Laser-induced breakdown spectroscopy (LIBS), which has recently emerged as tool for geochemical analysis outside the traditional laboratory setting, is an ideal tool for Li exploration because it is the only technique that can measure Li in minerals, rocks, soils, and brines in-situ in the field. In addition to being used in many products essential to modern life, Li is a necessary element for a reduced carbon future and Li–Cs–Ta (LCT) granitic pegmatites are an important source of Li. Such pegmatites can have varying degrees of enrichment in Li, Rb, Cs, Be, Sn, Ga, Ta>Nb, B, P, and F. We focus here on the LCT pegmatites of the Carolina Tin-Spodumene Belt (CTSB) situated in the Kings Mountain Shear Zone, which extends from South Carolina into North Carolina. The CTSB hosts both barren and fertile pegmatites, with Li-enriched pegmatites containing spodumene, K-feldspar, albite, quartz, muscovite, and beryl. We illustrate how handheld LIBS analysis can be used for real-time Li analysis in the field at a historically important CTSB pegmatite locality in Gaston County, N.C. in four contexts: (i) elemental detection and identification; (ii) microchemical mapping; (iii) depth profiling; and (iv) elemental quantitative analysis. Finally, as an example of a practical exploration application, we describe how handheld LIBS can be used to measure K/Rb ratios and Li contents of muscovite and rapidly determine the degree of pegmatite fractionation. This study demonstrates the potential of handheld LIBS to drastically reduce the time necessary to acquire geochemical data relevant to acquiring compositional information for pegmatites during a Li pegmatite exploration program.

Four voluminous ignimbrites (150–500 km³) erupted in rapid succession at 27 Ma in the central San Juan caldera cluster, Colorado. To reconstruct the timescales and thermal evolution of these magma reservoirs, we used zircon ID-TIMS U–Pb geochronology, zircon LA-ICP-MS geochemistry, thermal modeling, and zircon age and crystallization modeling. Zircon geochronology reveals dispersed zircon age spectra in all ignimbrites, with decreasing age dispersion through time that we term a ‘chimney sweeping’ event. Zircon whole-grain age modeling suggests that 2σ zircon age spans represent approximately one-quarter of total zircon crystallization timescales due to the averaging effect of whole-grain, individual zircon ages, resulting in zircon crystallization timescales of 0.8–2.7 m.y. Thermal and zircon crystallization modeling combined with Ti-in-zircon temperatures indicates that magma reservoirs were built over millions of years at relatively low magmatic vertical accretion rates (VARs) of 2–5 × 10^–3 m y⁻¹(2–5 × 10^–6km³y⁻¹ km⁻²), and we suggest that such low VARs were characteristic of the assembly of the greater San Juan magmatic body. Though we cannot unequivocally discern between dispersed zircon age spectra caused by inheritance (xenocrystic or antecrystic) versus prolonged crystallization from the same magma reservoir (autocrystic), our findings suggest that long-term magma input at relatively low VARs produced thermally mature upper crustal magma reservoirs resulting in protracted zircon crystallization timescales. Compiling all U–Pb ID-TIMS zircon ages of large ignimbrites, we interpret the longer timescales of subduction-related ignimbrites as a result of longer term, lower flux magmatism, and the shorter timescales of Snake River Plain ignimbrites as a result of shorter term, higher flux magmatism.

