Abs ac Ca bonyl sul ide (OCS) is used o quan i y he ca bon cap u e po en ial o he biosphe e because
o i s di ec co ela ion wi h CO2 up ake du ing pho osyn hesis. Howe e , o cons ain he u ban biosphe e
signal, i is necessa y o e alua e po en ial an h opogenic sou ces. We conduc ed wo sampling campaigns in
he Me opoli an A ea o Ba celona (AMB), Spain, du ing May ( ull COVID lockdown) and Oc obe 2020
o measu e he spa ial dis ibu ion and a iabili y o OCS in ou u ban land uses as ollows: buil , u ban
o es , u ban pa k, and pe i-u ban ag icul u e. The OCS backg ound le els de e mined a Tibidabo (442m
asl) we e app oxima ely 484±20 pp and 407±8 pp o May and Oc obe 2020, espec i ely, and ag eed
wi h o he seasonal su eys conduc ed in Eu ope du ing ha same pe iod. A e aged emissions we e in he
ange o +Δ12±40 pp o he ci y and we e +Δ9.4±40.9 pp o u ban +Δ22.1±48 pp o u ban g een
+Δ20.7±42.9 pp o ag icul u al and −Δ4.8±19.6 pp o o es . The u ban alues anged om neu al o
abo e backg ound, sugges ing nea by an h opogenic and ma ine emissions such as +Δ150 pp in Mon juic,
which is downwind o Ba celona's ha bo . Du ing he c op-g owing season in May, he ag icul u al a eas
consis en ly showed alues below he backg ound (up o −Δ76 pp in Ga à, up ake) a 7:00 UTC when he land
b eezes we e dominan , while la e in he mo ning, when he sea b eeze a e de eloped, he plan sink is masked
by he anspo o ma ine emissions. U ban o es s loca ed no h o Tibidabo showed OCS alues up o −Δ70
pp , sugges ing signi ican up ake by u ban o es s. We conclude ha de e mining he u ban biosphe e signal
using OCS as a ace is mo e complex han expec ed because he ma ine and an h opogenic emissions om he
po s ongly impac he spa ial- empo al dis ibu ion o OCS.
Plain Language Summa y Ca bonyl sul ide (OCS) is a gas used o quan i y he ca bon cap u e
po en ial o he biosphe e. Howe e , ci ies ha e po en ial an h opogenic OCS sou ces ha can impede a clea
cons ain o he u ban biosphe e signal. We conduc ed wo sampling campaigns in he Me opoli an A ea o
Ba celona (AMB), Spain, du ing May ( ull COVID lockdown) and Oc obe 2020 o measu e he a iabili y o
OCS in ou u ban land uses: buil , u ban o es , u ban pa k, and pe i-u ban ag icul u e. The OCS backg ound
le els de e mined a Tibidabo (we e app oxima ely 484±20 pp and 407±8 pp o May and Oc obe 2020,
espec i ely). The u ban buil si es we e ypically abo e backg ound, sugges ing nea by an h opogenic and
ma ine emissions. Du ing he c op-g owing season, he ag icul u al a eas consis en ly showed alues below
he backg ound sugges ing plan OCS up ake when he land b eezes we e dominan , while la e in he mo ning,
when he sea b eezes de eloped, he in luence o ma ine emission esul ed in alues abo e he backg ound.
U ban o es s showed signi ican OCS up ake. We conclude ha de e mining he u ban biosphe e signal using
OCS as a ace is mo e complex han expec ed because he ma ine and an h opogenic emissions om he po
s ongly impac he spa ial- empo al dis ibu ion o OCS.
ESTRUCH ETAL.
© 2023. The Au ho s.
This is an open access a icle unde
he e ms o he C ea i e Commons
A ibu ion-NonComme cial-NoDe i s
License, which pe mi s use and
dis ibu ion in any medium, p o ided he
o iginal wo k is p ope ly ci ed, he use is
non-comme cial and no modi ica ions o
adap a ions a e made.
Explo ing he In luence o Land Use on he U ban Ca bonyl
Sul ide Budge : A Case S udy o he Me opoli an A ea o
Ba celona
Ca me Es uch1,2 , Sau eu Bel iso3 , Alba Badia1 , Ve onica Vidal1,4 , Roge Cu coll1,5,
Mi eia Udina6 , Claudia G ossi5 , Josep-An on Mo guí1,7, Rica d Segu a1, Se gi Ven u a1,
Yolanda Sola6 , and Ga a Villalba1,8
1Ins i u de Ciència i Tecnologia Ambien als (ICTA), Uni e si a Au ònoma de Ba celona, Ba celona, Spain, 2Eu eca , Cen e
Tecnològic de Ca alunya, Clima e Change Resea ch Depa men , Ampos a, Spain, 3Labo a oi e des Sciences du Clima e de
l’En i onnemen , LSCE, Pa is-Saclay, F ance, 4Depa men o Compu e A chi ec u e and Ope a i e Sys ems, Uni e si a
Au ònoma de Ba celona (UAB), Ba celona, Spain, 5Ins i u e o Ene gy Techniques, Uni e si a Poli ècnica de Ca alunya,
Ba celona, Spain, 6Depa amen de Física Aplicada–Me eo ologia, Uni e si a de Ba celona, Ba celona, Spain, 7Depa amen
de Biologia E olu i a, Ecologia i Ciències Ambien als, Uni e si a de Ba celona, Ba celona, Spain, 8Depa men o
Chemical, Biological and En i onmen al Enginee ing, Uni e si a Au ònoma de Ba celona (UAB), Ba celona, Spain
Key Poin s:
• The u ban buil si es we e ypically
abo e backg ound, sugges ing nea by
an h opogenic and ma ine emissions
• Ag icul u al a eas consis en ly
showed alues below he backg ound
sugges ing plan Ca bonyl sul ide
(OCS) up ake when he land b eezes
we e dominan
• De e mining u ban biosphe e signal
using OCS is complex because ma ine
and an h opogenic emissions impac
i s spa ial- empo al dis ibu ion
Suppo ing In o ma ion:
Suppo ing In o ma ion may be ound in
he online e sion o his a icle.
Co espondence o:
G. Villalba,
[email p o ec ed]
Ci a ion:
Es uch, C., Bel iso, S., Badia, A.,
Vidal, V., Cu coll, R., Udina, M.,
e al. (2023). Explo ing he in luence
o land use on he u ban ca bonyl
sul ide budge : A case s udy o he
me opoli an a ea o Ba celona. Jou nal
o Geophysical Resea ch: A mosphe es,
128, e2023JD039497. h ps://doi.
o g/10.1029/2023JD039497
Recei ed 23 JUN 2023
Accep ed 26 NOV 2023
Au ho Con ibu ions:
Concep ualiza ion: Ca me Es uch,
Sau eu Bel iso, Ga a Villalba
Da a cu a ion: Josep-An on Mo guí,
Ga a Villalba
Funding acquisi ion: Ga a Villalba
In es iga ion: Ca me Es uch, Sau eu
Bel iso, Alba Badia, Ve onica Vidal,
Roge Cu coll, Mi eia Udina, Claudia
G ossi, Josep-An on Mo guí, Rica d
Segu a, Se gi Ven u a, Yolanda Sola,
Ga a Villalba
10.1029/2023JD039497
RESEARCH ARTICLE
1 o 21
Jou nal o Geophysical Resea ch: A mosphe es
ESTRUCH ETAL.
10.1029/2023JD039497
2 o 21
1. In oduc ion
Ca bonyl sul ide (he ea e OCS) is an a mosphe ic ace gas used o s udy he CO2 seques a ion capaci y o
ege a ion (Remaud e al.,2023; Whelan e al.,2018) because i is des oyed h ough pho osyn hesis in he
same way as CO2 wi hou p oducing any emissions h ough espi a ion (P o oschill-K ebs & Kesselmeie ,1992).
