showing 35 related works from this author
Strain Switching in van der Waals Heterostructures triggered by a Spin-Crossover Metal Organic Framework
2022
Van der Waals heterostructures (vdWHs) combine different layered materials with properties of interest,1 such as two-dimensional (2D) semimetals, semiconductors, magnets or superconductors. These heterostructures provide the possibility of engineering new materials with emergent functionalities that are not accessible in another way. Beyond inorganic 2D materials, layered molecular materials remain still rather unexplored, with only few examples regarding their isolation as atomically thin-layers. By a proper chemical design, the physical properties of these systems can be tuned, as illustrated by the so-called spin-crossover (SCO) compounds, in which a spin transition can be induced by app…
Switching the Magnetic Vortex Core in a Single Nanoparticle.
2016
Imaging and manipulating the spin structure of nano- and mesoscale magnetic systems is a challenging topic in magnetism, yielding a wide range of spin phenomena such as skyrmions, hedgehog-like spin structures, or vortices. A key example has been provided by the vortex spin texture, which can be addressed in four independent states of magnetization, enabling the development of multibit magnetic storage media. Most of the works devoted to the study of the magnetization reversal mechanisms of the magnetic vortices have been focused on micrometer-size magnetic platelets. Here we report the experimental observation of the vortex state formation and annihilation in individual 25 nm molecular-bas…
Pressure-Induced Collapse of the Charge Density Wave and Higgs Mode Visibility in 2H−TaS2
2019
The pressure evolution of the Raman active electronic excitations of the transition metal dichalcogenides $2H\text{\ensuremath{-}}{\mathrm{TaS}}_{2}$ is followed through the pressure phase diagram embedding incommensurate charge-density-wave and superconducting states. At high pressure, the charge-density wave is found to collapse at 8.5 GPa. In the coexisting charge-density-wave and superconducting orders, we unravel a strong in-gap superconducting mode, attributed to a Higgs mode, coexisting with the expected incoherent Cooper-pair breaking signature. The latter remains in the pure superconducting state reached above 8.5 GPa. Our report constitutes a new observation of such Raman active H…
Study of charge density waves in suspended 2H-TaS 2 and 2H-TaSe 2 by nanomechanical resonance
2021
The charge density wave (CDW) state in van der Waals systems shows interesting scaling phenomena as the number of layers can significantly affect the CDW transition temperature, $T_{CDW}$. However, it is often difficult to use conventional methods to study the phase transition in these systems due to their small size and sensitivity to degradation. Degradation is an important parameter which has been shown to greatly influence the superconductivity in layered systems. Since the CDW state competes with the onset of superconductivity, it is expected that $T_{CDW}$ will also be affected by the degradation. Here, we probe the CDW phase transition by the mechanical resonances of suspended 2H-TaS…
Enhanced superconductivity in atomically thin TaS2
2016
The ability to exfoliate layered materials down to the single layer limit has presented the opportunity to understand how a gradual reduction in dimensionality affects the properties of bulk materials. Here we use this top–down approach to address the problem of superconductivity in the two-dimensional limit. The transport properties of electronic devices based on 2H tantalum disulfide flakes of different thicknesses are presented. We observe that superconductivity persists down to the thinnest layer investigated (3.5 nm), and interestingly, we find a pronounced enhancement in the critical temperature from 0.5 to 2.2 K as the layers are thinned down. In addition, we propose a tight-binding …
Ultra-broad spectral photo-response in FePS3 air-stable devices
2021
Van der Waals materials with narrow energy gaps and efficient response over a broadband optical spectral range are key to widen the energy window of nanoscale optoelectronic devices. Here, we characterize FePS as an appealing narrow-gap p-type semiconductor with an efficient broadband photo-response, a high refractive index, and a remarkable resilience against air and light exposure. To enable fast prototyping, we provide a straightforward guideline to determine the thickness of few-layered FePS nanosheets extracted from the optical transmission characteristics of several flakes. The analysis of the electrical photo-response of FePS devices as a function of the excitation energy confirms a …
