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Fogwill, M. Dall'Os o and Z. A. Kanji, Fa aday Discuss., 2024, DOI: 10.1039/D4FD00160E.
Te es ial and Ma ine Sou ces o Ice Nuclea ing Pa icles in he
Eu asian A c ic
Guangyu Li1*, And é Wel i2, A ianna Rocchi3, Ge mán Pé ez Fogwill2, Manuel Dall’Os o3, and Zamin
A. Kanji1
1Ins i u e o A mosphe ic and Clima e Science, ETH Zu ich, Swi ze land
2Finnish Me eo ological Ins i u e, Helsinki, Finland
3Depa men o Ma ine Biology and Oceanog aphy, Ins i u e o Ma ine Sciences (ICM, CSIC), Ba celona, Spain
*Now a : Depa men o Ca bon Emissions and En i onmen al E olu ion, Deqing Academy o Sa elli e Applica ions, Deqing,
China
Co espondence: Guangyu Li ([email p o ec ed]) and Zamin A. Kanji (zamin.kanji@en .e hz.ch)
Abs ac .
Ice nuclea ing pa icles (INPs) ca alyze p ima y ice o ma ion in A c ic low-le el mixed-phase clouds, in luencing hei pe -
sis ence and adia i e p ope ies. Knowledge o he abundance and sou ces o INP o e he emo e A c ic Ocean is sca ce due
o limi ed da a co e age, pa icula ly in he Eu asian A c ic. This s udy p esen s summe ime measu emen s o INP concen a-
ions in seawa e , og wa e and ai om he ship-based A c ic Cen u y Expedi ion, explo ing he Ba en s, Ka a, and Lap e 5
Seas, and he adjacen high A c ic islands and a chipelagos in Augus and Sep embe 2021. Hea sensi i i y es s o ambien
ae osols e ealed ha hea -liable, biogenic INPs make up he majo i y o A c ic INP popula ions a empe a u es abo e -20
°C, and o a lesse ex en down o -25°C. INP con en in og wa e is ound o be simila o ambien ae osol, indica ing ha
INP in ma ine ai could also ac as cloud condensa ion nuclei. Measu emen s o ae osolized INPs using an on-boa d sea-sp ay
ae osol bubble ank gene a o exhibi a posi i e co ela ion wi h ambien INP concen a ions, bu no wi h INP abundance in10
seawa e samples. INP concen a ions in ai de i ed om sea wa e samples (using a NaCl con e sion ac o ep esen a i e
o he A c ic) we e signi ican ly lowe han hose measu ed in ambien ai o bubble ank expe imen s. INP concen a ions
in bubble ank expe imen s posi i ely co ela ed wi h he phospha e and luo escence signals in he wa e . This sugges s an
impo an ole o he ae osoliza ion mechanism o p e e en ially pa i ioning biogenic INPs o he a mosphe e.
1 In oduc ion15
Ice nuclea ing pa icles (INPs) igge p ima y ice o ma ion in mixed-phase clouds (MPCs), which modula es he cloud a-
dia i e and mic ophysical p ope ies (Ko ole e al., 2017; Se eze and Ba y, 2011). Accu a e simula ions o cloud p ope ies
in clima e models equi e a ealis ic ep esen a ion o INPs (Mu ay e al., 2021). The concen a ion o INPs in luences he
numbe , size, and phase pa i ioning o hyd ome eo s in clouds, which in u n a ec he cloud albedo, li e ime, and migh im-
pac p ecipi a ion pa e ns. In he A c ic, cloud co e impac s he egional ene gy balance while he amoun o snow-p oducing20
clouds a ec s he o ma ion o sea ice. A sca ci y o INP obse a ions limi s ou unde s anding o he abundance and sou ces
1
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o INPs in di e en en i onmen s. The Eu asian A c ic Ocean is o pa icula in e es because i could be he sou ce o highly
ac i e INPs (Po e e al., 2022).
INPs can o igina e om e es ial and ma ine sou ces. Mine al dus pa icles a e a signi ican e es ial sou ce, capable o
ini ia ing ice nuclea ion (IN) a empe a u es lowe han app oxima ely -15 °C (Hoose and Möhle , 2012). Known sou ces o 25
mine al dus nea he A c ic Ocean include he A c ic coas s o G eenland (Li e al., 2023), he Russia coas (Po e e al., 2022),
glacial ou wash plains in S alba d (Tobo e al., 2019), and sandy dese s on Iceland (Sanchez-Ma oquin e al., 2020). Ma ine
INP sou ces in he A c ic Ocean a e ela ed o sea-sp ay ae osol (SSA), gene a ed h ough wa e b eaking and bubble bu s ing,
which ep esen s ano he c ucial sou ce o INPs in he high-la i ude A c ic Ocean (Leck and Bigg, 2005; Wilson e al., 2015;
C eamean e al., 2018; P a he e al., 2008). The p oduc ion a e o SSA a ies wi h me eo ological condi ions (e.g., wind speed,30
and sea su ace empe a u e Quinn e al., 2015; G y he e al., 2014) and sea ice co e age (Quinn e al., 2015). Also bo h he
abundance o di e en componen s in seawa e and he ae osoliza ion p ocess a he ocean-a mosphe e in e ace impac ae osol
emission and pa i ioning (O’Dowd e al., 2015; P a he e al., 2008). In addi ion o ino ganic sea sal and sul a e, SSA con ains
ma ine biogenic ae osol, which can be composed o pa icula e mic obes, phy oplank on cell exuda es (C eamean e al., 2019;
Knop e al., 2011), and dissol ed o ganic mac omolecules (McCluskey e al., 2018b) eleased du ing phy oplank on blooms.35
These componen s can be IN-ac i e a empe a u es as high as -5 °C (Mu ay e al., 2012). I is hypo hesized ha he emission
o IN-ac i e ma ine biogenic ae osol could coincide wi h ma ine phy oplank on blooms and co-emission o biogenic ae osol
p ecu so s, such as Dime hylsul ide (DMS) and chlo ophyll-a(Gab ic e al., 2018; Rinaldi e al., 2013; Becagli e al., 2011).
