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Two-dimensional van der Waals materials have become an established platform to engineer flat bands which can lead to strongly-correlated emergent phenomena. In particular, the family of Ta dichalcogenides in the 1T phase presents a star-of-David charge density wave that creates a flat band at the Fermi level. For TaS2and TaSe2this flat band is at half filling leading to a magnetic insulating phase. In this work, we theoretically demonstrate that ligand substitution in the TaSe2-xTexsystem produces a transition from the magnetic insulator to a non-magnetic metal in which the flat band gets doped away from half-filling. Forx∈[0.846,1.231]the spin-polarized flat band is self-doped and the system becomes a magnetic metal. In this regime, we show that attractive interactions promote three different spin-triplet superconducting phases as a function ofx, corresponding to a nodal f-wave and two topologically-different chiral p-wave superconducting phases. Our results establish monolayer TaSe2-xTexas a promising platform for correlated flat band physics leading to unconventional superconducting states.
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A valley filter capable of generating a valley-polarized current is a crucial element in valleytronics, yet its implementation remains challenging. Here, we propose a valley filter made of a graphene bilayer which exhibits a 1D moiré pattern in the overlapping region of the two layers controlled by heterostrain. In the presence of a lattice modulation between layers, electrons propagating in one layer can have valley-dependent dissipation due to valley asymmetric interlayer coupling, thus giving rise to a valley-polarized current. Such a process can be described by an effective non-Hermitian theory, in which the valley filter is driven by a valley-resolved non-Hermitian skin effect. Nearly 100% valley polarization can be achieved within a wide parameter range and the functionality of the valley filter is electrically tunable. The non-Hermitian topological scenario of the valley filter ensures high tolerance against imperfections such as disorder and edge defects. Our work opens a new route for efficient and robust valley filters while significantly relaxing the stringent implementation requirements.
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CeSiI has been recently isolated in the ultrathin limit, establishing CeSiI as the first intrinsic two-dimensional van der Waals heavy-fermion material up to 85 K. We show that, due to the strong spin-orbit coupling, the local moments develop a multipolar real-space magnetic texture, leading to local pseudospins with a nearly vanishing net moment. To elucidate its Kondo-screened regime, we extract from first-principles the parameters of the Kondo lattice model describing this material. We develop a pseudofermion methodology in combination with ab initio calculations to reveal the nature of the heavy-fermion state in CeSiI. We analyze the competing magnetic interactions leading to an unconventional heavy-fermion order as a function of the magnetic exchange between the localized f-electrons and the strength of the Kondo coupling. Our results show that the magnetic exchange interactions promote an unconventional momentum-dependent Kondo-screened phase, establishing the nature of the heavy-fermion state observed in CeSiI.
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Identifying phase boundaries of interacting systems is one of the key steps to understanding quantum many-body models. The development of various numerical and analytical methods has allowed exploring the phase diagrams of many Hermitian interacting systems. However, numerical challenges and scarcity of analytical solutions hinder obtaining phase boundaries in non-Hermitian many-body models. Recent machine learning methods have emerged as a potential strategy to learn phase boundaries from various observables without having access to the full many-body wavefunction. Here, we show that a machine learning methodology trained solely on Hermitian correlation functions allows identifying phase boundaries of non-Hermitian interacting models. These results demonstrate that Hermitian machine learning algorithms can be redeployed to non-Hermitian models without requiring further training to reveal non-Hermitian phase diagrams. Our findings establish transfer learning as a versatile strategy to leverage Hermitian physics to machine learning non-Hermitian phenomena.
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Progress in layered van der Waals materials has resulted in the discovery of ferromagnetic and ferroelectric materials down to the monolayer limit. Recently, evidence of the first purely 2D multiferroic material was reported in monolayer NiI2. However, probing multiferroicity with scattering-based and optical bulk techniques is challenging on 2D materials, and experiments on the atomic scale are needed to fully characterize the multiferroic order at the monolayer limit. Here, scanning tunneling microscopy (STM) supported by density functional theory (DFT) calculations is used to probe and characterize the multiferroic order in monolayer NiI2. It is demonstrated that the type-II multiferroic order displayed by NiI2, arising from the combination of a magnetic spin spiral order and a strong spin-orbit coupling, allows probing the multiferroic order in the STM experiments. Moreover, the magnetoelectric coupling of NiI2 is directly probed by external electric field manipulation of the multiferroic domains. The findings establish a novel point of view to analyze magnetoelectric effects at the microscopic level, paving the way toward engineering new multiferroic orders in van der Waals materials and their heterostructures.
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Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate the construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.
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Quantum magnets provide a powerful platform to explore complex quantum many-body phenomena. One example is triplon excitations, exotic many-body modes emerging from propagating singlet-triplet transitions. We engineer a minimal quantum magnet from organic molecules and demonstrate the emergence of dispersive triplon modes in one- and two-dimensional assemblies probed with scanning tunneling microscopy and spectroscopy. Our results provide the first demonstration of dispersive triplon excitations from a real-space measurement.
