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Claudia Ojeda-Aristizabal

Publications and source records attributed to Claudia Ojeda-Aristizabal.

13 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↗

Lessons from $α$-RuCl3 for pursuing quantum spin liquid physics in atomically thin materials

Quantum spin liquids can arise from Kitaev magnetic interactions, and exhibit fractionalized excitations with the potential for a topological form of quantum computation. This review surveys recent experimental and theoretical progress on the pursuit of phenomena related to Kitaev magnetism in layered and exfoliatable materials, which offer numerous opportunities to apply powerful techniques from the field of atomically thin materials. We primarily focus on the antiferromagnetic Mott insulator $α$-RuCl3, which exhibits Kitaev couplings and is readily exfoliated to single- or few-layer sheets, and thus serves as a test bed for developing probes of Kitaev phenomena in atomically thin materials and devices. We introduce the Kitaev model and how it is realized in $α$-RuCl3 and other material candidates; and cover $α$-RuCl3 synthesis and fabrication into van der Waals heterostructure devices. A key discovery is a work-function-mediated charge transfer that heavily dopes both the $α$-RuCl3 and proximate materials, and can enhance Kitaev interactions by up to 50%. We further discuss a wide range of recent results in electronic transport and optical and tunneling spectroscopies of $α$-RuCl3 devices. The experimental techniques and theoretical insights developed for $α$-RuCl3 establish a framework for discovering and engineering superior two-dimensional Kitaev materials that may ultimately realize elusive quantum spin liquid phases.

cond-mat.str-el↗

Modification of the scattering mechanisms in bilayer graphene in proximity to a molecular thin film probed in the mesoscopic regime

Quantum coherent effects can be probed in multilayer graphene through electronic transport measurements at low temperatures. In particular, bilayer graphene is known to be susceptible to quantum interference corrections of the conductivity, presenting weak localization at all electronic densities, and dependent on different scattering mechanisms as well as on the trigonal warping of the electron dispersion near the K and K' valleys. Proximity effects with a molecular thin film influence these scattering mechanisms, which can be quantified through the known theory of magnetoconductance for bilayer graphene. Here, we present weak localization measurements in a copper-phthalocyanine / bilayer graphene / h-BN heterostructure that suggest an important suppression of trigonal warping effects in bilayer graphene (BLG), restoring the manifestation of the chirality of the charge carriers in the localization properties of BLG. Additionally, we observe a charge transfer of 3.6$\times$10$^{12}$cm$^{-2}$ from the BLG to the molecules, as well as a very small degradation of the mobility of the BLG/h-BN heterostructure upon the deposition of copper phthalocyanine (CuPc). The molecular arrangement of the CuPc thin film is characterized in a control sample through transmission electron microscopy, that we relate to the electronic transport results.

cond-mat.mes-hall↗

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↗

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↗

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↗

Signature of multilayer graphene strain-controlled domain walls in quantum Hall effect

Domain walls, topological defects that define the frontier between regions of different stacking in multilayer graphene, have proved to host exciting physics. The ability of tuning these topological defects in-situ in an electronic transport experiment brings a wealth of possibilities in terms of fundamental understanding of domain walls as well as for electronic applications. Here, we demonstrate through a MEMS (micro-electromechanical system) actuator and magnetoresistance measurements the effect of domain walls in multilayer graphene quantum Hall effect. Reversible and controlled uniaxial strain triggers these topological defects, manifested as new quantum Hall effect plateaus as well as a discrete and reversible modulation of the current across the device. Our findings are supported by theoretical calculations and constitute the first indication of the in-situ tuning of topological defects in multilayer graphene probed through electronic transport, opening the way to the use of reversible topological defects in electronic applications.

cond-mat.mes-hall↗

Competition between magnetic order and charge localization in Na$_2$IrO$_3$ thin crystal devices

