GEOPHYSICAL

RESEARCH
LETTERS,VOL.21,NO. 7, PAGES561-564,APRIL 1, 1994

Atmosphereberyllium-7 concentrationsover the Pacific

Ocean

Mitsuo Uematsux and Robert A. Duce2

Graduate
Schoolof Oceanography,
University
of RhodeIsland,Narragansett,
RhodeIsland

JosephM. Prospero
Rosenstiel
Schoolof MarineandAtmospheric
Science,
University
of Miami,Miami,Florida

Abstract. Atmospheric7Be is usedas a tracerof strato- depositionto the Pacific Ocean,we analyzedaerosolsamples
sphericanduppertropospheric air, but mostmeasurements of collectedfrom the Pacific islandsnetwork initiatedas a part of
7Bein surfaceair havebeenrestricted to continental
regions. the Sea-Air Exchange (SEAREX) program. Among the
We reportherethe extensivetemporaland arealdistributionof stationsof thenetwork,we couldmeasure thesamples for 7Be
atmosphericaerosol7Be concentrationin themarineboundary from the nine island stations:Midway, Oahu, and Enewetak in
layer. Measurements of 7Behavebeencarriedout for the the North Pacific; Nauru, Funafuti, American Samoa,
weekly filter samplescollected at the Pacific island stations Rarotonga, New Caledonia, and Norfolk in the South Pacific
where are located between 30 ø N and 30 ø S in 1981 and 1985. (see Figure 1). All stationsare locatedbetween30øN and 30øS.
High annual mean concentrationsamong the stations are In this paper,we discussthe resultsof the 7Be analysisof
observedat latitudebetween20ø and 30ø in bothhemispheres. aerosolsamplescollected at Midway and Oahu in 1981 and the
There is little seasonal variation of 7Be at the nine stations. nine stations in 1985. Studies of other substances for these
The lowest concentrationsare found in the equatorialregion samples have been published in elsewhere [e.g., Uematsu et
due to relatively little subsidenceof the air from the upper al., 1983; Prosperoet al., 1985; Savoie et al., 1989]
layer in this area and high precipitation within the ITCZ
(intertropicalconvergencezone) resultingin rapid removal of
the aerosolcontainingthe 7Be. The significantcorrelation Methods
between the 7Be concentrations and the nitrate concentrations
at the stationsin the North Pacific supportsthe assumption Atmospheric Sampling
that nitrate is transported from continental sources to the
Each samplingstationwas set up on the climatologically-
marine boundary layer through the free troposphereby the
westerlies.
determined windward shoreof the island. Weekly aerosolsam-
ples were collectedby using high-volume air samplingsystem
and Whattnan-4! filter (20 x 25 cm) at air flow rate of about
1.1 m 3 min '•.
Introduction Various filter materials have been used for collection of
aerosolparticlescontaining
7Be. We usedWhatman
4! filters,
Beryllium-7 is a natural radionuclide(53.3 day half-life)
but Microsorban filters [Feely et al., 1981], glassfiber filters
produced by cosmicraysin theupperatmosphere. 7Berapidly [Feely et al., 1981], and IPC filters [Dutkiewiez and Husain,
attachesto aerosolparticlesin the atmosphereand thuspro- 1985; Crecelius, 198!] have also been used.
videsa useful tool for the studyof aerosolbehaviorand for To testtheefficiencyof Whatman41 filtersfor 7Becollec-
identifyingsubstances transportedfrom the uppertroposphere tion, we collected two sets of aerosol samples using a
and the lower stratosphere(such as bomb fallout debris, vol- Whatman 41 filter followed by a glassfiber filter. These sam-
canic components injected into stratosphere,ozone and ples were collected at a coastalmarine site in Narragansett,
certain nitrogen species) into the planetary boundarylayer RhodeIsland. More than95 percentof thetotal7Be activity
[Dutldewicz and Husain, 1979; Dutkiewicz and Husain, 1985;
was detectedon the top Whatman 41 filter, with only a small
Lee et al., 1985]. Recently7Beis usedfor a testof the wet fraction of the activity on the glassfiber filter. Our studyindi-
scavengingparameterizationin a global climate simulation cates that Whatman 41 filters are also a suitable collection
model[Brost et al., 1991]. Because7Be concentrationalso
matrixfor aerosols
containing 7Bein themarineatmosphere.
vary by wet scavengingand mixing within the troposphere.
In orderto characterizethe temporaland arealdistribution
Determination of 7B e
of 7Be particlesin the marine boundarylayer and its
An eighthsectionof the filter was compressedinto a pellet
1Now
atHokkaido
Tokai
University,
Sapporo,
Japan. andplaceddirectlyon a 25% Ge(Li) detectorcoupledto a multi-
2Now
atTexas
A& M University,
College
Station,
Texas. channel
analyzer.The7Begammaray activitywasmeasured
at
477.6 keV. The overall uncertainty in the measuredatmo-
sphericconcentrationwas lessthan 15%. We have alsointer-
Copyright1994by the AmericanGeophysical
Union. calibrated our 7Be measurements with the Environmental
MeasurementsLaboratory (EML) of the U.S. Departmentof
Papernumber94GL00391 Energy.The 7Beconcentrations
wereagreedeachotherwithin
0094-8534/94/94GL-0039 !503.00 10 percent.
561
562 UEMATSU ET AL.: BERYLLIUM-7 OVER THE PACIFIC

