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Volume 11 Issue 5
Sep.  2026
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Article Contents
Thomas Meier, Meng Yang, Yishan Zhou, Yunhua Fu, Rui Zhang, Ziliang Wang, Tianyao Zheng, Rajesh Jana, Takeshi Nakagawa. T1–T2 microscale correlation relaxometry for in situ high-pressure nuclear magnetic resonance[J]. Matter and Radiation at Extremes, 2026, 11(5): 057803. doi: 10.1063/5.0320998
Citation: Thomas Meier, Meng Yang, Yishan Zhou, Yunhua Fu, Rui Zhang, Ziliang Wang, Tianyao Zheng, Rajesh Jana, Takeshi Nakagawa. T1–T2 microscale correlation relaxometry for in situ high-pressure nuclear magnetic resonance[J]. Matter and Radiation at Extremes, 2026, 11(5): 057803. doi: 10.1063/5.0320998

T1–T2 microscale correlation relaxometry for in situ high-pressure nuclear magnetic resonance

doi: 10.1063/5.0320998
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  • Corresponding author: a)Author to whom correspondence should be addressed: thomas.meier@sharps.ac.cn
  • Received Date: 2026-01-05
  • Accepted Date: 2026-06-03
  • Available Online: 2026-09-28
  • Publish Date: 2026-09-01
  • Over the last decade, frequency-domain in situ high-pressure nuclear magnetic resonance (NMR) spectroscopy in diamond anvil cells (DACs) has been employed as a structural and electronic probe of condensed matter systems at pressures well into the megabar range. However, extensive spin interactions and sample heterogeneities under pressure often lead to significant spectral overlap, inhibiting independent observation of chemically similar spin subspecies in the same sample. In this work, we introduce a time-domain relaxometry framework specifically suited for DAC experiments. Experimental flexibility and operational robustness are benchmarked on three hydrogen-rich molecular solids at pressures up to 72 GPa. We demonstrate that T1–T2 relaxometry can separate distinct proton populations in relaxation space even when the corresponding frequency-domain spectra are strongly broadened and overlapping, thereby establishing a practical route to relaxation-based high-pressure NMR analysis in molecular solids.
  • The authors have no conflicts to disclose.
    Conflict of Interest
    Thomas Meier: Conceptualization (equal); Data curation (equal); Formal analysis (equal); Funding acquisition (equal); Investigation (equal); Methodology (equal); Project administration (equal); Resources (equal); Software (equal); Supervision (equal); Validation (equal); Visualization (equal); Writing – original draft (equal); Writing – review & editing (equal). Meng Yang: Conceptualization (equal); Formal analysis (equal); Investigation (equal); Validation (equal); Visualization (equal); Writing – review & editing (equal). Yishan Zhou: Data curation (equal); Formal analysis (equal); Investigation (equal); Methodology (equal); Validation (equal); Visualization (equal); Writing – review & editing (equal). Yunhua Fu: Data curation (equal); Investigation (supporting); Methodology (supporting); Writing – review & editing (equal). Rui Zhang: Investigation (supporting); Visualization (equal); Writing – review & editing (equal). Ziliang Wang: Investigation (supporting); Software (supporting); Writing – review & editing (supporting). Tianyao Zheng: Software (supporting); Writing – review & editing (supporting). Rajesh Jana: Methodology (supporting); Writing – original draft (supporting); Writing – review & editing (supporting). Takeshi Nakagawa: Conceptualization (supporting); Investigation (supporting); Software (supporting); Writing – original draft (supporting); Writing – review & editing (supporting).
    Author Contributions
    Meng Yang and Yishan Zhou contributed equally to this work.
    T.M., M.Y., and Y.Z. were responsible for the concept of this study. Y.F., R.Z., Z.W., and T.Z. were responsible for its preparation. T.M., R.J., and T.N. carried out the experiments. T.M., M.Y., Y.Z., and Y.F. performed the data analysis. T.M., M.Y., Y.Z., R.J., and T.N. wrote the manuscript.
