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Alessandra Lanzara

Publications and source records attributed to Alessandra Lanzara.

At least 19 recordsLinked to original sources

Layer-Controlled Intermolecular Coupling and Many-Body Effects in C$_{60}$ Films

Crystalline C$_{60}$ is a molecular solid whose electronic properties emerge from the interplay of intermolecular hopping, electron correlations, and electron-vibration coupling. Unlike moir$\rm\acute{e}$ van der Waals heterostructures, where interaction strength is commonly tuned by twist angle, molecular materials offer a complementary route in which layer number, molecular orientation, and substrate registry provide experimentally accessible control parameters. Here we present a systematic thickness-dependent angle-resolved photoemission study of C$_{60}$ films, spanning the monolayer to the bulk limit. The HOMO-derived band exhibits a non-monotonic evolution: the intermediate-thickness film shows larger bandwidth, reduced effective mass, and pronounced gap-like and sub-band features. The experimental trends, together with Holstein-model simulations, point to strengthened effective intermolecular electronic coupling and enhanced electron-phonon-induced spectral renormalization in the intermediate-thickness regime. These results identify a dimensional crossover in C$_{60}$ films and establish layer number as an effective knob for engineering electronic structure and many-body interactions in molecular thin films.

cond-mat.mtrl-sci

Electric field controlled spin transport in a topological insulator interfaced with a ferroelectric antiferromagnet

Topological insulators have been explored extensively for spin-charge interconversion via magnetic interfaces, yet the true response of their spin-charge conversion, particularly in the absence of an external magnetic field, remains to be studied. Here, we report electric-field control of spin-charge conversion in the topological insulator Bi$_2$Te$_3$ with the antiferromagnetic multiferroic BiFeO$_3$, employing a nonlocal spin transport device. A systematic thickness dependence of the spin transport across the interface between Bi$_2$Te$_3$ and BiFeO$_3$ reveals a signature of topological surface-state-dominated spin transport in the bilayer system. The spin-charge conversion remains robust for thicknesses above 10 nm but falls rapidly with reducing thickness and vanishes at 5 nm. This is consistent with the hybridization-induced emergence of a trivial insulating phase, which is supported by the coherency factor estimated from the magnetoconductance of Bi$_2$Te$_3$. These results establish that spin-momentum-locked surface states dominate interfacial spin transport in the decoupled regime. Beyond presenting efficient spin-charge interconversion at an entirely insulating magnetic interface, this work also highlights sputter-deposited Bi$_2$Te$_3$ as a high-quality and scalable platform for integrating quantum materials into devices. The nonlocal spin transport approach presented here provides a simple and direct evidence of spin-charge conversion and opens an efficient and practical pathway toward designing energy-efficient spin-based devices.

cond-mat.mes-hall

Spin-Valley Locking in 2H-TaS2 and Its Co-Intercalated Counterpart: Roles of Surface Domains and Co Intercalation

Tuning and probing spin-valley coupling is key to understanding correlated ground states in 2$\it{H}$-TaS$_2$. Its magnetically intercalated analogue, Co$_{1/3}$TaS$_2$, introduces additional degrees of freedom, including modified interlayer coupling and magnetism, to modulate spin-valley physics. Surface-sensitive probes like ARPES are essential for accessing surface spin texture, yet previous studies on 2$\it{H}$-TMDs have reported conflicting results regarding spin-polarized bands, leaving open whether these discrepancies are intrinsic or extrinsic. Here we performed spatially resolved spin-ARPES measurements on 2$\it{H}$-TaS$_2$ and Co$_{1/3}$TaS$_2$. Our results reveal robust spin-valley locking on both compounds. Importantly, Co intercalation enhances interlayer hybridization and introduces magnetism while preserving the TaS$_2$-derived spin texture. We further observe a spatial reversal of the out-of-plane spin polarization, which we attribute to different surface domains. This effect complicates quantifying spin textures and may underlie prior inconsistent observations. Our findings provide microscopic insight into how interlayer interactions and surface domains together govern spin-valley phenomena in layered TMDs.

