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Title: Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians

Abstract

We present an implementation of a time-dependent semiempirical method (INDO/S) in NWChem using real-time (RT) propagation to address, in principle, the entire spectrum of valence electronic excitations. Adopting this model, we study the UV/vis spectra of medium-sized systems such as P3B2 and f-coronene, and in addition much larger systems such as ubiquitin in the gas phase and the betanin chromophore in the presence of two explicit solvents (water and methanol). RT-INDO/S provides qualitatively and often quantitatively accurate results when compared with RT- TDDFT or experimental spectra. Even though we only consider the INDO/S Hamiltonian in this work, our implementation provides a framework for performing electron dynamics in large systems using semiempirical Hartree–Fock Hamiltonians in general.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [2]
  1. Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455-0431, United States
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99338, United States
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1414779
Alternate Identifier(s):
OSTI ID: 1508253
Grant/Contract Number:  
SC0008666; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Name: Journal of Chemical Theory and Computation Journal Volume: 13 Journal Issue: 9; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ghosh, Soumen, Andersen, Amity, Gagliardi, Laura, Cramer, Christopher J., and Govind, Niranjan. Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians. United States: N. p., 2017. Web. doi:10.1021/acs.jctc.7b00618.
Ghosh, Soumen, Andersen, Amity, Gagliardi, Laura, Cramer, Christopher J., & Govind, Niranjan. Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians. United States. doi:10.1021/acs.jctc.7b00618.
Ghosh, Soumen, Andersen, Amity, Gagliardi, Laura, Cramer, Christopher J., and Govind, Niranjan. Tue . "Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians". United States. doi:10.1021/acs.jctc.7b00618.
@article{osti_1414779,
title = {Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians},
author = {Ghosh, Soumen and Andersen, Amity and Gagliardi, Laura and Cramer, Christopher J. and Govind, Niranjan},
abstractNote = {We present an implementation of a time-dependent semiempirical method (INDO/S) in NWChem using real-time (RT) propagation to address, in principle, the entire spectrum of valence electronic excitations. Adopting this model, we study the UV/vis spectra of medium-sized systems such as P3B2 and f-coronene, and in addition much larger systems such as ubiquitin in the gas phase and the betanin chromophore in the presence of two explicit solvents (water and methanol). RT-INDO/S provides qualitatively and often quantitatively accurate results when compared with RT- TDDFT or experimental spectra. Even though we only consider the INDO/S Hamiltonian in this work, our implementation provides a framework for performing electron dynamics in large systems using semiempirical Hartree–Fock Hamiltonians in general.},
doi = {10.1021/acs.jctc.7b00618},
journal = {Journal of Chemical Theory and Computation},
number = 9,
volume = 13,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/acs.jctc.7b00618

Citation Metrics:
Cited by: 5 works
Citation information provided by
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