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Signatures of chiral superconductivity in rhombohedral graphene

Abstract

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 computing1,2,3,4,5,6,7. Despite intensive search and prolonged studies of several candidate systems8,9,10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26, 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 Tc up to 300 mK and charge density ne 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, Rxx 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. 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) crossover27. Our observations establish a pure carbon material for the study of topological superconductivity, with the promise to explore Majorana modes and topological quantum computing.

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Fig. 1: Superconductivity in the flat bands of rhombohedral tetralayer graphene device T3 and pentalayer graphene device P1.
Fig. 2: TRSB and valley polarization in the neighbouring states in the tetralayer device T3.
Fig. 3: Spin and valley polarization in the superconducting states in the pentalayer device P1.
Fig. 4: Temperature-dependent anomalous Hall effects and phase boundary in the tetralayer device T3.
Fig. 5: Superconductivity close to the BCS–BEC crossover.

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Data availability

The data shown in the figures are available from https://doi.org/10.7910/DVN/IADV2O. Other data that support the findings of this study are available from the corresponding author on request.

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Acknowledgements

We acknowledge the helpful discussions with S. D. Sarma, J. Sau, X. G. Wen, S. Todadri, F. Zhang, A. Vishwanath, P. Lee, B. Ramshaw, E. A. Kim, A. MacDonald, T. Devakul and A. Young. This study was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under grant no. DE-SC0025325. Device fabrication was performed at the Harvard Center for Nanoscale Systems and MIT.nano. T.H. acknowledges support from a Mathworks Fellowship. L.F. was supported by a Simons Investigator Award from the Simons Foundation. Work in Basel was supported by the EU’s H2020 Marie Skłodowska-Curie Actions (MSCA) cofund Quantum Science and Technologies at the European Campus (QUSTEC) grant no. 847471, the Swiss National Science Foundation (grant no. 215757), the Georg H. Endress Foundation and WSS Research Center for Molecular Quantum Systems (molQ) of the Werner Siemens Foundation. K.W. and T.T. acknowledge support from the JSPS KAKENHI (grant nos. 20H00354, 21H05233 and 23H02052) and the World Premier International Research Center Initiative, MEXT, Japan.

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Contributions

L.J. supervised the project. T.H. and Z.L. performed the DC magneto-transport measurement. Z. Hadjri, A.A.C., O.S.S., H.W. and D.M.Z. performed some of the in-plane field measurements (Basel). T.H., L.S., Z.W., W.X., Y.Y. and S.Y. fabricated the devices. J.Y., J.S., Z.L. and T.H. helped with installing and testing the dilution refrigerator. T.H. and M.Z. performed the band-structure calculation. H.L., G.S., Z. Hua and P.X. helped with part of the measurements on device T1. K.W. and T.T. grew hBN crystals. L.F. contributed to data analysis. All authors discussed the results and wrote the paper.

Corresponding author

Correspondence to Long Ju.

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D.M.Z. is a co-founder of Basel Precision Instruments. The other authors declare no competing interests.

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Nature thanks Ying-Ming Xie, Petr Stepanov and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available.

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Extended data figures and tables

Extended Data Fig. 1 Superconductivity in rhombohedral tetralayer graphene device T2.

