We derive the expressions of the first and second harmonic signals on the basis of absorption spectral and lock-in theories, and determine the gas concentration according to the ratio of second and first harmonic sign...We derive the expressions of the first and second harmonic signals on the basis of absorption spectral and lock-in theories, and determine the gas concentration according to the ratio of second and first harmonic signals. It is found that the X and Y components of the harmonic signals are influenced by the phase shift between the detection and reference signal, and the phase shift can be any value in a range from 0 to 2π, which is different from the results obtained previously. Meanwhile, an additional item caused by the residual amplitude modulation will make a great contribution to the second harmonic signal, and may not be neglected under low absorbance conditions. Theoretical analysis indicates that subtracting back-ground signal from the second harmonic signal can remove the influence of this item, and can improve the measurement accuracy of gas concentration. On this basis, we select the transition of CO2 at 6527.64 cm-1 to analyse the approximation errors during the derivation by numerical simulation and then measure the CO2 concentration under low absorbance conditions, with absorbance varying from 1‰ to 6‰.展开更多
A compact prototype based on mid-infrared wavelength modulation spectroscopy（WMS）is developed for the simul-taneous monitoring of NO,NO2,and NH3 in the urban area.Three quantum cascade lasers（QCLs）with central fre...A compact prototype based on mid-infrared wavelength modulation spectroscopy（WMS）is developed for the simul-taneous monitoring of NO,NO2,and NH3 in the urban area.Three quantum cascade lasers（QCLs）with central frequencies around 1900.0 cm^-1,1600.0 cm^-1,and 1103.4 cm^-1are used for NO,NO2,and NH3detections,respectively,by timedivision multiplex.An open-path multi-pass cell of 60-m optical path length is applied to the instrument for high sensitivity and reducing the response time to less than 1 s.The prototype achieves a sub-ppb detection limit for all the three target gases with an average time of about 100 s.The instrument is installed in the Jiangsu environmental monitoring center to conduct performance tests on ambient air.Continuous 24-hour measurements show good agreement with the results of a reference instrument based on the chemiluminescence technique.展开更多
A novel wavelength modulation spectroscopy sensor for studying gas properties near 1.4 μm is developed, validated and used in a direct-connect supersonic combustion test facility. In this sensor there are two H2O tra...A novel wavelength modulation spectroscopy sensor for studying gas properties near 1.4 μm is developed, validated and used in a direct-connect supersonic combustion test facility. In this sensor there are two H2O transitions near 7185.60 cm^-1 and 7454.45 cm^-1 that are used to enable the measurements along the line-of-sight. According to an iterative algorithm, the gas pressure, temperature and species mole fraction can be measured simultaneously. The new sensor is used in the isolator and extender of the supersonic combustion test facility. In the isolator, the sensor resolves the transient and measured pressure, temperature and H2O mole fraction with accuracies of 2.5%, 8.2%, and 7.2%, respectively. Due to the non-uniform characteristic in the extender, the measured results cannot precisely characterize gas properties, but they can qualitatively describe the distinctions of different zones or the changes or fluctuations of the gas parameters.展开更多
A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed usin...A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed using concentration modulation(CM)spectroscopy.The intensities and orientations of the absorption peaks change with the demodulation phase,but the direction of one absorption peak of H2O is always opposite to the other peaks.The different spectral orientations of OH and H2O reflect the increase or the decrease of the number of particles in the energy levels.If more transient species can be detected in the discharge process,the dynamics of excitation,ionization,and decomposition of H2O can be better studied.This study shows that the demodulation phase relationship of CM spectrum can be used to study the population change of molecular energy levels.展开更多
For absorption linewidth inversion with wavelength modulation spectroscopy（WMS）, an optimized WMS spectral line fitting method was demonstrated to infer absorption linewidth effectively, and the analytical expressio...For absorption linewidth inversion with wavelength modulation spectroscopy（WMS）, an optimized WMS spectral line fitting method was demonstrated to infer absorption linewidth effectively, and the analytical expressions for relationships between Lorentzian linewidth and the separations of first harmonic peak-to-valley and second harmonic zero-crossing were deduced. The transition of CO_2 centered at 4991.25 cm^（-1） was used to verify the optimized spectral fitting method and the analytical expressions. Results showed that the optimized spectra fitting method was able to infer absorption accurately and compute more than 10 times faster than the commonly used numerical fitting procedure. The second harmonic zero-crossing separation method calculated an even 6 orders faster than the spectra fitting without losing any accuracy for Lorentzian dominated cases. Additionally, linewidth calculated through second harmonic zero-crossing was preferred for much smaller error than the first harmonic peak-to-valley separation method. The presented analytical expressions can also be used in on-line optical sensing applications, electron paramagnetic resonance, and further theoretical characterization of absorption lineshape.展开更多
