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Journal of Applied Physics

Ultrahigh-resolution, frequency-resolved resonance fluorescence imaging with a monoisotopic mercury atom cell

Alexey A Podshivalov, M. R. Shepard, Oleg I. Matveev, Benjamin W. Smith, James D. Winefordner

Published Nov 15, 1999• 7 citations
Publisher

Abstract

A novel method of ultrahigh-resolution, frequency-resolved imaging using atomic vapor cells is proposed. The method is based on the accurate measurement of the fluorescence signal intensity distribution along the absorption path length when the signal frequency is tuned to a wing of the atomic absorption line. Two-step resonance fluorescence of Hg202 vapor was used for one-dimensional imaging of the Hg resonance radiation at 253.7 nm. An imaging signal with a frequency difference of 500 MHz could be easily distinguished visually and even a frequency difference of 80 MHz could be detected after appropriate processing of the fluorescence imaging signal. Several other novel methods of one- and two-dimensional multifrequency imaging are discussed.

DOI
10.1063/1.371529

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Fluorescent excitation of mercury by the resonance frequency and by lower frequencies.—V

Robert John Strutt

Abstract It was shown at an early stage of the present workf that the characteristic fluorescence of mercury could be generated by wave-lengths much longer than the resonance line λ 2537; indeed, its excitation was traced as far as λ 3450. It was found also that the primary excitation by atomic absorption (core of the resonance line) could be distinguished from excitation by molecular absorption (wing of the resonance line). Although in the case of the longer waves it appears certain that the excited systems produced in the first instance by absorption are molecules and not atoms, yet it is possible that subsequent dissociation, or excitation by collision might lead to the formation of excited atoms in a secondary way.

