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R. Sankar

Publications and source records attributed to R. Sankar.

At least 55 records · Page 3Linked to original sources

Interplay of orbital effects and nanoscale strain in topological crystalline insulators

Orbital degrees of freedom can have pronounced effects on the fundamental properties of electrons in solids. In addition to influencing bandwidths, gaps, correlation strength and dispersion, orbital effects have also been implicated in generating novel electronic and structural phases, such as Jahn-Teller effect and colossal magnetoresistance. In this work, we show for the first time how the orbital nature of bands can result in non-trivial effects of strain on the band structure. We use scanning tunneling microscopy and quasiparticle interference imaging to study the effects of strain on the electronic structure of a heteroepitaxial thin film of a topological crystalline insulator, SnTe. We find a surprising effect where strain applied in one direction affects the band structure in the perpendicular direction. Our theoretical calculations indicate that this effect directly arises from the orbital nature of the conduction and valance bands. Our results imply that a microscopic model capturing strain effects on the band structure must include a consideration of the orbital nature of the bands.

cond-mat.mes-hall↗

Large transverse Hall-like signal in topological Dirac semimetal Cd3As2

Cadmium arsenide ($\rm Cd_3As_2$) is known for its inverted band structure and ultra-high electron mobility. It has been theoretically predicted and also confirmed by ARPES experiments to exhibit a 3D Dirac semimetal phase containing degenerate Weyl nodes. From magneto-transport measurements in high quality single crystals of $\rm Cd_3As_2$, a small effective mass $m^* \approx$ 0.05 $m_e$ is determined from the Shubnikov-de Haas (SdH) oscillations. In certain field orientations, we find a splitting of the SdH oscillation frequency in the FFT spectrum suggesting a possible lifting of the double degeneracy in accord with the helical spin texture at outer and inner Fermi surfaces with opposite chirality predicted by our \textit{ab initio} calculations. Strikingly, a large antisymmetric magnetoresistance with respect to the applied magnetic fields is uncovered over a wide temperature range in needle crystal of $\rm Cd_3As_2$ with its long axis along [112] crystal direction. It reveals a possible contribution of intrinsic anomalous velocity term in the transport equation resulting from a unique 3D Rashba-like spin splitted bands that can be obtained from band calculations with the inclusion of Cd antisite defects.

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Tellurium-bridged two-leg spin ladder in Ba$_2$CuTeO$_6$

We present single-crystal growth and magnetic property studies of tellurium-bridged copper spin-1/2 system Ba$_2$CuTeO$_6$. The spin-exchange interaction among copper spins via Cu-O-Te-O-Cu super-superexchange route leads to a novel two-leg spin ladder system. Spin susceptibility $χ$(T) data indicates that the triclinic Ba$_2$CuTeO$_6$ undergoes a stepwise crossover for exchange couplings revealed by a broad maximum near T$_{max}$$\sim$75~K and an anisotropic cusp in $\frac{dχ}{dT}$(T) to signify a three dimensional (3D) antiferromagnetic long-range ordering (LRO). The 3D LRO has been suggested from the anisotropic behavior of $χ$(T) with strong c-axis spin anisotropy and the signature of spin flop transition from the isothermal magnetization below $T_N$. Analysis of magnetic heat capacity (Cm) at $T_N$~15 K indicates that most of the spin entropy (~92% ) has already been released above $T_N$, which supports the picture of consecutive spin entropy reduction upon cooling with Te-bridged two-leg spin ladder system with strong intraladder and interladder couplings. Theoretical DFT+U calculations have been performed to search for the ground state magnetic configuration and also to evaluate exchange coupling constants that support the magnetic model deduced from the combined spin susceptibility and crystal structure symmetry analysis.

