Arima hot spring waters as a deep-seated brine from subducting slab
© Kusuda et al.; licensee Springer. 2014
Received: 3 June 2014
Accepted: 19 August 2014
Published: 19 September 2014
Non-volcanic hot springs are generally believed to originate through circulation of meteoric or buried sea water heated at depth. In this study, we report the geochemical characteristics of the Arima and Takarazuka hot spring waters, known as Arima-type deep brine, in a forearc region of southwestern Japan. We examine 14 water samples to determine the levels of 12 solute elements or components and the isotopic ratios of H, He, C, O, and Sr, and we perform correlation analysis of the data to deduce the source materials and origin of the deep brine. Moreover, we perform numerical modeling of oxygen and hydrogen isotopic fractionation along subducting slabs to examine the composition of slab-derived fluid as a possible candidate of the deep brine. The results suggest that the high salinity and solute concentrations with characteristic oxygen, hydrogen, carbon, and strontium isotope compositions, as well as high 3He/4He ratios, can be explained by a dehydrated component of the subducted Philippine Sea slab. Hence, this study may provide an invaluable understanding of geofluid processes over a significant depth range.
Various geophysical and geochemical studies suggest that within the mantle wedge and crust in subduction zones, fluid fluxes may trigger seismicity and magmatism throughout the system (e.g., Iwamori 2007; Hasegawa et al. 2008). The term 'fluid' in this case includes a variety of physical substances such as aqueous fluid, supercritical fluid, and melt (or magma), which are often referred to as 'geofluids.' Studies on geofluids may provide a clue to understanding the hydrological budget in subduction zones, as well as the global water and element cycling, since subduction zones are the major injection sites of water and chemical elements existing at the surface into the Earth's interior (Jarrard 2003; Fischer 2008; Iwamori and Albarède 2008; Shinohara 2013).
On the contrary, the nature and composition of such deep geofluids have been studied through high-pressure experiments on element partitioning (e.g., Brenan et al. 1995; Keppler 1996; Kogiso et al. 1997; Kessel et al. 2005), geochemical constraints on subducting materials and arc magmas (e.g., Ishikawa and Nakamura 1992; Plank and Langmuir 1998; Pearce et al. 2005; Nakamura et al. 2008; Kimura et al. 2009), and fluid inclusions in mantle-derived xenoliths (e.g., Schiano et al. 1995; Ishimaru and Arai 2008; Ionov 2010; Kawamoto et al. 2013), constraining elemental abundances and isotopic ratios of these geofluids.
In this study, we discuss the relationship between Arima-type brine and deep geofluids in a definitive manner. In particular, we examine multiple element and isotopes of the hot spring waters, including the oxygen and hydrogen isotopic composition of the slab-derived fluid, and we determine whether the characteristic O-H isotopic compositions of the Arima-type brine are explained by the slab fluid.
Multiple elemental and isotopic characterization
Sample and analytical methods
Sample and locality list
Name of springs
12 December 2007
12 December 2007
13 December 2007
13 December 2007
13 December 2007
13 December 2007
13 December 2007
13 December 2007
13 December 2007
Mint Resort Inn
14 December 2007
Ginsuiso Ginsen south
14 December 2007
Ginsuiso Ginsen north
14 December 2007
14 December 2007
14 December 2007
The studied area is within 600 m zonally and 900 m meridionally in Arima. In addition, two samples were obtained in Takarazuka, about 10 km east of Arima, where most of the springs flow naturally from shallow (40 m in depth) to deep (1500 m) reservoirs or flow paths along the faults (e.g., Kozuki 1962), with a temperature range of 19°C to 96°C (Table 1).