cond-mat.mtrl-sci

Discovery of Van Hove Singularities: Electronic Fingerprints of 3Q Magnetic Order in a van der Waals Quantum Magnet

Magnetically intercalated transition metal dichalcogenides are emerging as a rich platform for exploring exotic quantum states in van der Waals magnets. Among them, CoxTaS2 has attracted intense interest following the recent discovery of a distinctive 3Q magnetic ground state and a pronounced topological Hall effect below a critical doping of x=1/3, both intimately tied to cobalt concentration. To date, direct signatures of this enigmatic 3Q magnetic order in the electronic structure remain elusive. Here we report a comprehensive doping dependent angle resolved photoemission spectroscopy study that unveils these long-sought fingerprints. Our data reveal an unexpected "inverse Mexican hat" dispersion along the K-M-K direction, accompanied by two van Hove singularities. These features are consistent with theoretical predictions for a 3Q magnetic order near three-quarters band filling on a cobalt triangular lattice. These results provide evidence of 3Q magnetic order in the electronic structure, establishing TMD van der Waals magnets as tunable materials to explore the interplay between magnetism and topology.

cond-mat.mtrl-sci

Ultrafast creation of a light induced semimetallic state in strongly excited 1T-TiSe$_2$

Screening, a ubiquitous phenomenon associated with the shielding of electric fields by surrounding charges, has been widely adopted as a means to modify a material's properties. While so far most studies have relied on static changes of screening through doping or gating, here we demonstrate that screening can also drive the onset of distinct quantum states on the ultrafast timescale. By using time and angle-resolved photoemission spectroscopy we show that intense optical excitation can drive 1T-TiSe$_2$, a prototypical charge density wave material, almost instantly from a gapped into a semimetallic state. By systematically comparing changes in bandstructure over time and excitation strength with theoretical calculations we find that the appearance of this state is likely caused by a dramatic reduction of the screening length. In summary, this work showcases how optical excitation enables the screening driven design of a non-equilibrium semimetallic phase in TiSe$_2$, possibly providing a general pathway into highly screened phases in other strongly correlated materials.

cond-mat.mes-hall

Doping Dependence of Spin-Momentum Locking in Bismuth-Based High-Temperature Cuprate Superconductors

Non-zero spin orbit coupling has been reported in several unconventional superconductors due to the absence of inversion symmetry breaking. This contrasts with cuprate superconductors, where such interaction has been neglected for a long time. The recent report of a non-trivial spin orbit coupling in overdoped Bi2212 cuprate superconductor, has re-opened an old debate on both the source and role of such interaction and its evolution throughout the superconducting dome. Using high-resolution spin- and angle-resolved photoemission spectroscopy, we reveal a momentum-dependent spin texture throughout the hole-doped side of the superconducting phase diagram for single- and double-layer bismuth-based cuprates. The universality of the reported effect among different dopings and the disappearance of spin polarization upon lead substitution, suggest a common source. We argue that local structural fluctuations of the CuO planes and the resulting charge imbalance may cause local inversion symmetry breaking and spin polarization, which might be crucial for understanding cuprates physics.

cond-mat.str-el

New three-dimensional dispersion in the type-II Dirac semimetals PtTe$_2$ and PdTe$_2$ revealed through Angle Resolved Photoemission Spectroscopy

PtTe$_2$ and PdTe$_2$ are among the first transition metal dichalcogenides that were predicted to host type-II Dirac fermions, exotic particles prohibited in free space. These materials are layered and air-stable, which makes them top candidates for technological applications that take advantage of their anisotropic magnetotransport properties. Here, we provide a detailed characterization of the electronic structure of PtTe$_2$ and PdTe$_2$ using Angle Resolved Photoemission Spectroscopy (ARPES) and Density Functional Theory (DFT) calculations, unveiling a new three-dimensional dispersion in these materials. Through the use of circularly polarized light, we report a different behavior of such dispersion in PdTe$_2$ compared to PtTe$_2$, that we relate to a symmetry analysis of the dipole matrix element. Such analysis reveals a link between the observed circular dichroism and the different momentum-dependent terms in the dispersion of these two compounds, despite their close similarity in crystal structure. Additionally, our data shows a clear difference in the circular dichroic signal for the type-II Dirac cones characteristic of these materials, compared to their topologically protected surface states. Our work provides a useful reference for the ARPES characterization of other transition metal dichalcogenides with topological properties and illustrates the use of circular dichroism as a guide to identify the topological character of two otherwise equivalent band dispersions, and to recognize different attributes in the band structure of similar materials.