    The Python script used for data analysis in this study is available from the corresponding author upon reasonable request.
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  • [1]
    M. I. Eremets, High Pressure Experimental Methods, 1st ed. (Oxford University Press, Oxford, New York, 1996).
    [2]
    J. L. Yarger, R. A. Nieman, G. H. Wolf, and R. F. Marzke, “High-pressure 1H and 13C nuclear magnetic resonance in a diamond anvil cell,” J. Magn. Reson., Ser. A 114(2), 255–257 (1995).10.1006/jmra.1995.1134
    [3]
    T. Okuchi, “Collision and diffusion dynamics of dense molecular hydrogen by diamond anvil cell nuclear magnetic resonance,” J. Phys. Chem. C 116(3), 2179–2182 (2012).10.1021/jp206732f
    [4]
    T. Meier, N. Wang, D. Mager, J. G. Korvink, S. Petitgirard et al., “Magnetic flux tailoring through Lenz lenses for ultrasmall samples: A new pathway to high-pressure nuclear magnetic resonance,” Sci. Adv. 3(12), eaao5242 (2017).10.1126/sciadv.aao5242
    [5]
    T. Meier, A. P. Dwivedi, S. Khandarkhaeva, T. Fedotenko, N. Dubrovinskaia et al., “Table-top nuclear magnetic resonance system for high-pressure studies with in situ laser heating,” Rev. Sci. Instrum. 90(12), 123901–123912 (2019).10.1063/1.5128592
    [6]
    T. Meier, S. Petitgirard, S. Khandarkhaeva, and L. Dubrovinsky, “Observation of nuclear quantum effects and hydrogen bond symmetrisation in high pressure ice,” Nat. Commun. 9(1), 2766 (2018).10.1038/s41467-018-05164-x
    [7]
    T. Meier, F. Trybel, S. Khandarkhaeva, G. Steinle-Neumann, S. Chariton et al., “Pressure-induced hydrogen-hydrogen interaction in metallic FeH revealed by NMR,” Phys. Rev. X 9(3), 031008 (2019).10.1103/physrevx.9.031008
    [8]
    T. Meier, D. Laniel, and F. Trybel, “Direct hydrogen quantification in high-pressure metal hydrides,” Matter Radiat. Extremes 8(1), 018401 (2023).10.1063/5.0119159
    [9]
    C. P. Slichter, Principles of Magnetic Resonance, 2nd ed. (Springer, Berlin, Heidelberg, 1978).
    [10]
    M. Levitt, Spin Dynamics: Basics of Nuclear Magnetic Resonance, Concepts in Magnetic Resonance Part A, 2nd ed. (2009), Vol. 34A, pp. 60–61.
