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Title: Stochastic Real-Time Second-Order Green’s Function Theory for Neutral Excitations in Molecules and Nanostructures

Journal Article · · Journal of Chemical Theory and Computation
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [5]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. Columbia Univ., New York, NY (United States)
  4. Hebrew Univ. of Jerusalem (Israel)
  5. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel)
+ Show Author Affiliations

We present a real-time second-order Green’s function (GF) method for computing excited states in molecules and nanostructures, with a computational scaling of O(Ne3), where Ne is the number of electrons. The cubic scaling is achieved by adopting the stochastic resolution of the identity to decouple the 4-index electron repulsion integrals. To improve the time propagation and the spectral resolution, we adopt the dynamic mode decomposition technique and assess the accuracy and efficiency of the combined approach for a chain of hydrogen dimer molecules of different lengths. We find that the stochastic implementation accurately reproduces the deterministic results for the electronic dynamics and excitation energies. Furthermore, we provide a detailed analysis of the statistical errors, bias, and long-time extrapolation. Overall, the approach offers an efficient route to investigate excited states in extended systems with open or closed boundary conditions.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
Grant/Contract Number:
AC02-05CH11231; SC0022088
OSTI ID:
2323299
Journal Information:
Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 16 Vol. 19; ISSN 1549-9618
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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