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Topological phase diagram and saddle point singularity in a tunable topological crystalline insulator

We report the evolution of the surface electronic structure and surface material properties of a topological crystalline insulator (TCI) Pb1-xSnxSe as a function of various material parameters including composition x, temperature T and crystal structure. Our spectroscopic data demonstrate the electronic groundstate condition for the saddle point singularity, the tunability of surface chemical potential, and the surface states' response to circularly polarized light. Our results show that each material parameter can tune the system between trivial and topological phase in a distinct way unlike as seen in Bi2Se3 and related compounds, leading to a rich and unique topological phase diagram. Our systematic studies of the TCI Pb1-xSnxSe are valuable materials guide to realize new topological phenomena.

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Hierarchical spin-orbital polarisation of a giant Rashba system

The Rashba effect is one of the most striking manifestations of spin-orbit coupling in solids, and provides a cornerstone for the burgeoning field of semiconductor spintronics. It is typically assumed to manifest as a momentum-dependent splitting of a single initially spin-degenerate band into two branches with opposite spin polarisation. Here, combining polarisation-dependent and resonant angle-resolved photoemission measurements with density-functional theory calculations, we show that the two "spin-split" branches of the model giant Rashba system BiTeI additionally develop disparate orbital textures, each of which is coupled to a distinct spin configuration. This necessitates a re-interpretation of spin splitting in Rashba-like systems, and opens new possibilities for controlling spin polarisation through the orbital sector.

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Graphene-like conjugated pi-bond system in Pb1-xSnxSe

Following the identification of the pi bond in graphene, in this work, a pi bond constructed through side-to-side overlap of half-filled 6pz orbitals was observed in a non-carbon crystal of Pb1-xSnxSe (x=0.34) (PSS), a prototype topological crystalline insulator (TCI) and thermoelectric material with a high figure-of-merit (ZT). PSS compounds with a rock-salt type cubic crystal structure was found to consist of sigma bond connected covalent chains of Pb(Sn)-Se with an additional pi bond that is shared as a conjugated system among the four nearest neighbor Pb pairs in square symmetry within all (001) monoatomic layers per cubic unit cell. The pi bond formed with half-filled 6pz orbitals between Pb atoms is consistent with the calculated results from quantum chemistry. The presence of pi bonds was identified and verified with electron energy-loss spectroscopy (EELS) through plasmonic excitations and electron density (ED) mapping via an inverse Fourier transform of X-ray diffraction.

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Lifshitz transition and van Hove singularity in a Topological Dirac Semimetal

A topological Dirac semimetal is a novel state of quantum matter which has recently attracted much attention as an apparent 3D version of graphene. In this paper, we report critically important results on the electronic structure of the 3D Dirac semimetal Na3Bi at a surface that reveals its nontrivial groundstate. Our studies, for the first time, reveal that the two 3D Dirac cones go through a topological change in the constant energy contour as a function of the binding energy, featuring a Lifshitz point, which is missing in a strict 3D analog of graphene (in other words Na3Bi is not a true 3D analog of graphene). Our results identify the first example of a band saddle point singularity in 3D Dirac materials. This is in contrast to its 2D analogs such as graphene and the helical Dirac surface states of a topological insulator. The observation of multiple Dirac nodes in Na3Bi connecting via a Lifshitz point along its crystalline rotational axis away from the Kramers point serves as a decisive signature for the symmetry-protected nature of the Dirac semimetal's topological groundstate.

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Observation of a topological 3D Dirac semimetal phase in high-mobility Cd3As2

Experimental identification of three-dimensional (3D) Dirac semimetals in solid state systems is critical for realizing exotic topological phenomena and quantum transport such as the Weyl phases, high temperature linear quantum magnetoresistance and topological magnetic phases. Using high resolution angle-resolved photoemission spectroscopy, we performed systematic electronic structure studies on well-known compound Cd3As2. For the first time, we observe a highly linear bulk Dirac cone located at the Brillouin zone center projected onto the (001) surface which is consistent with a 3D Dirac semimetal phase in Cd3As2. Remarkably, an unusually high Dirac Fermion velocity up to 10.2 \textrmÅ{\cdot}$eV (1.5 \times 10^{6} ms^-1) is seen in samples where the mobility far exceeds 40,000 cm^2/V.s suggesting that Cd3As2 can be a promising candidate as a hypercone analog of graphene in many device-applications which can also incorporate topological quantum phenomena in a large gap setting. Our experimental identification of this novel topological 3D Dirac semimetal phase, distinct from a 3D topological insulator phase discovered previously, paves the way for exploring higher dimensional relativistic physics in bulk transport and for realizing novel Fermionic matter such as a Fermi arc nodal metal.

