jgrd51735-sup-0001

advertisement
Supplementary Material for
Source-diagnostic dual-isotope composition and optical properties of
water-soluble organic carbon and elemental carbon in the South Asian
outflow intercepted over the Indian Ocean
Carme Bosch1, August Andersson1, Elena Kirillova1, Krishnakant Budhavant
2, Suresh Tiwari3, P. S. Praveen2,4, Lynn M. Russell5, Nicholas D.
Beres6, Veerabhadran Ramanathan5 and Örjan Gustafsson1*
(1 Department of Applied Environmental Science (ITM) and Bolin Centre for
Climate Research, Stockholm University, 10691 Stockholm, Sweden
2 Maldives Climate Observatory at Hanimaadhoo (MCOH), Republic of the
Maldives
3 Indian Institute of Tropical Meteorology (Branch), Prof. Ramnath Vij
Marg, New Delhi, India
4 Institute for Advanced Sustainability Studies (IASS), Potsdam, Germany
5 Scripps Institute of Oceanography, University of California, San Diego,
La Jolla, California, USA
6 Division of Atmospheric Sciences, Desert Research Institute, Nevada
System of Higher Education, Reno, Nevada, USA)
Journal of Geophysical Research – Atmospheres, 2014
Introduction
This data set contains the supporting data about back trajectories,
aerosol optical depth, meteorological conditions and other measurements
done on atmospheric particulate matter during the intensive campaign
CARDEX, which was held at the Maldives Climate Observatory of Hanimaadhoo
(MCOH) during February-March 2012. Back trajectories and aerosol optical
depth are presented on the figure “fs01.pdf”. Meteorological conditions,
particulate mass and aethalometer-based black carbon during the campaign
are given on the figure “fs02.pdf”. Ionic composition and functional
group concentrations identified by Fourier transform infrared
spectroscopy on aerosols are shown on figure “fs03.pdf”. A literature
review on optical properties of Brown Carbon (BrC) is presented on figure
“fs04.pdf” and table “ts04.pdf”. Results of carbon isotope-based studies
of non-water-soluble organic carbon (NWSOC) during the campaign are shown
on figure “fs05.pdf”. A sensitivity analysis for the calculation of the
solar radiation absorbed by WS-BrC relative to EC (%) is summarized at
“fs06.pdf”. Tables “ts01.pdf” and “ts02.pdf” present the results of the
uncertainty analysis of d13C and fraction fossil analysis and table
“ts04.pdf” the results of the sensitivity analysis of putative
inadvertent inclusion of instrument-pyrolyzed carbon (PyrC) in the
Elemental Carbon (EC) isolate for the computed fraction fossil (ffossil).
Detailed data included in the present paper is presented at “ts05.pdf”,
“ts06.pdf” and “ts07.pdf”.
1. fs01.pdf Seven days air mass back-trajectories at 500 m height from
NOAA HYSPLIT and Aerosol Optical Depth (AOD) at 555 nm from NASA MISR
during the CARDEX campaign
2. fs02.pdf Panel A: relative humidity and temperature; Panel B: ambient
air particulate mass (PM2.5 and TSP) and wind speed; Panel C:
aethalometer-based black carbon (BC) and thermal-optical method-based
elemental carbon (EC) in PM2.5 during the CARDEX campaign
3. fs03.pdf Panel A: functional group concentrations identified by
Fourier transform infrared spectroscopy (FTIR); Panel B: concentrations
of inorganic ions identified by ion chromatography; Panel C: non-sea salt
potassium to non-sea salt sulfate ratio (nss-K+/nss-SO42-); Panel D:
elemental carbon (EC) to non-sea salt sulfate (nss-SO42-); Panel E: nonsea salt potassium and sulfate to total potassium and sulfate (nss-K+/K+
& nss-SO42-/SO42-)
4. fs04.pdf Mass absorption cross section (MAC) of water-soluble brown
carbon (WS-BrC) in MCOH during CARDEX (this study) and Delhi compared to;
reported values of MAC in WS-BrC sources such as biomass-burning organic
aerosols (BBOA), humic-like substances (HULIS) and secondary organic
aerosols (SOA) (Panel A); other reported ambient aerosol MAC of WS-BrC
(Panel B), cited literature included at the end of this file
5. fs05.pdf Two-dimensional dual-carbon isotope d13C vs D14C composition
of elemental carbon (EC), total organic carbon (TOC), water-soluble
organic carbon (WSOC) and non-water-soluble organic carbon (NWSOC) in
PM2.5 and TSP at MCOH during CARDEX
6. fs06.pdf Solar radiation absorbed by WS-BrC relative to EC (%) at MCOH
calculated doing the following assumptions: original case calculated with
experimental MAC365,WS-BrC, MAC550, BC =7.5 and AAEBC=1 (#1); using
experimental MAC440 of WS-BrC (#2); MAC365, WS-BrC * 0.70 (#3); MAC365,
WS-BrC * 2 (#4); MAC550, BC =6.3(#5); MAC550, BC =8.7(#6).
