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Applied Physics

Resonance-Mediated Two-Photon Absorption in Frequency-Domain under Intermediate-Strong Linearly Chirped Pulse

立庆 任

Published Jan 1, 2018• 0 citations
Publisher
DOI
10.12677/app.2018.88046

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Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.
We explore the connection between adiabatic rapid passage, a technique that allows for robust complete population transfer (CPT) in a resonant absorber, and self-induced transparency solitons. We employ the auxiliary differential equation finite-difference time-domain method to fully resolve the dynamics of femtosecond light pulses propagating through an absorbing two-level medium. Using the example of linearly chirped Gaussian pulses we find that the pulses achieving robust CPT for a single two-level system are also pulses that will transform into solitary waves when incident on a resonantly absorbing medium. At the entrance into the absorber strongly chirped, adiabatic pulses completely transfer the electronic population from the ground to the upper state. As the pulses suffer absorption they undergo a dynamic transition and quickly split into an off-resonant radiation part and one or several unchirped solitary pulses that may carry away some of the initially achieved population inversion. This spectral and temporal transformation process limits the spatial depths of the region of CPT in a dense absorber regardless of the initial pulse amplitude. We also show that the frequency-domain pulse area, defined as the spectral amplitude at the resonance frequency, allows for a better distinction between the regimes of $2\ensuremath{\pi}$-pulse and $0\ensuremath{\pi}$-pulse formation than time-domain measurements.
Abstract We theoretically and experimentally demonstrate the control of the intermediate state absorption in an ( n + m ) resonance-mediated multi-photon absorption process by the polarization-modulated femtosecond laser pulse. An analytical solution of the intermediate state absorption in a resonance-mediated multi-photon absorption process is obtained based on the time-dependent perturbation theory. Our theoretical results show that the control efficiency of the intermediate state absorption by the polarization modulation is independent of the laser intensity when the transition from the intermediate state to the final state is coupled by the single-photon absorption, but will be affected by the laser intensity when this transition is coupled by the non-resonant multi-photon absorption. These theoretical results are experimentally confirmed via a two-photon fluorescence control in (2 + 1) resonance-mediated three-photon absorption of Coumarin 480 dye and a single-photon fluorescence control in (1 + 2) resonance-mediated three-photon absorption of IR 125 dye.