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			<titleStmt><title level='a'>Enhanced superconductivity in spin–orbit proximitized bilayer graphene</title></titleStmt>
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				<date>01/12/2023</date>
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					<idno type="par_id">10406124</idno>
					<idno type="doi">10.1038/s41586-022-05446-x</idno>
					<title level='j'>Nature</title>
<idno>0028-0836</idno>
<biblScope unit="volume">613</biblScope>
<biblScope unit="issue">7943</biblScope>					

					<author>Yiran Zhang</author><author>Robert Polski</author><author>Alex Thomson</author><author>Étienne Lantagne-Hurtubise</author><author>Cyprian Lewandowski</author><author>Haoxin Zhou</author><author>Kenji Watanabe</author><author>Takashi Taniguchi</author><author>Jason Alicea</author><author>Stevan Nadj-Perge</author>
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			<abstract><ab><![CDATA[]]></ab></abstract>
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<div xmlns="http://www.tei-c.org/ns/1.0"><p>In the presence of a large perpendicular electric field, Bernal-stacked bilayer graphene (BLG) features several broken-symmetry metallic phases <ref type="bibr">[1]</ref><ref type="bibr">[2]</ref><ref type="bibr">[3]</ref> as well as magnetic-field-induced superconductivity <ref type="bibr">1</ref> . The superconducting state is quite fragile, however, appearing only in a narrow window of density and with a maximum critical temperature T c &#8776; 30 mK. Here we show that placing monolayer tungsten diselenide (WSe 2 ) on BLG promotes Cooper pairing to an extraordinary degree: superconductivity appears at zero magnetic field, exhibits an order of magnitude enhancement in T c and occurs over a density range that is wider by a factor of eight. By mapping quantum oscillations in BLG-WSe 2 as a function of electric field and doping, we establish that superconductivity emerges throughout a region for which the normal state is polarized, with two out of four spin-valley flavours predominantly populated. In-plane magnetic field measurements further reveal that superconductivity in BLG-WSe 2 can exhibit striking dependence of the critical field on doping, with the Chandrasekhar-Clogston (Pauli) limit roughly obeyed on one end of the superconducting dome, yet sharply violated on the other. Moreover, the superconductivity arises only for perpendicular electric fields that push BLG hole wavefunctions towards WSe 2 , indicating that proximity-induced (Ising) spin-orbit coupling plays a key role in stabilizing the pairing. Our results pave the way for engineering robust, highly tunable and ultra-clean graphene-based superconductors.</p><p>Strong interactions between electrons often lead to a rich competition of symmetry-breaking phases throughout the parameter space. This competition can be substantially altered by external perturbations that lower the energy for one of the phases at the expense of the others. One recent example of such a phase diagram modification occurs in magic-angle twisted bilayer graphene (BLG) <ref type="bibr">4</ref> aligned with hexagonal boron nitride (hBN), in which sublattice polarization stabilizes a Chern insulating phase near a filling of three electrons per moir&#233; unit cell at the expense of suppressing superconductivity <ref type="bibr">5,</ref><ref type="bibr">6</ref> . Here we investigate the symmetry-broken phases in Bernal-stacked BLG coupled to a WSe 2 monolayer and show that the phase diagram is altered such that superconductivity is strongly enhanced.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Asymmetry with displacement field</head><p>Figure <ref type="figure">1a</ref> shows the BLG-WSe 2 stack, whereas Fig. <ref type="figure">1b</ref> displays the corresponding valence bands in the presence of a perpendicular electric displacement field (D), taking into account induced spin-orbit coupling (SOC) by WSe 2 . In a finite D field, BLG features a bandgap at charge neutrality <ref type="bibr">7,</ref><ref type="bibr">8</ref> , trigonal warping <ref type="bibr">9</ref> and prominent Van Hove singularities (VHS) near the weakly dispersive band edge. Owing to the large density of states, interactions between electrons are greatly amplified when the chemical potential crosses the VHS. In addition, a finite D field substantially polarizes the low-energy electronic wavefunctions <ref type="bibr">7,</ref><ref type="bibr">9</ref> (Fig. <ref type="figure">1b</ref> insets) towards the top or bottom layers and on different sublattices A and B. When combined with WSe 2 placed on one side, BLG becomes an ideal platform for probing the interplay between electronic correlations <ref type="bibr">[1]</ref><ref type="bibr">[2]</ref><ref type="bibr">[3]</ref> and induced SOC <ref type="bibr">[10]</ref><ref type="bibr">[11]</ref><ref type="bibr">[12]</ref><ref type="bibr">[13]</ref><ref type="bibr">[14]</ref><ref type="bibr">[15]</ref><ref type="bibr">[16]</ref> .