We introduce a basis of counting functions that, by cleanly tessellating three-dimensional space, allows real space number counting Jastrow factors to be straightforwardly applied to general molecular situations. Here, by exerting direct control over electron populations in local regions of space and encoding pairwise correlations between these populations, these Jastrow factors allow even very simple reference wave functions to adopt nodal surfaces well suited to many strongly correlated settings. Being trivially compatible with traditional Jastrow factors and diffusion Monte Carlo and having the same cubic per-sample cost scaling as a single determinant trial function, these Jastrow factors thus offer a powerful new route to the simultaneous capture of weak and strong electron correlation effects in a wide variety of molecular and materials settings. In multiple strongly correlated molecular examples, we show that even when paired with the simplest possible single determinant reference, these Jastrow factors allow quantum Monte Carlo to out-perform coupled cluster theory and approach the accuracy of traditional multireference methods.
Van Der Goetz, Brett, et al. "Clean and Convenient Tessellations for Number Counting Jastrow Factors." Journal of Chemical Theory and Computation, vol. 15, no. 2, Jan. 2019. https://doi.org/10.1021/acs.jctc.8b01139
Van Der Goetz, Brett, Otis, Leon, & Neuscamman, Eric (2019). Clean and Convenient Tessellations for Number Counting Jastrow Factors. Journal of Chemical Theory and Computation, 15(2). https://doi.org/10.1021/acs.jctc.8b01139
Van Der Goetz, Brett, Otis, Leon, and Neuscamman, Eric, "Clean and Convenient Tessellations for Number Counting Jastrow Factors," Journal of Chemical Theory and Computation 15, no. 2 (2019), https://doi.org/10.1021/acs.jctc.8b01139
@article{osti_1543634,
author = {Van Der Goetz, Brett and Otis, Leon and Neuscamman, Eric},
title = {Clean and Convenient Tessellations for Number Counting Jastrow Factors},
annote = {We introduce a basis of counting functions that, by cleanly tessellating three-dimensional space, allows real space number counting Jastrow factors to be straightforwardly applied to general molecular situations. Here, by exerting direct control over electron populations in local regions of space and encoding pairwise correlations between these populations, these Jastrow factors allow even very simple reference wave functions to adopt nodal surfaces well suited to many strongly correlated settings. Being trivially compatible with traditional Jastrow factors and diffusion Monte Carlo and having the same cubic per-sample cost scaling as a single determinant trial function, these Jastrow factors thus offer a powerful new route to the simultaneous capture of weak and strong electron correlation effects in a wide variety of molecular and materials settings. In multiple strongly correlated molecular examples, we show that even when paired with the simplest possible single determinant reference, these Jastrow factors allow quantum Monte Carlo to out-perform coupled cluster theory and approach the accuracy of traditional multireference methods.},
doi = {10.1021/acs.jctc.8b01139},
url = {https://www.osti.gov/biblio/1543634},
journal = {Journal of Chemical Theory and Computation},
issn = {ISSN 1549-9618},
number = {2},
volume = {15},
place = {United States},
publisher = {American Chemical Society},
year = {2019},
month = {01}}
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing
Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; SC0017869
OSTI ID:
1543634
Alternate ID(s):
OSTI ID: 1567158 OSTI ID: 2522064
Journal Information:
Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 2 Vol. 15; ISSN 1549-9618
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 238, Issue 790https://doi.org/10.1098/rsta.1939.0008