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Quantum Monte Carlo for molecules

Conference ·
OSTI ID:5343552

An alternative approach to conventional quantum chemistry techniques for molecular studies is described. This approach uses the quantum Monte Carlo method, which was developed and used primarily in nuclear and condensed-matter physics. In this approach the many-body Schroedinger equation is re-interpreted as a diffusion equation. Simulation of the appropriate random walk process allows one to calculate expectation values of molecular properties. In principle these expectation values can be calculated exactly, subject only to statistical errors (which may be made arbitrarily small). In preliminary work on small molecules (H/sub 2/, LiH, Li/sub 2/, and H/sub 2/O), we use a simple but accurate approximation to ease the treatment of Fermi statistics. In that approximation, the calculated total energy remains an upper bound to the true energy. How good the bound is, as well as the magnitude of the statistical error, depends on the quality of an importance function which guides the diffusion into more probable regions of phase space. With relatively simple importance functions, we obtain from 75 to 100% of the correlation energy of the above-mentioned molecules.

Research Organization:
Lawrence Berkeley Lab., CA (USA)
DOE Contract Number:
AC03-76SF00098
OSTI ID:
5343552
Report Number(s):
LBL-16753; CONF-830589-3; ON: DE84005171
Country of Publication:
United States
Language:
English