We present a parallel implementation of a large-scale relativistic double-group configuration interaction (CI) program. It is applicable with a large variety of two- and four-component Hamiltonians. The parallel algorithm is based on a distributed data model in combination with a static load balancing scheme. The excellent scalability of our parallelization scheme is demonstrated in large-scale four-component multireference CI (MRCI) benchmark tests on two of the most common computer architectures, and we also discuss hardware-dependent aspects with respect to possible speedup limitations. With the new code we have been able to calculate accurate spectroscopic properties for the ground state and the first excited state of the BiH molecule using extensive basis sets. We focused, in particular, on an accurate description of the splitting of these two states which is caused by spin-orbit coupling. Our largest parallel MRCI calculation thereby comprised an expansion length of Slater determinants.
REFERENCES
1.
B. A.
Hess
and C. M.
Marian
, in Computational Molecular Spectroscopy
, edited by P.
Jensen
and P. R.
Buenker
(Wiley
, Sussex
, 1999
).2.
T.
Fleig
, in Relativistic Methods for Chemists
, edited by M.
Barysz
and Y.
Ishikawa
(Springer
, Berlin
, 2010
).3.
C. M.
Marian
, in Reviews in Computational Chemistry
, edited by K.
Lipkowitz
and D.
Boyd
(Wiley-VCH
, Weinheim
, 2001
), Vol. 17
, p. 99
.4.
S.
Yabushita
, Z.
Zhang
, and R. M.
Pitzer
, J. Phys. Chem.
103
, 5791
(1999
).5.
V.
Vallet
, L.
Maron
, C.
Teichteil
, and J. P.
Flament
, J. Chem. Phys.
113
, 1391
(2000
).6.
B. O.
Roos
and P.-Å.
Malmqvist
, Phys. Chem. Chem. Phys.
6
, 2919
(2004
).7.
M.
Kleinschmidt
, J.
Tatchen
, and C. M.
Marian
, J. Chem. Phys.
124
, 124101
(2006
).8.
H.-S.
Lee
, Y.-K.
Han
, M. C.
Kim
, C.
Bae
, and Y. S.
Lee
, Chem. Phys. Lett.
293
, 97
(1998
).9.
T.
Fleig
, Phys. Rev. A
72
, 052506
(2005
).10.
T.
Fleig
, H. J. Aa.
Jensen
, J.
Olsen
, and L.
Visscher
, J. Chem. Phys.
124
, 104106
(2006
).11.
L.
Visscher
and T.
Saue
, J. Chem. Phys.
113
, 3996
(2000
).12.
T.
Fleig
, J.
Olsen
, and C. M.
Marian
, J. Chem. Phys.
114
, 4775
(2001
).13.
T.
Fleig
, J.
Olsen
, and L.
Visscher
, J. Chem. Phys.
119
, 2963
(2003
).14.
DIRAC, a relativistic ab initio electronic structure program, Release DIRAC08 (
2008
), written by L.
Visscher
, H. J. Aa.
Jensen
, and T.
Saue
, with new contributions from R.
Bast
, S.
Dubillard
, K. G.
Dyall
, U.
Ekström
, E.
Eliav
, T.
Fleig
, A. S. P.
Gomes
, T. U.
Helgaker
, J.
Henriksson
, M.
Iliaš
, Ch. R.
Jacob
, S.
Knecht
, P.
Norman
, J.
Olsen
, M.
Pernpointner
, K.
Ruud
, P.
Salek
, and J.
Sikkema
(see http://dirac.chem.sdu.dk).15.
S.
Knecht
, H. J. Aa.
Jensen
, and T.
Fleig
, J. Chem. Phys.
128
, 014108
(2008
).16.
J.
Olsen
, B. O.
Roos
, P.
Jørgensen
, and H. J. Aa.
Jensen
, J. Chem. Phys.
89
, 2185
(1988
).17.
J.
Olsen
, P.
Jørgensen
, and J.
Simons
, Chem. Phys. Lett.
169
, 463
(1990
).18.
T.
Fleig
and L.
Visscher
, Chem. Phys.
311
, 113
(2005
).19.
G. F.
Koster
, J. O.
Dimmock
, R. G.
Wheeler
, and H.
Statz
, Properties of the Thirty-Two Point Groups
(Massachusetts Institute of Technology
, Cambridge, MA
, 1963
).20.
H. J. Aa.
Jensen
, K. G.
Dyall
, T.
Saue
, and K.
Fægri
, J. Chem. Phys.
104
, 4083
(1996
).21.
M.
Iliaš
and T.
Saue
, J. Chem. Phys.
126
, 064102
(2007
).22.
J.
Thyssen
, T.
Fleig
, and H. J. Aa.
Jensen
, J. Chem. Phys.
129
, 034109
(2008
).23.
S.
Knecht
, H. J. Aa.
Jensen
, and L. K.
Sørensen
(unpublished).25.
J.
Nieplocha
, B.
