TY - JOUR
T1 - Modeling Optical Spectra of Large Organic Systems Using Real-Time Propagation of Semiempirical Effective Hamiltonians
AU - Ghosh, Soumen
AU - Andersen, Amity
AU - Gagliardi, Laura
AU - Cramer, Christopher J.
AU - Govind, Niranjan
N1 - Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/9/12
Y1 - 2017/9/12
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jctc.7b00618
DO - 10.1021/acs.jctc.7b00618
M3 - Article
C2 - 28813603
AN - SCOPUS:85029226330
SN - 1549-9618
VL - 13
SP - 4410
EP - 4420
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 9
ER -