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MINERALOGY OF THE CALCITE-FLUORITE VEINS NEAR LONG LAKE, NEW YORK.

Interesting specimens of calcite, fluorite colored by dysprosium, chamosite, kainosite-(Y) and other minerals have been found in fresh roadcuts along New York State Route 30. The veins, exposed in 1995, have since been covered and are no longer accessible.

INTRODUCTION

Long Lake is located in Hamilton County, New York, a region of the state not well known for producing mineral specimens. Thus considerable interest attended the recent discovery of unusual calcite, fluorite and other minerals in veins cutting granitic gneiss exposed along State Route 30, 11.4 km north of Long Lake, at 44[degrees]02'42" N latitude, 74[degrees]31'16" W longitude.

These veins were exposed by blasting carried out in August of 1994 by the New York Department of Transportation as part of a road-widening project. The veins were visited by a few local collectors, but became more widely known by early 1995. Because of the orientation of the veins and their limited extent, accessible minerals were quickly removed by collectors. By May 1995, nearly all in situ minerals worthy of collecting had been removed to a depth of about 2 meters. By summer 1995, the area had been graded and seeded, the outcrop had been tarred, and specimens ceased to be available. For all practical purposes, collecting at this locality was limited to less than six months, during which many specimens of interest to both collectors and scientists were recovered.

GEOLOGY

The bedrock geology in the vicinity of the Long Lake calcite-fluorite veins is complex, consisting of a number of structurally deformed sedimentary and igneous rocks that have been metamorphosed to granulite facies. The calcite-fluorite vein occurrence itself is hosted by one such unit of granitic gneiss. The age of the veins is presently unknown, but is assumed to be post-metamorphic, based on field observations. Sm-Nd isotope studies currently underway may provide insight into the actual time of mineralization (Robert Darling, personal communication, 1997).

Two principal veins are located near the northern end of the outcrop on the west side of the road. These closely-spaced veins strike approximately 3000 (magnetic), have near-vertical dips, and are exposed for approximately 20 meters along the steeply inclined outcrop. Slim Pond, approximately 3.5 km to the south, has a parallel strike, suggesting a possible fault set in that orientation. Brecciation prior to or during mineralization is evidenced by blocks of gneiss "floating" in the mineral assemblage. Later crosscutting micro-faults and rare slickensided fluorite crystals indicate at least minor post-mineralization movement.

Similar veins exposed along the outcrop to the south and east are also mineralized, but are quite narrow (2 cm or less) and contain few pockets. While some specimens were retrieved from these smaller veins, most came from the two major veins described above.

MINERALOGY

The mineral assemblage of the Long Lake veins is a hydrothermal suite dominated by calcite and fluorite, but including chamosite, hematite, pyrite, quartz, cerian epidote and the rare mineral kainosite-(Y). The paragenetic sequence (Fig. 2) is complex, and clearly involves at least two stages of calcite deposition and several distinct stages of chamosite deposition.

Crystallization of fluorite and calcite incompletely covered the vein walls, leaving many cavities which were filled in by later-formed minerals. As a consequence, late-stage minerals can be found both on the vein walls and coating earlier-formed minerals. Thus the order of deposition of different minerals is not reliably reflected by their distance from the vein walls.

Calcite Ca[CO.sub.3]

Calcite occurs as crystals of two generations which bracketed the main period of fluorite deposition. Crystals of the two generations have quite different habits. Calcite-I, which was the first mineral to crystallize (with the exception of a thin layer of chamosite which often coats the vein walls), forms rhombohedral crystals, usually twinned on {00011}. These generally grew attached to the vein walls by one edge or corner of the triangleshaped twin. This habit is similar to that of some calcite from the Rossie lead mines in St. Lawrence County, New York.

Calcite-II often forms crystalographically continuous overgrowths on calcite-I, but has a prismatic habit and is generally untwinned. The most common habit of calcite-II has short prisms with rounded pinacoidal terminations which are typically opaque white. When these occur as overgrowths on calcite I, they sometimes fail to obscure the apex of the first generation rhombohedron, which is visible as a small protrusion or as a darker spot in the middle of the rounded white termination.

