Unique Gap Structure and Symmetry of the Charge Density Wave in Single-Layer VSe_{2}.

Single layers of transition metal dichalcogenides (TMDCs) are excellent candidates for electronic applications beyond the graphene platform; many of them exhibit novel properties including charge density waves (CDWs) and magnetic ordering. CDWs in these single layers are generally a planar projection of the corresponding bulk CDWs because of the quasi-two-dimensional nature of TMDCs; a different CDW symmetry is unexpected. We report herein the successful creation of pristine single-layer VSe_{2}, which shows a (sqrt[7]×sqrt[3]) CDW in contrast to the (4×4) CDW for the layers in bulk VSe_{2}. Angle-resolved photoemission spectroscopy from the single layer shows a sizable (sqrt[7]×sqrt[3]) CDW gap of ∼100 meV at the zone boundary, a 220 K CDW transition temperature twice the bulk value, and no ferromagnetic exchange splitting as predicted by theory. This robust CDW with an exotic broken symmetry as the ground state is explained via a first-principles analysis. The results illustrate a unique CDW phenomenon in the two-dimensional limit.

Experimental Observation of Hidden Berry Curvature in Inversion-Symmetric Bulk 2H-WSe_{2}.

We investigate the hidden Berry curvature in bulk 2H-WSe_{2} by utilizing the surface sensitivity of angle resolved photoemission (ARPES). The symmetry in the electronic structure of transition metal dichalcogenides is used to uniquely determine the local orbital angular momentum (OAM) contribution to the circular dichroism (CD) in ARPES. The extracted CD signals for the K and K^{'} valleys are almost identical, but their signs, which should be determined by the valley index, are opposite. In addition, the sign is found to be the same for the two spin-split bands, indicating that it is independent of spin state. These observed CD behaviors are what are expected from Berry curvature of a monolayer of WSe_{2}. In order to see if CD-ARPES is indeed representative of hidden Berry curvature within a layer, we use tight binding analysis as well as density functional calculation to calculate the Berry curvature and local OAM of a monolayer WSe_{2}. We find that measured CD-ARPES is approximately proportional to the calculated Berry curvature as well as local OAM, further supporting our interpretation.

Spectral Evidence for Emergent Order in Ba_{1-x}Na_{x}Fe_{2}As_{2}.

We report an angle-resolved photoemission spectroscopy study of the iron-based superconductor family, Ba_{1-x}Na_{x}Fe_{2}As_{2}. This system harbors the recently discovered double-Q magnetic order appearing in a reentrant C_{4} phase deep within the underdoped regime of the phase diagram that is otherwise dominated by the coupled nematic phase and collinear antiferromagnetic order. From a detailed temperature-dependence study, we identify the electronic response to the nematic phase in an orbital-dependent band shift that strictly follows the rotational symmetry of the lattice and disappears when the system restores C_{4} symmetry in the low temperature phase. In addition, we report the observation of a distinct electronic reconstruction that cannot be explained by the known electronic orders in the system.

Enhanced superconductivity in surface-electron-doped iron pnictide Ba(Fe1.94Co0.06)2As2.

The superconducting transition temperature (TC) in a FeSe monolayer on SrTiO3 is enhanced up to 100 K (refs ,,,). High TC is also found in bulk iron chalcogenides with similar electronic structure to that of monolayer FeSe, which suggests that higher TC may be achieved through electron doping, pushing the Fermi surface (FS) topology towards leaving only electron pockets. Such an observation, however, has been limited to chalcogenides, and is in contrast to the iron pnictides, for which the maximum TC is achieved with both hole and electron pockets forming considerable FS nesting instability. Here, we report angle-resolved photoemission characterization revealing a monotonic increase of TC from 24 to 41.5 K upon surface doping on optimally doped Ba(Fe1-xCox)2As2. The doping changes the overall FS topology towards that of chalcogenides through a rigid downward band shift. Our findings suggest that higher electron doping and concomitant changes in FS topology are favourable conditions for the superconductivity, not only for iron chalcogenides, but also for iron pnictides.