A dataset of >1190 published compositional analyses of muscovite from granitic pegmatites of varying mineralogical types was compiled to reevaluate the usefulness of K-Rb-Li systematics of muscovite as a tool for distinguishing mineralogically simple pegmatites from pegmatites with potential Li mineralization. Muscovite from (i) common, (ii) (Be-Nb-Ta-P)-enriched, (iii) Li-enriched, and (iv) REE- to F-enriched pegmatites contain Li contents that vary between 10 and 20,000 ppm depending on the degree of pegmatite fractionation. Common pegmatites are characterized by low degrees of fractionation as exhibited by K/Rb ratios ranging from 618 and 25 and Li contents generally being 1700 ppm. Muscovite from moderately to highly fractionated Li-rich pegmatites exhibit a wide range of K/Rb ratios and Li values: (i) K/Rb = 84 to 1.4 and Li = 35 to >18,100 ppm for spodumene pegmatites, (ii) K/Rb = 139 to 2 and Li = 139 to >18,500 ppm for petalite pegmatites, and (iii) K/Rb = 55 to 1.5 and Li = 743 to >17,800 ppm for lepidolite pegmatites. Pegmatites that host substantial REE- and F-rich minerals may carry muscovite with K/Rb ratios between 691 to 4 that has Li contents between 19 to 15,690 ppm. The K/Rb-Li behavior of muscovite can be useful in assessing the potential for Li mineralization in certain granitic pegmatite types. The proposed limits of K/Rb values and Li concentrations for identifying spodumene- or petalite-bearing pegmatites as part of an exploration program is reliable for Group 1 (LCT) pegmatite populations derived from S-type parental granites or anatectic melting of peraluminous metasedimentary rocks. However, it is not recommended for application to Group 2 (NYF) pegmatites affiliated with anorogenic to post-orogenic granitoids with A-type geochemical signatures or that derived by the anatexis of mafic rocks that generated REE- and F-rich melts.

The Carolina tin-spodumene belt, North Carolina, hosts one of the largest economic deposits of Li pegmatite ore in the United States, yet the petrogenesis of Carolina tin-spodumene belt pegmatites remains poorly understood. We use whole-rock and mineral trace element geochemistry to (1) evaluate the petrogenesis of Carolina tin-spodumene belt pegmatites, (2) compare their geochemistry to other Li-rich pegmatites worldwide, and (3) propose mineral chemistry indices for Li mineralization. Trace element modeling demonstrates that spodumene-bearing pegmatites are not related to the nearby Cherryville Granite through fractional crystallization, and rare earth element contents in plagioclase, garnet, and apatite indicate that spodumene-bearing pegmatites are also not derived from spodumene-free pegmatites. We prefer a petrogenesis in which both types of pegmatites and the Cherryville Granite are derived through similar, but individual, crustal anatectic events. Muscovite and K-feldspar K/Rb-Li systematics indicate that Carolina tin-spodumene belt pegmatites do not attain fractionation levels as high as those reached in the Oxford County pegmatite field in Maine or the Custer and Keystone pegmatite fields in South Dakota. Quartz and garnet Li abundances in Carolina tin-spodumene belt pegmatites are some of the highest in the world, and garnet rare earth element concentrations are the lowest. Contents of Ga, Mn, Ge, and Ti in spodumene allow for discrimination of pegmatites from the Carolina tin-spodumene belt, Maine, South Dakota, Canada, and Portugal. Based on this extensive trace element study, plagioclase, K-feldspar, quartz, muscovite, garnet, and apatite chemistry offer a comprehensive methodology to distinguish pegmatites with and without spodumene in the Carolina tin-spodumene belt, which may be useful in exploration for Li pegmatite ore worldwide.

Laser-induced breakdown spectroscopy (LIBS) is a technology for compositional analysis that is particularly effective for light elements, particularly Li, which is a critical commodity for emerging green technologies. This study undertook analysis by handheld LIBS of muscovite from the drill core, outcrop, and soil on the Carolina Lithium Prospect (CLP) in Gaston County, North Carolina (USA), which lies within the Carolina Tin-Spodumene Belt (CTSB). Abundances of the alkali elements Li, K, and Rb were determined for more than 130 muscovites from the Li-rich pegmatites to track the degree of pegmatite fractionation as a pathfinder for spodumene mineralization. Across the CTSB and including the CLP, muscovite Li contents vary over an order of magnitude, ranging from 0.04 to 0.74 wt. %, with their K/Rb ratios varying between 63 and 8, features that together document the highly evolved character of pegmatites within the CTSB district. On average, muscovite Li contents are greater in spodumene-bearing pegmatites at 0.21 ± 0.12 wt. % than for common quartz-feldspar pegmatites at 0.14 ± 0.08 wt. %. Although overlapping substantially in the middle portions of their distributions, muscovite K/Rb ratios are biased toward low values for spodumene-bearing pegmatites $(\stackrel{-}{\mathrm{X}}$ = 21 ± 6) compared to those for quartz-feldspar pegmatites $(\stackrel{-}{\mathrm{X}}$ = 33 ± 9). This study provides a framework for the use of LIBS analysis of muscovite in outcrop, drill core, and soil samples as an analytical tool for in-field and on-site geochemical analysis during Li pegmatite exploration and prospect evaluation.

