ACE-Asia Campaign. Aircraft-Based Aerosol Sampling During ACE-Asia and CRYSTAL-FACE Using an Aerodyne Aerosol Mass Spectrometer

Transcription

1 Aircraft-Based Aerosol Sampling During ACE-Asia and CRYSTAL-FACE Using an Aerodyne Aerosol Mass Spectrometer Roya Bahreini *, Jose L. Jimenez *, Alice Delia, Richard C. Flagan *, John H. Seinfeld *, John. T. Jayne and Douglas R. Worsnop * California Institute of Technology University of Colorado, Boulder Aerodyne Research Inc. ACE-Asia Campaign March-May Flights out of Iwakuni, Japan Goals: Characterize size, composition, hygroscopicity, and optical properties of the Asian aerosol Perform radiative closure studies of the western pacific atmosphere Perform regional-scale atmospheric modeling

2 First Airborne Deployment of an Twin Otter Cockpit =. m Power Consumption: W Weight: lb = 9 kg Depth: =. m =. m Size Calibration Results L t = v va vl v = vl + b D a + D* va v = vl + + D l b r x - Particle Time of Flight (s) nm nm 7 nm nm nm nm nm Particle velocity (m/s) nm nm nm nm 7 nm nm nm 7 9 Sample pressure (mbar) 7 9 Sample pressure (mbar)

3 Sensitivity Corrections Gain of the multiplier changes with time Need to take into account sensitivity changes γp Q =.kd A ρ m =.kd A ( γpρ ) γ d m =.k AP Corr AB Alt = ABAlt + f ( PGrd, PAlt ) M RT air P T AB AB Corr Alt Grd AB = ( AB t Alt Grd ) + f ( PGrd, P AB Grd Alt ) Air Beam-Pressure Variation x Air Beam (O + ) Lens Pressure.. O + Gas Beam (Hz).... Lens Pressure (Torr) Sampling Pressure (mbar)

4 Twin Otter Flight Tracks During ACE-Asia N. Korea Latitude, N RF RF RF S. Korea RF9 RF Japan RF7 RF7 RF RF RF RF,9,,, //-RF //-RF /9/-RF //-RF7 //-RF //-RF9 //-RF /7/-RF //-RF //-RF //-RF //-RF /7/-RF7 //-RF //-RF9 Longitude, E Mass vs. DMA Volume Total Mass (µg/m ) RF7 DMA (Wang, ) DMA Total Volume (µm /cm ) : AM /7/ : AM : AM Inferred density= g/cm Mass ratio of Organic/Sulfate ~.- density=.-. g/cm

5 Mass vs. DMA Volume RF9 DMA (Wang, ) Total Mass (ug/m) DMA Total Volume (um/cm) : AM // : AM : AM : AM : AM Mass/DMA Volume ~.7 ACE-Asia: RF9- Apr., Carmichael et al. Carmichael et al.

6 Sulfate Layers: RF9- Apr., Vertical Profiles of Sulfate and Organics RF9 (Apr. ) RF (Apr. 7) RF7 (Apr. 7) RF9 (Apr. ) RF (Apr. 7) RF7 (Apr. 7) Altitude (m) Altitude (m) Sulfate Mass Concentration (µg/m ) Organic Mass Concentration (µg/m )

7 Mixing State of Aerosols Ammonium dm/dlogda (µg/m ).... RF 7, 7 m Ammonium Sulfate 7 9 D a (nm) Sulfate dm/dlogda (µg/m ) Sulfate dm/dlogda (µg/m ) RF7, 7 m Sulfate Organics Organics dm/dlogda (µg/m ) 7 9 Da (nm) Major Fragments of Organics m/z=7 % m/z=7 % m/z=7 % m/z= % m/z= % m/z=7 % m/z= % m/z= % m/z=7 % m/z= % other m/z % c m/z= % m/z= % m/z= % m/z= % Ion Series Analysis: <: Unsaturated organics =-: Aliphatic organics >: Oxygenated organics =-: % =: % =: % =: % =: % =: % 7

8 vs. PILS Sulfate concentration (µg/m ) (a) : AM /7/ PILS Altitude : AM Twin Otter Altitude (m) 7 (µg/m ) (b) sulfate =.97*PILS r =.7 : line PILS ( / ) 7 vs. PILS Nitrate concentration (µg/m ) (C) : AM /7/ PILS Altitude : AM PILS size cut: ~ um NO seen on supermicron particles during ACE-Asia Possible NH NO evaporation in sampling inlet Twin Otter Altitude (m) (µg/m ) (d) Nitrate =.99*PILS r =. PILS (µg/m ) : line

