arXiv subjects

Abhay N. Pasupathy

Publications and source records attributed to Abhay N. Pasupathy.

72 records · Page 4Linked to original sources

arXiv2018

Magic Angle Spectroscopy

The electronic properties of heterostructures of atomically-thin van der Waals (vdW) crystals can be modified substantially by Moiré superlattice potentials arising from an interlayer twist between crystals. Moiré-tuning of the band structure has led to the recent discovery of superconductivity and correlated insulating phases in twisted bilayer graphene (TBLG) near the so-called "magic angle" of $\sim$1.1°, with a phase diagram reminiscent of high T$_c$ superconductors. However, lack of detailed understanding of the electronic spectrum and the atomic-scale influence of the Moiré pattern has so far precluded a coherent theoretical understanding of the correlated states. Here, we directly map the atomic-scale structural and electronic properties of TBLG near the magic angle using scanning tunneling microscopy and spectroscopy (STM/STS). We observe two distinct van Hove singularities (vHs) in the LDOS which decrease in separation monotonically through 1.1° with the bandwidth (t) of each vHs minimized near the magic angle. When doped near half Moiré band filling, the conduction vHs shifts to the Fermi level and an additional correlation-induced gap splits the vHs with a maximum size of 7.5 meV. We also find that three-fold (C$_3$) rotational symmetry of the LDOS is broken in doped TBLG with a maximum symmetry breaking observed for states near the Fermi level, suggestive of nematic electronic interactions. The main features of our doping and angle dependent spectroscopy are captured by a tight-binding model with on-site (U) and nearest neighbor Coulomb interactions. We find that the ratio U/t is of order unity, indicating that electron correlations are significant in magic angle TBLG. Rather than a simple maximization of the DOS, superconductivity arises in TBLG at angles where the ratio U/t is largest, suggesting a pairing mechanism based on electron-electron interactions.

cond-mat.mes-hall↗

arXiv2018

Visualizing the Nonlinear Coupling between Strain and Electronic Nematicity in the Iron Pnictides by Elasto-Scanning Tunneling Spectroscopy

Mechanical strain is a powerful technique for tuning electronic structure and interactions in quantum materials. In a system with tetragonal symmetry, a tunable uniaxial in-plane strain can be used to probe nematic correlations in the same way that a tunable magnetic field is used to probe magnetic correlations. Here, we present a new spectroscopic scanned probe technique that provides atomic-resolution insight into the effect of anisotropic strain on the electronic structure. We use this technique to study nematic fluctuations and nematic order across the phase diagram of a prototypical iron-based superconductor. By extracting quantitatively the electronic anisotropy as function of applied strain, we show that while true long range nematic order is established at the tetragonal to orthorhombic structural transition temperature, sizable nematic fluctuations persist to high temperatures and also to the overdoped end of the superconducting dome. Remarkably, we find that uniaxial strain in the pnictides significantly enhances the amplitude of the nematic fluctuations, indicating a strong nonlinear coupling between structure and electronic nematicity.

cond-mat.str-el↗

arXiv2018

Atomic scale characterization of graphene p-n junctions for electron-optical applications

Graphene p-n junctions offer a potentially powerful approach towards controlling electron trajectories via collimation and focusing in ballistic solid-state devices. The ability of p-n junctions to control electron trajectories depends crucially on the doping profile and roughness of the junction. Here, we use four-probe scanning tunneling microscopy and spectroscopy (STM/STS) to characterize two state-of-the-art graphene p-n junction geometries at the atomic scale, one with CMOS polySi gates and another with naturally cleaved graphite gates. Using spectroscopic imaging, we characterize the local doping profile across and along the p-n junctions. We find that realistic junctions exhibit non-ideality both in their geometry as well as in the doping profile across the junction. We show that the geometry of the junction can be improved by using the cleaved edge of van der Waals metals such as graphite to define the junction. We quantify the geometric roughness and doping profiles of junctions experimentally and use these parameters in Nonequilibrium Green's Function based simulations of focusing and collimation in these realistic junctions. We find that for realizing Veselago focusing, it is crucial to minimize lateral interface roughness which only natural graphite gates achieve, and to reduce junction width, in which both devices under investigation underperform. We also find that carrier collimation is currently limited by the non-linearity of the doping profile across the junction. Our work provides benchmarks of the current graphene p-n junction quality and provides guidance for future improvements.

