arXiv subjects

Abhay N. Pasupathy

Publications and source records attributed to Abhay N. Pasupathy.

At least 19 recordsLinked to original sources

arXiv2026

Engineering Vacuum Fluctuations in Hyperbolic Heterostructures

Vacuum fluctuations can be engineered using optical cavities, resonators, and surface-polaritonic modes, but extending such control deep inside a material remains challenging. Here we show that the vacuum field inside a hyperbolic material can be reshaped by a much thinner overlayer with opposite hyperbolicity. This effect requires overlap between the hyperbolic bands of the two materials and modifies the coupling between the vacuum field and matter excitations within the bottom material, without changing its intrinsic dielectric properties. As an application, we use Eliashberg theory to study a two-dimensional superconducting layer inside the bottom material, showing that the overlayer can remotely change its critical temperature. Our results may shed light on recent experiments reporting changes in superconductivity arising from a frequency-matched hyperbolic overlayer, and suggest an on-chip route to long-range control of matter excitations and collective material properties.

cond-mat.mes-hall↗

arXiv2026

Molecular spin qubits in a van der Waals bottle

Advancing quantum information technologies requires qubits whose coherence can be precisely engineered. Among the qubit platforms in development, molecular spin qubits (MSQs) stand out for their atomic scale tunability and chemical specificity, making them powerful candidates for sensing, simulation, and information processing. However, integrating MSQs into solid-state architectures without degrading their coherence remains a central challenge. Here, we introduce van der Waals (vdW) confinement within two-dimensional materials as a strategy for stabilizing quantum states in MSQs by engineering their local electronic, vibrational, and symmetry environments. Using cobaltocene as a model system, we show that confinement within vdW SnS2 and CdPS3 single crystals reorganizes the single-ion energy landscape and slows spin-lattice relaxation by over two orders of magnitude relative to unconfined cobaltocene. The confined MSQs adopt deterministic orientations and self-assemble into ordered, atomically precise superlattices, establishing vdW confinement as a pathway for integrating MSQs into functional quantum devices.

cond-mat.mtrl-sci↗

arXiv2026

Quantum Light Nano-Imaging

Entanglement and quantum correlations are central to the physics of quantum materials, yet they have remained notoriously difficult to access experimentally. Accessing these phenomena in solids requires quantum optical probes that operate at the native length and time scales of material excitations, below the diffraction limit of light. Developing the requisite tools has previously been infeasible due to the weak intensities of state-of-the-art quantum light sources and the inefficiency of light coupling in near-field light-matter interactions. In this work, we address these challenges and report the development of a quantum light scattering-type scanning near-field optical microscope (q-SNOM) that enables quantum-optical studies of solid-state systems with nanoscale spatial resolution. As a first demonstration, we visualize the self-interference of single hybrid light-matter polaritons in the prototypical van der Waals semiconductor MoS2. We also introduce a polaritonic time-of-flight metrology that exploits the temporal correlations among entangled photons to observe the quasiparticle propagation dynamics at femtosecond time scales. This work establishes a new experimental paradigm for exploring quantum effects in materials at the nanoscale.

cond-mat.mes-hall↗

arXiv2026

Advances in electrical contacts to single crystals of emerging materials for transport measurements

Transport measurements that probe electrical resistivity of a material under varying external stimuli, such as temperature, magnetic field, optical illumination, and gate voltage, are among the most important experimental techniques in condensed matter physics. These measurements provide critical insights into the fundamental electronic properties of materials. In recent years, they have facilitated the discovery and exploration of intriguing physical phenomena (e.g., superconductivity and quantum oscillations) and unique device functionalities (e.g., photoresponse and electrostatic gating effects) in various emerging materials, particularly in the form of single crystals. However, unlike large-scale wafers or thin films, newly synthesized single crystals often pose substantial challenges in establishing reliable electrical contacts due to their irregular geometries, limited dimensions, inherent structural characteristics, and potential susceptibility to degradation. In this review, we highlight recent technological advancements in the fabrication of high-quality, lithographically defined multi-terminal electrodes on both exfoliable and non-exfoliable single crystals for transport measurements. Our work provides a practical guide for researchers seeking to select appropriate contact-fabrication strategies tailored to unique characteristics of emerging crystals.

cond-mat.mtrl-sci↗

arXiv2026

Magnetic order, magnons, and crystal fields in van der Waals CeSiI

We report neutron, X-ray absorption, and resonant X-ray spectroscopy of magnetic excitations in the new heavy-fermion van-der-Waals superconductor CeSiI. We determined effective Hamiltonians and ground states of crystal electric fields and magnons. Isotropic Heisenberg interactions on a quasi two dimensional lattice, including ferromagnetic nearest-neighbor exchange as the dominant interaction, provide an excellent account to the low-energy measured dynamics and stabilize a co-rotating spin cycloid. Our study provides the basis to model CeSiI from first principles, thereby laying the ground for microscopic understanding of heavy-fermion physics, their unconventional superconductivity, and quantum criticality.

