©2011 Society of Economic Geologists, Inc. Economic Geology, v. 106, pp.

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SCIENTIFIC COMMUNICATIONS
TRACE ELEMENT GEOCHEMISTRY OF ENARGITE IN THE MANKAYAN DISTRICT, PHILIPPINES C. L. DEYELL†,1,*AND J. W. HEDENQUIST2
1 CODES,

the Australian Research Council’s Centre of Excellence in Ore Deposits, University of Tasmania, Private Bag 126, Hobart, Tasmania 7001, Australia of Earth Sciences, University of Ottawa, Ottawa, Ontario K1N6N5, Canada

2 Department

Abstract
We report the first laser ablation-inductively coupled plasma-mass spectroscopy (LA-ICP-MS) study of trace element substitution in enargite. Results indicate significant variability in the composition of enargite samples from a single ore system. Samples come from the Mankayan district, Philippines, which hosts the Lepanto high-sulfidation Cu-Au deposit, now mined out, and the adjacent Far Southeast porphyry Cu-Au deposit; the genetic relationship between these deposits has been documented in previous studies. LA-ICP-MS analyses indicate significant incorporation of Sb and Fe in enargite (locally exceeding 1 wt %). Other elements such as Bi, Sn, Se, Te, Ag, and Zn occur at concentrations exceeding 0.1 wt percent. The distribution of selected trace elements in enargite correlates with previously published variations in fluid inclusion homogenization and melting temperatures and gas compositions. The spatial distribution of data indicates enargite is enriched in Au and Te close to the Far Southeast porphyry. Enargite is enriched in Silver, Fe, and Pb in the center of Lepanto, and Zn (± Cd) is enrich the ore distal to the Far Southeast porphyry. Locally elevated Sb contents occur in samples from subsidiary branch vein structures and may indicate that mineralizing fluids along these structures were modified compared to those that formed the main orebody.

Introduction The Mankayan mineral district of northern Luzon, Philippines, is one of the richest mining districts in the Philippine archipelago. The region hosts several porphyry copper and epithermal precious and base-metal deposits, including the Lepanto high-sulfidation Cu-Au deposit and the adjacent Far Southeast porphyry Cu-Au deposit (Fig. 1). Several previous studies have documented the geologic (Garcia, 1991) and genetic relationship between the epithermal and porphyry systems (Arribas et al., 1995; Mancano and Campbell, 1995; Hedenquist et al., 1998; Imai, 2000; Chang et al., 2011), the latter based on fluid inclusion, stable isotope, and geochronological data. These studies have shown that the two deposits are genetically linked, and that the primary source of fluids responsible for both alteration and mineralization in the Lepanto system originated at depth within the Far Southeast porphyry system. Detailed studies of fluid inclusions in enargite have been instrumental in determining the genetic relationship between the Lepanto and Far Southeast orebodies (Mancano and Campbell, 1995; Lindaas et al., 1998). Enargite and luzonite occur as the most abundant sulfosalts in the Lepanto orebody, and also occur as an overprint to the upper parts of the Far Southeast porphyry system. Enargite is predominant in the southeastern part of the Lepanto deposit, near the Far Southeast system, whereas luzonite is dominant to the west (Imai, 1999). Studies have shown that fluid inclusions in the enargite record the overall progressive cooling and dilution of mineralizing fluids to the northwest, away from the Far Southeast
† Corresponding author: e-mail, c.wurst@comcast.net *Present address: Spectral International Inc., Arvada, Colorado.

porphyry system (Mancano and Campbell, 1995), and a more recent study of zoning in the earlier-formed alunite (Chang et al., 2011) is consistent with this northwesterly cooling. This district therefore provides an ideal site at which to examine trace element substitution in enargite, particularly in relation to zonation in or around ore deposits. Few other studies have examined the trace element variability in enargite, or other sulfosalts, in detail and these rely on electron microprobe data (e.g., Ackerman and Petersen, 1987; Takagi and Brimhall, 1998; Camprubi et al., 2001). In some cases, the concentration of elements such as Ag, Sb, Sn, V, and Pb within enargite have been shown to vary with distance from the center of the deposits. The development of laser ablation-inductively coupled plasma-mass spectroscopy (LA-ICP-MS) offers a reliable method for microanalyses of a diverse suite of elements at low detection limits. Several studies have applied this technology to the examination of trace elements in sulfides, and pyrite in particular (e.g., Norman et al., 2001; Morey et al., 2008; Cook et al., 2009; Pass et al., 2009), but the trace element chemistry of enargite, particularly across a deposit, has not yet been investigated with LA-ICP-MS. The objectives of this study are, therefore, to determine the suitability of LA-ICP-MS techniques for enargite trace element analysis, and to examine the range concentrations for a selection of trace elements. This study uses the same sample suite from the Mankayan district that was studied by Mancano and Campbell (1995) and Lindaas et al. (1998); our results define the zonation of trace elements in enargite across the Lepanto orebody. In addition, our study is the first to report trace element variability in enargite within an orebody and correlate the results with data from fluid inclusion infrared microthermometry on the same samples.

