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2 :=]-+*P-7($0/(5-$7"%-#-027( :=]-+*P-7( A/-0*N&(7."%+-(%-?1.07(.N(0-<(8$%*+,-7(10( 23-(%-#.2-(#$%10-($2#.783-%-B( L-72(-$%,1-%(.=7-%P$*.07(.N(-,-P$2-/(7#$,,( 0"+,-1( %$*.07(10(23-(N%--( 2% %-(0-$%(+,."/7B( ) #1+$,(8%./"+*.0( 5-$7"%-#-027( G$7-%(.8*+$,(8$%*+,-(+."02-%(UBDM^X("#( 9.0/-07$*.0(0"+,-1(_9R`(+."02-%(UBUD\^ KBU("#( OI(+.0/-07$*.0(0"+,-"7(_O9R`(+."02-%( UBUUK(^(KBU("#( 4$/1$,(>56(UBUD(^(UBJ\("#( 6#=1-02($-%.7.,(<10?(8%.=-7( UBJ(^(MX("#( UBK(^(JU("#( UBD(^(KBU("#( DU(^(JVU("#( A02-?%$*0?(0-83-,.#-2-%(_7"%N$+-($%-$`( 9"72.#(#$77(78-+(_Q J!:M _?``( J(
3 !"#$%&#' ()*+%$#,)*#' R"+,-$*.0(,10C-/(2.(+,."/(.";,.<( 510"2-7(2.(3."%7(N.%(?%.<23(2.( /-2-+2$=,-(71a-7(b(K(0#( cq J!:Md(-03$0+-#-02(.=7-%P-/( <123(-03$0+-/(8$%*+,-(8%./"+*.0( Q1?3-72(8$%*+,-(8%./"+*.0( $77.+1$2-/(<123(,.<(7"%N$+-($%-$( %$*.0( A02-%#-/1$2-(Q J :(#1e10?(%$*.( $77.+1$2-/(<123(31?3(8$%*+,-( 8%./"+*.0B((>%&(31?3($1%(#1e10?( <123(+.0P-+2-/(7"%N$+-($1%( K(
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7 !"#$%&# The dependence has exponents of order 1-2.
8 !"#$%&# C 1 is in the order of 1e-6 1e-7 [s -1 ]
9 A#8$+2(.N(0-<(8$%*+,-(N.%#$*.0(.0(23-( %$*.0(.N($-%.7.,7($0/(+,."/( +.0/-07$*.0(0"+,-1($%."0/(S-1]10? QB(5$27"1(-2($,B
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11 4-7",27'(P$,1/$*.0(
12 4-7",27'(A#8$+2(.N(R)I(.0(9R($0/(99R(
13 On the photochemical production of new particles in the coastal boundary layer O'Dowd, C., G. McFiggans, D. J. Creasey, L. Pirjola, C. Hoell, M. H. Smith, B. J. Allan, J. M. C. Plan e, D. E. Heard, J. D. Lee, M. J. Pilling, and M. Kulmala GEOPHYSICAL RESEARCH LETTERS, VOL. 26, NO. 12, PAGES , JUNE 15, 1999
14 Background Source regions for natural aerosol formation: free troposphere, boreal forests, background continental sites, coastal zones. Measurement: Mace Head, located on the west coast of Ireland, in May, 1997 Objective: Concurrent measurements of ultra-fine (r<5 nm) particle (UFP) formation, OH and SO 2 concentrations are examined to elucidate the processes leading to tidalrelated homogeneous heteromolecular nucleation
15 Results UFP concentrations approaching 300,000cm -3 are regularly encountered due to tidal-related events. nucleation UFP events correspond to peak OH concentration, suggesting a photochemical source for aerosol precursors. Total particle & OH concentration the Derived H 2 SO 4 production exhibited coherence with UFP concentration: H 2 SO 4 is likely to be involved in. Comparison of UFP concentrations and production rates of H 2 SO 4 molecules
