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Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Density Matrix Embedding TheorySep 18 2019We describe an efficient quantum embedding framework for realistic ab initio density matrix embedding (DMET) calculations in solids. We discuss in detail the choice of orbitals and mapping to a lattice, treatment of the virtual space and bath truncation, ... More

Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field TheorySep 18 2019We present an efficient ab initio dynamical mean-field theory (DMFT) implementation for quantitative simulations in solids. Our DMFT scheme employs ab initio Hamiltonians defined for impurities comprising the full unit cell or a supercell of atoms and ... More

Construction of Machine Learned Force Fields with Quantum Chemical Accuracy: Applications and Chemical InsightsSep 18 2019Highly accurate force fields are a mandatory requirement to generate predictive simulations. Here we present the path for the construction of machine learned molecular force fields by discussing the hierarchical pathway from generating the dataset of ... More

Sparking mashups to multifunctional alloy nanoparticlesSep 17 2019High-entropy alloy nanoparticle (HEA-NP) synthesis is challenging due to the seamless kinetic and thermodynamic interactions. Herein, we report that spark ablation, a rapidly quenched vapor source, creates 55 distinct types of ultrasmall alloy NPs with ... More

Single Photon Emission from a Plasmonic Light Source Driven by a Local Field-Induced Coulomb BlockadeSep 17 2019A hallmark of quantum control is the ability to make photons at the nanoscale whose temporal features are distinct from classical light sources. Through scanning tunneling microscopy induced luminescence (STML) we are able to generate plasmonic light ... More

Machine Learning Potential Energy SurfacesSep 17 2019Machine Learning techniques can be used to represent high-dimensional potential energy surfaces for reactive chemical systems. Two such methods are based on a reproducing kernel Hilbert space representation or on deep neural networks. They can achieve ... More

Graph Nets for Partial Charge PredictionSep 17 2019Atomic partial charges are crucial parameters for Molecular Dynamics (MD) simulations, molecular mechanics calculations, and virtual screening, as they determine the electrostatic contributions to interaction energies. Current methods for calculating ... More

Theoretical description of the ionization processes with a discrete basis set representation of the electronic continuumSep 17 2019In this work we present a new method of approximating the continuum wavefunctions with a discrete basis set. This method aims to be at least compatible with other well known methods of the electronic structure theory to describe processes in the electronic ... More

Time Dependent Adaptive Configuration Interaction Applied to Attosecond Charge MigrationSep 17 2019In this work, we present a time-dependent (TD) selected configuration interaction method based on our recently-introduced adaptive configuration interaction (ACI). We show that ACI, in either its ground or excited state formalisms, is capable of building ... More

Probability based enhanced samplingSep 17 2019Many physical and chemical processes of interest take place on timescales that cannot be explored using standard molecular dynamics simulations. This renders the use of enhanced sampling mandatory. Here we introduce an enhanced sampling method that is ... More

Probability distribution of the boundary local time of reflected Brownian motion in Euclidean domainsSep 17 2019How long does a diffusing molecule spend in a close vicinity of a confining boundary or a catalytic surface? This quantity known as the boundary local time plays the crucial role in the description of various surface-mediated phenomena such as heterogeneous ... More

Excess Thermal Energy and Latent Heat in Nanocluster Collisional GrowthSep 16 2019Nanoclusters can form and grow by nanocluster-monomer (condensation) and nanocluster-nanocluster (coagulation) collisions. During growth, product nanoclusters have elevated thermal energies due to potential and thermal energy exchange following a collision. ... More

Attosecond Transient Absorption Spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopySep 16 2019The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray ... More

Embedding via the Exact Factorization ApproachSep 16 2019We present a quantum electronic embedding method derived from the exact factorization approach to calculate static properties of a many-electron system. The method is exact in principle but the practical power lies in utilizing input from a low-level ... More