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identical in age (within analytical error) to the biotite alteration at depth. Mineralization occurred in both districts during the last 3 m. Fluid inclusion data indicate early quartz veins formed from hypersaline (50–55 wt % NaCl equiv) fluids at temperatures ~450° to 550°C (Hedenquist et al. pyrite. but the level of enargite ore is as shallow as 1. Geology and Ore Deposits in the Mankayan District The Mankayan district is located within the Luzon Central Cordillera. 1990. Bi-Te–bearing tennantite. Cu-Au mineralization (Figs. 1... 1. Near the southeastern end of the deposit. 2)..42 Ma (n = 5. Waters et al. 1). 1995) predates mineralization and is the principal host for the Lepanto orebody. 2000).. Map of the Mankayan district showing major geologic units and structures (based on mapping and compilation by LCMC Geological Staff.00 The Far Southeast porphyry Cu-Au deposit is centered on a shallow quartz diorite stock. Chang et al. The locations of major veins from the Victoria and Teresa mines are shown in bold black lines (projected to surface). Imai. 2) is largely controlled by the northwest-trending Lepanto fault. Cooke et al. Claveria et al. The unaltered Pleistocene Bato hornblende-biotite dacite postdates mineralization. 1991). 2011. Imai. 1995). At Lepanto.. 1991. Hedenquist et al. 1995...200 m to the northwest. Arribas et al. the oblique intersection of the Lepanto fault with east-west–trending branch faults.41 Ma (n = 6. 2000). and minor bornite. 1. 1995..1466 SCIENTIFIC COMMUNICATIONS FIG. Sajona et al. where it hosts the Lepanto orebody. which splay from the main 1466 . 1995). The geology of the Mankayan district consists of Cretaceous to early Tertiary basement. Garcia. (Arribas et al. Arribas et al. that intruded the basement Balili volcaniclastic unit. with the associated biotite dated at 1. that is. A large Miocene tonalite intrusion forms the western margin of the mineral district (Gonzalez. and Guinaoang). Chang et al. 1999. 1998. Garcia.. 1995).. comprising the Lepanto metavolcanic rocks (tectonized pillow basalts and basaltic to andesitic lava flows) and the Apaoan volcaniclastic rocks (Ringenbach et al. The ore interval is deepest at the southeast end. following the unconformity (Fig. Waters et al.. Mineralization is temporally and spatially related to PliocenePleistocene quartz diorite intrusions and dacitic volcanic rocks (Fig. Alunite within this alteration has been dated at 1. Fig.. These units are overlain unconformably by the Balili sequence (polymictic volcanic conglomerates). 2011).. 1991). Arribas et al. Mineralization is related to quartz stockwork veins with chalcopyrite. 1998. 1956. Garcia. 2011. 1956. Significant porphyry and epithermal mineralization occurs in both the Mankayan and Baguio districts of the cordillera (Fig. Also shown are the maximum extents of major orebodies (Lepanto..45 Ma (Arribas et al. as deep as 700 m elevation. dated at 1. 0361-0128/98/000/000-00 $6. Mineralization is also controlled by the unconformity between the Imbanguila dacite and the underlying basement rocks (Gonzalez. 2011). The Imbanguila hornblende dacite (2. 1991). Hollings et al. 1991. middle to late Miocene in age (Garcia.2–1. Arribas et al. 2002.y.. and rare native gold (Garcia.8 Ma. 2011. Cooke et al.. Far Southeast. 2). projected to surface. Quartz-alunite alteration occurs over the top of the porphyry and extends northwest. 2011). 2011..

6 wt % NaCl equiv. 3). in addition to the general northwestward flow of mineralizing fluids outward from the Far Southeast orebody (Mancano and Campbell.00 range from 4. A subset of the enargite samples (n = 12) was analyzed by electron probe microanalysis (EPMA) at the University of 1467 . from the top of the Far Southeast porphyry to the distal margins of the high-sulfidation deposit 2 km to the northwest. 2001). Claveria. The white line indicates the location of the Lepanto fault. 1995). Samples consisted of individual enargite grains. 2001). Lindaas et al. 2000). 2. They report higher N2/Ar and H2S/Ar ratios in samples from the branch veins. along with abundant pyrite. Mancano and Campbell (1995) examined the microthermometry of fluid inclusions hosted in enargite along a section from the Far Southeast porphyry to the Lepanto orebody (Table 1). Enargite and luzonite are the primary Cu sulfosalts. Hedenquist et al. Enargite crystals (Table 1) were taken from samples collected along the main Lepanto high-sulfidation orebody. Hedenquist et al. 1989. Imai.2 wt %). Schematic northwest-southeast cross section through the Lepanto and Far Southeast (FSE) deposits (from Garcia.. 1995). They showed a distinct cooling trend away from the porphyry center. galena. Chang et al.SCIENTIFIC COMMUNICATIONS 1467 FIG. 1956. Lepanto fault. as well as fluid inclusion and stable isotope data (Arribas et al. Garcia. 1998).. 1995. (1998). Methods of Analysis The sample suite used in this study is the same as that examined by Mancano and Campbell (1995) and Lindaas et al. and suggested upward flow of fluid along the branch fault intersections in the Lepanto orebody (Lindaas et al. and generally appears to be paragenetically later than the enargite-luzonite (Gonzalez. sphalerite. again from Far Southeast through to the Lepanto orebody. with a total 0361-0128/98/000/000-00 $6. The ore is hosted by strongly leached and silicified zones (with textures of both massive and vuggy quartz) that are surrounded by halos of quartz-alunite (± pyrophyllite. and diaspore. Mancano and Campbell.. Claveria. dickite. and lesser chalcopyrite and tetrahedrite-tennantite. using the same sample suite as Mancano and Campbell (1995).. all less than 1 cm in length. 1991). (1998) examined the composition of fluid inclusion gases (N2-CH4-Ar-H2SCO2-CH4) in enargite. A genetic relationship between the Far Southeast and Lepanto orebodies has been demonstrated previously by narrow age constraints. with an accompanying decrease in salinities (from averages of 3. kaolinite. Alteration and mineralization at Lepanto are typical of high-sulfidation epithermal deposits. 1998. Only one sample (U-85-21) had any visible mineral inclusions (tennantite). 2001). 1991). 1995. The main geologic units and the extent of epithermal Cu-Au and porphyry Cu-Au mineralization are shown (from Concepción and Cinco. Lindaas et al. with rare associated pyrite. 1998. combined with slightly higher salinities and homogenization temperatures (Th) of fluid inclusions from the same samples (Mancano and Campbell. results in a significantly wider ore zone (~400 m compared to ~100 m at its northwestern end...5 to 0. Rare Bi selenides and Sn-bearing phases (colusite) are also present (Claveria. 1998. and tellurides (calaverite and petzite).3 to 1. Gold mineralization is associated predominantly with tennantite-tetrahedrite and chalcopyrite. as well as samples from the hanging-wall and footwall branch veins (Fig. 2011).