Acco ding o he la es es ima ions, e es ial ege a ion and soils akes up om 530 o 670GgSy
−1 (Remaud
e al.,2023) he la ges na u al sink o a mosphe ic OCS. Su ace oceans a e he mos impo an na u al sou ce
o OCS con ibu ing di ec ly and indi ec ly, ha is, om he a mosphe ic oxida ion o ca bon disul ide and
dime hylsul ide, be ween 270 and 320 (Lenna z e al.,2017). The global budge o OCS is pa ially balanced by
an h opogenic emissions, which a e es ima ed o be 400GgSy
−1 (Campbell e al.,2015). Te es ial sinks and
na u al and an h opogenic sou ces a e gene ally sepa a ed in space and ime, and exhibi dis inc seasonal and
spa ial a ia ions (Remaud e al.,2023). Hence, land use changes a e expec ed o ha e a signi ican in luence on
he global budge o a mosphe ic OCS.
Al hough many s udies ha e e alua ed OCS budge s a egional and global scales, li le is known abou OCS
sou ces and sinks a he u ban scale. Unde s anding land use in luence on he budge o a mosphe ic OCS a he
u ban scale is much mo e di icul o es ablish because sou ces and sinks can coexis o e small dis ances. Fo
example, Commane e al.(2013) indi ec ly assessed OCS sou ces along he highly u banized coas line o Cali-
o nia whe e hey de ec ed biogenic OCS emissions om we lands in Sac amen o Bay, an h opogenic emissions
nea a s o age acili y and e ine y in he po o Los Angeles, and OCS loss du ing he day ime due o pho osyn-
he ic up ake in ege a ed a eas. Besis e al.(2021) also conduc ed a s udy ha iden i ied po en ial sou ces o OCS
a he ci y le el and obse ed he spa ial he e ogenei y in luencing OCS mixing a ios o Thessaloniki, G eece,
and iden i ied h ee loca ions whe e OCS concen a ions in inne -ci y a eas we e h ee imes highe han hose a
he sea on and whe e he was e managemen sys em was a sou ce o OCS. Acco ding o Zumkeh e al.(2018),
an h opogenic emissions o OCS due o aluminum, esiden ial and indus ial coal, TiO2, sol en s and i es in he
Me opoli an A ea o Ba celona con ibu e o 65% (178MgSy
−1) o he o al emissions in he Ca alonia egion
(276MgSy
−1, see Figu e S1 in Suppo ing In o ma ionS1). Howe e , a s udy by Bel iso e al.(2023) demon-
s a ed ha he Zumkeh e al.(2018) in en o y o F ance la gely o e es ima ed OCS an h opogenic emissions
by app oxima ely an o de o magni ude. A p e ious s udy by he same g oup used di ec measu emen s om a
sampling owe and compu ed back ajec o ies wi h he FLEXPART anspo model o ind ha he Pa is subu -
ban a ea was ac ing mainly as an OCS sink (Bel iso e al.,2022). Ano he u ban s udy o Innsb uck, Aus ia,
measu ed he hou ly exchange a es o OCS wi h an eddy co a iance owe and showed ha u ban OCS emissions
a e signi ican ly highe a noon du ing weekdays han du ing weekends, which sugges s ha oad a ic could be
a ne sou ce o OCS emissions.
The use o OCS as a pho osyn hesis ace has ecen ly ecei ed a en ion as a po en ial me hod o de e mine
he con ibu ion o he u ban biosphe e owa d educing he ca bon oo p in (Mallik e  al., 2016; Villalba
e al.,2021). Mallik e al.(2016) epo ed he i s eco ds o annual OCS mixing a ios o e an Indian ci y,
which we e subs an ially highe han oposphe ic alues, and hose alues changed seasonally wi h an obse ed
86% d op in OCS in No embe when ai masses changed om oceanic o con inen al. Villalba e al.(2021)
also obse ed changes in OCS ela ed o ai masses coming om ma ine and con inen al sou ces. This wo k
highligh ed he di icul y o cha ac e izing he biosphe e signal when he inpu masses a e con inen al due o he
he e ogenei y, hey p esen in OCS con en compa ed o s able ma ine condi ions.
This s udy aims o con ibu e o he unde s anding o he dynamics o OCS budge s in u ban a eas by explo ing
o wha ex en di e en u ban land uses can ha e an impac on a mosphe ic OCS mixing a ios in e ms o he
pa icula u ban clima e, geog aphy, and opog aphy a ec ing he anspo and mixing o OCS sou ces and
sinks. Mo i a ed by he p esen lack o in si u OCS con inuous measu emen s o p ope ly in e su ace OCS
(Remaud e al.,2022), we conduc ed an OCS measu emen campaign in he Me opoli an A ea o Ba celona
(AMB). We selec ed ou di e en land uses as sampling si es as ollows: o es , ag icul u al land, u ban pa ks
and impe ious a eas wi h he in en ion o unde s anding he ole o u ban land use on he OCS budge in a
coas al ci y whe e we would expec a mixing a io g adien be ween he sea (whe e OCS is p oduced) and he land
(OCS cap u e in ege a ed a eas). The selec ion o sampling a eas was based on hei po en ial as a sink o OCS
based on pho osyn he ic a es (Campbell e al.,2017; Villalba e al.,2021; Yang e al.,2018) o a local sou ce
based on an h opogenic in en o ies (Lee & B imblecombe,2016; Yan e al.,2019; Zumkeh e al.,2018). The
OCS sampling campaigns we e unded and conduc ed wi hin he p ojec In eg a ed Sys em Analysis o U ban
Me hodology: Ca me Es uch, Ga a
Villalba
P ojec Adminis a ion: Ga a Villalba
Resou ces: Ga a Villalba
Supe ision: Sau eu Bel iso, Ga a
Villalba
Visualiza ion: Ca me Es uch, Ve onica
Vidal, Roge Cu coll, Ga a Villalba
W i ing – o iginal d a : Ca me Es uch,
Ga a Villalba
W i ing – e iew & edi ing: Ca me
Es uch, Sau eu Bel iso, Alba Badia,
Roge Cu coll, Mi eia Udina, Claudia
G ossi, Ga a Villalba
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Jou nal o Geophysical Resea ch: A mosphe es
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Vege a ion and Ag icul u e (URBAG), which was inanced by he Eu opean Resea ch Council wi h he o e all
aim o unde s anding he in luence o g een in as uc u es on he u ban CO2 budge . As a coas al ci y wi h
in ense sea b eezes du ing he day, he AMB is an ideal case s udy o de e mine he con ibu ion o he u ban
biosphe e and o he an h opogenic sou ces o he o e all u ban OCS budge . The campaigns we e conduc ed
du ing he sp ing and ea ly au umn o 2020 and almos coincided wi h he OCS sp ing maximum and au umn
minimum (Mon zka e al.,2007). Fu he mo e, he May campaign ook place du ing he ull lockdown due o he
COVID pandemic, which helped cons ain he biosphe e signal gi en he educ ion in an h opogenic ac i i ies
ha a e po en ial sou ces o OCS such as ehicle exhaus (Zumkeh e al.,2017). We analyzed he obse ed OCS
concen a ions in e ms o land-use in luence while unde s anding he ole o local wea he condi ions, synop ic
e en s, and he plane a y bounda y laye by using a mosphe ic anspo models, clima e obse a ions and a mos-
phe ic ace s. Mo e speci ically, we a emp ed o answe he ollowing ques ion: Wha is he land-use in luence
on he u ban OCS budge ?
