arXiv subjects

Burkhard Schmidt

Publications and source records attributed to Burkhard Schmidt.

At least 37 records · Page 2Linked to original sources

arXiv2019

WavePacket: A Matlab package for numerical quantum dynamics. III: Quantum-classical simulations and surface hopping trajectories

WavePacket is an open-source program package for numerical simulations in quantum dynamics. Building on the previous Part I [Comp. Phys. Comm. 213, 223-234 (2017)] and Part II [Comp. Phys. Comm. 228, 229-244 (2018)] which dealt with quantum dynamics of closed and open systems, respectively, the present Part III adds fully classical and mixed quantum-classical propagations to WavePacket. In those simulations classical phase-space densities are sampled by trajectories which follow (diabatic or adiabatic) potential energy surfaces. In the vicinity of (genuine or avoided) intersections of those surfaces trajectories may switch between surfaces. To model these transitions, two classes of stochastic algorithms have been implemented: (1) J. C. Tully's fewest switches surface hopping and (2) Landau-Zener based single switch surface hopping. The latter one offers the advantage of being based on adiabatic energy gaps only, thus not requiring non-adiabatic coupling information any more. The present work describes the MATLAB version of WavePacket 6.0.2 which is essentially an object-oriented rewrite of previous versions, allowing to perform fully classical, quantum-classical and quantum-mechanical simulations on an equal footing, i.e., for the same physical system described by the same WavePacket input. The software package is hosted and further developed at the Sourceforge platform, where also extensive Wiki-documentation as well as numerous worked-out demonstration examples with animated graphics are available.

physics.comp-ph↗

arXiv2019

Two-Dimensional Water in Graphene Nanocapillaries Simulated with Different Force Fields: Rhombic Versus Square Structures, Proton Ordering, and Phase Transitions

Hydrogen bond patterns, proton ordering, and phase transitions of monolayer ice in two-dimensional hydrophobic confinement are fundamentally different from those found for bulk ice. To investigate the behavior of quasi-2D ice, we perform molecular dynamics simulations of water confined between fixed graphene plates at a distance of 0.65 nm. While experimental results are still limited and theoretical investigations are often based on a single force field model, this work presents a systematic study using different water force fields, i.e. SPCE, TIP3P, TIP4P, TIP4P/ICE, TIP5P. The water occupancy of the graphene capillary at a pressure of 1000 MPa is determined to be between 13.5 and 13.9 water molecules per square nanometer, depending on the choice of the water force field. To ensure complete sampling of the configurational space and to overcome barriers separating metastable structures, these simulations are based on the replica exchange molecular dynamics technique. We report different tetragonal hydrogen bond patterns which are classified as nearly square or as rhombic. While many of these arrangements are flat, in some cases puckered arrangements are found, too. Also the proton ordering of the quasi-2D water structures is considered, allowing to identify them as ferroelectric, ferrielectric or antiferroelectric. For temperatures between 200 K and 400 K we find several second-order phase transitions from one ice structure to another, changing in many cases both the arrangements of the oxygen atoms and the proton ordering. For temperatures between 400 K and 600 K there are melting-like transitions from a monolayer of ice to a monolayer of liquid water. These first-order phase transitions have a latent heat between 3.4 and 4.0 kJ/mol.

physics.chem-ph↗

arXiv2018

Electron Spin Resonance on the spin-1/2 triangular magnet NaYbS2

The delafossite structure of NaYbS2 contains a planar spin-1/2 triangular lattice of Yb3+ ions and features a possible realisation of a quantum spin-liquid state. We investigated the Yb3+ spin dynamics by Electron Spin Resonance (ESR) in single-crystalline samples of NaYbS2. Very clear spectra with a well-resolved and large anisotropy could be observed down to the lowest accessible temperature of 2.7 K. In contrast to the ESR properties of other known spin-liquid candidate systems, the resonance seen in NaYbS2 is accessible at low fields (< 1T) and is narrow enough for accurate characterisation of the relaxation rate as well as the g factor of the Yb3+ spins.

