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Journal of Physics B Atomic Molecular and Optical Physics

Coherent enhancement of resonance-mediated multiphoton absorption

Shian Zhang, Hui Zhang, Tianqing Jia, Zugeng Wang, Zhenrong Sun

Published Nov 29, 2010• 2 citations
Publisher

Abstract

In this paper, we theoretically investigate the coherent enhancement of resonance-mediated (2+2) four-photon absorption. It is found that by shaping the spectral phase with a π phase step, the resonance-mediated (2+2) four-photon transition probability can be enhanced. Furthermore, the coherent enhancement dependences on the detuning between the two two-photon absorptions, laser spectral bandwidth and laser centre frequency are explicitly discussed and analysed. We believe these theoretical results may play an important role in enhancing more complex resonance-mediated multiphoton absorption processes.

DOI
10.1088/0953-4075/43/24/245502

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Femtosecond coherent phase control of resonance mediated (2+1)(2+1)(2+1) three-photon absorption is studied both theoretically and experimentally. The regime is perturbative of third order. The photoexcitation coherently combines elements of both nonresonant and resonance-mediated multiphoton transitions. By proper simple pulse shaping the three-photon absorption in Na is effectively controlled experimentally, enhanced up to $\ensuremath{\sim}300%$ of the absorption induced by the transform-limited pulse. It is achieved by phase manipulating intra- and intergroup interferences involving two groups of three-photon excitation pathways: (i) on resonance and (ii) near resonance with the intermediate resonance state accessed by nonresonant two-photon transition.
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We theoretically and experimentally demonstrate the quantum coherent control of the resonance-mediated two-photon absorption in rare-earth ions by the phase-shaped femtosecond laser pulse. Our theoretical results show that the resonance-mediated two-photon absorption can be effectively controlled, but the control efficiency depends on the laser repetition rate in real experiment due to the long lifetime and the short decoherence time of the excited state, and the larger laser repetition rate yields the lower control efficiency. These theoretical results are experimentally confirmed in glass sample doped with Er3+ by utilizing the femtosecond lasers with low repetition rate of 1 kHz and high repetition rate of 80 MHz.
We extend the powerful frequency-domain analysis of femtosecond two-photon absorption to the intermediate-field regime of considerable absorption yields, where additionally to the weak-field nonresonant two-photon transitions also four-photon transitions play a role. Consequently, we rationally find that the absorption is enhanced over the transform-limited pulse by any shaped pulse having a spectral phase that is antisymmetric around one-half of the transition frequency and a spectrum that is asymmetric around it (red or blue detuned according to the system). The enhancement increases as the field strength increases. The theoretical results for Na are verified experimentally.