</p><p>Longitudinal resistance R xx measured as a function of carrier density n and D at zero magnetic field shows peaks or dips that emerge and separate from each other as |D| is increased (Fig. <ref type="figure">1c</ref>). These features can be associated with an interplay of Lifshitz transitions and breaking of spin and valley symmetries, similar to the case of hBN-encapsulated BLG <ref type="bibr">1</ref> . Importantly, the resulting phase diagram is strongly asymmetric with respect to the sign of D field. Focusing on hole doping, for both signs of D, the largest resistance peaks (red diagonal regions in Fig. <ref type="figure">1c</ref>) correspond to phases that possess a single spin-valley flavour-polarized Fermi surface, which we denote as FP(1) &#177; (FP(m) denotes a flavour-polarized phase with m degenerate Fermi pockets and &#177; denotes the sign of D; see Extended Data Fig. <ref type="figure">1</ref> for the identification of spin-valley degeneracy). For positive D, this resistive feature spans beyond D/&#1013; 0 = +1 V nm <ref type="bibr">-1</ref> , but is suppressed by D/&#1013; 0 = -0.75 V nm -1 for negative D, where &#1013; 0 is the vacuum permittivity.</p><p>The pronounced &#177;D asymmetry highlights the role of Ising SOC in defining the phase diagram of BLG-WSe 2 . Theoretical calculations <ref type="bibr">11,</ref><ref type="bibr">12</ref> (Fig. <ref type="figure">1b</ref>) confirm that Ising SOC is induced only on the top layer proximate to WSe 2 and that, correspondingly, the SOC-induced spin splitting in the valence band is largely restricted to D &gt; 0, consistent with the D-asymmetric experimental data (Fig. <ref type="figure">1c</ref>; see also Methods). By contrast, Rashba SOC is expected to produce splittings that are largely independent of the sign of D, and thus cannot account for the pronounced &#177;D asymmetry (see also Supplementary Information section 1).</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Superconductivity at zero magnetic field</head><p>The most striking difference in the BLG-WSe 2 phase diagram between positive and negative D fields is the emergence of a broad superconducting region at D &gt; 0 (see Extended Data Figs. <ref type="figure">2</ref><ref type="figure">3</ref><ref type="figure">4</ref>for additional data on other devices). No analogous region has been observed in hBN-encapsulated BLG, in which superconductivity only appears in a finite in-plane magnetic field <ref type="bibr">1</ref> . The critical current of the zero-magnetic-field superconductivity in BLG-WSe 2 exhibits non-trivial doping dependence (Fig. <ref type="figure">1d,</ref><ref type="figure">e</ref>), with two distinct maxima (the larger of which reaches 20 nA). By contrast, at D &lt; 0 a different phase (Fig. <ref type="figure">1e,</ref><ref type="figure">f</ref>) exhibiting highly nonlinear current-dependent resistance is observed for similar values of n and |D| (marked by a green arrow in Fig. <ref type="figure">1c</ref>). This resistive phase is suppressed by small magnetic fields and is similar to the previously reported zero-magnetic-field phase <ref type="bibr">1</ref> .</p><p>The evolution of critical temperature T c with n and D provides further insights into the superconducting phase (Fig. <ref type="figure">2a-c</ref>). The superconducting dome occupies a wide range of doping (approximately 2 &#215; 10 11 cm -2 ; see also Fig. <ref type="figure">1c</ref>) and features a maximal T c of approximately 300 mK. Figure <ref type="figure">2d</ref> shows R xx line cuts at different temperatures; insets show nonlinear current-voltage (I-V) curves at optimal doping, yielding a Berezinskii-Kosterlitz-Thouless (BKT) transition temperature T BKT &#8776; 260 mK (estimated by the temperature where V &#8733; I 3 ). We emphasize that the superconducting critical temperature observed here is an order of magnitude larger than the T c in hBN-encapsulated BLG. Moreover, the relatively high T c does not appear to be sensitive to minor changes of D field, further substantiating the robustness of the superconducting phase. Figure <ref type="figure">2e</ref>,f shows the evolution of the superconducting phase in the presence of an out-of-plane magnetic field B &#10178; . The maximal critical field B c&#10178; &#8776; 15 mT at base temperature yields a corresponding Ginzburg-Landau coherence length &#958; &#934; B = /(2&#960; ) &#8776; 150 nm GL 0 c &#8869; (&#934; 0 is the superconductor flux quantum), and the mean free path &#8467; mf of BLG-WSe 2 is around 10 &#181;m (see Methods and Extended Data Fig. <ref type="figure">5</ref>). Superconductivity thus resides deep in the clean limit, &#958; GL /&#8467; mf &lt; 0.02 similar to the case of hBN-encapsulated BLG and rhombohedral trilayer graphene <ref type="bibr">1,</ref><ref type="bibr">17</ref> . Another prominent feature of both the T and B &#10178; field dependence (Fig. <ref type="figure">2a-c,f</ref>) is a resistive peak that intersects the superconducting dome, effectively splitting it into two regions within a certain range of D fields (note the grey arrow in Fig. <ref type="figure">1c</ref>). This peak signals the presence of another phase that appears to compete with superconductivity. Both the doping range in which this state occurs and its disappearance at relatively low magnetic fields are features shared by the resistive phase observed for D &lt; 0 (see the green arrow in Fig. <ref type="figure">1c</ref>) and in hBN-encapsulated BLG <ref type="bibr">1</ref> . Moreover, both the resistive peak and superconductivity feature a broken-symmetry parent state with two large and emerging small Fermi pockets (see discussion below), indicating that transport in this region is highly sensitive to the exact details of the spin-valley ground states (see Extended Data Fig. <ref type="figure">6</ref> and Supplementary Information section 5 for possible competition between the ground states).