Natural logarithm wavelength modulation spectroscopy(ln-WMS) is demonstrated in this Letter. Unlike the conventional wavelength modulation spectroscopy(WMS)-2 f technique, it is a linear method even for large absorban...Natural logarithm wavelength modulation spectroscopy(ln-WMS) is demonstrated in this Letter. Unlike the conventional wavelength modulation spectroscopy(WMS)-2 f technique, it is a linear method even for large absorbance, which is the core advantage of ln-WMS. The treating method used in ln-WMS is to take the natural logarithm of the transmitted intensity. In order to determine the proper demodulation phase, the η-seeking algorithm is introduced, which minimizes the absolute value of the first harmonic within the non-absorbing region. Subsequently, the second harmonic of the absorption signal is extracted by setting the demodulating phase as 2η. To illustrate the validity of ln-WMS, it was applied to water vapor experimentally. The result shows that even if the absorbance(base-e) is between 1.60 and 6.26, the linearity between ln-WMS-2 f and volume fraction is still established. For comparison, measurement with conventional WMS-2 f was also done, whose response no longer kept linearity. The η values retrieved in continuous measurements and the residuals were shown so as to evaluate the performance of the η-seeking algorithm. Time consumed by this algorithm was roughly 0.28 s per measurement. As an alternative WMS strategy, ln-WMS has a wide range of potential applications, especially where the absorbance is large or varies over a wide area.展开更多
Multi-component and multi-point trace gas sensing in the wavelength modulation spectroscopy is demonstrated based on the frequency-division multiplexing and time-division multiplexing technology.A reference photodetec...Multi-component and multi-point trace gas sensing in the wavelength modulation spectroscopy is demonstrated based on the frequency-division multiplexing and time-division multiplexing technology.A reference photodetector is connected in series with a reference gas cell with the constant concentration to measure the second-harmonics peak of the components for wavelength stabilization in real time.The central wavelengths of the distributed feedback lasers are locked to the target gas absorption centers by the reference second-harmonics signal using a digital proportional-integral-derivative controller.The distributed feedback lasers with different wavelengths and modulation frequencies are injected into the gas cell to achieve multi-components gas measurement by the frequency-division multiplexing technology.In addition,multi-point trace gas sensing is achieved by the time-division multiplexing technology using a photoswitch and a relay unit.We use this scheme to detect methane(CH4)at 1650.9 nm and water vapor(H2O)at 1368.597 nm as a proof of principle with the gas cell path length of 10 cm.The minimum detection limits achieved for H2O and CH4 are 1.13 ppm and 11.85 ppm respectively,with three-point gas cell measurement;thus 10.5-fold and 10.1-fold improvements are achieved in comparison with the traditional wavelength modulation spectroscopy.Meanwhile,their excellent R-square values reach 0.9983 and 0.99564 for the concentration ranges of 500 ppm to 2000 ppm and 800 ppm to 2700 ppm,respectively.展开更多
Conventional wavelength modulation spectroscopy(WMS)is vulnerable to the influence of low-frequency noise.Accuracy of the method highly depends on the performance of the costly lock-in amplifier.In this article,we rep...Conventional wavelength modulation spectroscopy(WMS)is vulnerable to the influence of low-frequency noise.Accuracy of the method highly depends on the performance of the costly lock-in amplifier.In this article,we report a new and effective method for reconstructing second-harmonic signals through WMS based on fast Fourier transform(FFT).This method is less disturbed by low-frequency noise because it does not use a low-frequency ramp wave.Formulation and detection procedures were presented.The discrete second-harmonic waveform can be obtained by continuously changing the DC signal and FFT analysis in this method.Second-harmonic waveforms acquired by the two means are generally consistent.The experimental study validates the obtained gas concentration from 5% to 30%,showing a good linear relationship by the proposed method.The maximum relative error on concentration extraction is 2.87%;as for conventional WMS,this value is 4.50%.The developed measurement method may have potential in computed tomography.展开更多
A simple and robust technique is reported to offset lock a single semiconductor laser to the atom resonance line with a frequency difference easily adjustable from a few tens of megahertz up to tens of gigahertz. The ...A simple and robust technique is reported to offset lock a single semiconductor laser to the atom resonance line with a frequency difference easily adjustable from a few tens of megahertz up to tens of gigahertz. The proposed scheme makes use of the frequency modulation spectroscopy by modulating sidebands of a fiber electro-optic modulator output. The short-term performances of a frequency offset locked semiconductor laser are experimentally demonstrated with the Allan variance of around 3.9 × 10-11 at a 2 s integration time. This method may have many applications, such as in Raman optics for an atom interferometer.展开更多
Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic a...Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic absorption,(2)modulation spectroscopy,and(3)the most widely used Tauc-plot.The excitonic absorption is based on a many-particle theory,which is physically the most correct approach,but requires more stringent crystalline quality and appropriate sample preparation and experimental implementation.The Tauc-plot is based on a single-particle theo⁃ry that neglects the many-electron effects.Modulation spectroscopy analyzes the spectroscopy features in the derivative spectrum,typically,of the reflectance and transmission under an external perturbation.Empirically,the bandgap ener⁃gy derived from the three approaches follow the order of E_(ex)>E_(MS)>E_(TP),where three transition energies are from exci⁃tonic absorption,modulation spectroscopy,and Tauc-plot,respectively.In principle,defining E_(g) as the single-elec⁃tron bandgap,we expect E_(g)>E_(ex),thus,E_(g)>E_(TP).In the literature,E_(TP) is often interpreted as E_(g),which is conceptual⁃ly problematic.However,in many cases,because the excitonic peaks are not readily identifiable,the inconsistency be⁃tween E_(g) and E_(TP) becomes invisible.In this brief review,real world examples are used(1)to illustrate how excitonic absorption features depend sensitively on the sample and measurement conditions;(2)to demonstrate the differences between E_(ex),E_(MS),and E_(TP) when they can be extracted simultaneously for one sample;and(3)to show how the popular⁃ly adopted Tauc-plot could lead to misleading results.Finally,it is pointed out that if the excitonic absorption is not ob⁃servable,the modulation spectroscopy can often yield a more useful and reasonable bandgap than Tauc-plot.展开更多
The modulation transfer spectroscopy in an ytterbium hollow cathode lamp at 399 nm is measured. The error signal for frequency locking is optimized by measuring the dependences of its slope, linewidth and magnitude on...The modulation transfer spectroscopy in an ytterbium hollow cathode lamp at 399 nm is measured. The error signal for frequency locking is optimized by measuring the dependences of its slope, linewidth and magnitude on various parameters. Under the optimum condition, the laser frequency at 399 nm can be stabilized. The long-term stability of laser frequency is measured by monitoring the fluorescence signal of the ytterbium atomic beam induced by the locked laser. The laser frequency is shown to be tightly locked, and the stabilized laser is successfully applied to the cooling of ytterbium atoms.展开更多
We introduce a new method of simultaneously implementing frequency stabilization and frequency shift for semiconductor lasers. We name this method the frequency tunable modulation transfer spectroscopy （FTMTS）. To r...We introduce a new method of simultaneously implementing frequency stabilization and frequency shift for semiconductor lasers. We name this method the frequency tunable modulation transfer spectroscopy （FTMTS）. To realize a stable output of 780 nm semiconductor laser, an FTMTS optical heterodyne frequency stabilization system is constructed. Before entering into the frequency stabilization system, the probe laser passes through an acousto-optical modulator （AOM） twice in advance to achieve tunable frequency while keeping the light path stable. According to the experimental results, the frequency changes from 120 MHz to 190 MHz after the double-pass AOM, and the intensity of laser entering into the system is greatly changed, but there is almost no change in the error signal of the FTMTS spectrum. Using this signal to lock the laser frequency, we can ensure that the frequency of the laser changes with the amount of AOM shift. Therefore, the magneto-optical trap （MOT）-molasses process can be implemented smoothly.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
Studies on the kinetics of gas-phase chemical reactions currently rely on calculations or simulations and lack simple,fast,and accurate direct measurement methods.We developed a tunable laser molecular absorption spec...Studies on the kinetics of gas-phase chemical reactions currently rely on calculations or simulations and lack simple,fast,and accurate direct measurement methods.We developed a tunable laser molecular absorption spectroscopy measurement system to achieve direct measurements of such reactions by using wavelength modulated spectroscopy and performed online measurements and diagnostics of molecular concentration,reaction temperature,and pressure change during the redox reaction of ozone with nitrogen oxides(NOx)with 0.1 s temporal resolution.This study provides a promising diagnostic tool for studying gas-phase chemical reaction kinetics.展开更多
We report laser frequency stabilization with modulation transfer spectroscopy（MTS） on 85 Rb atoms. With both PZT（piezo-electric transducer） slow-loop feedback and current fastloop feedback to the laser head, we ge...We report laser frequency stabilization with modulation transfer spectroscopy（MTS） on 85 Rb atoms. With both PZT（piezo-electric transducer） slow-loop feedback and current fastloop feedback to the laser head, we get a linewidth narrowing less than 5 kHz simultaneously. Laser injection to a laser diode and frequency beating with another polarization spectroscopy based stabilization setup are also employed to check the narrow linewidth property. With the help of the technique, a linewidth around k Hz-level laser is obtained and pave the way for the locking of the lattice laser of ytterbium clock with transfer cavity technique. The setup can be used as a frequency reference for precise frequency control of atomic clock system.展开更多
We present a modulation transfer spectroscopy（MTS） configuration based on an acousto-optic modulator by using a variant of the typical double pass structure. One beam is modulated by using an acousto-optic modulator...We present a modulation transfer spectroscopy（MTS） configuration based on an acousto-optic modulator by using a variant of the typical double pass structure. One beam is modulated by using an acousto-optic modulator in opposite diffraction order to cancel the carrier frequency shift and produce a modulated pump beam. The line shape performance is investigated theoretically and experimentally. Laser frequency stabilization of the proposed configuration is demonstrated for the133 Cs ｜62 S1/2, F = 4 → ｜62 P3/2, F = 5 transition. The Allan deviations, which are measured by using beat note signals and the three-cornered hat method, are 3.6×10-11 in an integration time of 100 s and approximately 4×10-11 in a longer integration time.展开更多
