We theoretically study the exciton–exciton annihilation (EEA) in a molecular trimer MMM. The system is treated within a model of electronic states, and the coupling to a bath is incorporated using the quantum jump method. Two situations of initial excitation are compared. In the first one, a two-photon process populates configurations M*M*M and MM*M* so that two excitons reside on neighboring monomers M. Then, EEA can immediately proceed. In contrast, if the trimer initially is in the local configuration M*MM*, exciton diffusion must occur before the annihilation process can take place. For the trimer, this excitonic motion takes place on a very short time scale. In both cases, wave packets are prepared which show a different quantum dynamics where the latter depends on the couplings and decay rates. It is documented how fifth-order coherent two-dimensional spectroscopy can be used to directly map the EEA as a function of time.
REFERENCES
1.
R. S.
Knox
, Theory of Excitons
, Solid State Physics: Advances in Research and Applications Vol. 5 (Academic Press
, New York
, 1963
).2.
A. S.
Davydov
, Theory of Molecular Excitons
(Plenum
, New York
, 1971
).3.
V.
May
and O.
Kühn
, Charge and Energy Transfer Dynamics in Molecular Systems
, 3rd ed. (Wiley-VCH
, Weinheim
, 2011
).4.
The Physics and Chemistry of Wave Packets
, edited by J.
Yeazell
and T.
Uzer
(Wiley
, New York
, 2000
).5.
M.
Kasha
, Rev. Mod. Phys.
31
, 162
(1959
).6.
J.
Frenkel
, Phys. Rev.
37
, 17
(1931
).7.
J.
Süß
and V.
Engel
, J. Chem. Phys.
152
, 174305
(2020
).8.
Y.
Zaushitsyn
, K. G.
Jespersen
, L.
Valkunas
, V.
Sundström
, and A.
Yartsev
, Phys. Rev. B
75
, 195201
(2007
).9.
D. C.
Dai
and A. P.
Monkman
, Phys. Rev. B
87
, 045308
(2013
).10.
M. A.
Stevens
, C.
Silva
, D. M.
Russell
, and R. H.
Friend
, Phys. Rev. B
63
, 165213
(2001
).11.
S.
Cook
, H.
Liyuan
, A.
Furube
, and R.
Katoh
, J. Phys. Chem. C
114
, 10962
(2010
).12.
A. J.
Lewis
, A.
Ruseckas
, O. P. M.
Gaudin
, G. R.
Webster
, P. L.
Burn
, and I. D. W.
Samuel
, Org. Electron.
7
, 452
(2006
).13.
D.
Peckus
, A.
Devižis
, D.
Hertel
, K.
Meerholz
, and V.
Gulbinas
, Chem. Phys.
404
, 42
(2012
).14.
S.
Gòlinas
, J.
Kirkpatrick
, I. A.
Howard
, K.
Johnson
, M. W. B.
Wilson
, G.
Pace
, R. H.
Friend
, and C.
Silva
, J. Phys. Chem. B
117
, 4649
(2013
).15.
M.
Kasha
, Radiat. Res.
20
, 55
(1963
).16.
R. L.
Fulton
and M.
Gouterman
, J. Chem. Phys.
35
, 1059
(1961
).17.
M.
Schröter
, S. D.
Ivanov
, J.
Schulze
, S. P.
Polyutov
, Y.
Yan
, T.
Pullerits
, and O.
Kühn
, Phys. Rep.
567
, 1
(2015
).18.
B.
Engels
and V.
Engel
, Phys. Chem. Chem. Phys.
19
, 12604
(2017
).19.
H.
Marciniak
, X.-Q.
Li
, F.
Würthner
, and S.
Lochbrunner
, J. Phys. Chem. A
115
, 648
(2011
).20.
S.
Wolter
, J.
Aizezers
, F.
Fennel
, M.
Seidel
, F.
Würthner
, O.
Kühn
, and S.
Lochbrunner
, New J. Phys.
14
, 105027
(2012
).21.
F.
Fennel
and S.
Lochbrunner
, Phys. Rev. B
92
, 140301
(2015
).22.
S. F.
Völker
, A.
Schmiedel
, M.
Holzapfel
, K.
Renziehausen
, V.
Engel
, and C.
Lambert
, J. Phys. Chem. C
118
, 17467
(2014
).23.
K.
Hader
, V.
May
, C.
Lambert
, and V.
Engel
, Phys. Chem. Chem. Phys.
18
, 13368
(2016
).24.
K.
Hader
, C.
Consani
, T.
Brixner
, and V.
Engel
, Phys. Chem. Chem. Phys.
19
, 31989
(2017
).25.
J.
Dostál
, F.
Fennel
, F.
Koch
, S.
Herbst
, F.
Würthner
, and T.
Brixner
, Nat. Commun.
9
, 2466
(2018
).26.
P.
Malý
, J.
Lüttig
, A.
Turkin
, J.
Dostál
, C.
Lambert
, and T.
Brixner
, Chem. Sci.
11
, 456
(2020
).27.
D. M.
Jonas
, Annu. Rev. Phys. Chem.
54
, 425
(2003
).28.
F. D.
Fuller
and J. P.
Ogilvie
, Annu. Rev. Phys. Chem.
66
, 667
(2015
).29.
P.
Nuernberger
, S.
Ruetzel
, and T.
Brixner
, Angew. Chem., Int. Ed.
54
, 11368
(2015
).30.
B.
Brueggemann
and T.
Pullerits
, New J. Phys.
13
, 025024
(2011
).31.
J.
Süß
, J.
Wehner
, J.
Dostál
, T.
Brixner
, and V.
Engel
, J. Chem. Phys.
150
, 104304
(2019
).32.
T.
Renger
and V.
May
, Phys. Rev. Lett.
78
, 3406
(1997
).33.
B.
Brüggemann
, J. L.
Herek
, V.
Sundström
, T.
Pullerits
, and V.
May
, J. Phys. Chem. B
105
, 11391
(2001
).34.
K.
Mølmer
, Y.
Castin
, and J.
Dalibard
, J. Opt. Soc. Am. B
10
, 524
(1993
).35.
D. E.
Makarov
and H.
Metiu
, J. Chem. Phys.
111
, 10126
(1999
).36.
B.
Wolfseder
and W.
Domcke
, Chem. Phys. Lett.
235
, 370
(1995
).37.
P.
Saalfrank
, Chem. Phys.
211
, 265
(1996
).38.
J.
Albert
, M.
Falge
, M.
Keß
, J. G.
Wehner
, P.-P.
Zhang
, A.
Eisfeld
, and V.
Engel
, J. Chem. Phys.
142
, 212440
(2015
).39.
M.
Keß
and V.
Engel
, Chem. Phys. Lett.
650
, 41
(2016
).40.
F.
Glaab
, J. G.
Wehner
, C.
Lambert
, and V.
Engel
, J. Phys. Chem. A
123
, 5463
(2019
).41.
M.
Kasha
, Discuss. Faraday Soc.
9
, 14
(1950
).42.
D. J.
Tannor
, Introduction to Quantum Mechanics: A Time-Dependent Perspective
(University Science Books
, Sausalito
, 2007
).43.
P.
Kjellberg
, B.
Brüggemann
, and T.
Pullerits
, Phys. Rev. B
74
, 024303
(2006
).44.
S.
Mukamel
, Annu. Rev. Phys. Chem.
51
, 691
(2000
).© 2020 Author(s).
2020
Author(s)
You do not currently have access to this content.
