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arXiv:0910.3581

Symmetry-Based Selective Femtosecond Coherent Control of Transient Two-Photon Absorption

Andrey Gandman, Leonid Rybak, Bronstein, Michal, Naser Shakour, Zohar Amitay

Published Oct 19, 2009• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.0910.3581

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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.
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 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.
Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.
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.
Multiphoton femtosecond coherent control of is used for implementing innovative photo-induced analog coherent computation that generally might be a basis for future "smart hardware". The specific implemented computational task the classification of an unknown sequence into one of the three groups: (i) a constant sequence that is composed of identical numbers, (ii) a sequence that is antisymmetric around a given point, or (iii) neither. The input sequence is encoded into the spectral phases of a broadband femtosecond pulse and the computational task is being carried out by the multiphoton nonlinear response of the irradiated physical system. Here, it is the simultaneous coherent two- and three-photon absorption in atomic sodium (Na). The corresponding computational resources are the manifold of initial-to-final multiphoton excitation pathways photo-induced by the broad spectrum of the irradiating femtosecond pulse. The answer is obtained by measuring only two observables, which are two state-populations excited via the two- and three-photon absorption processes. Hence, the computational task is accomplished in a constant number of operations irrespective of the sequence length. As such, the presented scheme, where the femtosecond pulse serves as a query and the irradiated physical system serves as an oracle, provides a sufficient gain in the computational complexity.
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.