arXiv subjects

A. N. Pasupathy

Publications and source records attributed to A. N. Pasupathy.

At least 19 recordsLinked to original sources

arXiv2025

Sliding Disassembly of van der Waals Heterostructures

Many recent advances in our understanding of two-dimensional (2D) electron systems stem from van der Waals (vdW) heterostructures. The assembly process relies on the weak bonding across interfaces between layered vdW compounds, making it possible to construct exceptionally clean heterostructures from chemically and structurally distinct materials - a challenging task for traditional thin-film growth techniques. Here we demonstrate an additional, dynamic degree of freedom afforded by vdW interfaces, wherein we use microstructured polymer stamps to disassemble and reconfigure vdW heterostructures by sliding. We apply this technique to alter the dielectric environment of monolayer graphene, perform scanning tunneling microscopy on semiconducting and air-sensitive monolayers, and manipulate strain-sensitive moiré materials. Together these demonstrations suggest a new paradigm for assembling and dynamically modifying van der Waals heterostructures, with the potential to reveal new insights into 2D electron systems.

cond-mat.mes-hall↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2025

Formation of Frustrated Charge Density Waves in Kagome Metal LuNb$_6$Sn$_6$

The charge density wave (CDW), a translational symmetry breaking electronic liquid, plays a pivotal role in correlated quantum materials, such as high-T$_c$ superconductors and topological semimetals. Recently, CDWs that possibly intertwine with superconductivity and magnetism are observed in various kagome metals. However, the nature of CDWs and the role of the Fermi surface (FS) topology in these materials remain an unresolved challenge. In this letter, we reveal the formation of CDWs in the newly discovered kagome metal LuNb$_6$Sn$_6$. We observe a precursor CDW correlation that features a "yield sign"-like hollow triangle diffuse scattering pattern and nearly complete softening of a flat optical phonon band near Q$_H$=(1/3, 1/3, 1/2). The scattering intensity of the precursor CDW displays divergent behavior as decreasing temperature until T$_{CDW}$=70 K, where a competing CDW at Q$_{CDW}$=(1/3, 1/3, 1/3) emerges. Using scanning tunneling microscopy/spectroscopy, we image the frustrated CDW patterns that show a short phase coherence length about ~20 nm in real space. Combined with first principles calculations, our observations support frustrated lattice interactions that are modulated by the FS topology. These results shed light on the interplay between FS and CDW in quantum materials with nearly degenerate structural deformation patterns.

cond-mat.str-el↗

arXiv2023

First-order phase transition vs. spin-state quantum-critical scenarios in strain-tuned epitaxial cobaltite thin films

Pr-containing perovskite cobaltites exhibit unusual valence transitions, coupled to coincident structural, spin-state, and metal-insulator transitions. Heteroepitaxial strain was recently used to control these phenomena in the model (Pr$_{1-y}$Y$_y$)$_{1-x}$Ca$_x$CoO$_{3-δ}$ system, stabilizing a nonmagnetic insulating phase under compression (with a room-temperature valence/spin-state/metal-insulator transition) and a ferromagnetic metallic phase under tension, thus exposing a potential spin-state quantum critical point. The latter has been proposed in cobaltites and can be probed in this system as a function of a disorder-free variable (strain). We study this here via thickness-dependent strain relaxation in compressive SrLaAlO$_4$(001)/(Pr$_{0.85}$Y$_{0.15}$)$_{0.70}$Ca$_{0.30}$CoO$_{3-δ}$ epitaxial thin films to quasi-continuously probe structural, electronic, and magnetic behaviors across the nonmagnetic-insulator/ferromagnetic-metal boundary. High-resolution X-ray diffraction, electronic transport, magnetometry, polarized neutron reflectometry, and temperature-dependent magnetic force microscopy provide a detailed picture, including abundant evidence of temperature- and strain-dependent phase coexistence. This indicates a first-order phase transition as opposed to spin-state quantum-critical behavior, which we discuss theoretically via a phenomenological Landau model for coupled spin-state and magnetic phase transitions.

