scholarly journals Light extinction by secondary organic aerosol: an intercomparison of three broadband cavity spectrometers

2013 ◽  
Vol 6 (11) ◽  
pp. 3115-3130 ◽  
Author(s):  
R. M. Varma ◽  
S. M. Ball ◽  
T. Brauers ◽  
H.-P. Dorn ◽  
U. Heitmann ◽  
...  
Keyword(s):  
Refractive Index ◽  
Optical Cavity ◽  
Light Extinction ◽  
Organic Nitrates ◽  
Aerosol Extinction ◽  
Particle Phase ◽  
Extinction Coefficients ◽  
Enhanced Absorption ◽  
Intercomparison Study ◽  
Absorption Spectrometer

Abstract. Broadband optical cavity spectrometers are maturing as a technology for trace-gas detection, but only recently have they been used to retrieve the extinction coefficient of aerosols. Sensitive broadband extinction measurements allow explicit separation of gas and particle phase spectral contributions, as well as continuous spectral measurements of aerosol extinction in favourable cases. In this work, we report an intercomparison study of the aerosol extinction coefficients measured by three such instruments: a broadband cavity ring-down spectrometer (BBCRDS), a cavity-enhanced differential optical absorption spectrometer (CE-DOAS), and an incoherent broadband cavity-enhanced absorption spectrometer (IBBCEAS). Experiments were carried out in the SAPHIR atmospheric simulation chamber as part of the NO3Comp campaign to compare the measurement capabilities of NO3 and N2O5 instrumentation. Aerosol extinction coefficients between 655 and 690 nm are reported for secondary organic aerosols (SOA) formed by the NO3 oxidation of β-pinene under dry and humid conditions. Despite different measurement approaches and spectral analysis procedures, the three instruments retrieved aerosol extinction coefficients that were in close agreement. The refractive index of SOA formed from the β-pinene + NO3 reaction was 1.61, and was not measurably affected by the chamber humidity or by aging of the aerosol over several hours. This refractive index is significantly larger than SOA refractive indices observed in other studies of OH and ozone-initiated terpene oxidations, and may be caused by the large proportion of organic nitrates in the particle phase. In an experiment involving ammonium sulfate particles, the aerosol extinction coefficients as measured by IBBCEAS were found to be in reasonable agreement with those calculated using the Mie theory. The results of the study demonstrate the potential of broadband cavity spectrometers for determining the optical properties of aerosols.

scholarly journals Light extinction by Secondary Organic Aerosol: an intercomparison of three broadband cavity spectrometers

2013 ◽  
Vol 6 (4) ◽  
pp. 6685-6727 ◽  
Author(s):  
R. M. Varma ◽  
S. M. Ball ◽  
T. Brauers ◽  
H.-P. Dorn ◽  
U. Heitmann ◽  
...  
Keyword(s):  
Refractive Index ◽  
Optical Cavity ◽  
Light Extinction ◽  
Organic Nitrates ◽  
Aerosol Extinction ◽  
Particle Phase ◽  
Extinction Coefficients ◽  
Enhanced Absorption ◽  
Intercomparison Study ◽  
Absorption Spectrometer

Abstract. Broadband optical cavity spectrometers are maturing as a technology for trace gas detection, but only recently have they been used to retrieve the extinction coefficient of aerosols. Sensitive broadband extinction measurements allow explicit separation of gas and particle phase spectral contributions, as well as continuous spectral measurements of aerosol extinction in favourable cases. In this work, we report an intercomparison study of the aerosol extinction coefficients measured by three such instruments: a broadband cavity ring-down spectrometer (BBCRDS), a cavity-enhanced differential optical absorption spectrometer (CE-DOAS), and an incoherent broadband cavity-enhanced absorption spectrometer (IBBCEAS). Experiments were carried out in the SAPHIR atmospheric simulation chamber as part of the NO3Comp campaign to compare the measurement capabilities of NO3 and N2O5 instrumentation. Aerosol extinction coefficients between 655 and 690 nm are reported for secondary organic aerosols (SOA) formed by the NO3 oxidation of β-pinene under dry and humid conditions. Despite different measurement approaches and spectral analysis procedures, the three instruments retrieved aerosol extinction coefficients that were in close agreement. The refractive index of SOA formed from the β-pinene + NO3 reaction was 1.61, and was not measurably affected by the chamber humidity or by aging of the aerosol over several hours. This refractive index is significantly larger than SOA refractive indices observed in other studies of OH and ozone-initiated terpene oxidations, and may be caused by the large proportion of organic nitrates in the particle phase. In an experiment involving ammonium sulphate particles the aerosol extinction coefficients as measured by IBBCEAS were found to be in reasonable agreement with those calculated using Mie theory. The results of the study demonstrate the potential of broadband cavity spectrometers for determining the optical properties of aerosols.