A different, less common habit of calcite-II occurs as lustrous elongate prismatic crystals modified by a well-defined pinacoid and usually also the rare hexagonal dipyramid {7.7.14.2} They are transparent and colorless to very pale yellow, with horizontal striations on their prism faces. They easily might be mistaken for quartz crystals with unusual terminations. Careful goniometric study shows that the "prism" actually consists of faces of the true prism {1010}, which are strictly parallel to the c-axis, alternating with faces of a very steep positive rhombohedron such as {36.0.36.1}, which are consistently inclined to the c-axis by 1 to 1.5[degrees].

The two habits of calcite-II probably represent successive, closely spaced crystal growth events. While most of the elongated crystals were found loose, and many stubby crystals lack any apparent later overgrowth, a number of specimens preserve elongate crystals which at least partly overgrew stubby ones. No change in the stubby calcite or precipitation of other minerals appears to have occurred before the growth of the more elongate crystals, and no examples of the stubby calcite overgrowing elongate calcite have been seen. Thus, the two habits appear to represent two episodes of growth which occurred in relatively quick succession.

Fluorite [CaF.sub.2]

Fluorite occurs in approximately equal volume with calcite in the Long Lake veins, and has features which make it of interest to collectors and earth scientists alike.

The typical Long Lake fluorite crystal is between 1 and 2 cm in size, nearly colorless to blue-purple, and of octahedral habit but with irregular regions where the points of the octahedron should be. These irregular regions are composed of many small parallel "points" of octahedral habit on platforms of earlier cube faces. The overall morphology documents the incomplete transition from a cuboctahedral habit to an octahedral one.

Many crystals have dark olive-gray cube-shaped centers, which represent the initial morphology of the crystals. Occasionally, 1 to 2-mm gray cubic crystals, often overgrown with a thin rind of colorless fluorite, are found enclosed in calcite-I. These represent crystals which were arrested early in their growth when calcite crystallized around them. Other small crystals ([less than]1 cm) which apparently began to form relatively late, show simple octahedral morphology and lack the dark cube-shaped central zone. Some are colorless or evenly colored throughout, but others have color bands delineating former cube faces on a cuboctahedral crystal, now thoroughly grown out into the pure octahedral form.

While the overall color of individual crystals ranges from nearly colorless to blue-purple, most crystals show the typical occluded core, and many show other color zonation as well. Most common is a thin, dark blue zonation in the position of the cube face overgrown by octahedral "points" (Fig. 9), with subtle variations of color intensity best seen in sections of crystals (Fig. 10). These more subtle color variations include concentric patterns which probably represent changes in trace element composition on faces of a given form over time (growth zonation), and radially arranged patterns which indicate differential trace element incorporation into faces of different forms (cube and octahedron) growing at the same time (sectoral zonation). (For a discussion of these types of zonation, see Rakovan and Waychunas, 1996.)

Synchrotron X-ray fluorescence studies show that the fluorites are sector zoned with respect to the trace elements Sr, Y and the rare earth elements. The sectors under the octahedral faces are enriched in these elements relative to the cube sectors (Rakovan, 1998). Segregation of these elements between the cube and octahedral sectors may be due to different growth rates on the cube and octahedron faces or differences in their atomic structures.

The apparent colors of typical crystals vary with the source of light. In daylight and standard fluorescent light they appear blue to blue-gray, but in incandescent light they take on a warmer color, reaching a magenta-blue in halogen light. Very rarely, pale green and aqua colors of fluorite have been seen, but these specimens were not found in place, and may have come from a different vein. No euhedral crystals with these colors were recovered, and consequently their habit and position in the paragenetic sequence is unknown.

When crystal sections of typical fluorite are examined by cathodoluminescence an even stronger and more striking color zonation in various shades of blue, green and purple is revealed (Figs. 11 and 12). The calcite-I on which the fluorite grew shows a strong orange-red luminescence. The pattern of banding in the fluorite revealed by cathodoluminescence reinforces the above interpretation of the morphological development of these crystals, summarized in Figure 13.