The last four caldera-forming ignimbrites in the central San Juan caldera cluster, Colorado, erupted 1400 km³ in ≤80 kyr and alternated between zoned crystal-poor rhyolite to crystal-rich dacite and unzoned, crystal-rich dacite. The zoned 150 km³ Rat Creek Tuff (26·91 Ma), unzoned 250 km³ Cebolla Creek Tuff, and zoned 500 km³ Nelson Mountain Tuff (26·90 Ma) formed the nested San Luis caldera complex with slightly offset calderas, and the unzoned 500 km³ Snowshoe Mountain Tuff (26·87 Ma) formed the Creede caldera to the south. The Rat Creek Tuff, Nelson Mountain Tuff, and Snowshoe Mountain Tuff have similar mineral assemblages of plagioclase, sanidine, quartz, biotite, hornblende, clinopyroxene, Fe–Ti oxides, and accessory zircon, titanite, and apatite. The Cebolla Creek Tuff differs from the other three ignimbrites with more abundant hornblende and a lack of quartz and sanidine. Trace element compositions of interstitial glass are unique to each ignimbrite, correlating with mineral assemblages and inferred crystallization depths. Glass, feldspar, hornblende, and clinopyroxene thermobarometry calculations provide evidence for vertically extensive crustal magma reservoirs with a common magmatic zone at ∼435–470 MPa (∼16–17 km) showing a transition into shallow pre-eruptive reservoirs between ∼110 and 340 MPa (∼4–13 km), similar to the estimated magma reservoir architecture of the Altiplano Puna Volcanic Complex. The upper portions of the eruptible parts of the magma reservoirs of the Rat Creek Tuff (215 ± 50 MPa, ∼810–820 °C), Cebolla Creek Tuff (340 ± 20 MPa, ∼860–880 °C), Nelson Mountain Tuff (215 ± 20 MPa, ∼745–800 °C), and Snowshoe Mountain Tuff (110 ± 40 MPa, 825 ± 10 °C) occupied shallow levels in the crust similar to other magma reservoirs of the central San Juan caldera cluster. Trace element modelling correlates with a deep crystallization signature in the unzoned Cebolla Creek Tuff and Snowshoe Mountain Tuff, typified by a flat trend in Ba versus Sr whole-rock and glass chemistry. The zoned Rat Creek Tuff and Nelson Mountain Tuff are typified by a steep trend in Ba versus Sr chemistry interpreted as a shallower crystallization signature. Similarly, the unzoned Cebolla Creek Tuff and Snowshoe Mountain Tuff have flatter slopes in FeO versus An space of plagioclase chemistry interpreted as more abundant deep plagioclase crystallization and a difficulty in physically mixing with Fe-rich mafic recharge magma owing to higher viscosity. The zoned Rat Creek Tuff and Nelson Mountain Tuff have higher slopes in FeO versus An space of plagioclase chemistry interpreted as more abundant shallow plagioclase crystallization and more feasible mixing with Fe-rich mafic recharge magma owing to lower viscosity. The eruption of the Rat Creek Tuff was probably triggered by mafic injection, but the other three ignimbrites lack mingling textures in pumice, suggesting that other mechanisms were important in causing such large eruptions. After a prolonged period of mantle-derived magma injection and crustal heating (∼25 000 km³ Conejos Formation erupted during ∼35–29 Ma), the San Juan magmatic body became a robust and versatile producer of diverse eruptible magmas in short time periods during its Oligocene ignimbrite flare-up.