2. Me hods
2.1. S udy Si e
The wo expe imen al campaigns ook place in he Me opoli an A ea o Ba celona (AMB), loca ed in he NE
co ne o Spain, as shown in Figu e1. The AMB, wi h a o al su ace a ea o app oxima ely 640km
2 and
o e 3.3 million inhabi an s (16,160 people/km
2), is he se en h la ges u ban a ea and eigh h mos densely
Figu e 1. (a) A map o Spain showing he Me opoli an A ea o Ba celona (AMB, ed ec angle). O og aphy o he AMB
(b) and land use (c), whe e iplica es o colo ed do s ep esen he upwind, a ge , and downwind sampling loca ions (d).
Backg ound a mosphe ic OCS le els we e in es iga ed a he upwind sampling poin s a he si es o Tibidabo (highes al i ude
in he PBL), Ga à and Poble Nou (closes o he sho e). These si es a e depic ed wi h colo ed do s wi h whi e ci cles in b and
c. The ed diamond ep esen s he loca ion o ICTA and he blue one whe e he adiosondes we e launched and he adon
measu emen s we e pe o med (c).
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Jou nal o Geophysical Resea ch: A mosphe es
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10.1029/2023JD039497
4 o 21
popula ed egion in he Eu opean Union. I is also one o he mos indus ialized a eas in he wes e n EU (Que ol
e al.,2004), specializing in ood p oduc ion, chemicals, ehicle manu ac u ing, and gas p oduc ion and dis i-
bu ion (Ins i u d’Es adís ica de Ca alunya,2023). The AMB is bounded by he Besós Ri e in he no heas , he
Llob ega Ri e in he wes , he Collse ola moun ain ange o he no h, and he Medi e anean Sea o he sou h,
as shown in Figu e1. The AMB has a Medi e anean d y subhumid clima e wi h an annual p ecipi a ion o
app oxima ely 600mm, which is mainly concen a ed du ing sp ing and au umn, and a mean annual empe a u e
o 16.5°C. The o og aphy o he ci y ex ends om sea le el o 516m abo e sea le el (a.s.l.) a he moun ain ange
loca ed no hwes o he main u ban a eas.
Mo e han hal o he AMB's su ace a ea is co e ed by ege a ion in a ious o ms, including u ban o es (43%),
ag icul u al ields (8%) and u ban pa ks (4%), while 41% is co e ed by impe ious and o he in as uc u es (4%).
Land uses a e shaped by he ollowing physical cons ain s: c ops a e loca ed in he coas al plains o med by he
del a o he Llob ega Ri e , while u ban o es s composed o pine and holm oaks a e loca ed in he Collse ola
moun ain ange (Figu e1). U ban g een spaces a e sca e ed h oughou he me opolis and popula ed wi h o na-
men al species anging om acacias o plan ain ees and o namen al sh ubs and g asses.
2.2. Field Campaigns
Ai samples we e aken a he eigh si es shown wi h colo ed do s in Figu e1c, which we e selec ed o ep e-
sen he he e ogenei y o land use h oughou he AMB and a e summa ized in o ou land-use ca ego ies (see
Table1): ag icul u al a ea (loca ed in he Ga à and P a a eas), u ban o es (Tibidabo and Collse ola), u ban
g een (Mon juic and Guina dó) and u ban (Sag ada Familia and Poble Nou). We ook ai samples a each si e
(he ea e e e ed o as he a ge si e) and upwind and downwind o each a ge si e in an a emp o ollow he
ai mass low du ing i s ajec o y o e he a ge si e. The upwind and downwind sampling si es we e de e -
mined based on his o ical wind pa e ns and ajec o ies ypical o each a ge loca ion unde simila a mosphe ic
condi ions expec ed du ing he campaign and a e a ailable om he Me eo ological Se ice o Ca alonia (www.
me eo.ca ) and shown in Tex S1 in Suppo ing In o ma ionS1. No e ha in May and Oc obe 2020, obse ed
Campaign Si e (ele a ion) Land use ype Da e CWTs a SWC b PBLH ange (m) OCS 7:00 UTC (pp ) OCS 9:30 UTC (pp )
May 2020 Tibidabo (175–442m) Fo es 19/05 C N 19–441 478±20 494±9
Ga à (0–2m) Ag icul u al 21/05 U N 11–249 482.1±NA 495.5±10.7
Poble Nou (0–4m) U ban 21/05 U N 44–2,217 461±20 NA
Mon juic (42–98m) U ban g een 20/05 C N 327–883 485±14 490±5
P a (0–2m) Ag icul u al 25/05 E E 737–1,182 502±NA 508±2
Sag ada (37–55m) U ban 26/05 E E 771–1,900 460±6 NA
Collse ola (107–442m) Fo es 27/05 E E 395–1,079 441±39 497±3
Guina dó (115–169m) U ban g een 28/05 A SE 590–1,524 505±8 612±17
Oc obe 2020 Ga à (0–2m) Ag icul u al 23/10 U NW 21–5,019 401±9 403±3
Poble Nou (0–4m) U ban 15/10 CN N 287–571 405±23 426±45
Guina dó (115–169m) U ban g een 19/10 ASW SW 69–934 389±20 392±16
Sag ada (37–55m) U ban 20/10 SW SW 29–1,085 444±19 460±93
Mon juic (42–98m) U ban g een 21/10 CSW SW 92–734 425±NA 485±87
P a (0–2m) Ag icul u al 22/10 SW SW 103–495 468±24 490±37
No e. An unab idged e sion o his able wi h upwind and downwind OCS including a de ailed da a o backg ound measu emen s concen a ions (see Figu e4) is
a ailable in Tex S1 in Suppo ing In o ma ionS1.
aCWT: Ci cula ion wea he ype. The di e en ypes o CWTs a e cyclonic (C), an icyclonic (A), pu e ad ec i e (N, S, E, W, NE, SE, NW, SW), hyb id cyclone-ad ec i e
(CN, CNE, CE, CSE, CS, CSW, CW, CNW), hyb id an icyclone-ad ec i e (AN, ANE, AE, ASE, AS, ASW, AW, ANW, and unde ined (U)).
bSWC: Synop ic wind
componen summa izing he p essu e pa e n, on s, wind di ec ion and speed.
Table 1
Ci cula ion Wea he Type (CWT), Synop ic Wind Componen (SWC) and PBLH Ex ac ed F om WRF Simula ions Exp essed in Me e s Abo e G ound Le el (a.g.l),
A e aged OCS Concen a ions o All Measu emen s Taken Each Day Du ing he May and Oc obe Campaigns, and Exp essed in pp (Mean Values F om he Th ee
Si es, Mean Values±S anda d De ia ions)
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Jou nal o Geophysical Resea ch: A mosphe es
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wind pa e ns some imes di e ed om his o ical da a. The loca ions o he upwind, a ge , and downwind si es
a e shown o each poin using he same colo in Figu e1c. The spa ial dis ance among he h ee sampling poin s
o each si e anges om 500 o 4,000m. Sampling imes we e chosen o cap u e inland winds du ing he ea ly
mo ning (i.e., 4:00 and 7:00 UTC am) and he ypical sea b eezes ha de elop du ing he mo ning and ea ly a e -
noon (i.e., 9:30 and 11:00 UTC am). In each campaign, each place was measu ed one day, a he s ipula ed hou s.
The i s campaign ook place be ween 18 May and 28 May 2020, which was du ing a pe iod o in ense anspo
es ic ions due o he COVID-19 pandemic, and esul ed in highly signi ican ai pollu ion educ ions (Badia
e al.,2021). An h opogenic emissions d as ically dec eased, especially o he a ia ion (95%), oad anspo (up
o 85%), and mo e mode a ely acco ding o shipping (21%) and indus y (11%) sec o s (Gue a a e al.,2021).
