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D. Qian

Publications and source records attributed to D. Qian.

At least 37 records · Page 2Linked to original sources

Discovery (theoretical prediction and experimental observation) of a large-gap topological-insulator class with spin-polarized single-Dirac-cone on the surface

Recent theories and experiments have suggested that strong spin-orbit coupling effects in certain band insulators can give rise to a new phase of quantum matter, the so-called topological insulator, which can show macroscopic entanglement effects. Such systems feature two-dimensional surface states whose electrodynamic properties are described not by the conventional Maxwell equations but rather by an attached axion field, originally proposed to describe strongly interacting particles. It has been proposed that a topological insulator with a single spin-textured Dirac cone interfaced with a superconductor can form the most elementary unit for performing fault-tolerant quantum computation. Here we present an angle-resolved photoemission spectroscopy study and first-principle theoretical calculation-predictions that reveal the first observation of such a topological state of matter featuring a single-surface-Dirac-cone realized in the naturally occurring Bi$_2$Se$_3$ class of materials. Our results, supported by our theoretical predictions and calculations, demonstrate that undoped compound of this class of materials can serve as the parent matrix compound for the long-sought topological device where in-plane surface carrier transport would have a purely quantum topological origin. Our study further suggests that the undoped compound reached via n-to-p doping should show topological transport phenomena even at room temperature.

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Topological Control: Systematic control of topological insulator Dirac fermion density on the surface of Bi2Te3

Three dimensional (3D) topological insulators are quantum materials with a spin-orbit induced bulk insulating gap that exhibit quantum-Hall-like phenomena in the absence of applied magnetic fields. The proposed applications of topological insulators in device geometries rely on the ability to tune the chemical potential on their surfaces in the vicinity of the Dirac node. Here, we demonstrate a suite of surface control methods based on a combination of photo-doping and molecular-doping to systematically tune the Dirac fermion density on the topological (111) surface of Bi2Te3. Their efficacy is demonstrated via direct electronic structure topology measurements using high resolution angle-resolved photoemission spectroscopy (ARPES). These results open up new opportunities for probing topological behavior of Dirac electrons on the Bi2Te3 surface. At least one of the methods demonstrated here can be successfully applied to other topological insulators such as the Bi{1-x}Sb{x}, Sb2Te3 and Bi2Se3 which will be shown elsewhere. More importantly, our methods of topological surface state manipulation demonstrated here are highly suitable for future spectroscopic studies of topological phenomena which will complement the transport results gained from the traditional electrical gating techniques.

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First observation of spin-helical Dirac fermions and topological phases in undoped and doped Bi2Te3 demonstrated by spin-ARPES spectroscopy

Electron systems that possess light-like dispersion relations or the conical Dirac spectrum, such as graphene and bismuth, have recently been shown to harbor unusual collective states in high magnetic fields. Such states are possible because their light-like electrons come in spin pairs that are chiral,which means that their direction of propagation is tied to a quantity called pseudospin that describes their location in the crystal lattice. An emerging direction in quantum materials research is the manipulation of atomic spin-orbit coupling to simulate the effect of a spin dependent magnetic field,in attempt to realize novel spin phases of matter. This effect has been proposed to realize systems consisting of unpaired Dirac cones that are helical, meaning their direction of propagation is tied to the electron spin itself, which are forbidden to exist in graphene or bismuth. The experimental existence of topological order can not be determined without spin-resolved measurements. Here we report a spin-and angle-resolved photoemission study of the hexagonal surface of the Bi2Te3 and Bi{2-x}MnxTe3 series, which is found to exhibit a single helical Dirac cone that is fully spin-polarized. Our observations of a gap in the bulk spin-degenerate band and a spin-resolved surface Dirac node close to the chemical potential show that the low energy dynamics of Bi2Te3 is dominated by the unpaired spin-helical Dirac modes. Our spin-texture measurements prove the existence of a rare topological phase in this materials class for the first time, and suggest its suitability for novel 2D Dirac spin device applications beyond the chiral variety or traditional graphene.