A quantum cascade laser（QCL） based system for simultaneous detection of CO and CO_2 is developed.The QCL can scan over two neighboring CO（2055.40 cm^（-1）） and CO_2（2055.16 cm^（-1）） lines with a single curren...A quantum cascade laser（QCL） based system for simultaneous detection of CO and CO_2 is developed.The QCL can scan over two neighboring CO（2055.40 cm^（-1）） and CO_2（2055.16 cm^（-1）） lines with a single current scan.The wavelength modulation spectroscopy（ f = 20 k Hz） is utilized to enhance the signal-to-noise ratio.A white cell with an effective optical path length of 74 m is used.The calibration of the sensor is performed and minimum detection limits of 1.3 ppb（1 × 10^（-9））for CO and 0.44 ppm（1 × 10^（-6）） for CO_2 are achieved.展开更多
The CS radical was generated by discharging the mixture gas of CS2 and Helium. The Doppler limited spectra of CS were recorded in the region of 12350-12950 cm^-1 using optical heterodyne concentration modulation absor...The CS radical was generated by discharging the mixture gas of CS2 and Helium. The Doppler limited spectra of CS were recorded in the region of 12350-12950 cm^-1 using optical heterodyne concentration modulation absorption spectroscopy. Three hundred and twenty-six lines were recorded and assigned to the d^3△-a^3П （8,1） band, in which eighty-three transitions were first observed. A set of improved molecular constants for the d^3△（v=8） and a^3П（v=1） levels were determined by a non-linear least-squares fitting of all the lines to the effective Hamiltonian.展开更多
Optical clocks with thermal atoms are characterized by compact size,simple structure,reduced weight,and low power consumption and have the potential for broad out-of-the-lab and commercial applications.Here,we demonst...Optical clocks with thermal atoms are characterized by compact size,simple structure,reduced weight,and low power consumption and have the potential for broad out-of-the-lab and commercial applications.Here,we demonstrate a 459 nm optical clock based on the 6S_(1/2)-7P_(1/2)transition in thermal^(133)Cs atoms.Two methods,modulation transfer spectroscopy(MTS)and frequency modulation spectroscopy(FMS),are employed to stabilize the frequency of a 459 nm commercial laser to the atomic transition.The MTS-MTS and MTS-FMS beat-note measurements show short-term frequency stabilities of 3.7×10^(-13)/√t and 6.4×10^(-13)/√t,respectively,at the averaging time t.The 459 nm passive optical clock further serves as the pump for an active 1470 nm optical clock based on the cavityless lasing.The resultant 1470 nm output power reaches over 10μW and the pump-beam-induced light shift is estimated to be 2π×11 Hz with a fractional uncertainty of 2.4×10^(-18).These results demonstrate the feasibility of hybridizing passive and active optical clocks,providing a promising route toward compact multi-wavelength optical frequency standards.展开更多
This feature article illustrates the potential of polarization modulation infrared reflection absorption spectroscopy(PM IRRAS)to provide molecular-level information about the structure,orientation and conformation of...This feature article illustrates the potential of polarization modulation infrared reflection absorption spectroscopy(PM IRRAS)to provide molecular-level information about the structure,orientation and conformation of constituents of thin films at electrode surfaces.PM IRRAS relies on the surface selection rules stating that the p-polarized IR beam is enhanced,while the s-polarized beam is attenuated at the metal surface.The difference between p-and s-polarized beams eliminates the background of the solvent and provides IR spectra at a single electrode potential.In contrast,two other popular in situ IR spectroscopic techniques,namely,subtractively normalized interfacial Fourier transform infrared spectroscopy(SNIFTIRS)and surface-enhanced infrared reflection absorption spectroscopy(SEIRAS),provide potential difference spectra to remove the signal from the bulk solution.In this feature article,we provide a brief tutorial on how to run the PM IRRAS experiment and describe the methods used for background elimination first.The application of the PM IRRAS in the biomimetic research is then illustrated by three examples:construction of a tethered bilayer,reconstitution of colicin into a phospholipid bilayer and determination of the orientation of nucleolipids in a monolayer assembled at a gold electrode surface.Finally,the structural changes of graphene oxide during its electrochemical reduction are described to highlight the promising application of PM IRRAS in materials science.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.51176085 and 51206086)
文摘We derive the expressions of the first and second harmonic signals on the basis of absorption spectral and lock-in theories, and determine the gas concentration according to the ratio of second and first harmonic signals. It is found that the X and Y components of the harmonic signals are influenced by the phase shift between the detection and reference signal, and the phase shift can be any value in a range from 0 to 2π, which is different from the results obtained previously. Meanwhile, an additional item caused by the residual amplitude modulation will make a great contribution to the second harmonic signal, and may not be neglected under low absorbance conditions. Theoretical analysis indicates that subtracting back-ground signal from the second harmonic signal can remove the influence of this item, and can improve the measurement accuracy of gas concentration. On this basis, we select the transition of CO2 at 6527.64 cm-1 to analyse the approximation errors during the derivation by numerical simulation and then measure the CO2 concentration under low absorbance conditions, with absorbance varying from 1‰ to 6‰.
