carbon dioxide surface adsorption phenomenon may be importantfor determining novel and effective carbon sequestration processes using recycled concrete.

  7. Theoretical characterization of the potential energy surface for NH + NO

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.

    1992-01-01

    The potential energy surface (PES) for NH + NO was characterized using complete active space self-consistent field (CASSCF) gradient calculations to determine the stationary point geometries and frequencies followed by CASSCF/internally contracted configuration interaction (CCI) calculations to refine the energetics. The present results are in qualitative accord with the BAC-MP4 calculations, but there are differences as large as 8 kcal/mol in the detailed energetics. Addition of NH to NO on a (2)A' surface, which correlated with N2 + OH or H + N2O products, involves barriers of 3.2 kcal/mol (trans) and 6.3 kcal/mol (cis). Experimental evidence for these barriers is found in earlier works. The (2)A' surface has no barrier to addition, but does not correlate with products. Surface crossings between the barrierless (2)A' surface and the (2)A' surface may be important. Production of N2 + OH products is predicted to occur via a planar saddle point of (2)A' symmetry. This is in accord with the preferential formation of II(A') lambda doublet levels of OH in earlier experiments. Addition of NH (1)delta to NO is found to occur on an excited state surface and is predicted to lead to N2O product as observed in earlier works.

  8. Environmental surface cleanliness and the potential for contamination during handwashing.

    PubMed

    Griffith, Christopher J; Malik, Rifhat; Cooper, Rose A; Looker, Nick; Michaels, Barry

    2003-04-01

    Effective handwashing (including drying) is important in infection control. The ability of the various stages of handwashing to decrease skin-surface microbial counts has been documented. However, an important element, environmental surface cleanliness, and the potential for contamination of hands during the process has not been well studied or quantified. An examination of the adenosine triphosphate (a measure of residual organic soil), bacterial, and staphylococcal load on ward handwash station surfaces, which could be touched during handwashing, is reported. Hand contact surfaces tested consisted of approximately 620 each of: faucet handles, soap dispenser activator mechanisms, and folded paper-towel dispenser exits. Failure rates in excess of benchmark clean values were higher with adenosine triphosphate assays than microbial counts. This could indicate the presence of a higher level of general organic debris (eg, skin cells) as opposed to microbial contamination or could reflect greater assay sensitivity. Faucet handles were more likely to be contaminated and be in excess of benchmark values than paper-towel dispenser exits. However, the latter are likely to be the final surface touched during the handwashing process and overall nearly 20% were above microbiologic benchmark values. Many of the organisms isolated were staphylococci and the results are discussed within the context of microbial cross-contamination and potential pathogen spread.

  9. Can atom-surface potential measurements test atomic structure models?

    PubMed

    Lonij, Vincent P A; Klauss, Catherine E; Holmgren, William F; Cronin, Alexander D

    2011-06-30

    van der Waals (vdW) atom-surface potentials can be excellent benchmarks for atomic structure calculations. This is especially true if measurements are made with two different types of atoms interacting with the same surface sample. Here we show theoretically how ratios of vdW potential strengths (e.g., C₃(K)/C₃(Na)) depend sensitively on the properties of each atom, yet these ratios are relatively insensitive to properties of the surface. We discuss how C₃ ratios depend on atomic core electrons by using a two-oscillator model to represent the contribution from atomic valence electrons and core electrons separately. We explain why certain pairs of atoms are preferable to study for future experimental tests of atomic structure calculations. A well chosen pair of atoms (e.g., K and Na) will have a C₃ ratio that is insensitive to the permittivity of the surface, whereas a poorly chosen pair (e.g., K and He) will have a ratio of C₃ values that depends more strongly on the permittivity of the surface.

  10. 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.

  11. A test of H2-He potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Thibault, Franck; Wcisło, Piotr; Ciuryło, Roman

    2016-11-01

    The close-coupling method is used to calculate purely rotational relaxation rates and pressure broadening and shifting coefficients for H2-He collisions, in order to test various potential energy surfaces. Downward rate coefficients k3→1(T) and k2→0(T) are compared with experimental data, but the subtle differences in the potential energy surfaces are hardly reflected in these rates. Helium pressure broadening and shifting generalized cross sections for the isotropic Raman Q(1) lines of the fundamental bands of D2 and H2 as well as the purely rotational Stokes S0(1) line of H2 are therefore also considered. While these spectroscopic characteristics are much more sensitive to the precise form of the interaction potential, a proper validation cannot be performed without taking into account the influence of the translational motion on the molecular line shapes. After including this, it is found that the potential energy surface of Bakr, Smith and Patkowski [B.W. Bakr, D.G.A. Smith, K. Patkowski, J. Chem. Phys. 139, 144305 (2013)] allows the best reproduction of the experimental data.

  12. 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.

  13. Adiabatic tracking for photo- and magneto-association of Bose-Einstein condensates with Kerr nonlinearities

    NASA Astrophysics Data System (ADS)

    Gevorgyan, Mariam; Guérin, Stéphane; Leroy, Claude; Ishkhanyan, Artur; Jauslin, Hans-Rudolf

    2016-11-01

    We develop the method of adiabatic tracking for photo- and magneto-association of Bose-Einstein atomic condensates with models that include Kerr type nonlinearities. We show that the inclusion of these terms can produce qualitatively important modifications in the adiabatic dynamics, like the appearance of bifurcations, in which the trajectory that is being tracked loses its stability. As a consequence the adiabatic theorem does not apply and the adiabatic transfer can be strongly degraded. This degradation can be compensated by using fields that are strong enough compared with the values of the Kerr terms. The main result is that, despite these potentially detrimental features, there is always a choice of the detuning that leads to an efficient adiabatic tracking, even for relatively weak fields.

  14. Ultrafast adiabatic second harmonic generation

    NASA Astrophysics Data System (ADS)

    Dahan, Asaf; Levanon, Assaf; Katz, Mordechai; Suchowski, Haim

    2017-03-01

    We introduce a generalization of the adiabatic frequency conversion method for an efficient conversion of ultrashort pulses in the full nonlinear regime. Our analysis takes into account dispersion as well as two-photon processes and Kerr effect, allowing complete analysis of any three waves with arbitrary phase mismatched design and any nonlinear optical process. We use this analysis to design an efficient and robust second harmonic generation, the most widely used nonlinear process for both fundamental and applied research. We experimentally show that such design not only allows for very efficient conversion of various of ultrashort pulses, but is also very robust to variations in the parameters of both the nonlinear crystal and the incoming light. These include variation of more than 100 °C in the crystal temperature, a wide bandwidth of up to 75 nm and a chirp variation of 300 fs to 3.5 ps of the incoming pulse. Also, we show the dependency of the adiabatic second harmonic generation design on the pump intensity and the crystal length. Our study shows that two photon absorption plays a critical role in such high influence nonlinear dynamics, and that it must be considered in order to achieve agreement with experimental results.

  15. Ultrafast adiabatic second harmonic generation.

    PubMed

    Dahan, Asaf; Levanon, Assaf; Katz, Mordechai; Suchowski, Haim

    2017-03-01

    We introduce a generalization of the adiabatic frequency conversion method for an efficient conversion of ultrashort pulses in the full nonlinear regime. Our analysis takes into account dispersion as well as two-photon processes and Kerr effect, allowing complete analysis of any three waves with arbitrary phase mismatched design and any nonlinear optical process. We use this analysis to design an efficient and robust second harmonic generation, the most widely used nonlinear process for both fundamental and applied research. We experimentally show that such design not only allows for very efficient conversion of various of ultrashort pulses, but is also very robust to variations in the parameters of both the nonlinear crystal and the incoming light. These include variation of more than 100 °C in the crystal temperature, a wide bandwidth of up to 75 nm and a chirp variation of 300 fs to 3.5 ps of the incoming pulse. Also, we show the dependency of the adiabatic second harmonic generation design on the pump intensity and the crystal length. Our study shows that two photon absorption plays a critical role in such high influence nonlinear dynamics, and that it must be considered in order to achieve agreement with experimental results.

  16. Night side lunar surface potential in the Earth's magnetosphere

    NASA Astrophysics Data System (ADS)

    Saito, Yoshifumi; Ishikawa, Motohisa; Nishino, Masaki; Yokota, Shoichiro; Tsunakawa, Hideo

    2015-04-01

    In the Earth's magnetotail, Kaguya repeatedly encountered the plasmoid or plasma sheet. The low energy ion signatures including lobe cold ions, cold ion acceleration in the plasma sheet-lobe boundaries, and hot plasma sheet ions or fast flowing ions associated with plasmoids characterized the encounters. On the dayside of the Moon, tailward flowing cold ions and their acceleration were observed. However, on the night side, tailward flowing cold ions could not be observed since the Moon blocked them. In stead, ion acceleration by the spacecraft potential and the electron beam accelerated by the potential difference between lunar surface and spacecraft were simultaneously observed. Similar night side ion/electron signatures were often observed at low altitude <~50km when Kaguya was in the magnetotail lobe. When Kaguya stayed in the hemisphere where lobe plasma convection direction was from lobe toward the night side of the Moon, MAP-PACE ion sensors found that the lobe cold ions intruded into the night side of the Moon. The ExB drift motion by the dawn-to-dusk electric field facilitated the intrusion of the lobe cold ions. In addition, very cold ions flowing towards the Earth (towards the Moon) were observed in the opposite hemisphere. It was also found that the flow direction of the lobe cold ions intruded into the night side of the Moon gradually changed from tailward to Earthward (Moonward) while slightly increasing their energy. Acceleration of the intruded cold ions by the electrostatic potential distributed on the night side of the Moon could explain the characteristics of the ions. The electron beams accelerated by the potential difference between lunar surface and spacecraft were also simultaneously observed. These electron and ion data enabled us to determine both the night side lunar surface potential and spacecraft potential only from the observed data.

  17. The biofouling potential of flow on corrugated surfaces

    NASA Astrophysics Data System (ADS)

    Miño, Gastón L.; Rusconi, Roberto; Kantsler, Vasily; Stocker, Roman

    2015-11-01

    Both natural and man-made surfaces are rarely smooth, and are instead often characterized by geometric heterogeneity or roughness over a broad range of scales. Because of the predicted importance of the local interaction between microorganisms and surfaces, roughness at the microbial scale can be an important element in determining the outcome of microbe-surface interactions, which represent the first step in biofilm formation and biofouling. In microbial habitats this interaction often occurs in flowing fluids, which can be important because regions with high hydrodynamic shear can induce a strong reorientation of bacteria towards surfaces, promoting attachment. Here we study the combination of flow and surface topography using video microscopy of Escherichia coli in corrugated microfluidic channels. We report that flow preferentially promotes attachment to specific regions of a corrugated surface, as result of the hydrodynamics of bacteria swimming in flow. We compute from the data a ``Local Biofouling Potential'' (LBP) and compare this successfully with predictions of a mathematical model, yielding one step towards the ability to mechanistically predict and thus ultimately either prevent or induce biofouling.

  18. Calculating vibrational spectra using modified Shepard interpolated potential energy surfaces.

    PubMed

    Evenhuis, Christian R; Manthe, Uwe

    2008-07-14

    A potential energy interpolation approach based on modified Shepard interpolation and specifically designed for calculation of vibrational states is presented. The importance of the choice of coordinates for the rate of convergence is demonstrated. Studying the vibrational states of the water molecule as a test case, a coordinate system comprised of inverse bond distances and trigonometric functions of the bond angle is found to be particularly efficient. Different sampling schemes used to locate the reference points in the modified Shepard interpolation are investigated. A final scheme is recommended, which allows the construction of potential energy surfaces to sub-wave-number accuracy.

  19. A global potential energy surface for ArH2

    NASA Technical Reports Server (NTRS)

    Schwenke, David W.; Walch, Stephen P.; Taylor, Peter R.

    1992-01-01

    We describe a simple analytic representation of the ArH2 potential energy surface which well reproduces the results of extensive ab initio electronic structure calculations. The analytic representation smoothly interpolates between the dissociated H2 and strong bonding limits. In the fitting process, emphasis is made on accurately reproducing regions of the potential expected to be important for high temperature (ca. 3000 K) collision processes. Overall, the anisotropy and H2 bond length dependence of the analytic representation well reproduce the input data.

  20. A global potential energy surface for ArH2

    NASA Technical Reports Server (NTRS)

    Schwenke, David W.; Walch, Stephen P.; Taylor, Peter R.

    1993-01-01

    We describe a simple analytic representation of the ArH2 potential energy surface which well reproduces the results of extensive ab initio electronic structure calculations. The analytic representation smoothly interpolates between the dissociated H2 and strong bonding limits. In the fitting process, emphasis is made on accurately reproducing regions of the potential expected to be important for high temperature (ca. 3000 K) collision processes. Overall, the anisotropy and H2 bond length dependence of the analytic representation well reproduce the input data.

  1. Quantum mechanics of effective potential at a metal surface

    NASA Astrophysics Data System (ADS)

    Solomatin, Alexander

    In this thesis we study the nonuniform electron density system at a metal-vacuum interface via the corresponding local effective potential confining the electrons, the metal being represented by the jellium and structureless pseudopotential models. The study is performed within conventional Kohn-Sham (KS) density-functional theory and its recently derived quantum-mechanical interpretation. In the latter, properties are determined in terms of the separate electron correlations due to the Pauli exclusion principle, Coulomb repulsion and the correlation contribution to the kinetc energy. We have derived the exact analytical structure, valid for self-consistent orbitals, of the KS theory exchange potential in the classically forbidden region. This structure is image-potential-like of the form -alphasb{KS,x}(beta)chi where the parameter betasp2 is the ratio of the surface barrier height to the metal Fermi energy. For a Wigner-Seitz radius of rsb{s} = 4.1, which is approximately that for which jellium metal is stable, the decay coefficient is precisely 1/4. Over the metallic range of densities rsb{s} = 2-6, the coefficient ranges from 0.195 to 0.274. Thus, if the asymptotic structure of the KS exchange-correlation potential is the image potential, then this structure is due principally to KS exchange effects, the KS correlation contribution being an order of magnitude smaller. These results, then lead to the concept of an 'image' charge localized to the surface region for asymptotic positions of the electron. We have further derived the exact analytical structure in the vacuum of the Slater exchange potential, and of the Pauli-correlation and correlation-kinetic components of the KS exchange potential. These structures are all image-potential-like, decaying respectively as -alphasb{S}(beta)chi,\\ -alphasb{W}(beta)chi and alphasbsp{tsb{c}}{(1)}(beta)/chi. The Pauli-correlation component constitutes the major fraction of the KS exchange potential asymptotically, but there

  2. Temporal extent of surface potentials between closely spaced metals.

    PubMed

    Pollack, S E; Schlamminger, S; Gundlach, J H

    2008-08-15

    Variations in the electrostatic surface potential between the proof mass and electrode housing in the space-based gravitational wave mission Laser Interferometer Space Antenna (LISA) is one of the largest contributors of noise at frequencies below a few mHz. Torsion balances provide an ideal test bed for investigating these effects in conditions emulative of LISA. Our apparatus consists of a Au coated Cu plate brought near a Au coated Si plate pendulum suspended from a thin W wire. We have measured a white noise level of 30 microV/sqrt Hz above approximately 0.1 mHz, rising at lower frequencies, for the surface potential variations between these two closely spaced metals.

  3. Three-dimensional potential energy surface of Ar–CO

    SciTech Connect

    Sumiyoshi, Yoshihiro; Endo, Yasuki

    2015-01-14

    A three-dimensional intermolecular potential energy surface of the Ar–CO complex has been determined by fitting most of the previously reported spectroscopic data, where observed transition frequencies by microwave, millimeter-wave, submillimeter-wave, and infrared spectroscopy were reproduced simultaneously within their experimental accuracies. A free rotor model Hamiltonian considering all the freedom of motions for an atom-diatom system was applied to calculate vibration-rotation energies. A three-dimensional potential energy surface obtained by ab initio calculations at the CCSD(T)-F12b/aug-cc-pV5Z level of theory was parameterized by a model function consisting of 46 parameters. They were used as initial values for the least-squares analysis of the experimental data. A total of 20 parameters were optimized to reproduce all the spectroscopic data.

  4. Three-dimensional potential energy surface of Ar-CO.

    PubMed

    Sumiyoshi, Yoshihiro; Endo, Yasuki

    2015-01-14

    A three-dimensional intermolecular potential energy surface of the Ar-CO complex has been determined by fitting most of the previously reported spectroscopic data, where observed transition frequencies by microwave, millimeter-wave, submillimeter-wave, and infrared spectroscopy were reproduced simultaneously within their experimental accuracies. A free rotor model Hamiltonian considering all the freedom of motions for an atom-diatom system was applied to calculate vibration-rotation energies. A three-dimensional potential energy surface obtained by ab initio calculations at the CCSD(T)-F12b/aug-cc-pV5Z level of theory was parameterized by a model function consisting of 46 parameters. They were used as initial values for the least-squares analysis of the experimental data. A total of 20 parameters were optimized to reproduce all the spectroscopic data.

  5. Non-adiabatic transition probability dependence on conical intersection topography

    NASA Astrophysics Data System (ADS)

    Malhado, João Pedro; Hynes, James T.

    2016-11-01

    We derive a closed form analytical expression for the non-adiabatic transition probability for a distribution of trajectories passing through a generic conical intersection (CI), based on the Landau-Zener equation for the non-adiabatic transition probability for a single straight-line trajectory in the CI's vicinity. We investigate the non-adiabatic transition probability's variation with topographical features and find, for the same crossing velocity, no intrinsic difference in efficiency at promoting non-adiabatic decay between peaked and sloped CIs, a result in contrast to the commonly held view. Any increased efficiency of peaked over sloped CIs is thus due to dynamical effects rather than to any increased transition probability of topographical origin. It is also shown that the transition probability depends in general on the direction of approach to the CI, and that the coordinates' reduced mass can affect the transition probability via its influence on the CI topography in mass-scaled coordinates. The resulting predictions compare well with surface hopping simulation results.

  6. Non-adiabatic transition probability dependence on conical intersection topography.

    PubMed

    Malhado, João Pedro; Hynes, James T

    2016-11-21

    We derive a closed form analytical expression for the non-adiabatic transition probability for a distribution of trajectories passing through a generic conical intersection (CI), based on the Landau-Zener equation for the non-adiabatic transition probability for a single straight-line trajectory in the CI's vicinity. We investigate the non-adiabatic transition probability's variation with topographical features and find, for the same crossing velocity, no intrinsic difference in efficiency at promoting non-adiabatic decay between peaked and sloped CIs, a result in contrast to the commonly held view. Any increased efficiency of peaked over sloped CIs is thus due to dynamical effects rather than to any increased transition probability of topographical origin. It is also shown that the transition probability depends in general on the direction of approach to the CI, and that the coordinates' reduced mass can affect the transition probability via its influence on the CI topography in mass-scaled coordinates. The resulting predictions compare well with surface hopping simulation results.

  7. New analytical potential energy surface for the F(2P)+CH4 hydrogen abstraction reaction: kinetics and dynamics.

    PubMed

    Espinosa-García, J; Bravo, J L; Rangel, C

    2007-04-12

    A new potential energy surface for the gas-phase F(2P)+CH4 reaction and its deuterated analogues is reported, and its kinetics and dynamics are studied exhaustively. This semiempirical surface is completely symmetric with respect to the permutation of the four methane hydrogen atoms, and it is calibrated to reproduce the topology of the reaction and the experimental thermal rate constants. For the kinetics, the thermal rate constants were calculated using variational transition-state theory with semiclassical transmission coefficients over a wide temperature range, 180-500 K. The theoretical results reproduce the experimental variation with temperature. The influence of the tunneling factor is negligible, due to the flattening of the surface in the entrance valley, and we found a direct dependence on temperature, and therefore positive and small activation energies, in agreement with experiment. Two sets of kinetic isotope effects were calculated, and they show good agreement with the sparse experimental data. The coupling between the reaction coordinate and the vibrational modes shows qualitatively that the FH stretching and the CH3 umbrella bending modes in the products appear vibrationally excited. The dynamics study was performed using quasi-classical trajectory calculations, including corrections to avoid zero-point energy leakage along the trajectories. First, we found that the FH(nu',j') rovibrational distributions agree with experiment. Second, the excitation function presents an oscillatory pattern, reminiscent of a reactive resonance. Third, the state specific scattering distributions present reasonable agreement with experiment, and as the FH(nu') vibrational state increases the scattering angle becomes more forward. These kinetics and dynamics results seem to indicate that a single, adiabatic potential energy surface is adequate to describe this reaction, and the reasonable agreement with experiment (always qualitative and sometimes quantitative) lends

  8. Full-dimensional ground- and excited-state potential energy surfaces and state couplings for photodissociation of thioanisole

    NASA Astrophysics Data System (ADS)

    Li, Shaohong L.; Truhlar, Donald G.

    2017-02-01

    Analytic potential energy surfaces (PESs) and state couplings of the ground and two lowest singlet excited states of thioanisole (C6H5SCH3) are constructed in a diabatic representation based on electronic structure calculations including dynamic correlation. They cover all 42 internal degrees of freedom and a wide range of geometries including the Franck-Condon region and the reaction valley along the breaking S-CH3 bond with the full ranges of the torsion angles. The parameters in the PESs and couplings are fitted to the results of smooth diabatic electronic structure calculations including dynamic electron correlation by the extended multi-configurational quasi-degenerate perturbation theory method for the adiabatic state energies followed by diabatization by the fourfold way. The fit is accomplished by the anchor points reactive potential method with two reactive coordinates and 40 nonreactive degrees of freedom, where the anchor-point force fields are obtained with a locally modified version of the QuickFF package. The PESs and couplings are suitable for study of the topography of the trilayer potential energy landscape and for electronically nonadiabatic molecular dynamics simulations of the photodissociation of the S-CH3 bond.

  9. Full-dimensional ground- and excited-state potential energy surfaces and state couplings for photodissociation of thioanisole.

    PubMed

    Li, Shaohong L; Truhlar, Donald G

    2017-02-14

    Analytic potential energy surfaces (PESs) and state couplings of the ground and two lowest singlet excited states of thioanisole (C6H5SCH3) are constructed in a diabatic representation based on electronic structure calculations including dynamic correlation. They cover all 42 internal degrees of freedom and a wide range of geometries including the Franck-Condon region and the reaction valley along the breaking S-CH3 bond with the full ranges of the torsion angles. The parameters in the PESs and couplings are fitted to the results of smooth diabatic electronic structure calculations including dynamic electron correlation by the extended multi-configurational quasi-degenerate perturbation theory method for the adiabatic state energies followed by diabatization by the fourfold way. The fit is accomplished by the anchor points reactive potential method with two reactive coordinates and 40 nonreactive degrees of freedom, where the anchor-point force fields are obtained with a locally modified version of the QuickFF package. The PESs and couplings are suitable for study of the topography of the trilayer potential energy landscape and for electronically nonadiabatic molecular dynamics simulations of the photodissociation of the S-CH3 bond.

  10. Electronic structure, molecular bonding and potential energy surfaces

    SciTech Connect

    Ruedenberg, K.

    1993-12-01

    By virtue of the universal validity of the generalized Born-Oppenheimer separation, potential energy surfaces (PES`) represent the central conceptual as well as quantitative entities of chemical physics and provide the basis for the understanding of most physicochemical phenomena in many diverse fields. The research in this group deals with the elucidation of general properties of PES` as well as with the quantitative determination of PES` for concrete systems, in particular pertaining to reactions involving carbon, oxygen, nitrogen and hydrogen molecules.

  11. Wettability patterning of hydroxyapatite nanobioceramics induced by surface potential modification

    SciTech Connect

    Aronov, D.; Rosenman, G.; Karlov, A.; Shashkin, A.

    2006-04-17

    Hydroxyapatite is known as a substrate for effective adhesion of various biological cells and bacteria as well implantable biomimetic material replacing defective bone tissues. It is found that low energy electron irradiation induces its strong surface potential variation and gives rise to pronounced wettability modification. The found electron-modulation method of the hydroxyapatite wettability enables both wettability switching and its microscopic patterning, which may be used for fabrication of spatially arrayed hydroxyapatite for biological cells immobilization, gene transfer, etc.

  12. Downwash-velocity potential method for oscillating surfaces.

    NASA Technical Reports Server (NTRS)

    Haviland, J. K.; Yoo, Y. S.

    1973-01-01

    The application of the downwash-velocity potential method to the case of oscillating surfaces is developed, and calculated forces are given on rectangular airfoils of aspect ratio two rotating about midchord in subsonic flows. These are compared with other results published in the literature for reduced frequencies up to nine-tenths, and for Mach numbers up to nine-tenths. The concept of 'aerodynamic elements' is presented, the computed results representing three possible types of rectangular element.

  13. Theoretical characterization of the potential energy surface for NH + NO

    NASA Technical Reports Server (NTRS)

    Walch, Stephen P.

    1993-01-01

    The potential energy surface for NH + NO was characterized using complete active space self-consistent field (CASSCF) gradient calculation to determine the stationary point geometries and frequencies followed by CASSCF/internally contracted configuration interaction calculations to refine the energetics. The present results are in qualitative accord with the BAC-MP4 calculations, but there are differences as large as 8 kcal/mol in the detailed energetics.

  14. MCSCF potential energy surface for photodissociation of formaldehyde

    NASA Technical Reports Server (NTRS)

    Jaffe, R. L.; Morokuma, K.

    1976-01-01

    The ground state potential energy surface for the dissociation of formaldehyde (H2CO to H2 and CO) is calculated with the ab initio MCSCF method with an extended (4-31G) basis set. The location, barrier height, and force constants of the transition state are determined, and the normal coordinate analysis is carried out. The calculated barrier height is 4.5 eV. Based on the calculated quantities, the detailed mechanism of the photochemical dissociation is discussed.

  15. Theoretical studies of potential energy surfaces and computational methods

    SciTech Connect

    Shepard, R.

    1993-12-01

    This project involves the development, implementation, and application of theoretical methods for the calculation and characterization of potential energy surfaces involving molecular species that occur in hydrocarbon combustion. These potential energy surfaces require an accurate and balanced treatment of reactants, intermediates, and products. This difficult challenge is met with general multiconfiguration self-consistent-field (MCSCF) and multireference single- and double-excitation configuration interaction (MRSDCI) methods. In contrast to the more common single-reference electronic structure methods, this approach is capable of describing accurately molecular systems that are highly distorted away from their equilibrium geometries, including reactant, fragment, and transition-state geometries, and of describing regions of the potential surface that are associated with electronic wave functions of widely varying nature. The MCSCF reference wave functions are designed to be sufficiently flexible to describe qualitatively the changes in the electronic structure over the broad range of geometries of interest. The necessary mixing of ionic, covalent, and Rydberg contributions, along with the appropriate treatment of the different electron-spin components (e.g. closed shell, high-spin open-shell, low-spin open shell, radical, diradical, etc.) of the wave functions, are treated correctly at this level. Further treatment of electron correlation effects is included using large scale multireference CI wave functions, particularly including the single and double excitations relative to the MCSCF reference space. This leads to the most flexible and accurate large-scale MRSDCI wave functions that have been used to date in global PES studies.

  16. A Global Analytical Representation of the Potential Energy Surface of the FHF(-) Anion.

    PubMed

    Cornaton, Yann; Marquardt, Roberto

    2016-08-04

    A global analytical representation of the potential energy hypersurface of the lowest adiabatic electronic state of the FHF(-) anion is derived from ab initio calculations at the coupled cluster level of theory with full single and double and perturbative triple excitations using explicitly correlated atomic basis functions. The new compact function of interatomic distances combines covalent short-range and long-range electrostatic interaction forms and assesses accurately both the lowest reaction channels between the F(-) and HF fragments, with reaction enthalpies to within 1 kJ mol(-1), as well as vibrational terms to within 1.5 cm(-1) deviation from experimental values.

  17. Novel mixture model for the representation of potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Pham, Tien Lam; Kino, Hiori; Terakura, Kiyoyuki; Miyake, Takashi; Dam, Hieu Chi

    2016-10-01

    We demonstrate that knowledge of chemical physics on a materials system can be automatically extracted from first-principles calculations using a data mining technique; this information can then be utilized to construct a simple empirical atomic potential model. By using unsupervised learning of the generative Gaussian mixture model, physically meaningful patterns of atomic local chemical environments can be detected automatically. Based on the obtained information regarding these atomic patterns, we propose a chemical-structure-dependent linear mixture model for estimating the atomic potential energy. Our experiments show that the proposed mixture model significantly improves the accuracy of the prediction of the potential energy surface for complex systems that possess a large diversity in their local structures.

  18. The H 2O ++ Ground State Potential Energy Surface

    NASA Astrophysics Data System (ADS)

    Bunker, P. R.; Bludsky, Ota; Jensen, Per; Wesolowski, S. S.; Van Huis, T. J.; Yamaguchi, Y.; Schaefer, H. F.

    1999-12-01

    At the correlation-consistent polarized-valence quadruple-zeta complete active space self-consistent field second-order configuration interaction level of ab initio theory (cc-pVQZ CASSCF-SOCI), we calculated 129 points on the ground electronic state potential energy surface of the water dication H2O++; this calculation includes the energy of X3Σ- OH+ at equilibrium and the energy of the triplet oxygen atom. We determined the parameters in an analytical function that represents this surface out to the (OH+ + H+) and (O + 2H+) dissociation limits, for bending angles from 70 to 180°. There is a metastable minimum in this surface, at an energy of 43 600 cm-1 above the H+ + OH+ dissociation energy, and the geometry at this minimum is linear (D∞h), with an OH bond length of 1.195 Å. On the path to dissociation to H+ + OH+, there is a saddle point at an energy of 530 cm-1 above the minimum, and the geometry at the saddle point is linear (C∞ Kv) with OH bond lengths of 1.121 and 1.489 Å. Using the stabilization method, we calculated the lowest resonance on this surface. Relative to the metastable local minimum on the potential energy surface, the position of the lowest resonance for H2O++, D2O++, and T2O++ is 1977(85), 1473(25), and 1249(10) cm-1, respectively, where the width of each resonance (in cm-1) is given in parentheses.

  19. Quantum and classical dynamics in adiabatic computation

    NASA Astrophysics Data System (ADS)

    Crowley, P. J. D.; Äńurić, T.; Vinci, W.; Warburton, P. A.; Green, A. G.

    2014-10-01

    Adiabatic transport provides a powerful way to manipulate quantum states. By preparing a system in a readily initialized state and then slowly changing its Hamiltonian, one may achieve quantum states that would otherwise be inaccessible. Moreover, a judicious choice of final Hamiltonian whose ground state encodes the solution to a problem allows adiabatic transport to be used for universal quantum computation. However, the dephasing effects of the environment limit the quantum correlations that an open system can support and degrade the power of such adiabatic computation. We quantify this effect by allowing the system to evolve over a restricted set of quantum states, providing a link between physically inspired classical optimization algorithms and quantum adiabatic optimization. This perspective allows us to develop benchmarks to bound the quantum correlations harnessed by an adiabatic computation. We apply these to the D-Wave Vesuvius machine with revealing—though inconclusive—results.

  20. 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

  1. Oscillating streaming potential measurement system for macroscopic surfaces

    NASA Astrophysics Data System (ADS)

    Reischl, Martin; Köstler, Stefan; Kellner, Gerhard; Stana-Kleinschek, Karin; Ribitsch, Volker

    2008-11-01

    A method and instrumentation is described capable of streaming potential measurements of various macroscopic surfaces. It differs from other approaches due to the creation of an oscillatory flow of electrolyte solutions through or alongside the sample. This technique offers a wide range of applied flow frequency and amplitude resulting in a fast and highly accurate measurement. This enables the streaming potential detection at rather high ionic strength and in a short time regime, which allows the monitoring of adsorption processes. Streaming potential and applied pressure are measured simultaneously, together with the specific conductivity of the bulk solution, pH value, and temperature. Combining these data, the zeta potential (ζ ) for many different material types (fibers, films, foils, granules, and particles) can be calculated. The apparatus comprises reliable and robust measurements, simple handling, a high degree of automation, and advanced software control. With this setup, automated pH and concentration dependent ζ-potential measurements are possible for a variety of analytes and adsorbing species (e.g., ionic strength, surfactants, polyelectrolytes, and proteins); time-resolved measurements are facilitated down to the seconds time scale. The device allows the necessary sample preparation and equilibration outside the instrument using exchangeable sample holders. This offers the opportunity of high sample throughput.

  2. Manipulation of the graphene surface potential by ion irradiation

    SciTech Connect

    Ochedowski, O.; Kleine Bussmann, B.; Schleberger, M.; Ban d'Etat, B.; Lebius, H.

    2013-04-15

    We show that the work function of exfoliated single layer graphene can be modified by irradiation with swift (E{sub kin}=92 MeV) heavy ions under glancing angles of incidence. Upon ion impact individual surface tracks are created in graphene on silicon carbide. Due to the very localized energy deposition characteristic for ions in this energy range, the surface area which is structurally altered is limited to Almost-Equal-To 0.01 {mu}m{sup 2} per track. Kelvin probe force microscopy reveals that those surface tracks consist of electronically modified material and that a few tracks suffice to shift the surface potential of the whole single layer flake by Almost-Equal-To 400 meV. Thus, the irradiation turns the initially n-doped graphene into p-doped graphene with a hole density of 8.5 Multiplication-Sign 10{sup 12} holes/cm{sup 2}. This doping effect persists even after heating the irradiated samples to 500 Degree-Sign C. Therefore, this charge transfer is not due to adsorbates but must instead be attributed to implanted atoms. The method presented here opens up a way to efficiently manipulate the charge carrier concentration of graphene.

  3. Surface charge potentiates conduction through the cardiac ryanodine receptor channel

    PubMed Central

    1994-01-01

    Single channel currents through cardiac sarcoplasmic reticulum (SR) Ca2+ release channels were measured in very low levels of current carrier (e.g., 1 mM Ba2+). The hypothesis that surface charge contributes to these anomalously large single channel currents was tested by changing ionic strength and surface charge density. Channel identity and sidedness was pharmacologically determined. At low ionic strength (20 mM Cs+), Cs+ conduction in the lumen-->myoplasm (L-->M) direction was significantly greater than in the reverse direction (301.7 +/- 92.5 vs 59.8 +/- 38 pS, P < 0.001; mean +/- SD, t test). The Cs+ concentration at which conduction reached half saturation was asymmetric (32 vs 222 mM) and voltage independent. At high ionic strength (400 mM Cs+), conduction in both direction saturated at 550 +/- 32 pS. Further, neutralization of carboxyl groups on the lumenal side of the channel significantly reduced conduction (333.0 +/- 22.5 vs 216.2 +/- 24.4 pS, P < 0.002). These results indicate that negative surface charge exists near the lumenal mouth of the channel but outside the electric field of the membrane. In vivo, this surface charge may potentiate conduction by increasing the local Ca2+ concentration and thus act as a preselection filter for this poorly selective channel. PMID:8035165

  4. Adiabatic calorimetric decomposition studies of 50 wt.% hydroxylamine/water.

    PubMed

    Cisneros, L O; Rogers, W J; Mannan, M S

    2001-03-19

    Calorimetric data can provide a basis for determining potential hazards in reactions, storage, and transportation of process chemicals. This work provides calorimetric data for the thermal decomposition behavior in air of 50wt.% hydroxylamine/water (HA), both with and without added stabilizers, which was measured in closed cells with an automatic pressure tracking adiabatic calorimeter (APTAC). Among the data provided are onset temperatures, reaction order, activation energies, pressures of noncondensable products, thermal stability at 100 degrees C, and the effect of HA storage time. Discussed also are the catalytic effects of carbon steel, stainless steel, stainless steel with silica coating, inconel, titanium, and titanium with silica coating on the reaction self-heat rates and onset temperatures. In borosilicate glass cells, HA was relatively stable at temperatures up to 133 degrees C, where the HA decomposition self-heat rate reached 0.05 degrees C/min. The added stabilizers appeared to reduce HA decomposition rates in glass cells and at ambient temperatures. The tested metals and metal surfaces coated with silica acted as catalysts to lower the onset temperatures and increase the self-heat rates.

