In this paper, the completed investigation of a possible superconducting phase in monolayer indium selenide is determined using first-principles calculations for both the hole and electron doping systems. The hole-doped dependence of the Fermi surface is exclusively fundamental for monolayer InSe. It leads to the extensive modification of the Fermi surface from six separated pockets to two pockets by increasing the hole densities. For low hole doping levels of the system, below the Lifshitz transition point, superconductive critical temperatures $T_c \sim 55-75$ K are obtained within anisotropic Eliashberg theory depending on varying amounts of the Coulomb potential from 0.2 to 0.1. However, for some hole doping above the Lifshitz transition point, the combination of the temperature dependence of the bare susceptibility and the strong electron-phonon interaction gives rise to a charge density wave that emerged at a temperature far above the corresponding $T_c$. Having included non-adiabatic effects, we could carefully analyze conditions for which either a superconductive or charge density wave phase occurs in the system. In addition, monolayer InSe becomes dynamically stable by including non-adiabatic effects for different carrier concentrations at room temperature.
Sub-monolayer physical layer deposition of Zn on Ag(111) substrate at room temperature is investigated using Auger electron spectroscopy, low energy electron diffraction and scanning tunneling microscopy. We identified an original Zn highly-anisotropic structure in the shape of finger-like inserted dendrite in front of Zn monolayer growth. On the basis of STM observations, a mechanism of inserted dendritic growth and a mechanism of its transition to layered growth are proposed.
By using first-principles calculation, the interaction of O2 and H2O molecules with the pristine and the defective InSe monolayers is studied. It is predicted that the single Se and In vacancies exhibit significantly enhanced chemical activity toward the adsorbates compared with the perfect InSe lattice site, and the Se vacancies have a much higher chemical activity than the In vacancies. H2O molecule should be only physisorbed on the various InSe monolayers at ambient conditions, according to the calculated energies. The doping of the various InSe monolayers is discussed by the physisorbed H2…
We systematically investigated the phonon and electron transport properties of monolayer InSe and its Janus derivatives including monolayer In2SSe and In2SeTe by first-principles calculations. The breaking of mirror symmetry produce a distinguishable A1 peak in the Raman spectra of monolayer In2SSe and In2SeTe. The room-temperature thermal conductivity (\k{appa}) of monolayer InSe, In2SSe and In2SeTe is 44.6, 46.9, and 29.9 W/(m K), respectively. There is a competition effect between atomic mass, phonon group velocity and phonon lifetime. The \k{appa} can be further effectively modulated by sa…
In 2D-semiconductor-based field-effect transistors and optoelectronic devices, metal-semiconductor junctions are one of the crucial factors determining device performance. The Fermi-level (FL) pinning effect, which commonly caused by interfacial gap states, severely limits the tunability of junction characteristics, including barrier height and contact resistance. A tunneling contact scheme has been suggested to address the FL pinning issue in metal-2D-semiconductor junctions, whereas the experimental realization is still elusive. Here, we show that an oxidized-monolayer-enabled tunneling barr…
The quantum spin Hall (QSH) state was recently demonstrated in monolayers of the transition metal dichalcogenide 1T'-WTe$_2$ and is characterized by a band gap in the two-dimensional (2D) interior and helical one-dimensional (1D) edge states. Inducing superconductivity in the helical edge states would result in a 1D topological superconductor, a highly sought-after state of matter. In the present study, we use a novel dry-transfer flip technique to place atomically-thin layers of WTe$_2$ on a van der Waals superconductor, NbSe$_2$. Using scanning tunneling microscopy and spectroscopy (STM/STS)…
Recently fabricated InSe monolayers exhibit remarkable characteristics that indicate the potential of this material to host a number of many-body phenomena. Here, we consistently describe collective electronic effects in hole-doped InSe monolayers using advanced many-body techniques. To this end, we derive a realistic electronic-structure model from first principles that takes into account the most important characteristics of this material, including a flat band with prominent van Hove singularities in the electronic spectrum, strong electron-phonon coupling, and weakly-screened long-ranged C…
