Computational Screening of 2D Materials for Photocatalysis

The Journal of Physical Chemistry Letters, Год журнала: 2015, Номер 6(6), С. 1087 - 1098

Опубликована: Фев. 26, 2015

Two-dimensional (2D) materials exhibit a range of extraordinary electronic, optical, and mechanical properties different from their bulk counterparts with potential applications for 2D emerging in energy storage conversion technologies. In this Perspective, we summarize the recent developments field solar water splitting using review computational screening approach to rapidly efficiently discover more that possess suitable splitting. Computational tools based on density-functional theory can predict intrinsic photocatalyst such as electronic properties, optical absorbance, solubility aqueous solutions. enable exploration possible routes enhance photocatalytic activity by use strain, bias potential, doping, pH. We discuss future research directions needed method design optimization photocatalysis.

Язык: Английский

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Ab Initio Nonadiabatic Quantum Molecular Dynamics

Chemical Reviews, Год журнала: 2018, Номер 118(7), С. 3305 - 3336

Опубликована: Фев. 21, 2018

The Born–Oppenheimer approximation underlies much of chemical simulation and provides the framework defining potential energy surfaces that are used for our pictorial understanding phenomena. However, this breaks down when dynamics molecules in excited electronic states considered. Describing requires a quantum mechanical description nuclei. Chemical reaction on is critical many applications renewable energy, synthesis, bioimaging. Furthermore, it necessary order to connect with ultrafast pump–probe spectroscopic experiments. In review, we provide an overview methods can describe nonadiabatic dynamics, emphasis those able simultaneously address mechanics both electrons Such ab initio molecular solve Schrödinger equation alongside nuclear thereby avoid need precalculation coupling matrix elements. Two main families commonly employed simulate molecules: full such as multiconfigurational time-dependent Hartree method, classical trajectory-based approaches, trajectory surface hopping. third class intermediate between two: Gaussian basis set expansions built around trajectories.

Язык: Английский

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Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Chemical Reviews, Год журнала: 2018, Номер 118(15), С. 7026 - 7068

Опубликована: Май 16, 2018

Nonadiabatic mixed quantum–classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution nonadiabatic phenomena molecules and supramolecular assemblies. NA-MQC is characterized by partition molecular system into two subsystems: one be treated mechanically (usually but not restricted electrons) another dealt with classically (nuclei). The subsystems are connected through couplings terms enforce self-consistency. A local approximation underlies classical subsystem, implying that direct can simulated, without needing precomputed potential energy surfaces. split allows reducing costs, enabling treatment realistic systems diverse fields. Starting from three most well-established methods—mean-field Ehrenfest, trajectory surface hopping, multiple spawning—this review focuses on programs developed last 10 years. It stresses relations between their domains application. electronic structure commonly used together reviewed as well. accuracy precision simulations critically discussed, general guidelines choose an adequate method for each application delivered.

Язык: Английский

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Computational electrochemistry: prediction of liquid-phase reduction potentials

Physical Chemistry Chemical Physics, Год журнала: 2014, Номер 16(29), С. 15068 - 15106

Опубликована: Янв. 1, 2014

The article reviews recent developments and applications for predicting the standard reduction potentials of chemical reactions in solution.

Язык: Английский

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Attosecond Electron Dynamics in Molecules

Chemical Reviews, Год журнала: 2017, Номер 117(16), С. 10760 - 10825

Опубликована: Май 10, 2017

Advances in attosecond science have led to a wealth of important discoveries atomic, molecular, and solid-state physics are progressively directing their footsteps toward problems chemical interest. Relevant technical achievements the generation application extreme-ultraviolet subfemtosecond pulses, introduction experimental techniques able follow time electron dynamics quantum systems, development sophisticated theoretical methods for interpretation outcomes such experiments raised continuous growing interest phenomena, as demonstrated by vast literature on subject. In this review, after introducing physical mechanisms at basis pulse technology describing tools that complement research field, we will concentrate investigation ultrafast processes molecules, with emphasis molecules biological The measurement control electronic motion complex molecular structures is formidable challenge, both theory experiment, but indubitably tremendous impact chemistry years come.

Язык: Английский

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Polaritonic Chemistry with Organic Molecules

ACS Photonics, Год журнала: 2017, Номер 5(1), С. 205 - 216

Опубликована: Сен. 26, 2017

We present an overview of the general concepts polaritonic chemistry with organic molecules, i.e., manipulation chemical structure that can be achieved through strong coupling between confined light modes and molecules. Strong associated formation polaritons, hybrid light–matter excitations, lead to energy shifts in such systems amount a large fraction uncoupled transition energy. This has recently been shown significantly alter coupled which opens possibility manipulate control reactions. discuss current state theory for describing these changes several applications, particular focus on collective effects observed when many molecules are involved coupling.