Publisher's Note: “Attosecond state-resolved carrier motion in quantum materials probed by soft x-ray XANES” [Appl. Phys Rev. 8, 011408 (2021)]
2021
Recent developments in attosecond technology led to table-top x-ray spectroscopy in the soft x-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real-time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, and TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near-edge spectroscopy to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the ele…
Probing the spin dimensionality in single-layer CrSBr van der Waals heterostructures by magneto-transport measurements
2022
Two-dimensional (2D) magnetic materials offer unprecedented opportunities for fundamental physics and applied research in spintronics and magnonics. Beyond the pioneering studies on 2D CrI3 and Cr2Ge2Te6, this emerging field has expanded to 2D antiferromagnets exhibiting different spin anisotropies and textures. Of particular interest is the layered metamagnet CrSBr, a relatively air-stable semiconductor formed by antiferromagnetically-coupled ferromagnetic layers (Tc~150 K) that can be exfoliated down to the single-layer. It presents a complex magnetic behavior with a dynamic magnetic crossover leading to a low-temperature hidden order below T*~40 K. Here, we inspect the magneto-transport …
Ultrafast Coherent THz Lattice Dynamics Coupled to Spins in the van der Waals Antiferromagnet FePS3
2022
Coherent THz optical lattice and hybridized phonon–magnon modes are triggered by femtosecond laser pulses in the antiferromagnetic van der Waals semiconductor FePS3. The laser-driven lattice and spin dynamics are investigated in a bulk crystal as well as in a 380 nm-thick exfoliated flake as a function of the excitation photon energy, sample temperature and applied magnetic field. The pump-probe magneto-optical measurements reveal that the amplitude of a coherent phonon mode oscillating at 3.2 THz decreases as the sample is heated up to the Néel temperature. This signal eventually vanishes as the phase transition to the paramagnetic phase occurs, thus revealing its connection to the long-ra…
Attosecond state-resolved carrier motion in quantum materials probed by soft x-ray XANES
2021
Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the …
Investigation of Charge-Transfer Interactions Induced by Encapsulating Fullerene in a Mesoporous Tetrathiafulvalene-Based Metal-Organic Framework
2019
<p>The design of Metal-Organic Frameworks (MOFs) incorporating electroactive guest molecules in the pores has become a subject of great interest in order to install additional electrical functionalities within the framework while maintaining porosity. In this direction, understanding the charge-transfer (CT) process between the framework and the guest molecules is crucial towards the design of new electroactive MOFs. Herein, we present the encapsulation of fullerenes (C<sub>60</sub>) in a mesoporous tetrathiafulvalene(TTF)-based MOF. The CT process between the electron-acceptor C<sub>60 </sub>guest and the electron-donor TTF ligand is studied in detail by means…
van der Waals heterostructures based on atomically-thin superconductors
2021
Van der Waals heterostructures (vdWHs) allow the assembly of high-crystalline two-dimensional (2D) materials in order to explore dimensionality effects in strongly correlated systems and the emergence of potential new physical scenarios. In this work, it is illustrated the feasibility to integrate 2D materials in-between 2D superconductors. Particularly, it is presented the fabrication and electrical characterization of vertical vdWHs based on air-unstable atomically-thin transition metal dichalcogenides formed by NbSe2/TaS2/NbSe2 stacks, with TaS2 being the insulator 1T-TaS2 or the metal 2H-TaS2. Phase transitions as 1T-TaS2 charge density wave and NbSe2 superconductivity are detected. An …
Chemical Design and Magnetic Ordering in Thin Layers of 2D Metal–Organic Frameworks (MOFs)
2021
Through rational chemical design, and thanks to the hybrid nature of metal−organic frameworks (MOFs), it is possible to prepare molecule-based 2D magnetic materials stable at ambient conditions. Here, we illustrate the versatility of this approach by changing both the metallic nodes and the ligands in a family of layered MOFs that allows the tuning of their magnetic properties. Specifically, the reaction of benzimidazole-type ligands with different metal centers (MII = Fe, Co, Mn, Zn) in a solventfree synthesis produces a family of crystalline materials, denoted as MUV-1(M), which order antiferromagnetically with critical temperatures that depend on M. Furthermore, the incorporation o…
