Effect of quantum confinement on the dielectric function of PbSe

Monolayers of lead selenide nanocrystals of a few nanometers in height have been made by electrodeposition on a Au(111) substrate. These layers show a thickness-dependent dielectric function, which was determined using spectroscopic ellipsometry. The experimental results are compared with electronic structure calculations of the imaginary part of the dielectric function of PbSe nanocrystals. We demonstrate that the size-dependent variation of the dielectric function is affected by quantum confinement at well-identifiable points in the Brillouin zone, different from the position of the band-gap transition

Dirac Cones, Topological Edge States, and Nontrivial Flat Bands in Two-Dimensional Semiconductors with a Honeycomb Nanogeometry

We study theoretically two-dimensional single-crystalline sheets of semiconductors that form a honeycomb lattice with a period below 10 nm. These systems could combine the usual semiconductor properties with Dirac bands. Using atomistic tight-binding calculations, we show that both the atomic lattice and the overall geometry influence the band structure, revealing materials with unusual electronic properties. In rocksalt Pb chalcogenides, the expected Dirac-type features are clouded by a complex band structure. However, in the case of zinc-blende Cd-chalcogenide semiconductors, the honeycomb nanogeometry leads to rich band structures, including, in the conduction band, Dirac cones at two distinct energies and nontrivial flat bands and, in the valence band, topological edge states. These edge states are present in several electronic gaps opened in the valence band by the spin-orbit coupling and the quantum confinement in the honeycomb geometry. The lowest Dirac conduction band has S-orbital character and is equivalent to the pi-pi* band of graphene but with renormalized couplings. The conduction bands higher in energy have no counterpart in graphene; they combine a Dirac cone and flat bands because of their P-orbital character. We show that the width of the Dirac bands varies between tens and hundreds of meV. These systems emerge as remarkable platforms for studying complex electronic phases starting from conventional semiconductors. Recent advancements in colloidal chemistry indicate that these materials can be synthesized from semiconductor nanocrystals.Comment: 12 pages, 12 figure

Statistical analysis of time-resolved emission from ensembles of semiconductor quantum dots: Interpretation of exponential decay models

We present a statistical analysis of time-resolved spontaneous emission decay curves from ensembles of emitters, such as semiconductor quantum dots, with the aim of interpreting ubiquitous non-single-exponential decay. Contrary to what is widely assumed, the density of excited emitters and the intensity in an emission decay curve are not proportional, but the density is a time integral of the intensity. The integral relation is crucial to correctly interpret non-single-exponential decay. We derive the proper normalization for both a discrete and a continuous distribution of rates, where every decay component is multiplied by its radiative decay rate. A central result of our paper is the derivation of the emission decay curve when both radiative and nonradiative decays are independently distributed. In this case, the well-known emission quantum efficiency can no longer be expressed by a single number, but is also distributed. We derive a practical description of non-single-exponential emission decay curves in terms of a single distribution of decay rates; the resulting distribution is identified as the distribution of total decay rates weighted with the radiative rates. We apply our analysis to recent examples of colloidal quantum dot emission in suspensions and in photonic crystals, and we find that this important class of emitters is well described by a log-normal distribution of decay rates with a narrow and a broad distribution, respectively. Finally, we briefly discuss the Kohlrausch stretched-exponential model, and find that its normalization is ill defined for emitters with a realistic quantum efficiency of less than 100%.\ud \u

Topological states in multi-orbital HgTe honeycomb lattices

Research on graphene has revealed remarkable phenomena arising in the honeycomb lattice. However, the quantum spin Hall effect predicted at the K point could not be observed in graphene and other honeycomb structures of light elements due to an insufficiently strong spin-orbit coupling. Here we show theoretically that 2D honeycomb lattices of HgTe can combine the effects of the honeycomb geometry and strong spin-orbit coupling. The conduction bands, experimentally accessible via doping, can be described by a tight-binding lattice model as in graphene, but including multi-orbital degrees of freedom and spin-orbit coupling. This results in very large topological gaps (up to 35 meV) and a flattened band detached from the others. Owing to this flat band and the sizable Coulomb interaction, honeycomb structures of HgTe constitute a promising platform for the observation of a fractional Chern insulator or a fractional quantum spin Hall phase.Comment: includes supplementary materia

Planar nanocontacts with atomically controlled separation

We have developed a technology to reproducibly make gaps with distance control on the single atom scale. The gold contacts are flat on the nanometre scale and are fabricated on an oxidized aluminium film that serves as a gate. We show that these contacts are clean and can be stabilized via chemical functionalization. Deposition of conjugated molecules leads to an increase in the gap conductance of several orders of magnitude. Stable current-voltage characteristics at room temperature are slightly nonlinear. At low temperature, they are highly nonlinear and show a clear gate effect.Comment: 4 pages, 3 figure

Wide energy-window view on the density of states and hole mobility of poly(p-phenylene vinylene)

Using an electrochemically gated transistor, we achieved controlled and reversible doping of poly(p-phenylene vinylene) in a large concentration range. Our data open a wide energy-window view on the density of states (DOS) and show, for the first time, that the core of the DOS function is Gaussian, while the low-energy tail has a more complex structure. The hole mobility increases by more than four orders of magnitude when the electrochemical potential is scanned through the DOS.Comment: 4 pages, 4 figure

Robust zero-energy modes in an electronic higher-order topological insulator: the dimerized Kagome lattice

Quantum simulators are an essential tool for understanding complex quantum materials. Platforms based on ultracold atoms in optical lattices and photonic devices led the field so far, but electronic quantum simulators are proving to be equally relevant. Simulating topological states of matter is one of the holy grails in the field. Here, we experimentally realize a higher-order electronic topological insulator (HOTI). Specifically, we create a dimerized Kagome lattice by manipulating carbon-monoxide (CO) molecules on a Cu(111) surface using a scanning tunneling microscope (STM). We engineer alternating weak and strong bonds to show that a topological state emerges at the corner of the non-trivial configuration, while it is absent in the trivial one. Contrarily to conventional topological insulators (TIs), the topological state has two dimensions less than the bulk, denoting a HOTI. The corner mode is protected by a generalized chiral symmetry, which leads to a particular robustness against perturbations. Our versatile approach to quantum simulation with artificial lattices holds promises of revealing unexpected quantum phases of matter

Efficient steplike carrier multiplication in percolative networks of epitaxially connected PbSe nanocrystals

Carrier multiplication (CM) is a process in which a single photon excites two or more electrons. CM is of interest to enhance the efficiency of a solar cell. Until now, CM in thin films and solar cells of semiconductor nanocrystals (NCs) has been found at photon energies well above the minimum required energy of twice the band gap. The high threshold of CM strongly limits the benefits for solar cell applications. We show that CM is more efficient in a percolative network of directly connected PbSe NCs. The CM threshold is at twice the band gap and increases in a steplike fashion with photon energy. A lower CM efficiency is found for a solid of weaker coupled NCs. This demonstrates that the coupling between NCs strongly affects the CM efficiency. According to device simulations, the measured CM efficiency would significantly enhance the power conversion efficiency of a solar cell

Frequency-dependent spontaneous emission rate from CdSe and CdTe nanocrystals: influence of dark states

We studied the rate of spontaneous emission from colloidal CdSe and CdTe nanocrystals at room temperature. The decay rate, obtained from luminescence decay curves, increases with the emission frequency in a supra-linear way. This dependence is explained by the thermal occupation of dark exciton states at room temperature, giving rise to a strong attenuation of the rate of emission. The supra-linear dependence is in agreement with the results of tight-binding calculations.Comment: 11 page