Fangcheng Chou

Observation of a three-dimensional topological Dirac semimetal phase in high-mobility Cd3As2

Symmetry-broken three-dimensional (3D) topological Dirac semimetal systems with strong spin-orbit coupling can host many exotic Hall-like phenomena and Weyl fermion quantum transport. Here, using high-resolution angle-resolved photoemission spectroscopy, we performed systematic electronic structure studies on Cd3As2, which has been predicted to be the parent material, from which many unusual topological phases can be derived. We observe a highly linear bulk band crossing to form a 3D dispersive Dirac cone projected at the Brillouin zone centre by studying the (001)-cleaved surface. Remarkably, an unusually high in-plane Fermi velocity up to 1.5×10(6) ms(-1) is observed in our samples, where the mobility is known up to 40,000 cm2 V(-1) s(-1), suggesting that Cd3As2 can be a promising candidate as an anisotropic-hypercone (three-dimensional) high spin-orbit analogue of 3D graphene. Our discovery of the Dirac-like bulk topological semimetal phase in Cd3As2 opens the door for exploring higher dimensional spin-orbit Dirac physics in a real material.Understanding the spin-texture behavior of boundary modes in ultrathin topological insulator films is critically essential for the design and fabrication of functional nanodevices. Here by using spin-resolved photoemission spectroscopy with p-polarized light in topological insulator Bi2Se3 thin films, we report tunneling-dependent evolution of spin configuration in topological insulator thin films across the metal-toinsulator transition. We observe strongly binding energyand wavevector-dependent spin polarization for the topological surface electrons in the ultra-thin gapped-Diraccone limit. The polarization decreases significantly with enhanced tunneling realized systematically in thin insulating films, whereas magnitude of the polarization saturates to the bulk limit faster at larger wavevectors in thicker metallic films. We present a theoretical model which captures this delicate relationship between quantum tunneling and Fermi surface spin polarization. Our high-resolution spin-based spectroscopic results suggest that the polarization current can be tuned to zero in thin insulating films forming the basis for a future spin-switch nano-device.

Observation of a topological crystalline insulator phase and topological phase transition in Pb 1− x Sn x Te

A topological insulator protected by time-reversal symmetry is realized via spinorbit interaction driven band inversion. The topological phase in the Bi1−xSbx system is due to an odd number of band inversions. A related spin-orbit system, the Pb1−xSnxTe, has long been known to contain an even number of inversions based on band theory. Here we experimentally investigate the possibility of a mirror symmetry protected topological crystalline insulator phase in the Pb1−xSnxTe class of materials which has been theoretically predicted to exist in its end compound SnTe. Our experimental results show that at a finite-Pb composition above the topological inversion phase transition, the surface exhibits even number of spin-polarized Dirac cone states revealing mirror-protected topological order distinct from that observed in Bi1−xSbx. Our observation of the spin-polarized Dirac surface states in the inverted Pb1−xSnxTe and their absence in the non-inverted compounds related via a topological phase transition provide the experimental groundwork for opening the research on novel topological order in quantum devices.A topological insulator protected by time-reversal symmetry is realized via spin-orbit interaction-driven band inversion. The topological phase in the Bi(1-x)Sb(x) system is due to an odd number of band inversions. A related spin-orbit system, the Pb(1-x)Sn(x)Te, has long been known to contain an even number of inversions based on band theory. Here we experimentally investigate the possibility of a mirror symmetry-protected topological crystalline insulator phase in the Pb(1-x)Sn(x)Te class of materials that has been theoretically predicted to exist in its end compound SnTe. Our experimental results show that at a finite Pb composition above the topological inversion phase transition, the surface exhibits even number of spin-polarized Dirac cone states revealing mirror-protected topological order distinct from that observed in Bi(1-x)Sb(x). Our observation of the spin-polarized Dirac surface states in the inverted Pb(1-x)Sn(x)Te and their absence in the non-inverted compounds related via a topological phase transition provide the experimental groundwork for opening the research on novel topological order in quantum devices.

