Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

A new generation of effective core potentials from correlated calculations: 3d transition metal series

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5040472· OSTI ID:1477870
 [1];  [1];  [2];  [2];  [3];  [1]
  1. North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics
  2. North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics; Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
+ Show Author Affiliations
Recently, we have introduced a new generation of effective core potentials (ECPs) designed for accurate correlated calculations but equally useful for a broad variety of approaches. The guiding principle has been the isospectrality of all-electron and ECP Hamiltonians for a subset of valence many-body states using correlated, nearly-exact calculations. We present such ECPs for the 3d transition series Sc to Zn with Ne-core, i.e., with semi-core 3s and 3p electrons in the valence space. Besides genuine many-body accuracy, the operators are simple, being represented by a few gaussians per symmetry channel with resulting potentials that are bounded everywhere. The transferability is checked on selected molecular systems over a range of geometries. The ECPs show a high overall accuracy with valence spectral discrepancies typically ≈0.01-0.02 eV or better. Finally, they also reproduce binding curves of hydride and oxide molecules typically within 0.02-0.03 eV deviations over the full non-dissociation range of interatomic distances.
Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); North Carolina State Univ., Raleigh, NC (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
NA0003525
OSTI ID:
1477870
Alternate ID(s):
OSTI ID: 1475478
Report Number(s):
SAND--2018-5251J; 663180
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 149; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (37)

Biodiversity offsetting: Clearing up misunderstandings between conservation and economics to take further action journal February 2017
Symmetry and equivalence restrictions in electronic structure calculations journal July 1988
Improved relativistic energy-consistent pseudopotentials for 3d-transition metals journal September 2005
Pseudopotential methods in condensed matter applications journal April 1989
Relativistic Pseudopotentials: Their Development and Scope of Applications journal September 2011
Towards an exact description of electronic wavefunctions in real solids journal December 2012
Soft pseudopotentials for efficient quantum Monte Carlo calculations: From Be to Ne and Al to Ar journal May 2001
Exact decoupling of the Dirac Hamiltonian. I. General theory journal August 2004
Systematically convergent basis sets for transition metals. I. All-electron correlation consistent basis sets for the 3d elements Sc–Zn journal August 2005
Energy-consistent pseudopotentials for quantum Monte Carlo calculations journal June 2007
Energy-consistent small-core pseudopotentials for 3d-transition metals adapted to quantum Monte Carlo calculations journal October 2008
Compact effective potentials and efficient shared‐exponent basis sets for the first‐ and second‐row atoms journal December 1984
Ab initio relativistic effective potentials with spin‐orbit operators. I. Li through Ar journal March 1985
Energy‐adjusted a b i n i t i o pseudopotentials for the first row transition elements journal January 1987
Generation of pseudopotentials from correlated wave functions journal June 1994
Norm-conserving pseudopotentials with chemical accuracy compared to all-electron calculations journal March 2013
Communication: Toward an improved control of the fixed-node error in quantum Monte Carlo: The case of the water molecule journal April 2016
Shape and energy consistent pseudopotentials for correlated electron systems journal May 2017
Magnitude of pseudopotential localization errors in fixed node diffusion quantum Monte Carlo journal June 2017
A new generation of effective core potentials for correlated calculations journal December 2017
A new generation of effective core potentials from correlated calculations: 2nd row elements journal September 2018
Application of the multireference equation of motion coupled cluster method, including spin–orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co journal July 2015
Pseudopotentials that work: From H to Pu journal October 1982
Soft self-consistent pseudopotentials in a generalized eigenvalue formalism journal April 1990
Efficient pseudopotentials for plane-wave calculations journal January 1991
Separable dual-space Gaussian pseudopotentials journal July 1996
Optimized norm-conserving Vanderbilt pseudopotentials journal August 2013
Quantum Monte Carlo applied to solids journal December 2013
Pseudopotentials for quantum Monte Carlo studies of transition metal oxides journal February 2016
Ab initio Quantum Monte Carlo Calculations of Spin Superexchange in Cuprates: The Benchmarking Case of Ca 2 CuO 3 journal July 2014
Shape and energy consistent pseudopotentials for correlated electron systems text January 2017
Ab initio quantum Monte Carlo calculations of spin superexchange in cuprates: the benchmarking case of Ca$_2$CuO$_3$ text January 2014
Magnitude of pseudopotential localization errors in fixed node diffusion quantum Monte Carlo text January 2017
Separable Dual Space Gaussian Pseudo-potentials text January 1995
Application of the multireference equation of motion coupled cluster method, including spin–orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co text January 2015
Application of the multireference equation of motion coupled cluster method, including spin–orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co text January 2015
Application of the multireference equation of motion coupled cluster method, including spin–orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co text January 2015

