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Abhay N. Pasupathy

Publications and source records attributed to Abhay N. Pasupathy.

At least 37 records · Page 2Linked to original sources
arXiv2024

Uniaxial plasmon polaritons $\textit{via}$ charge transfer at the graphene/CrSBr interface

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10$^{13}$ cm$^{-2}$ holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

cond-mat.mes-hall↗
arXiv2024

Low-Energy Electronic Structure in the Unconventional Charge-Ordered State of ScV$_6$Sn$_6$

Kagome vanadates {\it A}V$_3$Sb$_5$ display unusual low-temperature electronic properties including charge density waves (CDW), whose microscopic origin remains unsettled. Recently, CDW order has been discovered in a new material ScV$_6$Sn$_6$, providing an opportunity to explore whether the onset of CDW leads to unusual electronic properties. Here, we study this question using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The ARPES measurements show minimal changes to the electronic structure after the onset of CDW. However, STM quasiparticle interference (QPI) measurements show strong dispersing features related to the CDW ordering vectors. A plausible explanation is the presence of a strong momentum-dependent scattering potential peaked at the CDW wavevector, associated with the existence of competing CDW instabilities. Our STM results further indicate that the bands most affected by the CDW are near vHS, analogous to the case of {\it A}V$_3$Sb$_5$ despite very different CDW wavevectors.

cond-mat.str-el↗
arXiv2024

Superconductivity in twisted bilayer WSe$_2$

The discovery of superconductivity in twisted bilayer and twisted trilayer graphene has generated tremendous interest. The key feature of these systems is an interplay between interlayer coupling and a moiré superlattice that gives rise to low-energy flat bands with strong correlations. Flat bands can also be induced by moiré patterns in lattice-mismatched and or twisted heterostructures of other two-dimensional materials such as transition metal dichalcogenides (TMDs). Although a wide range of correlated phenomenon have indeed been observed in the moiré TMDs, robust demonstration of superconductivity has remained absent. Here we report superconductivity in 5 degree twisted bilayer WSe$_2$ (tWSe$_2$) with a maximum critical temperature of 426 mK. The superconducting state appears in a limited region of displacement field and density that is adjacent to a metallic state with Fermi surface reconstruction believed to arise from antiferromagnetic order. A sharp boundary is observed between the superconducting and magnetic phases at low temperature, reminiscent of spin-fluctuation mediated superconductivity. Our results establish that moiré flat-band superconductivity extends beyond graphene structures. Material properties that are absent in graphene but intrinsic among the TMDs such as a native band gap, large spin-orbit coupling, spin-valley locking, and magnetism offer the possibility to access a broader superconducting parameter space than graphene-only structures.

cond-mat.mes-hall↗
arXiv2024

Superconducting magic-angle twisted trilayer graphene hosts competing magnetic order and moiré inhomogeneities

The microscopic mechanism of superconductivity in the magic-angle twisted graphene family, including magic-angle twisted trilayer graphene (MATTG), is poorly understood. Properties of MATTG, like Pauli limit violation, suggest unconventional superconductivity. Theoretical studies propose proximal magnetic states in the phase diagram, but direct experimental evidence is lacking. We show direct evidence for an in-plane magnetic order proximal to the superconducting state using two complementary electrical transport measurements. First, we probe the superconducting phase by using statistically significant switching events from superconducting to the dissipative state of MATTG. The system behaves like a network of Josephson junctions due to lattice relaxation-induced moiré inhomogeneity in the system. We observe non-monotonic and hysteretic responses in the switching distributions as a function of temperature and in-plane magnetic field. Second, in normal regions doped slightly away from the superconducting regime, we observe hysteresis in magnetoresistance with an in-plane magnetic field; showing evidence for in-plane magnetic order that vanishes $\sim$900 mK. Additionally, we show a broadened Berezinskii-Kosterlitz-Thouless transition due to relaxation-induced moiré inhomogeneity. We find superfluid stiffness $J_{\mathrm{s}}$$\sim$0.15 K with strong temperature dependence. Theoretically, the magnetic and superconducting order arising from the magnetic order's fluctuations have been proposed - we show direct evidence for both. Our observation that the hysteretic magnetoresistance is sensitive to the in-plane field may constrain possible intervalley-coherent magnetic orders and the resulting superconductivity that arises from its fluctuations.

cond-mat.mes-hall↗
arXiv2024

Stoner instabilities and Ising excitonic states in twisted transition metal dichalcogenides

