This work implements a variational determination of the elements of two-electron reduced density matrices corresponding to the ground and excited states of N-electron interacting systems based on the dispersion operator technique. The procedure extends the previously reported proposal [Nakata et al., J. Chem. Phys. 125, 244109 (2006)] to two-particle interaction Hamiltonians and N-representability conditions for the two-, three-, and four-particle reduced density matrices in the doubly occupied configuration interaction space. The treatment has been applied to describe electronic spectra using two benchmark exactly solvable pairing models: reduced Bardeen–Cooper–Schrieffer and Richardson–Gaudin–Kitaev Hamiltonians. The dispersion operator combined with N-representability conditions up to the four-particle reduced density matrices provides excellent results.

1.
A. J.
Coleman
,
Rev. Mod. Phys.
35
,
668
(
1963
).
2.
C.
Garrod
and
J. K.
Percus
,
J. Math. Phys.
5
,
1756
(
1964
).
3.
R. M.
Erdahl
,
Int. J. Quantum Chem.
13
,
697
718
(
1978
).
4.
D. A.
Mazziotti
and
R. M.
Erdahl
,
Phys. Rev. A
63
,
042113
(
2001
).
5.
D. A.
Mazziotti
,
Phys. Rev. A
65
,
062511
(
2002
).
6.
M. V.
Mihailovic
and
M.
Rosina
,
Nucl. Phys. A
237
,
221
(
1975
).
7.
J. R.
Hammond
and
D. A.
Mazziotti
,
Phys. Rev. A
73
,
062505
(
2006
).
8.
S.
Kais
, in
Reduced-Density-Matrix Mechanics: With Applications to Many-Electron Atoms and Molecules
, Advances in Chemical Physics Vol. 134, edited by
D. A.
Mazziotti
(
Wiley-Interscience
,
Hoboken, NJ
,
2007
).
9.
D. R.
Alcoba
,
R. C.
Bochicchio
,
L.
Lain
, and
A.
Torre
,
J. Chem. Phys.
133
,
144104
(
2010
).
10.
M.
Nakata
,
B. J.
Braams
,
M.
Fukuda
,
J. K.
Percus
,
M.
Yamashita
, and
Z.
Zhao
,
J. Chem. Phys.
125
,
244109
(
2006
).
11.
H.-Z.
Ye
,
M.
Welborn
,
N. D.
Ricke
, and
T.
Van Voorhis
,
J. Chem. Phys.
147
,
214104
(
2017
).
12.
E. V.
Ludeña
,
F. J.
Torres
, and
C.
Costa
,
J. Mod. Phys.
4
,
391
(
2013
).
13.
T.
Matsubara
and
H.
Matsuda
,
Prog. Theor. Phys.
16
,
569
(
1956
);
T.
Matsubara
and
H.
Matsuda
17
,
19
(
1957
).
14.
J.
Bardeen
,
L. N.
Cooper
, and
J. R.
Schrieffer
,
Phys. Rev.
108
,
1175
(
1957
).
15.
R. W.
Richardson
,
Phys. Rev.
141
,
949
956
(
1966
).
16.
A. Y.
Kitaev
,
Phys.-Usp.
44
,
131
(
2001
).
17.
G.
Ortiz
,
J.
Dukelsky
,
E.
Cobanera
,
C.
Esebbag
, and
C.
Beenakker
,
Phys. Rev. Lett.
113
,
267002
(
2014
).
18.
R. M.
Erdahl
and
H.
Grudziński
,
Rep. Math. Phys.
14
,
405
(
1978
).
19.
R.
Erdahl
and
B.
Jin
, in
Many-Electron Densities and Reduced Density Matrices
, Mathematical and Computational Chemistry book series, edited by
J.
Cioslowski
(
Kluwer
,
Boston, MA
,
2000
), Chap. 4, pp.
57
84
.
20.
P.
Ring
and
P.
Schuck
,
The Nuclear Many-Body Problem
(
Springer-Verlag
,
New York
,
1980
).
21.
D. S.
Koltun
and
J. M.
Eisenberg
,
Quantum Mechanics of Many Degrees of Freedom
(
Wiley
,
New York
,
1988
).
22.
L.
Bytautas
,
T. M.
Henderson
,
C. A.
Jiménez-Hoyos
,
J. K.
Ellis
, and
G. E.
Scuseria
,
J. Chem. Phys.
135
,
044119
(
2011
).
23.
F.
Weinhold
and
E. B.
Wilson
,
J. Chem. Phys.
46
,
2752
(
1967
).
24.
F.
Weinhold
and
E. B.
Wilson
,
J. Chem. Phys.
47
,
2298
(
1967
).
25.
T. M.
Henderson
,
I. W.
Bulik
, and
G. E.
Scuseria
,
J. Chem. Phys.
142
,
214116
(
2015
).
26.
W.
Poelmans
,
M.
Van Raemdonck
,
B.
Verstichel
,
S.
De Baerdemacker
,
A.
Torre
,
L.
