Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 12, Issue 8, Pages 3741-3750Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.6b00511
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Funding
- Louisiana Board of Regents [LEQSF(2014-17)-RD-A-03]
- National Science Foundation [CHE-1362641]
- Oak Ridge Associated Universities
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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 Fade 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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