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Enrico Giannini

Publications and source records attributed to Enrico Giannini.

At least 19 recordsLinked to original sources

Quasi-one-dimensional topological band structure and van Hove singularities in monolayer TaIrTe$_4$ from laser $μ$-ARPES

Recent transport experiments reported a quantum spin Hall insulator phase in monolayer 1T-TaIrTe$_4$ gated away from charge neutrality. This phase is not predicted by band structure calculations and has been attributed to an electronic instability induced by strong correlations at a putative van Hove singularity. Here, we investigate the electronic structure of exfoliated monolayer 1T-TaIrTe$_4$ using micro-focus laser angle resolved photoemission. We find a strongly anisotropic band structure susceptible to density wave instabilities. Our data further reveal a saddle point singularity in the density of states. However, we find that the saddle point lies at a density for which transport experiments found no anomalies. Moreover, the quasiparticle line widths suggest weak electron correlations only. This points to a secondary role of van Hove singularities and electron correlations in the transport phase diagram of monolayer 1T-TaIrTe$_4$.

cond-mat.mtrl-sci

Resolving growth-induced off-stoichiometry in AgCrSe$_2$ single crystals

The layered delafossite-like antiferromagnet AgCrSe$_2$ is a superionic conductor at high temperatures and has been reported to exhibit anomalous Hall behavior and Kondo physics at low temperatures. These extraordinary transport properties have been established almost exclusively on single crystals grown by chemical vapor transport, raising questions about the role of growth-induced off-stoichiometry. Using elemental analysis, single-crystal X-ray diffraction, and magnetization measurements, we show that such crystals are indeed systematically off-stoichiometric, with a general composition of Ag$_{1-x}$Cr(Se$_{2-y}$Cl$_y$) ($x \approx y \approx 0.08$) arising from the use of CrCl$_3$ as a transport agent. This off-stoichiometry manifests in altered magnetic properties, most notably a suppressed Néel temperature of 46\,K compared to 58\,K in stoichiometric polycrystalline samples prepared by solid-state synthesis. By optimizing an Ag/Se self-flux growth method, we obtained large single crystals of AgCrSe$_2$ that recover the magnetic transition temperature and saturation field of stoichiometric powder samples. These results establish self-flux growth as a route to high-quality stoichiometric AgCrSe$_2$ single crystals and provide a reliable platform for reassessing whether the reported anomalous transport phenomena are intrinsic or arise from off-stoichiometry.

cond-mat.mtrl-sci

Growth of Large Crystals of Janus Phase RhSeCl Using Self-Selecting Vapour Growth

In recent years, interest in 2D Janus materials has grown exponentially, particularly with regard to their applications in spintronics and optoelectronic devices. The defining feature of Janus materials is the ordered arrangement of different layer terminations - creating chemically distinct surfaces and an inherent out-of-plane polarity. Among the few known Janus materials, RhSeCl is particularly intriguing as a rare example of an intrinsic Janus compound. Owing to its exceptional chemical stability, RhSeCl offers a promising platform for exploring the physics related to the Janus-structure. However, synthesising large, high-quality crystals of this compound remains a significant challenge. Here, we report a novel synthetic pathway for growing crystals up to 6 mm in lateral size via a two-step self-selecting vapour growth reaction. We further present a comprehensive comparison of newly developed synthesis routes with all previously reported methods for RhSeCl. During these investigations, we identified a previously unreported impurity that forms in specific growth pathways and demonstrate how it can be avoided to obtain phase-pure few- and monolayer flakes. We showcase the reproducibility of the process to obtain high-quality, large single-crystals and flakes.