Au. Details of LA-ICP-MS methodology.3 –1. 3.7 –1.7 –1. Cd. Cu.2 –1. projected to surface (based on mapping and compilation by LCMC geologic staff). As.9 Min Tm2 (°C) –2 –1.3 –1. Fe.2 –1. Sample locations are superimposed on shaded areas showing the maximum extents of the Lepanto (light gray) and Far Southeast orebodies (dark gray). 2-2-2 2-5-2 2-6-4 2-8-4 2-9-2 2-12-1 2-13-2 2-18-2 2-19-2 2-19-3 3-6-2 3-6-3 3-25-4 4-2-1 4-3-1 4-3-2 U-85-21 UTM northing 1864100 1864955 1865811 1865160 1865195 1864250 1863810 1865480 1864415 1864290 1864390 1865175 1864425 1864460 1865165 1864732 1864274 UTM easting 265475 264395 263591 264220 264520 265365 265240 263845 265115 265405 265225 264520 265230 264675 264325 264673 265846 Elevation (m) 950 1030 1030 1070 950 700 900 1000 700 1100 950 1000 850 1030 1030 1030 592 Location1 FW MOB NOA MOB HW MOB FW MOB MOB FW MOB HW MOB FW MOB MOB FSE Mean Th2 (°C) 249 166 207 225 230 206 198 201 209 248 231 220 224 194 207 285 Max Th2 (°C) 267 196 207 238 259 245 214 223 241 254 245 252 237 232 219 294 Mean Tm2 (°C) –1.7 –1. laser analysis. 0361-0128/98/000/000-00 $6.5 –1. In this study.6 –1. with an average of five analyses per sample (using 50nA and 5-µm spot size).3 –1. Mo.2 –2. (in press). W. Fe. The entire sample suite (n = 17) was analyzed by LA-ICP-MS techniques. and interpretation are documented by Large et al. Enargite Samples from the Mankayan District. Sb. (2009) and Danyushevsky et al. Sn.7 –1 –1. Pb. V. Sb.3 –1. and Bi (Table 3). HW = hanging wall. the enargite samples were analyzed by LAICP-MS for a total of 17 elements: Ti.5 –2 –1. Zr. Te.9 –2 –2.2 –1.4 –1 –1.7 –2. FSE = Far Southeast orebody 2 Data from Mancano and Campbell (1995) Tasmania to determine their major and selected trace element compositions. NOA = northern extension zone.2 –1.00 1468 . depending on the enargite grain size. Ag. 64 points were analyzed in total (Table 2).8 –1. Zn. also at the University of Tasmania.8 –2. including descriptions of instrumentation.3 –1 –1 –1. Multiple enargite grains were analyzed from each FIG. MOB = main orebody (Lepanto).1468 SCIENTIFIC COMMUNICATIONS TABLE 1. These samples were analyzed for seven elements (S. Se.3 –2. and Bi).3 –2. data reduction.6 Note: Also shown are corresponding fluid inclusion homogenization (Th) and ice melting temperatures (Tm) from Mancano and Campbell (1995) 1 FW = footwall. Spot size varied between 60 and 100 µm. Te. Philippines Sample no. sam- ple preparation. Map showing the location of all enargite samples analyzed in this study.7 –1. Ba.

