Signatures of chiral superconductivity in rhombohedral graphene

Han, Tonghang; Lu, Zhengguang; Hadjri, Zach; Shi, Lihan; Wu, Zhenghan; Xu, Wei; Yao, Yuxuan; Cotten, Armel A.; Sedeh, Omid Sharifi; Weldeyesus, Henok; Yang, Jixiang; Seo, Junseok; Ye, Shenyong; Zhou, Muyang; Liu, Haoyang; Shi, Gang; Hua, Zhenqi; Watanabe, Kenji; Taniguchi, Takashi; Xiong, Peng; Zumbühl, Dominik M.; Fu, Liang; Ju, Long

doi:10.1038/s41586-025-09169-7

Signatures of chiral superconductivity in rhombohedral graphene

Journal Article · Thu May 22 00:00:00 EDT 2025 · Nature (London)

DOI:https://doi.org/10.1038/s41586-025-09169-7· OSTI ID:2571086

^[1]; ^[2]; Hadjri, Zach ^[1]; Shi, Lihan ^[1]; Wu, Zhenghan ^[1]; Xu, Wei ^[1]; ^[1]; Cotten, Armel A. ^[3]; ^[3]; Weldeyesus, Henok ^[3]; ^[1]; Seo, Junseok ^[1]; ^[1]; Zhou, Muyang ^[1]; Liu, Haoyang ^[4]; Shi, Gang ^[4]; ^[4]; ^[5]; ^[5]; Xiong, Peng ^[4] more »

Massachusetts Institute of Technology, Cambridge, MA (United States)
Massachusetts Institute of Technology, Cambridge, MA (United States); Florida State University, Tallahassee, FL (United States)
University of Basel (Switzerland)
Florida State University, Tallahassee, FL (United States)
National Institute for Materials Science, Tsukuba (Japan)

Chiral superconductors are unconventional superconducting states that break time-reversal symmetry spontaneously and typically feature Cooper pairing at non-zero angular momentum. Such states may host Majorana fermions and provide an important platform for topological physics research and fault-tolerant quantum computing. Despite intensive search and prolonged studies of several candidate systems, chiral superconductivity has remained elusive so far. Here we report the discovery of robust unconventional superconductivity in rhombohedral tetralayer and pentalayer graphene without moiré superlattice effects. We observed two superconducting states in the gate-induced flat conduction bands with T_c up to 300 mK and charge density n_e down to 2.4 ×10¹¹ cm⁻² in five devices. Spontaneous time-reversal-symmetry breaking (TRSB) owing to orbital motion of the electron is found and several observations indicate the chiral nature of these superconducting states, including: (1) in the superconducting state, R_xx shows magnetic hysteresis in varying out-of-plane magnetic field B_⊥—absent from all other superconductors; (2) the superconducting states are robust against in-plane magnetic field and are developed within a spin-polarized and valley-polarized quarter-metal (QM) phase; (3) the normal states show anomalous Hall signals at zero magnetic field and magnetic hysteresis. Here, we also observed a critical B_⊥ of 1.4 T, higher than any graphene superconductivity, which indicates a strong-coupling superconductivity close to the Bardeen–Cooper–Schrieffer (BCS)–Bose–Einstein condensate (BEC) crossover. Our observations establish a pure carbon material for the study of topological superconductivity, with the promise to explore Majorana modes and topological quantum computing.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Institute of Technology, Cambridge, MA (United States)

Sponsoring Organization:: JSPS KAKENHI; Quantum Science and Technologies at the European Campus (QUSTEC); Swiss National Science Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0025325

OSTI ID:: 2571086

Alternate ID(s):: OSTI ID: 2569393

Report Number(s):: DOELongJu--25325

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 8072 Vol. 643; ISSN 1476-4687; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (77)