Table 1. Summaryof Resultsand Estimationsfor 7Be

in the Network, 1985

30ø MeanAtmos. •'alculate

d '"'Observed
-
Station Lat. 7BeConc. Ppt• WetFlux Tot.Flux#
(mBqm'3) (my4) (kBqm'2y '1)
Midway 28øN 2.9 ñ 1.9' 1.10 1.3
(3.3 ñ •.3)
Oahu 21øN 3.1 ñ 1.5 0.65 0.9 1.0
(2.5 + 0.7)
Enewetak 1 IøN 1.7 ñ 0.6 1.47 1.0 1.2
Natru IøS 1.4 ñ 0.4 2.06 1.2 0.4
30'
Funafuti 9øS 1.6 ñ 0.5 3.54 2.4 1.2
Samoa 14øS 2.3 ñ 1.5 3.52 3.4 2.0
Rarotonga 21øS 3.0 ñ 2.0 2.06 2.6 2.6
New Caledonia 22øS 3.1 ñ 1.1 2.31 3.0 1.4
Norfolk 29øS 2.7 ñ 1.0 1.33 1.5 1.4
Figure 1. Samplingstationsfor the ?Be measurements
in
the SEAREX North and South Pacific Networks. The meanof 1981-82wasin the parenthesis.
* Standarddeviationof the samples.
!Taylor (1973). # Young and Silker (1980).
Results and Discussion
The mean concentrations of 7Be in 1981 and 1985 at each
Typical7Beconcentrations
in thelowerstratosphere
are-170
mBq m-• [DutkiewiczandHusain,1985]. Therefore,only a
station are presented in Table 1. Some of the 1981 filter
smallcontribution
of 7Befromthe lowerstratosphere
and/or
samples
werecombined
for thecounting
of 7Beactivity. upper tropospherewould be sufficient to produce a large
change
in the7Beconcentration
in surfaceair of marinebound-
Areal and Seasonal Variation
try layer. In contrast,the weeklyvaluesat Nauruarefairly low
The lowest annual mean concentrationat any site is 1.4 and constantthroughoutthe year, with a 30 percentcoefficient
mBqm'3,observedatNauruneartheequator.Theannual mean of variation (Figure 2). This is probably due to relatively
7Beconcentrations
arehighat latitudebetween 20ø and30ø in little stratospheric intrusionand descendingair from the upper
both hemispheres. These higher mean concentrationsare troposphereat this low latitude site coupled with a high
found at Midway and Oahu in the North Pacific and at precipitation rate, andthusrapidaerosol7Beremoval,within
Rarotonga,New Caledonia, and Norfolk in the South Pacific. the ITCZ.
The difference between the mean concentrations at these sites
and at N auruis significantat the 95 percentconfidencelevel as Atmospheric Deposition Rate of 7Be to the Ocean
determinedby a multiple comparisonmethod. This trend is Table 1.alsopresents
thecalculated
wet fluxesof 7Beto the
consistent with the latitudinal distribution of 7Be observed at oceansurfaceusing the mean annualprecipitationat eachsite
continentalstationsreportedby the EML. The maximum con- [Taylor, 1973], the observed mean atmospheric
centrations were observed at midlatitudes over North America concentration, and a scavenging ratio for the aerosol
[Viezee and Singh, 1980; Feely etal., 1981]. particles. A scavengingratio (the ratio of the concentration
There is little longitudinalvariation found in thesedata,as of a substance in rain to its concentration
in the atmosphere)
indicatedby comparingthe 7Be concentrations at New of 500 was usedfor aerosolover the ocean[Buat-Menardand
Caledoniaand at Rarotonga. Both thesesitesare locatednear Duce, 1986; Arimoto et al., 1985]. It is convenient to
20øS (3500 km apart) and have similar annualprecipitation estimatea wet flux for atmosphericparticles over remote
amounts(Table 1). It shouldbe notedthat the mean7Be con- marine regions by using the scavengingratio when the
centration of 2.4 mBqm'3 observed at all ninenetworksitesin concentrationin rain is not available [Uematsuet al., 1983;
thisstudyis -35 percentlessthanthemeanof-3.7 mBqm-3at Arimotoetal., 1985;Buat-MenardandDuce, 1986].
the continental sites [Dutldewicz and Husain, 1985]. This is Using a differentapproach,total depositionratesof 7Be
consistent with the result that the 7Be concentration in several into the Pacific and AtlanticOceanshavebeen determined by
air filter samplescollected on two cruisesin the Pacific aver- Young andSilker (1980) from measurements of the 7Be inven-
aged 70 percentof concentrationpredictedfrom the continen- tory in the respectivemarine water columns. The "observed"
tal measurements[Young and Silker, 1980]. This is presum- total depositionrates at the network stationspresentedin
ably due to differences between the oceansand continentsin Table 1 are obtainedfrom the 7Be inventorymap in their
precipitation scavenging and vertical mixing [Young and paper. In the remotemarineatmosphere, wet depositionis an
Silker, 1980]. importantremovalprocessfor submicrometer aerosols,prob-
There were no pronouncedseasonalpatternsat any of the ably accountingfor 50 - 80 percentof the total removalof
network stationsduring 1985 (Figure 2). However,large vari- these particles [Arimoto etal., 1985]. The calculated wet
ationsin atmospheric
7Bewere observedfrom weekto week, depositionrates using the scavengingratio model generally
exceptat the stationsnear the equator. The coefficientof vari- agree with Young and Silker's total fluxes within a factor of
ation is over 70 percent at Midway, Samoaand Rarotongain two. The primaryexceptionis that our calculateddeposition
1985. The highestweekly concentrationat any of the sites at Nauru is a factor of threehigherthan their estimatefor the
was 11.2 mBq m'3 at Rarotonga
in early May (Figure2). area near Nauru, where the 7Be concentrationin the surface
 UEMATSU ET AL.: BERYLLIUM-7 OVER THE PACIFIC 563

