Quantum Dynamics Effects in Photocatalysis

Nijamudheen, A.; Akimov, Alexey V.

doi:10.1002/9783527808175.ch19

Cited by 3 publications

(5 citation statements)

References 269 publications

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“…The excitation energies are computed as differences between the total electronic energies for each orbital occupation scheme. Unlike the simplistic 1-electron approximations that rely on energies of KS orbitals [25,26,28], the ΔSCF formulation includes Coulomb, exchange, and correlation contributions explicitly, so it can be expected to provide a better description of the electron-hole interactions. It has been argued that the ΔSCF method may even fix some of the TD-DFT shortcomings [205,206].…”

Section: Es Methods For Na-mdmentioning

confidence: 99%

“…Blumberger also reviewed NA-MD approaches in the context of modeling charge transfer in biological systems [23]. Modeling quant um nuclear effects, especially in the context of NAD has been recently reviewed by Joubert-Doriol and Izmaylov, [24] as well as by Nijamudheen and Akimov [25]. Numerous methodological advances of theory and practice of modeling NAD in complex systems have been reviewed recently by Wang et al [26].…”

Section: Introductionmentioning

confidence: 99%

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Modeling nonadiabatic dynamics in condensed matter materials: some recent advances and applications

Smith

Akimov

2019

J. Phys.: Condens. Matter

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This review focuses on recent developments in the field of nonadiabatic molecular dynamics (NA-MD), with particular attention given to condensed-matter systems. NA-MD simulations for small molecular systems can be performed using high-level electronic structure (ES) calculations, methods accounting for the quantization of nuclear motion, and using fewer approximations in the dynamical methodology itself. Modeling condensed-matter systems imposes many limitations on various aspects of NA-MD computations, requiring approximations at various levels of theory—from the ES, to the ways in which the coupling of electrons and nuclei are accounted for. Nonetheless, the approximate treatment of NA-MD in condensed-phase materials has gained a spin lately in many applied studies. A number of advancements of the methodology and computational tools have been undertaken, including general-purpose methods, as well as those tailored to nanoscale and condensed matter systems. This review summarizes such methodological and software developments, puts them into the broader context of existing approaches, and highlights some of the challenges that remain to be solved.

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Section: Es Methods For Na-mdmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Modeling nonadiabatic dynamics in condensed matter materials: some recent advances and applications

Smith

Akimov

2019

J. Phys.: Condens. Matter

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“…Processes such as electron transfer, charge transport, electronic friction at metal surfaces and nonradiative decay after photoexcitation often involve multiple PESs, with nonadiabatic (NA) transitions among them. In addition, for systems containing small mass elements, for example, hydrogen, zero‐point motion and tunneling effects may not be ignored and as a result require a quantum mechanical description of the nuclei . To address all these issues, the most ambitious approach is to treat the entire system, including the nuclei, quantum‐mechanically.…”

Section: Introductionmentioning

confidence: 99%

“…In addition, for systems containing small mass elements, for example, hydrogen, zero-point motion and tunneling effects may not be ignored and as a result require a quantum mechanical description of the nuclei. [33][34][35] To address all these issues, the most ambitious approach is to treat the entire system, including the nuclei, quantum-mechanically. Unfortunately, the formidable computational costs restrict the scope of the application and can only be applied to small systems within short time scales under the current computation resources.…”

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confidence: 99%

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

Zheng

Chu

Zhao

et al. 2019

WIREs Comput Mol Sci

247

258

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The ultrafast dynamics of photoexcited charge carriers in condensed matter systems play an important role in optoelectronics and solar energy conversion. Yet it is challenging to understand such multidimensional dynamics at the atomic scale. Combining the real‐time time‐dependent density functional theory with fewest‐switches surface hopping scheme, we develop time‐dependent ab initio nonadiabatic molecular dynamics (NAMD) code Hefei‐NAMD to simulate the excited carrier dynamics in condensed matter systems. Using this method, we have investigated the interfacial charge transfer dynamics, the electron–hole recombination dynamics, and the excited spin‐polarized hole dynamics in different condensed matter systems. The time‐dependent dynamics of excited carriers are studied in energy, real and momentum spaces. In addition, the coupling of the excited carriers with phonons, defects and molecular adsorptions are investigated. The state‐of‐art NAMD studies provide unique insights to understand the ultrafast dynamics of the excited carriers in different condensed matter systems at the atomic scale. This article is categorized under: Structure and Mechanism > Computational Materials Science Molecular and Statistical Mechanics > Molecular Dynamics and Monte‐Carlo Methods Electronic Structure Theory > Ab Initio Electronic Structure Methods Software > Simulation Methods

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“…Insights into reaction mechanism dynamics: Ab initio molecular dynamics simulations provide real-time insights into the movement of atoms and electrons during photocatalytic reactions, offering a dynamic perspective of the processes involved [88][89][90]. • Tailoring material properties: These methods aid in optimizing the properties of materials used in photocatalysis, such as band gaps and surface reactivity, leading to the design of materials that efficiently promote desired photochemical reactions [91][92][93][94].…”

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confidence: 99%

Advances in Computational Methods for Modeling Photocatalytic Reactions: A Review of Recent Developments

Gusarov

2024

Materials

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Photocatalysis is a fascinating process in which a photocatalyst plays a pivotal role in driving a chemical reaction when exposed to light. Its capacity to harness light energy triggers a cascade of reactions that lead to the formation of intermediate compounds, culminating in the desired final product(s). The essence of this process is the interaction between the photocatalyst’s excited state and its specific interactions with reactants, resulting in the creation of intermediates. The process’s appeal is further enhanced by its cyclic nature—the photocatalyst is rejuvenated after each cycle, ensuring ongoing and sustainable catalytic action. Nevertheless, comprehending the photocatalytic process through the modeling of photoactive materials and molecular devices demands advanced computational techniques founded on effective quantum chemistry methods, multiscale modeling, and machine learning. This review analyzes contemporary theoretical methods, spanning a range of lengths and accuracy scales, and assesses the strengths and limitations of these methods. It also explores the future challenges in modeling complex nano-photocatalysts, underscoring the necessity of integrating various methods hierarchically to optimize resource distribution across different scales. Additionally, the discussion includes the role of excited state chemistry, a crucial element in understanding photocatalysis.

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Quantum Dynamics Effects in Photocatalysis

Cited by 3 publications

References 269 publications

Modeling nonadiabatic dynamics in condensed matter materials: some recent advances and applications

Modeling nonadiabatic dynamics in condensed matter materials: some recent advances and applications

Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems

Advances in Computational Methods for Modeling Photocatalytic Reactions: A Review of Recent Developments

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