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Physical Review Letters

Quantum Control of the Angular Momentum Distribution in Multiphoton Absorption Processes

Nirit Dudovich, Dan Oron, Yaron R. Silberberg

Published Mar 12, 2004• 79 citations
Publisher

Abstract

The newly developed technique of polarization pulse shaping is applied to the control of two-photon absorption in atomic rubidium. This technique enables the manipulation of the transient vector properties of a light matter interaction. We establish that control can be exerted on the angular distribution of the final state, and demonstrate the ability to control the final state population of a nearly degenerate system, as well as to perform M-state resolved spectroscopy.

DOI
10.1103/physrevlett.92.103003

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The newly developed technique of polarization pulse shaping is applied to the control of two-photon absorption in atomic rubidium. This technique enables the manipulation of the transient vector properties of a light matter interaction. We establish that control can be exerted on the angular distribution of the final state, and demonstrate the ability to control the final state population of a nearly degenerate system, as well as to perform M-state resolved spectroscopy.
Multiphoton transitions can be reached by many routes through a continuum of virtual levels. We show that the transition probability of two-photon and multiphoton processes can be controlled by tailoring the shape of an ultrashort excitation pulse, so that the many paths leading to the final state interfere to give a desired probability amplitude. We analyze the effect of pulse shapes on N-photon absorption as well as on Raman transitions. We show theoretically that certain tailored dark pulses do not excite the system at all, while other shaped pulses induce transitions as effectively as transform limited pulses, even when their peak amplitudes are greatly reduced. These results are confirmed experimentally for two-photon transitions in atomic cesium.
Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light–matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.
This work focuses on the developments of ultrafast laser pulse shaping techniques and their application to diatomic molecular systems in order to reveal fundamental effects in light matter interaction. It describes the development of a new pulse shaper consisting of a sequence of four liquid crystal arrays and a polarizer. This pulse shaper is the first non- interferometric setup for unrestricted phase, amplitude, and polarization shaping. Moreover, a parametric encoding of the electrical field was developed which allowed for generating pulse sequences consisting of several sub-pulses. Each sub-pulse can be controlled in its physically apparent parameters: energy, position in time, phase, and chirps as well as state of polarization with ellipticity, orientation, and helicity. The feasibility of the setup is illustrated by systematic variations of single and double pulses, which are experimentally generated and measured. In these series of pulses, one of the pulses parameters is varied while the other parameters are kept constant. This proves the precise control of the pulse shape. Further, more complex pulses are shown to give an impression of the capabilities of this setup in combination with the parameterization. For some fields of application, it could be desirable to guide the phase, amplitude and polarization shaped pulses through an optical fiber. For example, life science could benefit from shaped pulses in the area of imaging and photodynamic therapy. In order to make the shaped pulses available at the distal end of an optical fiber, the effects of the fiber have to be compensated. In this work, the generation of phase, amplitude, and polarization shaped pulses after transmission trough an optical fiber is presented. This is demonstrated for two types of optical fibers – a standard single-mode fiber and a microstructured hollow core photonic crystal fiber. The procedure for the determined generation of parametrically shaped pulses differs for both types of optical fibers. The capabilities of parametrically shaped pulse sequences are – again – illustrated by a series of example pulses. The parametrically shaped pulses transmitted through the hollow core fiber are implemented in a coherent control experiment. For this purpose, the potassium dimer produced in a molecular beam serves as a test system. The multi-photon ionization is studied by a closed feedback loop optimization and shaper-assisted pump-probe spectroscopy. These experiments revealed the excitation path including the vibrational dynamics in the first and second excited state. Further, the relevance of the polarization control in the excitation process is highlighted. Moreover, coherent control techniques are applied to investigate the interaction of shaped femtosecond laser pulses with ultracold atoms and molecules. The focus of these experiments is the control of the photoassociation of a colliding atom pair to a bound molecule. This process is investigated using two-color pump-probe spectroscopy. The molecular transients are compared to theoretical calculations. The analysis of this data reveals the interaction process which is discussed in the time and frequency domain. In a second experiment, the multi-photon ionization of ultracold rubidium dimers is optimized in a closed feedback loop. In this optimization, a parameterization in the frequency domain is employed which extracts the relevant transition frequencies. In combination with a complementary experiment the excitation pathway was revealed.
Coherent control of resonant and non-resonant two-photon absorption processes was examined using a spatio-temporal pulse-shaping technique. By utilizing a combination of temporal focusing and femtosecond pulse-shaping techniques, we spatially control multiphoton absorption processes in a completely deterministic manner. Distinctive symmetry properties emerge through two-dimensional mapping of spatio-temporal data. These symmetries break down in the transition to strong fields, revealing details of strong-field effects such as power broadenings and dynamic Stark shifts. We also present demonstrations of chirp-dependent population transfer in atomic rubidium, as well as the spatial separation of resonant and non-resonant excitation pathways in atomic caesium.
We present and implement a new scheme for independent control of both the final and the transient population utilizing the symmetry properties of the system. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, different time evolutions of the transient population are photo-induced for a given (fixed) final state population. The model system is the Na atom. The work is conducted in the weak-field regime for which the transient two-photon excitation is described by second-order perturbation theory. One most attractive case is the extended family of third-order chirp pulses which control the population build-up duration independently of the final population.