Improving U-Pb Dating Accuracy for High-U Stalagmites in Quaternary Records

Abstract

This paper explores the accuracy of U-Pb dating of stalagmites with high uranium contents and high μ values of > 10 000, focusing on Quaternary records. Isotope dilution thermal ionization mass spectrometry (ID-TIMS) and laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) U-Pb dating methods are compared, and it is found that LA-ICP-MS U-Pb dating yields a better precision, especially for samples up to 3 Ma. This research highlights the importance of correcting ²³⁴U/²³⁸U disequilibrium for accurate dating, though ²³⁰Th/²³⁸U calibration is not necessary for Quaternary samples. Common lead correction has a minimal effect on high-uranium samples regardless of whether 2-D or 3-D linear regression is applied to the U-Pb concordia data. The results of the LA-ICP-MS U-Pb method are consistent with those of the ID-TIMS U-Pb method for samples up to 2 Ma, and the error can reach 1.1%–2.9%. Ultimately, this study provides a framework for improving the accuracy of U-Pb dating of high-resolution stalagmite records, which is crucial for paleoenvironment reconstruction.

Keywords

U-Pb dating / disequilibrium correction / common lead correction / high uranium content / accuracy for high-resolution stalagmite records / climate change / geochemistry

References

[1] Bajo P, Drysdale R N, Woodhead J D, et al.. Persistent Influence of Obliquity on Ice Age Terminations since the Middle Pleistocene Transition. Science, 2020, 367(6483): 1235-1239

[2] Bajo P, Drysdale R, Woodhead J, et al.. High-Resolution U-Pb Dating of an Early Pleistocene Stalagmite from Corchia Cave (Central Italy). Quaternary Geochronology, 2012, 14: 5-17

[3] Cheng H, Edwards R L, Sinha A, et al.. The Asian Monsoon over the Past 640 000 Years and Ice Age Terminations. Nature, 2016, 534(7609): 640-646

[4] Cheng T, Zhao J X, Feng Y X, et al.. In-situ LA-MC-ICPMS U-Pb Dating Method for Low-Uranium Carbonate Minerals. Chinese Science Bulletin, 2020, 65(2/3): 150-154

[5] Chew D M, Petrus J A, Kamber B S. U-Pb LA-ICPMS Dating Using Accessory Mineral Standards with Variable Common Pb. Chemical Geology, 2014, 363: 185-199

[6] Chew D M, Sylvester P J, Tubrett M N. U-Pb and Th-Pb Dating of Apatite by LA-ICPMS. Chemical Geology, 2011, 280(1/2): 200-216

[7] Denniston R F, Asmerom Y, Polyak V Y, et al.. Caribbean Chronostratigraphy Refined with U-Pb Dating of a Miocene Coral. Geology, 2008, 36(2): 151-154

[8] Drost K, Chew D, Petrus J A, et al.. An Image Mapping Approach to U-Pb LA-ICP-MS Carbonate Dating and Applications to Direct Dating of Carbonate Sedimentation. Geochemistry, Geophysics, Geosystems, 2018, 19(12): 4631-4648

[9] Engel J, Maas R, Woodhead J, et al.. A Single-Column Extraction Chemistry for Isotope Dilution U-Pb Dating of Carbonate. Chemical Geology, 2020, 531: 119311

[10] Engel J, Woodhead J, Hellstrom J, et al.. Corrections for Initial Isotopic Disequilibrium in the Speleothem U-Pb Dating Method. Quaternary Geochronology, 2019, 54: 101009

[11] Gao Y Y, Li Q L, Liu Y, et al.. Sims U-Pb and U-Th Zircon Age Determination for Quaternary Rocks. Quaternary Sciences, 2016, 36(5): 1015-1026(in Chinese with English Abstract)

[12] Hansman R J, Albert R, Gerdes A, et al.. Absolute Ages of Multiple Generations of Brittle Structures by U-Pb Dating of Calcite. Geology, 2018, 46(3): 207-210

[13] Hiess J, Condon D J, McLean N, et al.. ²³⁸U/²³⁵U Systematics in Terrestrial Uranium-Bearing Minerals. Science, 2012, 335(6076): 1610-1614

