Contrasting Transport Performance of Electron-and Hole-Doped Epitaxial Graphene for Quantum Resistance Metrology

Epitaxial graphene grown on silicon carbide(Si C/graphene)is a promising solution for achieving a highprecision quantum Hall resistance standard.Previous research mainly focused on the quantum resistance metrology of n-type Si C/graphene,while a comprehensive understanding of the quantum resistance metrology behavior of graphene with different doping types is lacking.Here,we fabricated both n-and p-type Si C/graphene devices via polymer-assisted molecular adsorption and conducted systematic magneto-transport measurements in a wide parameter space of carrier density and temperature.It is demonstrated that n-type devices show greater potential for development of quantum resistance metrology compared with p-type devices,as evidenced by their higher carrier mobility,lower critical magnetic field for entering quantized Hall plateaus,and higher robustness of the quantum Hall effect against thermal degeneration.These discrepancies can be reasonably attributed to the weaker scattering from molecular dopants for n-type devices,which is further supported by the analyses on the quantum interference effect in multiple devices.These results enrich our understanding of the charged impurity on electronic transport performance of graphene and,more importantly,provide a useful reference for future development of graphene-based quantum resistance metrology.

Metal substrates-induced phase transformation of monolayer transition metal dichalcogenides for hydrogen evolution catalysis

Monolayer transition metal dichalcogenides can normally exist in several structural polymorphs with distinct electrical,optical,and catalytic properties.Effective control of the relative stability and transformation of different phases in these materials is thus of critical importance for applications.Using density functional theory calculations,we investigate the effects of low-work-function metal substrates including Ti,Zr,and Hf on the structural,electronic,and catalytic properties of monolayer MoS_(2) and WS_(2).The results indicate that such substrates not only convert the energetically stable structure from the 1H phase to the 1T'/1T phase,but also significantly reduce the kinetic barriers of the phase transformation.Furthermore,our calculations also indicate that the 1T' phase of MoS_(2) with Zr or Hf substrate is a potential catalyst for the hydrogen evolution reaction.

Machine learning potential aided structure search for low-lying candidates of Au clusters

A machine learning(ML)potential for Au clusters is developed through training on a dataset including several different sized clusters.This ML potential accurately covers the whole configuration space of Au clusters in a broad size range,thus expressing a good performance in search of their global minimum energy structures.Based on our potential,the low-lying structures of 17 different sized Au clusters are identified,which shows that small sized Au clusters tend to form planar structures while large ones are more likely to be stereo,revealing the critical size for the two-dimensional(2D)to three-dimensional(3D)structural transition.Our calculations demonstrate that ML is indeed powerful in describing the interaction of Au atoms and provides a new paradigm on accelerating the search of structures.

Effect of Boundary Scattering on Magneto-Transport Performance in BN-Encapsulated Graphene

For conductors in the ballistic regime, electron-boundary scattering at the sample edge plays a dominant role in determining the transport performance, giving rise to many intriguing phenomena like low-field negative magnetoresistance effect. We systematically investigate the magneto-transport behaviors of BN-encapsulated graphene devices with narrow channel width W, wherein the bulk mean free path Lmfp can be very large and highly tunable. By comparing the magnetoresistance features and the amplitude of Lmfp in a large parameter space of temperature and carrier density, we reveal that the boundary-scattering-dominated negative magnetoresistance effect can still survive even when the ballistic ratio(Lmfp/W) is as low as 0.15. This striking value is much smaller than the expected value for achieving(quasi-) ballistic transport regime(Lmfp/W ≥ 1), and can be attributed to the ultra-low specularity of the sample edge of our graphene devices. These findings enrich our understanding of the effects of boundary scattering on channel transport, which is of vital importance for future designs of two-dimensional electronic devices with limited lateral sizes.

