Quantum Chemistry in the Age of Quantum Computing

Chemical Reviews, Год журнала: 2019, Номер 119(19), С. 10856 - 10915

Опубликована: Авг. 30, 2019

Practical challenges in simulating quantum systems on classical computers have been widely recognized the physics and chemistry communities over past century. Although many approximation methods introduced, complexity of mechanics remains hard to appease. The advent computation brings new pathways navigate this challenging complex landscape. By manipulating states matter taking advantage their unique features such as superposition entanglement, promise efficiently deliver accurate results for important problems chemistry, electronic structure molecules. In two decades, significant advances made developing algorithms physical hardware computing, heralding a revolution simulation systems. This Review provides an overview that are relevant chemistry. intended audience is both chemists who seek learn more about computing researchers would like explore applications

Язык: Английский

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TURBOMOLE: Modular program suite for ab initio quantum-chemical and condensed-matter simulations

The Journal of Chemical Physics, Год журнала: 2020, Номер 152(18)

Опубликована: Май 13, 2020

TURBOMOLE is a collaborative, multi-national software development project aiming to provide highly efficient and stable computational tools for quantum chemical simulations of molecules, clusters, periodic systems, solutions. The suite optimized widely available, inexpensive, resource-efficient hardware such as multi-core workstations small computer clusters. specializes in electronic structure methods with outstanding accuracy-cost ratio, density functional theory including local hybrids the random phase approximation (RPA), GW-Bethe-Salpeter methods, second-order Møller-Plesset theory, explicitly correlated coupled-cluster methods. based on Gaussian basis sets has been pivotal many fast low-scaling algorithms past three decades, integral-direct multipole resolution-of-the-identity approximation, imaginary frequency integration, Laplace transform, pair natural orbital This review focuses recent additions TURBOMOLE's functionality, excited-state RPA Green's function relativistic approaches, high-order molecular properties, solvation effects, systems. A variety illustrative applications along accuracy timing data are discussed. Moreover, available interfaces users well other summarized. current licensing, distribution, support model discussed, an overview workflow provided. Challenges communication outreach, infrastructure, funding highlighted.

Язык: Английский

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Machine-learned potentials for next-generation matter simulations

Nature Materials, Год журнала: 2021, Номер 20(6), С. 750 - 761

Опубликована: Май 27, 2021

Язык: Английский

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Machine Learning for Electronically Excited States of Molecules

Chemical Reviews, Год журнала: 2020, Номер 121(16), С. 9873 - 9926

Опубликована: Ноя. 19, 2020

Electronically excited states of molecules are at the heart photochemistry, photophysics, as well photobiology and also play a role in material science. Their theoretical description requires highly accurate quantum chemical calculations, which computationally expensive. In this review, we focus on not only how machine learning is employed to speed up such excited-state simulations but branch artificial intelligence can be used advance exciting research field all its aspects. Discussed applications for include dynamics simulations, static calculations absorption spectra, many others. order put these studies into context, discuss promises pitfalls involved techniques. Since latter mostly based chemistry provide short introduction electronic structure methods approaches nonadiabatic describe tricks problems when using them molecules.

Язык: Английский

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Non-adiabatic Excited-State Molecular Dynamics: Theory and Applications for Modeling Photophysics in Extended Molecular Materials

Chemical Reviews, Год журнала: 2020, Номер 120(4), С. 2215 - 2287

Опубликована: Фев. 10, 2020

Optically active molecular materials, such as organic conjugated polymers and biological systems, are characterized by strong coupling between electronic vibrational degrees of freedom. Typically, simulations must go beyond the Born–Oppenheimer approximation to account for non-adiabatic excited states. Indeed, dynamics is commonly associated with exciton photophysics involving charge energy transfer, well dissociation recombination. Understanding photoinduced in materials vital providing an accurate description formation, evolution, decay. This interdisciplinary field has matured significantly over past decades. Formulation new theoretical frameworks, development more efficient computational algorithms, evolution high-performance computer hardware extended these very large systems hundreds atoms, including numerous studies semiconductors biomolecules. In this Review, we will describe recent advances treatment decoherence surface-hopping methods, role solvent effects, trivial unavoided crossings, analysis data based on transition densities, implementations numerical methods. We also emphasize newly developed semiclassical approaches, Gaussian approximation, which retain phase width information significant interference effects while maintaining high efficiency approaches. The above developments have been employed successfully a variety materials.