9 0.3 3.05 3. As indicated in Table 5.77 18.06 99.1 0.9 0.88 48.81 18. 5).0 0. and Bi.7 3. with an average grade over the life of production of 3.26 0.65 17. 1994. The distribution of Sb to As ratios in the enargite (Fig.0 0.73 1. Claveria and Hedenquist. 60 to 100 µm for LA-ICP-MS analysis.27 16. Au is above detection in most enargite samples.60 18.0 0. fluid inclusions. but overall there are very few consistent elemental correlations in the enargite.0 3.9 0.03 48.3 ppm) close to detection. Te.69 1.0 1.59 0.05 99.9 wt percent Cu.0 0.SCIENTIFIC COMMUNICATIONS TABLE 2. with the exception of Cd. This compositional variability is due primarily to different combinations of Fe-Bi-Te-Sb-Sn-Se. In most cases.68 0. In general.12 48.9 0.26 48.4 0.0 0. with values up to 5. Te.28 100. and/or growth zones.1 0.4 g/t Au. EPMA values of minor elements Bi.07 99. Detection limits (averaged over all analyses) for the LA-ICPMS data are given in Table 4. and 2.g.07 99.1 2-2-2 32. Sb correlates weakly with Sn.88 17.0 0. Three distinct forms of Au occurrence are recognized in the Lepanto enargite.47 48.9 0.26 0. Te). Discussion Nature of Au in enargite The nature of Au in the enargite is of particular interest at Lepanto because Au was a significant contributor to the economic viability of the mine.19 0.0 0. 4) is variable. with the exception of rare Zr-bearing phases.79 0.03 99. Summary of Electron Microprobe (EPMA) Data for Selected Enargite Samples (data for each sample represents the mean of multiple data points) All samples Mean Wt % S Fe Cu As Sb Te Bi Total Fe Cu As Sb Te Bi 32. as well as inclusions containing variable combinations of Bi-Te-Sn-Fe (Fig.62 17.9 1.01 0. b).8 3.0 - 1469 4-3-2 32.21 48. 6a. 7b) and therefore it is thought to be structurally bound within the enargite crystal lattice (e. and particularly in Fe.06 0. and Mo (Table 4. and 70 ppm.78 18.1 1.and Sn-bearing phases (Tejada. and S for the majority of samples analyzed.0 0.19 0. compared with the EPMA beam (5 µm). V.64 1. There is significant variability in most elements analyzed.03 0.0 2-8-4 32.0 0. As. Ag-Bi.20 48.22 0. whereas this ratio is generally low in the main Lepanto orebody.2 0.1 1.0 1σ 0.9 3. 14 g/t Ag.0 2-9-2 31. in press). The larger beam size.0 0. Fig.65 18.13 99. Data reduction and quantification used stoichiometric Cu as the internal standard. Nearly all elements are consistently above ICP-MS detection limits (Table 3.9 3.11 99.02 48. most samples exhibit relatively simple compositional patterns determined from LA-ICP-MS (Fig.0 2-19-3 32. the latter largely from enargite (Chang et al.29 16.3 0.denotes below detection limit sample. Complex growth zoning was also noted locally.1 1. Analytical Results EPMA results EPMA analyses (Table 2) indicate near-stoichiometric enargite compositions of Cu.1 1.0 0. Fig.57 18.18 0.27 0. High Sb/As ratios occur in the branch vein structures. Both Bi and Te are consistently below detection for EPMA analyses. Danyushevsky et al. with mean values (2.0 0. In this study. LA-ICP-MS results A summary of enargite LA-ICP-MS data for each sample is given in Table 4.0 0. Weak correlations also occur between Ag-Sb.49 99. the Au exhibits smooth LAICP-MS traces in analytical traverses across enargite (Fig.28 48.0 0.5 3.02 48. 2011).0 0.0 2-18-2 32.79 17. provides a better estimate of the bulk composition of individual enargite grains and can be used to sample across small zones of compositional variability.48 0.1 0.0 3.0 4-2-1 32. 5).19 0. Both Cu and Au were mined from the deposit during large-scale mining operations from 1936 to 1996.66 1. with maximum values up to 70 ppm (Fig. moles based on 4 S Note: .7 3. Te-Se. Very few silicate inclusions are present.1 0.11 0.. 0361-0128/98/000/000-00 $6.0 3-6-3 32.1 0.60 2. 1989. The most common inclusion types are minor Au (± Ag. as discussed below. 28. selenides.17 100.. However. respectively). The Sb contents are variable.18 48.90 0.90 0.0 0.03 99.43 99..0 0.18 48.34 0.0 - No.0 1.03 100. and Te-Sb (Table 5).8 0.0 3-25-4 32.76 17.0 2-13-2 32.0 2-6-4 32.7 wt percent (sample 2-9-2).0 0.8 0.9 0. and the number of analyses per grain was dependent on crystal size.17 0.9 3.00 The compositional variability between multiple LA-ICPMS analyses of individual enargite crystals is due either to mineral inclusions. 2001).0 0. A direct comparison between the LA-ICP-MS and EPMA data cannot be made because the sample volume of the two techniques is significantly different.1 0. Previous studies have shown that the Au occurred mostly as electrum or in association with tellurides.89 0. based on the near-stoichiometric Cu/S ratios returned by EPMA analysis (Table 2). although locally very high values are reported in LA-ICP-MS results.16 48. Rare inclusions of native gold with elevated concentrations of 1469 .0 3.0 3-6-2 32. 6c).9 0. 5).0 3. and to a lesser extent with Te.1 0. Claveria. and Fe are below detection (with average detection limits of 16.0 3.1 1.