Evolution of the Fermi surface of Weyl semimetals in the transition metal pnictide family.

Topological Weyl semimetals (TWSs) represent a novel state of topological quantum matter which not only possesses Weyl fermions (massless chiral particles that can be viewed as magnetic monopoles in momentum space) in the bulk and unique Fermi arcs generated by topological surface states, but also exhibits appealing physical properties such as extremely large magnetoresistance and ultra-high carrier mobility. Here, by performing angle-resolved photoemission spectroscopy (ARPES) on NbP and TaP, we directly observed their band structures with characteristic Fermi arcs of TWSs. Furthermore, by systematically investigating NbP, TaP and TaAs from the same transition metal monopnictide family, we discovered their Fermiology evolution with spin-orbit coupling (SOC) strength. Our experimental findings not only reveal the mechanism to realize and fine-tune the electronic structures of TWSs, but also provide a rich material base for exploring many exotic physical phenomena (for example, chiral magnetic effects, negative magnetoresistance, and the quantum anomalous Hall effect) and novel future applications.

Dimensional Effects on the Charge Density Waves in Ultrathin Films of TiSe2.

Charge density wave (CDW) formation in solids is a critical phenomenon involving the collective reorganization of the electrons and atoms in the system into a wave structure, and it is expected to be sensitive to the geometric constraint of the system at the nanoscale. Here, we study the CDW transition in TiSe2, a quasi-two-dimensional layered material, to determine the effects of quantum confinement and changing dimensions in films ranging from a single layer to multilayers. Of key interest is the characteristic length scale for the transformation from a two-dimensional case to the three-dimensional limit. Angle-resolved photoemission spectroscopy (ARPES) measurements of films with thicknesses up to six layers reveal substantial variations in the energy structure of discrete quantum well states; however, the temperature-dependent band gap renormalization converges at just three layers. The results indicate a layer-dependent mixture of two transition temperatures and a very-short-range CDW interaction within a three-dimensional framework.

Spectroscopic evidence for negative electronic compressibility in a quasi-three-dimensional spin-orbit correlated metal.

Negative compressibility is a sign of thermodynamic instability of open or non-equilibrium systems. In quantum materials consisting of multiple mutually coupled subsystems, the compressibility of one subsystem can be negative if it is countered by positive compressibility of the others. Manifestations of this effect have so far been limited to low-dimensional dilute electron systems. Here, we present evidence from angle-resolved photoemission spectroscopy (ARPES) for negative electronic compressibility (NEC) in the quasi-three-dimensional (3D) spin-orbit correlated metal (Sr1-xLax)3Ir2O7. Increased electron filling accompanies an anomalous decrease of the chemical potential, as indicated by the overall movement of the deep valence bands. Such anomaly, suggestive of NEC, is shown to be primarily driven by the lowering in energy of the conduction band as the correlated bandgap reduces. Our finding points to a distinct pathway towards an uncharted territory of NEC featuring bulk correlated metals with unique potential for applications in low-power nanoelectronics and novel metamaterials.

Distinct Electronic Structure for the Extreme Magnetoresistance in YSb.

An extreme magnetoresistance (XMR) has recently been observed in several nonmagnetic semimetals. Increasing experimental and theoretical evidence indicates that the XMR can be driven by either topological protection or electron-hole compensation. Here, by investigating the electronic structure of a XMR material, YSb, we present spectroscopic evidence for a special case which lacks topological protection and perfect electron-hole compensation. Further investigations reveal that a cooperative action of a substantial difference between electron and hole mobility and a moderate carrier compensation might contribute to the XMR in YSb.

A stable three-dimensional topological Dirac semimetal Cd3As2.