Electronic, Structural and Functional Versatility in Tetrathiafulvalene-Lanthanide Metal-Organic Frameworks
2019
<div>Tetrathiafulvalene-Lanthanide (TTF-Ln) Metal-Organic Frameworks (MOFs) are an interesting class of multifunctional materials in which porosity can be combined with electronic properties such as electrical conductivity, redox activity, luminescence and magnetism. Herein we report a new family of isostructural TTF-Ln MOFs, denoted as <b>MUV-5(Ln)</b> (Ln = Gd, Tb, Dy, Ho, Er), exhibiting semiconducting properties as a consequence of the short intermolecular S···S contacts established along the chain direction between partially oxidised TTF moieties. In addition, this family shows photoluminescence properties and single-molecule magnetic behaviour, finding near-infrared …
Nanomechanical probing and strain tuning of the Curie temperature in suspended Cr2Ge2Te6-based heterostructures
2022
AbstractTwo-dimensional magnetic materials with strong magnetostriction are attractive systems for realizing strain-tuning of the magnetization in spintronic and nanomagnetic devices. This requires an understanding of the magneto-mechanical coupling in these materials. In this work, we suspend thin Cr2Ge2Te6 layers and their heterostructures, creating ferromagnetic nanomechanical membrane resonators. We probe their mechanical and magnetic properties as a function of temperature and strain by observing magneto-elastic signatures in the temperature-dependent resonance frequency near the Curie temperature, TC. We compensate for the negative thermal expansion coefficient of Cr2Ge2Te6 by fabrica…
Imaging the Magnetic Reversal of Isolated and Organized Molecular-Based Nanoparticles using Magnetic Force Microscopy
2015
In the race towards miniaturization in nanoelectronics, magnetic nanoparticles (MNPs) have emerged as potential candidates for their integration in ultrahigh-density recording media. Molecular-based materials open the possibility to design new tailor-made MNPs with variable composition and sizes, which benefit from the intrinsic properties of these materials. Before their implementation in real devices is reached, a precise organization on surfaces and a reliable characterization and manipulation of their individual magnetic behavior are required. In this paper, it is demonstrated how molecular-based MNPs are accurately organized on surfaces and how the magnetic properties of the individual…
Path to Overcome Material and Fundamental Obstacles in Spin Valves Based on MoS2 and Other Transition-Metal Dichalcogenides
2019
The recent introduction of two-dimensional materials into magnetic tunnel junctions (2D MTJs) offers very promising properties for spintronics, such as atomically defined interfaces, spin filtering, perpendicular anisotropy, and modulation of spin-orbit torque. Nevertheless, the difficulty of integrating exfoliated 2D materials into spintronic devices has limited exploration. Here the authors find a fabrication process leading to superior performance in MTJs based on transition-metal dichalcogenides, and further suggest a path to alleviate basic issues of technology and physics for 2D MTJs.
Proximity Effects on the Charge Density Wave Order and Superconductivity in Single-Layer NbSe2
2021
Collective electronic states such as the charge density wave (CDW) order and superconductivity (SC) respond sensitively to external perturbations. Such sensitivity is dramatically enhanced in two dimensions (2D), where 2D materials hosting such electronic states are largely exposed to the environment. In this regard, the ineludible presence of supporting substrates triggers various proximity effects on 2D materials that may ultimately compromise the stability and properties of the electronic ground state. In this work, we investigate the impact of proximity effects on the CDW and superconducting states in single-layer (SL) NbSe2 on four substrates of diverse nature, namely, bilayer graphene…
A fluorinated 2D magnetic coordination polymer
2021
Herein we show the versatility of coordination chemistry to design and expand a family of 2D materials by incorporating F groups at the surface of the layers. Through the use of a prefuntionalized organic linker with F groups, it is possible to achieve a layered magnetic material based on Fe(ii) centers that are chemically stable in open air, contrary to the known 2D inorganic magnetic materials. The high quality of the single crystals and their robustness allow to fabricate 2D molecular materials by micromechanical exfoliation, preserving the crystalline nature of these layers together with the desired functionalization.