Moiré transition metal dichalcogenide (TMD) systems provide a tunable platform for studying electron-correlation driven quantum phases. Such phases have so far been found at rational fillings of the moiré superlattice, and it is believed that lattice commensurability plays a key role in their stability. In this work, we show via magnetotransport measurements on twisted WSe2 that new correlated electronic phases can exist away from commensurability. The first phase is an antiferromagnetic metal that is driven by proximity to the van Hove singularity. The second is a re-entrant magnetic field-driven insulator. This insulator is formed from a small and equal density of electrons and holes with opposite spin projections - an Ising excitonic insulator.

cond-mat.str-el↗
arXiv2023

Electronic structure, magnetic and transport properties of antiferromagnetic Weyl semimetal GdAlSi

We report the topological electronic structure, magnetic, and magnetotransport properties of a noncentrosymmetric compound GdAlSi. Magnetic susceptibility shows an antiferromagnetic transition at $T_\mathrm{N}$ = 32 K. In-plane isothermal magnetization exhibits an unusual hysteresis behavior at higher magnetic field, rather than near zero field. Moreover, the hysteresis behavior is asymmetric under positive and negative magnetic fields. First-principles calculations were performed on various magnetic configurations, revealing that the antiferromagnetic state is the ground state, and the spiral antiferromagnetic state is a close competing state. The calculations also reveal that GdAlSi hosts multiple Weyl points near the Fermi energy. The band structure measured by angle-resolved photoemission spectroscopy (ARPES) shows relatively good agreement with the theory, with the possibility of Weyl nodes slightly above the Fermi energy. Within the magnetic ordered state, we observe an exceptionally large anomalous Hall conductivity (AHC) of ~ 1310 $Ω^{-1}$cm$^{-1}$ at 2 K. Interestingly, the anomalous Hall effect persists up to room temperature with a significant value of AHC (~ 155 $Ω^{-1}$cm$^{-1}$). Our analysis indicates that the large AHC originates from the Berry curvature associated with the multiple pairs of Weyl points near Fermi energy.

cond-mat.str-el↗
arXiv2023

Highly tunable room-temperature plexcitons in monolayer WSe2 /gap-plasmon nanocavities

The advancement of quantum photonic technologies relies on the ability to precisely control the degrees of freedom of optically active states. Here, we realize real-time, room-temperature tunable strong plasmon-exciton coupling in 2D semiconductor monolayers enabled by a general approach that combines strain engineering plus force- and voltage-adjustable plasmonic nanocavities. We show that the exciton energy and nanocavity plasmon resonance can be controllably toggled in concert by applying pressure with a plasmonic nanoprobe, allowing in operando control of detuning and coupling strength, with observed Rabi splittings >100 meV. Leveraging correlated force spectroscopy, nano-photoluminescence (nano-PL) and nano-Raman measurements, augmented with electromagnetic simulations, we identify distinct polariton bands and dark polariton states, and map their evolution as a function of nanogap and strain tuning. Uniquely, the system allows for manipulation of coupling strength over a range of cavity parameters without dramatically altering the detuning. Further, we establish that the tunable strong coupling is robust under multiple pressing cycles and repeated experiments over multiple nanobubbles. Finally, we show that the nanogap size can be directly modulated via an applied DC voltage between the substrate and plasmonic tip, highlighting the inherent nature of the concept as a plexcitonic nano-electro-mechanical system (NEMS). Our work demonstrates the potential to precisely control and tailor plexciton states localized in monolayer (1L) transition metal dichalcogenides (TMDs), paving the way for on-chip polariton-based nanophotonic applications spanning quantum information processing to photochemistry.

physics.optics↗
arXiv2023

Tunable magnetic domains in ferrimagnetic MnSb$_2$Te$_4$

Highly tunable properties make Mn(Bi,Sb)$_2$Te$_4$ a rich playground for exploring the interplay between band topology and magnetism: On one end, MnBi$_2$Te$_4$ is an antiferromagnetic topological insulator, while the magnetic structure of MnSb$_2$Te$_4$ (MST) can be tuned between antiferromagnetic and ferrimagnetic. Motivated to control electronic properties through real-space magnetic textures, we use magnetic force microscopy (MFM) to image the domains of ferrimagnetic MST. We find that magnetic field tunes between stripe and bubble domain morphologies, raising the possibility of topological spin textures. Moreover, we combine in situ transport with domain manipulation and imaging to both write MST device properties and directly measure the scaling of the Hall response with domain area. This work demonstrates measurement of the local anomalous Hall response using MFM, and opens the door to reconfigurable domain-based devices in the M(B,S)T family.

