M. Grifoni et al., DISSIPATIVE TUNNELING WITH PERIODIC POLYCHROMATIC DRIVING - EXACT RESULTS AND TRACTABLE APPROXIMATIONS, Chemical physics, 217(2-3), 1997, pp. 167-178
We investigate the long-time dynamics in dissipative two-level-systems
(TLS) when driven by - monochromatic or pulse-shaped - periodic field
s. The environmental influence is investigated within the noninteracti
ng-blip appoximation (NIBA), while no restrictions are assumed on the
driving force. With the focus being on electron-transfer (ET) reaction
s in condensed media, we consider a continuous Ohmic spectrum for the
bath modes. The asymptotic dynamics exhibits always the periodicity of
the external force. The induced oscillations show a smooth periodic b
ehavior which becomes richer, if, for example, multiphoton resonances
occur. For monochromatic driving, the oscillatory multiresonance patte
rn becomes gradually smoothed out when the temperature, and/or the Ohm
ic strength are sufficiently high. It may persist, however, for pulse-
shaped driving. Exact NIBA analytical and/or numerical solutions, for
both the Ohmic transfer rate and for the driven dynamics, are used to
determine the validity range of the short-time approximation for the b
ath correlation functions. The latter is frequently employed to invest
igate the ET dynamics. Our analysis shows that the short-time approxim
ation may give qualitative incorrect results at low temperatures. (C)
1997 Elsevier Science B.V.