Progressive Control of Rashba State on Topological Dirac Semimetal KZnBi.

Rashba states have been actively revisited as a platform for advanced applications such as spintronics and topological quantum computation. Yet, access to the Rashba state is restricted to the specific material sets, and the methodology to control the Rashba state is not established. Here, we report the Rashba states on the (001) surface of KZnBi, a 3D Dirac semimetal. Using angle-resolved photoemission spectroscopy and first-principles calculations, we investigated the evolution of Rashba states under different surface conditions controlled by alkali metal deposition. We observed that restoring surface ordering enables a Rashba state, which is absent in freshly cleaved surfaces. Interestingly, we were able to modify the dispersion of the Rashba state from an ordinary parabolic dispersion to a linearly dispersing Dirac-like state by additional alkali-metal deposition. Our findings provide a methodology for engineering the properties of Rashba states for advanced applications and redefine topological systems as generic hosts of Rashba states.

Band-selective gap opening by a C 4-symmetric order in a proximity-coupled heterostructure Sr2VO3FeAs.

Complex electronic phases in strongly correlated electron systems are manifested by broken symmetries in the low-energy electronic states. Some mysterious phases, however, exhibit intriguing energy gap opening without an apparent signature of symmetry breaking (e.g., high-TC cuprates and heavy fermion superconductors). Here, we report an unconventional gap opening in a heterostructured, iron-based superconductor Sr2VO3FeAs across a phase transition at T 0 ∼150 K. Using angle-resolved photoemission spectroscopy, we identify that a fully isotropic gap opens selectively on one of the Fermi surfaces with finite warping along the interlayer direction. This band selectivity is incompatible with conventional gap opening mechanisms associated with symmetry breaking. These findings, together with the unusual field-dependent magnetoresistance, suggest that the Kondo-type proximity coupling of itinerant Fe electrons to localized V spin plays a role in stabilizing the exotic phase, which may serve as a distinct precursor state for unconventional superconductivity.

Converting the Bulk Transition Metal Dichalcogenides Crystal into Stacked Monolayers via Ethylenediamine Intercalation.

We report the synthesis of ethylenediamine-intercalated NbSe2 and Li-ethylenediamine-intercalated MoSe2 single crystals with increased interlayer distances and their electronic structures measured by means of angle-resolved photoemission spectroscopy (ARPES). X-ray diffraction patterns and transmission electron microscopy images confirm the successful intercalation and an increase in the interlayer distance. ARPES measurement reveals that intercalated NbSe2 shows an electronic structure almost identical to that of monolayer NbSe2. Intercalated MoSe2 also returns the characteristic feature of the monolayer electronic structure, a direct band gap, which generates sizable photoluminescence even in the bulk form. Our results demonstrate that the properties and phenomena of the monolayer transition metal dichalcogenides can be achieved with large-scale bulk samples by blocking the interlayer interaction through intercalation.

Quantum electron liquid and its possible phase transition.

Purely quantum electron systems exhibit intriguing correlated electronic phases by virtue of quantum fluctuations in addition to electron-electron interactions. To realize such quantum electron systems, a key ingredient is dense electrons decoupled from other degrees of freedom. Here, we report the discovery of a pure quantum electron liquid that spreads up to ~3 Å in a vacuum on the surface of an electride crystal. Its extremely high electron density and weak hybridization with buried atomic orbitals show the quantum and pure nature of the electrons, which exhibit a polarized liquid phase, as demonstrated by our spin-dependent measurement. Furthermore, upon enhancing the electron correlation strength, the dynamics of the quantum electrons change to that of a non-Fermi liquid along with an anomalous band deformation, suggestive of a transition to a hexatic liquid crystal phase. Our findings develop the frontier of quantum electron systems and serve as a platform for exploring correlated electronic phases in a pure fashion.

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.

A novel quasi-one-dimensional topological insulator in bismuth iodide ß-Bi4I4.