</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Quantum oscillations</head><p>The D-field asymmetry is further highlighted by low field (B &#10178; &lt; 1 T) quantum oscillations measured at D/&#1013; 0 = 1 V nm -1 and -1 V nm -1 , which imply distinct Fermi surface structures within the superconductivity region for D &gt; 0 (Fig. <ref type="figure">3a,</ref><ref type="figure">c,</ref><ref type="figure">e</ref>) and within the resistive phase for D &lt; 0 (Fig. <ref type="figure">3b,</ref><ref type="figure">d,</ref><ref type="figure">f</ref>). Fourier transforms of the oscillations, taken with respect to 1/B &#10178; , reveal the phases in the relevant doping ranges. To resolve the relative sizes of the Fermi pockets of the different flavour-polarized phases, the Fourier transform of R xx (1/B &#10178; ) at low magnetic fields (0.05 T &lt; B &#10178; &lt; 0.6 T) is normalized by the frequency corresponding to the full doping density, f norm = n &#215; h/e, so that the resulting frequency f &#957; reveals the fraction of the total Fermi surface area enclosed by a cyclotron orbit (Fig. <ref type="figure">3c,</ref><ref type="figure">d</ref>). Here, h is Planck's constant and e the electron charge.</p><p>At D/&#1013; 0 = -1 V nm -1 , the resulting phase diagram is remarkably similar to that reported on hBN-encapsulated BLG without WSe 2 (ref. <ref type="bibr">1</ref> ; see also Extended Data Fig. <ref type="figure">7</ref>). In addition to the zero-field resistive phase discussed before (Fig. <ref type="figure">1f</ref>), at low densities (|n| &lt; 6 &#215; 10 11 cm -2 ) we observe a Fourier transform peak at f &#957; = 1/12 (along with its higher harmonics) corresponding to a spin-valley symmetric phase with 12 degenerate Fermi pockets produced by trigonal warping (denoted as Sym(12) -). Upon further hole doping, BLG transitions into another phase with two frequency peaks at f &#957; <ref type="bibr">(1)</ref> &lt; 1/2 and f &#957;</p><p>. This phase can be identified as a spin-valley flavour-polarized phase, denoted FP(2, 2) -, with two majority ( f &#957; (1) &lt; 1/2) and two minority ( f &#957; <ref type="bibr">(2)</ref> &lt; 1/12) flavours. The resemblance between our D &lt; 0 data and hBN-encapsulated BLG <ref type="bibr">1</ref> indicates that SOC does not play a major role for D &lt; 0.</p><p>At D/&#1013; 0 = 1 V nm -1 (Fig. <ref type="figure">3c,</ref><ref type="figure">e</ref>), at which the wavefunctions are strongly polarized towards WSe 2 , we see a few notable differences (see also Extended Data Fig. <ref type="figure">8</ref>). First, at low densities, one of the Fourier frequency peaks clearly appears below f &#957; = 1/12, indicating the existence of Fermi surfaces for which the occupancy is smaller relative to Sym( <ref type="formula">12</ref>) -. As we can identify two independent frequencies in this region, we denote this phase as FP(6, 6) + , with six bigger and six smaller Fermi pockets. The explicit flavour polarization here probably originates from spin-orbit-induced band splitting. Second, the transition between the FP(6, 6) + phase and the adjacent FP(2, 2) + phase (with two big and two small Fermi pockets) occurs at a lower hole density of |n| = 5 &#215; 10 11 cm -2 . Finally, we observe that superconductivity is established throughout the FP(2, 2) + phase (except a small region where it competes with the resistive phase) ending on the high doping side with the onset of another complex flavour-polarized phase characterized by the occurrence of additional frequency peaks (Fig. <ref type="figure">3c,</ref><ref type="figure">e</ref>; see also Supplementary Information section 5). Importantly, in FP(2, 2) + , as for FP(2, 2) -, we find that f f</p><p>. Given the non-interacting band structure of Fig. <ref type="figure">1b</ref>, this observation implies that the carriers in each minority flavour are spontaneously polarized to one of the trigonally warped pockets, pointing towards nematic order <ref type="bibr">18,</ref><ref type="bibr">19</ref> (Fig. <ref type="figure">4d,</ref><ref type="figure">e</ref>).</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Doping-dependent Pauli-limit violation</head><p>In-plane magnetic field measurements further illuminate the unconventional nature of superconductivity in BLG-WSe 2 (Fig. <ref type="figure">4</ref> and Extended Data Fig. <ref type="figure">9</ref>). Figure <ref type="figure">4a</ref> shows R xx as a function of density n and in-plane magnetic field B &#8741; for the superconducting region (dark blue) at D/&#1013; 0 = 1.1 V nm -1 . When approaching the superconductivity from low densities |n|, the in-plane critical field B c&#8741; quickly reaches a maximum near the phase boundary separating FP(2, 2) + and FP(6, 6) + , and then slowly decreases with further hole doping. Conversely, the critical temperature measured at zero B &#8741; field, T c 0 (red open circles), shows a more symmetric dome shape with a maximum at higher |n|. The interplay between B c&#8741; and T c 0 indicates that the violation of the Pauli limit</p><p>0 for a weak-coupling spin-singlet Bardeen-Cooper-Schrieffer (BCS) superconductor with g-factor g = 2) varies with doping.  , strongly violating the Pauli limit. Overall the PVR changes from roughly six to one as the doping is increased (Fig. <ref type="figure">4c</ref>; see also Extended Data Fig. <ref type="figure">9f</ref>). Note that the PVR values at the phase boundaries represent a lower limit owing to possible imperfect in-plane alignment of the sample (Methods).