Concept: Electronic band structure
Ultralow trap densities, exceptional optical and electronic properties have been reported for lead halide perovskites single crystals; however, ambiguities in basic properties, such as the band gap, and the electronic defect densities in the bulk and at the surface prevail. Here, we synthesize single crystals of methylammonium lead bromide (CH3NH3PbBr3), characterise the optical absorption and photoluminescence and show that the optical properties of single crystals are almost identical to those of polycrystalline thin films. We observe significantly longer lifetimes and show that carrier diffusion plays a substantial role in the photoluminescence decay. Contrary to many reports, we determine that the trap density in CH3NH3PbBr3 perovskite single crystals is 10(15) cm(-3), only one order of magnitude lower than in the thin films. Our enhanced understanding of optical properties and recombination processes elucidates ambiguities in earlier reports, and highlights the discrepancies in the estimation of trap densities from electronic and optical methods.Metal halide perovskites for optoelectronic devices have been extensively studied in two forms: single-crystals or polycrystalline thin films. Using spectroscopic approaches, Wenger et al. show that polycrystalline thin films possess similar optoelectronic properties to single crystals.
In a continuous search for the energy-efficient electronic switches, a great attention is focused on tunnel field-effect transistors (TFETs) demonstrating an abrupt dependence of the source-drain current on the gate voltage. Among all TFETs, those based on one-dimensional (1D) semiconductors exhibit the steepest current switching due to the singular density of states near the band edges, though the current in 1D structures is pretty low. In this paper, we propose a TFET based on 2D graphene bilayer which demonstrates a record steep subthreshold slope enabled by van Hove singularities in the density of states near the edges of conduction and valence bands. Our simulations show the accessibility of 3.5 × 10(4) ON/OFF current ratio with 150 mV gate voltage swing, and a maximum subthreshold slope of (20 μV/dec)(-1) just above the threshold. The high ON-state current of 0.8 mA/μm is enabled by a narrow (~0.3 eV) extrinsic band gap, while the smallness of the leakage current is due to an all-electrical doping of the source and drain contacts which suppresses the band tailing and trap-assisted tunneling.
Self-assembly of biological molecules on solid materials is central to the “bottom-up” approach to directly integrate biology with electronics. Inspired by biology, exquisite biomolecular nanoarchitectures have been formed on solid surfaces. We demonstrate that a combinatorially-selected dodecapeptide and its variants self-assemble into peptide nanowires on two-dimensional nanosheets, single-layer graphene and MoS2. The abrupt boundaries of nanowires create electronic junctions via spatial biomolecular doping of graphene and manifest themselves as a self-assembled electronic network. Furthermore, designed peptides form nanowires on single-layer MoS2 modifying both its electric conductivity and photoluminescence. The biomolecular doping of nanosheets defined by peptide nanostructures may represent the crucial first step in integrating biology with nano-electronics towards realizing fully self-assembled bionanoelectronic devices.
The newly discovered two-dimensional materials can be used to form atomically thin and sharp van der Waals heterostructures with nearly perfect interface qualities, which can transform the science and technology of semiconductor heterostructures. Owing to the weak van der Waals interlayer coupling, the electronic states of participating materials remain largely unchanged. Hence, emergent properties of these structures rely on two key elements: electron transfer across the interface and interlayer coupling. Here we show, using graphene-tungsten disulfide heterostructures as an example, evidence of ultrafast and highly efficient interlayer electron transfer and strong interlayer coupling and control. We find that photocarriers injected in tungsten disulfide transfer to graphene in 1 ps and with near-unity efficiency. We also demonstrate that optical properties of tungsten disulfide can be effectively tuned by carriers in graphene. These findings illustrate basic processes required for using van der Waals heterostructures in electronics and photonics.
Commonly, materials are classified as either electrical conductors or insulators. The theoretical discovery of topological insulators has fundamentally challenged this dichotomy. In a topological insulator, the spin-orbit interaction generates a non-trivial topology of the electronic band structure dictating that its bulk is perfectly insulating, whereas its surface is fully conducting. The first topological insulator candidate material put forward-graphene-is of limited practical use because its weak spin-orbit interactions produce a bandgap of ~ 0.01 K. Recent reexaminations of Bi2Se3 and Bi2Te3, however, have firmly categorized these materials as strong three-dimensional topological insulators. We have synthesized the first bulk material belonging to an entirely different, weak, topological class, built from stacks of two-dimensional topological insulators: Bi14Rh3I9. Its Bi-Rh sheets are graphene analogues, but with a honeycomb net composed of RhBi8 cubes rather than carbon atoms. The strong bismuth-related spin-orbit interaction renders each graphene-like layer a topological insulator with a 2,400 K bandgap.