Recent progress in the field of topological states of matter has largely been initiated by the discovery of bismuth and antimony chalcogenide bulk topological insulators (TIs; refs ,,,), followed by closely related ternary compounds and predictions of several weak TIs (refs ,,). However, both the conceptual richness of Z2 classification of TIs as well as their structural and compositional diversity are far from being fully exploited. Here, a new Z2 topological insulator is theoretically predicted and experimentally confirmed in the ß-phase of quasi-one-dimensional bismuth iodide Bi4I4. The electronic structure of ß-Bi4I4, characterized by Z2 invariants (1;110), is in proximity of both the weak TI phase (0;001) and the trivial insulator phase (0;000). Our angle-resolved photoemission spectroscopy measurements performed on the (001) surface reveal a highly anisotropic band-crossing feature located at the  point of the surface Brillouin zone and showing no dispersion with the photon energy, thus being fully consistent with the theoretical prediction.

Electronic Structure, Surface Doping, and Optical Response in Epitaxial WSe2 Thin Films.

High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.

Topological Fermi-arc surface state covered by floating electrons on a two-dimensional electride.

Two-dimensional electrides can acquire topologically non-trivial phases due to intriguing interplay between the cationic atomic layers and anionic electron layers. However, experimental evidence of topological surface states has yet to be verified. Here, via angle-resolved photoemission spectroscopy (ARPES) and scanning tunnelling microscopy (STM), we probe the magnetic Weyl states of the ferromagnetic electride [Gd2C]2+·2e-. In particular, the presence of Weyl cones and Fermi-arc states is demonstrated through photon energy-dependent ARPES measurements, agreeing with theoretical band structure calculations. Notably, the STM measurements reveal that the Fermi-arc states exist underneath a floating quantum electron liquid on the top Gd layer, forming double-stacked surface states in a heterostructure. Our work thus not only unveils the non-trivial topology of the [Gd2C]2+·2e- electride but also realizes a surface heterostructure that can host phenomena distinct from the bulk.

Singular Hall Response from a Correlated Ferromagnetic Flat Nodal-Line Semimetal.

Topological quantum phases are largely understood in weakly correlated systems, which have identified various quantum phenomena, such as the spin Hall effect, protected transport of helical fermions, and topological superconductivity. Robust ferromagnetic order in correlated topological materials particularly attracts attention, as it can provide a versatile platform for novel quantum devices. Here, a singular Hall response arising from a unique band structure of flat topological nodal lines in combination with electron correlation in a van der Waals ferromagnetic semimetal, Fe3GaTe2, with a high Curie temperature of Tc = 347 K is reported. High anomalous Hall conductivity violating the conventional scaling, resistivity upturn at low temperature, and a large Sommerfeld coefficient are observed in Fe3GaTe2, which implies heavy fermion features in this ferromagnetic topological material. The scanning tunneling microscopy, circular dichroism in angle-resolved photoemission spectroscopy, and theoretical calculations support the original electronic features of the material. Thus, low-dimensional Fe3GaTe2 with electronic correlation, topology, and room-temperature ferromagnetic order appears to be a promising candidate for robust quantum devices.

Coupling Between Electrons and Charge Density Wave Fluctuation and its Possible Role in Superconductivity.

In most charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-PdxTaSe2. Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, the estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields results closely resembling the known values of the superconducting dome. The results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights into the competing relationship not only for CDW but also for other competing orders.

Hole-Carrier-Dominant Transport in 2D Single-Crystal Copper.

In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole-like attribute of 2D single-crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single-crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.

Orbital selective Fermi surface shifts and mechanism of high T(c) superconductivity in correlated AFeAs (A=Li, Na).

Based on the dynamical mean field theory and angle resolved photoemission spectroscopy, we have investigated the mechanism of high T(c) superconductivity in stoichiometric LiFeAs. The calculated spectrum is in excellent agreement with the measured angle resolved photoemission spectroscopy. The Fermi surface (FS) nesting, which is predicted in the conventional density functional theory method, is suppressed due to the orbital-dependent correlation effect within the dynamical mean field theory method. We have shown that such marginal breakdown of the FS nesting is an essential condition to the spin-fluctuation mediated superconductivity, while the good FS nesting in NaFeAs induces a spin density wave ground state. Our results indicate that a fully charge self-consistent description of the correlation effect is crucial in the description of the FS nesting-driven instabilities.

