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Physical Review A

Pressure-induced extra resonances in nonlinear spectroscopy

G. Grynberg, P. R. Berman

Published Mar 1, 1990• 29 citations
Publisher

Abstract

We present three examples of pressure-induced extra resonances that can be observed in nonlinear spectroscopy: fluorescence of a ``three-level atom'' driven by two laser fields, two-photon ionization of a ``three-level atom'' (plus continuum) driven by two laser fields, and excitation of a ``four-level atom'' driven by four laser fields. We show that all these extra resonances can be interpreted in terms of quantum pathways, each pathway involving a collisionally aided excitation. We also demonstrate that the two first extra resonances can be obtained with incoherent fields, while relatively coherent fields are required in the last example.

DOI
10.1103/physreva.41.2677

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Physical Review A•Dec 1, 1989•3 citations
We present three examples of pressure-induced extra resonances that can be observed in nonlinear spectroscopy: fluorescence of a three-level atom'' driven by two laser fields, two-photon ionization of a three-level atom'' (plus continuum) driven by two laser fields, and excitation of a ``four-level atom'' driven by four laser fields. We show that all these extra resonances can be interpreted in terms of quantum pathways, each pathway involving a collisionally aided excitation. We also demonstrate that the two first extra resonances can be obtained with incoherent fields, while relatively coherent fields are required in the last example.
Using both a bare-atom and dressed-atom picture of atom-field interactions, we present a theory of the pressure-induced resonances that can arise when four radiation fields interact with a three-level quantum system. The four fields drive two coupled atomic transitions which share a common level, the levels being arranged in a ``ladder'' scheme. As the field frequencies are varied, certain resonant structures in the excitation spectrum of the upper state population appear only in the presence of collisions. The resonant structures result from processes that have been referred to in the past as collisionally aided radiative excitation (CARE) and pressure-induced extra resonances in four-wave mixing (PIER4). We show that both CARE- and PIER4-type resonances have a common origin, which can be linked to conservation of energy. In contrast to conventional PIER4 signals, line shapes calculated in this work result from a ``single atom'' rather than a collective emission. Moreover, the signals vanish unless the applied fields are relatively coherent, again in contrast to conventional PIER4.
Pressure-induced effects in nonlinear optics and spectroscopy are studied using a nonstandard-dressed-atom formalism for a set of two-level atoms. We consider a two-level atom interacting with two radiation fields whose frequencies differ by \ensuremath{\delta} and undergoing dephasing collisions with a perturber bath. The atom-field detunings are large compared with all relaxation rates in the problem. The system is described by a Hamiltonian of an atom dressed by a single-mode field with a coupling constant slowly varying in time at frequency \ensuremath{\delta}. We show that the collisionally aided excitation of the initially unpopulated dressed states is modulated in time. All the characteristics of the pressure-induced effects are deduced from the properties of this time-modulated excitation. Apart from already known phenomena (pressure-induced extra resonances in four-wave mixing, pressure-induced phase shifts, etc.) that are reinterpreted using this approach, we present a new effect that can be described as fluorescence beats. Finally, we show that this approach gives a firm basis for use of a model involving collision-induced gratings and we interpret the pressure-induced effects in the context of this model.
Experiments on pressure-induced extra resonances in degenerate four-wave mixing involving Zeeman coherence have been performed on Ba atoms in an argon atmosphere under conditions of large detunings from the Ba resonance line. The dependence on the detuning gives evidence for a breakdown of the impact approximation, when the laser is detuned by more than 5\ifmmode\times\else\texttimes\fi{}1011{10}^{11}1011 rad ${\mathrm{sec}}^{\ensuremath{-}1}$; the behavior can be interpreted semiquantitatively by a model based on optical collisions.
A competition between resonant multiphoton ionization (MPI) and third harmonic generation (THG) involving three-photon resonances was first reported by Miller et al.1 Recently, a similar competing process involving four-photon resonances was observed in the multiphoton ionization of Hg2. In this paper we report a similar observation in the three- and four-photon excitation spectra of Kr and Ar. Both the multiphoton ionization and the VUV radiation generated in the focal volume are measured over a broad range of gas pressures (0.01-100 Torr) and laser fluences. The 5s, 5f, and 6p′ levels of Kr and the 4s, 4p′, and 7p levels of Ar are investigated. The spectral lines are observed to broaden and to shift from line center as a function of increasing gas pressure and laser intensity. The effect observed in three-photon resonant lines is explained by the occurrence of a competition between MPI and THG.1 A similar effect observed in the four-photon resonances is interpreted as the result of THG enhanced by the four-photon levels—a five-photon process. However, it is not clear why the four-photon spectral line-width becomes narrower when the gas pressure is further increased; this is discussed.
Using a fully quantized dressed-atom approach, we present a theory and interpretation of the pressure-induced resonances in four-wave mixing (PIER4) that may arise when three incident fields interact with an ensemble of two-level atoms. The PIER4 resonances are seen to arise from a collisionally created modulation of a dressed-state population when an operator approach is used to solve the problem and from a level crossing between collisionally populated dressed states when an occupation-number formalism is used.