Many recent studies show that superconductivity not only exists in atomically thin monolayers but can exhibit enhanced properties such as higher transition temperature and stronger critical field. Nevertheless, besides being air unstable, weak tunability in these intrinsically metallic monolayers has posed a severe limitation in exploring monolayer superconductivity, hence hindering possible applications in electronic devices. Using field effect gating, we prepared monolayer superconductivity in easily accessible CVD-grown WS2, a typical ambient stable semiconducting transition metal dichalcog…
Two-dimensional (2D) InSe and WS$_2$ exhibit promising characteristics for optoelectronic and photoelectrochemical applications, e.g. photodetection and photocatalytic water splitting. However, both of them have poor absorption of visible light due to wide band gaps. 2D InSe has high electron mobility but low hole mobility, while 2D WS$_2$ is on the opposite. Here, we design a 2D heterostructure composed of their monolayers and study its optoelectronic properties by first-principles calculations. Our results show that the heterostructure has a direct band gap of 2.19 eV, which is much smaller …
Van der Waals (vdW) heterostructures continue to attract intense interest as a route of designing materials with novel properties that cannot be found in naturally occurring materials. Unfortunately, this approach is currently limited to only a few layers that can be stacked on top of each other. Here we report a bulk material consisting of superconducting monolayers interlayered with monolayers displaying charge density waves (CDW). This bulk vdW heterostructure is created by phase transition of 1T-TaS2 to 6R at 800 °C in an inert atmosphere. Electron microscopy analysis directly shows the pr…
Liquid-phase chemical exfoliation is ideal to achieve industry scale production of two-dimensional (2D) materials for a wide range of application such as printable electronics, catalysis and energy storage. However, many impactful 2D materials with potentials in quantum technologies can only be studied in lab settings due to their air-sensitivity, and loss of physical performance after chemical processing. Here, we report a simple chemical exfoliation method to create a stable, aqueous, surfactant-free, superconducting ink containing phase-pure 1T'-WS$_2$ monolayers that are isotructural to th…
Thermoelectric properties of monolayer indium selenide (InSe) are investigated by using Boltzman transport theory and first-principles calculations as a function of Fermi energy and crystal orientation. We find that the maximum power factor of p-type (n-type) monolayer InSe can be as large as 0.049 (0.043) W/K$^2$m at 300 K in the armchair direction. The excellent thermoelectric performance of monolayer InSe is attributed to both of its Seebeck coefficient and electrical conductivity. The large Seebeck coefficient originates from the moderate (about 2 eV) band gap of monolayer InSe as an indir…
The spin-orbit coupling can lead to exotic states of matter and unexpected behavior of the system properties. In this paper, we investigate the influence of spin-orbit coupling induced by proximity effects on a monolayer of superconductor (with s-wave or d-wave pairing) placed on an insulating bulk. We show that the critical temperatures $T_{c}$ of the superconducting states can be tuned by the spin-orbit coupling both in the case of on-site and inter-site pairing. Moreover, we discuss a possibility of changing the location of the maximal $T_{c}$ from the half-filling into the underdoped or ov…
Making a metal contact to the two-dimensional semiconductor MoS2 without creating a Schottky barrier is a challenge. Using density functional calculations we show that, although the Schottky barrier for electrons obeys the Schottky-Mott rule for high work function ($\gtrsim 4.7$ eV) metals, the Fermi level is pinned at 0.1-0.3 eV below the conduction band edge of MoS2 for low work function metals, due to the metal-MoS2 interaction. Inserting a boron nitride (BN) monolayer between the metal and the MoS2 disrupts this interaction, and restores the MoS2 electronic structure. Moreover, a BN layer …
Motivated by recent experimental progress, we study the effect of mechanical deformations on the superconducting pairing symmetries in monolayer black phosphorus (MBP). Starting with phonon-mediated intervalley spin-singlet electron-electron pairing and making use of realistic band parameters obtained through first-principles calculations, we show that the application of weak mechanical strain in the plane of MBP can change the effective $s$-wave and $p$-wave symmetry of the superconducting correlations into effective $d$-wave and $f$-wave symmetries, respectively. This prediction of a change …
The precise value of the $g$-factor in graphene is of fundamental interest for all spin-related properties and their application. We investigate monolayer graphene on a Si/SiO2 substrate by resistively detected electron spin resonance (ESR). Surprisingly, the magnetic moment and corresponding g-factor of 1.952+/-0.002 is insensitive to charge carrier type, concentration, and mobility.