[14] Hu Z C, Gao S, Liu Y S, et al.. Signal Enhancement in Laser Ablation ICP-MS by Addition of Nitrogen in the Central Channel Gas. Journal of Analytical Atomic Spectrometry, 2008, 23(8): 1093-1101

[15] Johnson S P, De Waele B, Liyungu K A. U-Pb Sensitive High-Resolution Ion Microprobe (SHRIMP) Zircon Geochronology of Granitoid Rocks in Eastern Zambia: Terrane Subdivision of the Mesoproterozoic Southern Irumide Belt. Tectonics, 2006, 25(6): TC6004

[16] Kanner L C, Burns S J, Cheng H, et al.. High-Resolution Variability of the South American Summer Monsoon over the last Seven Millennia: Insights from a Speleothem Record from the Central Peruvian Andes. Quaternary Science Reviews, 2013, 75: 1-10

[17] Klaus J S, Meeder J F, McNeill D F, et al.. Expanded Florida Reef Development during the Mid-Pliocene Warm Period. Global and Planetary Change, 2017, 152: 27-37

[18] Li Q, Parrish R R, Horstwood M S A, et al.. U-Pb Dating of Cements in Mesozoic Ammonites. Chemical Geology, 2014, 376: 76-83

[19] Li T Y, Shen C C, Li H C, et al.. Oxygen and Carbon Isotopic Systematics of Aragonite Speleothems and Water in Furong Cave, Chongqing, China. Geochimica et Cosmochimica Acta, 2011, 75(15): 4140-4156

[20] Li T Y, Wang X F, Chen C J, et al.. Testing the Initial ²³⁰Th/²³²Th for “Known Age Carbonate” and Its Significance for ²³⁰Th Dating and Paleoclimate Research. Quaternary International, 2022, 607: 113-119

[21] Liu E T, Zhao J X, Pan S Q, et al.. A New Technology of Basin Fluid Geochronology: In-situ U-Pb Dating of Calcite. Earth Science, 2019, 44: 698-712(in Chinese with English Abstract)

[22] Ludwig K R. On the Treatment of Concordant Uranium-Lead Ages. Geochimica et Cosmochimica Acta, 1998, 62(4): 665-676

[23] Luo K, Zhou J X, Feng Y X, et al.. In Situ U-Pb Dating of Calcite from the South China Antimony Metallogenic Belt. iScience, 2020, 23(10): 101575

[24] Mason A J, Henderson G M. Correction of Multi-Collector-ICP-MS Instrumental Biases in High-Precision Uranium-Thorium Chronology. International Journal of Mass Spectrometry, 2010, 295(1/2): 26-35

[25] Mason A J, Henderson G M, Vaks A. An Acetic Acid-Based Extraction Protocol for the Recovery of U, Th and Pb from Calcium Carbonates for U- (Th) -Pb Geochronology. Geostandards and Geoanalytical Research, 2013, 37(3): 261-275

[26] Meyer M C, Cliff R A, Spötl C, et al.. Speleothems from the Earliest Quaternary: Snapshots of Paleoclimate and Landscape Evolution at the Northern Rim of the Alps. Quaternary Science Reviews, 2009, 28(15/16): 1374-1391

[27] Neymark L A, Amelin Y V, Paces J B. ²⁰⁶Pb-²³⁰Th-²³⁴U-²³⁸U and ²⁰⁷Pb-²³⁵U Geochronology of Quaternary Opal, Yucca Mountain, Nevada. Geochimica et Cosmochimica Acta, 2000, 64(17): 2913-2928

[28] Nicholson S L, Pike A W G, Hosfield R, et al.. Pluvial Periods in Southern Arabia over the last 1.1 Million-Years. Quaternary Science Reviews, 2020, 229: 106112

[29] Nuriel P, Weinberger R, Kylander-Clark A R C, et al.. The Onset of the Dead Sea Transform Based on Calcite Age-Strain Analyses. Geology, 2017, 45(7): 587-590

