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Chemical Physics Letters

Disorder and spectral line shapes in two-level systems

Prathamesh Mahesh Shenai, Wu-Jun Shi, Vladimir Chernyak, Yang Zhao

Published Jul 20, 2013• 1 citation
Publisher
DOI
10.1016/j.cplett.2013.07.032

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We have carried out a theoretical and numerical study of disorder-induced changes in the absorption line shape of a chromophore embedded in a host matrix. The stochastic sudden jump model is employed wherein the host matrix molecules are treated as noninteracting two-level systems (TLSs) occupying points on a three-dimensional lattice with randomly oriented dipole moments. By systematically controlling the degree of positional disorder (α) attributed to them, a perfectly crystalline (α = 0) or a glassy environment (α = 1) or a combination of the two is obtained. The interaction between the chromophore and the TLSs is assumed to be of the dipole-dipole form. With an increase in α, the broadening of the absorption line shape was found to follow a power-law behavior. More importantly, it is revealed in the long-time limit that the resultant line shape is Gaussian in the absence of disorder but transforms to Lorentzian for a completely disordered environment. For an arbitrarily intermediate value of α, the resultant line shape can be approximately fitted by a linear combination of Gaussian and Lorentzian components. The Lorentzian profile for the disordered medium is attributed to the chomophore-TLS pairs with vanishingly small separation between them.
Multiphoton transition probability can be manipulated by tailoring the ultrashort laser pulses. In this paper, we theoretically and experimentally investigate the influence of the absorption bandwidth and line shape on the coherent control of two-photon transitions in two-level system by manipulating the femtosecond laser pulse with the $\ensuremath{\pi}$ spectral phase step. A coherent feature with a coherent peak and two coherent dips can be achieved if the absorption bandwidth is less than twice of the laser spectral bandwidth. The absorption bandwidth decides the coherent peak or dip intensity, and the absorption line shape affects the symmetry of the two coherent dips.