Trace element partitioning in plagioclase feldspar

Compilation and interpretation of experimental and natural Nernst partition coefficient (^{plagioclase/melt}D) data show that, with a few exceptions, increases in ^{plagioclase/melt}D correlate with decreasing anorthite-content of plagioclase. In contrast, increases of ^{plagioclase/melt}D for Ga, Sc, Cu, Zn, Zr, Hf and Ti, are better correlated against decreasing melt MgO or increasing melt SiO₂ contents. ^{plagioclase/melt}D for Ti and the rare earth elements (REE) show little dependence on temperature, but increase as the melt water content increases. ^{plagioclase/melt}D for K and Sr are sensitive to pressure. Variations of D₀ (the strain compensated partition coefficient), r₀ (the size of the site into which REE substitute), and E (Young’s Modulus of this site) were parameterized against variations of melt SiO₂, the An-content of plagioclase, and other combinations of variables, allowing ^{plagioclase/melt}D_REE-Y to be calculated from a variety of input parameters. The interrelations of temperature, melt MgO and SiO₂ content, and plagioclase anorthite-content for wet and dry systems were also parameterized to facilitate interpolation where such data are lacking. When combined, these semi-empirical parameterizations yield ^{plagioclase/melt}D results comparable to available experimental and natural data.     

Relationship between plagioclase crystallization and cooling rate in basaltic melts

Rock textures commonly preserve a record of the near-surface crystallization history of volcanic rocks. Under conditions of simple cooling without convection or mixing, textures will reflect sample cooling rate, the temperature at which crystallization was initiated, and the distribution of mineral phase precipitation across the crystallization interval. Compilation of plagioclase size and number density data on natural (dike, sill and lava lake) and experimental samples suggests that (1) growth and nucleation rates of plagioclase in natural basaltic samples are a predictable function of cooling rate, and (2) the observed crystallization rate dependence on cooling rate is similar to that observed in experiments initiated at subliquidus temperatures. Comparison of natural and experimental samples thus suggests that most basalts crystallize under conditions of heterogeneous nucleation, with the number density of preexisting nucleii partially controlling textural responses to cooling rate changes. Time scales of crystallization and cooling in magmatic systems are intimately linked through a balance between heat removal from the system and heat evolved through crystallization. Evaluation of textural data in the context of recent numerical models of crystallization in simple (one- and two-component systems) provides new insight into regularities in the crystallization behavior of basaltic magmas. For example, the rate of change in crystal size (and number density, as dictated by mass balance) has been used as a measure of the relative importance of time scales of crystallization and cooling in numerical models of crystallizing systems. In natural samples, plagioclase size scales with the length scale of cooling such that a logarithmic plot of grain size as a function of normalized distance across the dike has a slope that appears approximately independent of dike width (solidification time). Comparison with available textural data for other phenocryst phases suggests that the same may be true for pyroxene and magnetite crystallization, with each phase having a characteristic slope probably controlled by the thermodynamic properties of the crystallizing phase. Measured crystal size distributions are unimodal and show maximum frequencies in the smaller size classes; distributions broaden and the grain size at peak frequency increases with increasing crystallization times (decreasing cooling rates). In contrast, partially crystallized Makaopuhi lava lake samples have crystal size distributions that decrease exponentially with increasing crystal size. Measured size distributions in dikes can be explained by late stage modification of Makaopuhi-type distributions through loss of small crystals, possibly the consequence of growth without nucleation. Finally, this compilation of the textural response of basaltic magmas to changes in cooling rate suggests that empirical calibrations of crystallization rate dependence on cooling rate from natural samples provide a reasonable model for plagioclase crystallization in near-surface basaltic systems. Predicted growth rates will be slow and relatively constant (10^-10–10^-11 cm/s) for crystallization times expected in most shallow volcanic systems (<1000 years).     

Modeling H,Na, and K diffusion in plagioclase feldspar by relating point defect parameters to bulk properties

Hydrogen and alkali ion diffusion in plagioclase feldspars is important to study the evolution of the crust and the kinetics of exsolution and ion-exchange reactions in feldspars. Using the available PVT equation of state of feldspars, we show that the diffusivities of H and alkali in plagioclase feldspars as a function of temperature can be successfully reproduced in terms of the bulk elastic and expansivity data through a thermodynamic model that interconnects point defect parameters with bulk properties. Our calculated diffusion coefficients of H, Na, and K well agree with experimental ones when uncertainties are considered. Additional point defect parameters such as activation enthalpy, activation entropy, and activation volume are also predicted. Furthermore, the electrical conductivity of feldspars inferred from our predicted diffusivities of H, Na, and K through the Nernst–Einstein equation is compared with previous experimental data.     