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Recent emergence of low-dimensional unconventional superconductors and their exotic interface properties calls for new approaches to probe the pairing symmetry, a fundamental and frequently elusive property of the superconducting condensate. Here, we introduce the unique capability of tunneling Andreev reflection (TAR) to probe unconventional pairing symmetry, utilizing the sensitivity of this technique to specific Andreev reflections. Specifically, suppression of the lowest-order Andreev reflection due to quantum interference but emergence of the higher-order Andreev processes provides direct evidence of the sign-changing order parameter in the paradigmatic FeSe superconductor. TAR spectroscopy also reveals two superconducting gaps, points to a possibility of a nodal gap structure, and directly confirms that superconductivity is locally suppressed along the nematic twin boundary, with preferential and near-complete suppression of the larger energy gap. Our findings therefore enable new, atomic-scale insight into microscopic, inhomogeneous, and interfacial properties of emerging quantum materials.
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Unconventional superconductors represent one of the fundamental directions in modern quantum materials research. In particular, nodal superconductors are known to appear naturally in strongly correlated systems, including cuprate superconductors and heavy-fermion systems. Van der Waals materials hosting superconducting states are well known, yet nodal monolayer van der Waals superconductors have remained elusive. Here, using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS) experiments, it is shown that pristine monolayer 1H-TaS2 realizes a nodal superconducting state. Non-magnetic disorder drives the nodal superconducting state to a conventional gapped s-wave state. Furthermore, many-body excitations emerge close to the gap edge, signalling a potential unconventional pairing mechanism. The results demonstrate the emergence of nodal superconductivity in a van der Waals monolayer, providing a building block for van der Waals heterostructures exploiting unconventional superconducting states.
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Scattering processes in quantum materials emerge as resonances in electronic transport, including confined modes, Andreev states, and Yu-Shiba-Rusinov states. However, in most instances, these resonances are driven by a single scattering mechanism. Here, we show the appearance of resonances due to the combination of two simultaneous scattering mechanisms, one from superconductivity and the other from graphene p-n junctions. These resonances stem from Andreev reflection and Klein tunneling that occur at two different interfaces of a hole-doped region of graphene formed at the boundary with superconducting graphene due to proximity effects from Bi_{2}Sr_{2}Ca_{1}Cu_{2}O_{8+δ}. The resonances persist with gating from p^{+}-p and p-n configurations. The suppression of the oscillation amplitude above the bias energy which is comparable to the induced superconducting gap indicates the contribution from Andreev reflection. Our experimental measurements are supported by quantum transport calculations in such interfaces, leading to analogous resonances. Our results put forward a hybrid scattering mechanism in graphene-high-temperature superconductor heterojunctions of potential impact for graphene-based Josephson junctions.
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Two-dimensional magnetic materials provide an ideal platform to explore collective many-body excitations associated with spin fluctuations. In particular, it should be feasible to explore, manipulate, and ultimately design magnonic excitations in two-dimensional van der Waals magnets in a controllable way. Here we demonstrate the emergence of moiré magnon excitations, stemming from the interplay of spin-excitations in monolayer CrBr3 and the moiré pattern arising from the lattice mismatch with the underlying substrate. The existence of moiré magnons is further confirmed via inelastic quasiparticle interference, showing the appearance of a dispersion pattern correlated with the moiré length scale. Our results provide a direct visualization in real-space of the dispersion of moiré magnons, demonstrating the versatility of moiré patterns in creating emergent many-body excitations.
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Spectral functions of non-Hermitian Hamiltonians can reveal the existence of topologically nontrivial line gaps and the associated topological edge modes. However, the computation of spectral functions in a non-Hermitian many-body system remains an open challenge. Here, we put forward a numerical approach to compute spectral functions of a non-Hermitian many-body Hamiltonian based on the kernel polynomial method and the matrix-product state formalism. We show that the local spectral functions computed with our algorithm reveal topological spin excitations in a non-Hermitian spin model, faithfully reflecting the nontrivial line gap topology in a many-body model. We further show that the algorithm works in the presence of the non-Hermitian skin effect. Our method offers an efficient way to compute local spectral functions in non-Hermitian many-body systems with tensor networks, allowing us to characterize line gap topology in non-Hermitian quantum many-body models.
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Ferroelectric van der Waals heterostructures provide a natural platform to design a variety of electrically controllable devices. In this work, we demonstrate that AB bilayer graphene encapsulated in MoTe2 acts as a valley valve that displays a switchable built-in topological gap, leading to ferroelectrically driven topological channels. Using a combination of ab initio calculations and low energy models, we show that the ferroelectric order of MoTe2 allows the control of the gap opening in bilayer graphene and leads to topological channels between different ferroelectric domains. Moreover, we analyze the effect that the moiré modulation between MoTe2 and graphene layers has in the topological modes, demonstrating that the edge states are robust against moiré modulations of the ferroelectrically-induced electric potential. Our results put forward ferroelectric/graphene heterostructures as versatile platforms to engineer switchable built-in topological channels without requiring an external electric bias.