Molecular stabilization of chemically exfoliated bare MnPS3 layers
2021
Transition metal chalcogenophosphates of general formula MPX3 have attracted recent interest in the field of 2D materials due to the possibility of tuning their properties when reaching the 2D limit. Several works address this challenge by dry mechanical exfoliation. However, only a few of them use a scalable approach. In this work, we apply a general chemical protocol to exfoliate MnPS3. The method uses in a first step chemical intercalation and liquid phase exfoliation, followed in a second step by the addition of molecules used as capping agents on the inorganic layers. Therefore, molecules of different nature prompts the quality of the exfoliated material and its stabilization in aqueou…
Simplified feedback control system for scanning tunneling microscopy
2021
A Scanning Tunneling Microscope (STM) is one of the most important scanning probe tools available to study and manipulate matter at the nanoscale. In a STM, a tip is scanned on top of a surface with a separation of a few \AA. Often, the tunneling current between tip and sample is maintained constant by modifying the distance between the tip apex and the surface through a feedback mechanism acting on a piezoelectric transducer. This produces very detailed images of the electronic properties of the surface. The feedback mechanism is nearly always made using a digital processing circuit separate from the user computer. Here we discuss another approach, using a computer and data acquisition thr…
Photoluminescence Enhancement by Band Alignment Engineering in MoS 2 /FePS 3 van der Waals Heterostructures
2022
Single-layer semiconducting transition metal dichalcogenides (2H-TMDs) display robust excitonic photoluminescence emission, which can be improved by controlled changes to the environment and the chemical potential of the material. However, a drastic emission quench has been generally observed when TMDs are stacked in van der Waals heterostructures, which often favor the nonradiative recombination of photocarriers. Herein, we achieve an enhancement of the photoluminescence of single-layer MoS2 on top of van der Waals FePS3. The optimal energy band alignment of this heterostructure preserves light emission of MoS2 against nonradiative interlayer recombination processes and favors the charge t…
Charge-transfer interactions between fullerenes and a mesoporous tetrathiafulvalene-based metal–organic framework
2019
The design of metal–organic frameworks (MOFs) incorporating electroactive guest molecules in the pores has become a subject of great interest in order to obtain additional electrical functionalities within the framework while maintaining porosity. Understanding the charge-transfer (CT) process between the framework and the guest molecules is a crucial step towards the design of new electroactive MOFs. Herein, we present the encapsulation of fullerenes (C60) in a mesoporous tetrathiafulvalene (TTF)-based MOF. The CT process between the electron-acceptor C60 guest and the electron-donor TTF ligand is studied in detail by means of different spectroscopic techniques and density functional theor…
Coherent coupling between vortex bound states and magnetic impurities in 2D layered superconductors
2021
Bound states in superconductors are expected to exhibit a spatially resolved electron-hole asymmetry which is the hallmark of their quantum nature. This asymmetry manifests as oscillations at the Fermi wavelength, which is usually tiny and thus washed out by thermal broadening or by scattering at defects. Here we demonstrate theoretically and confirm experimentally that, when coupled to magnetic impurities, bound states in a vortex core exhibit an emergent axial electron-hole asymmetry on a much longer scale, set by the coherence length. We study vortices in 2H-NbSe2 and in 2H-NbSe1.8S0.2 with magnetic impurities, characterizing these with detailed Hubbard-corrected density functional calcu…
Tunable Strong Coupling of Mechanical Resonance between Spatially Separated FePS3 Nanodrums
2021
Coupled nanomechanical resonators made of two-dimensional materials are promising for processing information with mechanical modes. However, the challenge for these types of systems is to control the coupling. Here, we demonstrate strong coupling of motion between two suspended membranes of the magnetic 2D material FePS$_3$. We describe a tunable electromechanical mechanism for control over both the resonance frequency and the coupling strength using a gate voltage electrode under each membrane. We show that the coupling can be utilized for transferring data from one drum to the other by amplitude modulation. Finally, we also study the temperature dependence of the coupling, and in particul…
Magnetic and electronic phase transitions probed by nanomechanical resonators
2020
The reduced dimensionality of two-dimensional (2D) materials results in characteristic types of magnetically and electronically ordered phases. However, only few methods are available to study this order, in particular in ultrathin insulating antiferromagnets that couple weakly to magnetic and electronic probes. Here, we demonstrate that phase transitions in thin membranes of 2D antiferromagnetic FePS3, MnPS3 and NiPS3 can be probed mechanically via the temperature-dependent resonance frequency and quality factor. The observed relation between mechanical motion and antiferromagnetic order is shown to be mediated by the specific heat and reveals a strong dependence of the Néel temperature of…
Raman Spectra of ZrS2 and ZrSe2 from Bulk to Atomically Thin Layers
2016
In the race towards two-dimensional electronic and optoelectronic devices, semiconducting transition metal dichalcogenides (TMDCs) from group VIB have been intensively studied in recent years due to the indirect to direct band-gap transition from bulk to the monolayer. However, new materials still need to be explored. For example, semiconducting TMDCs from group IVB have been predicted to have larger mobilities than their counterparts from group VIB in the monolayer limit. In this work we report the mechanical exfoliation of ZrX2 (X = S, Se) from bulk down to the monolayer and we study the dimensionality dependence of the Raman spectra in ambient conditions. We observe Raman signal from bul…
Quantum Phases and Spin Liquid Properties of 1T-TaS2
2021
Quantum materials exhibiting magnetic frustration are connected to diverse phenomena including high-Tc superconductivity, topological order and quantum spin liquids (QSLs). A QSL is a quantum phase (QP) related to a quantum-entangled fluid-like state of matter. Previous experiments on QSL candidate materials are usually interpreted in terms of a single QP, although theories indicate that many distinct QPs are closely competing in typical frustrated spin models. Here we report on combined temperature-dependent muon spin relaxation and specific heat measurements for the triangular-lattice QSL candidate material 1T-TaS2 that provide evidence for competing QPs. The measured properties are assig…
Low-Frequency Imaginary Impedance at the Superconducting Transition of 2H - NbSe2
2020
The superconducting transition leads to a sharp resistance drop in a temperature interval that can be a small fraction of the critical temperature ${T}_{c}$. A superconductor exactly at ${T}_{c}$ is thus very sensitive to all kinds of thermal perturbation, including the heat dissipated by the measurement current. We show that the interaction between electrical and thermal currents leads to a sizable imaginary impedance at frequencies of the order of tens of hertz at the resistive transition of single crystals of the layered material $2H$-${\mathrm{Nb}\mathrm{Se}}_{2}$. We explain the result using models developed for transition-edge sensors. By measuring under magnetic fields and at high cu…
Controlling the anisotropy of a van der Waals antiferromagnet with light
2020
Ultrafast optical control of magnetic anisotropy in a van der Waals antiferromagnet activates a sub-THz two-dimensional magnon.