Graphene like 2D materials have attracted tremendous attention in the field of photocatalytic water splitting. Indium Selenide (InSe) is one such potential material. Here, we report the effect of Tellurium on InSe monolayer for the photocatalytic water splitting by means of density functional calculations. The calculated bandgaps fall within the visible region of the solar spectrum indicating these materials could absorb a significant amount of solar light. Density of states calculations show that the covalent character is present between the atoms which is typical for the layered system. The …
First-principles calculations are performed to investigate the effects of the adsorption of gas molecules (CO, NO, NO2, H2S, N2, H2O, O2, NH3 and H2) on the electronic properties of atomically thin indium selenium (InSe). Our study shows that the lone-pair states of Se are located at the top of the valence band of InSe and close to the Fermi energy level, implying its high sensitivity to external adsorbates. Among these gas molecules, H2 and H2S are strong donors, NO, NO2, H2O and NH3 are effective acceptors, while CO and N2 exhibit negligible charge transfer. The O2 molecule has very limited …
The iron-based superconductors are an ideal platform to reveal the enigma of the unconventional superconductivity and potential topological superconductivity. Among them, the monolayer Fe(Se,Te)/SrTiO3(001), which is proposed to be topological nontrivial, shows interface-enhanced high-temperature superconductivity in the two dimensional limit. However, the experimental studies on the superconducting pairing mechanism of monolayer Fe(Se,Te) films are still limited. Here, by measuring quasiparticle interference in monolayer Fe(Se,Te)/SrTiO3(001), we report the observation of the anisotropic stru…
Vertical integration of two-dimensional (2D) van der Waals (vdW) materials with different quantum ground states is predicted to lead to novel electronic properties that are not found in the constituent layers. Here, we present the direct synthesis of superconductor-magnet hybrid heterostructures by combining superconducting niobium diselenide (NbSe$_2$) with the monolayer (ML) vanadium diselenide (VSe$_2$). More significantly, the in-situ growth in ultra-high vacuum (UHV) allows to produce a clean and an atomically sharp interfaces. Combining different characterization techniques and density-f…
A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 1,000 and 10,000 cm2/Vs at room and liquid-helium temperatures, respectively, allowing the observation of the fully…
Monolayer NbSe$_2$ is a nodal topological Ising superconductor at magnetic in-plane fields exceeding the Pauli limit, with nodal points strictly on high symmetry lines in the Brillouin zone. Here, we use a combined numerical and group-theoretical approach in real-space to characterize the unconventional superconducting state in monolayer transition metal dichalcogenides. Even with a conventional pairing interaction, the superconducting state is intrinsically parity-mixed and robust against on-site disorder. The interplay between the Zeeman magnetic field, strong spin-orbit interaction, and ele…
Two-dimensional boron structures, due to the diversity of properties, attract great attention because of their potential applications in nanoelectronic devices. A series of \ce{TiB_x} ($4\leq x \leq 11$) monolayers are efficiently constructed through our motif based method and theoretically investigated through high-throughput first-principles calculations. The configurations are generated based on motifs of boron triangular/quadrilateral fragments and multicoordinate titanium-centered boron molecular wheels. Besides priviously reported \ce{TiB4} which was discovered by global search method, w…
In this study, we report the mechanical properties and fracture mechanism of pre-cracked and defected InSe nanosheet samples using molecular dynamics (MD) simulations. We noticed that the failure of pre-cracked and defected InSe nanosheet is governed by brittle type fracture. Armchair directional bonds exhibit a greater resistance for crack propagation relative to the zigzag directional ones. Thus, fracture strength of the pre-cracked sheet is slightly higher for zigzag directional loading than that for armchair. We evaluated the limitation of the applicability of Griffith's criterion for sing…
Monolayer WTe$_2$, a centrosymmetric transition metal dichacogenide, has recently been established as a quantum spin Hall insulator and found superconducting upon gating. Here we study the pairing symmetry and topological nature of superconducting WTe$_2$ with a microscopic model at mean-field level. Surprisingly, we find that the spin-triplet phases in our phase diagram all host Majorana modes localized on two opposite corners. Even when the conventional pairing is favored, we find that an intermediate in-plane magnetic field exceeding the Pauli limit stabilizes an unconventional equal-spin p…
The pairing mechanism of high-temperature superconductivity in cuprates remains the biggest unresolved mystery in condensed matter physics. To solve the problem, one of the most effective approaches is to investigate directly the superconducting CuO2 layers. Here, by growing CuO2 monolayer films on Bi2Sr2CaCu2O8+δ substrates, we identify two distinct and spatially separated energy gaps centered at the Fermi energy, a smaller U-like gap and a larger V-like gap on the films, and study their interactions with alien atoms by low-temperature scanning tunneling microscopy. The newly discovered U-lik…