cond-mat.str-el↗

arXiv2026

Programmable, Spontaneous Superlattice Memory in a Monolayer Topological Insulator

Memory is a foundational concept across disciplines, from neurobiology and electronics to artificial intelligence and quantum gravity. In materials, memory effects typically arise from ferroic orders, such as ferroelectricity and ferromagnetism, where information is stored in charge or spin degrees of freedom. Here, we report a surprising discovery of a nonvolatile superlattice memory effect in monolayer TaIrTe4, a dual quantum spin Hall insulator, where information is encoded through sharply contrasting lattice periodicities. In particular, in a pristine monolayer, we observe the spontaneous emergence of a long-period superlattice that can be programmed ON and OFF in a nonvolatile manner by electrostatic tuning of low-energy electronic states. This switching toggles the system between two structural configurations with unit cell areas differing by nearly two orders of magnitude. Mechanistically, our results reveal two independent and distinct instabilities, one in the lattice and the other in the QSH electrons, which are coupled, leading to electrostatic control of lattice configurations with nonvolatile memory. This finding is enabled by combining linear and nonlinear transport measurements, Raman spectroscopy, and scanning tunneling microscopy, which probe complementary aspects of the underlying orders. Remarkably, this nonvolatile memory effect stabilizes a spontaneous superlattice with a periodicity on the few-nanometer scale that remains robust across a wide doping range, persists over days, and survives above 70 K. Combined with the QSH topology, this stability offers a promising route to nonvolatile memory control of topological flat bands and their filling enabled quantum states. Our preliminary data indeed show the emergence of new insulating states at fractional superlattice fillings, which can be clearly switched ON and OFF together with the superlattice.

cond-mat.mes-hall↗

arXiv2026

Design and fabrication of guiding patterns for topography-based searching of 2D devices for scanning tunneling microscopy measurements

We report the design and fabrication of guiding patterns for topography-based searching of two-dimensional (2D) devices for scanning tunneling microscopy (STM) measurements. Sub-micron geometric coordinate markers were etched into SiO2/Si wafers, serving as both substrates for 2D device integration and guiding maps for sample navigation. Here, we used a monolayer graphene/h-BN device with an active area of smaller than 20 um x 20 um as a model system and demonstrated that the device could be reliably located in STM solely through topographic imaging of the guiding patterns and in situ stage calibration, without reliance on optical viewports or capacitive sensing. Atomically resolved topographic imaging and tunneling spectroscopy were also obtained. Our proposed navigation strategy is fully compatible with standard device fabrication procedures and requires no hardware modification to existing STM setups. As such, it offers a practical alternative for locating miniaturized devices in STM, shedding light on studying emerging quantum phenomena in 2D systems.

cond-mat.str-el↗

arXiv2025

Mapping the moiré potential in multi-layer rhombohedral graphene

Rhombohedral graphene (rG) aligned with hexagonal boron nitride (hBN) has been shown to host flat bands that stabilize various strongly correlated quantum phases, including Mott insulators, integer, and fractional quantum anomalous Hall phases. In this work, we use scanning tunneling microscopy/spectroscopy (STM/STS) to visualize the dispersion of flat bands with doping and applied displacement fields in a hBN-aligned rhombohedral trilayer graphene (rtG)/hBN moiré superlattice. In addition to the intrinsic flat bands of rtG induced by the displacement field, we observe low-energy features originating from moiré potential-induced band folding. Real-space variations of the spectroscopic features allow us to quantify the spatial structure of the moiré potential at the rtG/hBN interface. Importantly, we find that accurately capturing the moiré site-dependent spectra requires incorporating a moiré potential acting on the top graphene layer with a sign opposite to that of the bottom layer into the continuum model. Our results thus provide key experimental and theoretical insights into understanding the role of the moire superlattice in rG/hBN heterostructures.

cond-mat.mes-hall↗

arXiv2025

Cavity-altered superconductivity

Is it feasible to alter the ground state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge. Here, we devised and implemented a novel platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br ($κ$-ET). The frequencies of infrared (IR) hyperbolic modes of hBN match the IR-active carbon-carbon stretching molecular resonance of ($κ$-ET) implicated in superconductivity. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the carbon-carbon stretching mode in ($κ$-ET). Meissner effect measurements via magnetic force microscopy demonstrate a strong suppression of superfluid density near the hBN/($κ$-ET) interface. Non-resonant control heterostructures, including RuCl$_3$/($κ$-ET) and hBN/$\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}_{8+x}$, do not display the superfluid suppression. These observations suggest that hBN/($κ$-ET) realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground state properties of complex quantum materials.