Tannin-controlled micelles and fibrils of $κ$-caseinSep 16 2019Effects of green tea tannin epigallocatechin-gallate (EGCG) on thermal-stress-induced amyloid fibril formation of reduced carboxymethylated bovine milk protein $\kappa$-casein (RCMK) were studied by dynamical light scattering (DLS) and small angle x-rays ... More

Computing spatially resolved rotational hydration entropies from atomistic simulationsSep 16 2019For a first principles understanding of macromolecular processes, a quantitative understanding of the underlying free energy landscape and in particular its entropy contribution is crucial. The stability of biomolecules, such as proteins, is governed ... More

Derivation of a Local Volume-Averaged Model and a Stable Numerical Algorithm for Multi-Dimensional Simulations of Conversion BatteriesSep 16 2019In this article, we derive a general form of local volume-averaging theory and apply it to a model of zinc-air conversion batteries. Volume-averaging techniques are frequently used for the macroscopic description of micro-porous electrodes. We extend ... More

RPA natural orbitals and their application to post-Hartree-Fock electronic structure methodsSep 16 2019We present a method to approximate post-Hartree-Fock correlation energies by using approximate natural orbitals obtained by the random phase approximation (RPA). We demonstrate the method by applying it to the helium atom, the hydrogen and fluorine molecule, ... More

RPA natural orbitals and their application to post-Hartree-Fock electronic structure methodsSep 16 2019Sep 17 2019We present a method to approximate post-Hartree-Fock correlation energies by using approximate natural orbitals obtained by the random phase approximation (RPA). We demonstrate the method by applying it to the helium atom, the hydrogen and fluorine molecule, ... More

Ultraslow radiative cooling of C$_n^-$ ($n=3-5$)Sep 16 2019Ultraslow radiative cooling lifetimes and adiabatic detachment energies for three astrochemically relevant anions, C$_n^-$ ($n=3-5$), are measured using the Double ElectroStatic Ion Ring ExpEriment (DESIREE) infrastructure at Stockholm University. DESIREE ... More

Multireference configuration interaction and perturbation theory without reduced density matricesSep 16 2019The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wavefunctions in large active spaces. We present a stochastic formulation ... More

Enantio-discrimination via light deflection effectSep 16 2019We propose a theoretical method for enantio-discrimination based on the light deflection effect in four-level models of chiral molecules. This four-level model consists of a cyclic three-level subsystem coupled by three strong driving fields and an auxiliary ... More

Global optimization of parameters in the reactive force field ReaxFF for SiOHSep 15 2019We have used unbiased global optimization to fit a reactive force field to a given set of reference data. Specifically, we have employed genetic algorithms (GA) to fit ReaxFF to SiOH data, using an in-house GA code that is parallelized across reference ... More

Compelling alternative theories for exclusion zone phenomena in water and other liquidsSep 15 2019The existence of the exclusion zone (EZ), a layer of water in which plastic microspheres are repelled from hydrophilic surfaces, has now been independently demonstrated by several groups. A better understanding of the mechanisms which generate EZs would ... More

How to learn from inconsistencies: Integrating molecular simulations with experimental dataSep 15 2019Molecular simulations and biophysical experiments can be used to provide independent and complementary insights into the molecular origin of biological processes. A particularly useful strategy is to use molecular simulations as a modelling tool to interpret ... More

Systematic Microsolvation Approach with a Cluster-Continuum Scheme and Conformational SamplingSep 14 2019Solvation is a notoriously difficult and nagging problem for the rigorous theoretical description of chemistry in the liquid phase. Successes and failures of various approaches ranging from implicit solvation modeling through dielectric continuum embedding ... More

Direct detection of polar structure formation in helium nanodroplets by beam deflection measurementsSep 14 2019Long-range intermolecular forces are able to steer polar molecules submerged in superfluid helium nanodroplets into highly polar metastable configurations. We demonstrate that the presence of such special structures can be identified, in a direct and ... More