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First direct observation of Spin-textures in Topological Insulators : Spin-resolved ARPES as a probe of topological quantum spin Hall effect and Berry's phase

A topologically ordered material is characterized by a rare quantum organization of electrons that evades the conventional spontaneously broken symmetry based classification of condensed matter. Exotic spin transport phenomena such as the dissipationless quantum spin Hall effect have been speculated to originate from a novel topological order whose identification requires a spin sensitive measurement, which does not exist to this date in any system (neither in Hg(Cd)Te quantum wells nor in the topological insulator BiSb). Using Mott polarimetry, we probe the spin degrees of freedom of these quantum spin Hall states and demonstrate that topological quantum numbers are uniquely determined from spin texture imaging measurements. Applying this method to the Bi{1-x}Sb{x} series, we identify the origin of its novel order and unusual chiral properties. These results taken together constitute the first observation of surface electrons collectively carrying a geometrical quantum (Berry's) phase and definite chirality (mirror Chern number, n_M =-1), which are the key electronic properties for realizing topological computing bits with intrinsic spin Hall-like topological phenomena. Our spin-resolved results not only provides the first clear proof of a topological insulating state in nature but also demonstrate the utility of spin-resolved ARPES technique in measuring the quantum spin Hall phases of matter.

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A topological Dirac insulator in a quantum spin Hall phase : Experimental observation of first strong topological insulator

When electrons are subject to a large external magnetic field, the conventional charge quantum Hall effect \cite{Klitzing,Tsui} dictates that an electronic excitation gap is generated in the sample bulk, but metallic conduction is permitted at the boundary. Recent theoretical models suggest that certain bulk insulators with large spin-orbit interactions may also naturally support conducting topological boundary states in the extreme quantum limit, which opens up the possibility for studying unusual quantum Hall-like phenomena in zero external magnetic field. Bulk Bi$_{1-x}$Sb$_x$ single crystals are expected to be prime candidates for one such unusual Hall phase of matter known as the topological insulator. The hallmark of a topological insulator is the existence of metallic surface states that are higher dimensional analogues of the edge states that characterize a spin Hall insulator. In addition to its interesting boundary states, the bulk of Bi$_{1-x}$Sb$_x$ is predicted to exhibit three-dimensional Dirac particles, another topic of heightened current interest. Here, using incident-photon-energy-modulated (IPEM-ARPES), we report the first direct observation of massive Dirac particles in the bulk of Bi$_{0.9}$Sb$_{0.1}$, locate the Kramers' points at the sample's boundary and provide a comprehensive mapping of the topological Dirac insulator's gapless surface modes. These findings taken together suggest that the observed surface state on the boundary of the bulk insulator is a realization of the much sought exotic "topological metal". They also suggest that this material has potential application in developing next-generation quantum computing devices.

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Fermi surface topology and low-lying quasiparticle structure of magnetically ordered Fe1+xTe

We report the first photoemission study of Fe1+xTe - the host compound of the newly discovered iron-chalcogenide superconductors. Our results reveal a pair of nearly electron- hole compensated Fermi pockets, strong Fermi velocity renormalization and an absence of a spin-density-wave gap. A shadow hole pocket is observed at the "X"-point of the Brillouin zone which is consistent with a long-range ordered magneto-structural groundstate. No signature of Fermi surface nesting instability associated with Q= pi(1/2, 1/2) is observed. Our results collectively reveal that the Fe1+xTe series is dramatically different from the undoped phases of the high Tc pnictides and likely harbor unusual mechanism for superconductivity and quantum magnetic order.

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Experimental determination of the microscopic origin of magnetism in parent iron pnictides

Like high Tc cuprates, the newly discovered iron based superconductors lie in close proximity to a magnetically ordered parent phase. However, while the magnetic order in parent cuprates is known to derive from a spin-spin local superexchange interaction, a plethora of experiments including neutron scattering have so far been unable to conclusively resolve whether a local moment Heisenberg description applies in parent iron based compounds, or whether magnetism arises from a collective SDW order instability. These two alternatives can in principle be distinguished by measuring the low energy momentum-resolved bulk-representative electronic structure of the magnetically ordered phase. Using a combination of polarization dependent ARPES and STM, we have isolated the complete low-lying bulk representative electronic structure of magnetic SrFe2As2 with d-orbital symmetry specificity for the first time. Our results show that while multiple bands with different iron d-orbital character indeed contribute to charge transport, only one pair of bands with opposite mirror symmetries microscopically exhibit an itinerant SDW instability with energy scales on the order of 50 meV. The orbital resolved band topology below T_SDW point uniquely to a nesting driven band hybridization mechanism of the observed antiferromagnetism in the iron pnictides, and is consistent with an unusual anisotropic nodal-density-wave state. In addition, these results place strong constraints on many theories of pnictide superconductivity that require a strict local moment magnetism starting point.