Analyses of the luminescence spectrum of fluorite were made by John Hanchar of Rensselaer Polytechnic Institute, using a Patco ELM-3 luminoscope (12 kV, 0.7 mA, [sim]l5m Torr vacuum, working range 440-770 nm with 8 nm/step, 40 steps total, calibration with a Hg-Ar lamp). The results (J. Hanchar, personal communication, 1995), reproduced in Figure 14, indicate that the major element responsible for the luminescence is the rare earth element dysprosium, with possible contributions from terbium. Dysprosium was also identified as a constituent in kainosite-(Y) (see below). Since the intensity of the peaks in luminescence spectra bears no simple relationship to concentration, the concentration of dysprosium in the fluorite cannot be inferred from these observations. Wavelength-dispersive electron microprobe analyses of typical fluorite did not detect any elements other than Ca and F (method detection limit for REE [sim]200-600 ppm; [sim]100 ppm for most other elements).

Typically, larger fluorite crystals are attached to the edges of calcite-I crystals, which in turn are attached to the vein walls or their initial chamosite coating. While some fluorite is attached directly to the vein walls, most of the crystals formed on earlier minerals. The geometry of many specimens indicates that the rhombohedral crystals of calcite-I tended to grow with their c axes parallel or sub-parallel to the vein walls. This is the configuration which would allow the crystals to most rapidly reach the interior of the vein where saturated fluids would facilitate further growth. Crystals which started growth in less favorable orientations either grew more slowly, or may even have dissolved again. This model is consistent with the concept of geometric competition (Grigor'ev, 1965). The maze of calcite crystals encrusting the vein walls when fluorite deposition started may have decreased fluid flow through the vein margins, initially allowing fluorite to grow faster in open spaces more interior to t he veins. Later, conditions favoring nucleation at many sites produced numerous smaller crystals.

Chamosite [([Fe.sup.2+],[Mg,[Fe.sup.3+]).sub.5]A1([Si.sub.3]A1)[O.sub.10][(OH,O ).sub.8]

Three generations of chamosite are present in the Long Lake veins. The earliest consists of a thin, dark green coating on the vein walls. The middle generation occurs as dark green hemispheres of well-formed platy crystals, often perched on calcite-I, and sometimes associated with cerian epidote. Some of this chamosite makes small but attractive specimens. The latest generation is a yellowish to olive-green late-stage void filling or coating on minerals exposed in open pockets. In some cases, this chamosite occurs as golden colored platy crystals and flakes.

Electron microprobe analyses of chamosite of the second and third (golden phase) generations yielded the following empirical formulae ([Fe.sup.2+], [Fe.sup.3+] and OH determined by stoichiometry):

Chamosite-II ([Fe.sub.3.74][Mg.sub.1.19][A1.sub..06][Mn.sub..04][Ca.sub..01])A1([S i.sub.2.86][A1.sub.1.14])[O.sub.10][(OH).sub.8]

Chamosite-III ([Fe.sub.3.61][Mg.sub.1.16][Ca.sub..20][Mn.sub..02][K.sub..02])([A1.s ub..93][Fe.sub..07])([Si.sub.3.16][Al.sub..84])[O.sub.10][(OH).sub.8]

The major differences between these two are that chamosite-III has more calcium, is relatively Si-rich (at the expense of Al), and probably contains some [Fe.sup.3+].

Epidote [(Ca,Ce).sub.2][(Al,Fe).sub.3][([Si0.sub.4]).sub.3](OH)

A rare-earth-bearing epidote-group mineral occurs abundantly as microscopic hemispherical aggregates of bladed olive-brown crystals attached primarily to calcite-I and fluorite. Crystals which are undamaged can form attractive microspecimens, but most crystals which occur in open pockets are damaged.

Electron microprobe analysis of one sample yielded the following formula ([Fe.sup.2+], [Fe.sub.3+] and OH determined stoichiometrically):

([Ca.sub.1.24][Ce.sub..40][La.sub..18][Nd.sub..15])([Al.sub.1.65][[Fe .sup.3+].sub..01])[([Si.sub.1.03][O.sub.4]).sub.3](OH)

This indicates that allanite-(Ce) may be present too.

Hematite [Fe.sub.2][O.sub.3]

Hematite occurs as red earthy material, often found in the centers of hemispherical clusters of cerian epidote attached to fluorite, and sometimes as coatings on internal fractures in calcite-I. Less commonly, hematite is found as metallic black platy crystals ([less than]1 mm) that show ruby-red highlights produced by internal reflections. X-ray powder diffraction analysis shows that these crystals are indeed hematite and not lepidocrocite. The crystals are usually isolated or in small, randomly oriented groups, attached to calcite-I and associated with fluorite. Rarely, they occur as delicate hemispherical aggregates, which are hollow and lined with red hematite. Platy hematite occurs overgrown by fluorite attached to calcite-I, enclosed in fluorite, and encrusting fluorite, indicating that the fluorite and hematite were deposited synchronously. Based on the specimens available, calcite-II is later than hematite, without overlap.