Stochastic Resolution of Identity for Real-Time Second-Order Green's Function: Ionization Potential and Quasi-particle SpectrumSep 14 2019We develop a stochastic resolution of identity approach to the real-time second-order Green's function (real-time sRI-GF2) theory, extending our recent work for imaginary-time Matsubara Green's function {\em J. Chem. Phys.} {\bf 151}, 044114 (2019)). ... More

Quantum simulations of excited states with active-space downfolded HamiltoniansSep 13 2019Many-body techniques based on the double unitary coupled cluster ansatz (DUCC) can be used to downfold electronic Hamiltonians into low-dimensional active spaces. It can be shown that the resulting dimensionality reduced Hamiltonians are amenable for ... More

Numerical analysis of polymer diffusiophoresis by means of the molecular dynamicsSep 13 2019We report a numerical study of the diffusiophoresis of short polymers using non-equilibrium molecular dynamics simulations. More precisely, we consider polymer chains in a fluid containing a solute which has a concentration gradient, and examine the variation ... More

Efficient evaluation of AGP reduced density matricesSep 13 2019We propose and implement an algorithm to calculate the norm and reduced density matrices of the antisymmetrized geminal power (AGP) of any rank with polynomial cost. Our method scales quadratically per element of the reduced density matrices. Numerical ... More

Low-energy electron escape from liquid interfaces: charge and quantum effectsSep 13 2019The high surface sensitivity and controlled surface charge state of submicron sized droplets is exploited to study low-energy electron transport through liquid interfaces using photoelectron imaging. Already a few charges on a droplet are found to modify ... More

Ring Polymer Molecular Dynamics and Active Learning of Moment Tensor Potential for Gas-Phase Barrierless Reactions: Application to S + H2Sep 13 2019Ring polymer molecular dynamics (RPMD) has proven to be an accurate approach for calculating thermal rate coefficients of various chemical reactions. For wider application of this methodology, efficient ways to generate the underlying full-dimensional ... More

A sustainable, clean and efficient pathway to obtaining ethyl-esters of volatile fatty acids through the use of aluminium chloride hexahydrateSep 13 2019A new process for obtaining ethyl-esters of volatile fatty acids with ethanol is proposed by using aluminium chloride hexahydrate as a catalyst. Besides a good activity, since thermodynamic conversion of volatile fatty acids was achieved already after ... More

The Rising Sun Envelope Method: an automatic and accurate peak location technique for XANES measurementsSep 13 2019The lack of theoretical understanding of X-Ray Absorption Near Edge Structure (XANES) spectroscopy makes the development of analysis tools for its study a necessity. Here, an algorithm for judicious choice of local minima and maxima points of XANES spectrum ... More

Prediction of many-electron wavefunctions using atomic potentials: extended basis sets and molecular dissociationSep 12 2019A one-electron Schroedinger equation based on special one-electron potentials for atoms is shown to exist that produces orbitals for an arbitrary molecule that are sufficiently accurate to be used without modification to construct single- and multi-determinant ... More

Effect of surface morphology on kinetic compensation effectSep 12 2019As part of a systematic study on the kinetic compensation effect, we use kinetic Monte Carlo simulations to observe the effects of substrate topology on the transient variations in the Arrhenius parameters - effective activation energy $E_{a}$, and preexponential ... More

Threshold dissociation of the 1-ethynylpyrene cation at internal energies relevant to H I regionsSep 12 2019Photoelectron photoion coincidence spectroscopy has been used to measure the threshold photoelectron spectrum of 1-ethynylpyrene and to obtain the breakdown graph describing the dissociation of the 1-ethynylpyrene cation. The threshold photoelectron measurement ... More

Quantifying Doping Levels in Carbon Nanotubes by Optical SpectroscopySep 11 2019Controlling doping is essential for a successful integration of semiconductor materials into device technologies. However, the assessment of doping levels and the distribution of charge carriers in carbon nanotubes or other nanoscale semiconductor materials ... More