Язык: Английский

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Multiscale Simulations of Biological Membranes: The Challenge To Understand Biological Phenomena in a Living Substance

Chemical Reviews, Год журнала: 2019, Номер 119(9), С. 5607 - 5774

Опубликована: Март 12, 2019

Biological membranes are tricky to investigate. They complex in terms of molecular composition and structure, functional over a wide range time scales, characterized by nonequilibrium conditions. Because all these features, simulations great technique study biomembrane behavior. A significant part the processes biological takes place at level; thus computer method choice explore how their properties emerge from specific features interplay among numerous molecules gives rise function spatial scales larger than ones. In this review, we focus on broad theme. We discuss current state-of-the-art that, until now, have largely focused rather narrow picture complexity membranes. Given this, also challenges that should unravel foreseeable future. Numerous such as actin-cytoskeleton network, glycocalyx transport under ATP-driven conditions so far received very little attention; however, potential solve them would be exceptionally high. major milestone for research one day could say genuinely membranes, not just lipid bilayers.

Язык: Английский

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Grand-canonical approach to density functional theory of electrocatalytic systems: Thermodynamics of solid-liquid interfaces at constant ion and electrode potentials

The Journal of Chemical Physics, Год журнала: 2018, Номер 150(4)

Опубликована: Ноя. 30, 2018

Properties of solid-liquid interfaces are immense importance for electrocatalytic and electrochemical systems, but modeling such at the atomic level presents a serious challenge approaches beyond standard methodologies needed. An atomistic computational scheme needs to treat least part system quantum mechanically describe adsorption reactions, while entire is in thermal equilibrium. The experimentally relevant macroscopic control variables temperature, electrode potential, choice solvent ions, these need be explicitly included model as well; this calls thermodynamic ensemble with fixed ion potentials. In work, general framework within density functional theory (DFT) electron chemical potentials grand canonical (GC) established interfaces. Starting from fully mechanical description multi-component GC-DFT nuclei electrons, systematic coarse-graining employed establish various schemes including (i) combination classical electronic DFTs GC (ii) on simplest chemically physically sound way obtain (modified) Poisson-Boltzmann (mPB) implicit models. detailed rigorous derivation clearly establishes which approximations needed well highlights details interactions omitted vein feasibility. transparent also allow removing some constraints if We implement mPB models linear dielectric continuum GPAW code test their capabilities capacitance study different partly periodic charged systems. Our well-defined DFT electrolytes inadequacy current treating properties interface.

Язык: Английский

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Polarizable embedding QM/MM: the future gold standard for complex (bio)systems?

Physical Chemistry Chemical Physics, Год журнала: 2020, Номер 22(26), С. 14433 - 14448

Опубликована: Янв. 1, 2020

We provide a perspective of the induced dipole formulation polarizable QM/MM, showing how efficient implementations will enable their application to modeling dynamics, spectroscopy, and reactivity in complex biosystems.

Язык: Английский

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Molecular excited states through a machine learning lens

Nature Reviews Chemistry, Год журнала: 2021, Номер 5(6), С. 388 - 405

Опубликована: Май 20, 2021

Язык: Английский

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Tracking Polariton Relaxation with Multiscale Molecular Dynamics Simulations

The Journal of Physical Chemistry Letters, Год журнала: 2019, Номер 10(18), С. 5476 - 5483

Опубликована: Авг. 27, 2019

When photoactive molecules interact strongly with confined light modes in optical cavities, new hybrid light–matter states form. They are known as polaritons and correspond to coherent superpositions of excitations the cavity photon. The polariton energies thus potential energy surfaces changed respect bare molecules, such that formation is considered a promising paradigm for controlling photochemical reactions. To effectively manipulate photochemistry light, need remain polaritonic state long enough reaction on modified surface take place. understand what determines this lifetime, we have performed atomistic molecular dynamics simulations room-temperature ensembles rhodamine chromophores coupled single mode 15 fs lifetime. We investigated three popular experimental scenarios followed relaxation after optically pumping (i) lower polariton, (ii) upper or (iii) uncoupled states. results suggest lifetimes accessible limited by ultrafast photoemission due low lifetime reversible population transfer into "dark" manifold. Dark but much smaller contributions from photon, decreasing their emission rates hence increasing lifetimes. find between dark determined overlap absorption spectra. Importantly, excitation can also be transferred "upward" dark-state reservoir broad spectra chromophores, contrary common conception these processes "one-way" down polariton. Our chemistry relying taking place within manifold requires cavities sufficiently and, at same time, strong coupling strengths prevent back-transfer

Язык: Английский

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