Electric-field-controlled superconductor–ferromagnetic insulator transition Ma, Likuan; Lei, Bin; Wang, Naizhou Science Bulletin, Vol. 64, Issue 10 https://doi.org/10.1016/j.scib.2019.04.022	journal	May 2019
Superconductivity on the border of itinerant-electron ferromagnetism in UGe2 Saxena, S. S.; Agarwal, P.; Ahilan, K. Nature, Vol. 406, Issue 6796 https://doi.org/10.1038/35020500	journal	August 2000
Coexistence of superconductivity and ferromagnetism in URhGe Aoki, Dai; Huxley, Andrew; Ressouche, Eric Nature, Vol. 413, Issue 6856 https://doi.org/10.1038/35098048	journal	October 2001
Superconductivity in a layered perovskite without copper Maeno, Y.; Hashimoto, H.; Yoshida, K. Nature, Vol. 372, Issue 6506 https://doi.org/10.1038/372532a0	journal	December 1994
Unconventional superconductivity in magic-angle graphene superlattices Cao, Yuan; Fatemi, Valla; Fang, Shiang Nature, Vol. 556, Issue 7699 https://doi.org/10.1038/nature26160	journal	March 2018
Topological superconductivity in monolayer transition metal dichalcogenides Hsu, Yi-Ting; Vaezi, Abolhassan; Fischer, Mark H. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14985	journal	April 2017
Direct imaging of the coexistence of ferromagnetism and superconductivity at the LaAlO₃/SrTiO₃ interface Bert, Julie A.; Kalisky, Beena; Bell, Christopher Nature Physics, Vol. 7, Issue 10, p. 767-771 https://doi.org/10.1038/nphys2079	journal	September 2011
Chiral superconductivity from repulsive interactions in doped graphene Nandkishore, Rahul; Levitov, L. S.; Chubukov, A. V. Nature Physics, Vol. 8, Issue 2 https://doi.org/10.1038/nphys2208	journal	January 2012
Induced superconductivity in the quantum spin Hall edge Hart, Sean; Ren, Hechen; Wagner, Timo Nature Physics, Vol. 10, Issue 9 https://doi.org/10.1038/nphys3036	journal	August 2014
Phonon-mediated unconventional superconductivity in rhombohedral stacked multilayer graphene Viñas Boström, Emil; Fischer, Ammon; Profe, Jonas B. npj Computational Materials, Vol. 10, Issue 1 https://doi.org/10.1038/s41524-024-01345-z	journal	July 2024
Evidence for time-reversal symmetry-breaking kagome superconductivity Deng, Hanbin; Liu, Guowei; Guguchia, Z. Nature Materials https://doi.org/10.1038/s41563-024-01995-w	journal	August 2024
Impact of spin–orbit coupling on superconductivity in rhombohedral graphene Yang, Jixiang; Shi, Xiaoyan; Ye, Shenyong Nature Materials, Vol. 24, Issue 7 https://doi.org/10.1038/s41563-025-02156-3	journal	March 2025
Tunable fractional Chern insulators in rhombohedral graphene superlattices Xie, Jian; Huo, Zihao; Lu, Xin Nature Materials, Vol. 24, Issue 7 https://doi.org/10.1038/s41563-025-02225-7	journal	April 2025
Correlated insulator and Chern insulators in pentalayer rhombohedral-stacked graphene Han, Tonghang; Lu, Zhengguang; Scuri, Giovanni Nature Nanotechnology https://doi.org/10.1038/s41565-023-01520-1	journal	October 2023
Spontaneous broken-symmetry insulator and metals in tetralayer rhombohedral graphene Liu, Kai; Zheng, Jian; Sha, Yating Nature Nanotechnology, Vol. 19, Issue 2 https://doi.org/10.1038/s41565-023-01558-1	journal	November 2023
Nanoscale imaging of equilibrium quantum Hall edge currents and of the magnetic monopole response in graphene Uri, Aviram; Kim, Youngwook; Bagani, Kousik Nature Physics, Vol. 16, Issue 2 https://doi.org/10.1038/s41567-019-0713-3	journal	December 2019
