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Qingrui Cao

Publications and source records attributed to Qingrui Cao.

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Fermiology and the Candidate Chiral Superconductor in Rhombohedral Tetralayer Graphene

Chiral superconductivity, in which the phase of the superconducting order parameter winds in momentum space, has long been sought for its close link to topological superconductivity. Recent work reported a superconductor in rhombohedral multilayer graphene emerging from a time-reversal symmetry broken normal state, suggesting that it could be a chiral superconductor. However, the possibility of chirality depends on the symmetry and structure of the normal-state Fermi surface, which have not been directly measured. Here we measure quantum oscillations in rhombohedral tetralayer graphene over a broad range of the phase diagram, including the superconducting region. At densities well above the onset of superconductivity, we reproduce previously-reported oscillations consistent with a spin- and valley-polarized quarter metal with a single simply-connected Fermi pocket. As the carrier density is reduced, we find a transition to a complex "multitone" state that persists through the superconducting region. This state's spectrum of quantum oscillations is incompatible with a simply-connected quarter metal. The next-simplest candidate normal states suggested by our microscopic modeling (fully-polarized annular, nematic, and three-pocket states) are inconsistent with our measurements, albeit difficult to rule out entirely. The normal state is thus seen to be richer than previously envisaged, reshaping the search for the superconducting mechanism and the possible chirality of the pairing channel.

cond-mat.supr-con

Visualizing orbital magnetism in electron doped rhombohedral multilayer graphene

Electron doped rhombohedral multilayer graphene at high displacement field features an exceptionally flat band minimum with near-ideal quantum geometry. Experiments in this regime observe the formation of a 'quarter metal,' in which the electron liquid condenses into a single spin- and valley flavor. Remarkably, recent experiments have found a zero resistance state in the same region of the density- and displacement-field-tuned parameter space, attributed to the formation of a chiral superconductor from an orbitally ferromagnetic normal state. Here, we use nanoSQUID-on-tip magnetometry to map the orbital magnetization of electron-doped rhombohedral graphene devices ranging in thickness between 3 and 15 layers. Magnetization within the quarter metal phases peaks at finite density, consistent with concentration of the Berry curvature in a finite-momentum 'ring of fire'. Correlating transport and local magnetometry data in a superconducting tetralayer sample reveals a finite orbital ferromagnetic moment, providing direct evidence of valley polarization in the superconducting ground state. We further show that widely observed stochastic switching of the resistivity in both metallic and superconducting regimes arises from a density-tuned sign change in the valley-resolved total magnetic moment. This leads to the formation of metastable magnetic domains under typical gate control sequences and can also be harnessed for electric-field controlled switching of the magnetization across the entire device. Finally, high resolution measurements of the magnetization across a superconducting transition allow us to put an upper bound on the 'condensation magnetization' of 0.1 Bohr magneton per carrier, placing a strong quantitative restriction on theoretical models for ferromagnetic superconductivity.

cond-mat.mes-hall

Anomalously Enhanced Diffusivity of Moiré Excitons via Manipulating the Interplay with Correlated Electrons

Semiconducting transitional metal dichalcogenides (TMDCs) moiré superlattice provides an exciting platform for manipulating excitons. The in-situ control of moiré potential confined exciton would usher in unprecedented functions of excitonic devices but remains challenging. Meanwhile, as a dipolar composite boson, interlayer exciton in the type-II aligned TMDC moiré superlattice strongly interacts with fermionic charge carriers. Here, we demonstrate active manipulation of the exciton diffusivity by tuning their interplay with correlated carriers in moiré potentials. At fractional fillings where carriers are known to form generalized Wigner crystals, we observed suppressed diffusivity of exciton. In contrast, in Fermi liquid states where carriers dynamically populate all moiré traps, the repulsive carrier-exciton interaction can effectively reduce the moiré potential confinement seen by the exciton, leading to enhanced diffusivity with the increase of the carrier density. Notably, the exciton diffusivity is enhanced by orders of magnitude near the Mott insulator state, and the enhancement is much more pronounced for the 0-degree than the 60-degree aligned WS2/WSe2 heterobilayer due to the more localized nature of interlayer excitons. Our study inspires further engineering and controlling exotic excitonic states in TMDC moiré superlattices for fascinating quantum phenomena and novel excitonic devices.