cond-mat.str-el↗
arXiv2023

Interplay between local moment and itinerant magnetism in the layered metallic antiferromagnet TaFe$_{1.14}$Te$_3$

Two-dimensional (2D) antiferromagnets have garnered considerable interest for the next generation of functional spintronics. However, many available bulk materials from which 2D antiferromagnets are isolated are limited by their sensitivity to air, low ordering temperatures, and insulating transport properties. TaFe$_{1+y}$Te$_3$ offers unique opportunities to address these challenges with increased air stability, metallic transport properties, and robust antiferromagnetic order. Here, we synthesize TaFe$_{1+y}$Te$_3$ ($y$ = 0.14), identify its structural, magnetic, and electronic properties, and elucidate the relationships between them. Axial-dependent high-field magnetization measurements on TaFe$_{1.14}$Te$_3$ reveal saturation magnetic fields ranging between 27-30 T with a saturation magnetic moment of 2.05-2.12 $μ_B$. Magnetotransport measurements confirm TaFe$_{1.14}$Te$_3$ is metallic with strong coupling between magnetic order and electronic transport. Angle-resolved photoemission spectroscopy measurements across the magnetic transition uncover a complex interplay between itinerant electrons and local magnetic moments that drives the magnetic transition. We further demonstrate the ability to isolate few-layer sheets of TaFe$_{1.14}$Te$_3$ through mechanical exfoliation, establishing TaFe$_{1.14}$Te$_3$ as a potential platform for 2D spintronics based on metallic layered antiferromagnets.

cond-mat.mtrl-sci↗
arXiv2023

Smectic Pair Density Wave Order in EuRbFe4As4

The pair density wave (PDW) is a novel superconducting state in which Cooper pairs carry center-of-mass momentum in equilibrium, leading to the breaking of translational symmetry. Experimental evidence for such a state exists in high magnetic field and in some materials that feature density wave orders that explicitly break translational symmetry. However, evidence for a zero-field PDW state that exists independent of other spatially ordered states has so far been elusive. Here, we show that such a state exists in the iron pnictide superconductor EuRbFe4As4 (Eu-1144), a material that features coexisting superconductivity (Tc ~ 37K) and magnetism (Tm ~ 15 K). We show from the Spectroscopic Imaging Scanning Tunneling Microscopy (SI-STM) measurements that the superconducting gap at low temperature has long-range, unidirectional spatial modulations with an incommensurate period of ~8 unit cells. Upon raising the temperature above Tm, the modulated superconductor disappears, but a uniform superconducting gap survives to Tc. When an external magnetic field is applied, gap modulations disappear inside the vortex halo. The SI-STM and bulk measurements show the absence of other density wave orders, showing that the PDW state is a primary, zero-field superconducting state in this compound. Both four-fold rotational symmetry and translation symmetry are recovered above Tm, indicating that the PDW is a smectic order.

cond-mat.supr-con↗
arXiv2023

Spontaneous Exciton Dissociation in Transition Metal Dichalcogenide Monolayers

Since the seminal work on MoS2 monolayers, photoexcitation in atomically-thin transition metal dichalcogenides (TMDCs) has been assumed to result in excitons with large binding energies (~ 200-600 meV). Because the exciton binding energies are order-of-magnitude larger than thermal energy at room temperature, it is puzzling that photocurrent and photovoltage generation have been observed in TMDC-based devices, even in monolayers with applied electric fields far below the threshold for exciton dissociation. Here, we show that the photoexcitation of TMDC monolayers results in a substantial population of free charges. Performing ultrafast terahertz (THz) spectroscopy on large-area, single crystal WS2, WSe2, and MoSe2 monolayers, we find that ~10% of excitons spontaneously dissociate into charge carriers with lifetimes exceeding 0.2 ns. Scanning tunnelling microscopy reveals that photo-carrier generation is intimately related to mid-gap defect states, likely via trap-mediated Auger scattering. Only in state-of-the-art quality monolayers14, with mid-gap trap densities as low as 10^9 cm^-2, does intrinsic exciton physics start to dominate the THz response. Our findings reveal that excitons or excitonic complexes are only the predominant quasiparticles in photo-excited TMDC monolayers at the limit of sufficiently low defect densities.

