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Marco Gobbi

Publications and source records attributed to Marco Gobbi.

At least 19 recordsLinked to original sources

Rate Programmable Ionic-Redox Switching with Tunable Volatility in CuCrP2S6

Metal thiophosphates are emerging as a multifunctional material platform for neuromorphic electronics due to their accessible polar phases and ion dynamics on biologically relevant timescales. While resistive switching in these materials is frequently attributed to ferroelectric or antiferroelectric polarization, the intrinsic role of ion dynamics remains underexplored. Here, we isolate and demonstrate purely ion-driven resistive switching in paraelectric CuCrP2S6. Robust and reproducible resistive switching is observed in the absence of measurable ferroelectricity. The conductance can be tuned through both voltage amplitude and sweep rate, revealing a rate dependence characteristic of ion dynamics. The resulting resistance states exhibit controllable volatility, where switching rate determines the decay time constant of the readout current, attributed to ionic relaxation. Using either inert or reactive electrodes, we observe electrical evidence of solid-state redox activity associated with the interfacial reduction of native Cu+ ions, enabling controlled formation of filamentary conduction pathways. Analysis of this process allows extraction of the Cu+ diffusion coefficient, providing quantitative insight into the underlying transport kinetics. The understanding of ionic-redox based resistive switching in CuCrP2S6 is crucial for unleashing its full potential as a material platform for dual- or multi-mode operation.

cond-mat.mtrl-sci

Ferroelectric hysteresis in singly aligned graphene-hBN moir\'e superlattices

Ferroelectric materials have the unique ability to maintain an electric polarization which can be reversed under an external applied electric field. This property makes them valuable for applications such as non-volatile random-access memories, transducers, actuators and electro optic modulators. Recently, emergent unconventional ferroelectricity has been demonstrated in moir\'e superlattices of bilayer graphene and hexagonal boron nitride (hBN) hosting non centrosymmetric stacking order. Whether this phenomenon is also present in noncentrosymmetric single layer graphene (SLG)-hBN moir\'e superlattices is still under debate. Here we demonstrate a ferroelectric response in an SLG-hBN moir\'e superlattice. Through Hall measurements, we pinpoint the origin of the hysteretic behavior to abnormal charge screening due to the moir\'e superlattice band and estimate the spontaneous polarization magnitude in the moir\'e superlattice structure. Temperature dependent measurements confirm that the hysteretic behavior persists from 2K up to room temperature, opening opportunities for high-mobility, ultrathin non-volatile devices

cond-mat.mes-hall

Surface lone-pair polarization probed by quantum-geometric transport in tellurium

Stereochemically active lone pairs are ubiquitous microscopic sources of polarity in molecules and solids, but their collective behavior in crystals is often hidden by symmetry or confined to surfaces. Here we show that quantum-geometry transport provides a sensitive probe of surface lone-pair polarization in trigonal tellurium. This surface polarization appears microscopically as an inversion-odd dipolar component of the crystal potential, which shifts the center of mass of Bloch wavepackets and produces quantum-geometric corrections to their velocity. We describe this lone-pair polar texture through a minimal three-component lattice model, and we show that the resulting linear and nonlinear transport coefficients probe, respectively, the second and first moments of the net polarization field. Because rectified voltages in tellurium flakes are directly proportional to the surface lone-pair polarization, our results provide a microscopic route to understanding and engineering polarization-driven, quantum-geometric electronic devices based on tellurium allotropes.

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

A new helical InSeI polymorph: crystal structure and polarized Raman spectroscopy study

Tetragonal InSeI is an interesting low-dimensional metal chalcohalide due to its composition and anisotropic crystal structure composed of helical chains, which give rise to optoelectronic properties with potential application in photodetectors, optical thermometers, and spintronic devices. However, experimental works lack on the study of its anisotropic or chiral behavior. Here we present the crystal structure of an unreported InSeI polymorph and study its lattice dynamics in bulk crystals and exfoliated nanowires by polarized Raman spectroscopy for two non-equivalent crystallographic planes. We determine the orientation of the helical chains and distinguish between crystallographic planes by linearly polarized measurements, evaluating the angle-dependent intensity of the modes, which allows assigning each mode to its representation. Circularly polarized Raman measurements do not reveal chiral phonons, despite the helical chains and anisotropic crystal structure. These results offer insight into the crystal structure of InSeI, which is fundamental for the fabrication of orientation-dependent optoelectronic and spintronic devices.

cond-mat.mtrl-sci

Anomalous Nonlinear Magnetoconductivity in van der Waals Magnet CrSBr

Nonlinear magnetoconductivity (NLMC) is a nonreciprocal transport response arising in non-centrosymmetric materials. However, this ordinary NLMC signal vanishes at zero magnetic field, limiting its potential for applications. Here, we report the observation of an anomalous NLMC controlled by internal order parameters such as the magnetization or N\'eel vectors. We achieve this response by breaking both inversion and time-reversal symmetry in artificial van der Waals heterostructures based on the magnetic CrSBr and insulating hBN. The nonreciprocal signal can be tuned between two different states in ferromagnetic monolayer CrSBr and among four different states in antiferromagnetic bilayer CrSBr, thanks to its metamagnetic transition. Remarkably, this output signal in the ferromagnetic (antiferromagnetic) state of CrSBr is three (one) orders of magnitude higher than those previously measured. A conductivity scaling analysis reveals the Berry connection polarizability as the origin of the anomalous NLMC. Our results pave the way for high-frequency rectifiers with magnetically switchable output polarity as well as for an efficient electrical readout of the magnetic state of antiferromagnetic materials.

