Using a diagrammatic superoperator formalism we calculate optical signals at molecular junctions where a single molecule is coupled to two metal leads which are held at different chemical potentials. The molecule starts in a nonequilibrium steady state whereby it continuously exchanges electrons with the leads with a constant electron flux. Expressions for frequency domain optical signals measured in response to continuous laser fields are derived by expanding the molecular correlation functions in terms of its many-body states. The nonunitary evolution of molecular states is described by the quantum master equation.
REFERENCES
1.
W. E.
Moerner
and L.
Orrit
, Science
283
, 1670
(1999
).2.
W. E.
Moerner
and L.
Kador
, Phys. Rev. Lett.
62
, 2535
(1989
).3.
D.
Brinks
, R.
Hinder
, E. M. H. P.
van Dijk
, F. D.
Stefani
, J. B.
Nieder
, J.
Hernando
, and N. F.
van Hulst
, R. Soc. Chem.
43
, 2476
(2014
).4.
M. D.
Levenson
, Phys. Today
30
, 44
(1977
).5.
S.
Rahav
and S.
Mukamel
, PNAS
107
, 4825
(2010
).6.
S.
Rahav
, O.
Roslyak
, and S.
Mukamel
, J. Chem. Phys.
131
, 194510
(2009
).7.
S.
Datta
, Electronic Transport in Mesoscopic Systems
(Cambridge University Press
, Cambridge
, 1997
).8.
Y. H.
Kwok
, H.
Xie
, C. Y.
Yam
, X.
Zheng
, and G. H.
Chen
, J. Chem. Phys.
139
, 224111
(2013
);
[PubMed]
X.
Zheng
, F.
Wang
, C. Y.
Yam
, Y.
Mo
, and G. H.
Chen
, Phys. Rev. B
75
, 195127
(2007
).9.
10.
S.
Ballmann
, R.
Härtle
, P. B.
Coto
, M.
Elbing
, M.
Mayor
, M. R.
Bryce
, M.
Thoss
, and H. B.
Weber
, Phys. Rev. Lett.
109
, 056801
(2012
).11.
U.
Harbola
, M.
Esposito
, and S.
Mukamel
, Phys. Rev. B
74
, 235309
(2006
).12.
R.
Zhang
, Y.
Zhang
, Z. C.
Dong
, S.
Jiang
, C.
Zhang
, L. G.
Chen
, L.
Zhang
, Y.
Liao
, J.
Aizpurua
, Y.
Luo
, J. L.
Yang
, and J. G.
Hou
, Nature (London)
498
, 82
(2013
).13.
X. H.
Qiu
, G. V.
Nazin
, and W.
Ho
, Science
299
, 542
(2003
).14.
J. H.
Tian
, B.
Liu
, X.
Li
, Z.-L.
Yang
, B.
Ren
, S.-T.
Wu
, N.
Tao
, and Z.-Q.
Tian
, J. Am. Chem. Soc.
128
, 14748
(2006
).15.
D. R.
Ward
, N. J.
Halas
, J. W.
Ciszek
, J. M.
Tour
, Y.
Wu
, P.
Nordlander
, and D.
Natelson
, Nano Lett.
8
, 919
(2008
).16.
M.
Galperin
and A.
Nitzan
, Phys. Rev. Lett.
95
, 206802
(2005
).17.
U.
Harbola
, J. B.
Maddox
, and S.
Mukamel
, Phys. Rev. B
73
, 075211
(2006
).18.
M.
Galperin
, M. A.
Ratner
, and A.
Nitzan
, J. Chem. Phys.
130
, 144109
(2009
).19.
M.
Galperin
and A.
Nitzan
, J. Phys. Chem. Lett.
2
, 2110
–2113
(2011
);20.
C. A.
Marx
, U.
Harbola
, and S.
Mukamel
, Phys. Rev. A
77
, 022110
(2008
).21.
U.
Harbola
and S.
Mukamel
, Phys. Rep.
465
, 191
(2008
).22.
S.
Mukamel
, Phys. Rev. A
71
, 024503
(2005
).23.
24.
J.-S.
Wang
, B. K.
Agarwalla
, H.
Li
, and J.
Thingna
, Front. Phys.
1
, (2013
).25.
H.
Haug
and A. P.
Jauho
, Quantum Kinetics in Transport and Optics of Semiconductors
(Springer-Verlag
, Berlin, Heidelberg
, 2008
).26.
G.
Lindblad
, Commun. Math. Phys.
48
, 119
(1976
).27.
S.
Rahav
and S.
Mukamel
, J. Chem. Phys.
133
, 244106
(2010
).28.
S.
Mukamel
, Principles of Nonlinear Optical Spectroscopy
(Oxford University Press
, Oxford
, 1995
).29.
E. O.
Potma
and S.
Mukamel
, in Coherent Raman Scattering Microscopy
, edited by J.-X.
Cheng
and X. S.
Xie
(Taylor and Francis Group
, 2013
), Chap. 1.30.
D.
Brinks
, F. D.
Stefani
, F.
Kulzer
, R.
Hildner
, T. H.
Taminiau
, Y.
Avlasevich
, K.
Müllen
, and N. F.
van Hulst
, Nature (London)
465
, 905
(2010
).© 2014 AIP Publishing LLC.
2014
AIP Publishing LLC
You do not currently have access to this content.
