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Laser Physics

Quantum coherent control of blue, green and red emissions from codoped lanthanide ions of Er3+/Tm3+/Yb3+by two shaped infrared ultrashort laser beams

Wenjing Cheng, Shian Zhang, Tianqing Jia, Jing Ma, Zhenrong Sun

Published Dec 10, 2013• 2 citations

Abstract

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.

DOI: 10.1088/1054-660x/24/1/015402

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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 Pr3+ ion system is enhanced by a factor of 12.3 by a ∏-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.

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.

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.

Upconversion luminescence (UCL) of lanthanide-doped nanomaterials is usually a low-efficiency nonlinear process, involving multi-step, multi-channel transitions in a multi-level system. Here, we demonstrate quantum control and enhancement of multi-color (e.g., red and green) UCLs of NaYF4:Yb3+/Er3+ nanoparticles with metallic Fabry-Perot micro-cavities. Besides realization of controlled single-color UCLs, their internal quantum efficiencies are strongly enhanced, up to 3–4 orders of times. Experimental results indicate that the controlled single-color UCLs and enhancements are caused not only by modifications of the spontaneous radiation rates for the red- and green-color transitions but also by influencing the intermediate transitions to result in modified distributions of electrons in each of the multiple Er3+ levels, facilitating emission of either red- or green-color light. This work suggests a way to control photon emissions in systems with multi-channel transitions and/or multi-step excitations.

Multiphoton transition probability can be manipulated by tailoring the ultrashort laser pulses. In this paper, we theoretically and experimentally investigate the influence of the absorption bandwidth and line shape on the coherent control of two-photon transitions in two-level system by manipulating the femtosecond laser pulse with the $\ensuremath{\pi}$ spectral phase step. A coherent feature with a coherent peak and two coherent dips can be achieved if the absorption bandwidth is less than twice of the laser spectral bandwidth. The absorption bandwidth decides the coherent peak or dip intensity, and the absorption line shape affects the symmetry of the two coherent dips.

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.