Real-space imaging and control of chiral anomaly induced current at room temperature in topological Dirac semimetal.

Chiral fermions (CFs) in condensed matters, distinguished by right (+) or left (-) handedness, hold a promise for emergent quantum devices. Although a chiral anomaly induced current, Jchiral = J(+) - J(-), occurs in Weyl semimetals due to the charge imbalance of the CFs, monitoring spatial flow and temporal dynamics of Jchiral has not been demonstrated yet. Here, we report real-space imaging and control of Jchiral on the topological Dirac semimetal KZnBi at room temperature (RT) by near-field terahertz (THz) spectroscopy, establishing a relation for an electromagnetic control of Jchiral. In THz electric and external magnetic fields, we visualize a spatial flow of coherent Jchiral in macroscopic length scale and monitor its temporal dynamics in picosecond time scale, revealing its ultralong transport length around 100 micrometers. Such coherent Jchiral is further found to be controlled according to field directions, suggesting the feasibility of information science with topological Dirac semimetals at RT.

Deep learning-based statistical noise reduction for multidimensional spectral data.

In spectroscopic experiments, data acquisition in multi-dimensional phase space may require long acquisition time, owing to the large phase space volume to be covered. In such a case, the limited time available for data acquisition can be a serious constraint for experiments in which multidimensional spectral data are acquired. Here, taking angle-resolved photoemission spectroscopy (ARPES) as an example, we demonstrate a denoising method that utilizes deep learning as an intelligent way to overcome the constraint. With readily available ARPES data and random generation of training datasets, we successfully trained the denoising neural network without overfitting. The denoising neural network can remove the noise in the data while preserving its intrinsic information. We show that the denoising neural network allows us to perform a similar level of second-derivative and line shape analysis on data taken with two orders of magnitude less acquisition time. The importance of our method lies in its applicability to any multidimensional spectral data that are susceptible to statistical noise.

Antiperovskite Gd3 SnC: Unusual Coexistence of Ferromagnetism and Heavy Fermions in Gd Lattice.

Inverted structures of common crystal lattices, referred to as antistructures, are rare in nature due to their thermodynamic constraints imposed by the switched cation and anion positions in reference to the original structure. However, a stable antistructure formed with mixed bonding characters of constituent elements in unusual valence states can provide unexpected material properties. Here, a heavy-fermion behavior of ferromagnetic gadolinium lattice in Gd3 SnC antiperovskite is reported, contradicting the common belief that ferromagnetic gadolinium cannot be a heavy-fermion system due to the deep energy level of localized 4f-electrons. The specific heat shows an unusually large Sommerfeld coefficient of ≈1114 mJ mol-1 K-2 with a logarithmic behavior of non-Fermi-liquid state. It is demonstrated that the heavy-fermion behavior in the non-Fermi-liquid state appears to arise from the hybridized electronic states of gadolinium 5d-electrons participating in metallic GdGd and covalent GdC bonds. These results accentuate the unusual chemical bonds in CGd6 octahedra with the dual characters of gadolinium 5d-electrons for the emergence of heavy fermions.

Direct observation of kink evolution due to Hund's coupling on approach to metal-insulator transition in NiS2-xSex.

Understanding characteristic energy scales is a fundamentally important issue in the study of strongly correlated systems. In multiband systems, an energy scale is affected not only by the effective Coulomb interaction but also by the Hund's coupling. Direct observation of such energy scale has been elusive so far in spite of extensive studies. Here, we report the observation of a kink structure in the low energy dispersion of NiS2-xSex and its characteristic evolution with x, by using angle resolved photoemission spectroscopy. Dynamical mean field theory calculation combined with density functional theory confirms that this kink originates from Hund's coupling. We find that the abrupt deviation from the Fermi liquid behavior in the electron self-energy results in the kink feature at low energy scale and that the kink is directly related to the coherence-incoherence crossover temperature scale. Our results mark the direct observation of the evolution of the characteristic temperature scale via kink features in the spectral function, which is the hallmark of Hund's physics in the multiorbital system.

