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arXiv:0710.0149 · Physical Review Letters

Multichannel Selective Femtosecond Coherent Control Based on Symmetry Properties

Zohar Amitay, Andrey Gandman, Lev Chuntonov, Leonid Rybak

Published May 16, 2008• 40 citations
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Abstract

We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.

DOI
10.1103/physrevlett.100.193002

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Journal of Physics B Atomic Molecular and Optical Physics•Mar 26, 2008•21 citations
We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.
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.
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.
We introduce a new scheme for generating short-wavelength coherent broadband radiation with well-controlled spectral characteristics. It is based on shaping long-wavelength femtosecond pulse to coherently control atomic resonance-mediated (2+1) three-photon excitation to a broad far-from-resonance continuum. Here, the spectrum (central frequency and bandwidth) of deep-ultraviolet coherent broadband radiation generated in Na vapor is experimentally controlled by tuning the linear chirp we apply to the driving phase-shaped near-infrared femtosecond pulse. This is a first step in implementing the full scheme for producing shaped femtosecond pulses at wavelengths down-to the vacuum-ultraviolet range.
We present and experimentally demonstrate for the first time the observation and femtosecond coherent control over the temporal evolution of a transient population that is excited via nonresonant two-photon absorption. Based on symmetry properties of the two-photon absorption process, the exciting femtosecond pulses are phase-shaped to photoinduce different evolutions of the transient excited population for a given final excited population. As a study case, we focus here on the attractive case of two-photon dark pulses that, although inducing zero final population (hence, the terminology of "dark pulses"), they induce a transient excited population during the pulse irradiation that can significantly deviate from zero. This nonzero transient population can be viewed as the bright side of such dark pulses. The symmetry-based coherent control is demonstrated first with dark pulses that we shape to induce transient excited population that at all times is kept below different target levels. Then, it is further demonstrated with pairs of dark pulses where one is rationally shaped to induce temporal evolution of the transient excited population that is the inverse of the evolution induced by the other. The work is conducted in the weak-field regime with the sodium atom as the model system. The approach developed here is general, conceptually simple, and very effective.
We study in detail coherent phase control of femtosecond resonance-mediated (2+1)(2+1)(2+1) three-photon absorption and its dependence on the spectral bandwidth of the excitation pulse. The regime is the weak-field regime of third perturbative order. The corresponding interference mechanism involves a group of three-photon excitation pathways that are on resonance with the intermediate state and a group of three-photon excitation pathways that are near resonant with it. The model system of the study is atomic sodium (Na), for which experimental and numerical-theoretical results are obtained. Prominent among the results is our finding that with simple proper pulse shaping an increase in the excitation bandwidth leads to a corresponding increase in the enhancement of the three-photon absorption over the absorption induced by the (unshaped) transform-limited pulse. For example, here, a 40 nm bandwidth leads to an order-of-magnitude enhancement over the transform-limited absorption.
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.