- Open Access
Spatial Correlations of Charge Density Wave Order across the Transition in
Phys. Rev. Lett. 136, 016504 – Published 6 January, 2026
DOI: https://doi.org/10.1103/776d-dnmf
Abstract
Charge density waves (CDWs) involve coupled amplitude and phase degrees of freedom, but direct access to local amplitude correlations remains experimentally challenging. Here, we report cryogenic four-dimensional scanning transmission electron microscopy measurements of CDW ordering in a flake of 24 nm thickness, enabled by liquid-helium-based cooling. By mapping the spatial distribution of CDW superlattice intensities at nanometer-scale resolution and analyzing their autocorrelations, we extract the temperature-dependent correlation length associated with the local amplitude of the CDW order parameter, independent of global phase coherence. Our results reveal that a finite local CDW amplitude is already established well above the transition temperature. When the system is cooled below the transition temperature down to 20 K, the correlation length extends to nearly 110 nm, and the local CDW amplitude is found to strongly anticorrelate with the local strain field.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (57)
- J. M. Tranquada, B. J. Sternlieb, J. D. Axe, Y. Nakamura, and S. Uchida, Evidence for stripe correlations of spins and holes in copper oxide superconductors, Nature (London) 375, 561 (1995).
- A. M. Gabovich, A. I. Voitenko, J. F. Annett, and M. Ausloos, Charge- and spin-density-wave superconductors, Supercond. Sci. Technol. 14, R1 (2001).
- N. N. Wang et al., Competition between charge-density-wave and superconductivity in the kagome metal , Phys. Rev. Res. 3, 043018 (2021).
- F. H. Yu, D. H. Ma, W. Z. Zhuo, S. Q. Liu, X. K. Wen, B. Lei, J. J. Ying, and X. H. Chen, Unusual competition of superconductivity and charge-density-wave state in a compressed topological kagome metal, Nat. Commun. 12, 3645 (2021).
- S. Lee et al., Generic character of charge and spin density waves in superconducting cuprates, Proc. Natl. Acad. Sci. U.S.A. 119, e2119429119 (2022).
- D. Bhoi, S. Khim, W. Nam, B. S. Lee, C. Kim, B.-G. Jeon, B. H. Min, S. Park, and K. H. Kim, Interplay of charge density wave and multiband superconductivity in , Sci. Rep. 6, 24068 (2016).
- Y. Sur et al., Enhanced superconductivity near a pressure-induced quantum critical point of strongly coupled charge density wave order in , NPG Asia Mater. 17, 8 (2025).
- S. Park et al., Superconductivity emerging from a stripe charge order in nanoflakes, Nat. Commun. 12, 3157 (2021).
- G. Grüner, The dynamics of charge-density waves, Rev. Mod. Phys. 60, 1129 (1988).
- X. Zhu, Y. Cao, J. Zhang, E. W. Plummer, and J. Guo, Classification of charge density waves based on their nature, Proc. Natl. Acad. Sci. U.S.A. 112, 2367 (2015).
- R. Hovden et al., Atomic lattice disorder in charge-density-wave phases of exfoliated dichalcogenides (), Proc. Natl. Acad. Sci. U.S.A. 113, 11420 (2016).
- S. H. Sung et al., Endotaxial stabilization of 2D charge density waves with long-range order, Nat. Commun. 15, 1403 (2024).
- D. E. Moncton, J. D. Axe, and F. J. DiSalvo, Study of superlattice formation in and by neutron scattering, Phys. Rev. Lett. 34, 734 (1975).
- G. Grüner, Density Waves in Solids, 1st ed. (CRC Press, Boca Raton, 1994).
- W. L. McMillan, Microscopic model of charge-density waves in , Phys. Rev. B 16, 643 (1977).
- C. M. Varma and A. L. Simons, Strong-coupling theory of charge-density-wave transitions, Phys. Rev. Lett. 51, 138 (1983).
- V. J. Emery and S. A. Kivelson, Importance of phase fluctuations in superconductors with small superfluid density, Nature (London) 374, 434 (1995).