cond-mat.mes-hall

Linearly dispersive bands at the onset of correlations in K$_x$C$_{60}$ films

Molecular crystals are a flexible platform to induce novel electronic phases. Due to the weak forces between molecules, intermolecular distances can be varied over relatively larger ranges than interatomic distances in atomic crystals. On the other hand, the hopping terms are generally small, which results in narrow bands, strong correlations and heavy electrons. Here, by growing K$_x$C$_{60}$ fullerides on hexagonal layered Bi$_2$Se$_3$, we show that upon doping the series undergoes a Mott transition from a molecular insulator to a correlated metal, and an in-gap state evolves into highly dispersive Dirac-like fermions at half filling, where superconductivity occurs. This picture challenges the commonly accepted description of the low energy quasiparticles as appearing from a gradual electron doping of the conduction states, and suggests an intriguing parallel with the more famous family of the cuprate superconductors. More in general, it indicates that molecular crystals offer a viable route to engineer electron-electron interactions.

cond-mat.mes-hall

Establishing Coherent Momentum-Space Electronic States in Locally Ordered Materials

In our understanding of solids, the formation of highly spatially coherent electronic states, fundamental to command the quantum behavior of materials, relies on the existence of discrete translational symmetry of the crystalline lattice. In contrast, in the absence of long-range order, as in the case of non-crystalline materials, the electronic states are localized and electronic coherence does not develop. This brings forward the fundamental question whether long range order is necessary condition to establish coherence and structured momentum-dependent electronic state, and how to characterize it in the presence of short-range order. Here we study Bi$_2$Se$_3$, a material that exists in its crystalline form with long range order, in amorphous form, with short and medium range order, and in its nanocrystalline form, with reduced short range order. By using angle resolved photoemission spectroscopy to directly access the electronic states in a momentum resolved manner, we reveal that, even in the absence of long-range order, a well-defined real-space length scale is sufficient to produce dispersive band structures. Moreover, we observe for the first time a repeated Fermi surface structure of duplicated annuli, reminiscent of Brillouin zone-like repetitions. These results, together with our simulations using amorphous Hamiltonians, reveal that the typical momentum scale where coherence occurs is the inverse average nearest-neighbor distance, the direct fingerprint of the local order of the underlying atomic structure. These results, not only lead the way to a new understanding of electronic coherence in solids, but also open the way to the realization of novel momentum-dependent quantum phenomena such as momentum pairing and spin-orbit coupling, in a much broader class of materials than the currently studied ones, lacking long range crystalline translational symmetry.

cond-mat.mtrl-sci

Observation of spin-momentum locked surface states in amorphous Bi$_{2}$Se$_{3}$

Crystalline symmetries have played a central role in the identification of topological materials. The use of symmetry indicators and band representations have enabled a classification scheme for crystalline topological materials, leading to large scale topological materials discovery. In this work we address whether amorphous topological materials, which lie beyond this classification due to the lack of long-range structural order, exist in the solid state. We study amorphous Bi$_2$Se$_3$ thin films, which show a metallic behavior and an increased bulk resistance. The observed low field magnetoresistance due to weak antilocalization demonstrates a significant number of two dimensional surface conduction channels. Our angle-resolved photoemission spectroscopy data is consistent with a dispersive two-dimensional surface state that crosses the bulk gap. Spin resolved photoemission spectroscopy shows this state has an anti-symmetric spin texture resembling that of the surface state of crystalline Bi$_2$Se$_3$. These experimental results are consistent with theoretical photoemission spectra obtained with an amorphous tight-binding model that utilizes a realistic amorphous structure. This discovery of amorphous materials with topological properties uncovers an overlooked subset of topological matter outside the current classification scheme, enabling a new route to discover materials that can enhance the development of scalable topological devices.

