Moisture measurement is of great needs in semiconductor industry, combustion diagnosis, meteorology, and atmospheric studies. We present an optical hygrometer based on cavity ring-down spectroscopy （CRDS）. By using ...Moisture measurement is of great needs in semiconductor industry, combustion diagnosis, meteorology, and atmospheric studies. We present an optical hygrometer based on cavity ring-down spectroscopy （CRDS）. By using different absorption lines of H20 in the 1.56 and 1.36 gm regions, we are able to determine the relative concentration （mole fraction） of water vapor from a few percent down to the 10-12 level. The quantitative accuracy is examined by comparing the CRDS hygrometer with a commercial chilled-mirror dew-point meter. The high sensitivity of the CRDS instrument allows a water detection limit of 8 pptv.展开更多
A two-channel thermal dissociation cavity ring down spectroscopy （CRDS） instrument has been built for in situ, real-time measurement of NO2 and total RNO2 （peroxy nitrates and alkyl nitrates） in ambient air, with ...A two-channel thermal dissociation cavity ring down spectroscopy （CRDS） instrument has been built for in situ, real-time measurement of NO2 and total RNO2 （peroxy nitrates and alkyl nitrates） in ambient air, with a NO2 detection limit of 0.10 ppbv at 1 s. A 6-day long measurement was conducted at urban site of Hefei by using the CRDS instrument with a time resolution of 3 s. A commercial molybdenum converted chemiluminescence （Mo-CL） instrument was also used for comparison. The average RNO2 concentration in the 6 days was measured to be 1.94 ppbv. The Mo-CL instrument overestimated the NO2 concentration by a bias of ＋1.69 ppbv in average, for the reason that it cannot distinguish RNO2 from NO2. The relative bias could be over 100% during the afternoon hours when NO2 was low but RNO2 was high.展开更多
Saturation spectroscopy is frequently used to obtain sub-Doppler measurement of atomic and molecular transitions. Optical resonant cavities can be used to enhance the effective absorption path length, and the laser po...Saturation spectroscopy is frequently used to obtain sub-Doppler measurement of atomic and molecular transitions. Optical resonant cavities can be used to enhance the effective absorption path length, and the laser power inside the cavity as well to saturate very weak ro-vibrational transitions of molecules. Three different cavity-enhanced methods, cavity enhanced absorption spectroscopy, cavity ring-down spectroscopy, and noise-immune cavity enhanced optical heterodyne molecular spectroscopy (NICE-OHMS), were compared by measuring the Lamb dip of a C2H2 line at 1.4 μm using a cavity with a finesse of 120000. The center of the line was determined by different cavity-enhanced methods, each giving a sub-kHz (δv/v≈10-12) statistical uncertainty. The sensitivity and precision of different methods were analyzed and compared. As demonstrated in this study, the NICE-OHMS method is the most sensitive one, but more investigation on the systematic uncertainty is necessary before its application in metrology studies toward a sub-kHz accuracy.展开更多
High-resolution ro-vibrational spectroscopy of ^15N2^16O in 1650-3450 cm-1 region is studied using highly enriched isotopologue sample. The positions of more than 7300 lines of ^15N2^16O isotopologue were measured wit...High-resolution ro-vibrational spectroscopy of ^15N2^16O in 1650-3450 cm-1 region is studied using highly enriched isotopologue sample. The positions of more than 7300 lines of ^15N2^16O isotopologue were measured with a typical accuracy of 5.0×10-4 cm-1. The transitions were rovibrationally assigned on the basis of the global effective Hamiltonian model. The band by band analysis allowed for the determination of the rovibrational parameters of a total of 73 bands. 29 of them are newly reported and more rotational transitions have been observed for the others. The maximum deviation of the preidictions of the effective Hamiltonian model is up to 0.70 cm-1 for the ^15N2^16O species.展开更多
Transitions of the 6υ3 overtone band of ^14N2 ^16O near 775 nm have been studied by continuous-wave cavity ring-down spectroscopy. Line positions and intensities were derived from a fit of the line shape using a hard...Transitions of the 6υ3 overtone band of ^14N2 ^16O near 775 nm have been studied by continuous-wave cavity ring-down spectroscopy. Line positions and intensities were derived from a fit of the line shape using a hard-collisional profile. The line positions determined with absolute accuracy of 5×10^-4 cm^-1 allowed us to reveal finer ro-vibrational couplings taking place after J〉14 except a strong anharmonic interaction identified by the effective Hamiltonian model. The absolute line intensities have also been retrieved with an estimated accuracy of 2% for a majority of the unblended lines. A new set of ro-vibrational and dipole moment parameters were derived from the experimental values. A comparison between the line positions and intensities of the 6υ3 band obtained in this work and those from previous studies is given.展开更多