Analytical results of the Arima and Takarazuka hot spring waters and gases
δ 180SMOW (‰)
δ DSMOW (‰)
δ 13CPDB (‰)
Elemental and isotopic composition
The results are listed in Table 2. Both the solute concentrations and the isotopic ratios of hydrogen, helium, carbon, oxygen, and strontium exhibited wide variations. The chlorine concentration ranges from 14 to approximately 40,000 ppm (up to twice that of seawater), the lithium concentration ranges from 0.02 to 51.90 ppm (0.2 to 300 times that of seawater), and the air-normalized 3He/4He ratio ranges from 2.33 to 7.51 (close to that of the upper mantle represented by mid-ocean ridge basalt). In order to discuss origin of the brines that may potentially involve multiple source materials and processes, analyses based on multiple element/isotope data, as shown in Table 2, are useful for clarifying, for example, the association of elements/isotopes derived from individual sources. Such multiple element/isotope studies, including hydrocarbon species, on brine or gas from various tectonic settings such as subduction zones (e.g., Mutnovsky Volcano, Kamchatka; Zelenski et al. 2012), ocean islands (e.g., Socorro Island, Mexico; Taran et al. 2010), and continental-oceanic rifts (Salton Sea, USA; Mazzini et al. 2011) have been successfully used to identify various sources. These sources include altered basaltic oceanic crust (AOC), oceanic sediment, and continental and mantle sources, and their modification by chemical and thermal processes such as mixing, serpentinization, and near-surface cooling.
The new dataset and the linear trends confirm the previous results, which suggest mixing of local meteoric water in the Arima area (δD approximately -50‰ with nearly zero for all the solute concentrations, Masuda et al. 1985) and a deep-seated brine (e.g., Matsubaya et al. 1973; Tanaka et al. 1984; Masuda et al. 1985). Based on the new data, we quantitatively estimated the deep brine composition. The previously observed relationship between 3H and δD of the Arima hot spring waters, δD of the tritium-free water, i.e., a pure deep brine, is inferred to be -30‰ to -35‰ (Tanaka et al. 1984). Then, the least squares regression lines at δD = -30‰ to -35‰ provide the estimate on the brine composition: Cl- = 42,000 mg/L, Na+ = 21,000 mg/L, Li+ = 55 mg/L, Br- = 84 mg/L, Ca2+ = 3,100 mg/L, Sr2+ = 86 mg/L, NH4+ = 8.8 mg/L, K+ = 3,700 mg/L, and δ18O = +6‰ at δD = -33‰, which are similar to but slightly more diluted than the previous estimates by Masuda et al. (1985).
Oxygen and hydrogen isotopes of slab-derived fluid
In order to test the origin of the deep brine, a numerical model was developed to estimate the oxygen and hydrogen isotope compositions of the slab-derived fluid. The model considers the thermal structure along the subducting slab in a 2D across-arc section, stability and dehydration reaction of hydrous mineral phases, and the resultant partitioning of oxygen and hydrogen isotopes between the fluid and the residual mineral phases.
First, the thermal structure of the subduction zone was calculated because dehydration from subducting slabs is controlled thermodynamically and hence chiefly by temperature and pressure. Since dehydration mainly occurs within hydrated oceanic crusts consisting of both sediment and AOC rather than the underlying oceanic mantle (e.g., Iwamori 2007), the temperature distribution along the surface of a slab is calculated as a function of subduction velocity (V), slab age (a), and subduction angle (θ), using an analytical expression based on that reported by England and Wilkins (2004). As a result, we estimated the thermal profile along the slab surface for the subducting Philippine Sea slab (V = 4 cm/year, a = 15 Ma, θ = 20°) beneath the southwestern Japan arc, as well as that for the Pacific slab (V = 10 cm/year, a = 120 Ma, θ = 30°) beneath the northeastern Japan arc. These thermal profiles, shown in Additional file 1: Figure S1, are similar to those obtained in 2D numerical simulation (e.g., approximately 600°C at 3 GPa; Iwamori 2007).