The second campaign ook place om he 13 o he 27 o Oc obe 2020, when he an h opogenic ac i i y e u ned
o no mal.
The empe a u e anged om 20°C o 24°C du ing May and 14°C o 20°C du ing Oc obe . Samples we e collec ed
a 7:00 UTC and 9:30 UTC, and o some speci ic days chosen a he beginning and a he end o he campaign,
we pe o med addi ional sampling a 4:00 UTC and 11:00 UTC o he Tibidabo, Ga à and Poble Nou upwind
loca ions o de e mine he backg ound concen a ion o OCS. The wea he was s able du ing bo h campaigns
wi h one day o sligh p ecipi a ion du ing each sampling campaign, which accumula ed 2.6 and 1.6mm du ing
May 29 and Oc obe 26, espec i ely. The ai mass in luence was mos ly cyclonic and ad ec i e wi h some days
cha ac e ized by an icyclonic ci cula ion. Synop ic winds we e mos ly no h and eas du ing he May campaign
and p edominan ly sou hwes du ing Oc obe as summa ized in Table S2 in Suppo ing In o ma ionS1.
We eco ded empe a u e, ai p essu e, wind di ec ion and wind speed a each sampling si e using a po able
anemome e (Skywa ch Xplo e 4). The ela i e humidi y was ob ained om he Me eo ological Se ice o Ca a-
lonia o he i s campaign (Se ei Me eo ològic de Ca alunya,2023), and addi ionally, i was egis e ed on si e
using a digi al hyg ome e (TFA Dos mann®, p ecision ±4%) du ing he Oc obe campaign.
2.3. OCS Measu emen s and Analysis
Samples we e collec ed in cylind ical bo osilica e glass lasks (1L olume, No mag Labo und P ozess echnik
GmbH, Ge many) wi h Kel-F PCTFE al es i ed a bo h ends. This lask ma e ial showed he lowes pe mea-
ion o gases compa ed o o he sealing ma e ials (S u m e al.,2004). To ensu e he quali y o he measu emen
echnique and epea abili y o he expe imen , wo lasks connec ed o each o he in a po able de ice we e
simul aneously illed in se ies (see Tex S2 in Suppo ing In o ma ionS1, U ban si es, o de ice pic u es). The
inle was ins alled a 3.5m abo e g ound le el (m a.g.l.) and ai , a e passing h ough a magnesium pe chlo a e
desiccan ube o emo e mois u e and a il e o emo e pa icles, was pumped o he lasks wi h he help o a
diaph agm pump (KNF N84.4 ANDC). Be o e aking he sample, ai was lushed h ough he lasks o a leas
10min. A ha ime, we checked ha he low was s eady and be ween 2.0 and 3.5Lmin
−1. The lask sampling
ook abou o 10min o be comple ed. A e lushing, he exi al e was closed, and he lasks we e p essu ized
wi h sample ai o app oxima ely 1.5ba . Samples om he a ge , upwind and downwind si es we e aken a he
exac same momen o simula e an Eule ian app oxima ion in which he sampling poin emains ixed (Leelőssy
e al.,2016).
Flasks we e sen o he Labo a oi e des Sciences du Clima e de l’En i onnemen , LSCE, Pa is-Saclay, F ance,
o OCS analyses. Flasks we e s o ed o a maximum o 2mon hs be o e analysis. OCS was analyzed ollowing
he analy ical me hod desc ibed in Bel iso e al.(2016, 2022). In his p ocedu e, a mosphe ic OCS (500ml)
is apped using an au oma ed sampling sys em (En ech P7100 p econcen a o ) and hen analyzed by gas
ch oma og aphy wi h pulsed lame pho ome y de ec ion (PFPD, Va ian Model 3,800, Bel iso e al.,2016). Cali-
b a ion was pe o med e e y week using a calib a ion gas supplied by Ai P oduc s (Bel iso e al.,2016). The
di e ence be ween he assigned alue o an NOAA long- e m ai s anda d (NOAA-2004 scale) and he a e age
o mul iple analyses o ha same s anda d was smalle han 1.5%. The d i be ween calib a ions was assessed on
a daily basis using a sho - e m a ge gas (Bel iso e al.,2016).
2.4. De e mining he Plane a y Bounda y Laye Heigh
I is necessa y o de e mine he plane a y bounda y laye heigh (PBLH) o unde s and i s in luence on he
accumula ion and dilu ion o OCS concen a ion a each si e o e he u ban a ea. PBLH measu emen s we e
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no possible a he eigh a ge si es, bu a leas he PBLH was calcula ed om measu emen s aken on he
campus o he Uni e si y o Ba celona (Figu e1, label: Radiosonde/Radon) using wo di e en echniques as
ollows: (a) based on obse ed measu emen s om a adiosonde (RSD) s a ion ins alled on he oo o he Physics
Depa men o he Uni e si y o Ba celona (41°23′03″ N 2°07′01″E), which is pa o he Global Me eo ological
Ne wo k (GCOS,2016); and (b) ia a lase ceilome e (CL-31, Vaisala Inc., Finland) loca ed a he same place
wi h a measu emen ange up o 7.6km, 10-m e ical esolu ion and a empo al esolu ion o 16s. Fo he la e ,
he PBLH is es ima ed om he ceilome e da a using he Vaisala Bounda y-Laye View so wa e (BL-VIEW)
Enhanced G adien me hod (VAISALA,2020)—see de ails in Ga cia-Dalmau e al.(2021)— ollowed by selec-
ion algo i hms acco ding o he me hodology o Lo e ane e al.(2016).
To de e mine he PBLH based on adiosonde measu emen s, we ollowed a obus nume ical p ocedu e p oposed
by Liu and Liang(2010) using midday adiosonde (RSD) obse a ions om he selec ed pe iods o s udy and
conside ing 1100 UTC as he launching ime. The PBLH was compu ed ollowing he ai pa cel me hod o a
con ec i e domina ed bounda y laye (Holzwo h,1964; Seibe e al.,2000; S ull,1988) as he heigh whe e ai
pa cel e olu ion ollowing a d y adiaba ic e olu ion om su ace in e sec s wi h he en i onmen empe a u e
p o ile. The calcula ed PBLH om RSD was isually co ec ed o sol e he me hod e o s and mos ly ela ed o
he p esence o se e al empe a u e in e sion laye s. A de ailed explana ion o he me hod and how we applied i
o ou case s udy is p esen ed in Suppo ing In o ma ionS1 (Tex S3).
In his s udy, we also analyzed adon, which is a adioac i e and noble gas known o be a good a mosphe ic ace
(G ossi e al.,2012), o be e unde s and he e olu ion o he PBLH and o co obo a e he PBLH calcula ed om
he ceilome e obse a ions using he me hod p oposed by G i i hs e al.(2013). Hou ly a mosphe ic concen a-
ions o Rn we e measu ed du ing Oc obe 2020 using an A mosphe ic Radon MONi o (ARMON) a he Ba ce-
lona School o Indus ial Enginee ing s a ion (41°23′03″ N 2°07′01″E, 10m a.g.l) a he same si e ha adiosonde
and ceilome e da a we e eco ded and iden i ied wi h he label Radiosonde/Radon in Figu e1c. The moni o ing
was designed and buil by he Uni e si a Poli ècnica de Ca alunya as desc ibed by G ossi e al.(2012). Due o
COVID-19 es ic ions, no adon da a we e eco ded o May 2020 because he equipmen had o be shu down.
The es ima ions o PBLH using adiosonde and ceilome e we e also compa ed wi h PBLH simula ed using he
Wea he Resea ch and Fo ecas ing model (WRF). WRF simula ions we e pe o med o ob ain in o ma ion on
he main anspo p ocesses and he e ical mixing condi ions h oughou he AMB as desc ibed in Sec ion2.6.