cond-mat.supr-con↗

arXiv2025

Charge Density Wave and Ferromagnetism in Intercalated CrSBr

In materials with one-dimensional electronic bands, electron-electron interactions can produce intriguing quantum phenomena, including spin-charge separation and charge density waves (CDW). Most of these systems, however, are non-magnetic, motivating a search for anisotropic materials where the coupling of charge and spin may affect emergent quantum states. Here, chemical intercalation of the van der Waals magnetic semiconductor CrSBr yields $Li_{0.17(2)} (tetrahydrofuran)_{0.26(3)} CrSBr$, which possess an electronically driven quasi-1D CDW with an onset temperature above room temperature. Concurrently, electron doping increases the magnetic ordering temperature from 132 K to 200 K and switches its interlayer magnetic coupling from antiferromagnetic to ferromagnetic. The spin-polarized nature of the anisotropic bands that give rise to this CDW enforces an intrinsic coupling of charge and spin. The coexistence and interplay of ferromagnetism and charge modulation in this exfoliatable material provides a promising platform for studying tunable quantum phenomena across a range of temperatures and thicknesses.

cond-mat.mtrl-sci↗

arXiv2024

Glassy Relaxation Dynamics in the Two-Dimensional Heavy Fermion Antiferromagnet CeSiI

The recent discovery of the van der Waals (vdW) layered heavy fermion antiferromagnetic metal CeSiI offers promising potential for achieving accessible quantum criticality in the two-dimensional (2D) limit. CeSiI exhibits both heavy fermion behavior and antiferromagnetic (AFM) ordering, while the exact magnetic structure and phase diagram have yet to be determined. Here, we investigate magnetic properties of atomically thin CeSiI devices with thicknesses ranging from 2-15 vdW layers. The thickness-dependent magnetotransport measurement reveals an intrinsic 2D nature of heavy fermion behavior and antiferromagnetism. Notably, we also find an isotropic, time-dependent hysteresis in both magnetoresistance and Hall resistance, showing glassy relaxation dynamics. This glassy behavior in magnetic structures may suggest the presence of spin glass phases or multipolar ordering, further establishing CeSiI as an intriguing material system for investigating the interplay between magnetic orders and the Kondo effect.

cond-mat.str-el↗

arXiv2024

Optical Band Engineering of Monolayer WSe2 in a Scanning Tunneling Microscope

Intense electromagnetic fields can result in dramatic changes in the electronic properties of solids. These changes are commonly studied using optical probes of the modified electronic structure. Here we use optical-scanning tunneling microscopy (optical-STM) equipped with near-field continuous wave (CW) laser excitation to directly measure the electronic structure of light-dressed states in a monolayer transition metal dichalcogenide (TMD) semiconductor, WSe2. We find that the effective tunneling gap and tunneling density of states are strongly influenced by the intensity of the electromagnetic field when the applied field is resonant with the bandgap of the semiconductor. Our findings indicate that CW laser excitation can be used to generate light-dressed electronic states of quantum materials when confined strongly to the nanoscale.

cond-mat.mtrl-sci↗

arXiv2024

Electronic Bound States in the Continuum in a 2D Metal

Bound states in the continuum (BICs) are quantum states that remain localized despite existing within a continuum of extended, delocalized states. They defy conventional wave theories and could be instrumental for quantum technologies that rely on the precise control of quantum states. While optical BICs have been realized in photonic systems, achieving electronic bound states in a metallic background remains an ongoing challenge. Here, we observe two defect states that remain localized within the metallic continuum of Pd5AlI2, a two-dimensional van der Waals metal. The emergence of these states is a manifestation of the hopping interference in the Pd5AlI2 lattice. This interference results in a (quasi) flat band and spatially localized eigenstates that are orthogonal to the metallic continuum thus avoiding hybridization with extended states.

