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Semiconducting heterojunctions (HJs), comprised of atomically thin transition metal dichalcogenides (TMDs), have shown great potentials in electronic and optoelectronic applications. Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons, tunable electronic structures and optical properties, and other superior advantages to these inorganic HJs. Here, we report a direct probe of the interfacial electronic structures of a crystalline monolayer (ML) perylene-3,4,9,10-tetracarboxylic-dianhydride (PTCDA)/ML-WSe2 HJ using scanning tunneling microscopy, photoluminescence, and first-principle calculations. Strong PTCDA/WSe2 interfacial interactions lead to appreciable hybridization of the WSe2 conduction band with PTCDA unoccupied states, accompanying with a significant amount of PTCDA-to-WSe2 charge transfer (by 0.06 e/PTCDA). A type-II band alignment was directly determined with a valence band offset of ∼ 1.69 eV, and an apparent conduction band offset of ∼ 1.57 eV. Moreover, we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.

Stacking of two-dimensional (2D) van der Waals (vdW) atomic sheets has been established as a powerful approach to fabricating new materials with broad versatilities and emergent functionalities. Here we demonstrate a bottom-up approach to fabricating isolated single W6Te6 wires and their lateral assemblies, offering a unique platform for investigating the elegant role of vdW coupling in 1D systems with atomic precision. We find experimentally and theoretically a single W6Te6 wire is a 1D semiconductor with a band gap of ∼60 meV, and a semiconductor-to-metal transition takes place upon interwire vdW stacking. The metallic multiwires exhibit strong Tomonaga-Luttinger liquid characteristics with the correlation parameter g varying from g = 0.086 for biwire to g = 0.136 for six-wire assemblies, all much reduced from the Fermi liquid regime (g = 1). The present study demonstrates wire-by-wire vdW stacking is a versatile means for fabrication of 1D systems with tunable electronic properties.

The fabrication of one-dimensional (1D) magnetic systems on solid surfaces, although of high fundamental interest, has yet to be achieved for a crossover between two-dimensional (2D) magnetic layers and their associated 1D spin chain systems. In this study, we report the fabrication of 1D single-unit-cell-width CrCl3 atomic wires and their stacked few-wire arrays on the surface of a van der Waals (vdW) superconductor NbSe2. Scanning tunneling microscopy/spectroscopy and first-principles calculations jointly revealed that the single wire shows an antiferromagnetic large-bandgap semiconducting state in an unexplored structure different from the well-known 2D CrCl3 phase. Competition among the total energies and nanostructure-substrate interfacial interactions of these two phases result in the appearance of the 1D phase. This phase was transformable to the 2D phase either prior to or after the growth for in situ or ex situ manipulations, in which the electronic interactions at the vdW interface play a nontrivial role that could regulate the dimensionality conversion and structural transformation between the 1D-2D CrCl3 phases., Comment: 4 figures

The hybridization of magnetism and superconductivity has been an intriguing playground for correlated electron systems, hosting various novel physical phenomena. Usually, localized d- or f-electrons are central to magnetism. In this study, by placing a PTCDA (3,4,9,10-perylene tetracarboxylic dianhydride) molecular monolayer on ultra-thin Pb films, we built a hybrid magnetism/superconductivity (M/SC) system consisting of only sp electronic levels. The magnetic moments reside in the unpaired molecular orbital originating from interfacial charge-transfers. We reported distinctive tunneling spectroscopic features of such a Kondo screened pi-electron impurity lattice on a superconductor in the regime of TK>>delta suggesting the formation of a two-dimensional bound states band. Moreover, moir\'e superlattices with tunable twist angle and the quantum confinement in the ultra-thin Pb films provide easy and flexible implementations to tune the interplay between the Kondo physics and the superconductivity, which are rarely present in M/SC hybrid systems., Comment: 4 figures

Manipulation of artificial molecular rotors/motors is a key issue in the field of molecular nanomachines. Here we assemble non-planar SnPc molecules on an FeO film to form two kinds of rotors with different apparent morphologies, rotational speeds and stabilities. Both kinds of rotors can switch to each other