    [11]
    Y. Zhou, Y. Fu, M. Yang, I. Osmond, R. Jana et al., “Diffusion-driven transient hydrogenation in metal superhydrides at extreme conditions,” Nat. Commun. 16(1), 1135 (2025).10.1038/s41467-025-56033-3
    [12]
    T. Meier, D. Laniel, M. Pena-Alvarez, F. Trybel, S. Khandarkhaeva et al., “Nuclear spin coupling crossover in dense molecular hydrogen,” Nat. Commun. 11(1), 6334 (2020).10.1038/s41467-020-19927-y
    [13]
    T. Meier, S. Khandarkhaeva, J. Jacobs, N. Dubrovinskaia, and L. Dubrovinsky, “Improving resolution of solid state NMR in dense molecular hydrogen,” Appl. Phys. Lett. 115(13), 131903 (2019).10.1063/1.5123232
    [14]
    T. Meier, A. Aslandukova, F. Trybel, D. Laniel, T. Ishii et al., “In situ high-pressure nuclear magnetic resonance crystallography in one and two dimensions,” Matter Radiat. Extremes 6(6), 068402–068411 (2021).10.1063/5.0065879
    [15]
    [16]
    A. G. Redfield, “On the theory of relaxation processes,” IBM J. Res. Dev. 1(1), 19–31 (1957).10.1147/rd.11.0019
    [17]
    [18]
    E. C. Reynhardt and C. J. Terblanche, “13C relaxation in natural diamond,” Chem. Phys. Lett. 269(5–6), 464–468 (1997).10.1016/S0009-2614(97)00309-6
    [19]
    Y.-Q. Song, L. Venkataramanan, M. D. Hürlimann, M. Flaum, P. Frulla et al., “T1–T2 correlation spectra obtained using a fast two-dimensional Laplace inversion,” J. Magn. Reson. 154(2), 261–268 (2002).10.1006/jmre.2001.2474
    [20]
    P. Galvosas, Y. Qiao, M. Schönhoff, and P. T. Callaghan, “On the use of 2D correlation and exchange NMR spectroscopy in organic porous materials,” Magn. Reson. Imaging 25(4), 497–500 (2007).10.1016/j.mri.2006.11.009
    [21]
    N. Bloembergen, E. M. Purcell, and R. V. Pound, “Relaxation effects in nuclear magnetic resonance absorption,” Phys. Rev. 73(7), 679–712 (1948).10.1103/physrev.73.679
    [22]
    H. Y. Carr and E. M. Purcell, “Effects of diffusion on free precession in nuclear magnetic resonance experiments,” Phys. Rev. 94(3), 630–638 (1954).10.1103/physrev.94.630
    [23]
    S. Meiboom and D. Gill, “Modified spin-echo method for measuring nuclear relaxation times,” Rev. Sci. Instrum. 29(8), 688–691 (1958).10.1063/1.1716296
    [24]
    T. Meier, S. Khandarkhaeva, S. Petitgirard, T. Körber, A. Lauerer et al., “NMR at pressures up to 90 GPa,” J. Magn. Reson. 292, 44–47 (2018).10.1016/j.jmr.2018.05.002
    [25]
    Y. Akahama and H. Kawamura, “High-pressure Raman spectroscopy of diamond anvils to 250 GPa: Method for pressure determination in the multimegabar pressure range,” J. Appl. Phys. 96(7), 3748–3751 (2004).10.1063/1.1778482
    [26]
    Y. Akahama and H. Kawamura, “Pressure calibration of diamond anvil Raman gauge to 310 GPa,” J. Appl. Phys. 100(4), 043516–043518 (2006).10.1063/1.2335683
    [27]
    T. J. Koller, S. Jin, V. Krol, S. J. Ambach, U. Ranieri et al., “Simple molecules under high-pressure and high-temperature conditions: Synthesis and characterization of α- and β-C(NH)2 with fully sp3-hybridized carbon,” Angew. Chem., Int. Ed. 63(7), e202318214 (2024).10.1002/anie.202318214
    [28]
    Q. Hu and H.-k. Mao, “Role of hydrogen and proton transportation in Earth’s deep mantle,” Matter Radiat. Extremes 6(6), 068101–068111 (2021).10.1063/5.0069643
    [29]
    C. Ji, B. Li, W. Liu, J. S. Smith, A. Björling et al., “Crystallography of low Z material at ultrahigh pressure: Case study on solid hydrogen,” Matter Radiat. Extremes 5(3), 038401 (2020).10.1063/5.0003288
    [30]
    H. Yuan and L. Zhang, “In situ determination of crystal structure and chemistry of minerals at Earth’s deep lower mantle conditions,” Matter Radiat. Extremes 2(3), 117–128 (2017).10.1016/j.mre.2017.01.002
    [31]
    H.-k. Mao and W. L. Mao, “Key problems of the four-dimensional Earth system,” Matter Radiat. Extremes 5(3), 038102–038105 (2020).10.1063/1.5139023
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