基金Project supported by the National Key Scientific Instrument and Equipment Development,China(Grant No.2014YQ060537)the National Key Research and Development Program,China(Grant No.2016YFC0201103)
文摘A compact prototype based on mid-infrared wavelength modulation spectroscopy（WMS）is developed for the simul-taneous monitoring of NO,NO2,and NH3 in the urban area.Three quantum cascade lasers（QCLs）with central frequencies around 1900.0 cm^-1,1600.0 cm^-1,and 1103.4 cm^-1are used for NO,NO2,and NH3detections,respectively,by timedivision multiplex.An open-path multi-pass cell of 60-m optical path length is applied to the instrument for high sensitivity and reducing the response time to less than 1 s.The prototype achieves a sub-ppb detection limit for all the three target gases with an average time of about 100 s.The instrument is installed in the Jiangsu environmental monitoring center to conduct performance tests on ambient air.Continuous 24-hour measurements show good agreement with the results of a reference instrument based on the chemiluminescence technique.
基金supported by the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.21403299)
文摘A novel wavelength modulation spectroscopy sensor for studying gas properties near 1.4 μm is developed, validated and used in a direct-connect supersonic combustion test facility. In this sensor there are two H2O transitions near 7185.60 cm^-1 and 7454.45 cm^-1 that are used to enable the measurements along the line-of-sight. According to an iterative algorithm, the gas pressure, temperature and species mole fraction can be measured simultaneously. The new sensor is used in the isolator and extender of the supersonic combustion test facility. In the isolator, the sensor resolves the transient and measured pressure, temperature and H2O mole fraction with accuracies of 2.5%, 8.2%, and 7.2%, respectively. Due to the non-uniform characteristic in the extender, the measured results cannot precisely characterize gas properties, but they can qualitatively describe the distinctions of different zones or the changes or fluctuations of the gas parameters.
基金the National Natural Science Foundation of China(No.61625501,No.61427816)the Open Fund of the State Key Laboratory of High Field Laser Physics(SIOM)the Open Fund of the State Key Laboratory of Precision Spectroscopy。
文摘A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed using concentration modulation(CM)spectroscopy.The intensities and orientations of the absorption peaks change with the demodulation phase,but the direction of one absorption peak of H2O is always opposite to the other peaks.The different spectral orientations of OH and H2O reflect the increase or the decrease of the number of particles in the energy levels.If more transient species can be detected in the discharge process,the dynamics of excitation,ionization,and decomposition of H2O can be better studied.This study shows that the demodulation phase relationship of CM spectrum can be used to study the population change of molecular energy levels.
基金Project supported by the National Natural Science Foundation of China(Grant No.61505142)the Tianjin Natural Science Foundation(Grant No.16JCQNJC02100)
文摘For absorption linewidth inversion with wavelength modulation spectroscopy（WMS）, an optimized WMS spectral line fitting method was demonstrated to infer absorption linewidth effectively, and the analytical expressions for relationships between Lorentzian linewidth and the separations of first harmonic peak-to-valley and second harmonic zero-crossing were deduced. The transition of CO_2 centered at 4991.25 cm^（-1） was used to verify the optimized spectral fitting method and the analytical expressions. Results showed that the optimized spectra fitting method was able to infer absorption accurately and compute more than 10 times faster than the commonly used numerical fitting procedure. The second harmonic zero-crossing separation method calculated an even 6 orders faster than the spectra fitting without losing any accuracy for Lorentzian dominated cases. Additionally, linewidth calculated through second harmonic zero-crossing was preferred for much smaller error than the first harmonic peak-to-valley separation method. The presented analytical expressions can also be used in on-line optical sensing applications, electron paramagnetic resonance, and further theoretical characterization of absorption lineshape.