cond-mat.mes-hall↗

arXiv2018

Dictionary Learning in Fourier Transform Scanning Tunneling Spectroscopy

Modern high-resolution microscopes, such as the scanning tunneling microscope, are commonly used to study specimens that have dense and aperiodic spatial structure. Extracting meaningful information from images obtained from such microscopes remains a formidable challenge. Fourier analysis is commonly used to analyze the underlying structure of fundamental motifs present in an image. However, the Fourier transform fundamentally suffers from severe phase noise when applied to aperiodic images. Here, we report the development of a new algorithm based on nonconvex optimization, applicable to any microscopy modality, that directly uncovers the fundamental motifs present in a real-space image. Apart from being quantitatively superior to traditional Fourier analysis, we show that this novel algorithm also uncovers phase sensitive information about the underlying motif structure. We demonstrate its usefulness by studying scanning tunneling microscopy images of a Co-doped iron arsenide superconductor and prove that the application of the algorithm allows for the complete recovery of quasiparticle interference in this material. Our phase sensitive quasiparticle interference imaging results indicate that the pairing symmetry in optimally doped NaFeAs is consistent with a sign-changing s+- order parameter.

physics.comp-ph↗

arXiv2018

Via Method for Lithography Free Contact and Preservation of 2D Materials

Atomically thin 2D materials span the common components of electronic circuits as metals, semi-conductors, and insulators, and can manifest correlated phases such as superconductivity, charge density waves, and magnetism. An ongoing challenge in the field is to incorporate these 2D materials into multi-layer hetero-structures with robust electrical contacts while preventing disorder and degradation. In particular, preserving and studying air-sensitive 2D materials has presented a significant challenge since they readily oxidize under atmospheric conditions. We report a new technique for contacting 2D materials, in which metal via contacts are integrated into flakes of insulating hexagonal boron nitride, and then placed onto the desired conducting 2D layer, avoiding direct lithographic patterning onto the 2D conductor. The metal contacts are planar with the bottom surface of the boron nitride and form robust contacts to multiple 2D materials. These structures protect air-sensitive 2D materials for months with no degradation in performance. This via contact technique will provide the capability to produce atomic printed circuit boards that can form the basis of more complex multi-layer heterostructures.

cond-mat.mes-hall↗

arXiv2017

Temperature-Driven Topological Transition in 1T'-MoTe2

The topology of Weyl semimetals requires the existence of unique surface states. Surface states have been visualized in spectroscopy measurements, but their connection to the topological character of the material remains largely unexplored. 1T'-MoTe2, presents a unique opportunity to study this connection. This material undergoes a phase transition at 240K that changes the structure from orthorhombic (putative Weyl semimetal) to monoclinic (trivial metal), while largely maintaining its bulk electronic structure. Here we show from temperature-dependent quasiparticle interference measurements that this structural transition also acts as a topological switch for surface states in 1T'-MoTe2. At low temperature, we observe strong quasiparticle scattering, consistent with theoretical predictions and photoemission measurements for the surface states in this material. In contrast, measurements performed at room temperature show the complete absence of the scattering wavevectors associated with the trivial surface states. These distinct quasiparticle scattering behaviors show that 1T'-MoTe2 is ideal for separating topological and trivial electronic phenomena via temperature dependent measurements.

cond-mat.mtrl-sci↗

arXiv2017

Achieving Large, Tunable Strain in Monolayer Transition-Metal Dichalcogenides

We describe a facile technique based on polymer encapsulation to apply several percent controllable strains to monolayer and few-layer Transition Metal Dichalcogenides (TMDs). We use this technique to study the lattice response to strain via polarized Raman spectroscopy in monolayer WSe2 and WS2. The application of strain causes mode-dependent redshifts, with larger shift rates observed for in-plane modes. We observe a splitting of the degeneracy of the in-plane E' modes in both materials and measure the Gruneisen parameters. At large strain, we observe that the reduction of crystal symmetry can lead to a change in the polarization response of the A' mode in WS2. While both WSe2 and WS2 exhibit similar qualitative changes in the phonon structure with strain, we observe much larger changes in mode positions and intensities with strain in WS2. These differences can be explained simply by the degree of iconicity of the metal-chalcogen bond.