5 1.5 2.5 0.2 1.1 4.1 128.1 0.3 934.9 0.7 28.5 0.7 8.6 0.3 0.9 0.4 0.2 176.0 24.6 128.3 0.0 0.0 0.3 0.1 415.6 0.2 n/a 6.8 39.6 70.9 0.5 0.4 411.6 4.2 384.2 8.8 934.2 16.1 4.0 n/a 116.7 1.1 273.3 20.0 36.3 0.1 28.2 0.9 73.4 10.1 335.9 0.0 0.1 3.3 17.1 0.0 11.2 1.4 1.9 0.2 114.1 0.6 0.2 1.7 6.4 0.1 0.6 0.5 0.3 0.0 77.0 0.2 8.9 550.5 0.9 0.6 18.4 n/a 64.2 30.8 1132.2 30.6 3.1 1.3 15.1 10.7 7.8 34.8 0.4 .7 66.1 2.6 59.6 1.2 18.1 1.2 2.5 0.2 8.8 0.9 83.9 24. Element 2-19-3 (n = 6) Mean 1σ Ti (ppm) V (ppm) Fe (ppm) Zn (ppm) Se (ppm) Zr (ppm) Mo (ppm) Ag (ppm) Cd (ppm) Sn (ppm) Sb (%) Te (ppm) Ba (ppm) W (ppm) Au (ppm) Pb (ppm) Bi (ppm) 13.6 20.0 n/a 1.6 33.4 0.0 0.2 14.2 0.3 17.9 0.7 2.3 4.0 n/a 729.3 0.7 1.1 41.6 3.1 0.7 0.3 72.4 99.8 128.9 0.9 997.7 0. Summary of LA-ICP-MS Data for Mankayan Enargite Samples 2-5-2 (n = 3) Mean 1σ 7.0 n/a 39.0 1716.5 0361-0128/98/000/000-00 $6.5 0.3 9.9 200.4 2498.5 39.7 0.4 88.5 0.5 88.2 0.3 243.7 0.8 15.8 2.1 0.5 0.1 0.6 120.8 4.2 0.1 36.0 157.2 0.1 6.3 86.0 15.8 90.5 2.6 2.7 960.9 142.7 149.0 2.1 0.1 41.1 21.4 0.1 6.3 32.4 0.9 0.6 140.0 1.0 10.1 0.9 10.6 65.1 17.4 1414.2 0.3 0.7 2.5 24.3 115.0 0.2 1.0 2.5 188.3 17.3 4-3-2 (n = 6) Mean 1σ 10.7 0.8 192.8 0.1 0.6 2.0 n/a 12.8 11.0 67.2 0.3 0.5 0.2 0.9 0.0 3.1 0.6 108.1 164.9 0.0 n/a 527.9 57.3 2.6 0.9 0.9 26.4 0.4 2-6-4 (n = 5) Mean 1σ 2-8-4 (n = 5) Mean 1σ 2-9-2 (n = 5) Mean 1σ 2-12-1 (n = 4) Mean 1σ 2-13-2 (n = 7) Mean 1σ 2-18-2 (n = 4) Mean 1σ 2-19-2 (n = 5) Mean 1σ 38.0 0.1 33.6 452.1 0.6 0.5 0.2 81.0 21.2 27.2 0.6 1.6 167.4 16.7 10.6 0.6 5.4 1.7 0.9 0.5 6.1 22.6 1154.0 n/a 0.2 n/a 0.7 3-6-3 (n = 7) Mean 1σ 3-25-4 (n = 6) Mean 1σ 4-2-1 (n = 5) Mean 1σ 4-3-1 (n = 3) Mean 1σ 8.0 2.1 641.5 10.8 46.5 9.9 425.9 207.8 2.9 0.0 2.3 77.1 2.9 3.6 0.4 0.5 2318.5 0.0 0.1 114.4 0.0 4.0 611.6 1.2 0. Element 2-2-2 (n = 6) Mean 1σ Ti (ppm) V (ppm) Fe (ppm) Zn (ppm) Se (ppm) Zr (ppm) Mo (ppm) Ag (ppm) Cd (ppm) Sn (ppm) Sb (%) Te (ppm) Ba (ppm) W (ppm) Au (ppm) Pb (ppm) Bi (ppm) 10.4 93.8 11.5 127.8 6.1 78.7 2.3 0.7 2.9 0.8 0.5 0.3 164.5 38.1 0.5 0.3 n/a 0.6 8.0 0.0 0.9 2.3 984.1 28.7 11.9 708.7 n/a 0.9 10.1 385.6 21.0 0.9 0.6 21.2 0.1 0.5 3.1 18152.8 2.1 n/a 0.0 0.0 n/a 34.4 7.3 1058.4 1.2 27.8 0.5 100.9 0.5 1.0 0.1 0.8 66.0 229.4 9.5 10.0 0.0 58.2 506.7 17.1 0.1 41.7 530.4 5.2 0.2 68.5 200.8 0.1 0.3 824.0 0.1470 TABLE 3.1 1.6 0.7 0.1 1.7 0.4 22.9 19.8 0.2 0.5 5.5 432.7 30.00 SCIENTIFIC COMMUNICATIONS Sample no.6 0.4 13.2 13.8 0.0 9.9 9.9 344.2 40.1 4.9 0.6 83.1 1.8 2.5 1.3 0.1 0.0 0.6 2.7 0.5 52.0 6.8 0.0 0.1 77.1 0.1 190.9 22.0 19.0 0.7 0.6 0.6 0.2 682.8 9.1 32.6 92.5 46.2 344.6 0.0 0.8 0.3 U-85-21 (n = 3) Mean 1σ 6.4 14.7 7.7 0.0 21.0 694.8 3.6 33.4 1134.4 1.1 9.4 0.1 0.4 0.8 6.1 5.4 2.1 n/a 1.8 13.0 0.5 12.4 0.1 0.6 0.0 0.3 0.4 0.6 1316.7 0.5 0.3 0.6 178.5 6.5 44.4 0.9 235.1 0.3 460.9 2.4 151.8 108.7 0.8 n/a 28.9 80.6 39.4 0.5 19.2 0.2 5.0 0.0 0.8 3-6-2 (n = 7) Mean 1σ 11.4 7.3 851.2 70.2 85.8 0.4 1.1 37.5 875.0 58.5 352.0 0.1 24.2 n/a 5.6 510.5 1.1 5.4 368.3 1701.1 0.8 43.2 0.1 75.0 21.5 38.3 29.8 3.2 13.2 0.4 0.3 1.1 0.4 817.9 100.5 34.9 133.1 0.3 1.0 2.3 13.6 10.7 0.4 49.2 1.4 29.1 1.2 41.6 0.5 378.6 0.1 134.0 900.2 645.1 1.0 1.6 2.0 0.0 n/a 1.2 0.5 0.8 28.8 35.1 0.9 0.0 7441.1 104.1 4.2 143.0 653.3 8.1 1.0 0.6 604.2 34.4 1.1 2.4 2.0 n/a 1.2 0.0 8.1 2.2 0.2 15.5 10.5 306.5 559.1 1.6 0.0 0.6 3.3 0.0 0.9 205.3 2.5 61.0 8.1 0.1 5.4 0.4 0.4 57.7 0.6 20.1 16.2 0.6 3.9 0.5 19.5 0.1 1128.3 194.5 200.8 387.8 0.0 0.0 n/a 0.4 48.8 1470 Sample no.4 0.4 3.4 0.4 115.5 647.4 0.2 650.9 221.