基金supported by the National Key Research and Development Program of China (No. 2018YFF0109600)。
文摘Natural logarithm wavelength modulation spectroscopy(ln-WMS) is demonstrated in this Letter. Unlike the conventional wavelength modulation spectroscopy(WMS)-2 f technique, it is a linear method even for large absorbance, which is the core advantage of ln-WMS. The treating method used in ln-WMS is to take the natural logarithm of the transmitted intensity. In order to determine the proper demodulation phase, the η-seeking algorithm is introduced, which minimizes the absolute value of the first harmonic within the non-absorbing region. Subsequently, the second harmonic of the absorption signal is extracted by setting the demodulating phase as 2η. To illustrate the validity of ln-WMS, it was applied to water vapor experimentally. The result shows that even if the absorbance(base-e) is between 1.60 and 6.26, the linearity between ln-WMS-2 f and volume fraction is still established. For comparison, measurement with conventional WMS-2 f was also done, whose response no longer kept linearity. The η values retrieved in continuous measurements and the residuals were shown so as to evaluate the performance of the η-seeking algorithm. Time consumed by this algorithm was roughly 0.28 s per measurement. As an alternative WMS strategy, ln-WMS has a wide range of potential applications, especially where the absorbance is large or varies over a wide area.
基金This work was supported by the Research Fund for the Doctoral Program of Liao Cheng University(Grant No.318051543)and the National Natural Science Foundation of China(Grant No.61475085).
文摘Multi-component and multi-point trace gas sensing in the wavelength modulation spectroscopy is demonstrated based on the frequency-division multiplexing and time-division multiplexing technology.A reference photodetector is connected in series with a reference gas cell with the constant concentration to measure the second-harmonics peak of the components for wavelength stabilization in real time.The central wavelengths of the distributed feedback lasers are locked to the target gas absorption centers by the reference second-harmonics signal using a digital proportional-integral-derivative controller.The distributed feedback lasers with different wavelengths and modulation frequencies are injected into the gas cell to achieve multi-components gas measurement by the frequency-division multiplexing technology.In addition,multi-point trace gas sensing is achieved by the time-division multiplexing technology using a photoswitch and a relay unit.We use this scheme to detect methane(CH4)at 1650.9 nm and water vapor(H2O)at 1368.597 nm as a proof of principle with the gas cell path length of 10 cm.The minimum detection limits achieved for H2O and CH4 are 1.13 ppm and 11.85 ppm respectively,with three-point gas cell measurement;thus 10.5-fold and 10.1-fold improvements are achieved in comparison with the traditional wavelength modulation spectroscopy.Meanwhile,their excellent R-square values reach 0.9983 and 0.99564 for the concentration ranges of 500 ppm to 2000 ppm and 800 ppm to 2700 ppm,respectively.
基金supported in part by the National Natural Science Foundation of China(Nos.61411130312 and 61308053)Guangdong Provincial Key Laboratory of Semiconductor Micro Display(No.2020B121202003)Foshan Science and Technology Bureau。
文摘Conventional wavelength modulation spectroscopy(WMS)is vulnerable to the influence of low-frequency noise.Accuracy of the method highly depends on the performance of the costly lock-in amplifier.In this article,we report a new and effective method for reconstructing second-harmonic signals through WMS based on fast Fourier transform(FFT).This method is less disturbed by low-frequency noise because it does not use a low-frequency ramp wave.Formulation and detection procedures were presented.The discrete second-harmonic waveform can be obtained by continuously changing the DC signal and FFT analysis in this method.Second-harmonic waveforms acquired by the two means are generally consistent.The experimental study validates the obtained gas concentration from 5% to 30%,showing a good linear relationship by the proposed method.The maximum relative error on concentration extraction is 2.87%;as for conventional WMS,this value is 4.50%.The developed measurement method may have potential in computed tomography.
基金supported by the National Natural Science Foundation of China(No.61473166)
文摘A simple and robust technique is reported to offset lock a single semiconductor laser to the atom resonance line with a frequency difference easily adjustable from a few tens of megahertz up to tens of gigahertz. The proposed scheme makes use of the frequency modulation spectroscopy by modulating sidebands of a fiber electro-optic modulator output. The short-term performances of a frequency offset locked semiconductor laser are experimentally demonstrated with the Allan variance of around 3.9 × 10-11 at a 2 s integration time. This method may have many applications, such as in Raman optics for an atom interferometer.