  5. Pseudospectral Gaussian quantum dynamics: Efficient sampling of potential energy surfaces.

    PubMed

    Heaps, Charles W; Mazziotti, David A

    2016-04-28

    Trajectory-based Gaussian basis sets have been tremendously successful in describing high-dimensional quantum molecular dynamics. In this paper, we introduce a pseudospectral Gaussian-based method that achieves accurate quantum dynamics using efficient, real-space sampling of the time-dependent basis set. As in other Gaussian basis methods, we begin with a basis set expansion using time-dependent Gaussian basis functions guided by classical mechanics. Unlike other Gaussian methods but characteristic of the pseudospectral and collocation methods, the basis set is tested with N Dirac delta functions, where N is the number of basis functions, rather than using the basis function as test functions. As a result, the integration for matrix elements is reduced to function evaluation. Pseudospectral Gaussian dynamics only requires O(N) potential energy calculations, in contrast to O(N(2)) evaluations in a variational calculation. The classical trajectories allow small basis sets to sample high-dimensional potentials. Applications are made to diatomic oscillations in a Morse potential and a generalized version of the Henon-Heiles potential in two, four, and six dimensions. Comparisons are drawn to full analytical evaluation of potential energy integrals (variational) and the bra-ket averaged Taylor (BAT) expansion, an O(N) approximation used in Gaussian-based dynamics. In all cases, the pseudospectral Gaussian method is competitive with full variational calculations that require a global, analytical, and integrable potential energy surface. Additionally, the BAT breaks down when quantum mechanical coherence is particularly strong (i.e., barrier reflection in the Morse oscillator). The ability to obtain variational accuracy using only the potential energy at discrete points makes the pseudospectral Gaussian method a promising avenue for on-the-fly dynamics, where electronic structure calculations become computationally significant.

  6. On the Potential Predictability of Seasonal Land-Surface Climate

    SciTech Connect

    Phillips, T J

    2001-10-01

    The chaotic behavior of the continental climate of an atmospheric general circulation model is investigated from an ensemble of decadal simulations with common specifications of radiative forcings and monthly ocean boundary conditions, but different initial states of atmosphere and land. The variability structures of key model land-surface processes appear to agree sufficiently with observational estimates to warrant detailed examination of their predictability on seasonal time scales. This predictability is inferred from several novel measures of spatio-temporal reproducibility applied to eleven model variables. The reproducibility statistics are computed for variables in which the seasonal cycle is included or excluded, the former case being most pertinent to climate model simulations, and the latter to predictions of the seasonal anomalies. Because the reproducibility metrics in the latter case are determined in the context of a ''perfectly'' known ocean state, they are properly viewed as estimates of the potential predictability of seasonal climate. Inferences based on these reproducibility metrics are shown to be in general agreement with those derived from more conventional measures of potential predictability. It is found that the land-surface variables which include the seasonal cycle are impacted only marginally by changes in initial conditions; moreover, their seasonal climatologies exhibit high spatial reproducibility. In contrast, the reproducibility of a seasonal land-surface anomaly is generally low, although it is considerably higher in the Tropics; its spatial reproducibility also fluctuates in tandem with warm and cold phases of the El Nino/Southern Oscillation phenomenon. However, the detailed sensitivities to initial conditions depend somewhat on the land-surface process: pressure and temperature anomalies exhibit the highest temporal reproducibilities, while hydrological and turbulent flux anomalies show the highest spatial reproducibilities

  7. Pharmaceutical and biomedical potential of surface engineered dendrimers.

    PubMed

    Satija, Jitendra; Gupta, Umesh; Jain, Narendra Kumar

    2007-01-01

    Dendrimers are hyperbranched, globular, monodisperse, nanometric polymeric architecture, having definite molecular weight, shape, and size (which make these an inimitable and optimum carrier molecule in pharmaceutical field). Dendritic architecture is having immense potential over the other carrier systems, particularly in the field of drug delivery because of their unique properties, such as structural uniformity, high purity, efficient membrane transport, high drug pay load, targeting potential, and good colloidal, biological, and shelf stability. Despite their enormous applicability in different areas, the inherent cytotoxicity, reticuloendothelial system (RES) uptake, drug leakage, immunogenicity, and hemolytic toxicity restricted their use in clinical applications, which is primarily associated with cationic charge present on the periphery due to amine groups. To overcome this toxic nature of dendrimers, some new types of nontoxic, biocompatible, and biodegradable dendrimers have been developed (e.g., polyester dendrimer, citric acid dendrimer, arginine dendrimer, carbohydrate dendrimers, etc.). The surface engineering of parent dendrimers is graceful and convenient strategy, which not only shields the positive charge to make this carrier more biomimetic but also improves the physicochemical and biological behavior of parent dendrimers. Thus, surface modification chemistry of parent dendrimers holds promise in pharmaceutical applications (such as solubilization, improved drug encapsulation, enhanced gene transfection, sustained and controlled drug release, intracellular targeting) and in the diagnostic field. Development of multifunctional dendrimer holds greater promise toward the biomedical applications because a number of targeting ligands determine specificity in the same manner as another type of group would secure stability in biological milieu and prolonged circulation, whereas others facilitate their transport through cell membranes. Therefore, as a

  8. Molecular dynamics investigations of the dissociation of SiO2 on an ab initio potential energy surface obtained using neural network methods.

    PubMed

    Agrawal, Paras M; Raff, Lionel M; Hagan, Martin T; Komanduri, Ranga

    2006-04-07

    The neural network (NN) procedure to interpolate ab initio data for the purpose of molecular dynamics (MD) simulations has been tested on the SiO(2) system. Unlike other similar NN studies, here, we studied the dissociation of SiO(2) without the initial use of any empirical potential. During the dissociation of SiO(2) into Si+O or Si+O(2), the spin multiplicity of the system changes from singlet to triplet in the first reaction and from singlet to pentet in the second. This paper employs four potential surfaces. The first is a NN fit [NN(STP)] to a database comprising the lowest of the singlet, triplet, and pentet energies obtained from density functional calculations in 6673 nuclear configurations. The other three potential surfaces are obtained from NN fits to the singlet, triplet, and pentet-state energies. The dissociation dynamics on the singlet-state and NN(STP) surfaces are reported. The results obtained using the singlet surface correspond to those expected if the reaction were to occur adiabatically. The dynamics on the NN(STP) surface represent those expected if the reaction follows a minimum-energy pathway. This study on a small system demonstrates the application of NNs for MD studies using ab initio data when the spin multiplicity of the system changes during the dissociation process.

  9. Molecular dynamics investigations of the dissociation of SiO2 on an ab initio potential energy surface obtained using neural network methods

    NASA Astrophysics Data System (ADS)

    Agrawal, Paras M.; Raff, Lionel M.; Hagan, Martin T.; Komanduri, Ranga

    2006-04-01

    The neural network (NN) procedure to interpolate ab initio data for the purpose of molecular dynamics (MD) simulations has been tested on the SiO2 system. Unlike other similar NN studies, here, we studied the dissociation of SiO2 without the initial use of any empirical potential. During the dissociation of SiO2 into Si +O or Si +O2, the spin multiplicity of the system changes from singlet to triplet in the first reaction and from singlet to pentet in the second. This paper employs four potential surfaces. The first is a NN fit [NN(STP)] to a database comprising the lowest of the singlet, triplet, and pentet energies obtained from density functional calculations in 6673 nuclear configurations. The other three potential surfaces are obtained from NN fits to the singlet, triplet, and pentet-state energies. The dissociation dynamics on the singlet-state and NN(STP) surfaces are reported. The results obtained using the singlet surface correspond to those expected if the reaction were to occur adiabatically. The dynamics on the NN(STP) surface represent those expected if the reaction follows a minimum-energy pathway. This study on a small system demonstrates the application of NNs for MD studies using ab initio data when the spin multiplicity of the system changes during the dissociation process.

  10. The electrochemical surface forces apparatus: the effect of surface roughness, electrostatic surface potentials, and anodic oxide growth on interaction forces, and friction between dissimilar surfaces in aqueous solutions.

    PubMed

    Valtiner, Markus; Banquy, Xavier; Kristiansen, Kai; Greene, George W; Israelachvili, Jacob N

    2012-09-11

    We present a newly designed electrochemical surface forces apparatus (EC-SFA) that allows control and measurement of surface potentials and interfacial electrochemical reactions with simultaneous measurement of normal interaction forces (with nN resolution), friction forces (with μN resolution), and distances (with Å resolution) between apposing surfaces. We describe three applications of the developed EC-SFA and discuss the wide-range of potential other applications. In particular, we describe measurements of (1) force-distance profiles between smooth and rough gold surfaces and apposing self-assembled monolayer-covered smooth mica surfaces; (2) the effective changing thickness of anodically growing oxide layers with Å-accuracy on rough and smooth surfaces; and (3) friction forces evolving at a metal-ceramic contact, all as a function of the applied electrochemical potential. Interaction forces between atomically smooth surfaces are well-described using DLVO theory and the Hogg-Healy-Fuerstenau approximation for electric double layer interactions between dissimilar surfaces, which unintuitively predicts the possibility of attractive double layer forces between dissimilar surfaces whose surface potentials have similar sign, and repulsive forces between surfaces whose surface potentials have opposite sign. Surface roughness of the gold electrodes leads to an additional exponentially repulsive force in the force-distance profiles that is qualitatively well described by an extended DLVO model that includes repulsive hydration and steric forces. Comparing the measured thickness of the anodic gold oxide layer and the charge consumed for generating this layer allowed the identification of its chemical structure as a hydrated Au(OH)(3) phase formed at the gold surface at high positive potentials. The EC-SFA allows, for the first time, one to look at complex long-term transient effects of dynamic processes (e.g., relaxation times), which are also reflected in friction

  11. Coupling of surface energy with electric potential makes superhydrophobic surfaces corrosion-resistant.

    PubMed

    Ramachandran, Rahul; Nosonovsky, Michael

    2015-10-14

    We study the correlation of wetting properties and corrosion rates on hydrophobized cast iron. Samples of different surface roughnesses (abraded by sandpaper) are studied without coating and with two types of hydrophobic coatings (stearic acid and a liquid repelling spray). The contact angles and contact angle hysteresis are measured using a goniometer while corrosion rates are measured by a potentiodynamic polarization test. The data show a decrease in corrosion current density and an increase in corrosion potential after superhydrophobization. A similar trend is also found in the recent literature data. We conclude that a decrease in the corrosion rate can be attributed to the changing open circuit potential of a coated surface and increased surface area making the non-homogeneous (Cassie-Baxter) state possible. We interpret these results in light of the idea that the inherent surface energy is coupled with the electric potential in accordance with the Lippmann law of electrowetting and Le Châtelier's principle and, therefore, hydrophobization leads to a decrease in the corrosion potential. This approach can be used for novel anti-corrosive coatings.

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

    SciTech Connect

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

    2008-10-15

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

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

    SciTech Connect

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

    2004-06-01

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

  14. Forces on nuclei moving on autoionizing molecular potential energy surfaces.

    PubMed

    Moiseyev, Nimrod

    2017-01-14

    Autoionization of molecular systems occurs in diatomic molecules and in small biochemical systems. Quantum chemistry packages enable calculation of complex potential energy surfaces (CPESs). The imaginary part of the CPES is associated with the autoionization decay rate, which is a function of the molecular structure. Molecular dynamics simulations, within the framework of the Born-Oppenheimer approximation, require the definition of a force field. The ability to calculate the forces on the nuclei in bio-systems when autoionization takes place seems to rely on an understanding of radiative damages in RNA and DNA arising from the release of slow moving electrons which have long de Broglie wavelengths. This work addresses calculation of the real forces on the nuclei moving on the CPES. By using the transformation of the time-dependent Schrödinger equation, previously used by Madelung, we proved that the classical forces on nuclei moving on the CPES correlated with the gradient of the real part of the CPES. It was proved that the force on the nuclei of the metastable molecules is time independent although the probability to detect metastable molecules exponentially decays. The classical force is obtained from the transformed Schrödinger equation when ℏ=0 and the Schrödinger equation is reduced to the classical (Newtonian) equations of motion. The forces on the nuclei regardless on what potential energy surface they move (parent CPES or product real PESs) vary in time due to the autoionization process.

  15. An Ab Initio Based Potential Energy Surface for Water

    NASA Technical Reports Server (NTRS)

    Partridge, Harry; Schwenke, David W.; Langhoff, Stephen R. (Technical Monitor)

    1996-01-01

    We report a new determination of the water potential energy surface. A high quality ab initio potential energy surface (PES) and dipole moment function of water have been computed. This PES is empirically adjusted to improve the agreement between the computed line positions and those from the HITRAN 92 data base. The adjustment is small, nonetheless including an estimate of core (oxygen 1s) electron correlation greatly improves the agreement with experiment. Of the 27,245 assigned transitions in the HITRAN 92 data base for H2(O-16), the overall root mean square (rms) deviation between the computed and observed line positions is 0.125/cm. However the deviations do not correspond to a normal distribution: 69% of the lines have errors less than 0.05/cm. Overall, the agreement between the line intensities computed in the present work and those contained in the data base is quite good, however there are a significant number of line strengths which differ greatly.

  16. Adiabatic heating in impulsive solar flares

    NASA Technical Reports Server (NTRS)

    Maetzler, C.; Bai, T.; Crannell, C. J.; Frost, K. J.

    1977-01-01

    The dynamic X-ray spectra of two simple, impulsive solar flares are examined together with H alpha, microwave and meter wave radio observations. X-ray spectra of both events were characteristic of thermal bremsstrahlung from single temperature plasmas. The symmetry between rise and fall was found to hold for the temperature and emission measure. The relationship between temperature and emission measure was that of an adiabatic compression followed by adiabatic expansion; the adiabatic index of 5/3 indicated that the electron distribution remained isotropic. Observations in H alpha provided further evidence for compressive energy transfer.

  17. Arbitrary amplitude electro-acoustic solitary waves in an adiabatic dusty plasma

    NASA Astrophysics Data System (ADS)

    Tanjia, Fatema; Mamun, A. A.

    2008-12-01

    The properties of different types of electro-acoustic (namely ion-acoustic (IA), dust ion-acoustic (DIA), and dust-acoustic (DA)) solitary waves (SWs) in an adiabatic dusty plasma (containing negatively charged cold dust, adiabatic hot ions and inertia-less adiabatic hot electrons) are investigated by the pseudo-potential approach. The combined effects of the adiabatic electrons and ions, and negatively charged dust on the basic properties (critical Mach number, amplitude and width) of the arbitrary amplitude electro-acoustic SWs are systematically and explicitly examined. It is found that the combined effects of the adiabatic electrons and ions, and negatively charged dust significantly modify the basic properties (critical Mach number, amplitude and width) of the SWs. It is also found that due to the effect of the adiabaticity of electrons, the negative DIA SWs (which are found to exist in a dusty plasma containing isothermal electrons, cold ions and negatively charged static dust) disappear, i.e. due to the effect of adiabatic electrons, one cannot have negative DIA SWs for any possible set of dusty plasma parameters.

  18. Surface-wave potential for triggering tectonic (nonvolcanic) tremor

    USGS Publications Warehouse

    Hill, D.P.

    2010-01-01

    Source processes commonly posed to explain instances of remote dynamic triggering of tectonic (nonvolcanic) tremor by surface waves include frictional failure and various modes of fluid activation. The relative potential for Love- and Rayleigh-wave dynamic stresses to trigger tectonic tremor through failure on critically stressed thrust and vertical strike-slip faults under the Coulomb-Griffith failure criteria as a function of incidence angle is anticorrelated over the 15- to 30-km-depth range that hosts tectonic tremor. Love-wave potential is high for strike-parallel incidence on low-angle reverse faults and null for strike-normal incidence; the opposite holds for Rayleigh waves. Love-wave potential is high for both strike-parallel and strike-normal incidence on vertical, strike-slip faults and minimal for ~45?? incidence angles. The opposite holds for Rayleigh waves. This pattern is consistent with documented instances of tremor triggered by Love waves incident on the Cascadia mega-thrust and the San Andreas fault (SAF) in central California resulting from shear failure on weak faults (apparent friction, ????? 0.2). However, documented instances of tremor triggered by surface waves with strike-parallel incidence along the Nankai megathrust beneath Shikoku, Japan, is associated primarily with Rayleigh waves. This is consistent with the tremor bursts resulting from mixed-mode failure (crack opening and shear failure) facilitated by near-lithostatic ambient pore pressure, low differential stress, with a moderate friction coefficient (?? ~ 0.6) on the Nankai subduction interface. Rayleigh-wave dilatational stress is relatively weak at tectonic tremor source depths and seems unlikely to contribute significantly to the triggering process, except perhaps for an indirect role on the SAF in sustaining tremor into the Rayleigh-wave coda that was initially triggered by Love waves.

  19. 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.

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

    DOE PAGES

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

    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

  1. Adiabatic far-field sub-diffraction imaging.

    PubMed

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

    2015-08-10

    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.

  2. 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 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. PMID:26258769

  3. Polarizable interaction potential for water from coupled cluster calculations. I. Analysis of dimer potential energy surface

    NASA Astrophysics Data System (ADS)

    Bukowski, Robert; Szalewicz, Krzysztof; Groenenboom, Gerrit C.; van der Avoird, Ad

    2008-03-01

    A six-dimensional interaction potential for the water dimer has been fitted to ab initio interaction energies computed at 2510 dimer configurations. These energies were obtained by combining the supermolecular second-order energies extrapolated to the complete basis set limit from up to quadruple-zeta quality basis sets with the contribution from the coupled-cluster method including single, double, and noniterative triple excitations computed in a triple-zeta quality basis set. All basis sets were augmented by diffuse functions and supplemented by midbond functions. The energies have been fitted using an analytic form with the induction component represented by a polarizable term, making the potential directly transferable to clusters and the bulk phase. Geometries and energies of stationary points on the potential surface agree well with the results of high-level ab initio geometry optimizations.

  4. CO dimer: new potential energy surface and rovibrational calculations.

    PubMed

    Dawes, Richard; Wang, Xiao-Gang; Carrington, Tucker

    2013-08-15

    The spectrum of CO dimer was investigated by solving the rovibrational Schrödinger equation on a new potential energy surface constructed from coupled-cluster ab initio points. The Schrödinger equation was solved with a Lanczos algorithm. Several 4D (rigid monomer) global ab initio potential energy surfaces (PESs) were made using a previously reported interpolating moving least-squares (IMLS) fitting procedure specialized to describe the interaction of two linear fragments. The potential has two nonpolar minima giving rise to a complicated set of energy level stacks, which are very sensitive to the shapes and relative depths of the two wells. Although the CO dimer has defied previous attempts at an accurate purely ab initio description our best surface yields results in good agreement with experiment. Root-mean-square (rms) fitting errors of less than 0.1 cm(-1) were obtained for each of the fits using 2226 ab initio data at different levels. This allowed direct assessment of the quality of various levels of ab initio theory for prediction of spectra. Our tests indicate that standard CCSD(T) is slow to converge the interaction energy even when sextuple zeta bases as large as ACV6Z are used. The explicitly correlated CCSD(T)-F12b method was found to recover significantly more correlation energy (from singles and doubles) at the CBS limit. Correlation of the core-electrons was found to be important for this system. The best PES was obtained by extrapolation of calculations at the CCSD(T)(AE)-F12b/CVnZ-F12 (n = 3,4) levels. The calculated energy levels were compared to 105 J ≤ 10 levels from experiment. The rms error for 68 levels with J ≤ 6 is only 0.29 cm(-1). The calculated energy levels were assigned stack labels using several tools. New stacks were found. One of them, stack y1, has an energy lower than many previously known stacks and may be observable.

  5. 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.

  6. Adiabatic Quantum Search in Open Systems.

    PubMed

    Wild, Dominik S; Gopalakrishnan, Sarang; Knap, Michael; Yao, Norman Y; Lukin, Mikhail D

    2016-10-07

    Adiabatic quantum algorithms represent a promising approach to universal quantum computation. In isolated systems, a key limitation to such algorithms is the presence of avoided level crossings, where gaps become extremely small. In open quantum systems, the fundamental robustness of adiabatic algorithms remains unresolved. Here, we study the dynamics near an avoided level crossing associated with the adiabatic quantum search algorithm, when the system is coupled to a generic environment. At zero temperature, we find that the algorithm remains scalable provided the noise spectral density of the environment decays sufficiently fast at low frequencies. By contrast, higher order scattering processes render the algorithm inefficient at any finite temperature regardless of the spectral density, implying that no quantum speedup can be achieved. Extensions and implications for other adiabatic quantum algorithms will be discussed.

  7. Adiabatic Quantum Search in Open Systems

    NASA Astrophysics Data System (ADS)

    Wild, Dominik S.; Gopalakrishnan, Sarang; Knap, Michael; Yao, Norman Y.; Lukin, Mikhail D.

    2016-10-01

    Adiabatic quantum algorithms represent a promising approach to universal quantum computation. In isolated systems, a key limitation to such algorithms is the presence of avoided level crossings, where gaps become extremely small. In open quantum systems, the fundamental robustness of adiabatic algorithms remains unresolved. Here, we study the dynamics near an avoided level crossing associated with the adiabatic quantum search algorithm, when the system is coupled to a generic environment. At zero temperature, we find that the algorithm remains scalable provided the noise spectral density of the environment decays sufficiently fast at low frequencies. By contrast, higher order scattering processes render the algorithm inefficient at any finite temperature regardless of the spectral density, implying that no quantum speedup can be achieved. Extensions and implications for other adiabatic quantum algorithms will be discussed.

  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. 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.

  10. Simulation of periodically focused, adiabatic thermal beams

    SciTech Connect

    Chen, C.; Akylas, T. R.; Barton, T. J.; Field, D. M.; Lang, K. M.; Mok, R. V.

    2012-12-21

    Self-consistent particle-in-cell simulations are performed to verify earlier theoretical predictions of adiabatic thermal beams in a periodic solenoidal magnetic focusing field [K.R. Samokhvalova, J. Zhou and C. Chen, Phys. Plasma 14, 103102 (2007); J. Zhou, K.R. Samokhvalova and C. Chen, Phys. Plasma 15, 023102 (2008)]. In particular, results are obtained for adiabatic thermal beams that do not rotate in the Larmor frame. For such beams, the theoretical predictions of the rms beam envelope, the conservations of the rms thermal emittances, the adiabatic equation of state, and the Debye length are verified in the simulations. Furthermore, the adiabatic thermal beam is found be stable in the parameter regime where the simulations are performed.

  11. Accurate quantum wave packet calculations for the F + HCl → Cl + HF reaction on the ground 1(2)A' potential energy surface.

    PubMed

    Bulut, Niyazi; Kłos, Jacek; Alexander, Millard H

    2012-03-14

    We present converged exact quantum wave packet calculations of reaction probabilities, integral cross sections, and thermal rate coefficients for the title reaction. Calculations have been carried out on the ground 1(2)A' global adiabatic potential energy surface of Deskevich et al. [J. Chem. Phys. 124, 224303 (2006)]. Converged wave packet reaction probabilities at selected values of the total angular momentum up to a partial wave of J = 140 with the HCl reagent initially selected in the v = 0, j = 0-16 rovibrational states have been obtained for the collision energy range from threshold up to 0.8 eV. The present calculations confirm an important enhancement of reactivity with rotational excitation of the HCl molecule. First, accurate integral cross sections and rate constants have been calculated and compared with the available experimental data.

  12. An approach to optimised calculations of the potential energy surfaces for the case of electron transfer reactions at a metal/solution interface

    NASA Astrophysics Data System (ADS)

    Bronshtein, Michael D.; Nazmutdinov, Renat R.; Schmickler, Wolfgang

    2004-12-01

    An effective computational scheme to construct the adiabatic potential energy surfaces (APES) along the reaction coordinates for an electron transfer reaction occurring by two steps at a metal electrode is considered in the framework of the Anderson-Newns model. Two Theorems have been proved which predict the existence of all possible solutions of the Anderson-Newns equations at arbitrary values of the key parameters and point out the region for each solution. Asymptotic formulas for solutions near multiple roots have been derived and combined in an effective way with numerical routines. The analysis of some important properties of the APES, which can be of interest for modelling the electrochemical electron transfer processes, is presented as well. The APES describing the reduction of Zn(II) and In(III) aqua-complexes at a mercury electrode have been built and discussed.

  13. Stabilized quasi-Newton optimization of noisy potential energy surfaces

    SciTech Connect

    Schaefer, Bastian; Goedecker, Stefan; Alireza Ghasemi, S.; Roy, Shantanu

    2015-01-21

    Optimizations of atomic positions belong to the most commonly performed tasks in electronic structure calculations. Many simulations like global minimum searches or characterizations of chemical reactions require performing hundreds or thousands of minimizations or saddle computations. To automatize these tasks, optimization algorithms must not only be efficient but also very reliable. Unfortunately, computational noise in forces and energies is inherent to electronic structure codes. This computational noise poses a severe problem to the stability of efficient optimization methods like the limited-memory Broyden–Fletcher–Goldfarb–Shanno algorithm. We here present a technique that allows obtaining significant curvature information of noisy potential energy surfaces. We use this technique to construct both, a stabilized quasi-Newton minimization method and a stabilized quasi-Newton saddle finding approach. We demonstrate with the help of benchmarks that both the minimizer and the saddle finding approach are superior to comparable existing methods.

  14. Stabilized quasi-Newton optimization of noisy potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Schaefer, Bastian; Ghasemi, S. Alireza; Roy, Shantanu; Goedecker, Stefan; Goedecker Group Team

    Optimizations of atomic positions belong to the most frequently performed tasks in electronic structure calculations. Many simulations like global minimum searches or the identification of chemical reaction pathways can require the computation of hundreds or thousands of minimizations or saddle points. To automatize these tasks, optimization algorithms must not only be efficient but also very reliable. Unfortunately, computational noise in forces and energies is inherent to electronic structure codes. This computational noise poses a severe problem to the stability of efficient optimization methods like the limited-memory Broyden-Fletcher-Goldfarb-Shanno algorithm. In this talk a recently published technique that allows to obtain significant curvature information of noisy potential energy surfaces is presented. This technique was used to construct both, a stabilized quasi-Newton minimization method and a stabilized quasi-Newton saddle finding approach. With the help of benchmarks both the minimizer and the saddle finding approach were demonstrated to be superior to comparable existing methods.

  15. Stabilized quasi-Newton optimization of noisy potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Schaefer, Bastian; Alireza Ghasemi, S.; Roy, Shantanu; Goedecker, Stefan

    2015-01-01

    Optimizations of atomic positions belong to the most commonly performed tasks in electronic structure calculations. Many simulations like global minimum searches or characterizations of chemical reactions require performing hundreds or thousands of minimizations or saddle computations. To automatize these tasks, optimization algorithms must not only be efficient but also very reliable. Unfortunately, computational noise in forces and energies is inherent to electronic structure codes. This computational noise poses a severe problem to the stability of efficient optimization methods like the limited-memory Broyden-Fletcher-Goldfarb-Shanno algorithm. We here present a technique that allows obtaining significant curvature information of noisy potential energy surfaces. We use this technique to construct both, a stabilized quasi-Newton minimization method and a stabilized quasi-Newton saddle finding approach. We demonstrate with the help of benchmarks that both the minimizer and the saddle finding approach are superior to comparable existing methods.

  16. Improved DFT Potential Energy Surfaces via Improved Densities.

    PubMed

    Kim, Min-Cheol; Park, Hansol; Son, Suyeon; Sim, Eunji; Burke, Kieron

    2015-10-01

    Density-corrected DFT is a method that cures several failures of self-consistent semilocal DFT calculations by using a more accurate density instead. A novel procedure employs the Hartree-Fock density to bonds that are more severely stretched than ever before. This substantially increases the range of accurate potential energy surfaces obtainable from semilocal DFT for many heteronuclear molecules. We show that this works for both neutral and charged molecules. We explain why and explore more difficult cases, for example, CH(+), where density-corrected DFT results are even better than sophisticated methods like CCSD. We give a simple criterion for when DC-DFT should be more accurate than self-consistent DFT that can be applied for most cases.

  17. An exploration of the ozone dimer potential energy surface

    SciTech Connect

    Azofra, Luis Miguel; Alkorta, Ibon; Scheiner, Steve

    2014-06-28

    The (O{sub 3}){sub 2} dimer potential energy surface is thoroughly explored at the ab initio CCSD(T) computational level. Five minima are characterized with binding energies between 0.35 and 2.24 kcal/mol. The most stable may be characterized as slipped parallel, with the two O{sub 3} monomers situated in parallel planes. Partitioning of the interaction energy points to dispersion and exchange as the prime contributors to the stability, with varying contributions from electrostatic energy, which is repulsive in one case. Atoms in Molecules analysis of the wavefunction presents specific O⋯O bonding interactions, whose number is related to the overall stability of each dimer. All internal vibrational frequencies are shifted to the red by dimerization, particularly the antisymmetric stretching mode whose shift is as high as 111 cm{sup −1}. In addition to the five minima, 11 higher-order stationary points are identified.

  18. A new diabatic representation of the coupled potential energy surfaces for Na(3p P-2) + H2 yields Na(3s S-2) + H2 or NaH + H

    NASA Technical Reports Server (NTRS)

    Halvick, Philippe; Truhlar, Donald G.

    1992-01-01

    A diabatic representation is presented of the coupled potential-energy surfaces for Na(3p P-2) + H2 yields Na (3s S-2) + H2 or NaH + H. The representation is designed to yield, upon diagonalization, realistic values for the two lowest energy adiabatic states at both asymptotes of the chemical reaction as well as near the conical intersection in the three-body interaction region. It is economical to evaluate and portable. It is suitable for dynamics calculations on both the quenching process and the electronically nonadiabatic chemical reaction.

  19. Restructuring of an Ir(210) electrode surface by potential cycling.

    PubMed

    Soliman, Khaled A; Kolb, Dieter M; Kibler, Ludwig A; Jacob, Timo

    2014-01-01

    This study addresses the electrochemical surface faceting and restructuring of Ir(210) single crystal electrodes. Cyclic voltammetry measurements and in situ scanning tunnelling microscopy are used to probe structural changes and variations in the electrochemical behaviour after potential cycling of Ir(210) in 0.1 M H2SO4. Faceted structures are obtained electrochemically as a function of time by cycling at a scanrate of 1 V·s(-1) between -0.28 and 0.70 V vs SCE, i.e., between the onset of hydrogen evolution and the surface oxidation regime. The electrochemical behaviour in sulfuric acid solution is compared with that of thermally faceted Ir(210), which shows a sharp characteristic voltammetric peak for (311) facets. Structures similar to thermally-induced faceted Ir(210) are obtained electrochemically, which typically correspond to polyoriented facets at nano-pyramids. These structures grow anisotropically in a preferred direction and reach a height of about 5 nm after 4 h of cycling. The structural changes are reflected in variations of the electrocatalytic activity towards carbon monoxide adlayer oxidation.

  20. Restructuring of an Ir(210) electrode surface by potential cycling

    PubMed Central

    Soliman, Khaled A; Kolb, Dieter M; Jacob, Timo

    2014-01-01

    Summary This study addresses the electrochemical surface faceting and restructuring of Ir(210) single crystal electrodes. Cyclic voltammetry measurements and in situ scanning tunnelling microscopy are used to probe structural changes and variations in the electrochemical behaviour after potential cycling of Ir(210) in 0.1 M H2SO4. Faceted structures are obtained electrochemically as a function of time by cycling at a scanrate of 1 V·s−1 between −0.28 and 0.70 V vs SCE, i.e., between the onset of hydrogen evolution and the surface oxidation regime. The electrochemical behaviour in sulfuric acid solution is compared with that of thermally faceted Ir(210), which shows a sharp characteristic voltammetric peak for (311) facets. Structures similar to thermally-induced faceted Ir(210) are obtained electrochemically, which typically correspond to polyoriented facets at nano-pyramids. These structures grow anisotropically in a preferred direction and reach a height of about 5 nm after 4 h of cycling. The structural changes are reflected in variations of the electrocatalytic activity towards carbon monoxide adlayer oxidation. PMID:25247118

  1. A highly accurate ab initio potential energy surface for methane

    NASA Astrophysics Data System (ADS)

    Owens, Alec; Yurchenko, Sergei N.; Yachmenev, Andrey; Tennyson, Jonathan; Thiel, Walter

    2016-09-01

    A new nine-dimensional potential energy surface (PES) for methane has been generated using state-of-the-art ab initio theory. The PES is based on explicitly correlated coupled cluster calculations with extrapolation to the complete basis set limit and incorporates a range of higher-level additive energy corrections. These include core-valence electron correlation, higher-order coupled cluster terms beyond perturbative triples, scalar relativistic effects, and the diagonal Born-Oppenheimer correction. Sub-wavenumber accuracy is achieved for the majority of experimentally known vibrational energy levels with the four fundamentals of 12CH4 reproduced with a root-mean-square error of 0.70 cm-1. The computed ab initio equilibrium C-H bond length is in excellent agreement with previous values despite pure rotational energies displaying minor systematic errors as J (rotational excitation) increases. It is shown that these errors can be significantly reduced by adjusting the equilibrium geometry. The PES represents the most accurate ab initio surface to date and will serve as a good starting point for empirical refinement.

  2. 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…

  3. Microscopically derived potential energy surfaces from mostly structural considerations

    SciTech Connect

    Ermamatov, M.J.; Hess, Peter O.

    2016-08-15

    A simple procedure to estimate the quadrupole Potential-Energy-Surface (PES) is presented, using mainly structural information, namely the content of the shell model space and the Pauli exclusion principle. Further microscopic properties are implicitly contained through the use of results from the Möller and Nix tables or experimental information. A mapping to the geometric potential is performed yielding the PES. The General Collective Model is used in order to obtain an estimate on the spectrum and quadrupole transitions, adjusting only the mass parameter. First, we test the conjecture on known nuclei, deriving the PES and compare them to known data. We will see that the PES approximates very well the structure expected. Having acquired a certain confidence, we predict the PES of several chain of isotopes of heavy and super-heavy nuclei and at the end we investigate the structure of nuclei in the supposed island of stability. One of the main points to show is that simple assumptions can provide already important information on the structure of nuclei outside known regions and that spectra and electromagnetic transitions can be estimated without using involved calculations and assumptions. The procedure does not allow to calculate binding energies. The method presented can be viewed as a starting point for further improvements.

  4. POTLIB 2001: A potential energy surface library for chemical systems

    NASA Astrophysics Data System (ADS)

    Duchovic, Ronald J.; Volobuev, Yuri L.; Lynch, Gillian C.; Truhlar, Donald G.; Allison, Thomas C.; Wagner, Albert F.; Garrett, Bruce C.; Corchado, Jose C.

    2002-04-01

    POTLIB 2001 is a computer program library of global chemical potential energy surface (PES) functions (91 functions in version 1.0) along with test data, a suite of utility programs, and a convenient user interface. The PES programs are written in ANSI standard FORTRAN77 and can be used to determine the Born-Oppenheimer potential energy of chemical systems as a function of the internal coordinates. The accompanying test data allow users to verify local implementations of this library. Finally, the utility programs permit use of this library in conjunction with a variety of chemical dynamics and chemical kinetics computer codes. Interface routines are provided for the POLYRATE and ABCRATE program packages of Truhlar and co-workers, the VENUS96 program package of Hase and co-workers, and the VARIFLEX program package of Klippenstein and co-workers; the routines in this library can also be used in conjunction with the DYNASOL program package of Zhang and co-workers. This article describes the library and the utility programs and outlines the systematic conventions used for interfaces in the computer programs contained in the library. Adherence to these conventions will allow future PESs to be compatible with this library.

  5. Suppression of repeated adiabatic shear banding by dynamic large strain extrusion machining

    NASA Astrophysics Data System (ADS)

    Cai, S. L.; Dai, L. H.

    2014-12-01

    High speed machining (HSM) is an advanced production technology with great future potential. Chip serration or segmentation is a commonly observed phenomenon during high speed machining of metals, which is found to be ascribed to a repeated shear band formation fueled by thermo-plastic instability occurring within the primary shear zone. The occurrence of serrated chips leads to the cutting force fluctuation, decreased tool life, degradation of the surface finish and less accuracy in machine parts during high speed machining. Hence, understanding and controlling serrated chip formation in HSM are extremely important. In this work, a novel dynamic large strain extrusion machining (DLSEM) technique is developed for suppressing formation of serrated chips. The systematic DLSEM experiments of Ti-6Al-4V and Inconel 718 alloy with varying degrees of imposed extrusion constraint were carried out. It is found that there is a prominent chip morphology transition from serrated to continuous state and shear band spacing decreases with the constraint degree increasing. In order to uncover underlying mechanism of the imposed extrusion constraint suppressing repeated adiabatic shear banding in DLSEM, new theoretical models are developed where the effects of extrusion constraint, material convection due to chip flow and momentum diffusion during shear band propagation are included. The analytical expressions for the onset criterion of adiabatic shear band and shear band spacing in DLSEM are obtained. The theoretical predictions are in agreement with the experimental results.