Thermodynamic evidence for a two-component superconducting order parameter in Sr2RuO4 Ghosh, Sayak; Shekhter, Arkady; Jerzembeck, F. Nature Physics, Vol. 17, Issue 2 https://doi.org/10.1038/s41567-020-1032-4	journal	September 2020
Evidence for chiral superconductivity on a silicon surface Ming, F.; Wu, X.; Chen, C. Nature Physics, Vol. 19, Issue 4 https://doi.org/10.1038/s41567-022-01889-1	journal	January 2023
Single-component superconductivity in UTe2 at ambient pressure Theuss, Florian; Shragai, Avi; Grissonnanche, Gaël Nature Physics, Vol. 20, Issue 7 https://doi.org/10.1038/s41567-024-02493-1	journal	May 2024
Nematicity and orbital depairing in superconducting Bernal bilayer graphene Holleis, Ludwig; Patterson, Caitlin L.; Zhang, Yiran Nature Physics, Vol. 21, Issue 3 https://doi.org/10.1038/s41567-024-02776-7	journal	February 2025
Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid Kasahara, Y.; Ohnishi, T.; Mizukami, Y. Nature, Vol. 559, Issue 7713 https://doi.org/10.1038/s41586-018-0274-0	journal	July 2018
Signatures of tunable superconductivity in a trilayer graphene moiré superlattice Chen, Guorui; Sharpe, Aaron L.; Gallagher, Patrick Nature, Vol. 572, Issue 7768 https://doi.org/10.1038/s41586-019-1393-y	journal	July 2019
Constraints on the superconducting order parameter in Sr2RuO4 from oxygen-17 nuclear magnetic resonance Pustogow, A.; Luo, Yongkang; Chronister, A. Nature, Vol. 574, Issue 7776 https://doi.org/10.1038/s41586-019-1596-2	journal	September 2019
Superconductors, orbital magnets and correlated states in magic-angle bilayer graphene Lu, Xiaobo; Stepanov, Petr; Yang, Wei Nature, Vol. 574, Issue 7780 https://doi.org/10.1038/s41586-019-1695-0	journal	October 2019
Chiral superconductivity in heavy-fermion metal UTe2 Jiao, Lin; Howard, Sean; Ran, Sheng Nature, Vol. 579, Issue 7800 https://doi.org/10.1038/s41586-020-2122-2	journal	March 2020
Tunable strongly coupled superconductivity in magic-angle twisted trilayer graphene Park, Jeong Min; Cao, Yuan; Watanabe, Kenji Nature, Vol. 590, Issue 7845 https://doi.org/10.1038/s41586-021-03192-0	journal	February 2021
Superconductivity in rhombohedral trilayer graphene Zhou, Haoxin; Xie, Tian; Taniguchi, Takashi Nature, Vol. 598, Issue 7881 https://doi.org/10.1038/s41586-021-03926-0	journal	September 2021
Half- and quarter-metals in rhombohedral trilayer graphene Zhou, Haoxin; Xie, Tian; Ghazaryan, Areg Nature, Vol. 598, Issue 7881 https://doi.org/10.1038/s41586-021-03938-w	journal	September 2021
Time-reversal symmetry-breaking charge order in a kagome superconductor Mielke, C.; Das, D.; Yin, J. -X. Nature, Vol. 602, Issue 7896 https://doi.org/10.1038/s41586-021-04327-z	journal	February 2022
Quantum cascade of correlated phases in trigonally warped bilayer graphene Seiler, Anna M.; Geisenhof, Fabian R.; Winterer, Felix Nature, Vol. 608, Issue 7922 https://doi.org/10.1038/s41586-022-04937-1	journal	August 2022
Enhanced superconductivity in spin–orbit proximitized bilayer graphene Zhang, Yiran; Polski, Robert; Thomson, Alex Nature, Vol. 613, Issue 7943 https://doi.org/10.1038/s41586-022-05446-x	journal	January 2023
Topological kagome magnets and superconductors Yin, Jia-Xin; Lian, Biao; Hasan, M. Zahid Nature, Vol. 612, Issue 7941 https://doi.org/10.1038/s41586-022-05516-0	journal	December 2022
Orbital multiferroicity in pentalayer rhombohedral graphene Han, Tonghang; Lu, Zhengguang; Scuri, Giovanni Nature, Vol. 623, Issue 7985 https://doi.org/10.1038/s41586-023-06572-w	journal	October 2023