[30] Nuriel P, Wotzlaw J F, Ovtcharova M, et al.. The Use of ASH-15 Flowstone as a Matrix-Matched Reference Material for Laser-Ablation U-Pb Geochronology of Calcite. Geochronology, 2021, 3(1): 35-47

[31] Paton C, Hellstrom J, Paul B, et al.. Iolite: Freeware for the Visualisation and Processing of Mass Spectrometric Data. Journal of Analytical Atomic Spectrometry, 2011, 26(12): 2508-2518

[32] Paton C, Woodhead J D, Hellstrom J C, et al.. Improved Laser Ablation U-Pb Zircon Geochronology through Robust Downhole Fractionation Correction. Geochemistry, Geophysics, Geosystems, 2010, 11(3): Q0AA06

[33] Petrus J A, Kamber B S. VizualAge: a Novel Approach to Laser Ablation ICP-MS U-Pb Geochronology Data Reduction. Geostandards and Geoanalytical Research, 2012, 36(3): 247-270

[34] Pickering R, Dirks P H G M, Jinnah Z, et al.. Australopithecus Sedibaat 1.977 Ma and Implications for the Origins of the GenusHomo. Science, 2011, 333(6048): 1421-1423

[35] Polyak V, Hill C, Asmerom Y. Age and Evolution of the Grand Canyon Revealed by U-Pb Dating of Water Table-Type Speleothems. Science, 2008, 319(5868): 1377-1380

[36] Porcelli D, Swarzenski P W, et al.Bourdon B, Henderson G M, Lundstrom C C, et al.. The Behavior of U- and Th-Series Nuclides in Groundwater. Uranium-Series Geochemistry, 2003317-362

[37] Richards D A, Bottrell S H, Cliff R A, et al.. U-Pb Dating of a Speleothem of Quaternary Age. Geochimica et Cosmochimica Acta, 1998, 62(23/24): 3683-3688

[38] Ring U, Gerdes A. Kinematics of the Alpenrhein-Bodensee Graben System in the Central Alps: Oligocene/Miocene Transtension Due to Formation of the Western Alps Arc. Tectonics, 2016, 35(6): 1367-1391

[39] Roberts N M W, Drost K, Horstwood M S A, et al.. Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS) U-Pb Carbonate Geochronology: Strategies, Progress, and Limitations. Geochronology, 2020, 2(1): 33-61

[40] Roberts N M W, Rasbury E T, Parrish R R, et al.. A Calcite Reference Material for LA-ICP-MS U-Pb Geochronology. Geochemistry, Geophysics, Geosystems, 2017, 18(7): 2807-2814

[41] Roberts N M W, Walker R J. U-Pb Geochronology of Calcite-Mineralized Faults: Absolute Timing of Rift-Related Fault Events on the Northeast Atlantic Margin. Geology, 2016, 44(7): 531-534

[42] Roberts N M W, Žák J, Vacek F, et al.. No More Blind Dates with Calcite: Fluid-Flow Vs. Fault-Slip along the Očkov Thrust, Prague Basin. Geoscience Frontiers, 2021, 12(4): 101143

[43] Shen A J, Hu A P, Cheng T, et al.. Laser Ablation in situ U-Pb Dating and Its Application to Diagenesis-Porosity Evolution of Carbonate Reservoirs. Petroleum Exploration and Development, 2019, 46(6): 1127-1140

[44] Simonetti A, Heaman L M, Chacko T, et al.. In Situ Petrographic Thin Section U-Pb Dating of Zircon, Monazite, and Titanite Using Laser Ablation-MC-ICP-MS. International Journal of Mass Spectrometry, 2006, 253(1/2): 87-97

[45] Sniderman J M K, Woodhead J D, Hellstrom J, et al.. Pliocene Reversal of Late Neogene Aridification. Proceedings of the National Academy of Sciences of the United States of America, 2016, 113(8): 1999-2004

[46] Stacey J S, Kramers J D. Approximation of Terrestrial Lead Isotope Evolution by a Two-Stage Model. Earth and Planetary Science Letters, 1975, 26(2): 207-221