  6. Footprinting molecular electrostatic potential surfaces for calculation of solvation energies.

    PubMed

    Calero, Christian Solis; Farwer, Jochen; Gardiner, Eleanor J; Hunter, Christopher A; Mackey, Mark; Scuderi, Serena; Thompson, Stuart; Vinter, Jeremy G

    2013-11-07

    A liquid is composed of an ensemble of molecules that populate a large number of different states, so calculation of the solvation energy of a molecule in solution requires a method for summing the interactions with the environment over all of these states. The surface site interaction model for the properties of liquids at equilibrium (SSIMPLE) simplifies the surface of a molecule to a discrete number of specific interaction sites (SSIPs). The thermodynamic properties of these interaction sites can be characterised experimentally, for example, through measurement of association constants for the formation of simple complexes that feature a single H-bonding interaction. Correlation of experimentally determined solution phase H-bond parameters with gas phase ab initio calculations of maxima and minima on molecular electrostatic potential surfaces (MEPS) provides a method for converting gas phase calculations on isolated molecules to parameters that can be used to estimate solution phase interaction free energies. This approach has been generalised using a footprinting technique that converts an MEPS into a discrete set of SSIPs (each described by a polar interaction parameter, εi). These SSIPs represent the molecular recognition properties of the entire surface of the molecule. For example, water is described by four SSIPs, two H-bond donor sites and two H-bond acceptor sites. A liquid mixture is described as an ensemble of SSIPs that represent the components of the mixture at appropriate concentrations. Individual SSIPs are assumed to be independent, so speciation of SSIP contacts can be calculated based on properties of the individual SSIP interactions, which are given by the sum of a polar (εiεj) and a non-polar (E(vdW)) interaction term. Results are presented for calculation the free energies of transfer of a range of organic molecules from the pure liquid into water, from the pure liquid into n-hexadecane, from n-hexadecane into water, from n-octanol into

  7. Shortcuts to adiabaticity: suppression of pair production in driven Dirac dynamics

    NASA Astrophysics Data System (ADS)

    Deffner, Sebastian

    2016-01-01

    Achieving effectively adiabatic dynamics in finite time is a ubiquitous goal in virtually all areas of modern physics. So-called shortcuts to adiabaticity refer to a set of methods and techniques that allow us to produce in a short time the same final state that would result from an adiabatic, infinitely slow process. In this paper we generalize one of these methods—the fast-forward technique—to driven Dirac dynamics. As our main result we find that shortcuts to adiabaticity for the (1+1)-dimensional Dirac equation are facilitated by a combination of both scalar and pseudoscalar potentials. Our findings are illustrated for two analytically solvable examples, namely charged particles driven in spatially homogeneous and linear vector fields.

  8. Competing adiabatic Thouless pumps in enlarged parameter spaces

    NASA Astrophysics Data System (ADS)

    Lopes, Pedro L. e. S.; Ghaemi, Pouyan; Ryu, Shinsei; Hughes, Taylor L.

    2016-12-01

    The transfer of conserved charges through insulating matter via smooth deformations of the Hamiltonian is known as quantum adiabatic, or Thouless, pumping. Central to this phenomenon are Hamiltonians whose insulating gap is controlled by a multidimensional (usually two-dimensional) parameter space in which paths can be defined for adiabatic changes in the Hamiltonian, i.e., without closing the gap. Here, we extend the concept of Thouless pumps of band insulators by considering a larger, three-dimensional parameter space. We show that the connectivity of this parameter space is crucial for defining quantum pumps, demonstrating that, as opposed to the conventional two-dimensional case, pumped quantities depend not only on the initial and final points of Hamiltonian evolution but also on the class of the chosen path and preserved symmetries. As such, we distinguish the scenarios of closed/open paths of Hamiltonian evolution, finding that different closed cycles can lead to the pumping of different quantum numbers, and that different open paths may point to distinct scenarios for surface physics. As explicit examples, we consider models similar to simple models used to describe topological insulators, but with doubled degrees of freedom compared to a minimal topological insulator model. The extra fermionic flavors from doubling allow for extra gapping terms/adiabatic parameters—besides the usual topological mass which preserves the topology-protecting discrete symmetries—generating an enlarged adiabatic parameter space. We consider cases in one and three spatial dimensions, and our results in three dimensions may be realized in the context of crystalline topological insulators, as we briefly discuss.

  9. Constrained Broyden Dimer Method with Bias Potential for Exploring Potential Energy Surface of Multistep Reaction Process.

    PubMed

    Shang, Cheng; Liu, Zhi-Pan

    2012-07-10

    To predict the chemical activity of new matter is an ultimate goal in chemistry. The identification of reaction pathways using modern quantum mechanics calculations, however, often requires a high demand in computational power and good chemical intuition on the reaction. Here, a new reaction path searching method is developed by combining our recently developed transition state (TS) location method, namely, the constrained Broyden dimer method, with a basin-filling method via bias potentials, which allows the system to walk out from the energy traps at a given reaction direction. In the new method, the reaction path searching starts from an initial state without the need for preguessing the TS-like or final state structure and can proceed iteratively to the final state by locating all related TSs and intermediates. In each elementary reaction step, a reaction direction, such as a bond breaking, needs to be specified, the information of which is refined and preserved as a normal mode through biased dimer rotation. The method is tested successfully on the Baker reaction system (50 elementary reactions) with good efficiency and stability and is also applied to the potential energy surface exploration of multistep reaction processes in the gas phase and on the surface. The new method can be applied for the computational screening of new catalytic materials with a minimum requirement of chemical intuition.

  10. Use of models to map potential capture of surface water

    USGS Publications Warehouse

    Leake, Stanley A.

    2006-01-01

    The effects of ground-water withdrawals on surface-water resources and riparian vegetation have become important considerations in water-availability studies. Ground water withdrawn by a well initially comes from storage around the well, but with time can eventually increase inflow to the aquifer and (or) decrease natural outflow from the aquifer. This increased inflow and decreased outflow is referred to as “capture.” For a given time, capture can be expressed as a fraction of withdrawal rate that is accounted for as increased rates of inflow and decreased rates of outflow. The time frames over which capture might occur at different locations commonly are not well understood by resource managers. A ground-water model, however, can be used to map potential capture for areas and times of interest. The maps can help managers visualize the possible timing of capture over large regions. The first step in the procedure to map potential capture is to run a ground-water model in steady-state mode without withdrawals to establish baseline total flow rates at all sources and sinks. The next step is to select a time frame and appropriate withdrawal rate for computing capture. For regional aquifers, time frames of decades to centuries may be appropriate. The model is then run repeatedly in transient mode, each run with one well in a different model cell in an area of interest. Differences in inflow and outflow rates from the baseline conditions for each model run are computed and saved. The differences in individual components are summed and divided by the withdrawal rate to obtain a single capture fraction for each cell. Values are contoured to depict capture fractions for the time of interest. Considerations in carrying out the analysis include use of realistic physical boundaries in the model, understanding the degree of linearity of the model, selection of an appropriate time frame and withdrawal rate, and minimizing error in the global mass balance of the model.

  11. The performance of the quantum adiabatic algorithm on spike Hamiltonians

    NASA Astrophysics Data System (ADS)

    Kong, Linghang; Crosson, Elizabeth

    Spike Hamiltonians arise from optimization instances for which the adiabatic algorithm provably out performs classical simulated annealing. In this work, we study the efficiency of the adiabatic algorithm for solving the “the Hamming weight with a spike” problem by analyzing the scaling of the spectral gap at the critical point for various sizes of the barrier. Our main result is a rigorous lower bound on the minimum spectral gap for the adiabatic evolution when the bit-symmetric cost function has a thin but polynomially high barrier, which is based on a comparison argument and an improved variational ansatz for the ground state. We also adapt the discrete WKB method for the case of abruptly changing potentials and compare it with the predictions of the spin coherent instanton method which was previously used by Farhi, Goldstone and Gutmann. Finally, our improved ansatz for the ground state leads to a method for predicting the location of avoided crossings in the excited energy states of the thin spike Hamiltonian, and we use a recursion relation to understand the ordering of some of these avoided crossings as a step towards analyzing the previously observed diabatic cascade phenomenon.

  12. Adiabatic dynamics with classical noise in optical lattice

    NASA Astrophysics Data System (ADS)

    Xu, Guanglei; Daley, Andrew

    2016-05-01

    The technique of adiabatic state preparation is an interesting potential tool for the realisation of sensitive many-body states with ultra-cold atoms at low temperatures. However, questions remain regarding the influence of classical noise in these adiabatic dynamics. We investigate such dynamics in a situation where a level dressing scheme can make amplitude noise in an optical lattice proportional to the Hamiltonian, leading to a quantum Zeno effect for non-adiabatic transitions. We compute the dynamics using stochastic many-body Schrödinger equation and master equation approaches. Taking the examples of 1D Bose-Hubbard model from Mott insulator phase to superfluid phase and comparing with analytical calculations for a two-level system, we demonstrate that when the total time for the process is limited, properly transformed noise can lead to an increased final fidelity in the state preparation. We consider the dynamics also in the presence of imperfections, studying the resulting heating and dephasing for the many-body states, and identifying optimal regimes for future experiments.

  13. Standardization of surface potential measurements of graphene domains

    PubMed Central

    Panchal, Vishal; Pearce, Ruth; Yakimova, Rositza; Tzalenchuk, Alexander; Kazakova, Olga

    2013-01-01

    We compare the three most commonly used scanning probe techniques to obtain a reliable value of the work function in graphene domains of different thickness. The surface potential (SP) of graphene is directly measured in Hall bar geometry via a combination of electrical functional microscopy and spectroscopy techniques, which enables calibrated work function measurements of graphene domains in ambient conditions with values Φ1LG ~4.55 ± 0.02 eV and Φ2LG ~ 4.44 ± 0.02 eV for single- and bi-layer, respectively. We demonstrate that frequency-modulated Kelvin probe force microscopy (FM-KPFM) provides more accurate measurement of the SP than amplitude-modulated (AM)-KPFM. The discrepancy between experimental results obtained by different techniques is discussed. In addition, we use FM-KPFM for contactless measurements of the specific components of the device resistance. We show a strong non-Ohmic behavior of the electrode-graphene contact resistance and extract the graphene channel resistivity. PMID:24008915

  14. An Accurate Potential Energy Surface for H2O

    NASA Technical Reports Server (NTRS)

    Schwenke, David W.; Partridge, Harry; Langhoff, Stephen R. (Technical Monitor)

    1997-01-01

    We have carried out extensive high quality ab initio electronic structure calculations of the ground state potential energy surface (PES) and dipole moment function (DMF) for H2O. A small adjustment is made to the PES to improve the agreement of line positions from theory and experiment. The theoretical line positions are obtained from variational ro-vibrational calculations using the exact kinetic energy operator. For the lines being fitted, the root-mean-square error was reduced from 6.9 to 0.08 /cm. We were then able to match 30,092 of the 30,117 lines from the HITRAN 96 data base to theoretical lines, and 80% of the line positions differed less than 0.1 /cm. About 3% of the line positions in the experimental data base appear to be incorrect. Theory predicts the existence of many additional weak lines with intensities above the cutoff used in the data base. To obtain results of similar accuracy for HDO, a mass dependent correction to the PH is introduced and is parameterized by simultaneously fitting line positions for HDO and D2O. The mass dependent PH has good predictive value for T2O and HTO. Nonadiabatic effects are not explicitly included. Line strengths for vibrational bands summed over rotational levels usually agree well between theory and experiment, but individual line strengths can differ greatly. A high temperature line list containing about 380 million lines has been generated using the present PES and DMF

  15. A hybrid low power biopatch for body surface potential measurement.

    PubMed

    Yang, Geng; Chen, Jian; Xie, Li; Mao, Jia; Tenhunen, Hannu; Zheng, Li-Rong

    2013-05-01

    This paper presents a wearable biopatch prototype for body surface potential measurement. It combines three key technologies, including mixed-signal system on chip (SoC) technology, inkjet printing technology, and anisotropic conductive adhesive (ACA) bonding technology. An integral part of the biopatch is a low-power low-noise SoC. The SoC contains a tunable analog front end, a successive approximation register analog-to-digital converter, and a reconfigurable digital controller. The electrodes, interconnections, and interposer are implemented by inkjet-printing the silver ink precisely on a flexible substrate. The reliability of printed traces is evaluated by static bending tests. ACA is used to attach the SoC to the printed structures and form the flexible hybrid system. The biopatch prototype is light and thin with a physical size of 16 cm × 16 cm. Measurement results show that low-noise concurrent electrocardiogram signals from eight chest points have been successfully recorded using the implemented biopatch.

  16. Spectroscopic properties and potential energy surfaces of GeH

    NASA Astrophysics Data System (ADS)

    Balasubramanian, K.; Li, Junqing

    1988-04-01

    MCSCF (complete active space SCF) followed by configuration interaction calculations are carried out on 12 electronic states of GeH. Relativistic configuration interaction calculations are carried out with the objective of computing the spin-orbit corrections for the low-lying states. These calculations reveal the existence of 10 bound electronic states of GeH for which spectroscopic properties are computed. The three experimentally observed bands ( a- X, A- X, B- X) are assigned and the uncertainties in the experimental Te and ωe values of these states are corrected. In addition, the spectroscopic properties of 8 states are calculated which are yet to be observed. The spin-orbit coupling constant for the ground state X( 2Π) is calculated to be 869 cm -1. An accurate dissociation energy of 2.81 eV was obtained using {MCSCF}/{SOCI} calculation which employed a large Gaussian basis set questioning the experimental De of ˜3.3 eV obtained from the predissociation in the A2Δ state. It is shown that the intersection of the repulsive 4Π curve which dissociates into the ground state atoms causes predissociation in the A( 2Δ) , B( 2Σ +) , 2Σ +(III), and 2Π(II) states. The potential energy surfaces of a few excited states contain barriers. The calculated ground state dipole moment of 0.098 D is in disagreement with an experimental value of 1.24 D, questioning the experimental dipole moment.

  17. Fowler-Nordheim emission modified by laser pulses in the adiabatic regime

    NASA Astrophysics Data System (ADS)

    Rokhlenko, A.; Lebowitz, J. L.

    2016-06-01

    We investigate enhanced field emission due to a continuous or pulsed oscillating field added to a constant electric field E at the emitter surface. When the frequency of oscillation, field strength, and property of the emitter material satisfy the Keldysh condition γ<1 /2 , one can use the adiabatic approximation for treating the oscillating field, i.e., consider the tunneling through the instantaneous Fowler-Nordheim barrier created by both fields. Due to the great sensitivity of the emission to the field strength, the average tunneling current can be much larger than the current produced by only the constant field. We carry out the computations for arbitrary strong constant electric fields, beyond the commonly used Fowler-Nordheim approximation which exhibit, in particular, an important property of the wave function inside the potential barrier where it is found to be monotonically decreasing without oscillations.

  18. Detectability of Potentially Entrained Microorganisms at the Surface of Europa

    NASA Technical Reports Server (NTRS)

    Dalton, J. B.

    2002-01-01

    New spectral measurements of bacteria taken at cryogenic temperatures provide insights on the surface composition of Europa as well as the detectability of microbes on the surface. Additional information is contained in the original extended abstract.

  19. Quantum dynamics on a three-sheeted six-dimensional ab initio potential-energy surface of the phosphine cation: Simulation of the photoelectron spectrum and the ultrafast radiationless decay dynamics

    SciTech Connect

    Bhattacharyya, Swarnendu Domcke, Wolfgang; Dai, Zuyang

    2015-11-21

    A diabatic three-sheeted six-dimensional potential-energy surface has been constructed for the ground state and the lowest excited state of the PH{sub 3}{sup +} cation. Coupling terms of Jahn-Teller and pseudo-Jahn-Teller origin up to eighth order had to be included to describe the pronounced anharmonicity of the surface due to multiple conical intersections. The parameters of the diabatic Hamiltonian have been optimized by fitting the eigenvalues of the potential-energy matrix to ab initio data calculated at the CASSCF/MRCI level employing the correlation-consistent triple-ζ basis. The theoretical photoelectron spectrum of phosphine and the non-adiabatic nuclear dynamics of the phosphine cation have been computed by propagating nuclear wave packets with the multiconfiguration time-dependent Hartree method. The theoretical photoelectron bands obtained by Fourier transformation of the autocorrelation function agree well with the experimental results. It is shown that the ultrafast non-radiative decay dynamics of the first excited state of PH{sub 3}{sup +} is dominated by the exceptionally strong Jahn-Teller coupling of the asymmetric bending vibrational mode together with a hyperline of conical intersections with the electronic ground state induced by the umbrella mode. Time-dependent population probabilities have been computed for the three adiabatic electronic states. The non-adiabatic Jahn-Teller dynamics within the excited state takes place within ≈5 fs. Almost 80% of the excited-state population decay to the ground state within about 10 fs. The wave packets become highly complex and delocalized after 20 fs and no further significant transfer of electronic population seems to occur up to 100 fs propagation time.

  20. Classical molecular dynamics simulation of electronically non-adiabatic processes.

    PubMed

    Miller, William H; Cotton, Stephen J

    2016-12-22

    Both classical and quantum mechanics (as well as hybrids thereof, i.e., semiclassical approaches) find widespread use in simulating dynamical processes in molecular systems. For large chemical systems, however, which involve potential energy surfaces (PES) of general/arbitrary form, it is usually the case that only classical molecular dynamics (MD) approaches are feasible, and their use is thus ubiquitous nowadays, at least for chemical processes involving dynamics on a single PES (i.e., within a single Born-Oppenheimer electronic state). This paper reviews recent developments in an approach which extends standard classical MD methods to the treatment of electronically non-adiabatic processes, i.e., those that involve transitions between different electronic states. The approach treats nuclear and electronic degrees of freedom (DOF) equivalently (i.e., by classical mechanics, thereby retaining the simplicity of standard MD), and provides "quantization" of the electronic states through a symmetrical quasi-classical (SQC) windowing model. The approach is seen to be capable of treating extreme regimes of strong and weak coupling between the electronic states, as well as accurately describing coherence effects in the electronic DOF (including the de-coherence of such effects caused by coupling to the nuclear DOF). A survey of recent applications is presented to illustrate the performance of the approach. Also described is a newly developed variation on the original SQC model (found universally superior to the original) and a general extension of the SQC model to obtain the full electronic density matrix (at no additional cost/complexity).

  1. Adiabatic optimization versus diffusion Monte Carlo methods

    NASA Astrophysics Data System (ADS)

    Jarret, Michael; Jordan, Stephen P.; Lackey, Brad

    2016-10-01

    Most experimental and theoretical studies of adiabatic optimization use stoquastic Hamiltonians, whose ground states are expressible using only real nonnegative amplitudes. This raises a question as to whether classical Monte Carlo methods can simulate stoquastic adiabatic algorithms with polynomial overhead. Here we analyze diffusion Monte Carlo algorithms. We argue that, based on differences between L1 and L2 normalized states, these algorithms suffer from certain obstructions preventing them from efficiently simulating stoquastic adiabatic evolution in generality. In practice however, we obtain good performance by introducing a method that we call Substochastic Monte Carlo. In fact, our simulations are good classical optimization algorithms in their own right, competitive with the best previously known heuristic solvers for MAX-k -SAT at k =2 ,3 ,4 .

  2. Nonadiabatic exchange dynamics during adiabatic frequency sweeps.

    PubMed

    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.

  3. The stability of TiC surfaces in the environment with various carbon chemical potential and surface defects

    NASA Astrophysics Data System (ADS)

    Mao, Jianjun; Li, Shasha; Zhang, Yanxing; Chu, Xingli; Yang, Zongxian

    2016-11-01

    The low-index surfaces of TiC are studied using the first-principles method based on density functional theory. The surface energy of TiC is calculated with consideration of the surface orientation, termination and carbon chemical potential, as well as the influence of surface vacancy defects of various concentrations. It is found that the surface relaxation results in rumpling of the (001) and (110) surfaces and the contraction of the (111) surfaces. The relative stability of the low-index surfaces of TiC varies with the carbon chemical potential, surface defects and vacancy concentrations, which will have an effect on the nanoparticles morphology and catalytic performance in practical applications. The results will serve as a guidance for understanding and designing novel TiC nanocatalysts with special morphology.

  4. 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.

  5. 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.

  6. On adiabatic invariant in generalized Galileon theories

    SciTech Connect

    Ema, Yohei; Jinno, Ryusuke; Nakayama, Kazunori; Mukaida, Kyohei E-mail: jinno@hep-th.phys.s.u-tokyo.ac.jp E-mail: kazunori@hep-th.phys.s.u-tokyo.ac.jp

    2015-10-01

    We consider background dynamics of generalized Galileon theories in the context of inflation, where gravity and inflaton are non-minimally coupled to each other. In the inflaton oscillation regime, the Hubble parameter and energy density oscillate violently in many cases, in contrast to the Einstein gravity with minimally coupled inflaton. However, we find that there is an adiabatic invariant in the inflaton oscillation regime in any generalized Galileon theory. This adiabatic invariant is useful in estimating the expansion law of the universe and also the particle production rate due to the oscillation of the Hubble parameter.

  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 cluster-state quantum computing

    SciTech Connect

    Bacon, Dave; Flammia, Steven T.

    2010-09-15

    Models of quantum computation (QC) are important because they change the physical requirements for achieving universal QC. For example, one-way QC requires the preparation of an entangled ''cluster'' state, followed by adaptive measurement on this state, a set of requirements which is different from the standard quantum-circuit model. Here we introduce a model based on one-way QC but without measurements (except for the final readout), instead using adiabatic deformation of a Hamiltonian whose initial ground state is the cluster state. Our results could help increase the feasibility of adiabatic schemes by using tools from one-way QC.

  9. Markovian quantum master equation beyond adiabatic regime.

    PubMed

    Yamaguchi, Makoto; Yuge, Tatsuro; Ogawa, Tetsuo

    2017-01-01

    By introducing a temporal change time scale τ_{A}(t) for the time-dependent system Hamiltonian, a general formulation of the Markovian quantum master equation is given to go well beyond the adiabatic regime. In appropriate situations, the framework is well justified even if τ_{A}(t) is faster than the decay time scale of the bath correlation function. An application to the dissipative Landau-Zener model demonstrates this general result. The findings are applicable to a wide range of fields, providing a basis for quantum control beyond the adiabatic regime.

  10. Markovian quantum master equation beyond adiabatic regime

    NASA Astrophysics Data System (ADS)

    Yamaguchi, Makoto; Yuge, Tatsuro; Ogawa, Tetsuo

    2017-01-01

    By introducing a temporal change time scale τA(t ) for the time-dependent system Hamiltonian, a general formulation of the Markovian quantum master equation is given to go well beyond the adiabatic regime. In appropriate situations, the framework is well justified even if τA(t ) is faster than the decay time scale of the bath correlation function. An application to the dissipative Landau-Zener model demonstrates this general result. The findings are applicable to a wide range of fields, providing a basis for quantum control beyond the adiabatic regime.

  11. Fitting and using model Hamiltonian in non-adiabatic molecular dynamics simulations

    NASA Astrophysics Data System (ADS)

    Smale, Jonathan Ross

    In order to study computationally increasingly complex systems using theoretical methods model, Hamiltonians are required to accurately describe the potential energy surface they represent. Also ab-initio methods improve the calculation of the excited states of these complex systems becomes increasingly feasible. One such model Hamiltonian described herein, the Vibronic Coupling Hamiltonian, has previously shown its versatility and ability to describe a variety of non-adiabatic problems. This thesis describes a new method, a genetic algorithm, for the parameterisation of the Vibronic Coupling Hamiltonian to describe both previously calculated potential energy surfaces (allene and pentatetraene) and newly calculated (cyclo-butadiene and toluene) potential energy surfaces. In order to test this genetic algorithm, quantum nuclear dynamics calculations were performed using the multi-configurational time dependent Hartree method and the results compared to experiment..

  12. Communication: On the competition between adiabatic and nonadiabatic dynamics in vibrationally mediated ammonia photodissociation in its A band

    NASA Astrophysics Data System (ADS)

    Xie, Changjian; Zhu, Xiaolei; Ma, Jianyi; Yarkony, David R.; Xie, Daiqian; Guo, Hua

    2015-03-01

    Non-adiabatic processes play an important role in photochemistry, but the mechanism for conversion of electronic energy to chemical energy is still poorly understood. To explore the possibility of vibrational control of non-adiabatic dynamics in a prototypical photoreaction, namely, the A-band photodissociation of NH 3 ( X ˜ 1 A 1 ) , full-dimensional state-to-state quantum dynamics of symmetric or antisymmetric stretch excited NH 3 ( X ˜ 1 A 1 ) is investigated on recently developed coupled diabatic potential energy surfaces. The experimentally observed H atom kinetic energy distributions are reproduced. However, contrary to previous inferences, the NH 2 ( A ˜ 2 A 1 ) /NH 2 ( X ˜ 2 B 1 ) branching ratio is found to be small regardless of the initial preparation of NH 3 ( X ˜ 1 A 1 ) , while the internal state distribution of the preeminent fragment, NH 2 ( X ˜ 2 B 1 ) , is found to depend strongly on the initial vibrational excitation of NH 3 ( X ˜ 1 A 1 ) . The slow H atoms in photodissociation mediated by the antisymmetric stretch fundamental state are due to energy sequestered in the internally excited NH 2 ( X ˜ 2 B 1 ) fragment, rather than in NH 2 ( A ˜ 2 A 1 ) as previously proposed. The high internal excitation of the NH 2 ( X ˜ 2 B 1 ) fragment is attributed to the torques exerted on the molecule as it passes through the conical intersection seam to the ground electronic state of NH3. Thus in this system, contrary to previous assertions, the control of electronic state branching by selective excitation of ground state vibrational modes is concluded to be ineffective. The juxtaposition of precise quantum mechanical results with complementary results based on quasi-classical surface hopping trajectories provides significant insights into the non-adiabatic process.

  13. 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.

  14. A global potential energy surface and dipole moment surface for silane

    SciTech Connect

    Owens, Alec; Yurchenko, Sergei N.; Yachmenev, Andrey; Thiel, Walter

    2015-12-28

    A new nine-dimensional potential energy surface (PES) and dipole moment surface (DMS) for silane have been generated using high-level ab initio theory. The PES, CBS-F12{sup HL}, reproduces all four fundamental term values for {sup 28}SiH{sub 4} with sub-wavenumber accuracy, resulting in an overall root-mean-square error of 0.63 cm{sup −1}. The PES is based on explicitly correlated coupled cluster calculations with extrapolation to the complete basis set limit, and incorporates a range of higher-level additive energy corrections to account for core-valence electron correlation, higher-order coupled cluster terms, and scalar relativistic effects. Systematic errors in computed intra-band rotational energy levels are reduced by empirically refining the equilibrium geometry. The resultant Si–H bond length is in excellent agreement with previous experimental and theoretical values. Vibrational transition moments, absolute line intensities of the ν{sub 3} band, and the infrared spectrum for {sup 28}SiH{sub 4} including states up to J = 20 and vibrational band origins up to 5000 cm{sup −1} are calculated and compared with available experimental results. The DMS tends to marginally overestimate the strength of line intensities. Despite this, band shape and structure across the spectrum are well reproduced and show good agreement with experiment. We thus recommend the PES and DMS for future use.

  15. A global potential energy surface and dipole moment surface for silane.

    PubMed

    Owens, Alec; Yurchenko, Sergei N; Yachmenev, Andrey; Thiel, Walter

    2015-12-28

    A new nine-dimensional potential energy surface (PES) and dipole moment surface (DMS) for silane have been generated using high-level ab initio theory. The PES, CBS-F12(HL), reproduces all four fundamental term values for (28)SiH4 with sub-wavenumber accuracy, resulting in an overall root-mean-square error of 0.63 cm(-1). The PES is based on explicitly correlated coupled cluster calculations with extrapolation to the complete basis set limit, and incorporates a range of higher-level additive energy corrections to account for core-valence electron correlation, higher-order coupled cluster terms, and scalar relativistic effects. Systematic errors in computed intra-band rotational energy levels are reduced by empirically refining the equilibrium geometry. The resultant Si-H bond length is in excellent agreement with previous experimental and theoretical values. Vibrational transition moments, absolute line intensities of the ν3 band, and the infrared spectrum for (28)SiH4 including states up to J = 20 and vibrational band origins up to 5000 cm(-1) are calculated and compared with available experimental results. The DMS tends to marginally overestimate the strength of line intensities. Despite this, band shape and structure across the spectrum are well reproduced and show good agreement with experiment. We thus recommend the PES and DMS for future use.

  16. Adiabatic Deformation and Strain Localization

    DTIC Science & Technology

    1982-08-01

    4,1978, p. 180·184. 17. TURLEY , D. M. The Nature of the White Erching Surface Layers Produced During Reaming Ulrra-High Strength Steel. Mater. Sci...Ducker 1 AFFDL/FES, J. Hodges 1 AFFDL/TST, Library Air Force Test and Eva luation Cente r, Kir tland Air Force Base , NM 87115 ATTN: AFTEC-JT No

  17. Quantum-mechanical approach to predissociation of water dimers in the vibrational adiabatic representation: Importance of channel interactions

    SciTech Connect

    Mineo, H.; Kuo, J. L.; Niu, Y. L.; Lin, S. H.; Fujimura, Y.

    2015-08-28

    The results of application of the quantum-mechanical adiabatic theory to vibrational predissociation (VPD) of water dimers, (H{sub 2}O){sub 2} and (D{sub 2}O){sub 2}, are presented. We consider the VPD processes including the totally symmetric OH mode of the dimer and the bending mode of the fragment. The VPD in the adiabatic representation is induced by breakdown of the vibrational adiabatic approximation, and two types of nonadiabatic coupling matrix elements are involved: one provides the VPD induced by the low-frequency dissociation mode and the other provides the VPD through channel interactions induced by the low-frequency modes. The VPD rate constants were calculated using the Fermi golden rule expression. A closed form for the nonadiabatic transition matrix element between the discrete and continuum states was derived in the Morse potential model. All of the parameters used were obtained from the potential surfaces of the water dimers, which were calculated by the density functional theory procedures. The VPD rate constants for the two processes were calculated in the non-Condon scheme beyond the so-called Condon approximation. The channel interactions in and between the initial and final states were taken into account, and those are found to increase the VPD rates by 3(1) orders of magnitude for the VPD processes in (H{sub 2}O){sub 2} ((D{sub 2}O){sub 2}). The fraction of the bending-excited donor fragments is larger than that of the bending-excited acceptor fragments. The results obtained by quantum-mechanical approach are compared with both experimental and quasi-classical trajectory calculation results.

  18. Electrostatic potentials for metal-oxide surfaces and interfaces

    NASA Astrophysics Data System (ADS)

    Streitz, F. H.; Mintmire, J. W.

    1994-10-01

    As most technologically important metals will form oxides readily, any complete study of adhesion at real metal surfaces must include the metal-oxide interface. The role of this ubiquitous oxide layer cannot be overlooked, as the adhesive properties of the oxide or oxide-metal system can be expected to differ profoundly from the adhesive properties of a bare metal surface. We report on the development of a computational method for molecular-dynamics simulations, which explicitly includes variable charge transfer between anions and cations. This method is found to be capable of describing the elastic properties, surface energies, and surface relaxation of crystalline metal oxides accurately. We discuss in detail results using this method for α-alumina and several of its low-index faces.

  19. 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)

  20. 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…

  1. Tailor-made functional surfaces: potential elastomeric biomaterials I.

    PubMed

    Desai, Shrojal; Bodas, Dhananjay; Patil, K R; Patole, Milind; Singh, R P

    2003-01-01

    In the present investigation, different functional monomers, like hydroxyethyl methacrylate, acrylic acid, N-vinyl pyrrolidone and glycidyl methacrylate, have been grafted onto the surface of EPDM film (approx. 200 microm) using simultaneous photo-grafting (lambda > or = 290 nm) and cold plasma-grafting techniques, to alter the surface properties, such as hydrophilicity and, therefore, biocompatibility. Here, we have carried out simultaneous plasma-grafting, unlike the conventional post plasma-grafting. The effect of different surface grafting techniques on the degree of surface modification and resultant biocompatibility has been investigated. The chemical changes on the polymer backbone are followed from the results of attenuated total reflection Fourier transform infrared (ATR-FT-IR) spectroscopy and X-ray photoelectron spectroscopy (XPS), which shows the peaks corresponding to the functional groups of the monomers grafted onto the film surface. The morphology of the modified surfaces was investigated using scanning electron microscopy (SEM) technique. The induced hydrophilicity and resultant cell compatibility were followed from the water contact angle measurements and in vitro human carcinoma cell adhesion/proliferation tests, respectively. All the grafted samples exhibited variable cell compatibilities depending upon the type of monomer and their degree of grafting; however, always better than the neat samples. Hydroxyethyl methacrylate and acrylic acid showed exceptionally high cell compatibility in terms of cell adhesion and proliferation.

  2. Adiabatic and Non-adiabatic quenches in a Spin-1 Bose Einstein Condensate

    NASA Astrophysics Data System (ADS)

    Boguslawski, Matthew; Hebbe Madhusudhana, Bharath; Anquez, Martin; Robbins, Bryce; Barrios, Maryrose; Hoang, Thai; Chapman, Michael

    2016-05-01

    A quantum phase transition (QPT) is observed in a wide range of phenomena. We have studied the dynamics of a spin-1 ferromagnetic Bose-Einstein condensate for both adiabatic and non-adiabatic quenches through a QPT. At the quantum critical point (QCP), finite size effects lead to a non-zero gap, which makes an adiabatic quench possible through the QPT. We experimentally demonstrate such a quench, which is forbidden at the mean field level. For faster quenches through the QCP, the vanishing energy gap causes the reaction timescale of the system to diverge, preventing the system from adiabatically following the ground state. We measure the temporal evolution of the spin populations for different quench speeds and determine the exponents characterizing the scaling of the onset of excitations, which are in good agreement with the predictions of Kibble-Zurek mechanism.

  3. Fixed-point adiabatic quantum search

    NASA Astrophysics Data System (ADS)

    Dalzell, Alexander M.; Yoder, Theodore J.; Chuang, Isaac L.

    2017-01-01

    Fixed-point quantum search algorithms succeed at finding one of M target items among N total items even when the run time of the algorithm is longer than necessary. While the famous Grover's algorithm can search quadratically faster than a classical computer, it lacks the fixed-point property—the fraction of target items must be known precisely to know when to terminate the algorithm. Recently, Yoder, Low, and Chuang [Phys. Rev. Lett. 113, 210501 (2014), 10.1103/PhysRevLett.113.210501] gave an optimal gate-model search algorithm with the fixed-point property. Previously, it had been discovered by Roland and Cerf [Phys. Rev. A 65, 042308 (2002), 10.1103/PhysRevA.65.042308] that an adiabatic quantum algorithm, operating by continuously varying a Hamiltonian, can reproduce the quadratic speedup of gate-model Grover search. We ask, can an adiabatic algorithm also reproduce the fixed-point property? We show that the answer depends on what interpolation schedule is used, so as in the gate model, there are both fixed-point and non-fixed-point versions of adiabatic search, only some of which attain the quadratic quantum speedup. Guided by geometric intuition on the Bloch sphere, we rigorously justify our claims with an explicit upper bound on the error in the adiabatic approximation. We also show that the fixed-point adiabatic search algorithm can be simulated in the gate model with neither loss of the quadratic Grover speedup nor of the fixed-point property. Finally, we discuss natural uses of fixed-point algorithms such as preparation of a relatively prime state and oblivious amplitude amplification.

  4. Adiabatic burst evaporation from bicontinuous nanoporous membranes.

    PubMed

    Ichilmann, Sachar; Rücker, Kerstin; Haase, Markus; Enke, Dirk; Steinhart, Martin; Xue, Longjian

    2015-05-28

    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 10(7) μm(3) 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.

  5. 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.

  6. 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.

  7. Benchmark ab Initio Characterization of the Complex Potential Energy Surface of the F(-) + CH3CH2Cl Reaction.

    PubMed

    Tajti, Viktor; Czako, Gabor

    2017-03-24

    We compute benchmark structures, frequencies, and relative energies for the stationary points of the potential energy surface of the F- + CH3CH2Cl reaction using explicitly-correlated ab initio levels of theory. CCSD(T)-F12b geometries and harmonic vibrational frequencies are obtained with the aug-cc-pVTZ and aug-cc-pVDZ basis sets, respectively. The benchmark relative energies are determined using a high-level composite method based on CCSD(T)-F12b/aug-cc-pVQZ frozen-core energies, CCSD(T)-F12b/cc-pCVTZ-F12 core electron correlation effects, and CCSD(T)-F12b/aug-cc-pVDZ zero-point energy corrections. The SN2 channel leading to Cl- + CH3CH2F (-33.2) can proceed via back-side (-11.5), front-side (29.1), and double-inversion (18.0) transition states, whereas the bimolecular elimination (E2) products, Cl- + HF + C2H4 (-19.3), can be formed via anti (-15.0) and syn (-7.3) saddle points, whose best adiabatic energies relative to F- + CH3CH2Cl are shown in parentheses in kcal/mol. Besides the SN2 and E2 channels, the 0 K reaction enthalpies of the HF + H3C-CHCl- (29.4), H- + H3C-CHClF (46.2), H- + FH2C-CH2Cl (51.1), and FCl- + CH3CH2 (49.7) product channels are determined. Utilizing the new benchmark data, the performance of the DF-MP2, MP2, MP2-F12, CCSD(T), and CCSD(T)-F12b methods with aug-cc-pVDZ and aug-cc-pVTZ basis sets is tested.