2.5. WRF Simula ions o he U ban A mosphe e
The WRF 4.3 model (Skama ock e al.,2021) coupled wi h he mul ilaye u ban canopy scheme BEP-BEM
(Salamanca e al.,2010) was used in his s udy o simula e he u ban a mosphe e o e he AMB o be e unde -
s and he in luence o local wea he condi ions and PBL de elopmen on OCS concen a ions. The WRF con ig-
u a ion used o his s udy consis s o 3 wo-way nes ed domains wi h ho izon al esolu ions o 9, 3, and 1km
co e ing he Ibe ian Peninsula, he Ca alan e i o y, and he AMB, espec i ely, wi h 45 e ical laye s up o
100hPa (see Figu e S2 in Suppo ing In o ma ionS1). The physics pa ame e iza ion o he plane a y bounda y
laye is he Boulac scheme, which has been shown o be he mos sui able o esol e he u bulence in ensi y in
con ec i e si ua ions o he AMB (Segu a e al.,2021). We included 11 u ban local clima e zone (LCZ) clas-
si ica ions (S ewa & Oke,2012) o he inne mos domain and each had a speci ic alue o he mal, adia i e
and geome ic pa ame e s o he buildings and g ound, which a e used by he BEP-BEM o compu e he hea
and momen um luxes in u ban a eas (Gilabe e al.,2021; Ribei o e al.,2021; Yu & S einbe ge ,2011). We
conduc ed simula ions o May and Oc obe 2020 using me eo ological ini ial and bounda y condi ions om
ERA5 (Cope nicus,2023). Table S3 in Suppo ing In o ma ionS1 u he desc ibes he model cha ac e is ics
and expe imen al con igu a ions. The model simula ions we e alida ed using empe a u e, wind speed and
wind di ec ion obse a ions om 14 me eo ological s a ions o he Me eoca ne wo k (h ps://www.me eo.ca /
obse acions/xema).
2.6. FLEXPART Back T ajec o ies
FLEXPART back ajec o ies we e calcula ed o de e mine he p ecedence o ai sampled a he a ious si es
o es ablish whe he he ai mass in luence was local o egional. FLEXPART (FLEXible PARTicle dispe sion
model) is a Lag angian anspo and dispe sion model ha is used o calcula ing he long- ange and mesoscale
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dispe sion o ai pollu an s (S ohl e al.,2005). The FLEXPART e sion
adap ed o he WRF mesoscale model (B ioude e al.,2013) was used o
calcula e back ajec o ies o ai ace s om each o he sampling si es a
he sampling imes. The back ajec o ies we e compu ed om he ou pu o
he WRF model a he nes ed domain o 1km wi h 16 e ical le els om
0 o 2,000m a.g.l. Each back ajec o y was calcula ed o 24h a e he
sampling ime. The numbe o pa icles eleased o he a mosphe e in he
simula ion was 2,000. F om he 3D back ajec o ies, only he laye s om
0 o 100m abo e g ound le el we e used o he s udy o oo p in s, as i is
whe e he exchange among he land/ocean - a mosphe e akes place.
3. Resul s
3.1. OCS Sample Repea abili y and Accu acy in U ban En i onmen s
We pe o med a p ecision analysis o he GC measu emen s o lask-ai
samples acco ding o he me hods de eloped by Bel iso e  al. (2022) o
assess he epea abili y and accu acy o he OCS measu emen s in an u ban
en i onmen . Eigh pai s o lasks in o al we e selec ed andomly om he
May and Oc obe campaigns, and each lask was analyzed wice consecu-
i ely o OCS. The a e age di e ence be ween duplica ed measu emen s,
ha is, he in a lask di e ence, was 9.8±8.7 pp (median=8.2 pp , in e -
qua ile ange (IQR)=3.6–12.7 pp , n=16, 90 h pe cen ile=16.5 pp , 6.3%
o ou lie s), as shown in Figu e2a. I was sligh ly highe han ha epo ed
by Bel iso o samples collec ed in a u al a ea o e whea and apeseed
c ops (Bel iso e al.,2022), i.e., 9.3±7.2 pp (median=7.5 pp , in e qua ile
ange (IQR)=4.5–12.5 pp , n=58, 5.2% o ou lie s, bu in ha case, he
90 h pe cen ile was 19.5 pp ). Figu e2c shows ha among he 54 lasks (each
analyzed wice consecu i ely), ou displayed mixing a ios highe han he
90 h pe cen ile (i.e., 22.9 pp ), while he median and IQR o he in a lask
di e ence (7.7 pp and 3.3–12.1 pp , espec i ely) appea o be highly
consis en wi h he da a displayed in Figu e2a. Consis ency is also ound in
e ms o he p opo ion o abe an de e mina ions o OCS mixing a ios (i.e.,
6.3% (Figu es2a) and 7.4% (Figu e2c)). I was concluded ha he p ecision
o GC measu emen s o lask-ai samples emained unchanged o e he wo
campaigns and was consis en wi h ha epo ed by Bel iso e al.(2022).
The a e age di e ence be ween lasks o he same pai (i.e., he in e lask
di e ence) was also analyzed in a duplica e manne and was 10.1±14.0 pp
(median=4.8 pp , IQR=0.05–18.6 pp , n=8, no ou lie , Figu e2b). Hence, he in e lask di e ence du ing he
AMB s udy displayed highe a iabili y han ha o Bel iso e al.(2022), ha is, 5.5±4.5 pp (median=4.9 pp ,
IQR=2.2–8.0 pp , n=29, a 6.9% p opo ion o ou lie s was epo ed in ha s udy). The in e lask di e ence was
also assessed om a single analysis o he con en o each lask. The median, IQR and 90 h pe cen ile we e 12.1
pp , 4.3–22.5 pp and 45.0 pp , espec i ely, wi h n=95 (Figu e2d). We epo ed he exis ence o six ou lie s
(i.e., a p opo ion o 6.3%) exhibi ing in e lask di e ences highe han 45.0 pp and up o 360 pp . The in e lask
di e ence calcula ed om pai s o lasks each analyzed only once o OCS (Figu e2d) displays highe a iabili y
han ha om pai s o lasks analyzed wice consecu i ely (Figu e2b).
Consequen ly, al hough he ou ou lie s displayed in Figu e2c should ha e been disca ded, we a bi a ily ein-
co po a ed hose exhibi ing in a lask di e ences in he ange o 22.9 pp (i.e., he 90 h pe cen ile) and 36.8 pp .
Acco ding o Bel iso e al.(2022), da a om pai s o lasks exhibi ing in e lask di e ences highe han 14 pp
should be disca ded. No e ha his h eshold is app oxima ely wice ha se by Mon zka e al.(2007). Al hough
he in e lask di e ence calcula ed om pai s o lasks each analyzed only once o OCS could o igina e om
abe an da a (Figu e2d), nobody e e documen ed he high equency dis ibu ion o OCS mixing a ios nex
o po en ial u ban sou ces o ha gas. In o he wo ds, al hough lasks a e supposed o be simul aneously illed
in pai s, he p ocess o p essu iza ion o wo lasks connec ed in se ies could gene a e concen a ion g adien s
Figu e 2. Analysis p ecision o OCS measu emen s om lask-ai samples
collec ed in he AMB showing he 10 h, 25 h, median, 75 h and 90 h
pe cen iles. Panels (a, c) show Δ in e lask di e ences in OCS concen a ion
be ween wo consecu i e analyses o he con en o each lask (median o lask
1 minus ha o lask 2), whe eas (b, d) show he Δ in e lask di e ences in
OCS concen a ion be ween lasks o he same pai . The diamonds co espond
o he ou lie s (>90 h pe cen ile), which a e o e 23 pp in panel (c) and
o e 45 pp in (d). Ou lie s a e labeled acco ding o he loca ion and ime o
sample collec ion. The codes o each sampling si e a e si e, loca ion and ime
UTC (si es: Tib: Tibidabo, P a: P a , Pob: Poble Nou, Mon: Mon juic, Gui:
Guina dó; loca ion: U: Upwind, D: Donwind, T: Ta ge ). No e ha his o ical
wind da a was used o ha pu pose. The label colo s ep esen he campaigns
and co espond o ed o May and blue o Oc obe .
