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Covadonga Álvarez-García

Publications and source records attributed to Covadonga Álvarez-García.

6 recordsLinked to original sources

Molecule-intercalated van der Waals Josephson junctions uncover complex multiband superconductivity

Intercalation of molecular species provides a route to tailor the electronic structure in van der Waals superconductors, yet intercalated compounds have rarely been integrated into phase-sensitive quantum devices. Here, we realize hybrid molecular Josephson junctions based on TaS2/NbSe2 heterostructures. Selective intercalation of the TaS2 electrode induces monolayer-like Ising superconductivity, while the junctions exhibit asymmetric Fraunhofer interference, field-induced and spontaneous Josephson diode effects. The zero-field diode disappears upon reversing the electrode stacking and re-emerges after intercalating the lower NbSe2 electrode. These findings indicate that the hybrid superconducting electrode hosts unconventional superconductivity underlying the nonreciprocal transport, while molecular intercalation acts as a tuning knob for its internal phase structure. This behavior is consistent with a time-reversal-symmetry-breaking multiband superconducting state characterized by a nontrivial relative phase between superconducting condensates. Our results establish hybrid molecular Josephson junctions as a quantum-device platform for phase-sensitive investigation and integration of molecularly engineered superconductors, opening opportunities to uncover and engineer unconventional superconducting phases.

cond-mat.supr-con↗

Efficient non-volatile electric control of magnetosensing in CrSBr

In two-dimensional crystals, electrostatic gating can modulate the charge carrier density, thereby tuning their electrical properties. In magnetic materials such as CrSBr, this approach can also enable direct electrical control of magnetoresistance. Non-volatile gating is particularly attractive since it allows the carrier density to be maintained at a desired level without the need for a continuous gate bias, offering significant advantages for technological applications. Here, we demonstrate a simple device architecture in which a solution-processed ferroelectric P(VDF-TrFE) layer is integrated directly onto a CrSBr channel, enabling non-volatile control of its magnetoresistance. We investigate the magnetotransport response over a broad temperature range and demonstrate a reproducible and robust gate dependence. Notably, the ferroelectric gate achieves a gating efficiency approximately one order of magnitude higher than that of a conventional SiO$_2$ dielectric, highlighting the potential of ferroelectric gating for electrical control of 2D magnetic materials.

cond-mat.mes-hall↗

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↗

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 α-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↗

Ferromagnetism above 200 K in organic-ion intercalated CrSBr

CrSBr is a van der Waals magnetic semiconductor exhibiting antiferromagnetic order below 140 K. It has emerged as a promising platform for engineering 2D magnetism because its intertwined electronic, optical, and magnetic properties can be profoundly modified via external stimuli such as electrical gating or magnetic fields. However, other strategies for tuning magnetism in layered materials, such as molecular intercalation, remain largely unexplored for CrSBr. Here, we demonstrate that the intercalation of tetramethylammonium (TMA) and tetrapropylammonium (TPA) ions into CrSBr induces a transition from antiferromagnetic to ferromagnetic order, while significantly enhancing the magnetic transition temperature to 190 K (TMA) and 230 K (TPA). The resulting intercalates are air-stable and exhibit large, hysteretic magnetoresistance exceeding 60% at 50 K in the TPA case. Besides, intercalation introduces symmetry-breaking structural changes in each CrSBr plane, revealed by Raman microscopy and corroborated by density functional theory (DFT) calculations. These findings highlight molecular intercalation as a powerful and versatile route to tailor the magnetic properties of CrSBr and unlock its potential to fabricate robust, high-temperature 2D magnetic devices.

cond-mat.mtrl-sci↗

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↗