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Antiferromagnetism of Ni2NbBO6 with S = 1 dimer quasi-one-dimensional armchair chains

Long range antiferromagnetic (AFM) ordering of Ni spins in Ni2NbBO6 has been studied with single crystal from spin susceptibility measurement and comparedwith the ab initio calculation results consistently. Below TN = 23.5 K, the S = 1 spins align along the a direction for edge-shared NiO6 octahedra which form crystallographic armchair chains along the b direction. The isothermal magnetization M(H) below TN shows spin-flop transition for magnetic field above 36 kOe along the a axis,which indicates the spin anisotropy is along the a direction. The electronic and magnetic structures of Ni2NbBO6 have also been explored theoretically using density functional theory with generalized gradient approximation plus on-site Coulomb interaction (U). These calculations support the experimentally observed antiferromagnetism of Ni2NbBO6. In particular, the long range AFM ordering below TN can be dissected into armchair chains which consists of S = 1 dimers of J2 = 2.43 meV with ferromagnetic (FM) intrachain and interchain couplings of size half |J2|.

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Strain engineering Dirac surface states in heteroepitaxial topological crystalline insulator thin films

In newly discovered topological crystalline insulators (TCIs), the unique crystalline protection of the surface state (SS) band structure has led to a series of intriguing predictions of strain generated phenomena, from the appearance of pseudo-magnetic fields and helical flat bands, to the tunability of the Dirac SS by strain that may be used to construct "straintronic" nanoswitches. However, practical realization of this exotic phenomenology via strain engineering is experimentally challenging and is yet to be achieved. In this work, we have designed an experiment to not only generate and measure strain locally, but to also directly measure the resulting effects on the Dirac SS. We grow heteroepitaxial thin films of TCI SnTe in-situ and measure them by using high-resolution scanning tunneling microscopy (STM). Large STM images were analyzed to determine picoscale changes in the atomic positions which reveal regions of both tensile and compressive strain. Simultaneous Fourier-transform STM was then used to determine the effects of strain on the Dirac electrons. We find that strain continuously tunes the momentum space position of the Dirac points, consistent with theoretical predictions. Our work demonstrates the fundamental mechanism necessary for using TCIs in strain-based applications, and establishes these systems as highly tunable platforms for nanodevices.

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Two-step antiferromagnetic transition and moderate triangular frustration in Li2Co(WO4)2

We present a detailed investigation of the magnetic properties of the spin-$\frac{3}{2}$ system Li$_2$Co(WO$_4$)$_2$ by means of magnetic susceptibility and specific heat. Our experimental results show that in Li$_2$Co(WO$_4$)$_2$ a short-range antiferromagnetic (AFM) correlations appear near $χ$$_{max}$ $\sim$ 11 K and two successive long-range AFM phase transitions are observed at T$_{N1}$$\sim$ 9 K and T$_{N2}$$\sim$ 7 K. The frustration factor, $\mid$$Θ$$\mid$/T$_{N1}$$\sim$3, indicates that the system is moderately frustrated, which is identifiable by the broken triangular symmetry within both $ab$- and $bc$-planes for the triclinic crystal structure. The magnetic isotherm at temperatures below T$_{N2}$ shows a field-induced spin-flop transition, and a complete H-T phase diagram for the two-step AFM system is mapped. $Ab$~$initio$ band structure calculations suggest that the strongest exchange coupling does not correspond to the shortest Co-Co distance along the $a$-axis, but rather along the diagonal direction through a Co-O-W-O-Co super-superexchange path within the $bc$-plane