Язык: Английский

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Recent Advances in the Theory and Molecular Simulation of Biological Electron Transfer Reactions

Chemical Reviews, Год журнала: 2015, Номер 115(20), С. 11191 - 11238

Опубликована: Окт. 20, 2015

ADVERTISEMENT RETURN TO ISSUEReviewNEXTRecent Advances in the Theory and Molecular Simulation of Biological Electron Transfer ReactionsJochen Blumberger*View Author Information Department Physics Astronomy, University College London, Gower Street, London WC1E 6BT, U.K.*E-mail: [email protected]Cite this: Chem. Rev. 2015, 115, 20, 11191–11238Publication Date (Web):October 2015Publication History Received18 May 2015Published online20 October inissue 28 2015https://doi.org/10.1021/acs.chemrev.5b00298Copyright © 2015 American Chemical SocietyRIGHTS & PERMISSIONSACS Editors’ ChoiceArticle Views20656Altmetric-Citations250LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated by Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence for given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InReddit (15 MB) Get e-AlertsSUBJECTS:Bioinorganic chemistry,Charge transfer,Chemical calculations,Electrical energy,Free energy e-Alerts

Язык: Английский

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Charge Transport in Molecular Materials: An Assessment of Computational Methods

Chemical Reviews, Год журнала: 2017, Номер 117(15), С. 10319 - 10357

Опубликована: Июнь 23, 2017

The booming field of molecular electronics has fostered a surge computational research on electronic properties organic solids. In particular, with respect to microscopic understanding transport and loss mechanisms, theoretical studies assume an ever-increasing role. Owing the tremendous diversity materials, great number methods have been put forward suit every possible charge regime, material, need for accuracy. With this review article we aim at providing compendium available methods, their foundations, ranges validity. We illustrate these through applications found in literature. focus is crystals, but mention made wherever techniques are suitable use other related materials such as disordered or polymeric systems.

Язык: Английский

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Computational Approach to Molecular Catalysis by 3d Transition Metals: Challenges and Opportunities

Chemical Reviews, Год журнала: 2018, Номер 119(4), С. 2453 - 2523

Опубликована: Окт. 30, 2018

Computational chemistry provides a versatile toolbox for studying mechanistic details of catalytic reactions and holds promise to deliver practical strategies enable the rational in silico catalyst design. The reactivity nontrivial electronic structure effects, common systems based on 3d transition metals, introduce additional complexity that may represent particular challenge standard computational strategies. In this review, we discuss challenges capabilities modern methods reaction mechanisms promoted by metal molecular catalysts. Particular focus will be placed ways addressing multiconfigurational problem calculations role expert bias utilization available methods. development density functionals designed address metals is also discussed. Special emphasis account solvation effects multicomponent nature systems. This followed an overview recent studies processes catalysts metals. Cases involve noninnocent ligands, systems, metal-ligand metal-metal cooperativity, as well modeling complex such metal-organic frameworks are presented. Conventionally, heavily dependent chemical intuition input researcher. Recent developments advanced automated path analysis hold eliminating human-bias from catalysis studies. A brief these approaches presented final section review. paper closed with general concluding remarks.

Язык: Английский

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Recent Progress in Surface Hopping: 2011–2015

The Journal of Physical Chemistry Letters, Год журнала: 2016, Номер 7(11), С. 2100 - 2112

Опубликована: Май 12, 2016

Developed 25 years ago, Tully's fewest switches surface hopping (FSSH) has proven to be the most popular approach for simulating quantum-classical dynamics in a broad variety of systems, ranging from gas phase, liquid and solid phases, biological nanoscale materials. FSSH is widely adopted as fundamental platform introduce modifications needed. Significant progress been made recently enhance accuracy efficiency technique. Various limitations standard FSSH-associated with quantum nuclear effects, interference decoherence, trivial or "unavoided" crossings, superexchange, representation dependence-have lifted. These advances are needed allow one treat many important phenomena chemistry, physics, materials, related disciplines. Examples include charge transport extended systems such organic solids, singlet fission molecular aggregates, Auger-type exciton multiplication, recombination relaxation dots other Auger-assisted transfer, nonradiative luminescence quenching, electron-hole recombination. This Perspective summarizes recent formulation nonadiabatic provides an outlook on future hopping.

Язык: Английский

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