16 Nucleation can be explained by ternary nucleation of H 2 SO 4, NH 3 and H 2 O. Growth to detectable sizes can only be explained by condensation of an additional species X. According to a condensation growth and aerosol dynamics model, the aerosol production and growth can be explained by using an instantaneous nucleation rate of 10 7 cm -3 s -l and a concentration of 5x10 7 cm -3 for condensable vapor. Modeled aerosol total concentration
17 9$0(+.7#1+(%$&7($f-+2(+,."/( +.0/-07$*.0(0"+,-1(=&($,2-%10?(0-<( 8$%*+,-(N.%#$*.0g( FB4B()1-%+-($0/()BFB(6/$#7(_JUUW`(
18 A02%.[S$+C?%."0/( ha.0y$-%.7.,(+,-$%y$1%(3& i( 9.7#1+(%$&7(!(1.0(N.%#$*.0(!99R(_+,1#$2-( -f-+27`( DDY&-$%(7.,$%(+&+,-(!.,$%(#10'(Q1?3-%(+.7#1+(%$&(j"e(2.(2% %-( Q& (.N(8$8-%'( 9.",/(/-+%-$7-7(10(+.7#1+(%$&(j"e(.P-%(23-(,$72( +-02"%&(8$%2,&(-e8,$10(<$%#10?g(
19 5-23./7( 5./-,-/(?,.=$,($00"$,($P-%$?-(-f-+27(.N( +.7#1+(%$&7(.0'( R"+,-$*.0(%$2-7( 99R($2(UBJk(7"8-%7$2"%$*.0(_99R UBJk`(!.,$%(#101#"#(_DWZV`($0/(#$e1#"#(_DWWU`( L<.(71#",$*.0(2&8-7'( 5:>TAG(c#.%-(%-$,17*+(0"+,-$*.0(71#",$*.0d( A:RGA5AL(c$77"#-(-P-%&(1.0(8%./"+-/(<1,,( 0"+,-$2-($(8$%*+,-(8%.P1/-/(-0."?3(Q J!: M d(
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21 4-7",27[>17+"771.0( 99R( *P-(2.(+3$0?-7(10(0"+,-$*.0(%$2-( 62(N$72-%(0"+,-$*.0(%$2-7E(#.%-(0#Y71a-/(8$%*+,-7( $%-(+.#8-*0?(N.%(+.0/-07$=,-(?$7-7( 99R(/"-(8%1#$%1,&(2.($023%.8.?-01+(-# ( 9$,+",$2-/(+3$0?-7(10(7.,$%(%-j-+2$0+-(<-%-( 2<.(.%/-%7(.N(#$?012"/-(2..(7#$,,(2.(-e8,$10( +3$0?-7(10(+,."/(+.P-%(.%(JU 23 (+-02"%&(+,1#$2-( +3$0?-(
22 Organic condensation: a vital link connecting aerosol formation to CCN concentrations How do organics affect size distribution of ultrafine particles? Increase CCN: condensation on ultrafine particles Decrease CCN: condensation on larger particles scavenging of ultrafine particles, reducing CCN Problem: fraction of VOC thermodynamic properties well known (esp. volatility) I. Riipinen1,2, J. R. Pierce3, T. Yli- Juuti2, T. Nieminen2, S. H akkinen2, M. Ehn2, H. Junninen2, K. Lehtipalo2, T. Pet aj a2, J. Slowik4,*, R. Chang4, N. C. Shantz5, J. Abbatt4, W. R. Leaitch5, V.