7. ts01.pdf Results of ?13C and fraction fossil in TOC, EC and WSOC and
its uncertainty ranges estimated using a Monte Carlo approach in PM2.5
samples
7.1. Column “Start time” sampling start time YY/MM/dd hh:mm LT (UTC+5:00)
7.2. Column “Stop time” sampling stop time YY/MM/dd hh:mm LT (UTC+5:00)
7.3. Column “d13C” d13C values for TOC/EC/WSOC measured at NOSAMS (‰)
7.4. Column “Error” measurement error for d13C TOC/EC/WSOC values (‰)
7.5. Column “fraction fossil” blank corrected fraction fossil value for
TOC/EC/WSOC
7.6. Column “Error” measurement error for fraction fossil of TOC/EC/WSOC
8. ts02.pdf Results of ?13C and fraction fossil in TOC, EC and WSOC and
its uncertainty ranges estimated using a Monte Carlo approach in TSP
samples
8.1. Column “Start time” sampling start time YY/MM/dd hh:mm LT (UTC+5:00)
8.2. Column “Stop time” sampling stop time YY/MM/dd hh:mm LT (UTC+5:00)
8.3. Column “d13C” d13C values for TOC/EC/WSOC measured at NOSAMS (‰)
8.4. Column “Error” measurement error for d13C TOC/EC/WSOC values (‰)
8.5. Column “fraction fossil” blank corrected fraction fossil value for
TOC/EC/WSOC
8.6. Column “Error” measurement error for fraction fossil of TOC/WC/WSOC
9. ts03.pdf Results of the sensitivity analysis of putative inadvertent
inclusion of instrument-pyrolyzed carbon (PyrC) in the EC isolate for the
computed fraction fossil (ffossil) of the “true” EC for the CARDEX
campaign samples. Uncertainty ranges are estimated using the Monte Carlo
approach described at Chen, B., et al. (2013), Source Forensics of Black
Carbon Aerosols from China, Environ. Sci. Technol., 47, 9102-9108.
9.1. Column “Fraction of PyrC in the EC isolate (%)” assumed fraction of
pyrolyzed carbon included in the elemental carbon isolate
9.2. Column “true EC fraction fossil (%) in PM2.5” fraction fossil of
elemental carbon without pyrolyzed carbon in PM2.5 samples from CARDEX
campaign
9.3. Column “Error (%) in PM2.5” measurement error for fraction fossil of
EC estimated using a Monte Carlo approach
9.4. Column “true EC fraction fossil (%) in TSP” fraction fossil of
elemental carbon without pyrolyzed carbon in TSP samples from CARDEX
campaign
9.5. Column “Error (%) in TSP” measurement error for fraction fossil of
EC estimated using a Monte Carlo approach
10. ts04.pdf Literature review of Mass absorption cross section (MAC) and
Absorption Ångström Exponent (AAE) values for Brown Carbon in source and
ambient aerosols. Cited literature included at the end of this file
10.1. Column “Site/Aerosol source” indicates site of the measured ambient
aerosol or the measured aerosol source
10.2. Column “MAC(m2g-1)” mass absorption cross section
10.3. Column “lambda(nm)” wavelength of the MAC measurement
10.4. Column “AAE” Absorption Ångström Exponent
10.5. Column ”Method” method description
10.6. Column ”Reference” citation of the literature source
11. ts05.pdf WSOC concentrations, Mass absorption cross section (MAC365)
and Absorption Ångström Exponent (AAE) in PM2.5 samples during CARDEX
campaign
11.1. Column “Start time” sampling start time YY/MM/dd hh:mm LT
(UTC+5:00)
11.2. Column “Stop time” sampling stop time YY/MM/dd hh:mm LT (UTC+5:00)
11.3. Column “WSOC” water-soluble organic carbon concentrations
11.4. Column “AAE” Absorption Ångström Exponent computed between 330 –
400 nm
11.5. Column “MAC365” Mass absorption cross section at 365 nm
12. ts06.pdf
campaign
12.1. Column
(UTC+5:00)
12.2. Column
12.3. Column
12.4. Column
12.5. Column
OC, EC and TC concentrations in PM2.5 samples during CARDEX
“Start time” sampling start time YY/MM/dd hh:mm LT
“Stop time” sampling stop time YY/MM/dd hh:mm LT (UTC+5:00)
“OC” organic carbon concentration
“EC” elemental carbon concentration
“TC” total carbon concentration
13. ts07.pdf Period averages of functional group
identified by Fourier transform infrared spectroscopy
CARDEX campaign (μg m-3)
concentrations
(FTIR) during
References
Chen, Y., and T. C. Bond (2010), Light absorption by organic carbon from
wood combustion, Atmos. Chem. Phys., 10, 1773-1787.