As he A c ic wa ms and sea ice e ea s, ma ine biological p ocesses a e likely o become mo e ac i e which could change
he ma ine INP emission. Unco e ing he sou ces and unde s anding he mechanisms o ma ine biogenic ae osol elease in o40
he a mosphe e is he e o e needed o p edic ing he abundance o A c ic low-le el MPCs in he u u e (Ickes e al., 2020; Si
e al., 2019).
In his wo k, we p esen ship-bo ne measu emen s o INP concen a ions (NINP) sampled om di e en en i onmen s (sea-
wa e , og wa e , ma ine ai , and ai om a bubble ank gene a o ) and ela ed ae osol p ope ies du ing he A c ic Cen u y
Expedi ion in he summe o 2021 o e he Ba en s, Ka a and Lap e Seas and he adjacen high A c ic islands and a chipelagos45
in he Eu asian A c ic, a egion ha has no been s udied be o e.
2 Me hods
2.1 Campaign o e iew
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Figu e 1. Posi ion o ins umen a ion on boa d o he RV Akademik T yoshniko (adap ed om essel plans by he A c ic and An a c ic
Resea ch Ins i u e). Heigh is p o ided ela i e o he app oxima e wa e line in he on iew (le panel), and dis ance om he ship’s
bow in he op iew ( igh panel). A SSA bubble ank gene a o was ope a ed on he 1s deck, online measu emen equipmen o ae osol
cha ac e iza ion was loca ed on he 2nd deck, and ae osol sample collec o and og wa e sample we e ins alled on he 6 h deck.
The A c ic Cen u y Expedi ion ook place om 5 h Augus o 6 h Sep embe 2021, s a ing and ending a he po o
Mu mansk, Russia. Figu e 1 shows he loca ion o expe imen s, ins umen s and sample s on boa d he esea ch essel (RV)50
Akademik T yoshniko epo ed in his wo k. De ailed in o ma ion on ins umen con igu a ions and hei unc ions in each
sec o is gi en in Table 1. Fo measu emen s on he 1s deck, an ae osol gene a ion bubble ank (BT) sys em o con olled
SSA gene a ion was se up. Inside he BT, ae osol is gene a ed by simula ing he bubble-bu s ing mechanisms using wa e
je s o c ea e bubbles. Wa e samples include 32 L seawa e collec ed a 2 m dep h wi h Niskin bo les using a Conduc i -
i y–Tempe a u e–Dep h (CTD) ose e sampling sys em o eshwa e samples collec ed on land using sampling bucke s (see55
sampled wa e loca ions in Fig. 2). The SSA gene a ed in he BT was collec ed on il e s o NINP measu emen s, and cha ac-
e ized o he size dis ibu ion by a scanning mobili y pa icle size (SMPS) and an op ical pa icle coun e (OPC). F esh and
seawa e samples used o BT expe imen s we e also il e ed o biochemical analysis (see Rocchi e al., 2024 o de ails on BT
expe imen s and analysis o biological a iables). On he 2nd deck, an ae osol con aine con igu ed as a labo a o y included
in e al sampling o ambien ae osol by a liquid impinge ( o INP analysis), and con inuous cha ac e iza ion o pa icle size60
dis ibu ions wi h an SMPS and an ae odynamic pa icle size (APS). On he 6 h deck, se e al og wa e collec o s we e in-
s alled nex o a low olume PM10 il e sample (LVS) (Table 1). The LVS sampled ambien ae osol con inuously o 12 h pe
il e along he ship ack du ing he campaign. The og wa e and il e s we e analyzed o INPs in he labo a o y a e he
3
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Table 1. O e iew o ins umen a ion se -up on he esea ch essel RV Akademik T yoshniko du ing he A c ic Cen u y Expedi ion ( o he
onboa d loca ion, see Fig. 1)
On-boa d loca ion Ins umen Tempo al esolu ion Flow a e Func ion
1s deck
CTD- ose e S a ion-based - Seawa e sampling
Ae osol gene a o (BT) S a ion-based - Ae osol gene a ion om sampled wa e
SMPS (BT-ae osol) 4 min 0.6 L min-1 Online pa icle size dis ibu ion (< 0.6 µm)
OPC (BT-ae osol) 5 s 2.83 L min-1 Online pa icle size dis ibu ion (> 0.3 µm)
Wa e il e S a ion-based - Wa e il a ion o biochemical analysis
BT ae osol il e 6-20 h 10 L min-1 Ae osol collec ion on il e s o o line INP analysis
2nd deck
Impinge 3 h 300 L min-1 Ae osol collec ion in wa e o o line INP analysis
SMPS 4 min 0.6 L min-1 Ambien pa icle size dis ibu ion (0.012 - 0.6 µm)
APS 4 min 1 L min-1 Ambien pa icle size dis ibu ion (0.5 - 20 µm)
6 h deck Fog wa e collec o 6-12 h - Fog wa e collec ion o o line INP analysis
LVS (PM10 inle ) 12 h 38.3 L min-1 Ae osol collec ion on il e s o o line INP analysis
campaign. Addi ionally, se e al nea -sho e su ace mic olaye (SML) and unde lying subsu ace seawa e (SSW) samples we e
collec ed. The loca ions o og wa e , sea- and eshwa e , SML and SSW samples a e ma ked in Fig. 2. De ailed expe imen al65
se ups o sample collec ions and measu emen s a e desc ibed in he ollowing sec ion.
