Spectral condensation near molecular transitions in intracavity laser spectroscopy with vertical external cavity surface emitting lasers
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文摘
Vertical external cavity surface emitting lasers (VeCSELs) are ideal amplification media for intracavity laser absorption spectroscopy (ICLAS) around 1 μm. However, we noted that, in some spectra recorded by ICLAS-VeCSEL, the observed line profiles of very weak overtone transitions were clearly asymmetric, this distortion being more pronounced for the strongest lines. More spectacular effects were observed when we investigated the acetylene spectrum: while the weakest absorption lines appeared as dips superimposed on the baseline as usual in ICLAS, the strongest lines mostly disappeared and were replaced by emission lines slightly blue shifted from the absorption line center. This effect, called “spectral condensation”, was, in fact, discovered near atomic transitions, more than 30 years ago, using pulsed lasers. Using acetylene and water as absorbers, we have systematically studied the different factors of importance for spectral condensation and showed that it increases with the pumping rate, the generation time and the line intensity. Spectral condensation was also found to increase with the pressure of the intracavity gas sample up to a value of a few Torrs, and to decrease afterwards. The appearance of spectral condensation has been shown to be highly correlated to time oscillations of the total laser power. Of importance for intensity measurements, this systematic study has showed that condensation effects may appear for long generation times even at low pumping rate and even with extremely weak absorption lines. A discussion of the results in relation with different interpretations available in the literature is presented with a particular emphasis on the theory based on the coherent interaction of electro-magnetic field with optically dense resonant extended medium leading to a parametrical amplification without population inversion.