MIDWAY
(28øN)
atmospheric
concentrations
of 7Bearesimilarin thetwohemi-
.

spheres,but the removal rates are apparentlygreaterin the

South Pacific. It must be a result of either a longitudinally
nonuniform removal rate in different regions of the South
Pacificor higherinputrateof 7Beto themarineboundary
layer
in the southernhemisphere.
The imbalanceof the 7Be flux betweenthe tropicalNorth
and SouthPacific may be relatedto the nonuniformdistribu-
S "'-'0 '"N "O 'd 'F 'M"•'"A'M 'd ' J 'A 'S '0 '
A 8.6
tion of annualprecipitationover the Pacific Ocean. In the
I

•øN)
central North.Pacific, the annualprecipitation[Taylor, 1973]
varies less with longitudethan with latitude between0ø and
30øN(70- 500 cm yr'•). In contrast, thereis a highprecipita-
tion area in the western and central South Pacific (120- 500
cm yr-•) and a low precipitationarea in the easternSouth
Pacific(<50 cm yr't). In the low precipitation
area,minimal
wet removalmay causerelativelyhigh 7Be concentratiot/s
within the surface air. The 7Be enriched air over the eartorn
J 'F""'M 'A 'M 'J 'J 'A 'S""O 'N .......
D 'd SouthPacificmay be transported
to the centralSouthPacific
by the southeasttrade winds,wherethe aerosolparticlescould
•uRu (•os)
beremoved
byrainmoreefficiently.
In fact,atmospheric
7Be
concentrationsat a near-coastalsite at Lima, Peru [Feely et al.,
1981] where the annualprecipitationis only -3 cm yr't
(12øS), are approximatelytwice as high as thoseat American
Samoa (14øS).
Relationship between 7Be and nitrate in marine
boundary layer
',.) • F 'M'"'A 'M ' J 'J 'A 'S '0 'N "D 'J
According to Prospero and Savoie [1989], 40- 70% of
nitrate in the marine boundary layer of the Pacific Ocean is
from the continentalsourceswhich are predominantlyanthro-
pogenic. In addition, a high correlation betweenthe nitrate
concentrations and the concentrations of 2•øpb was observed at
American Samoa, but there was no correlation between the
nitrate concentrations
and the concentrations
of •3e.
Therefore, they concludedthat the stratosphereand uppertro-
posphereare probably not the major sourcesfor nitrate over
the tropical South Pacific [Savoie et al., 1989].
In the central North Pacific, a significant correlation(n =
NORFOLK(29øS)
33, r= 0.84) betweenthe nitrateconcentrations[Prospero
.
et
al., 1985] and the concentrationof *Be were found at the
Midway station during the year of !981 (see Figure 3). A
similar correlation (n = 44, r = 0.83) was observedat Oahu sta-
tion during the observed periods. This relation does not,

1200
J F M A M J J A S O N D

1000'
Figure2. Temporalvariationof weeklyatmospheric'
7Be
concentrationsat the stationsbetween 30øN and 30øS during
the period from January 1985 to January 1986, except the . 8o0,
Midway station(1981-1982). • 600' ß

water was close to detectionlimit and nearly uniform through 1• 400-

themixing layer depthof 100 m in the watercolumn. Thus
200'
theircalculated?Beinventoryin oceanicsurfacewatersmay
havehigh uncertainties
in this region.
The marineboundarylayer?Be concentration
is nearly
symmetrical in the Pacific atmosphere in the two
Be-7 (mBq/SCM)
hemispheres.
However,
ourestimated
wetfluxes
attheSouth
Pacificstationsaretwiceashighasthoseat theNorthPacific Figure3. The relationshipsbetweennitrateand7Beat the
stations.Thistrendof higher?Bedepositionoverthewestern Midway stationin !98! and at the Oahe stationin !981 and
andcentralSouthPacificcanalsobe seenon the?Beinventory 1985. Somesamplesare combinedto measurethe 7Be 0

mappresentedby Young and Silker [1980]. In otherwords, activity.