cond-mat.mes-hall↗
arXiv2023

Coupled Ferroelectricity and Superconductivity in Bilayer $T_d$-MoTe$_2$

Achieving electrostatic control of quantum phases is at the frontier of condensed matter research. Recent investigations have revealed superconductivity tunable by electrostatic doping in twisted graphene heterostructures and in two-dimensional (2D) semimetals such as WTe$_2$. Some of these systems have a polar crystal structure that gives rise to ferroelectricity, in which the interlayer polarization exhibits bistability driven by external electric fields. Here we show that bilayer $T_d$-MoTe$_2$ simultaneously exhibits ferroelectric switching and superconductivity. Remarkably, a field-driven, first-order superconductor-to-normal transition is observed at its ferroelectric transition. Bilayer $T_d$-MoTe$_2$ also has a maximum in its superconducting transition temperature ($T_\textrm{c}$) as a function of carrier density and temperature, allowing independent control of the superconducting state as a function of both doping and polarization. We find that the maximum $T_\textrm{c}$ is concomitant with compensated electron and hole carrier densities and vanishes when one of the Fermi pockets disappears with doping. We argue that this unusual polarization-sensitive 2D superconductor is driven by an interband pairing interaction associated with nearly nested electron and hole Fermi pockets.

cond-mat.supr-con↗
arXiv2023

Machine Learning Microscopic Form of Nematic Order in twisted double-bilayer graphene

Modern scanning probe techniques, like scanning tunneling microscopy (STM), provide access to a large amount of data encoding the underlying physics of quantum matter. In this work, we analyze how convolutional neural networks (CNN) can be employed to learn effective theoretical models from STM data on correlated moiré superlattices. These engineered systems are particularly well suited for this task as their enhanced lattice constant provides unprecedented access to intra-unit-cell physics and their tunability allows for high-dimensional data sets within a single sample. Using electronic nematic order in twisted double-bilayer graphene (TDBG) as an example, we show that including correlations between the local density of states (LDOS) at different energies allows CNNs not only to learn the microscopic nematic order parameter, but also to distinguish it from heterostrain. These results demonstrate that neural networks constitute a powerful methodology for investigating the microscopic details of correlated phenomena in moiré systems and beyond.

cond-mat.str-el↗
arXiv2023

Electronic and magnetic properties of the topological semimetal SmMg$_2$Bi$_2$

Dirac semimetals show nontrivial physical properties and can host exotic quantum states like Weyl semimetals and topological insulators under suitable external conditions. Here, by combining angle-resolved photoemission spectroscopy measurements (ARPES) and first-principle calculations, we demonstrate that Zintl-phase compound SmMg$_2$Bi$_2$ belongs to the close proximity to a topological Dirac semimetallic state. ARPES results show a Dirac-like band crossing at the zone-center near the Fermi level ($E_\mathrm {F}$) which is further confirmed by first-principle calculations. Theoretical studies also reveal that SmMg$_2$Bi$_2$ belongs to a $Z_2$ topological class and hosts spin-polarized states around the $E_\mathrm {F}$. Zintl's theory predicts that the valence state of Sm in this material should be Sm$^{2+}$, however we detect many Sm-4$f$ multiplet states (flat-bands) whose energy positions suggest the presence of both Sm$^{2+}$ and Sm$^{3+}$. It is also evident that these flat-bands and other dispersive states are strongly hybridized when they cross each other. Due to the presence of Sm$^{3+}$ ions, the temperature dependence of magnetic susceptibility $χ(T)$ shows Curie-Weiss-like contribution in the low temperature region, in addition to the Van Vleck-like behaviour expected for the Sm$^{2+}$ ions. The present study will help in better understanding of the electronic structure, magnetism and transport properties of related materials.

cond-mat.str-el↗
arXiv2023

Unconventional Nonlocal Relaxation Dynamics in a Twisted Graphene Moire Superlattice

The electronic and structural properties of atomically thin materials can be controllably tuned by assembling them with an interlayer twist. During this process, constituent layers spontaneously rearrange themselves in search of a lowest energy configuration. Such relaxation phenomena can lead to unexpected and novel material properties. Here, we study twisted double trilayer graphene (TDTG) using nano-optical and tunneling spectroscopy tools. We reveal a surprising optical and electronic contrast, as well as a stacking energy imbalance emerging between the moiré domains. We attribute this contrast to an unconventional form of lattice relaxation in which an entire graphene layer spontaneously shifts position during fabrication. We analyze the energetics of this transition and demonstrate that it is the result of a non-local relaxation process, in which an energy gain in one domain of the moire lattice is paid for by a relaxation that occurs in the other.