Next, slab dehydration and the isotopic fractionation of oxygen and hydrogen were calculated, based on the phase relation of the subducted materials. Although oceanic sediments initially contain 10 to 30 wt% H2O (Plank and Langmuir 1998), most of water is liberated, decreasing to 2 to 4 wt% by extensive compaction and dehydration of minerals at depths shallower than 30 km (You et al. 1996; Hyndman and Peacock 2003; Kasahara 2003). The sedimentary column currently delivered to deep sea trenches is typically 50 to 500-m thick, and sediment 350-m-thick subducts from the Nankai Trough (Plank and Langmuir 1998). These values are 1/100 to 1/10 thinner than the AOC thickness, limiting its impact on the water budget in subduction zones. Considering these factors, although oceanic sediments still contain 1 to 2 wt% of H2O at depths greater than 100 km, the AOC-derived fluids are thought to be a major source that supplies deep-seated fluids to the overlying mantle wedge and the arc crust over the slab depth ranging from 30 to 100 km (Iwamori 2007), including the Arima area (Figure 1). Therefore, to simplify the model, we considered only dehydration of AOC and its phase relations for dehydration reaction (Schmidt and Poli 1998). It should be noted, however, that several key elements/isotopes such as carbon and lead, which are particularly concentrated in sediments, may have significant impacts on the fluid compositions (e.g., Sano and Marty 1995; Aizawa et al. 1999; Nakamura et al. 2008), as will be subsequently discussed.
A model was then designed to estimate the isotopic characteristics of slab-derived fluids for the hydrogen and oxygen stable isotopic ratios that constitute the characteristic features of Arima-type brine. The major constituent minerals of AOC at the pressure-temperature condition beneath the Arima area (i.e., 1.5 to 2.4 GPa and 400°C to 500°C, including uncertainty in the estimates), where major dehydration of AOC occurs, are amphibole (22% to 48% in modal composition), lawsonite (22% to 36%), chlorite (0% to 13%), and epidote (9% to 22%; Schmidt and Poli 1998). Accordingly, the following water/mineral isotopic fractionation factors (α) for the major constituent minerals of AOC are used.
where T is the absolute temperature. Epidote is one of the major constituent minerals in AOC at up to 22 wt% (Schmidt and Poli 1998) for the P-T range of interest up to 3 GPa and 600°C in this study, respectively. Matthews et al. (1983) reported that below 600°C, the oxygen exchange reaction is very slow between water and zoisite, the Fe-free end-member of epidote group minerals; therefore, no isotopic fractionation occurs. Instead, dissolution-precipitation appears to occur. In addition, the zoisite-water fractionation factor constrained by mineral-pair equations is around unity (Matthews et al. 1983), causing no 18O/16O fractionation. For these reasons, we ignored epidote in our estimates.
The Rayleigh fractionation of oxygen and hydrogen isotopes was calculated by numerically integrating the following equation along the calculated P-T path for the Philippine Sea slab to obtain the compositional path in Figure 3: Δδf /1,000 = -(1-F)/F (αf/r - 1) × ln (1 - F) (Equation 7), where Δδf is the change in isotopic ratio of the fluid corresponding to the infinitesimal change in P-T (‰), F is the extent of dehydration reaction constrained from the phase diagram as a function of P-T (weight fraction), and αf/r is the isotopic fractionation coefficient between the fluid and the bulk rock calculated as ΣXi αi, where Xi represents the weight fraction of mineral i, and αi is the fractionation factor derived from Equation 1 to 6.