</p><p>The large PVR of B c&#8741; /B p &#8776; 6 on the low hole doping side of the superconducting dome evokes the phenomenology of Ising superconductivity observed in transition metal dichalcogenides <ref type="bibr">[20]</ref><ref type="bibr">[21]</ref><ref type="bibr">[22]</ref> . Ising superconductivity refers to a scenario in which pairing connects time-reversed states, for example, k, &#8593;&#10217; | and | k -,&#8595;&#10217; (with k being the wavevector), with spins oriented along a fixed quantization axis selected by Ising SOC. Here, the Ising SOC strength &#955; I &#8776; 0.7 meV, estimated from quantum Hall measurements at small D (see Methods and Extended Data Fig. <ref type="figure">10</ref>), far exceeds the superconducting gap &#916; = 0.76k B T c &#8776; 0.02 meV (k B is the Boltzmann constant) estimated from weak-coupling BCS scaling. The resulting Cooper pairs enjoy resilience against in-plane fields that rotate the spins away from this preferred axis, naturally leading to substantial Pauli-limit violation as measured on the low hole doping side of the dome. The substantial PVR reduction for higher hole doping is more puzzling and implies that the ground state cannot evolve into a predominantly spin or spin-valley polarized (SVP) phase. This reduction could emerge from a doping-dependent change in the flavour polarization of the parent FP(2, 2) + state (see below and Supplementary Information section 7) or in-plane depairing effects (or the interplay between the two). As proof of concept, we consider a simple model that incorporates two depairing mechanisms: Rashba SOC (which favours in-plane spin orientation; see Methods) and orbital in-plane magnetic field effects, both of which compete with the Ising SOC and suppress the PVR (Supplementary Information sections 9 and 10 for details). The solution of a self-consistent superconducting gap equation for this model captures the observed PVR evolution (Fig. <ref type="figure">4c</ref> inset and Extended Data Fig. <ref type="figure">11</ref>) provided that the effective Rashba spin splitting increases with hole density, which may be expected if superconductivity arises from minority Fermi pockets that grow with hole doping.  <ref type="figure">11</ref> and Supplementary Information section 10). d,e, Fermi surfaces of the FP(2, 2) + phase with Ising SOC and nematic order (d), or allowing for IVC order (e). Dashed Fermi pockets correspond to the condition that nematic order is absent. f, Schematics of a proposed scenario in which Ising SOC tilts the energy balance towards IVC order, within which the development of superconductivity is more favoured at the expense of a state which is not conducive to pairing, for example, a valley polarized (VP) state.</p><p>The extended superconducting phase space in BLG-WSe 2 clearly contrasts observations in hBN-encapsulated bilayer and trilayer graphene <ref type="bibr">1,</ref><ref type="bibr">17</ref> , in which superconductivity occurs only within a narrow density range around the symmetry-broken phase boundaries. Moreover, the coincidence of the doping range exhibiting superconductivity with the FP(2, 2) + phase (Fig. <ref type="figure">3c,</ref><ref type="figure">e</ref>) at D &gt; 0 strongly hints that (1) superconductivity descends from the latter broken-symmetry parent state and (2) SOC plays a key role in selecting a symmetry-breaking order conducive to pairing. These observations constrain the possible mechanisms that can lead to T c enhancement <ref type="bibr">23,</ref><ref type="bibr">24</ref> (Methods). Figure <ref type="figure">4f</ref> depicts a phenomenologically motivated scenario wherein multiple nearly degenerate broken-symmetry orders compete. If the FP(2, 2) + phase is, for example, valley polarized in the absence of SOC, then broken inversion and time-reversal symmetries would heavily disfavour pairing, consistent with the absence of superconductivity in BLG-WSe 2 at D &lt; 0 and hBN-encapsulated BLG at zero magnetic field <ref type="bibr">1</ref> . Turning on Ising SOC could then tip the balance in favour of orders that facilitate Cooper pairing. One candidate for this parent state is a primarily spin-valley polarized phase arising because of an interaction-enhanced Ising SOC strength (Supplementary Information sections 5 and 7); however, superconductivity emerging from such a state would exhibit a much larger Pauli-limit violation, which would vary far less with doping (Supplementary Information sections 8-10). We suggest instead that Ising SOC can promote inter-valley coherent (IVC) order that is also amenable to pairing while maintaining compatibility with observed trends (Supplementary Information section 7).</p><p>The nature of superconductivity in graphene-based systems-both moir&#233; and crystalline <ref type="bibr">[25]</ref><ref type="bibr">[26]</ref><ref type="bibr">[27]</ref><ref type="bibr">[28]</ref><ref type="bibr">[29]</ref><ref type="bibr">[30]</ref><ref type="bibr">[31]</ref> -presents an ongoing puzzle. The enticing general similarity between BLG-WSe 2 and moir&#233; graphene superlattices (with WSe 2 <ref type="bibr">32,</ref><ref type="bibr">33</ref> or without <ref type="bibr">[34]</ref><ref type="bibr">[35]</ref><ref type="bibr">[36]</ref><ref type="bibr">[37]</ref><ref type="bibr">[38]</ref> ) can be noticed, as in both systems superconductivity appears intimately connected to the symmetry-broken state in which two out of four spin-valley flavours are predominately populated. Future efforts are needed to address the origin of apparent striking distinctions between different superconducting phases in graphene systems. Finally, induced SOC <ref type="bibr">16,</ref><ref type="bibr">39,</ref><ref type="bibr">40</ref> along with other parameters such as virtual tunnelling <ref type="bibr">24</ref> depends on the relative orientation of WSe 2 (or other transition metal dichalcogenides) and graphene, and is thus tunable-providing a rich landscape for further explorations.