Symmetry-restricted functionals in one-body reduced density matrix functional theorySep 11 2019In many of the approximate functionals in one-body reduced density matrix (1RDM) functional theory, the approximate two-body reduced density matrix (2RDM) in the natural orbital representation only depends on the natural occupation numbers. In Phys. Rev. ... More

Flux-conserving diagrammatic formulation of optical spectroscopy of open quantum systemsSep 11 2019We present a theoretical approach to optical spectroscopy of open nonequilibrium systems, which generalizes traditional nonlinear optical spectroscopy tools by imposing charge and energy conservation at all levels of approximation. Both molecular and ... More

Estimating configurational entropy and energy of molecular systems from computed spectral densitySep 10 2019Most methods for estimating configurational entropy from molecular simulation data yield upper limits except for harmonic systems where they are exact. Problems arise at diffusive systems and the presence of conformational transitions. Covariance-based ... More

Controlling sub-cycle electron dynamics with plasmonic bichromatic counter-rotating circularly polarised fieldsSep 10 2019The use of bi-chromatic counter-rotating laser field is known to generate high-order harmonics with non-zero ellipticity. By combining such a laser pulse with a plasmonic field, we propose a way to influence the sub-cycle dynamics of the high-harmonic ... More

Hot Carrier Mobility Dynamics Unravel Competing Sub-ps Cooling Processes in Lead Halide PerovskitesSep 10 2019The outstanding photovoltaic performances of lead halide perovskite (LHP) thin film solar cells are due in particular to the large diffusion length of photocarriers. The mechanism behind this property and its dependence on the various anions and cations ... More

Incorporating long-range physics in atomic-scale machine learningSep 10 2019The most successful and popular machine learning models of atomic-scale properties derive their transferability from a locality ansatz. The properties of a large molecule or a bulk material are written as a sum over contributions that depend on the configurations ... More

Enhanced solvation force extrapolation for speeding up molecular dynamics simulations of complex biochemical liquidsSep 10 2019We propose an enhanced approach to the extrapolation of mean potential forces acting on atoms of solute macromolecules due to their interactions with solvent atoms in complex biochemical liquids. It improves and extends previous extrapolation schemes ... More

Adiabatic Elimination and Sub-space Evolution of Open Quantum SystemsSep 10 2019Efficient descriptions of open quantum systems can be obtained by performing an adiabatic elimination of the fast degrees of freedom and formulating effective operators for the slow degrees of freedom in reduced dimensions. Here, we perform the construction ... More

Adiabatic Elimination and Sub-space Evolution of Open Quantum SystemsSep 10 2019Sep 11 2019Efficient descriptions of open quantum systems can be obtained by performing an adiabatic elimination of the fast degrees of freedom and formulating effective operators for the slow degrees of freedom in reduced dimensions. Here, we perform the construction ... More

The Making Of A Theory Of The Vitreous Solid State: From 1 milli-K To 1 kilo-KSep 09 2019This is a short account of the basic principles of a comprehensive theory of the vitreous state, looking at glasses and their eventual <<melting>> into a liquid state (the inverse glass <<transition>>) from the perspective of their low-temperature properties, ... More

Symmetry in Multiple Self-Consistent-Field Solutions of Transition-Metal ComplexesSep 09 2019We use a method based on metadynamics to locate multiple low-energy Unrestricted Hartree--Fock (UHF) self-consistent-field (SCF) solutions of two model octahedral $d^1$ and $d^2$ transition-metal complexes, $[\mathrm{MF}_6]^{3-} (\mathrm{M} = \mathrm{Ti}, ... More

Step edge-mediated assembly of periodic arrays of long graphene nanoribbons on Au(111)Sep 09 2019The influence of substrate steps on the bottom-up synthesis of atomically precise graphene nanoribbons (GNRs) on an Au(111) surface is investigated. A straight surface step is found to promote the assembly of long and compact arrays of polymers with enhanced ... More