cond-mat.mtrl-sci

Stoichiometry and Phase Control in K$_{1-x}$CrSe$_2$ via Self-Flux Synthesis

Layered delafossite-type magnetic materials, such as KCrSe$_2$, are promising platforms for studying magnetic systems and potential frustration on triangular lattices. Synthesis, structure-type control, and off-stoichiometries remain major challenges in the investigation of these delafossite-type magnets. Starting from the same self-flux composition (K:Cr:Se = 8:1:8), we isolated three distinct K$_{1-x}$CrSe$_2$ phases with $x$ = 0, 0.13--0.17, and 0.32--0.35, each adopting a different structure type depending on the quenching temperature applied. The phase evolution indicates a sequence of transformations during synthesis between compounds with varying degrees of potassium deficiency. Building on these insights into phase stability and crystal growth, we successfully grew single crystals of full-stoichiometric KCrSe$_2$ -- enabling direction-dependent magnetization measurements. These measurements reveal a pronounced field dependence of the Néel temperature at low external fields, as well as a weak metamagnetic transition. Our findings demonstrate that even a simple parameter -- such as quenching temperature -- can be used to control stoichiometry, direct phase formation, and ultimately tune the magnetic properties of delafossite-type materials.

cond-mat.mtrl-sci

Structural Modulation and Enhanced Magnetic Ordering in Incommensurate K$_{1-{x}}$CrSe$_2$ Crystals

Layered delafossite-type compounds and related transition metal dichalcogenides, characterized by their triangular net structures, serve as prototypical systems for exploring the intricate interplay between crystal structure and magnetic behavior. Herein, we report on the discovery of the compound K$_{1-x}$CrSe$_2$ ($x \approx$ 0.13), an incommensurately modulated phase. Single crystals of this compound were grown for the first time using a K/Se self-flux. We find a monoclinic crystal structure with incommensurate modulation, that can be rationalized by a 3+1 dimensional model. This modulation compensates for the under-stoichiometry of K cations, creating pronounced undulations in the CrSe$_2$ layers. Our anisotropic magnetization measurements reveal that K$_{1-x}$CrSe$_2$ undergoes a transition to a long-range magnetically ordered state below $T_{\mathrm N}$ = 133 K, a temperature 1.6 to 3.3 times higher than in earlier reported KCrSe$_2$ compounds. Our findings open new avenues for tuning the magnetic properties of these layered materials through structural modulation.

cond-mat.mtrl-sci

Doping Tunable CDW Phase Transition in Bulk 1T-ZrSe$_2$

Tuneable electronic properties in transition metal dichalcogenides (TMDs) are essential to further their use in device applications. Here, we present a comprehensive scanning tunnelling microscopy and spectroscopy study of a doping-induced charge density wave (CDW) in semiconducting bulk 1T-ZrSe$_2$. We find that atomic impurities which locally shift the Fermi level ($E_F$) into the conduction band trigger a CDW reconstruction concomitantly to the opening of a gap at $E_F$. Our findings shed new light on earlier photoemission spectroscopy and theoretical studies of bulk 1T-ZrSe$_2$, and provide a local understanding of the electron-doping mediated CDW transition observed in semiconducting TMDs.

cond-mat.str-el

Feedback loop dependent charge density wave imaging by scanning tunneling spectroscopy

Scanning Tunneling Spectroscopy (STS) is a unique technique to probe the local density of states (LDOS) at the atomic scale by measuring the tunneling conductance between a sharp tip and a sample surface. However, the technique suffers of well-known limitations, the so-called set-point effect, which can potentially introduce artifacts in the measurements. We compare several STS imaging schemes applied to the LDOS modulations of the charge density wave state on atomically flat surfaces, and demonstrate that only constant-height STS is capable of mapping the intrinsic LDOS. In the constant-current STS, commonly used and easier-to-implement, the tip-sample distance variations imposed by the feedback loop result in set-point-dependent STS images and possibly mislead the identification of the CDW gap edges.

cond-mat.mtrl-sci

Controlling the Magnetic Properties of the van der Waals Multiferroic Crystals Co$_{1-x}$Ni$_{x}$I$_2$

