The forward–backward semiclassical dynamics methodology [J. Phys. Chem. 103, 7753, 9479 (1999)] is reformulated in the interaction representation. The new version of the method allows for a fully quantum mechanical description of a low-dimensional subsystem of interest, along with a semiclassical forward–backward treatment of the solvent coordinates and their coupling to the reference subsystem. Application to the long-time tunneling dynamics in a symmetric double-well system coupled to a harmonic bath shows that the interaction FBSD is capable of capturing quantitatively the tunneling and decoherence effects induced by weakly dissipative environments.
REFERENCES
1.
2.
3.
4.
5.
W. H.
Miller
, Adv. Chem. Phys.
25
, 69
(1974
).6.
W. H.
Miller
, Adv. Chem. Phys.
30
, 77
(1975
).7.
M. S. Child, Semiclassical Mechanics with Molecular Applications (Clarendon, Oxford, 1991).
8.
M. A.
Sepulveda
, S.
Tomsovic
, and E. J.
Heller
, Phys. Rev. Lett.
69
, 402
(1992
).9.
10.
M. A.
Sepulveda
and F.
Grossmann
, Adv. Chem. Phys.
XCVI
, 191
(1996
).11.
S.
Garashchuk
, F.
Grossmann
, and D.
Tannor
, J. Chem. Soc., Faraday Trans.
93
, 781
(1997
).12.
13.
14.
15.
16.
17.
18.
19.
20.
21.
22.
23.
A. R.
Walton
and D. E.
Manolopoulos
, Mol. Phys.
84
, 961
(1996
).24.
M. L.
Brewer
, J. S.
Hulme
, and D. E.
Manolopoulos
, J. Chem. Phys.
106
, 4832
(1997
).25.
26.
27.
28.
V.
Batista
, M. T.
Zanni
, J.
Greenblatt
, D. M.
Neumark
, and W. H.
Miller
, J. Chem. Phys.
110
, 3736
(1999
).29.
30.
31.
32.
33.
34.
35.
36.
37.
38.
39.
40.
41.
42.
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