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Physical Review A

Optical-pumping dips in a homogeneously broadened fluorescence line

Charles M. Klimcak, James C. Camparo

Published Oct 1, 1984• 18 citations
Publisher

Abstract

Several authors have recently discussed and observed optical-pumping dips in inhomogeneously broadened spectral lines. We have observed a qualitatively similar, but fundamentally distinct phenomenon: optical-pumping dips in a homogeneously broaded ${D}_{1}$ line of $^{87}\mathrm{Rb}$. To our knowledge this represents the first observation of homogeneous-optical-pumping dips.

DOI
10.1103/physreva.30.1791

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Several authors have recently discussed and observed optical-pumping dips in inhomogeneously broadened spectral lines. We have observed a qualitatively similar, but fundamentally distinct phenomenon: optical-pumping dips in a homogeneously broaded D1{D}_{1}D1​ line of 87Rb^{87}\mathrm{Rb}87Rb. To our knowledge this represents the first observation of homogeneous-optical-pumping dips.
The technique of optical pumping dips has been employed to generate subnatural structure in a 87Rb^{87}\mathrm{Rb}87Rb D1{D}_{1}D1​ line (natural width 5.6 MHz). Structure as narrow as 1.4 MHz was observed. These experiments represent the first observation of subnatural spectral structure generated without requiring atomic coherence. Additionally, line shapes observed in these studies may be analyzed to yield transition dipole moments without requiring internal standards or an absolute calibration of fluorescence collection efficiency in the experimental apparatus.
The extraordinarily short optical dephasing time of organic dye molecules in polymer hosts is known to be under 20 fs between 100 and 200 K. Short dephasing times suggest enormously broadened homogeneous linewidths on the order of 10 nm. Direct observation of single dye molecule fluorescence spectra shows a similarly broadened line, giving comparable dephasing times for room temperature measurements. While this single molecule linewidth agrees with that of the bulk sample, it is inaccurate to attribute this broadening to homogeneous mechanisms. Repeated single molecule fluorescence measurements permit determination of the homogeneous nature of this linewidth, as distinct from the inhomogeneous nature of dispersion in bulk samples. Spectral diffusion in single molecule spectra is evidenced by multiple peaks, visible despite broad spectra lines at room temperature. In the particular experiment discussed in this thesis, fluorescence from single organic dye molecules in thin polymethyl methacrylate films was studied with scanning confocal microscopy. Photon antibunching exhibited by the photon-pair correlation function g(2) (τ) at τ = 0 confirms that single molecule emission spectra were obtained.
Inhomogeneous broadening of optical transitions of 87^{87}87Rb atoms in nanofiber-based optical lattices