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Online content</head><p>Any methods, additional references, Nature Research reporting summaries, source data, extended data, supplementary information, acknowledgements, peer review information; details of author contributions and competing interests; and statements of data and code availability are available at <ref type="url">https://doi.org/10.1038/s41586-022-05446-x</ref>.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Article</head></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Methods</head></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Device fabrication</head><p>All the devices have a dual-graphite gate structure with graphite electrodes and were assembled as follows. First, a thin hBN flake (10-30 nm) is picked up by using a propylene carbonate film previously placed on a polydimethylsiloxane stamp. Then, the hBN flake is used to pick up crystals in the sequence of graphite top gate, top hBN dielectric, an exfoliated monolayer of WSe 2 (commercial source, HQ graphene), BLG, graphite electrodes, bottom hBN dielectric and graphite bottom gate. Care was taken to approach and pick up each flake slowly. In the last step, the whole stack is dropped onto a Si/SiO 2 substrate at 150 &#176;C whereas the propylene carbonate is released at 180 &#176;C. The propylene carbonate is then cleaned off with N-methyl-2-pyrrolidinone. The final geometry is defined by dry etching with a CHF 3 /O 2 plasma and deposition of ohmic edge contacts (Ti/Au, 5 nm/100 nm); see Extended Data Fig. <ref type="figure">2</ref>.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Measurements</head><p>All measurements were performed in a dilution refrigerator (Oxford Triton) with a base temperature of approximately 30 mK, by using standard low-frequency lock-in amplifier techniques. Unless otherwise specified, measurements were taken at the base temperature. Frequencies of the lock-in amplifiers (Stanford Research, models 865a) were kept in the range of 7-40 Hz to reduce the electronic noise and measure the device's d.c. properties. The a.c. excitation was kept at less than 5 nA (most measurements were taken at 0.5-1 nA to preserve the linearity of the system and avoid disturbing the fragile states at low temperatures). Each of the d.c. fridge lines pass through cold filters, including 4 pi filters that filter out a range from approximately 80 MHz to more than 10 GHz, as well as a two-pole resistor-capacitor low-pass filter. Top-gate voltage (v t ) and bottom-gate voltage (v b ) are swept to adjust doping density n = (c t v t + c b v b )/e and displacement field D = (c t v t - c b v b )/2, where c t and c b are top-and bottom-gate capacitance per area calculated from the Landau fan diagram. Note that following this conversion, we observe a small intrinsic D-field offset (D/&#1013; 0 &#8776; 0.025 &#177; 0.005 V nm -1 ; Supplementary Fig. <ref type="figure">1</ref>), which might be related to WSe 2 being placed on one side or asymmetry in top and bottom hBN thicknesses.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Reproducibility of zero-magnetic-field superconductivity</head><p>Extended Data Figure <ref type="figure">2b</ref>,c shows optical images of BLG-WSe 2 devices. We use a dual-graphite gate structure to minimize charge disorder <ref type="bibr">41</ref> . Superconductivity and symmetry-breaking features are exactly the same between different contacts in one device (Extended Data Fig. <ref type="figure">2d,</ref><ref type="figure">e</ref>), owing to the exceptionally high quality of crystalline graphene. Contacts 1-3 of the first device D1 were used for the measurements in the main text. Extended Data Figures <ref type="figure">2</ref><ref type="figure">3</ref><ref type="figure">4</ref>show enhanced superconductivity from three other devices. We found that superconductivity occasionally onsets at a larger D field (D/&#1013; 0 &#8819; 1 V nm -1 ) with another flavour-polarized parent state (FP(2, m &gt; 2) + ). Slight differences between the devices could originate from different SOC strengths <ref type="bibr">16,</ref><ref type="bibr">39,</ref><ref type="bibr">40</ref> induced by WSe 2 ; see below for further discussion. We measured seven BLG-WSe 2 devices in total, and in five we observed zero-magnetic-field superconductivity. The measurements in the other two devices were limited to |D|/&#1013; 0 &#8804; 1 V nm -1 ; on the basis of the phase diagram obtained in the accessible range of D, we speculate that they would also exhibit superconductivity for larger positive D. Finally, we emphasize that none of the measured devices showed zero-magnetic-field superconductivity for D &lt; 0 down to D/&#1013; 0 = -1 V nm -1 (and in some instances to D/&#1013; 0 = -1.1 V nm -1 ).</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Identifying different spin-valley flavour-polarized phases</head><p>BLG-WSe 2 realizes rather complex spin-valley flavour-polarized phases for both positive and negative D fields (Extended Data Figs. <ref type="figure">1,</ref><ref type="figure"/> 7 and 8). We argue that the D &lt; 0 phase diagram is similar to that of hBN-encapsulated BLG, whereas the D &gt; 0 phase diagram has essential differences associated with the interplay between SOC and strong correlations.