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Physical Review Letters

Coherent Control of Angular Momentum Transfer in Resonant Two-Photon Light-Matter Interaction

D. A. Malik, Alexey V. Kimel, Andrei I. Kirilyuk, Th. Rasing, Wim J. van der Zande

Published Mar 29, 2010• 7 citations
Publisher

Abstract

We show experimentally and theoretically that a polarization-shaped femtosecond laser pulse with a zero net angular momentum creates a net angular momentum in atomic rubidium during resonant two-photon excitation. The necessary conditions for the creation of a nonzero angular momentum as well as the excitation efficiencies are analyzed in the framework of second-order time-dependent perturbation theory.

DOI
10.1103/physrevlett.104.133001

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We show experimentally and theoretically that a polarization-shaped femtosecond laser pulse with a zero net angular momentum creates a net angular momentum in atomic rubidium during resonant two-photon excitation. The necessary conditions for the creation of a nonzero angular momentum as well as the excitation efficiencies are analyzed in the framework of second-order time-dependent perturbation theory.
We have investigated multiphoton-ionization passages of rubidium atoms initiated from the excited 5P3/25{P}_{3/2}5P3/2​ energy state. For this we used coherent control schemes based on femtosecond laser pulse shaping applied to cold atoms spatially isolated in a magneto-optical trap. With programed laser pulses of spectral $\ensuremath{\pi}$-phase step, of which location was varied within the laser spectrum, the sequential two-photon-ionization passage along the 5P3/25{P}_{3/2}5P3/2​-5D5D5D continuum was probed in terms of trap-loss spectroscopy. The coherent control two-photon-ionization method unveiled not only the resonantly enhanced two-photon ionization but also the asymmetric nature of the ionization profile structure given as a function of the spectral phase step location. Experimental results show good agreement with the second-order perturbation calculation of the constituent possible ionization passages.
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.
It has been shown that the femtosecond laser polarization modulation is a very simple and well-established method to control the multi-photon absorption process by the light–matter interaction. Previous studies mainly focused on the multi-photon absorption control in the weak field. In this paper, we further explore the polarization control behavior of multi-photon absorption process in the intermediate femtosecond laser field. In the weak femtosecond laser field, the second-order perturbation theory can well describe the non-resonant two-photon absorption process. However, the higher order nonlinear effect (e.g., four-photon absorption) can occur in the intermediate femtosecond laser field, and thus it is necessary to establish new theoretical model to describe the multi-photon absorption process, which includes the two-photon and four-photon transitions. Here, we construct a fourth-order perturbation theory to study the polarization control behavior of this multi-photon absorption under the intermediate femtosecond laser field excitation, and our theoretical results show that the two-photon and four-photon excitation pathways can induce a coherent interference, while the coherent interference is constructive or destructive that depends on the femtosecond laser center frequency. Moreover, the two-photon and four-photon transitions have the different polarization control efficiency, and the four-photon absorption can obtain the higher polarization control efficiency. Thus, the polarization control efficiency of the whole excitation process can be increased or decreased by properly designing the femtosecond laser field intensity and laser center frequency. These studies can provide a clear physical picture for understanding and controlling the multi-photon absorption process in the intermediate femtosecond laser field, and also can provide a theoretical guidance for the future experimental realization.
Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cut-off position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
We propose and develop a method for theoretical description of circularly (elliptically) polarized optical pulse resonant coherent interactions with two-level atoms. The method is based on the time-evolution equations of a two-level quantum system in the presence of a time-dependent dipole perturbation for electric dipole transitions between states with total angular-momentum projection difference $(\ensuremath{\Delta}{J}_{z}=\ifmmode\pm\else\textpm\fi{}1)$ excited by a circularly polarized electromagnetic field [Feynman et al., J. Appl. Phys. 28, 49 (1957)]. The adopted real-vector representation approach allows for coupling with the vectorial Maxwell's equations for the optical wave propagation and thus the resulting Maxwell pseudospin equations can be numerically solved in the time domain without any approximations. The model permits a more exact study of the ultrafast coherent pulse propagation effects taking into account the vector nature of the electromagnetic field and hence the polarization state of the optical excitation. We demonstrate self-induced transparency effects and formation of polarized solitons. The model represents a qualitative extension of the well-known optical Maxwell-Bloch equations valid for linearly polarized light and a tool for studying coherent quantum control mechanisms.