- H. Ding, T. Yokoya, J. C. Campuzano, T. Takahashi, M. Randeria, M. R. Norman, T. Mochiku, K. Kadowaki, and J. Giapintzakis, Spectroscopic evidence for a pseudogap in the normal state of underdoped high- superconductors, Nature (London) 382, 51 (1996).
- U. Chatterjee et al., Emergence of coherence in the charge-density wave state of , Nat. Commun. 6, 6313 (2015).
- K. Iwaya, T. Hanaguri, A. Koizumi, K. Takaki, A. Maeda, and K. Kitazawa, Electronic state of investigated by STM/STS, Physica (Amsterdam) 329–333B, 1598 (2003).
- A. Soumyanarayanan, M. M. Yee, Y. He, J. van Wezel, D. J. Rahn, K. Rossnagel, E. W. Hudson, M. R. Norman, and J. E. Hoffman, Quantum phase transition from triangular to stripe charge order in , Proc. Natl. Acad. Sci. U.S.A. 110, 1623 (2013).
- C. J. Arguello et al., Visualizing the charge density wave transition in in real space, Phys. Rev. B 89, 235115 (2014).
- B. Guster et al., Coexistence of elastic modulations in the charge density wave state of , Nano Lett. 19, 3027 (2019).
- G. Gye, E. Oh, and H. W. Yeom, Topological landscape of competing charge density waves in , Phys. Rev. Lett. 122, 016403 (2019).
- E. Oh, G. Gye, and H. W. Yeom, Defect-selective charge-density-wave condensation in , Phys. Rev. Lett. 125, 036804 (2020).
- S. Yoshizawa, K. Sagisaka, and H. Sakata, Visualization of alternating triangular domains of charge density waves in by scanning tunneling microscopy, Phys. Rev. Lett. 132, 056401 (2024).
- H. K. Kim, S. Y. Kim, C. J. Won, S.-W. Cheong, J. Kim, J. S. Kim, and T.-H. Kim, Dimensional crossover of charge order in with strong interlayer coupling, Phys. Rev. B 107, 045112 (2023).
- K. A. Moler, Imaging quantum materials, Nat. Mater. 16, 1049 (2017).
- J. A. Wilson, F. J. Di Salvo, and S. Mahajan, Charge-density waves in metallic, layered, transition-metal dichalcogenides, Phys. Rev. Lett. 32, 882 (1974).
- C. H. Chen, Electron diffraction study of the charge-density wave superlattice in , Solid State Commun. 49, 645 (1984).
- D. E. Moncton, J. D. Axe, and F. J. DiSalvo, Neutron scattering study of the charge-density wave transitions in and , Phys. Rev. B 16, 801 (1977).
- C. Berthier, D. Jerome, and P. Molinie, NMR study on a single crystal: A microscopic investigation of the charge density waves state, J. Phys. C 11, 797 (1978).
- C.-H. Du, W. J. Lin, Y. Su, B. K. Tanner, P. D. Hatton, D. Casa, B. Keimer, J. P. Hill, C. S. Oglesby, and H. Hohl, X-ray scattering studies of , a superconductor and charge density wave material, under high external magnetic fields, J. Phys. Condens. Matter 12, 5361 (2000).
- T. Wu, H. Mayaffre, S. Krämer, M. Horvatić, C. Berthier, W. N. Hardy, R. Liang, D. A. Bonn, and M.-H. Julien, Incipient charge order observed by NMR in the normal state of , Nat. Commun. 6, 6438 (2015).
- C. Ophus, Four-dimensional scanning transmission electron microscopy (4D-STEM): From scanning nanodiffraction to ptychography and beyond, Microsc. Microanal. 25, 563 (2019).
- J. L. Hart, S. Siddique, N. Schnitzer, S. D. Funni, L. F. Kourkoutis, and J. J. Cha, In operando cryo-STEM of pulse-induced charge density wave switching in , Nat. Commun. 14, 8202 (2023).