The structurally related compounds NiI$_2$ and CoI$_2$ are multiferroic van der Waals materials, in which helimagnetic orders exist simultaneously with electric polarization. Here, we report on the evolution of the crystal structure and of the magnetic properties across the solid solution Co$_{1-x}$Ni$_{x}$I$_2$. We have successfully grown crystals of the whole range of the solid solution, i.e. $x = 0-1$, by employing the self-selecting vapor growth (SSVG) technique and by carefully tuning the synthesis conditions according to the chemical composition. Our structural investigations show that the crystal symmetry changes from $P\bar{3}m1$ to $R\bar{3}m$ when Ni substitutes for Co beyond $x = 0.2$. Both the lattice parameters and magnetic properties evolve continuously and smoothly from one end member to the other, showing that they can be finely tuned by the chemical composition. We also observe that the Ni substitution degree in the solid solution affects the metamagnetic transition typical for CoI$_2$ at high magnetic fields. In particular, we find the existence of the metamagnetic transition similar to that for CoI$_2$ in the NiI$_2$ structure. Based on magnetic measurements we construct the phase diagram of the Co$_{1-x}$Ni$_{x}$I$_2$ system. Controlling the magnetic properties by the chemical composition may open new pathways for the fabrication of electronic devices made of two-dimensional (2D) flakes of multiferroic van der Waals materials.

cond-mat.mtrl-sci

Multiple antiferromagnetic phases and magnetic anisotropy in exfoliated CrBr$_3$ multilayers

In twisted two-dimensional (2D) magnets, the stacking dependence of the magnetic exchange interaction can lead to regions of ferromagnetic and antiferromagnetic interlayer order, separated by non-collinear, skyrmion-like spin textures. Recent experimental searches for these textures have focused on CrI$_3$, known to exhibit either ferromagnetic or antiferromagnetic interlayer order, depending on layer stacking. However, the very strong uniaxial anisotropy of CrI$_3$ disfavors smooth non-collinear phases in twisted bilayers. Here, we report the experimental observation of three distinct magnetic phases -- one ferromagnetic and two antiferromagnetic -- in exfoliated CrBr$_3$ multilayers, and reveal that the uniaxial anisotropy is significantly smaller than in CrI$_3$. These results are obtained by magnetoconductance measurements on CrBr$_3$ tunnel barriers and Raman spectroscopy, in conjunction with density functional theory calculations, which enable us to identify the stackings responsible for the different interlayer magnetic couplings. The detection of all locally stable magnetic states predicted to exist in CrBr$_3$ and the excellent agreement found between theory and experiments, provide complete information on the stacking-dependent interlayer exchange energy and establish twisted bilayer CrBr$_3$ as an ideal system to deterministically create non-collinear magnetic phases.

cond-mat.mtrl-sci

Unravelling the Nature of Spin Excitations Disentangled from Charge Contributions in a Doped Cuprate Superconductor

The nature of the spin excitations in superconducting cuprates is a key question toward a unified understanding of the cuprate physics from long-range antiferromagnetism to superconductivity. The intense spin excitations up to the over-doped regime revealed by resonant inelastic X-ray scattering bring new insights as well as questions like how to understand their persistence or their relation to the collective excitations in ordered magnets (magnons). Here, we study the evolution of the spin excitations upon hole-doping the superconducting cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ by disentangling the spin from the charge excitations in the experimental cross section. We compare our experimental results against density matrix renormalization group calculations for a $t$-$J$-like model on a square lattice. Our results unambiguously confirm the persistence of the spin excitations, which are closely connected to the persistence of short-range magnetic correlations up to high doping. This suggests that the spin excitations in hole-doped cuprates are related to magnons -- albeit short-ranged.

cond-mat.supr-con

Band Gap Opening in Bilayer Graphene-CrCl$_3$/CrBr$_3$/CrI$_3$ van der Waals Interfaces