cond-mat.mtrl-sci

Electronic transport mechanisms in a thin crystal of the Kitaev candidate $α$-RuCl$_3$ probed through guarded high impedance measurements

$α$-RuCl$_3$ is considered to be the top candidate material for the experimental realization of the celebrated Kitaev model. It is however known that additional interactions beyond the Kitaev model trigger in $α$-RuCl$_3$, a long-range zigzag antiferromagnetic ground state. In this work, we investigate a nanoflake of $α$-RuCl$_3$ through guarded high impedance measurements aimed at reaching through electronic transport, the regime where the system turns into a zigzag antiferromagnet. We investigated a variety of temperatures (\SI{1.45}{\kelvin} - \SI{175}{\kelvin}) and out-of-plane magnetic fields ranging up to \SI{11}{\tesla}. We found a clear signature of a structural phase transition at $\approx 160$\,K as reported for thin crystals of $α$-RuCl$_3$, as well as a thermally activated behavior at temperatures above $\approx 30$\,K with a characteristic activation energy significantly smaller than the energy gap that we observe for $α$-RuCl$_3$ bulk crystals through our Angle Resolved Photoemission Spectroscopy (ARPES) experiments. Additionally we found that below $\approx 30$\,K, transport is ruled by Efros-Shklovskii (ES) VRH. These observations point to the presence of Coulomb impurities in our thin crystals. Most importantly, our data shows that below the magnetic ordering transition known for bulk $α$-RuCl$_3$ ($\approx 7$\,K), there is a clear deviation from VRH or thermal activation transport mechanisms. Our work demonstrates the possibility of reaching through specialized high impedance measurements, the thrilling ground states predicted for $α$-RuCl$_3$ at low temperatures in the frame of the Kitaev model, and informs about the transport mechanisms in this material in a wide temperature range as well as on important characteristic quantities such as the localization length of the impurities in a thin $α$-RuCl$_3$ crystal.

cond-mat.str-el

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric spin structures. The rare earth nickelate NdNiO3 is known to be a noncollinear antiferromagnet where the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here, we find that for low electron doping, the magnetic order on the nickel site is preserved while electronically a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by the bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of the rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.

cond-mat.str-el

Revealing the order parameter dynamics of 1T-TiSe$_2$ following optical excitation

The formation of a charge density wave state is characterized by an order parameter. The way it is established provides unique information on both the role that correlation plays in driving the charge density wave formation and the mechanism behind its formation. Here we use time and angle resolved photoelectron spectroscopy to optically perturb the charge-density phase in 1T-TiSe$_2$ and follow the recovery of its order parameter as a function of energy, momentum and excitation density. Our results reveal that two distinct orders contribute to the gap formation, a CDW order and pseudogap-like order, manifested by an overall robustness to optical excitation. A detailed analysis of the magnitude of the the gap as a function of excitation density and delay time reveals the excitonic long-range nature of the CDW gap and the short-range Jahn-Teller character of the pseudogap order. In contrast to the gap, the intensity of the folded Se$_{4p}$* band can only give access to the excitonic order. These results provide new information into the the long standing debate on the origin of the gap in TiSe$_2$ and place it in the same context of other quantum materials where a pseudogap phase appears to be a precursor of long-range order.

cond-mat.str-el

Polarization dependent photoemission as a probe of the magnetic ground state in the layered ferromagnet VI3

Layered ferromagnets are thrilling materials from both a fundamental and technological point of view. VI3 is an interesting example, with a complex magnetism that differentiates it from the first reported Cr based layered ferromagnets. Here, we show in an indirect way through Angle Resolved Photoemission Spectroscopy (ARPES) experiments, the importance of spin-orbit coupling setting the electronic properties of this material. Our light polarized photoemission measurements point to a ground state with a half-filled e'_+- doublet, where a gap opening is triggered by spin-orbit coupling enhanced by electronic correlations.

