A laser-induced fluorescence instrument for aircraft measurements of sulfurdioxide in the upper troposphere and lower stratosphere

Abstract. This work describes the development and testing of a new instrument for in situ measurements of sulfur dioxide (SO2) on airborne platforms in the upper troposphere and lower stratosphere (UT–LS). The instrument is based on the laser-induced fluorescence technique and uses the fifth harmonic of a tunable fiber-amplified semiconductor diode laser system at 1084.5 nm to excite SO2 at 216.9 nm. Sensitivity and background checks are achieved in flight by additions of SO2 calibration gas and zero air, respectively. Aircraft demonstration was performed during the NASA Volcano-Plume Investigation Readiness and Gas-Phase and Aerosol Sulfur (VIRGAS) experiment, which was a series of flights using the NASA WB-57F during October 2015 based at Ellington Field and Harlingen, Texas. During these flights, the instrument successfully measured SO2 in the UT–LS at background (non-volcanic) conditions with a precision of 2 ppt at 10 s and an overall uncertainty determined primarily by instrument drifts of ±(16 % + 0.9 ppt).

[1]  Y. Matsumi,et al.  Laser-induced fluorescence instrument for measuring atmospheric SO2 , 2005 .

[2]  Anne P. Thorne,et al.  High-resolution photoabsorption cross section measurements of SO2, 2: 220 to 325 nm at 295 K , 2003 .

[3]  Arthur L. Lane,et al.  A compilation of the absorption cross-sections of SO2 from 106 to 403 nm , 1993 .

[4]  John E. Barnes,et al.  Increase in background stratospheric aerosol observed with lidar at Mauna Loa Observatory and Boulder, Colorado , 2009 .

[5]  J. B. Paul,et al.  First direct measurements of formaldehyde flux via eddy covariance: implications for missing in-canopy formaldehyde sources , 2011 .

[6]  D. Fahey,et al.  A two-channel, tunable diode laser-based hygrometer for measurement of water vapor and cirrus cloud ice water content in the upper troposphere and lower stratosphere , 2015 .

[7]  R. Neely,et al.  The Persistently Variable “Background” Stratospheric Aerosol Layer and Global Climate Change , 2011, Science.

[8]  Jorge Lima,et al.  Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation , 2011, Nature.

[9]  Thomas F. Hanisco,et al.  Aircraft-borne, laser-induced fluorescence instrument for the in situ detection of hydroxyl and hydroperoxyl radicals , 1994 .

[10]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[11]  J. Brand,et al.  The ?*-? (2350 ) band system of sulphur dioxide , 1972 .

[12]  David S. Lee,et al.  Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application , 2010 .

[13]  H. Okabe Fluorescence and predissociation of sulfur dioxide , 1971 .

[14]  J. Lelieveld,et al.  The contribution of outdoor air pollution sources to premature mortality on a global scale , 2015, Nature.

[15]  Anne P. Thorne,et al.  High‐resolution photoabsorption cross‐section measurements of SO2 at 160 K between 199 and 220 nm , 2009 .

[16]  Vijay Kumar,et al.  Quantitative photoabsorption and flourescence spectroscopy of SO2 at 188–231 and 278.7–320 nm , 1992 .

[17]  G. Wolfe,et al.  A new airborne laser-induced fluorescence instrument for in situ detection of formaldehyde throughout the troposphere and lower stratosphere , 2014 .

[18]  J. Kar,et al.  CALIPSO detection of an Asian tropopause aerosol layer , 2011 .

[19]  W. Randel,et al.  Definitions and sharpness of the extratropical tropopause: A trace gas perspective , 2004 .

[20]  Louisa Emmons,et al.  Asian Monsoon Transport of Pollution to the Stratosphere , 2010, Science.

[21]  Jeffrey P. Koplow,et al.  Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifIer. , 2002 .

[22]  I. Riipinen,et al.  Direct Observations of Atmospheric Aerosol Nucleation , 2013, Science.

[23]  P. Jensen,et al.  The calculation of the vibrational states of SO2 in the C̃1B2 electronic state up to the SO(3Σ−)+O(3P) dissociation limit , 2000 .

[24]  T. Petäjä,et al.  A new atmospherically relevant oxidant of sulphur dioxide , 2012, Nature.

[25]  J. Pickering,et al.  High‐resolution photoabsorption cross‐section measurements of SO2 at 295 K between 198 and 220 nm , 1999 .

[26]  C. Voigt,et al.  The airborne mass spectrometer AIMS – Part 2: Measurements of trace gases with stratospheric or tropospheric origin in the UTLS , 2015 .

[27]  Tami C. Bond,et al.  Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom , 2006 .

[28]  L. Heidt,et al.  Trace gases in the Antarctic atmosphere , 1989 .

[29]  M. Rodgers,et al.  Single photon laser-induced fluorescence detection of NO and SO(2) for atmospheric conditions of composition and pressure. , 1982, Applied optics.

[30]  D. Fahey,et al.  Computer-controlled Teflon flow control valve , 1999 .

[31]  Hiroshi Hara,et al.  A global assessment of precipitation chemistry and deposition of sulfur, nitrogen, sea salt, base cations, organic acids, acidity and pH, and phosphorus , 2014 .

[32]  S. Rice,et al.  Comment on “Decay fluorescence from single vibronic levels of SO2” , 1973 .

[33]  S. J. Ciciora,et al.  A compact, fast UV photometer for measurement of ozone from research aircraft , 2012 .

[34]  D. Weisenstein,et al.  Efficient formation of stratospheric aerosol for climate engineering by emission of condensible vapor from aircraft , 2010 .

[35]  A. Stohl,et al.  East Asian SO 2 pollution plume over Europe – Part 1: Airborne trace gas measurements and source identification by particle dispersion model simulations , 2009 .

[36]  D. Weisenstein,et al.  The impact of geoengineering aerosols on stratospheric temperature and ozone , 2009 .