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e lec ing he he e ogeneous dis ibu ion o OCS nex o po en ial u ban sou ces o ha gas, in ou case samples
ook 10min o ill ou in se ies. In ligh o his possibili y, we decided o a bi a ily alida e he six ou lie s
epo ed in Figu e2d and in es iga e whe he in e lask di e ences highe han 45 pp would be si e dependen
o would esul om abe an da a.
3.2. E alua ion o WRF Simula ions
We an WRF BEP-BEM simula ions in May 2020 and Oc obe 2020 o ob ain high- esolu ion me eo ological
da a, a mosphe ic s abili y, and PBLH du ing he sampling pe iods. S a is ical analyses o he oo -mean-squa e
e o (RMSE), mean bias (MB) and co ela ion ac o (R) we e used o e alua e pe o mances o he model
compa ed wi h g ound-based me eo ological obse a ions om Me eoca (see Sec ion2.6). The nea -su ace
ela i e humidi y (RH), empe a u e (T) and wind speed (WS) s a is ical analyses a e displayed in Figu es S3
and S4 in Suppo ing In o ma ionS1 o campaigns in May and Oc obe , espec i ely. The e is an o e all good
pe o mance o he modeled RH, T and WS in compa ison wi h he obse a ions wi h an a e age e o o ±14%
o RH, ±1.7 o 1.9°C o T and ±1.65ms −1 o WS. This s a is ical analysis is a ailable in Table S4 in Suppo ing
In o ma ionS1.
Du ing he May campaign, he e we e p edominan no he ly winds om he no h om he 18 h un il he 21s ,
and he ci cula ion wea he ypes we e hyb id-cyclonic o cyclonic egimes, while he second hal (25 h h ough
he 28 h) was cha ac e ized by winds om he eas wi h a Medi e anean Sea ai mass in luence and ad en i e
egimes, wi h he excep ion o he 28 h, which was an icyclonic wi h a sou heas synop ic wind componen and
local ma i ime ai mass in luence. Du ing he Oc obe campaign, wes e ly and sou he ly winds cha ac e ized by
ad en i e ci cula ion wea he ypes p e ailed o mos o he pe iod wi h a cyclonic no h in luence and egional
con inen al ai mass in he i s 2days swi ching o a ma i ime in luence o he es o he campaign. Table1
summa izes hese wea he pa e ns o each day o he wo campaigns.
3.3. Plane a y Bounda y Laye Heigh Calcula ions and E alua ion
We had adiosonde and ceilome e da a o calcula e he PBLH in one loca ion o he Me opoli an A ea o
Ba celona, which we compa ed o he WRF-BEP BEM simula ed PBLH and es ablished ha he WRF model
pe o med easonably well in e ms o bounda y laye de elopmen . Fu he mo e, WRF-BEP BEM was alida ed
in e ms o empe a u e, wind di ec ion and speed, and ela i e humidi y. Thus, we we e able o employ WRF
me eo ological ou pu such as wind di ec ion and speed o explain he obse ed OCS concen a ions, mainly
in e m o hei accumula ion in o low o high PBLH and possible anspo pa e ns. Fo he same eason, he
a mosphe ic s abili y classes, based on he adon ace me hod, may gi e mo e in o ma ion on he a mosphe ic
episodes analyzed in o he s udy.
The PBLH om he WRF BEP-BEM simula ions was compa ed agains ceilome e es ima ions and adiosonde
obse a ions a 11:00 UTC o each day o he campaigns (see Figu e3). All da a ime se ies ollow he expec ed
PBLH diu nal pa e n wi h a apid g ow h o he PBLH du ing he mo ning, a maximum ha was eached a
midday, and a dec ease du ing he a e noon. The PBLH calcula ed by he WRF model is gene ally highe han
ha es ima ed by he ceilome e and adiosonde. Du ing he i s pe iod o May and i s days o Oc obe when
he e a e con inen al egional ai masses wi h p e ailing la ge-scale no he n winds, we no iced an impo an
di e ence be ween he ceilome e , adiosonde, and WRF alues in some cases up o 150m di e ence a 11
UTC. In his si ua ion, he la ge-scale winds domina e he bounda y-laye scales, which limi he capaci y o he
WRF model o es ima e he PBLH and leads o high unce ain y in he adiosonde obse a ions (S ull,1988).
The in e se co ela ion be ween a mosphe ic adon concen a ions and he ceilome e -based PBLH is uni o mly
main ained du ing he en i e Oc obe campaign as you can see in Figu e S5 in Suppo ing In o ma ionS1 how
PBLH a e a is maximum a 00:00 UTC while a mosphe ic adon concen a ion a e a i s lowes , and he opposi e
beha io is seen a ound 12:UTC (see Figu es S5 and S6 in Suppo ing In o ma ionS1), which u he indica es
an o e es ima ion o he PBLH by WRF du ing s ong wind e en s in ea ly Oc obe . The highes adon ac i i y
concen a ions (be ween 0.01 and 0.05 Bqm
−3) a e obse ed du ing nigh ime (21–2h ) when he PBLH eaches
i s minimum, whe eas he lowes alues (be ween 1 and 2Bqm
−3) a e obse ed du ing diu nal hou s (11–16h )
when
222Rn is dilu ed due o a well-de eloped PBL.
The o e es ima ed PBLH modeled alues in May a e consis en wi h an o e p edic ion o he 2m empe a u e
seen o a s a ion loca ed 1.2km om he adiosonde launching loca ion. In con as , be e ag eemen be ween
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he modeled and obse ed PBLH (bo h adiosonde and ceilome e ) is seen du ing he second hal o he May
campaign om he 25 h o 28 h o May (Figu e3a), when he eas e ly winds lead o a mo e s able a mosphe e.
Oc obe showed be e ag eemen o e all among he PBLH alues ob ained om he ceilome e , RSD and WRF
model due o highe a mosphe ic s abili y. The sou h-eas e ly weak winds gene ally lead o s able condi ions and
local scale dominance whe e he PBLH can be well es ima ed.
3.4. WRF-FLEXPART Foo p in s
FLEXPART simula ions showed ha he sampling campaign co e ed di e en synop ic si ua ions and di e en
ai mass o igins. Tex S4 in Suppo ing In o ma ionS1 shows ha du ing he May campaign, wo main di ec ions
we e obse ed as ollows: one coming om he no hwes ollowing he Llob ega Ri e basin (days 18, 19, and
21 o May) and ano he om he no heas wi h mo e sea in luence (days 20 and 25 o May) and some o he s
wi h mo e land in luence (such as days 26, 27, and 28 o May). Gene ally, he simula ion a 09:30 UTC shows
mo e sea o igin o he ai masses a i ing a sampling poin s han he simula ions a 07:00 UTC in acco dance
wi h he sea‒land b eeze egimes.
Du ing he Oc obe campaign, he ai masses mainly came om he no hwes ollowing he Llob ega Ri e
basin (days 15, 19, and 27 o Oc obe ), al hough a si ua ion wi h s ong winds coming om he sou h was
obse ed be ween he 20 h and 21s o Oc obe . A s onge b eeze egime is obse ed du ing his mon h wi h
gene al changes in he o igin o ai masses be ween he simula ions a 07:00 and 09:30 UTC.
