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1.
Phys Rev Lett ; 129(16): 163201, 2022 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-36306764

RESUMEN

Narrow optical resonances of atoms or molecules have immense significance in various precision measurements, such as testing fundamental physics and the generation of primary frequency standards. In these studies, accurate transition centers derived from fitting the measured spectra are demanded, which critically rely on the knowledge of spectral line profiles. Here, we propose a new mechanism of Fano-like resonance induced by distant discrete levels and experimentally verify it with Doppler-free spectroscopy of vibration-rotational transitions of CO_{2}. The observed spectrum has an asymmetric profile and its amplitude increases quadratically with the probe laser power. Our results facilitate a broad range of topics based on narrow transitions.

2.
J Chem Phys ; 156(4): 044201, 2022 Jan 28.
Artículo en Inglés | MEDLINE | ID: mdl-35105067

RESUMEN

The (30012) ← (00001) band of 12C16O2 in the 1.6 µm region is used for satellite observation of carbon dioxide in the Earth's atmosphere. Here, we report a Doppler-free spectroscopy study of this band with comb-locked wavelength-modulated cavity-enhanced absorption spectroscopy. Frequencies of 18 transitions with the rotational quantum numbers up to 42 were determined with sub-kHz accuracy, corresponding to a fractional uncertainty at the 10-12 level. With this precision, we revealed an anomalous decrease of the line shift and an increase of the line broadening for the Lamb dips of CO2 in the low-pressure regime compared to values obtained from Doppler-limited spectra at higher pressures.

3.
Rev Sci Instrum ; 92(7): 073003, 2021 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-34340416

RESUMEN

Interactions between a molecule and two or more laser fields are of great interest in various studies, but weak and highly overlapping transitions hinder precision measurements. We present the method of comb-locked cavity-assisted double resonance spectroscopy based on narrow-linewidth continuous-wave lasers, which allows for state-selective pumping and probing of molecules. By locking two near-infrared diode lasers to one cavity with a finesse at the order of 105, we measured all three types of double resonances. Carbon monoxide molecules with selected speeds along the laser beam were excited to vibrationally excited states, and absorption spectra with sub-MHz linewidths were observed. Positions of double resonance transitions were determined with an accuracy of 3.7 kHz, which was verified by comparing to Lamb-dip measurements. The present work paves the way to the pump-probe study of highly excited molecules with unprecedented precision.

4.
Opt Lett ; 45(17): 4863-4866, 2020 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-32870877

RESUMEN

Precision measurement of ro-vibrational transitions in the electronic ground state of the hydrogen molecule can be used to test quantum electrodynamics and also to determine the dimensionless proton-to-electron mass ratio. Saturation spectroscopy of the 2-0 overtone transitions of hydrogen deuterium (HD) were measured with three cavity-enhanced spectroscopy methods. With a sensitivity at the 10-13cm-1 level, we revealed a dispersion-like lineshape instead of a conventional Lamb "dip," which explains the significant discrepancy among previous independent measurements. The spectra can be fit well by using the Fano profile. Centers of R(1) and R(3) lines were determined as 217 105 182 111 (19)stat(240)syskHz and 220 704 305 234 (20)stat(240)syskHz, respectively.

5.
Opt Express ; 27(26): 37559-37567, 2019 Dec 23.
Artículo en Inglés | MEDLINE | ID: mdl-31878535

RESUMEN

Temperature dependence of molecular absorption line shape is important information for spectroscopic studies and applications. In this work, we report a comb-locked cavity ring-down spectrometer employing a cryogenic cooler to perform absorption spectroscopy measurements at temperatures between 40 K and 300 K. As a demonstration, we recorded the spectrum of the R(0) line in the (2-0) band of HD at 46 K. The temperature was also confirmed by the Doppler width of the HD line. Spectra of CH4 near 1.394 µm were also recorded in a wide temperature range of 70-300 K. Lower-state energies of methane lines were analyzed by fitting these spectra, which can be directly compared with the HITRAN and TheoReTS databases. Considerable deviations were observed, indicating the need to investigate the assignments of the methane lines in this region.

6.
Opt Express ; 27(5): 6106-6115, 2019 Mar 04.
Artículo en Inglés | MEDLINE | ID: mdl-30876204

RESUMEN

Noise-immune cavity enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is extremely sensitive in detecting weak absorption. However, the use of NICE-OHMS for metrology study was also hindered by its sensitivity to influence from various experimental conditions such as the residual amplitude modulation. Here we demonstrate to use NICE-OHMS for precision measurements of Lamb-dip spectra of molecules. After a dedicated investigation of the systematic uncertainties in the NICE-OHMS measurement, the transition frequency of a ro-vibrational line of C2H2 near 789 nm was determined to be 379 639 280 915.3±1.2 kHz (fractional uncertainty 3.2 × 10-12), agreeing well with, but more accurate than, the value determined from previous cavity ring-down spectroscopy measurements. The study indicates the possibility to implement the very sensitive NICE-OHMS method for frequency metrology of molecules, or a molecular clock, in the near-infrared.

7.
Rev Sci Instrum ; 88(4): 043108, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-28456258

RESUMEN

We present a new method of comb-locked cavity ring-down spectroscopy for the Lamb-dip measurement of molecular ro-vibrational transitions. By locking both the probe laser frequency and a temperature-stabilized high-finesse cavity to an optical frequency comb, we realize saturation spectroscopy of molecules with kilohertz accuracy. The technique is demonstrated by recording the R(9) line in the υ = 3 - 0 overtone band of CO near 1567 nm. The Lamb-dip spectrum of such a weak line (transition rate 0.0075 s-1) is obtained using an input laser power of only 3 mW, and the position is determined to be 191 360 212 770 kHz with an uncertainty of 7 kHz (δν/ν∼3.5×10-11), which is currently limited by our rubidium clock.

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