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Gas isotopic signatures (He, C, and Ar) in the Lake Kivu region
(western branch of the East African rift system):
Geodynamic and volcanological implications
D. Tedesco,1,2 F. Tassi,3,4 O. Vaselli,1,4 R. J. Poreda,5 T. Darrah,5 E. Cuoco,2 and M. M. Yalire6
Received 24 November 2008; revised 28 August 2009; accepted 20 October 2009; published 29 January 2010.
[1] On 17 January 2002, the city of Goma was partly destroyed by two of the several lava
flows erupted from a roughly N-S oriented fracture system opened along the southern flank
of Mount Nyiragongo (Democratic Republic of Congo), in the western branch of the East
African rift system. A humanitarian and scientific response was promptly organized by
international, governmental, and nongovernmental agencies coordinated by the United
Nations and the European Union. Among the different scientific projects undertaken to
study the mechanisms triggering this and possible future eruptions, we focused on the
isotopic (He, C, and Ar) analysis of the magmatic-hydrothermal and cold gas discharges
related to the Nyiragongo volcanic system, the Kivu and Virunga region. The studied area
includes the Nyiragongo volcano, its surroundings, and peripheral areas inside and outside
the rift. They have been subdivided into seven regions characterized by distinct 3He/4He
(expressed as R/Rair) ratios and/or d13C-CO2 values. The Nyiragongo summit crater
fumaroles, whose R/Rair and d 13C-CO2 values are up to 8.73 and from 3.5% to 4.0%
VPDB, respectively, show a clear mantle, mid-ocean ridge basalt (MORB)-like
contribution. Similar mantle-like He isotopic values (6.5–8.3 R/Rair) are also found in
CO2-rich gas emanations (mazukus) along the northern shoreline of Lake Kivu main
basin, whereas the 13dC-CO2 values range from 5.3% to 6.8% VPDB. The mantle
influence progressively decreases in (1) dissolved gases of Lake Kivu (2.6–5.5 R/Rair)
and (2) the distal gas discharges within and outside the two sides of the rift (from 0.1
to 1.7 R/Rair). Similarly, d 13C-CO2 ratios of the peripheral gas emissions are lighter
(from 5.9% to 11.6% VPDB) than those of the crater fumaroles. Therefore, the
spatial distribution of He and C signatures in the Lake Kivu region is mainly produced
by mixing of mantle-related (e.g., Nyiragongo crater fumaroles and/or mazukus gases)
and crustal-related (e.g., gas discharges in the Archean craton) fluids. The CO2/3He
ratio (up to 10 1010) is 1 order of magnitude higher than those found in MORB,
and it is due to the increasing solubility of CO2 in the foiditic magma feeding the
Nyiragongo volcano. However, the exceptionally high 40Ar*/4He ratio (up to 8.7) of
the Nyiragongo crater fumaroles may be related to the difference between He and Ar
solubility in the magmatic source. The results of the present investigation suggest that
in this area the uprising of mantle-originated f luids seems strongly controlled by
regional tectonics in relation to the geodynamic assessment of the rift. These fluids are
mainly localized in a relatively small zone between Lake Kivu and Nyiragongo
volcano, with important implications in terms of volcanic activity.
Citation: Tedesco, D., F. Tassi, O. Vaselli, R. J. Poreda, T. Darrah, E. Cuoco, and M. M. Yalire (2010), Gas isotopic signatures
(He, C, and Ar) in the Lake Kivu region (western branch of the East African rift system): Geodynamic and volcanological implications,
J. Geophys. Res., 115, B01205, doi:10.1029/2008JB006227.
1
Office for the Coordination of Humanitarian Affairs, United Nations,
Geneva, Switzerland.