1 Zr 0.03 0. based on mean wt percent EPMA results.SCIENTIFIC COMMUNICATIONS TABLE 4. 0361-0128/98/000/000-00 $6.1 Sb 0.03 0. Map showing 100*Sb/As ratios in enargite.2 0. Range of enargite LA-ICP-MS trace element data for all analyses in this study (as ppm).0 Sn 0.03 0.3 Ag 0.14 2.38 0.0 Fe 4.2 Te 0. 4.0 Au 0.3 0.0 Mo 0.0 Cd 1. projected to surface. The mean of all analyses and mean detection limits (DL) for each element are also shown.04 0. 5.02 0.0 1471 Bi 0.0 Zn 0.08 0. white circles are from the main Lepanto orebody and northern extension zone.03 1.00 1471 .32 0.17 0. LA-ICP-MS Detection Limits (values in ppm) Element Mean 1σ Ti 0.1 Ba 0. Sample locations are superimposed on shaded areas showing the maximum extents of the Lepanto (light gray) and Far Southeast orebodies (dark gray).09 0.2 V 0.02 0.0 Pb 0.1 Se 1. FIG.0 W 0.33 0.03 0.0 Note: Data shown are average values for all analyses in this study FIG. Gray circles represent samples taken from hanging-wall and foot wall branch veins.

Photomicrographs and raw LA-ICP-MS element data (shown as element counts over time) for selected enargite samples. Black circles on photographs indicate the locations of associated LA-ICP-MS analyses. 0361-0128/98/000/000-00 $6. 6. (C) Sample U-85-21.1472 SCIENTIFIC COMMUNICATIONS Counts 100 10 0 20 40 60 80 100 120 Time(s) 100000 Counts 100 10 0 20 40 60 80 100 120 Time(s) 100000 Counts 100 10 0 20 40 60 80 100 120 Time(s) FIG. (B) Sample 2-19-2. Scale bar = 100 µm.00 1472 . (A) Sample 2-12-1.

0 0.1 0.0 0.0 -0. 1998). Similar trends are observed between Bi and Se with respect to fluid inclusion Tm measurements (Fig. However. 8).1 0.2 0.0 0. In contrast.1 0. Skinner.0 0.0 1.3 1..0 0.1 0.1 0. Fig 8c).0 0.3 1.0 0.0 0. and gradually increase to a maximum (>10 ppm) at Th values of ~210°C (Fig. 8a).0 0.0 0.0 0.0 0. Hedenquist et al. In contrast.0 0.0 0.0 0.1 0.0 0. 1969).0 0.0 0. Ackerman and Petersen. 1998. although specific element enrichments or depletions appear to vary between deposits (e.g.0 0. 7a). Correlations of Pb and Te (Fig.3 0.1 0.0 0. corresponding to enargite mineralization that overprints the Far Southeast porphyry in a hydrothermal breccia (sample U85-21). Te values exhibit an overall positive trend with respect to Th (Fig.1 0. Mo. Average Pb concentrations are lowest (<1 ppm) in samples with the highest recorded Th measurements.1 0.0 0.0 0. averaging about 4 mol percent Cu3SbS4. Correlation Matrix Showing “r” Values of Elements Based on Average LA-ICP-MS Results Ti Ti V Fe Zn Se Zr Mo Ag Cd Sn Sb Te Ba W Au Pb Bi 1.0 0. d).0 0.2 0.1 0. Pósfai and Buseck.0 0.0 0.1 0. there is poor correlation between the datasets and few trends are present. but there is no consistent zonation in Sb values away from the Far Southeast deposit or the Lepanto main orebody.g..SCIENTIFIC COMMUNICATIONS TABLE 5. there is no similar trend in samples from the branch veins.. we suggest that the variation in Sb/(Sb+As) content of the enargite can be attributed to different fluid pathways and different fluid compositions.0 0.0 0.0 0.1 1.3 0.0 0.0 0.1 0.0 0. 8c.0 0.0 0.2 0. Te.00 Sb substitution in enargite The nature and temperature dependence of Sb substitution in enargite is well documented in studies of phase relationships between enargite and the luzonite-famatinite solid-solution series (e. as well as temperature. 9) indicates that there is a broad trend of increasing Sb/(Sb+As) with decrease in temperature in samples from the main Lepanto orebody and northern extension zone. which formed at the lowest temperature. 8a.0 0.1 1. with the lowest Se values corresponding to the lowest salinity measurements. Takagi and Brimhall. Chang et al.2 0. perhaps due to Bi remaining in high salinity solutions. In most samples.0 0.0 0. low Bi correlates with high salinity. there is a strong association of Au with anomalies of Fe-Ag-Pb-Bi ± Sn.1 0. Mineralizing fluids within the branch veins had generally higher Sb/(Sb+As) ratios compared to the predominantly northwestward flowing fluids sourced from the Far Southeast porphyry (e.0 0.0 0.0 0. These data suggest that temperature is not the only factor that determines Sb concentrations in enargite at Lepanto.0 0.0 0.0 0.0 0.0 0..0 0. 7c).0 0.1 V 1.4 0. Maske and Skinner.0 0.1 0.1 1.4 1.1 0.1 0. and only a few analyses had values above 10 mol percent Cu3SbS4 (Table 2).0 0. The highest Sb/(Sb+As) ratios occur in the branch vein structures (Fig.4 0.4 0.3 0.1 0.0 0. Studies have shown that Sb can substitute in the enargite crystal structure up to a maximum of about 20 mol percent Cu3SbS4 (Springer.0 0.6 0.2 Fe Zn Se Zr Mo Ag Cd Sn Sb Te Ba W Au Pb 1473 Bi 1. relatively lower Te concentrations occur at the highest Th value.e. Camprubi et al..0 0.0 0.1 0. The third occurrence of Au is as complicated growth zones and/or multi-element inclusions within the enargite (Fig.0 0.1 0. 1960.1 1.2 0. selected elements show some trends with respect to either homogenization temperature (Th) or fluid salinity (Tm) (Fig. However.2 1.0 0.1 0.0 0.1 0.0 0.0 0.0 0.g.1 0.0 0.0 0.2 0. due to the large range of LA-ICPMS results for individual elements within a single enargite sample. 1998). In the present study.2 0..0 0. 1971.1 0. 1987.1 1.1 0.1 0. 9). which have variable Sb/(Sb+As) over a range of temperatures.0 0.3 1.0 0.0 0.3 1.0 0. and Pb also occur in the enargite (Fig.1 0.0 0.0 0.2 0. 1473 .2 0.1 0.4 0.1 0.0 0. A comparison of Sb/(Sb+As) ratios in samples from the deposit to fluid inclusion homogenization temperatures (Fig.0 0. Se concentrations exhibit a weak positive correlation with respect to fluid salinity.0 0.1 0. In these analyses of growth zones and/or inclusions.0 Ag. i. A strong negative correlation occurs between Bi and increasing fluid salinity (lower Tm values.2 0.0 0. Sb contents of the enargite are low.1 0.0 0.. 8b). b) to fluid inclusion homogenization temperatures show opposite trends.2 0.0 1.0 0.0 0.2 0.0 0.0 0.1 0. using the data from Mancano and Campbell (1995) (Table 1).1 0.0 0.3 1. 1998).0 0. (2011) found a similar pattern in terms of Pb having the highest concentration in alunite samples that are distal.1 0.4 0. Comparison with fluid inclusion measurements Direct comparison of the enargite LA-ICP-MS data (Table 4) and fluid inclusion homogenization and melting temperature measurements can be made for the same samples. However. Given the results of the fluid inclusion gas study and the recognition of additional fluid input along the branch structures (Lindaas et al.0 0.1 0. 0361-0128/98/000/000-00 $6. Spatial distribution of trace elements in enargite Trace element substitution in Cu sulfosalts has previously been shown to vary with distance from some epithermal orebodies.

