arXiv subjects

Francesco Calavalle

Publications and source records attributed to Francesco Calavalle.

13 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

Directional strong coupling at the nanoscale between hyperbolic polaritons and organic molecules

Strong coupling (SC) is a fundamental concept in physics that describes extreme interactions between light and matter. Recent experiments have demonstrated SC at the nanometer scale, where strongly confined polaritons, rather than photons, couple to quantum emitters or molecular vibrations. Coupling with the latter is generally referred to as vibrational SC (VSC) and is of significant fundamental and technological interest, as it can be an effective tool for modifying molecular properties. However, the implementation of VSC, especially at the nanoscale, depends on the development of tuning mechanisms that allow control over the coupling strength and, eventually, its directionality, opening the door for the selective coupling of specific molecular vibrations. Here we report the observation of directional VSC. Specifically, we show nanoscale images of propagating hyperbolic phonon polaritons (PhPs) coupled to pentacene molecules revealing that the fingerprint of VSC for propagating polaritons -- a marked anti-crossing in their dispersion at the vibrational resonance -- can be modulated as a function of the direction of propagation. In addition, we show that VSC can exhibit an optimal condition for thin molecular layers, characterized by a maximum coupling strength along one single direction. This phenomenon is understood by analysing the overlap of the polariton field with molecular layers of varying thicknesses. Apart from their fundamental importance, our findings promise novel applications for directional sensing or local directional control of chemical properties at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2025

Symmetry Origin and Microscopic Mechanism of Electrical Magnetochiral Anisotropy in Tellurium

Non-linear transport effects in response to external magnetic fields, i.e. electrical magnetochiral anisotropy (eMChA), have attracted much attention for their importance to study quantum and spin-related phenomena. Indeed, they have permitted the exploration of topological surface states and charge-to-spin conversion processes in low-symmetry systems. Nevertheless, despite the inherent correlation between the symmetry of the material under examination and its non-linear transport characteristics, there is a lack of experimental demonstration to delve into this relationship and to unveil their microscopic mechanisms. Here, we study eMChA in chiral elemental Tellurium (Te) along different crystallographic directions, establishing the connection between the different eMChA components and the crystal symmetry of Te. We observed different longitudinal eMChA components with collinear current and magnetic field, demonstrating experimentally the radial angular momentum texture of Te. We also measured a transverse non-linear resistance which, as the longitudinal counterpart, scales bilinearly with current and magnetic fields, illustrating that they are different manifestations of the same effect. Finally, we study the scaling law of the eMChA, evidencing that extrinsic scattering from dynamic sources is the dominant microscopic mechanism. These findings underscore the efficacy of symmetry-based investigations in understanding and predicting non-linear transport phenomena, with potential applications in spintronics and energy harvesting.

cond-mat.mes-hall↗

arXiv2024

A seamless graphene spin valve based on proximity to van der Waals magnet Cr$_2$Ge$_2$Te$_6$

Pristine graphene is potentially an ideal medium to transport spin information. Proximity effects, where a neighbouring material is used to alter the properties of a material in adjacent (or proximitized) regions, can also be used in graphene to generate and detect spins by acquiring spin-orbit coupling or magnetic exchange coupling. However, the development of seamless spintronic devices that are based uniquely on proximity effects remains challenging. Here, we report a two-dimensional graphene spin valve that is enabled by proximity to the van der Waals magnet Cr$_2$Ge$_2$Te$_6$. Spin precession measurements show that graphene acquires both spin-orbit coupling and magnetic exchange coupling when interfaced with the Cr$_2$Ge$_2$Te$_6$. This leads to spin generation by both electrical spin injection and the spin Hall effect, while retaining long-distance spin transport. The simultaneous presence of spin-orbit coupling and magnetic exchange coupling also leads to a sizeable anomalous Hall effect.

