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IEEE Journal of Quantum Electronics

Single-atom detection by SONRES

Jerry A. Gelbwachs, C. Klein, John E. Wessel

Published Feb 1, 1978• 23 citations
Publisher

Abstract

The new method of atomic fluorescence detection, called saturated optical nonresonant emission spectroscopy (SONRES), has been modeled for a three-level atom, and experiments on sodium have been conducted that support the model. A rate equation analysis yielded expressions for excited-state atomic populations and saturation intensity. The detection of sodium in buffer gases that promote collisional transfer of excitation between 32P1/2→ 32p3/2both without quenching the fluorescence emission and with quenching was considered. Experimental results are presented for sodium in argon. At -25°C, approximately 180 atoms/cm3were monitored with a S/N of ∼ 15 representing detection at the level of one part in 1017. The signal at this temperature was generated by less than a single atom in the laser beam.

DOI
10.1109/jqe.1978.1069744

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Physical Review A•May 1, 1999•3 citations
The new method of atomic fluorescence detection, called saturated optical nonresonant emission spectroscopy (SONRES), has been modeled for a three-level atom, and experiments on sodium have been conducted that support the model. A rate equation analysis yielded expressions for excited-state atomic populations and saturation intensity. The detection of sodium in buffer gases that promote collisional transfer of excitation between 32P1/2→ 32p3/2both without quenching the fluorescence emission and with quenching was considered. Experimental results are presented for sodium in argon. At -25°C, approximately 180 atoms/cm3were monitored with a S/N of ∼ 15 representing detection at the level of one part in 1017. The signal at this temperature was generated by less than a single atom in the laser beam.
Coherence transfer accompanying 32P1/2 → 32P3/2 excitation transfer in sodium, induced in collisions with noble gas atoms, has been investigated using methods of sensitized fluorescence. Oriented 32P1/2 sodium atoms were produced by irradiating a mixture of sodium vapor and a noble gas with D1σ+ resonance radiation, and their subsequent collisions with the buffer gas atoms resulted in the simultaneous transfer of coherence and excitation from the 2P1/2 state to the 2P3/2 state. Measurements of the ratio of circular polarizations of the D2 sensitized fluorescence and D1 resonance fluorescence resulted in the following cross sections for coherence transfer. Na–He : 7.1 ± 0.7 Å2; Na–Ne : 6.2 ± 0.6 Å2; Na–Ar : 12.0 ± 1.2 Å2; Na–Kr : 6.8 ± 0.7 Å2; Na–Xe : 6.9 ± 0.7 Å2.
The resonant excitation of the sodium D2 transition by laser radiation was investigated experimentally in this thesis. Line polarization measurement of the resonance fluorescence was employed to investigate the excitation process. The sodium atoms, which were collimated in a very narrow beam, were excited by a monochromatic laser beam with the frequency tuned to resonance with the 32S 112(F=2) - 32P312 hyperfine transition. The direction of the laser beam was perpendicular to the atomic beam and the fluorescence photons were detected along a direction perpendicular to both the laser and atomic beams. The experimental measurements were performed to determine the effect due to the variation of the laser intensity and frequency on the line polarization. A theoretical expression of the line polarization as a function of density matrix elements of the upper excited hyperfine sub -states was derived. A full quantum electrodynamic theory was used to derive an atomic operator equation of motion which was needed to calculate atomic operator elements. These elements then yielded the corresponding density matrix elements. The experimental results and the theoretical modelling were in a good agreement. The first experimental results for the line polarization of the highly excited states, 42D512 and 42D312, are also presented. The use of two lasers enabled these highly excited states to be excited. The line polarization of the fluorescence for transitions from the 4D level down to lower states is derived in terms of the density matrix elements of the upper excited states. Two limiting cases for the theoretical predictions of the line polarization are considered.
Collisional transfer of excitation from mercury to sodium was investigated using methods of sensitized fluorescence. A mixture of mercury and sodium vapors at low pressure was irradiated with Hg 2537 Å resonance radiation, producing a population of Hg(63P1) atoms whose inelastic collisions with ground-state sodium atoms resulted in a transfer of excitation energy to close-lying S, P, and D states in sodium. The subsequent decay of these states manifested itself in the emission of a sensitized fluorescent spectrum. Absolute intensity measurements on the components of the spectrum yielded 21 cross sections whose magnitudes range from 0.02 to 38.5 Å2 and which exhibit a pronounced resonance with ΔE, the energy defect between Hg (63P1) and the appropriate level in sodium.
Collisional energy transfer between atoms and molecules proved to be an efficient method for excitation of new laser lines and spectroscopy of states forbidden for direct excitation or emission by parity conservation [1]. We have studied a number of stimulated emissions in the near IR 800 - 850nm in Na atom via Na2X—A transitions. Two tunable dye lasers have been employed, the first one scanning the X—A molecular transition and the second one tuned to Na 3p-4d single photon resonance, Fig.1. Taking the collision rate coefficient for the reaction
The intensity ratio D2/D1 for the sodium doublet has been measured for radiation from excited sodium atoms which result from the optical dissociation of sodium iodide vapor by ultraviolet light in the 2082→2500 A region. With shorter wavelength ultraviolet light as exciting source, the D2/D1 ratio is 0.98 and increases to above 1.5 with longer exciting wavelengths. Addition of foreign gases cause the observed D2/D1 ratio to increase to 1.89 for large foreign gas pressure. Cross sections for the transfer of excited sodium atoms from the 32P32 to the 32P½ state and vice versa due to collisions with foreign molecules have been measured as they depend on the relative velocity between excited sodium atom and foreign molecule. The Doppler broadening of the separate D lines emitted in the atomic fluorescence of sodium iodide has been estimated from absorption measurements. Both lines show equal broadening within the experimental error of the observations. Measurements were made with a photomultiplier tube. The sodium doublet was resolved with a reflection grating monochromator.
Optical pumping of the ground states of sodium can radically alter the shape of the laser-induced fluorescence excitation spectrum, complicating measurements of temperature, pressure, etc., which are based on these spectra. Modeling of the fluorescence using rate equations for the eight hyperfine states of the sodium D manifolds can be used to quantify the contribution to the ground state pumping of transitions among the hyperfine excited states induced by collisions with buffer gas atoms. This model is used here to determine, from the shape of experimental spectra, cross sections for $\ensuremath{\Delta}F$ transitions of the P3/2{P}_{3/2}P3/2​ state induced by collisions with helium and argon atoms, for a range of values assumed for the ${P}_{1/2}, \ensuremath{\Delta}F$ cross sections. The hyperfine cross sections measured using this method, which to our knowledge is novel, are compared with cross sections for transitions involving polarized magnetic substates mF{m}_{F}mF​ measured previously using polarization sensitive absorption. Also, fine-structure transition $(\ensuremath{\Delta}J)$ cross sections were measured in the pumped vapor, giving agreement with previous measurements made in the absence of pumping.