  8. Electronic states and potential energy surfaces of H2Te, H2Po, and their positive ions

    NASA Astrophysics Data System (ADS)

    Sumathi, K.; Balasubramanian, K.

    1990-06-01

    Geometries, bond energies, ionization potentials, dipole moments, other one-electron properties, and potential energy surfaces of six valence electronic states of H2Te and H2Po species are obtained using the relativistic complete active space multiconfiguration self-consistent field (CASSCF) followed by full second-order configuration interaction (SOCI) and relativistic configuration interaction (RCI) calculations including spin-orbit coupling. In addition, Rydberg states of H2Te and H2Se are studied to interpret the experimental spectra. The potential energy surfaces of two electronic states of H2Te+ and H2Po+ are obtained. The ground states of both H2Te and H2Po are found to be of X 1A1(A1) symmetry with bent (C2v) equilibrium geometries of H2Te:re =1.668 Å, θe=91.2°; and H2Po:re =1.835 Å and θe=90.9°. The ground states of H2Te+ and H2Po+ are X 2B1 with H2Te+:re =1.676 Å, θe=90.7° and H2Po+:re =1.828 Å and θe=88°. The De (HTe-H) and De (HPo-H) including spin-orbit effects are calculated as 63.2 and 39.4 kcal/mol, respectively. The X 2B1(E)-A 2A1(E) energy separations of H2Te+ and H2Po+ ions are calculated as 66.6 and 76 kcal/mol, respectively. The adiabatic IPs of H2Te and H2Po are calculated as 8.47 and 7.79 eV, respectively. In addition CASSCF/SOCI/RCI calculations are also carried out on the X 2Π3/2 and 2Π1/2 states of TeH and PoH diatomics. The X 2Π3/2-2Π1/2 energy separations of TeH and PoH are computed as 3710 and 9920 cm-1, respectively. Spin-orbit effects are thus found to be very significant for PoH and H2Po. All excited states of H2Te and H2Po are above 3.7 and 3.1 eV, respectively. Properties and energy separations of H2Te and H2Po are compared with the lighter group (VI) H2Ch species.

  9. Full dimensional potential energy surface for the ground state of H{sub 4}{sup +} system based on triatomic-in-molecules formalism

    SciTech Connect

    Sanz-Sanz, Cristina E-mail: cristina.sanz@gmail.com; Roncero, Octavio; Paniagua, Miguel; Aguado, Alfredo

    2013-11-14

    In this work, we present a global potential energy surface for the ground electronic state of the H{sub 4}{sup +} based on ab initio calculations. The final fit is based on triatomics-in-molecules (TRIM) approximation and it includes extra four-body terms for the better description of some discrepancies found on the TRIM model. The TRIM method itself allows a very accurate description of the asymptotic regions. The global fit uses more than 19 000 multireference configuration interaction ab initio points. The global potential energy surface has an overall root mean square error of 0.013 eV for energies up to 2 eV above the global minimum. This work presents an analysis of the stationary points, reactant and product channels, and crossing between the two lowest TRIM adiabatic states. It is as well included a brief description of the two first excited states of the TRIM matrix, concluding that TRIM method is a very good approximation not only for the ground state but also for at least two of the excited states of H{sub 4}{sup +} system.

  10. Effect of Magnetic Field Gradient on Plasma Detachment Induced by Breaking of Adiabatic Plasma Expansion

    NASA Astrophysics Data System (ADS)

    Chung, K. S.; Kim, June Young; Chung, Kyoung-Jae; Hwang, Y. S.

    2016-10-01

    A magnetic field gradient that is a variation in the magnetic field around the ion flow has been investigated as a primary parameter for ion detachment in the magnetic nozzle geometries. Some scale lengths of magnetic field are controlled by two solenoid coils outside the diffusion chamber of a ECR-driven linear plasma device. The axial and radial profiles of the plasma potential and electron temperature are measured by a Langmuir probe array for the various magnetic field configurations in the downstream. The local adiabaticity, strong constant magnetic moment, is satisfied with a linear relationship between the change in effective electron temperature and the change in plasma potential in the low magnetic field gradient. Whereas, with an increasing non-homogeneity of the magnetic field in the direction of the flow, the breaking of adiabatic plasma expansion is identified to measure the nonlinear process which is the variation for an adiabatic exponent. Such the loss of adiabaticity is also explained in terms of non-adiabaticity parameter i.e. degree of demagnetization. This research was supported by National R&D Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning (Nos. 2014M1A7A1A02030165 and 2014M1A7A1A03045367).

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

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

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

  12. Fuel models and fire potential from satellite and surface observations

    USGS Publications Warehouse

    Burgan, R.E.; Klaver, R.W.; Klarer, J.M.

    1998-01-01

    A national 1-km resolution fire danger fuel model map was derived through use of previously mapped land cover classes and ecoregions, and extensive ground sample data, then refined through review by fire managers familiar with various portions of the U.S. The fuel model map will be used in the next generation fire danger rating system for the U.S., but it also made possible immediate development of a satellite and ground based fire potential index map. The inputs and algorithm of the fire potential index are presented, along with a case study of the correlation between the fire potential index and fire occurrence in California and Nevada. Application of the fire potential index in the Mediterranean ecosystems of Spain, Chile, and Mexico will be tested.

  13. Diabatic Versus Adiabatic Calculation of Torsion-Vibration Interactions

    NASA Astrophysics Data System (ADS)

    Hougen, Jon T.

    2013-06-01

    The introductory part of this talk will deal briefly with two historical topics: (i) use of the words adiabatic, nonadiabatic, and diabatic in thermodynamics and quantum mechanics, and (ii) application of diabatic and adiabatic ideas to vibrational energy level calculations for a pair of diatomic-molecule potential energy curves exhibiting an avoided crossing. The main part of the talk will be devoted to recent work with Li-Hong Xu and Ron Lees on how ab initio projected frequency calculations for small-amplitude vibrations along the large-amplitude internal rotation path in methanol can best be used to help guide experimental assignments and fits in the IR vibrational spectrum. The three CH stretching vibrations for CH_{3}OH can conveniently be represented as coefficients multiplying three different types of basis vibrations, i.e., as coefficients of: (i) the local mode C-H_i bond displacements δr_{i} for hydrogens H_{1}, H_{2} and H_{3} of the methyl top, (ii) symmetrized linear combinations of the three δr_{i} of species A_{1} oplus E in the permutation-inversion group G_{6} = C_{3v} appropriate for methanol, or (iii) symmetrized linear combinations of the three δr_{i} of species 2A_{1} oplus A_{2} in the permutation-inversion group G_{6}. In this talk, we will focus on diabatic and adiabatic computations for the A_{1} oplus E basis vibrations of case (ii) above. We will briefly explain how Jahn-Teller-like and Renner-Teller-like torsion-vibration interaction terms occurring in the potential energy expression in the diabatic calculation become torsion-vibration Coriolis interaction terms occurring in the kinetic energy expression of the adiabatic calculations, and also show how, for algebraically solvable parameter choices, the same energy levels are obtained from either calculation. A final conclusion as to which approach is computationally superior for the numerical data given in a quantum chemistry output file has not yet been arrived at.

  14. Adsorption of lysozyme on base metal surfaces in the presence of an external electric potential.

    PubMed

    Ei Ei, Htwe; Nakama, Yuhi; Tanaka, Hiroshi; Imanaka, Hiroyuki; Ishida, Naoyuki; Imamura, Koreyoshi

    2016-11-01

    The impact of external electric potential on the adsorption of a protein to base metal surfaces was examined. Hen egg white lysozyme (LSZ) and six types of base metal plates (stainless steel SUS316L (St), Ti, Ta, Zr, Cr, or Ni) were used as the protein and adsorption surface, respectively. LSZ was allowed to adsorb on the surface under different conditions (surface potential, pH, electrolyte type and concentration, surface material), which was monitored using an ellipsometer. LSZ adsorption was minimized in the potential range above a certain threshold and, in the surface potential range below the threshold, decreasing the surface potential increased the amount of protein adsorbed. The threshold potential for LSZ adsorption was shifted toward a positive value with increasing pH and was lower for Ta and Zr than for the others. A divalent anion salt (K2SO4) as an electrolyte exhibited the adsorption of LSZ in the positive potential range while a monovalent salt (KCl) did not. A comprehensive consideration of the obtained results suggests that two modes of interactions, namely the electric force by an external electric field and electrostatic interactions with ionized surface hydroxyl groups, act on the LSZ molecules and determine the extent of suppression of LSZ adsorption. All these findings appear to support the view that a base metal surface can be controlled for the affinity to a protein by manipulating the surface electric potential as has been reported on some electrode materials.

  15. Wright Valley Sediments as Potential Analogs for Martian Surface Processes

    NASA Astrophysics Data System (ADS)

    Englert, P. A. J.; Bishop, J. L.; Patel, S.; Gibson, E. K.; Koeberl, C.

    2015-12-01

    The Antarctic Dry Valleys (ADV) may provide a unique terrestrial analog for current Martian surface processes. The Wright Valley located in the ADV contains streams, lakes and ponds that host highly saline, sedimentary environments. This project highlights comparisons of formation and salt accumulation processes at the Don Juan Pond (DJP) and Don Quixote Pond (DQP). These are located in the north and south forks of the Wright Valley, which are unique areas where unusual terrestrial processes can be studied. DQP is located in the western part of the north fork about 100 m above mean seawater level. The DQP Valley walls are up to 2500 m high and the brine is seasonally frozen. DJP from the south fork is located ~9 km west of Lake Vanda. The basin floor is 117 m above mean seawater level with activity to the north and south rising above 1000 m. The DJP brine does not freeze and may be a model environment for Ca and Cl weathering and distribution on Mars. Our findings indicate that DJP and DQP have formed in similar climatic and geological environments, but likely experienced different formation conditions. Samples were collected from surface, soil pits and depth profiles during the 1979/1980, the 1990/1991 and the 2005/2006 field seasons. Elemental abundances and mineralogy were evaluated for several sets of sediments. The DJP basin shows low surface abundances of halite and relatively high abundances of sulfates throughout with gypsum or anhydrite dominating at different locations. The DQP area has high surface abundances of halite with gypsum present as the major sulfate. Two models have been proposed to explain these differences: DQP may have formed through a combination of shallow and some deep groundwater influx, while deep groundwater upwelling likely played the dominant role of salt formation at DJP. Our study seeks to understand the formation of DQP and DJP as unique terrestrial processes and as models for Ca, Cl, and S weathering and distribution on Mars.

  16. Bending light via adiabatic optical transition in longitudinally modulated photonic lattices.

    PubMed

    Han, Bin; Xu, Lei; Dou, Yiling; Xu, Jingjun; Zhang, Guoquan

    2015-10-29

    Bending light in a controllable way is desired in various applications such as beam steering, navigating and cloaking. Different from the conventional way to bend light by refractive index gradient, transformation optics or special beams through wavefront design such as Airy beams and surface plasmons, we proposed a mechanism to bend light via resonant adiabatic optical transition between Floquet-Bloch (FB) modes from different FB bands in longitudinally modulated photonic lattices. The band structure of longitudinally modulated photonic lattices was calculated by employing the concept of quasi-energy based on the Floquet-Bloch theory, showing the existence of band discontinuities at specific resonant points which cannot be revealed by the coupled-mode theory. Interestingly, different FB bands can be seamlessly connected at these resonant points in longitudinally modulated photonic lattices driven by adiabatically varying the longitudinal modulation period along the propagation direction, which stimulates the adiabatic FB mode transition between different FB bands.

  17. Bending light via adiabatic optical transition in longitudinally modulated photonic lattices

    PubMed Central

    Han, Bin; Xu, Lei; Dou, Yiling; Xu, Jingjun; Zhang, Guoquan

    2015-01-01

    Bending light in a controllable way is desired in various applications such as beam steering, navigating and cloaking. Different from the conventional way to bend light by refractive index gradient, transformation optics or special beams through wavefront design such as Airy beams and surface plasmons, we proposed a mechanism to bend light via resonant adiabatic optical transition between Floquet-Bloch (FB) modes from different FB bands in longitudinally modulated photonic lattices. The band structure of longitudinally modulated photonic lattices was calculated by employing the concept of quasi-energy based on the Floquet-Bloch theory, showing the existence of band discontinuities at specific resonant points which cannot be revealed by the coupled-mode theory. Interestingly, different FB bands can be seamlessly connected at these resonant points in longitudinally modulated photonic lattices driven by adiabatically varying the longitudinal modulation period along the propagation direction, which stimulates the adiabatic FB mode transition between different FB bands. PMID:26511890

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

    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

  19. 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

  20. Quantum-Classical Correspondence of Shortcuts to Adiabaticity

    NASA Astrophysics Data System (ADS)

    Okuyama, Manaka; Takahashi, Kazutaka

    2017-04-01

    We formulate the theory of shortcuts to adiabaticity in classical mechanics. For a reference Hamiltonian, the counterdiabatic term is constructed from the dispersionless Korteweg-de Vries (KdV) hierarchy. Then the adiabatic theorem holds exactly for an arbitrary choice of time-dependent parameters. We use the Hamilton-Jacobi theory to define the generalized action. The action is independent of the history of the parameters and is directly related to the adiabatic invariant. The dispersionless KdV hierarchy is obtained from the classical limit of the KdV hierarchy for the quantum shortcuts to adiabaticity. This correspondence suggests some relation between the quantum and classical adiabatic theorems.

  1. Influence of surface conductivity on the apparent zeta potential of calcite.

    PubMed

    Li, Shuai; Leroy, Philippe; Heberling, Frank; Devau, Nicolas; Jougnot, Damien; Chiaberge, Christophe

    2016-04-15

    Zeta potential is a physicochemical parameter of particular importance in describing the surface electrical properties of charged porous media. However, the zeta potential of calcite is still poorly known because of the difficulty to interpret streaming potential experiments. The Helmholtz-Smoluchowski (HS) equation is widely used to estimate the apparent zeta potential from these experiments. However, this equation neglects the influence of surface conductivity on streaming potential. We present streaming potential and electrical conductivity measurements on a calcite powder in contact with an aqueous NaCl electrolyte. Our streaming potential model corrects the apparent zeta potential of calcite by accounting for the influence of surface conductivity and flow regime. We show that the HS equation seriously underestimates the zeta potential of calcite, particularly when the electrolyte is diluted (ionic strength ⩽ 0.01 M) because of calcite surface conductivity. The basic Stern model successfully predicted the corrected zeta potential by assuming that the zeta potential is located at the outer Helmholtz plane, i.e. without considering a stagnant diffuse layer at the calcite-water interface. The surface conductivity of calcite crystals was inferred from electrical conductivity measurements and computed using our basic Stern model. Surface conductivity was also successfully predicted by our surface complexation model.

  2. Intersections of potential energy surfaces of short-lived states: the complex analogue of conical intersections.

    PubMed

    Feuerbacher, Sven; Sommerfeld, Thomas; Cederbaum, Lorenz S

    2004-02-15

    Whereas conical intersections between potential energy surfaces of bound states are well known, the interaction of short-lived states has been investigated only rarely. Here, we present several systematically constructed model Hamiltonians to study the topology of intersecting complex potential energy surfaces describing short-lived states: We find the general phenomenon of doubly intersecting complex energy surfaces, i.e., there are two points instead of one as in the case of bound states where the potential energy surfaces coalesce. In addition, seams of intersections of the respective real and imaginary parts of the potential energy surfaces emanate from these two points. Using the Sigma* and Pi* resonance states of the chloroethene anion as a practical example, we demonstrate that our complete linear model Hamiltonian is able to reproduce all phenomena found in explicitly calculated ab initio complex potential energy surfaces.

  3. Adiabatic Quantum Simulation of Quantum Chemistry

    NASA Astrophysics Data System (ADS)

    Babbush, Ryan; Love, Peter J.; Aspuru-Guzik, Alán

    2014-10-01

    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.

  4. Ramsey numbers and adiabatic quantum computing.

    PubMed

    Gaitan, Frank; Clark, Lane

    2012-01-06

    The graph-theoretic Ramsey numbers are notoriously difficult to calculate. In fact, for the two-color Ramsey numbers R(m,n) with m, n≥3, only nine are currently known. We present a quantum algorithm for the computation of the Ramsey numbers R(m,n). We show how the computation of R(m,n) can be mapped to a combinatorial optimization problem whose solution can be found using adiabatic quantum evolution. We numerically simulate this adiabatic quantum algorithm and show that it correctly determines the Ramsey numbers R(3,3) and R(2,s) for 5≤s≤7. We then discuss the algorithm's experimental implementation, and close by showing that Ramsey number computation belongs to the quantum complexity class quantum Merlin Arthur.

  5. Comment on ``Adiabatic theory for the bipolaron''

    NASA Astrophysics Data System (ADS)

    Smondyrev, M. A.; Devreese, J. T.

    1996-05-01

    Comments are given on the application of the Bogoliubov-Tyablikov approach to the bipolaron problem in a recent paper by Lakhno [Phys. Rev. B 51, 3512 (1995)]. This author believes that his model (1) is the translation-invariant adiabatic theory of bipolarons and (2) gives asymptotically exact solutions in the adiabatic limit while the other approaches are considered as either phenomenological or variational in nature. Numerical results by Lakhno are in contradiction with all other papers published on the subject because his model leads to much lower energies. Thus, the author concludes that bipolarons ``are more stable than was considered before.'' We prove that both the analytical and the numerical results presented by Lakhno are wrong.

  6. 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.

  7. Shortcuts to adiabaticity from linear response theory

    DOE PAGES

    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

  8. 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.

  9. 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.

  10. Adiabatic quantum simulation of quantum chemistry.

    PubMed

    Babbush, Ryan; Love, Peter J; Aspuru-Guzik, Alán

    2014-10-13

    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.

  11. Multiphoton adiabatic passage for atom optics applications

    SciTech Connect

    Demeter, Gabor; Djotyan, Gagik P.

    2009-04-15

    We study the force exerted on two-level atoms by short, counterpropagating laser pulses. When the counterpropagating pulses overlap each other partially, multiphoton adiabatic processes are possible in several configurations, which amplify the force exerted on the atoms. We investigate the practical usefulness of such multiphoton adiabatic transitions for the manipulation of the atoms' mechanical state. In particular, we compare the efficiency of a pair of constant frequency, oppositely detuned laser pulses and that of a pair of frequency-chirped pulses. We also consider the case of prolonged exposure to a sequence of laser pulses for a duration that is comparable to or much larger than the spontaneous lifetime of the atoms. We use numerical methods to calculate the reduction of the force and the heating of the atomic ensemble when spontaneous emission cannot be neglected during the interaction. In addition, we derive simple approximate formulas for the force and the heating, and compare them to the numerical results.

  12. Adiabatic quantum optimization for associative memory recall

    DOE PAGES

    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

  13. 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.

  14. 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

  15. Negative plasma potential relative to electron-emitting surfaces.

    PubMed

    Campanell, M D

    2013-09-01

    Most works on plasma-wall interaction predict that with strong electron emission, a nonmonotonic "space-charge-limited" (SCL) sheath forms where the plasma potential is positive relative to the wall. We show that a fundamentally different sheath structure is possible where the potential monotonically increases toward a positively charged wall that is shielded by a single layer of negative charge. No ion-accelerating presheath exists in the plasma and the ion wall flux is zero. An analytical solution of the "inverse sheath" regime is demonstrated for a general plasma-wall system where the plasma electrons and emitted electrons are Maxwellian with different temperatures. Implications of the inverse sheath effect are that (a) the plasma potential is negative, (b) ion sputtering vanishes, (c) no charge is lost at the wall, and (d) the electron energy flux is thermal. To test empirically what type of sheath structure forms under strong emission, a full plasma bounded by strongly emitting walls is simulated. It is found that inverse sheaths form at the walls and ions are confined in the plasma. This result differs from past particle-in-cell simulation studies of emission which contain an artificial "source sheath" that accelerates ions to the wall, leading to a SCL sheath at high emission intensity.

  16. Effect of surface potential on epithelial cell adhesion, proliferation and morphology.

    PubMed

    Chang, Hsun-Yun; Kao, Wei-Lun; You, Yun-Wen; Chu, Yi-Hsuan; Chu, Kuo-Jui; Chen, Peng-Jen; Wu, Chen-Yi; Lee, Yu-Hsuan; Shyue, Jing-Jong

    2016-05-01

    Cell adhesion is the basis of individual cell survival, division and motility. Hence, understanding the effects that the surface properties have on cell adhesion, proliferation and morphology are crucial. In particular, surface charge/potential has been identified as an important factor that affects cell behavior. However, how cells respond to incremental changes in surface potential remains unclear. By using binary self-assembled monolayer (SAM) modified Au surfaces that are similar in mechanical/chemical properties and provide a series of surface potentials, the effect of surface potential on the behavior of cells can be studied. In this work, the effect of surface potential on epithelial cells, including human embryonic kidney (HEK293T) and human hepatocellular carcinoma (HepG2), were examined. The results showed that the adhesion density of epithelial cells increased with increasing surface potential, which is similar to but varied more significantly compared with fibroblasts. The proliferation rate is found to be independent of surface potential in both cell types. Furthermore, epithelial cells show no morphological change with respect to surface potential, whereas the morphology of the fibroblasts clearly changed with the surface potential. These differences between the cell types were rationalized by considering the difference in extracellular matrix composition. Laminin-dominant epithelial cells showed higher adhesion density and less morphological change than did fibronectin-dominant fibroblasts because the more significant adsorption of positively charged laminin on the surface enhanced the adhesion of epithelial cells. In contrast, due to the dominance of negatively charged fibronectin that adsorbed weakly on the surface, fibroblasts had to change their morphology to fit the inhomogeneous fibronectin-adsorbed area.

  17. 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.

  18. 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.

  19. On the Definition of Surface Potentials for Finite-Difference Operators

    NASA Technical Reports Server (NTRS)

    Tsynkov, S. V.; Bushnell, Dennis M. (Technical Monitor)

    2001-01-01

    For a class of linear constant-coefficient finite-difference operators of the second order, we introduce the concepts similar to those of conventional single- and double-layer potentials for differential operators. The discrete potentials are defined completely independently of any notion related to the approximation of the continuous potentials on the grid. We rather use all approach based on differentiating, and then inverting the differentiation of a function with surface discontinuity of a particular kind, which is the most general way of introducing surface potentials in the theory of distributions. The resulting finite-difference "surface" potentials appear to be solutions of the corresponding continuous potentials. Primarily, this pertains to the possibility of representing a given solution to the homogeneous equation on the domain as a variety of surface potentials, with the density defined on the domain's boundary. At the same time the discrete surface potentials can be interpreted as one specific realization of the generalized potentials of Calderon's type, and consequently, their approximation properties can be studied independently in the framework of the difference potentials method by Ryaben'kii. The motivation for introducing and analyzing the discrete surface potentials was provided by the problems of active shielding and control of sound, in which the aforementioned source terms that drive the potentials are interpreted as the acoustic control sources that cancel out the unwanted noise on a predetermined region of interest.

  20. Calculation of the surface potential and surface charge density by measurement of the three-phase contact angle.

    PubMed

    Horiuchi, H; Nikolov, A; Wasan, D T

    2012-11-01

    The silica/silicon wafer is widely used in the semiconductor industry in the manufacture of electronic devices, so it is essential to understand its physical chemistry and determine the surface potential at the silica wafer/water interface. However, it is difficult to measure the surface potential of a silica/silicon wafer directly due to its high electric resistance. In the present study, the three-phase contact angle (TPCA) on silica is measured as a function of the pH. The surface potential and surface charge density at the silica/water surface are calculated by a model based on the Young-Lippmann equation in conjunction with the Gouy-Chapman model for the electric double layer. In measurements of the TPCA on silica, two distinct regions were identified with a boundary at pH 9.5-showing a dominance of the surface ionization of silanol groups below pH 9.5 and a dominance of the dissolution of silica into the aqueous solution above pH 9.5. Since the surface chemistry changes above pH 9.5, the model is applied to solutions below pH 9.5 (ionization dominant) for the calculation of the surface potential and surface charge density at the silica/aqueous interface. In order to evaluate the model, a galvanic mica cell was made of a mica sheet and the surface potential was measured directly at the mica/water interface. The model results are also validated by experimental data from the literature, as well as the results obtained by the potentiometric titration method and the electro-kinetic measurements.

  1. 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.

  2. Adiabatic graph-state quantum computation

    NASA Astrophysics Data System (ADS)

    Antonio, B.; Markham, D.; Anders, J.

    2014-11-01

    Measurement-based quantum computation (MBQC) and holonomic quantum computation (HQC) are two very different computational methods. The computation in MBQC is driven by adaptive measurements executed in a particular order on a large entangled state. In contrast in HQC the system starts in the ground subspace of a Hamiltonian which is slowly changed such that a transformation occurs within the subspace. Following the approach of Bacon and Flammia, we show that any MBQC on a graph state with generalized flow (gflow) can be converted into an adiabatically driven holonomic computation, which we call adiabatic graph-state quantum computation (AGQC). We then investigate how properties of AGQC relate to the properties of MBQC, such as computational depth. We identify a trade-off that can be made between the number of adiabatic steps in AGQC and the norm of \\dot{H} as well as the degree of H, in analogy to the trade-off between the number of measurements and classical post-processing seen in MBQC. Finally the effects of performing AGQC with orderings that differ from standard MBQC are investigated.

  3. 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.

  4. An accurate global potential energy surface, dipole moment surface, and rovibrational frequencies for NH(3).

    PubMed

    Huang, Xinchuan; Schwenke, David W; Lee, Timothy J

    2008-12-07

    A global potential energy surface (PES) that includes short and long range terms has been determined for the NH(3) molecule. The singles and doubles coupled-cluster method that includes a perturbational estimate of connected triple excitations and the internally contracted averaged coupled-pair functional electronic structure methods have been used in conjunction with very large correlation-consistent basis sets, including diffuse functions. Extrapolation to the one-particle basis set limit was performed and core correlation and scalar relativistic contributions were included directly, while the diagonal Born-Oppenheimer correction was added. Our best purely ab initio PES, denoted "mixed," is constructed from two PESs which differ in whether the ic-ACPF higher-order correlation correction was added or not. Rovibrational transition energies computed from the mixed PES agree well with experiment and the best previous theoretical studies, but most importantly the quality does not deteriorate even up to 10 300 cm(-1) above the zero-point energy (ZPE). The mixed PES was improved further by empirical refinement using the most reliable J=0-2 rovibrational transitions in the HITRAN 2004 database. Agreement between high-resolution experiment and rovibrational transition energies computed from our refined PES for J=0-6 is excellent. Indeed, the root mean square (rms) error for 13 HITRAN 2004 bands for J=0-2 is 0.023 cm(-1) and that for each band is always

  5. 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.

  6. Creation and Transfer of Coherence via Technique of Stimulated Raman Adiabatic Passage in Triple Quantum Dots.

    PubMed

    Tian, Si-Cong; Wan, Ren-Gang; Wang, Chun-Liang; Shu, Shi-Li; Wang, Li-Jie; Tong, Chun-Zhu

    2016-12-01

    We propose a scheme for creation and transfer of coherence among ground state and indirect exciton states of triple quantum dots via the technique of stimulated Raman adiabatic passage. Compared with the traditional stimulated Raman adiabatic passage, the Stokes laser pulse is replaced by the tunneling pulse, which can be controlled by the externally applied voltages. By varying the amplitudes and sequences of the pump and tunneling pulses, a complete coherence transfer or an equal coherence distribution among multiple states can be obtained. The investigations can provide further insight for the experimental development of controllable coherence transfer in semiconductor structure and may have potential applications in quantum information processing.

  7. Piecewise Adiabatic Population Transfer in a Molecule via a Wave Packet

    SciTech Connect

    Shapiro, Evgeny A.; Peer, Avi; Ye Jun; Shapiro, Moshe

    2008-07-11

    We propose a class of schemes for robust population transfer between quantum states that utilize trains of coherent pulses, thus forming a generalized adiabatic passage via a wave packet. We study piecewise stimulated Raman adiabatic passage with pulse-to-pulse amplitude variation, and piecewise chirped Raman passage with pulse-to-pulse phase variation, implemented with an optical frequency comb. In the context of production of ultracold ground-state molecules, we show that with almost no knowledge of the excited potential, robust high-efficiency transfer is possible.

  8. Non-equilibrium scale invariance and shortcuts to adiabaticity in a one-dimensional Bose gas

    PubMed Central

    Rohringer, W.; Fischer, D.; Steiner, F.; Mazets, I. E.; Schmiedmayer, J.; Trupke, M.

    2015-01-01

    We present experimental evidence for scale invariant behaviour of the excitation spectrum in phase-fluctuating quasi-1d Bose gases after a rapid change of the external trapping potential. Probing density correlations in free expansion, we find that the temperature of an initial thermal state scales with the spatial extension of the cloud as predicted by a model based on adiabatic rescaling of initial eigenmodes with conserved quasiparticle occupation numbers. Based on this result, we demonstrate that shortcuts to adiabaticity for the rapid expansion or compression of the gas do not induce additional heating. PMID:25867640

  9. Protecting and accelerating adiabatic passage with time-delayed pulse sequences.

    PubMed

    Sampedro, Pablo; Chang, Bo Y; Sola, Ignacio R

    2016-05-21

    Using numerical simulations of two-photon electronic absorption with femtosecond pulses in Na2 we show that: (i) it is possible to avoid the characteristic saturation or dumped Rabi oscillations in the yield of absorption by time-delaying the laser pulses; (ii) it is possible to accelerate the onset of adiabatic passage by using the vibrational coherence starting in a wave packet; and (iii) it is possible to prepare the initial wave packet in order to achieve full state-selective transitions with broadband pulses. The findings can be used, for instance, to achieve ultrafast adiabatic passage by light-induced potentials and understand its intrinsic robustness.

  10. Electronic non-adiabatic states: towards a density functional theory beyond the Born–Oppenheimer approximation

    PubMed Central

    Gidopoulos, Nikitas I.; Gross, E. K. U.

    2014-01-01

    A novel treatment of non-adiabatic couplings is proposed. The derivation is based on a theorem by Hunter stating that the wave function of the complete system of electrons and nuclei can be written, without approximation, as a Born–Oppenheimer (BO)-type product of a nuclear wave function, X(R), and an electronic one, ΦR(r), which depends parametrically on the nuclear configuration R. From the variational principle, we deduce formally exact equations for ΦR(r) and X(R). The algebraic structure of the exact nuclear equation coincides with the corresponding one in the adiabatic approximation. The electronic equation, however, contains terms not appearing in the adiabatic case, which couple the electronic and the nuclear wave functions and account for the electron–nuclear correlation beyond the BO level. It is proposed that these terms can be incorporated using an optimized local effective potential. PMID:24516183

  11. Dynamics of an optomechanical system with quadratic coupling: Effect of first order correction to adiabatic elimination

    PubMed Central

    Jiang, Cheng; Cui, Yuanshun; Chen, Guibin

    2016-01-01

    We explore theoretically the dynamics of an optomechanical system in which a resonantly driven cavity mode is quadratically coupled to the displacement of a mechanical resonator. Considering the first order correction to adiabatic elimination, we obtain the analytical expression of optomechanical damping rate which is negative and depends on the position of the mechanical resonator. After comparing the numerical results between the full simulation of Langevin equations, adiabatic elimination, and first order correction to adiabatic elimination, we explain the dynamics of the system in terms of overall mechanical potential and optomechanical damping rate. The antidamping induced by radiation pressure can result in self-sustained oscillation of the mechanical resonator. Finally, we discuss the time evolution of the intracavity photon number, which also shows that the effect of first order correction cannot be neglected when the ratio of the cavity decay rate to the mechanical resonance frequency becomes smaller than a critical value. PMID:27752125

  12. Dynamic potential and surface morphology study of sertraline membrane sensors.

    PubMed

    Khater, M M; Issa, Y M; Hassib, H B; Mohammed, S H

    2015-05-01

    New rapid, sensitive and simple electrometric method was developed to determine sertraline hydrochloride (Ser-Cl) in its pure raw material and pharmaceutical formulations. Membrane sensors based on heteropolyacids as ion associating material were prepared. Silicomolybdic acid (SMA), silicotungstic acid (STA) and phosphomolybdic acid (PMA) were used. The slope and limit of detection are 50.00, 60.00 and 53.24 mV/decade and 2.51, 5.62 and 4.85 μmol L(-1) for Ser-ST, Ser-PM and Ser-SM membrane sensors, respectively. Linear range is 0.01-10.00 for the three sensors. These new sensors were used for the potentiometric titration of Ser-Cl using sodium tetraphenylborate as titrant. The surface morphologies of the prepared membranes with and without the modifier (ion-associate) were studied using scanning and atomic force microscopes.

  13. Dynamic potential and surface morphology study of sertraline membrane sensors

    PubMed Central

    Khater, M.M.; Issa, Y.M.; Hassib, H.B.; Mohammed, S.H.

    2014-01-01

    New rapid, sensitive and simple electrometric method was developed to determine sertraline hydrochloride (Ser-Cl) in its pure raw material and pharmaceutical formulations. Membrane sensors based on heteropolyacids as ion associating material were prepared. Silicomolybdic acid (SMA), silicotungstic acid (STA) and phosphomolybdic acid (PMA) were used. The slope and limit of detection are 50.00, 60.00 and 53.24 mV/decade and 2.51, 5.62 and 4.85 μmol L−1 for Ser-ST, Ser-PM and Ser-SM membrane sensors, respectively. Linear range is 0.01–10.00 for the three sensors. These new sensors were used for the potentiometric titration of Ser-Cl using sodium tetraphenylborate as titrant. The surface morphologies of the prepared membranes with and without the modifier (ion-associate) were studied using scanning and atomic force microscopes. PMID:26257944

  14. Accurate ab initio potential energy surfaces for the 3A'' and 3A' electronic states of the O(3P)+HBr system.

    PubMed

    de Oliveira-Filho, Antonio G S; Ornellas, Fernando R; Peterson, Kirk A

    2012-05-07

    In this work, we report the construction of potential energy surfaces for the (3)A('') and (3)A(') states of the system O((3)P) + HBr. These surfaces are based on extensive ab initio calculations employing the MRCI+Q/CBS+SO level of theory. The complete basis set energies were estimated from extrapolation of MRCI+Q/aug-cc-VnZ(-PP) (n = Q, 5) results and corrections due to spin-orbit effects obtained at the CASSCF/aug-cc-pVTZ(-PP) level of theory. These energies, calculated over a region of the configuration space relevant to the study of the reaction O((3)P) + HBr → OH + Br, were used to generate functions based on the many-body expansion. The three-body potentials were interpolated using the reproducing kernel Hilbert space method. The resulting surface for the (3)A('') electronic state contains van der Waals minima on the entrance and exit channels and a transition state 6.55 kcal/mol higher than the reactants. This barrier height was then scaled to reproduce the value of 5.01 kcal/mol, which was estimated from coupled cluster benchmark calculations performed to include high-order and core-valence correlation, as well as scalar relativistic effects. The (3)A(') surface was also scaled, based on the fact that in the collinear saddle point geometry these two electronic states are degenerate. The vibrationally adiabatic barrier heights are 3.44 kcal/mol for the (3)A('') and 4.16 kcal/mol for the (3)A(') state.

  15. Intermolecular potential energy surface and thermophysical properties of ethylene oxide

    NASA Astrophysics Data System (ADS)

    Crusius, Johann-Philipp; Hellmann, Robert; Hassel, Egon; Bich, Eckard

    2014-10-01

    A six-dimensional potential energy hypersurface (PES) for two interacting rigid ethylene oxide (C2H4O) molecules was determined from high-level quantum-chemical ab initio calculations. The counterpoise-corrected supermolecular approach at the MP2 and CCSD(T) levels of theory was utilized to determine interaction energies for 10178 configurations of two molecules. An analytical site-site potential function with 19 sites per ethylene oxide molecule was fitted to the interaction energies and fine tuned to agree with data for the second acoustic virial coefficient from accurate speed of sound measurements. The PES was validated by computing the second virial coefficient, shear viscosity, and thermal conductivity. The values of these properties are substantiated by the best experimental data as they tend to fall within the uncertainty intervals and also obey the experimental temperature functions, except for viscosity, where experimental data are insufficient. Due to the lack of reliable data, especially for the transport properties, our calculated values are currently the most accurate estimates for these properties of ethylene oxide.