cond-mat.mes-hall↗
arXiv2022

Strongly-overdoped La$_{2-x}$Sr$_x$CuO$_4$: Evidence for Josephson-coupled grains of strongly-correlated superconductor

The interpretation of how superconductivity disappears in cuprates at large hole doping has been controversial. To address this issue, we present an experimental study of single-crystal and thin film samples of La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) with $x\ge0.25$. In particular, measurements of bulk susceptibility on LSCO crystals with $x=0.25$ indicate an onset of diamagnetism at $T_{c1}=38.5$ K, with a sharp transition to a phase with full bulk shielding at $T_{c2}=18$ K, independent of field direction. Strikingly, the in-plane resistivity only goes to zero at $T_{c2}$. Inelastic neutron scattering on $x=0.25$ crystals confirms the presence of low-energy incommensurate magnetic excitations with reduced strength compared to lower doping levels. The ratio of the spin gap to $T_{c2}$ is anomalously large. Our results are consistent with a theoretical prediction for strongly overdoped cuprates by Spivak, Oreto, and Kivelson, in which superconductivity initially develops within disconnected self-organized grains characterized by a reduced hole concentration, with bulk superconductivity occurring only after superconductivity is induced by proximity effect in the surrounding medium of higher hole concentration. Beyond the superconducting-to-metal transition, local differential conductance measurements on an LSCO thin film suggest that regions with pairing correlations survive, but are too dilute to support superconducting order. Future experiments will be needed to test the degree to which these results apply to overdoped cuprates in general.

cond-mat.supr-con↗
arXiv2022

High-Throughput $\textit{Ab Initio}$ Design of Atomic Interfaces using InterMatch

Forming a hetero-interface is a materials-design strategy that can access an astronomically large phase space. However, the immense phase space necessitates a high-throughput approach for optimal interface design. Here we introduce a high-throughput computational framework, InterMatch, for efficiently predicting charge transfer, strain, and superlattice structure of an interface by leveraging the databases of individual bulk materials. Specifically, the algorithm reads in the lattice vectors, density of states, and the stiffness tensors for each material in their isolated form from the Materials Project. From these bulk properties, InterMatch estimates the interfacial properties. We benchmark InterMatch predictions for the charge transfer against experimental measurements and supercell density-functional theory calculations. We then use InterMatch to predict promising interface candidates for doping transition metal dichalcogenide MoSe$_2$. Finally, we explain experimental observation of factor of 10 variation in the supercell periodicity within a few microns in graphene/$α$-RuCl$_3$ by exploring low energy superlattice structures as a function of twist angle using InterMatch. We anticipate our open-source InterMatch algorithm accelerating and guiding ever-growing interfacial design efforts. Moreover, the interface database resulting from the InterMatch searches presented in this paper can be readily accessed through https://contribs.materialsproject.org/projects/intermatch/ .

cond-mat.mtrl-sci↗
arXiv2022

Ultra Localized Optoelectronic Properties of Nanobubbles in 2D Semiconductors

The optical properties of transition metal dichalcogenides have previously been modified at the nanoscale by using mechanical and electrical nanostructuring. However, a clear experimental picture relating the local electronic structure with emission properties in such structures has so far been lacking. Here, we use a combination of scanning tunneling microscopy (STM) and near-field photoluminescence (nano-PL) to probe the electronic and optical properties of single nano-bubbles in bilayer heterostructures of WSe2 on MoSe2. We show from tunneling spectroscopy that there are electronic states deeply localized in the gap at the edge of such bubbles, which are independent of the presence of chemical defects in the layers. We also show a significant change in the local bandgap on the bubble, with a continuous evolution to the edge of the bubble over a length scale of ~20 nm. Nano-PL measurements observe a continuous redshift of the interlayer exciton on entering the bubble, in agreement with the band to band transitions measured by STM. We use self-consistent Schrödinger-Poisson (SP) simulations to capture the essence of the experimental results and find that strong doping in the bubble region is a key ingredient to achieving the observed localized states, together with mechanical strain.

cond-mat.mes-hall↗