+32. DMS Lovelock. et al., DMSP Liss DMS. Eriksson, DMS HS,SO SO SO. Koga. DMS MSA 0* Davison DMS,**- +* /*

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1 1- / * / + * - +1 * + SD +2 2 * 3 +* /* DMS MSA x +2 : Key words: Antarctica sulfur isotope ratio biogenic dimethylsulfide DMS Lovelock et al +31 DMS HS - Möller MSA + 33* 2/0* * 2/0* * * 2/// -+3* * : * Koga et al +333 ; DMS MSA 0* Davison et al +330 DMSP Liss et al +331 DMS DMSP DMS Eriksson 3/ DMS +30- DMS DMS **-

2 / *++ mol HCl +* BaCl - - Ba S Ssample S Sstd */ mm ADVAN- CDT EA- Nielsen +31 Calhoun et al +33+ ; Norman et al **0 Dual Inlet DI-IRMS + Fig + Location of the sampling point TEC C*/ A*/ A Giesemann et al +33 2** Ba / Ba * mg +* Ba *** V O **+ Sn Carlo Elba NC/** Finnigan MAT MAT/ + Thermo Electron Conflow EA- IRMS *** ** Fig S S Canyon Diablo troilite CDT */ mm ADVANTEC C*/ A*1A 0 / - S S sample d S + - S S +*** std

3 1- / * EA-IRMS Fig The illustration of EA-IRMS system Table + Analytical condition of Elemental Analy- Table Sulfur isotope composition of Ba zer (EA) for sulfur isotope analysis reagent samples ** DI- IRMS * Ba NIST NBS-+1 d S * - IRMS *- *-0 MSS-- / d S - / +32- Sigma-Aldrich Inc Merck & Co Inc + * +0 + Ba Ba +* SiO VO / Yanagisawa and Sakai +32- Calhoun et al +33+ ; Norman et al **0 Finnigan MAT MAT/ DI-IRMS Ba d S +0 +

4 / *++ Cl +333 Dionex; ** i Ba 3 - Fig * + SD d S and d S of in surface snow cover +2 2 * 3 - Relationship between collected at Antarctica k Na sam sam d S concentration Table - The results of analytical data d S sam d Ssam sea d Ssam sam sam * /+ +31/ d Na ; Wilson sam S sea +312 Cl Na Na *- ; Rees et al Pruett et al ** RIDSA Cl S **-; Kawamura et al **1 Cl d k Cl

5 1- / * / : +2 1 / / * DMS MSA Koga et al +333 d S Sanusi et al **0; Calhoun et al +33+ ; Romero and Thiemens **- / 2* -* d S +2 +* /* d S samd Ssead SRsea d S R d S d S *- R R * + */ *3 */ sam d S + 0 * + sea SD d S +2 sea d S Fig d S Relationship between sea-salt contribution and d S in snow cover at Antarctica Fig / / The range of d S values for sea-salt sulfate and biogenic sulfur by literatures

6 / *++ Giesemann A Jäger H-J Norman AL Krouse H / R and Brand WA +33 : On-line sulfur-isotope determination using an elemental analyzer coupled to a mass spectrometer Anal Chem Ba +* **-: +2 ** + +1 * + S Jonsell U Haon ME Morth CM and Torssander P **/: Sulfur isotopic signals in two shallow ice cores from Dronning Maud Land Antarctica Tellus /1B + -/* D: +2 2 * 3 +* /* d S +2 + Kawamura K Narukawa M Li SM and Barrie L + A **1: Size distributions of dicarboxylic acids DMS MSA x +2 and inorganic ions in atmospheric aerosols collected during polar sunrise in the Canadian high Arctic J Geophys Res ++ D +*-*1 doi: +* +*3/ **0 JD **2 Koga S Nagao I Tanaka H and Mouri H +333: Methanesulfonate and non-sea-salt sulfate concentrations in aerosols at Syowa Antarctica J Meteor Soc Japan 11 +// +0 Liss PS Hatton AD Malin G Nightingale PD and Turner SM +331: Marine sulphur emission Phil Trans RSoc Lond B -/ +/3 +03 Lovelock JE Maggs R J and Rasmussen RA +31 : Atmospheric dimethyl sulphide and the natural sulphur cycle Nature -1 / / Möller D +32 : On the global natural sulphur emis- sion Atmos Environ **: Nielsen H +31 : Isotopic composition of the major contributors to atmospheric sulfur Tellus XXVI Alexander B Thiemens MH Farquhar J Kaufman A J Savarino J and Delmas R J **-: East +- + Norman AL Anlauf K Hayden K Thompson B Antarctic ice core sulfur isotope measurements Brook JR Li SM and Bottenheim J **0: Aeroover a complete glacial-interglacial cycle J Geo- sol sulphate and its oxidation on the Pacific NW phys Res +*2 120 doi: +* +*3 /**- JD **-/+ xoast: S and O isotopes in PM / Atmos Environ Calhoun JA Bates TS and Charlson R J +33+ : * Sulfur isotope measurements of submicrometer Pruett LE Kreutz K J Wadleigh M Mayewski P sulfate aerosol particles over the Pacific Ocean A and Kubatov A **: Sulfur isotopic measure- Geophys Res Lett * ments from a West Antarctic ice core: implica- Davison B Hewitt CN O Dowd CD Lowe JA tions for sulfate source and transport Annal Gla- Smith MH Schwikowski M Baltensperger U and Harrison RM +330 : Dimethyl sulfide methciol Rees CE Jenkins W J and Monster J +312: The ane sulfonic acid and physicochemical aerosol pro- sulphur isotopic composition of ocean water sulperties in Atlantic air from the United Kingdom to phate Geochim Cosmochim Acta Halley Bay J Geophys Res +*+ 2// 201 Romero AB and Thiemens MH **-: Mass- Eriksson E +30-: The yearly circulation of sulfur in independent sulfur isotopic compositions in prenature J Geophys Res 02 **+ **2 sent-day sulfate aerosols J Geophys Res +*2 D Ayers GP +333 : +0 / doi: +* +*3 /**- JD **-00* -/ + Sanusi AA Norman AL Burridge C Wadleigh

7 1- / * M and Tang WW **0: Determination of the S Yanagisawa F and Sakai H +32-: Thermal decomisotope composition of Methanesulfonic acis Anal Chem position of barium sulfate vanadium pentaoxide silica glass mixture for preparation of sulfur +333: dioxide in sulfur isotope ratio measurement Ana- + 2 lytical Chemistry // 32/ 321 Wilson TRS +31/ : Salinity and the major elements +32-: of sea water Chemical oceanography Vol + Riley and Skirrow eds London Academic Press -0/ / Sulfur isotopic composition of snow cover collected at Syowa station Antarctica Naofumi A * Fumitaka Y Toshitaka S + KATA ANAGISAWA UZUKI Naoyoshi I Hidenao H and Akira U - WATA ASEGAWA EDA + Graduate School of Science and Engineering Yamagata University + + Kojirakawa Yamagata Yamagata 33* 2/0* Faculty of Science Yamagata University + + Kojirakawa Yamagata Yamagata 33* 2/0* - Institute for Environmental Sciences + 1 Ienomae Obuchi Rokkasho Aomori *-3-+ Faculty of Science University of Toyama -+3* Gofuku Toyama Toyama 3-* 2/// * Present a$ liation: Institute for Environmental Sciences + 1 Ienomae Obuchi Rokkasho Aomori *-3-+ *++ +- *++ / ++ *++ 1 *++ 1 /