Kainosite-(Y) [Ca.sub.2][(Y,Ce).sub.2][Si.sub.4][O.sub.12]([CO.sub.3])[cdotp][H.sub .2]O

Kainosite-(Y) is a relatively rare mineral, and Long Lake is the second known occurrence of kainosite-(Y) in New York State. Kainosite-(Y) was previously found in cavities in pegmatite veins excavated from the Delaware Aqueduct, shaft 23, Bronxville, NY, and studied by Fred Pough (Louis Moyd, personal communication, 1996). At Long Lake, kainosite-(Y) occurs as well-formed flesh-colored, translucent to opaque prismatic crystals which reach several millimeters in size (Figs. 20 and 21). The habit is somewhat variable because different (h01} prisms develop to varying degrees on different crystals, even on the same specimen. The lack of material well-suited for goniometry has hindered a full exploration of kainosite-(Y) morphology, but the drawing illustrates the typical habit.

Deciphering the position of kainosite-(Y) in the paragenetic sequence at Long Lake is difficult, in part because of the scarcity of material, and in part because other minerals do not seem to overgrow kainosite-(Y). Kainosite-(Y) is associated with, but earlier than, chamosite-III coating fluorite and breccia blocks. It is found on cerian epidote in similar settings, and is mostly later than the epidote. It occurs with quartz, cerian epidote, and fluorite in crystal aggregates unattached to the vein walls, in which fluorite forms the core, incompletely overgrown by epidote, followed by growth of isolated groups of kainosite-(Y) crystals and finally quartz. It also occurs in small voids in calcite I which appear to be miniature gash veins formed by tectonic shearing, where it is associated with chamosite-II, which may either pre-date or postdate it.

Kainosite-(Y) crystals are commonly etched, but examples showing no evidence of etching are also found, sometimes within millimeters of etched crystals. Crystals occurring in small pockets in calcite-I are almost always free of etching. These observations indicate that the etching is probably a result of late-stage weathering, and not geochemical changes during deposition of the vein assemblage.

Electron microprobe analysis of the kainosite-(Y) yields the empirical formula ([CO.sub.3] and [H.sub.2]O determined stoichiometrically): [Ca.sub.2.05]([Y.sub.1.41][Dy.sub..11][Gd.sub..10][Er.sub..07][Nd.sub ..06][Yb.sub..06][Sm.sub..05][Ho.sub..03][Ce.sub..01][Lu.sub..01])[Si .sub.4.05][O.sub.12]([CO.sub.3])[H.sub.2]O, which is quite comparable to the ideal formula. As has been observed in kainosite-(Y) from other localities (Adams et al., 1964; Heinrich et al., 1962), the heavy rare earths predominate over the light rare earths, with dysprosium being most abundant.

Pyrite [FeS.sub.2]

Pyrite occurs infrequently as small ([less than]1 mm) cubes modified by the pyritohedron {012}, usually attached to fluorite or to micro-minerals which overgrow fluorite. The pyrite has a dark brown color indicative of replacement by goethite.

Quartz [SiO.sub.2]

Quartz occurs as prismatic crystals, which are usually small ([less than]2 mm), but sometimes exceed 1 cm in length. The morphology of these crystals is typical of quartz from hydrothermal veins, with moderately developed prisms, and faces of the positive rhombohedron r{1011} usually somewhat larger than those of the negative rhombohedron z {0111}. Faces of the trigonal dipyramid s{1121} are often present, but faces of trigonal trapezohedra such as x{5161} have not been observed.

Long Lake quartz often has an orange-brown surface coating which is presumed to be an iron oxide/hydroxide. Dauphine twinning is commonly revealed by different luster on the r{1011} and z{0111} portions of faces of the termination. Rarely, one rhombohedron is more strongly coated with iron oxide/hydroxide than the other (compare Henderson, 1984). One example of what appears to be a contact Dauphine twin has been found (Fig. 23).