  16. Intermolecular potential energy surface and thermophysical properties of ethylene oxide

    SciTech Connect

    Crusius, Johann-Philipp Hassel, Egon; Hellmann, Robert; Bich, Eckard

    2014-10-28

    A six-dimensional potential energy hypersurface (PES) for two interacting rigid ethylene oxide (C{sub 2}H{sub 4}O) molecules was determined from high-level quantum-chemical ab initio calculations. The counterpoise-corrected supermolecular approach at the MP2 and CCSD(T) levels of theory was utilized to determine interaction energies for 10178 configurations of two molecules. An analytical site-site potential function with 19 sites per ethylene oxide molecule was fitted to the interaction energies and fine tuned to agree with data for the second acoustic virial coefficient from accurate speed of sound measurements. The PES was validated by computing the second virial coefficient, shear viscosity, and thermal conductivity. The values of these properties are substantiated by the best experimental data as they tend to fall within the uncertainty intervals and also obey the experimental temperature functions, except for viscosity, where experimental data are insufficient. Due to the lack of reliable data, especially for the transport properties, our calculated values are currently the most accurate estimates for these properties of ethylene oxide.

  17. 3D Printed Potential and Free Energy Surfaces for Teaching Fundamental Concepts in Physical Chemistry

    ERIC Educational Resources Information Center

    Kaliakin, Danil S.; Zaari, Ryan R.; Varganov, Sergey A.

    2015-01-01

    Teaching fundamental physical chemistry concepts such as the potential energy surface, transition state, and reaction path is a challenging task. The traditionally used oversimplified 2D representation of potential and free energy surfaces makes this task even more difficult and often confuses students. We show how this 2D representation can be…

  18. Determination of caloric values of agricultural crops and crop waste by Adiabatic Bomb Calorimetry

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Calorific values of agricultural crops and their waste were measured by adiabatic bomb calorimetry. Sustainable farming techniques require that all potential sources of revenue be utilized. A wide variety of biomass is beginning to be used as alternative fuels all over the world. The energy potentia...

  19. Analytical approximation of the InGaZnO thin-film transistors surface potential

    NASA Astrophysics Data System (ADS)

    Colalongo, Luigi

    2016-10-01

    Surface-potential-based mathematical models are among the most accurate and physically based compact models of thin-film transistors, and in turn of indium gallium zinc oxide TFTs, available today. However, the need of iterative computations of the surface potential limits their computational efficiency and diffusion in CAD applications. The existing closed-form approximations of the surface potential are based on regional approximations and empirical smoothing functions that could result not accurate enough in particular to model transconductances and transcapacitances. In this work we present an extremely accurate (in the range of nV) and computationally efficient non-iterative approximation of the surface potential that can serve as a basis for advanced surface-potential-based indium gallium zinc oxide TFTs models.

  20. Microbial population and functional dynamics associated with surface potential and carbon metabolism

    PubMed Central

    Ishii, Shun'ichi; Suzuki, Shino; Norden-Krichmar, Trina M; Phan, Tony; Wanger, Greg; Nealson, Kenneth H; Sekiguchi, Yuji; Gorby, Yuri A; Bretschger, Orianna

    2014-01-01

    Microbial extracellular electron transfer (EET) to solid surfaces is an important reaction for metal reduction occurring in various anoxic environments. However, it is challenging to accurately characterize EET-active microbial communities and each member's contribution to EET reactions because of changes in composition and concentrations of electron donors and solid-phase acceptors. Here, we used bioelectrochemical systems to systematically evaluate the synergistic effects of carbon source and surface redox potential on EET-active microbial community development, metabolic networks and overall electron transfer rates. The results indicate that faster biocatalytic rates were observed under electropositive electrode surface potential conditions, and under fatty acid-fed conditions. Temporal 16S rRNA-based microbial community analyses showed that Geobacter phylotypes were highly diverse and apparently dependent on surface potentials. The well-known electrogenic microbes affiliated with the Geobacter metallireducens clade were associated with lower surface potentials and less current generation, whereas Geobacter subsurface clades 1 and 2 were associated with higher surface potentials and greater current generation. An association was also observed between specific fermentative phylotypes and Geobacter phylotypes at specific surface potentials. When sugars were present, Tolumonas and Aeromonas phylotypes were preferentially associated with lower surface potentials, whereas Lactococcus phylotypes were found to be closely associated with Geobacter subsurface clades 1 and 2 phylotypes under higher surface potential conditions. Collectively, these results suggest that surface potentials provide a strong selective pressure, at the species and strain level, for both solid surface respirators and fermentative microbes throughout the EET-active community development. PMID:24351938

  1. Non-adiabatic effects in near-adiabatic mixed-field orientation and alignment

    NASA Astrophysics Data System (ADS)

    Maan, Anjali; Ahlawat, Dharamvir Singh; Prasad, Vinod

    2016-11-01

    We present a theoretical study of the impact of a pair of moderate electric fields tilted an angle with respect to one another on a molecule. As a prototype, we consider a molecule with large rotational constant (with corresponding small rotational period) and moderate dipole moment. Within rigid-rotor approximation, the time-dependent Schrodinger equation is solved using fourth-order Runge-Kutta method. We have analysed that lower rotational states are significantly influenced by variation in pulse durations, the tilt angle between the fields and also on the electric field strengths. We also suggest a control scheme of how the rotational dynamics, orientation and alignment of a molecule can be enhanced by a combination of near-adiabatic pulses in comparision to non-adiabatic or adiabatic pulses.

  2. Characterization of the thrombogenic potential of surface oxides on stainless steel for implant purposes

    NASA Astrophysics Data System (ADS)

    Shih, Chun-Che; Shih, Chun-Ming; Su, Yea-Yang; Chang, Mau-Song; Lin, Shing-Jong

    2003-12-01

    Marketed stents are manufactured from various metals and passivated with different degrees of surface oxidation. The functional surface oxides on the degree of antithrombotic potential were explored through a canine femoral extracorporeal circuit model. Related properties of these oxide films were studied by open-circuit potential, current density detected at open-circuit potential, the electrochemical impedance spectroscopy, transmission electron microscopy, Auger spectroscopy (AES), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy. Experimental evidences showed that blood clot weight after a 30-min follow-up was significantly lower for the stainless steel wire passivated with amorphous oxide (AO) compared to the wire passivated with polycrystalline oxide (PO) or commercial as-received wire coils (AS). Surface characterizations showed that a stable negative current density at open-circuit potential and a significant lower potential were found for the wire surface passivated with AO than for the surface passivated with PO. Time constant of AO is about 25 times larger than that of polycrystalline oxide. Significant difference in oxide grain sizes was found between PO and AO. Surface chemistries revealed by the AES and XPS spectra indicated the presence of a Cr- and oxygen-rich surface oxide for AO, and a Fe-rich and oxygen-lean surface oxide for PO. These remarkable characteristics of AO surface film might have a potential to provide for excellent antithrombotic characteristics for the 316L stainless steel stents.

  3. Potential surfaces for O atom-polymer reactions

    NASA Technical Reports Server (NTRS)

    Laskowski, B. C.; Jaffe, R. L.

    1987-01-01

    Ab initio quantum chemistry methods are used to study the energetics of interactions of O atoms with organic compounds. Polyethylene (CH2)n has been chosen as the model system to study the interactions of O(3P) and O(1D) atoms with polymers. In particular, H abstraction is investigated and polyethylene is represented by a C3 (propane) oligomeric model. The gradient method, as implemented in the GRADSCF package of programs, is used to determine the geometries and energies of products and reactants. The saddle point, barrier geometry is determined by minimizing the squares of the gradients of the potential with respect to the internal coordinates. To correctly describe the change in bonding during the reaction at least a two configuration MCSCF (multiconfiguration self consistent field) or GVB (generalized valence bond) wave function has to be used. Basis sets include standard Pople and Dunning sets, however, increased with polarization functions and diffuse p functions on both the C and O atoms. The latter is important due to the O(-) character of the wave function at the saddle point and products. Normal modes and vibrational energy levels are given for the reactants, saddle points and products. Finally, quantitative energetics are obtained by implementing a small CAS (complete active space) approach followed by limited configuration interaction (CI) calculations. Comparisons are made with available experimental data.

  4. Non-adiabatic molecular dynamics with complex quantum trajectories. I. The diabatic representation.

    PubMed

    Zamstein, Noa; Tannor, David J

    2012-12-14

    We extend a recently developed quantum trajectory method [Y. Goldfarb, I. Degani, and D. J. Tannor, J. Chem. Phys. 125, 231103 (2006)] to treat non-adiabatic transitions. Each trajectory evolves on a single surface according to Newton's laws with complex positions and momenta. The transfer of amplitude between surfaces stems naturally from the equations of motion, without the need for surface hopping. In this paper we derive the equations of motion and show results in the diabatic representation, which is rarely used in trajectory methods for calculating non-adiabatic dynamics. We apply our method to the first two benchmark models introduced by Tully [J. Chem. Phys. 93, 1061 (1990)]. Besides giving the probability branching ratios between the surfaces, the method also allows the reconstruction of the time-dependent wavepacket. Our results are in quantitative agreement with converged quantum mechanical calculations.

  5. Potential effects of forest management on surface albedo

    NASA Astrophysics Data System (ADS)

    Otto, J.; Bréon, F.-M.; Schelhaas, M.-J.; Pinty, B.; Luyssaert, S.

    2012-04-01

    Currently 70% of the world's forests are managed and this figure is likely to rise due to population growth and increasing demand for wood based products. Forest management has been put forward by the Kyoto-Protocol as one of the key instruments in mitigating climate change. For temperate and boreal forests, the effects of forest management on the stand-level carbon balance are reasonably well understood, but the biophysical effects, for example through changes in the albedo, remain elusive. Following a modeling approach, we aim to quantify the variability in albedo that can be attributed to forest management through changes in canopy structure and density. The modelling approach chains three separate models: (1) a forest gap model to describe stand dynamics, (2) a Monte-Carlo model to estimate the probability density function of the optical path length of photons through the canopy and (3) a physically-based canopy transfer model to estimate the interaction between photons and leaves. The forest gap model provides, on a monthly time step the position, height, diameter, crown size and leaf area index of individual trees. The Monte-Carlo model computes from this the probability density function of the distance a photon travels through crown volumes to determine the direct light reaching the forest floor. This information is needed by the canopy transfer model to calculate the effective leaf area index - a quantity that allows it to correctly represent a 3D process with a 1D model. Outgoing radiation is calculated as the result of multiple processes involving the scattering due to the canopy layer and the forest floor. Finally, surface albedo is computed as the ratio between incident solar radiation and calculated outgoing radiation. The study used two time series representing thinning from below of a beech and a Scots pine forest. The results show a strong temporal evolution in albedo during stand establishment followed by a relatively stable albedo once the canopy

  6. Ab initio potential energy and dipole moment surfaces for CS2: determination of molecular vibrational energies.

    PubMed

    Pradhan, Ekadashi; Carreón-Macedo, José-Luis; Cuervo, Javier E; Schröder, Markus; Brown, Alex

    2013-08-15

    The ground state potential energy and dipole moment surfaces for CS2 have been determined at the CASPT2/C:cc-pVTZ,S:aug-cc-pV(T+d)Z level of theory. The potential energy surface has been fit to a sum-of-products form using the neural network method with exponential neurons. A generic interface between neural network potential energy surface fitting and the Heidelberg MCTDH software package is demonstrated. The potential energy surface has also been fit using the potfit procedure in MCTDH. For fits to the low-energy regions of the potential, the neural network method requires fewer parameters than potfit to achieve high accuracy; global fits are comparable between the two methods. Using these potential energy surfaces, the vibrational energies have been computed for the four most abundant CS2 isotopomers. These results are compared to experimental and previous theoretical data. The current potential energy surfaces are shown to accurately reproduce the low-lying vibrational energies within a few wavenumbers. Hence, the potential energy and dipole moments surfaces will be useful for future study on the control of quantum dynamics in CS2.

  7. He-LiF surface interaction potential from fast atom diffraction

    SciTech Connect

    Schueller, A.; Winter, H.; Gravielle, M. S.; Miraglia, J. E.; Pruneda, J. M.

    2009-12-15

    Diffraction patterns produced by grazing scattering of fast atoms from insulator surfaces are used to examine the atom-surface interaction. The method is applied to He atoms colliding with a LiF(001) surface along axial crystallographic channels. The projectile-surface potential is obtained from an accurate density-functional theory calculation, which includes polarization effects and surface relaxation. For the description of the collision process we employ the surface eikonal approximation, which takes into account quantum interference between different projectile paths. The dependence of projectile spectra on the parallel and perpendicular incident energies is experimentally and theoretically analyzed, demonstrating the range of applicability of the proposed model.

  8. Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering

    NASA Astrophysics Data System (ADS)

    Schreck, Simon; Pietzsch, Annette; Kennedy, Brian; Såthe, Conny; Miedema, Piter S.; Techert, Simone; Strocov, Vladimir N.; Schmitt, Thorsten; Hennies, Franz; Rubensson, Jan-Erik; Föhlisch, Alexander

    2016-01-01

    Thermally driven chemistry as well as materials’ functionality are determined by the potential energy surface of a systems electronic ground state. This makes the potential energy surface a central and powerful concept in physics, chemistry and materials science. However, direct experimental access to the potential energy surface locally around atomic centers and to its long-range structure are lacking. Here we demonstrate how sub-natural linewidth resonant inelastic soft x-ray scattering at vibrational resolution is utilized to determine ground state potential energy surfaces locally and detect long-range changes of the potentials that are driven by local modifications. We show how the general concept is applicable not only to small isolated molecules such as O2 but also to strongly interacting systems such as the hydrogen bond network in liquid water. The weak perturbation to the potential energy surface through hydrogen bonding is observed as a trend towards softening of the ground state potential around the coordinating atom. The instrumental developments in high resolution resonant inelastic soft x-ray scattering are currently accelerating and will enable broad application of the presented approach. With this multidimensional potential energy surfaces that characterize collective phenomena such as (bio)molecular function or high-temperature superconductivity will become accessible in near future.

  9. Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering.

    PubMed

    Schreck, Simon; Pietzsch, Annette; Kennedy, Brian; Såthe, Conny; Miedema, Piter S; Techert, Simone; Strocov, Vladimir N; Schmitt, Thorsten; Hennies, Franz; Rubensson, Jan-Erik; Föhlisch, Alexander

    2016-01-29

    Thermally driven chemistry as well as materials' functionality are determined by the potential energy surface of a systems electronic ground state. This makes the potential energy surface a central and powerful concept in physics, chemistry and materials science. However, direct experimental access to the potential energy surface locally around atomic centers and to its long-range structure are lacking. Here we demonstrate how sub-natural linewidth resonant inelastic soft x-ray scattering at vibrational resolution is utilized to determine ground state potential energy surfaces locally and detect long-range changes of the potentials that are driven by local modifications. We show how the general concept is applicable not only to small isolated molecules such as O2 but also to strongly interacting systems such as the hydrogen bond network in liquid water. The weak perturbation to the potential energy surface through hydrogen bonding is observed as a trend towards softening of the ground state potential around the coordinating atom. The instrumental developments in high resolution resonant inelastic soft x-ray scattering are currently accelerating and will enable broad application of the presented approach. With this multidimensional potential energy surfaces that characterize collective phenomena such as (bio)molecular function or high-temperature superconductivity will become accessible in near future.

  10. Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering

    PubMed Central

    Schreck, Simon; Pietzsch, Annette; Kennedy, Brian; Såthe, Conny; Miedema, Piter S.; Techert, Simone; Strocov, Vladimir N.; Schmitt, Thorsten; Hennies, Franz; Rubensson, Jan-Erik; Föhlisch, Alexander

    2016-01-01

    Thermally driven chemistry as well as materials’ functionality are determined by the potential energy surface of a systems electronic ground state. This makes the potential energy surface a central and powerful concept in physics, chemistry and materials science. However, direct experimental access to the potential energy surface locally around atomic centers and to its long-range structure are lacking. Here we demonstrate how sub-natural linewidth resonant inelastic soft x-ray scattering at vibrational resolution is utilized to determine ground state potential energy surfaces locally and detect long-range changes of the potentials that are driven by local modifications. We show how the general concept is applicable not only to small isolated molecules such as O2 but also to strongly interacting systems such as the hydrogen bond network in liquid water. The weak perturbation to the potential energy surface through hydrogen bonding is observed as a trend towards softening of the ground state potential around the coordinating atom. The instrumental developments in high resolution resonant inelastic soft x-ray scattering are currently accelerating and will enable broad application of the presented approach. With this multidimensional potential energy surfaces that characterize collective phenomena such as (bio)molecular function or high-temperature superconductivity will become accessible in near future. PMID:26821751

  11. Calculation of the structure, potential energy surface, vibrational dynamics, and electric dipole properties for the Xe:HI van der Waals complex.

    PubMed

    Preller, M; Grunenberg, J; Bulychev, V P; Bulanin, M O

    2011-05-07

    We report the structure and spectroscopic characteristics for the Xe:HI van der Waals binary isomers determined from variational solutions of two-dimensional and three-dimensional (3D) vibrational Schrödinger equations. The solutions are based on a potential energy surface computed at the coupled-cluster level of theory including single and double excitations and a non-iterative perturbation treatment of triple excitations [CCSD(T)]. The dipole moment surface was calculated using quadratic configuration interaction (QCISD). The global potential minimum is shown to be located at the anti-hydrogen-bonded Xe-IH isomer, 21 cm(-1) below the secondary local minimum associated with the hydrogen-bonded Xe-HI isomeric form. The dissociation energy from the global minimum is 245.9 cm(-1). 3D Schrödinger equations are solved for the rotational quantum numbers J = k = 0, 1, and 2, without invoking an adiabatic separation of high- and low-frequency degrees of freedom. The vibrational ground state resides in the Xe-HI potential well, while the first excited state, 8.59 cm(-1) above the ground, occupies the Xe-IH well. We find that intra-complex dynamics exhibits a sudden transformation upon increase of the r(HI) bond length, accompanied by abrupt changes in the geometric and dipole parameters. A similar chaotic behavior is predicted to occur for Xe:DI at a shorter r(DI) bond length, which implies stronger coupling between low- and high-frequency motions in the heavier complex. Our calculations confirm a strong enhancement for the r(HI) stretch fundamental and a significant weakening for the first overtone vibrational transitions in Xe:HI, as compared to those in the free HI molecule. A qualitative explanation of this, earlier experimentally detected effect is suggested.

  12. Quantized adiabatic transport in momentum space.

    PubMed

    Ho, Derek Y H; Gong, Jiangbin

    2012-07-06

    Though topological aspects of energy bands are known to play a key role in quantum transport in solid-state systems, the implications of Floquet band topology for transport in momentum space (i.e., acceleration) have not been explored so far. Using a ratchet accelerator model inspired by existing cold-atom experiments, here we characterize a class of extended Floquet bands of one-dimensional driven quantum systems by Chern numbers, reveal topological phase transitions therein, and theoretically predict the quantization of adiabatic transport in momentum space. Numerical results confirm our theory and indicate the feasibility of experimental studies.

  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. Shortcuts to adiabaticity for quantum annealing

    NASA Astrophysics Data System (ADS)

    Takahashi, Kazutaka

    2017-01-01

    We study the Ising Hamiltonian with a transverse field term to simulate the quantum annealing. Using shortcuts to adiabaticity, we design the time dependence of the Hamiltonian. The dynamical invariant is obtained by the mean-field ansatz, and the Hamiltonian is designed by the inverse engineering. We show that the time dependence of physical quantities such as the magnetization is independent of the speed of the Hamiltonian variation in the infinite-range model. We also show that rotating transverse magnetic fields are useful to achieve the ideal time evolution.

  15. 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.

  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. Cavity-state preparation using adiabatic transfer

    NASA Astrophysics Data System (ADS)

    Larson, Jonas; Andersson, Erika

    2005-05-01

    We show how to prepare a variety of cavity field states for multiple cavities. The state preparation technique used is related to the method of stimulated adiabatic Raman passage. The cavity modes are coupled by atoms, making it possible to transfer an arbitrary cavity field state from one cavity to another and also to prepare nontrivial cavity field states. In particular, we show how to prepare entangled states of two or more cavities, such as an Einstein-Podolsky-Rosen state and a W state, as well as various entangled superpositions of coherent states in different cavities, including Schrödinger cat states. The theoretical considerations are supported by numerical simulations.

  18. Generalized Ramsey numbers through adiabatic quantum optimization

    NASA Astrophysics Data System (ADS)

    Ranjbar, Mani; Macready, William G.; Clark, Lane; Gaitan, Frank

    2016-09-01

    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.

  19. A three-dimensional He-CO potential energy surface with improved long-range behavior

    NASA Astrophysics Data System (ADS)

    McBane, George C.

    2016-12-01

    A weakness of the "CBS + corr" He-CO potential energy surface (Peterson and McBane, 2005) has been rectified by constraining the potential to adopt accurate long-range behavior for He-CO distances well beyond 15a0 . The resulting surface is very similar to the original in the main part of the interaction. Comparison with accurately known bound-state energies indicates that the surface is slightly improved in the region sampled by the highest lying bound states. The positions of shape and Feshbach resonances within a few cm-1 of the j = 1 excitation threshold are essentially unchanged. The low-energy scattering lengths changed noticeably. The revised surface generates a small negative limiting scattering length for collisions with 4He, while the original surface gave a small positive one. Both surfaces yield scattering lengths quite different from the widely used surface of Heijmen et al. (1997) for both He isotopes.

  20. Global triplet potential energy surfaces for the N2(X(1)Σ) + O((3)P) → NO(X(2)Π) + N((4)S) reaction.

    PubMed

    Lin, Wei; Varga, Zoltan; Song, Guoliang; Paukku, Yuliya; Truhlar, Donald G

    2016-01-14

    This work presents two global triplet potential energy surfaces (PESs) for the high-energy reaction N2(X(1)Σ) + O((3)P) → NO(X(2)Π) + N((4)S)-in particular, for the lowest energy (3)A' and (3)A″ PESs. In order to obtain the energies needed for fitting analytic surfaces, we carried out multireference configuration interaction (MRCI) calculations based on wave functions obtained from state-averaged complete active space self-consistent field calculations for 2280 geometries for the three lowest (3)A″ states and for 2298 geometries for the three lowest (3)A' states. The lowest-energy (3)A' and (3)A″ states at each of these geometries were then improved by applying the dynamically scaled external correlation (DSEC) method to all MRCI points, and the resulting DSEC energies were used for construction of the ground-state PES for each symmetry. The many-body component of the DSEC energies for the three-dimensional (3)A' and (3)A″ PESs was then least-squares fitted in terms of permutationally invariant polynomials in mixed exponential-Gaussian bond order variables. The global and local minima as well as the transition structures of both the (3)A' and the (3)A″ analytic PES were explored. In agreement with previous work, we find that the reverse reaction is barrierless on the (3)A″ surface along the minimum energy pathway. However, we have explored several new local minima and transition structures on the (3)A' PES. Furthermore, based on the newly found minima and transition structures, two independent reaction mechanisms have been illustrated for the reaction path on the (3)A' PES. The analytic surfaces may be used for dynamics calculations of electronically adiabatic reactive scattering and energy transfer.

  1. Cardiac Body Surface Potentials in Rats with Experimental Pulmonary Hypertension during Ventricular Depolarization.

    PubMed

    Suslonova, O V; Smirnova, S L; Roshchevskaya, I M

    2016-11-01

    The spatial and the amplitude-temporal parameters of cardiac body surface potentials were examined in female Wistar rats with experimental pulmonary hypertension during ventricular depolarization. The cardiac body surface potentials have been led from 64 subcutaneous electrodes evenly distributed across the chest surface prior to and 4 weeks after subcutaneous injection of a single dose of monocrotaline (60 mg/kg). Right ventricular hypertrophy and electrophysiological remodeling of the heart developed in rats with experimental pulmonary hypertension in 4 weeks after monocrotaline injection; these changes led to a significant increase in amplitude and temporal characteristics of the cardioelectric field on the body surface in comparison with the initial state.

  2. Surface potential and permeability of rock cores under asphaltenic oil flow conditions

    SciTech Connect

    Alkafeef, S.F.; Gochin, R.J.; Smith, A.L.

    1995-12-31

    The surface properties, wetting behaviour and permeability of rock samples are central to understanding recovery behaviour in oil reservoirs. This paper will present a method new to petroleum engineering to show how area/length ratios for porous systems can be obtained by combining streaming potential and streaming current measurements on rock cores. This has allows streaming current measurements (independent of surface conductivity errors) to be made on rock samples using hydrocarbon solvents with increasing concentrations of asphaltene. Negative surface potentials for the rock became steadily more positive as asphaltene coated the pore surfaces, with permeability reduction agreeing well with petrographic analysis.

  3. Structure and stability of pyrophyllite edge surfaces: Effect of temperature and water chemical potential

    NASA Astrophysics Data System (ADS)

    Kwon, Kideok D.; Newton, Aric G.

    2016-10-01

    The surfaces of clay minerals, which are abundant in atmospheric mineral dust, serve as an important medium to catalyze ice nucleation. The lateral edge surface of 2:1 clay minerals is postulated to be a potential site for ice nucleation. However, experimental investigations of the edge surface structure itself have been limited compared to the basal planes of clay minerals. Density functional theory (DFT) computational studies have provided insights into the pyrophyllite edge surface. Pyrophyllite is an ideal surrogate mineral for the edge surfaces of 2:1 clay minerals as it possesses no or little structural charge. Of the two most-common hydrated edge surfaces, the AC edge, (1 1 0) surface in the monoclinic polytype notation, is predicted to be more stable than the B edge, (0 1 0) surface. These stabilities, however, were determined based on the total energies calculated at 0 K and did not consider environmental effects such as temperature and humidity. In this study, atomistic thermodynamics based on periodic DFT electronic calculations was applied to examine the effects of environmental variables on the structure and thermodynamic stability of the common edge surfaces in equilibrium with bulk pyrophyllite and water vapor. We demonstrate that the temperature-dependent vibrational energy of sorbed water molecules at the edge surface is a significant component of the surface free energy and cannot be neglected when determining the surface stability of pyrophyllite. The surface free energies were calculated as a function of temperature from 240 to 600 K and water chemical potential corresponding to conditions from ultrahigh vacuum to the saturation vapor pressure of water. We show that at lower water chemical potentials (dry conditions), the AC and B edge surfaces possessed similar stabilities; at higher chemical potentials (humid conditions) the AC edge surface was more stable than the B edge surface. At high temperatures, both surfaces showed similar stabilities

  4. Development of a "First Principles" Water Potential with Flexible Monomers: Dimer Potential Energy Surface, VRT Spectrum, and Second Virial Coefficient.

    PubMed

    Babin, Volodymyr; Leforestier, Claude; Paesani, Francesco

    2013-12-10

    The development of a "first principles" water potential with flexible monomers (MB-pol) for molecular simulations of water systems from gas to condensed phases is described. MB-pol is built upon the many-body expansion of the intermolecular interactions, and the specific focus of this study is on the two-body term (V2B) representing the full-dimensional intermolecular part of the water dimer potential energy surface. V2B is constructed by fitting 40,000 dimer energies calculated at the CCSD(T)/CBS level of theory and imposing the correct asymptotic behavior at long-range as predicted from "first principles". The comparison of the calculated vibration-rotation tunneling (VRT) spectrum and second virial coefficient with the corresponding experimental results demonstrates the accuracy of the MB-pol dimer potential energy surface.

  5. Numerical simulations of solar spicules: Adiabatic and non-adiabatic studies

    NASA Astrophysics Data System (ADS)

    Kuźma, B.; Murawski, K.; Zaqarashvili, T. V.; Konkol, P.; Mignone, A.

    2017-01-01

    Aims: We aim to study the formation and evolution of solar spicules using numerical simulations of a vertical velocity pulse that is launched from the upper chromosphere. Methods: With the use of the PLUTO code, we numerically solved adiabatic and non-adiabatic magnetohydrodynamic (MHD) equations in 2D cylindrical geometry. We followed the evolution of spicules triggered by pulses that are launched in a vertical velocity component from the upper chromosphere. Then we compared the results obtained with and without non-adiabatic terms in the MHD equations. Results: Our numerical results reveal that the velocity pulse is steepened into a shock that propagates upward into the corona. The chromospheric cold and dense plasma follows the shock and rises into the corona with the mean speed of 20-25 km s-1. The nonlinear wake behind the pulse in the stratified atmosphere leads to quasi-periodic rebound shocks, which lead to quasi-periodic rising of chromospheric plasma into the corona with a period close to the acoustic cut-off period of the chromosphere. We found that the effect of non-adiabatic terms on spicule evolution is minor; the general properties of spicules such as their heights and rising-time remain slightly affected by these terms. Conclusions: In the framework of the axisymmetric model we devised, we show that the solar spicules can be triggered by the vertical velocity pulses, and thermal conduction and radiative cooling terms do not exert any significant influence on the dynamics of these spicules.

  6. Inner-Helmholtz potential development at the hematite (α-Fe2O3) (001) surface

    SciTech Connect

    Boily, Jean-François; Chatman, Shawn; Rosso, Kevin M.

    2011-08-01

    Electric potentials of the (001) plane of hematite were measured as a function of pH and ionic strength in solutions of sodium nitrate and oxalic acid using the single-crystal electrode approach. The surface is predominantly charge-neutral in the pH 4-14 range, and develops a positive surface potential below pH 4 due to protonation of μ-OH0 sites (pK1,1,0 int = -1.34). This site is resilient to deprotonation up to at least pH 14 (-pK-1,1,0 int >> 21). The associated Stern layer capacitance of 0.62 F/m2 is smaller than typical values of powders, and possibly arises from a lower degree of surface solvation. Acid-promoted dissolution under elevated concentrations of HNO3 etches the (001) surface, yielding a convoluted surface populated by OH20.5+ sites. The resulting surface potential was therefore larger under these conditions than in the absence of dissolution. Oxalate ions also promoted (001) dissolution. Associated electric potentials were strongly negative, with values as large as -0.5 V, possibly from metal-bonded interactions with oxalate. The hematite surface can also acquire negative potentials in the pH 7-11 range due to surface complexation and/or precipitation of iron species (0.003 Fe/nm2) produced from acidic conditions. Oxalate-bearing systems also result in negative potentials in the same pH range, and may include ferric-oxalate surface complexes and/or surface precipitates. All measurements can be modeled by a thermodynamic model that can be used to predict inner-Helmholtz potentials of hematite electrodes.

  7. 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.

  8. Adiabatic following for a three-state quantum system

    NASA Astrophysics Data System (ADS)

    Huang, Wei; Shore, Bruce W.; Rangelov, Andon; Kyoseva, Elica

    2017-01-01

    Adiabatic time-evolution - found in various forms of adiabatic following and adiabatic passage - is often advantageous for controlled manipulation of quantum systems due to its insensitivity to deviations in the pulse shapes and timings. In this paper we discuss controlled adiabatic evolution of a three-state quantum system, a natural advance to the widespread use of two-state systems in numerous contemporary applications. We discuss, and illustrate, not only possibilities for population transfer but also for creating, with prescribed relative phase, 50:50 superpositions of two Zeeman sublevels in a letter-vee coupling linkage.

  9. Adiabatic approximation via hodograph translation and zero-curvature equations

    NASA Astrophysics Data System (ADS)

    Karasev, M. V.

    2014-04-01

    For quantum as well classical slow-fast systems, we develop a general method which allows one to compute the adiabatic invariant (approximate integral of motion), its symmetries, the adiabatic guiding center coordinates and the effective scalar Hamiltonian in all orders of a small parameter. The scheme does not exploit eigenvectors or diagonalization, but is based on the ideas of isospectral deformation and zero-curvature equations, where the role of "time" is played by the adiabatic (quantization) parameter. The algorithm includes the construction of the zero-curvature adiabatic connection and its splitting generated by averaging up to an arbitrary order in the small parameter.

  10. Ultrafast hydrogen migration in acetylene cation driven by non-adiabatic effects.

    PubMed

    Madjet, Mohamed El-Amine; Li, Zheng; Vendrell, Oriol

    2013-03-07

    Non-adiabatic dynamics of the acetylene cation is investigated using mixed quantum-classical dynamics based on trajectory surface hopping. To describe the non-adiabatic effects, two surface hopping methods are used, namely, Tully's fewest switches and Landau-Zener surface hopping. Similarities and differences between the results based on those two methods are discussed. We find that the photoionization of acetylene into the first excited state A(2)Σg(+) drives the molecule from the linear structure to a trans-bent structure. Through a conical intersection the acetylene cation can relax back to either the ground state of acetylene or vinylidene. We conclude that hydrogen migration always takes place after non-radiative electronic relaxation to the ground state of the monocation. Based on the analysis of correlation functions we identify coherent oscillations between acetylene and vinylidene with a period of about 70 fs after the electronic relaxation.

  11. Adiabatic approximation for the Rabi model with broken inversion symmetry

    NASA Astrophysics Data System (ADS)

    Shen, Li-Tuo; Yang, Zhen-Biao; Wu, Huai-Zhi

    2017-01-01

    We study the properties and behavior of the Rabi model with broken inversion symmetry. Using an adiabatic approximation approach, we explore the high-frequency qubit and oscillator regimes, and obtain analytical solutions for the qubit-oscillator system. We demonstrate that, due to broken inversion symmetry, the positions of two potentials and zero-point energies in the oscillators become asymmetric and have a quadratic dependence on the mean dipole moments within the high-frequency oscillator regime. Furthermore, we find that there is a critical point above which the qubit-oscillator system becomes unstable, and the position of this critical point has a quadratic dependence on the mean dipole moments within the high-frequency qubit regime. Finally, we verify this critical point based on the method of semiclassical approximation.

  12. Adiabatic rotation of effective spin. II. Spin-rotational relaxation

    NASA Astrophysics Data System (ADS)

    Serebrennikov, Yu. A.; Steiner, U. E.

    1994-05-01

    The theory of electron spin-rotational (SR) relaxation in systems with an effective spin Seff=1/2 is formulated in terms of the adiabatic rotation of effective spin (ARES) approach. It is shown that SR relaxation results from the orientational random walk of the axes of the intramolecular electric field potential (ligand field) to which a spin-bearing atomic center is exposed. The validity of the stochastic treatment presented here is not limited by the Redfield conditions. The general expression obtained for the time constant of electron spin relaxation in liquid phase reproduces the well-known result of Hubbard-Atkins-Kivelson theory if it is specialized to the case of systems with weak spin-orbit coupling.

  13. Stabilization of Thin-Shell Implosions Using a High-Foot Adiabat-Shaped Drive on the National Ignition Facility

    NASA Astrophysics Data System (ADS)

    Lafon, Marion; Gauthier, Pascal; Masse, Laurent

    2016-10-01

    The High Foot (HF) campaign on the National Ignition Facility (NIF) has improved the neutron yield by an order of magnitude as compared to the implosions reported during the National Ignition Campaign (NIC) while dramatically lowering the ablation-front instability growth. However, this yield increase came at the expense of reduced fuel compression due to higher fuel adiabat. Thinner shell adiabat-shaped HF implosions have been designed to combine the ablation front stability benefits of the current HF pulses with the demonstrated high fuel compressibility of the NIC implosions and increased implosion velocity. This is accomplished by using a hybrid adiabat-shaping technique which both lowers the laser power between the first and second pulses to enhance the ablative stabilization at early times and precisely tailors the rise-to-peak drive to prevent undesired shocks from propagating in the fuel and depositing additional entropy. Ablation front growth factor spectra are generated from two-dimensional simulations with the FCI2 radiation hydrodynamics code. Linear analysis of the instability growth demonstrates that adiabat-shaped pulses provide a path to control and reduce ablation front instability growth while placing the fuel on a lower adiabat to achieve the alpha-heating-dominated regime. Adiabat-shaped pulses without picket are also investigated as a potential way to enhance the stability of the holhraum walls at early times.

  14. Quantitative analysis of molecular surfaces: areas, volumes, electrostatic potentials and average local ionization energies.

    PubMed

    Bulat, Felipe A; Toro-Labbé, Alejandro; Brinck, Tore; Murray, Jane S; Politzer, Peter

    2010-11-01

    We describe a procedure for performing quantitative analyses of fields f(r) on molecular surfaces, including statistical quantities and locating and evaluating their local extrema. Our approach avoids the need for explicit mathematical representation of the surface and can be implemented easily in existing graphical software, as it is based on the very popular representation of a surface as collection of polygons. We discuss applications involving the volumes, surface areas and molecular surface electrostatic potentials, and local ionization energies of a group of 11 molecules.

  15. 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.

  16. The genesis of adiabatic shear bands

    PubMed Central

    Landau, P.; Osovski, S.; Venkert, A.; Gärtnerová, V.; Rittel, D.