cond-mat.str-el↗

arXiv2023

Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) material heterostructures. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

cond-mat.mes-hall↗

arXiv2019

Seeing moiré superlattices

Moiré superlattices in van der Waals (vdW) heterostructures have given rise to a number of emergent electronic phenomena due to the interplay between atomic structure and electron correlations. A lack of a simple way to characterize moiré superlattices has impeded progress in the field. In this work we outline a simple, room-temperature, ambient method to visualize real-space moiré superlattices with sub-5 nm spatial resolution in a variety of twisted vdW heterostructures including but not limited to conducting graphene, insulating boron nitride and semiconducting transition metal dichalcogenides. Our method utilizes piezoresponse force microscopy, an atomic force microscope modality which locally measures electromechanical surface deformation. We find that all moiré superlattices, regardless of whether the constituent layers have inversion symmetry, exhibit a mechanical response to out-of-plane electric fields. This response is closely tied to flexoelectricity wherein electric polarization and electromechanical response is induced through strain gradients present within moiré superlattices. Moiré superlattices of 2D materials thus represent an interlinked network of polarized domain walls in a non-polar background matrix.

cond-mat.mes-hall↗

arXiv2019

Linear Scaling of the Superfluid Density with the Critical Temperature in the Layered Superconductor 2H-NbSe_2

We report on high-pressure (p_max = 2.1 GPa) muon spin rotation experiments probing the temperature-dependent magnetic penetration depth in the layered superconductor 2H-NbSe_2. Upon increasing the pressure, we observe a substantial increase of the superfluid density n_s, which we find to scale linearly with T_c. This linear scaling is considered a hallmark feature of unconventional superconductivity, especially in high-temperature cuprate superconductors. Our current results, along with our earlier findings on 1T'-MoTe_2 (Z. Guguchia et. al., Nature Communications 8, 1082 (2017)), demonstrate that this linear relation is also an intrinsic property of the superconductivity in transition metal dichalcogenides, whereas the ratio T_c/T_F is approximately a factor of 20 lower than the ratio observed in hole-doped cuprates. We, furthermore, find that the values of the superconducting gaps are insensitive to the suppression of the quasi-two-dimensional CDW state, indicating that the CDW ordering and the superconductivity in 2H-NbSe_2 are independent of each other.

cond-mat.supr-con↗

arXiv2019

Absence of dissipationless transport in clean 2D superconductors

Dissipationless charge transport is one of the defining properties of superconductors (SC). The interplay between dimensionality and disorder in determining the onset of dissipation in SCs remains an open theoretical and experimental problem. In this work, we present measurements of the dissipation phase diagrams of SCs in the two dimensional (2D) limit, layer by layer, down to a monolayer in the presence of temperature (T), magnetic field (B), and current (I) in 2H-NbSe2. Our results show that the phase-diagram strongly depends on the SC thickness even in the 2D limit. At four layers we can define a finite region in the I-B phase diagram where dissipationless transport exists at T=0. At even smaller thicknesses, this region shrinks in area. In a monolayer, we find that the region of dissipationless transport shrinks towards a single point, defined by T=B=I=0. In applied field, we show that time-dependent-Ginzburg-Landau (TDGL) simulations that describe dissipation by vortex motion, qualitatively reproduce our experimental I-B phase diagram. Last, we show that by using non-local transport and TDGL calculations that we can engineer charge flow and create phase boundaries between dissipative and dissipationless transport regions in a single sample, demonstrating control over non-equilibrium states of matter.

cond-mat.mes-hall↗

arXiv2018

Hundredfold Enhancement of Light Emission via Defect Control in Monolayer Transition-Metal Dichalcogenides

Two dimensional (2D) transition-metal dichalcogenide (TMD) based semiconductors have generated intense recent interest due to their novel optical and electronic properties, and potential for applications. In this work, we characterize the atomic and electronic nature of intrinsic point defects found in single crystals of these materials synthesized by two different methods - chemical vapor transport and self-flux growth. Using a combination of scanning tunneling microscopy (STM) and scanning transmission electron microscopy (STEM), we show that the two major intrinsic defects in these materials are metal vacancies and chalcogen antisites. We show that by control of the synthetic conditions, we can reduce the defect concentration from above $10^{13} /cm^2$ to below $10^{11} /cm^2$. Because these point defects act as centers for non-radiative recombination of excitons, this improvement in material quality leads to a hundred-fold increase in the radiative recombination efficiency.

cond-mat.mtrl-sci↗

arXiv2018

Extreme Sensitivity of the Superconducting State in Thin Films

All non-interacting two-dimensional electronic systems are expected to exhibit an insulating ground state. This conspicuous absence of the metallic phase has been challenged only in the case of low-disorder, low density, semiconducting systems where strong interactions dominate the electronic state. Unexpectedly, over the last two decades, there have been multiple reports on the observation of a state with metallic characteristics on a variety of thin-film superconductors. To date, no theoretical explanation has been able to fully capture the existence of such a state for the large variety of superconductors exhibiting it. Here we show that for two very different thin-film superconductors, amorphous indium-oxide and a single-crystal of 2H-NbSe2, this metallic state can be eliminated by filtering external radiation. Our results show that these superconducting films are extremely sensitive to external perturbations leading to the suppression of superconductivity and the appearance of temperature independent, metallic like, transport at low temperatures. We relate the extreme sensitivity to the theoretical observation that, in two-dimensions, superconductivity is only marginally stable.