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2D ferroelectric materials provide a promising platform for the electrical control of quantum states. In particular, due to their 2D nature, they are suitable for influencing the quantum states of deposited molecules via the proximity effect. Here, electrically controllable molecular states in phthalocyanine molecules adsorbed on monolayer ferroelectric material SnTe are reported. The strain and ferroelectric order in SnTe are found to create a transition between two distinct orbital orders in the adsorbed phthalocyanine molecules. By controlling the polarization of the ferroelectric domain using scanning tunneling microscopy (STM), it is successfully demonstrated that orbital order can be manipulated electrically. The results show how ferroelastic coupling in 2D systems allows for control of molecular states, providing a starting point for ferroelectrically switchable molecular orbital ordering and ultimately, electrical control of molecular magnetism.
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Magnetic frustrations in two-dimensional materials provide a rich playground to engineer unconventional phenomena. However, despite intense efforts, a realization of tunable frustrated magnetic order in two-dimensional materials remains an open challenge. Here we propose Coulomb engineering as a versatile strategy to tailor magnetic ground states in layered materials. Using the frustrated van der Waals monolayer 1T-TaS2as an example, we show how long-range Coulomb interactions renormalize the low energy nearly flat band structure, leading to a Heisenberg model which depends on the Coulomb interactions. Based on this, we show that superexchange couplings in the material can be precisely tailored by means of environmental dielectric screening, ultimately allowing to externally drive the material towards a tunable frustrated regime. Our results put forward Coulomb engineering as a powerful tool to manipulate magnetic properties of van der Waals materials.
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Direct detection of superconductivity has long been a key strength of point-contact Andreev reflection. However, its applicability to atomic-scale imaging is limited by the mechanical contact of the Andreev probe. To this end, we present a new method to probe Andreev reflection in a tunnel junction, leveraging tunneling spectroscopy and junction tunability to achieve quantitative detection of Andreev scattering. This method enables unambiguous assignment of superconducting origins of current-carrying excitations, as well as detection of higher order Andreev processes in atomic-scale junctions. We furthermore revealed distinct sensitivity of Andreev reflection to natural defects, such as step edges, even in classical superconductors. The methodology opens a new path to nano- and atomic-scale imaging of superconducting properties, including disordered superconductors and proximity to phase transitions.
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Transition metal dichalcogenides (TMDC) are a rich family of two-dimensional materials displaying a multitude of different quantum ground states. In particular, d3 TMDCs are paradigmatic materials hosting a variety of symmetry broken states, including charge density waves, superconductivity, and magnetism. Among this family, NbSe2 is one of the best-studied superconducting materials down to the monolayer limit. Despite its superconducting nature, a variety of results point toward strong electronic repulsions in NbSe2. Here, we control the strength of the interactions experimentally via quantum confinement and use low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS) to demonstrate that NbSe2 is in close proximity to a correlated insulating state. This reveals the coexistence of competing interactions in NbSe2, creating a transition from a superconducting to an insulating quantum correlated state by confinement-controlled interactions. Our results demonstrate the dramatic role of interactions in NbSe2, establishing NbSe2 as a correlated superconductor with competing interactions.
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The search for artificial topological superconductivity has been limited by the stringent conditions required for its emergence. As exemplified by the recent discoveries of various correlated electronic states in twisted van der Waals materials, moiré patterns can act as a powerful knob to create artificial electronic structures. Here, we demonstrate that a moiré pattern between a van der Waals superconductor and a monolayer ferromagnet creates a periodic potential modulation that enables the realization of a topological superconducting state that would not be accessible in the absence of the moiré. The magnetic moiré pattern gives rise to Yu-Shiba-Rusinov minibands and periodic modulation of the Majorana edge modes that we detect using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS). Moiré patterns and, more broadly, periodic potential modulations are powerful tools to overcome the conventional constraints for realizing and controlling topological superconductivity.
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Heavy-fermion systems represent one of the paradigmatic strongly correlated states of matter1-5. They have been used as a platform for investigating exotic behaviour ranging from quantum criticality and non-Fermi liquid behaviour to unconventional topological superconductivity4-12. The heavy-fermion phenomenon arises from the exchange interaction between localized magnetic moments and conduction electrons leading to Kondo lattice physics, and represents one of the long-standing open problems in quantum materials3. In a Kondo lattice, the exchange interaction gives rise to a band with heavy effective mass. This intriguing phenomenology has so far been realized only in compounds containing rare-earth elements with 4f or 5f electrons1,4,13,14. Here we realize a designer van der Waals heterostructure where artificial heavy fermions emerge from the Kondo coupling between a lattice of localized magnetic moments and itinerant electrons in a 1T/1H-TaS2 heterostructure. We study the heterostructure using scanning tunnelling microscopy and spectroscopy and show that depending on the stacking order of the monolayers, we can reveal either the localized magnetic moments and the associated Kondo effect, or the conduction electrons with a heavy-fermion hybridization gap. Our experiments realize an ultimately tunable platform for future experiments probing enhanced many-body correlations, dimensional tuning of quantum criticality and unconventional superconductivity in two-dimensional artificial heavy-fermion systems15-17.
RESUMEN
Moiré patterns in van der Waal materials can be used for designing magnetic structures.