cond-mat.mes-hall↗

arXiv2024

Tailoring Photoluminescence by Strain-Engineering in Layered Perovskite Flakes

Strain is an effective strategy to modulate the optoelectronic properties of 2D materials, but it has been almost unexplored in layered hybrid organic-inorganic metal halide perovskites (HOIPs) due to their complex band structure and mechanical properties. Here, we investigate the temperature-dependent microphotoluminescence (PL) of 2D $(C_6H_5CH_2CH_2NH_3)_2Cs_3Pb_4Br_{13}$ HOIP subject to biaxial strain induced by a $SiO_2$ ring platform on which flakes are placed by viscoelastic stamping. At 80 K, we found that a strain of <1% can change the PL emission from a single peak (unstrained) to three well-resolved peaks. Supported by micro-Raman spectroscopy, we show that the thermomechanically generated strain modulates the bandgap due to changes in the octahedral tilting and lattice expansion. Mechanical simulations demonstrate the coexistence of tensile and compressive strain along the flake. The observed PL peaks add an interesting feature to the rich phenomenology of photoluminescence in 2D HOIPs, which can be exploited in tailored sensing and optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2023

Exchange bias in molecule/Fe3GeTe2 van der Waals heterostructures via spinterface effects

The exfoliation of layered magnetic materials generates atomically thin flakes characterized by an ultrahigh surface sensitivity, which makes their magnetic properties tunable via external stimuli, such as electrostatic gating and proximity effects. Another powerful approach to tailor magnetic materials is molecular functionalization, which leads to hybrid interface states with peculiar magnetic properties, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, we demonstrate the emergence of spinterface effects at the interface between flakes of the prototypical layered magnetic metal Fe3GeTe2 and thin films of paramagnetic Co-phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3GeTe2, indicating that the unpaired spins in Co-phthalocyanine develop antiferromagnetic ordering by proximity and pin the magnetization reversal of Fe3GeTe2. The effect is strongest for a Fe3GeTe2 thickness of 20 nm, for which the exchange bias field reaches -840 Oe and is measurable up to approximately 110 K. This value compares very favorably with previous exchange bias fields reported for Fe3GeTe2 in all-inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials.

cond-mat.mtrl-sci↗

arXiv2022

Gate-tuneable and chirality-dependent charge-to-spin conversion in Tellurium nanowires

Chiral materials are the ideal playground for exploring the relation between symmetry, relativistic effects, and electronic transport. For instance, chiral organic molecules have been intensively studied to electrically generate spin-polarized currents in the last decade, but their poor electronic conductivity limits their potential for applications. Conversely, chiral inorganic materials such as Tellurium are excellent electrical transport materials, but have not been explored to enable the electrical control of spin polarization in devices. Here, we demonstrate the all-electrical generation, manipulation, and detection of spin polarization in chiral single-crystalline Tellurium nanowires. By recording a large (up to 7%) and chirality-dependent unidirectional magnetoresistance, we show that the orientation of the electrically generated spin polarization is determined by the nanowire handedness and uniquely follows the current direction, while its magnitude can be manipulated by an electrostatic gate. Our results pave the way for the development of magnet-free chirality-based spintronic devices.

cond-mat.mes-hall↗

arXiv2021

Room-temperature operation of a molecular spin photovoltaic device on a transparent substrate

Incorporating multifunctionality along with the spin-related phenomenon in a single device is of great interest for the development of next generation spintronic devices. One of these challenges is to couple the photo-response of the device together with its magneto-response to exploit the multifunctional operation at room temperature. Here, the multifunctional operation of a single layer p-type molecular spin valve is presented, where the device shows a photovoltaic effect at the room temperature on a transparent glass substrate. The generated photovoltage is almost three times larger than the applied bias to the device which facilitates the modulation of the magnetic response of the device both with bias and light. It is observed that the photovoltage modulation with light and magnetic field is linear with the light intensity. The device shows an increase in power conversion efficiency under magnetic field, an ability to invert the current with magnetic field and under certain conditions it can act as a spin-photodetector with zero power consumption in the standby mode. The room temperature exploitation of the interplay among light, bias and magnetic field in the single device with a p-type molecule opens a way towards more complex and efficient operation of a complete spin-photovoltaic cell.

physics.app-ph↗

arXiv2021

Real-space observation of vibrational strong coupling between propagating phonon polaritons and organic molecules

Phonon polaritons (PPs) in van der Waals (vdW) materials can strongly enhance light-matter interactions at mid-infrared frequencies, owing to their extreme infrared field confinement and long lifetimes. PPs thus bear potential for achieving vibrational strong coupling (VSC) with molecules. Although the onset of VSC has recently been observed spectroscopically with PP nanoresonators, no experiments so far have resolved VSC in real space and with propagating modes in unstructured layers. Here, we demonstrate by real-space nanoimaging that VSC can be achieved between propagating PPs in thin vdW crystals (specifically h-BN) and molecular vibrations in adjacent thin molecular layers. To that end, we performed near-field polariton interferometry, showing that VSC leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict VSC for nanometer-thin molecular layers and PPs in few-layer vdW materials, which could make propagating PPs a promising platform for ultra-sensitive on-chip spectroscopy and strong coupling experiments.