a, Optical micrograph and illustration of the structure of rhombohedral tetralayer graphene, in which the electrons are polarized to the layer far away from WSe2. Scale bar, 3 μm. b, Four-terminal resistance Rxx as a function of ne and gate displacement field D/ε0. Four regions show zero Rxx (labelled as SC1–SC4, respectively) and superconductivity. SC1 and SC2 show fluctuations, whereas SC3 and SC4 are smooth. c, Temperature dependence of the four superconducting states, with critical temperatures extracted from the comparison of IV with the BKT model. See Extended Data Fig. 2. d, Differential resistance dVxx/dI as a function of current I and out-of-plane magnetic field B in the SC3 and SC4 states. Both states show peaks of dV/dI as a signature of superconductivity at small magnetic fields. The superconductivity is killed below 30 mT, similar to that of most graphene-based superconductors. e,f, Rxx and Rxy maps at 0.1 T, extracted by symmetrizing and antisymmetrizing the data taken at B = ±0.1 T. The fluctuations in SC1, SC2 and neighbouring states all disappear. In f, SC1 (SC2) is surrounded (neighboured) by states that show anomalous Hall signals. The value of normal Hall signals at the same ne can be seen in the high-D part of the map. g,h, Magnetic hysteresis scans of Rxy taken at the red and orange circle positions in d, showing loops that are consistent with the anomalous Hall signals in f. i, Rxx map taken at B = 1.5 T. The period of quantum oscillations indicates a QM (as labelled by the arrow) that neighbours SC1. Combined with the anomalous Hall signals as shown in f, this QM is a spin-polarized and valley-polarized phase. j, Rxx in SC1 (at ne = 0.55 × 1012 cm−2 and D/ε0 = 1.02 V nm−1) as a function of time, featuring fluctuations when gate voltages are fixed. k,l, Representative magnetic hysteresis of Rxx taken in SC1 (at ne = 0.57 × 1012 cm−2 and D/ε0 = 1.05 V nm−1) and SC2 (at ne = 0.7 × 1012 cm−2 and D/ε0 = 1.16 V nm−1). We note that one of the four terminals was damaged during measurement, resulting in only three-terminal resistance measurement being possible.

Extended Data Fig. 2 Detailed characterizations of SC1–SC4 in device T2.

a,b, Differential resistance dVxx/dI versus I and B for SC1 and SC2 in device T2, respectively. The vanishing differential resistance persists to about 1 T and about 0.6 T in SC1 and SC2, respectively. c, Bne map at D/ε0 = 1.14 V nm−1. dg, Temperature dependence of longitudinal and differential resistances and BKT fitting for SC1–SC4. These are taken at representative (ne, D) combinations corresponding to Extended Data Fig. 1c. Panels in the same column correspond to a specific superconducting state. Zero resistance, differential resistance peak at critical current and the BKT scaling (VxxI3, as indicated by the dashed lines in the lower panels) can be seen for all four of the superconducting states.

Extended Data Fig. 3 Anomalous Hall effects and TRSB in the normal state of SC1 and SC2 in device T2.

a,b, Symmetrized Rxx and antisymmetrized Rxy map at 0.1 T and 450 mK, above the critical temperatures of SC1 and SC2. The dashed curves in b outline the boundary of SC1 and SC2, inside which clear anomalous Hall signals can be seen in the normal states. c,d, Magnetic hysteresis scans at the dot and triangle positions in b. Clear hysteresis loops can be seen in both the states surrounding SC1, as well as in SC1 and SC2. e,f, Temperature-dependent antisymmetrized Rxy hysteresis at a state in SC1 and SC2, respectively. Curves are shifted vertically for clarity.

Extended Data Fig. 4 Superconductivities in device T3.

a, Optical micrograph of the device. Scale bar, 3 μm. b, Temperature-dependent differential resistance dVxx/dI versus I at a typical (ne, D) inside the SC1 region, featuring zero resistance at low current and a pair of peaks at critical current. c, Temperature-dependent Rxx at a constant D, featuring a density range of zero resistance that corresponds to SC1. df, Differential resistance at typical neD positions inside SC1 and SC3. The vanishing differential resistance persists to about 1 T for SC1, whereas that of SC3 persists to only about 50 mT. g, Rxx as a function of ne and B at D/ε0 = 1.113 V nm−1 in SC3. The density range corresponding to SC3 continues shrinking on B. h, Differential resistance measurement in SC1, showing the superconducting diode effect. i, Representative magnetic hysteresis of Rxx taken in SC1 (at ne = 0.5 × 1012 cm−2 and D/ε0 = 0.985 V nm−1).

Extended Data Fig. 5 Magnetic hysteresis, coercive field and superconducting critical temperature in SC1 in device T3.

a, Rxx as a function of the out-of-plane magnetic field at different ne and D/ε0 = 0.985 V nm−1. The curves are shifted vertically for clarity. The dashed horizontal lines indicate the shift of each curve (which corresponds to zero resistance). Orange and blue arrows indicate the coercive fields, which is defined as the closest-to-zero magnetic field, in which Rxx increases rapidly. b, Colour map of Rxx versus T and ne. c, Summary of the coercive fields and the superconducting Tc at different ne and D/ε0 = 0.985 V nm−1. df, Same as ac but for D/ε0 = 1.015 V nm−1.