Composition of plagioclase feldspar in modern deep-sea sands: relationship to tectonic setting

Microprobe analysis of plagioclase in deep-sea sands from various tectonic settings gives averages ranging from 19% An for trailing-edge continental margins to 56% An for basins on the ocean side of an island arc. For each setting except island arcs, anomalously high amounts of pure albite are found. These albitic grains may be recycled from pre-existing sedimentary rocks. Potassium-rich plagioclase, thought to be indicative of a volcanic provenance, is less abundant than would be expected from the proportion of volcanic rock fragments. Perhaps such high-K plagioclases are less resistant to weathering than low-K plagioclase.     

Enthalpies of ordering in the plagioclase feldspar solid solution

Enthalpies of solution in lead borate at ~700°C have been measured for 36 natural and heat treated plagioclase feldspars. The samples made up two series, as characterised by TEM and XRD. A “low” series contained the natural ordered material and a “high” series the same samples annealed at high temperatures to induce cation disorder. Enthalpy of solution differences between the two series give the enthalpy changes associated with the disordering reactions: low albite → high albite: ~3 kcal/mole “e” structure → Cī high albite structure: ~ 1.4-2.8 kcal/mole Il? structure →- Cl? high albite structure: ~0.7-1.9 kcal/mole Il? structure equilibrated at low temperature → Il? structure equilibrated at high temperature: ~ 1.8?0.8 kcal/mole.ΔH_soln data for the high series overlap with the data of Newtonet al. (1980) for synthetic high structural state plagioclases except in the composition range ~An₉₀–An₁₀₀. They are consistent with an interpretation of the solid solution as being composed, at high temperatures, of two ideal (zero heat of mixing) segments, one with Cl? symmetry and one with Il symmetry, and having a non-first order (continuous) order/disorder transformation between them. The low series can also be separated into two distinct trends, for Il? and “e” structures.Values of the enthalpy change due to disordering (ΔH_ord) also show a number of systematic trends. Firstly, the values for e → Cl? are larger than for Il? → Cl? in the composition range where both e and Il? structures are observed (~An₆₅-An₇₂). Secondly, the enthalpy change on disordering the most ordered e structures at An-rich compositions is larger than for Ab-rich e structures. The apparent change in ΔH_ord, which occurs at ~An₅₀, may be important for the origin of the Bøggild miscibility gap. Thirdly, the large enthalpy change of the e structure, due to ordering, may be sufficient to stabilise it relative even to a mixture of low albite plus anorthite. Values for the enthalpy change on disordering Il? anorthites and bytownites to a Cl? structure have been estimated by assuming that the Cl? solid solution is ideal (non-enthalpic) and then extrapolating a straight line through the data for Ab-rich compositions to pure anorthite.     

Oxygen diffusion in anhydrous sanidine feldspar

Oxygen exchange experiments have been performed between single crystals of sanidine feldspar and oxygen gas enriched in ¹⁸O, at temperatures in the range 869–1053 °C, total pressure 1 atmosphere, for times up to 28 days. Oxygen isotope diffusion profiles in a direction perpendicular to (001) were determined with an ion microprobe. The experimental data obey a single Arrhenius relationship of the form D = 8.4 × 10⁻¹¹ exp. (−245 ± 15 kJ mol⁻¹/RT) m²s⁻¹. The results indicate that oxygen diffusion in anhydrous sanidine feldspar is marginally slower than oxygen diffusion in anhydrous anorthite. Comparison with published atomistic simulation studies suggests that oxygen transport in feldspar is by an interstitial mechanism. Received: 17 October 1997 / Accepted: 6 July 1998     

Determination of the character of oriented potash feldspar overgrowth on plagioclase crystals in igneous rocks

A metod for determining the kind of potash feldspar overgrowths on plagioelase in igneous rocks is described and applied to different rocks types. The character of these overgrowths in volcanic and hypabyssal rocks seems to differ from that encountered in plutonic rocks.     