10 0 20 40 60 80 100 120 Time(s) 0361-0128/98/000/000-00 $6. and (C) Sample 4-3-2.00 1474 . (A) Sample 3-25-4. 7. (B) Sample 3-6-3.1474 1000000 SCIENTIFIC COMMUNICATIONS 100000 10000 Counts 1000 100 10 0 20 40 60 80 100 120 Time(s) 10000000 1000000 100000 Counts 10000 1000 100 10 0 20 40 60 80 100 120 Time(s) 10000000 1000000 100000 Counts 10000 1000 100 FIG. Raw LA-ICP-MS element data (selected elements only) for selected Au-bearing enargite samples showing variability of Au occurrences.

c: Bi.SCIENTIFIC COMMUNICATIONS 100 A 1475 10000 B 10 1000 Pb (ppm) Te (ppm) 180 210 240 270 300 100 1 10 0. 100 MOB & NOA FW & HW Sb/Sb+As *100 10 1 0.75 100 100 10 10 1 1 -2 0. Scatter plot showing enargite EPMA 100*Sb/(Sb+As) (element levels as wt %) compared to mean fluid inclusion homogenization temperatures (Th) from Mancano and Campbell (1995).1 1 0.25 -1 -0.00 FIG.5 -1. Fluid inclusion data from Mancano and Campbell (1995). MOB = main Lepanto orebody.75 -1. Abbreviations: FW = footwall. 1475 . d: Se) with fluid inclusion homogenization (Th) and average melting (Tm) temperatures.01 150 0. 9.1 150 180 210 240 270 300 mean Th (°C) 10000 C mean Th (°C) 10000 D 1000 1000 Bi (ppm) Se (ppm) -1. b: Te. NOA = northern extension zone.75 -1.1 -2 -1. Errors shown are 1 standard deviation on EPMA measurements. HW = hanging wall.5 -1.75 mean Tm (°C) mean Tm (°C) FIG.1 150 170 190 210 230 250 270 mean Th (°C) 0361-0128/98/000/000-00 $6. Comparison of selected LA-ICP-MS trace element contents of enargite (a: Pb.25 -1 -0. 8.