Spin orbit assisted Mott insulators such as sodium iridate (Na$_2$IrO$_3$) have been an important subject of study in the recent years. In these materials, the interplay of electronic correlations, spin-orbit coupling, crystal field effects and a honeycomb arrangement of ions bring exciting ground states, predicted in the frame of the Kitaev model. The insulating character of Na$_2$IrO$_3$ has hampered its integration to an electronic device, desirable for applications, such as the manipulation of quasiparticles interesting for topological quantum computing. Here we show through electronic transport measurements supported by Angle Resolved Photoemission Spectroscopy (ARPES) experiments, that electronic transport in Na$_2$IrO$_3$ is ruled by variable range hopping and it is strongly dependent on the magnetic ordering transition known for bulk Na$_2$IrO$_3$, as well as on external electric fields. Electronic transport measurements allow us to deduce a value for the localization length and the density of states in our Na$_2$IrO$_3$ thin crystals devices, offering an alternative approach to study insulating layered materials.

cond-mat.mes-hall↗

Orbital character effects in the photon energy and polarization dependence of pure C60 photoemission

Recent direct experimental observation of multiple highly-dispersive C$_{60}$ valence bands has allowed for a detailed analysis of the unique photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C$_{60}$ molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C$_{60}$ band manifolds which allows for a more precise determination of the orbital character within the HOMO-2. Our observations and analysis provide important considerations for the connection between molecular and crystalline C$_{60}$ electronic structure, past and future band structure studies, and for increasingly popular C$_{60}$ electronic device applications, especially those making use of heterostructures.

cond-mat.mes-hall↗

Observation of highly dispersive bands in pure thin film C$_{60}$

While long-theorized, the direct observation of multiple highly dispersive C$_{60}$ valence bands has eluded researchers for more than two decades due to a variety of intrinsic and extrinsic factors. Here we report a realization of multiple highly dispersive (330-520 meV) valence bands in pure thin film C$_{60}$ on a novel substrate--the three-dimensional topological insulator Bi$_{2}$Se$_{3}$--through the use of angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. The effects of this novel substrate reducing C$_{60}$ rotational disorder are discussed. Our results provide important considerations for past and future band structure studies as well as the increasingly popular C$_{60}$ electronic device applications, especially those making use of heterostructures.

cond-mat.mes-hall↗

Why do Collapsed Carbon Nanotubes Twist?

We study the collapsing and subsequent spontaneous twisting of a carbon nanotube by in-situ transmission electron microscopy. A custom-sized nanotube is first created in the microscope by selectively extracting shells from a parent multi-wall tube. The few-wall, large-diameter daughter nanotube is driven to collapse via mechanical stimulation, after which the ribbon-like collapsed tube spontaneously twists along its long axis. In-situ diffraction experiments fully characterize the uncollapsed and collapsed tubes. From the experimental observations and associated theoretical analysis, the origin of the twisting is determined to be compressive strain due to charge imbalance.

cond-mat.mes-hall↗

Characterization of collective ground states in single-layer NbSe2

Layered transition metal dichalcogenides (TMDs) are ideal systems for exploring the effects of dimensionality on correlated electronic phases such as charge density wave (CDW) order and superconductivity. In bulk NbSe2 a CDW sets in at TCDW = 33 K and superconductivity sets in at Tc = 7.2 K. Below Tc these electronic states coexist but their microscopic formation mechanisms remain controversial. Here we present an electronic characterization study of a single 2D layer of NbSe2 by means of low temperature scanning tunneling microscopy/spectroscopy (STM/STS), angle-resolved photoemission spectroscopy (ARPES), and electrical transport measurements. We demonstrate that 3x3 CDW order in NbSe2 remains intact in 2D. Superconductivity also still remains in the 2D limit, but its onset temperature is depressed to 1.9 K. Our STS measurements at 5 K reveal a CDW gap of Δ = 4 meV at the Fermi energy, which is accessible via STS due to the removal of bands crossing the Fermi level for a single layer. Our observations are consistent with the simplified (compared to bulk) electronic structure of single-layer NbSe2, thus providing new insight into CDW formation and superconductivity in this model strongly-correlated system.

cond-mat.mes-hall↗