Within a generic model, we discuss the possibility of coherent control of charge fluxes in unbiased molecular junctions. The control is induced by resonances between the Rabi frequency due to a pumping laser field and internal characteristic frequencies of pre-designed molecular donor-bridge-acceptor complexes. Two models are considered: a coherently controlled molecular charge pump and a molecular switch. The study generalizes previous consideration of light induced current [M. Galperin and A. Nitzan, Phys. Rev. Lett.95, 206802 (2005) https://doi.org/10.1103/PhysRevLett.95.206802] and of a molecular electron pump [R. Volkovich and U. Peskin, Phys. Rev. B83, 033403 (2011) https://doi.org/10.1103/PhysRevB.83.033403] and accounts for the coherently driven charge transport in an unbiased molecular junction with symmetric coupling to leads. Numerical examples demonstrate the feasibility of the control mechanism for realistic junctions parameters.

1.
A.
Nitzan
and
M. A.
Ratner
,
Science
300
,
1384
(
2003
).
2.
A. P.
Horsfield
,
D. R.
Bowler
,
H.
Ness
,
C. G.
Sanchez
,
T. N.
Todorov
, and
A. J.
Fisher
,
Rep. Prog. Phys.
69
,
1195
(
2006
).
3.
S.
Sanvito
and
A.
Rocha
,
J. Comput. Theor. Nanosci.
3
,
624
(
2006
).
4.
S. M.
Lindsay
and
M. A.
Ratner
,
Adv. Mater.
19
,
23
(
2007
).
5.
M.
Galperin
,
M. A.
Ratner
,
A.
Nitzan
, and
A.
Troisi
,
Science
319
,
1056
(
2008
).
6.
L.
Bogani
and
W.
Wernsdorfer
,
Nature Mater.
7
,
179
(
2008
).
7.
S.
Andergassen
,
V.
Meden
,
H.
Schoeller
,
J.
Splettstoesser
, and
M. R.
Wegewijs
,
Nanotechnology
21
,
272001
(
2010
).
8.
I.
Thanopoulos
,
E.
Paspalakis
, and
V.
Yannopapas
,
Nanotechnology
19
,
445202
(
2008
).
9.
W.
Haiss
,
T.
Albrecht
,
H.
van Zalinge
,
S. J.
Higgins
,
D.
Bethell
,
H.
Hoebenreich
,
D.
Schiffrin
,
R. J.
Nichols
,
A. M.
Kuznetsov
,
J.
Zhang
,
Q.
Chi
, and
J.
Ulstrup
,
J. Phys. Chem. B
111
,
6703
(
2007
).
10.
S.
Kohler
,
J.
Lehmann
, and
P.
Hanggi
,
Superlattices Microstruct.
34
,
419
(
2003
).
11.
C.
Patoux
,
C.
Coudret
,
J.-P.
Launay
,
C.
Joachim
, and
A.
Gourdon
,
Inorg. Chem.
36
,
5037
(
1997
).
12.
H.
Lee
,
Y.-C.
Cheng
, and
G. R.
Fleming
,
Science
316
,
1462
(
2007
).
13.
M.
Mayor
,
H. B.
Weber
,
J.
Reichert
,
M.
Elbing
,
C.
von Hanisch
,
D.
Beckmann
, and
M.
Fistcher
,
Angew. Chem. Int. Ed.
42
,
5834
(
2003
).
14.
M.
Shapiro
and
P.
Brumer
,
Principles of the Quantum Control of Molecular Processes
(
Wiley
,
New York
,
2003
).
15.
A.
Assion
,
T.
Baumert
,
M.
Bergt
,
T.
Brixner
,
B.
Kiefer
,
V.
Seyfried
,
M.
Strehle
, and
G.
Gerber
,
Science
282
,
919
(
1998
).
16.
C. A.
Stafford
,
D. M.
Cardamone
, and
S.
Mazumdar
,
Nanotechnology
18
,
424014
(
2007
).
17.
D. M.
Cardamone
,
C. A.
Stafford
, and
S.
Mazumdar
,
Nano Lett.
6
,
2422
(
2006
).
18.
R. H.
Goldsmith
,
M. R.
Wasilewski
, and
M. A.
Ratner
,
J. Am. Chem. Soc.
129
,
13066
(
2007
).
19.
G. C.
Solomon
,
D. Q.
Andrews
,
R. P.
van Duyne
, and
M. A.
Ratner
,
J. Am. Chem. Soc.
130
,
7788
(
2008
).
20.
G. C.
Solomon
,
D. Q.
Andrews
,
R. H.
Goldsmith
,
T.
Hansen
,
M. R.
Wasilewski
,
R. P.
van Duyne
, and
M. A.
Ratner
,
J. Am. Chem. Soc.
130
,
17301
(
2008
).
21.
G. C.
Solomon
,
D. Q.
Andrews
,
T.
Hansen
,
R. H.
Goldsmith
,
M. R.
Wasilewski
,
R. P.
van Duyne
, and
M. A.
Ratner
,
J. Chem. Phys.
129
,
054701
(
2008
).
22.