combined with variations in elements such as Au and Zn. Results indicate significant variability in trace element compositions of enargite samples from a single ore deposit. Concepción.. Steele for assistance with electron microprobe analyses. R. East Tintic district. T.. elevated Sb and Sb/(Sb+As) ratios in the enargite occur in samples from the branch vein structures. General trends in the spatial distribution of some elements suggest enrichment in Au and Te (in particular) close to the Far Southeast porphyry system. Our results have implications for exploration around enargite-rich high sulfidation ore deposits. to a lesser extent. 1995. The footprint of the Lepanto and Far Southeast deposits are indicated.10a. Sn. to a lesser extent. there is significant variability in some elements between individual grains and/or samples.. 10e. white circles are from the main Lepanto orebody (MOB) and northern extension zone (NOA). b). Fe and Pb in the center of the Lepanto orebody. Only enargite is enriched in Sb within the branch vein structures. 337–340. As noted above. a greater degree of wall-rock interaction. and telluride accessory phases in the deposit (e. the average of Fe is typically <0. the most abundant trace elements recorded in the enargite are those that also form discrete sulfosalt. 0361-0128/98/000/000-00 $6. where the paleotemperatures were the highest (Mancano and Campbell. Lateral variations in the trace element geochemistry of enargite.]: Geological Society of America Abstracts. by contrast. Conclusions We report the first LA-ICP-MS study of trace element substitution in enargite.01 wt percent. Gilbert for technical assistance with the LA-ICP-MS instrument.3 wt percent. based on both EPMA (Table 2) and LA-ICPMS analyses (Table 4). Hobart. 2001). J. A. averaging 1. a) Au. Hedenquist.. that mineralizing fluids introduced along the branch veins were distinctly different compared to those that flowed from the Far Southeast porphyry northwest along the Lepanto fault to form the main orebody. thereby providing explorers with the best chance of locating any cogenetic porphyry-style mineralization. or both. d) Pb. V (Fig. p. are consistent with the conclusion of Lindaas et al. Enargite is enriched in elements such as Ag and. (1998). Comments and contributions by D. whereas concentrations of Au and Zn are highest in enargite from the main Lepanto orebody and the overprint to the Far Southeast system (Fig. Arribas. who suggested a distinct upflow of mineralizing fluids along the branch vein structures.. and Petersen. from distal Zn enrichment to proximal Ag. Jr.W. with lower Au but higher Sb contents. Ag and Zn are also present at values exceeding 0.00 1476 . Similar results are recorded in the Mankayan district. Elements such as Sn and Te show little variability between the main orebody and branch vein structures. b) Te. f). Claveria and Hedenquist. 1995).. 1995. as ICP-MS detection limits are one to two orders of magnitude lower than electron microprobe levels. LCMC is acknowledged for approving the use of updated geological maps and information. 1995). Pb (Fig. Danyushevsky for assistance with interpretation of LA-ICP-MS data. Te. Contemporaneous formation of adjacent porphyry and epithermal Cu-Au deposits over 300 ka in northern Luzon. These data. These data are consistent with the conclusions of Lindaas et al. Sample locations are superimposed on shaded areas showing the maximum extent of the Lepanto (light gray) and Far Southeast orebodies (dark gray). 23. Gray circles represent samples taken from hanging-wall and footwall branch veins.R. Acknowledgments This study was funded by a NSERC PDF fellowship to C. Results from this study of the Lepanto deposit indicate significant incorporation of Sb in enargite. with analytical expenses funded through CODES. and Garcia. to a lesser extent. 19 (7). Fe. T. White are gratefully acknowledged. Plan maps showing trace element contents of enargite based on mean LA-ICP-MS results. v.. e). L. FIG.A. and f) Cd. nor the temperature. this branch vein fluid may have had a slightly different composition to the fluid originating from the Far Southeast porphyry and that flowed along the Lepanto fault. Claveria. p. where 70 percent of the ore originated. 10c).1 wt percent. e) Zn.. 1994. and. whereas Zn (± Cd) enrich the enargite distal to the Far Southeast porphyry. 1995). D. Te. and Pb enrichment. c) Ag.. Philippines: Geology. Cd (Fig. Other elements such as Bi.1476 SCIENTIFIC COMMUNICATIONS 2001). 1998). 10. Centre of Excellence in Ore Deposits. Mancano for providing the polished samples from his original study of fluid inclusions in enargite.. D. along with Fe and. Itaya. selenide. Critical reviews by James Pope and David John are appreciated. Mineral chemistry of tennantite in the Trixie mine.. REFERENCES Ackerman. E. however.S. Enargite samples close to the Far Southeast porphyry system are relatively enriched in elements such as Au. The distribution of some trace elements in the enargite samples from Lepanto can be related to systematic variations in fluid inclusion homogenization and melting temperatures (Mancano and Campbell. 9a). where several elements are preferentially enrich or deplete the ore relative to their distance from the Far Southeast porphyry (Fig. (1998). 1987.U. 657. Deyell. as well as broad changes in fluid inclusion gas chemistry (Lindaas et al. projected to surface. Arribas et al. (in press) for analysis of pyrite and other sulfides is also applicable to enargite. Se. may help to locate the center of hydrothermal activity.. 10a. v. and S. The distribution of elements between enargite samples in the main Lepanto orebody is also different to that within the branch vein structures. Utah [abs. We thank D. This may have been caused by a different fluid ascent path.g. In general. Cooke and N. where temperatures were lower (Mancano and Campbell. Okada. to a lesser extent. The only elements that enrich the northwestern distal extent of the Lepanto deposit are Zn and. 10). Our results indicate that the trace element content of enargite is influenced by a range of factors and does not solely reflect the composition of the mineralizing fluids. The LA-ICP-MS technique has significant advantages over EPMA analysis. The methodology described by Danyushevsky et al. Locally. Jr. J.. The main Lepanto orebody is preferentially enriched in Ag near the core of the epithermal deposit (Fig.

00 1477 .SCIENTIFIC COMMUNICATIONS 1477 0361-0128/98/000/000-00 $6.

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