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@ARTICLE{Cuzzocrea:877891,
author = {Cuzzocrea, Alice and Scemama, Anthony and Briels, Willem
and Moroni, Saverio and Filippi, Claudia},
title = {{V}ariational {P}rinciples in {Q}uantum {M}onte {C}arlo:
{T}he {T}roubled {S}tory of {V}ariance {M}inimization},
journal = {Journal of chemical theory and computation},
volume = {16},
number = {7},
issn = {1549-9626},
address = {Washington, DC},
reportid = {FZJ-2020-02496},
pages = {4203-4212},
year = {2020},
abstract = {We investigate the use of different variational principles
in quantum Monte Carlo, namely, energy and variance
minimization, prompted by the interest in the robust and
accurate estimation of electronic excited states. For two
prototypical, challenging molecules, we readily reach the
accuracy of the best available reference excitation energies
using energy minimization in a state-specific or
state-average fashion for states of different or equal
symmetry, respectively. On the other hand, in variance
minimization, where the use of suitable functionals is
expected to target specific states regardless of the
symmetry, we encounter severe problems for a variety of wave
functions: as the variance converges, the energy drifts away
from that of the selected state. This unexpected behavior is
sometimes observed even when the target is the ground state
and generally prevents the robust estimation of total and
excitation energies. We analyze this problem using a very
simple wave function and infer that the optimization finds
little or no barrier to escape from a local minimum or local
plateau, eventually converging to a lower-variance state
instead of the target state. For the increasingly complex
systems becoming in reach of quantum Monte Carlo
simulations, variance minimization with current functionals
appears to be an impractical route.},
cin = {IBI-4},
ddc = {610},
cid = {I:(DE-Juel1)IBI-4-20200312},
pnm = {551 - Functional Macromolecules and Complexes (POF3-551)},
pid = {G:(DE-HGF)POF3-551},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:32419451},
UT = {WOS:000607532300019},
doi = {10.1021/acs.jctc.0c00147},
url = {https://juser.fz-juelich.de/record/877891},
}