We report experimental investigations of transport through bilayer graphene (BLG)/chromium trihalide (CrX$_3$; X=Cl, Br, I) van der Waals interfaces. In all cases, a large charge transfer from BLG to CrX$_3$ takes place (reaching densities in excess of $10^{13}$ cm$^{-2}$), and generates an electric field perpendicular to the interface that opens a band gap in BLG. We determine the gap from the activation energy of the conductivity and find excellent agreement with the latest theory accounting for the contribution of the $σ$ bands to the BLG dielectric susceptibility. We further show that for BLG/CrCl$_3$ and BLG/CrBr$_3$ the band gap can be extracted from the gate voltage dependence of the low-temperature conductivity, and use this finding to refine the gap dependence on the magnetic field. Our results allow a quantitative comparison of the electronic properties of BLG with theoretical predictions and indicate that electrons occupying the CrX$_3$ conduction band are correlated.

cond-mat.mes-hall

Probing magnetism in exfoliated VI$_3$ layers with magnetotransport

We perform magnetotransport experiments on VI$_3$ multilayers, to investigate the relation between ferromagnetism in bulk and in exfoliated layers. The magnetoconductance measured on field-effect transistors and tunnel barriers shows that the Curie temperature of exfoliated multilayers is $T_C$ = 57 K, larger than in bulk ($T_{\rm C,bulk}$ = 50 K). Below $T \approx$ 40 K, we observe an unusual evolution of the tunneling magnetoconductance, analogous to the phenomenology observed in bulk. Comparing the magnetoconductance measured for fields applied in- or out-of-plane corroborates the analogy, allows us to determine that the orientation of the easy-axis in multilayers is similar to that in bulk, and suggests that the in-plane component of the magnetization points in different directions in different layers. Besides establishing that the magnetic state of bulk and multilayers are similar, our experiments illustrate the complementarity of magnetotransport and magneto-optical measurements to probe magnetism in 2D materials.

cond-mat.mes-hall

Magnetization dependent tunneling conductance of ferromagnetic barriers

Recent experiments on van der Waals antiferrmagnets such as CrI3, CrCl3 and MnPS3 have shown that using atomically thin layers as tunnel barriers and measuring the temperature ($T$) and magnetic field ($H$) dependence of the conductance allows their magnetic phase diagram to be mapped. In contrast, barriers made of CrBr3 -- the sole van der Waals ferromagnet investigated in this way -- were found to exhibit small and featureless magnetoconductance, seemingly carrying little information about magnetism. Here we show that -- despite these early results -- the conductance of CrBr3 tunnel barriers does provide detailed information about the magnetic state of atomically thin CrBr3 crystals for $T$ both above and below the Curie temperature ($T_C = 32$ K). Our analysis establishes that the tunneling conductance depends on $H$ and $T$ exclusively through the magnetization $M(H,T)$, over the entire temperature range investigated (2-50 K). The phenomenon is reproduced in detail by the spin-dependent Fowler-Nordheim model for tunneling, and is a direct manifestation of the spin splitting of the CrBr3 conduction band. These findings demonstrate that the investigation of magnetism by tunneling conductance measurements is not limited to antiferromagnets, but can also be applied to ferromagnetic materials.

cond-mat.mtrl-sci

Multiband charge density wave exposed in a transition metal dichalcogenide

In the presence of multiple bands, well-known electronic instabilities may acquire new complexity. While multiband superconductivity is the subject of extensive studies, the possibility of multiband charge density waves (CDWs) has been largely ignored so far. Here, combining energy dependent scanning tunnelling microscopy (STM) topography with a simple model of the charge modulations and a self-consistent calculation of the CDW gap, we find evidence for a multiband CDW in 2H-NbSe$_2$. This CDW not only involves the opening of a gap on the inner band around the K-point, but also on the outer band. This leads to spatially out-of-phase charge modulations from electrons on these two bands, which we detect through a characteristic energy dependence of the CDW contrast in STM images.

cond-mat.str-el

Insight into the charge density wave gap from contrast inversion in topographic STM images

