Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cav...Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.展开更多
We report construction of an iodine-stabilized laser frequency standard at 532 nm based on modulation transfer spectroscopy(MTS)technology with good reproducibility.A frequency stability of 2.5×10^(-14)at 1 s ave...We report construction of an iodine-stabilized laser frequency standard at 532 nm based on modulation transfer spectroscopy(MTS)technology with good reproducibility.A frequency stability of 2.5×10^(-14)at 1 s averaging time is achieved,and the frequency reproducibility has a relative uncertainty of 3.5×10^(-13),demonstrating the great stability of our setup.The systematic uncertainty of the iodine-stabilized laser frequency standard is evaluated,especially the contribution of the residual amplitude modulation(RAM).The contribution of the RAM in MTS cannot be evaluated directly.To solve this problem,we theoretically deduce the MTS signal with RAM under large modulation depth,and prove that the non-symmetric shape of the MTS signal is directly related to the MTS effect.The non-symmetric shape factor can be calibrated with a frequency comb,and in real experiments,this value can be obtained by least-squares fitting of the MTS signal,from which we can infer the RAMinduced frequency shift.The full frequency uncertainty is evaluated to be 5.3 kHz(corresponding to a relative frequency uncertainty of 9.4×10^(-12)).The corrected transition frequency has a difference from the BIPM-recommended value of 2 kHz,which is within 1σ uncertainty,proving the validity of our evaluation.展开更多
Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of pre...Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of precision spectroscopy and trace gas detection.Here,we report the development of a mid-infrared Fourier transform spectrometer based on an optical frequency comb combined with a Herriott-type multipass cell.Using this instrument,the broadband absorption spectra of several important molecules,including methane,acetylene,water molecules and nitrous oxide,are measured by near real-time data acquisition in the 2800-3500 cm^(-1)spectral region.The achieved minimum detectable absorption of the instrument is 4.4×10^(-8)cm^(-1)·Hz^(-1/2)per spectral element.Broadband spectra of H_(2)0 are fited using the Voigt profile multispectral fitting technique and the consistency of the concentration inversion is 1%.Our system also enables precise spectroscopic measurements,and it allows the determination of the spectral line positions and upper state constants of N_(2)O in the(0002)-(1000)band,with results in good agreement with those reported by Toth[Appl.Opt.30,5289(1991)].展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.U21A2028,42022051,62275250,42030609,41627810,91644107,and 91544228).
文摘Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.
基金the National Key Research and Development Program of China(Grant No.2017YFA0304401)Key-Area Research and Development Program of GuangDong Province,China(Grant No.2019B030330001)the National Natural Science Foundation of China(Grant Nos.11174095,61875065,91536116,and 11804108).
文摘We report construction of an iodine-stabilized laser frequency standard at 532 nm based on modulation transfer spectroscopy(MTS)technology with good reproducibility.A frequency stability of 2.5×10^(-14)at 1 s averaging time is achieved,and the frequency reproducibility has a relative uncertainty of 3.5×10^(-13),demonstrating the great stability of our setup.The systematic uncertainty of the iodine-stabilized laser frequency standard is evaluated,especially the contribution of the residual amplitude modulation(RAM).The contribution of the RAM in MTS cannot be evaluated directly.To solve this problem,we theoretically deduce the MTS signal with RAM under large modulation depth,and prove that the non-symmetric shape of the MTS signal is directly related to the MTS effect.The non-symmetric shape factor can be calibrated with a frequency comb,and in real experiments,this value can be obtained by least-squares fitting of the MTS signal,from which we can infer the RAMinduced frequency shift.The full frequency uncertainty is evaluated to be 5.3 kHz(corresponding to a relative frequency uncertainty of 9.4×10^(-12)).The corrected transition frequency has a difference from the BIPM-recommended value of 2 kHz,which is within 1σ uncertainty,proving the validity of our evaluation.
基金supported by the National Natural Science Foundation China(No.42022051,No.U21A2028)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.Y202089)the HFIPS Director's Fund(No.YZJJ202101,No.BJPY2023A02).
文摘Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of precision spectroscopy and trace gas detection.Here,we report the development of a mid-infrared Fourier transform spectrometer based on an optical frequency comb combined with a Herriott-type multipass cell.Using this instrument,the broadband absorption spectra of several important molecules,including methane,acetylene,water molecules and nitrous oxide,are measured by near real-time data acquisition in the 2800-3500 cm^(-1)spectral region.The achieved minimum detectable absorption of the instrument is 4.4×10^(-8)cm^(-1)·Hz^(-1/2)per spectral element.Broadband spectra of H_(2)0 are fited using the Voigt profile multispectral fitting technique and the consistency of the concentration inversion is 1%.Our system also enables precise spectroscopic measurements,and it allows the determination of the spectral line positions and upper state constants of N_(2)O in the(0002)-(1000)band,with results in good agreement with those reported by Toth[Appl.Opt.30,5289(1991)].