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Dirac mass generation from crystal symmetry breaking on the surfaces of topological crystalline insulators

The tunability of topological surface states (SS) and controllable opening of the Dirac gap are of fundamental and practical interest in the field of topological materials. In topological crystalline insulators (TCIs), a spontaneously generated Dirac gap was recently observed, which was ascribed to broken cubic crystal symmetry. However, this structural distortion has not been directly observed so far, and the microscopic mechanism of Dirac gap opening via crystal symmetry breaking remains elusive. In this work, we present scanning tunneling microscopy (STM) measurements of a TCI Pb$_{1-x}$Sn$_x$Se for a wide range of alloy compositions spanning the topological and non-topological regimes. STM topographies directly reveal a symmetry-breaking distortion on the surface, which imparts mass to the otherwise massless Dirac electrons - a mechanism analogous to the long sought-after Higgs mechanism in particle physics. Remarkably, our measurements show that the Dirac gap scales with alloy composition, while the magnitude of the distortion remains nearly constant. Based on theoretical calculations, we find the Dirac mass is controlled by the composition-dependent SS penetration depth, which determines the weight of SS in the distorted region that is confined to the surface. Finally, we discover the existence of SS in the non-topological regime, which have the characteristics of gapped, double-branched Dirac fermions.

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Enhanced quasiparticle dynamics of quantum well states: the giant Rashba system BiTeI and topological insulators

In the giant Rashba semiconductor BiTeI electronic surface scattering with Lorentzian linewidth is observed that shows a strong dependence on surface termination and surface potential shifts. A comparison with the topological insulator Bi2Se3 evidences that surface confined quantum well states are the origin of these processes. We notice an enhanced quasiparticle dynamics of these states with scattering rates that are comparable to polaronic systems in the collision dominated regime. The Eg symmetry of the Lorentzian scattering contribution is different from the chiral (RL) symmetry of the corresponding signal in the topological insulator although both systems have spin-split surface states.

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Saddle point singularity and topological phase diagram in a tunable topological crystalline insulator (TCI)

A topological crystalline insulator (TCI) is a new phase of topological matter, which is predicted to exhibit distinct topological quantum phenomena, since space group symmetries replace the role of time-reversal symmetry in the much-studied Z$_2$ topological insulators. Utilizing high-resolution angle-resolved photoemission spectroscopy (ARPES), we reveal the momentum space nature of interconnectivity of the Fermi surface pockets leading to a saddle point singularity within the topological surface state alone in the TCI Pb$_{0.7}$Sn$_{0.3}$Se. Moreover, we show that the measured momentum-integrated density of states exhibits pronounced peaks at the saddle point energies, demonstrating the van Hove singularities (VHSs) in the topological surface states, whose surface chemical potential, as we show, can be tuned via surface chemical gating, providing access to the topological correlated physics on the surface. Our experimental data reveal a delicate relationship among lattice constant, band gap and spin-orbit coupling strength associated with the topological phase transition in Pb$_{1-x}$Sn$_{x}$Se. Furthermore, we explore the robustness of the TCI phase with VHS in Pb$_{1-x}$Sn$_{x}$Se, which shows a variety of distinct topological phase transitions driven by either thermal instability or broken crystalline symmetry, and thus revealing a rich topological phase diagram connectivity in Pb$_{1-x}$Sn$_{x}$Se for the first time.