Bayesian Design of Experiments: Implementation, Validation and Application to Chemical KineticsSep 09 2019Bayesian experimental design (BED) is a tool for guiding experiments founded on the principle of expected information gain. I.e., which experiment design will inform the most about the model can be predicted before experiments in a laboratory are conducted. ... More

Neural network interpolation of exchange-correlation functionalSep 09 2019Density functional theory (DFT) is one of the most widely used tools to solve the many-body Schrodinger equation. The core uncertainty inside DFT theory is the exchange-correlation (XC) functional, the exact form of which is still unknown. Therefore, ... More

Phoretic Active MatterSep 09 2019These notes are an account of a series of lectures given at the Les Houches Summer School ``Active Matter and Non-equilibrium Statistical Physics'' during August and September 2018. The lectures can be viewed online at [http://www.ds.mpg.de/lmp/lectures/les-houches-2018]. ... More

Accurate biomolecular simulations account for electronic polarizationSep 09 2019In this perspective, we discuss where and how accounting for electronic many-body polarization affects the accuracy of classical molecular dynamics simulations of biomolecules.While the effects of electronic polarization are highly pronounced for molecules ... More

Variational control forces for enhanced sampling of nonequilibrium molecular dynamics simulationsSep 09 2019We introduce a variational algorithm to estimate the likelihood of a rare event within a nonequilibrium molecular dynamics simulation through the evaluation of an optimal control force. Optimization of a control force within a chosen basis is made possible ... More

Synergistic Effect of One- and Two-dimensional Connected Coral-like Li$_{6.25}$Al$_{0.25}$La$_3$Zr$_2$O$_{12}$ in PEO-Based Composite Solid State ElectrolyteSep 07 2019As one of the most promising next-generation energy storage device, lithium metal batteries have been extensively investigated. However, the poor safety issue and undesired lithium dendrites growth hinder the development of lithium metal batteries. The ... More

Ultrafast long-range energy transport via light-matter coupling in organic semiconductor filmsSep 07 2019The formation of exciton-polaritons allows the transport of energy over hundreds of nanometres at velocities up to 10^6 m s^-1 in organic semiconductors films in the absence of external cavity structures.

Orientational instability and spontaneous rotation of active nematic dropletsSep 07 2019In experiments, an individual chemically active liquid crystal (LC) droplet submerged in the bulk of a surfactant solution may self-propel along a straight, helical, or random trajectory. In this paper, we develop a minimal model capturing all three types ... More

A Simplified Approach to Simulating Raman Spectra from Ab Initio Molecular DynamicsSep 06 2019We describe a simplified approach to simulating Raman spectra using ab initio molecular dynamics (AIMD) calculations. Our protocol relies on on-the-fly calculations of approximate molecular polarizabilities using a sum over orbitals (as opposed to states) ... More

Spectroscopic assessment of charge mobility in organic semiconductorsSep 06 2019Rapid progress in organic electronics demands new highly efficient organic semiconducting materials. Nevertheless, only few materials have been created so far that show reliable band-like transport with high charge mobilities, which reflects the two main ... More

Towards a background-free neutrinoless double beta decay experiment based on a fluorescent bicolor sensorSep 06 2019Neutrinoless double beta decay ($\beta\beta0\nu$) is a putative nuclear decay that can occur if, and only if, neutrinos are their own antiparticles. Due to the smallness of neutrino masses, the lifetime of $\beta\beta0\nu$ is expected to be larger than ... More

Towards a background-free neutrinoless double beta decay experiment based on a fluorescent bicolor sensorSep 06 2019Sep 14 2019Searching for neutrinoless double beta decays ($\beta\beta0\nu$) is the only practical way to establish if the neutrinos are their own antiparticles. Due to the smallness of neutrino masses, the lifetime of $\beta\beta0\nu$ is expected to be at least ... More