Ferric iron partitioning between plagioclase and silicate liquid: thermodynamics and petrological applications

A series of Fe and Mg partition experiments between plagioclase and silicate liquid were performed in the system SiO₂-Al₂O₃-Fe₂O₃-FeO-MgO-CaO-Na₂O under oxygen fugacities from below the IW buffer up to that of air. A thermodynamic model of plagioclase solid solution for the (CaAl,NaSi,KSi)(Fe³⁺,Al³⁺)Si₂O₈-Ca(Fe²⁺,Mg)Si₃O₈ system is proposed and is calibrated by regression analysis based on new and previously reported experimental data of Fe and Mg partitioning between plagioclase and silicate liquid, and reported thermodynamic properties of end members, ternary feldspar and silicate liquid. Using the derived thermodynamic model, FeO^t, MgO content and Mg/(Fe^t+Mg) in plagioclase can be predicted from liquid composition with standard deviations of ǂ.34 wt% (relative error =9%) and ǂ.08 wt% (14%) and ǂ.7 (8%) respectively. Calculated Fe³⁺-Al exchange chemical potentials of plagioclase, m_{Fe^{3 +} ( Al )- 1} ^Pl{\rm \mu }_{{\rm Fe}^{{\rm 3 + }} \left( {{\rm Al}} \right)_{{\rm - 1}} }^{{\rm Pl}} agree with those calculated using reported thermodynamic models for multicomponent spinel, m_{Fe^{3 +} ( Al )- 1} ^Sp{\rm \mu }_{{\rm Fe}^{{\rm 3 + }} \left( {{\rm Al}} \right)_{{\rm - 1}} }^{{\rm Sp}} and clinopyroxene, m_{Fe^{3 +} ( Al )- 1} ^Cpx{\rm \mu }_{{\rm Fe}^{{\rm 3 + }} \left( {{\rm Al}} \right)_{{\rm - 1}} }^{{\rm Cpx}} . The FeO^t content of plagioclase coexisting with spinel or clinopyroxene is affected by Fe³⁺/(Fe³⁺+Al) and Mg/(Fe+Mg) of spinel or clinopyroxene and temperature, while it is independent of the anorthite content of plagioclase. Three oxygen barometers based on the proposed model are investigated. Although the oxygen fugacities predicted by the plagioclase-liquid oxygen barometer are scattered, this study found that plagioclase-spinel-clinopyroxene-oxygen and plagioclase-olivine-oxygen equilibria can be used as practical oxygen barometers. As a petrological application, prediction of plagioclase composition and f_O2 are carried out for the Upper Zone of the Skaergaard intrusion. The estimated oxygen fugacities are well below QFM buffer and consistent with the estimation of oxidization states in previous studies.     

Shock-effects on the K-Ar system of plagioclase feldspar and the age of anorthosite inclusions from North-Eastern Minnesota

Artificial shock pressures up to 52.5 GPa have no influence on the K-Ar system of plagioclase feldspar. The ⁴⁰Ar-³⁹Ar analysis of feldspar (labradorite An₆₇ from anorthosite of North-Eastern Minnesota) shocked up to 45 GPa—in vacuo, to prevent massive entrapment of atmospheric argon-shows that the age spectra and the argon diffusion properties remain unaltered. Similar feldspar samples (labradorite An₅₁ from Nain, Labrador), shocked in air up to 52.5 GPa and dated by the conventional K-Ar method, also yield the same age as unshocked samples but with a higher atmospheric argon contribution. The Minnesota anorthosite has an ⁴⁰Ar-³⁹Ar age of 1075 ± 10 m.y. No information on a possible previous history of the anorthosite became apparent.     

Neodymium diffusion in orthopyroxene: Experimental studies and applications to geological and planetary problems