cond-mat.supr-con↗

arXiv2017

Magnetism in Semiconducting Molybdenum Dichalcogenides

Transition metal dichalcogenides (TMDs) are interesting for understanding fundamental physics of two-dimensional materials (2D) as well as for many emerging technologies, including spin electronics. Here, we report the discovery of long-range magnetic order below TM = 40 K and 100 K in bulk semiconducting TMDs 2H-MoTe2 and 2H-MoSe2, respectively, by means of muon spin-rotation (muSR), scanning tunneling microscopy (STM), as well as density functional theory (DFT) calculations. The muon spin rotation measurements show the presence of a large and homogeneous internal magnetic fields at low temperatures in both compounds indicative of long-range magnetic order. DFT calculations show that this magnetism is promoted by the presence of defects in the crystal. The STM measurements show that the vast majority of defects in these materials are metal vacancies and chalcogen-metal antisites which are randomly distributed in the lattice at the sub-percent level. DFT indicates that the antisite defects are magnetic with a magnetic moment in the range of 0.9-2.8 mu_B. Further, we find that the magnetic order stabilized in 2H-MoTe2 and 2H-MoSe2 is highly sensitive to hydrostatic pressure. These observations establish 2H-MoTe2 and 2H-MoSe2 as a new class of magnetic semiconductors and opens a path to studying the interplay of 2D physics and magnetism in these interesting semiconductors.

cond-mat.mtrl-sci↗

arXiv2017

Possible topologically non-trivial superconducting order parameter in type-II Weyl semimetal T_d-MoTe_2

MoTe_2, with the orthorhombic T_d phase, is a new type (type-II) of Weyl semimetal, where the Weyl Fermions emerge at the boundary between electron and hole pockets. Non-saturating magnetoresistance (MR), and superconductivity were also observed in T_d-MoTe_2. Understanding the superconductivity in T_d-MoTe_2, which was proposed to be topologically non-trivial, is of eminent interest. Here, we report high-pressure (p_max = 1.3 GPa) muon spin rotation experiments on the temperature-dependent magnetic penetration depth in T_d-MoTe_2. A substantial increase of the superfluid density n_s/m^* and a linear scaling with T_c is observed under pressure. Moreover, the superconducting order parameter in T_d-MoTe_2 is determined to be two gap (s+s)-wave symmetric. We also excluded time reversal symmetry breaking in the SC state with sensitive zero-field $μ$SR experiments. Considering the previous report \cite{Balicas1} on the strong suppression of T_c in T_d-MoTe_2 by disorder, we suggest that s^{+-} (topological order parameter) state is more likely to be realized in MoTe_2 than the s^{++} (trivial) state. Should s^{+-} be the SC gap symmetry, the T_d-MoTe_2 is, to our knowledge, the first known example of a time reversal invariant topological (Weyl) superconductor.

cond-mat.supr-con↗

arXiv2016

Engineering the structural and electronic phases of MoTe2 through W substitution

MoTe$_2$ is an exfoliable transition metal dichalcogenide (TMD) which crystallizes in three symmetries, the semiconducting trigonal-prismatic $2H-$phase, the semimetallic $1T^{\prime}$ monoclinic phase, and the semimetallic orthorhombic $T_d$ structure. The $2H-$phase displays a band gap of $\sim 1$ eV making it appealing for flexible and transparent optoelectronics. The $T_d-$phase is predicted to possess unique topological properties which might lead to topologically protected non-dissipative transport channels. Recently, it was argued that it is possible to locally induce phase-transformations in TMDs, through chemical doping, local heating, or electric-field to achieve ohmic contacts or to induce useful functionalities such as electronic phase-change memory elements. The combination of semiconducting and topological elements based upon the same compound, might produce a new generation of high performance, low dissipation optoelectronic elements. Here, we show that it is possible to engineer the phases of MoTe$_2$ through W substitution by unveiling the phase-diagram of the Mo$_{1-x}$W$_x$Te$_2$ solid solution which displays a semiconducting to semimetallic transition as a function of $x$. We find that only $\sim 8$ \% of W stabilizes the $T_d-$phase at room temperature. Photoemission spectroscopy, indicates that this phase possesses a Fermi surface akin to that of WTe$_2$.