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Observation of a bulk 3D Dirac multiplet, Lifshitz transition, and nestled spin states in Na3Bi

Symmetry or topology protected Dirac fermion states in two and three dimensions constitute novel quantum systems that exhibit exotic physical phenomena. However, none of the studied spin-orbit materials are suitable for realizing bulk multiplet Dirac states for the exploration of interacting Dirac physics. Here we present experimental evidence, for the first time, that the compound Na3Bi hosts a bulk spin-orbit Dirac multiplet and their interaction or overlap leads to a Lifshitz transition in momentum space - a condition for realizing interactions involving Dirac states. By carefully preparing the samples at a non-natural-cleavage (100) crystalline surface, we uncover many novel electronic and spin properties in Na3Bi by utilizing high resolution angle- and spin-resolved photoemission spectroscopy measurements. We observe two bulk 3D Dirac nodes that locate on the opposite sides of the bulk zone center point $Γ$, which exhibit a Fermi surface Lifshitz transition and a saddle point singularity. Furthermore, our data shows evidence for the possible existence of theoretically predicted weak 2D nontrivial spin-orbit surface state with helical spin polarization that are nestled between the two bulk Dirac cones, consistent with the theoretically calculated (100) surface-arc-modes. Our main experimental observation of a rich multiplet of Dirac structure and the Lifshitz transition opens the door for inducing electronic instabilities and correlated physical phenomena in Na3Bi, and paves the way for the engineering of novel topological states using Na3Bi predicted in recent theory.

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Mapping the unconventional orbital texture in topological crystalline insulators

The newly discovered topological crystalline insulators (TCIs) harbor a complex band structure involving multiple Dirac cones. These materials are potentially highly tunable by external electric field, temperature or strain and could find future applications in field-effect transistors, photodetectors, and nano-mechanical systems. Theoretically, it has been predicted that different Dirac cones, offset in energy and momentum-space, might harbor vastly different orbital character, a unique property which if experimentally realized, would present an ideal platform for accomplishing new spintronic devices. However, the orbital texture of the Dirac cones, which is of immense importance in determining a variety of materials properties, still remains elusive in TCIs. Here, we unveil the orbital texture in a prototypical TCI Pb$_{1-x}$Sn$_x$Se. By using Fourier-transform (FT) scanning tunneling spectroscopy (STS) we measure the interference patterns produced by the scattering of surface state electrons. We discover that the intensity and energy dependences of FTs show distinct characteristics, which can directly be attributed to orbital effects. Our experiments reveal the complex band topology involving two Lifshitz transitions and establish the orbital nature of the Dirac bands in this new class of topological materials, which could provide a different pathway towards future quantum applications.

cond-mat.str-el↗

Observation of Dirac node formation and mass acquisition in a topological crystalline insulator

In the recently discovered topological crystalline insulators (TCIs), topology and crystal symmetry intertwine to create surface states with a unique set of characteristics. Among the theoretical predictions for TCIs is the possibility of imparting mass to the massless Dirac fermions by breaking crystal symmetry, as well as a Lifshitz transition with a change of Fermi surface topology. Here we report high resolution scanning tunneling microscopy studies of a TCI, Pb1-xSnxSe. We demonstrate the formation of zero mass Dirac fermions protected by crystal symmetry and the mechanism of mass generation via symmetry breaking, which constitute the defining characteristics of TCIs. In addition, we show two distinct regimes of fermiology separated by a Van-Hove singularity at the Lifshitz transition point. Our work paves the way for engineering the Dirac band gap and realizing interaction-driven topological quantum phenomena in TCIs.

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Anomalous behavior in the phonon dispersion of the (001) surface of Bi$_2$Te$_3$ determined from helium atom-surface scattering measurements

We employ inelastic helium atom-surface scattering to measure the low energy phonon dispersion along high-symmetry directions on the surface of the topological insulator Bi$_2$Te$_3$. Results indicate that one particular low-frequency branch experiences noticeable mode softening attributable to the interaction between Dirac fermion quasiparticles and phonons on the surface. This mode softening constitutes a renormalization of the real part of the phonon self-energy. We obtain the imaginary part, and hence lifetime information, via a Hilbert transform. In doing so we are able to calculate an average branch specific electron-phonon coupling constant $<λ_ν> = 1.44$.

cond-mat.mtrl-sci↗