scholarly journals Initial investigation of the wavelength dependence of optical properties measured with a new multi-pass Aerosol Extinction Differential Optical Absorption Spectrometer (AE-DOAS)

2012 ◽  
Vol 5 (4) ◽  
pp. 709-721 ◽  
Author(s):  
R. T. Chartier ◽  
M. E. Greenslade
Keyword(s):  
Refractive Index ◽  
Optical Absorption ◽  
Radiative Forcing ◽  
Wavelength Dependence ◽  
Polystyrene Latex ◽  
Light Extinction ◽  
Aerosol Extinction ◽  
New Instrument ◽  
The Impact ◽  
Absorption Spectrometer

Abstract. Atmospheric aerosols directly affect climate by scattering and absorbing radiation. The magnitude of the impact is dependent upon the wavelength of light, but is often estimated near 550 nm. When light scattering and absorption by aerosols is approximated, the wavelength dependence of the refractive index for specific components is lost. As a result, climate models would have inherent uncertainties for aerosol contributions to radiative forcing when considering the entire solar spectrum. An aerosol extinction differential optical absorption spectrometer has been developed to directly measure aerosol extinction at mid-ultraviolet to near infrared wavelengths. The instrument consists of a spectrometer coupled to a closed White-type multi-pass gas cell with an adjustable path length of up to approximately 20 m. Laboratory measurements of various gases are compared with known absorption cross sections. Additionally, the extinction of monodisperse samples of polystyrene latex spheres are measured and compared to Mie theory generated with refractive index values from the literature to validate the new instrument. The polystyrene experiments also emphasize the ability of the new instrument to retrieve the wavelength dependent refractive index, especially in the ultraviolet wavelength regions where variability is expected. The spectrometer will be a significant advancement for determining wavelength dependent complex refractive indices in future laboratory studies as well as provide the ability to monitor ambient aerosol light extinction.

scholarly journals Initial investigation of the wavelength dependence of optical properties measured with a new multi-pass aerosol extinction differential optical absorption spectrometer (AE-DOAS)

2011 ◽  
Vol 4 (5) ◽  
pp. 6315-6349
Author(s):  
R. T. Chartier ◽  
M. E. Greenslade
Keyword(s):  
Refractive Index ◽  
Optical Absorption ◽  
Radiative Forcing ◽  
Wavelength Dependence ◽  
Polystyrene Latex ◽  
Light Extinction ◽  
Aerosol Extinction ◽  
New Instrument ◽  
The Impact ◽  
Absorption Spectrometer

Abstract. Atmospheric aerosols directly affect climate by scattering and absorbing radiation. The magnitude of the impact is dependent upon the wavelength of light, but is often estimated near 550 nm. When light scattering and absorption by aerosols is approximated, the wavelength dependence of the refractive index for specific components is lost. As a result, climate models would have inherent uncertainties for aerosol contributions to radiative forcing when considering the entire solar spectrum. An aerosol extinction differential optical absorption spectrometer has been developed to directly measure aerosol extinction at mid-ultraviolet to near infrared wavelengths. The instrument consists of a spectrometer coupled to a closed White-type multi-pass gas cell with an adjustable path length of up to approximately 20 m. Laboratory measurements of various gases are compared with known absorption cross sections. Additionally, the extinction of monodisperse samples of polystyrene latex spheres are measured and compared to Mie theory generated with refractive index values from the literature to validate the new instrument. The polystyrene experiments also emphasize the ability of the new instrument to retrieve the wavelength dependent refractive index, especially in the ultraviolet wavelength regions where variability is expected. The spectrometer will be a significant advancement for determining wavelength dependent complex refractive indices in future laboratory studies as well as provide the ability to monitor ambient aerosol light extinction.

scholarly journals Measurement of glyoxal using an incoherent broadband cavity enhanced absorption spectrometer

2008 ◽  
Vol 8 (4) ◽  
pp. 16517-16553 ◽  
Author(s):  
R. A. Washenfelder ◽  
A. O. Langford ◽  
H. Fuchs ◽  
S. S. Brown
Keyword(s):  
Rayleigh Scattering ◽  
Optical Cavity ◽  
Field Measurements ◽  
Array Detector ◽  
Enhanced Absorption ◽  
Minimum Detectable Absorption ◽  
Wide Range ◽  
Path Lengths ◽  
A Charge ◽  
Absorption Spectrometer