Response of microbial growth to orthophosphate and organic carbon influx in copper and plastic based plumbing water systems.

Consequences of orthophosphate addition for corrosion control in water distribution pipes with respect to microbial growth were investigated using batch and dynamic tests. Batch tests showed that the release of copper in either low or high organic carbon content water was decreased by 69% and 56% with addition 206 microg PO(4)-P, respectively. Dosing of orthophosphate against corrosion did not increase microbial growth potential in the water and in the biofilm in both corroded and uncorroded systems receiving tap water with a low content of organic carbon and of biodegradable organic fraction. However, in tap water having a high concentration of organic carbon from acetate addition, orthophosphate addition promoted the growth of bacteria, allowed more bacteria to assemble on corroded and uncorroded surfaces, and increased the consumption of organic carbon. Orthophosphate consumption did not exceed 1% of the amount of easily biodegradable organic carbon required for microbial growth, and the orthophosphate demand for corrosion control greatly exceeded the nutritional requirement of microbial growth. The results of the dynamic tests demonstrated that there was a significant effect of interaction between biodegradable organic carbon and orthophosphate on biofilm growth, whereby the effect of orthophosphate flux on microbial growth was dependent on the levels of biodegradable organic carbon. Controlling an easily biodegradable organic carbon would be therefore necessary to minimize the microbial growth potential induced by orthophosphate-based anticorrosion treatment.

Treatment of landfill leachate by white rot fungus in combination with zeolite filters.

This article presents the experimental work for the treatment of landfill leachate in a combined process using the white rot fungus Phanerochaete chrysosporium and the natural zeolite Clinoptilolite. Clinoptilolite was used in a pretreatment step as a sink for ammonia nitrogen and, on average it reduced the levels of ammonia nitrogen, soluble chemical oxygen demand (COD) and color by 72, 4.7, and 25%, respectively. The reductions by fungal treatment alone were 16.6, 21.5, and 31.2%, respectively. However, a reduction in nitrogen loading greatly enhanced fungal treatment efficiency. A high C/N ratio in the leachate was found preferable for the fungal treatment. With the synergy created by pretreatment and fungal growth that was stimulated by the addition of a growth medium, the process could remove ammonia nitrogen, soluble COD (SCOD) and color at levels as high as 81.5, 65, and 59%, respectively. The ratio of SBOD5/SCOD increased from 0.1 to 0.17 upon treatment, indicating that the process rendered the leachate more amenable to the biological process. This result suggested that the preliminary reduction of ammonia nitrogen was essential in making the fungal process practicable for landfill leachate treatment.

Evaluation of bioassays for analyzing biodegradable dissolved organic carbon in drinking water.

Three different bioassays for analysis of biodegradable dissolved organic carbon (BDOC) were evaluated to identify which method is most applicable to analysis of drinking water. The determination of BDOC is primarily based on the differences between initial and final DOC levels during a certain incubation period using indigenous bacterial consortium as an inoculum. The assay procedures basically differ in the preparation method of inoculum. Inoculum was added in the form of suspended bacteria in one assay. In the other two assays, bacterial inoculum attached to either sand or inert media was used in a continuous reactor column. Standard solutions containing sodium acetate, sodium oxalate, or glucose at 1 mg C/L, and tap water were tested. The bioassay using bacteria attached to sand was shown to be superior to the two other methods for BDOC determination in terms of its incubation period, recovery, and reproducibility. Tap water samples, when analyzed by this assay, could not be guaranteed for biological stability due to their high BDOC concentrations (0.17 to 0.23 mg/L) that corresponded to 26-36% of the initial DOC level.