Prediction of quantum anomalous Hall effect in CrI_(3)/ScCl_(2)bilayer heterostructure

Based on first-principles calculations,a two-dimensional(2D)van der Waals(vd W)bilayer heterostructure consisting of two topologically trivial ferromagnetic(FM)monolayers CrI_(3)and ScCl_(2)is proposed to realize the quantum anomalous Hall effect(QAHE)with a sizable topologically nontrivial band gap of 4.5 me V.Its topological nature is attributed to an interlayer band inversion between the monolayers and critically depends on the symmetry of the stacking configuration.We further demonstrate that the topologically nontrivial band gap can be increased nearly linearly by the application of a perpendicular external pressure and reaches 8.1 me V at 2.7 GPa,and the application of an external out-of-plane electric field can also modulate the band gap and convert the system back to topologically trivial via eliminating the band inversion.An effective model is developed to describe the topological phase evolution in this bilayer heterostructure.This work provides a new candidate system based on 2D vd W materials for realization of potential high-temperature QAHE with considerable controllability.

Giant-Capacitance-Induced Wide Quantum Hall Plateaus in Graphene on LaAlO3/SrTiO3 Heterostructures

Hybrid structures of two distinct materials provide an excellent opportunity to optimize functionalities.We report the realization of wide quantum Hall plateaus in graphene field-effect devices on the LaAlO3/SrTiO3 heterostructures.Well-defined quantized Hall resistance plateaus at filling factors ν=±2 can be obtained over wide ranges of the magnetic field and gate voltage,e.g.,extending from 2 T to a maximum available magnetic field of 9 T.By using a simple band diagram model,it is revealed that these wide plateaus arise from the ultralarge capacitance of the ultra-thin LAO layer acting as the dielectric layer.This is distinctly different from the case of epitaxial graphene on Si C substrates,where the realization of giant Hall plateaus relies on the charge transfer between the graphene layer and interface states in SiC.Our results offer an alternative route towards optimizing the quantum Hall performance of graphene,which may find its applications in the further development of quantum resistance metrology.

Electron-Exciton Coupling in 1T-TiSe_(2)Bilayer

Excitons in solid state are bosons generated by electron-hole pairs as the Coulomb screening is sufficiently reduced.The exciton condensation can result in exotic physics such as super-fluidity and insulating state.In charge density wave(CDW)state,1T-TiSe_(2) is one of the candidates that may host the exciton condensation.However,to envision its excitonic effect is still challenging,particularly at the two-dimensional limit,which is applicable to future devices.Here,we realize the epitaxial 1T-TiSe_(2) bilayer,the two-dimensional limit for its 2×2×2 CDW order,to explore the exciton-associated effect.By means of high-resolution scanning tunneling spectroscopy and quasiparticle interference,we discover an unexpected state residing below the conduction band and right within the CDW gap region.As corroborated by our theoretical analysis,this mysterious phenomenon is in good agreement with the electron-exciton coupling.Our study provides a material platform to explore exciton-based electronics and opto-electronics.

Interplay between the atomic structures and superconductivity of two-monolayer Pb films

Superconductors with reduced dimensionality have been widely explored for their exotic superconducting behaviors.Especially,at the two-dimensional limit,two-monolayer Pb films with two types of structures provide an ideal platform to unveil the underlying superconducting mechanism[Science 324,1314(2009)].Here,by combining scanning tunneling microscopy(STM)with the first-principle calculations,we successfully identify that these two types have different atomic lattice structures with varying stacking phases,which further enables us to calculate the phonon spectrum and electron phonon coupling strength of each type.The theoretical calculations are in good agreement with tunneling spectroscopy measurements of the superconducting transition temperatures(T_(c)),which established a correlation between atomic structures and superconductivity.Moreover,it was observed that the higher T_(c)of these two types also possess higher out-of-plane upper critical magnetic fields(Hc2).These findings will provide important new insights into two-dimensional superconductivity at the atomic level.