Extended Data Fig. 6 Magnetic hysteresis, quantum oscillations and temperature dependence of SC1 in device T3.

a, The neD map of Rxx taken at zero magnetic field in device T3. b, Landau fan diagram taken at D/ε0 = 1.123 V nm−1, revealing quantum oscillations starting at B ≈ 1.5 T. c, Fast Fourier transform spectra of data in b. A diagonal feature above fv = 1 suggests a QM state with annular Fermi surface. However, the low-frequency component of this annular Fermi-surfaced metal is not clear from the data. d, Out-of-plane magnetic field scans of Rxx at different (ne, D) indicated by the coloured dots in a. Magnetic hysteresis was observed across a large range of (ne, D) parameter space across SC1. eg, Upper panels, Rxx as a function of T and ne at three displacement fields cutting through SC1. In all cases, there is a clear boundary as indicated by the black arrow at above Tc. This boundary shifts to lower ne values as the temperature is lowered. Superconductivity domes emerge within the phase to the right of this boundary, suggesting that this phase to the right (the spin-polarized and valley-polarized QM) is the parent state of SC1. Lower panels, linecuts at T = 400 mK from the upper panels, featuring kinks that correspond to the phase boundary between the spin-polarized and valley-polarized QM and the metal state at lower densities.

Extended Data Fig. 7 Superconductivities in device T1.

a, Optical micrograph and device configuration, in which electrons are polarized to the bottom layer of tetralayer graphene with WSe2 at proximity. Scale bar, 3 μm. b,c, The neD maps of Rxx at B = 0 T and base temperature, corresponding to opposite sweeping directions of ne, respectively. Three superconducting regions labelled as SC1–SC3 similar to in devices T2 and T3 can be seen. Some fluctuations can be seen in SC1, SC2 and the neighbouring metallic region. d, The neD map of Rxx at B = 1.5 T and base temperature, featuring the quantum oscillations of a QM to the right of the SC1 region. e,f, The neD map of Rxx and Rxy at B = 0.1 T and base temperature. The fluctuations and SC3 are both suppressed, similar to those observed in device T2. gj, Magnetic hysteresis scans of Rxy taken at the dot, triangle, diamond and star positions in f, showing jumps/loops that are consistent with the anomalous Hall signals in f. k,l, Representative magnetic hysteresis of Rxx taken in SC1 (at ne = 0.54 × 1012 cm−2 and D/ε0 = 1.03 V nm−1) and SC2 (at ne = 0.72 × 1012 cm−2 and D/ε0 = 1.17 V nm−1).

Extended Data Fig. 8 Temperature and magnetic field dependence of superconductivity in device T1.

ac, Temperature dependence of Rxx, the difference resistance dVxx/dI versus I and the BKT fitting of SC1, respectively. d, Temperature-dependent antisymmetrized Rxy hysteresis at a state in SC1. eg, Temperature dependence of Rxx, the difference resistance dV/dI versus I and the BKT fitting of SC2, respectively. h, Temperature-dependent antisymmetrized Rxy hysteresis at a state in SC2. i,j, Rxx and Rxy as a function of ne and B at D/ε0 = 1.075 V nm−1 (corresponding to SC1), respectively. The phase boundary between the QM and SC1 remains at the same ne, indicating that the orbital magnetism is continuous across the boundary and SC1 is orbital magnetic. k,l, Rxx and Rxy as a function of ne and B at D/ε0 = 1.03 V nm−1 (corresponding to SC1), respectively. The phase boundary between the QM and SC1 remains at the same ne, whereas the left boundary of SC1 even moves against the neighbouring state in magnetic field, confirming the orbital magnetic nature of SC1. m,n, Rxx and Rxy as a function of ne and B at D/ε0 = 1.17 V nm−1 (corresponding to SC2), respectively. The phase boundaries between SC2 and neighbouring states move towards SC2 under magnetic field.

