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Physical Review A

Coherent quantum control of green emission in Er3+ -doped glass by π -phase-shaped ultrashort laser pulses

Wenjing Cheng, Tianqing Jia, Xiaoying Shang, Shian Zhang, Jing Ma, Donghai Feng, Zhenrong Sun, Jianrong Qiu

Published Feb 3, 2014• 3 citations
Publisher

Abstract

We experimentally and theoretically study the coherent quantum control of green emission in Er${}^{3+}$-doped glass by $\ensuremath{\pi}$-phase-shaped 800-nm femtosecond laser pulses. The experimental results show that the green emission intensity is enhanced over the transform-limited pulse by $\ensuremath{\pi}$-phase-shaped pulses as the laser field increases to several 10${}^{12}$ W/cm${}^{2}$. Coherent control of multiphoton absorption is studied based on the fourth-order perturbation theory, and the theoretical results accord well with the experimental observations.

DOI
10.1103/physreva.89.023401

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We experimentally and theoretically study the coherent quantum control of green emission in Er3+{}^{3+}3+-doped glass by \ensuremathπ\ensuremath{\pi}\ensuremathπ-phase-shaped 800-nm femtosecond laser pulses. The experimental results show that the green emission intensity is enhanced over the transform-limited pulse by \ensuremathπ\ensuremath{\pi}\ensuremathπ-phase-shaped pulses as the laser field increases to several 1012{}^{12}12 W/cm2{}^{2}2. Coherent control of multiphoton absorption is studied based on the fourth-order perturbation theory, and the theoretical results accord well with the experimental observations.
The enhancement and tunable color emissions from codoped lanthanide ions of Er3+/Tm3+/Yb3+ have been studied extensively in recent decades. In this paper, we present a new scheme for quantum coherent control of two-photon absorption (TPA) and color emission in codoped lanthanide ions of Er3+/Tm3+/Yb3+ by properly phase shaping two infrared ultrashort laser beams at central frequencies of 10 650 cm−1 and 7650 cm−1, respectively. Compared with the results irradiated by transform-limited pulses, the TPA probabilities of the blue, green and red emissions are independently controlled in the ranges 0–13.3, 0–14.5 and 0–1.0, respectively. The effects of the energy states of lanthanide ions and the laser spectral bandwidths on the coherent features are also discussed. The TPA probabilities for the blue and green emissions increase with the laser spectral bandwidths and decrease with the energy bandwidths of the final level states. As the intermediate energy level shifts in the range 10 100–10 500 cm−1, the TPA probabilities for the blue and green emissions change in the ranges 7–15 and 8–17, respectively.
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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.
Controlling stimulated emission is of importance because it competes with absorption and fluorescence under intense laser excitation. We performed resonant nonlinear optical spectroscopy measurements using femtosecond pulses shaped by π- or π/2-step phase functions and carried out calculations based on density matrix representation to elucidate the experimental results. In addition, we compared enhancements obtained when using other pulse shaping functions (chirp, third-order dispersion, and a time-delayed probe). The light transmitted through the high optical density solution was dominated by an intense stimulated emission feature that was 14 times greater for shaped pulses than for transform limited pulses. Coherent enhancement depending on the frequency, temporal, and phase characteristics of the shaped pulse is responsible for the experimental observations.
Enhancing the photoluminescence and depressing the background emission are important problems in rare earth ion-doped materials.In this letter, the two-photon absorption (TPA) probability in a Pr 3+ ion system is enhanced by a factor of 12.3 by a π-phase step scanning of ultrashort laser pulses.This level is significantly higher than that achieved by a transform-limit pulse.However, the laser intensity of shaped pulse is reduced to 37% of the initial transform-limited pulse.In this method, the TPA probability can also be reduced to 58%.Furthermore, the effect of the shift of the intermediate energy level and the bandwidth of final states on TPA probability is discussed.
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.