Three-dimensional (3D) topological Dirac semimetals (TDSs) are a recently proposed state of quantum matter that have attracted increasing attention in physics and materials science. A 3D TDS is not only a bulk analogue of graphene; it also exhibits non-trivial topology in its electronic structure that shares similarities with topological insulators. Moreover, a TDS can potentially be driven into other exotic phases (such as Weyl semimetals, axion insulators and topological superconductors), making it a unique parent compound for the study of these states and the phase transitions between them. Here, by performing angle-resolved photoemission spectroscopy, we directly observe a pair of 3D Dirac fermions in Cd3As2, proving that it is a model 3D TDS. Compared with other 3D TDSs, for example, ß-cristobalite BiO2 (ref. 3) and Na3Bi (refs 4, 5), Cd3As2 is stable and has much higher Fermi velocities. Furthermore, by in situ doping we have been able to tune its Fermi energy, making it a flexible platform for exploring exotic physical phenomena.

Bandwidth and Electron Correlation-Tuned Superconductivity in Rb_{0.8}Fe_{2}(Se_{1-z}S_{z})_{2}.

We present a systematic angle-resolved photoemission spectroscopy study of the substitution dependence of the electronic structure of Rb_{0.8}Fe_{2}(Se_{1-z}S_{z})_{2} (z=0, 0.5, 1), where superconductivity is continuously suppressed into a metallic phase. Going from the nonsuperconducting Rb_{0.8}Fe_{2}S_{2} to superconducting Rb_{0.8}Fe_{2}Se_{2}, we observe little change of the Fermi surface topology, but a reduction of the overall bandwidth by a factor of 2. Hence, for these heavily electron-doped iron chalcogenides, we have identified electron correlation as explicitly manifested in the quasiparticle bandwidth to be the important tuning parameter for superconductivity, and that moderate correlation is essential to achieving high T_{C}.

Electronic structure of a quasi-freestanding MoS2 monolayer.

Several transition-metal dichalcogenides exhibit a striking crossover from indirect to direct band gap semiconductors as they are thinned down to a single monolayer. Here, we demonstrate how an electronic structure characteristic of the isolated monolayer can be created at the surface of a bulk MoS2 crystal. This is achieved by intercalating potassium in the interlayer van der Waals gap, expanding its size while simultaneously doping electrons into the conduction band. Our angle-resolved photoemission measurements reveal resulting electron pockets centered at the K̅ and K' points of the Brillouin zone, providing the first momentum-resolved measurements of how the conduction band dispersions evolve to yield an approximately direct band gap of ∼1.8 eV in quasi-freestanding monolayer MoS2. As well as validating previous theoretical proposals, this establishes a novel methodology for manipulating electronic structure in transition-metal dichalcogenides, opening a new route for the generation of large-area quasi-freestanding monolayers for future fundamental study and use in practical applications.

Electronic structure of the iron-based superconductor LaOFeP.

The recent discovery of superconductivity in the iron oxypnictide family of compounds has generated intense interest. The layered crystal structure with transition-metal ions in planar square-lattice form and the discovery of spin-density-wave order near 130 K (refs 10, 11) seem to hint at a strong similarity with the copper oxide superconductors. An important current issue is the nature of the ground state of the parent compounds. Two distinct classes of theories, distinguished by the underlying band structure, have been put forward: a local-moment antiferromagnetic ground state in the strong-coupling approach, and an itinerant ground state in the weak-coupling approach. The first approach stresses on-site correlations, proximity to a Mott-insulating state and, thus, the resemblance to the high-transition-temperature copper oxides, whereas the second approach emphasizes the itinerant-electron physics and the interplay between the competing ferromagnetic and antiferromagnetic fluctuations. The debate over the two approaches is partly due to the lack of conclusive experimental information on the electronic structures. Here we report angle-resolved photoemission spectroscopy (ARPES) of LaOFeP (superconducting transition temperature, T(c) = 5.9 K), the first-reported iron-based superconductor. Our results favour the itinerant ground state, albeit with band renormalization. In addition, our data reveal important differences between these and copper-based superconductors.