Figu e 3. The ime se ies o modeled PBLH (blue line) oge he wi h he Ceilome e ( ed line) and he Radiosonde (blue
shade) o (a) May and (b) Oc obe campaigns. Shaded blue a eas indica e he PBLH using wo di e en de ini ions o i s
calcula ion. Ve ical lines co espond o he 4 a.m., 7 a.m., 9:30 a.m., and 11 a.m. UTC sampling imes on a daily basis.
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he no h whe e he ag icul u al ields a e loca ed. This indica es ha he OCS d awdown migh no be en i ely a
local e ec o ag icul u e bu could also be due o a mo e egional e ec o OCS aken up by soil and ege a ion
du ing he nigh all o e Ca alonia and hen ad ec ed by he land b eeze o e he AMB. Howe e , by 9:30 UTC,
OCS concen a ions inc eased (up o an ΔOCS o +116 o he downwind si e) when ai masses we e coming
om he u ban and po a eas and despi e PBLH de elopmen , which eached 1,380m ha mo ning. Du ing he
Oc obe campaign, sou hwes e ly winds p edomina ed bo h a 7:00 and 9:30 UTC, which b ough in ai masses
om he po and Ga à u ban a ea wi h high indus ial ac i i y esul ing in ΔOCS be ween +82 and +40 pp a
7:00 UTC. A 9:30 UTC, ΔOCS alues dec eased sligh ly and had less a iabili y anging om +49 o +55 pp ,
and his indica ed a mo e homogenous ai mix u e due o a mo e de eloped PBL, which inc eased om 21–84
o 380–519m o ha loca ion. Du ing Oc obe , ai anspo had much mo e in luence on he OCS budge han
he ag icul u al land use as i did du ing he May campaign when he ields we e in ull pho osyn he ic ac i i y.
The opposi e beha io was obse ed a he El P a ag icul u al si e, whe e a deep PBLH (1,200m) and egional
ai mass in luence occu ed in May, while a mo e s able si ua ion and lowe PBLH (691m) domina ed in Oc obe .
In gene al, he alues we e simila o he backg ound OCS o May wi h ΔOCS alues o +25, +37, and +22 pp
a 7:00 UTC and e en highe enhancemen s a 9:30 (+17, +44 and +173 pp , Figu e7b). FLEXPART back ajec-
o ies in May showed ai masses coming om he eas wi h longe esiden ial imes loca ed in he sea bu s ill
ecei ed in luence om he ai po and he po o Ba celona. Du ing he Oc obe campaign, El P a had highe
OCS enhancemen s a bo h sampling imes (ΔOCS o +70, +33, and +80 pp o 7:00 UTC; +7, +122, and +77
pp o 9:30 UTC), which, gi en he low PBLH, sugges s a local OCS sou ce. The FLEXPART showed ha ai
masses came om he eas indica ing ma ine in luence and/o om he po o Ba celona, whe e ac i i ies, such
as ai na iga ion and ma i ime a ic, had eco e ed 100% a e he lockdown. The lowe OCS concen a ions
in May compa ed o Oc obe highligh he signi ican sink o ag icul u e du ing he g owing season as was seen
o he Ga à loca ion.
Figu e 7. OCS enhancemen (Δ OCS) in pp calcula ed as he measu e o OCS minus backg ound OCS (484 pp o May
and 407 pp o Oc obe ) o each campaign a he wo u ban pa ks as ollows: (a) Ga à and (b) El P a . The black a ow
shows he wind di ec ion and speed measu ed on si e, and he absence o an a ow indica es ha he e was no wind blowing
a he momen o measu emen . A small map embedded in he lowe igh -hand co ne o each panel shows he esidence ime
on a loga i hmic scale o he ai masses a i ing a he sampling si e as de e mined wi h he FLEXPART model.
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To summa ize, he luc ua ions in OCS mixing a ios in u ban pa ks seemed o be mo e hea ily in luenced by
he di ec ion and in ensi y o he wind. In u ban o es s, he e was a clea educ ion o OCS compa ed o u ban
pa ks and buil en i onmen . Du ing he May campaign wi h he signi ican a ic educ ion due o he COVID
es ic ions, we saw a educ ion o OCS concen a ions compa ed o Oc obe - leading us o he conclusion ha
an h opogenic sou ces in u ban a eas a e signi ican . The pe i-u ban ag icul u al a eas did no show lowe alues
o OCS as was expec ed, mos likely due o he high in luence o he ai po and he seapo ha we e close by.
In gene al, i was di icul o de e mine i he e was any signi ican OCS d awdown by ege a ion, excep in
u ban o es ed a eas, while OCS mixing a ios well abo e backg ound le els e idenced signi ican u ban sou ces
o OCS.
4.2. Conside a ions o OCS S udies in U ban Ecosys ems
An h opogenic emissions a e he p ima y sou ce o OCS on a plane a y scale, ollowed by oceanic lux (Remaud
e al.,2023), hey a e signi ican a he local and u ban scales. In ou s udy, he peaks o OCS concen a ions we e
mos ly due o ai masses coming om he po o he ci y, as was he case o Mon juic in Oc obe o Ga à du ing
he May campaign, and eached alues o 665 pp o Mon juic and 600 pp o Ga à (up o ΔOCS o +258 and
+193 pp , espec i ely).
The e a e a ious po en ial sou ces o OCS in u ban a eas, such as he e osion o au omobile i es agains
asphal , ehicle exhaus umes, na u al gas combus ion and indus ial p ocesses including oil e ine ies and
aluminum p oduc ion (Yan e al.,2019). In ac , in hei in en o y, Yan e al. quan i ied he o al emissions in
2015 o China alone as 174GgSy
−1 wi h he highes con ibu ions coming om indus ial OCS emission
p ocesses (120GgSy
−1). In ha same s udy, he o al ehicle exhaus was esponsible o 3GgSy
−1, which
is app oxima ely hal o he yea ly global es ima e o 6GgSy
−1 gi en by Lee and B imblecombe(2016). The
la e s udy also indica ed ha he hea y uel oil used in ships is a signi ican sou ce o he OCS budge and
p oduces 30GgSy
−1. The AMB quali ies o all hese po en ial sou ces and i has a hea ily ansi ed ma ine
po ha also has a combined cycle gas u bine powe plan ha uns on na u al gas as well as an in ense use
o p i a e ehicles wi hin he ci y.
Figu e 7. (Con inued)
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Addi ionally, a b oad a ie y o sul ides a e p oduced by was ewa e whe e ola ile o ganic compounds (VOC)
such as me hane hiol (MeSH), dime hyl sul ide (DMS), ca bon disul ide (CS2), dime hyl disul ide(DMDS), dime-
hyl isul ide (DMTS) and OCS a e gene a ed in anoxic en i onmen s o sewe s (Lee & B imblecombe,2016),
and i has been no ed ha he mic obial ac i i y in hese anoxic sedimen s is closely linked o he p oduc ion
o OCS (Ki z e al.,2019). Sul ide emissions om u ban was ewa e ne wo ks a e equen ly de ec ed due o
hei bad odo as is he case o Ba celona (Eijo-Río e al.,2015) and Thessaloniki (Besis e al.,2021). In ou
s udy, he sampling si es o Sag ada Familia in Oc obe (ΔOCS o +150 pp ) and Poble Nou (ΔOCS o +50
pp ) concu wi h loca ions o a combined sewe sys em p e iously epo ed o ha e high peaks o H2S, which
indica ed a po en ial OCS sou ce om was ewa e . Un o una ely, cons aining his signal om o he po en ial
u ban sou ces was ou o he scope o he p esen s udy. Howe e , he obse a ions p o ided by ou measu emen
campaigns could se e o es ima e an h opogenic OCS sou ces when compa ed o simula ions o OCS mole
ac ions combined wi h emission in en o ies and plan up ake luxes as was ecen ly done o he Ne he lands
by Zanche a e al.(2023).
