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Bruner A, LaMaster D, Lopata K. Accelerated Broadband Spectra Using Transition Dipole Decomposition and Padé Approximants. J Chem Theory Comput. 2016;12(8):3741-50doi: 10.1021/acs.jctc.6b00511.
Bruner, A., LaMaster, D., & Lopata, K. (2016). Accelerated Broadband Spectra Using Transition Dipole Decomposition and Padé Approximants. Journal of chemical theory and computation, 12(8), 3741-50. https://doi.org/10.1021/acs.jctc.6b00511
Bruner, Adam, et al. "Accelerated Broadband Spectra Using Transition Dipole Decomposition and Padé Approximants." Journal of chemical theory and computation vol. 12,8 (2016): 3741-50. doi: https://doi.org/10.1021/acs.jctc.6b00511
Bruner A, LaMaster D, Lopata K. Accelerated Broadband Spectra Using Transition Dipole Decomposition and Padé Approximants. J Chem Theory Comput. 2016 Aug 09;12(8):3741-50. doi: 10.1021/acs.jctc.6b00511. Epub 2016 Jul 14. PMID: 27359347.
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J Chem Theory Comput. 2016 Aug 09;12(8):3741-50. doi: 10.1021/acs.jctc.6b00511. Epub 2016 Jul 14.

Accelerated Broadband Spectra Using Transition Dipole Decomposition and Padé Approximants.

Journal of chemical theory and computation

Adam Bruner, Daniel LaMaster, Kenneth Lopata

Affiliations

  1. Department of Chemistry, Louisiana State University , Baton Rouge, Louisiana 70803, United States.
  2. Center for Computation & Technology, Louisiana State University , Baton Rouge, Louisiana 70803, United States.

PMID: 27359347 DOI: 10.1021/acs.jctc.6b00511

Abstract

We present a method for accelerating the computation of UV-visible and X-ray absorption spectra in large molecular systems using real-time time-dependent density functional theory (TDDFT). This approach is based on deconvolution of the dipole into molecular orbital dipole pairs developed by Repisky, et al. [Repisky et al., J. Chem. Theory Comput. 2015, 11, 980-911] followed by Padé approximants to their Fourier transforms. By combining these two techniques, the required simulation time is reduced by a factor of 5 or more, and moreover, the transition dipoles yield the molecular orbital contributions to each transition, akin to the coefficients in linear-response TDDFT. We validate this method on valence and core-level spectra of gas-phase water and nickel porphyrin, where the results are essentially equivalent to conventional linear response. This approach makes real-time TDDFT competitive against linear response for large molecular and material systems with a high density of states.

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