[47] Tera F, Wasserburg G J. U-Th-Pb Systematics in Three Apollo 14 Basalts and the Problem of Initial Pb in Lunar Rocks. Earth and Planetary Science Letters, 1972, 14(3): 281-304

[48] Vaks A, Gutareva O S, Breitenbach S F M, et al.. Speleothems Reveal 500 000-Year History of Siberian Permafrost. Science, 2013, 340(6129): 183-186

[49] Vaks A, Mason A J, Breitenbach S F M, et al.. Palaeoclimate Evidence of Vulnerable Permafrost during Times of Low Sea Ice. Nature, 2020, 577(7789): 221-225

[50] Vermeesch P. IsoplotR: A Free and Open Toolbox for Geochronology. Geoscience Frontiers, 2018, 9(5): 1479-1493

[51] Vermeesch P. Unifying the U-Pb and Th-Pb Methods: Joint Isochron Regression and Common Pb Correction. Geochronology, 2020, 2(1): 119-131

[52] Walker J, Cliff R A, Latham A G. U-Pb Isotopic Age of the StW 573 Hominid from Sterkfontein, South Africa. Science, 2006, 314(5805): 1592-1594

[53] Wang Y J, Cheng H, Edwards R L, et al.. Millennial- and Orbital-Scale Changes in the East Asian Monsoon over the Past 224 000 years. Nature, 2008, 451(7182): 1090-1093

[54] Wendt I. A Three-Dimensional U-Pb Discordia Plane to Evaluate Samples with Common Lead of Unknown Isotopic Composition. Chemical Geology, 1984, 46(1): 1-12

[55] Woodhead J, Hellstrom J, Maas R, et al.. U-Pb Geochronology of Speleothems by MC-ICPMS. Quaternary Geochronology, 2006, 1(3): 208-221

[56] Woodhead J, Hellstrom J, Pickering R, et al.. U and Pb Variability in Older Speleothems and Strategies for Their Chronology. Quaternary Geochronology, 2012, 14: 105-113

[57] Woodhead J, Petrus J. Exploring the Advantages and Limitations of in situ U-Pb Carbonate Geochronology Using Speleothems. Geochronology, 2019, 1(1): 69-84

[58] Woodhead J, Reisz R, Fox D, et al.. Speleothem Climate Records from Deep Time? Exploring the Potential with an Example from the Permian. Geology, 2010, 38(5): 455-458

[59] Woodhead J, Hand S J, Archer M, et al.. Developing a Radiometrically-Dated Chronologic Sequence for Neogene Biotic Change in Australia, from the Riversleigh World Heritage Area of Queensland. Gondwana Research, 2016, 29(1): 153-167

[60] Wu S T, Yang Y H, Roberts N M W, et al.. In situ Calcite U-Pb Geochronology by High-Sensitivity Single-Collector LA-SF-ICP-MS. Science China Earth Sciences, 2022, 65(6): 1146-1160

[61] Yang P, Wu G H, Nuriel P, et al.. In situ LA-ICPMS U-Pb Dating and Geochemical Characterization of Fault-Zone Calcite in the Central Tarim Basin, Northwest China: Implications for Fluid Circulation and Fault Reactivation. Chemical Geology, 2021, 568: 120125

[62] Yang X L, Liu R K, Zhang R, et al.. A Stalagmite δ¹⁸O Record from Jinfo Cave, Southern China Reveals Early-Mid Holocene Variations in the East Asian Summer Monsoon. Quaternary International, 2020, 537: 61-68

[63] Yokoyama T, Kimura J I, Mitsuguchi T, et al.. U-Pb Dating of Calcite Using LA-ICP-MS: Instrumental Setup for Non-Matrix-Matched Age Dating and Determination of Analytical Areas Using Elemental Imaging. Geochemical Journal, 2018, 52(6): 531-540

[64] Zhao Z X, Shi W. LA-(MC-)ICP-MS U-Pb Dating Technique of Calcite and Its Application in Brittle Structures. Journal of Earth Sciences and Environment, 2019, 41(5): 505-516(in Chinese with English Abstract)

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