- M. Kerminen2,6, D. R. Worsnop2,7, S. N. Pandis1,8, N. M. Donahue1, and M. Kulmala2 1Center for Atmospheric Particle Studies (CAPS), Carnegie Mellon University, 15213, Pittsburgh, PA, USA 2Department of Physics, University of Helsinki, 00014, Helsinki, Finland 3Department of Physics and Atmospheric Science, Dalhousie University, B3H 3J5, Halifax, NS, Canada 4Department of Chemistry, University of Toronto, M5S 3H6, Toronto, ON, Canada 5Science and Technology Branch, Environment Canada, M3H 5T4, Toronto, ON, Canada 6Finnish Meteorological Institute, 00880, Helsinki, Finland 7Aerodyne Research Inc., 01821, Billerica, MA, USA 8Institute of Chemical Engineering and High Temperature Processes (ICE- HT) Foundation for Research & Technology, Hellas (FORTH), 26504, Patra, Greece *now at: Paul Scherrer Institute, 5232 Villigen PSI, Switzerland Received: 10 December 2010 Published in Atmos. Chem. Phys. Discuss.: 6 January 2011 Revised: 12 April 2011 Accepted: 13 April 2011 Published: 27 April 2011
23 Look at expected growth rate from [H 2 SO 4 ], compare with observed growth rates explains less than 10% of observed GR and mass flux Contribution from low-volatility organics could explain GR
24 Thermodynamic equilibrium approaches insufficient for modeling organic contribution to particle number Neglecting organic condensation leads to under prediction of [CCN]
25 N,M1'O.&$-.%'B"-)#)%'A).6,*M')0"-' L)-".%'P)-"#&#' D<'Q$*0"6>'N<(<'N.*##)*>'R<;<'="-9,*"*>';<'S.%';.#>'N<'A,1.0.,*"*>'T<'R,,#.*"*>' D<'D<'B.%&)>';<'=)944$%.>';<'=$%9.%.' U+,"*+"<'R)%$9"':VJ<'B4-,%'VW>'JKKE' U$**,'X0"2'.*6';.-M.-"&'O6"Y' Z+&)7"-':V>'JKVV'?BU'EFI['
26 S.%-$,(N.%-727(/.(0.2(3$P-( 8%1#$%&(7."%+-7(23$2(-#12( l0-(8$%*+,-7(!",n"%1+($+1/(23."?32(2.(=-( % =,-(N.%(0-<(8$%*+,-( N.%#$*.0E(="2(0.2(-0."?3( 7",N"%1+($+1/(10(23-( $2#.783-%-(2.(-e8,$10(.=7-%P-/(?%.<23(%$2-7( Q.#.?-0."7(0"+,-$*.0(10( 23-7-(%-?1.07(8%-P1."7,&( 72"/1-/(=&'( )$,,$7($0/(H$%%1.(10(I10173( G$8,$0/( 678P%-2-0(10(!<-/-0( S$+C?%."0/(
27 5-23./.,.?&($0/(4-7",27( 5-23./.,.?&( L%$]-+2.%1-7(<-%-("7-/( 2.(+$,+",$2-(*#-(.N( 2%$078.%2(.P-%(,$0/( $0/(#-$7"%-/(0"#=-%( 71a-(/172%1="*.0( L-%8-0-(-# ( <-%-(-7*#$2-/(.P-%( 78$+-($0/(*#-( 4-7",27( R$2"%$,,&(-#1m-/( 2-%8-0-7(.P-%(N.%-727( +.02%1="2-(2.(R)IB(( Q J!: M E(Q J :E($0/(RQ K ( $,7.(+.02%1="2-(2.(R)IB((
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29 *"$&-.%'+%$#&"-'*$+%"./)*'\O(O]'',)*^9"6,.&"6'*$+%"./)*'\X;O]
30 I%.#(/1%-+2(#-$7"%-#-02(8-.8,-(8.102-/(."2(23$2(0-"2%$,( +,"72-%( 0"+,-$*.0( /.#10$2-7( <31,-( 1.0Y#-/1$2-/( 0"+,-$*.07( $++."02( N.%( ( DUk(.%(,-77( N.%( 8$%*+,-7( %$0?10?( N%.#(JYK0#( H1-<8.102(.N( 2317( 8$8-%'( 1.0Y#-/1$2-/( 0"+,-$*.0( 17( $( /.#10$02(N.%#$*.0(#./-(N.%(8$%*+,-7($2(71a-($=."2(J(0#B(((!"+)97,*./)*_' *"M./0"' +1.-M"6' 4.-/+%"`' 4)#,/0"' +1.-M"6'4.-/+%"#'!'*"$&-.%'+%$#&"- )0"-"#/9.&"6 $*6"-"#/9.&"6