2
1. Introduction
Environmental Sciences Department, Naples 2 University, Caserta,
Italy. [2] The western branch (WB) of the East African rift
3
Istituto di Geologia Ambientale e GeoIngegneria, CNR, Rome, Italy. system (EARS), the latter including the Ethiopian and
4
Earth Sciences Department, University of Florence, Florence, Italy. Kenya branches (Figure 1), is an 3000 km long seismi-
5
Environmental and Earth Sciences Department, Rochester University,
Rochester, New York, USA. cally active corridor that borders the mechanically strong
6
Goma Volcano Observatory, Goma, Democratic Republic of Congo. [e.g., Petit and Ebinger, 2000] and thick [e.g., Ritsema et
al., 1998] Archaean Tanzania craton. The eruptive activity
Copyright 2010 by the American Geophysical Union. of the WB is substantially lower than that of the volcanic
0148-0227/10/2008JB006227$09.00
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
Figure 1. Map of the Kivu volcanic province with major tectonic lines and locations of gas sampling
sites.
systems located in the eastern branch of the EARS and can whose eight main EW-oriented volcanic edifices [e.g.,
be related to four main volcanic districts: (1) the Toro- Mavonga, 2007] can be grouped as follows: (1) Muhavura
Ankole region (western Uganda), (2) the Virunga, (3) the (4127 m above sea level (asl)), Gahunga (3474 m asl) and
Kivu provinces (at the border between the Democratic Sabinyo (3647 m asl) (eastern group); (2) Visoke (3911 m asl),
Republic of Congo with Uganda, Rwanda, and Burundi), Karisimbi (4506 m asl), and Mikeno (4437 m asl) (central
and (4) the Rungwe volcanic field (southwestern Tanzania). group); and (3) Nyiragongo (3470 m asl) and Nyamuragira
[3] The dominant volcanism consists of silica-undersatu- (3056 m asl) (western group).
rated mafic products and includes ultrapotassic, hypersodic, [4] With the exception of the short-lived eruption of
and carbonatitic compositions [Furman, 2007, and referen- Visoke in 1956, the westernmost volcanoes have had
ces therein]. Presently, the volcanic activity is concentrated frequent historical activity. The Nyamuragira volcano is
in the middle Miocene Virunga Volcanic Province (VVP), characterized by flank eruptions, consisting of frequent
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
K-rich Hawaiian-type lava flows [e.g., Hayashi et al., 1992], Tolstikhin, 1984]). The R/Rair values of the mid-ocean ridge
although an active lava lake was present from 1921 to 1938 basalt (MORB) and hot spot and plume volcanic fluids are
and then disappeared [e.g., Mavonga et al., 2006]. Since 8 ± 1 and up to 20 or more, respectively [Craig and Lupton,
1928, the Nyiragongo volcano has been known for its 1976]. Fluids related to continental and arc volcanoes have
semipermanent active lava lake, whose level, up to our last a wide range of R/Rair values (between 3 and 8) depending
visit to the crater (April 2009), has been continuously on the degree of crustal contamination affecting the mantle
changing [Tedesco, 2009]. An important rise of the lava source [Poreda and Craig, 1989; Hilton et al., 2002].
lake has triggered the lateral eruption on 10 January 1977 [7] Carbon isotopic values of CO2 (hereafter reported as
[Tazieff, 1979]. Later, an active lake was present in 1982 (up d13C-CO2 VPDB%) in mantle-related fluids usually range
to 1985) [Durieux, 2002/2003] and again in 1994 – 1995 between 3% and 7% VPDB, depending on the different
[Tedesco, 2002/2003]. The Nyiragongo volcano resumed its geodynamic settings of the volcanic region. Fluids of
activity in January 2002 with an approximately 15 km long magmatic systems producing basaltic lava, such as Etna
N-S oriented fissure eruption [Komorowski et al., 2002/ and Hawaii, show d 13C-CO2 values approximately 3%
2003; Tedesco et al., 2007] generating silica-undersaturated VPDB [Gerlach and Taylor, 1990; Poreda et al., 1992;
(SiO2 < 40 wt %) products [Santo et al., 2002/2003; Allard et al., 1997]. More positive d13C-CO2 values (0% to