cond-mat.str-el↗

arXiv2018

Dynamics of polar polarizable rotors acted upon by unipolar electromagnetic pulses: From the sudden to the adiabatic regime

We study, analytically as well as numerically, the dynamics that arises from the interaction of a polar polarizable rigid rotor with single unipolar electromagnetic pulses of varying length, $Δτ$, with respect to the rotational period of the rotor, $τ_r$. In the sudden, non-adiabatic limit, $Δτ\ll τ_r$, we derive analytic expressions for the rotor's wavefunctions, kinetic energies, and field-free evolution of orientation and alignment. We verify the analytic results by solving the corresponding time-dependent Schrödinger equation numerically and extend the temporal range of the interactions considered all the way to the adiabatic limit, $Δτ\gg τ_r$, where general analytic solutions beyond the field-free case are no longer available. The effects of the orienting and aligning interactions as well as of their combination on the post-pulse populations of the rotational states are visualized as functions of the orienting and aligning kick strengths in terms of populations quilts. Quantum carpets that encapsulate the evolution of the rotational wavepackets provide the space-time portraits of the resulting dynamics. The population quilts and quantum carpets reveal that purely orienting, purely aligning, or even-break combined interactions each exhibit a sui generis dynamics. In the intermediate temporal regime, we find that the wavepackets as functions of the orienting and aligning kick strengths show resonances that correspond to diminished kinetic energies at particular values of the pulse duration.

quant-ph↗

arXiv2018

Symmetric Tops Subject to Combined Electric Fields: Conditional Quasi-Solvability via the Quantum Hamilton-Jacobi Theory

We make use of the Quantum Hamilton-Jacobi (QHJ) theory to investigate conditional quasi-solvability of the quantum symmetric top subject to combined electric fields (symmetric top pendulum). We derive the conditions of quasi-solvability of the time-independent Schroedinger equation as well as the corresponding finite sets of exact analytic solutions. We do so for this prototypical trigonometric system as well as for its anti-isospectral hyperbolic counterpart. An examination of the algebraic and numerical spectra of these two systems reveals mutually closely related patterns. The QHJ approach allows to retrieve the closed-form solutions for the spherical and planar pendula and the Razavy system that had been obtained in our earlier work via Supersymmetric Quantum Mechanics as well as to find a cornucopia of additional exact analytic solutions.

math-ph↗

arXiv2018

WavePacket: A Matlab package for numerical quantum dynamics. II: Open quantum systems, optimal control, and model reduction

WavePacket is an open-source program package for numeric simulations in quantum dynamics. It can solve time-independent or time-dependent linear Schrödinger and Liouville-von Neumann-equations in one or more dimensions. Also coupled equations can be treated, which allows, e.g., to simulate molecular quantum dynamics beyond the Born-Oppenheimer approximation. Optionally accounting for the interaction with external electric fields within the semi-classical dipole approximation, WavePacket can be used to simulate experiments involving tailored light pulses in photo-induced physics or chemistry. Being highly versatile and offering visualization of quantum dynamics 'on the fly', WavePacket is well suited for teaching or research projects in atomic, molecular and optical physics as well as in physical or theoretical chemistry. Building on the previous Part I which dealt with closed quantum systems and discrete variable representations, the present Part II focuses on the dynamics of open quantum systems, with Lindblad operators modeling dissipation and dephasing. This part also describes the WavePacket function for optimal control of quantum dynamics, building on rapid monotonically convergent iteration methods. Furthermore, two different approaches to dimension reduction implemented in WavePacket are documented here. In the first one, a balancing transformation based on the concepts of controllability and observability Gramians is used to identify states that are neither well controllable nor well observable. Those states are either truncated or averaged out. In the other approach, the H2-error for a given reduced dimensionality is minimized by H2 optimal model reduction techniques, utilizing a bilinear iterative rational Krylov algorithm.