- J. L. Hart, H. Pan, S. Siddique, N. Schnitzer, K. Mallayya, S. Xu, L. F. Kourkoutis, E. Kim, and J. J. Cha, Real-space visualization of a defect-mediated charge density wave transition, Proc. Natl. Acad. Sci. U.S.A. 121, e2402129121 (2024).
- J. M. Shen, A. Stangel, S. H. Sung, I. E. Baggari, K. Sun, and R. Hovden, Melting of charge density waves in low dimensions, arXiv:2505.07569.
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/776d-dnmf for technical details on sample characterization, liquid He cooling holder design, CDW peak intensity analysis, assessment of beam-induced specimen damage, and estimation of Se vacancy concentration, which includes Refs. [40–46].
- J. Oh, S. Kim, C. Jeong, J. Manassa, J. Schwartz, S. Yoon, R. Hovden, H. R. Byon, and Y. Yang, Correlative 3D mapping of structure, composition, and valence state dynamics in battery cathodes via simultaneous ADF-EDS-EELS tomography, arXiv:2509.23034.
- Y. Yang et al., Deciphering chemical order/disorder and material properties at the single-atom level, Nature (London) 542, 75 (2017).
- J. Zhou et al., Observing crystal nucleation in four dimensions using atomic electron tomography, Nature (London) 570, 500 (2019).
- H. Jo et al., Direct strain correlations at the single-atom level in three-dimensional core-shell interface structures, Nat. Commun. 13, 5957 (2022).
- C. Jeong et al., Revealing the three-dimensional arrangement of polar topology in nanoparticles, Nat. Commun. 15, 3887 (2024).
- C. Jeong, J. Lee, H. Jo, K. Lee, S. Lee, C. Ophus, P. Ercius, E. Cho, and Y. Yang, Atomic-scale 3D structural dynamics and functional degradation of Pt alloy nanocatalysts during the oxygen reduction reaction, Nat. Commun. 16, 8026 (2025).
- J. Lee and Y. Yang, Advancing atomic electron tomography with neural networks, Appl. Microsc. 55, 7 (2025).
- B. M. Murphy, J. Stettner, M. Traving, M. Sprung, I. Grotkopp, M. Müller, C. S. Oglesby, M. Tolan, and W. Press, Surface behaviour at the charge density wave transition in , Physica (Amsterdam) 336B, 103 (2003).
- K. Cho et al., Using controlled disorder to probe the interplay between charge order and superconductivity in , Nat. Commun. 9, 2796 (2018).
- J.-K. Kim, A. J. F. de Souza, and D. P. Landau, Numerical computation of finite size scaling functions: An alternative approach to finite size scaling, Phys. Rev. E 54, 2291 (1996).
- https://chat.openai.com/chat
- The experimental 4D-STEM data and analysis codes are available at a public website (https://mdail.kaist.ac.kr/NbSe2_CDW_Correlation), and they can also be accessed through an open repository (10.5281/zenodo.17823449).
- T. Malis, S. C. Cheng, and R. F. Egerton, EELS log-ratio technique for specimen-thickness measurement in the TEM, J. Electron Microsc. Tech. 8, 193 (1988).
- E. J. Kirkland, Advanced Computing in Electron Microscopy, 2nd ed. (Springer Science & Business Media, New York, 2010).
- C. Ophus, A fast image simulation algorithm for scanning transmission electron microscopy, Adv. Struct. Chem. Image 3, 13 (2017).
- A. Pryor, C. Ophus, and J. Miao, A streaming multi-GPU implementation of image simulation algorithms for scanning transmission electron microscopy, Adv. Struct. Chem. Image 3, 15 (2017).
- L. Rangel DaCosta et al., prismatic 2.0—Simulation software for scanning and high resolution transmission electron microscopy (STEM and HRTEM), Micron 151, 103141 (2021).
- C. D. Malliakas and M. G. Kanatzidis, Nb–Nb interactions define the charge density wave structure of , J. Am. Chem. Soc. 135, 1719 (2013).