Towards a background-free neutrinoless double beta decay experiment based on a fluorescent bicolor sensorSep 06 2019Sep 09 2019Neutrinoless double beta decay ($\beta\beta0\nu$) is a putative nuclear decay that can occur if, and only if, neutrinos are their own antiparticles. Due to the smallness of neutrino masses, the lifetime of $\beta\beta0\nu$ is expected to be larger than ... More

Towards a background-free neutrinoless double beta decay experiment based on a fluorescent bicolor sensorSep 06 2019Sep 10 2019Neutrinoless double beta decay ($\beta\beta0\nu$) is a putative nuclear decay that can occur if, and only if, neutrinos are their own antiparticles. Due to the smallness of neutrino masses, the lifetime of $\beta\beta0\nu$ is expected to be larger than ... More

ExoMol molecular line lists XXXVI: $X\ {}^2Π- X\ {}^2Π$ and $A\ {}^2Σ^+ - X\ {}^2Π$ transitions of SHSep 05 2019The GYT line list covering rotational, rovibrational and rovibronic transitions of the mercapto radical SH is presented. This work extends and replaces the SNaSH line list [Yurchenko et al., 2018, MNRAS, 478, 270] which covers the ground (electronic) ... More

Accurate real-time evolution of electron densities and ground-state properties from generalized Kohn-Sham theorySep 05 2019The exact time-dependent Kohn-Sham (KS) exchange-correlation (xc) potential is not easily approximated due to its nonphysical properties; the burden of capturing xc effects solely within a multiplicative potential gives rise to pathological features, ... More

Ab-Initio Solution of the Many-Electron Schrödinger Equation with Deep Neural NetworksSep 05 2019Given access to accurate solutions of the many-electron Schr\"odinger equation, nearly all chemistry could be derived from first principles. Exact wavefunctions of interesting chemical systems are out of reach because they are NP-hard to compute in general, ... More

Polaritonic Coupled-Cluster TheorySep 05 2019We develop coupled-cluster theory for systems of electrons strongly coupled to photons, providing a promising theoretical tool in polaritonic chemistry with a perspective of application to all types of fermion-boson coupled systems. We show benchmark ... More

Self-learning Hybrid Monte Carlo: A First-principles ApproachSep 05 2019We propose a novel approach called Self-Learning Hybrid Monte Carlo (SLHMC) which is a general method to make use of machine learning potentials to accelerate the statistical sampling of first-principles density-functional-theory (DFT) simulations. The ... More

Triatomic butterfly moleculesSep 04 2019We detail the rich electronic and vibrational structure of triatomic "butterfly" molecules, ultra-long-range Rydberg molecules bound by resonant $p$-wave scattering. We divide these molecules into two sub-classes depending on their parity under reflection ... More

Making Many-Body Interactions Nearly Pairwise Additive: The Polarized Many-Body Expansion ApproachSep 04 2019The Many-Body Expansion (MBE) is a useful tool to simulate condensed phase chemical systems, often avoiding the steep computational cost of usual electronic structure methods. However, it often requires higher than 2-body terms to achieve quantitative ... More

Motion of objects embedded in lipid bilayer membranes: advection and effective viscositySep 04 2019An interfacial regularized Stokeslet scheme is presented to predict the motion of solid bodies (e.g. proteins or gel-phase domains) embedded within flowing lipid bilayer membranes. The approach provides a numerical route to calculate velocities and angular ... More

Regression-clustering for Improved Accuracy and Training Cost with Molecular-Orbital-BasedMachine LearningSep 04 2019Machine learning (ML) in the representation of molecular-orbital-based (MOB) features has been shown to be an accurate and transferable approach to the prediction of post-Hartree-Fock correlation energies. Previous applications of MOB-ML employed Gaussian ... More

Regression-clustering for Improved Accuracy and Training Cost with Molecular-Orbital-Based Machine LearningSep 04 2019Sep 06 2019Machine learning (ML) in the representation of molecular-orbital-based (MOB) features has been shown to be an accurate and transferable approach to the prediction of post-Hartree-Fock correlation energies. Previous applications of MOB-ML employed Gaussian ... More

