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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 1 , 2 , 3 , 4 , 5 , 6 – 7 . Despite intensive search and prolonged studies of several candidate systems 8 , 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 T c up to 300 mK and charge density n e down to 2.4 × 10 11  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. 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 27 . Our observations establish a pure carbon material for the study of topological superconductivity, with the promise to explore Majorana modes and topological quantum computing. Observations indicating the chiral nature of superconducting states in five rhombohedral tetralayer and pentalayer graphene devices without moiré superlattice effects are reported, establishing a pure carbon material for the study of topological superconductivity.

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 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. 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.

Unconventional superconductors exhibit multiple broken symmetries and exceed the range of the Bardeen-Cooper-Schrieffer (BCS) theory. For instance, time-reversal symmetry can be broken in addition to the gauge symmetry, resulting in superconductors that can be enhanced or induced by a magnetic field. However, such unconventional superconductivities are more vulnerable to impurities than their BCS counterparts, requiring highly ordered and clean material systems to observe them. Crystalline rhombohedral multilayer graphene is a promising platform to explore unconventional superconductivity due to its superior material quality and gate-tunable strong correlation effects. Here we report transport measurements of rhombohedral tetralayer and pentalayer graphene, where a spectrum of superconductivities in a clean limit are observed. Three of them (SC2-4) show highly unusual enhancements by magnetic fields: 1. SC2 is strengthened by an in-plane field; 2. SC3 is boosted by a small out-of-plane field; 3. SC4 is induced by an in-plane field. All these superconductors are robust against an in-plane field up to 8.5 Tesla, exceeding the Pauli limit of conventional superconductors by tens of times and suggesting their unconventional nature. Moreover, we observed that proximitized spin-orbit coupling generates a plethora of new superconductors in the phase diagram, while maintaining the high quality of bare rhombohedral graphene. Our work establishes a family of new superconductors in rhombohedral multilayer graphene, which also provides an ideal platform to engineer non-Abelian quasiparticles by proximitizing with quantum anomalous Hall states existing in the same material system.

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 tetra- and penta-layer graphene in the absence of 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 as low as 2.4*1011 cm-2 in three tetralayer and two pentalayer devices. Spontaneous time-reversal-symmetry-breaking (TRSB) due to electron's orbital motion 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, which is absent from all other superconductors; 2. the superconducting states are immune to in-plane magnetic field and are developed within a spin- and valley-polarized quarter-metal phase; 3. the normal states show anomalous Hall signals at zero magnetic field and magnetic hysteresis. We also observed a critical B of up to 1.4 Tesla, higher than any graphene superconductivity reported so far and indicates a strong-coupling superconductivity close to the BCS-BEC crossover. Our observations establish a pure carbon material for the study of topological superconductivity, and pave the way to explore Majorana modes and topological quantum computing.

Tunnel junctions are one of the key elements of chip-scale microsystems serving various technologies from classical microelectronics to quantum information. Aluminium and its oxide (AlOx) have dominated cryogenic tunnel junction technology for decades due to the high quality of AlOx barriers and Al superconducting properties below 1.2 K. However, many applications require non-superconducting junctions, either standalone or in combination with superconducting technology, motivating efforts to suppress Al superconductivity through magnetic fields, doping, or proximity effects -- approaches that so far suffered from integration compatibility and scalability issues. Here, we present a CMOS-compatible normal-metal tunnel junction technology based on TiW alloy and AlOx barriers. We demonstrate wafer-scale fabrication of TiW/Al-AlOx/TiW junctions and validate their performance in Coulomb blockade thermometers operating down to 20 mK, confirming robust normal-state behavior. This TiW-based architecture offers a scalable solution for non-superconducting tunnel junctions across a broad temperature range, enabling integration into advanced cryogenic, quantum and nanoelectronic chip-level systems.

Unconventional superconductors exhibit multiple broken symmetries and exceed the range of the Bardeen-Cooper-Schrieffer (BCS) theory. For instance, time-reversal symmetry can be broken in addition to the gauge symmetry, resulting in superconductors that can be enhanced or induced by a magnetic field. However, such unconventional superconductivities are more vulnerable to impurities than their BCS counterparts, requiring highly ordered and clean material systems to observe them. Crystalline rhombohedral multilayer graphene is a promising platform to explore unconventional superconductivity due to its superior material quality and gate-tunable strong correlation effects. Here we report transport measurements of rhombohedral tetralayer and pentalayer graphene, where a spectrum of superconductivities in a clean limit are observed. Three of them (SC2-4) show highly unusual enhancements by magnetic fields: 1. SC2 is strengthened by an in-plane field; 2. SC3 is boosted by a small out-of-plane field; 3. SC4 is induced by an in-plane field. All these superconductors are robust against an in-plane field up to 8.5 Tesla, exceeding the Pauli limit of conventional superconductors by tens of times and suggesting their unconventional nature. Moreover, we observed that proximitized spin-orbit coupling generates a plethora of new superconductors in the phase diagram, while maintaining the high quality of bare rhombohedral graphene. Our work establishes a family of new superconductors in rhombohedral multilayer graphene, which also provides an ideal platform to engineer non-Abelian quasiparticles by proximitizing with quantum anomalous Hall states existing in the same material system.

Spin-polarized superconductors offer a rare platform for studying electronic correlations, but few candidate systems have been experimentally confirmed to date. Here, we report the observation of a spin-polarized superconducting state, denoted SC5, in WSe2-proximitized rhombohedral trilayer graphene. At in-plane magnetic field B|| = 0 T, SC5 has a critical temperature of 68 mK and an out-of-plane critical magnetic field of only 12 mT. Surprisingly, these values are significantly enhanced as B|| increases, and the superconductivity persists to B|| = 8.8 T. This value corresponds to a record-high Pauli-limit violation ratio of at least 80 among all superconductors, while the true critical field is beyond the limit of our instrument. We conclude that SC5 experiences a canting crossover from Ising-type to spin-polarized superconductor with increased B||.