physics.optics↗

arXiv2020

Tailoring Superconductivity in Large-Area Single-Layer NbSe2 via Self-Assembled Molecular Adlayers

Two-dimensional transition metal dichalcogenides (TMDs) represent an ideal testbench for the search of materials by design, because their optoelectronic properties can be manipulated through surface engineering and molecular functionalization. However, the impact of molecules on intrinsic physical properties of TMDs, such as superconductivity, remains largely unexplored. In this work, the critical temperature (TC) of large-area NbSe2 monolayers is manipulated, employing ultrathin molecular adlayers. Spectroscopic evidence indicates that aligned molecular dipoles within the self-assembled layers act as a fixed gate terminal, collectively generating a macroscopic electrostatic field on NbSe2. This results in an \sim 55\% increase and a 70\% decrease in TC depending on the electric field polarity, which is controlled via molecular selection. The reported functionalization, which improves the air stability of NbSe2, is efficient, practical, up-scalable, and suited to functionalize large-area TMDs. Our results indicate the potential of hybrid 2D materials as a novel platform for tunable superconductivity.

cond-mat.supr-con↗

arXiv2020

Strong interfacial exchange field in a heavy metal/ferromagnetic insulator system determined by spin Hall magnetoresistance

Spin-dependent transport at heavy metal/magnetic insulator interfaces is at the origin of many phenomena at the forefront of spintronics research. A proper quantification of the different interfacial spin conductances is crucial for many applications. Here, we report the first measurement of the spin Hall magnetoresistance (SMR) of Pt on a purely ferromagnetic insulator (EuS). We perform SMR measurements in a wide range of temperatures and fit the results by using a microscopic model. From this fitting procedure we obtain the temperature dependence of the spin conductances ($G_s$, $G_r$ and $G_i$), disentangling the contribution of field-like torque ($G_i$), damping-like torque ($G_r$), and spin-flip scattering ($G_s$). An interfacial exchange field of the order of 1 meV acting upon the conduction electrons of Pt can be estimated from $G_i$, which is at least three times larger than $G_r$ below the Curie temperature. Our work provides an easy method to quantify this interfacial spin-splitting field, which play a key role in emerging fields such as superconducting spintronics and caloritronics, and topological quantum computation.

cond-mat.mes-hall↗

arXiv2020

Tuning Ambipolarity in a Polymer Field Effect Transistor using Graphene electrodes

Polymer field-effect transistors with 2D graphene electrodes are devices that merge the best of two worlds: on the one hand, the low-cost and processability of organic materials and, on the other hand, the chemical robustness, extreme thinness and flexibility of graphene. Here, we demonstrate the tuning of the ambipolar nature of the semiconductor polymer N2200 from Polyera ActiveInk by incorporating graphene electrodes in a transistor geometry. Our devices show a balanced ambipolar behavior with high current ON-OFF ratio and charge carrier mobilities. These effects are caused by both the effective energy barrier modulation and by the weak electric field screening effect at the graphene-polymer interface. Our results provide a strategy to integrate 2D graphene electrodes in ambipolar transistors in order to improve and modulate their characteristics, paving the way for the design of novel organic electronic devices.

physics.app-ph↗

arXiv2020

Top Dielectric Induced Ambipolarity in an n-channel dual-gated Organic Field Effect Transistor

The realization of both p-type and n-type operations in a single organic field effect transistor (OFET) is critical for simplifying the design of complex organic circuits. Typically, only p-type or n-type operation is realized in an OFET, while the respective counterpart is either suppressed by charge trapping or limited by the injection barrier with the electrodes. Here we show that only the presence of a top dielectric turns an n-type polymer semiconductor (N2200, Polyera ActiveInk) into an ambipolar one, as detected from both bottom and top gated OFET operation. The effect is independent of the channel thickness and the top dielectric combinations. Variable temperature transfer characteristics show that both the electrons and holes can be equally transported through the bulk of the polymer semiconductor.

physics.app-ph↗