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Optics Letters

Single-shot imaging of ground-state hydrogen atoms with a nonlinear laser spectroscopic technique

M. Linvin, Z. S. Li, Johan Zetterberg, Marcus Aldén

Published May 17, 2007• 11 citations
Publisher

Abstract

We report on a novel nonlinear laser spectroscopic technique for single-shot imaging of ground-state hydrogen atoms in harsh environments. H atoms from the ground state were first pumped to the 2s state via a two-photon excitation with a 243 nm laser beam, and the population of the 2s state was further probed through the 2s-4p transition with conventional polarization spectroscopy at 486 nm. A single Nd:YAG-pumped optical parametric oscillator laser system was enough to provide both laser beams. Single-shot visualization of native H atoms in an atmospheric pressure premixed H(2)/O(2) flame is demonstrated.

DOI
10.1364/ol.32.001569

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We report on a novel nonlinear laser spectroscopic technique for single-shot imaging of ground-state hydrogen atoms in harsh environments. H atoms from the ground state were first pumped to the 2s state via a two-photon excitation with a 243 nm laser beam, and the population of the 2s state was further probed through the 2s-4p transition with conventional polarization spectroscopy at 486 nm. A single Nd:YAG-pumped optical parametric oscillator laser system was enough to provide both laser beams. Single-shot visualization of native H atoms in an atmospheric pressure premixed H(2)/O(2) flame is demonstrated.
We demonstrate an ultrafast parametric four-wave mixing method for the collisional-quenching-free detection of atomic hydrogen. Two photons of 243 nm light resonantly excite the n = 1 to n = 2 transition of atomic hydrogen, and a third probe photon scatters from the electronic coherence to generate the parametric emission of a degenerate signal photon. Laser-induced photofragmentation fluorescence from water, also excited with the same 243 nm pulses, is used as a convenient method to visualize beam overlap in space and time. The femtosecond time resolution enables the suppression of unwanted nonresonant contributions to the signal and separation from resonant mixing in water molecules because of the significantly different coherence lifetimes. A folded BOXCARS phase-matching configuration yields a spatially isolated, laser-like, signal beam, amenable to measurements in highly luminous backgrounds. Measurements in an H2/CH4/air flame demonstrate quantitative agreement with simulated H-atom concentration profiles. A coherence decay time constant of 42 ps is recorded in the atmospheric pressure flame.
Abstract : Research on this AASERT grant was focussed on the optical spectroscopy of trapped cold hydrogen for use as a spectroscopic tool and as a means of studying the gas. The grant supported research by two graduate students. During the grant an optical signal on the 1S - 2S transition in cold trapped hydrogen was observed, opening the way to a new form of ultra high resolution spectroscopy. The optical signal will also provide a valuable tool for manipulating a Bose condensate in hydrogen. The condensate can absorb two photons form a single running wave. The recoil is enough to sweep the atoms out of the trap, creating a new type of atom laser beam.
We investigate the excited-state dynamics of hydrogen (H) atoms in flames by using a femtosecond (fs) pump-probe scheme and measuring directional emission signals. An approximately 100-fs pump pulse at 205.1 nm excites H atoms through a two-photon process (n = 3 ←← n = 1), which is followed by detection of the forward emission signals induced by a broadband fs probe pulse near 656 nm. Above a certain threshold, we observe a quadratic dependence of the emission signal on the pump laser energy. Moreover, the linewidth of the forward emission signal varies with the probe delay and the probe laser energy. This behavior can be explained in terms of superradiance. We perform a theoretical analysis and compare the experimental results with the theory, and conclude that, within the conditions of our experiment, the behavior of the atomic system involves atomic coherence, which is produced non-adiabatically and corresponds to a superradiant process. Variations in the duration of the gain time window and lifetime of the excited-state H atoms in flames are explored at different flame conditions (i.e., equivalence ratio and heights above the burner). The fs pump-probe technique demonstrated here can also be extended to characterize the time-resolved population dynamics and the corresponding collisional energy transfer rates for energy levels involved in laser-induced fluorescence detection of H atoms in flames relevant to practical combustion applications.
Second harmonic generation (SHG) in free atoms is one of the unsolved problems in nonlinear optics. The most probable mechanism is due to Stark mixing between nearby excited states through an electric field caused by charge separation through the process of three-photon ionization. To test the mechanism, atomic hydrogen appears to be the best candidate because of its well-known electronic structure and large dipole moments of its excited states. In this work we report on the observation of SHG in atomic hydrogen in the Lyman-α region. Pulsed dye laser radiation was doubled and tuned to 243 nm for excitation of the 2s ← 1s transition at 121.6 nm by a two-photon resonance process. A cw atomic beam was used with hydrogen atoms generated in a dc discharge of H2 gas. The laser beam was focused ~1 mm below the nozzle where the hydrogen atom density was estimated to be 1013 cm−3. The second harmonic radiation was strongly enhanced by adding an external dc field of up to 10 kV/cm. Stark splitting was clearly observed at higher fields.
The authors report the observation of the 1S-2S two-photon transition in atomic hydrogen in an atomic beam, excited by light from a narrow-band continuous-wave laser. The excitation takes place in a collision-free environment and detection of the resonance is carried out by Stark-quenching the metastable atoms some distance from the interaction region. This approach removes the limitations of cell excitation employed in previous experiments with continuous-wave lasers, and should allow the full precision of modern tunable laser techniques to be applied to the 1S-2S transition. It also gives a new method for producing a collimated beam of metastable atoms which has particular applications to a variety of future experiments with cold hydrogen.