</p><p>For D &lt; 0, at low |D| and high |n|, FFT shows a prominent peak at f &#957; = 1/4 corresponding to a flavour-symmetric phase that preserves the fourfold spin-valley degeneracy (Sym(4) -; Extended Data Fig. <ref type="figure">1m</ref>). The spin-valley symmetry still holds for high |D| and low |n|, but smaller Fermi pockets are produced by trigonal warping within each flavour, and therefore the system is flavour-symmetric with f &#957; = 1/12 (Sym(12) -; Extended Data Fig. <ref type="figure">1k</ref>). As mentioned in the main text, the diagonal largest-resistance region is a single spin-valley flavour-polarized phase (FP(1) -; Extended Data Fig. <ref type="figure">1i</ref>) that peaks at f &#957; = 1. The remaining flavourpolarized phases have multiple Fermi pockets with distinct Fermi surface areas. At slightly higher |n| adjacent to FP(1) -, the FFT in the region exhibits peaks around f &lt; 1</p><p>. This is a flavour-polarized phase with one majority flavour and one (or more) small Fermi pocket (FP(1, 1) -). At the region we observed the nonlinear resistive phase, the Fermi surface has two frequency peaks near</p><p>, and corresponds to a flavour-polarized phase with two majority (</p><p>) and two minority (</p><p>) flavours (FP(2, 2) -; Extended Data Fig. <ref type="figure">1j</ref>). At lower |n| next to FP(2, 2) -, a flavoursymmetric phase emerges with 12 trigonally warped pockets (Sym(12) -; Extended Data Fig. <ref type="figure">1l</ref>).</p><p>At D &gt; 0, by contrast, the spin degeneracy in each valley is explicitly lifted by Ising SOC (Fig. <ref type="figure">1b</ref>). At high D and low |n|, instead of showing frequency at f &#957; = 1/12, quantum oscillations at the band edge exhibit a peak around f &#957; = 1/6 (Extended Data Fig. <ref type="figure">1f</ref>), and this is consistent with Ising-induced spin splitting such that holes are from small trigonally warped Fermi pockets of single spin species in each valley (FP(6) + ). The region next to FP(2, 2) + also shows different frequencies (FP (6, 6) + ; Extended Data Fig. <ref type="figure">1g</ref>): this can be attributed to Isinginduced band splitting with one spin more filled ( f &gt; 1/12</p><p>) and another spin less filled ( f &lt; 1/12</p><p>) in each valley. Flavour-polarized phases, such as FP(1) + , FP(1, 1) + and FP(2, 2) + (Extended Data Fig. <ref type="figure">1c,</ref><ref type="figure">d,</ref><ref type="figure">e</ref>), are overall not changed much in terms of FFT frequencies, although spin-valley configurations are most likely different from the D &lt; 0 cases. We note that the &#177;D asymmetry of the phase diagram is reflected in both D and n for which flavour-polarized phases extend or onset. Focusing on FP(1) &#177; , besides the asymmetric D extension mentioned in the main text, FP(1) + also onsets at a lower |n| compared with FP(1) - at the same |D|. This is consistent with the picture of Ising SOC. With proximitized Ising SOC at +D, the two spin species in each valley are split in energy: one moves up and the other moves down. Therefore, one spin in each valley is preferentially filled compared with the other, which makes it easier (at lower |n|) to reach the VHS and to trigger flavour polarization.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Similarity to hBN-encapsulated BLG at D &lt; 0</head><p>As discussed in the previous section, at D &lt; 0 the symmetry-broken phases resemble those observed in hBN-encapsulated BLG. In FP(2, 2) -, we observed the resistive phase showing nonlinear critical current behaviour (Fig. <ref type="figure">1f</ref>) at zero magnetic field. The similarity is also supported by fan diagrams and FFT (Extended Data Figs. <ref type="figure">1</ref> and<ref type="figure">7</ref>) as flavour-symmetric and flavour-polarized states observed in hBN-encapsulated BLG are well reproduced at D &lt; 0. However, we did not observe superconductivity with finite in-plane magnetic field at D &lt; 0. The absence of field-induced superconductivity in this regime may reflect a slightly higher electron temperature (approximately 30 mK) and small in-plane-field misalignment. We thus cannot rule out the onset of superconductivity upon more careful characterization. Alternatively, Rashba SOC (which contrary to Ising SOC need not be suppressed at D &lt; 0) is expected to compete against spin polarization favoured by an in-plane field, thus potentially precluding field-induced superconductivity.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Transverse magnetic focusing with out-of-plane magnetic field</head><p>The mean free path &#8467; mf of BLG-WSe 2 is around 10 &#181;m. Extended Data Figure <ref type="figure">5a</ref> shows non-local resistance R nl as a function of n and B &#10178; for D/&#1013; 0 = 0.6 V nm -1 measured with the configuration shown in Extended Data Fig. <ref type="figure">5c</ref>. Data at density n = -7 &#215; 10 11 cm -2 show a pronounced feature around B &#10178; &#8776; 20 mT, which indicates a transverse magnetic focusing <ref type="bibr">42</ref> that is comparable with the electrodes separation of 5 &#181;m, and translates to a mean free path &#8467; mf &#8819; &#960;L/2 &#8776; 7.9 &#181;m. The magnetic focusing feature appears over wide density ranges, including the density (approximately -3 &#215; 10 11 cm -2 ) at which superconductivity is observed at this D field.