Topological and superconducting properties of monolayered CoN and CoP:A first-principles comparative study

Two-dimensional systems that simultaneously harbor superconductivity and nontrivial band topology may serve as appealing platforms for realizing topological superconductivity with promising applications in fault-tolerant quantum computing.Here,based on first-principles calculations,we show that monolayered Co N and Co P with the isovalent Fe Se-like structure are stable in freestanding form,even though their known bulk phases have no resemblance to layering.The two systems are further revealed to display intrinsic band inversions due to crystal field splitting,and such orderings are preserved with the inclusion of spin-orbit coupling(SOC),which otherwise is able to open a curved band gap,yielding a non-zero Z2 topological invariant in each case.Such a mechanism of topologicalization is distinctly contrasted with that identified recently for the closely related monolayers of CoX(X=As,Sb,Bi),where the SOC plays an indispensable role in causing a nontrivial band inversion.Next,we demonstrate that,by applying equi-biaxial tensile strain,the electron-phonon coupling strength in monolayered CoN can be significantly enhanced,yielding a superconducting transition temperature(Tc)up to 7-12 K for the Coulomb pseudopotential ofμ*=0.2-0.1,while the CoP monolayer shows very low Tc even under pronounced strain.Their different superconducting behaviors can be attributed to different variations in lattice softening and electronic density of states around the Fermi level upon pressuring.Our central findings enrich the understanding of different mechanisms of band inversions and topologicalization and offer platforms for achieving the coexistence of superconductivity and nontrivial band topology based on two-dimensional systems.

Correlation-enhanced electron-phonon coupling for accurate evaluation of the superconducting transition temperature in bulk FeSe

It has been widely recognized that,based on standard density functional theory calculations of the electron-phonon coupling,the superconducting transition temperature(T_(c))in bulk FeSe is exceptionally low(almost 0 K)within the Bardeen-Cooper-Schrieffer formalism.Yet the experimentally observed T_(c)is much higher(∼10 K),and the underlying physical origin remains to be fully explored,especially at the quantitative level.Here we present the first accurate determination of T_(c)in FeSe where the correlation-enhanced electron-phonon coupling is treated within first-principles dynamical mean-field theory.Our studies treat both the multiple electronic bands across the Fermi level and phononic bands,and reveal that all the optical phonon modes are effectively coupled with the conduction electrons,including the important contributions of a single breathing mode as established by previ-ous experiments.Accordingly,each of those phonon modes contributes pronouncedly to the electron pairing,and the resultant T_(c)is drastically enhanced to the experimentally observed range.The approach developed here should be broadly applicable to other superconducting systems where correlation-enhanced electron-phonon coupling plays an important role.

Atomically thin α-In2Se3: an emergent two-dimensional room temperature ferroelectric semiconductor

Room temperature ferroelectric thin films are the key element of high-density nonvolatile memories in modern electronics. However, with the further miniaturization of the electronic devices beyond the Moore’s law, conventional ferroelectrics suffer great challenge arising from the critical thickness effect, where the ferroelectricity is unstable if the film thickness is reduced to nanometer or single atomic layer limit. Two-dimensional(2D) materials, thanks to their stable layered structure, saturate interfacial chemistry, weak interlayer couplings, and the benefit of preparing stable ultra-thin film at 2D limit, are promising for exploring 2D ferroelectricity and related device applications. Therefore, it provides an effective approach to overcome the limitation in conventional ferroelectrics with the study of 2D ferroelectricity in van der Waals(vdW) materials. In this review article,we briefly introduce recent progresses on 2D ferroelectricity in layered vdW materials. We will highlight the study on atomically thin α-In2Se3, which is an emergent ferroelectric semiconductor with the coupled in-plane and out-of-plane ferroelectricity. Furthermore, two prototype ferroelectric devices based on ferroelectric α-In2Se3 will also be reviewed.

A simple and efficient criterion for ready screening of potential topological insulators

Topological materials are a new and rapidly expanding class of quantum matter. To date, identification of the topological nature of a given compound material demands specific determination of the appropriate topological invariant through detailed electronic structure calculations. Here we present an efficient criterion that allows ready screening of potential topological materials, using topological insulators as prototypical examples. The criterion is inherently tied to the band inversion induced by spin-orbit coupling,and is uniquely defined by a minimal number of two elemental physical properties of the constituent elements: the atomic number and Pauling electronegativity. The validity and predictive power of the criterion is demonstrated by rationalizing many known topological insulators and potential candidates in the tetradymite and half-Heusler families, and the underlying design principle is naturally also extendable to predictive discoveries of other classes of topological materials.