564 UEMATSU ET AL.' BERYLLIUM-7 OVER THE PACIFIC

however, imply that the sourcesof the nitrate are the strato- elementsat the EnewetakAtoll: 2 transportto the oceansby wet and
sphere. Because,such a high correlationwas not observedat drydeposition, J. Geophys.Res.,90,2391-2408,1985.
the stationsin the South Pacific. The high nitrate concentra- Brost,R.A., J. Feichter,M. Heimann,Three-Dimensional Simulationof
tions in the North Pacific stations are believed to be
7Be in a GlobalClimateModel, J. Geophys.Res.96, 22423-22445,
1991.
originated anthropogenicsources. There is a pronounced Buat-Menard,P., and R. A. Duce, Precipitationscavengingof aerosol
transportpattern of continentalsubstances from Asia to the particlesoverremote marine regions,
Nature,321,508-510,1986.
centralNorth Pacific region [Uematsuet al., 1983]. The air Crecelius,E. A., Predictionof marineatmospheredepositionratesusing
parcelsare lifted by frontal or convectiveprocessesto high total7Bedeposition velocities,
Atmos.Environ.,
15,579-582, 1981.
elevations (400- 500 hPa) over Asia and transported to Dutkiewicz,V. A., and L. Husain,Determination of stratospheric
ozone
eastwardby the westerlies,then descendedgraduallyas they atground levelusing7Be/Ozone Rations,
Geophys. Res.Lett.,6, 171-
pass aroundthe anticycloneover the centralNorth Pacific 174, 1979.
region [Merrill et al., 1989]. By aircraftobservation
over the Dutkiewicz,V. A., and L. Husain,Stratospheric
andtropospheric
com-
Northeast Pacific [Andteac et al., 1988], the higher porteros
of Be-7in surfaceAir, J. Geophys.
Res.,90, 5783-5788,
1985.
concentrations of nitrate and nss sulfate were found in the free
Fee!y,H., L. Toonkel,andR. Larsen,AnnualReportof theSurface Air
tropospherewhere transportfrom Asia dominated. A few
Sampling Program, Rep.EML-395,appendix, Environ.Mens.Lab.,
episodiceventsof high ?Be concentrations at the South U.S. Dep.Energy,New York, 1981.
Pacific stations (such as the Rarotonga station) might be John,W., andG. Reischl,Measurements of thefiltrationefficiencies
of
associatedwith stratosphericintrusionsbecausethe nitrate selected filtertypes,Atoms.Erwiron.,12,2015-2019,1978.
concentrations did not covaryat thosetimes. Therefore,7Be Lee,S.C., A. i. Saleh,A.D. Banavali,L. Jonooby, andP. K. Kuroda,
can be usedfor a tracer of descendingair massfrom the free Beryllium-7deposition at Fayetteville,
Arkansas, andexcess polo-
troposphererather than the stratosphereto the marine nium-210from the 1980eruptionof Mr. St. Helens,Geochem.
J., 19,
boundarylayer with a few exceptions. 317-322, 1985.
Merrill, J.T., M. Uematsu,R. Bleck, Meteorologicalanalysisof long
rangetransportof mineralaerosolsover the North Pacific J.
Conclusions
Geophys. Res.94, 8584-8598,1989.
