TY - JOUR
T1 - New Dimension in Ab Initio Electronic Structure Theory
T2 - Temperature, Pressure, and Chemical Potential
AU - Hirata, So
N1 - This work was supported by the U.S. Department of Energy (DoE), Office of Science, Office of Basic Energy Sciences under Grant No. DE-SC0006028 and also by the Center for Scalable Predictive methods for Excitations and Correlated phenomena (SPEC), which is funded by the U.S. DoE, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences as part of the Computational Chemical Sciences (CCS) program at Pacific Northwest National Laboratory (PNNL) under FWP 70942. PNNL is a multiprogram national laboratory operated by Battelle Memorial Institute for the U.S. DoE. This work was also supported by the Guggenheim Fellowship.
PY - 2025/4/17
Y1 - 2025/4/17
N2 - Ab initio electronic structure theory has transformed gas-phase molecular science with its predictive ability. In the attempt to bring such predictive ability to macroscopic systems and condensed matter, the theory must integrate quantum mechanics with statistical thermodynamics so that thermodynamic functions such as free energy, internal energy, entropy, and chemical potentials are computed as functions of temperature in a systematically converging series of approximations. A general, versatile strategy of elevating any ab initio electronic structure theory to nonzero temperatures is introduced and discussed.
AB - Ab initio electronic structure theory has transformed gas-phase molecular science with its predictive ability. In the attempt to bring such predictive ability to macroscopic systems and condensed matter, the theory must integrate quantum mechanics with statistical thermodynamics so that thermodynamic functions such as free energy, internal energy, entropy, and chemical potentials are computed as functions of temperature in a systematically converging series of approximations. A general, versatile strategy of elevating any ab initio electronic structure theory to nonzero temperatures is introduced and discussed.
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U2 - 10.1021/acs.jpclett.5c00631
DO - 10.1021/acs.jpclett.5c00631
M3 - Review article
C2 - 40183225
AN - SCOPUS:105001977912
SN - 1948-7185
VL - 16
SP - 3632
EP - 3645
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 15
ER -