Isotopic analysis of the oxygen in Long Lake quartz gave a [[delta].sup.18]O value of 16.77% relative to Standard Mean Ocean Water.

Titanite [CaTiSiO.sub.5]

Titanite occurs rarely as small, pink, spear-shaped crystals which form sub-parallel clusters reaching 1 mm in size. The majority of the specimens were part of a single sample of calcite-filled vein, and were discovered accidentally when the calcite was dissolved away in a search for fluorite. We believe this sample may have come from a narrow vein located about 30 meters south of the two veins which produced the majority of the specimens described in this paper. One specimen was also found among the materials from the major veins.

The titanite crystal groups occur on chamosite-II and are closely associated with cerian epidote, kainosite-(Y) and quartz. On the sample which produced the majority of the specimens, titanite is definitely later in the paragenesis than chamosite, probably later than cerian epidote, definitely earlier than quartz, and of uncertain relationship to kainosite-(Y). Because of the small number of specimens recovered, and uncertainties about the outcrop location of the major sample and the paragenetic position of this species, titanite is not included in the paragenesis diagram in Figure 2.

DISCUSSION

Hydrothermal veins similar to those at Long Lake are rare, but not unknown in other Grenvillian rocks. The calcite-galena veins near Rossie, St. Lawrence County, New York, often carry small amounts of blue-green octahedral fluorite crystals; the Coal Hill vein, southwest of Rossie, hosts minor amounts of cerian epidote and synchysite-(Ce); and cerian epidote has been identified in similar veins near Mineral Point, north of Rossie (Robinson et al., in press). Cerian epidote is also commonly associated with calcite crystals from the Madawaska (Faraday) mine near Bancroft, Ontario. Kainosite-(Y) associated with fluorite, calcite, chamosite, quartz and other minerals has been described from the Bicroft mine near Bancroft, Ontario (Pouliot et al., 1964). Graham and Ellsworth (1930) described kainosite-(Y) from a brecciated calcite-apatite vein in North Burgess township, Lanark County, Ontario. Cavities in brecciated blocks of feldspar from the New York feldspar quarry near Buckingham, Quebec, have been found to c ontain microscopic crystals of both cerian epidote and kainosite-(Y) associated with calcite, fluorite, pyrite and quartz (Canadian Museum of Nature, Mineral Occurrence Collection). Finally, Hogarth (1972) reported kainosite-(Y) from the nearby Evans Lou pegmatite.

Geochemical data for most of these occurrences are scant to non-existent, and little can be said with certainty about their origins. Table 1 gives electron microprobe trace element analyses and stable isotope analyses of calcites from some of these occurrences. Except for calcite-II, the trace element contents and [C.sup.13]-[O.sup.18] signatures of the other calcites are overall quite similar. The variable Mg content is probably related to the host rock, since the Long Lake and Buckingham occurrences are hosted by granitic rocks, and the other occurrences by Grenville marble or rocks in close proximity to Grenville marble. The unique trace element and isotopic composition of calcite-II, its association with etched crystals of calcite-I, and its late position in the paragenetic sequence suggest that it probably formed by near-surface groundwater dissolution and re-precipitation of calcite-I.

Fluid inclusion studies of fluorite from Long Lake (Bird and Darling, 1996) reveal primary three-phase fluid inclusions consisting of vapor, brine, and a single halite crystal. Freezing experiments indicate that the liquid from which the fluorite crystallized was a calcium-rich brine containing [sim]25 weight % [CaCl.sub.2] and 10 weight % NaCl. (For comparison, Atlantic Ocean water contains 3.5% total dissolved salts by weight.) This brine is the most saline yet documented from New York State (Robert Darling, personal communication, 1996). Heating the inclusions yields liquid-vapor homogenization temperatures of [sim]133[degrees]C, and a final halite dissolution temperature of [sim]172[degrees]C (Bird and Darling, 1996).