Topological nodal-line fermions in spin-orbit metal PbTaSe2

Topological semimetals can support one-dimensional Fermi lines or zero-dimensional Weyl points in momentum space, where the valence and conduction bands touch. While the degeneracy points in Weyl semimetals are robust against any perturbation that preserves translational symmetry, nodal lines require protection by additional crystalline symmetries such as mirror reflection. Here we report, based on a systematic theoretical study and a detailed experimental characterization, the existence of topological nodal-line states in the non-centrosymmetric compound PbTaSe2 with strong spin-orbit coupling. Remarkably, the spin-orbit nodal lines in PbTaSe2 are not only protected by the reflection symmetry but also characterized by an integer topological invariant. Our detailed angle-resolved photoemission measurements, first-principles simulations and theoretical topological analysis illustrate the physical mechanism underlying the formation of the topological nodal-line states and associated surface states for the first time, thus paving the way towards exploring the exotic properties of the topological nodal-line fermions in condensed matter systems.

Observation of Dirac Node Formation and Mass Acquisition in a Topological Crystalline Insulator

Half-Massless Certain materials, such as topological crystalline insulators (TCIs), host robust surface states that have a Dirac (graphene-like) dispersion associated with massless carriers; the breaking of protective symmetry within such materials should cause the carriers to acquire mass. Okada et al. (p. 1496, published online 29 August) used scanning tunneling microscopy to map out the energies of the electronic levels of the TCI Pb1-xSnxSe as a function of the strength of an external magnetic field. The massless Dirac fermions coexisted with massive ones, presumably as a consequence of a distortion of the crystalline structure affecting only one of the two mirror symmetries. Scanning tunneling spectroscopy of Pb1–xSnxSe in a magnetic field reveals two types of Dirac fermions. In topological crystalline insulators (TCIs), topology and crystal symmetry intertwine to create surface states with distinct characteristics. The breaking of crystal symmetry in TCIs is predicted to impart mass to the massless Dirac fermions. Here, we report high-resolution scanning tunneling microscopy studies of a TCI, Pb1-xSnxSe that reveal the coexistence of zero-mass Dirac fermions protected by crystal symmetry with massive Dirac fermions consistent with crystal symmetry breaking. In addition, we show two distinct regimes of the Fermi surface topology 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.

Phase Transformation and Lithiation Effect on Electronic Structure of LixFePO4: An In-Depth Study by Soft X-ray and Simulations

Through soft X-ray absorption spectroscopy, hard X-ray Raman scattering, and theoretical simulations, we provide the most in-depth and systematic study of the phase transformation and (de)lithiation effect on electronic structure in Li(x)FePO(4) nanoparticles and single crystals. Soft X-ray reveals directly the valence states of Fe 3d electrons in the vicinity of Fermi level, which is sensitive to the local lattice distortion, but more importantly offers detailed information on the evolution of electronic states at different electrochemical stages. The soft X-ray spectra of Li(x)FePO(4) nanoparticles evolve vividly with the (de)lithiation level. The spectra fingerprint the (de)lithiation process with rich information on Li distribution, valency, spin states, and crystal field. The high-resolution spectra reveal a subtle but critical deviation from two-phase transformation in our electrochemically prepared samples. In addition, we performed both first-principles calculations and multiplet simulations of the spectra and quantitatively determined the 3d valence states that are completely redistributed through (de)lithiation. This electronic reconfiguration was further verified by the polarization-dependent spectra collected on LiFePO(4) single crystals, especially along the lithium diffusion direction. The evolution of the 3d states is overall consistent with the local lattice distortion and provides a fundamental picture of the (de)lithiation effects on electronic structure in the Li(x)FePO(4) system.

Observation of topological nodal fermion semimetal phase in ZrSiS

The search for new topological phases of matter is a major new direction in condensed matter physics. Recent experimental realizations of Dirac and Weyl semimetal phases pave the way to look for other exotic phases of matter in real materials. In this paper, the authors present a systematic angle-resolved photoemission spectroscopy study of ZrSiS, a potential topological nodal semimetal candidate. Their systematic measurements establish the spinless nodal fermion semimetal phase in ZrSiS, which is supported by their first-principles calculations. This work puts forward the ZrSiS-type material family as a new platform to explore exotic states of quantum matter.