Cited By (6)

The Role of High-Order Electron Correlation Effects in a Model System for Non-valence Correlation-bound Anions text January 2020
A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: Improving reproducibility and reducing the trial-wave-function bias journal October 2019
A new generation of effective core potentials from correlated calculations: 4s and 4p main group elements and first row additions journal October 2019
Variational and diffusion quantum Monte Carlo calculations with the CASINO code journal April 2020
Diffusion quantum Monte Carlo calculations with a recent generation of effective core potentials for ionization potentials and electron affinities journal December 2019
Variational and Diffusion Quantum Monte Carlo Calculations with the CASINO Code text January 2020

Figures / Tables (66)

FIG. 1(p. 3)figure FIG. 1
FIG. 2(p. 6)figure FIG. 2
FIG. 3(p. 7)figure FIG. 3
TABLE I(p. 7)table TABLE I
FIG. 4(p. 8)figure FIG. 4
Table II(p. 8)table Table II
FIG. 5(p. 9)figure FIG. 5
Table III(p. 9)table Table III
FIG. 6(p. 10)figure FIG. 6
TABLE IV(p. 10)table TABLE IV
FIG. 7(p. 11)figure FIG. 7
TABLE V(p. 11)table TABLE V
FIG. 8(p. 12)figure FIG. 8
TABLE VI(p. 12)table TABLE VI
FIG. 9(p. 13)figure FIG. 9
TABLE VII(p. 13)table TABLE VII
FIG. 10(p. 14)figure FIG. 10
TABLE VIII(p. 14)table TABLE VIII
FIG. 11(p. 15)figure FIG. 11
TABLE IX(p. 15)table TABLE IX
FIG. 12(p. 16)figure FIG. 12
TABLE X(p. 16)table TABLE X
TABLE XI(p. 16)table TABLE XI
FIG. 13(p. 17)figure FIG. 13
TABLE XII(p. 18)table TABLE XII
TABLE XIII(p. 19)table TABLE XIII
TABLE XIV(p. 19)table TABLE XIV
TABLE I(p. 24)table TABLE I
TABLE II(p. 25)table TABLE II
Table III(p. 25)table Table III
TABLE IV(p. 26)table TABLE IV
TABLE V(p. 26)table TABLE V
TABLE VI(p. 26)table TABLE VI
TABLE VII(p. 27)table TABLE VII
TABLE VIII(p. 27)table TABLE VIII
TABLE IX(p. 28)table TABLE IX
TABLE X(p. 28)table TABLE X
TABLE XI(p. 29)table TABLE XI
TABLE XII(p. 30)table TABLE XII
TABLE XIII(p. 30)table TABLE XIII
TABLE XIV(p. 31)table TABLE XIV
TABLE XV(p. 32)table TABLE XV
TABLE XVI(p. 33)table TABLE XVI
TABLE XVII(p. 33)table TABLE XVII
TABLE XIX(p. 34)table TABLE XIX
TABLE XVIII(p. 34)table TABLE XVIII
TABLE XX(p. 35)table TABLE XX
TABLE XXI(p. 35)table TABLE XXI
TABLE XXII(p. 36)table TABLE XXII
TABLE XXIV(p. 37)table TABLE XXIV
Table XXV(p. 38)table Table XXV
Table XXVI(p. 38)table Table XXVI
TABLE XXVII(p. 39)table TABLE XXVII
TABLE XXVIII(p. 39)table TABLE XXVIII
TABLE XXIX(p. 40)table TABLE XXIX
TABLE XXX(p. 40)table TABLE XXX
TABLE XXXI(p. 41)table TABLE XXXI
TABLE XXXII(p. 41)table TABLE XXXII
TABLE XXXIII(p. 41)table TABLE XXXIII
TABLE XXXIV(p. 42)table TABLE XXXIV
Table XXXV(p. 43)table Table XXXV
Table XXXVI(p. 43)table Table XXXVI
TABLE XXXVII(p. 44)table TABLE XXXVII
TABLE XXXVIII(p. 44)table TABLE XXXVIII
TABLE XXXIX(p. 45)table TABLE XXXIX
TABLE XL(p. 46)table TABLE XL

Similar Records

New generation of effective core potentials from correlated calculations: 2nd row elements
Journal Article · Fri Sep 14 00:00:00 EDT 2018 · Journal of Chemical Physics · OSTI ID:1441470
A new generation of effective core potentials for correlated calculations
Journal Article · Mon Dec 11 23:00:00 EST 2017 · Journal of Chemical Physics · OSTI ID:1421640

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
correlation energy
effective core potentials
molecular properties
oxides
transition metals