    2016-01-01

    Adiabatic shear banding (ASB) is a unique dynamic failure mechanism that results in an unpredicted catastrophic failure due to a concentrated shear deformation mode. It is universally considered as a material or structural instability and as such, ASB is hardly controllable or predictable to some extent. ASB is modeled on the premise of stability analyses. The leading paradigm is that a competition between strain (rate) hardening and thermal softening determines the onset of the failure. It was recently shown that microstructural softening transformations, such as dynamic recrystallization, are responsible for adiabatic shear failure. These are dictated by the stored energy of cold work, so that energy considerations can be used to macroscopically model the failure mechanism. The initial mechanisms that lead to final failure are still unknown, as well as the ASB formation mechanism(s). Most of all - is ASB an abrupt instability or rather a gradual transition as would be dictated by microstructural evolutions? This paper reports thorough microstructural characterizations that clearly show the gradual character of the phenomenon, best described as a nucleation and growth failure mechanism, and not as an abrupt instability as previously thought. These observations are coupled to a simple numerical model that illustrates them. PMID:27849023

  17. Accurate Variational Description of Adiabatic Quantum Optimization

    NASA Astrophysics Data System (ADS)

    Carleo, Giuseppe; Bauer, Bela; Troyer, Matthias

    Adiabatic quantum optimization (AQO) is a quantum computing protocol where a system is driven by a time-dependent Hamiltonian. The initial Hamiltonian has an easily prepared ground-state and the final Hamiltonian encodes some desired optimization problem. An adiabatic time evolution then yields a solution to the optimization problem. Several challenges emerge in the theoretical description of this protocol: on one hand, the exact simulation of quantum dynamics is exponentially complex in the size of the optimization problem. On the other hand, approximate approaches such as tensor network states (TNS) are limited to small instances by the amount of entanglement that can be encoded. I will present here an extension of the time-dependent Variational Monte Carlo approach to problems in AQO. This approach is based on a general class of (Jastrow-Feenberg) entangled states, whose parameters are evolved in time according to a stochastic variational principle. We demonstrate this approach for optimization problems of the Ising spin-glass type. A very good accuracy is achieved when compared to exact time-dependent TNS on small instances. We then apply this approach to larger problems, and discuss the efficiency of the quantum annealing scheme in comparison with its classical counterpart.

  18. 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)

  19. The formation of multiple adiabatic shear bands

    NASA Astrophysics Data System (ADS)

    Zhou, F.; Wright, T. W.; Ramesh, K. T.

    2006-07-01

    In a previous paper, Zhou et al. [2006. A numerical methodology for investigating adiabatic shear band formation. J. Mech. Phys. Solids, 54, 904-926] developed a numerical method for analyzing one-dimensional deformation of thermoviscoplastic materials. The method uses a second order algorithm for integration along characteristic lines, and computes the plastic flow after complete localization with high resolution and efficiency. We apply this numerical scheme to analyze localization in a thermoviscoplastic material where multiple shear bands are allowed to form at random locations in a large specimen. As a shear band develops, it unloads neighboring regions and interacts with other bands. Beginning with a random distribution of imperfections, which might be imagined as arising qualitatively from the microstructure, we obtain the average spacing of shear bands through calculations and compare our results with previously existing theoretical estimates. It is found that the spacing between nucleating shear bands follows the perturbation theory due to Wright and Ockendon [1996. A scaling law for the effect of inertia on the formation of adiabatic shear bands. Int. J. Plasticity 12, 927-934], whereas the spacing between mature shear bands is closer to that predicted by the momentum diffusion theory of Grady and Kipp [1987. The growth of unstable thermoplastic shear with application to steady-wave shock compression in solids. J. Mech. Phys. Solids 35, 95-119]. Scaling laws for the dependence of band spacing on material parameters differ in many respects from either theory.

  20. 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.

  1. Non-adiabatic Rayleigh-Taylor instability

    NASA Astrophysics Data System (ADS)

    Canfield, Jesse; Denissen, Nicholas; Reisner, Jon

    2016-11-01

    Onset of Rayleigh-Taylor instability (RTI) in a non-adiabatic environment is investigated with the multi-physics numerical model, FLAG. This work was inspired by laboratory experiments of non-adiabatic RTI, where a glass vessel with a layer of tetrahyrdofuran (THF) below a layer of toluene was placed inside a microwave. THF, a polar solvent, readily absorbs electromagnetic energy from microwaves. Toluene, a non-polar solvent, is nearly transparent to microwave heating. The presence of a heat source in the THF layer produced convection and a time-dependent Atwood number (At). The system, initially in stable hydrostatic equilibrium At < 0 , was set into motion by microwave induced, volumetric heating of the THF. The point when At > 0 , indicates that the system is RTI unstable. The observed dominant mode at the onset of RTI was the horizontal length scale of the vessel. This scale is contrary to classical RTI, where the modes start small and increases in scale with time. It is shown that the dominant RTI mode observed in the experiments was determined by the THF length scale prior to RTI. The dominant length scale transitions from the THF to the toluene via the updrafts and downdrafts in the convective cells. This happens when At passes from negative to positive. This work was funded by the Advanced Simulation and Computing Program.

  2. Adiabatic effects of electrons and ions on electro-acoustic solitary waves in an adiabatic dusty plasma

    NASA Astrophysics Data System (ADS)

    Tanjia, Fatema; Mamun, A. A.

    2009-02-01

    A dusty plasma consisting of negatively charged cold dust, adiabatic hot ions, and inertia-less adiabatic hot electrons has been considered. The adiabatic effects of electrons and ions on the basic properties of electro-acoustic solitary waves associated with different types of electro-acoustic (viz. ion-acoustic (IA), dust ion-acoustic (DIA), and dust acoustic (DA)) waves are thoroughly investigated by the reductive perturbation method. It is found that the basic properties of the IA, DIA, and DA waves are significantly modified by the adiabatic effects of ions and inertia-less electrons. The implications of our results in space and laboratory dusty plasmas are briefly discussed.

  3. Measurements of the Effect of Adiabat on Shell Decompression in Direct-Drive Implosions on OMEGA

    NASA Astrophysics Data System (ADS)

    Michel, D. T.; Hu, S. X.; Radha, P. B.; Davis, A. K.; Craxton, R. S.; Glebov, V. Yu.; Goncharov, V. N.; Igumenshchev, I. V.; Stoeckl, C.; Froula, D. H.

    2016-10-01

    Measurements of the effect of adiabat (α) on the shell thickness were performed in direct-drive implosions. The maximum in-flight shell thickness was obtained using a novel technique where the outer and inner surfaces of the shell were simultaneously measured using self-emission images of the imploding target. When reducing the shell's adiabat from α = 6 to α = 4.5 , the shell thickness was measured to decrease from 75 μm to 60 μm, but when decreasing the adiabat further (α = 1.8), the shell thickness was measured to increase to 75 μm. The measured shell thickness, shell trajectories, neutron bang time, and neutron yield were reproduced by two-dimensional simulations that include laser imprint, nonlocal thermal transport, cross-beam energy transfer, and first-principles equation-of-state models. These results show that the decompression of the shell measured for low-adiabat implosions was a result of laser imprint. Additional information on the evolution of the density profile was obtained using x-ray radiography. The backlighter was created with six of the 60 OMEGA laser beams, with the pointings and energies of other beams adjusted to maintain a uniform implosion. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

  4. Faceted Surface Grain Morphology of Rapidly Solidified Alumina: Characterization and Potential Applications

    SciTech Connect

    Harimkar, Sandip; Kenik, Edward A; Shim, Sanghoon; Dahotre, Narendra B

    2009-01-01

    This communication reports on the characterization of novel surface microstructure formed in rapidly solidified porous alumina ceramic. Advanced characterization techniques such as Orientation Imaging Microscopy (OIM) and Atomic Force Microscopy (AFM) are used to understand the crystallographic and morphological aspects of the resultant microstructure. Potential applications of laser surface modified alumina ceramics are presented.

  5. Representing potential energy surfaces by high-dimensional neural network potentials.

    PubMed

    Behler, J

    2014-05-07

    The development of interatomic potentials employing artificial neural networks has seen tremendous progress in recent years. While until recently the applicability of neural network potentials (NNPs) has been restricted to low-dimensional systems, this limitation has now been overcome and high-dimensional NNPs can be used in large-scale molecular dynamics simulations of thousands of atoms. NNPs are constructed by adjusting a set of parameters using data from electronic structure calculations, and in many cases energies and forces can be obtained with very high accuracy. Therefore, NNP-based simulation results are often very close to those gained by a direct application of first-principles methods. In this review, the basic methodology of high-dimensional NNPs will be presented with a special focus on the scope and the remaining limitations of this approach. The development of NNPs requires substantial computational effort as typically thousands of reference calculations are required. Still, if the problem to be studied involves very large systems or long simulation times this overhead is regained quickly. Further, the method is still limited to systems containing about three or four chemical elements due to the rapidly increasing complexity of the configuration space, although many atoms of each species can be present. Due to the ability of NNPs to describe even extremely complex atomic configurations with excellent accuracy irrespective of the nature of the atomic interactions, they represent a general and therefore widely applicable technique, e.g. for addressing problems in materials science, for investigating properties of interfaces, and for studying solvation processes.

  6. Streaming potential revisited: the influence of convection on the surface conductivity.

    PubMed

    Saini, Rakesh; Garg, Abhinandan; Barz, Dominik P J

    2014-09-16

    Electrokinetic phenomena play an important role in the electrical characterization of surfaces. In terms of planar or porous substrates, streaming potential and/or streaming current measurements can be used to determine the zeta potential of the substrates in contact with aqueous electrolytes. In this work, we perform electrical impedance spectroscopy measurements to infer the electrical resistance in a microchannel with the same conditions as for a streaming potential experiment. Novel correlations are derived to relate the streaming current and streaming potential to the Reynolds number of the channel flow. Our results not only quantify the influence of surface conductivity, and here especially the contribution of the stagnant layer, but also reveal that channel resistance and therefore zeta potential are influenced by the flow in the case of low ionic strengths. We conclude that convection can have a significant impact on the electrical double layer configuration which is reflected by changes in the surfaces conductivity.

  7. Hydrophobicity, surface tension, and zeta potential measurements of glass-reinforced hydroxyapatite composites.

    PubMed

    Lopes, M A; Monteiro, F J; Santos, J D; Serro, A P; Saramago, B

    1999-06-15

    Wettability and zeta potential studies were performed to characterize the hydrophobicity, surface tension, and surface charge of P2O5-glass-reinforced hydroxyapatite composites. Quantitative phase analysis was performed by the Rietveld method using GSAS software applied to X-ray diffractograms. Surface charge was assessed by zeta potential measurements. Protein adsorption studies were performed using vitronectin. Contact angles and surface tensions variation with time were determined by the sessile and pendent drop techniques, respectively, using ADSA-P software. The highest (-18.1 mV) and lowest (-28.7 mV) values of zeta potential were found for hydroxyapatite (HA) and beta-tricalcium phosphate (beta-TCP), respectively, with composite materials presenting values in between. All studied bioceramic materials showed similar solid surface tension. For HA and beta-TCP, solid surface tensions of 46.7 and 45.3 mJ/m2, respectively, were obtained, while composites presented intermediate surface tension values. The dispersive component of surface tension was the predominant one for all materials studied. Adhesion work values between the vitronectin solution and HA and beta-TCP were found to be 79.8 and 88.0 mJ/m2, respectively, while the 4.0 wt % glass composites showed slightly lower values than the 2.5 wt % ones. The presence of beta-TCP influenced surface charge, hydrophobicity, and protein adsorption of the glass-reinforced HA composites, and therefore indirectly affected cell-biomaterial interactions.

  8. Transporting and manipulating single electrons in surface-acoustic-wave minima

    NASA Astrophysics Data System (ADS)

    Ford, Christopher J. B.

    2017-03-01

    A surface acoustic wave (SAW) can produce a moving potential wave that can trap and drag electrons along with it. We review work on using a SAW to create moving quantum dots containing single electrons, with the aims of developing a current standard, emitting single photons, transferring single electrons between static quantum dots, and investigating non-adiabatic effects.

  9. Full-dimensional diabatic potential energy surfaces including dissociation: the ²E″ state of NO₃.

    PubMed

    Eisfeld, Wolfgang; Vieuxmaire, Olivier; Viel, Alexandra

    2014-06-14

    A scheme to produce accurate full-dimensional coupled diabatic potential energy surfaces including dissociative regions and suitable for dynamical calculations is proposed. The scheme is successfully applied to model the two-sheeted surface of the (2)E″ state of the NO3 radical. An accurate potential energy surface for the NO₃⁻ anion ground state is developed as well. Both surfaces are based on high-level ab initio calculations. The model consists of a diabatic potential matrix, which is expanded to higher order in terms of symmetry polynomials of symmetry coordinates. The choice of coordinates is key for the accuracy of the obtained potential energy surfaces and is discussed in detail. A second central aspect is the generation of reference data to fit the expansion coefficients of the model for which a stochastic approach is proposed. A third ingredient is a new and simple scheme to handle problematic regions of the potential energy surfaces, resulting from the massive undersampling by the reference data unavoidable for high-dimensional problems. The final analytical diabatic surfaces are used to compute the lowest vibrational levels of NO₃⁻ and the photo-electron detachment spectrum of NO₃⁻ leading to the neutral radical in the (2)E″ state by full dimensional multi-surface wave-packet propagation for NO3 performed using the Multi-Configuration Time Dependent Hartree method. The achieved agreement of the simulations with available experimental data demonstrates the power of the proposed scheme and the high quality of the obtained potential energy surfaces.

  10. A Modified Adiabatic Quantum Algorithm for Evaluation of Boolean Functions

    NASA Astrophysics Data System (ADS)

    Sun, Jie; Lu, Songfeng; Liu, Fang

    2015-09-01

    In this paper, we propose a modified construction of the quantum adiabatic algorithm for Boolean functions studied by M. Andrecut et al. [13, 14]. Our algorithm has the time complexity O(1) for the evaluation of Boolean functions, without additional computational cost of implementing the driving Hamiltonian, which is required by the adiabatic evolution described in [13, 14].

  11. 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.

  12. 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…

  13. 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)

  14. Distribution of the surface potential of epitaxial HgCdTe

    SciTech Connect

    Novikov, V. A. Grigoryev, D. V.; Bezrodnyy, D. A.; Dvoretsky, S. A.

    2014-09-08

    We studied the distribution of surface potential of the Hg{sub 1−x}Cd{sub x}Te epitaxial films grown by molecular beam epitaxy. The studies showed that the variation of the spatial distribution of surface potential in the region of the V-defect can be related to the variation of the material composition of epitaxial film. The V-defect is characterized by increased of Hg content with respect to the composition of the solid solution of Hg{sub 1−x}Cd{sub x}Te epitaxial film. In this paper, it was demonstrated that the unformed V-defects can be observed together with the macroscopic V-defects on the epitaxial film surface. These unformed V-defects can allow the creation of a complex surface potential distribution profile due to the redistribution of the solid solution composition.

  15. The PyPES library of high quality semi-global potential energy surfaces.

    PubMed

    Sibaev, Marat; Crittenden, Deborah L

    2015-11-05

    In this article, we present a Python-based library of high quality semi-global potential energy surfaces for 50 polyatomic molecules with up to six atoms. We anticipate that these surfaces will find widespread application in the testing of new potential energy surface construction algorithms and nuclear ro-vibrational structure theories. To this end, we provide the ability to generate the energy derivatives required for Taylor series expansions to sixth order about any point on the potential energy surface in a range of common coordinate systems, including curvilinear internal, Cartesian, and normal mode coordinates. The PyPES package, along with FORTRAN, C, MATLAB and Mathematica wrappers, is available at http://sourceforge.net/projects/pypes-lib.

  16. The Adiabatic Contraction of Dark Matter Halos in Numerical Simulations

    NASA Astrophysics Data System (ADS)

    Jesseit, R.; Burkert, A.; Naab, T.

    The flatness of rotation curves in the outer parts of galaxies led to the postulation of a dark component to compensate for the missing mass. The origin of this component is still unknown. Bahcall & Soneira first pointed out in 1985 that a unique ratio for disk to halo mass is needed to produce the flat and featureless rotation curves in agreement with observations. They called this the disk-halo conspiracy. To explain this conspiracy Blumenthal et al. proposed that an adiabtically forming baryonic disk can influence the density structure of its surrounding dark halo. They assumed that the time scale of the baryonic infall is very slow such and the change of mass inside the orbit of a dark matter particle is neglegible. They further assumed that the dark matter particles revolve on circular orbits and are dissipationless. In this case their radial action integral is an adiabatic invariant during the contraction. Blumenthal et al. could find the final density profile of the dark matter, if the final distribution of the baryonic matter is known, through an iterative algorithm. We tested the above assumptions using collisionless N-body simulations. We set up a dark matter halo with a Hernquist density profile and analytically added the potential of an exponential disk. Initially the disk had a very large scale length compared to the halo scale length. During the simulation we reduced the sclae length of the disk and followed the evolution of the dark component. We examined different contraction speeds as well as different combinations of disk mass and scale lenght. We find that the theoretical prediction for the adiabatic contraction is

  17. Adiabatic principles in atom-diatom collisional energy transfer

    SciTech Connect

    Hovingh, W.J.

    1993-01-01

    This work describes the application of numerical methods to the solution of the time dependent Schroedinger equation for non-reactive atom-diatom collisions in which only one of the degrees of freedom has been removed. The basic method involves expanding the wave function in a basis set in two of the diatomic coordinates in a body-fixed frame (with respect to the triatomic complex) and defining the coefficients in that expansion as functions on a grid in the collision coordinate. The wave function is then propagated in time using a split operator method. The bulk of this work is devoted to the application of this formalism to the study of internal rotational predissociation in NeHF, in which quasibound states of the triatom predissociate through the transfer of energy from rotation of the diatom into translational energy in the atom-diatom separation coordinate. The author analyzes the computed time dependent wave functions to calculate the lifetimes for several quasibound states; these are in agreement with time independent quantum calculations using the same potential. Moreover, the time dependent behavior of the wave functions themselves sheds light on the dynamics of the predissociation processes. Finally, the partial cross sections of the products in those processes is determined with multiple exit channels. These show strong selectivity in the orbital angular momentum of the outgoing fragments, which the author explains with an adiabatic channel interpretation of the wave function's dynamics. The author also suggests that the same formalism might profitably be used to investigate the quantum dynamics of [open quotes]quasiresonant vibration-rotation transfer[close quotes], in which remarkably strong propensity rules in certain inelastic atom-diatom collision arise from classical adiabatic invariance theory.

  18. Semiclassical Monte-Carlo approach for modelling non-adiabatic dynamics in extended molecules

    PubMed Central

    Gorshkov, Vyacheslav N.; Tretiak, Sergei; Mozyrsky, Dmitry

    2013-01-01

    Modelling of non-adiabatic dynamics in extended molecular systems and solids is a next frontier of atomistic electronic structure theory. The underlying numerical algorithms should operate only with a few quantities (that can be efficiently obtained from quantum chemistry), provide a controlled approximation (which can be systematically improved) and capture important phenomena such as branching (multiple products), detailed balance and evolution of electronic coherences. Here we propose a new algorithm based on Monte-Carlo sampling of classical trajectories, which satisfies the above requirements and provides a general framework for existing surface hopping methods for non-adiabatic dynamics simulations. In particular, our algorithm can be viewed as a post-processing technique for analysing numerical results obtained from the conventional surface hopping approaches. Presented numerical tests for several model problems demonstrate efficiency and accuracy of the new method. PMID:23864100

  19. On the Electronic Nature of the Surface Potential at the Vapor-Liquid Interface of Water

    SciTech Connect

    Kathmann, S M; Kuo, I; Mundy, C J

    2008-02-05

    The surface potential at the vapor-liquid interface of water is relevant to many areas of chemical physics. Measurement of the surface potential has been experimentally attempted many times, yet there has been little agreement as to its magnitude and sign (-1.1 to +0.5 mV). We present the first computation of the surface potential of water using ab initio molecular dynamics. We find that the surface potential {chi} = -18 mV with a maximum interfacial electric field = 8.9 x 10{sup 7} V/m. A comparison is made between our quantum mechanical results and those from previous molecular simulations. We find that explicit treatment of the electronic density makes a dramatic contribution to the electric properties of the vapor-liquid interface of water. The E-field can alter interfacial reactivity and transport while the surface potential can be used to determine the 'chemical' contribution to the real and electrochemical potentials for ionic transport through the vapor-liquid interface.

  20. Biofilm formation by Listeria monocytogenes on stainless steel surface and biotransfer potential

    PubMed Central

    de Oliveira, Maíra Maciel Mattos; Brugnera, Danilo Florisvaldo; Alves, Eduardo; Piccoli, Roberta Hilsdorf

    2010-01-01

    An experimental model was proposed to study biofilm formation by Listeria monocytogenes ATCC 19117 on AISI 304 (#4) stainless steel surface and biotransfer potential during this process. In this model, biofilm formation was conducted on the surface of stainless steel coupons, set on a stainless steel base with 4 divisions, each one supporting 21 coupons. Trypic Soy Broth was used as bacterial growth substrate, with incubation at 37 °C and stirring of 50 rpm. The number of adhered cells was determined after 3, 48, 96, 144, 192 and 240 hours of biofilm formation and biotransfer potential from 96 hours. Stainless steel coupons were submitted to Scanning Electron Microscopy (SEM) after 3, 144 and 240 hours. Based on the number of adhered cells and SEM, it was observed that L. monocytogenes adhered rapidly to the stainless steel surface, with mature biofilm being formed after 240 hours. The biotransfer potential of bacterium to substrate occurred at all the stages analyzed. The rapid capacity of adhesion to surface, combined with biotransfer potential throughout the biofilm formation stages, make L. monocytogenes a potential risk to the food industry. Both the experimental model developed and the methodology used were efficient in the study of biofilm formation by L. monocytogenes on stainless steel surface and biotransfer potential. PMID:24031469

  1. Accelerating the search for global minima on potential energy surfaces using machine learning

    NASA Astrophysics Data System (ADS)

    Carr, S. F.; Garnett, R.; Lo, C. S.

    2016-10-01

    Controlling molecule-surface interactions is key for chemical applications ranging from catalysis to gas sensing. We present a framework for accelerating the search for the global minimum on potential surfaces, corresponding to stable adsorbate-surface structures. We present a technique using Bayesian inference that enables us to predict converged density functional theory potential energies with fewer self-consistent field iterations. We then discuss how this technique fits in with the Bayesian Active Site Calculator, which applies Bayesian optimization to the problem. We demonstrate the performance of our framework using a hematite (Fe2O3) surface and present the adsorption sites found by our global optimization method for various simple hydrocarbons on the rutile TiO2 (110) surface.

  2. 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.

  3. 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.

  4. 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.

  5. An adiabatic demagnetization refrigerator for SIRTF

    NASA Astrophysics Data System (ADS)

    Timbie, P. T.; Bernstein, G. M.; Richards, P. L.

    1989-02-01

    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 Astrophysics Data System (ADS)

    Serlemitsos, A. T.; Kunes, E.; Sansebastian, M.

    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. On stress collapse in adiabatic shear bands

    NASA Astrophysics Data System (ADS)

    Wright, T. W.; Walter, J. W.

    T HE DYNAMICS of adiabatic shear band formation is considered making use of a simplified thermo/visco/plastic flow law. A new numerical solution is used to follow the growth of a perturbation from initiation, through early growth and severe localization, to a slowly varying terminal configuration. Asymptotic analyses predict the early and late stage patterns, but the timing and structure of the abrupt transition to severe localization can only be studied numerically, to date. A characteristic feature of the process is that temperature and plastic strain rate begin to localize immediately, but only slowly, whereas the stress first evolves almost as if there were no perturbation, but then collapses rapidly when severe localization occurs.

  8. Index Theory and Adiabatic Limit in QFT

    NASA Astrophysics Data System (ADS)

    Wawrzycki, Jarosław

    2013-08-01

    The paper has the form of a proposal concerned with the relationship between the three mathematically rigorous approaches to quantum field theory: (1) local algebraic formulation of Haag, (2) Wightman formulation and (3) the perturbative formulation based on the microlocal renormalization method. In this project we investigate the relationship between (1) and (3) and utilize the known relationships between (1) and (2). The main goal of the proposal lies in obtaining obstructions for the existence of the adiabatic limit ( confinement problem in the phenomenological standard model approach). We extend the method of deformation of Dütsch and Fredenhagen (in the Bordeman-Waldmann sense) and apply Fedosov construction of the formal index—an analog of the index for deformed symplectic manifolds, generalizing the Atiyah-Singer index. We present some first steps in realization of the proposal.

  9. 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.

  10. 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.

  11. 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.

  12. 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.

  13. An Integrated Development Environment for Adiabatic Quantum Programming

    SciTech Connect

    Humble, Travis S; McCaskey, Alex; Bennink, Ryan S; Billings, Jay Jay; D'Azevedo, Eduardo; Sullivan, Blair D; Klymko, Christine F; Seddiqi, Hadayat

    2014-01-01

    Adiabatic quantum computing is a promising route to the computational power afforded by quantum information processing. The recent availability of adiabatic hardware raises the question of how well quantum programs perform. Benchmarking behavior is challenging since the multiple steps to synthesize an adiabatic quantum program are highly tunable. We present an adiabatic quantum programming environment called JADE that provides control over all the steps taken during program development. JADE captures the workflow needed to rigorously benchmark performance while also allowing a variety of problem types, programming techniques, and processor configurations. We have also integrated JADE with a quantum simulation engine that enables program profiling using numerical calculation. The computational engine supports plug-ins for simulation methodologies tailored to various metrics and computing resources. We present the design, integration, and deployment of JADE and discuss its use for benchmarking adiabatic quantum programs.

  14. Adiabatic theory, Liapunov exponents, and rotation number for quadratic Hamiltonians

    NASA Astrophysics Data System (ADS)

    Delyon, François; Foulon, Patrick

    1987-11-01

    We consider the adiabatic problem for general time-dependent quadratic Hamiltonians and develop a method quite different from WKB. In particular, we apply our results to the Schrödinger equation in a strip. We show that there exists a first regular step (avoiding resonance problems) providing one adiabatic invariant, bounds on the Liapunov exponents, and estimates on the rotation number at any order of the perturbation theory. The further step is shown to be equivalent to a quantum adiabatic problem, which, by the usual adiabatic techniques, provides the other possible adiabatic invariants. In the special case of the Schrödinger equation our method is simpler and more powerful than the WKB techniques.

  15. Adiabatic vs. non-adiabatic determination of specific absorption rate of ferrofluids

    NASA Astrophysics Data System (ADS)

    Natividad, Eva; Castro, Miguel; Mediano, Arturo

    2009-05-01

    The measurement of temperature variations in adiabatic conditions allows the determination of the specific absorption rate of magnetic nanoparticles and ferrofluids from the correct incremental expression, SAR=(1/ m MNP) C(Δ T/Δ t). However, when measurements take place in non-adiabatic conditions, one must approximate this expression by SAR≈ Cβ/ m MNP, where β is the initial slope of the temperature vs. time curve during alternating field application. The errors arising from the use of this approximation were estimated through several experiments with different isolating conditions, temperature sensors and sample-sensor contacts. It is concluded that small to appreciable errors can appear, which are difficult to infer or control.

  16. Communication: On the competition between adiabatic and nonadiabatic dynamics in vibrationally mediated ammonia photodissociation in its A band

    SciTech Connect

    Xie, Changjian; Zhu, Xiaolei; Yarkony, David R. E-mail: yarkony@jhu.edu E-mail: hguo@unm.edu; Ma, Jianyi E-mail: yarkony@jhu.edu E-mail: hguo@unm.edu; Xie, Daiqian E-mail: yarkony@jhu.edu E-mail: hguo@unm.edu; Guo, Hua E-mail: yarkony@jhu.edu E-mail: hguo@unm.edu

    2015-03-07

    Non-adiabatic processes play an important role in photochemistry, but the mechanism for conversion of electronic energy to chemical energy is still poorly understood. To explore the possibility of vibrational control of non-adiabatic dynamics in a prototypical photoreaction, namely, the A-band photodissociation of NH{sub 3}(X{sup ~1}A{sub 1}), full-dimensional state-to-state quantum dynamics of symmetric or antisymmetric stretch excited NH{sub 3}(X{sup ~1}A{sub 1}) is investigated on recently developed coupled diabatic potential energy surfaces. The experimentally observed H atom kinetic energy distributions are reproduced. However, contrary to previous inferences, the NH{sub 2}(A{sup ~2}A{sub 1})/NH{sub 2}(X{sup ~2}B{sub 1}) branching ratio is found to be small regardless of the initial preparation of NH{sub 3}(X{sup ~1}A{sub 1}), while the internal state distribution of the preeminent fragment, NH{sub 2}(X{sup ~2}B{sub 1}), is found to depend strongly on the initial vibrational excitation of NH{sub 3}(X{sup ~1}A{sub 1}). The slow H atoms in photodissociation mediated by the antisymmetric stretch fundamental state are due to energy sequestered in the internally excited NH{sub 2}(X{sup ~2}B{sub 1}) fragment, rather than in NH{sub 2}(A{sup ~2}A{sub 1}) as previously proposed. The high internal excitation of the NH{sub 2}(X{sup ~2}B{sub 1}) fragment is attributed to the torques exerted on the molecule as it passes through the conical intersection seam to the ground electronic state of NH{sub 3}. Thus in this system, contrary to previous assertions, the control of electronic state branching by selective excitation of ground state vibrational modes is concluded to be ineffective. The juxtaposition of precise quantum mechanical results with complementary results based on quasi-classical surface hopping trajectories provides significant insights into the non-adiabatic process.

  17. The sea surface currents as a potential factor in the estimation and monitoring of wave energy potential

    NASA Astrophysics Data System (ADS)

    Zodiatis, George; Galanis, George; Nikolaidis, Andreas; Stylianoy, Stavros; Liakatas, Aristotelis

    2015-04-01

    The use of wave energy as an alternative renewable is receiving attention the last years under the shadow of the economic crisis in Europe and in the light of the promising corresponding potential especially for countries with extended coastline. Monitoring and studying the corresponding resources is further supported by a number of critical advantages of wave energy compared to other renewable forms, like the reduced variability and the easier adaptation to the general grid, especially when is jointly approached with wind power. Within the framework, a number of countries worldwide have launched research and development projects and a significant number of corresponding studies have been presented the last decades. However, in most of them the impact of wave-sea surface currents interaction on the wave energy potential has not been taken into account neglecting in this way a factor of potential importance. The present work aims at filling this gap for a sea area with increased scientific and economic interest, the Eastern Mediterranean Sea. Based on a combination of high resolution numerical modeling approach with advanced statistical tools, a detailed analysis is proposed for the quantification of the impact of sea surface currents, which produced from downscaling the MyOcean-FO regional data, to wave energy potential. The results although spatially sensitive, as expected, prove beyond any doubt that the wave- sea surface currents interaction should be taken into account for similar resource analysis and site selection approaches since the percentage of impact to the available wave power may reach or even exceed 20% at selected areas.

  18. Surface-potential-based compact modeling of dynamically depleted SOI MOSFETs

    NASA Astrophysics Data System (ADS)

    Wu, Weimin; Yao, Wei; Gildenblat, Gennady

    2010-05-01

    We present a complete surface-potential-based compact model of dynamically depleted (DD) SOI MOSFETs. The surface potential equation of DD-SOI MOSFETs was reconditioned to avoid the unphysical behaviors near the flat-band voltage. In order to capture the dynamic depletion effect, the coupling equation for the front and back surface potentials was reformulated to include the back gate effect, which is not available in other surface-potential-based DD-SOI compact models. The new formulation of surface potential and coupling equations was verified by comparing with numerical computations combining the Pao-Sah double integral based formulation and the exact coupling equation. To obtain explicit expressions for the terminal charges and drain current, a new symmetric linearization method has been proposed. The complete model, PSP-SOI DD is implemented in the context of the PSP and PSP-SOI PD models and includes all the secondary effects, floating body simulation capability, etc. The new model has been extensively verified with 2D TCAD simulation results and accurately captures the manifestation of the dynamic depletion effect observed in the device characteristics.

  19. Interatomic potentials between noble gas and Ag atoms from axial surface channeling

    NASA Astrophysics Data System (ADS)

    Schüller, A.; Winter, H.

    2007-08-01

    He, Ne, and Ar atoms with energies from 3 keV to 60 keV are scattered from a Ag(1 1 1) surface under axial surface channeling conditions. From peaked structures in the angular distributions owing to "rainbow-scattering" we derive effective scattering potentials. We compare the observed rainbow angles with results from computer simulations using different types of established interatomic potentials and focus on a detailed discussion for potential energies larger than 10 eV. It turns out that an approximation proposed by O'Connor and Biersack using a Moliere potential with an adjustment of the screening length [D.J. O'Connor, J.P. Biersack, Nucl. Instr. and Meth. B 15 (1986) 14) is in good agreement with the experimental data. In our simulations we investigate the sensitivity of the rainbow angles on a variation of the interatomic potential.

  20. Vibrational quenching of excitonic splittings in H-bonded molecular dimers: adiabatic description and effective mode approximation.

    PubMed

    Kopec, Sabine; Ottiger, Philipp; Leutwyler, Samuel; Köppel, Horst

    2012-11-14

    The quenching of the excitonic splitting in hydrogen-bonded molecular dimers has been explained recently in terms of exciton coupling theory, involving Förster's degenerate perturbation theoretical approach [P. Ottiger, S. Leutwyler, and H. Köppel, J. Chem. Phys. 136, 174308 (2012)]. Here we provide an alternative explanation based on the properties of the adiabatic potential energy surfaces. In the proper limit, the lower of these surfaces exhibits a double-minimum shape, with an asymmetric distortion that destroys the geometric equivalence of the excitonically coupled monomers. An effective mode is introduced that exactly reproduces the energy gain and amount of distortion that occurs in a multi-dimensional normal coordinate space. This allows to describe the quenched exciton splitting as the energy difference of the two (S(1) and S(2)) vibronic band origins in a one-dimensional (rather than multi-dimensional) vibronic calculation. The agreement with the earlier result (based on Förster theory) is excellent for all five relevant cases studied. A simple rationale for the quenched exciton splitting as nonadiabatic tunneling splitting on the lower double-minimum potential energy surface is given.

  1. The potential of electron beam radiation for simultaneous surface modification and bioresorption control of PLLA.

    PubMed

    Cairns, Marie-Louise; Dickson, Glenn R; Orr, John F; Farrar, David; Hardacre, Christopher; Sa, Jacinto; Lemoine, Patrick; Mughal, Muhammad Zeeshan; Buchanan, Fraser J

    2012-09-01

    Bioresorbable polymers have been widely investigated as materials exhibiting significant potential for successful application in the fields of tissue engineering and drug delivery. Further to the ability to control degradation, surface engineering of polymers has been highlighted as a key method central to their development. Previous work has demonstrated the ability of electron beam (e-beam) technology to control the degradation profiles and bioresorption of a number of commercially relevant bioresorbable polymers (poly-l-lactic acid (PLLA), L-lactide/DL-lactide co-polymer (PLDL) and poly(lactic-co-glycolic acid (PLGA)). This work investigates the further potential of e-beam technology to impart added biofunctionality through the manipulation of polymer (PLLA) surface properties. PLLA samples were subjected to e-beam treatments in air, with varying beam energies and doses. Surface characterization was then performed using contact angle analysis, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and atomic force microscopy. Results demonstrated a significant increase in surface wettability post e-beam treatment. In correlation with this, XPS data showed the introduction of oxygen-containing functional groups to the surface of PLLA. Raman spectroscopy indicated chain scission in the near surface region of PLLA (as predicted). However, e-beam effects on surface properties were not shown to be dependent on beam energy or dose. E-beam irradiation did not seem to affect the surface roughness of PLLA as a direct consequence of the treatment.

  2. Zeta potentials of polydimethylsiloxane surfaces modified by polybrene of different concentrations.

    PubMed

    Song, Yongxin; Li, Jun; Li, Dongqing

    2016-02-01

    Zeta potential is an important parameter for characterizing the electrokinetic properties of a solid-liquid interface. In this paper, zeta potentials of polydimethylsiloxane surfaces modified by polybrene (PB) solutions of different concentrations in Phosphate buffer solution and pure water were reported. The zeta potentials were measured by an induction current method. The measurements were validated both by a calibration curve based on the data reported in the published papers and by comparing the zeta potential determined by using the Smoluchowski equation and the measured velocity of the electrokinetic motion of particles in a microchannel.

  3. Temperature gradients due to adiabatic plasma expansion in a magnetic nozzle

    NASA Astrophysics Data System (ADS)

    Sheehan, J. P.; Longmier, B. W.; Bering, E. A.; Olsen, C. S.; Squire, J. P.; Ballenger, M. G.; Carter, M. D.; Cassady, L. D.; Díaz, F. R. Chang; Glover, T. W.; Ilin, A. V.

    2014-08-01

    A mechanism for ambipolar ion acceleration in a magnetic nozzle is proposed. The plasma is adiabatic (i.e., does not exchange energy with its surroundings) in the diverging section of a magnetic nozzle so any energy lost by the electrons must be transferred to the ions via the electric field. Fluid theory indicates that the change in plasma potential is proportional to the change in average electron energy. These predictions were compared to measurements in the VX-200 experiment which has conditions conducive to ambipolar ion acceleration. A planar Langmuir probe was used to measure the plasma potential, electron density, and electron temperature for a range of mass flow rates and power levels. Axial profiles of those parameters were also measured, showing consistency with the adiabatic ambipolar fluid theory.