Fractional quantum anomalous Hall effect in multilayer graphene Lu, Zhengguang; Han, Tonghang; Yao, Yuxuan Nature, Vol. 626, Issue 8000 https://doi.org/10.1038/s41586-023-07010-7	journal	February 2024
Superconducting diode effect and interference patterns in kagome CsV3Sb5 Le, Tian; Pan, Zhiming; Xu, Zhuokai Nature, Vol. 630, Issue 8015 https://doi.org/10.1038/s41586-024-07431-y	journal	May 2024
Tunable superconductivity in electron- and hole-doped Bernal bilayer graphene Li, Chushan; Xu, Fan; Li, Bohao Nature, Vol. 631, Issue 8020 https://doi.org/10.1038/s41586-024-07584-w	journal	June 2024
Unconventional superconductivity in chiral molecule–TaS2 hybrid superlattices Wan, Zhong; Qiu, Gang; Ren, Huaying Nature, Vol. 632, Issue 8023 https://doi.org/10.1038/s41586-024-07625-4	journal	June 2024
Extended quantum anomalous Hall states in graphene/hBN moiré superlattices Lu, Zhengguang; Han, Tonghang; Yao, Yuxuan Nature, Vol. 637, Issue 8048 https://doi.org/10.1038/s41586-024-08470-1	journal	January 2025
Superconductivity and spin canting in spin–orbit-coupled trilayer graphene Patterson, Caitlin L.; Sheekey, Owen I.; Arp, Trevor B. Nature, Vol. 641, Issue 8063 https://doi.org/10.1038/s41586-025-08863-w	journal	May 2025
Twist-programmable superconductivity in spin–orbit-coupled bilayer graphene Zhang, Yiran; Shavit, Gal; Ma, Huiyang Nature, Vol. 641, Issue 8063 https://doi.org/10.1038/s41586-025-08959-3	journal	May 2025
Superconductivity and correlated phases in non-twisted bilayer and trilayer graphene Pantaleón, Pierre A.; Jimeno-Pozo, Alejandro; Sainz-Cruz, Héctor Nature Reviews Physics, Vol. 5, Issue 5 https://doi.org/10.1038/s42254-023-00575-2	journal	April 2023
Periodic table for topological insulators and superconductors Kitaev, Alexei; Lebedev, Vladimir; Feigel’man, Mikhail ADVANCES IN THEORETICAL PHYSICS: Landau Memorial Conference, AIP Conference Proceedings https://doi.org/10.1063/1.3149495	conference	January 2009
High-sensitivity heat-capacity measurements on Sr ₂ RuO ₄ under uniaxial pressure Li, You-Sheng; Kikugawa, Naoki; Sokolov, Dmitry A. Proceedings of the National Academy of Sciences, Vol. 118, Issue 10 https://doi.org/10.1073/pnas.2020492118	journal	March 2021
Observation of odd-parity superconductivity in UTe ₂ Li, Zixuan; Moir, Camilla M.; McKee, Nathan J. Proceedings of the National Academy of Sciences, Vol. 122, Issue 13 https://doi.org/10.1073/pnas.2419734122	journal	March 2025
Chiral superconductors Kallin, Catherine; Berlinsky, John Reports on Progress in Physics, Vol. 79, Issue 5 https://doi.org/10.1088/0034-4885/79/5/054502	journal	April 2016
Topological superconductors: a review Sato, Masatoshi; Ando, Yoichi Reports on Progress in Physics, Vol. 80, Issue 7 https://doi.org/10.1088/1361-6633/aa6ac7	journal	May 2017
Polar Kerr effect as probe for time-reversal symmetry breaking in unconventional superconductors Kapitulnik, Aharon; Xia, Jing; Schemm, Elizabeth New Journal of Physics, Vol. 11, Issue 5 https://doi.org/10.1088/1367-2630/11/5/055060	journal	May 2009
Superconductivity in a Strong Spin-Exchange Field Fulde, Peter; Ferrell, Richard A. Physical Review, Vol. 135, Issue 3A https://doi.org/10.1103/PhysRev.135.A550	journal	August 1964