cond-mat.mes-hall

Nanoscale ferroelectric programming of van der Waals heterostructures

The ability to create superlattices in van der Waals (vdW) heterostructures via moiré interference heralded a new era in the science and technology of two-dimensional materials. Through precise control of the twist angle, flat bands and strongly correlated phases have been engineered. The precise twisting of vdW layers is in some sense a bottom-up approach--a single parameter can dial in a wide range of periodic structures. Here, we describe a top-down approach to engineering nanoscale potentials in vdW layers using a buried programmable ferroelectric layer. Ultra-low-voltage electron beam lithography (ULV-EBL) is used to program ferroelectric domains in a ferroelectric Al_{1-x}B_{x}N thin film through a graphene/hexagonal boron nitride (hBN) heterostructure that is transferred on top. We demonstrate ferroelectric field effects by creating a lateral p-n junction, and demonstrate spatial resolution down to 35 nm, limited by the resolution of our scanned probe characterization methods. This innovative, resist-free patterning method is predicted to achieve 10 nm resolution and enable arbitrary programming of vdW layers, opening a pathway to create new phases that are inaccessible by moiré techniques. The ability to "paint" different phases of matter on a single vdW "canvas" provides a wealth of new electronic and photonic functionalities.

cond-mat.mtrl-sci

Tunneling Spectroscopy of Two-Dimensional Materials Based on Via Contacts

We introduce a novel planar tunneling architecture for van der Waals heterostructures based on via contacts, namely metallic contacts embedded into through-holes in hexagonal boron nitride ($h$BN). We use the via-based tunneling method to study the single-particle density of states of two different two-dimensional (2D) materials, NbSe$_2$ and graphene. In NbSe$_2$ devices, we characterize the barrier strength and interface disorder for barrier thicknesses of 0, 1 and 2 layers of $h$BN and study the dependence on tunnel-contact area down to $(44 \pm 14)^2 $ nm$^2$. For 0-layer $h$BN devices, we demonstrate a crossover from diffusive to point contacts in the small-contact-area limit. In graphene, we show that reducing the tunnel barrier thickness and area can suppress effects due to phonon-assisted tunneling and defects in the $h$BN barrier. This via-based architecture overcomes limitations of other planar tunneling designs and produces high-quality, ultra-clean tunneling structures from a variety of 2D materials.

cond-mat.mes-hall

Direct measurement of ferroelectric polarization in a tunable semimetal

Ferroelectricity, the electrostatic counterpart to ferromagnetism, has long been thought to be incompatible with metallicity due to screening of electric dipoles and external electric fields by itinerant charges. Recent measurements, however, demonstrated signatures of ferroelectric switching in the electrical conductance of bilayers and trilayers of WTe$_2$, a semimetallic transition metal dichalcogenide with broken inversion symmetry. An especially promising aspect of this system is that the density of electrons and holes can be continuously tuned by an external gate voltage. This degree of freedom enables investigation of the interplay between ferroelectricity and free carriers, a previously unexplored regime. Here, we employ capacitive sensing in dual-gated mesoscopic devices of bilayer WTe$_2$ to directly measure the spontaneous polarization in the metallic state and quantify the effect of free carriers on the polarization in the conduction and valence bands, separately. We compare our results to a low-energy model for the electronic bands and identify the layer-polarized states that contribute to transport and polarization simultaneously. Bilayer WTe$_2$ is thus shown to be a canonical example of a ferroelectric metal and an ideal platform for exploring polar ordering, ferroelectric transitions, and applications in the presence of free carriers.

cond-mat.mes-hall

Observation of the Interlayer Exciton Gases in WSe$_2$ -p: WSe$_2$ Heterostructures

Interlayer excitons (IXs) possess a much longer lifetime than intralayer excitons due to the spatial separation of the electrons and holes; hence, they have been pursued to create exciton condensates for decades. The recent emergence of two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs), and of their van der Waals heterostructures (HSs), in which two different 2D materials are layered together, has created new opportunities to study IXs. Here we present the observation of IX gases within two stacked structures consisting of hBN/WSe$_2$/hBN/p: WSe$_2$/hBN. The IX energy of the two different structures differed by 82 meV due to the different thickness of the hBN spacer layer between the TMD layers. We demonstrate that the lifetime of the IXs is shortened when the temperature and the pump power increase. We attribute this nonlinear behavior to an Auger process.

cond-mat.mtrl-sci