Proceedings of the Royal Society of London Series A Containing Papers of a Mathematical and Physical Character•Mar 3, 1933•0 citations
A novel method of ultrahigh-resolution, frequency-resolved imaging using atomic vapor cells is proposed. The method is based on the accurate measurement of the fluorescence signal intensity distribution along the absorption path length when the signal frequency is tuned to a wing of the atomic absorption line. Two-step resonance fluorescence of Hg202 vapor was used for one-dimensional imaging of the Hg resonance radiation at 253.7 nm. An imaging signal with a frequency difference of 500 MHz could be easily distinguished visually and even a frequency difference of 80 MHz could be detected after appropriate processing of the fluorescence imaging signal. Several other novel methods of one- and two-dimensional multifrequency imaging are discussed.
Characteristics of a novel type of ultranarrow-band image detector have been experimentally studied. The principle of this new imaging approach is to detect a resonance-ionization and (or) fluorescence-imaging signal formed on a thin planar cell filled with atomic vapor. A planar vapor cell with a thickness of 1.6 mm was used for imaging 253.7-nm radiation by Hg atoms. One- and two-dimensional images were produced and detected with ionization and fluorescence-signal acquisition. The feasibility of atomic-vapor image detectors with a spectral resolution of several megahertz is discussed.
Abstract In a previous paper on this subject I examined in some detail the fluorescence excited by the atomic resonance line 2537, and by frequencies lower than this, which act by absorption in the region of longer wave-length than 2537. The fact that this absorption-region is immediately juxtaposed to the atomic line, and that the absorption is (at any rate on a rough view) stronger the nearer we go to the line, makes the distinction between the two cases difficult ; and it must be admitted that the phenomena themselves are not at first sight so distinctive as might be expected, if we take the obvious view that in one case absorption is by atoms and in the other by molecules. This has led some writers to the opinion that atomic absorption does not act at all in giving rise to band-fluorescence. It was shown, however, in the communication mentioned that a discontinuity of intensity in the fluorescence can be observed as the exciting beam traverses the vapour, and is robbed of its more absorbable component. The initial fluorescence due to the core of the resonance line is referred to as the “core effect,” and the much weaker fluorescence distinguishable after the core effect has died out is called the “wing effect,” because it is excited by the wing, or outer region, of the line. With dense vapour, however, excitation can be observed more than 1000 A. to the long wave side of the line, and the term “wing effect” is extended to the whole of this region, because no reason has been found for restricting it. It was found (loc. cit., p. 9) that the core effect is cut out by a supplementary absorption cell of mercury vapour producing a reversal of the line only 0.1 A. in breadth. I wish now to emphasise that this reversal agrees exactly in position with the narrow atomic emission line from a cold source within less than this amount.
A sealed, compact mercury atomic-absorption resonance ionization imaging detector has been developed and evaluated. The sensitivity of the detector as well as its ability to form two-dimensional images has been demonstrated. Images of faint light (1000 photons) have been recorded by image summation. It is shown that one can obtain high-quality images with a spatial resolution of at least 130 mum by detecting the ionic component of the imaging signal. Distortion, more noise, and poorer spatial resolution were observed when the electron component of the signal was detected. We studied the influence of voltage on the cell electrodes to find the conditions for optimum signal-to-noise ratio.
Improvements in spectral resolution and sensitivity of a cesium based resonance fluorescence imaging monochromator (RFIM) are described. Alignment of the two lasers used in the excitation scheme in a co-propagating geometry have resulted in a detector spectral bandpass (270 MHz) that is narrower than the Doppler broadened profile (380 MHz) of cesium vapor at room temperature. Improvements in the experimental design, namely the addition of an image intensifier and cooled charge-coupled device (CCD) camera, have resulted in increased sensitivity; we report a limit of detection of 10 8 photons per pixel limited by image intensifier noise. Images of the cesium D 2 line emission (852.12 nm) from a cesium hollow cathode lamp were compared to an argon emission line (4Sº 1/2 → 4P 3/2 ) at 852.14 nm from a silver/argon hollow cathode lamp as a demonstration of the spectral resolution. The ability of the RFIM to discriminate between photons exciting the F = 4 vs. F = 3 ground state hyperfine level (a frequency difference of 9.2 GHz) of the cesium 6 2 S 1/2 state was also investigated to further demonstrate the spectral selectivity. The potential use of the described RFIM for chemical imaging applications is discussed.
It is experimentally demonstrated that use of an extremely thin cell (ETC) with the thickness of a Rb atomic vapor column of ∼400 nm allows one to resolve a large number of individual transitions between Zeeman sublevels of the D1 line of 87Rb and 85Rb in the sub-Doppler fluorescence excitation spectra in an external magnetic field of ∼200 G. It is revealed that due to the peculiarities of the Zeeman effect for different hyperfine levels of Rb, all allowed transitions between magnetic sublevels can be clearly resolved for 87RbF_g = 1 --> F_e = 1, 2 and F_g = 2 --> F_e = 1, 2 fluorescence excitation. Also, relatively good spectral resolution can be achieved for 85RbF_g = 2 --> F_e = 2, 3 fluorescence excitation. Some partial resolution of transitions between magnetic sublevels is achieved for 85RbF_g = 3 --> F_e = 2, 3 fluorescence excitation. The spectral resolution of individual transitions allows one to easily observe both linear and nonlinear Zeeman effects in the fluorescence excitation spectra obtained with the help of the ETC. In the fluorescence spectra of a cell of usual length there is no evidence of a spectral resolution of individual transitions at B ∼ 200 G. A simple magnetometer based on ETC with Rb with a submicrometer spatial resolution is described.
Abstract It was shown at an early stage of the present workf that the characteristic fluorescence of mercury could be generated by wave-lengths much longer than the resonance line λ 2537; indeed, its excitation was traced as far as λ 3450. It was found also that the primary excitation by atomic absorption (core of the resonance line) could be distinguished from excitation by molecular absorption (wing of the resonance line). Although in the case of the longer waves it appears certain that the excited systems produced in the first instance by absorption are molecules and not atoms, yet it is possible that subsequent dissociation, or excitation by collision might lead to the formation of excited atoms in a secondary way.