cond-mat.mes-hall

Exciton-Driven Renormalization of Quasiparticle Band Structure in Monolayer MoS2

Optical excitation serves as a powerful approach to control the electronic structure of layered Van der Waals materials via many-body screening effects, induced by photoexcited free carriers, or via light-driven coherence, such as optical Stark and Bloch-Siegert effects. Although theoretical work has also pointed to an exotic mechanism of renormalizing band structure via excitonic correlations in bound electron-hole pairs (excitons), experimental observation of such exciton-driven band renormalization and the full extent of their implications is still lacking, largely due to the limitations of optical probes and the impact of screening effects. Here, by using extreme-ultraviolet time-resolved angle-resolved photoemission spectroscopy together with excitonic many-body theoretical calculations, we directly unmask the band renormalization effects driven by excitonic correlations in a monolayer semiconductor. We revealed a surprising bandgap opening, increased by 40 meV, and a simultaneous enhancement of band effective mass. Our findings unmask the novel exciton-driven mechanism towards the band engineering in photoexcited semiconducting materials, opening a new playground to manipulate the transient energy states in layered quantum materials via optical controls of excitonic many-body correlations.

cond-mat.mtrl-sci

Mapping the dispersion of the occupied and unoccupied band structure in photoexcited 1T-TiSe$_2$

Charge density waves (CDW) are states of broken symmetry with a periodic modulation of charge and lattice typically leading to the opening of a gap in the band structure. In the model CDW system 1T-TiSe$_2$ such a gap opens up between its Se$_{4p}$ valence and Ti$_{3d}$ conduction band, accompanied by a change of dispersion. These changes are crucial in understanding the CDW phase, as they provide a measure of the Se$_{4p}$-Ti$_{3d}$ hybridization strength and characteristic mechanistic features. Using time- and angle-resolved photoelectron spectroscopy (trARPES), the unoccupied band structure is populated with near-infrared (NIR) pump pulses which allows to to directly visualize the parabolically-shaped Ti$_{3d}$ conduction band. Furthermore, we observe a transient change of effective mass in the Se$_{4p}$ valence band following photoexcitation. This occurs alongside an overall reduction due to weakening of the CDW phase and is accompanied by an oscillating component with the frequency of the characteristic A$_{1g}$ phonon. These observations, enabled by trAPRES, highlight the importance of the lattice contributions in establishing the CDW order in 1T-TiSe$_2$.

cond-mat.str-el

Observation of a flat and extended surface state in a topological semimetal

A topological flatband, also known as drumhead states, is an ideal platform to drive new exotic topological quantum phases. Using angle-resolved photoemission spectroscopy experiments, we reveal the emergence of a highly localized possible drumhead surface state in a topological semimetal BaAl4 and provide its full energy and momentum space topology. We find that the observed surface state is highly localized in momentum, inside a square-shaped bulk Dirac nodal loop, and in energy, leading to a flat band and a peak in the density of state. These results establish this class of materials as a possible experimental realization of drumhead surface states and provide an important reference for future studies of fundamental physics of topological quantum phase transition.

cond-mat.mes-hall

Correlation-Driven Electron-Hole Asymmetry in Graphene Field Effect Devices

Electron-hole asymmetry is a fundamental property in solids that can determine the nature of quantum phase transitions and the regime of operation for devices. The observation of electron-hole asymmetry in graphene and recently in the phase diagram of bilayer graphene has spurred interest into whether it stems from disorder or from fundamental interactions such as correlations. Here, we report an effective new way to access electron-hole asymmetry in 2D materials by directly measuring the quasiparticle self-energy in graphene/Boron Nitride field effect devices. As the chemical potential moves from the hole to the electron doped side, we see an increased strength of electronic correlations manifested by an increase in the band velocity and inverse quasiparticle lifetime. These results suggest that electronic correlations play an intrinsic role in driving electron hole asymmetry in graphene and provide a new insight for asymmetries in more strongly correlated materials.

cond-mat.mes-hall