Memory cells are an important building block of digital electronics. We combine here the unique electronic properties of semiconducting monolayer MoS2 with the high conductivity of graphene to build a 2D heterostructure capable of information storage. MoS2 acts as a channel in an intimate contact with graphene electrodes in a field-effect transistor geometry. Our prototypical all-2D transistor is further integrated with a multilayer graphene charge trapping layer into a device that can be operated as a nonvolatile memory cell. Because of its band gap and 2D nature, monolayer MoS2 is highly sensitive to the presence of charges in the charge trapping layer, resulting in a factor of 10(4) difference between memory program and erase states. The two-dimensional nature of both the contact and the channel can be harnessed for the fabrication of flexible nanoelectronic devices with large-scale integration.
We study multiple electron transfer from a CdSe quantum dot (QD) to ZnO, which is a prerequisite for successful utilization of multiple exciton generation for photovoltaics. By using ultrafast time-resolved spectroscopy we observe competition between electron injection into ZnO and quenching of multiexcitons via Auger recombination. We show that fast electron injection dominates over biexcitonic Auger recombination and multiple electrons can be transferred into ZnO. A kinetic component with time constant of a few tens of picoseconds was identified as the competition between injection of the second electron from a doubly excited QD and a trion Auger recombination. Moreover, we demonstrate that the multiexciton harvesting efficiency changes significantly with QD size. Within a narrow QD diameter range from 2 nm to 4 nm, the efficiency of electron injection from a doubly-excited QD can vary from 30% to 70% in our system.
Two kinds of Cu(2)O-ZnO nano-heteroarchitectures were fabricated through a hydrothermal method. By utilizing polyethyleneimine (PEI) as a binding agent, ZnO nanoparticles were uniformly self-assembled onto Cu(2)O micro structures. Photoluminescence (PL), field emission and photocatalytic activities of the composite samples were investigated and compared with those of the pure Cu(2)O samples. The results reveal that ZnO nanoparticles combined on Cu(2)O microstructures remarkably changed the PL signals, and significantly enhanced the field emission and photocatalytic activities. The novel PL properties, enhanced field emission and photocatalysis activities are attributed to the electron transition and the inhibition of photo-induced electron-hole pairs recombination, which stem from interfacial defect states and energy band differentials at the interface of Cu(2)O and ZnO. The surface nano-protrusions, large surface area and better dye adsorption induced by ZnO nanoparticles are responsible for the field emission and photocatalysis improvements as well.
Nonblinking excitonic emission from near-infrared and type-II nanocrystal quantum dots (NQDs) is reported for the first time. To realize this unusual degree of stability at the single-dot level, novel InP/CdS core/shell NQDs were synthesized for a range of shell thicknesses (∼1-11 monolayers of CdS). Ensemble spectroscopy measurements (photoluminescence peak position and radiative lifetimes) and electronic structure calculations established the transition from type-I to type-II band alignment in these heterostructured NQDs. More significantly, single-NQD studies revealed clear evidence for blinking suppression that was not strongly shell-thickness dependent, while photobleaching and biexciton lifetimes trended explicitly with extent of shelling. Specifically, very long biexciton lifetimes-up to >7 ns-were obtained for the thickest-shell structures, indicating dramatic suppression of nonradiative Auger recombination. This new system demonstrates that electronic structure and shell thickness can be employed together to effect control over key single-dot and ensemble NQD photophysical properties.
Photocatalysis is a promising advanced water treatment technology, and recently the possibility of using hydrogenation to improve the photocatalytic efficiency of titanium dioxide has generated much research interest. Herein we report that the use of high temperature hydro-genation to prepare black TiO2 primarily results in the for-mation of bulk defects in the material without affecting its electronic band structure. The hydrogenated TiO2 exhibited significantly worse photocatalytic activity under simulated sunlight compared to the unhydrogenated control, and thus we propose that high temperature hydrogenation can be counterproductive to improving the photocatalytic activity of TiO2, due to its propensity to form bulk vacancy defects.