Chakrabarti et al., 2009]. Two lava flows originated by this approximately 2% VPDB) in volcanic systems, e.g.,
activity entered the city of Goma (500,000 inhabitants in Vulcano Island [Tedesco and Nagao, 1996; Capasso et al.,
2002, more than 600,000 in 2008), causing the death of 1999], Mt. Vesuvius [Tedesco and Scarsi, 1998, Chiodini et
about 170 people and leaving more than 100,000 homeless al., 2001], and Nysiros [Brombach et al., 2003], generally
[Tedesco et al., 2007]. The United Nations and European imply the presence of limestone interactions with the mag-
Union funded several research projects following the 2002 matic fluid or within the magmatic reservoir. Strongly
eruptive event, owing to the political and economic impor- negative d13C-CO2 values (20% VPDB) are often relat-
tance that the Nyiragongo volcano plays in such an unstable ed to the degradation of organic matter at relatively shallow
area. This study includes an isotopic (carbon, helium, and depth [O’Leary, 1988; Hoefs, 2008], whereas CO2 produced
argon) survey of gas discharges collected in 2003 and 2005 by thermometamorphic processes in sedimentary realms
from the summit crater of the Nyiragongo volcano and the generally shows d13C-CO2 values 0% VPDB [Tedesco,
portion of the rift that extends north and south of Lake Kivu, 1997; Tedesco and Scarsi, 1998; Minissale, 2004]. Interme-
including several areas outside the rift (Figure 1). The main diate d 13C-CO2 values between those characterizing the
goal of the current research is to constrain the origin of the different fluid source regions can commonly be produced
various fluid sources in order to investigate the complex by mixing processes and/or fractionation effects (e.g., pro-
relationships among rift tectonics, mantle degassing, the longed interaction of alkaline waters with a CO2-rich gas
existence of different fluid source regions, and the potential phase) [Tedesco, 1997; Minissale et al., 1997; Chiodini et
future activity of Nyiragongo volcano. al., 1999; Minissale, 2004]. Argon has three stable isotopes,
the two of most interest being ‘‘primitive’’ 36Ar and
2. Helium, Carbon, and Argon Isotope Ratios ‘‘radiogenic’’ 40Ar. There is virtually no primordial 40Ar in
in Different Fluid Source Regions the Earth [Ozima and Kudo, 1972], being entirely produced
by 40K decay. Theoretical calculations, based on the atmo-
[5] The isotopic values of He, C, and Ar of fluid discharges spheric 40Ar budget and the estimate of the total 40K content
and fluid inclusions can be considered powerful tracers of of the Earth, indicate that approximately half of all 40Ar
interactions between mantle- and crust-derived fluids in produced within our planet since its formation is retained
different geodynamic settings [e.g., Polyak and Tolstikhin, within the solid Earth [Poreda and Farley, 1992; O’Nions
1985]. In particular, the He isotopic ratio can be used to and Tolstikhin, 1996]. However, 40Ar does not seem to be
intimately define the various sources of fumarolic gases and homogeneously distributed within the mantle. MORB lavas
to model hydrothermal fluid circulation patterns related to are indeed typically characterized by 40Ar/36Ar ratios up to
volcanic and hydrothermal activity [e.g., Giggenbach et al., 28,000 [Farley and Poreda, 1993; Sarda et al., 1985], which
1993; Tedesco and Scarsi, 1998], since 3He is essentially are 5 to 10 times higher than those of lower mantle xenoliths,
primordial and retained in the Earth’s interior at the time of its the latter being comprised between 307 and 1870 [Poreda
formation, whereas 4He is mainly derived from the decay of and Farley, 1992; Farley and Poreda, 1993; Nagao and
U and Th series isotopes in both mantle and crust. As a Takahashi, 1993].
consequence, 3He/4He ratios higher than the local (crustal)
production rate indicate the presence of degassing of mantle-
3. Mantle Source(s) in the EARS
derived fluids.