Inhomogeneous time-reversal symmetry breaking in Sr 2 RuO 4 Willa, Roland; Hecker, Matthias; Fernandes, Rafael M. Physical Review B, Vol. 104, Issue 2 https://doi.org/10.1103/PhysRevB.104.024511	journal	July 2021
Multilayer graphenes as a platform for interaction-driven physics and topological superconductivity Ghazaryan, Areg; Holder, Tobias; Berg, Erez Physical Review B, Vol. 107, Issue 10 https://doi.org/10.1103/PhysRevB.107.104502	journal	March 2023
Paired states of fermions in two dimensions with breaking of parity and time-reversal symmetries and the fractional quantum Hall effect Read, N.; Green, Dmitry Physical Review B, Vol. 61, Issue 15 https://doi.org/10.1103/PhysRevB.61.10267	journal	April 2000
Classification of topological insulators and superconductors in three spatial dimensions Schnyder, Andreas P.; Ryu, Shinsei; Furusaki, Akira Physical Review B, Vol. 78, Issue 19 https://doi.org/10.1103/PhysRevB.78.195125	journal	November 2008
Trigonal warping and Berry’s phase N π in ABC-stacked multilayer graphene Koshino, Mikito; McCann, Edward Physical Review B, Vol. 80, Issue 16 https://doi.org/10.1103/PhysRevB.80.165409	journal	October 2009
Stable topological superconductivity in a family of two-dimensional fermion models Cheng, Meng; Sun, Kai; Galitski, Victor Physical Review B, Vol. 81, Issue 2 https://doi.org/10.1103/PhysRevB.81.024504	journal	January 2010
Band structure of A B C -stacked graphene trilayers Zhang, Fan; Sahu, Bhagawan; Min, Hongki Physical Review B, Vol. 82, Issue 3 https://doi.org/10.1103/PhysRevB.82.035409	journal	July 2010
Unifying Optical Selection Rules for Excitons in Two Dimensions: Band Topology and Winding Numbers Cao, Ting; Wu, Meng; Louie, Steven G. Physical Review Letters, Vol. 120, Issue 8 https://doi.org/10.1103/PhysRevLett.120.087402	journal	February 2018
Possibility of Coexistence of Bulk Superconductivity and Spin Fluctuations in U Pt 3 Stewart, G. R.; Fisk, Z.; Willis, J. O. Physical Review Letters, Vol. 52, Issue 8 https://doi.org/10.1103/PhysRevLett.52.679	journal	February 1984
Experimental evidence for a first-order vortex-lattice-melting transition in untwinned, single crystal YBa 2 Cu 3 O 7 Safar, H.; Gammel, P. L.; Huse, D. A. Physical Review Letters, Vol. 69, Issue 5 https://doi.org/10.1103/PhysRevLett.69.824	journal	August 1992
Experimental determination of the superconducting pairing state in YBCO from the phase coherence of YBCO-Pb dc SQUIDs Wollman, D. A.; Van Harlingen, D. J.; Lee, W. C. Physical Review Letters, Vol. 71, Issue 13 https://doi.org/10.1103/PhysRevLett.71.2134	journal	September 1993
Pairing symmetry in cuprate superconductors Tsuei, C. C.; Kirtley, J. R. Reviews of Modern Physics, Vol. 72, Issue 4, p. 969-1016 https://doi.org/10.1103/RevModPhys.72.969	journal	October 2000
Inhomogeneous superconductivity in condensed matter and QCD Casalbuoni, Roberto; Nardulli, Giuseppe Reviews of Modern Physics, Vol. 76, Issue 1 https://doi.org/10.1103/RevModPhys.76.263	journal	February 2004
Non-Abelian anyons and topological quantum computation Nayak, Chetan; Simon, Steven H.; Stern, Ady Reviews of Modern Physics, Vol. 80, Issue 3 https://doi.org/10.1103/RevModPhys.80.1083	journal	September 2008
The electronic properties of graphene Castro Neto, A. H.; Guinea, F.; Peres, N. M. R. Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162 https://doi.org/10.1103/RevModPhys.81.109	journal	January 2009