  4. High volume hydraulic fracturing operations: potential impacts on surface water and human health.

    PubMed

    Mrdjen, Igor; Lee, Jiyoung

    2016-08-01

    High volume, hydraulic fracturing (HVHF) processes, used to extract natural gas and oil from underground shale deposits, pose many potential hazards to the environment and human health. HVHF can negatively affect the environment by contaminating soil, water, and air matrices with potential pollutants. Due to the relatively novel nature of the process, hazards to surface waters and human health are not well known. The purpose of this article is to link the impacts of HVHF operations on surface water integrity, with human health consequences. Surface water contamination risks include: increased structural failure rates of unconventional wells, issues with wastewater treatment, and accidental discharge of contaminated fluids. Human health risks associated with exposure to surface water contaminated with HVHF chemicals include increased cancer risk and turbidity of water, leading to increased pathogen survival time. Future research should focus on modeling contamination spread throughout the environment, and minimizing occupational exposure to harmful chemicals.

  5. Modeling Solar-Wind Heavy-Ions' Potential Sputtering of Lunar KREEP Surface

    NASA Technical Reports Server (NTRS)

    Barghouty, A. F.; Meyer, F. W.; Harris, R. P.; Adams, J. H., Jr.

    2012-01-01

    Recent laboratory data suggest that potential sputtering may be an important weathering mechanism that can affect the composition of both the lunar surface and its tenuous exosphere; its role and implications, however, remain unclear. Using a relatively simple kinetic model, we will demonstrate that solar-wind heavy ions induced sputtering of KREEP surfaces is critical in establishing the timescale of the overall solar-wind sputtering process of the lunar surface. We will also also show that potential sputtering leads to a more pronounced and significant differentiation between depleted and enriched surface elements. We briefly discuss the impacts of enhanced sputtering on the composition of the regolith and the exosphere, as well as of solar-wind sputtering as a source of hydrogen and water on the moon.

  6. Quantum Dynamics of Vinylidene Photodetachment on an Accurate Global Acetylene-Vinylidene Potential Energy Surface.

    PubMed

    Guo, Lifen; Han, Huixian; Ma, Jianyi; Guo, Hua

    2015-08-06

    Vinylidene is a high-energy isomer of acetylene, and the rearrangement of bonds in the two species serves as a prototype for isomerization reactions. Here, a full-dimensional quantum mechanical study of the vinylidene vibration is carried out on a recently developed global acetylene-vinylidene potential energy surface by simulating the photodetachment dynamics of the vinylidene anion. Several low-lying vibrational levels of the anion were first determined on a new ab initio based potential energy surface, and their photoelectron spectra were obtained within the Condon approximation. The vibrational features of the vinylidene isomer are found to agree well with the experiment in both positions and intensities, validating the global acetylene-vinylidene potential energy surface.

  7. Permutation invariant potential energy surfaces for polyatomic reactions using atomistic neural networks

    NASA Astrophysics Data System (ADS)

    Kolb, Brian; Zhao, Bin; Li, Jun; Jiang, Bin; Guo, Hua

    2016-06-01

    The applicability and accuracy of the Behler-Parrinello atomistic neural network method for fitting reactive potential energy surfaces is critically examined in three systems, H + H2 → H2 + H, H + H2O → H2 + OH, and H + CH4 → H2 + CH3. A pragmatic Monte Carlo method is proposed to make efficient choice of the atom-centered mapping functions. The accuracy of the potential energy surfaces is not only tested by fitting errors but also validated by direct comparison in dynamically important regions and by quantum scattering calculations. Our results suggest this method is both accurate and efficient in representing multidimensional potential energy surfaces even when dissociation continua are involved.

  8. Scaling evaluation of the effect of surface characteristics on potential for deep convection over uniform terrain

    NASA Technical Reports Server (NTRS)

    Segal, M.; Arritt, R. W.; Clark, C.; Rabin, R.; Brown, J.

    1995-01-01

    The effect of surface characteristics on the daytime change in the potential for development of deep convection resulting from surface flux of heat and moisture is evaluated by conceptual, scaling, and numerical modeling approaches. It is shown that deep convection depends significantly on the Bowen ratio; for smaller Bowen ratio, the thermodynamic potential for deep convection increases. The elevation and the intensity of the capping stable layer have an opposing impact on deep convection: increasing moisture accumulation through evapotranspiration was supportive but was counteracted by the enhancement of dry entrainment. Based on an approximnate treatment of the effect of cloudiness on solar irradiance, it was found that development of fair weather cumulus has a secondary effect on deep convection potential. Observational and operational aspects of the influence of surface conditions on evapotranspiration and development of deep convection are presented.

  9. New potential energy surface for the HCS(+)-He system and inelastic rate coefficients.

    PubMed

    Dubernet, Marie-Lise; Quintas-Sánchez, Ernesto; Tuckey, Philip

    2015-07-28

    A new high quality potential energy surface is calculated at a coupled-cluster single double triple level with an aug-cc-pV5Z basis set for the HCS(+)-He system. This potential energy surface is used in low energy quantum scattering calculations to provide a set of (de)-excitation cross sections and rate coefficients among the first 20 rotational levels of HCS(+) by He in the range of temperature from 5 K to 100 K. The paper discusses the impact of the new ab initio potential energy surface on the cross sections at low energy and provides a comparison with the HCO(+)-He system. The HCS(+)-He rate coefficients for the strongest transitions differ by factors of up to 2.5 from previous rate coefficients; thus, analysis of astrophysical spectra should be reconsidered with the new rate coefficients.

  10. Polar/apolar compounds induce leukemia cell differentiation by modulating cell-surface potential.

    PubMed Central

    Arcangeli, A; Carlà, M; Del Bene, M R; Becchetti, A; Wanke, E; Olivotto, M

    1993-01-01

    The mechanism of action of polar/apolar inducers of cell differentiation, such as dimethyl sulfoxide and hexamethylene-bisacetamide, is still obscure. In this paper evidence is provided that their effects on murine erythroleukemia cells are modulated by various extracellular cations as a precise function of the cation effects on membrane surface potential. The interfacial effects of the inducers were directly measured on the charged electrode, showing that both dimethyl sulfoxide and hexamethylene-bisacetamide, at the effective concentrations for cell differentiation and within the physiological range of charge density, adsorb at the charged surface and produce a potential shift. A linear correlation was found between this shift and the inducer effects on cell differentiation. Besides offering a different interpretation of the mechanism of action of the inducers, these findings indicate that surface potential has a signaling function. They may also be relevant to cancer treatments based on tumor-cell commitment to terminal differentiation. Images Fig. 1 PMID:8516337

  11. Surface and subsurface geologic risk factors to ground water affecting brownfield redevelopment potential.

    PubMed

    Kaufman, Martin M; Murray, Kent S; Rogers, Daniel T

    2003-01-01

    A model is created for assessing the redevelopment potential of brownfields. The model is derived from a space and time conceptual framework that identifies and measures the surface and subsurface risk factors present at brownfield sites. The model then combines these factors with a contamination extent multiplier at each site to create an index of redevelopment potential. Results from the application of the model within an urbanized watershed demonstrate clear differences between the redevelopment potential present within five different near-surface geologic units, with those units containing clay being less vulnerable to subsurface contamination. With and without the extent multiplier, the total risk present at the brownfield sites within all the geologic units is also strongly correlated to the actual costs of remediation. Thus, computing the total surface and subsurface risk within a watershed can help guide the remediation efforts at broad geographic scales, and prioritize the locations for redevelopment.

  12. Nonequilibrium adiabatic molecular dynamics simulations of methane clathrate hydrate decomposition

    NASA Astrophysics Data System (ADS)

    Alavi, Saman; Ripmeester, J. A.

    2010-04-01

    Nonequilibrium, constant energy, constant volume (NVE) molecular dynamics simulations are used to study the decomposition of methane clathrate hydrate in contact with water. Under adiabatic conditions, the rate of methane clathrate decomposition is affected by heat and mass transfer arising from the breakup of the clathrate hydrate framework and release of the methane gas at the solid-liquid interface and diffusion of methane through water. We observe that temperature gradients are established between the clathrate and solution phases as a result of the endothermic clathrate decomposition process and this factor must be considered when modeling the decomposition process. Additionally we observe that clathrate decomposition does not occur gradually with breakup of individual cages, but rather in a concerted fashion with rows of structure I cages parallel to the interface decomposing simultaneously. Due to the concerted breakup of layers of the hydrate, large amounts of methane gas are released near the surface which can form bubbles that will greatly affect the rate of mass transfer near the surface of the clathrate phase. The effects of these phenomena on the rate of methane hydrate decomposition are determined and implications on hydrate dissociation in natural methane hydrate reservoirs are discussed.

  13. Conservation of the pure adiabatic state in Ehrenfest dynamics of the photoisomerization of molecules

    PubMed Central

    Miyamoto, Yoshiyuki; Tateyama, Yoshitaka; Oyama, Norihisa; Ohno, Takahisa

    2015-01-01

    We examined real-time-propagation time-dependent density functional theory (rtp-TDDFT) coupled with molecular dynamics (MD), which uses single-particle representation of time-evolving wavefunctions allowing exchange of orbital characteristics between occupied and empty states making the effective Kohn-Sham Hamiltonian dependent on the potential energy surfaces (PESs). This scheme is expected to lead to mean-field average of adiabatic potential energy surfaces (PESs), and is one of Ehrenfest (mean-field) approaches. However, we demonstrate that the mean-field average can be absent in simulating photoisomerization of azobenzene and ethylene molecules. A transition from the S2 to the S1 excited state without the mean- field average was observed after examining several rtp-TDDFT-MD trajectories of a photoexcited azobenzene molecule. The subsequent trans-cis isomerization was observed in our simulation, which is consistent with experimental observation and supported by previous calculations. The absence of the mean-field average of PESs was also observed for the transition between the S1 and S0 states, indicating that the MD simulation was on a single PES. Conversely, we found no transition to the ground state (S0 state) when we performed a MD simulation of an S1 excited ethylene molecule owing to the constraint on the occupation number of each molecular orbital. Thus, we conclude that, at least for azobenzene and ethylene molecules, the rtp-TDDFT-MD is an on-the-fly simulation that can automatically see the transition among the PESs of excited states without the mean-field average unless the simulation reaches the PES of the S0 state. PMID:26658633

  14. Effects of PV Module Soiling on Glass Surface Resistance and Potential-Induced Degradation

    SciTech Connect

    Hacke, Peter; Button, Patrick; Hendrickson, Alex; Spataru, Sergiu; Glick, Stephen

    2015-06-14

    The goals of the project were: Determine applicability of transmission line method (TLM) to evaluate sheet resistance of soils on module glass;
    Evaluate various soils on glass for changes in surface resistance and their ability to promote potential-induced degradation with humidity (PID);
    Evaluate PID characteristics, rate, and leakage current increases on full-size mc-Si modules associated with a conductive soil on the surface.

  15. Ab initio potential energy surface for the highly nonlinear dynamics of the KCN molecule

    SciTech Connect

    Párraga, H.; Arranz, F. J. Benito, R. M.; Borondo, F.

    2013-11-21

    An accurate ab initio quantum chemistry study at level of quadratic configuration interaction method of the electronic ground state of the KCN molecule is presented. A fitting of the results to an analytical series expansion was performed to obtain a global potential energy surface suitable for the study of the associated vibrational dynamics. Additionally, classical Poincaré surfaces of section for different energies and quantum eigenstates were calculated, showing the highly nonlinear behavior of this system.

  16. Plasma Membrane Surface Potential: Dual Effects upon Ion Uptake and Toxicity1

    PubMed Central

    Wang, Peng; Kinraide, Thomas B.; Zhou, Dongmei; Kopittke, Peter M.; Peijnenburg, Willie J.G.M.

    2011-01-01

    Electrical properties of plasma membranes (PMs), partially controlled by the ionic composition of the exposure medium, play significant roles in the distribution of ions at the exterior surface of PMs and in the transport of ions across PMs. The effects of coexisting cations (commonly Al3+, Ca2+, Mg2+, H+, and Na+) on the uptake and toxicity of these and other ions (such as Cu2+, Zn2+, Ni2+, Cd2+, and H2AsO4−) to plants were studied in terms of the electrical properties of PMs. Increased concentrations of cations or decreased pH in rooting media, whether in solution culture or in soils, reduced the negativity of the electrical potential at the PM exterior surface (ψ0o). This reduction decreased the activities of metal cations at the PM surface and increased the activities of anions such as H2AsO4−. Furthermore, the reduced ψ0o negativity increased the surface-to-surface transmembrane potential difference, thus increasing the electrical driving force for cation uptake and decreasing the driving force for anion uptake across PMs. Analysis of measured uptake and toxicity of ions using electrostatic models provides evidence that uptake and toxicity are functions of the dual effects of ψ0o (i.e. altered PM surface ion activity and surface-to-surface transmembrane potential difference gradient). This study provides novel insights into the mechanisms of plant-ion interactions and extends current theory to evaluate ion bioavailability and toxicity, indicating its potential utility in risk assessment of metal(loid)s in natural waters and soils. PMID:21119046

  17. On the General Class of Models of Adiabatic Evolution

    NASA Astrophysics Data System (ADS)

    Sun, Jie; Lu, Songfeng; Liu, Fang

    2016-10-01

    The general class of models of adiabatic evolution was proposed to speed up the usual adiabatic computation in the case of quantum search problem. It was shown [8] that, by temporarily increasing the ground state energy of a time-dependent Hamiltonian to a suitable quantity, the quantum computation can perform the calculation in time complexity O(1). But it is also known that if the overlap between the initial and final states of the system is zero, then the computation based on the generalized models of adiabatic evolution can break down completely. In this paper, we find another severe limitation for this class of adiabatic evolution-based algorithms, which should be taken into account in applications. That is, it is still possible that this kind of evolution designed to deal with the quantum search problem fails completely if the interpolating paths in the system Hamiltonian are chosen inappropriately, while the usual adiabatic evolutions can do the same job relatively effectively. This implies that it is not always recommendable to use nonlinear paths in adiabatic computation. On the contrary, the usual simple adiabatic evolution may be sufficient for effective use.

  18. Effects of EOS adiabat on hot spot dynamics

    NASA Astrophysics Data System (ADS)

    Cheng, Baolian; Kwan, Thomas; Wang, Yi-Ming; Batha, Steven

    2013-10-01

    Equation of state (EOS) and adiabat of the pusher play significant roles in the dynamics and formation of the hot spot of an ignition capsule. For given imploding energy, they uniquely determine the partition of internal energy, mass, and volume between the pusher and the hot spot. In this work, we apply the new scaling laws recently derived by Cheng et al. to the National Ignition Campaign (NIC) ignition capsules and study the impacts of EOS and adiabat of the pusher on the hot spot dynamics by using the EOS adiabat index as an adjustable model parameter. We compare our analysis with the NIC data, specifically, for shots N120321 and N120205, and with the numerical simulations of these shots. The predictions from our theoretical model are in good agreements with the NIC data when a hot adiabat was used for the pusher, and with code simulations when a cold adiabat was used for the pusher. Our analysis indicates that the actual adiabat of the pusher in NIC experiments may well be higher than the adiabat assumed in the simulations. This analysis provides a physical and systematic explanation to the ongoing disagreements between the NIC experimental results and the multi-dimensional numerical simulations. This work was performed under the auspices of the U.S. Department of Energy by the Los Alamos National Laboratory under contract number W-7405-ENG-36.

  19. Non-adiabatic perturbations in Ricci dark energy model

    SciTech Connect

    Karwan, Khamphee; Thitapura, Thiti E-mail: nanodsci2523@hotmail.com

    2012-01-01

    We show that the non-adiabatic perturbations between Ricci dark energy and matter can grow both on superhorizon and subhorizon scales, and these non-adiabatic perturbations on subhorizon scales can lead to instability in this dark energy model. The rapidly growing non-adiabatic modes on subhorizon scales always occur when the equation of state parameter of dark energy starts to drop towards -1 near the end of matter era, except that the parameter α of Ricci dark energy equals to 1/2. In the case where α = 1/2, the rapidly growing non-adiabatic modes disappear when the perturbations in dark energy and matter are adiabatic initially. However, an adiabaticity between dark energy and matter perturbations at early time implies a non-adiabaticity between matter and radiation, this can influence the ordinary Sachs-Wolfe (OSW) effect. Since the amount of Ricci dark energy is not small during matter domination, the integrated Sachs-Wolfe (ISW) effect is greatly modified by density perturbations of dark energy, leading to a wrong shape of CMB power spectrum. The instability in Ricci dark energy is difficult to be alleviated if the effects of coupling between baryon and photon on dark energy perturbations are included.

  20. Charging of silver bromide aqueous interface: evaluation of interfacial equilibrium constants from surface potential data.

    PubMed

    Preočanin, Tajana; Supljika, Filip; Kallay, Nikola

    2010-06-01

    A single crystal silver bromide electrode (SCr-AgBr) was used to measure the inner surface potential (Ψ(0)) at the silver bromide aqueous electrolyte interface as a function of the activities of Br(-) and Ag(+). Absolute values of the surface potential were calculated from electrode potentials of SCr-AgBr using the value of point of zero charge (pBr(pzc)=6.9 [H.A. Hoyen, R.M. Cole, J. Colloid Interface Sci. 41 (1972) 93.]) as the value of point of zero potential. Measurements were performed in potassium nitrate aqueous solutions. The Ψ(0)(pBr) function was linear and slightly dependent on the ionic strength. The reduction values of the slope with respect to the Nernst equation, expressed by the α coefficient, were 0.880,0.935, and 0.950 at ionic strengths of 10(-4), 10(-3), and 10(-2) mol dm(-3), respectively. The results were successfully interpreted by employing the surface complexation model, developed originally for metal oxides and adapted for silver halides. The thermodynamic ("intrinsic") equilibrium constants for binding of bromide (K(n)(∘)) and silver (K(p)(∘)) ions on the corresponding sites at the silver bromide surface were evaluated as lgK(n)(∘)=3.98; lgK(p)(∘)=2.48. Symmetrical counterion surface association was assumed and equilibrium constants were obtained as lgK(NO(3)(-))(∘)=lgK(K(+))(∘)=4.30.

  1. In situ surface potential evolution along Au/Gd:CeO2 electrode interfaces

    NASA Astrophysics Data System (ADS)

    Zhu, Jiaxin; Wang, Jiaying; Mebane, David S.; Nonnenmann, Stephen S.

    2017-04-01

    We present an investigation of electroactive Au/gadolinium doped ceria electrode interfaces under CO2/CO co-electrolysis environments using a combination of in situ high temperature scanning surface potential microscopy (HT-SSPM) and modified Poisson-Cahn (PC) models. Here charged surface adsorbate-oxygen vacancy interactions manifested in HT-SSPM potential profiles as small perturbations of opposite sign in reference to the applied biases. The positive deviation of surface potential on Au from applied cathodic biases is attributed to the work function difference between gold (ϕAu ˜ 5.31 eV) and graphitic carbon deposits (ϕC ˜ 5.0 eV) formed through CO disproportionation. The negative potential deviation from the applied anodic bias is attributed to negatively charged carboxylates. Results of the PC model confirmed the affinity of oxygen vacancies for the surface, thus supporting in situ experimental evidence of surface vacancy accumulation/depletion processes induced by cathodic/anodic biases.

  2. The molecular potential energy surface and vibrational energy levels of methyl fluoride. Part II.

    PubMed

    Manson, Steven A; Law, Mark M; Atkinson, Ian A; Thomson, Grant A

    2006-06-28

    New analytical bending and stretching, ground electronic state, potential energy surfaces for CH(3)F are reported. The surfaces are expressed in bond-length, bond-angle internal coordinates. The four-dimensional stretching surface is an accurate, least squares fit to over 2000 symmetrically unique ab initio points calculated at the CCSD(T) level. Similarly, the five-dimensional bending surface is a fit to over 1200 symmetrically unique ab initio points. This is an important first stage towards a full nine-dimensional potential energy surface for the prototype CH(3)F molecule. Using these surfaces, highly excited stretching and (separately) bending vibrational energy levels of CH(3)F are calculated variationally using a finite basis representation method. The method uses the exact vibrational kinetic energy operator derived for XY(3)Z systems by Manson and Law (preceding paper, Part I, Phys. Chem. Chem. Phys., 2006, 8, DOI: 10.1039/b603106d). We use the full C(3v) symmetry and the computer codes are designed to use an arbitrary potential energy function. Ultimately, these results will be used to design a compact basis for fully coupled stretch-bend calculations of the vibrational energy levels of the CH(3)F system.

  3. The impact of surface area, volume, curvature, and Lennard-Jones potential to solvation modeling.

    PubMed

    Nguyen, Duc D; Wei, Guo-Wei

    2017-01-05

    This article explores the impact of surface area, volume, curvature, and Lennard-Jones (LJ) potential on solvation free energy predictions. Rigidity surfaces are utilized to generate robust analytical expressions for maximum, minimum, mean, and Gaussian curvatures of solvent-solute interfaces, and define a generalized Poisson-Boltzmann (GPB) equation with a smooth dielectric profile. Extensive correlation analysis is performed to examine the linear dependence of surface area, surface enclosed volume, maximum curvature, minimum curvature, mean curvature, and Gaussian curvature for solvation modeling. It is found that surface area and surfaces enclosed volumes are highly correlated to each other's, and poorly correlated to various curvatures for six test sets of molecules. Different curvatures are weakly correlated to each other for six test sets of molecules, but are strongly correlated to each other within each test set of molecules. Based on correlation analysis, we construct twenty six nontrivial nonpolar solvation models. Our numerical results reveal that the LJ potential plays a vital role in nonpolar solvation modeling, especially for molecules involving strong van der Waals interactions. It is found that curvatures are at least as important as surface area or surface enclosed volume in nonpolar solvation modeling. In conjugation with the GPB model, various curvature-based nonpolar solvation models are shown to offer some of the best solvation free energy predictions for a wide range of test sets. For example, root mean square errors from a model constituting surface area, volume, mean curvature, and LJ potential are less than 0.42 kcal/mol for all test sets. © 2016 Wiley Periodicals, Inc.

  4. Adiabatic quantum state transfer in tight-binding chains using periodic driving fields

    NASA Astrophysics Data System (ADS)

    Longhi, S.

    2014-09-01

    A method for high-fidelity coherent adiabatic transport in a zig-zag tight-binding chain, based on application of two external periodic driving fields, is theoretically proposed. The method turns out to be robust against imperfections and disorder of the static lattice Hamiltonian, is tolerant to next-nearest neighborhood interactions, and enables coherent transport in long chains without the need for a local control and timing of the trapping potential.

  5. Fluorescence quenching studies of potential-dependent DNA reorientation dynamics at glassy carbon electrode surfaces.

    PubMed

    Li, Qin; Cui, Chenchen; Higgins, Daniel A; Li, Jun

    2012-09-05

    The potential-dependent reorientation dynamics of double-stranded DNA (ds-DNA) attached to planar glassy carbon electrode (GCE) surfaces were investigated. The orientation state of surface-bound ds-DNA was followed by monitoring the fluorescence from a 6-carboxyfluorescein (FAM6) fluorophore covalently linked to the distal end of the DNA. Positive potentials (i.e., +0.2 V vs open circuit potential, OCP) caused the ds-DNA to align parallel to the electrode surface, resulting in strong dipole-electrode quenching of FAM6 fluorescence. Switching of the GCE potential to negative values (i.e., -0.2 V vs OCP) caused the ds-DNA to reorient perpendicular to the electrode surface, with a concomitant increase in FAM6 fluorescence. In addition to the very fast (submilliseconds) dynamics of the initial reorientation process, slow (0.1-0.9 s) relaxation of FAM6 fluorescence to intermediate levels was also observed after potential switching. These dynamics have not been previously described in the literature. They are too slow to be explained by double layer charging, and chronoamperometry data showed no evidence of such effects. Both the amplitude and rate of the dynamics were found to depend upon buffer concentration, and ds-DNA length, demonstrating a dependence on the double layer field. The dynamics are concluded to arise from previously undetected complexities in the mechanism of potential-dependent ds-DNA reorientation. The possible origins of these dynamics are discussed. A better understanding of these dynamics will lead to improved models for potential-dependent ds-DNA reorientation at electrode surfaces and will facilitate the development of advanced electrochemical devices for detection of target DNAs.

  6. [ASSESSMENT OF POTENTIAL RISK FOR CONTAMINATION OF SURFACE WATER RESERVOIRS BY PATHOGENS OF HUMAN PARASITIC DISEASES].

    PubMed

    Khromenkova, E P; Dimidova, L L; Dumbadze, O S; Aidinov, G T; Shendo, G L; Agirov, A Kh; Batchaev, Kh Kh

    2015-01-01

    Sanitary and parasitological studies of the waste effluents and surface reservoir waters were conducted in the south of Russia. The efficiency of purification of waste effluents from the pathogens of parasitic diseases was investigated in the region's sewage-purification facilities. The water of the surface water reservoirs was found to contain helminthic eggs and larvae and intestinal protozoan cysts because of the poor purification and disinfection of service fecal sewage waters. The poor purification and disinvasion of waste effluents in the region determine the potential risk of contamination of the surface water reservoirs and infection of the population with the pathogens of human parasitic diseases.

  7. Interfacial Segregation in Disordered Block Copolymers: Effect of Tunable Surface Potentials

    SciTech Connect

    Mansky, P.; Russell, T.P.; Hawker, C.J.; Mays, J.; Cook, D.C.; Satija, S.K.

    1997-07-01

    The response of disordered P({ital d}-S-{ital b}-MMA) diblock copolymers to variable strength surface fields has been studied by neutron reflectivity. Surface interactions were controlled by end grafting P(S-{ital r}-MMA) random copolymers with various styrene contents onto Si substrates. The degree interfacial segregation of the block copolymer was proportional to the surface potential. A first-order transition in the degree of segregation was observed as the brush composition was varied. Conditions were found which yielded neutral boundary conditions {ital simultaneously} at the vacuum and substrate interfaces. {copyright} {ital 1997} {ital The American Physical Society}

  8. Bohm potential effect on the propagation of electrostatic surface wave in semi-bounded quantum plasmas

    NASA Astrophysics Data System (ADS)

    Lee, Myoung-Jae; Jung, Young-Dae

    2017-02-01

    High frequency electrostatic wave propagation in a dense and semi-bounded electron quantum plasma is investigated with consideration of the Bohm potential. The dispersion relation for the surface mode of quantum plasma is derived and numerically analyzed. We found that the quantum effect enhances the frequency of the wave especially in the high wave number regime. However, the frequency of surface wave is found to be always lower than that of the bulk wave for the same quantum wave number. The group velocity of the surface wave for various quantum wave number is also obtained.

  9. Negative electrostatic surface potential of protein sites specific for anionic ligands.

    PubMed Central

    Ledvina, P S; Yao, N; Choudhary, A; Quiocho, F A

    1996-01-01

    Determination of the crystal structure of an "open" unliganded active mutant (T141D) form of the Escherichia coli phosphate receptor for active transport has allowed calculation of the electrostatic surface potential for it and two other comparably modeled receptor structures (wild type and D137N). A discovery of considerable implication is the intensely negative potential of the phosphate-binding cleft. We report similar findings for a sulfate transport receptor, a DNA-binding protein, and, even more dramatically, redox proteins. Evidently, for proteins such as these, which rely almost exclusively on hydrogen bonding for anion interactions and electrostatic balance, a noncomplementary surface potential is not a barrier to binding. Moreover, experimental results show that the exquisite specificity and high affinity of the phosphate and sulfate receptors for unions are insensitive to modulations of charge potential, but extremely sensitive to conditions that leave a hydrogen bond donor or acceptor unpaired. Images Fig. 1 Fig. 2 Fig. 3 PMID:8692896

  10. Negative electrostatic surface potential of protein sites specific for anionic ligands.

    PubMed

    Ledvina, P S; Yao, N; Choudhary, A; Quiocho, F A

    1996-06-25

    Determination of the crystal structure of an "open" unliganded active mutant (T141D) form of the Escherichia coli phosphate receptor for active transport has allowed calculation of the electrostatic surface potential for it and two other comparably modeled receptor structures (wild type and D137N). A discovery of considerable implication is the intensely negative potential of the phosphate-binding cleft. We report similar findings for a sulfate transport receptor, a DNA-binding protein, and, even more dramatically, redox proteins. Evidently, for proteins such as these, which rely almost exclusively on hydrogen bonding for anion interactions and electrostatic balance, a noncomplementary surface potential is not a barrier to binding. Moreover, experimental results show that the exquisite specificity and high affinity of the phosphate and sulfate receptors for unions are insensitive to modulations of charge potential, but extremely sensitive to conditions that leave a hydrogen bond donor or acceptor unpaired.

  11. Spatial potential ripples of azimuthal surface modes in topological insulator Bi2Te3 nanowires

    PubMed Central

    Muñoz Rojo, Miguel; Zhang, Yingjie; Manzano, Cristina V.; Alvaro, Raquel; Gooth, Johannes; Salmeron, Miquel; Martin-Gonzalez, Marisol

    2016-01-01

    Topological insulators (TI) nanowires (NW) are an emerging class of structures, promising both novel quantum effects and potential applications in low-power electronics, thermoelectrics and spintronics. However, investigating the electronic states of TI NWs is complicated, due to their small lateral size, especially at room temperature. Here, we perform scanning probe based nanoscale imaging to resolve the local surface potential landscapes of Bi2Te3 nanowires (NWs) at 300 K. We found equipotential rings around the NWs perimeter that we attribute to azimuthal 1D modes. Along the NW axis, these modes are altered, forming potential ripples in the local density of states, due to intrinsic disturbances. Potential mapping of electrically biased NWs enabled us to accurately determine their conductivity which was found to increase with the decrease of NW diameter, consistent with surface dominated transport. Our results demonstrate that TI NWs can pave the way to both exotic quantum states and novel electronic devices. PMID:26751282

  12. Improved Potential Energy Surface of Ozone Constructed Using the Fitting by Permutationally Invariant Polynomial Function

    DOE PAGES

    Ayouz, Mehdi; Babikov, Dmitri

    2012-01-01

    New global potential energy surface for the ground electronic state of ozone is constructed at the complete basis set level of the multireference configuration interaction theory. A method of fitting the data points by analytical permutationally invariant polynomial function is adopted. A small set of 500 points is preoptimized using the old surface of ozone. In this procedure the positions of points in the configuration space are chosen such that the RMS deviation of the fit is minimized. New ab initio calculations are carried out at these points and are used to build new surface. Additional points are addedmore » to the vicinity of the minimum energy path in order to improve accuracy of the fit, particularly in the region where the surface of ozone exhibits a shallow van der Waals well. New surface can be used to study formation of ozone at thermal energies and its spectroscopy near the dissociation threshold.« less

  13. Visualization of GaN surface potential using terahertz emission enhanced by local defects

    NASA Astrophysics Data System (ADS)

    Sakai, Yuji; Kawayama, Iwao; Nakanishi, Hidetoshi; Tonouchi, Masayoshi

    2015-09-01

    Wide-gap semiconductors have received significant attention for their advantages over existing semiconductors in energy-efficient power devices. To realize stable and reliable wide-gap semiconductor devices, the basic physical properties, such as the electric properties on the surface and at the interface, should be revealed. Here, we report visualization of terahertz (THz) emission from the surface of GaN, which is excited by ultraviolet femtosecond laser pulses. We found that the THz emission is enhanced by defects related to yellow luminescence, and this phenomenon is explained through the modification of band structures in the surface depletion layer owing to trapped electrons at defect sites. Our results demonstrate that the surface potential in a GaN surface could be detected by laser-induced THz emission. Moreover, this method enables feasible evaluation of the distribution of non-radiative defects, which are undetectable with photoluminescence, and it contributes to the realization normally-off GaN devices.

  14. Visualization of GaN surface potential using terahertz emission enhanced by local defects.

    PubMed

    Sakai, Yuji; Kawayama, Iwao; Nakanishi, Hidetoshi; Tonouchi, Masayoshi

    2015-09-09

    Wide-gap semiconductors have received significant attention for their advantages over existing semiconductors in energy-efficient power devices. To realize stable and reliable wide-gap semiconductor devices, the basic physical properties, such as the electric properties on the surface and at the interface, should be revealed. Here, we report visualization of terahertz (THz) emission from the surface of GaN, which is excited by ultraviolet femtosecond laser pulses. We found that the THz emission is enhanced by defects related to yellow luminescence, and this phenomenon is explained through the modification of band structures in the surface depletion layer owing to trapped electrons at defect sites. Our results demonstrate that the surface potential in a GaN surface could be detected by laser-induced THz emission. Moreover, this method enables feasible evaluation of the distribution of non-radiative defects, which are undetectable with photoluminescence, and it contributes to the realization normally-off GaN devices.

  15. Superhydrophobic poly(L-lactic acid) surface as potential bacterial colonization substrate

    PubMed Central

    2011-01-01

    Hydrophobicity is a very important surface property and there is a growing interest in the production and characterization of superhydrophobic surfaces. Accordingly, it was recently shown how to obtain a superhydrophobic surface using a simple and cost-effective method on a polymer named poly(L-lactic acid) (PLLA). To evaluate the ability of such material as a substrate for bacterial colonization, this work assessed the capability of different bacteria to colonize a biomimetic rough superhydrophobic (SH) PLLA surface and also a smooth hydrophobic (H) one. The interaction between these surfaces and bacteria with different morphologies and cell walls was studied using one strain of Staphylococcus aureus and one of Pseudomonas aeruginosa. Results showed that both bacterial strains colonized the surfaces tested, although significantly higher numbers of S. aureus cells were found on SH surfaces comparing to H ones. Moreover, scanning electron microscopy images showed an extracellular matrix produced by P. aeruginosa on SH PLLA surfaces, indicating that this bacterium is able to form a biofilm on such substratum. Bacterial removal through lotus leaf effect was also tested, being more efficient on H coupons than on SH PLLA ones. Overall, the results showed that SH PLLA surfaces can be used as a substrate for bacterial colonization and, thus, have an exceptional potential for biotechnology applications. PMID:22018163

  16. 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.

  17. The Measurement and Research of Surface Potentials of Human Tooth in vitro

    DTIC Science & Technology

    2007-11-02

    dental hard tissue, no mater enamel , dentin or cementum, is formed mostly by the mineral, hydroxyapatite . It is soaked in the electrolyte surroundings...of the potentials, the surface potentials between mid-spots of enamel crown’s buccal side and tooth root were measured with electrochemical...property made by Klein and Amberson, 1932, had suggested that the dental enamel was an electrostatic ion screen and it had permselectivity[1]. Then

  18. Foraging on the potential energy surface: A swarm intelligence-based optimizer for molecular geometry

    NASA Astrophysics Data System (ADS)

    Wehmeyer, Christoph; Falk von Rudorff, Guido; Wolf, Sebastian; Kabbe, Gabriel; Schärf, Daniel; Kühne, Thomas D.; Sebastiani, Daniel

    2012-11-01

    We present a stochastic, swarm intelligence-based optimization algorithm for the prediction of global minima on potential energy surfaces of molecular cluster structures. Our optimization approach is a modification of the artificial bee colony (ABC) algorithm which is inspired by the foraging behavior of honey bees. We apply our modified ABC algorithm to the problem of global geometry optimization of molecular cluster structures and show its performance for clusters with 2-57 particles and different interatomic interaction potentials.

  19. High temperature and dynamic testing of AHSS for an analytical description of the adiabatic cutting process

    NASA Astrophysics Data System (ADS)

    Winter, S.; Schmitz, F.; Clausmeyer, T.; Tekkaya, A. E.; F-X Wagner, M.

    2017-03-01

    In the automotive industry, advanced high strength steels (AHSS) are widely used as sheet part components to reduce weight, even though this leads to several challenges. The demand for high-quality shear cutting surfaces that do not require reworking can be fulfilled by adiabatic shear cutting: High strain rates and local temperatures lead to the formation of adiabatic shear bands (ASB). While this process is well suited to produce AHSS parts with excellent cutting surface quality, a fundamental understanding of the process is still missing today. In this study, compression tests in a Split-Hopkinson Pressure Bar with an initial strain rate of 1000 s-1 were performed in a temperature range between 200 °C and 1000 °C. The experimental results show that high strength steels with nearly the same mechanical properties at RT may possess a considerably different behavior at higher temperatures. The resulting microstructures after testing at different temperatures were analyzed by optical microscopy. The thermo-mechanical material behavior was then considered in an analytical model. To predict the local temperature increase that occurs during the adiabatic blanking process, experimentally determined flow curves were used. Furthermore, the influence of temperature evolution with respect to phase transformation is discussed. This study contributes to a more complete understanding of the relevant microstructural and thermo-mechanical mechanisms leading to the evolution of ASB during cutting of AHSS.