quant-ph↗

arXiv2017

Néel temperature and reentrant H-T phase diagram of quasi-2D frustrated magnets

In quasi-2D quantum magnets the ratio of Néel temperature $T_\text N$ to Curie-Weiss temperature $Θ_\text{CW}$ is frequently used as an empirical criterion to judge the strength of frustration. In this work we investigate how these quantities are related in the canonical quasi-2D frustrated square or triangular $J_1$-$J_2$ model. Using the self-consistent Tyablikov approach for calculating $T_\text N$ we show their dependence on the frustration control parameter $J_2/J_1$ in the whole Néel and columnar antiferromagnetic phase region. We also discuss approximate analytical results. In addition the field dependence of $T_\text N(H)$ and the associated possible reentrance behavior of the ordered moment due to quantum fluctuations is investigated. These results are directly applicable to a class of quasi-2D oxovanadate antiferromagnets. We give clear criteria to judge under which conditions the empirical frustration ratio $f=Θ_\text{CW}/T_\text N$ may be used as measure of frustration strength in the quasi-2D quantum magnets.

cond-mat.str-el↗

arXiv2017

Frustrated two dimensional quantum magnets

We overview physical effects of exchange frustration and quantum spin fluctuations in (quasi-) two dimensional (2D) quantum magnets ($S=1/2$) with square, rectangular and triangular structure. Our discussion is based on the $J_1$-$J_2$ type frustrated exchange model and its generalizations. These models are closely related and allow to tune between different phases, magnetically ordered as well as more exotic nonmagnetic quantum phases by changing only one or two control parameters. We survey ground state properties like magnetization, saturation fields, ordered moment and structure factor in the full phase diagram as obtained from numerical exact diagonalization computations and analytical linear spin wave theory. We also review finite temperature properties like susceptibility, specific heat and magnetocaloric effect using the finite temperature Lanczos method. This method is powerful to determine the exchange parameters and g-factors from experimental results. We focus mostly on the observable physical frustration effects in magnetic phases where plenty of quasi-2D material examples exist to identify the influence of quantum fluctuations on magnetism.

cond-mat.str-el↗

arXiv2017

Model reduction of controlled Fokker--Planck and Liouville-von Neumann equations

Model reduction methods for bilinear control systems are compared by means of practical examples of Liouville-von Neumann and Fokker--Planck type. Methods based on balancing generalized system Gramians and on minimizing an H2-type cost functional are considered. The focus is on the numerical implementation and a thorough comparison of the methods. Structure and stability preservation are investigated, and the competitiveness of the approaches is shown for practically relevant, large-scale examples.

math.NA↗

arXiv2017

Conditional quasi-exact solvability of the quantum planar pendulum and of its anti-isospectral hyperbolic counterpart

We have subjected the planar pendulum eigenproblem to a symmetry analysis with the goal of explaining the relationship between its conditional quasi-exact solvability (C-QES) and the topology of its eigenenergy surfaces, established in our earlier work [Frontiers in Physical Chemistry and Chemical Physics 2, 1-16, (2014)]. The present analysis revealed that this relationship can be traced to the structure of the tridiagonal matrices representing the symmetry-adapted pendular Hamiltonian, as well as enabled us to identify many more -- forty in total to be exact -- analytic solutions. Furthermore, an analogous analysis of the hyperbolic counterpart of the planar pendulum, the Razavy problem, which was shown to be also C-QES [American Journal of Physics 48, 285 (1980)], confirmed that it is anti-isospectral with the pendular eigenproblem. Of key importance for both eigenproblems proved to be the topological index $κ$, as it determines the loci of the intersections (genuine and avoided) of the eigenenergy surfaces spanned by the dimensionless interaction parameters $η$ and $ζ$. It also encapsulates the conditions under which analytic solutions to the two eigenproblems obtain and provides the number of analytic solutions. At a given $κ$, the anti-isospectrality occurs for single states only (i.e., not for doublets), like C-QES holds solely for integer values of $κ$, and only occurs for the lowest eigenvalues of the pendular and Razavy Hamiltonians, with the order of the eigenvalues reversed for the latter. For all other states, the pendular and Razavy spectra become in fact qualitatively different, as higher pendular states appear as doublets whereas all higher Razavy states are singlets.