Palmer
, V.
Tipparaju
, M.
Krishnan
, H.
Trease
, and E.
Apra
, Int. J. High Perform. Comput. Appl.
20
, 203
(2006
).27.
M.
Wang
, A. J.
May
, and P. J.
Knowles
, Comput. Phys. Commun.
180
, 2673
(2009
).28.
M.
Klene
, M. A.
Robb
, M. J.
Frisch
, and P.
Celani
, J. Chem. Phys.
113
, 5653
(2000
).29.
Z.
Gan
, Y.
Alexeev
, M. S.
Gordon
, and R. A.
Kendall
, J. Chem. Phys.
119
, 47
(2003
).30.
B.
Suo
, G.
Zhai
, Y.
Wang
, Z.
Wen
, X.
Hu
, and L.
Li
, J. Comput. Chem.
26
, 88
(2005
).31.
K.
Tanaka
, Y.
Mochizuki
, T.
Ishikawa
, H.
Terashima
, and H.
Tokiwa
, Theor. Chem. Acc.
117
, 397
(2007
).32.
M.
Kleinschmidt
, C. M.
Marian
, M.
Waletzke
, and S.
Grimme
, J. Chem. Phys.
130
, 044708
(2009
).33.
Y.
Kurashige
and T.
Yanai
, J. Chem. Phys.
130
, 234114
(2009
).34.
M.
Kleinschmidt
(private communication).35.
A.
Heimer
, Z. Phys.
95
, 328
(1935
).36.
A.
Heimer
and E.
Hulthén
, Nature (London)
127
, 557
(1931
).37.
E.
Hulthén
and A.
Heimer
, Nature (London)
129
, 399
(1932
).38.
B.
Lindgren
and Ch.
Nilsson
, J. Mol. Spectrosc.
55
, 407
(1975
).39.
H. G.
Hedderich
and P. F.
Bernath
, J. Mol. Spectrosc.
158
, 170
(1993
).40.
R. D.
Urban
, P.
Polomsky
, and H.
Jones
, Chem. Phys. Lett.
181
, 485
(1991
).41.
A. M. R. P.
Bopegedera
, C. R.
Brazier
, and P. F.
Bernath
, Chem. Phys. Lett.
162
, 301
(1989
).42.
K.
Balasubramanian
, Chem. Phys. Lett.
114
, 201
(1985
).43.
K.
Balasubramanian
, J. Mol. Spectrosc.
115
, 258
(1986
).44.
A. B.
Alekseyev
, R. J.
Buenker
, H. P.
Liebermann
, and G.
Hirsch
, J. Chem. Phys.
100
, 2989
(1994
).45.
G. A.
DiLabio
and P. A.
Christiansen
, Chem. Phys. Lett.
277
, 473
(1997
).46.
Y. K.
Han
, C.
Bae
, S. K.
Son
, and Y. S.
Lee
, J. Chem. Phys.
112
, 2684
(1999
).47.
H.
Stoll
, B.
Metz
, and M.
Dolg
, J. Comput. Chem.
23
, 767
(2001
).48.
T.
Zeng
, D. G.
Fedorov
, and M.
Klobukowski
, J. Chem. Phys.
131
, 124109
(2009
).49.
50.
B. A.
Hess
, C. M.
Marian
, U.
Wahlgren
, and O.
Gropen
, Chem. Phys. Lett.
251
, 365
(1996
).51.
B.
Schimmelpfennig
, program AMFI, Stockholm University
, Sweden, 1996
.52.
M.
Iliaš
, V.
Kello
, L.
Visscher
, and B.
Schimmelpfennig
, J. Chem. Phys.
115
, 9667
(2001
).53.
54.
K. G.
Dyall
, Theor. Chem. Acc.
109
, 284
(2003
).55.
K. G.
Dyall
, Theor. Chem. Acc.
115
, 441
(2006
).56.
T. H.
Dunning
, Jr., J. Chem. Phys.
90
, 1007
(1989
).57.
K. P.
Huber
and G.
Herzberg
, NIST Chemistry WebBook
, NIST Standard Reference Database Number 69, Eds. P. J.
Linstrom
and W. G.
Mallard
, National Institute of Standards and Technology
, Gaithersburg MD, 20899, http://webbook.nist.gov (retrieved 10 December 2008
).58.
L. K.
Sørensen
, J.
Olsen
, and T.
Fleig
(unpublished).59.
S. R.
Knecht
, “Parallel relativistic multiconfiguration methods: New powerful tools for heavy-element electronic-structure studies
,” Dissertation, Heinrich-Heine-Universität Düsseldorf
, 2009
. http://docserv.uni-duesseldorf.de/servlets/DocumentServlet?id=13226.60.
R.
Ansaloni
, G. L.
Bendazzoli
, S.
Evangelisti
, and E.
Rossi
, Comput. Phys. Commun.
128
, 496
(2000
).© 2010 American Institute of Physics.
2010
American Institute of Physics
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