Extended Data Fig. 9 Superconductivities in device P1.

a, Optical micrograph of the device. Scale bar, 3 μm. b, The neD map of Rxx at B = 1.5 T and base temperature, featuring the quantum oscillations corresponding to the QM state neighbouring SC1. c,d, The neD map of Rxx and Rxy at B = 0.1 T and base temperature, respectively. e,f, Magnetic hysteresis of Rxy at the green triangle and square positions in d. g,h, Temperature dependence of antisymmetrized Rxy in SC1 (corresponding to the red dot position in d) and SC2 (corresponding to the blue dot position in d), respectively. Curves are shifted vertically for clarity. h,i, Rxx and Rxy as a function of ne and B at D/ε0 = 0.955 V nm−1, respectively. The phase boundary between the QM and SC1 shifts to slightly higher density, suggesting the orbital magnetic nature of SC1. j, The neB map of Rxx at D/ε0 = 1.05 V nm−1, cutting through SC2. k, Magnetic field dependence of Rxx in two representative states inside SC1. We use 10% (indicated by the blue dots) of the normal state resistance to extract the Tc and 5% (red dots) and 15% (green dots) of the normal state resistance to extract the uncertainty of Tc in Fig. 5. l, dVxx/dI versus I in SC1 and SC2 at (0.61 × 1012 cm−2, 0.94 V nm−1) and (0.85 × 1012 cm−2, 1.05 V nm−1), respectively, featuring zero resistance at small current and the resistance spikes at critical current. m, The neD map of Rxx, highlighting (by the orange dashed curve) the phase boundary between the spin-polarized and valley-polarized QM and an UM. n, Temperature-dependent Rxx linecut at D/ε0 = 0.92 V nm−1, in which the QM–UM phase boundary (indicated by the orange dashed arrow) gradually shifts as T is lowered. The SC1 state develops to the right of the boundary, indicating the QM as the parent state of SC1. o, Linecuts from n, showing the QM–UM phase boundary as a kink (orange arrow) in Rxx, which shifts to lower ne as T is lowered.

Extended Data Fig. 10 Superconductivities in device P2.

a, Optical micrograph and illustration of the device configuration. Scale bar, 3 μm. b, Magnetic hysteresis in SC1 (at ne = 0.61 × 1012 cm−2 and D/ε0 = 0.95 V nm−1) and SC2 (at ne = 0.87 × 1012 cm−2 and D/ε0 = 1.07 V nm−1) at base temperature, respectively. c, The neD map of Rxx at zero magnetic field, featuring SC1–SC3. d, The neD map of Rxx at B = 1.5 T, featuring the QM state to the higher density side of SC1. e,f, The neD map of Rxx and Rxy at B = 0.1 T and base temperature. g, Temperature-dependent magnetic hysteresis of Rxy at the star position in e. Curves are shifted vertically for clarity. h,i, Rxx and Rxy as a function of ne and B along the dashed line in e, respectively. The phase boundary between the QM and SC1 shifts to slightly higher density, suggesting the orbital magnetic nature of SC1.

Extended Data Fig. 11 Comparison between the highest superconducting transition temperatures of SC1 in devices T1–T3 and P1.

ad, Upper panels, Rxx as a function of temperature and charge density at a constant D that corresponds to the highest Tc, in the four devices, respectively. Lower panels, the same plots as in the upper panels with a small unified colour scale for a fair comparison. The BKT fitting reveals an increase of TBKT from device T1 to T3, corresponding to a weakening of spin–orbit-coupling effect.

Extended Data Fig. 12 Calculation of the effective mass and Fermi energy in tetralayer and pentalayer rhombohedral graphene.

a, Calculation at a fixed potential difference between the top-most and bottom-most layers Δ = 90 meV in tetralayer graphene. b, Calculation at a fixed charge density ne = 0.5 × 1012 cm−2 in tetralayer graphene. c, Calculation at a fixed potential difference Δ = 110 meV in pentalayer graphene. d, Calculation at a fixed charge density ne = 0.6 × 1012 cm−2 in pentalayer graphene.

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Han, T., Lu, Z., Hadjri, Z. et al. Signatures of chiral superconductivity in rhombohedral graphene. Nature (2025). https://doi.org/10.1038/s41586-025-09169-7

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