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Applied Physics Letters

Single and two-photon fluorescence control of Er3+ ions by phase-shaped femtosecond laser pulse

Shian Zhang, Shuwu Xu, Jingxin Ding, Chenhui Lu, Tianqing Jia, Jianrong Qiu, Zhenrong Sun

Published Jan 6, 2014• 19 citations
Publisher

Abstract

We experimentally demonstrate the control of the single and two-photon fluorescence (SPF and TPF) in Er3+ ions by shaping the femtosecond laser pulse with a π or square phase modulation. With the low laser intensity (8.4 × 1010 W/cm2), SPF keeps a constant while TPF is effectively suppressed by the two control schemes. With the high laser intensity (1.2 × 1013 W/cm2), both SPF and TPF are simultaneously enhanced or suppressed by the π phase modulation, and SPF is enhanced while TPF is effectively suppressed by the square phase modulation. The up/down-conversion fluorescence enhancement, suppression, or tuning by the optical control method can greatly expand its applications in various related fields.

DOI
10.1063/1.4860995

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We experimentally demonstrate the control of the single and two-photon fluorescence (SPF and TPF) in Er3+ ions by shaping the femtosecond laser pulse with a π or square phase modulation. With the low laser intensity (8.4 × 1010 W/cm2), SPF keeps a constant while TPF is effectively suppressed by the two control schemes. With the high laser intensity (1.2 × 1013 W/cm2), both SPF and TPF are simultaneously enhanced or suppressed by the π phase modulation, and SPF is enhanced while TPF is effectively suppressed by the square phase modulation. The up/down-conversion fluorescence enhancement, suppression, or tuning by the optical control method can greatly expand its applications in various related fields.
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In this paper, we theoretically demonstrate that the (2+1+1) resonance enhanced multi-photon ionization photoelectron spectroscopy in sodium atom can be effectively controlled by shaping femtosecond laser pulse with a π phase step modulation in weak laser field, involving its total photoelectron energy, maximal photoelectron intensity, and spectroscopic bandwidth. Our results show that the total photoelectron energy can be suppressed but not enhanced, the maximal photoelectron intensity can be enhanced and also suppressed, and the photoelectron spectroscopy can be tremendously narrowed. These theoretical results can provide a feasible scheme to achieve the high-resolution photoelectron spectroscopy and study the excited state structure in atomic and molecular systems.
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 experimentally and theoretically study the coherent quantum control of green emission in Er3+{}^{3+}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 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.
Abstract Controlling the up-conversion luminescence of rare-earth ions in real-time, in a dynamical and reversible manner, is very important for their application in laser sources, fiber-optic communications, light-emitting diodes, color displays and biological systems. In previous studies, the up-conversion luminescence control mainly focused on the weak femtosecond laser field. Here, we further extend this control behavior from weak to intermediate femtosecond laser fields. In this work, we experimentally and theoretically demonstrate that the up-conversion luminescence in Dy 3+ ion doped glass can be artificially controlled by a π phase step modulation, but the up-conversion luminescence control behavior will be affected by the femtosecond laser intensity, and the up-conversion luminescence is suppressed by lower laser intensity while enhanced by higher laser intensity. We establish a new theoretical model (i.e. the fourth-order perturbation theory) to explain the physical control mechanism by considering the two- and four-photon absorption processes, and the theoretical results show that the relative weight of four-photon absorption in the whole excitation process will increase with the increase in laser intensity, and the interference between two- and four-photon absorptions results in up-conversion luminescence control modulation under different laser intensities. These theoretical and experimental works can provide a new method to control and understand up-conversion luminescence in rare-earth ions, and also may open a new opportunity to the related application areas of rare-earth ions.
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.