quant-ph↗

arXiv2017

Hydrodynamic Electron Flow and Hall Viscosity

In metallic samples of small enough size and sufficiently strong momentum-conserving scattering, the viscosity of the electron gas can become the dominant process governing transport. In this regime, momentum is a long-lived quantity whose evolution is described by an emergent hydrodynamical theory. Furthermore, breaking time-reversal symmetry leads to the appearance of an odd component to the viscosity called the Hall viscosity, which has attracted considerable attention recently due to its quantized nature in gapped systems but still eludes experimental confirmation. Based on microscopic calculations, we discuss how to measure the effects of both the even and odd components of the viscosity using hydrodynamic electronic transport in mesoscopic samples under applied magnetic fields.

cond-mat.str-el↗

arXiv2016

WavePacket: A Matlab package for numerical quantum dynamics. I: Closed quantum systems and discrete variable representations

WavePacket is an open-source program package for the numerical simulation of quantum-mechanical dynamics. It can be used to solve time-independent or time-dependent linear Schrödinger and Liouville-von Neumann-equations in one or more dimensions. Also coupled equations can be treated, which allows to simulate molecular quantum dynamics beyond the Born-Oppenheimer approximation. Optionally accounting for the interaction with external electric fields within the semiclassical dipole approximation, WavePacket can be used to simulate experiments involving tailored light pulses in photo-induced physics or chemistry.The graphical capabilities allow visualization of quantum dynamics 'on the fly', including Wigner phase space representations. Being easy to use and highly versatile, WavePacket is well suited for the teaching of quantum mechanics as well as for research projects in atomic, molecular and optical physics or in physical or theoretical chemistry.The present Part I deals with the description of closed quantum systems in terms of Schrödinger equations. The emphasis is on discrete variable representations for spatial discretization as well as various techniques for temporal discretization.The upcoming Part II will focus on open quantum systems and dimension reduction; it also describes the codes for optimal control of quantum dynamics.The present work introduces the MATLAB version of WavePacket 5.2.1 which is hosted at the Sourceforge platform, where extensive Wiki-documentation as well as worked-out demonstration examples can be found.

quant-ph↗

arXiv2016

CePdAl - a Kondo lattice with partial frustration

Magnetic frustration, which is well-defined in insulating systems with localized magnetic moments, yields exotic ground states like spin ices, spin glasses, or spin liquids. In metals magnetic frustration is less well defined because of the incipient delocalization of magnetic moments by the interaction with conduction electrons, viz., the Kondo effect. Hence, the Kondo effect and magnetic frustration are antithetic phenomena. Here we present experimental data of electrical resistivity, magnetization, specific heat and neutron diffraction on CePdAl, which is one of the rare examples of a geometrically frustrated Kondo lattice, demonstrating that the combination of Kondo effect and magnetic frustration leads to an unusual ground state.

cond-mat.str-el↗

arXiv2016

Curvature-dependent adsorption of water inside and outside armchair carbon nanotubes

The curvature dependence of the physisorption properties of a water molecule inside and outside an armchair carbon nanotube (CNTs) is investigated by an incremental density-fitting local coupled cluster treatment with single and double excitations and perturbative triples (DF-LCCSD(T)) study. Our results show that a water molecule outside and inside (n, n) CNTs (n=4, 5, 6, 7, 8, 10) is stabilized by electron correlation. The adsorption energy of water inside CNTs decreases quickly with the decrease of curvature (increase of radius) and the configuration with the oxygen pointing towards the CNT wall is the most stable one. However, when the water molecule is adsorbed outside the CNT, the adsorption energy varies only slightly with the curvature and the configuration with hydrogens pointing towards the CNT wall is the most stable one. We also use the DF-LCCSD(T) results to parametrize Lennard-Jones (LJ) force fields for the interaction of water both with the inner and outer sides of CNTs and with graphene representing the zero curvature limit. It is not possible to reproduce all DF-LCCSD(T) results for water inside and outside CNTs of different curvature by a single set of LJ parameters, but two sets have to be used instead. Each of the two resulting sets can reproduce three out of four minima of the effective potential curves reasonably well. These LJ models are then used to calculate the water adsorption energies of larger CNTs, approaching the graphene limit, thus bridging the gap between CNTs of increasing radius and flat graphene sheets.