cond-mat.mtrl-sci↗

arXiv2024

Two-Fold Anisotropic Superconductivity in Bilayer T$_d$-MoTe$_2$

Noncentrosymmetric 2D superconductors with large spin-orbit coupling offer an opportunity to explore superconducting behaviors far beyond the Pauli limit. One such superconductor, few-layer T$_d$-MoTe$_2$, has large upper critical fields that can exceed the Pauli limit by up to 600%. However, the mechanisms governing this enhancement are still under debate, with theory pointing towards either spin-orbit parity coupling or tilted Ising spin-orbit coupling. Moreover, ferroelectricity concomitant with superconductivity has been recently observed in the bilayer, where strong changes to superconductivity can be observed throughout the ferroelectric transition pathway. Here, we report the superconducting behavior of bilayer T$_d$-MoTe$ _2$ under an in-plane magnetic field, while systematically varying magnetic field angle and out-of-plane electric field strength. We find that superconductivity in bilayer MoTe$_2$ exhibits a two-fold symmetry with an upper critical field maxima occurring along the b-axis and minima along the a-axis. The two-fold rotational symmetry remains robust throughout the entire superconducting region and ferroelectric hysteresis loop. Our experimental observations of the spin-orbit coupling strength (up to 16.4 meV) agree with the spin texture and spin splitting from first-principles calculations, indicating that tilted Ising spin-orbit coupling is the dominant underlying mechanism.

cond-mat.supr-con↗

arXiv2024

Quantum Noise Spectroscopy of Criticality in an Atomically Thin Magnet

Dynamic critical fluctuations in magnetic materials encode important information about magnetic ordering in the associated critical exponents. Using nitrogen-vacancy centers in diamond, we implement $T_2$ (spin-decoherence) noise magnetometry to study critical dynamics in a 2D Van der Waals magnet CrSBr. By analyzing NV decoherence on time scales approaching the characteristic correlation time $τ_c$ of critical fluctuations, we extract the critical exponent $ν$ for the correlation length. Our result deviates from the Ising prediction and highlights the role of long-range dipolar interactions in 2D CrSBr. Furthermore, analyzing the divergence of the correlation length suggests the possibility of 2D-XY criticality in CrSBr in a temperature window near $T_C$ where static magnetic domains are absent. Our work provides a first demonstration of $T_2$ noise magnetometry to quantitatively analyze critical scaling behavior in 2D materials.

cond-mat.mes-hall↗

arXiv2024

Frustrated hopping from orbital decoration of a primitive two-dimensional lattice

Materials hosting flat electronic bands are a central focus of condensed matter physics as promising venues for novel electronic ground states. Two-dimensional (2D) geometrically frustrated lattices such as the kagome, dice, and Lieb lattices are attractive targets in this direction, anticipated to realize perfectly flat bands. Synthesizing these special structures, however, poses a formidable challenge, exemplified by the absence of solid-state materials realizing the dice and Lieb lattices. An alternative route leverages atomic orbitals to create the characteristic electron hopping of geometrically frustrated lattices. This strategy promises to expand the list of candidate materials to simpler structures, but is yet to be demonstrated experimentally. Here, we report the realization of frustrated hopping in the van der Waals (vdW) intermetallic Pd$_5$AlI$_2$, emerging from orbital decoration of a primitive square lattice. Using angle-resolved photoemission spectroscopy and quantum oscillations measurements, we demonstrate that the band structure of Pd$_5$AlI$_2$ includes linear Dirac-like bands intersected at their crossing point by a flat band, essential characteristics of frustrated hopping in the Lieb and dice lattices. Moreover, Pd$_5$AlI$_2$ is exceptionally stable, with the unusual bulk band structure and metallicity persisting in ambient conditions down to the monolayer limit. Our ability to realize an electronic structure characteristic of geometrically frustrated lattices establishes orbital decoration of primitive lattices as a new approach towards electronic structures that remain elusive to prevailing lattice-centric searches.

cond-mat.str-el↗

arXiv2024

Electronic interactions in Dirac fluids visualized by nano-terahertz spacetime interference of electron-photon quasiparticles

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in tera-hertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.

cond-mat.str-el↗

arXiv2024

Deep learning analysis of polaritonic waves images

Deep learning (DL) is an emerging analysis tool across sciences and engineering. Encouraged by the successes of DL in revealing quantitative trends in massive imaging data, we applied this approach to nano-scale deeply sub-diffractional images of propagating polaritonic waves in complex materials. We developed a practical protocol for the rapid regression of images that quantifies the wavelength and the quality factor of polaritonic waves utilizing the convolutional neural network (CNN). Using simulated near-field images as training data, the CNN can be made to simultaneously extract polaritonic characteristics and materials parameters in a timescale that is at least three orders of magnitude faster than common fitting/processing procedures. The CNN-based analysis was validated by examining the experimental near-field images of charge-transfer plasmon polaritons at Graphene/α-RuCl3 interfaces. Our work provides a general framework for extracting quantitative information from images generated with a variety of scanning probe methods.

cond-mat.mtrl-sci↗