Enhanced Tantalum Superconducting Resonator Performance via All-Surface Organic Monolayer Passivation
Technical University of Munich（慕尼黑工业大学）；Indian Institute of Technology Roorkee（罗克基印度理工学院）；Fraunhofer Institute for Electronic Microsystems and Solid State Technologies (EMFT)（弗劳恩霍夫电子微系统和固态技术研究所）
The two-dimensional (2D) semiconductor indium selenide (InSe) has attracted significant interest due its unique electronic band structure, high electron mobility and wide tunability of its band gap energy achieved by varying the layer thickness. All these features make 2D InSe a potential candidate for advanced electronic and optoelectronic applications. Here, we report on the discovery of new polymorphs of InSe with enhanced electronic properties. Using a global structure search that combines artificial swarm intelligence with first-principles energetic calculations, we identify polymorphs th…
Recent studies on superconductivity in NbSe$_2$ have demonstrated a large anisotropy in the superconducting critical field when the material is reduced to a single monolayer. Motivated by this recent discovery, we use density functional theory (DFT) calculations to quantitatively address the superconducting properties of bulk and monolayer NbSe$_2$. We demonstrate that NbSe$_2$ is close to a ferromagnetic instability, and analyze our results in the context of experimental measurements of the spin susceptibility in NbSe$_2$. We show how this magnetic instability, which is pronounced in a single…
The capability to switch electrically between superconducting and insulating states of matter represents a novel paradigm in the state-of-the-art engineering of correlated electronic systems. An exciting possibility is to turn on superconductivity in a topologically non-trivial insulator, which provides a route to search for non-Abelian topological states. However, existing demonstrations of superconductor-insulator switches have involved only topologically trivial systems, and even those are rare due to the stringent requirement to tune the carrier density over a wide range. Here we report re…
We find that several layer-phase group-III monochalcogenides, including GaS, GaSe and InSe, are piezoelectric in the monolayer form. First-principles calculations reveal that the piezoelectric coefficients of monolayer GaS, GaSe and InSe are on the same order of magnitude as the earlier discovered two-dimensional piezoelectric materials, such as BN and MoS2 monolayers. Our study expands the family of two dimensional piezoelectric materials, suggesting that strong piezoelectric response can occur in a wide range of two dimensional materials with broken inversion symmetry. The co-existence of pi…
The ability to imprint a given material property to another through proximity effect in layered two-dimensional materials has opened the way to the creation of designer materials. Here, we use molecular-beam epitaxy (MBE) for a direct synthesis of a superconductor-magnet hybrid heterostructure by combining superconducting niobium diselenide (NbSe$_2$) with the monolayer ferromagnetic chromium tribromide (CrBr$_3$). Using different characterization techniques and density-functional theory (DFT) calculations, we have confirmed that the CrBr$_3$ monolayer retains its ferromagnetic ordering with a…
The exploration of superconductivity in low-dimensional materials has attracted intensive attention for decades. Based on first-principles electronic structure calculations, we have systematically investigated the electronic and superconducting properties of the two-dimensional electride Ba$_2$N in the monolayer limit. Our results show that monolayer Ba$_2$N has a low work function of 3.0 eV and a predicted superconducting transition temperature ($T_c$) of 3.4 K. The superconductivity can be further improved with the tensile strain, which results from the increase of density of states at the F…
We present a comprehensive study of the electronic structure of the layered semiconductor InSe using density functional theory. We calculate the band structure of the monolayer and bulk material with the band gap corrected using hybrid functionals. The band gap of the monolayer is 2.4 eV. The band edge states are surprising isotropic. The electron affinities and band offsets are then calculated for heterostructures as would be used in tunnel field effect transistors (TFETs). The ionization potential of InSe is quite large, similar to that of HfSe2 or SnSe2, and so InSe is suitable to act as th…
NbSe$_{2}$ and NbS$_{2}$ are isostructural two-dimensional materials that exhibit contrasting superconducting properties when reduced to the single monolayer limit. Monolayer NbSe$_{2}$ is an Ising superconductor, while there have been no reports of superconductivity in monolayer NbS$_{2}$. NbS$_{x}$Se$_{2-x}$ alloys exhibit an intriguing non-monotonic dependence of the superconducting transition temperature with sulfur content, which has been interpreted as a manifestation of fractal superconductivity. However, several key questions about this result are not known: (1) Does the electronic str…
High temporal stability of niobium superconducting resonators by surface passivation with organophosphonate self-assembled monolayers
