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arXiv:0710.1226 · Optics Express

NIR femtosecond phase control of resonance-mediated generation of coherent UV radiation

Leonid Rybak, Lev Chuntonov, Andrey Gandman, Naser Shakour, Zohar Amitay

Published Dec 16, 2008• 7 citations
arXivHTMLPDF

Abstract

Shaped near-infrared (NIR) femtosecond pulses are used for the first time to control the generation of coherent deep-ultraviolet (UV) radiation in an atomic resonance-mediated (2+1) three-photon excitation. The broadband excitation coherently involves pathways that are on resonance with the intermediate resonance state as well as pathways that are near resonance with it. Experimental and theoretical results are presented for phase controlling the total emitted UV yield in atomic sodium. Depending on the NIR spectrum of the excitation pulse, the coherent UV emission is either predominantly due to a single excited real state that is accessed resonantly or due to a manifold of virtual states. The former leads to a narrowband UV emission, while the latter leads to a broadband UV radiation. Basic phase control is exercised in both cases, with excellent agreement between experiments and calculations. The tunability is over an order-of-magnitude UV-yield range.

DOI
10.1364/oe.16.021738

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International Conference on Ultrafast Phenomena•Jan 1, 1996•0 citations
Shaped near-infrared (NIR) femtosecond pulses are used for the first time to control the generation of coherent deep-ultraviolet (UV) radiation in an atomic resonance-mediated (2+1) three-photon excitation. The broadband excitation coherently involves pathways that are on resonance with the intermediate resonance state as well as pathways that are near resonance with it. Experimental and theoretical results are presented for phase controlling the total emitted UV yield in atomic sodium. Depending on the NIR spectrum of the excitation pulse, the coherent UV emission is either predominantly due to a single excited real state that is accessed resonantly or due to a manifold of virtual states. The former leads to a narrowband UV emission, while the latter leads to a broadband UV radiation. Basic phase control is exercised in both cases, with excellent agreement between experiments and calculations. The tunability is over an order-of-magnitude UV-yield range.
We investigate the use of shaped near-infrared (NIR) femtosecond pulses to control the generation of coherent broadband deep-ultraviolet (DUV) radiation in an atomic resonance-mediated (2+1) three-photon excitation to a broad far-from-resonance continuum. Previously, we have shown control over the total emitted DUV yield. Here, we experimentally demonstrate phase control over the spectral characteristics (central frequency and bandwidth) of the emitted broadband DUV radiation. It is achieved by tuning the linear chirp applied to the exciting NIR femtosecond pulse. The study is conducted with Na vapor.
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 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.
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 show experimentally that spectral phase manipulation of ultrashort extreme-uv light pulses can induce and control coherent transient excitation of the He(1s3p)\mathrm{He}(1s3p)He(1s3p) excited state by the nonresonant components of the broadband extreme-ultraviolet light. The spectral phase manipulation of the 15th harmonic of an intense 805nm805\phantom{\rule{0.3em}{0ex}}\mathrm{nm}805nm, 80fs80\phantom{\rule{0.3em}{0ex}}\mathrm{fs}80fs pulse is achieved by propagation of the euv light through a variable optical density of He gas. The acquired spectral phase due to the dispersive interaction of the off-resonance components in the euv pulse with the He(1s3p)\mathrm{He}(1s3p)He(1s3p) resonance enhances and modifies the transient excitation. The temporal evolution of the coherently prepared transient He(1s3p)\mathrm{He}(1s3p)He(1s3p) amplitude is probed by ionization to the continuum with a 400nm400\phantom{\rule{0.3em}{0ex}}\mathrm{nm}400nm, 80fs80\phantom{\rule{0.3em}{0ex}}\mathrm{fs}80fs pulse.
Resonant and near-resonant two-photon excitations with ultrashort laser pulses of forbidden atomic transitions give access to a wide class of nonlinear-optical processes such as two-photon absorption, stimulated Raman scattering, four-wave sum- and difference-frequency mixing. The latter has proofed to be a powerful tool for efficient femtosecond pulse generation in the VUV-spectral range [1]. Nevertheless, up to now only few experimental results have been obtained which allow the direct observation of the coherent dynamics in two-photon induced radiation-matter interactions (see experimental papers [2-5] and monograph [6]).