Description, 1T-NbSe2 is a correlated insulator with localized magnetic moments exhibiting Kondo resonances when exchange-coupled to 2H-NbSe2., Monolayer group V transition metal dichalcogenides in their 1T phase have recently emerged as a platform to investigate rich phases of matter, such as spin liquid and ferromagnetism, resulting from strong electron correlations. Newly emerging 1T-NbSe2 has inspired theoretical investigations predicting collective phenomena such as charge transfer gap and ferromagnetism in two dimensions; however, the experimental evidence is still lacking. Here, by controlling the molecular beam epitaxy growth parameters, we demonstrate the successful growth of high-quality single-phase 1T-NbSe2. By combining scanning tunneling microscopy/spectroscopy and ab initio calculations, we show that this system is a charge transfer insulator with the upper Hubbard band located above the valence band maximum. To demonstrate the electron correlation resulted magnetic property, we create a vertical 1T/2H NbSe2 heterostructure, and we find unambiguous evidence of exchange interactions between the localized magnetic moments in 1T phase and the metallic/superconducting phase exemplified by Kondo resonances and Yu-Shiba-Rusinov–like bound states.

Stacking of two-dimensional (2D) van der Waals (vdW) atomic sheets has been established as a powerful approach to fabricating new materials with broad versatilities and emergent functionalities. Here we demonstrate a bottom-up approach to fabricating isolated single W

Monolayer and few layer antimony allotropes fabricated on oxide layers are essential for practical applications in fields of solar cells, electronic and photonic devices. Here the antimony structural phases are systemically studied on corrugated copper oxide of Cu(111) by atomically-resolved scanning tunneling microscopy (STM). We find that initial deposition of Sb atoms causes the structural changes of the underlying oxide layer and sequentially gives rise to the formation of flat (√7 × √7)-Sb and buckled antimonene phases. Finally, a nanoring-like antimony configuration is observed with triangle-shaped atomic arrays closely packing and shows high stabilities for oxygen exposure. The (√7 × √7) phase exhibits the metallic property with energetically continuous electronic states existing near Fermi level. For the antimonene and nanoring phases, band gap signatures are observed, implying the semiconducting features. Our results provide a method for fabricating stable elemental allotropes on oxide surfaces.

Significant work function changes from bare Pt(111) surface to 1 monolayer and 2 monolayers of ultrathin iron oxide (FeO) films on it are investigated by means of scanning tunneling microscopy/spectroscopy (STM/STS). With FeO layer-by-layer growth, a continuous reduction of the work function along with the surface vacuum level (VL) shifting is observed. We found that the compression of the electron spill-out at the metal-oxide interface and the substantial reconstruction of 2 ML FeO film, respectively, make major contributions to the first and the second reductions of the work function. The rectifying effect in FeO films is also observed, which is attributed to the downward shift of band alignment imposed by the total change in surface dipole. Our work shows that the polar oxide films play an important role to adjust surface electronic structures for enhancing device functionality.

Antimony nanostructures fabricated on metal oxide layers are essential for practical applications in fields of solar cells, electronic and photonic devices. Here the antimony phases were systemically studied on the copper oxide of Cu(110). By high-resolution scanning tunneling microscopy (STM), we revealed that a wrinkled antimony phase was formed on the CuO surface regardless of the initial oxide structure. It exhibited an armchair-like configuration making up of protruded and dipped Sb atoms as confirmed by STM and density functional theory calculations. Further Sb deposition caused the armchair-like phase distorting and subsequently gave rise to formation of a c(2 × 2)-Sb phase. Finally, another kind of wrinkled phase was successfully fabricated. It consisted of two zigzagged antimony chains with protruded and dipped Sb atoms alternately distributing. By analysis of the atomically-resolved STM topographies, several kinds of dislocations have been observed and the corresponding geometric models are addressed. The armchair and zigzag phases both exhibited high stabilities for oxygen exposure. Conductance measurements imply that each phase interacts with the underlying layer. Our results might provide a way for fabricating stable ultrathin materials with a well-defined edge structure on oxide surfaces.

The photoluminescence (PL) properties of a GaInP epilayer with an ultrathin AlAs interfacial layer grown on Ge were investigated by time-resolved photoluminescence spectroscopy and temperature-dependent PL spectroscopy. A double-exponential PL decay with two time constants was observed, where the fast component is attributed to the emission from ordered GaInP while the slow component is related to localized states. Increased thickness of the AlAs interfacial layer resulted in an increased PL decay time due to the increased degree of order of the GaInP. Furthermore, the broad PL peak around 1.57 eV appearing in the GaInP epilayer after insertion of the AlAs layer might be attributed to phosphorus-vacancy-related deep levels.