cond-mat.mes-hall↗

arXiv2015

Nature of the Quantum Metal in a Two-Dimensional Crystalline Superconductor

Two-dimensional (2D) materials are not expected to be metals at low temperature due to electron localization. Consistent with this, pioneering studies on thin films reported only superconducting and insulating ground states, with a direct transition between the two as a function of disorder or magnetic field. However, more recent works have revealed the presence of an intermediate metallic state occupying a substantial region of the phase diagram whose nature is intensely debated. Here, we observe such a state in the disorder-free limit of a crystalline 2D superconductor, produced by mechanical co-lamination of NbSe$_2$ in inert atmosphere. Under a small perpendicular magnetic field, we induce a transition from superconductor to the intermediate metallic state. We find a new power law scaling with field in this phase, which is consistent with the Bose metal model where metallic behavior arises from strong phase fluctuations caused by the magnetic field.

cond-mat.supr-con↗

arXiv2015

Structure and Control of Charge Density Waves in Two-Dimensional 1T-TaS2

The layered transition metal dichalcogenides host a rich collection of charge density wave (CDW) phases in which both the conduction electrons and the atomic structure display translational symmetry breaking. Manipulating these complex states by purely electronic methods has been a long-sought scientific and technological goal. Here, we show how this can be achieved in 1T-TaS2 in the two-dimensional (2D) limit. We first demonstrate that the intrinsic properties of atomically-thin flakes are preserved by encapsulation with hexagonal boron nitride in inert atmosphere. We use this facile assembly method together with TEM and transport measurements to probe the nature of the 2D state and show that its conductance is dominated by discommensurations. The discommensuration structure can be precisely tuned in few-layer samples by an in-plane electric current, allowing continuous electrical control over the discommensuration-melting transition in 2D.

cond-mat.mes-hall↗

arXiv2014

Quasiparticle Interference, quasiparticle interactions and the origin of the charge density-wave in 2H-NbSe$_{2}$

We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe$_{2}$, that we measure by scanning tunneling spectroscopic imaging. We show from the momentum and energy dependence of the quasiparticle interference that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe$_{2}$. We demonstrate that by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wavevector and energy dependence of the important electronic scattering processes thereby obtaining direct information both about the fermiology and the interactions. In 2H-NbSe$_{2}$, we use this combination to show that the important near-Fermi-surface electronic physics is dominated by the coupling of the quasiparticles to soft mode phonons at a wave vector different from the CDW ordering wave vector.

cond-mat.str-el↗

arXiv2013

Visualization of Electron Nematicity and Unidirectional Antiferroic Fluctuations at High Temperatures in NaFeAs

The driving forces behind electronic nematicity in the iron pnictides remain hotly debated. We use atomic-resolution variable-temperature scanning tunneling spectroscopy to provide the first direct visual evidence that local electronic nematicity and unidirectional antiferroic (stripe) fluctuations persist to temperatures almost twice the nominal structural ordering temperature in the parent pnictide NaFeAs. Low-temperature spectroscopic imaging of nematically-ordered NaFeAs shows anisotropic electronic features that are not observed for isostructural, non-nematic LiFeAs. The local electronic features are shown to arise from scattering interference around crystalline defects in NaFeAs, and their spatial anisotropy is a direct consequence of the structural and stripe-magnetic order present at low temperature. We show that the anisotropic features persist up to high temperatures in the nominally tetragonal phase of the crystal. The spatial distribution and energy dependence of the anisotropy at high temperatures is explained by the persistence of large amplitude, short-range, unidirectional, antiferroic (stripe) fluctuations, indicating that strong density wave fluctuations exist and couple to near-Fermi surface electrons even far from the structural and density wave phase boundaries.

cond-mat.supr-con↗

arXiv2013

Visualizing the Charge Density Wave Transition in 2H-NbSe2 in Real Space

We report the direct observation in real space of the charge density wave (CDW) phase transition in pristine 2H-NbSe2 using atomic-resolution scanning tunneling microscopy (STM). We find that static CDW order is established in nanoscale regions in the vicinity of defects at temperatures that are several times the bulk transition temperature Tcdw. On lowering the temperature, the correlation length of these patches increases steadily until CDW order is established in all of space, demonstrating the crucial role played by defects in the physics of the transition region. The nanoscale CDW order has an energy and temperature-independent wavelength. Spectroscopic imaging measurements of the real-space phase of the CDW indicate that an energy gap in NbSe2 occurs at 0.7eV below the Fermi energy in the CDW phase, suggesting that strong electron-lattice interactions and not Fermi surface physics is the dominant cause for CDW formation in NbSe2.

cond-mat.str-el↗