RESUMO
Precision measurements of molecular transitions to highly excited states are needed in potential energy surface modeling, state-resolved chemical dynamics studies, and astrophysical spectra analysis. Selective pumping and probing of molecules are often challenging due to the high state density and weak transition moments. We present a mid-infrared and near-infrared double-resonance spectroscopy method for precision measurements. As a demonstration, Doppler-free stepwise two-photon absorption spectra of 13CO2 were recorded by pumping the fundamental transition of R14 (00011)-(00001) and probing the P15 (00041)-(00011) transition enhanced by a high-finesse optical cavity, and the transition frequencies were determined with an accuracy of a few kilohertz.
RESUMO
Precision measurements on the hydrogen molecule are of fundamental importance in understanding molecular theory. Comparison of accurate experimental data and theoretical results are used to test the quantum electrodynamics theory and determine physical constants used in the calculation. We review recent advances and perspectives in the precision spectroscopy of molecular hydrogen, representing state-of-the-art molecular spectroscopy methods and cutting-edge high-precision calculations.
RESUMO
Selective pumping and probing of highly excited states of molecules are essential in various studies but are also challenging because of high density of states, weak transition moments, and lack of precise spectroscopy data. We develop a comb-locked cavity-assisted double-resonance spectroscopy (COCA-DR) method for precision measurements using low-power continuous-wave lasers. A high-finesse cavity locked with an optical frequency comb is used to enhance both the pumping power and the probing sensitivity. As a demonstration, Doppler-free stepwise two-photon absorption spectra of CO2 were recorded by using two milliwatt diode lasers (1.60 and 1.67 µm), and the rotation energies in a highly excited state (CO-stretching quanta = 8) were determined with an unprecedented accuracy of a few kilohertz.
RESUMO
The resolution of any spectroscopic or interferometric experiment is ultimately limited by the total time a particle is interrogated. Here we demonstrate the first molecular fountain, a development which permits hitherto unattainably long interrogation times with molecules. In our experiments, ammonia molecules are decelerated and cooled using electric fields, launched upwards with a velocity between 1.4 and 1.9 m/s and observed as they fall back under gravity. A combination of quadrupole lenses and bunching elements is used to shape the beam such that it has a large position spread and a small velocity spread (corresponding to a transverse temperature of <10 µK and a longitudinal temperature of <1 µK) when the molecules are in free fall, while being strongly focused at the detection region. The molecules are in free fall for up to 266 ms, making it possible, in principle, to perform sub-Hz measurements in molecular systems and paving the way for stringent tests of fundamental physics theories.
RESUMO
Long-lived radioactive krypton isotopes, (81)Kr (t1/2 = 229,000 year) and (85)Kr (t1/2 = 10.76 year), are ideal tracers. (81)Kr is cosmogenic and can be used for dating groundwater beyond the (14)C age. (85)Kr is a fission product and can be applied in atmospheric studies, nuclear safety inspections, and dating young groundwater. It has long been a challenge to analyze radio-krypton in small samples, in which the total number of such isotopes can be as low as 1 × 10(5). This work presents a system developed to analyze (81)Kr and (85)Kr from a few liters of air samples. A separation system based on cryogenic distillation and gas chromatographic separation is used to extract krypton gas with an efficiency of over 90% from air samples of 1-50 L. (85)Kr/Kr and (81)Kr/Kr ratios in krypton gases are determined from single-atom counting using a laser-based atom trap. In order to test the performance of the system, we have analyzed various samples collected from ambient air and extracted from groundwater, with a minimum size of 1 L. The system can be applied to analyze (81)Kr and (85)Kr in environmental samples including air, groundwater, and ices.
RESUMO
A cavity ring-down (CRD) spectrometer is built with a continuous-wave Ti:sapphire ring laser. Using a pair of R approximately 0.999 95 high-reflective mirrors, the noise-equivalent minimum detectable absorption loss reaches 7 x 10(-11)/cm over the spectral range of 780-830 nm. A thermal-stabilized Fabry-Perot interferometer is applied to calibrate the CRD spectrum with an accuracy of 1 x 10(-4) cm(-1). The quantitative measurement is carried out for the line profile measurements of some overtone absorption lines of C(2)H(2) near 787 nm. Doppler determined line shape has been observed with milli-Torr acetylene gas in the ring-down cavity. The instrumental line width is estimated from the line profile fitting to be <1 x 10(-4) cm(-1). It demonstrates that the CRD spectrometer with extremely high sensitivity is also very suitable for quantitative measurements including precise line profile studies in the near-infrared.
RESUMO
A midinfrared laser spectrometer is built up based on the difference frequency generation (DFG) of a Nd:YAG (yttrium aluminum garnet) laser and a tunable Ti:sapphire (Ti:Sa) laser. Tuning the Ti:Sa laser and operating properly with the periodically poled lithium niobate crystal, the DFG emission is tunable in the spectral range of 2.3-5.0 microm. The 1064 nm Nd:YAG laser frequency is stabilized to the 10(-6) cm(-1) level on a Doppler-broadened I(2) absorption line at 532 nm. As a result, the DFG emission frequency is stabilized within 1x10(-4) cm(-1). The measurement of an absorption line of CH(4) near 3 mum demonstrates that the DFG spectrometer is very suitable for the molecular absorption line profile studies in the midinfrared region.