Carbon dioxide pressure-broadened ro-vibrational transitions belonging to thev^2＋3v^3 band of H2160 have been measured with a sensitive cavity ring-down spectrometer. Water vapor of relatively low pressures （〈0.5 T...Carbon dioxide pressure-broadened ro-vibrational transitions belonging to thev^2＋3v^3 band of H2160 have been measured with a sensitive cavity ring-down spectrometer. Water vapor of relatively low pressures （〈0.5 Torr） was used to limit the self-collisions among water molecules. After the calibration using the precise atomic transitions of Rb and a thermo- stabilized Fabry-Perot interferometer, 10^-5 cm^-1 frequency accuracy has been achieved. Line parameters are derived from least-squares fitting of the spectra using the ＂soft＂ collision model. The retrieved line parameters can be applied in the study of water absorption in the CO2-rich atmospheres of planets like Venus and Mars.展开更多
The infrared absorption spectra of the CO monomer isolated in solid N2 have been recorded at various temperatures between 4.5 and 30 K. The absorption features of the fundamen- tal stretching mode show its linewidth a...The infrared absorption spectra of the CO monomer isolated in solid N2 have been recorded at various temperatures between 4.5 and 30 K. The absorption features of the fundamen- tal stretching mode show its linewidth and matrix-induced frequency shift to be weakly temperature-dependent. As the temperature of the matrix was raised, an increase in the linewidth together with a redshift in the central frequency was observed. These observations were explained in terms of the quenching of the CO rotational states by the N2 matrix into closely-lying librational states. A quantitative model was then used to calculate the energy difference between these librational states. Results show that they can be thermally populated through the absorption of matrix phonons.展开更多
Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH...Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH3 and SbH3 are calculated with the density functional theory and at the correlated MP2 level, respectively. The calculated band intensities are in good agreement with the available experimental data. The contribution to the band intensities from the different terms in the polynomial expansion of the dipole moments of four group V hydrides （NH3, PH3, AsH3 and SbH3） are discussed. It is concluded that the breakdown of the bond dipole approximation must be considered. The intensity “borrowing” effect due to the wave function mixing among the stretching vibrational states is found to be less significant for the molecules that reach the local mode limit.展开更多
基金jointly supported by the National Natural Science Foundation of China(No.22273093,No.41905018,No.21903080)the Ministry of Science and Technology of China(No.2022YFF0606500)。
基金supported by the National Natural Science Foundation of China(No.22125302,No.22173099,No.22288201,No.21873089,and No.21973037)the Guangdong Science and Technology Program(No.2019ZT08L455 and No.2019JC01X091)the Shenzhen Science and Technology Program(No.ZDSYS20200421111001787).
基金This work was supported by the National Basic Research Program of China （No.2013BAK12B00 and No.2013CB834602） and the National Natural Science Foundation of China （No.21225314 and No.21427804）.
文摘Moisture measurement is of great needs in semiconductor industry, combustion diagnosis, meteorology, and atmospheric studies. We present an optical hygrometer based on cavity ring-down spectroscopy （CRDS）. By using different absorption lines of H20 in the 1.56 and 1.36 gm regions, we are able to determine the relative concentration （mole fraction） of water vapor from a few percent down to the 10-12 level. The quantitative accuracy is examined by comparing the CRDS hygrometer with a commercial chilled-mirror dew-point meter. The high sensitivity of the CRDS instrument allows a water detection limit of 8 pptv.
文摘A two-channel thermal dissociation cavity ring down spectroscopy （CRDS） instrument has been built for in situ, real-time measurement of NO2 and total RNO2 （peroxy nitrates and alkyl nitrates） in ambient air, with a NO2 detection limit of 0.10 ppbv at 1 s. A 6-day long measurement was conducted at urban site of Hefei by using the CRDS instrument with a time resolution of 3 s. A commercial molybdenum converted chemiluminescence （Mo-CL） instrument was also used for comparison. The average RNO2 concentration in the 6 days was measured to be 1.94 ppbv. The Mo-CL instrument overestimated the NO2 concentration by a bias of ＋1.69 ppbv in average, for the reason that it cannot distinguish RNO2 from NO2. The relative bias could be over 100% during the afternoon hours when NO2 was low but RNO2 was high.
基金supported by the National Natural Science Foundation of China (No.21688102, No.91436209, and No.21427804)the Chinese Academy of Science (No.XDB21020100)
文摘Saturation spectroscopy is frequently used to obtain sub-Doppler measurement of atomic and molecular transitions. Optical resonant cavities can be used to enhance the effective absorption path length, and the laser power inside the cavity as well to saturate very weak ro-vibrational transitions of molecules. Three different cavity-enhanced methods, cavity enhanced absorption spectroscopy, cavity ring-down spectroscopy, and noise-immune cavity enhanced optical heterodyne molecular spectroscopy (NICE-OHMS), were compared by measuring the Lamb dip of a C2H2 line at 1.4 μm using a cavity with a finesse of 120000. The center of the line was determined by different cavity-enhanced methods, each giving a sub-kHz (δv/v≈10-12) statistical uncertainty. The sensitivity and precision of different methods were analyzed and compared. As demonstrated in this study, the NICE-OHMS method is the most sensitive one, but more investigation on the systematic uncertainty is necessary before its application in metrology studies toward a sub-kHz accuracy.