Regression-clustering for Improved Accuracy and Training Cost with Molecular-Orbital-Based Machine LearningSep 04 2019Sep 09 2019Machine learning (ML) in the representation of molecular-orbital-based (MOB) features has been shown to be an accurate and transferable approach to the prediction of post-Hartree-Fock correlation energies. Previous applications of MOB-ML employed Gaussian ... More

FCHL revisited: faster and more accurate quantum machine learningSep 04 2019We introduce the FCHL19 representation for atomic environments in molecules or condensed-phase systems. Machine learning models based on FCHL19 are able to yield predictions of atomic forces and energies of query compounds with chemical accuracy on the ... More

Electrocrystallization of Supercooled Water Confined by Graphene WallsSep 04 2019Any structural transformation of water is sensitive to an external electric field, since water molecules have dipole moments. We study influence of external uniform electric field on crystallization of supercooled water enclosed between two graphene planes. ... More

Suppression of Penning ionization by orbital angular momentum conservationSep 04 2019The efficient suppression of Penning-ionizing collisions is a stringent requirement to achieve quantum degeneracy in metastable rare gases. Thus far, such loss processes have been avoided by electron-spin polarizing the collision partners. Here, we report ... More

Dissociation Energy of Molecular Hydrogen IsotopologuesSep 04 2019The nonrelativistic energy together with relativistic and quantum electrodynamic corrections for all the molecular hydrogen isotopologues (D$_2$, T$_2$, HD, HT, DT) were evaluated without expansion in the electron-nucleus mass ratio. The obtained results ... More

Self-consistent approach to the description of relaxation processes in classical multiparticle systemsSep 03 2019The concept of time correlation functions is a very convenient theoretical tool in describing relaxation processes in multiparticle systems because, on one hand, correlation functions are directly related to experimentally measured quantities (for example, ... More

Thermodynamic stability of droplets, bubbles and thick films in open and closed poresSep 03 2019A fluid in a pore can form diverse heterogeneous structures. We combine a capillary description with the cubic-plus-association equation of state to study the thermodynamic stability of droplets, bubbles and films of water at 358 K in a cylindrically ... More

Microwave heating and collapse of methane hydrate by molecular dynamics simulationsSep 03 2019Microwave heating of methane hydrate is investigated with electrostatic molecular dynamics simulations. The structure I of methane hydrate is constructed. When the methane hydrate with a density of 0.91 $\rm{g/cm}^3$ and temperature of 273 K is exposed ... More

Microwave heating and collapse of methane hydrate by molecular dynamics simulationsSep 03 2019Sep 05 2019Microwave heating of methane hydrate is investigated with electrostatic molecular dynamics simulations. The structure I of methane hydrate is constructed. When the methane hydrate with a density of 0.91 $\rm{g/cm}^3$ and temperature of 273 K is exposed ... More

Insights into Hydration Dynamics and Cooperative Interactions in Glycerol-Water Mixtures by Terahertz Dielectric SpectroscopySep 02 2019We report relaxation dynamics of glycerol-water mixtures as probed by megahertz-to-terahertz dielectric spectroscopy in a frequency range from 50 MHz to 0.5 THz at room temperature. The dielectric relaxation spectra reveal several polarization processes ... More

A Bayesian approach to NMR crystal structure determinationSep 02 2019Nuclear Magnetic Resonance (NMR) spectroscopy is particularly well-suited to determine the structure of molecules and materials in powdered form. Structure determination usually proceeds by finding the best match between experimentally observed NMR chemical ... More

Magnetic quantum number resolved state-to-state chemistrySep 02 2019We extend state-to-state chemistry to a realm where besides vibrational, rotational and hyperfine quantum states magnetic quantum numbers are also resolved. For this, we make use of the Zeeman effect which energetically splits levels of different magnetic ... More