2.2 Sample collec ion
2.2.1 Ambien ae osol samples
F om he ae osol con aine labo a o y on he 2nd deck, ambien ae osols we e collec ed (3 imes a day o 3 hou s) each in o
15 mL ul a-pu e wa e (W4502-1L, Sigma-Ald ich) using a high low- a e impinge (Co iolis®µ, Be in Ins umen s, wi h a70
lowe limi ae odynamic cu -o size o 0.5 µm) a a low a e o 300 L min-1. On he 6 h deck, ae osol pa icles we e collec ed
on o 47 mm polyca bona e memb ane il e s (Wha man, 0.4 µm po e size) using he LVS (Model DPA14, Digi el) wi h a PM10
inle . In he ollowing, hese il e samples a e e e ed o as LVS il e s. The LVS inle was app oxima ely 25 m abo e sea le el.
The ope a ing low a e was main ained a 38.3 L min-1 o 12-hou sampling in e als. The sampling was empo a ily hal ed
when he wind di ec ion was de ec ed o o igina e om he ship’s chimney, in o de o p e en con amina ion om exhaus 75
emissions. The impinge and LVS il e samples we e s o ed a -20 °C on boa d and o anspo un il hey we e used o he
INP analysis a e he campaign back a he labo a o y a ETH Zu ich. Du ing he campaign, a o al o 75 impinge and 50 LVS
il e samples we e collec ed.
4
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Figu e 2. Map o wa e sampling loca ions du ing he A c ic Cen u y Expedi ion. The g ay as e isks ep esen he ship’s ack (1 h in e al)
h oughou he expedi ion.
2.2.2 Ae osol samples collec ed om BT
The BT ae osol gene a ion sys em (Medina-Pé ez e al., 2020) was used o cha ac e ize ae osols p oduced om bubble bu s ing.80
The BT consis s o a 60 L s ainless-s eel cylind ical ank. Fo ope a ion, he BT was illed wi h 30 L o wa e collec ed ei he
wi h he CTD- ose e (sea wa e ) o on islands (island un-o o eshwa e ). Wa e in he BT was ci cula ed o he op ia
a pe is al ic pump and showe ed back o he wa e su ace as plunging je s a a low a e o 12 L min-1. The sp ay ae osol
o ms a he wa e su ace ia bubble bu s ing (O’Dowd e al., 2015). Pa icle- ee ai was supplied in o he ank headspace
a 60 L min-1 o p e en ae osol om concen a ing (see Rocchi e al., 2024 o de ailed expe imen al se up). Two equen ly85
egene a ed di usion d ye s we e used o d y he wa e sp ay ae osol o pa icle size dis ibu ion measu emen s and il e
collec ion. 47 mm polyca bona e memb ane il e s (Wha man, 0.4 µm po e size) we e used o collec ae osols gene a ed om
he BT. The sample low a e was app oxima ely 10 L min-1 o a du a ion o 6 o 20 hou s. BT il e s we e s o ed ozen
a -20 °C un il INP analysis was conduc ed back in he labo a o y a ETH Zu ich. The INP concen a ion measu ed om
5
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ambien ae osols and ae osoliza ion om BT we e no co ec ed o eezing poin dep ession, ollowing he ep esen a ion o 90
a mosphe ic imme sion eezing occu ing in dilu e cloud d ople s wi h wa e ac i i y ∼1.
2.2.3 En i onmen al wa e samples
A o al o 21 og wa e samples we e collec ed using he ins umen s shown in Fig. 3 (a). An a ay o 7 cac us-like collec o s
we e ixed by he whi e clamps and moun ed on he ailing a he 6 h deck on boa d. Once co e ed in og, he og wa e / os
deposi s on o he sha p ips o he "cac us" and d ips down/mel s in o a glass bo le a ached a he bo om.95
Figu e 3. (a) Fog wa e sample collec o ; (b) Collec ion o SML.