[6] Mantle degassing is intimately associated with mag- [8] The Cenozoic volcanism over the eastern and central
matic activity in ocean basins and continental settings. African plate shows two distinct relationships with the
Mantle degassing mainly occurs in ocean basins, in corre- mantle: rift- and hot spot-related volcanism [Pik et al.,
spondence with the formation of oceanic lithosphere 2006]. However, the nature of the mantle beneath the EARS
[Clarke et al., 1969] and less commonly in continental is still a matter of debate, likely due to the fact that the
environments [Torgersen, 1989]. Fluids enriched in radio- geophysical data do not provide complete coverage of the
genic helium, typically found in the crustal environment, are area and uncertainties in the African plate kinematics of
characterized by R/Rair values of about 0.01 (where R is the the last 45 Myr do not discriminate whether one or two
3
He/4He isotopic ratio measured in the sample and Rair is the diachronous plumes are interacting with heterogeneous lith-
3
He/4He ratio of air equal to 1.39 106 [Mamyrin and osphere [e.g., Paslick et al., 1995; Simonetti and Bell, 1994;
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
Kalt et al., 1997; Ebinger and Furman, 2002/2003; Furman, [13] Gas samples from hydrothermal discharges consist-
2007]. However, He isotope systematics clearly define the ing of bubbling pools were collected at the following sites:
presence of at least one plume at the triple junction of the Gulf (1) Rambo, a group of springs (with a discharge temperature
of Aden, the Red Sea, and Ethiopian rift [Marty et al., 1993, ranging from 50°C to 72°C) located in the Archean crys-
1996; Scarsi and Craig, 1996; Pik et al., 2006], whereas the talline basement outcrops of the eastern border of the rift a
determination of a second plume, based on current Pb and He few kilometers from the city of Goma on the Rwanda side
isotopic data, is ambiguous. Helium isotope systematics, of lake Kivu, (2) Mai ya Moto, ‘‘hot water’’ in Swahili
particularly in lava phenocrysts, have recently provided some (discharge temperature of 96°C), located north of Nyira-
insights about the interactions between mantle and crustal gongo volcano (Figure 1), (3) Kankule (discharge temper-
environments in the EARS [e.g., Marty et al., 1993, 1996; atures of 67°C), and (4) Muganzo (discharge temperatures
Darling et al., 1995; Scarsi and Craig, 1996; Graham, 2002; of 68.5°C), with Kankule and Muganzo both located on the
Pik et al., 2006]. The He isotope signature (R/Rair up to 20) of south side of Lake Kivu (Figure 1), in the volcanic realm of
fluid inclusions and gas discharges collected in Ethiopia the dormant Kahusi volcano.
(Afar), Yemen, and Djibouti [Scarsi and Craig, 1996; Pik [14] The sampling network also includes three soda
et al., 2006], associated with the Oligocene onward prerift springs: (1) Tingi (30°C), located close to the western rift
flood basalts, shows the existence of a lower mantle source border (Figure 1), in a relatively tiny area characterized by
region [Schilling et al., 1992; Deniel et al., 1994], typical of the presence of numerous thermal fluid discharges; (3)
other volcanic provinces on the Earth, where large volumes Kisuma (39°C), on the sedimentary hills of Masisi, approx-
of lavas have been emitted, such as the Deccan and the imately 50 km west of the rift; and (3) Makera (19°C),
Siberian plateau [Basu et al., 1993]. R/Rair values lower than located outside the rift 90 km NW of Goma (Figure 1).
6 were measured in the same area and are likely due to either [15] Four samples of dissolved gas were also collected
(1) accumulation of 4He in old lavas or (2) crustal contam- from different locations within Lake Kivu: (1) two samples
ination that could have affected both old and young lavas in the main basin at the depth of 320 m, using the facilities
[Marty et al., 1996; Pik et al., 2006]. of the local gas methane power plant at Cap Rubona (Figure
[9] A distinct type of volcanism, presumably related to 1), (2) one at the maximum depth of 475 m, and (3) one at
shallow (<400 km) mantle upwelling, characterizes the WB the maximum depth of 148 m of Kabuno Bay, which is a
of the EARS, where R/Rair from 5.7 to 8.9 were measured relatively small sub-basin located in the most northwest
[Graham, 2002; Pik et al., 2006]. Similarly, volcanic products portion of Lake Kivu (Figure 1).
and gas discharges of the Kenya rift [e.g., Darling et al., [16] To complete the sampling network, two samples of
1995] have a MORB-like He isotopic signature. olivine and clinopyroxene phenocrysts from Rumoka crater
[10] The only existing He isotopic data in the VVP are (belonging to the Nyamulagira domain) and one sample of
those measured in (1) one sample of dissolved gas collected clinopyroxene from Mudja lava tunnel, Nyiragongo realm
from the depth of 320 m in the Lake Kivu (R/Rair = 3) and were also collected and analyzed. The Rumoka crater,
(2) one from the several CO2-rich gas vents bordering the located half way between Goma and Sake (Figure 1),
northern shoreline of the lake (R/Rair = 5) (R. Poreda erupted in 1912. This perfectly preserved crater is also the
(personal communication, 2003) as cited by Schoell et al. site at its bottom of one of the biggest and most dangerous
[1988] and Tuttle et al. [1990]). mazuku (Table 1). The Mudja lava tunnel is located in the