Realizing high thermoelectric performance via selective resonant doping in oxyselenide BiCuSeO

Tuning the charge carrier concentration is imperative to optimize the thermoelectric(TE)performance of a material.For BiCuSeO based oxyselenides,doping efforts have been limited to optimizing the carrier concentration.In the present work,dual-doping of In and Pb at Bi site is introduced for p-type BiCuSeO to realize the electric transport channels with intricate band characteristics to improve the power factor(PF).Herein,the impurity resonant state is realized via doping of resonant dopant In over Pb,where Pb comes forward to optimize the Fermi energy in the dual-doped BiCuSeO system to divulge the significance of complex electronic structure.The manifold roles of dual-doping are used to adjust the elevation of the PF due to the significant enhancement in electrical properties.Thus,the combined experimental and theoretical study shows that the In/Pb dual doping at Bi sites gently reduces bandgap,introduces resonant doping states with shifting down the Fermi level into valence band(VB)with a larger density of state,and thus causes to increase the carrier concentration and effective mass(m*),which are favorable to enhance the electronic transport significantly.As a result,both improved ZTmax=0.87(at 873 K)and high ZTave=0.5(at 300–873 K)are realized for InyBi(1−x)−yPbxCuSeO(where x=0.06 and y=0.04)system.The obtained results successfully demonstrate the effectiveness of the selective dual doping with resonant dopant inducing band manipulation and carrier engineering that can unlock new prospects to develop high TE materials.

Two-dimensional Sb cluster superlattice on Si substrate fabricated by a two-step method

Nanoclusters consisting of a few atoms have attracted a lot of research interests due to their exotic size-dependent properties. Here, well-ordered two-dimensional Sb cluster superlattice was fabricated on Si substrate by a two-step method and characterized by scanning tunneling microscopy. High resolution scanning tunneling microscope measurements revealed the fine structures of the Sb clusters, which consist of several Sb atoms ranging from 2 to 7. Furthermore, the electronic structure of the nanocluster displays the quantized energy-level which is due to the single-electron tunneling effects. We believe that the fabrication of Sb cluster superlattice broadens the species of the cluster superlattice and provides a promising candidate to further explore the novel physical and chemical properties of the semimetal nanocluster.

Proximity effects in topological insulator heterostructures

Topological insulators （Tls） are bulk insulators that possess robust helical conducting states along their interfaces with conventional insulators. A tremendous research effort has recently been devoted to TI-based heterostructures, in which con- ventional proximity effects give rise to a series of exotic physical phenomena. This paper reviews our recent studies on the potential existence of topological proximity effects at the interface between a topological insulator and a normal insu- lator or other topologically trivial systems. Using first-principles approaches, we have realized the tunability of the vertical location of the topological helical state via intriguing dual-proximity effects. To further elucidate the control parameters of this effect, we have used the graphene-based heterostructures as prototypical systems to reveal a more complete phase diagram. On the application side of the topological helical states, we have presented a catalysis example, where the topo- logical helical state plays an essential role in facilitating surface reactions by serving as an effective electron bath, These discoveries lay the foundation for accurate manipulation of the real space properties of the topological helical state in TI- based heterostructures and pave the way for realization of the salient functionality of topological insulators in future device applications.

Giant Rashba-like spin-orbit splitting with distinct spin texture in two-dimensional heterostructures

Based on first-principles density functional theory calculation,we discover a novel form of spin-orbit(SO)splitting in two-dimensional(2D)heterostructures composed of a single Bi(111)bilayer stacking with a 2D semiconducting In_(2)Se_(2) or a 2D ferroelectricα-In_(2)Se_(3) layer.Such SO splitting has a Rashba-like but distinct spin texture in the valence band around the maximum,where the chirality of the spin texture reverses within the upper spin-split branch,in contrast to the conventional Rashba systems where the upper branch and lower branch have opposite chirality solely in the region below the band crossing point.The ferroelectric nature ofα-In_(2)Se_(3) further enables the tuning of the spin texture upon the reversal of the electric polarization with the application of an external electric field.Detailed analysis based on a tight-binding model reveals that such SO splitting texture results from the interplay of complex orbital characters and substrate interaction.This finding enriches the diversity of SO splitting systems and is also expected to promise for spintronic applications.