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Electrons on the surface of Bi2Se3 form a topologically-ordered two dimensional gas with a non-trivial Berry's phase

The interface between a superconductor and a topological insulator has been proposed to harbor novel quasiparticles that realize physical schemes for fault-tolerant quantum computation. Here, we present high resolution angle-resolved photoemission experimental results, which along with first principles calculations, suggest that the surface-edge states of Bi2Se3 form a topological 2D metal. When magnetic atoms are deposited, the surface tends to lose Kramers' degeneracy and a k-space connection thread between the bulk valence and conduction bands is lost. Our observed states carry a πBerry's phase suggesting that although the real materials are often electron doped fully undoped Bi2Se3 would be a Z2 topological insulator at room temperature.

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Tightly-bound Cooper pair, quasiparticle kinks and clues on the pairing potential in a high Tc FeAs Superconductor

We present a systematic photoemission study of the newly discovered high Tc superconductor class (Sr/Ba)1-xKxFe2As2. By utilizing a unique photon energy range and scattering geometry we resolve the details of the single particle dynamics of interacting electrons on the central Fermi surfaces of this series which shows overall strong coupling behavior (2D/kBTc = 6). Quasiparticle dispersion kinks are observed in a binding energy range of 15 to 50 meV which matches the magnetic excitation energy scales (parameterized by J1,J2). The size of the Cooper pair wavefunction is found to be less than 20A indicating a short in-plane scale uncharacteristic of a BCS-phonon scenario but suggestive of a phase factor in the global order parameter. The kink likely reflects contributions from the strongly frustrated fluctuating spin excitations and the soft phonons around 20-40 meV. Our results provide important clue to the nature of the pairing potential realized in these superconductors.

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Anomalous metallic state of Cu$_{0.07}$TiSe$_2$: an optical spectroscopy study

We report an optical spectroscopy study on the newly discovered superconductor Cu$_{0.07}$TiSe$_2$. Consistent with the development from a semimetal or semiconductor with a very small indirect energy gap upon doping TiSe$_2$, it is found that the compound has a low carrier density. Most remarkably, the study reveals a substantial shift of the "screened" plasma edge in reflectance towards high energy with decreasing temperature. This phenomenon, rarely seen in metals, indicates either a sizeable increase of the conducting carrier concentration or/and a decrease of the effective mass of carriers with reducing temperature. We attribute the shift primarily to the later effect.

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Anisotropic softening of collective charge modes in the vicinity of critical doping in a doped Mott insulator

Momentum resolved inelastic resonant x-ray scattering is used to map the evolution of charge excitations over a large range of energies, momenta and doping levels in the electron doped Mott insulator class Nd$_{2-x}$Ce$_x$CuO$_4$. As the doping induced AFM-SC (antiferromagnetic-superconducting) transition is approached, we observe an anisotropic softening of collective charge modes over a large energy scale along the Gamma to (π,π)-direction, whereas the modes exhibit broadening ($\sim$ 1 eV) with relatively little softening along Gamma to (π,0) with respect to the parent Mott insulator (x=0). Our study indicates a systematic collapse of the gap consistent with the scenario that the system dopes uniformly with electrons even though the softening of the modes involves an unusually large energy scale.

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Semimetal to semimetal charge density wave transition in 1T-TiSe$_2$

We report an infrared study on 1$T$-TiSe$_2$, the parent compound of the newly discovered superconductor Cu$_x$TiSe$_2$. Previous studies of this compound have not conclusively resolved whether it is a semimetal or a semiconductor: information that is important in determining the origin of its unconventional CDW transition. Here we present optical spectroscopy results that clearly reveal that the compound is metallic in both the high-temperature normal phase and the low-temperature CDW phase. The carrier scattering rate is dramatically different in the normal and CDW phases and the carrier density is found to change with temperature. We conclude that the observed properties can be explained within the scenario of an Overhauser-type CDW mechanism.