The calculation starts with an average composition of AOC (δD = -40‰, δ18O = +8‰) obtained from a DSDP Hole 504B drill core >1,000-m long that includes fine-grained basalt to dolerite (Muehlenbachs 1986; Kawahata et al. 1987), as shown by the open star labeled ‘0 km’ in Figure 3. The δD value used (i.e., -40‰) is within the range reported from ODP/IODP Hole 1256D (-64‰ to -25‰, Shilobreeva et al. 2011). A shallow dehydration of this AOC produces relatively light oxygen isotopes (δ18O of approximately 0‰) and heavy hydrogen isotopes (δD of approximately -15‰) compared with those estimated in the Arima deep brine, which evolves toward the bottom right of the diagram. The results, showing larger δ18O and smaller δD values as the subduction progresses, reflect continuous dehydration and Rayleigh isotopic fractionation. The subducted young Shikoku Basin and its extinct spreading center (approximately 15 Ma; Okino et al. 1994; Sano et al. 2009) beneath the Arima area may share thermal and hydration conditions with a young oceanic crust at the 504B site off the Costa Rica Rift (approximately 6 Ma), partly justifying the assumed isotopic composition in Figure 3. Nevertheless, subducting slabs exhibit significant compositional variability, e.g., δD = -30‰ to -60‰, including sediment, AOC, and serpentinite (Kawahata et al. 1987; Giggenbach 1992; Matsuhisa 1992; Shaw et al. 2008), and causes significant uncertainty in the quantitative results of our model. As a consequence, the slab dehydration depth estimated for the Arima deep brine ranges from 45 to 70 km, as shown by the pink circle in Figure 3).
Beneath the Arima area, the depth of the Philippine Sea slab surface is estimated to be 50 to 70 km with relatively large uncertainty (Figure 1; Nakajima and Hasegawa 2007; Hirose et al. 2008). Our numerical model suggests that the slab-derived fluid at such depth has an isotopic composition similar to that of geochemically estimated deep brine within the uncertainty, as shown in Figure 3.
The estimated brine composition of δD at approximately -30‰ is similar to that estimated from analysis on back-arc basin basalts or melt inclusions from the Mariana subduction zone such as -25‰ (Poreda 1985) and -32‰ (Shaw et al. 2008), respectively, and the mass balance of subduction zone-scale material cycling at δD = -27‰ (Kazahaya 1997). The compositional range resembles magmatic fluids, although Arima is far from the volcanoes and is located in the forearc region in terms of northwestward subduction of the Philippine Sea Plate from the Nankai Trough. Westward subduction of the Pacific Plate causes magmatism in central Japan (e.g., Nakamura et al. 2008); Arima is located approximately 300 km west in the backarc region of the magmatism (Figure 1). The current understanding of the magma genesis, including the regional understanding along the entire Japan arcs (Iwamori 2007), indicates no magmatic production or supply beneath the Arima area.
Discussion and conclusions
However, as discussed in the previous section, the Arima hot spring is different in that no magmatic activity is expected beneath the area and no thick sedimentary basin exists (Kozuki 1962). Since the absolute concentrations of 3He in AOC, oceanic sediment, and ASW are four to six orders of magnitude lower than those in MORB (Zelenski et al. 2012), the high 3He/4He ratios found in the Arima hot springs are attributed to mantle helium incorporated in the fluid upon its ascent in the mantle. Arima is located in an area with hot springs of relatively high 3He/4He ratios (greater than 2.5 Ra) known as the Kinki Spot (Sano and Wakita 1985; Figure 1). The Philippine Sea slab subducted beneath the Kinki Spot is young and hot because it is associated with the former spreading ridge (Sano et al. 2009), which may have enhanced the degassing of the mantle.
The 3He/4He ratios are along the mixing line between the air and the mantle component, although the proportions of mixing differ from those identified from the solute concentrations (Figure 4). It is argued that shallow reservoirs exist beneath Arima (e.g., Masuda et al. 1985), where the meteoric water saturated with air mixes with both the deep brine and the exsolved gas and may cause variable mixing of the solutes and the gases. The broad negative correlation between the major solute elements and 3He/4He (Figure 2; Figure 5a) suggests that the spring waters diluted significantly by meteoric water in the shallow reservoir (e.g., AW-1, AW-2, and AW-9, Figures 2 and 3) have been fluxed by high 3He/4He gases (e.g., AG-1 and AG-5, Table 2 and Figure 5a) possibly derived from the deep brine (e.g., AW-3, AW-4, and AW-5) that ascends to the surface without being re-gassed.
