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Daniel Margineda

Publications and source records attributed to Daniel Margineda.

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Signatures of time-reversal-symmetry breaking in multiband 2H-TaS2 revealed by zero-field Josephson nonreciprocity

Superconductors that spontaneously break time-reversal symmetry host complex order parameters and are widely regarded as a hallmark of unconventional superconductivity. Whether such symmetry breaking can also arise in superconductors with nominally isotropic spin-singlet pairing remains an open question. Here we report a zero-field Josephson diode effect in noncentrosymmetric 2H-TaS2/2H-NbSe2 van der Waals junctions. The diode efficiency shows no systematic correlation with supercurrent amplitude, TaS2 thickness, or normal-state resistance, arguing against simple extrinsic, purely interfacial, or transparency-driven mechanisms. Time-reversal-symmetric scenarios are further tested using symmetry-controlled and molecule-intercalated control devices, in which the nonreciprocal response is absent or strongly reduced. Normal-state Hall transport in TaS2 exhibits a nonlinear response consistent with multiband correlated electronic states. Within a Josephson framework, our modelling shows that interband scattering acts as a phase-locking mechanism generating an intrinsic anomalous phase difference and a nonsinusoidal asymmetric current-phase relation, leading to finite zero-field rectification. Together, zero-field Josephson nonreciprocity and nonlinear Hall transport provide complementary evidence for a multiband superconducting phase structure in 2H-TaS2, consistent with intrinsic time-reversal-symmetry breaking.

cond-mat.supr-con

Degenerate monolayer Ising superconductors via chiral-achiral molecule intercalation

Engineering unconventional superconductors is a central challenge in condensed matter physics. Molecule-intercalated TaS2 superlattices have recently been reported to host such states, yet their origin remains debated, underscoring the urgent need for controlled, device-integrated studies. Here, we report that nanometer-thick TaS2 and NbSe2 intercalated with chiral and achiral organic cations instead exhibit robust monolayer-like Ising superconductivity, with no evidence of unconventional pairing. Using high-quality superlattices integrated into devices, we disentangle the roles of interlayer coupling and charge transfer in shaping their superconducting behavior. In TaS2, intercalation induces interlayer decoupling regardless of molecular size or symmetry, yielding monolayer-like Ising superconductivity. NbSe2 instead retains quasi-three-dimensional transport, with a gradual Ising enhancement and near-monolayer behavior only at the largest interlayer spacing. Transport remains reciprocal across all superlattices, consistent with preserved inversion symmetry and incompatible with parity-breaking superconductivity and noncentrosymmetric monolayers. We attribute the behavior to electronically detached monolayers with opposite spin-split bands, coupled through thermal and tunneling processes, which overall preserve inversion symmetry. These findings establish molecular intercalation compounds as a robust, device-ready, platform for engineering advanced superconducting superlattices.

cond-mat.supr-con

Galvanic intercalation of molecular cations into van der Waals materials

The intercalation of molecular species between the layers of van der Waals (vdW) crystals is a powerful approach to combine the remarkable physical properties of vdW materials with the chemical versatility of organic molecules. However, the full transformative potential of molecular intercalation remains underexplored, largely due to the lack of simple, broadly applicable methods that preserve high crystalline quality down to the few-layer limit. Here, we introduce a simple galvanic approach to intercalate different molecules into various vdW materials under ambient conditions, leveraging the low reduction potential of selected metals. We employ our method, which is particularly well-suited for the in-situ intercalation of few-layer-thick crystals, to intercalate nine vdW materials, including magnets and superconductors, with molecules ranging from conventional alkylammonium ions to metallorganic and bio-inspired chiral cations. Notably, intercalation leads to an unprecedented transition from antiferromagnetic to ferrimagnetic ordering in {\alpha}-RuCl3 and to a molecule-dependent enhancement of the superconducting transition in 2H-TaS2. These results establish our approach as a versatile technique for engineering atomically thin quantum materials and heterostructures, unlocking the transformative effects of molecular intercalation.

cond-mat.mtrl-sci

Supercurrent diode with high winding vortex

Nonreciprocal supercurrent refers to the phenomenon where the maximum dissipationless current in a superconductor depends on its direction of flow. This asymmetry underlies the operation of superconducting diodes and is often associated with the presence of vortices. Here, we investigate supercurrent nonreciprocal effects in a superconducting weak-link hosting distinct types of vortices. We demonstrate how the winding number of the vortex, its spatial configuration, and the shape of the superconducting lead can steer the sign and amplitude of the supercurrent rectification. We identify a general criterion for optimizing the rectification amplitude based on vortex patterns, focusing on configurations where the first harmonic of the supercurrent vanishes. We prove that supercurrent nonreciprocal effects can be used to diagnose high-winding vortex and to distinguish between different types of vorticity. Our results provide a toolkit for controlling supercurrent rectification through vortex phase textures and detecting unconventional vortex states.

cond-mat.supr-con

Back-action supercurrent diodes

Back-action refers to a response that retro-acts on a system to tailor its properties with respect to an external stimulus. This effect is at the heart of many electronic devices such as amplifiers, oscillators, and sensors. Here, we demonstrate that back-action can be exploited to achieve non-reciprocal transport in superconducting circuits. In our devices, dissipationless current flows in one direction whereas dissipative transport occurs in the opposite direction. Supercurrent diodes presented so far rely on magnetic elements or vortices to mediate charge transport or external magnetic fields to break time-reversal symmetry. Back-action solely turns a conventional reciprocal superconducting weak link with no asymmetry between the current bias directions into a rectifier, where the critical current amplitude depends on the bias sign. The self-interaction of the supercurrent stems from the gate tunability of the critical current in metallic and semiconducting systems, which promotes nearly ideal magnetic field-free rectification with selectable polarity.

cond-mat.mes-hall

Sign reversal diode effect in superconducting Dayem nanobridges

Supercurrent diodes are nonreciprocal electronic elements whose switching current depends on their flow direction. Recently, a variety of composite systems combining different materials and engineered asymmetric superconducting devices have been proposed. Yet, ease of fabrication and tunable sign of supercurrent rectification joined to large efficiency have not been assessed in a single platform so far. We demonstrate that all-metallic superconducting Dayem nanobridges naturally exhibit nonreciprocal supercurrents under an external magnetic field, with a rectification efficiency up to $\sim 27\%$. Our niobium nanostructures are tailored so that the diode polarity can be tuned by varying the amplitude of an out-of-plane magnetic field or the temperature in a regime without magnetic screening. We show that sign reversal of the diode effect may arise from the high-harmonic content of the current phase relation in combination with vortex phase windings present in the bridge or an anomalous phase shift compatible with anisotropic spin-orbit interactions.

cond-mat.supr-con

Radio-frequency manipulation of state populations in an entangled fluorine-muon-fluorine system

Entangled spin states are created by implanting muons into single crystal LiY0.95Ho0.05F4 to form a cluster of correlated, dipole-coupled local magnetic moments. The resulting states have well-defined energy levels allowing experimental manipulation of the state populations by electromagnetic excitation. Experimental control of the evolution of the muon spin polarization is demonstrated through application of continuous, radio-frequency magnetic excitation fields. A semiclassical model of quantum, dipole-coupled spins interacting with a classical, oscillating magnetic field accounts for the muon spin evolution. On application of the excitation field, this model shows how changes in the state populations lead to the experimentally observed effects, thus enabling a spectroscopic probe of entangled spin states with muons.

quant-ph