To compa e any en ichmen o INPs be ween he sea su ace mic olaye (SML, a sub-millime e laye loca ed a he in e ace
be ween he ocean and a mosphe e) and subsu ace wa e (SSW), seawa e was sampled a he coas al egions (see Fig. 2)
accessed by a helicop e . Fou SML samples we e collec ed ollowing he p ocedu e shown in 3 (b). A clean glass pla e is
epea edly e ically subme ged and wi hd awn om he sea su ace o collec SML samples ( an Pinx e en e al., 2017). The
hin mic olaye ilm a ached o he pla e is hen ans e ed in o sample bo les using a Te lon sc ape o wipe down he glass100
pla e. Fou SSW bulk seawa e samples we e sampled by di ec ly subme ging sample bo les o abou 50 cm below he ocean
su ace in pa allel o he SML sampling.
Fo BT expe imen s, 30 L (o he sampled 32 L) o ei he sea o eshwa e was used o ae osol gene a ion. The 13 seawa e
samples we e collec ed om a dep h o 2∼4 m using he uppe mos Niskin bo le om a SEA-BIRD CTD ose e sampling
sys em. The 3 eshwa e samples we e collec ed using a plas ic bucke om an island i e , island lake, and island uno (a 105
6
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he sho e o Pionee Island, Oc obe Re olu ion Island, and a Lake on Cape Ba ano , espec i ely, see Fig. 2). 2 L o each
wa e sample was il e ed o analyze biogeochemical a iables (Rocchi e al., 2024). All samples ( og wa e , SML and SSW,
wa e il e s, wa e il a es, and un il e ed wa e ) we e s o ed ozen a -20 °C un il analyses.
Conduc i i y was measu ed p io o analyzing he INP concen a ions o seawa e samples o accoun o he eezing poin
dep ession om dissol ed sea sal . The co ec ed eezing empe a u e we e calcula ed acco ding o Koop and Zob is (2009),110
and ollowing he p ocedu e o Wilson e al. (2015).
2.3 INP analysis wi h DRople Ice Nuclei Coun e Zu ich (DRINCZ)
Aqueous pa icle suspensions we e used o imme sion-mode INP analysis using DRINCZ (Da id e al., 2019). A e ozen
s o age, impinge samples we e allowed o mel a 4 °C o e nigh be o e analysis. Memb ane il e samples we e imme sed in
10 o 15 mL ul a-pu e wa e and agi a ed using a sonica o o 30 min o esuspend he pa icles om il e s in o he wa e . Each115
liquid sample was pipe ed in o a Polyme ase Chain Reac ion (PCR) ay wi h 96 aliquo s o 50 µL and cooled in an e hanol
ba h a 1 °C min-1. F eezing e en s we e de ec ed op ically om he change in anspa ency o an aliquo upon eezing. INP
concen a ion (NINP) was de i ed om he ozen ac ion o aliquo s a each in ege empe a u e ollowing Vali (1971). Fo
ae osol samples collec ed by impinge and LVS il e s, NINP is calcula ed as pe olume o sampled ai :
NINP, ai (T) = −
ln1−N z(T)
N o
Valiquo
·Vwa e
V low (1)120
Whe e NINP(T) is he INP concen a ion a empe a u e T,N z(T) is he numbe o ozen aliquo s a empe a u e T,N o
is he o al numbe o aliquo s (N o = 96), Valiquo is he aliquo olume (Valiquo = 50 µL). Vwa e is he o al wa e olume o
he impinge sample o he olume o wa e used o suspend LVS il e s, and V low is he sampled ai olume, which is he
p oduc o he sampling low a e and sampling ime. Fo he og, esh and seawa e samples, NINP is quan i ied as pe olume
o sampled wa e :125
NINP, wa e (T) = −
ln1−N z(T)
N o
Valiquo (2)
The NINP in og wa e was con e ed o NINP in ai :
NINP, ai (T) = NINP, og wa e (T)·F og, ai (3)
Whe e F og, ai is he liquid wa e con en (LWC) o og wa e in g m-3 con e ed o a olume o wa e in he ai . Fo
simpli ica ion, F og, ai was aken om og laye measu emen s o Cos abloz e al. (2024) who epo ed a LWC o 0.1 g m-3ai
130
o og up o 50 m abo e g ound (Cos abloz e al., 2024). The con e sion ac o om pe olume o liquid o pe olume o ai
is F og, ai = 1 ×10-7 L og wa e L-1ai .
7
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Field blanks unde going he same p ocedu es as he samples we e collec ed e e y h ee days du ing he campaign. The
NINP we e co ec ed o he backg ound o he blanks acco ding o Vali (2019), by sub ac ing he di e en ial INP spec um
o he blanks om he samples. Based on he limi o de ec ion (LOD) om he collec ed sample olume and he pu i y o 135
he nano-pu e wa e , he highes empe a u e o NINP de ec ion was app oxima ely -5 °C (abo e which sampled ai olumes
a e deemed oo low o de ec any INPs), and he lowes empe a u e a which NINP can be eliably epo ed is -25 °C (below
which nano-pu e wa e ini ia es eezing). The o e all unce ain y o he epo ed eezing empe a u es is ±0.9 °C (Da id
e al., 2019).