Structure and optical properties of GaInP epilayer with the ultrathin interfacial layers grown on germanium by metal–organic vapor-phase epitaxy (MOVPE) were characterized by high resolution transmission electron microscopy (HRTEM), photoluminescence (PL), Raman as well as surface morphology measurement. A five angstroms (5 A) AlAs interfacial layer results in the decrease of PL intensity arising from the emission of [Ge (Ga,In) − V (Ga,In) ] complex. With the incorporation of AlAs interfacial layer, an increased ordered degree of GaInP epilayer is observed. On the basis of the combination of step–terrace-reconstruction (STR) mode with the dimer-induced-stress model, a CuPt-B type ordering of GaInP which is related to AlAs reconstruction with 2× periodicity process is proposed to explain this effect. Long range order occurs as a consequence of the minimization of the strain energy with increased interfacial layer thickness from 5 A to 5 nm.

Molecular rotors, motors and gears play important roles in artificial molecular machines, in which rotor and motor matrices are highly desirable for large-scale bottom-up fabrication of molecular machines. Here we demonstrate the fabrication of a highly ordered molecular rotor matrix by depositing nonplanar dipolar titanyl phthalocyanine (TiOPc, C32H16N8OTi) molecules on a Moire patterned dipolar FeO/Pt(111) substrate. TiOPc molecules with O atoms pointing outwards from the substrate (upward) or towards the substrate (downward) are alternatively adsorbed on the fcc sites by strong lateral confinement. The adsorbed molecules, i.e. two kinds of molecular rotors, show different scanning tunneling microscopy images, thermal stabilities and rotational characteristics. Density functional theory calculations clarify that TiOPc molecules anchoring upwards with high adsorption energies correspond to low-rotational-rate rotors, while those anchoring downwards with low adsorption energies correspond to high-rotational-rate rotors. A robust rotor matrix fully occupied by low-rate rotors is fabricated by depositing molecules on the substrate at elevated temperature. Such a paradigm opens up a promising route to fabricate functional molecular rotor matrices, driven motor matrices and even gear groups on solid substrates.

Bernal-stacked bilayer germanene with a stable buckled honeycomb structure has been successfully synthesized on Cu(111). Structural and electronic characterizations as well as theoretical calculations unequivocally demonstrate for the first time the presence of a nearly linear energy dispersion in the vicinity of the Fermi energy, as expected of the Dirac signature for theoretical freestanding germanene.

Germanene, a one-atom-thick Ge layer with a honeycomb structure is prepared in an ultra-high vacuum system by deposition of Ge on Pt(111) at room temperature followed by annealing at 600—750 K for 30 min.

Germanene, a 2D honeycomb lattice analogous to graphene, is fabricated on a Pt(111) surface. It exhibits a buckled configuration with a (3 x 3) superlattice coinciding with the substrate's (root 19 x root 19) superstructure. Covalent bonds exist throughout the germanene layer. The resulting high-quality germanene enables researchers to explore the fundamentals of germanene and its potential applications.

Tailoring of the assembly structure of organic molecular monolayer is of great importance to improve the performance of molecular devices. In this work, a typical ionic compound, namely KCl, was used to mediate the rearrangement of 3, 4, 9, 10-perylene tetracarboxylic dianhydride (PTCDA) monolayer on Ag(100). Combined scanning tunneling microscopy (STM) and low energy electron diffraction (LEED) results indicate that both molecule and molecular superlattice would rotate after the dosing of KCl. The density functional theory calculation shows that KCl would exist in the form of molecules rather than ions on Ag(100) and demonstrates that experimentally observed structural transition induced by KCl molecules is energetically favored.

The growth, structure of Pt(111) supported double-layer FeO and the adsorption of titanyl phthalocyanine (TiOPc) molecules with tunable site and orientation were presented. According to the atomic-resolution STM image, the structure was rationalized as (8 root 3 x 8 root 3) R30 degrees/Pt(111) nanostructure constructed by Fe species coordinated with different number of oxygen on top of nonrotated (8 x 8) FeO/Pt(111) structure. Due to the modulation of the stacking of Fe atoms in the second layer relative to the O atoms in the second layer and the underlying layer, the interface and total dipole moment periodically vary within (8 root 3 x 8 root 3) R30 degrees/Pt(111) structure. The resulted periodically distributed dipole-dipole interaction benefits the growth of TiOPc molecules with area-selective sites and molecular orientations. Thus, this study provides a reliable method to govern the adsorption process of the polar molecules for potential applications in future functional molecular devices. (C) 2014 AIP Publishing LLC.