cond-mat.mes-hall↗

arXiv2016

Distinct surface and bulk charge density waves in ultrathin 1T-TaS2

We employ low-frequency Raman spectroscopy to study the nearly commensurate (NC) to commensurate (C) charge density wave (CDW) transition in 1T-TaS2 ultrathin flakes protected from oxidation. We identify new modes originating from C phase CDW phonons that are distinct from those seen in bulk 1T-TaS2. We attribute these to CDW modes from the surface layers. By monitoring individual modes with temperature, we find that surfaces undergo a separate, low-hysteresis NC-C phase transition that is decoupled from the transition in the bulk layers. This indicates the activation of a secondary phase nucleation process in the limit of weak interlayer interaction, which can be understood from energy considerations.

cond-mat.mtrl-sci↗

arXiv2016

Atomic Lattice Disorder in Charge Density Wave Phases of Exfoliated Dichalcogenides (1T-TaS2)

Charge density waves (CDW) and their concomitant periodic lattice distortions (PLD) govern the electronic properties in many layered transition-metal dichalcogenides. In particular, 1T-TaS2 undergoes a metal-to-insulator phase transition as the PLD becomes commensurate with the crystal lattice. Here we directly image PLDs of the nearly-commensurate (NC) and commensurate (C) phases in thin exfoliated 1T-TaS2 using atomic resolution scanning transmission electron microscopy at room and cryogenic temperature. At low temperatures, we observe commensurate PLD superstructures, suggesting ordering of the CDWs both in- and out-of-plane. In addition, we discover stacking transitions in the atomic lattice that occur via one bond length shifts. Interestingly, the NC PLDs exist inside both the stacking domains and their boundaries. Transitions in stacking order are expected to create fractional shifts in the CDW between layers and may be another route to manipulate electronic phases in layered dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2014

Experimental evidence for a Bragg glass density wave phase in a transition-metal dichalcogenide

Analysis of the spatial dependence of current-voltage characteristics obtained from scanning tunneling microscopy experiments indicates that the charge density wave (CDW) occurring in NbSe$_2$ is subject to locally strong pinning by a non-negligible density of defects, but that on the length scales accessible in this experiment the material is in a "Bragg glass" phase where dislocations and anti-dislocations occur in bound pairs and free dislocations are not observed. A Landau theory-based analysis is presented showing how a strong local modulation may produce only a weak long range effect on the CDW phase.

cond-mat.dis-nn↗

arXiv2012

Molecular beam growth of graphene nanocrystals on dielectric substrates

We demonstrate the growth of graphene nanocrystals by molecular beam methods that employ a solid carbon source, and that can be used on a diverse class of large area dielectric substrates. Characterization by Raman and Near Edge X-ray Absorption Fine Structure spectroscopies reveal a sp2 hybridized hexagonal carbon lattice in the nanocrystals. Lower growth rates favor the formation of higher quality, larger size multi-layer graphene crystallites on all investigated substrates. The surface morphology is determined by the roughness of the underlying substrate and graphitic monolayer steps are observed by ambient scanning tunneling microscopy.

cond-mat.mtrl-sci↗

arXiv2011

Visualizing Individual Nitrogen Dopants in Monolayer Graphene

In monolayer graphene, substitutional doping during growth can be used to alter its electronic properties. We used scanning tunneling microscopy (STM), Raman spectroscopy, x-ray spectroscopy, and first principles calculations to characterize individual nitrogen dopants in monolayer graphene grown on a copper substrate. Individual nitrogen atoms were incorporated as graphitic dopants, and a fraction of the extra electron on each nitrogen atom was delocalized into the graphene lattice. The electronic structure of nitrogen-doped graphene was strongly modified only within a few lattice spacings of the site of the nitrogen dopant. These findings show that chemical doping is a promising route to achieving high-quality graphene films with a large carrier concentration.

cond-mat.mtrl-sci↗

arXiv2010

Nanoscale Proximity Effect in the High Temperature Superconductor Bi-2212

High temperature cuprate superconductors exhibit extremely local nanoscale phenomena and strong sensitivity to doping. While other experiments have looked at nanoscale interfaces between layers of different dopings, we focus on the interplay between naturally inhomogeneous nanoscale regions. Using scanning tunneling microscopy to carefully track the same region of the sample as a function of temperature, we show that regions with weak superconductivity can persist to elevated temperatures if bordered by regions of strong superconductivity. This suggests that it may be possible to increase the maximum possible transition temperature by controlling the distribution of dopants.

cond-mat.supr-con↗

arXiv2008

Electronic Origin of the Inhomogeneous Pairing Interaction in the High-Tc Superconductor Bi2Sr2CaCu2O8+d