Contrasting room-temperature hydrogen sensing capabilities of Pt-SnO2 and Pt-TiO2 composite nanoceramics

Contrasting room-temperature hydrogen sensing behaviors have been revealed for Pt-TiO2 and Pt-SnO2 composite nanoceramics. In the case of the Pt-TiO2 nanoceramics, the ultrahigh hydrogen sensitivities are lost abruptly when the oxygen/hydrogen concentration ratio in ambient atmosphere reaches a critical value. However, in the case of the Pt-SnO2 nanoceramics, such a phenomenon does not occur, and the extraordinary room-temperature hydrogen sensing capabilities are observed in the presence of oxygen in air. Our combined experimental and theoretical investigations establish a unified mechanism for both the systems, which is rooted in hydrogen chemisorption on the surface and interstitial lattice sites of SnO2 and TiO2; the difference in stability of the chemisorbed hydrogen on SnO2 and TiO2 is considered responsible for the contrasting hydrogen sensing capabilities. The central findings are helpful in enriching our microscopic understanding of hydrogen interaction with various metal oxide semiconductors （MOSs） at room temperature in varying mixed gaseous concentrations, and they could be instrumental in developing reliable room-temperature hydrogen sensors based on bulk MOSs.

Surface-adsorbed ions on TiO2 nanosheets for selective photocatalytic CO2 reduction

A method based on the adsorption of ions on the surface of two-dimensional （2D） nanosheets has been developed for photocatalytic COz reduction. Isolated Bi ions, confined on the surface of TiO2 nanosheets using a simple ionic adsorption method facilitate the formation of a built-in electric field that effectively promotes charge carrier separation. This leads to an improved performance of the photocatalytic COa reduction process with the preferred conversion to CH4. The proposed surface ion-adsorption method is expected to provide an effective approach for the design of highly efficient photocatalytic systems. These findings could be very valuable in photocatalytic CO2 reduction applications.

Selective flattening of magnon bands in kagome-lattice ferromagnets with Dzyaloshinskii-Moriya interaction

There is growing interest in revealing exotic properties of collective spin excitations in kagome-lattice ferromagnets such as magnon Hall effects,topological magnon insulators,and flat magnon bands.Using the well-established nearest-neighbor Heisenberg ferromagnet model with Dzyaloshinskii-Moriya interaction(DMI),in this study we uncover intriguing new aspects in the selectivity and topology of flat magnon bands.Among the three magnon bands(except for the top one,which is flat in the absence of DMI),we observe that each of the three bands can be selectively flattened at the critical DMI of D=±√3 J/3 and D=±√3 J.With a general DMI,the magnon bands become non-flat;however,there are nested lines that create a David star pattern for all three magnon bands whose flatness is robust during changing exchange coupling or DMIs.Contrary to prevailing belief,we show that each of the three flat bands is actually topologically trivial at critical DMIs.Furthermore,we show that while the middle band remains topologically trivial,for the other two bands,D=0 corresponds to the topological phase transition where their Chern numbers get interchanged;when D=±√3 J,the system undergoes a phase transition to the nonferromagnetic state.These central findings increase our understanding of spin excitations for future magnonics applications.

Predicting the lattice thermal conductivity of alloyed compounds from the perspective of configurational entropy

Accurate evaluation of lattice thermal conductivity is usually a tough task from the theoretical side,especially for alloyed systems with fractional stoichiometry.Using the tetradymite family as a prototypical class of examples,we propose a reliable approach for rapid prediction on the lattice thermal conductivity at arbitrary composition by utilizing the concept of configurational entropy.Instead of performing time-consuming first-principles calculations,the lattice thermal conductivities of any alloyed tetradymites can be readily obtained from a few samples with integer stoichiometry.The strong predictive power is demonstrated by good agreement between our results and those reported experimentally.In principle,such an effective method can be applicable to any other material families,which is very beneficial for high-throughput design of systems with desired thermal conductivity.