outskirt of the Mudja village, between the Nyiragongo
4. Sampling and Analytical Methods crater and the city of Goma (Figure 1).
4.1. Description of the Sampling Sites
4.2. Sampling Procedure
[11] Fumarolic gas samples were collected within the
Nyiragongo summit crater at platform 1 (Goma 1 and [17] Preevacuated 60– 250 mL glass flasks filled with
Goma 2, with outlet temperature of 82°C and 84°C, respec- 20 – 100 mL of a 4 N NaOH and 0.15 M Cd(OH) 2
tively) and platform 2 (fractures 1 to 8, with outlet temper- suspension [Giggenbach, 1975; Montegrossi et al., 2001]
ature ranging from 118°C to 393°C). The two lava platforms were used on line, with (1) a titanium tube and dewar glass
are located at an altitude of 190 and 290 m lower than the tubes and (2) silicone/tygon tubes connected to a plastic
crater rim, respectively (Figure 1). Platform 1 corresponds to funnel, to sample gases from fumarolic vents and boiling
the lava lake level prior to the 1977 eruption, while platform 2 pools, respectively [Tassi et al., 2004; Vaselli et al., 2006].
is related to the lava lake level during the 1994 – 1995 The mazukus were sampled by using a dewar silicon tube
eruptive cycle [Durieux, 2002/2003; Tedesco, 2002/2003]. inserted into the vents at a depth between 0.5 and 1 m. The
3
[12] Most of the gas emissions collected in the area He/4He, 40Ar/36Ar, and He/Ne ratios were determined in
surrounding the Nyiragongo volcano within the rift consist headspace gases of the glass flasks. A further aliquot of gas
of the so-called mazukus (the local Kinyarwanda word for in 50 mL preevacuated flasks was also collected from each
‘‘evil winds’’), which are cold (20°C–26°C) low-flux gas site for determining the d 13C-CO2 values. The dissolved gas
emanations seeping out from old fractured and altered lava, samples from Lake Kivu main basin and Kabuno Bay basin
or in depressed areas in the Nyamulagira and Nyiragongo were collected by using 150 mL preevacuated glass flasks,
lava fields [Vaselli et al., 2002/2003]. The mazukus are following the procedure described by Tassi et al. [2008].
prevalently located (1) in the vicinity of northern shoreline 4.3. Analytical Procedure
of Lake Kivu and (2) close to and within the village of Sake
[18] Concentrations of CO2 were determined in the soda
to the west (Figure 1), the latter being built on historical
samples by automatic titration with 0.5 N HCl solution,
lava flows of Nyamulagira volcano.
following the procedure of Montegrossi et al. [2001]. The
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
13
C/12C ratios in CO2 were determined by mass spectrom- mended value: +1.58% VPDB) and international (NBS 19
etry, after a two-step extraction and purification procedures carbonate, recommended value: 1.95% VPDB) standards
of the gas mixtures by using liquid N2 and a solid-liquid produced values of 1.59 ± 0.04 and 1.95 ± 0.06, respectively.