2.4 Hea ea men o INP samples140
Mac omolecules o igina ing om biological species (e.g., bac e ia and phy oplank on), ypically comp ised o p o eins can
e ec i ely ca alyze ice nuclea ion (Hill e al., 2016) and a e hea labile. Hea ing e ec i ely un olds he p o einaceous s uc u e,
deg ading hei IN abili y (Hill e al., 2016; Pumme e al., 2015). In he pos -campaign hea ea men , liquid samples ex ac ed
om he 50 LVS il e s we e subjec ed o 95 °C o 20 min. A e cooling o oom empe a u e, he samples we e edis ibu ed
o PCR ays o INP analysis using DRINCZ. By compa ing he IN ac i i y be o e and a e hea ing, i is possible o assess145
he con ibu ion o hea -labile species o he INP popula ion, which is a p oxy o indica e he p esence o biological INPs (Hill
e al., 2016).
2.5 Pa icle size dis ibu ion
In he ae osol con aine labo a o y on he 2nd deck, he size dis ibu ion o submic on ambien ae osol was measu ed using an
SMPS (Model 3938, consis ing o a 3082 classi ie , a 3081 long di e en ial mobili y analyze , and a 3787 Condensa ion Pa icle150
Coun e , TSI Inc.). The SMPS ope a ed a a sampling low a e o 0.6 L min-1 wi h a shea h- o-sample a io o 10:1, co e ing
a size ange o app oxima ely 12 o 600 nm in elec ical mobili y diame e . A cha ge co ec ion was applied o accoun o
he misclassi ica ion o la ge pa icles ca ying mul iple cha ges. Concu en ly, he size dis ibu ion o coa se-mode pa icles
( anging om app oxima ely 0.5 o 20 µm in ae odynamic diame e ) was moni o ed using an APS (Model 3321, TSI Inc.)
a a low a e o 1 L min-1. Bo h he SMPS and APS we e synch onized o a ime esolu ion o 4 minu es o ensu e aligned155
size dis ibu ions. The elec ical mobili y diame e s ob ained om he SMPS and ae odynamic diame e s om he APS we e
con e ed o olume-equi alen diame e s, assuming an a e age pa icle densi y o 2 g cm-3 (Li e al., 2022; Tobo e al., 2019).
To moni o he ae osol size p ope ies gene a ed om he BT expe imen s, pa icle size dis ibu ion measu emen s we e
conduc ed using a combina ion o an SMPS and an OPC (Model GT-526S, Me One). Two di usion d ye s illed wi h silica gel
we e used o d y he pa icles be o e en e ing he SMPS and he OPC. The SMPS was con igu ed he same as in he ae osol160
con aine . The OPC p o ided 6-binned pa icle coun in op ical diame e (i.e., > 0.3 µm, > 0.5 µm, > 1 µm, > 2.5 µm, > 5 µm
and > 10 µm) o ex end he ange o size dis ibu ions.
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Figu e 7. Cumula i e INP spec a o sea su ace mic olaye (SML) and subsu ace seawa e (SSW) samples. E o ba s show he 95 %
con idence in e als. Li e a u e da a (Gong e al., 2020a; I ish e al., 2017; Wilson e al., 2015) o p e ious measu emen s o NINP in seawa e
a di e en loca ions a e shown o compa ison. The eezing empe a u es o seawa e NINP a e co ec ed o eezing poin dep ession.
3.2 Ocean-a mosphe e pa i ioning o INPs275
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Figu e 8. Cumula i e INP spec a o BT-gene a ed pa icles, classi ied acco ding o he sampling loca ion. "Island wa e bodies" indica es
wa e collec ed om island i e s and lakes, "MilliQ" deno es a e e ence expe imen wi h pu e wa e . All o he ca ego ies a e seawa e
samples. "close o island" indica ed ha he ship loca ion was less han 15 km om he coas line.
F om he isola ed expe imen s o di e en wa e samples in he BT, we dis inguish he abundance o INPs gene a ed by sp ay
ae osoliza ion o he wa e samples based on he sampling loca ion. Figu e 8 shows he INP spec a o ae osolized pa icles
om he BT expe imen s (NINP, BT). O e all, eshwa e samples ha we e collec ed om i e s and lakes on islands (labeled as
"Island wa e bodies") and seawa e samples collec ed close- o-islands p oduced highe ae osolized NINP compa ed o seawa e
samples a he away om land (see Fig. 8) suppo ing s ong e es ial INP sou ces. The "island wa e bodies" showing he280
lowes eezing empe a u e (Land_075BIS) was sampled on Pionee Island in he bay in b ackish wa e s as e ealed by he
in e media e salini y le el (see Table ?? in he Appendix). The Land_80 sample was a seawa e sample di ec ly in con ac wi h
land. Gi en he highes INP concen a ions we e obse ed o samples wi h ze o and high salini y (Land_078 and Land_80,
espec i ely), he con ac o land appea s o con ol he INP concen a ions obse ed a he han he salini y le el. The in luence
o salini y is u he discussed la e sec ions. F om he seawa e samples collec ed a di e en loca ions, NINP, BT was highes 285
o samples ob ained close o islands. Fo seawa e samples, educed NINP, BT was associa ed wi h inc eased sea ice co e age,
i.e., NINP, BT p oduced om samples collec ed in he open ocean con ained mo e INPs han samples om wi hin he MIZ/ice
pack.