Carbon dioxide is one of the dominant volatiles in magmatic fluids and gases in subduction zones, which is also one of the distinguishing characteristics of Arima-type brine, and could have originated from slab fluids (Jarrard 2003; Fischer 2008). The plausible sources of carbon are (1) organic carbon in sediments, which are mainly in the continental crust although subducted oceanic sediments are reported to have similar values, (2) carbonate in subducted MORB (AOC), and (3) inorganic carbonate in subducted marine limestones (Nissenbaum et al. 1972; Marty and Jambon 1987; Sano and Marty 1995). In order to identify the origin of carbon, the correlation between δ13C and CO2/3He ratios is useful; in fact, hot spring gases in subduction zones can be explained by three-component mixing, as shown in Figure 5b (Sano and Marty 1995). Within this context, the observed carbon isotopic compositions of the Arima hot spring waters also suggest possible involvement of deep-seated slab materials such as subducted MORB and limestone rather than organic carbon from a shallow sedimentary reservoir (Figure 5b). The poor correlation between the major solute, mostly derived from subducted MORB, and the carbon isotopic ratios, mostly buffered by subducted limestone, may reflect decoupled processes of different lithologies in a subducted slab such as dehydration versus decarbonation.
The CO2/3He ratios vary significantly over four orders of magnitude with broadly constant δ13C (Figure 5b). Low CO2/3He samples (AW-1, AW-2, and AW-9; Figure 5b) exhibited relatively high 3He/4He (Figure 5a) and low solute concentrations (Figure 4), when compared with the high CO2/3He samples (AW-3, AW-4, and AW-5) with low 3He/4He and high solute concentrations. Sano and Marty (1995) argued that the CO2/3He ratio of bubbling gas is lower than that of volcanic hydrothermal water which exsolves the gas because CO2 is much more soluble to water than He. They suggested that significant CO2/3He fractionation occurs during the ascent of deep hydrothermal fluids associated with decompressional degassing. Such a fractionation mechanism may consistently explain the lower CO2/3He samples (AW-1, AW-2, AW-9) that have been fluxed by the gas with low CO2/3He and high 3He/4He ratios in a meteoric water-dominated shallow reservoir, in addition to the high CO2/3He samples (AW-3, AW-4, AW-5) that contain more of the deep brine component from which the gas has been exsolved.
It has been argued that a high concentration of Cl- indicates an extensive water-rock interaction either at depth of a high temperature or with the granitic basement rocks at a relatively shallow depth (Edmunds et al. 1985). In the latter case, Cl- is derived from granitic rocks by acid hydrolysis of biotite and plagioclase. Since hydrolysis of biotite could generate Cl-, Li+, K+, and other species in the groundwater, Cl- and Li+ can be considered as conservative products of biotite alteration. On the contrary, the acid hydrolysis of plagioclase may contribute to the principal sources of Na+ and Ca2+ in the groundwater without supplying Cl- or Li+. Molar Cl-/Li+ and Na+/Ca2+ ratios of the sampled waters, however, reach up to about 150 and 12, respectively, which are significantly larger than the stoichiometry deduced from the above reactions. Although the possibility of such an excess of Na+ and Cl- owing to decreases in Ca2+, K+, and Mg2+ through the formation of clay minerals in the aquifer cannot be entirely ruled out, it appears difficult to attain the high salinity (approximately 42,000 ppm Cl) solely by chemical interactions between the basement granites and water (Edmunds et al. 1985).
Numerical forward modeling in this study suggests that slab fluids with δ18O-δD values similar to the Arima-type brine are produced along the subducted Pacific slab beneath the northeastern Japan arc (Figure 3). However, the produced fluid reacts with the mantle wedge just above the slab to form serpentinite due to the cold geotherm along the slab (Iwamori 2007). Therefore, the fluid is absorbed by the mantle and subducted to the deeper part along the slab, which may explain the absence of the Arima-type brine, to our knowledge, in the non-volcanic forearc region of northeastern Japan arc. On the contrary, in a warmer environment beneath the southwestern Japan arc, such an ‘absorption’ effect by serpentinite is greatly reduced (Iwamori 2007), and the slab fluid may escape to the surface without significant reaction with the country rocks, possibly guided by large faults at crustal levels.