Abstract. We describe an instrument for simultaneous measurements of glyoxal (CHOCHO) and nitrogen dioxide (NO2) using cavity enhanced absorption spectroscopy with a broadband light source. The output of a Xenon arc lamp is coupled into a 1 m optical cavity, and the spectrum of light exiting the cavity is recorded by a grating spectrometer with a charge-coupled device (CCD) array detector. The mirror reflectivity and effective path lengths are determined from the known Rayleigh scattering of He and dry zero air (N2+O2). Least-squares fitting, using published reference spectra, allow the simultaneous retrieval of CHOCHO, NO2, O4, and H2O in the 441 to 469 nm spectral range. For a 1-min sampling time, the minimum detectable absorption is 4×10−10 cm−1, and the precision (±1σ) on signal for measurements of CHOCHO and NO2 is 29 pptv and 20 pptv, respectively. We directly compare the incoherent broadband cavity enhanced absorption spectrometer to 404 and 532 nm cavity ringdown instruments for CHOCHO and NO2 detection, and find linear agreement over a wide range of concentrations. The instrument has been tested in the laboratory with both synthetic and real air samples, and the demonstrated sensitivity and specificity suggest a strong potential for field measurements of both CHOCHO and NO2.

scholarly journals Assessment of NAAPS-RA performance in Maritime Southeast Asia during CAMP<sup>2</sup>Ex

2021 ◽  
Author(s):  
Eva-Lou Edwards ◽  
Jeffrey S. Reid ◽  
Peng Xian ◽  
Sharon P. Burton ◽  
Anthony L. Cook ◽  
...  
Keyword(s):  
Southeast Asia ◽  
Cloud Condensation Nuclei ◽  
Particle Mass ◽  
High Spectral Resolution ◽  
Light Extinction ◽  
Aerosol Extinction ◽  
Hygroscopic Growth ◽  
Extinction Coefficients ◽  
Wide Range ◽  
Aerosol Properties

Abstract. Monitoring and modeling aerosol particle lifecycle in Southeast Asia (SEA) is challenged by high cloud cover, complex meteorology, and the wide range of aerosol species, sources, and transformations found throughout the region. Satellite observations are limited, and there are few in situ observations of aerosol extinction profiles, aerosol properties, and environmental conditions. Therefore, accurate aerosol model outputs are crucial for the region. This work evaluates the Navy Aerosol Analysis and Prediction System Reanalysis (NAAPS-RA) aerosol optical thickness (AOT) and light extinction products using airborne aerosol and meteorological measurements from the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) in SEA. Modeled AOTs and extinction coefficients were compared to those retrieved with a High Spectral Resolution Lidar (HSRL-2). Correlations were highest for AOT in the mixed layer (AOTML; R2 = 0.83, bias = 0.00, root mean square error [RMSE] = 0.03) compared to total AOT (R2 = 0.68, bias = 0.01, RMSE = 0.14), although the correlations between the observations and 1° × 1° degree NAAPS-RA outputs were weaker in regions with strong gradients in aerosol properties, such as near areas of active convection. Correlations between simulated and retrieved aerosol extinction coefficients were highest from 145–500 m (R2 = 0.75, bias = 0.01 km−1, RMSE = 0.08 km−1) and decreased with increasing altitude (R2 = 0.69 and 0.26, bias = 0.00 and 0.00 km−1, RMSE = 0.09 and 0.00 km−1 for 500–1500 m and > 1500 m, respectively), which was likely a result of the use of bulk cloud mixing parameterizations. We also investigated the role of possible relative humidity (RH) errors in extinction simulations. Despite negative biases in modeled RH (−4.9, −7.7, and −2.3 % for altitudes < 500 m, 500–1500 m, and > 1500 m, respectively), AOT and extinction agreement with the HSRL-2 did not change significantly at any altitude when RHs from dropsondes were substituted into the model. Improvements may have been stunted due to errors in how NAAPS-RA modeled physics of particle hygroscopic growth, dry particle mass concentrations, and/or dry mass extinction efficiencies, especially when combined with AOT corrections from data assimilation. Specifically, the model overestimated the hygroscopicity of (i) smoke particles from biomass burning in the Maritime Continent (MC), and (ii) anthropogenic emissions transported from East Asia. This work provides insight into how certain environmental and microphysical properties influence AOT and extinction simulations, which can then be interpreted in the context of modeling global concentrations of particle mass and cloud condensation nuclei (CCN).

scholarly journals Measurement of glyoxal using an incoherent broadband cavity enhanced absorption spectrometer

2008 ◽  
Vol 8 (24) ◽  
pp. 7779-7793 ◽  
Author(s):  
R. A. Washenfelder ◽  
A. O. Langford ◽  
H. Fuchs ◽  
S. S. Brown
Keyword(s):  
Rayleigh Scattering ◽  
Optical Cavity ◽  
Field Measurements ◽  
Array Detector ◽  
Enhanced Absorption ◽  
Cavity Enhanced Absorption Spectroscopy ◽  
Wide Range ◽  
Path Lengths ◽  
A Charge ◽  
Absorption Spectrometer