We have determined the Nd³⁺ diffusion kinetics in natural enstatite crystals as a function of temperature, f(O₂) and crystallographic direction at 1 bar pressure and applied these data to several terrestrial and planetary problems. The diffusion is found to be anisotropic with the diffusion parallel to the c-axial direction being significantly greater than that parallel to a- and b-axis. Also, D(//a) is likely to be somewhat greater than D(//b). Diffusion experiments parallel to the b-axial direction as a function of f(O₂) do not show a significant dependence of D(Nd³⁺) on f(O₂) within the range defined by the IW buffer and 1.5 log unit above the WM buffer. The observed diffusion anisotropy and weak f(O₂) effect on D(Nd³⁺) may be understood by considering the crystal structure of enstatite and the likely diffusion pathways. Using the experimental data for D(Nd³⁺), we calculated the closure temperature of the Sm-Nd geochronological system in enstatite during cooling as a function of cooling rate, grain size and geometry, initial (peak) temperature and diffusion direction. We have also evaluated the approximate domain of validity of closure temperatures calculated on the basis of an infinite plane sheet model for finite plane sheets showing anisotropic diffusion. These results provide a quantitative framework for the interpretation of Sm-Nd mineral ages of orthopyroxene in planetary samples. We discuss the implications of our experimental data to the problems of melting and subsolidus cooling of mantle rocks, and the resetting of Sm-Nd mineral ages in mesosiderites. It is found that a cooling model proposed earlier [Ganguly J., Yang H., Ghose S., 1994. Thermal history of mesosiderites: Quantitative constraints from compositional zoning and Fe-Mg ordering in orthopyroxene. Geochim. Cosmochim. Acta 58, 2711-2723] could lead to the observed ∼90 Ma difference between the U-Pb age and Sm-Nd mineral age for mesosiderites, thus obviating the need for a model of resetting of the Sm-Nd mineral age by an “impulsive disturbance” [Prinzhoffer A, Papanastassiou D.A, Wasserburg G.J., 1992. Samarium-neodymium evolution of meteorites. Geochim. Cosmochim. Acta 56, 797-815].     

Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems: 5. Results of K-feldspar hydrolysis experiments

This paper explores how dissolution and precipitation reactions are coupled in batch reactor experimental systems at elevated temperatures. This is the fifth paper in our series of ‘‘Coupled Alkali Feldspar Dissolution and Secondary Mineral Precipitation in Batch Systems.’’ In the previous four papers we presented batch experiments of alkali-feldspar hydrolysis and explored the coupling of dissolution and precipitation reactions(Fu et al. in Chem Geol91:955–964, 2009; Zhu and Lu in Geochim Cosmochim Acta 73:3171–3200, 2009; Zhu et al.in Geochim Cosmochim Acta 74:3963–3983, 2010; Lu et al. in Appl Geochem30:75–90, 2013). Here, we present the results of additionalK-rich feldspar hydrolysis experiments at 150 °C. Our solution chemistry measurements have constrained feldspar dissolution rates, and our high resolution transmission electron microscopy work has identified boehmite precipitation. Reaction path modeling of K-feldspar dissolution and boehmite precipitation simulated the coupled reactions, but only with forced changes of boehmite rate law in the middle of experimental duration. The results which are reported in this article lend further support to our hypothesis that slow secondary mineral precipitation explains part of the wellknown apparent discrepancy between lab measured and field estimated feldspar dissolution rates(Zhu et al. in Water–rock interaction, 2004).     

Grain boundary diffusion of oxygen,potassium and calcium in natural and hot-pressed feldspar aggregates

 Grain boundary diffusion rates of oxygen, potassium and calcium in fine-grained feldspar aggregates were determined experimentally. The starting materials were a natural albite rock from the Tanco pegmatite and aggregates hot-pressed from fragments of Amelia albite or Ab, Or and An composition glasses. The technique employed isotopic tracers (¹⁸O, ⁴¹K, ⁴²Ca) either evaporated onto the surface or in an aqueous solution surrounding the sample, and depth profiling using an ion microprobe (SIMS). From the depth profiles, the product of the grain boundary diffusion coefficient (D′) and effective boundary width (δ) was calculated using numerical solutions to the appropriate diffusion equation. The experimental reproducibility of D′δ is a factor of 3. A separate determination of D′ independent of δ yields an effective grain boundary width of ∼3 nm, consistent with high resolution TEM observations of a physical grain boundary width <5 nm. Oxygen (as molecular water) grain boundary diffusion rates were determined in the Ab and Or aggregates at 450°–800° C and 100 MPa (hydrothermal), potassium rates in Or aggregates at 450°–700° C both at 0.1 MPa (in air) and at 100 MPa (hydrothermal), and calcium rates in An aggregates at 700°–1100° C and 0.1 MPa (in air). Oxygen grain boundary diffusion rates are similar in all three of the Ab aggregates and in the Or aggregate. Potassium and oxygen depth profiles measured in the same samples yield different D′δ values, confirming a diffusional transport mechanism. Potassium diffusion in the Or aggregate has a greater activation energy (216 vs 78 kJ/mol) than oxygen, and the Arrhenius relations cross at ∼625° C. Potassium D′δ values in Or aggregates are about a factor of five greater in hydrothermal experiments at 100 MPa than in experiments at 0.1 MPa in air. Calcium grain boundary diffusion rates in An aggregates are 4 to 5 orders of magnitude slower than potassium in Or and have a greater (291 kJ/mol) activation energy. This suggests that differences in formal charge and/or size of diffusing species may play an important role in their relative grain boundary diffusion rates. Received: 24 December 1993 / Accepted: 16 June 1994     

