Coherent population transfer in molecules coupled with a dissipative environment by intense ultrashort chirped pulse. II. A simple model

Abstract

We have developed a simple and physically clear picture of adiabatic rapid passage (ARP) in molecules in solution by careful examination of all the conditions needed for ARP. The relaxation effects were considered in the framework of the Landau-Zener model for random crossing of levels. The model enables us to include into consideration non-Markovian Gaussian-correlated noise. It explains all the numerical results obtained in the first paper of the series [B. D. Fainberg and V. A. Gorbunov, J. Chem. Phys. 117, 7222 (2002)], in particular, that for positive chirp pulse excitation relaxation favors more efficient population transfer with respect to the relaxation-free system with frozen nuclear motion. We also relate parameters of non-Markovian Gaussian-correlated noise with irreversible dephasing time of an optical transition by calculating the photon echo signal attenuation.

Adiabatic Passage in a Three-State System with Non-Markovian Relaxation: The Role of Excited-State Absorption and Two-Exciton Processes

“…(33), which is in excellent agreement with numerical calculations. In addition, the model gives us an extra criterion for coherent population transfer to those we have obtained before for a two-state system [27]. New criterion, Eq.…”

“…(34) expresses an extra criterion for coherent population transfer to those we have obtained before for a two-level system [27], Eqs. (17) and (18).…”

“…The picture of randomly fluctuating levels [27] offers a simple and physically clear explanation of numerical results [26] obtained for population transfer in a two-state system. Here we shall generalize the Landau-Zener (LZ) calculations putting in a third level [50] to random crossing of levels.…”

“…(26) over random crossing of levels described by Gaussian random noise induced by intra-and intermolecular fluctuations. It can be easily done for a differentiable ( non-Markovian) Gaussian process [27], bearing in mind an independence of α andα from each other for such processes. Therefore, we shall consider in this section a differentiable ( non-Markovian) Gaussian noise, as opposed to previuous sections.…”

Chirped-pulse manipulated carrier dynamics in low-temperature molecular-beam-epitaxy grown GaAs

“…Chirped-pulse manipulated carrier dynamics in low-temperature molecular-beam-epitaxy grown GaAs Selective carrier population transfer using chirped pulses has been extensively studied based on their potential applications in various areas, such as optical quantum control, [1][2][3][4][5][6][7][8] spectroscopy, 9 and Bose-Einstein condensates. 10 The chirped pulse control of carriers in direct band-gap semiconductors was discussed 11 to enable the optimization ultrafast optoelectronic devices under chirped pulse illumination.…”