基金Supported by Bissell Distinguished Professor Endowment Fund at UNC-Charlotte。
文摘Although there are numerous optical spectroscopy techniques and methods that have been used to extract the fundamental bandgap of a semiconductor,most of them belong to one of these three approaches:(1)the excitonic absorption,(2)modulation spectroscopy,and(3)the most widely used Tauc-plot.The excitonic absorption is based on a many-particle theory,which is physically the most correct approach,but requires more stringent crystalline quality and appropriate sample preparation and experimental implementation.The Tauc-plot is based on a single-particle theo⁃ry that neglects the many-electron effects.Modulation spectroscopy analyzes the spectroscopy features in the derivative spectrum,typically,of the reflectance and transmission under an external perturbation.Empirically,the bandgap ener⁃gy derived from the three approaches follow the order of E_(ex)>E_(MS)>E_(TP),where three transition energies are from exci⁃tonic absorption,modulation spectroscopy,and Tauc-plot,respectively.In principle,defining E_(g) as the single-elec⁃tron bandgap,we expect E_(g)>E_(ex),thus,E_(g)>E_(TP).In the literature,E_(TP) is often interpreted as E_(g),which is conceptual⁃ly problematic.However,in many cases,because the excitonic peaks are not readily identifiable,the inconsistency be⁃tween E_(g) and E_(TP) becomes invisible.In this brief review,real world examples are used(1)to illustrate how excitonic absorption features depend sensitively on the sample and measurement conditions;(2)to demonstrate the differences between E_(ex),E_(MS),and E_(TP) when they can be extracted simultaneously for one sample;and(3)to show how the popular⁃ly adopted Tauc-plot could lead to misleading results.Finally,it is pointed out that if the excitonic absorption is not ob⁃servable,the modulation spectroscopy can often yield a more useful and reasonable bandgap than Tauc-plot.
基金Project supported by the National Natural Science Foundation of China(Grant No.10774044)the National Key Basic Research and Development Program of China(Grant No.2010CB922903)+1 种基金the Science and Technology Commission of Shanghai Municipality of China(Grant No.07JC14019)Shanghai Pujiang Talent Program of China(Grant No.07PJ14038)
文摘The modulation transfer spectroscopy in an ytterbium hollow cathode lamp at 399 nm is measured. The error signal for frequency locking is optimized by measuring the dependences of its slope, linewidth and magnitude on various parameters. Under the optimum condition, the laser frequency at 399 nm can be stabilized. The long-term stability of laser frequency is measured by monitoring the fluorescence signal of the ytterbium atomic beam induced by the locked laser. The laser frequency is shown to be tightly locked, and the stabilized laser is successfully applied to the cooling of ytterbium atoms.
基金Project supported by the National Key Scientific Instrument and Equipment Development Project,China(Grant No.2014YQ35046103)
文摘We introduce a new method of simultaneously implementing frequency stabilization and frequency shift for semiconductor lasers. We name this method the frequency tunable modulation transfer spectroscopy （FTMTS）. To realize a stable output of 780 nm semiconductor laser, an FTMTS optical heterodyne frequency stabilization system is constructed. Before entering into the frequency stabilization system, the probe laser passes through an acousto-optical modulator （AOM） twice in advance to achieve tunable frequency while keeping the light path stable. According to the experimental results, the frequency changes from 120 MHz to 190 MHz after the double-pass AOM, and the intensity of laser entering into the system is greatly changed, but there is almost no change in the error signal of the FTMTS spectrum. Using this signal to lock the laser frequency, we can ensure that the frequency of the laser changes with the amount of AOM shift. Therefore, the magneto-optical trap （MOT）-molasses process can be implemented smoothly.
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 in part by the National Natural Science Foundation of China(No.52176064)Tianjin Natural Science Foundation(No.20JCYBJC00160).
文摘Studies on the kinetics of gas-phase chemical reactions currently rely on calculations or simulations and lack simple,fast,and accurate direct measurement methods.We developed a tunable laser molecular absorption spectroscopy measurement system to achieve direct measurements of such reactions by using wavelength modulated spectroscopy and performed online measurements and diagnostics of molecular concentration,reaction temperature,and pressure change during the redox reaction of ozone with nitrogen oxides(NOx)with 0.1 s temporal resolution.This study provides a promising diagnostic tool for studying gas-phase chemical reaction kinetics.
基金Supported by the National Natural Science Foundation of China(61227805,11574352,91536104,91636215)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB21030700)
文摘We report laser frequency stabilization with modulation transfer spectroscopy（MTS） on 85 Rb atoms. With both PZT（piezo-electric transducer） slow-loop feedback and current fastloop feedback to the laser head, we get a linewidth narrowing less than 5 kHz simultaneously. Laser injection to a laser diode and frequency beating with another polarization spectroscopy based stabilization setup are also employed to check the narrow linewidth property. With the help of the technique, a linewidth around k Hz-level laser is obtained and pave the way for the locking of the lattice laser of ytterbium clock with transfer cavity technique. The setup can be used as a frequency reference for precise frequency control of atomic clock system.