Technical University of Munich（慕尼黑工业大学）；Fraunhofer Institute for Electronic Microsystems and Solid-State Technologies（弗劳恩霍夫电子微系统和固态技术研究所）；Walther-Meißner-Institut, Bayerische Akademie der Wissenschaften（瓦尔特·迈斯纳研究所，巴伐利亚科学院）
Two-dimensional (2D) atomic materials possess very different properties from their bulk counterparts. While changes in the single-particle electronic properties have been extensively investigated, modifications in the many-body collective phenomena in the exact 2D limit, where interaction effects are strongly enhanced, remain mysterious. Here we report a combined optical and electrical transport study on the many-body collective-order phase diagram of 2D NbSe$_2$. Both the charge density wave (CDW) and the superconducting phase have been observed down to the monolayer limit. While the supercon…
Spectroscopic evidence of disorder-induced quantum phase transitions in monolayer Fe(Te,Se) superconductor
Peking University（北京大学）；ShanghaiTech University（上海科技大学）；Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area (Guangdong)（粤港澳大湾区量子科学中心（广东））；Renmin University of China（中国人民大学）；The Ohio State University（俄亥俄州立大学）；Hefei National Laboratory（合肥国家实验室）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）
We investigate the effects of the in-plane biaxial strain and charge doping on the charge density wave (CDW) order of monolayer $1T$-TiSe$_2$ by using the first-principles calculations. Our results show that the tensile strain can significantly enhance the CDW order, while both compressive strain and charge doping (electrons and holes) suppress the CDW instability. The tensile strain may provide an effective method for obtaining higher CDW transition temperature on the basis of monolayer $1T$-TiSe$_2$. We also discuss the potential superconductivity in charge-doped monolayer $1T$-TiSe$_2$. Con…
Motivated by the high superconducting transition temperature of monolayer FeSe on SrTiO3, we propose a potential three-dimensional high-temperature superconductor superlattice FeSe-SrTiO3 and study its structural stability and electronic structure using density functional theory. We find that the binding energy between the FeSe and SrTiO3 layers is about 0.7 eV per (Fe2Se2) unit and that it saturates already within a single TiO2 atomic layer of SrTiO3. In addition we analyzed the dynamical stability of the superlattice and compared it to the case of bulk SrTiO3.
We show that electron-phonon coupling can induce strong electron pairing in an FeSe monolayer on a SrTiO3 substrate (experimental indications for superconducting Tc are between 65 and 109K). The role of the SrTiO3 substrate in increasing the coupling is two-fold. First, the interaction of the FeSe and TiO2 terminated face of SrTiO3 prevents the FeSe monolayer from undergoing a shear-type (orthorhombic, nematic) structural phase transition. Second, the substrate allows an anti-ferromagnetic ground state of FeSe which opens electron-phonon coupling channels within the monolayer that are prevente…
We performed angle-resolved photoemission spectroscopy studies on a series of FeTe$_{1-x}$Se$_{x}$ monolayer films grown on SrTiO$_{3}$. The superconductivity of the films is robust and rather insensitive to the variations of the band position and effective mass caused by the substitution of Se by Te. However, the band gap between the electron- and hole-like bands at the Brillouin zone center decreases towards band inversion and parity exchange, which drive the system to a nontrivial topological state predicted by theoretical calculations. Our results provide a clear experimental indication th…
It is well known that superconductivity in Fe-based materials is favoured under tetragonal symmetry, whereas competing orders such as spin-density-wave (SDW) and nematic orders emerge or are reinforced upon breaking the fourfold (C4) symmetry. Accordingly, suppression of orthorhombicity below the superconducting transition temperature (Tc) is found in underdoped compounds. Epitaxial film growth on selected substrates allows the design of crystal specific lattice distortions. Here we show that despite the breakdown of the C4 symmetry induced by a 5% difference in the lattice parameters, monolay…
Proximity effect facilitates the penetration of Cooper pairs that permits superconductivity in normal metal, offerring a promising approach to turn heterogeneous materials into superconducting and develop exceptional quantum phenomena. Here, we have systematically investigated proximity-induced anisotropic superconductivity in monolayer Ni-Pb binary alloy by combining scanning tunneling microscopy/ spectroscopy(STM/STS) with theoretical calculations. By means of high temperature growth, the(3root3by3root3)R30o Ni-Pb surface alloy has been fabricated on the Pb(111), where the appearance of doma…
The significantly enhanced superconducting transition temperature ($T_c$) of an FeSe monolayer on SrTiO$_3$(001) substrate has attracted extensive attention in recent years. Here, based on first-principles electronic structure calculations, we propose another candidate substrate LaO(001) for the epitaxial growth of FeSe monolayer to realize superconductivity. Our calculations show that for the optimal adsorption structure of FeSe monolayer on LaO(001), the stripe antiferromagnetic state and the dimer antiferromagnetic state are almost energetically degenerate, indicating the existence of stron…
