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Optics Letters

Quantum focusing and coherent control of nonresonant two-photon absorption in frequency domain

Baihong Li, Yonggang Xu, Lan An, Qianlan Lin, Haifei Zhu, Fukun Lin, Yongfang Li

Published Apr 10, 2014• 4 citations
Publisher

Abstract

We theoretically investigate the nonresonant two-photon absorption (TPA) process in a two-level atom induced by a weak chirped pulse in the frequency domain. According to the extremum condition of the two-photon transition probability (TPTP) at the transition center frequency, we propose a Fresnel-inspired pulse tailoring scheme for TPA that is significantly different from that of Broers et al. [Phys. Rev. A46, 2749 (1992)]. Using this scheme, the TPTP can be focused or eliminated completely by constructively or destructively modulating various pathways of the quantum interference. Our results are a significant improvement on those obtained by Broers et al. and will have potential applications in selective two-photon microscopy and spectroscopy.

DOI
10.1364/ol.39.002443

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We theoretically investigate the nonresonant two-photon absorption (TPA) process in a two-level atom induced by a weak chirped pulse in the frequency domain. According to the extremum condition of the two-photon transition probability (TPTP) at the transition center frequency, we propose a Fresnel-inspired pulse tailoring scheme for TPA that is significantly different from that of Broers et al. [Phys. Rev. A46, 2749 (1992)]. Using this scheme, the TPTP can be focused or eliminated completely by constructively or destructively modulating various pathways of the quantum interference. Our results are a significant improvement on those obtained by Broers et al. and will have potential applications in selective two-photon microscopy and spectroscopy.
Abstract In this study, the nonresonant two-photon absorption process in a two-level atom, induced by a weak chirped pulse, is theoretically investigated in the frequency domain. An analytical expression of the wave function expressed by Fresnel functions is obtained, and the two-photon transition probability (TPTP) versus the integral bandwidth, spectral width, and chirp parameter is analyzed. The results indicate that the oscillation evolution of the TPTP result from quantum diffraction of the wave function, which can be explained by analogy with Fresnel diffraction from a wide slit in the spatial domain. Moreover, the ratio between the real and imaginary parts of the excited state wave function and, hence, the atomic polarization, can be controlled by the initial phase of the excitation pulse. In some special initial phase of the excitation pulse, the wave functions with purely real or imaginary parts can be obtained by measuring the population probability. This work provides a novel perspective for understanding the physical details of the interactions between atoms and chirped light pulses in the multiphoton process.
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.
Abstract The dynamics of two two-photon absorption (TPA) pathways in a four-level quantum system driven by a laser pulse is investigated in this work. An analytical solution for pulse shaping is proposed to be globally optimal for constructive interference between the two pathways, and accurate spectral boundaries for phase modulation are obtained. The TPA rate can be enhanced by a factor of 8.33 with the optimal pulse instead of the transform limited pulse (TL pulse). Simple control strategies modulating both amplitudes and phases are also designed to increase the TPA amplitude along one pathway while decreasing that along the other simultaneously. The strategies are intuitive and the two pathway amplitudes can differ by two orders of magnitude.
A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.
We theoretically investigate the coherent enhancement of resonant two-photon transitions (TPT) in a three-level atomic system. The TPT can be coherently enhanced by modulating spectral amplitude due to eliminating the destructive interference, though partial laser energy losses. Maximal enhancement of TPT can be achieved by modulating spectral phase due to establishing completely constructive interference. Our research provides a theoretical basis for experimental investigation and appears to have potential application on coherent control in the complicated quantum system.