  20. On the origin of the electrostatic surface potential of Aspergillus niger spores in acidic environments.

    PubMed

    Wargenau, Andreas; Fleissner, André; Bolten, Christoph Josef; Rohde, Manfred; Kampen, Ingo; Kwade, Arno

    2011-12-01

    The electrostatic surface potential of fungal spores is generally regarded as potentially influencing spore aggregation and pellet formation in submerged cultures of filamentous fungi. Spores of Aspergillus niger are typically characterized by negative zeta potentials over a wide range of pH values. In this study, this particular behavior is ascribed to the presence of an extensive melanin coating. It is proposed on the basis of zeta potential and pigment extraction experiments that this outermost layer affects the pH-dependent surface potential in two manners: (i) by the addition of negative charges to the spore surface and (ii) by the pH-dependent release of melanin pigment. Chemical analyses revealed that deprotonation of melanin-bound carboxyl groups is most probably responsible for pigment release under acidic conditions. These findings were incorporated into a simple model which has the ability to qualitatively explain the results of zeta potential experiments and, moreover, to provide the basis for quantitative investigations on the role of electrostatics in spore aggregation.

  1. Adiabatic measurements of magneto-caloric effects in pulsed high magnetic fields up to 55 T

    NASA Astrophysics Data System (ADS)

    Kihara, T.; Kohama, Y.; Hashimoto, Y.; Katsumoto, S.; Tokunaga, M.

    2013-07-01

    Magneto-caloric effects (MCEs) measurement system in adiabatic condition is proposed to investigate the thermodynamic properties in pulsed magnetic fields up to 55 T. With taking the advantage of the fast field-sweep rate in pulsed field, adiabatic measurements of MCEs were carried out at various temperatures. To obtain the prompt response of the thermometer in the pulsed field, a thin film thermometer is grown directly on the sample surfaces. The validity of the present setup was demonstrated in the wide temperature range through the measurements on Gd at about room temperature and on Gd3Ga5O12 at low temperatures. The both results show reasonable agreement with the data reported earlier. By comparing the MCE data with the specific heat data, we could estimate the entropy as functions of magnetic field and temperature. The results demonstrate the possibility that our approach can trace the change in transition temperature caused by the external field.

  2. Fully adiabatic 31P 2D-CSI with reduced chemical shift displacement error at 7 T--GOIA-1D-ISIS/2D-CSI.

    PubMed

    Chmelík, M; Kukurová, I Just; Gruber, S; Krššák, M; Valkovič, L; Trattnig, S; Bogner, W

    2013-05-01

    A fully adiabatic phosphorus (31P) two-dimensional (2D) chemical shift spectroscopic imaging sequence with reduced chemical shift displacement error for 7 T, based on 1D-image-selected in vivo spectroscopy, combined with 2D-chemical shift spectroscopic imaging selection, was developed. Slice-selective excitation was achieved by a spatially selective broadband GOIA-W(16,4) inversion pulse with an interleaved subtraction scheme before nonselective adiabatic excitation, and followed by 2D phase encoding. The use of GOIA-W(16,4) pulses (bandwidth 4.3-21.6 kHz for 10-50 mm slices) reduced the chemical shift displacement error in the slice direction ∼1.5-7.7 fold, compared to conventional 2D-chemical shift spectroscopic imaging with Sinc3 selective pulses (2.8 kHz). This reduction was experimentally demonstrated with measurements of an MR spectroscopy localization phantom and with experimental evaluation of pulse profiles. In vivo experiments in clinically acceptable measurement times were demonstrated in the calf muscle (nominal voxel volume, 5.65 ml in 6 min 53 s), brain (10 ml, 6 min 32 s), and liver (8.33 ml, 8 min 14 s) of healthy volunteers at 7 T. High reproducibility was found in the calf muscle at 7 T. In combination with adiabatic excitation, this sequence is insensitive to the B1 inhomogeneities associated with surface coils. This sequence, which is termed GOIA-1D-ISIS/2D-CSI (goISICS), has the potential to be applied in both clinical research and in the clinical routine.

  3. Unconventional nanotubes self-assembled in alumina channels: morphology and surface potential of isolated nanostructures at surfaces.

    PubMed

    Palermo, Vincenzo; Liscio, Andrea; Talarico, Anna Maria; Zhi, Linjie; Müllen, Klaus; Samorì, Paolo

    2007-06-15

    Synthetic nanographenes have been self-assembled from solution on the surface of nanometric channels of an alumina membrane template. By controlling the interplay between intermolecular and interfacial interactions, the molecules have been adsorbed either 'face-on' or 'edge-on' on the pore's surfaces, leading to the formation of columnar stacks in the latter case. Upon thermal treatment at high temperature, the molecular cross-linking of the columns has been triggered, transforming the delicate supramolecular arrangement into robust carbon nanotubes, with the graphitic planes at predetermined orientations with respect to the tube axis. Scanning force microscopy characterization of single nanotubes deposited from suspensions on mica showed that the nanotubes can self-assemble on flat surfaces adopting preferential alignments which reflect the threefold symmetry of the mica substrate. Kelvin probe force microscopy studies revealed that the nanotubes possess a surface potential much smaller than the work function of both graphite and conventional vacuum-processed nanotubes, providing evidence for their more confined electronic structure.

  4. Computation of surface electrical potentials of plant cell membranes . Correspondence To published zeta potentials from diverse plant sources

    PubMed

    Kinraide; Yermiyahu; Rytwo

    1998-10-01

    A Gouy-Chapman-Stern model has been developed for the computation of surface electrical potential (psi0) of plant cell membranes in response to ionic solutes. The present model is a modification of an earlier version developed to compute the sorption of ions by wheat (Triticum aestivum L. cv Scout 66) root plasma membranes. A single set of model parameters generates values for psi0 that correlate highly with published zeta potentials of protoplasts and plasma membrane vesicles from diverse plant sources. The model assumes ion binding to a negatively charged site (R- = 0.3074 &mgr;mol m-2) and to a neutral site (P0 = 2.4 &mgr;mol m-2) according to the reactions R- + IZ &rlharr; RIZ-1 and P0 + IZ &rlharr; PIZ, where IZ represents an ion of charge Z. Binding constants for the negative site are 21, 500 M-1 for H+, 20,000 M-1 for Al3+, 2,200 M-1 for La3+, 30 M-1 for Ca2+ and Mg2+, and 1 M-1 for Na+ and K+. Binding constants for the neutral site are 1/180 the value for binding to the negative site. Ion activities at the membrane surface, computed on the basis of psi0, appear to determine many aspects of plant-mineral interactions, including mineral nutrition and the induction and alleviation of mineral toxicities, according to previous and ongoing studies. A computer program with instructions for the computation of psi0, ion binding, ion concentrations, and ion activities at membrane surfaces may be requested from the authors.

  5. Quantum adiabatic optimization and combinatorial landscapes

    NASA Astrophysics Data System (ADS)

    Smelyanskiy, V. N.; Knysh, S.; Morris, R. D.

    2004-09-01

    In this paper we analyze the performance of the Quantum Adiabatic Evolution algorithm on a variant of the satisfiability problem for an ensemble of random graphs parametrized by the ratio of clauses to variables, γ=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 (instead of only energy) is used, and are able to show the existence of a dynamic threshold γ=γd starting with some value of K —the number of variables in each clause. Beyond the dynamic threshold, the algorithm 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. We have been able to map the ensemble of random graphs onto another ensemble with fluctuations significantly reduced. This enabled us to obtain tight upper bounds on the satisfiability transition and to recompute the dynamical transition using the extended set of landscapes.

  6. 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.

  7. Adiabatic quantum algorithm for search engine ranking.

    PubMed

    Garnerone, Silvano; Zanardi, Paolo; Lidar, Daniel A

    2012-06-08

    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.

  8. 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.

  9. On the persistence of adiabatic shear bands

    NASA Astrophysics Data System (ADS)

    Boakye-Yiadom, S.; Bassim, M. N.; Al-Ameeri, S.

    2012-08-01

    It is generally agreed that the initiation and development of adiabatic shear bands (ASBs) are manifestations of damage in metallic materials subjected to high strain rates and large strains as those due to impact in a Hopkinson Bar system. Models for evolution of these bands have been described in the literature. One question that has not received attention is how persistent these bands are and whether their presence and effect can be reversed or eliminated by using a process of thermal (heat treatment) or thermo-mechanical treatment that would relieve the material from the high strain associated with ASBs and their role as precursors to crack initiation and subsequent failure. Since ASBs are more prevalent and more defined in BCC metals including steels, a study was conducted to investigate the best conditions of generating ASBs in a heat treatable steel, followed by determining the best conditions for heat treatment of specimens already damaged by the presence of ASBs in order to relieve the strains due to ASBs and restore the material to an apparent microstructure without the "scars" due to the previous presence of ASBs. It was found that heat treatment achieves the curing from ASBs. This presentation documents the process undertaken to achieve this objective.

  10. Adiabatic Spin Pumping with Quantum Dots

    NASA Astrophysics Data System (ADS)

    Mucciolo, Eduardo R.

    Electronic transport in mesoscopic systems has been intensively studied for more the last three decades. While there is a substantial understanding of the stationary regime, much less is know about phase-coherent nonequilibrium transport when pulses or ac perturbations are used to drive electrons at low temperatures and at small length scales. However, about 20 years ago Thouless proposed to drive nondissipative currents in quantum systems by applying simultaneously two phase-locked external perturbations. The so-called adiabatic pumping mechanism has been revived in the last few years, both theoretically and experimentally, in part because of the development of lateral semiconductor quantum dots. Here we will explain how open dots can be used to create spin-polarized currents with little or no net charge transfer. The pure spin pump we propose is the analog of a charge battery in conventional electronics and may provide a needed circuit element for spin-based electronics. We will also discuss other relevant issues such as rectification and decoherence and point out possible extensions of the mechanism to closed dots.

  11. General background conditions for K-bounce and adiabaticity

    NASA Astrophysics Data System (ADS)

    Romano, Antonio Enea

    2017-03-01

    We study the background conditions for a bounce uniquely driven by a single scalar field model with a generalized kinetic term K( X), without any additional matter field. At the background level we impose the existence of two turning points where the derivative of the Hubble parameter H changes sign and of a bounce point where the Hubble parameter vanishes. We find the conditions for K( X) and the potential which ensure the above requirements. We then give the examples of two models constructed according to these conditions. One is based on a quadratic K( X), and the other on a K( X) which is avoiding divergences of the second time derivative of the scalar field, which may otherwise occur. An appropriate choice of the initial conditions can lead to a sequence of consecutive bounces, or oscillations of H. In the region where these models have a constant potential they are adiabatic on any scale and because of this they may not conserve curvature perturbations on super-horizon scales. While at the perturbation level one class of models is free from ghosts and singularities of the classical equations of motion, in general gradient instabilities are present around the bounce time, because the sign of the squared speed of sound is opposite to the sign of the time derivative of H. We discuss how this kind of instabilities could be avoided by modifying the Lagrangian by introducing Galilean terms in order to prevent a negative squared speed of sound around the bounce.

  12. Surface packing determines the redox potential shift of cytochrome c adsorbed on gold.

    PubMed

    Zanetti-Polzi, Laura; Daidone, Isabella; Bortolotti, Carlo Augusto; Corni, Stefano

    2014-09-17

    Thermodynamic and dynamic properties of iso-1-cytochrome c covalently bound to a bare gold surface are here investigated by large scale atomistic simulations. The reduction potential of the protein for low and high surface concentrations is calculated showing a good agreement with experimental estimates. The origin of the dependence of the reduction potential on the surface concentration is investigated and is demonstrated to stem from the changing polarizability of the environment surrounding the protein, a mechanism reminiscent of crowding effects. Moreover, structural analyses are performed revealing relevant changes induced by the presence of the electrode on the dynamic properties of cytochrome c. In particular, one of the two cavities previously identified on the protein surface [Bortolotti et al. J. Am. Chem. Soc., 2012, 134, 13670], and that reversibly open in cytochrome c freely diffusing in solution, is found to be deformed when the protein is adsorbed on gold. This modification exemplifies a mechanism that potentially leads to changes in the protein properties by surface-induced modification of its dynamical behavior.

  13. How surface potential determines the kinetics of the first hole transfer of photocatalytic water oxidation.

    PubMed

    Waegele, Matthias M; Chen, Xihan; Herlihy, David M; Cuk, Tanja

    2014-07-30

    Interfacial hole transfer between n-SrTiO3 and OH(-) was investigated by surface sensitive transient optical spectroscopy of an in situ photoelectrochemical cell during water oxidation. The kinetics reveal a single rate constant with an exponential dependence on the surface hole potential, spanning time scales from 3 ns to 8 ps over a ≈1 V increase. A voltage- and laser illumination-induced process moves the valence band edge at the n-type semiconductor/water interface to continuously change the surface hole potential. This single step of the water oxidation reaction is assigned to the first hole transfer h(+) + OH(-) → OH(•). The kinetics quantify how much a change in the free energy difference driving this first hole transfer reduces the activation barrier. They are also used to extrapolate the kinetic rate due to the activation barrier when that free energy difference is zero, or the Nernstian potential. This is the first time transient spectroscopy has enabled the separation of the first hole transfer from the full four hole transfer cycle and a direct determination of these two quantities. The Nernstian potential for OH(-)/OH(•) is also suggested, in rough agreement with gas-phase studies. The observation of a distinct, much longer time scale upon picosecond hole transfer to OH(-) suggests that a dominant, more stable intermediate of the water oxidation reaction, possibly a surface bound oxo, may result.

  14. Divacancy binding energy, formation energy and surface energy of BCC transition metals using MEAM potentials

    NASA Astrophysics Data System (ADS)

    Uniyal, Shweta; Chand, Manesh; Joshi, Subodh; Semalty, P. D.

    2016-05-01

    The modified embedded atom method (MEAM) potential parameters have been employed to calculate the unrelaxed divacancy formation energy, binding energy and surface energies for low index planes in bcc transition metals. The calculated results of divacancy binding energy and vacancy formation energy compare well with experimental and other available calculated results.

  15. Computer Series 41: Potential-Energy Surfaces and Transition-State Theory.

    ERIC Educational Resources Information Center

    Moss, S. J.; Coady, C. J.

    1983-01-01

    Describes computer programs involving the London-Eyring-Polany-Sato method (LEPS). The programs provide a valuable means of introducing students to potential energy surfaces and to the foundations of transition state theory. Program listings (with copies of student scripts) or programs on DOS 3.3 disc are available from authors. (JN)

  16. POTENTIAL INHALATION EXPOSURE TO VOLATILE CHEMICALS IN WATER-BASED HARD-SURFACE CLEANERS

    EPA Science Inventory

    Potential inhalation exposure of building occupants to volatile chemicals in water-based hard-surface cleaners was evaluated by analyzing 267 material safety data sheets (MSDSs). Among the 154 chemicals reported, 44 are volatile or semi-volatile. Hazardous air pollutants (HAPs) r...

  17. Dopant gas effect on silicon chemical vapor depositions: A surface potential model

    NASA Technical Reports Server (NTRS)

    Chang, C. A.

    1975-01-01

    A surface potential model is proposed to consistently explain the known dopant gas effects on silicon chemical vapor deposition. This model predicts that the effects of the same dopant gases on the diamond deposition rate using methane and carbon tetrachloride should be opposite and similar to those of silane, respectively. Available data are in agreement with this prediction.

  18. Surface study of films formed on copper and brass at open circuit potential

    NASA Astrophysics Data System (ADS)

    Procaccini, R.; Schreiner, W. H.; Vázquez, M.; Ceré, S.

    2013-03-01

    The corrosion resistance of Cu-Zn alloys strongly depends on the quality of the protective passive film. This study focuses on the influence of Zn on the composition of oxide films on copper and brass (Cu77Zn21Al2) in borax 0.1 mol L-1 (pH 9.2) solution, where the solubility of copper oxides is minimal. The effect of the presence of chloride ions at low concentration (0.01 mol L-1) in the electrolyte was also evaluated. Both conditions were studied using a set of different electrochemical, optical and surface techniques such as cyclic voltammetry, differential reflectance, X-ray photoelectron spectroscopy and Raman spectroscopy. A duplex Cu2O/CuO layer forms on copper at potentials positive to the open circuit potential (OCP), while in the case of brass, zinc compounds are also incorporated to the surface film. It also became evident that a surface film can be formed on these materials even at potentials negative to the OCP. Zn(II) species are the main constituents of the films growing on brass, while copper oxides are incorporated to the surface film when approaching the OCP. The presence of chloride ions at low concentrations contributes to the dissolution of the oxo-hydroxides formed during the early stages of the aging process at open circuit potential. Also, copper chloro-compounds are formed, as shown by Raman spectroscopy for both copper and brass electrodes.

  19. Vibrational dynamics of the bifluoride ion. I. Construction of a model potential surface

    NASA Astrophysics Data System (ADS)

    Epa, V. C.; Choi, J. H.; Klobukowski, M.; Thorson, W. R.

    1990-01-01

    Construction of an extended model potential surface for the bifluoride ion [FHF-] is described, based on ab initio calculations for the free ion at the CID (configuration interaction, double replacement) level with a Huzinaga-Dunning double-zeta basis set. 710 data points were generated, for displacements in the three noncyclic vibrational coordinates exploring the potential surface to a height at least 30 000 cm-1 above its minimum, and giving a realistic account of the dissociation into HF+F-. Analogous calculations were made for HF and F- using the same basis. The predicted hydrogen bond energy (De) is 48.13 kcal/mol, with equilibrium F-F separation Re =4.2905 a.u., in good agreement with other recent calculations. A model potential has been constructed, based on a superposition of Morse potentials associated with each H-F distance plus a fairly structureless correction function expressible as a 36-term least-squares polynomial in the prolate spheroidal coordinates used to describe vibrational displacements. The resulting model surface fits all 710 ab initio data points with an r.m.s. deviation of 65.6 cm-1, and points less than 15 000 cm-1 above the minimum with a deviation of 26.3 cm-1. This surface provides the basis for a series of vibrational dynamics studies on the FHF- system being done in this laboratory.

  20. Lunar Surface Electric Potential Changes Associated with Traversals through the Earth's Foreshock

    NASA Technical Reports Server (NTRS)

    Collier, Michael R.; Hills, H. Kent; Stubbs, Timothy J.; Halekas, Jasper S.; Delory, Gregory T.; Espley, Jared; Farrell, William M.; Freeman, John W.; Vondrak, Richard

    2011-01-01

    We report an analysis of one year of Suprathermal Ion Detector Experiment (SIDE) Total Ion Detector (TID) resonance events observed between January 1972 and January 1973. The study includes only those events during which upstream solar wind conditions were readily available. The analysis shows that these events are associated with lunar traversals through the dawn flank of the terrestrial magnetospheric bow shock. We propose that the events result from an increase in lunar surface electric potential effected by secondary electron emission due to primary electrons in the Earth's foreshock region (although primary ions may play a role as well). This work establishes (1) the lunar surface potential changes as the Moon moves through the terrestrial bow shock, (2) the lunar surface achieves potentials in the upstream foreshock region that differ from those in the downstream magnetosheath region, (3) these differences can be explained by the presence of energetic electron beams in the upstream foreshock region and (4) if this explanation is correct, the location of the Moon with respect to the terrestrial bow shock influences lunar surface potential.

  1. A generalized complementary relationship between actual and potential evaporation defined by a reference surface temperature

    NASA Astrophysics Data System (ADS)

    Aminzadeh, Milad; Roderick, Michael L.; Or, Dani

    2016-01-01

    The definition of potential evaporation remains widely debated despite its centrality for hydrologic and climatic models. We employed an analytical pore-scale representation of evaporation from terrestrial surfaces to define potential evaporation using a hypothetical steady state reference temperature that is common to both air and evaporating surface. The feedback between drying land surfaces and overlaying air properties, central in the Bouchet (1963) complementary relationship, is implicitly incorporated in the hypothetical steady state where the sensible heat flux vanishes and the available energy is consumed by evaporation. Evaporation rates predicted based on the steady state reference temperature hypothesis were in good agreement with class A pan evaporation measurements suggesting that evaporation from pans occurs with negligible sensible heat flux. The model facilitates a new generalization of the asymmetric complementary relationship with the asymmetry parameter b analytically predicted for a wide range of meteorological conditions with initial tests yielding good agreement between measured and predicted actual evaporation.

  2. Detection of a strongly negative surface potential at Saturn's moon Hyperion.

    PubMed

    Nordheim, T A; Jones, G H; Roussos, E; Leisner, J S; Coates, A J; Kurth, W S; Khurana, K K; Krupp, N; Dougherty, M K; Waite, J H

    2014-10-28

    On 26 September 2005, Cassini conducted its only close targeted flyby of Saturn's small, irregularly shaped moon Hyperion. Approximately 6 min before the closest approach, the electron spectrometer (ELS), part of the Cassini Plasma Spectrometer (CAPS) detected a field-aligned electron population originating from the direction of the moon's surface. Plasma wave activity detected by the Radio and Plasma Wave instrument suggests electron beam activity. A dropout in energetic electrons was observed by both CAPS-ELS and the Magnetospheric Imaging Instrument Low-Energy Magnetospheric Measurement System, indicating that the moon and the spacecraft were magnetically connected when the field-aligned electron population was observed. We show that this constitutes a remote detection of a strongly negative (∼ -200 V) surface potential on Hyperion, consistent with the predicted surface potential in regions near the solar terminator.

  3. Detection of a strongly negative surface potential at Saturn's moon Hyperion

    NASA Astrophysics Data System (ADS)

    Nordheim, T. A.; Jones, G. H.; Roussos, E.; Leisner, J. S.; Coates, A. J.; Kurth, W. S.; Khurana, K. K.; Krupp, N.; Dougherty, M. K.; Waite, J. H.

    2014-10-01

    On 26 September 2005, Cassini conducted its only close targeted flyby of Saturn's small, irregularly shaped moon Hyperion. Approximately 6 min before the closest approach, the electron spectrometer (ELS), part of the Cassini Plasma Spectrometer (CAPS) detected a field-aligned electron population originating from the direction of the moon's surface. Plasma wave activity detected by the Radio and Plasma Wave instrument suggests electron beam activity. A dropout in energetic electrons was observed by both CAPS-ELS and the Magnetospheric Imaging Instrument Low-Energy Magnetospheric Measurement System, indicating that the moon and the spacecraft were magnetically connected when the field-aligned electron population was observed. We show that this constitutes a remote detection of a strongly negative (~ -200 V) surface potential on Hyperion, consistent with the predicted surface potential in regions near the solar terminator.

  4. Ab initio potential energy and dipole moment surfaces of the F(-)(H2O) complex.

    PubMed

    Kamarchik, Eugene; Toffoli, Daniele; Christiansen, Ove; Bowman, Joel M

    2014-02-05

    We present full-dimensional, ab initio potential energy and dipole moment surfaces for the F(-)(H2O) complex. The potential surface is a permutationally invariant fit to 16,114 coupled-cluster single double (triple)/aVTZ energies, while the dipole surface is a covariant fit to 11,395 CCSD(T)/aVTZ dipole moments. Vibrational self-consistent field/vibrational configuration interaction (VSCF/VCI) calculations of energies and the IR-spectrum are presented both for F(-)(H2O) and for the deuterated analog, F(-)(D2O). A one-dimensional calculation of the splitting of the ground state, due to equivalent double-well global minima, is also reported.

  5. Detection of a strongly negative surface potential at Saturn's moon Hyperion

    PubMed Central

    Nordheim, T A; Jones, G H; Roussos, E; Leisner, J S; Coates, A J; Kurth, W S; Khurana, K K; Krupp, N; Dougherty, M K; Waite, J H

    2014-01-01

    On 26 September 2005, Cassini conducted its only close targeted flyby of Saturn's small, irregularly shaped moon Hyperion. Approximately 6 min before the closest approach, the electron spectrometer (ELS), part of the Cassini Plasma Spectrometer (CAPS) detected a field-aligned electron population originating from the direction of the moon's surface. Plasma wave activity detected by the Radio and Plasma Wave instrument suggests electron beam activity. A dropout in energetic electrons was observed by both CAPS-ELS and the Magnetospheric Imaging Instrument Low-Energy Magnetospheric Measurement System, indicating that the moon and the spacecraft were magnetically connected when the field-aligned electron population was observed. We show that this constitutes a remote detection of a strongly negative (∼ −200 V) surface potential on Hyperion, consistent with the predicted surface potential in regions near the solar terminator. PMID:26074639

  6. CAS SCF/CI calculations of potential energy surfaces of He 3+ and He 2+

    NASA Astrophysics Data System (ADS)

    Balasubramanian, K.; Liao, M. Z.; Lin, S. H.

    1987-12-01

    Complete active space MC SCF (CAS SCF) calculations followed by second-order configuration interaction (SOCI) calculations are carried out on the potential energy surfaces (bending surface, linear surfaces) of the 2Σ g+ ground state of He 3+. The potential minimum for the 2Σ g+ state occurs at a linear geometry with HeHe bond length of 1.248 Å. The binding energy of He 3+ with respect to He + He + + He was calculated to be 2.47 eV at the SOCI level. The energy required to dissociate He 3+ ( 2Σ g+) into He 2+ ( 2Σ u+) and He( 1S) is calculated to be 0.14 eV. The same level of SOCI calculations of He 2+ yield a De value of 2.36 eV.

  7. Surface potential at a ferroelectric grain due to asymmetric screening of depolarization fields

    SciTech Connect

    Genenko, Yuri A. Hirsch, Ofer; Erhart, Paul

    2014-03-14

    Nonlinear screening of electric depolarization fields, generated by a stripe domain structure in a ferroelectric grain of a polycrystalline material, is studied within a semiconductor model of ferroelectrics. It is shown that the maximum strength of local depolarization fields is rather determined by the electronic band gap than by the spontaneous polarization magnitude. Furthermore, field screening due to electronic band bending and due to presence of intrinsic defects leads to asymmetric space charge regions near the grain boundary, which produce an effective dipole layer at the surface of the grain. This results in the formation of a potential difference between the grain surface and its interior of the order of 1 V, which can be of either sign depending on defect transition levels and concentrations. Exemplary acceptor doping of BaTiO{sub 3} is shown to allow tuning of the said surface potential in the region between 0.1 and 1.3 V.

  8. Spatial distribution of potential near surface moisture flux at Yucca Mountain

    SciTech Connect

    Flint, A.L.; Flint, L.E.

    1994-12-31

    An estimate of the areal distribution of present-day surface liquid moisture flux at Yucca Mountain was made using field measured water contents and laboratory measured rock properties. Using available data for physical and hydrologic properties (porosity, saturated hydraulic conductivity moisture retention functions) of the volcanic rocks, surface lithologic units that are hydrologically similar were delineated. Moisture retention and relative permeability functions were assigned to each surface unit based on the similarity of the mean porosity and saturated hydraulic conductivity of the surface unit to laboratory samples of the same lithology. The potential flux into the mountain was estimated for each surface hydrologic unit using the mean saturated hydraulic conductivity for each unit and assuming all matrix flow. Using measured moisture profiles for each of the surface units, estimates were made of the depth at which seasonal fluctuations diminish and steady state downward flux conditions are likely to exist. The hydrologic properties at that depth were used with the current relative saturation of the tuff, to estimate flux as the unsaturated hydraulic conductivity. This method assumes a unit gradient. The range in estimated flux was 0.02 mm/yr for the welded Tiva Canyon to 13.4 mm/yr for the nonwelded Paintbrush Tuff. The areally averaged flux was 1.4 mm/yr. The major zones of high flux occur to the north of the potential repository boundary where the nonwelded tuffs are exposed in the major drainages.

  9. On the influence of the intermolecular potential on the wetting properties of water on silica surfaces

    NASA Astrophysics Data System (ADS)

    Pafong, E.; Geske, J.; Drossel, B.

    2016-09-01

    We study the wetting properties of water on silica surfaces using molecular dynamics (MD) simulations. To describe the intermolecular interaction between water and silica atoms, two types of interaction potential models are used: the standard BródkA and Zerda (BZ) model and the Gulmen and Thompson (GT) model. We perform an in-depth analysis of the influence of the choice of the potential on the arrangement of the water molecules in partially filled pores and on top of silica slabs. We find that at moderate pore filling ratios, the GT silica surface is completely wetted by water molecules, which agrees well with experimental findings, while the commonly used BZ surface is less hydrophilic and is only partially wetted. We interpret our simulation results using an analytical calculation of the phase diagram of water in partially filled pores. Moreover, an evaluation of the contact angle of the water droplet on top of the silica slab reveals that the interaction becomes more hydrophilic with increasing slab thickness and saturates around 2.5-3 nm, in agreement with the experimentally found value. Our analysis also shows that the hydroaffinity of the surface is mainly determined by the electrostatic interaction, but the van der Waals interaction nevertheless is strong enough that it can turn a hydrophobic surface into a hydrophilic surface.

  10. Recent characterization activities of Midway Valley as a potential repository surface facility site

    SciTech Connect

    Gibson, J.D.; Wesling, J.R.; Swan, F.H.; Bullard, T.F.

    1992-01-31

    Midway Valley, located at the eastern base of Yucca Mountain, Nye County, Nevada, has been identified as a possible location for the surface facilities of a potential high-level nuclear-waste repository. This structural and topographic valley is bounded by two north- trending, down-to-the-west normal faults: the Paintbrush Canyon fault on the east and the Bow Ridge fault on the west. Surface and near-surface geological data have been acquired from Midway Valley during the past three years with particular emphasis on evaluating the existence of Quaternary faults. A detailed (1:6000) surficial geological map has been prepared based on interpretation of new and existing aerial photographs, field mapping, soil pits, and trenches. No evidence was found that would indicate displacement of these surficial deposits along previously unrecognized faults. However, given the low rates of Quaternary faulting and the extensive areas that are covered by late Pleistocene to Holocene deposits south of Sever Wash, Quaternary faulting between known faults cannot be precluded based on surface evidence alone. Middle to late Pleistocene alluvial fan deposits (Unit Q3) exist at or near the surface throughout Midway Valley. Confidence is increased that the potential for surface fault rupture in Midway Valley can be assessed by excavations that expose the deposits and soils associated with Unit Q3 or older units (middle Pleistocene or earlier).

  11. Adiabatic shear bands localization in materials undergoing deformations

    NASA Astrophysics Data System (ADS)

    Ryabov, P. N.; Kudryashov, N. A.; Muratov, R. V.

    2017-01-01

    We consider the adiabatic shear banding phenomenon in composite materials undergoing the high speed shear deformations. The mathematical model of adiabatic shear banding in thermo-visco-plastic material is given. New two step numerical algorithm which is based on the Courant-Isaacson-Rees scheme that allows one to simulate fully localized plastic flow from initial stage of localization is proposed. To test this numerical algorithm we use three benchmark problems. The testing results show the accuracy and efficiency of proposed algorithm. The features of adiabatic shear bands formation in composites are studied. The existence of characteristic depth of localization in composites is shown. Influence of initial temperature distribution on the processes of adiabatic shear bands formation in composites is considered.

  12. 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.

  13. Ultrafast stimulated Raman parallel adiabatic passage by shaped pulses

    SciTech Connect

    Dridi, G.; Guerin, S.; Hakobyan, V.; Jauslin, H. R.; Eleuch, H.

    2009-10-15

    We present a general and versatile technique of population transfer based on parallel adiabatic passage by femtosecond shaped pulses. Their amplitude and phase are specifically designed to optimize the adiabatic passage corresponding to parallel eigenvalues at all times. We show that this technique allows the robust adiabatic population transfer in a Raman system with the total pulse area as low as 3{pi}, corresponding to a fluence of one order of magnitude below the conventional stimulated Raman adiabatic passage process. This process of short duration, typically picosecond and subpicosecond, is easily implementable with the modern pulse shaper technology and opens the possibility of ultrafast robust population transfer with interesting applications in quantum information processing.

  14. Adiabatic effects on nonlinear dust-acoustic solitary and shock waves in a strongly coupled dusty plasma

    SciTech Connect

    Rahman, M. S.; Mamun, A. A.

    2011-12-15

    A theoretical investigation has been performed on a strongly coupled dusty plasma containing strongly correlated negatively charged dust grains and weakly correlated adiabatic electrons and ions. The adiabatic effects on the dust-acoustic (DA) solitary and shock waves propagating in such a strongly coupled dusty plasma are taken into account. The DA solitary and shock waves are found to exist with negative potential only. It has been shown that the strong correlation among the charged dust grains is a source of dissipation and is responsible for the formation of the DA shock waves. It has also been found that the effects of adiabaticity significantly modify the basic features (e.g., amplitude, width, speed, etc.) of the DA solitary and shock waves. It has been suggested that a laboratory experiment be performed to test the theory presented in this work.

  15. Vulnerability of surface water bodies to potential contamination by ammunition residues from military training ranges

    NASA Astrophysics Data System (ADS)

    Tranquille Temgoua, André Guy; Martel, Richard; Gabriel, Uta; Furlan, Adriana; Jouveau, Marie-Juliette

    2014-05-01

    Over the last decade, a major effort has been made by Canadian Forces to understand the hydrodynamic of groundwater flow on range training areas (RTA). However, there is also a need to study surface water bodies and especially its vulnerability to potential contamination by ammunition residues. Nearly half of the surface (42%) of the studied RTA is located on bedrock prone to high rate of surface runoff. Rugged terrain is located to the north of the RTA, whereas to the south; the surface is on deltaic sediment made of sand that is favorable to high infiltration rate. Digital Elevation Models (DEMs) of topography were used in Geographic Information System (GIS) Software (ArcGis) to derive hydrologic processes. The GIS grid cells encompass basic terrain flow data that can be used to represent the flow processes at the free surface. They can also be used to derive a wide variety of information useful for the study of hydrologic processes such as topographic slope, water flow direction, contributing and drainage areas, catchments, watersheds and channel networks. The free surface flow was defined everywhere in the RTA but more specifically around targets locations, firing positions, and in impact areas. The developed methodology allows determining the hydrologic network with potential accumulation areas. The main objective is to identify areas where surficial geology and hydrological properties are favorable to rainfall-runoff and to establish if the quality of surface water may be altered by training ranges activities and subsequently if potential contaminants may migrate to receptors such as lakes and rivers. Vulnerable sectors that have high, medium or low rainfall-runoff index and surface water flow accumulation were shown on a regional map. Many other local maps were produced to define in more details surface water vulnerability in specific ranges. The possible relationship between the detection of ammunition residues in surface water bodies, the vulnerability

  16. Theoretical study of HCN-water interaction: five dimensional potential energy surfaces.

    PubMed

    Sánchez, Ernesto Quintas; Dubernet, Marie-Lise

    2017-03-01

    A new five-dimensional potential energy surface is calculated at the coupled-cluster CCSD(T) level of theory for the HCN-water system, treating both monomers as rigid rotors. The associated methodology, which combines extensive ab initio calculations of moderate accuracy (CCSD(T)/AVDZ) and a fitting procedure involving a much lower angular coverage with more accurate ab initio calculations (CCSD(T)/CBS), is described in detail. This methodology provides a time-saving approach to compute quantitatively accurate potential energy surfaces with reasonable computational effort. Our potential reproduces the main features reported in the literature, and will allow us to perform the first quantum and semi-classical simulations of the collisional dynamic on this system.

  17. Potential energy surface and bound states of the NH3-Ar and ND3-Ar complexes.

    PubMed

    Loreau, J; Liévin, J; Scribano, Y; van der Avoird, A

    2014-12-14

    A new, four-dimensional potential energy surface for the interaction of NH3 and ND3 with Ar is computed using the coupled-cluster method with single, double, and perturbative triple excitations and large basis sets. The umbrella motion of the ammonia molecule is explicitly taken into account. The bound states of both NH3-Ar and ND3-Ar are calculated on this potential for total angular momentum values from J = 0 to 10, with the inclusion of Coriolis interactions. The energies and splittings of the rovibrational levels are in excellent agreement with the extensive high-resolution spectroscopic data accumulated over the years in the infrared and microwave regions for both complexes, which demonstrates the quality of the potential energy surface.

  18. A "First Principles" Potential Energy Surface for Liquid Water from VRT Spectroscopy of Water Clusters

    SciTech Connect

    Goldman, N; Leforestier, C; Saykally, R J

    2004-05-25

    We present results of gas phase cluster and liquid water simulations from the recently determined VRT(ASP-W)III water dimer potential energy surface. VRT(ASP-W)III is shown to not only be a model of high ''spectroscopic'' accuracy for the water dimer, but also makes accurate predictions of vibrational ground-state properties for clusters up through the hexamer. Results of ambient liquid water simulations from VRT(ASP-W)III are compared to those from ab initio Molecular Dynamics, other potentials of ''spectroscopic'' accuracy, and to experiment. The results herein represent the first time that a ''spectroscopic'' potential surface is able to correctly model condensed phase properties of water.

  19. 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.

  20. 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.