Microprobe mineralogy of plagioclase, clinopyroxene and amphibole as records of cooling rate in the Shirotori—Hiketa dike swarm, northeastern Shikoku, Japan

A compositional gap between hypersolidus plagioclase and subsolidus plagioclase, most of which must have formed by devitrification, decreases in An % with decreasing cooling rate, probably reflecting a melt composition derived by in situ differentiation. Augitic pyroxenes, crystallized from a quickly cooling magma, tend to contain more Al, Ti, Na(+K) and Fe³⁺, and less Si and Mn. Compositional breaks between hypersolidus and subsolidus amphiboles with respect to the components of edenite and titanoamphibole, decrease in width with decreasing cooling rate. Subcalcic hornblende seems to grow from differentiated magmas in the course of moderate to rapid cooling.     

Argon diffusion in plagioclase and implications for thermochronometry: A case study from the Bushveld Complex, South Africa

Plagioclase is not only the most abundant mineral in the Earth’s crust, but is present in almost all terrestrial tectonic settings and is widespread in most extraterrestrial material. Applying the K-Ar system to this common mineral would provide a powerful tool for quantifying thermal histories in a wide variety of settings. Nonetheless, plagioclase has rarely been used for thermochronometry, largely due to difficulties in simultaneously acquiring precise geochronologic data and quantifying argon diffusion kinetics from a mineral with low-K concentration. Here we describe an analytical technique that generates high-precision ⁴⁰Ar/³⁹Ar data and quantifies Ar diffusion kinetics of low-K minerals. We present results of five diffusion experiments conducted on single crystals of plagioclase from the Bushveld Complex, South Africa. The observed diffusion kinetics yield internally consistent thermochronological constraints, indicating that plagioclase is a reliable thermochronometer. Individual grains have activation energies of 155-178 kJ/mol and ln(D₀/a²) varies between 3.5 and 6.5. These diffusion parameters correspond to closure temperatures of 225-300 °C, for a 10 °C/Ma cooling rate. Age spectra generally conform to single-domain diffusive loss profiles, suggesting that grain-scale diffusion dominates argon transport in this fairly simple plagioclase. Conjointly examining several single-grain analyses enables us to distinguish episodic reheating from slow cooling and indicates that the Bushveld Complex cooled rapidly and monotonically from magmatic temperature to <300 °C over 3 Ma, followed by protracted cooling to ambient crustal temperatures of 150-200 °C over ∼600 Ma.     

Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems: 4. Numerical modeling of kinetic reaction paths

This paper explores how dissolution and precipitation reactions are coupled in batch reactor experimental systems at elevated temperatures. This is the fourth paper in our series of “Coupled Alkali Feldspar Dissolution and Secondary Mineral Precipitation in Batch Systems”. In our third paper, we demonstrated via speciation-solubility modeling that partial equilibrium between secondary minerals and aqueous solutions was not attained in feldspar hydrolysis batch reactors at 90-300 °C and that a strong coupling between dissolution and precipitation reactions follows as a consequence of the slower precipitation of secondary minerals (Zhu and Lu, 2009). Here, we develop this concept further by using numerical reaction path models to elucidate how the dissolution and precipitation reactions are coupled. Modeling results show that a quasi-steady state was reached. At the quasi-steady state, dissolution reactions proceeded at rates that are orders of magnitude slower than the rates measured at far from equilibrium. The quasi-steady state is determined by the relative rate constants, and strongly influenced by the function of Gibbs free energy of reaction (ΔG_r) in the rate laws.To explore the potential effects of fluid flow rates on the coupling of reactions, we extrapolate a batch system (Ganor et al., 2007) to open systems and simulated one-dimensional reactive mass transport for oligoclase dissolution and kaolinite precipitation in homogeneous porous media. Different steady states were achieved at different locations along the one-dimensional domain. The time-space distribution and saturation indices (SI) at the steady states were a function of flow rates for a given kinetic model. Regardless of the differences in SI, the ratio between oligoclase dissolution rates and kaolinite precipitation rates remained 1.626, as in the batch system case (Ganor et al., 2007). Therefore, our simulation results demonstrated coupling among dissolution, precipitation, and flow rates.Results reported in this communication lend support to our hypothesis that slow secondary mineral precipitation explains part of the well-known apparent discrepancy between lab measured and field estimated feldspar dissolution rates (Zhu et al., 2004). Here we show how the slow secondary mineral precipitation provides a regulator to explain why the systems are held close to equilibrium and show how the most often-quoted “near equilibrium” explanation for an apparent field-lab discrepancy can work quantitatively. The substantiated hypothesis now offers the promise of reconciling part of the apparent field-lab discrepancy.     