Abstract. We describe an instrument for simultaneous measurements of glyoxal (CHOCHO) and nitrogen dioxide (NO2) using cavity enhanced absorption spectroscopy with a broadband light source. The output of a Xenon arc lamp is coupled into a 1 m optical cavity, and the spectrum of light exiting the cavity is recorded by a grating spectrometer with a charge-coupled device (CCD) array detector. The mirror reflectivity and effective path lengths are determined from the known Rayleigh scattering of He and dry zero air (N2+O2). Least-squares fitting, using published reference spectra, allow the simultaneous retrieval of CHOCHO, NO2, O4, and H2O in the 441 to 469 nm spectral range. For a 1-min sampling time, the precision (±1σ) on signal for measurements of CHOCHO and NO2 is 29 pptv and 20 pptv, respectively. We directly compare measurements made with the incoherent broadband cavity enhanced absorption spectrometer with those from cavity ringdown instruments detecting CHOCHO and NO2 at 404 and 532 nm, respectively, and find linear agreement over a wide range of concentrations. The instrument has been tested in the laboratory with both synthetic and real air samples, and the demonstrated sensitivity and specificity suggest a strong potential for field measurements of both CHOCHO and NO2.

scholarly journals A broadband cavity enhanced absorption spectrometer for aircraft measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water vapor

2016 ◽  
Vol 9 (2) ◽  
pp. 423-440 ◽  
Author(s):  
K.-E. Min ◽  
R. A. Washenfelder ◽  
W. P. Dubé ◽  
A. O. Langford ◽  
P. M. Edwards ◽  
...  
Keyword(s):  
Nitrogen Dioxide ◽  
Cross Sections ◽  
Nitrous Acid ◽  
Aircraft Measurements ◽  
Charge Coupled Device ◽  
Light Emitting ◽  
Enhanced Absorption ◽  
Field Campaigns ◽  
A Charge ◽  
Absorption Spectrometer

Abstract. We describe a two-channel broadband cavity enhanced absorption spectrometer (BBCEAS) for aircraft measurements of glyoxal (CHOCHO), methylglyoxal (CH3COCHO), nitrous acid (HONO), nitrogen dioxide (NO2), and water (H2O). The instrument spans 361–389 and 438–468 nm, using two light-emitting diodes (LEDs) and a single grating spectrometer with a charge-coupled device (CCD) detector. Robust performance is achieved using a custom optical mounting system, high-power LEDs with electronic on/off modulation, high-reflectivity cavity mirrors, and materials that minimize analyte surface losses. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns to date. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s. The accuracy is 5.8, 9.0, and 5.0 %, limited mainly by the available absorption cross sections.

scholarly journals A broadband optical cavity spectrometer for measuring weak near-ultraviolet absorption spectra of gases

2011 ◽  
Vol 4 (3) ◽  
pp. 425-436 ◽  
Author(s):  
J. Chen ◽  
D. S. Venables
Keyword(s):  
Absorption Spectra ◽  
Cross Sections ◽  
Optical Cavity ◽  
Absorption Cross ◽  
Enhanced Absorption ◽  
Cavity Enhanced Absorption Spectroscopy ◽  
Near Ultraviolet ◽  
Low Concentrations ◽  
Measured Absorption ◽  
Atmospheric Observations

Abstract. Accurate absorption spectra of gases in the near–ultraviolet (300 to 400 nm) are essential in atmospheric observations and laboratory studies. This paper describes a novel incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) instrument for measuring very weak absorption spectra from 335 to 375 nm. The instrument performance was validated against the 3B1-X1A1 transition of SO2. The measured absorption varied linearly with SO2 column density and the resulting spectrum agrees well with published spectra. Using the instrument, we report new absorption cross-sections of O3, acetone, 2-butanone, and 2-pentanone in this spectral region, where literature data diverge considerably. In the absorption minimum between the Huggins and Chappuis bands, our absorption spectra fall at the lower range of reported ozone absorption cross-sections. The spectra of the ketones agree with prior spectra at moderate absorptions, but differ significantly at the limits of other instruments' sensitivity. The collision-induced absorption of the O4 dimer at 360.5 nm was also measured and found to have a maximum cross-section of ca. 4.0×10−46 cm5 molecule−2. We demonstrate the application of the instrument to quantifying low concentrations of the short-lived radical, BrO, in the presence of stronger absorptions from Br2 and O3.

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