Non-Adiabatic Molecular Dynamics Methods for Materials Discovery

Furche, Filipp; Parker, Shane M.; Muuronen, Mikko J.; Roy, Saswata

doi:10.2172/1351540

Non-Adiabatic Molecular Dynamics Methods for Materials Discovery

Technical Report · Tue Apr 04 04:00:00 EDT 2017

DOI:https://doi.org/10.2172/1351540· OSTI ID:1351540

^[1]; Parker, Shane M. ^[2]; Muuronen, Mikko J. ^[2]; Roy, Saswata ^[2]

Univ. of California, Irvine, CA (United States); University of California, Irvine
Univ. of California, Irvine, CA (United States)

The flow of radiative energy in light-driven materials such as photosensitizer dyes or photocatalysts is governed by non-adiabatic transitions between electronic states and cannot be described within the Born-Oppenheimer approximation commonly used in electronic structure theory. The non-adiabatic molecular dynamics (NAMD) methods based on Tully surface hopping and time-dependent density functional theory developed in this project have greatly extended the range of molecular materials that can be tackled by NAMD simulations. New algorithms to compute molecular excited state and response properties efficiently were developed. Fundamental limitations of common non-linear response methods were discovered and characterized. Methods for accurate computations of vibronic spectra of materials such as black absorbers were developed and applied. It was shown that open-shell TDDFT methods capture bond breaking in NAMD simulations, a longstanding challenge for single-reference molecular dynamics simulations. The methods developed in this project were applied to study the photodissociation of acetaldehyde and revealed that non-adiabatic effects are experimentally observable in fragment kinetic energy distributions. Finally, the project enabled the first detailed NAMD simulations of photocatalytic water oxidation by titania nanoclusters, uncovering the mechanism of this fundamentally important reaction for fuel generation and storage.

Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

DOE Contract Number:: SC0008694

OSTI ID:: 1351540

Report Number(s):: DOE-UCI--SC0008694; 9498245051

Country of Publication:: United States

Language:: English

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Non-adiabatic molecular dynamics
acetaldehyde
excited states
photochemistry
radiationless transitions
response theory
time-dependent density functional theory
titanium dioxide

Ab initio non-adiabatic molecular dynamics Tapavicza, Enrico; Bellchambers, Gregory D.; Vincent, Jordan C. https://doi.org/10.1039/c3cp51514a The current record is supplemented by this journal	journal	January 2013
Unphysical divergences in response theory Parker, Shane M.; Roy, Saswata; Furche, Filipp https://doi.org/10.1063/1.4963749 The current record is supplemented by this journal	journal	October 2016
Importance of Vibronic Effects in the UV–Vis Spectrum of the 7,7,8,8-Tetracyanoquinodimethane Anion Tapavicza, Enrico; Furche, Filipp; Sundholm, Dage https://doi.org/10.1021/acs.jctc.6b00720 The current record is supplemented by this journal	journal	September 2016
First-order derivative couplings between excited states from adiabatic TDDFT response theory Ou, Qi; Bellchambers, Gregory D.; Furche, Filipp https://doi.org/10.1063/1.4906941 The current record is supplemented by this journal	journal	February 2015
Mechanism of photocatalytic water oxidation on small TiO ₂ nanoparticles Muuronen, Mikko; Parker, Shane M.; Berardo, Enrico https://doi.org/10.1039/C6SC04378J The current record is supplemented by this journal	journal	January 2017
Turbomole Furche, Filipp; Ahlrichs, Reinhart; Hättig, Christof https://doi.org/10.1002/wcms.1162 The current record is supplemented by this journal	journal	July 2013
Dinitrogen Reduction via Photochemical Activation of Heteroleptic Tris(cyclopentadienyl) Rare-Earth Complexes Fieser, Megan E.; Bates, Jefferson E.; Ziller, Joseph W. https://doi.org/10.1021/ja400664s The current record is supplemented by this journal	journal	March 2013
Accelerating molecular property calculations with nonorthonormal Krylov space methods Furche, Filipp; Krull, Brandon T.; Nguyen, Brian D. https://doi.org/10.1063/1.4947245 The current record is supplemented by this journal	journal	May 2016
That Little Extra Kick: Nonadiabatic Effects in Acetaldehyde Photodissociation Vincent, Jordan C.; Muuronen, Mikko; Pearce, Kirk C. https://doi.org/10.1021/acs.jpclett.6b02037 The current record is supplemented by this journal	journal	October 2016
Metal effects on ligand non-innocence in Group 5 complexes of the redox-active [ONO] pincer ligand Hananouchi, Steven; Krull, Brandon T.; Ziller, Joseph W. https://doi.org/10.1039/C4DT02259A The current record is supplemented by this journal	journal	January 2014
Brominated Luciferins Are Versatile Bioluminescent Probes Steinhardt, Rachel C.; Rathbun, Colin M.; Krull, Brandon T. https://doi.org/10.1002/cbic.201600564 The current record is supplemented by this journal	journal	December 2016
Dinitrogen Reduction, Sulfur Reduction, and Isoprene Polymerization via Photochemical Activation of Trivalent Bis(cyclopentadienyl) Rare-Earth-Metal Allyl Complexes Fieser, Megan E.; Johnson, Casey W.; Bates, Jefferson E. https://doi.org/10.1021/acs.organomet.5b00613 The current record is supplemented by this journal	journal	August 2015

Non-Adiabatic Molecular Dynamics Methods for Materials Discovery

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