physics.chem-ph↗

arXiv2016

Evidence for hydrodynamic electron flow in PdCoO$_2$

Electron transport is conventionally determined by the momentum-relaxing scattering of electrons by the host solid and its excitations. The electrical resistance is set by geometrical factors and the resistivity, which is a microscopic property of the solid. Hydrodynamic fluid flow through channels, in contrast, is determined by geometrical factors, boundary scattering and the viscosity of the fluid, which is governed by momentum-conserving internal collisions. A long-standing question in the physics of solids, brought into focus by the advent of new calculational techniques, has been whether the viscosity of the electron fluid plays an observable role in determining the resistance. At first sight this seems unlikely, because in almost all known materials the rate of momentum-relaxing collisions dominates that of the momentum-conserving ones that give the viscous term. Here, we show this is not always the case. We report experimental evidence that the resistance of restricted channels of the ultra-pure two-dimensional metal PdCoO$_2$ has a large viscous contribution. Comparison with theory allows an estimate of the electronic viscosity in the range between $6\times 10^{-3}$~kg(ms)$^{-1}$ and $3\times 10^{-4}$~kg(ms)$^{-1}$, which brackets that of water at room temperature.

cond-mat.str-el↗

arXiv2015

Thermodynamics of anisotropic triangular magnets with ferro- and antiferromagnetic exchange

We investigate thermodynamic properties like specific heat $c_{V}$ and susceptibility $χ$ in anisotropic $J_1$-$J_2$ triangular quantum spin systems ($S=1/2$). As a universal tool we apply the finite temperature Lanczos method (FTLM) based on exact diagonalization of finite clusters with periodic boundary conditions. We use clusters up to $N=28$ sites where the thermodynamic limit behavior is already stably reproduced. As a reference we also present the full diagonalization of a small eight-site cluster. After introducing model and method we discuss our main results on $c_V(T)$ and $χ(T)$. We show the variation of peak position and peak height of these quantities as function of control parameter $J_2/J_1$. We demonstrate that maximum peak positions and heights in Néel phase and spiral phases are strongly asymmetric, much more than in the square lattice $J_1$-$J_2$ model. Our results also suggest a tendency to a second side maximum or shoulder formation at lower temperature for certain ranges of the control parameter. We finally explicitly determine the exchange model of the prominent triangular magnets Cs$_2$CuCl$_4$ and Cs$_{2}$CuBr$_{4}$ from our FTLM results.

cond-mat.str-el↗

arXiv2015

Supersymmetry and eigensurface topology of the spherical quantum pendulum

We undertook a mutually complementary analytic and computational study of the full-fledged spherical (3D) quantum rotor subject to combined orienting and aligning interactions characterized, respectively, by dimensionless parameters $η$ and $ζ$. By making use of supersymmetric quantum mechanics (SUSY QM), we found two sets of conditions under which the problem of a spherical quantum pendulum becomes analytically solvable. These conditions coincide with the loci $ζ=\frac{η^2}{4k^2}$ of the intersections of the eigenenergy surfaces spanned by the $η$ and $ζ$ parameters. The integer topological index $k$ is independent of the eigenstate and thus of the projection quantum number $m$. These findings have repercussions for rotational spectra and dynamics of molecules subject to combined permanent and induced dipole interactions.

quant-ph↗

arXiv2014

Supersymmetry and eigensurface topology of the planar quantum pendulum

We make use of supersymmetric quantum mechanics (SUSY QM) to find three sets of conditions under which the problem of a planar quantum pendulum becomes analytically solvable. The analytic forms of the pendulum's eigenfuntions make it possible to find analytic expressions for observables of interest, such as the expectation values of the angular momentum squared and of the orientation and alignment cosines as well as of the eigenenergy. Furthermore, we find that the topology of the intersections of the pendulum's eigenenergy surfaces can be characterized by a single integer index whose values correspond to the sets of conditions under which the analytic solutions to the quantum pendulum problem exist.

physics.chem-ph↗