Cheng, Y., et al. (2011), Mass absorption efficiency of elemental carbon
and water-soluble organic carbon in Beijing, China, Atmos. Chem. Phys.,
11, 11497-11510.
Chung, C. E., et al. (2012), Carbonaceous aerosol AAE inferred from insitu aerosol measurements at the Gosan ABC super site, and the
implications for brown carbon aerosol, Atmos. Chem. Phys., 12, 6173-6184.
Du, Z., et al. (2014), A yearlong study of water-soluble organic carbon
in Beijing II: Light absorption properties, Atmos. Environ. 89, 235-241.
Hecobian, A., et al. (2010), Water-Soluble Organic Aerosol material and
the light-absorption characteristics of aqueous extracts measured over
the Southeastern United States, Atmos. Chem. Phys., 10, 5965-5977.
Hoffer, A., et al. (2006), Optical properties of humic-like substances
(HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563-3570.
Kirchstetter, T. W., et al. (2004), Evidence that the spectral dependence
of light absorption by aerosols is affected by organic carbon, J.
Geophys. Res.-Atmos., 109, D21208, doi:10.1029/2004JD0049999
Kirchstetter, T. W., and T. L. Thatcher (2012), Contribution of organic
carbon to wood smoke particulate matter absorption of solar radiation,
Atmos. Chem. Phys., 12, 6067-6072.
Kirillova, E., et al. (2014a), Water-soluble organic carbon aerosols
during a full New Delhi winter: Isotope-based source apportionment and
optical properties, J. Geophys. Res.-Atmos. Accepted.
Kirillova, E. N., et al. (2014b), Sources and light absorption of watersoluble brown carbon aerosols in the outflow from northern China, Atmos.
Chem. Phys., 14, 1413-1422.
Lambe, A. T., et al. (2013), Relationship between Oxidation Level and
Optical Properties of Secondary Organic Aerosol, Environ. Sci. Technol.,
47, 6349-6357.
Liu, J., et al. (2013), Size-resolved measurements of brown carbon in
water and methanol extracts and estimates of their contribution to
ambient fine-particle light absorption, Atmos. Chem. Phys., 13, 1238912404.
Srinivas, B. and M.M. Sarin, (2013), Light-absorbing organic aerosols
(brown carbon) over the tropical Indian Ocean: impact of biomass burning
emissions, Environ. Res. Lett., 8, doi:10.1088/1748-9326/8/4/044042
Srinivas, B. and M.M. Sarin, (2014), Brown carbon in atmospheric outflow
from the Indo-Gangetic Plain: Mass absorption efficiency and temporal
variability, Atmos. Environ., 89, 835-843.
Wang, L., et al., (2013), Estimate of aerosol absorbing components of
black carbon, brown carbon, and dust from ground-based remote sensing
data of sun-sky radiometers, J. Geophys. Res.-Atmos., 118, 6534-6543.
Yang, M., et al., (2009), Attribution of aerosol light absorption to
black carbon, brown carbon, and dust in China – interpretations of
atmospheric measurements during EAST-AIRE, Atmos. Chem. Phys., 9, 20352050.
Zhang, X. L., et al. (2011), Light-absorbing soluble organic aerosol in
Los Angeles and Atlanta: A contrast in secondary organic aerosol,
Geophys. Res. Lett., 38, L21810, doi:10.1029/2011GL049385
Zhang, X. L., et al. (2013), Sources, Composition and Absorption Angstrom
Exponent of Light-absorbing Organic Components in Aerosol Extracts from
the Los Angeles Basin, Environ. Sci. Technol., 47, 3685-3693.
Download