Lain
,
G. E.
Massaccesi
,
D. R.
Alcoba
,
P.
Bultinck
, and
D.
Van Neck
,
J. Chem. Theory Comput.
11
,
4064
4076
(
2015
).
27.
D. R.
Alcoba
,
A.
Torre
,
L.
Lain
,
G. E.
Massaccesi
,
O. B.
Oña
,
E. M.
Honoré
,
W.
Poelmans
,
D.
Van Neck
,
P.
Bultinck
, and
S.
De Baerdemacker
,
J. Chem. Phys.
148
,
024105
(
2018
).
28.
D. R.
Alcoba
,
A.
Torre
,
L.
Lain
,
G. E.
Massaccesi
,
O. B.
Oña
, and
E.
Ríos
,
J. Chem. Phys.
150
,
164106
(
2019
).
29.
O. B.
Oña
,
A.
Torre
,
L.
Lain
,
D. R.
Alcoba
,
E.
Ríos
, and
G. E.
Massaccesi
,
J. Chem. Phys.
153
,
084101
(
2020
).
30.
D. R.
Alcoba
,
P.
Capuzzi
,
A.
Rubio-García
,
J.
Dukelsky
,
G. E.
Massaccesi
,
O. B.
Oña
,
A.
Torre
, and
L.
Lain
,
J. Chem. Phys.
149
,
194105
(
2018
).
31.
A.
Rubio-García
,
J.
Dukelsky
,
D. R.
Alcoba
,
P.
Capuzzi
,
O. B.
Oña
,
E.
Ríos
,
A.
Torre
, and
L.
Lain
,
J. Chem. Phys.
151
,
154104
(
2019
).
32.
G. E.
Massaccesi
,
A.
Rubio-García
,
P.
Capuzzi
,
E.
Ríos
,
O. B.
Oña
,
J.
Dukelsky
,
L.
Lain
,
A.
Torre
, and
D. R.
Alcoba
,
J. Stat. Mech.: Theory Exp.
2021
,
013110
.
33.
J. A.
Gomez
,
T. M.
Henderson
, and
G. E.
Scuseria
,
J. Chem. Phys.
150
,
144108
(
2019
).
34.
J.
Dukelsky
,
C.
Esebbag
, and
P.
Schuck
,
Phys. Rev. Lett.
87
,
066403
(
2001
).
35.
J.
Dukelsky
,
S.
Pittel
, and
G.
Sierra
,
Rev. Mod. Phys.
76
,
643
662
(
2004
).
36.
G.
Ortiz
,
R.
Somma
,
J.
Dukelsky
, and
S.
Rombouts
,
Nucl. Phys. B
707
,
421
457
(
2005
).
37.
M.
Piris
and
R.
Cruz
,
Int. J. Quantum Chem.
53
,
353
(
1995
).
38.
G.
Sierra
,
J.
Dukelsky
,
G. G.
Dussel
,
J.
von Delft
, and
F.
Braun
,
Phys. Rev. B
61
,
R11890
R11893
(
2000
).
39.
A.
Rubio-García
,
D. R.
Alcoba
,
P.
Capuzzi
, and
J.
Dukelsky
,
J. Chem. Theory Comput.
14
,
4183
4192
(
2018
).
40.
A. J.
Coleman
and
V. I.
Yukalov
,
Reduced Density Matrices: Coulson’s Challenge
, Lecture Notes in Chemistry (
Springer-Verlag
,
New York
,
2000
).
41.
G.
Moore
and
N.
Read
,
Nucl. Phys. B
360
,
362
396
(
1991
).
42.
M.
Ibañez
,
J.
Links
,
G.
Sierra
, and
S.-Y.
Zhao
,
Phys. Rev. B
79
,
180501(R)
(
2009
).
43.
S. M. A.
Rombouts
,
J.
Dukelsky
, and
G.
Ortiz
,
Phys. Rev. B
82
,
224510
(
2010
).
44.
M.
Yamashita
,
K.
Fujisawa
,
K.
Nakata
,
M.
Nakata
,
M.
Fukuda
,
K.
Kobayashi
, and
K.
Goto
, “
A high-performance software package for semidefinite programs: SDPA 7
,” Technical Report B-460,
Department of Mathematical and Computing Science, Tokyo Institute of Technology
,
2010
.
45.
M.
Yamashita
,
K.
Fujisawa
,
M.
Fukuda
,
K.
Kobayashi
,
K.
Nakata
, and
M.
Nakata
, in
Semidefinite, Cone and Polynomial Optimization
, edited by
M. F.
Anjos
and
J. B.
Lasserre
(
Springer
,
New York
,
2011
), p.
687
.
46.
M.
Nakata
, “
A numerical evaluation of highly accurate multiple-precision arithmetic version of semidefinite programming solver: SDPA-GMP, -QD and -DD
,” in
Proceedings of the 2010 IEEE Multi-Conference on Systems and Control
(
IEEE
,
2010
), pp.
29
34
.
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