TY - JOUR
T1 - Stochastic Real-Time Second-Order Green’s Function Theory for Neutral Excitations in Molecules and Nanostructures
AU - Mejía, Leopoldo
AU - Yin, Jia
AU - Reichman, David R.
AU - Baer, Roi
AU - Yang, Chao
AU - Rabani, Eran
N1 - Publisher Copyright:
© 2023 American Chemical Society
PY - 2023/8/22
Y1 - 2023/8/22
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85168428153&partnerID=8YFLogxK
U2 - 10.1021/acs.jctc.3c00296
DO - 10.1021/acs.jctc.3c00296
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C2 - 37539990
AN - SCOPUS:85168428153
SN - 1549-9618
VL - 19
SP - 5563
EP - 5571
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 16
ER -