Charge density waves (CDWs) are understood in great details in one dimension, but they remain largely enigmatic in two dimensional systems. In particular, numerous aspects of the associated energy gap and the formation mechanism are not fully understood. Two long standing riddles are the amplitude and position of the CDW gap with respect to the Fermi level ($E_F$) and the frequent absence of CDW contrast inversion (CI) between opposite bias scanning tunneling microscopy (STM) images. Here, we find compelling evidence that these two issues are intimately related. Combining density functional theory and STM to analyse the CDW pattern and modulation amplitude in 1$T$-TiSe$_2$, we find that CI takes place at an unexpected negative sample bias because the CDW gap opens away from $E_F$, deep inside the valence band. This bias becomes increasingly negative as the CDW gap shifts to higher binding energy with electron doping. This study shows the importance of CI in STM images to identify periodic modulations with a CDW and to gain valuable insight into the CDW gap, whose measurement is notoriously controversial.

cond-mat.mes-hall

A hydrodynamical description for magneto-transport in the strange metal phase of Bi-2201

High temperature superconductors are strongly coupled systems which present a complicated phase diagram with many coexisting phases. This makes it difficult to understand the mechanism which generates their singular transport properties. Hydrodynamics, which mostly relies on the symmetries of the system without referring to any specific microscopic mechanism, constitutes a promising framework to analyze these materials. In this paper we show that in the strange metal phase of the cuprates, a whole set of transport coefficients are described by a universal hydrodynamic framework once one accounts for the effects of quantum critical charge density waves. We corroborate our theoretical prediction by measuring the DC transport properties of Bi-2201 close to optimal doping, proving the validity of our approach. Our argument can be used as a consistency check to understand the universality class governing the behavior of high temperature cuprate superconductors.

cond-mat.str-el

Multi-frequency Shubnikov-de Haas oscillations in topological semimetal Pt$_2$HgSe$_3$

Monolayer jacutingaite (Pt$_2$HgSe$_3$) has been recently identified as a candidate quantum spin Hall system with a 0.5 eV band gap, but no transport measurements have been performed so far on this material, neither in monolayer nor in the bulk. By using a dedicated high-pressure technique, we grow crystals enabling the exfoliation of 50-100 nm thick layers and the realization of devices for controlled transport experiments. Magnetoresistance measurements indicate that jacutingaite is a semimetal, exhibiting Shubnikov-de Haas (SdH) resistance oscillations with a multi-frequency spectrum. We adapt the Lifshitz-Kosevich formula to analyze quantitatively the SdH resistance oscillations in the presence of multiple frequencies, and find that the experimental observations are overall reproduced well by band structure ab-initio calculations for bulk jacutingaite. Together with the relatively high electron mobility extracted from the experiments ($\approx 2000$ cm$^2$/Vs, comparable to what is observed in WTe$_2$ crystals of the same thickness), our results indicate that monolayer jacutingaite should provide an excellent platform to investigate transport in 2D quantum spin Hall systems.

cond-mat.mes-hall

Synthetic Semimetals with van der Waals Interfaces

The assembly of suitably designed van der Waals (vdW) heterostructures represents a new approach to produce artificial systems with engineered electronic properties. Here, we apply this strategy to realize synthetic semimetals based on vdW interfaces formed by two different semiconductors. Guided by existing ab-initio calculations, we select WSe$_2$ and SnSe$_2$ mono and multilayers to assemble vdW interfaces, and demonstrate the occurrence of semimetallicity by means of different transport experiments. Semimetallicity manifests itself in a finite minimum conductance upon sweeping the gate over a large range in ionic liquid gated devices, which also offer spectroscopic capabilities enabling the quantitative determination of the band overlap. The semimetallic state is additionally revealed in Hall effect measurements by the coexistence of electrons and holes, observed by either looking at the evolution of the Hall slope with sweeping the gate voltage or with lowering temperature. Finally, semimetallicity results in the low-temperature metallic conductivity of interfaces of two materials that are themselves insulating. These results demonstrate the possibility to implement a state of matter that had not yet been realized in vdW interfaces, and represent a first step towards using these interfaces to engineer topological or excitonic insulating states.

cond-mat.mes-hall