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Optics Letters

Ultranarrow extraresonant antiholes in pump–probe spectroscopy induced by inelastic collisions

A. D. Wilson‐Gordon, Harry Friedmann

Published Apr 15, 1989• 20 citations
Publisher

Abstract

Pump-probe spectroscopy with copropagating pump and probe beams of an open two-level system where, as a result of inelastic collisions, the lower state of an optical transition relaxes faster to reservoir states than the upper state does, may yield an antihole in the probe spectral profile whose linewidth is subnatural and unaffected by Doppler broadening.

DOI
10.1364/ol.14.000390

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Pump-probe spectroscopy with copropagating pump and probe beams of an open two-level system where, as a result of inelastic collisions, the lower state of an optical transition relaxes faster to reservoir states than the upper state does, may yield an antihole in the probe spectral profile whose linewidth is subnatural and unaffected by Doppler broadening.
We calculate the two-level pump-probe absorption coefficient including both upper-to-lower-level decay and level decays to a still lower lying reservoir level. We carried out calculations of probe absorption profile for arbitrary ratios of natural width and detuning to the Doppler width associated with a given transition. This theory accounts for contributions from all velocity subclasses of atoms, not only those which are Doppler shifted into resonance with the laser field (Doppler limit).1 We observe and explain new line shape features based on dissimilar decays.
We demonstrate a new technique for saturated-absorption spectroscopy by use of copropagating beams that does not have the problem of crossover resonances. The pump beam is locked to a transition, and its absorption signal is monitored while the probe beam is scanned. As the probe comes into resonance with another transition, the pump absorption is reduced and the signal shows a Doppler-free dip. We use this technique to measure hyperfine intervals in the D2 line of 85Rb with a precision of 70 kHz and to resolve hyperfine levels in the D2 line of 39K that are less than 10 MHz apart.
In this paper we present theoretical calculations relating to pump-probe and four-wave mixing spectroscopy. In pump-probe spectroscopy, one measures the absorption profile for the situation when an arbitrary strong pump field drives a given transition and a probe (weak) field drives the same transition. We have studied the influence of level degeneracy and field polarization on pump-probe and four-wave mixing signals. Our results indicate that for some closed systems (no population loss to the reservoir) it is possible to observe resonances that are characterized by the ground state width. Previous calculations indicate that for a nondegenerate system this resonance can appear only for an open system, the so-called "pressure induced resonances.”1 Our result, which contradicts this conclusion, can be understood by noting the fact that there are in general three irreducible tensor2 (in general) contributions to the line shape (K = 0 population, K = 1 orientation, and K = 2 alignment). Thus, even if the system is closed for the population it may still remain open for orientation or alignment; this effect is responsible for the narrow resonance. Specific calculations are presented for J = 1/2 → 1/2 and J = 1→2 transitions.
We study pump–probe and four-wave mixing spectroscopy for moderately intense copropagating pump and probe beams (Rabi frequencies 2|V1,2|) interacting with an open two-level system where the lower state of an optical transition relaxes faster to reservoir states than the upper state does. The probe absorption spectrum displays an ultranarrow extraresonant antihole (ERA) when |V1| ≥ |V2| and a ultranarrow dip when |V1| < |V2|. The pump and probe absorption profiles display opposite tendencies except for the case of |V1| = |V2| when identical ERA’s are produced. The four-wave mixing spectrum shows an extraresonant dip for |V1| ≥ |V2| and an ERA when |V1| < |V2| The subnatural features are not power broadened.
A theory of pump-probe spectroscopy is developed in which optical fields drive two-quantum, Raman-like transitions between ground-state sublevels. Three fields are incident on an ensemble of atoms. Two of the fields act as the pump field for the two-quantum transitions. The absorption or gain of an additional probe field is monitored as a function of its detuning from one of the fields which constitutes the pump field. Although the probe absorption spectrum displays features common to those found in pump-probe spectroscopy of single-quantum transitions, new interference effects are found to modify the spectrum. Many of these features can be explained within the context of a dressed-atom picture.