Near-IR (~1.5 µm) and mid-IR (~8 µm) laser heterodyne radiometers have been recently developed for ground-based remote sensing greenhouse gases in the atmospheric column. Field campaigns have been performed. The developed LHR instruments as well as the preliminary results of their applications to the measurements of CH4, N2O, CO2 (including 13CO2/12CO2), H2O vapor (and its isotopologue HDO) in the atmospheric column will be presented and discussed.
In this presentation, we report on the high-sensitivity and high-selectivity measurement of HONO by off-beam quartz-enhanced photoacoustic spectroscopy (QEPAS) in a very small gas sample volume (of ~ 40 mm3) resulting in a ultrashort residence time of less than 10 ms (compared to ~ 7 min for a conventional 210 m multipass cell or ~ 10-min. integration time for currently used chemical analytical instruments). A minimum detection limit of 66 ppbv (1σ) HONO was achieved at 70 mbar using a laser output power of 50 mW and 1 s integration time. This MDL was down to 7 ppbv at the optimal integration time of 150 s.
A photoacoustic (PA) spectrophone was developed for filter-free measurement of black carbon (BC) mass absorption coefficient (MAC) in the spectral region of ~ 442 nm using a blue diode laser. The PA sensor was characterized and calibrated using NO2 at standard calibrated concentrations, as well as at indoor and outdoor air concentrations via a side-by-side intercomparison with a commercial NOx analyzer. Black carbon (graphite) and volcanic ash samples were measured under laboratory condition. MAC of BC and volcanic ash sample were determined based on the measured particles optical absorption coefficient by the PA spectrophone, in combination with the mass concentration measured using a scanning mobility particle sizer (SMPS). A minimum detectable absorption coefficient (1σ) of ~ 1.2 Mm-1 for BC was achieved with a time solution of 1 second.
Global efforts to mitigate climate change have largely focused on reducing emissions of carbon dioxide (CO2), which is responsible for 55-60% of current anthropogenic radiative forcing on warming impact. Because of its long lifetime (~130 years [1]) in the atmosphere, long-lasting CO2 will remain the primary driver of long-term temperature rise even if new CO2 emissions dropped to zero. A "fast-action" climate mitigation strategies is therefore strongly needed to provide more sizeable short-term benefits than CO2 reductions by reducing emission of short-lived climate pollutants (SLCPs), having atmospheric lifetimes of less than 20 years [2], which would allow for short-term drops in atmospheric concentrations and hence slow climate change over the next several decades. Monitoring of climatically and environmentally active SLCPs is important not only for policy-based reporting, but also for basic process-based understanding of climate related processes in the atmosphere. In this talk, we will overview our recent progress in the developments and applications of laser-based optical instruments for the measurements of environmental and livestock emitted methane (CH4), as well as the measurement of black carbon (BC) absorption. The experimental detail, the preliminary measurement results, the corresponding data processing and analysis will be presented.
An incoherent broadband cavity enhanced UV-LED spectrometer (IBBCEAS) was developed to detect atmospheric HONO and NO2. Using a UV light emitting diode (LED) operating at ~ 366 nm in combination with a high finesse optical cavity, HONO and NO2 were able to be simultaneously measured with high sensitivity. Detection limits (for SNR=1) of 0.3 ppbv for HONO and 1 ppbv for NO2 were achieved with an optimum acquisition time of 120 s. Stability of the developed cavity enhanced UV-LED spectrometer has been characterized by means of an Allan variance analysis. Daytime and nighttime concentrations of atmospheric HONO and NO2 were measured and compared with data from LOPAP for HONO and blue light converter-based NOx analyzer for NO2. The present work performed in a real atmospheric environment demonstrates the feasibility of using IBBCEAS technique for interference (chemical and spectral) free measurement of HONO. Experimental detail will be presented, the problems encountered during the real atmospheric measurement will be discussed.
W. Chen, T. Wu, W. Zhao, G. Wysocki, X. Cui, C. Lengignon, R. Maamary, E. Fertein, C. Coeur, A. Cassez, Y. Wang, W. Zhang, X. Gao, W. Liu, F. Dong, G. Zha, Xu Zheng, T. Wang
Chemically reactive short-lived species play a crucial role in tropospheric processes affecting regional air quality and
global climate change. Contrary to long-lived species (such as greenhouse gases), fast, accurate and precise monitoring
changes in concentration of atmospheric short-lived species represents a real challenge due to their short life time (~1 s
for OH radical) and very low concentration in the atmosphere (down to 106 molecules/cm3, corresponding to 0.1 pptv at
standard temperature and pressure).
We report on our recent progress in instrumentation developments for spectroscopic sensing of trace reactive species.
Modern photonic sources such as quantum cascade laser (QCL), distributed feedback (DFB) diode laser, light emitting
diode (LED), difference-frequency generation (DFG) parametric source are implemented in conjunction with highsensitivity
spectroscopic measurement techniques for : (1) nitrous acid (HONO) monitoring by QCL-based long optical
pathlength absorption spectroscopy and LED-based IBBCEAS (incoherent broadband cavity-enhanced absorption
spectroscopy); (2) DFB laser-based hydroxyl free radical (OH) detection using WM-OA-ICOS (wavelength modulation
off-axis integrated cavity output spectroscopy) and FRS (Faraday rotation spectroscopy), respectively; (3) nitrate radical
(NO3) and nitrogen dioxide (NO2) simultaneous measurements with IBBCEAS approach.
Applications in field observation and in smog chamber study will be presented.
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