Experimental discovery of a topological Weyl semimetal state in TaP

Photoemission established tantalum phosphide as a Weyl semimetal, which hosts exotic Weyl fermion quasiparticles and Fermi arcs. Weyl semimetals are expected to open up new horizons in physics and materials science because they provide the first realization of Weyl fermions and exhibit protected Fermi arc surface states. However, they had been found to be extremely rare in nature. Recently, a family of compounds, consisting of tantalum arsenide, tantalum phosphide (TaP), niobium arsenide, and niobium phosphide, was predicted as a Weyl semimetal candidates. We experimentally realize a Weyl semimetal state in TaP. Using photoemission spectroscopy, we directly observe the Weyl fermion cones and nodes in the bulk, and the Fermi arcs on the surface. Moreover, we find that the surface states show an unexpectedly rich structure, including both topological Fermi arcs and several topologically trivial closed contours in the vicinity of the Weyl points, which provides a promising platform to study the interplay between topological and trivial surface states on a Weyl semimetal’s surface. We directly demonstrate the bulk-boundary correspondence and establish the topologically nontrivial nature of the Weyl semimetal state in TaP, by resolving the net number of chiral edge modes on a closed path that encloses the Weyl node. This also provides, for the first time, an experimentally practical approach to demonstrating a bulk Weyl fermion from a surface state dispersion measured in photoemission.

Intermixing-seeded growth for high-performance planar heterojunction perovskite solar cells assisted by precursor-capped nanoparticles

This work proposes a novel approach to modulate the nucleation and growth of perovskite crystals in planar perovskite (CH3NH3PbI3−xClx) solar cells by intermixing precursor-capped inorganic nanoparticles of PbS. A small amount of dispersed PbS nanoparticles which were covered with perovskite precursor molecules of methylammonium iodide (CH3NH3I, MAI) through the ligand-exchange treatment functioned as effective seed-like nucleation sites to promote the formation of perovskite lattice structures. Through this intermixing-seeded growth technique, substantial morphological improvements, such as increased crystal domains, enhanced coverage, and uniformity, were realized in the perovskite thin films, and the corresponding solar cell devices exhibited a promising power conversion efficiency of 17.4%, showing an enhancement of approximately 25% compared to that of the controlled pristine solar cell device. The substantially enhanced crystal orientation, particularly along the direction perpendicular to the substrate, was evident from the synchrotron-based grazing incidence wide-angle X-ray scattering data. This observation was consistent with the enhanced carrier diffusion lengths and excellent reproducibility of high fill factors of the planar heterojunction perovskite devices fabricated through the proposed technique.

Observation of monolayer valence band spin-orbit effect and induced quantum well states in MoX2

Transition metal dichalcogenides [corrected] have attracted much attention recently due to their potential applications in spintronics and photonics because of the indirect to direct band gap transition and the emergence of the spin-valley coupling phenomenon upon moving from the bulk to monolayer limit. Here, we report high-resolution angle-resolved photoemission spectroscopy on MoSe2 single crystals and monolayer films of MoS2 grown on highly ordered pyrolytic graphite substrate. Our experimental results resolve the Fermi surface trigonal warping of bulk MoSe2, and provide evidence for the critically important spin-orbit split valence bands of monolayer MoS2. Moreover, we systematically image the formation of quantum well states on the surfaces of these materials, and present a theoretical model to account for these experimental observations. Our findings provide important insights into future applications of transition metal dichalcogenides in nanoelectronics, spintronics and photonics devices as they critically depend on the spin-orbit physics of these materials.

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

The tunability of topological surface states and controllable opening of the Dirac gap are of fundamental and practical interest in the field of topological materials. In the newly discovered topological crystalline insulators (TCIs), theory predicts that the Dirac node is protected by a crystalline symmetry and that the surface state electrons can acquire a mass if this symmetry is broken. Recent studies have detected signatures of a spontaneously generated Dirac gap in TCIs; however, the mechanism of mass formation remains elusive. In this work, we present scanning tunnelling microscopy (STM) measurements of the TCI Pb1-xSnxSe for a wide range of alloy compositions spanning the topological and non-topological regimes. The STM topographies 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. Interestingly, the measured Dirac gap decreases on approaching the trivial phase, whereas the magnitude of the distortion remains nearly constant. Our data and calculations reveal that the penetration depth of Dirac surface states controls the magnitude of the Dirac mass. At the limit of the critical composition, the penetration depth is predicted to go to infinity, resulting in zero mass, consistent with our measurements. Finally, we discover the existence of surface states in the non-topological regime, which have the characteristics of gapped, double-branched Dirac fermions and could be exploited in realizing superconductivity in these materials.