9 vs. PILS Ammonium concentration (µg/m ) (e) : AM /7/ PILS Altitude : AM Twin Otter Altitude (m).. (f) Ammonium =.*PILS r =. : line (µg/m ) PILS (µg/m ). vs. MOUDI y =.x R =. Sulfate (ug/m ) - - Filter MOUDI size cut: ~ um NO seen on supermicron particles during ACE-Asia Possible NH NO evaporation in sampling inlet y =.x Nitrate (ug/m ) R =. c - - Filter 9

10 CRYSTAL-FACE Campaign July Flights out of Key West, FL Goals: Investigate tropical cloud chemical and physical properties and formation processes Characterize tracer distribution and aerosols (CCN, composition) in lower troposphere as well as in and around the cirrus anvils Measure the radiative flux below and above the anvil Developing Convective Systems Mass Concentration (µg/m ) Before Take-Off Sulfate Organics CCN (Vanreken et al., ) CNC (Jonsson, ) CCN/CPC Concentration (cm - ) 7: PM 7// : PM 9: PM : PM Mass Concentration (µg/m ) CCN/CPC Concentration (cm - ) 7: PM 7// 7: PM 7: PM : PM

11 Developing Convective Systems Mass Concentration (µg/m ) Sulfate Organics Altitude 7: PM 7// : PM : PM 9: PM 9: PM : PM : PM Altitude (m) Mass vs. DMA Volume Varutbangkul,

12 Summary ACE-Asia Submicron aerosols were present in discrete layers SO - was a major component of submicron aerosols and was observed in all flights Organics, NO -, and NH + were detected on some layers SO - size distribution was relatively uniform at various altitudes for several flights Very good correlation of mass and DMA volume CRYSTAL-FACE SO - and organics were the major components of submicron aerosols Back-up Slides

13 vs. DMA Sulfate dm/dlogd p (µg/m ) m DMA DMA dv/dlogd p (µm /cm ) D p (nm) m: Organics/SO =. m: Organics/SO =. DMA distribution has more of the organics effect at m Sulfate dm/dlogd p (µg/m ) m DMA DMA dv/dlogd p (µm /cm ) D p (nm) Vertical Profiles of Aerosol species RF, :-: Organics.*SO.*NH.*NO Altitude (m) Scaled Mass Concentration (µg/m )

14 Sulfate Layers during ACE-Asia Signal from SO + (m/z = amu) Signal from SO + (m/z = amu) Summary of ACE-Asia Observations Nuetr. Index NH /SO (mass) NO /SO (mass) NH /NO (mass) Org/SO (mass) NH /SO (mol) NO /SO (mol) NH /NO (mol) Average StdDev

15 Major Fragments of Organics m/z=7 % m/z=7 % m/z=7 % m/z= % m/z= % m/z=7 % m/z= % m/z= % m/z=7 % m/z= % other m/z % c m/z= % m/z= % m/z= % m/z= % =-: % diene, alkyne, cycloalkene, polyunsatd oxygen organic =: % alkene, cycloalkane, diunsatd cyclic alcohol =: % cyclic/unsatd ester, diketone =: % satd carbonyl, cyclic ether, cycloalkanol =: % cycloalkanol, alkyl amine, amide, carbamate =: % aliphatic alcohol and ether acid, ester, cyclic acetal Sulfate dm/dlogd a (scaled) Marine Layer RF9 (m) RF(m) RF7 (7m) Marine vs. Pollution Layer Sulfate dm/dlogd a (scaled) Pollution Layer RF9 (m) RF (m) RF7 ( m) D a (nm) Sulfate Marine Pollution Marine dm/dlogd a D a (nm) Pollution dm/dlogd a 7 7 D a (nm)

16 Ammonium dm/dlogd a (scaled) (c) RF9 (m) RF7 (7m) Marine vs. Pollution Layer D a (nm) Marine dm/dlogd a Ammonium Marine Pollution Ammonium dm/dlogd a (scaled) (d) RF9 (m) RF(m) RF7 (m) Pollution dm/dlogd a D a (nm) 7 7 D a (nm). Developing Convective Systems Mass Concentration (µg/m ) Sulfate Organics Altitude 7: PM 7// : PM : PM 9: PM 9: PM : PM : PM Altitude (m). Estimated Density (µg/m ).... 7: PM 7// : PM : PM 9: PM 9: PM : PM : PM