The local pseudopotential (LPP) is an important component of orbital-free density functional theory, a promising large-scale simulation method that can maintain information on a material’s electron state. The LPP is usually extracted from solid-state density functional theory calculations, thereby it is difficult to assess its transferability to cases involving very different chemical environments. Here, we reveal a fundamental relation between the first-principles norm-conserving pseudopotential (NCPP) and the LPP. On the basis of this relationship, we demonstrate that the LPP can be constructed optimally from the NCPP for a large number of elements using the optimized effective potential method. Specially, our method provides a unified scheme for constructing and assessing the LPP within the framework of first-principles pseudopotentials. Our practice reveals that the existence of a valid LPP with high transferability may strongly depend on the element.
REFERENCES
1.
Y. A.
Wang
and E. A.
Carter
, Theoretical Methods in Condensed Phase Chemistry
(Springer
, 2002
), pp. 117
–184
.2.
V. V.
Karasiev
and S. B.
Trickey
, Comput. Phys. Commun.
183
, 2519
(2012
).3.
T. A.
Wesolowski
, Recent Progress in Orbital-Free Density Functional Theory
, Recent Advances in Computational Chemistry
(World Scientific Publishing Company
, 2013
).4.
V. V.
Karasiev
, D.
Chakraborty
, and S.
Trickey
, Many-Electron Approaches in Physics, Chemistry and Mathematics
(Springer
, 2014
), pp. 113
–134
.5.
I.
Shin
and E. A.
Carter
, Modell. Simul. Mater. Sci. Eng.
20
, 015006
(2012
).6.
A. M.
Vora
, Phys. Chem. Liq.
48
, 723
(2010
).7.
V.
Lignres
and E.
Carter
, in Handbook of Materials Modeling
, edited by S.
Yip
(Springer
, Netherlands
, 2005
), pp. 137
–148
.8.
B.
Zhou
, V. L.
Ligneres
, and E. A.
Carter
, J. Chem. Phys.
122
, 044103
(2005
).9.
N.
Bhatt
, P.
Vyas
, A.
Jani
, and V.
Gohel
, J. Phys. Chem. Solids
66
, 797
(2005
).10.
H.
Jiang
and W.
Yang
, J. Chem. Phys.
121
, 2030
(2004
).11.
D. J.
González
, L. E.
González
, J. M.
López
, and M. J.
Stott
, J. Chem. Phys.
115
, 2373
(2001
).12.
M.
Pearson
, E.
Smargiassi
, and P.
Madden
, J. Phys.: Condens. Matter
5
, 3221
(1993
).13.
M. S.
Daw
and M. I.
Baskes
, Phys. Rev. B
29
, 6443
(1984
).14.
M. S.
Daw
and M. I.
Baskes
, Phys. Rev. Lett.
50
, 1285
(1983
).15.
C.
Huang
and E. A.
Carter
, Phys. Rev. B
81
, 045206
(2010
).16.
J.
Xia
, C.
Huang
, I.
Shin
, and E. A.
Carter
, J. Chem. Phys.
136
, 084102
(2012
).17.
W. E.
Pickett
, Comput. Phys. Rep.
9
, 115
(1989
).18.
D.
Vanderbilt
, Phys. Rev. B
41
, 7892
(1990
).19.
P.
Hohenberg
and W.
Kohn
, Phys. Rev.
136
, B864
(1964
).20.
W.
Kohn
and L. J.
Sham
, Phys. Rev.
140
, A1133
(1965
).21.
L.
Goodwin
, R.
Needs
, and V.
Heine
, J. Phys.: Condens. Matter
2
, 351
(1990
).22.
C.
Fiolhais
, J. P.
Perdew
, S. Q.
Armster
, J. M.
MacLaren
, and M.
Brajczewska
, Phys. Rev. B
51
, 14001
(1995
).23.
C.
Fiolhais
, J. P.
Perdew
, S. Q.
Armster
, J. M.
MacLaren
, and M.
Brajczewska
, Phys. Rev. B
53
, 13193
(1996
).24.
S.
Watson
, B.
Jesson
, E.
Carter
, and P.
Madden
, Europhys. Lett.)
