A process-based model for non-equilibrium clumped isotope effects in carbonates
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In extreme pH environments where [CO3 2-] is dominant (pH > 9.5), shifts in chemical and isotopic equilibrium of the H2O-DIC-CaCO3 system cause carbonates to follow a different equilibrium TΔi relationship.
“This means that in extreme pH environments (such as where [CO 3 2-] is dominant, pH > 9.5), shifts in the chemical and isotopic equilibrium of the H 2 O-DIC-CaCO 3 system cause carbonates to follow a different equilibrium Ti relationship (Tripati et al. 2015, Watkins & Hunt 2015).”
From Frontiers of Carbonate Clumped Isotope Thermometry (2023) · cites this paper as Watkins & Hunt 2015
The Figure 5 caption (section 7 Summary; page unavailable) describes pH-dependent clumped-isotope compositions as a model of non-equilibrium calcite, with apparent temperatures calculated using an equilibrium calcite calibration. Section 6.4.1 likewise describes pH and growth-rate effects as possible offsets from the true equilibrium value. The paper does not say that high pH gives carbonates a different equilibrium temperature–clumped-isotope relationship; it distinguishes such offsets from equilibrium. (LLM, conf=0.85)
Checked by a reasoning model — may be wrong.
Experimental — accuracy not yet measuredThese rates are also below the equilibrium or slow growth limits cited in Watkins et al. (2014, 2013, 2015).
“These rates are also below the equilibrium or slow growth limits cited in Watkins et al. (2014Watkins et al. ( , 2013Watkins et al. ( , 2015)).”
From Reconstructing the temperature and origin of CO2 mineralisation in CarbFix calcite using clumped, carbon and oxygen isotopes (2024) · cites this paper as Watkins et al., 2015
Section 6.3 (page unavailable) describes an equilibrium composition in the limit of extremely slow calcite growth, supporting the reference to a slow-growth or equilibrium limit. It does not establish that the citing paper’s unspecified rates fall below that limit, so the rate comparison is not verified by this source. (LLM, conf=0.82)
Experimental — accuracy not yet measuredThe higher pH in Laghetto Basso (8.2 versus 7.4 at Devils Hole) has a negligible effect (≤ 0.05‰) on 18O/16O fractionation at the very slow growth rates considered.
“Although pH is expected to influence 18O/16O fractionation between water and rapidly-precipitating calcite, this effect decreases with slower crystallization rates27,33, and becomes negligible (≤ 0.05‰) at the very slow growth rates considered here.”
From Most Earth-surface calcites precipitate out of isotopic equilibrium (2019) · cites this paper as [33]
The Figure 2 caption (section 7 Summary; page unavailable) supports the qualitative point that growth rate changes the modeled oxygen-isotope composition and that calcite approaches equilibrium at very slow growth. Section 5.2 identifies Devils Hole as a slowly grown, near-equilibrium example. Our copy does not establish a ≤0.05‰ effect for the stated pH difference or growth rates, and it does not discuss Laghetto Basso. (LLM, conf=0.84)
Experimental — accuracy not yet measuredKinetics will also have an effect on isotopic fractionation of carbonates.
“Kinetics will also have an effect on such fractionation (e.g., Hill et al., 2014; Tripati et al., 2015; Watkins and Hunt, 2015; Guo, 2019), but is beyond the scope of the present study.”
From Theoretical constraints on the effects of added cations on clumped, oxygen, and carbon isotope signatures of dissolved inorganic carbon species and minerals (2020) · cites this paper as Watkins and Hunt, 2015
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“They observed a relatively wide range in 47xtl at a given temperature of about 0.006 , comparable to other experimental studies that lacked such controls (e.g., Ghosh et al., 2006a; Dennis and Schrag, 2010; Zaarur et al., 2013; Defliese et al., 2015).”
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“The Zaarur et al. (2013) calibration is similar to the Ghosh et al. (2006a) calibration whereas the Hill et al. (2014) calibration is similar to the Dennis and Schrag (2010) and Kluge et al. (2015) calibrations (see Fig.”
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“This result does not conflict with previous proposals that kinetic clumped isotope effects in surface corals may be due to rapid hydration of excess CO2 (Saenger et al., 2012; Eiler et al., 2014).”
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“28 (acid digestion at 25 ◦C; Tripati et al., 2015) for the comparison to experimental data.”
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“According to our model, the data from Tang et al. (2014) would be unable to resolve the expected pH- or rate-dependence on 47xtl, consistent with their findings.”
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Comment on egusphere-2023-2581
Clark, A. J., Torres-Romero, I., Jaggi, M., et al. (2024) · doi:10.5194/egusphere-2023-2581-rc1
Comment on egusphere-2023-2581
Clark, A. J., Torres-Romero, I., Jaggi, M., et al. (2024) · doi:10.5194/egusphere-2023-2581-rc2
Clark, A. J. (2024) · doi:10.5194/egusphere-2023-2581-ac2
- Authors
- Watkins, J. M., & Hunt, J. D.
- Affiliations
- University of Oregon (US)
- ENVIRON (United States) (US)
- Corresponding author
- Watkins, J.M.
- ORCID
- Watkins, J.M.
- Venue
- Earth and Planetary Science Letters
- Publisher
- Elsevier BV
- Published
- 2015-12
- Volume
- 432
- Pages
- 152-165
- ISSN
- 0012-821X (ISSN-L)
- OpenAlex
- W1913208140
- Cited by
- 105
- References
- 51
- Citations by year
- 2026: 4 · 2025: 6 · 2024: 11 · 2023: 14 · 2022: 9 · 2021: 17 · 2020: 11 · 2019: 13 · 2018: 9 · 2017: 7 · 2016: 4
- FWCI
- 4.64
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Earth and Planetary Science Letters (acceptedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- University of Oregon
- U.S. Department of Energy (DE-AC02-05CH11231)
- Topics
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Geology and Paleoclimatology Research
- Physical Sciences › Earth and Planetary Sciences › Paleontology › Paleontology and Stratigraphy of Fossils
- Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
- Keywords
- clumped isotopes, calcite, kinetic isotope fractionation, carbon isotopes, oxygen isotopes, crystal growth rate, carbonate mineralogy, foraminifera, coccoliths, deep-sea corals, dissolved inorganic carbon
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