cond-mat.mes-hall

Engineering magnetism in hybrid organic-inorganic metal halide perovskites

The chemical and structural flexibility of hybrid organic-inorganic metal halide perovskites (HOIPs) provides an ideal platform for engineering not only their well-studied optical properties, but also their magnetic ones. In this review we present HOIPs from a new perspective, turning the attention to their magnetic properties and their potential as new class of on-demand low-dimensional magnetic materials. Focusing on HOIPs containing transition metals, we comprehensively present the progress that has been made in preparing, understanding and exploring magnetic HOIPs. First, we briefly introduce HOIPs in terms of composition and crystal structure and examine the synthesis protocols commonly used to prepare those showing magnetic properties. Then, we present their rich magnetic behavior and phenomenology; discuss their origin and guidelines for tuning them by changing the perovskite phase, chemical composition and dimensionality; and showcase their potential application in magneto-optoelectronics and spintronics. Finally, we describe the current challenges in the field, such as their integration into devices, as well as the emerging possibilities of moving from magnetic doping to pure transition metal-based HOIPs, which will motivate further studies in the future.

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

Unveiling Photoluminescence Signatures of Magneto-Optical Coupling in Layered Hybrid Manganese Chloride Perovskites

Understanding the interplay between magnetic ordering and light emission is crucial for developing magneto-optical technologies. However, this phenomenon is poorly understood since observations of this coupling vary significantly across materials. In this context, hybrid organic-inorganic metal halide perovskites (HOIPs) that incorporate Mn2+ ions are a chemically and structurally tunable platform for exploring this phenomenon, since they exhibit magnetic ordering and photoluminescence (PL) emission. Here, we study two antiferromagnetic Mn-based HOIPs with different organic cations that result in distinct lattice stiffness, Mn2+-Mn2+ distance and octahedral distortion. Temperature-dependent PL excitation spectroscopy reveals changes in crystal field splitting energy and Racah parameters well above the N\'eel temperature (TN), indicating the emergence of Mn2+-Mn2+ magnetic interactions prior to reach long-range magnetic ordering. These variations align with the observed changes in temperature-PL evolution. The compound with a more rigid lattice shows stronger changes closer to TN, suggesting combined effects of magnetic polarons and spin-canting. In contrast, magnetic polaron-induced magnetic modifications prevail in the HOIP with a softer lattice. These results reveal the complexity of the magneto-optical coupling in Mn-based HOIPs and provide new insights into this field extensible to other 2D materials that exhibit this phenomenon with potential for advanced magneto-optical applications.

cond-mat.mtrl-sci

Gate-tunable charge-spin interconversion in graphene/heavy-metal heterostructures

Spintronics has emerged as a promising field for next-generation devices, offering functionalities beyond complementary metal-oxide-semiconductor (CMOS). A critical challenge in spintronics is to develop systems that can efficiently generate spin currents and enable their long-distance transport. Here, we demonstrate a graphene (Gr)/heavy metal (HM) heterostructure system that combines strong charge-spin interconversion efficiency, induced by the spin Hall effect, with a long spin diffusion length. By employing an industry-friendly magnetron sputtering technique, we deposit HM layers onto few-layer Gr while minimizing structural damage. The proximity effect from the HM enhances the spin Hall angle of Gr while limiting the reduction in its spin diffusion length. Additionally, the spin Hall angle can be tuned via an applied gate voltage, offering high controllability of the system. Importantly, these properties are observed across heterostructures composed of different HMs, indicating the generality of this approach. Our findings establish Gr/HM heterostructures as a scalable and versatile platform for spin current generation, paving the way for advanced spintronic devices with high efficiency, long spin propagation, and straightforward fabrication processes.

cond-mat.mes-hall

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

Tunable magnetism in 2D organic-ion-intercalated MnPS3 via molecule-dependent vacancy generation

The magnetic properties of van der Waals materials are profoundly influenced by structural defects. The layered antiferromagnet MnPS3 offers a unique opportunity to explore defect-related magnetism, as Mn2+ vacancies can be generated by the intercalation of specific guest molecules. However, the effectiveness of this process in atomically thin flakes and the extent of the magnetic tunability remain unclear. Here, we show that the magnetic properties of MnPS3 can be tailored through the intercalation of different guest molecules. Notably, the insertion of four alkylammonium ions introduces different populations of Mn2+ vacancies, leading to a transition from the pristine antiferromagnetic state to more complex magnetic textures, including a ferrimagnetic state displaying a magnetic saturation of 1 uB/atom. Moreover, we show that the intercalation of few-nm-thick flakes also leads to the emergence of a ferrimagnetic response. This in-flake intercalation, which can be monitored in real time using optical microscopy, can be interrupted before completion, generating lateral heterostructures between pristine and intercalated areas. This approach opens the way to the use of partial intercalation to define regions with distinct magnetic properties within a single flake.