G. C.
Solomon
,
D. Q.
Andrews
,
R. P.
van Duyne
, and
M. A.
Ratner
,
ChemPhysChem
10
,
257
(
2009
).
23.
S.-H.
Ke
,
W.
Yang
, and
H. U.
Baranger
,
Nano Lett.
8
,
3257
(
2008
).
24.
G.-Q.
Li
,
M.
Schreiber
, and
U.
Kleinekathoefer
,
New J. Phys.
10
,
085005
(
2008
).
25.
G.-Q.
Li
,
M.
Schreiber
, and
U.
Kleinekathoefer
,
Europhys. Lett.
79
,
27006
(
2007
).
26.
Z.
Qian
,
R.
Li
,
X.
Zhao
,
S.
Hou
, and
S.
Sanvito
,
Phys. Rev. B
78
,
113301
(
2008
).
27.
J.
Franco
,
M.
Shapiro
, and
P.
Brumer
,
J. Chem. Phys.
128
,
244906
(
2008
).
28.
S.
Kohler
,
J.
Lehmann
, and
P.
Hanggi
,
Phys. Rep.
406
,
379
(
2005
).
29.
R.
Volkovich
and
U.
Peskin
,
Phys. Rev. B
83
,
033403
(
2011
).
30.
D. N.
Bertan
,
J. N.
Onuchichic
, and
J. J.
Hopfield
,
J. Chem. Phys.
86
,
4488
(
1987
).
31.
A. A.
Stuchebrukhov
,
J. Chem. Phys.
104
,
8424
(
1996
).
32.
I.
Franco
,
M.
Shapiro
, and
P.
Brumer
,
Phys. Rev. Lett.
99
,
126802
(
2007
).
33.
M.
Sukharev
and
M.
Galperin
,
Phys. Rev. B
81
,
165307
(
2010
).
34.
B. D.
Fainberg
,
M.
Sukharev
,
T.-H.
Park
, and
M.
Galperin
,
Phys. Rev. B
83
,
205425
(
2011
).
35.
A. P.
Jauho
,
N. S.
Wingreen
, and
Y.
Meir
,
Phys. Rev. B
50
,
5528
(
1994
).
36.
B.
Thimmel
,
P.
Nalbach
, and
O.
Terzidis
,
Eur. Phys. J. B
9
,
207
(
1999
).
37.
P.
Zhang
,
Q.-K.
Xue
, and
X. C.
Xie
,
Phys. Rev. Lett.
91
,
196602
(
2003
).
38.
F.
Grosmann
,
Phys. Rev. B
70
,
113306
(
2004
).
39.
M.
Strass
,
P.
Hanggi
, and
S.
Kohler
,
Phys. Rev. Lett.
95
,
130601
(
2005
).
40.
J.
Fransson
and
J.-X.
Zhu
,
Phys. Rev. B
78
,
113307
(
2008
).
41.
J.
Fransson
and
M.
Galperin
,
Phys. Rev. B
81
,
075311
(
2010
).
42.
J.
Fransson
and
M.
Galperin
,
Phys. Chem. Chem. Phys.
13
,
14350
(
2011
).
43.
L. D.
Landau
and
E. M.
Lifshitz
,
Quantum Mechanics. Non-relativistic Theory
(
Pergamon
,
New York
,
1991
).
44.
R.
Jorn
and
T.
Seideman
,
Acc. Chem. Res.
43
,
1186
(
2010
).
45.
M.
Galperin
and
A.
Nitzan
,
Phys. Rev. Lett.
95
,
206802
(
2005
).
46.
M.
Galperin
and
A.
Nitzan
,
J. Chem. Phys.
124
,
234709
(
2006
).
47.
B. D.
Fainberg
,
M.
Jouravlev
, and
A.
Nitzan
,
Phys. Rev. B
76
,
245329
(
2007
).
48.
M.
Esposito
and
M.
Galperin
,
Phys. Rev. B
79
,
205303
(
2009
).
49.
M.
Esposito
and
M.
Galperin
,
J. Phys. Chem. C
114
,
20362
(
2010
).
50.
H.-P.
Breuer
and
F.
Petruccione
,
The Theory of Open Quantum Systems
(
Oxford University Press
,
Oxford
,
2003
).
51.
A.
Nitzan
,
Chemical Dynamics in Condensed Phases
(
Oxford University Press
,
Oxford
,
2006
).
52.
M.
Leijnse
and
M. R.
Wegewijs
,
Phys. Rev. B
78
,
235424
(
2008
).
53.
S.
Koller
,
M.
Grifoni
,
M.
Leijnse
, and
M. R.
Wegewijs
,
Phys. Rev. B
82
,
235307
(
2010
).
54.
In Refs. 40 and 41, we have shown that in the case of quadratic Hamiltonian the QME equations are obtained from the NEGF formulation by substituting zero-order quasi-particle approximation in place of a full retarded Green function.
55.
R.
Volkovich
,
M.
Caspary Toroker
, and
U.
Peskin
,
J. Chem. Phys.
129
,
034501
(
2008
).
You do not currently have access to this content.