Measurements
of 7Befor the filter samples
collectedfrom Prospero,
J. M., D.L. Savoie,R.T. Nees,Particulate
sulfateandnitratein
the boundarylayer overthe North PacificOcean, J. Geophys.Res.
the island stationsover the Pacific Ocean lead to the following
90, 10586-10596,1985.
conclusions:
Prospero,
J. M., D.L. Savoie,Effectof continental
sources
on nitrate
1. Higher concentrationsare observedat latitude between concentrations
over the Pacific ocean. Nature, 339, 687-689, 1989.
20ø and 30ø in both hemispheres.There is little seasonalvari- Savoie, D.L., J.M. Prospero,E.S. Saltzman,Non-sea-saltsulfateand
ation of 7Be over the Pacific Ocean. nitrate in trade wind aerosolsat Barbados:evidencefor long-range
2. The lowest concentrations are found in the equatorial transport.J. Geophys. Res.94,5069-5080,1989.
region due to relatively little air descendingin this area andTaylor,R.C.,An atlasof Pacificislandsrainfall,Data Rep.25, HIG-73-
high precipitationwithin the !TCZ resultingin rapid removal 9, HawaiiInst.Geophys. Univ.Hawaii,Honolulu,HI, 1973.
of the aerosolcontainingthe 7Be. Uematsu,M., R. A. Duce,J. M. Prospero, L. Q. Chen,J. T. Merrill, and
3. The imbalance of the 7Be flux between the North and R. L. McDonald,Transportof mineralaerosolfrom Asia over the
NorthPacificOcean,J. Geophys. Res.,88, 5343-5352, 1983.
SouthPacific may be related to the nonuniformdistributionof
Viezee,W., andH. B. Singh,The distribution of Beryllium-7in thetro-
annualprecipitationover the Pacific Ocean. posphere:implicationson stratospheric/tropospheric air exchange,
4. The significantcorrelationbetweenthe 7Be concentra- Geophys.Res.Lett.,7, 805-808,1980.
tions and the nitrate concentrations at the stations in the
Young,J. A., andW. B. Silker,Aerosoldeposition velocitieson the
North Pacific suggeststhat nitrate is bringingdown from the Pacificand Atlantic Oceanscalculatedfrom 7Be measurements,
free troposphere
to the marineboundarylayer. Earth Planet. Sci. Lett., 50, 92-104, 1980.

Acknowledgments.This researchwas supportedby NSF grantsOCE

R. A. Duce, Collegeof Geosciences
and Maritime Studies,TexasA
84-05605, OCE 84-05609, ATM 83-11694, and ATM 83-11335 as a
& M University, College Station, TX 77843-3148. (e-mail:
part of the SEAREX Programand the North PacificTropospheric rduce@ocean.tamu.edu)
Transportand DepositionStudy. We thank to R. Larsenat EML
J. M. Prospero,Division of Marne and AtmosphericChemistry,
providingusefulcomments
for theanalysis.
RosenstielSchoolof Marine and AtmosphericScience,Universityof
Miami,Miami,FL 33149. (e-mail:jprospero@rsmas.miami.edu)
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November
29, 1993;revisedFebruary1, 1994;accepted
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