Observation of temperature-induced crossover to an orbital-selective Mott phase in A(x)Fe(2-y)Se2 (A=K, Rb) superconductors.

Using angle-resolved photoemission spectroscopy, we observe the low-temperature state of the A(x)Fe(2-y)Se(2) (A=K, Rb) superconductors to exhibit an orbital-dependent renormalization of the bands near the Fermi level-the d(xy) bands heavily renormalized compared to the d(xz)/d(yz) bands. Upon raising the temperature to above 150 K, the system evolves into a state in which the d(xy) bands have depleted spectral weight while the d(xz)/d(yz) bands remain metallic. Combined with theoretical calculations, our observations can be consistently understood as a temperature-induced crossover from a metallic state at low temperatures to an orbital-selective Mott phase at high temperatures. Moreover, the fact that the superconducting state of A(x)Fe(2-y)Se(2) is near the boundary of such an orbital-selective Mott phase constrains the system to have sufficiently strong on-site Coulomb interactions and Hund's coupling, highlighting the nontrivial role of electron correlation in this family of iron-based superconductors.

Measurement of coherent polarons in the strongly coupled antiferromagnetically ordered iron-chalcogenide Fe1.02Te using angle-resolved photoemission spectroscopy.

The nature of metallicity and the level of electronic correlations in the antiferromagnetically ordered parent compounds are two important open issues for the iron-based superconductivity. We perform a temperature-dependent angle-resolved photoemission spectroscopy study of Fe(1.02)Te, the parent compound for iron chalcogenide superconductors. Deep in the antiferromagnetic state, the spectra exhibit a "peak-dip-hump" line shape associated with two clearly separate branches of dispersion, characteristics of polarons seen in manganites and lightly doped cuprates. As temperature increases towards the Néel temperature (T(N)), we observe a decreasing renormalization of the peak dispersion and a counterintuitive sharpening of the hump linewidth, suggestive of an intimate connection between the weakening electron-phonon (e-ph) coupling and antiferromagnetism. Our finding points to the highly correlated nature of the Fe(1.02)Te ground state featured by strong interactions among the charge, spin, and lattice and a good metallicity plausibly contributed by the coherent polaron motion.

Creation and control of a two-dimensional electron liquid at the bare SrTiO3 surface.

Many-body interactions in transition-metal oxides give rise to a wide range of functional properties, such as high-temperature superconductivity, colossal magnetoresistance or multiferroicity . The seminal recent discovery of a two-dimensional electron gas (2DEG) at the interface of the insulating oxides LaAlO(3) and SrTiO(3) (ref. 4) represents an important milestone towards exploiting such properties in all-oxide devices. This conducting interface shows a number of appealing properties, including a high electron mobility, superconductivity and large magnetoresistance, and can be patterned on the few-nanometre length scale. However, the microscopic origin of the interface 2DEG is poorly understood. Here, we show that a similar 2DEG, with an electron density as large as 8×10(13) cm(-2), can be formed at the bare SrTiO(3) surface. Furthermore, we find that the 2DEG density can be controlled through exposure of the surface to intense ultraviolet light. Subsequent angle-resolved photoemission spectroscopy measurements reveal an unusual coexistence of a light quasiparticle mass and signatures of strong many-body interactions.

Subband structure of a two-dimensional electron gas formed at the polar surface of the strong spin-orbit perovskite KTaO3.

We demonstrate the formation of a two-dimensional electron gas (2DEG) at the (100) surface of the 5d transition-metal oxide KTaO3. From angle-resolved photoemission, we find that quantum confinement lifts the orbital degeneracy of the bulk band structure and leads to a 2DEG composed of ladders of subband states of both light and heavy carriers. Despite the strong spin-orbit coupling, our measurements provide a direct upper bound for the potential Rashba spin splitting of only Δk(parallel)}~0.02 Å(-1) at the Fermi level. The polar nature of the KTaO3(100) surface appears to help mediate the formation of the 2DEG as compared to nonpolar SrTiO3(100).