mixture of liquid N2 and trichloroethylene. During the [19] Gas samples for the isotopic analysis were purified in
period of analysis, internal (San Vincenzo marble, recom- a high vacuum line constructed of stainless steel and
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
Corning-1724 glass to minimize helium diffusion. Water (Table 1). The fluid discharge collected at Tingi, in the
vapor and CO2 were cryogenically trapped at 90°C and western peripheral side of the rift (Figure 1), has 1.68 R/Rair,
195°C, respectively, whereas N2 and O2 were removed by a value particularly low if compared to those measured in
the reaction with a Zr-Al alloy (SAES-ST707). Argon and nearby mazukus of Sake (e.g., Source, Ecole, Birere, and
Ne were adsorbed on activated charcoal at 196°C and at Gisimba) just 0.5 to 1 km away (Figure 1, Table 1). Rambo
233°C, respectively. SAES-ST-101 Getters (one in the hot springs, located just outside the eastern border of the rift
inlet line and two in the mass spectrometer) reduced the (Figure 1), show the lowest R/Rair values (ranging between
HD+ background to 1000 ions/s. 0.09 and 0.21) of the entire data set (Table 1). The R/Rair
[20] Helium isotope ratios and concentrations were ana- values in dissolved gases of Lake Kivu at depths of 320
lyzed on a VG 5400 Rare Gas Mass Spectrometer fitted (Cap Rubona) and 475 m (lake bottom) are 2.65 – 2.79 and
with a Faraday cup (resolution of 200) and a Johnston 3.18, respectively, whereas the gas sample collected from
electron multiplier (resolution of 600) for sequential anal- Kabuno Bay basin (Figure 1) has 5.54 R/Rair. The thermal
yses of the 4He (Faraday cup) and 3He (multiplier) beams. springs located within and outside the rift north of Nyir-
On the axial collector (resolution of 600), 3He+ was agongo volcano (Mai ya Moto, Kisuma, and Makera
completely separated from HD+, with a baseline separation springs; Figure 1) have 0.67, 0.76, and 1.09 R/Rair, respec-
of <2% of the HD+ peak. The contribution of HD+ to the tively. These isotopic values are similar to those measured at
3
He peak was <0.1 ion/s at 1000 ions/s of HD+. For 2 Kankule and Muganzo (0.68 and 0.75 R/Rair, respectively)
106 cm3 STP of He with an air ratio (sensitivity of 2 in the southwestern lakeside.
104 A/torr), the 3He signal averaged 2500 ions/s with a
background signal of 15 cps, due to either scattered 4He 5.2. Carbon Isotopes
ions or the formation of 4He ions at lower voltage potentials [24] The d13C-CO2 values of Nyiragongo crater gas
within the source of the mass spectrometer. Analytical error discharges are between 4.04% and 3.55% VPDB, a
for He isotope determination was <0.3%. The 3He/4He range typical of high-temperature fluids from basaltic sys-
ratios (R) were corrected for the addition of air by employ- tems [Gerlach and Taylor, 1990; Poreda et al., 1992; Allard
ing the standard air correction calculation [Craig and et al., 1997]. Conversely, the d 13C-CO2 values of (1) the
Lupton, 1976]. mazukus of the northern shoreline of Lake Kivu main basin
[21] After completion of the He isotopic analysis, 40Ar/36Ar and (2) those located close to Sake village (Figure 1) vary
ratios were measured with the same VG 5400 mass spec- from 6.76% to 5.29% and from 11.65% to 10.48%
trometer. Sensitivity for Ar concentration was 4.2 104 A/ VPDB, respectively. It is worth noting that the d13C-CO2
torr on the Faraday cup. Precision for the 40Ar/36Ar ratios values of the dissolved gas samples collected from Lake
averaged 0.2%. Kivu main basin (5.43% and 5.60% VPDB at depth of
[22] Carbon dioxide concentrations and the ratio of 320 and 475 m, respectively) and from Kabuno Bay basin
CO2/3He in olivine phenocrysts were obtained by crushing (10.29% VPDB), are similar to those of the geographi-
under high vacuum between two zirconia plates in an all- cally analogous mazukus (Figure 1). Tingi spring (Figure 1)
metal ‘‘Nupro-valve’’ crusher assembly. CO2 concentrations has a d 13C-CO2 value of 6.58% VPDB.
were measured by a capacitance manometer in a calibrated [25] The distal gas discharges located within the rift north
volume. Helium concentration was measured by compari- of Nyiragongo volcano (Mai ya Moto springs) and south of
son to an aliquot of Yellowstone MM standard. Reproduc- Lake Kivu (Kankule and Muganzo springs) show d13C-CO2
ibility and checks on CO2 yield (i.e., loss of CO2 by values between 7.02% and 5.90% VPDB, slightly less
adsorption) were made by repeated sequential crushing of negative than those of the thermal fluids discharged outside
a high concentration CO2 olivine Samoan xenolith (total the rift (Kisuma and Makera springs at west and Rambo
CO2 = 0.1 cm3/g, He = 750 cm3/g). Five sequential crushing soda springs at east; Figure 1), where d 13C-CO2 values vary
steps showed a variation in the CO2/3He ratio of less than between 8.44% and 7.23% VPDB.
