Entangled two-photon absorption with Brownian-oscillator fluctuations.

Abstract

We theoretically investigate the two-photon absorption signals of a three-band (g, e, f) system diagonally coupled to an over-damped Brownian oscillator bath, which induces random Gaussian modulations of energy levels with an arbitrary degree of correlation. For fast modulation, extra 2ωeg and 2ωfe peaks may obscure the g-f transitions in the classical two-photon absorption (CTPA) spectra for nearly resonant e states. These peaks arise from one-photon resonant g-e or e-f transitions. In the slow modulation limit, these peaks vanish because of the short tails of the Gaussian line shape. CTPA strongly depends on the correlations between energy fluctuations. In entangled two-photon absorption, the extra peaks are eliminated because of the broad one-photon but narrow two-photon spectrum of the twin photons. The variation of the coherences between f states with the correlation between energy fluctuations is explored.