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In Figu e 9 he NINP, BT, ambien NINP ( om LVS il e s) and NINP in ai de i ed om he SML and SSW samples a e shown.
To con e he NINP in he SML and SSW samples o ha in ai , a ac o o 10-10 was used ha ep esen s he a io o NaCl290
in he a mosphe e o ha in seawa e o he A c ic (Gong e al., 2020b). Fi s , we no e ha he BT-gene a ed INPs o e lap
s ongly wi h he ambien measu emen s. This sugges s ha he ambien INP has s ong local sou ces om he seawa e . Due
o inc eased mixing and dilu ion in he ambien , i is also expec ed ha NINP, BT would be biased highe in he BT han in he
ambien as seen in Fig. 9. Secondly, he NINP de i ed o SML and SSW a e much lowe han hose measu ed in ambien ai
and in he BT. This s ongly suppo s he ac ha he ae osol p oduc ion mechanisms ha occu a he sea su ace (and in he295
BT) a e esponsible o p e e en ially pa i ioning INPs o he ai bo ne phase. Modeling he bubble o je bu s ing p ocess a
he sea su ace is c ucial o cap u e he ue lux o INPs om he ocean o he a mosphe e since he en ichmen o ai bo ne
INPs canno simply be ep esen ed by he mass ans e o NaCl.
Figu e 9. A mosphe ic NINP as a unc ion o empe a u e measu ed om ambien ai by LVS il e wi h he PM10 inle (g ay shaded a ea),
BT-ae osol collec ed on il e s ( ed), and NINP de i ed om SML (g een) and SSW (blue) samples, espec i ely. The ac o used o con e
NINP in he SML and SSW samples o concen a ion in ai is 10-10 (Gong e al., 2020a).
3.3 Co ela ions o NINP wi h SSA size and bio-chemical seawa e p ope ies
Figu e. 10 shows he co ela ion be ween a selec ion o a iables measu ed om he BT expe imen s du ing he A c ic Cen u y300
campaign. Spea man ank co ela ion coe icien s we e calcula ed due o he unknown dis ibu ion o each in es iga ed pa am-
e e . No ably, NINP, BT nega i ely co ela es wi h salini y, e lec ing INP- ich island wa e bodies. In addi ion, weak o mode a e
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co ela ions we e ound be ween NINP, BT and seawa e empe a u e (Tseawa e ). This could be a pu ely la i udinal o seasonal
e ec . Howe e , highe wa e empe a u e is epo ed o boos ma ine biological p oduc i i y by lowe ing he ac i a ion ene gy
o enzymes (Hall e al., 2008), he eby inc easing he emission o IN-ac i e ma ine biogenic ae osol.305
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Figu e 10. Spea man ank co ela ion ma ix o a iables measu ed om he BT expe imen s du ing he A c ic Cen u y campaign, wi h
he coe icien s shown in each box. The c oss-co ela ed pa ame e s a e NINP, BT measu ed a h ee selec ed empe a u es (T= -10, -15
and -20 °C); he salini y and empe a u e o wa e samples (Tseawa e ) used o BT expe imen s; and quan i y o nu ien s and biological
and e es ial sou ce indica o s measu ed om he wa e samples, including chlo ophyll-aconcen a ion, luo escence, concen a ions o
glucose, dissol ed o ganic ca bon (DOC), o al dissol ed ni ogen (TDN), ni a e (NO3–), phospha e (PO43– ) and silica e. Addi ionally, he
numbe concen a ion o ae osolized pa icles wi h diame e s > 0.5 µm measu ed om he OPC (n>0.5), n<0.3 and n<0.05 measu ed om SMPS
we e c oss-compa ed. The as e isks ep esen esul s wi h s a is ical signi icance (p< 0.05). Smoo hed ime s amps (in minu es) we e applied
o di e en da a se s o co ela ion analyses.
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Concen a ions o se e al componen s we e measu ed o he wa e samples used in he BT expe imen s. Figu e 10 shows
some o e all posi i e and signi ican co ela ions we e ound be ween NINP, BT and chl-a(excep T= -15 °C), luo escence and
phospha e. Al hough nei he o hese componen s is epo ed o be IN-ac i e, hei abundance is a ace o p omo ed ma ine
biological ac i i y, om which IN-ac i e o ganics and biogenic exuda es can o igina e. Recen ly i was shown ha luo escen
pa icle concen a ions a e a good p edic o o INPs o dus and biological o igin (Gao e al., 2024). No clea co ela ion310
be ween NINP, BT and DOC was ound in con as o McCluskey e al. (2018b) who sugges ed ha a posi i e co ela ion is
indica i e o sub-0.2 µm DOC componen s ac ing as ma ine INPs. S ong co ela ions we e also no obse ed be ween NINP, BT
and TDN and NO3–. A signi ican and mode a e co ela ion was ound be ween NINP, BT and silica e concen a ion. A biological
o igin o silica e in he ocean om ma ine dia oms and mic oalgae wi h siliceous cells has been epo ed (e.g., Thalassiosi a
pseudonana) o be IN-ac i e (Knop e al., 2011). Ano he possibili y o he posi i e co ela ion wi h silica e is he p esence315
o dus - ype INPs. Co nwell e al. (2020) showed in a labo a o y s udy ha he seawa e doped wi h dus can be e-ae osolized
wi h e ained IN ac i i y and added o he a mosphe ic INP popula ions du ing bubble bu s ing. This pa hway o INP ans e
could be esponsible o he ela i ely high NINP ae osolized om land-sou ced eshwa e o seawa e samples collec ed
app oaching islands (see Fig. 8) ha a e o en ich in suspended sedimen s due o he lu ial ou wash.