It is also noted that the amount of fluid generated from the slab is maximum at depths of 30 to 80 km and is greatly reduced deeper than 100 km in most subduction zones (Iwamori 1998). Instead, beneath the northeastern Japan arc, the subducted serpentinite along the slab undergoes dehydration and supplies fluids upward beneath the arc volcanic zones, causing melting in a high-temperature region of the central part of the mantle wedge (Iwamori 1998). Then, hydrous magma is fed to a shallow chamber, where degassing may create volcanic waters and gases. Therefore, δ18O-δD compositions of the volcanic thermal waters, widely known as ‘andesitic water’ having δ18O = +5‰ to +10‰ and δD = -10‰ to -30‰ (Taran et al. 1989; Giggenbach 1992), integrate and reflect these processes of slab dehydration, sepentinite formation-dehydration, reaction with the mantle to cause melting, and degassing, as discussed by Matsuhisa (1992). In this context, andesitic water and the Arima-type brine as suggested in this study are believed to reflect different origins, although their δ18O-δD ranges overlap.
The estimated solute concentrations in the Arima deep brine (e.g., 42,000 ppm Cl; 3,700 ppm K; 84 ppm Br; Br/Cl ~ 2.0 × 10-3) are consistent with the recent knowledge on slab-derived fluids, e.g., 12,000 to 240,000 ppm Cl, 600 to 3,700 ppm for K, Br/Cl ~ 1.0 to 3.7 × 10-3 for fluids derived from subducted serpentinite (Kendrick et al. 2011), and 5.1 wt% NaCl (approximately 30,000 ppm Cl) for fluid inclusions in the mantle xenoliths (Kawamoto et al. 2013). On the contrary, the Philippine Sea slab-derived fluid compositions estimated from volcanic rocks in central Japan (Nakamura and Iwamori 2013) have higher concentrations for K and Sr (64,000 and 268 ppm, respectively), possibly reflecting different dehydration conditions of higher pressure and temperature beneath the volcanic region compared with those in the forearc region in southwestern Japan (Nakamura et al. 2014). It is also noted that during deep processes of dehydration and melting in subduction zones, Cl and F are reported to behave very differently (Straub and Layne 2003), which may explain the poor correlation between the major solute including Cl and F (Figure 2).
In any case, the composition of the Arima brine appears to retain the deep fluid signatures derived from multiple sources such as the subducted Philippine Sea slab and the overlying mantle, including (i) AOC for most water and hence hydrogen and oxygen isotopes in addition to associated elements such as Cl, Na, Li, Br, Ca, and Sr (Figure 2), (ii) subducted sediment, particularly limestone, for carbon, and (iii) mantle wedge for a high 3He/4He component. These signatures indicate that deep-seated fluid may reach the surface without significant interaction during its ascent, such as through channel flow from depth, as also suggested from the seismic velocity variations (Iwamori and Nakakuki 2013) and trace element transport in subduction zones (Ikemoto and Iwamori 2014). However, only a small amount of contamination by the basement granitic rocks with very high 87Sr/86Sr may have affected the Sr isotopic ratio of the fluid, and some crustal helium with low 3He/4He could have affected the degassed water samples such as AW-3, AW-4, and AW-5 with relatively low He content (Table 2). If such a fracture system is a dominant mode of fluid transport, the Arima-type brine may put direct constraints on both the compositions and processes of slab fluid at depth.
The authors would like to thank HA Takahashi, M Takahashi, M Tanimizu, and T Ishikawa for their help in elemental and isotopic analyses, M Totani for his kind arrangement and assistance in sampling hot spring waters in the Arima area, and the two anonymous referees for constructive review that greatly improved the manuscript.
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