10% (total range) for the five steps and heating of the 5.3. Argon Isotopes
crusher to 100° did not release measurable CO2. From this
experiment, we concluded that neither the zirconia surfaces [26] The 40Ar/36Ar ratios from the majority of the gas
nor the olivine powder adsorbed significant amount of CO2. discharges of the Nyiragongo volcano and its surroundings
The blanks were <5 105 cm3 and 4 1010 cm3 for are equal to that of air (296), with the exception of (1) the
CO2 and He, respectively, for 0.55 g of sample. crater emissions of platform 1 collected in 2003 (Goma 1
and Goma 2 samples; Table 1), (2) the samples collected at
Rambo springs, and (3) the dissolved gas samples of the
5. Results deep water of Lake Kivu and Kabuno Bay basins. In these
5.1. Helium Isotopes samples, the 40Ar/36Ar ratios range between 313 and 384,
[23] The R/Rair values of gases collected at platform 1 and indicating 10% to 30% of the Ar emanates from a radio-
platform 2 of Nyiragongo summit crater are up to 8.73, genic source. By assuming that 36Ar is entirely derived from
similar to those (8.13 R/Rair) measured in the fluid inclu- air, the concentration of radiogenic Ar (40Ar*) (Table 1) in
sions of the Mudja lava tunnel. Gases released from the gas samples is commonly calculated, as follows:
mazukus have relatively high R/Rair values (between 6.51
and 8.35), although located tens of kilometers away from h i
the central crater (Figure 1) and affected by significant air 40
Ar* ¼36 Ar 40
Ar=36 Ar 295:5 :
contamination, as shown by the relatively low He/Ne ratios measured
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
Figure 4. CO2/3He versus d13C-CO2 binary diagram for gas discharges collected at the Kivu volcanic
province. Symbols are as in Figure 2. Inset represents, without the possible end-members and at a larger
scale, the variation of our samples.
(2) the radiogenic-rich Rambo springs (R/Rair 0.1 and 6.3. Magmatic Degassing and Gas Fractionation
40
Ar*/4He 0.1 –0.2). Dissolved gases in Lake Kivu plot at [39] There is no attempt to rigorously model the fraction-
intermediate position (Figure 5). It is worth noting that the ation of CO2 and He out of the lava because there are only
40
Ar*/4He ratios of the crater fumaroles are much higher three complete sets of data of samples from the summit
than the 40Ar*/4He ratio produced by the present-day fumaroles. Although we collected the fumarolic gases as
radiogenic decaying process in the mantle (0.27 ± 0.02), close as possible to the lava lake, there is only limited
calculated on the basis of measured K/(U + Th) ratios in knowledge of the original CO2/3He in this lava and even
MORB [Jochum et al., 1983] and the ‘‘bulk earth’’ value of less data on the mantle concentration of He or CO2. On the
0.55 for 4.5 Ga of radiogenic production. In this respect, the basis of the available data, we can only conclusively state
40
Ar*/4He ratio is strongly dependent on the magma
degassing process regulating the partition equilibrium
between the melt and the gaseous phase, because the
solubility of He in the magma melt is about a factor of
4 higher than that of Ar [Lux, 1987]. Thus, if the melt has an
initial ‘‘bulk earth’’ 40Ar*/4He ratio of 0.55 [e.g., Poreda and
Farley, 1992], then the first gas off the magma reservoir will
have a 40Ar*/4He ratio of about 2.2. According to these
considerations, the measured 40Ar*/4He ratios of the Nyir-
agongo crater fumaroles are likely the result of fractionation
during degassing processes caused by the differences in
solubility of He and Ar within the magma. Conversely, the
40
Ar*/4He ratios may differ from the ‘‘bulk earth value’’
because of unique K/(U + Th) (ultra-potassic magmas) ratios
in the source region. The correlations between the highest
excess 40Ar*, coupled with the highest (R/Rair)c of the
region, suggests the measured ratio is the closest to (not
equivalent to) the true signature of the mantle. However, the
coupling of the lowest (R/Rair)c and 40Ar* suggests the
presence of an ubiquitous crustal end-member.