In e ms o ege a ed land uses, we ound one case o a signi ican OCS d awdown in ag icul u al si es du ing he
g owing season o May. In addi ion o pho osyn he ic up ake (Campbell e al.,2008,2017; Mon zka e al.,2007),
wa e logged soils ha e been epo ed o ac as sinks o OCS when plan ed wi h c ops (Yi e al.,2008). The
ag icul u al ields o he Llob ega basin a e mos ly i iga ed by inunda ion, which could u he in ensi y he
OCS up ake and explain he OCS d awdown a 7:00 UTC when pho osyn he ic ac i i y was high. We also ound
alues indica ing up ake du ing he g owing season in Collse ola Fo es , which is in ag eemen wi h o he s udies
e alua ing o es OCS up ake (Bel iso e al.,2016; Campbell e al.,2008,2017).
Finally, de e mining he in luence o land use on he o e all u ban OCS budge equi es a eliable backg ound
measu emen . In gene al, backg ound le els o OCS a e associa ed wi h ai masses coming om he sea because
he s abili y p o ided by oceans esul s in cons an OCS concen a ions, a leas a a seasonal scale (Mon zka
e al.,2007), as was he case o San F ancisco (Villalba e al.,2021). Howe e , his is no applicable o he AMB
because he con ec ion egime is qui e peculia . The AMB has a unique land‒sea ai mass exchange in which
sea b eezes unde speci ic condi ions do no b ing new ai masses bu a he ecycle ai masses ha o igina ed
o e he u ban a ea, howe e , a deepe esea ch should be done in his ega d, since ma ine con ibu ion canno
be neglec ed. This ype o p ocess has been obse ed by Jaén e al.(2021), who desc ibed how ozone plumes
s ay o e he sho e due o ad ec i e p ocesses du ing hea episodes such as hea wa es. The he mal componen
o con ec i e p ocesses c ea ing episodes o ai eci cula ion on he Spanish eas e n coas has also been docu-
men ed by Millán e al.(2000), whe e hey ou line how he sea b eeze can a o he o ma ion o laye s o s a -
i ied ai ese oi s in heigh s whe e compounds accumula e ha can la e e u n o he land. This pa icula sea
b eeze ci cula ion cons ic s local en ila ion and exace ba es he accumula ion o an h opogenic gases emi ed
in he AMB.
5. Conclusions
We pe o med wo measu emen campaigns o OCS mixing a ios in he Me opoli an A ea o Ba celona (AMB)
o explo e o wha ex en di e en u ban land uses can ha e an impac on he OCS mixing a ios measu ed on
lask samples ega ding a pa icula u ban clima e, geog aphy, and opog aphy o AMB. Ai samples we e aken
a loca ions ep esen ing ou di e en land uses as ollows: u ban pa ks, o es s, ag icul u al ields and impe i-
ous u ban landscapes.
Based on he in e lask compa ison desc ibed in 2.3, we de e mined ha he OCS measu emen unce ain y can
be as high as +53 pp , which e lec s ha nea -su ace measu emen s in u ban he e ogeneous en i onmen s esul
in highe unce ain ies han in homogenous u al en i onmen s. We also compa ed a e age OCS concen a ions
±σ wi h alues obse ed om ICOS- LSCE in Gi -su -Y e e (GIF), which we e aken a he same momen as
ou campaign (Figu e S3 in Suppo ing In o ma ionS1). We obse ed how mean OCS concen a ions and σ in
he AMB we e sys ema ically highe han in GIF, which sugges s ha an h opogenic emissions could a ec he
inc ease in unce ain y.
The abili y o cap u e a pho osyn he ic signal appea s weak in ege a ed a eas wi hin he ci y, such as pa ks, and
is elega ed o o es s and pe i-u ban ag icul u al a eas. U ban pa ks showed alues signi ican ly highe han he
es ablished backg ound alue, bo h in May (i.e., up o +144 pp ) and in Oc obe (i.e., up o +150 pp ), which
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shows he in luence o an h opogenic sou ces, possibly om he po and he ci y cen e , which masks he possi-
bili y o cap u ing he signal om he ege a ion. The u ban o es sugges ed OCS up ake alues up o −33 pp ,
which indica es a signi ican pho osyn hesis sink in dense ege a ion masses e en wi hin ci y limi s.
The u ban a ea showed a a ie y o signals om almos neu al o abo e he backg ound alue, which sugges s
nea by emission sou ces. In ou case, we ound he explana ion o some p ocess alues ha may be aligned wi h
u ban a ic bu abo e all wi h he indus ial ac i i y o he po and ai po (e.g., high OCS alues in Mon juic
when he wind came di ec ly om he po ). We can also hink o o he biogenic p ocesses ha p oduce OCS
p ocesses linked o human ac i i y on u ban land such as he was e sys em. These p ocesses should be s udied
in mo e de ail in u u e wo ks. We ha e no been able o cap u e an e ec o u ban ege a ion on OCS up ake;
ins ead, he pe i-u ban a ea o ag icul u e and o es s may ha e mo e impo an oles in he OCS dynamics in
ci ies.
Las , ag icul u al a eas showed a clea d awdown du ing he g owing season o he loca ion o Ga à, whe e we
we e able o disca d egional in luences and in ense ai mixing. OCS enhancemen s in Oc obe e lec he loss o
pho osyn he ic up ake and he e u n o business as usual a ic and nea by ai po and po ac i i ies.
O e all, he a iabili y o OCS in he u ban ecosys em was highe han we expec ed. The URBAG campaigns o
OCS measu emen s showed e idence ha he use o OCS as a ace gas o de e mine he con ibu ion o he u ban
biosphe e o he CO2 budge is a complica ed ask and ha he ege a ion signal is di icul o de ec because local
an h opogenic ac i i ies ha e a signi ican in luence. The u ban ecosys em is complex in e ms o land up ake,
ma ine emissions, and an h opogenic emissions om he ci y po , and s ongly impac s he spa ial- empo al
dis ibu ion o OCS in he AMB and impedes a clea cons ain o he biosphe e signal.
Da a A ailabili y S a emen
The da a acqui ed du ing he URBAG measu emen campaigns used o he analysis o land in luence in his
s udy a e a ailable a ZENODO ia h ps://doi.o g/10.5281/zenodo.8072833 wi h C ea i e Commons A ibu ion
4.0 In e na ional license (Villalba, G.,2023).
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Acknowledgmen s
This wo k has been made possible hanks
o he inancial suppo o he Eu opean
Resea ch Council (ERC) Consolida o
p ojec : In eg a ed Sys em Analysis
o U ban Vege a ion and Ag icul u e
(818002-URBAG), he Spanish Minis y
o Science, Inno a ion and Uni e si-
ies, h ough he “Ma ia de Maez u”
p og amme o Uni s o Excellence
(CEX2019-000940-M), and he unding
and ecogni ion awa ded o he esea ch
g oup Sos enip a (2021 SGR 00734) by
he Depa men o Resea ch and Uni e -
si ies o he Gene ali a de Ca alunya.
This wo k also has been g an ed by he
Spanish Minis y o Science and Inno a-
ion MCIN AEI/10.13039/501100011033
unde con ac PID2020-113614RB-C21,
by he Spanish Go e nmen unde G an
PRE2018-085425 and by he Ca a-
lan Go e nmen unde con ac 2021
SGR 00574. The au ho s acknowledge
he compu e esou ces a PICASSO
and he echnical suppo p o ided
by he Uni e sidad de Málaga (G an
RES-AECT-2020-2-0004).
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