31 n10-*+(71#",$*.0($0/(+.#8$%17.0(<123(#-$7"%-#-02 :=7-%P-/(/$2$ A5R(5./-,
32 L3-(+.02%1="*.07(.N(78-+1l+( 8% (
33 60$,&*+$,(102-%8%-2$*.0(
34 ;".#$-"9"*&#')5'O"8'D.-/+%"' P)-9./)*'.*6'a%&-.b*"'D.-/+%"' c-)8&1'!.&"#'.&'.'(%".*' ()*/*"*&.%'U,&"( 4BFB(o-=-%E(-2($,B(DWWX(
35 A02%./"+*.0( )%-P1."7(72"/&($2(%-#.2-(#$%10-( 712-( >.(7$#-(8% (.++"%($2( %-#.2-(+.0*0-02$,(712-g(4./0-&( <$7(/-2-%#10-/(2.(l0/(."2B(!$#8,10?(712-(<$7($(#."02$10(10( 9.,.%$/.(!$#8,-/(%-,$*P-,&(+,-$0E(/%&($1%( N%.#(N%--(2% %-( 5-$7"%-/(?$7(83$7-(Q J!: M E(Q J :E( $0/(.23-%( (
36 4-7",27( I-<-%(",2%$l0-(8$%*+,-7(<3-0( $-%.7.,(7"%N$+-($%-$( %$*.07(<-%-(31?3( R.(-P1/-0+-(23$2(31?3-%(4Q( 10+%-$7-/(",2%$l0-(8$%*+,-( N.%#$*.0( Q J!: M (,-P-,7($0/(",2%$l0-( 8$%*+,-( %$*.07(<-%-( 72%.0?,&(+.%%-,$2-/( R-<(8$%*+,-(N.%#$*.0(.++"%%-/($2(#"+3(,.<-%(,-P-,7(.N(Q J U($0/(Q J!: M (23$0( -e8-+2-/( :=7-%P-/(?%.<23(%$2-7(<-%-( \YDU(*#-7(31?3-%(23$0( +$,+",$2-/(?%.<23(%$2-7(
37 9.0+,"71.07( Q J!: M (17($(8%-+"%7.%(.N(0-<(8$%*+,-(N.%#$*.0( Q J!: M (,-P-,7($0/($#=1-02($-%.7.,(7"%N$+-($%-$( %$*.07(<-%-(#.72(1#8.%2$02(N$+2.%7($f-+*0?( R)I(!8-+1-7(.23-%(23$0(Q J!: M (+.02%1="2-/(2.(",2%$l0-( 8$%*+,-(?%.<23(="2(0.2(0-+-77$%1,&(2.(R)I(
38 !"#$"%&'()*+%$,'#-"*(./0"$*#1(#"(,$%,'1(&** '(*%*2%$/'()*%,/1&+3"$"*%(4*'/+-'#%,'1(&*
39 !"#$%&'()*+,-./0)1+"1-'2340&/# &"1(&02+")*+2(56(&/#+ "#/*+7"3'&+#')#0)1&"1/')2++ 8)*/&0#19+:;,<+4=3'1402/2+ &0-"/)2+"-./%('(2+ >/&0#19+?(")1/6=/)% "%)/1(*0+'6+"+3'2/1/70+ #5/-"10+2= *."#$+ /)7'57/)%+140+/)65(0)#0+' &"1(&0+')+3"1/#50+ )(#50"1/')+&"102+
40 !"#$%&' ()*%+,%+-#"&'-)'-&.-)*"&',-#/*0"' 1/*+%,$23/*3'456!7'1%&"0'/)#%'89:;<=$"1' >%' -' %)"<2"-+' 89:;<=$"1'.A<BC<BD' E' 56!F' G/#$' )?*0"-#/%)'+-#"3',+"&/*#"&'H2'#$"'(!I'1"*$-)/31'-)&'#$"'*%)&")3-#/%)' %J' 0%G'.%0-#/0"' J+%1' 3?**"33/."' %K/&-#/%)' #-L")'/)#%'-**%?)#M' N%' "3#/1-#"' #"1,"+-#?+"' 3")3/#/./#2F' #G%' +?)3' G"+"' /)#"+<*%1,-+"&O' H-3"0/)"' #"1,"+-#?+"3F' -)&' -' 3"*%)&' G/#$' -00' #"1,"+-#?+"3' -+%?)&'#$"'H-3"0/)"'*0/1-#"'3#-#"M'
41 !"#$%&'("#) *+,-+./0&.+)(#$.+/'+'1)#&$%+/0("#)./0+)(').+2&$0+21) /')3+%%)/')!4)$"#$+#0./0("#'5)
42 !"#$%&'("#) *+,-+./0&.+)(#$.+/'+'1)!!2) $"#$+#0./0("#')/.+).+3&$0+3)
Growth of atmospheric clusters involving cluster cluster collisions: comparison of different growth rate methods
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