NINP, BT is nega i ely co ela ed wi h pa icle concen a ions n>0.5 ae osolized om he wa e samples, indica ing ha he ab-320
solu e loading o SSA (domina ed by NaCl) does no de e mine he abundance o ae osolized INPs (suppo ing he conclusions
om Figu e 9) and emphasizes ha NINP canno always be p edic ed by ae osol numbe concen a ion (Li e al., 2022) like
pa ame e iza ions o dus y o highly pollu ed a mosphe es (DeMo e al., 2015; Niemand e al., 2012; DeMo e al., 2010).
Howe e , he nega i e co ela ion be ween NINP, BT and n<0.3 and n<0.05 do no suppo ha ine ae osol mode could be used
as p edic o s o INP concen a ions. The absence o a posi i e co ela ion wi h ae osol numbe concen a ion o di e en size325
anges s eng hens ou conclusion ha NINP canno always be p edic ed by ae osol numbe concen a ions as has been obse ed
elsewhe e in he A c ic (Li e al., 2022; Pa amono e al., 2020; Lache e al., 2018). Combining he co ela ion analyses o
NINP, BT wi h biological indica o s (i.e., Chl-a, luo escence, PO43– ) and silica e, we in e ha he ae osoliza ion p ocesses a
he wa e -ai in e ace p e e en ially pa i ions he IN-ac i e species o he ae osol phase and ha he composi ion (phospha e,
silica e) and luo escence in o ma ion a e c ucial o p edic INP concen a ions (Gao e al., 2024).330
The ela i e abundance o INPs in di e en samples aken simul aneously including ambien ai (impinge samples), seawa-
e samples (CTD seawa e ), and BT-ae osolized SSA a e shown in Fig. 11. The compa ison e eals insigni ican co ela ions
be ween NINP in ambien ai and he coinciden ally sampled seawa e (Fig. 11 a). In con as , a s a is ically signi ican co -
ela ion was ound be ween ai bo ne (NINP, ambien ) and BT-ae osolized (NINP, BT) INP concen a ions a he selec ed eezing
empe a u es (Fig. 11 b). NINP, BT a e p esen in highe concen a ions compa ed o ambien INPs by abou an o de o magni-335
ude due o he absence o dilu ion in he BT-ae osolized ai . The posi i e co ela ions sugges ha he BT expe imen s simula e
a ealis ic ae osoliza ion p ocess a he sea-ai in e ace, and he seawa e can be a conside able sou ce o INPs in he A c ic
Ocean. The da a om Fig. 11 (b) sugges ha SSA is a sou ce o INPs, bu he absence o a posi i e co ela ion wi h NINP
de i ed om seawa e in Fig. 11 (a) sugges s o he wise. This addi ional suppo is ha he missing ac o o wa e samples is
he ae osoliza ion p ocess ha en iches INPs in he ai , which canno simply be accoun ed o by he lux o SSA om wa e o340
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Figu e 11. Compa isons be ween ambien NINP measu ed om impinge samples and coinciden NINP measu ed om (a) seawa e (b) BT-
ae osol il e s. The dashed lines indica e he linea eg ession in he loga i hmic scale, and only he s a is ically signi ican (p< 0.05) alues
(co ela ion coe icien s) a e shown in he igu e. The co ela ion coe icien s o all da a a e gi en in Tab. ??.
ai . The mechanisms o INP ae osoliza ion a he ocean-ai in e ace could be impac ed by se e al compounding ac o s, e.g.,
an en ichmen o INPs a he sea su ace mic olaye (Wilson e al., 2015), dissol ed species and hei abundance ( an Pinx e en
e al., 2017; Coch an e al., 2016), biological p oduc i i y (C eamean e al., 2019; Rinaldi e al., 2013), sea su ace empe a u e
( an Pinx e en e al., 2017; Ladino e al., 2016), wind speed (Lewis e al., 2004), and sea ice concen a ions (Gab ic e al.,
2018).345
4 Conclusions
This s udy p esen s summe ime obse a ions o NINP and ae osol ela ed p ope ies o e he Ba en s, Ka a, and Lap e Seas
in he Eu asian A c ic om Augus o Sep embe 2021. Va iabili y in NINP is highly in luenced by local sou ces, and o
some ex en me eo ological condi ions, and po en ially long- ange anspo . A se ies o online and o line measu emen s we e
applied o in es iga e he INP abundance in seawa e , og, and ambien ai o unde s and he sou ces o he INP and p oduc ion350
mechanisms.
