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Journal of Nonlinear Optical Physics & Materials

NON-RESONANT TWO-PHOTON ABSORPTION CONTROL BY TWO TIME-DELAYED LASER PULSES

Chenhui Lu, Shian Zhang, Tianqing Jia, Jianrong Qiu, Zhenrong Sun

Published Mar 1, 2013• 3 citations
Publisher

Abstract

In this paper, we theoretically investigate the control of the non-resonant two-photon absorption induced by two time-delayed laser pulses, and an analytical solution for the dependence of the two-photon transition probability on the time delay and relative carrier-envelope phase of the two laser pulses is achieved. We show that the two-photon absorption can be significantly enhanced or completely suppressed by varying the time delay between the two laser pulses or their relative carrier-envelope phase. We also show that the two-photon absorption can be selectively excited when two excited states are simultaneously excited. Furthermore, we discuss the two-photon absorption control in the molecular system and analyze the effect of the absorption bandwidth on the control efficiency of the two-photon absorption.

DOI
10.1142/s0218863513500082

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In this paper, we theoretically investigate the control of the non-resonant two-photon absorption induced by two time-delayed laser pulses, and an analytical solution for the dependence of the two-photon transition probability on the time delay and relative carrier-envelope phase of the two laser pulses is achieved. We show that the two-photon absorption can be significantly enhanced or completely suppressed by varying the time delay between the two laser pulses or their relative carrier-envelope phase. We also show that the two-photon absorption can be selectively excited when two excited states are simultaneously excited. Furthermore, we discuss the two-photon absorption control in the molecular system and analyze the effect of the absorption bandwidth on the control efficiency of the two-photon absorption.
We theoretically study the control of two-photon excitation to bound and dissociative states in a molecule induced by trains of laser pulses, which are equivalent to certain sets of spectral phase modulated pulses. To this end, we solve the time-dependent Schr\"odinger equation for the interaction of molecular model systems with an external intense laser field. Our numerical results for the temporal evolution of the population in the excited states show that, in the case of an excited dissociative state, control schemes, previously validated for the atomic case, fail due to the coupling of electronic and nuclear motion. In contrast, for excitation to bound states the two-photon excitation probability is controlled via the time delay and the carrier-envelope phase difference between two consecutive pulses in the train.
In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape). The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth. Our results demonstrate that, the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field, and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.
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Temporal phase control over the multi-photoionization of NO is investigated experimentally. The coherent excitation of the molecular system is achieved by a sequence of two phase-related non-Fourier-transform-limited laser pulses delivered by a nanosecond dye laser. The phase-locked pulses are produced by making use of an actively stabilized interferometer with a tunable path-length difference. As the coherence time of the laser is comparable with the inhomogenous dephasing time of the medium, the measurements are performed with temporally overlapped pulses. In order to avoid the modulation of the ionic signal coming from optical interference, the linear polarizations of the two pulses are crossed. The quantum modulation of the signal versus the time delay between the two pulses is observed for the three following distinct processes: (a) two-photon resonant four-photon ionization of the ground vibronic state; (b) two-photon absorption of the A-X transition followed by ionization; and (c) two-photon ionization of the electronically excited state A. As a result, temporal phase control over bound-bound and bound-free transitions is demonstrated. The efficiency of the control process is shown to be limited by the presence of uncoupled excitation channels inherent to the method employed. The advantage in using a sequence of cross-polarized pulses for the controlling processes is discussed.
We theoretically and experimentally demonstrate the control of the intermediate state absorption in (1+2) resonance-mediated multiphoton absorption process by shaping the femosecond laser pulse. A theoretical model is proposed to investigate the intermediate state absorption of (1+2) resonance-mediated three-photon absorption process in the molecular system, and an analytical solution is obtained on the basis of time-dependent perturbation theory. Our theoretical results show that the intermediate state absorption can be enhanced by controlling the laser spectral phase due to final state absorption reduction, and this absorption enhancement efficiency increases with the increase of the laser intensity. These theoretical results are experimentally confirmed in IR144 dye by varying the laser spectral phase with a sinusoidal modulation function.
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.