Second-order perturbation theory with spin-symmetry projected Hartree-FockSep 02 2019We propose two different schemes for second-order perturbation theory with spin-projected Hartree-Fock. Both schemes employ the same ansatz for the first-order wave function, which is a linear combination of spin-projected configurations. The first approach ... More

Stochastic many-body perturbation theory for electron correlation energiesSep 01 2019Treating electron correlation more accurately and efficiently is at the heart of the development of electronic structure methods. In the present work, we explore the use of stochastic approaches to evaluate high-order electron correlation energies, whose ... More

Effective modelling of adsorption monolayers built of complex moleculesAug 31 2019Random sequential adsorption algorithm is a popular tool for modelling structure of monolayers built in irreversible adsorption experiments. However, this algorithm becomes very inefficient when the density of molecules in a layer rises. This problem ... More

Charge regulation radically modifies electrostatics in membrane stacksAug 31 2019Motivated by biological membrane-containing organelles in plants and photosynthetic bacteria, we study charge regulation in a model membrane stack. Considering (de)protonation as the simplest mechanism of charge equilibration between the membranes and ... More

Accurate and efficient DFT-based diabatization for hole and electron transfer using absolutely localized molecular orbitalsAug 30 2019Diabatic states and the couplings between them are important for quantifying, elucidating, and predicting the rates and mechanisms of many chemical and biochemical processes. Here, we propose and investigate approaches to accurately compute diabatic couplings ... More

Thermalization and Sub-Poissonian Density Fluctuations in a Degenerate Molecular Fermi GasAug 30 2019Sep 04 2019We observe thermalization in the production of a degenerate Fermi gas of polar ${}^{40}\text{K}{}^{87}\text{Rb}$ molecules. By measuring the atom--dimer elastic scattering cross section near the Feshbach resonance, we show that Feshbach molecules rapidly ... More

Thermalization and Sub-Poissonian Density Fluctuations in a Degenerate Molecular Fermi GasAug 30 2019We observe thermalization in the production of a degenerate Fermi gas of polar ${}^{40}\text{K}{}^{87}\text{Rb}$ molecules. By measuring the atom--dimer elastic scattering cross section near the Feshbach resonance, we show that Feshbach molecules rapidly ... More

Anomalous protein adsorption/desorption kinetics on low-fouling surfacesAug 30 2019In this work, protein-surface interactions were probed in terms of adsorption and desorption of a model protein, bovine serum albumin, on a low fouling surface with single-molecule localization microscopy. Single-molecule experiments enable precise determination ... More

Discontinuous Galerkin discretization for quantum simulation of chemistryAug 30 2019Methods for electronic structure based on Gaussian and molecular orbital discretizations offer a well established, compact representation that forms much of the foundation of correlated quantum chemistry calculations on both classical and quantum computers. ... More

The influence of impurities on the charge carrier mobility of small molecule organic semiconductorsAug 30 2019Future prospects of the organic light emitting diode (OLED) technology rely on the development of new organic semiconductors with optical and electronic properties outperforming those of presently available materials. Computational materials design is ... More

Spectroscopic characterization of aluminum monofluoride with relevance to laser cooling and trappingAug 30 2019Here we report on spectroscopic measurements of the aluminum monofluoride molecule (AlF) that are relevant to laser cooling and trapping experiments. We measure the detailed energy level structure of AlF in the X$^1\Sigma^+$ electronic ground state, in ... More

Transition from Static to Dynamic Friction in an Array of Frictional DisksAug 30 2019The nature of an instability that controls the transition from static to dynamical friction is studied in the the context of an array of frictional disks that are pressed from above on a substrate. In this case the forces are all explicit and Newtonian ... More

Quantum Nature of the Hydrogen Bond from Ambient Conditions down to Ultra-low TemperaturesAug 30 2019Many experimental techniques such as tagging photodissociation and helium nanodroplet isolation spectroscopy operate at very low temperatures in order to investigate hydrogen bonding. To elucidate the differences between such ultra-cold and usual ambient ... More