Rare earth diffusion kinetics in garnet: Experimental studies and applications

We determined the diffusion coefficient of Sm in almandine garnet as function of temperature at 1 bar and fO₂ corresponding to that of wüstite-iron buffer, and to a limited extent, that of a few other selected rare earth elements in almandine and pyrope garnets. Both garnets were demonstrated to have metastably survived the diffusion annealing at conditions beyond their stability fields. The experimental diffusion profiles were analyzed by secondary ion mass spectrometry, and in addition, by Rutherford back scattering spectroscopy for two samples. Transmission electron microscopic study of an almandine crystal that was diffusion-annealed did not reveal any near-surface fast diffusion path. Using reasonable approximations and theoretical analysis of vacancy diffusion, the experimental data were used to develop an expression of rare earth element (REE) diffusion coefficient in garnet as a function of temperature, pressure, fO₂, ionic radius, and matrix composition. Calculation of the closure temperature for the Sm-Nd decay system in almandine garnet in a metamorphic terrain shows very good agreement with that constrained independently. Modeling of the REE evolution in melt and residual garnet suggests that for dry melting condition, the REE pattern in the melt should commonly conform closely to that expected for equilibrium melting. However, for much lower solidus temperatures that would prevail in the presence of a H₂O-CO₂ fluid, the concentration of light REE in the melt could be significantly lower than that under equilibrium melting condition. A reported core and rim differences in the REE content of a garnet crystal in a mantle xenolith in kimberlite have been reproduced by assuming that the REE zoning was a consequence of entrapment in a magma derived from an external source for ∼32,000 yr before the eruption.     

Constraining cooling histories: rutile and titanite chronology and diffusion modelling in NW Bhutan

U–Pb analyses of rutile and titanite commonly yield ages that constrain the timing of cooling rather than the timing of their crystallization. Rutile which grew at or close to peak temperature conditions in a mafic granulite, intermediate granulite and mafic amphibolite within juxtaposed litho/tectonostratigraphic units in the Greater Himalayan Sequence (GHS) of NW Bhutan yield LA–MC–ICP–MS U–Pb lower intercept cooling ages of 10.1 ± 0.4, 10.8 ± 0.1 and 10.0 ± 0.3 Ma, respectively. Numerical finite‐difference diffusion models constrained by previously published temperature–time and Pb diffusion data suggest that these ages are best explained by rapid cooling from peak temperature conditions of ～800 °C at 14 Ma in the granulite‐bearing unit and ～650 °C at 12 Ma in the amphibolite‐bearing unit. The good fit between the model and analysed ages confirms the relatively high retention of Pb in rutile suggested by the experimental data. Titanite that grew during an exhumation‐related amphibolite facies overprint on an eclogite facies mineral assemblage from the neighbouring Jomolhari Massif yields a U–Pb lower intercept cooling age of 14.6 ± 1.2 Ma. Diffusion modelling suggests that this age is too old to be consistent with the temperature–time paths inferred for the rutile‐bearing samples. Instead, the titanite age suggests cooling from ～650 °C at an earlier time of 17–15 Ma, implying that the high‐grade rocks in the Jomolhari Massif experienced a different cooling history from the rest of the GHS in NW Bhutan. Together these data show that high‐grade rocks from three apparently different structural levels of the GHS in NW Bhutan experienced rapid cooling at >40 °C Ma^?1 at varying times. The highest grade granulite facies rocks were exhumed from deeper structural levels that are not exposed, not preserved, or not yet recognized west of eastern Nepal. A progressive along‐strike change in tectonic regime, metamorphic history and/or exhumation mechanism across the orogen is implied by these thermochronologic data.