The majo i y o ambien ae osol samples collec ed on LVS il e s we e p one o deg ada ion in INP concen a ion a e
hea ing o 95 °C o 20 min, indica ing he p esence o p o einaceous o biogenic INPs ha a e hea -labile. By compa ing
NINP in he ambien ai o o he en i onmen s, simila NINP was obse ed in og wa e compa ed o ambien ai , indica ing
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INPs a e no en iched in og wa e and a e likely cloud condensing nuclei. INPs in og should be conside ed in s udies o INP355
dis ibu ion and a ailabili y due o i s ole as an in e media e ese oi and o he o ma ion o ice ogs in he a mosphe ic
li ecycle o INPs. No clea end was obse ed o INP en ichmen in he SML compa ed o SSW, which is bo h in ag eemen
wi h and in con as o p e ious s udies. The equency o ma ine biological ac i i y, such as phy oplank on blooms, lu ial
inpu o sedimen INPs, along wi h he a iabili y in sea su ace mixing and ocean s a e, could in luence he abundance o INPs
in di e en ocean laye s.360
A compa ison o NINP in he SML, SSW and CTD seawa e samples o in si u ae osol measu emen s om a BT sys em
and ambien INPs om he LVS il e s e eals ha he bubble-bu s ing mechanism is impo an in ans e ing INP om
he ocean o he a mosphe e. The abundance o INPs in he BT-sp ayed ae osols showed a dependence on he composi ion
o wa e componen s, wi h e es ial eshwa e possessing highe NINP compa ed o seawa e samples. In acco dance, a
educed NINP, BT was associa ed wi h a longe dis ance o land o an inc eased sea ice co e age whe e he subsu ace seawa e 365
samples we e collec ed. Based on he co ela ion analyses be ween NINP, BT and biological ac i i y, his s udy suppo s he
impo an ole o ma ine biogenic ae osol as a sou ce o INPs in he emo e A c ic Ocean a om e es ial sou ces. Ou
esul s highligh key ela ionships, such as he s ong co ela ion be ween INP abundance and local biogenic ac o s (e.g.,
chlo ophyll and luo escence signals). These co ela ions sugges ha in eg a ing eal- ime biological ac i i y da a, especially
du ing phy oplank on blooms, could imp o e model pa ame e iza ions o A c ic INP emissions. Las ly, o he e ec s may be370
p esen in addi ion o he composi ion du ing he SSA gene a ion and INP pa i ioning in he ocean and a mosphe e, including
he en ichmen o IN-ac i e ma e ials in he sea su ace mic olaye , sea ice co e age, ad ec ion, and mixing in di e en ocean
laye s.
Da a a ailabili y. The da a om his s udy a e all inco po a ed in o he main ex and will be made a ailable addi ionally h ough he ETH
Lib a y wi h a pe sis en DOI upon success ul pee - e iew o he manusc ip .375
Au ho con ibu ions. GL pe o med sample p ocessing and da a analysis, p oduced igu es, in e p e ed esul s, and co-w o e he manusc ip .
GL and AW pa icipa ed in he campaign and conduc ed in si u sampling and measu emen s. AW con ibu ed o he manusc ip p epa a ion
and acqui ed unding. AR conduc ed he ae osol gene a ion bubble ank expe imen and collec ed samples o biochemical analysis. GPF
pe o med INP analysis and hea ea men o il e samples, CTD seawa e samples, and BT-ae osolized il e samples. IT p o ided he
LAGRANTO backwa d ajec o y da a. MD p o ided he esea ch idea on INP pa i ioning using he INP esul s om he bubble ank. ZAK380
supe ised he p ojec , ob ained unding, and was in ol ed in expe imen and campaign planning, da a in e p e a ion, and manusc ip w i ing.
All au ho s e iewed he manusc ip .
Compe ing in e es s. The au ho s decla e ha no compe ing in e es s a e p esen .
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Acknowledgemen s. This esea ch used samples and/o da a p o ided by he A c ic Cen u y Expedi ion, a join ini ia i e led by he Swiss
Pola Ins i u e (SPI), he An a c ic and A c ic Resea ch Ins i u e (AARI), and GEOMAR Helmhol z Cen e o Ocean Resea ch Kiel (GEO-385
MAR), and unded by he Swiss Pola Founda ion. GL and ZAK acknowledge ha his p ojec has been made possible by a g an om he
Swiss Pola Ins i u e, D . F ede ik Paulsen. GPF acknowledges unding om he Academy o Finland (g an no. 342227). ZAK acknowl-
edges his p ojec has ecei ed unding om he Ho izon Eu ope p og amme unde G an Ag eemen No 101137680. We acknowledge all
hose in ol ed in he ieldwo k associa ed wi h he A c ic Cen u y Expedi ion, including echnical suppo om D . Michael Rösch. We ac-
knowledge D . on Jackowski and D . Engel o sha ing biogeochemical da a o CTD wa e samples. We acknowledge F anziska Aemisegge 390
and I is Thu nhe calcula ed he backwa d ajec o ies used in his s udy. We would like o hank D . Xu Fang om ETH o p o iding he
ICP-OES ins umen wi h assis ance on sample p epa a ion and measu emen s.
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