41
, 37
(1998
).25.
B. J.
Jesson
and P. A.
Madden
, J. Chem. Phys.
113
, 5924
(2000
).26.
B.
Zhou
, Y.
Alexander Wang
, and E. A.
Carter
, Phys. Rev. B
69
, 125109
(2004
).27.
B.
Wang
and M. J.
Stott
, Phys. Rev. B
68
, 195102
(2003
).28.
B.
Zhou
and E. A.
Carter
, J. Chem. Phys.
122
, 184108
(2005
).29.
C.
Huang
and E. A.
Carter
, Phys. Chem. Chem. Phys.
10
, 7109
(2008
).30.
T.
Grabo
, T.
Kreibich
, S.
Kurth
, and E.
Gross
, in Strong Coulomb Correlations in Electronic Structure Calculations: Beyond Local Density Approximations
, edited by V.
Anisimov
(Gordon and Breach Science Publishers, Amsterdam
, 2000
), Vol. 203
.31.
J. C.
Slater
, Phys. Rev.
81
, 385
(1951
).32.
J.
Krieger
, Y.
Li
, and G.
Iafrate
, Density Functional Theory
, edited by E. K. U.
Gross
and R. M.
Dreizler
(Plenum Press
, New York
, 1995
), p. 191
.33.
D. M.
Bylander
and L.
Kleinman
, Phys. Rev. B
52
, 14566
(1995
).34.
M.
Miao
, Philos. Mag. B
80
, 409
(2000
).35.
S.
Kümmel
and J. P.
Perdew
, Phys. Rev. B
68
, 035103
(2003
).36.
D. R.
Hamann
, M.
Schlüter
, and C.
Chiang
, Phys. Rev. Lett.
43
, 1494
(1979
).37.
N.
Troullier
and J. L.
Martins
, Phys. Rev. B
43
, 1993
(1991
).38.
M.
Fuchs
and M.
Scheffler
, Comput. Phys. Commun.
119
, 67
(1999
).39.
See supplementary material at http://dx.doi.org/10.1063/1.4944989 for detailed derivation of the OEP equation for OEPP and test results of pseudo-atoms.
40.
S. G.
Louie
, S.
Froyen
, and M. L.
Cohen
, Phys. Rev. B
26
, 1738
(1982
).41.
L.
Kleinman
and D. M.
Bylander
, Phys. Rev. Lett.
48
, 1425
(1982
).42.
M.
Segall
, P. J.
Lindan
, M. J.
Probert
, C.
Pickard
, P.
Hasnip
, S.
Clark
, and M.
Payne
, J. Phys.: Condens. Matter
14
, 2717
(2002
).43.
D. M.
Ceperley
and B. J.
Alder
, Phys. Rev. Lett.
45
, 566
(1980
).44.
J. P.
Perdew
, K.
Burke
, and M.
Ernzerhof
, Phys. Rev. Lett.
77
, 3865
(1996
).45.
W.
Mi
, X.
Shao
, C.
Su
, Y.
Zhou
, S.
Zhang
, Q.
Li
, H.
Wang
, L.
Zhang
, M.
Miao
, Y.
Wang
et al., Comput. Phys. Commun.
200
, 87
(2016
).46.
Y. A.
Wang
, N.
Govind
, and E. A.
Carter
, Phys. Rev. B
60
, 16350
(1999
).47.
A.
Nagy
, Phys. Rev. A
55
, 3465
(1997
).48.
G. B.
Bachelet
, D. R.
Hamann
, and M.
Schlüter
, Phys. Rev. B
26
, 4199
(1982
).49.
G.
Kerker
, J. Phys. C: Solid State Phys.
13
, L189
(1980
).50.
D.
Vanderbilt
, Phys. Rev. B
32
, 8412
(1985
).51.
F.
Birch
, Phys. Rev.
71
, 809
(1947
).53.
J.
Lehtomäki
, I.
Makkonen
, M. A.
Caro
, A.
Harju
, and O.
Lopez-Acevedo
, J. Chem. Phys.
141
, 234102
(2014
).© 2016 AIP Publishing LLC.
2016
AIP Publishing LLC
You do not currently have access to this content.