cond-mat.mtrl-sci

Enhanced Superconductivity in 2H-TaS2 Devices Through in-situ Molecular Intercalation

The intercalation of guest species into the gap of van der Waals materials often leads to the emergence of intriguing phenomena, such as superconductivity. While intercalation-induced superconductivity has been reported in several bulk crystals, reaching a zero-resistance state in flakes remains challenging. Here, we show a simple method for enhancing the superconducting transition in tens-of-nm thick 2H-TaS2 crystals contacted by gold electrodes through in-situ intercalation. Our approach enables measuring the electrical characteristics of the same flake before and after intercalation, permitting us to precisely identify the effect of the guest species on the TaS2 transport properties. We find that the intercalation of amylamine molecules into TaS2 flakes causes a suppression of the charge density wave and an increase in the superconducting transition, with an onset temperature above 3 K. Additionally, we show that a fully developed zero-resistance state can be achieved in flakes by engineering the conditions of the chemical intercalation. Our findings pave the way for the integration of chemically tailored intercalation compounds in scalable quantum technologies.

cond-mat.supr-con

Detecting Lifshitz Transitions Using Nonlinear Conductivity in Bilayer Graphene

The second-order nonlinear electrical response (NLER) is an intrinsic property of inversion symmetry-broken systems which can provide deep insights into the electronic band structures of atomically thin quantum materials. However, the impact of Fermi surface reconstructions, also known as Lifshitz transitions, on the NLER has remained elusive. We investigated NLER in bilayer graphene (BLG), where the low-energy bands undergo Lifshitz transitions. Here, NLER undergoes a sign change near the Lifshitz transitions even at elevated temperatures $T\gtrsim10~$K. At the band edge, NLER in BLG is modulated by both extrinsic scattering and interfacial-strain-induced intrinsic Berry curvature dipole, both of which can be finely tuned externally by varying doping and interlayer potential. Away from the band edge, BLG exhibits second-order conductivity exceeding $30~\mu$mV$^{-1}\Omega^{-1}$ at 3K higher than any previous report. Our work establishes NLER as a reliable tool to probe Lifshitz transitions in quantum materials.

cond-mat.mes-hall

Second-Order Conductivity Probes a Cascade of Singularities in a Moir\'e Superlattice

Systems lacking inversion symmetry inherently demonstrate a nonlinear electrical response (NLER) to an applied electric bias, emerging through extrinsic mechanisms. This response is highly sensitive to the electronic band structure, which can be engineered with remarkable precision in moir\'e superlattices formed from atomically thin quantum materials. Moir\'e superlattices host complex Fermi surface reconstructions near van Hove singularities (vHSs) in the electronic density of states. However, the role of these reconstructions in shaping NLER remains insufficiently understood. In this work, we systematically explore NLER in moir\'e superlattices of twisted double bilayer graphene (tDBLG) by tuning the Fermi level across multiple moir\'e bands on both sides of the charge neutrality point. We observe sharp variations and sign reversals in the NLER appearing via extrinsic pathways near mid-band vHSs. The second-order conductivity close to the vHSs demonstrates a much higher value than previous reports of extrinsic NLER in any other material. Our results demonstrate that NLER can serve as a sensitive probe of Fermi surface reconstructions and establish tDBLG as a versatile and highly efficient platform for generating and controlling the nonlinear electrical response.

cond-mat.mes-hall

Orbital Hall conductivity and orbital diffusion length of Vanadium thin films by Hanle magnetoresistance

In spintronics, the spin Hall effect has been widely used to generate and detect spin currents in materials with strong spin-orbit coupling such as Pt and Ta. Recently, its orbital counterpart has drawn attention as a new tool to generate and detect orbital currents and thus investigate orbital transport parameters. In this study, we investigate vanadium (V), a $3d$ transition metal with weak spin-orbit coupling but with a theoretically large orbital Hall conductivity. We measure a large Hanle magnetoresistance in V thin films with a magnitude comparable to that of heavy metals and at least one order of magnitude higher than the spin Hall magnetoresistance observed in a Y$_3$Fe$_5$O$_{12}$/V bilayer, pointing to the orbital Hall origin of the effect. A fit of the magnetic-field dependence and thickness dependence of the Hanle magnetoresistance to the standard diffusion model allows us to quantify the orbital diffusion length (~2 nm) and the orbital Hall conductivity (~78 ($\hbar/2e$) $\Omega^{-1}$cm$^{-1}$) of V. The obtained orbital Hall conductivity is two orders of magnitude smaller than theoretical calculations of the intrinsic value, suggesting there is an important role of disorder.

cond-mat.mes-hall

Nonvolatile Electric Control of Antiferromagnet CrSBr

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway towards the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components which would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200 % change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

cond-mat.mes-hall

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