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Sample alignment with in-plane magnetic field</head><p>In-plane field measurements were performed by mounting the sample vertically with a homemade frame. It is inevitable to introduce a small B &#10178; component when the B &#8741; field is applied owing to the imperfect vertical sample alignment. Transverse magnetic focusing in B &#8741; is a reliable measurement for the angle misalignment as the cyclotron orbits only couple to the B &#10178; component. Extended Data Figure <ref type="figure">5b</ref> shows R nl as a function of n and B &#8741; . The B &#8741; plot qualitatively matches the B &#10178; plot (Extended Data Fig. <ref type="figure">5a</ref>) except for the scaling of the B field axis. The R nl peak feature that appears at B &#10178; &#8776; 20 mT roughly matches the same feature in the in-plane field at B &#8741; &#8776; 7 T. This indicates an in-plane-field misalignment angle &#952; mis &#8776; tan -1 (20 mT/7 T) &#8776; 0.16&#176;.</p><p>Such angle misalignment results in an underestimation of in-plane critical field at regions where B c&#10178; is small, that is, near the phase boundaries. Extended Data Figure <ref type="figure">9c</ref> shows R xx versus n and B &#8741; measured at D/&#1013; 0 &#8776; 1 V nm -1 . At the phase boundary between FP(6, 6) + and FP(2, 2) + (n &#8776; -5 &#215; 10 11 cm -2 ), superconductivity disappears around B &#8741; = 0.7 T, which indicates an out-of-plane field component B &#10178; = 0.7 T &#215; tan(0.16&#176;) &#8776; 2 mT. The B &#10178; = 2 mT component roughly matches B c&#10178; at the same density (Fig. <ref type="figure">2f</ref>). Therefore, we conclude that the PVR around the phase boundaries in Fig. <ref type="figure">4c</ref> only serves as a lower limit as B c&#10178; is rather low at the relevant densities; hence B &#10178; is a main driver for superconductivity suppression at those regions. By contrast, at the density range at which B c&#8741; is roughly consistent with the Pauli limit (higher |n|), superconductivity shows much higher B c&#10178; (Fig. <ref type="figure">2f</ref>). The suppression of superconductivity is then mainly caused by B &#8741; at higher |n|.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Ising SOC</head><p>In the main text, we show that the asymmetric n-D phase diagram provides strong evidence of Ising SOC. Quantum oscillations of the noninteracting phases at D &gt; 0 further support the existence of Ising SOC (Extended Data Fig. <ref type="figure">1</ref> and<ref type="figure">10</ref>). To quantify WSe 2 -induced Ising SOC, we probe the octet zeroth Landau level (LL) in BLG, as few-meV-scale Ising SOC can rearrange the energies of these states. Note that these LL energies are not sensitive to Rashba SOC <ref type="bibr">13</ref> . Previous experiments <ref type="bibr">14,</ref><ref type="bibr">15</ref> have shown that one can quantify the Ising SOC H &#955;&#964; s = z z I 1 2 I (&#955; I is the Ising SOC strength, and &#964; z and s z are Puali matrices in the valley and spin space, respectively) with LLs on opposite graphene layers: the sets of two LLs that cross at &#957; = &#177;3 filling factors have opposite layer polarization, such that their energy difference (at zero D) is given by &#916;E = E Z &#177; &#955; I /2 (E Z is the Zeeman gap between spin-up and spin-down LLs)-only one of the two LLs (with layer polarization close to the WSe 2 ) is affected by the Ising SOC. Therefore, the critical field B* &#8869; that makes &#916;E vanish is</p><p>I (with &#956; B being the Bohr magneton). In Extended Data Fig. <ref type="figure">10a-e</ref>, B* &#8776; 3T &#8869; is the magnetic field at which yellow and green arrows level at the same D, yielding &#955; I &#8776; 0.7 meV.</p><p>Independently, &#955; I can also be extracted from the doping-dependent FFT splitting of quantum oscillations. The inset of Extended Data Fig. <ref type="figure">10h</ref> shows the FFT splitting B split as a function of doping at D/&#1013; 0 = 0.2 V nm -1 . Ising-type splitting is suppressed with increasing |n|, in contrast to Rashba-type splitting, which increases with increasing |n|. The observed splitting is consistent with the value of &#955; I &#8776; 0.7 meV extracted from the quantum Hall measurements, as shown in the inset of Extended Data Fig. <ref type="figure">10h</ref> by comparing it to the band splitting predicted from the band structure calculations at the same D field. This method is, however, less clean than the LL extraction, because Rashba SOC additionally contributes to a spin splitting for both signs of D (see below).</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Rashba SOC</head><p>The effect of Rashba SOC is more subtle in the experiment. Quantum oscillations at higher B &#10178; field provide an upper bound on the Rashba SOC parameter &#955; R &#8818; 4 meV, consistent with previous studies reporting &#955; R ranging from 1 to 15 meV (refs. <ref type="bibr">10,</ref><ref type="bibr">11,</ref><ref type="bibr">43,</ref><ref type="bibr">44</ref> ). Extended Data Figure <ref type="figure">10f-i</ref> shows &#916;R xx versus 1/B &#10178; and the corresponding FFT measured at D/&#1013; 0 = 0.2 V nm -1 and -0.1 V nm -1 , respectively. At D &gt; 0 (Extended Data Fig. <ref type="figure">10h</ref>), FFT reveals a frequency splitting, whereas at D &lt; 0 the splitting is absent (Extended Data Fig. <ref type="figure">10i</ref>). These observations are consistent with the interpretation that, at D &gt; 0, the splitting is mainly caused