We present the results of the spectral line-shape study of the first measurement of the extremely weak (7-0) band of the CO molecule. Measurements were done with a highly sensitive cavity ring-down spectrometer. Collisional narrowing, analyzed in terms of speed-dependent effects, was observed for the first time for transitions with line intensities below 2⋅10 cm/molecule at 296 K.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
December 2023
The air-broadened lines from the oxygen B band were measured for the first time in controlled laboratory conditions with a high signal-to-noise ratio using frequency-stabilized cavity ring-down spectroscopy (FS-CRDS) referenced to the optical frequency comb. Spectra measured at various pressures and temperatures were analyzed with an advanced line-shape model, considering the speed-dependence of collisional broadening and shift, and the effect of velocity-changing collisions. The temperature dependence of collisional broadening and shift is determined, whereas no significant temperature dependence of speed-dependent parameters and Dicke narrowing was observed.
View Article and Find Full Text PDFIntensities of 14 lines in the sixth overtone (7-0) band of carbon monoxide (12C16O) are measured in the visible range between 14 300 and 14 500 cm-1 using a frequency-stabilized cavity ring-down spectrometer. This is the first observation of such a high and weak overtone spectrum of the CO molecule. A theoretical model is constructed and tested based on the use of a high accuracy ab initio dipole moment curve and a semi-empirical potential energy curve.
View Article and Find Full Text PDFWe demonstrate a mirror position actuator that operates in a wide temperature range from room temperature to a deep cryogenic regime (10 K). We use a Michelson interferometer to measure the actuator tuning range (and piezoelectric efficiency) in the full temperature range. We demonstrate an unprecedented range of tunability of the mirror position in the cryogenic regime (over 22 μm at 10 K).
View Article and Find Full Text PDFWe present the results of direct measurements of the line mixing parameters for two pairs of overlapping transitions at the band head of the oxygen B band. Measurements were performed with the frequency-stabilized cavity ring-down spectrometer assisted by an optical frequency comb. The recorded spectra were analyzed with line profiles comprising speed dependence, Dicke narrowing, and line mixing.
View Article and Find Full Text PDFFrequency-based cavity mode-dispersion spectroscopy (CMDS), previously applied for Doppler-limited molecular spectroscopy, is now employed for the first time for saturation spectroscopy. Comparison with two intensity-based, cavity-enhanced absorption spectroscopy techniques, i.e.
View Article and Find Full Text PDFWe report the most accurate, to the best of our knowledge, measurement of the position of the weak quadrupole S(2) 2-0 line in $ {{\rm D}_2} $D. The spectra were collected with a frequency-stabilized cavity ringdown spectrometer (FS-CRDS) with an ultrahigh finesse optical cavity ($ {\cal F} = 637 000 $F=637000) and operating in the frequency-agile, rapid scanning spectroscopy (FARS) mode. Despite working in the Doppler-limited regime, we reached 40 kHz of statistical uncertainty and 161 kHz of absolute accuracy, achieving the highest accuracy for homonuclear isotopologues of molecular hydrogen.
View Article and Find Full Text PDFFrequency combs have made optical metrology accessible to hundreds of laboratories worldwide and they have set new benchmarks in multi-species trace gas sensing for environmental, industrial and medical applications. However, current comb spectrometers privilege either frequency precision and sensitivity through interposition of a cw probe laser with limited tuning range, or spectral coverage and measurement time using the comb itself as an ultra-broadband probe. We overcome this restriction by introducing a comb-locked frequency-swept optical synthesizer that allows a continuous-wave laser to be swept in seconds over spectral ranges of several terahertz while remaining phase locked to an underlying frequency comb.
View Article and Find Full Text PDFA spectroscopic method free from systematic errors is desired for many challenging applications of gas detection. Although existing cavity-enhanced techniques exhibit very high precision, their accuracy strongly depends on propagation of the light amplitude through an optical system and its detection. Here, we demonstrate that the frequency-based molecular dispersion spectroscopy, involving sub-Hz-level precision in frequency measurements of optical cavity resonances, leads to sub-per-mille accuracy and a wide dynamic range, both previously unattainable by any other spectroscopic technique.
View Article and Find Full Text PDFThe response of an optical cavity to incomplete extinction of nearly resonant incident light was experimentally examined. Measurements were performed using a Pound-Drever-Hall-locked frequency-stabilized cavity ring-down spectrometer (CRDS) that allowed the laser frequency detuning from the cavity resonance center to be controlled at Hz-level resolution. It is shown that an insufficient laser light extinction ratio combined with a phase shift and frequency detuning may lead to non-exponential cavity pumping and decay signals.
View Article and Find Full Text PDFWe present a cavity-enhanced direct optical frequency comb spectroscopy system with a virtually imaged phased array (VIPA) spectrometer and either a dither or a Pound-Drever-Hall (PDH) locking scheme used for stable transmission of the comb through the cavity. A self-referenced scheme for frequency axis calibration is shown along with an analysis of its accuracy. A careful comparison between both locking schemes is performed based on near-IR measurements of the carbon monoxide ν=3←0 band P branch transitions in a gas sample with known composition.
View Article and Find Full Text PDFRecent developments in optical metrology have tremendously improved the precision and accuracy of the horizontal (frequency) axis in measured spectra. However, the vertical (typically absorbance) axis is usually based on intensity measurements that are subject to instrumental errors which limit the spectrum accuracy. Here we report a one-dimensional spectroscopy that uses only the measured frequencies of high-finesse cavity modes to provide complete information about the dispersive properties of the spectrum.
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