TY - JOUR
T1 - Multicomponent Cholesky Decomposition
T2 - Application to Nuclear-Electronic Orbital Theory
AU - Liu, Aodong
AU - Zhang, Tianyuan
AU - Hammes-Schiffer, Sharon
AU - Li, Xiaosong
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/9/26
Y1 - 2023/9/26
N2 - The Cholesky decomposition technique is commonly used to reduce the memory requirement for storing two-particle repulsion integrals in quantum chemistry calculations that use atomic orbital bases. However, when quantum methods use multicomponent bases, such as nuclear-electronic orbitals, additional challenges are introduced due to asymmetric two-particle integrals. This work proposes several multicomponent Cholesky decomposition methods for calculations using nuclear-electronic orbital density functional theory. To analyze the errors in different Cholesky decomposition components, benchmark calculations using water clusters are carried out. The largest benchmark calculation is a water cluster (H2O)27 where all 54 protons are treated quantum mechanically. This study provides energetic and complexity analyses to demonstrate the accuracy and performance of the proposed multicomponent Cholesky decomposition method.
AB - The Cholesky decomposition technique is commonly used to reduce the memory requirement for storing two-particle repulsion integrals in quantum chemistry calculations that use atomic orbital bases. However, when quantum methods use multicomponent bases, such as nuclear-electronic orbitals, additional challenges are introduced due to asymmetric two-particle integrals. This work proposes several multicomponent Cholesky decomposition methods for calculations using nuclear-electronic orbital density functional theory. To analyze the errors in different Cholesky decomposition components, benchmark calculations using water clusters are carried out. The largest benchmark calculation is a water cluster (H2O)27 where all 54 protons are treated quantum mechanically. This study provides energetic and complexity analyses to demonstrate the accuracy and performance of the proposed multicomponent Cholesky decomposition method.
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U2 - 10.1021/acs.jctc.3c00686
DO - 10.1021/acs.jctc.3c00686
M3 - Article
C2 - 37699735
AN - SCOPUS:85172425474
SN - 1549-9618
VL - 19
SP - 6255
EP - 6262
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 18
ER -