by Ising SOC; however, at D &lt; 0, the Ising effect is strongly diminished and the Rashba SOC strength &#955; R is not big enough to induce an observable splitting. The FFT peak at D &lt; 0 (Extended Data Fig. <ref type="figure">10i</ref>) has a full-width at half-maximum around 0.8 T, which translates to an upper bound for the bare Rashba SOC strength &#955; R &#8818; 5 meV by comparing with the spin splitting predicted from band structure calculations at the same density n = -2 &#215; 10 12 cm -2 and displacement field D/&#1013; 0 = -0.1 V nm -1 . An upper bound on Rashba SOC can also be extracted from the observed spin splitting at positive D/&#1013; 0 = 0.2 V nm -1 , assuming Ising SOC &#955; I = 0.7 meV (Extended Data Fig. <ref type="figure">10h,</ref><ref type="figure">inset</ref>). From this analysis we find an upper bound &#955; R &#8818; 4 meV, roughly consistent with the bound from the negative D-field data.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Phenomenology of the additional superconducting BLG-WSe 2 devices</head><p>Extended Data Figures <ref type="figure">3</ref> and<ref type="figure">4</ref> show detailed measurements on two additional superconducting devices D3 and D4. Similar to the one in the main text, the two devices also show zero-magnetic-field enhanced superconductivity (T c &#8776; 200 mK) in a wide density range. Key differences are that superconductivity onsets at larger D fields (D/&#1013; 0 &#8819; 1 V nm -1 ) and the flavour-polarized phase hosting superconductivity appears to have multiple minority Fermi pockets together with two majority pockets (denoted as FP(2, m &gt; 2) + ). The variations of the correlated phases among different devices could originate from ground state selection by Ising SOC of different magnitudes; for example, the two additional devices D3 and D4 have Ising SOC &#955; I &#8819; 1.6 meV, which is stronger than &#955; I = 0.7 meV for the device shown in the main text. The smaller SOC for device D1 shown in the main text may originate from the alignment between BLG and WSe 2 ; see Supplementary Fig. <ref type="figure">2</ref>.</p></div>
<div xmlns="http://www.tei-c.org/ns/1.0"><head>Possible mechanisms for T c enhancement</head><p>Experimentally, we observe enhanced superconductivity that develops at zero magnetic field and only for positive D fields, in which Ising SOC is clearly detected. No superconductivity is observed for the negative sign of D for which experimental signatures of SOC are diminished. Moreover, the magnetic field dependence of the superconducting phase is completely altered in comparison with the previously reported superconductivity in hBN-encapsulated BLG <ref type="bibr">1</ref> . These observations strongly indicate that SOC plays a key role in the observation of enhanced superconductivity, although other effects are probably still relevant. In the following, we briefly discuss several other possible origins for the T c enhancement.</p><p>(1) Possible enhancement of T c due to screening. Screening of Coulomb interactions by WSe 2 would be expected to enhance T c if phonons were the pairing glue. However, this screening should be negligible in the case here for two reasons: (a) WSe 2 is an insulator and acts as a dielectric so no additional screening is expected from it; and (b) the graphene interlayer distance in BLG is less than 1 nm, which is much smaller compared with the typical interparticle distance at hole densities at which superconductivity is observed (approximately 15 nm). In this case, screening would be expected to act in a symmetric way in both layers of BLG (and thus for both signs of the D field), contrary to observations. We note that this line of arguments rules out the simplest case of screening of long-range Coulomb interactions whereas other, short-range terms, could still be possible (see also point (3)). ( <ref type="formula">2</ref>) Modifications of phonon bands by WSe 2 . A change in the phonon spectrum is indeed to be expected, as was recently experimentally documented in WSe 2 -proximitized monolayer graphene <ref type="bibr">45</ref> . There, the WSe 2 layer was found to dramatically increase the mobility of graphene at room temperature, which was interpreted to follow from gapping out the acoustic phonon modes. In this case, a simple BCS treatment of superconductivity mediated by acoustic phonons would predict a decrease in T c (assuming the phonon physics is similar for BLG). It may be possible to avoid this reduction if the pairing glue is frequency dependent, but strong constraints are expected in what kind of model can reproduce the data. (3) New types of attractive term mediated by virtual tunnelling to WSe 2 are also possible, as was explored in a recent theoretical work <ref type="bibr">24</ref> . Such effects can contribute to an enhancement of T c , but do not explain which normal state is selected by interactions in the presence of SOC. (4) When doping WSe 2 , superconductivity originating from a dynamical screening of the Coulomb interaction could be realized with the 'slower' electron gas from WSe 2 acting as a retarded polarizable medium for the electrons in BLG, as was purposed in ref. <ref type="bibr">23</ref> . Such a mechanism can result in a superconductivity with T c &#8776; 100 mK the case of monolayer graphene-WSe 2 structure. However, there is no experimental signature indicating that WSe 2 is doped at the relevant doping range in the experiment. </p></div></body>
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