[38] Then the relatively low 40Ar*/4He ratios (0.1 – 0.2) of Figure 5. R/Rair versus 40Ar*/4He binary diagram for gas
Rambo springs, representing the crustal end-member, are discharges collected at the Kivu volcanic province, where
likely related to the typical 4He enrichment of fluids 40
Ar* is the radiogenic argon calculated by using the
circulating in crustal environment [e.g., Torgersen et al., following equation: 40Ar* = 36Ar(40Ar/36Ar 295.5). The
1988; Hu et al., 1998]. theoretical 40Ar*/4He ratio in the MORB (0.27 ± 0.02)
was calculated on the basis of measured K/(U+Th) ratio
[Jochum et al., 1983].
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B01205 TEDESCO ET AL.: He AND C IN THE EASTERN AFRICAN RIFT B01205
that given the observed magmatic compositions present at of the summit crater result from increased CO2 solubility in
Nyriagongo, the CO2/3He in the residual melt will increase the foiditic magma that feed Nyiragongo volcano. The high
40
with continued degassing because CO2 is 5 times more Ar*/4He ratios result from the differences of solubility in
soluble than He in these strongly silica-undersaturated lavas the melt between He and Ar.
[Dixon et al., 1997]. There is some uncertainty in the CO2 [42] The crater fumaroles and the mazuku gas emissions
solubility estimate because it is an extrapolation from have similar R/Rair values indicating a common mantle
experimental measurements in moderately undersaturated origin. However, the d 13C-CO2 values seem to show that
lavas; however, the magma will evolve toward higher the CO2 discharged at the mazukus is fractionated by
CO2/3He as observed in the summit fumarole collected over scrubbing, although minor addition of biogenic CO2 cannot
4 years. Thus, the lowest CO2/3He most closely reflects the be ruled out. Thus, the uprising fluids feeding the mazukus
magmatic condition after correction for solubility effects. are exposed to a significant interaction with local ground-
This interpretation is confirmed by the argon isotope ratio water and meteoric water, which obviously does not occur
which decreases from a value of 350 to the air ratio within along the crater plumbing system. As already suggested by
2 years, despite the high He/Ne ratio (700). As discussed previous investigation [Tedesco et al., 2007], this could also
above, argon is much less soluble than helium (about a imply that crater and mazuku fluids are not fed by the same
factor of 4) in all silica-undersaturated lavas and will rapidly reservoir, but more likely by two totally independent
degas from an evolving magmatic system [Lux, 1987]. The reservoirs, one located beneath the crater, the second several
40
Ar*/He ratio of 0.8 in the fumarole differs from the ‘‘bulk kilometers away in the region between Nyiragongo and
earth’’ value of 0.55 (closed system evolution for 4.5 Ga) Lake Kivu. As a consequence, volcanic activity at Nyir-
because of the combined effects of solubility and fractional agongo volcanic system could involve eruptive episodes
degassing. A 40Ar*/He ratio of 0.8 reflects a magmatic ratio from the central crater and/or fissures within the flanks of
of 0.2; if the Nyriagongo magma initially had a ‘‘bulk the volcanic edifice or through peripheral cones. These
earth’’ 40Ar*/He ratio of 0.55, then the fact that the results indicate that these activities may also take place
magmatic value differs from 0.55 would indicate that the anywhere else in the active ‘‘corridor’’ described by both
lava has partially degassed. A simple Rayleigh fractionation the R/Rair and d 13C-CO2 isotopes. This means that future
calculation suggests that about 25% of the helium and about volcanic episodes could occur close or even within the
5% of the CO2 have escaped. This calculation also suggests heavily populated city of Goma or at the bottom of Lake
that the original CO2/3He is about 3 1011 or very CO2 Kivu without necessarily being accompanied by a signifi-
rich. Because of the great difference in noble gas and carbon cant increase or variation of activity inside the main
dioxide solubilities, these ratios change quickly and dra- Nyiragongo crater. This possible (and horrifying) scenario
matically in degassing Si-undersaturated lavas. Thus, by has important implications for future studies and for assess-
2005 and 2007, all of the 40Ar* has degassed leaving behind ing volcanic hazards related to the activity of the entire
only the admixed atmospheric argon. Nyiragongo (Virunga volcanic system).
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