Identifying the mechanism of superconductivity in the high-temperature cuprate superconductors is one of the major outstanding problems in physics. We report local measurements of the onset of superconducting pairing in the high-transition temperature (Tc) superconductor Bi2Sr2CaCu2O8+d using a lattice-tracking spectroscopy technique with a scanning tunneling microscope. We can determine the temperature dependence of the pairing energy gaps, the electronic excitations in the absence of pairing, and the effect of the local coupling of electrons to bosonic excitations. Our measurements reveal that the strength of pairing is determined by the unusual electronic excitations of the normal state, suggesting that strong electron-electron interactions rather than low-energy (<0.1 volts) electron-boson interactions are responsible for superconductivity in the cuprates.

cond-mat.supr-con↗

arXiv2007

Visualizing pair formation on the atomic scale in the high-Tc superconductor Bi2Sr2CaCu2O8+d

Pairing of electrons in conventional superconductors occurs at the superconducting transition temperature Tc, creating an energy gap D in the electronic density of states (DOS). In the high-Tc superconductors, a partial gap in the DOS exists for a range of temperatures above Tc. A key question is whether the gap in the DOS above Tc is associated with pairing, and what determines the temperature at which incoherent pairs form. Here we report the first spatially resolved measurements of gap formation in a high-Tc superconductor, measured on Bi2Sr2CaCu2O8+d samples with different Tc values (hole concentration of 0.12 to 0.22) using scanning tunnelling microscopy. Over a wide range of doping from 0.16 to 0.22 we find that pairing gaps nucleate in nanoscale regions above Tc. These regions proliferate as the temperature is lowered, resulting in a spatial distribution of gap sizes in the superconducting state. Despite the inhomogeneity, we find that every pairing gap develops locally at a temperature Tp, following the relation 2D/kBTp = 8. At very low doping (<0.14), systematic changes in the DOS indicate the presence of another phenomenon, which is unrelated and perhaps competes with electron pairing. Our observation of nanometre-sized pairing regions provides the missing microscopic basis for understanding recent reports of fluctuating superconducting response above Tc in hole-doped high-Tc copper oxide superconductors.

cond-mat.supr-con↗

arXiv2006

Phonons in Molecular Quantum Dots: Density Functional Calculation of Franck-Condon Emission Rates in External Fields

We report the calculation of various phonon overlaps and their corresponding phonon emission probabilities for the problem of an electron tunneling onto and off of the buckyball-dimer molecular quantum dot $C_{72}$, both with and without the influence of an external field. We show that the stretch mode of the two balls of the dumbbell couples most strongly to the electronic transition, and in turn that a field in the direction of the bond between the two $C_{36}$ balls is most effective at further increasing the phonon emission into the stretch mode. As the field is increased, phonon emission increases in probability with an accompanying decrease in probability of the dot remaining in the ground vibrational state. We also present a simple model to gauge the effect of molecular size on the phonon emission of molecules similar to our $C_{72}$ molecule, including the experimentally tested $C_{140}$. In our approach we do not assume that the hessians of the molecule are identical for different charge states. Our treatment is hence a generalization of the traditional phonon overlap calculations for coupled electron-photon transition in solids.

cond-mat.mes-hall↗

arXiv2005

From ballistic transport to tunneling in electromigrated ferromagnetic breakjunctions

We fabricate ferromagnetic nanowires with constrictions whose cross section can be reduced gradually from 100 nm to the atomic scale and eventually to the tunneling regime by means of electromigration. These devices are mechanically stable against magnetostriction and magnetostatic effects. We measure magnetoresistances ~ 0.3% for 100*30 nm^2 constrictions, increasing to a maximum of 80% for atomic-scale widths. These results are consistent with a geometrically-constrained domain wall trapped at the constriction. For the devices in the tunneling regime we observe large fluctuations in MR, between -10 and 85%.

cond-mat.mes-hall↗

arXiv2004

Transistor behavior via Au clusters etched from electrodes in an acidic gating solution: metal nanoparticles mimicking conducting polymers

We report that the electrical conductance between closely-spaced gold electrodes in acid solution can be turned from off [insulating; I] to on [conducting; C] to off again by monotonically sweeping a gate voltage applied to the solution. We propose that this ICI transistor action is due to an electrochemical process dependent on nanoparticles etched from the surface of the gold electrodes. These measurements mimic closely the characteristics of nanoscale acid-gated polyaniline transistors, so that researchers should guard against misinterpreting this effect in future molecular-electronics experiments.

cond-mat.mtrl-sci↗