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Science

Nonlinear Spectroscopy

Richard G. Brewer

Published Oct 20, 1972• 60 citations
Publisher

Abstract

Although nonlinear spectroscopy evolved slowly in its initial stages, it is now becoming an important new branch of atomic and molecular spectroscopy. A variety of phenomena are being observed for the first time, either in steady state or in transient behavior. In a sense, the methods of microwave and nuclear magnetic resonance spectroscopy are now being reproduced in the optical region, and with the same precision and detail.

DOI
10.1126/science.178.4058.247

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The aim of this book is to present new results in rapidly developing fields of nonlinear optics such as atomic coherence, magneto-optics of atomic media, Doppler-free spectroscopy, time-domain spectroscopy of dense atomic vapors, frequency comb spectroscopy and atom-surface interactions. The discovery of such coherent effects as coherent population trapping (CPT), electromagnetically induced transparency (EIT) and electromagnetically induced absorption (EIA) opened a new avenue for development in many fields of nonlinear optics. Investigations during the last decade have shown many related new results and approaches in nonlinear optics. These include nonlinear magneto-optical processes (NMOP) in the context of high precision magnetometry, quantum information storage and processing, magnetic resonance imaging and magnetic particle detection; the use of ultra-thin (nanometric length) atomic vapor cells in magneto-optical experiments, which show new peculiarities of both coherent effects and NMOP; the use of frequency and amplitude modulated laser beams for NMOP studies in atomic vapors with the aim of extending the range of ultra-precise magnetometers to stronger, particularly geomagnetic fields; application of the counter-propagating beam technique to reveal the Doppler free nonlinear Faraday rotation signals, as a spectroscopic tool and for applications; enhanced nonlinearity due to atomic coherence in multi-state systems; experimental study of EIT in solids; the use of the phase stabilized frequency domain combs of femtosecond laser pulses for velocity selective optical pumping of atomic hyperfine levels, as a direct frequency comb spectroscopy; time-domain nonlinear spectroscopy of dense atomic vapors; atom-surface interactions and laser induced adsorption and desorption of alkali atoms on the surface of solid materials for nanotechnology applications

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Quantum control of optical four-wave mixing with femtosecond !-3! laser pulses: coherent ac Stark nonlinear spectroscopy

Carles Serrat

The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w

•Jan 1, 2008•0 citations
Although nonlinear spectroscopy evolved slowly in its initial stages, it is now becoming an important new branch of atomic and molecular spectroscopy. A variety of phenomena are being observed for the first time, either in steady state or in transient behavior. In a sense, the methods of microwave and nuclear magnetic resonance spectroscopy are now being reproduced in the optical region, and with the same precision and detail.
The dynamics of nuclear spins in atomic and molecular environments have been examined in exquisite detail over the past 27 years by the methods of pulsed nuclear magnetic resonance. The early discovery of the spin echo by Erwin Hahn and the transient nutation effect by Henry Torrey initiated the field by introducing coherent transient phenomena to radio-frequency spectroscopy. An entire class of coherent spin transients could be observed by a simple variation of the rf pulse sequence, and from the decay characteristics the various spin-dephasing mechanisms could be examined separately. In short, these methods allowed decomposition of the spin-transition linewidth into its broadening components, and also offered new and versatile ways for performing high-resolution rf spectroscopy.
A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of 13CH^{13}\mathrm{CH}13CH3F_{3}\mathrm{F}3​F by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.
The aim of this book is to present new results in rapidly developing fields of nonlinear optics such as atomic coherence, magneto-optics of atomic media, Doppler-free spectroscopy, time-domain spectroscopy of dense atomic vapors, frequency comb spectroscopy and atom-surface interactions. The discovery of such coherent effects as coherent population trapping (CPT), electromagnetically induced transparency (EIT) and electromagnetically induced absorption (EIA) opened a new avenue for development in many fields of nonlinear optics. Investigations during the last decade have shown many related new results and approaches in nonlinear optics. These include nonlinear magneto-optical processes (NMOP) in the context of high precision magnetometry, quantum information storage and processing, magnetic resonance imaging and magnetic particle detection; the use of ultra-thin (nanometric length) atomic vapor cells in magneto-optical experiments, which show new peculiarities of both coherent effects and NMOP; the use of frequency and amplitude modulated laser beams for NMOP studies in atomic vapors with the aim of extending the range of ultra-precise magnetometers to stronger, particularly geomagnetic fields; application of the counter-propagating beam technique to reveal the Doppler free nonlinear Faraday rotation signals, as a spectroscopic tool and for applications; enhanced nonlinearity due to atomic coherence in multi-state systems; experimental study of EIT in solids; the use of the phase stabilized frequency domain combs of femtosecond laser pulses for velocity selective optical pumping of atomic hyperfine levels, as a direct frequency comb spectroscopy; time-domain nonlinear spectroscopy of dense atomic vapors; atom-surface interactions and laser induced adsorption and desorption of alkali atoms on the surface of solid materials for nanotechnology applications
The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w