Like the Long Lake veins, the calcite-galena veins near Rossie, New York also strike west-northwest with near-vertical dips, and are hosted by Grenville-age granitic gneisses. Interestingly, studies of primary fluid inclusions in sphalerite, fluorite and calcite from the Rossie veins also yield results very similar to those reported above (Ayuso et al., 1987). These investigators found that primary fluid inclusions in the Rossie vein minerals also consist of threephase inclusions with a single daughter crystal of halite, and homogenization temperatures of 104[degrees] to 152[degrees]C (sphalerite), 90[degrees] to 130[degrees]C (calcite) and 110[degrees] to 150[degrees]C (fluorite). Likewise, freezing and halite solution runs showed the total salinity of the brine to be in the range 26 to 31 equivalent weight % NaCl, with other salts such as KCl, [MgCl.sub.2] or [CaCl.sub.2] likely present. Plots of lead isotope ratios by the same authors yielded a secondary isochron, which was interpreted as lacking age sign ificance as a result of the mixing of solutions which evolved from distinctly different, long-lived environments.

Thus, the Long Lake and Rossie veins appear to be similar both structurally and mineralogically. The trace element and [C.sup.13] - [O.sup.18] compositions of calcite from each occurrence also are similar, as are the fluid inclusion data obtained from their principal minerals. It has long been known that the age of the Rossie veins is post-Ordovician (Smyth, 1903; Buddington, 1934; Brown, 1983), and recently, a K-Ar date obtained from adularia from Rossie indicates its age is 186.3 [+ or -] Ma, concurrent with Appalachian tectonism (Robinson et al., in press). Whether the veins at Long Lake are also Appalachian in age may be answered by Sm-Nd isotope studies presently underway (Robert Darling, personal communication, 1997).

ACKNOWLEDGEMENTS

Steve Condon told RPR about the Long Lake site (GWR discovered it independently), and contributed many specimens for study. Dr. John Hanchar measured luminescence spectra of fluorite and provided data for inclusion in this paper. The Oberlin College Geology Department provided access to thin-section-making equipment and a luminoscope for examining fluorite sections. Dr. Ken Krieger of the Water Quality Laboratory of Heidelberg College offered use of a Wild stereomicroscope with iris diaphragm, with which photographs of several of the smaller minerals were obtained. Dr. Bill Cook used his unique X-ray technique to identify some of the forms of kainosite. Dr. Robert Darling provided fluid inclusion data and is attempting to date the minerals. Jerry Van Velthuizen identified the hematite. This work was supported, in part, by the Canadian Museum of Nature, RAC Research Grant EPN100 to GWR.

REFERENCES

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BIRD, B. C., and DARLING, R. 5. (1996) Fluid inclusion study of the Long Lake calcite-fluorite vein, Central Adirondacks. Geological Society of America Abstracts with Programs. 28 (3), 39.

BROWN, C. E. (1983) Mineralization, mining and mineral resources in the Beaver Creek area of the Grenville lowlands in St. Lawrence County, New York. United States Geological Survey Professional Paper 1279, 21 p.

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GRAHAM, R. P. D., and ELLSWORTH, H. V. (1930) Cenosite from North Burgess Township, Lanark County, Ontario. American Mineralogist, 15, 205-219.

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HEINRICH, E. W., BORUP, R. A., and SALOTTI, C. A. (1962) Cenosite from Cotopaxi, Colorado. American Mineralogist, 47, 328-336.

HENDERSON, W. A., JR. (1984) Hematite overgrowths delineating Dauphine twinning in quartz. Mineralogical Record, 15, 227-229.

HOGARTH, D. D. (1972) The Evans-Lou pegmatite, Quebec: A unique yttrium-niobium-bismuth-vanadium mineral assemblage. Mineralogical Record, 3, 69-77

POULIOT, G., MAXWELL, J. A., and ROBINSON, S. C. (1964) Cenosite from Bancroft, Ontario. Canadian Mineralogist, 8, 1-10.

RAKOVAN, J. (1998) Sectoral zoning (SZ) of REEs in fluorite: Indication of the heterogeneous nature and distribution of surface protosites. International Mineralogical Association Program with Abstracts. In press.

RAKOVAN, J., and WAYCHUNAS, G. (1996) Luminescence in minerals. Mineralogical Record, 27, 7-19.

ROBINSON, G. W., DIX, G., CHAMBERLAIN, S. C., and HALL, C. (in press) Famous mineral localities: Rossie, New York, Mineralogical Record.

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Author:Richards, R. Peter; Robinson, George W.
Publication:The Mineralogical Record
Geographic Code:1U2NY
Date:Sep 1, 2000
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