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Coherent control of third-harmonic generation and multiphoton ionization: Experimental and theoretical studies

Roberto Buffa, R. Eramo, CAVALIERI, STEFANO, Lorenzo Fini

Published Jan 1, 2005• 0 citations
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Abstract

The effect of temporal coherent control on the two-photon-resonant third-harmonic generation and multiphoton ionization into the continuum states of an atomic system is experimentally and theoretically investigated by means of a pair of partially incoherent, identical laser pulses. The evidence of quantum interference as a function of the delay between the pulses is reported. The transition from the resonant to the nonresonant case is also shown. The obtained results agree with the prediction of a theoretical model showing that the onset of quantum interference appears to be related to the coherence time of the laser radiation, which is much shorter than the pulse duration.

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Physical Review A•Mar 9, 2007•70 citations
The effect of temporal coherent control on the two-photon-resonant third-harmonic generation and multiphoton ionization into the continuum states of an atomic system is experimentally and theoretically investigated by means of a pair of partially incoherent, identical laser pulses. The evidence of quantum interference as a function of the delay between the pulses is reported. The transition from the resonant to the nonresonant case is also shown. The obtained results agree with the prediction of a theoretical model showing that the onset of quantum interference appears to be related to the coherence time of the laser radiation, which is much shorter than the pulse duration.
The effect of temporal coherent control on the two-photon resonant third-harmonic generation in the continuum of ionization of an atomic system is experimentally investigated by means of a pair of partially incoherent, identical laser pulses. The evidence of quantum interference in the third-harmonic generation, as a function of delay between pulses, is reported. The transition from a resonant to a nonresonant case is also shown. The results agree with the predictions of a recently published theoretical model showing that the onset of quantum interference appears to be related to the coherence time of the laser radiation that is much shorter than the pulse duration.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
As a succession of two pulses propagates through a medium which exhibits a resonance (single or multiphoton), the resonant parts of the susceptibility will depend on the relative phase of the two pulses, provided the delay between the pulses is shorter than the phase relaxation time of the interaction. As a result of this "coherent interaction", the reradiation of the sample (the fluorescence, the absorption and the generation of harmonics) will be a periodic function of the phase difference and delay between the two pulses of the sequence 1. The study of these coherent effects is important, because one expect to find conditions under which the maximum harmonic conversion to much shorter wavelengths can be greatly enhanced 2. The presence of the multiphoton resonance enhances the nonlinear susceptibility responsible for the harmonic generation, but reduces also the maximum achievable conversion efficiency because of resonant losses (depletion of the fundamental by multiphoton absorption). The latter effect can be eliminated by a judicious choice of the pulse sequencing and phasing. In addition to demonstrating, for the first time, coherent interaction enhancement in harmonic generation, the data of third harmonic versus relative phase of the pulse sequences enable us to measure the phase angle of the third order susceptibility (hence the contribution of the continuum relative to that of the resonance).
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.
We present a theoretical study of the main characteristics of two-color photoionization spectra obtained when atoms are subjected to an intense radiation pulse containing the fundamental of an infrared laser and one of its higher harmonics. The frequency of the latter is chosen to be high enough that the atom can be ionized by a single photon. The calculation is performed by numerical integration of the time-dependent Schrödinger equation for a (three-dimensional) hydrogen atom. We present the general properties of the spectra and angular distributions as well as the possible occurrence of interferences between the laser-assisted process and above-threshold ionization. Our results indicate that such interference effects, which can lead to partial coherent control of the photoionization process, can be observed at moderate laser intensities within the reach of currently operated laser and harmonic sources.
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.