Hidden itinerant-spin phase in heavily overdoped La(2-x)Sr(x)CuO4 superconductors revealed by dilute Fe doping: a combined neutron scattering and angle-resolved photoemission study.

We demonstrated experimentally a direct way to probe a hidden propensity to the formation of a spin-density wave in a nonmagnetic metal with strong Fermi surface nesting. Substituting Fe for a tiny amount of Cu (1%) induced an incommensurate magnetic order below 20 K in heavily overdoped La(2-x)Sr(x)CuO(4). Elastic neutron scattering suggested that this order cannot be ascribed to the localized spins on Cu or doped Fe. Angle-resolved photoemission revealed a strong Fermi surface nesting inherent in the pristine La(2-x)Sr(x)CuO(4) that likely drives this order. Our finding presents the first example of the long-sought "itinerant-spin extreme" of cuprates, where the spins of itinerant doped holes define the magnetic ordering ground state; it complements the current picture of cuprate spin physics that highlights the predominant role of localized spins at lower dopings.

Single Dirac cone topological surface state and unusual thermoelectric property of compounds from a new topological insulator family.

Angle resolved photoemission spectroscopy study on TlBiTe2 and TlBiSe2 from a thallium-based ternary chalcogenides family revealed a single surface Dirac cone at the center of the Brillouin zone for both compounds. For TlBiSe2, the large bulk gap (∼200 meV) makes it a topological insulator with better mechanical properties than the previous binary 3D topological insualtor family. For TlBiTe2, the observed negative bulk gap indicates it as a semimetal, instead of a narrow-gap semiconductor as conventionally believed; this semimetality naturally explains its mysteriously small thermoelectric figure of merit comparing to other compounds in the family. Finally, the unique band structures of TlBiTe2 also suggest it as a candidate for topological superconductors.

Interplay of negative electronic compressibility and capacitance enhancement in lightly-doped metal oxide Bi0.95La0.05FeO3 by quantum capacitance model.

Light-sensitive capacitance variation of Bi0.95La0.05FeO3 (BLFO) ceramics has been studied under violet to UV irradiation. The reversible capacitance enhancement up to 21% under 405 nm violet laser irradiation has been observed, suggesting a possible degree of freedom to dynamically control this in high dielectric materials for light-sensitive capacitance applications. By using ultraviolet photoemission spectroscopy (UPS), we show here that exposure of BLFO surfaces to UV light induces a counterintuitive shift of the O2p valence state to lower binding energy of up to 243 meV which is a direct signature of negative electronic compressibility (NEC). A decrease of BLFO electrical resistance agrees strongly with the UPS data suggesting the creation of a thin conductive layer on its insulating bulk under light irradiation. By exploiting the quantum capacitance model, we find that the negative quantum capacitance due to this NEC effect plays an important role in this capacitance enhancement.

Spectral weight reduction of two-dimensional electron gases at oxide surfaces across the ferroelectric transition.

The discovery of a two-dimensional electron gas (2DEG) at the [Formula: see text] interface has set a new platform for all-oxide electronics which could potentially exhibit the interplay among charge, spin, orbital, superconductivity, ferromagnetism and ferroelectricity. In this work, by using angle-resolved photoemission spectroscopy and conductivity measurement, we found the reduction of 2DEGs and the changes of the conductivity nature of some ferroelectric oxides including insulating Nb-lightly-substituted [Formula: see text], [Formula: see text] (BTO) and (Ca,Zr)-doped BTO across paraelectric-ferroelectric transition. We propose that these behaviours could be due to the increase of space-charge screening potential at the 2DEG/ferroelectric regions which is a result of the realignment of ferroelectric polarisation upon light irradiation. This finding suggests an opportunity for controlling the 2DEG at a bare oxide surface (instead of interfacial system) by using both light and ferroelectricity.