Topological insulators and superconductors Qi, Xiao-Liang; Zhang, Shou-Cheng Reviews of Modern Physics, Vol. 83, Issue 4 https://doi.org/10.1103/RevModPhys.83.1057	journal	October 2011
Observation of half-quantum flux in the unconventional superconductor β-Bi ₂ Pd Li, Yufan; Xu, Xiaoying; Lee, M. -H. Science, Vol. 366, Issue 6462 https://doi.org/10.1126/science.aau6539	journal	October 2019
Tuning superconductivity in twisted bilayer graphene Yankowitz, Matthew; Chen, Shaowen; Polshyn, Hryhoriy Science, Vol. 363, Issue 6431 https://doi.org/10.1126/science.aav1910	journal	January 2019
Nearly ferromagnetic spin-triplet superconductivity Ran, Sheng; Eckberg, Chris; Ding, Qing-Ping Science, Vol. 365, Issue 6454 https://doi.org/10.1126/science.aav8645	journal	August 2019
Evidence for an edge supercurrent in the Weyl superconductor MoTe ₂ Wang, Wudi; Kim, Stephan; Liu, Minhao Science, Vol. 368, Issue 6490 https://doi.org/10.1126/science.aaw9270	journal	April 2020
Multicomponent superconducting order parameter in UTe ₂ Hayes, I. M.; Wei, D. S.; Metz, T. Science, Vol. 373, Issue 6556 https://doi.org/10.1126/science.abb0272	journal	August 2021
Imaging orbital ferromagnetism in a moiré Chern insulator Tschirhart, C. L.; Serlin, M.; Polshyn, H. Science, Vol. 372, Issue 6548 https://doi.org/10.1126/science.abd3190	journal	June 2021
Spectroscopy signatures of electron correlations in a trilayer graphene/hBN moiré superlattice Yang, Jixiang; Chen, Guorui; Han, Tianyi Science, Vol. 375, Issue 6586 https://doi.org/10.1126/science.abg3036	journal	March 2022
Isospin magnetism and spin-polarized superconductivity in Bernal bilayer graphene Zhou, Haoxin; Holleis, Ludwig; Saito, Yu Science, Vol. 375, Issue 6582 https://doi.org/10.1126/science.abm8386	journal	February 2022
Observation of a Chern insulator in crystalline ABCA-tetralayer graphene with spin-orbit coupling Sha, Yating; Zheng, Jian; Liu, Kai Science, Vol. 384, Issue 6694 https://doi.org/10.1126/science.adj8272	journal	April 2024
Interface-induced superconductivity in magnetic topological insulators Yi, Hemian; Zhao, Yi-Fan; Chan, Ying-Ting Science, Vol. 383, Issue 6683 https://doi.org/10.1126/science.adk1270	journal	February 2024
Large quantum anomalous Hall effect in spin-orbit proximitized rhombohedral graphene Han, Tonghang; Lu, Zhengguang; Yao, Yuxuan Science, Vol. 384, Issue 6696 https://doi.org/10.1126/science.adk9749	journal	May 2024
Electronic Structure of Multilayer Graphene Min, Hongki; MacDonald, Allan H. Progress of Theoretical Physics Supplement, Vol. 176 https://doi.org/10.1143/PTPS.176.227	journal	January 2008
Crossover from Bardeen-Cooper-Schrieffer to Bose-Einstein Condensation and the Unitary Fermi Gas Randeria, Mohit; Taylor, Edward Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031113-133829	journal	March 2014

Similar Records

Revealing the Origin of Time-Reversal Symmetry Breaking in Fe-Chalcogenide Superconductor FeTe1-xSex

Journal Article · Tue Jan 24 19:00:00 EST 2023 · Physical Review Letters · OSTI ID:1960163

Extended quantum anomalous Hall states in graphene/hBN moiré superlattices

Journal Article · Tue Jan 21 19:00:00 EST 2025 · Nature (London) · OSTI ID:2569394

Related Subjects

36 MATERIALS SCIENCE
Chiral Superconductivity
Electronic properties and devices
Rhombohedral Grapehene
Superconducting properties and materials

Signatures of chiral superconductivity in rhombohedral graphene

Citation Formats

References (77)

Similar Records

Related Subjects