A Local Study of the Transport Mechanisms in MoS2 Layers for Magnetic Tunnel Junctions
2018
MoS2-based vertical spintronic devices have attracted an increasing interest thanks to theoretical predictions of large magnetoresistance signals. However, experimental performances are still far from expectations. Here, we carry out the local electrical characterization of thin MoS2 flakes in a Co/Al2O3/MoS2 structure through conductive tip AFM measurements. We show that thin MoS2 presents a metallic behavior with a strong lateral transport contribution that hinders the direct tunnelling through thin layers. Indeed, no resistance dependence is observed with the flake thickness. These findings reveal a spin depolarization source in the MoS2-based spin valves, thus pointing to possible solut…
O-Doped Nanographenes: A Pyrano/Pyrylium Route Towards Semiconducting Cationic Mixed-Valence Complexes
2020
Herein we report an efficient synthesis to prepare O‐doped nanographenes, which derive from the longitudinally and latitudinally p‐extension of pyrene. The derivatives are highly fluorescent and feature low‐oxidation potentials. Exploiting electrooxidation, crystals of cationic mixed valence (MV) complexes were grown in which the organic salts organize into face‐to‐face p‐ p stacks, a favorable solid‐state arrangement for organic electronics. Variable‐temperature EPR measurements and relaxation studies suggest a strong electron delocalization along the longitudinal axis of the columnar p‐stacking architectures. Electric measurements of single crystals of the MV salts exhibited a semiconduct…
Graphene related magnetic materials: micromechanical exfoliation of 2D layered magnets based on bimetallic anilate complexes with inserted [FeIII(aca…
2015
The syntheses, structures and magnetic properties of the coordination compounds of formula [FeIII(acac2-trien)][MnIICrIII(Cl2 An)3]·(CH3CN)2 (1), [FeIII(acac2-trien)][MnIICrIII(Br2An)3]·(CH3CN)2 (2) and [GaIII(acac2-trien)][MnIICrIII(Br2An)3]·(CH3CN)2 (3) are reported. They exhibit a 2D anionic network formed by Mn(II) and Cr(III) ions linked through anilate ligands, while the [FeIII(acac2-trien)]+ or [GaIII(acac2-trien)]+ charge-compensating cations are placed inside the hexagonal channels of the 2D network, instead of being inserted in the interlamellar spacing. Thus, these crystals are formed by hybrid layers assembled through van der Waals interactions. The magnetic properties indicate …
Out-of-plane transport of 1T-TaS2/graphene-based van der Waals heterostructures
2021
Due to their anisotropy, layered materials are excellent candidates for studying the interplay between the in-plane and out-of-plane entanglement in strongly correlated systems. A relevant example is provided by 1T-TaS2, which exhibits a multifaceted electronic and magnetic scenario due to the existence of several charge density wave (CDW) configurations. It includes quantum hidden phases, superconductivity and exotic quantum spin liquid (QSL) states, which are highly dependent on the out-of-plane stacking of the CDW. In this system, the interlayer stacking of the CDW is crucial for the interpretation of the underlying electronic and magnetic phase diagram. Here, thin-layers of 1T-TaS2 are …
Attosecond soft-X-ray spectroscopy of a transition metal dichalcogenide material
2019
We use attosecond soft X-ray pulses between 284 eV to 543 eV for orbital-selective and real-time probing of the opto-electronic response of semi metallic TiS2.