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Charge collective modes in an incommensurately modulated cuprate

We report the first measurement of collective charge modes of insulating Sr14Cu24O41 using inelastic resonant x-ray scattering over the complete Brillouin zone. Our results show that the intense excitation modes at the charge gap edge predominantly originate from the ladder-containing planar substructures. The observed ladder modes (E vs. Q) are found to be dispersive for momentum transfers along the "legs" but nearly localized along the "rungs". Dispersion and peakwidth characteristics are similar to the charge spectrum of 1D Mott insulators, and we show that our results can be understood in the strong coupling limit (U >> t_{ladder}> t_{chain}). The observed behavior is in marked contrast to the charge spectrum seen in most two dimensional cuprates. Quite generally, our results also show that momentum-tunability of inelastic scattering can be used to resolve mode contributions in multi-component incommensurate systems.

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Emergence of Fermi pockets in an excitonic CDW melted novel superconductor

A superconducting (SC) state (Tc ~ 4.2K) has very recently been observed upon successful doping of the CDW ordered triangular lattice TiSe$_2$, with copper. Using high resolution photoemission spectroscopy we identify, for the first time, the momentum space locations of the doped electrons that form the Fermi sea of the parent superconductor. With doping, we find that the kinematic nesting volume increases whereas the coherence of the CDW order sharply drops. In the superconducting doping, we observe the emergence of a large density of states in the form of a narrow electron pocket near the \textit{L}-point of the Brillouin Zone with \textit{d}-like character. The \textit{k}-space electron distributions highlight the unconventional interplay of CDW to SC cross-over achieved through non-magnetic copper doping.

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Complete d-Band Dispersion and the Mobile Fermion Scale in NaxCoO2

We utilize fine-tuned polarization selection coupled with excitation-energy variation of photoelectron signal to image the \textit{complete d}-band dispersion relation in sodium cobaltates. A hybridization gap anticrossing is observed along the Brillouin zone corner and the full quasiparticle band is found to emerge as a many-body entity lacking a pure orbital polarization. At low dopings, the quasiparticle bandwidth (Fermion scale, many-body \textit{E$_F$} $\sim$ 0.25 eV) is found to be smaller than most known oxide metals. The low-lying density of states is found to be in agreement with bulk-sensitive thermodynamic measurements for nonmagnetic dopings where the 2D Luttinger theorem is also observed to be satisfied.

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Low-lying quasiparticle states and hidden collective charge instabilities in parent cobaltate superconductors (NaxCoO2)

We report a state-of-the-art photoemission (ARPES) study of high quality single crystals of the NaxCoO2 series focusing on the fine details of the low-energy states. The Fermi velocity is found to be small (< 0.5 eV.A) and only weakly anisotropic over the Fermi surface at all dopings setting the size of the pair wavefunction to be on the order of 10-20 nanometers. In the low doping regime the exchange inter-layer splitting vanishes and two dimensional collective instabilities such as 120-type fluctuations become kinematically allowed. Our results suggest that the unusually small Fermi velocity and the unique symmetry of kinematic instabilities distinguish cobaltates from other unconventional oxide superconductors such as the cuprates or the ruthenates.

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Quasiparticle coherence and the nature of the metal-insulator phase transition in Na$_x$CoO$_2$

Layered cobaltates embody novel realizations of correlated quantum matter on a spin-1/2 triangular lattice. We report a high-resolution systematic photoemission study of the insulating cobaltates (Na1/2CoO2 and K1/2CoO2). Observation of single-particle gap opening and band-folding provides direct evidence of anisotropic particle-hole instability on the Fermi surface due to its unique topology. Kinematic overlap of the measured Fermi surface is observed with the $\sqrt{3}$x$\sqrt{3}$ cobalt charge-order Brillouin zone near x=1/3 but not at x=1/2 where insulating transition is actually observed. Unlike conventional density-waves, charge-stripes or band insulators, the on-set of the gap depends on the quasiparticle's quantum coherence which is found to occur well below the disorder-order symmetry breaking temperature of the crystal (the first known example of its kind).

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Low-lying electronic structure of doped triangular cobaltates

We report detailed Fermi surface topology and quasiparticle dynamics of the host cobaltate Na0.7CoO2. A direct mapping of the Fermi surface is carried out by angle-resolved photoemission spectroscopy (ARPES). Fermi surface at temperature 16K is a hole-pocket centered around the Gamma-point. The highly correlated nature of the electron liquid is evidenced from strong on-site Coulomb interaction seen through a valence satellite and via renormalization of the quasiparticle dispersion. The quasiparticle exhibits spectral coherence only below 150K which includes the non-Fermi liquid regime.

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