基金This work is supported by the National Natural Science Foundation of China （No.20903085）, the NKBRSF 2010CB9230, and RFBR-Russia （No.06-05- 39016）. The support of the Groupement de Recherche International SAMIA （Spectroscopie d＇Absorption des Mol@cules d＇Interet Atmospherique） between CNRS （France）, RFBR （Russia） and CAS （China） is also acknowledged.
文摘High-resolution ro-vibrational spectroscopy of ^15N2^16O in 1650-3450 cm-1 region is studied using highly enriched isotopologue sample. The positions of more than 7300 lines of ^15N2^16O isotopologue were measured with a typical accuracy of 5.0×10-4 cm-1. The transitions were rovibrationally assigned on the basis of the global effective Hamiltonian model. The band by band analysis allowed for the determination of the rovibrational parameters of a total of 73 bands. 29 of them are newly reported and more rotational transitions have been observed for the others. The maximum deviation of the preidictions of the effective Hamiltonian model is up to 0.70 cm-1 for the ^15N2^16O species.
基金This work was supported by the National Key Basic Research Program of China （2013CB834602 and 2013BAK12B02）, and the National Natural Science Foundation of China （No.21473172, No.21411130183, No.21303176）.
文摘Transitions of the 6υ3 overtone band of ^14N2 ^16O near 775 nm have been studied by continuous-wave cavity ring-down spectroscopy. Line positions and intensities were derived from a fit of the line shape using a hard-collisional profile. The line positions determined with absolute accuracy of 5×10^-4 cm^-1 allowed us to reveal finer ro-vibrational couplings taking place after J〉14 except a strong anharmonic interaction identified by the effective Hamiltonian model. The absolute line intensities have also been retrieved with an estimated accuracy of 2% for a majority of the unblended lines. A new set of ro-vibrational and dipole moment parameters were derived from the experimental values. A comparison between the line positions and intensities of the 6υ3 band obtained in this work and those from previous studies is given.
基金ACKNOWLEDGMENTS This work is supported by the National Natural Science Foundation （No.21225314 and No.20903085）, the National Basic Research Program of China （No.2013CB834602） and the Fundamental Research Funds for the Central Universities.
文摘Carbon dioxide pressure-broadened ro-vibrational transitions belonging to thev^2＋3v^3 band of H2160 have been measured with a sensitive cavity ring-down spectrometer. Water vapor of relatively low pressures （〈0.5 Torr） was used to limit the self-collisions among water molecules. After the calibration using the precise atomic transitions of Rb and a thermo- stabilized Fabry-Perot interferometer, 10^-5 cm^-1 frequency accuracy has been achieved. Line parameters are derived from least-squares fitting of the spectra using the ＂soft＂ collision model. The retrieved line parameters can be applied in the study of water absorption in the CO2-rich atmospheres of planets like Venus and Mars.
基金ACKNOWLEDGMENTS This work was supported by the Young International Scientist Fellowship from the Chinese Academy of Sciences, the National Natural Science Foundation （No.21225314 and No.11150110457）, the National Basic Research Program of China （No.2010CB923300）, and the Fundamental Research Funds for the Central Universities .
文摘The infrared absorption spectra of the CO monomer isolated in solid N2 have been recorded at various temperatures between 4.5 and 30 K. The absorption features of the fundamen- tal stretching mode show its linewidth and matrix-induced frequency shift to be weakly temperature-dependent. As the temperature of the matrix was raised, an increase in the linewidth together with a redshift in the central frequency was observed. These observations were explained in terms of the quenching of the CO rotational states by the N2 matrix into closely-lying librational states. A quantitative model was then used to calculate the energy difference between these librational states. Results show that they can be thermally populated through the absorption of matrix phonons.
基金Project supported by the National Natural Science Foundation of China （Grant Nos 20103007 and 20473079）.
文摘Stretching vibrational band intensities of XH3 （X=N, Sb） molecules are investigated employing three-dimensional dipole moment surfaces combined with the local mode Hamiltonian model. The dipole moment surfaces of NH3 and SbH3 are calculated with the density functional theory and at the correlated MP2 level, respectively. The calculated band intensities are in good agreement with the available experimental data. The contribution to the band intensities from the different terms in the polynomial expansion of the dipole moments of four group V hydrides （NH3, PH3, AsH3 and SbH3） are discussed. It is concluded that the breakdown of the bond dipole approximation must be considered. The intensity “borrowing” effect due to the wave function mixing among the stretching vibrational states is found to be less significant for the molecules that reach the local mode limit.