基金Project supported by the National Key Research and Development Program of China(Grant No.2016YFA0302101)the Foundation of China Academy of Space Technologythe Initiative Program of State Key Laboratory of Precision Measurement Technology and Instruments,China
文摘We present a modulation transfer spectroscopy（MTS） configuration based on an acousto-optic modulator by using a variant of the typical double pass structure. One beam is modulated by using an acousto-optic modulator in opposite diffraction order to cancel the carrier frequency shift and produce a modulated pump beam. The line shape performance is investigated theoretically and experimentally. Laser frequency stabilization of the proposed configuration is demonstrated for the133 Cs ｜62 S1/2, F = 4 → ｜62 P3/2, F = 5 transition. The Allan deviations, which are measured by using beat note signals and the three-cornered hat method, are 3.6×10-11 in an integration time of 100 s and approximately 4×10-11 in a longer integration time.
基金Project supported by the National Key Scientific Instrument and Equipment Development Project of China(Grnat No.2014YQ060537)the National Basic Research Program of China(Grant No.2013CB632803)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA05040102)the National Natural Science Foundation of China(Grant No.41405134)
文摘A quantum cascade laser（QCL） based system for simultaneous detection of CO and CO_2 is developed.The QCL can scan over two neighboring CO（2055.40 cm^（-1）） and CO_2（2055.16 cm^（-1）） lines with a single current scan.The wavelength modulation spectroscopy（ f = 20 k Hz） is utilized to enhance the signal-to-noise ratio.A white cell with an effective optical path length of 74 m is used.The calibration of the sensor is performed and minimum detection limits of 1.3 ppb（1 × 10^（-9））for CO and 0.44 ppm（1 × 10^（-6）） for CO_2 are achieved.
文摘The CS radical was generated by discharging the mixture gas of CS2 and Helium. The Doppler limited spectra of CS were recorded in the region of 12350-12950 cm^-1 using optical heterodyne concentration modulation absorption spectroscopy. Three hundred and twenty-six lines were recorded and assigned to the d^3△-a^3П （8,1） band, in which eighty-three transitions were first observed. A set of improved molecular constants for the d^3△（v=8） and a^3П（v=1） levels were determined by a non-linear least-squares fitting of all the lines to the effective Hamiltonian.
基金provided by CAS Project for Young Scientists in Basic Research(Grant No.YSBR-085)National Time Service Center(Grant No.E239SC1101)+1 种基金the funding of Wenzhou Major Science&Technology Innovation Key Project(Grant No.ZG2023021)supported by Innovation Program for Quantum Science and Technology(Grant No.2021ZD0303200).
文摘Optical clocks with thermal atoms are characterized by compact size,simple structure,reduced weight,and low power consumption and have the potential for broad out-of-the-lab and commercial applications.Here,we demonstrate a 459 nm optical clock based on the 6S_(1/2)-7P_(1/2)transition in thermal^(133)Cs atoms.Two methods,modulation transfer spectroscopy(MTS)and frequency modulation spectroscopy(FMS),are employed to stabilize the frequency of a 459 nm commercial laser to the atomic transition.The MTS-MTS and MTS-FMS beat-note measurements show short-term frequency stabilities of 3.7×10^(-13)/√t and 6.4×10^(-13)/√t,respectively,at the averaging time t.The 459 nm passive optical clock further serves as the pump for an active 1470 nm optical clock based on the cavityless lasing.The resultant 1470 nm output power reaches over 10μW and the pump-beam-induced light shift is estimated to be 2π×11 Hz with a fractional uncertainty of 2.4×10^(-18).These results demonstrate the feasibility of hybridizing passive and active optical clocks,providing a promising route toward compact multi-wavelength optical frequency standards.
基金This research was funded by Discovery Grants from the Natural Sciences and Engineering Research Council of Canada(JL:RGPIN-2022-03958AC:RGPIN-2022-04238).
文摘This feature article illustrates the potential of polarization modulation infrared reflection absorption spectroscopy(PM IRRAS)to provide molecular-level information about the structure,orientation and conformation of constituents of thin films at electrode surfaces.PM IRRAS relies on the surface selection rules stating that the p-polarized IR beam is enhanced,while the s-polarized beam is attenuated at the metal surface.The difference between p-and s-polarized beams eliminates the background of the solvent and provides IR spectra at a single electrode potential.In contrast,two other popular in situ IR spectroscopic techniques,namely,subtractively normalized interfacial Fourier transform infrared spectroscopy(SNIFTIRS)and surface-enhanced infrared reflection absorption spectroscopy(SEIRAS),provide potential difference spectra to remove the signal from the bulk solution.In this feature article,we provide a brief tutorial on how to run the PM IRRAS experiment and describe the methods used for background elimination first.The application of the PM IRRAS in the biomimetic research is then illustrated by three examples:construction of a tethered bilayer,reconstitution of colicin into a phospholipid bilayer and determination of the orientation of nucleolipids in a monolayer assembled at a gold electrode surface.Finally,the structural changes of graphene oxide during its electrochemical reduction are described to highlight the promising application of PM IRRAS in materials science.
