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Daniel Vanmaekelbergh

Publications and source records attributed to Daniel Vanmaekelbergh.

8 recordsLinked to original sources

Vanishing quantum confinement enables bright and thermally excited multi-carrier emission from semiconductor nanocrystals

Recently, nanocrystals in the regime of vanishing quantum confinement-termed bulk nanocrystals (BNCs)-have demonstrated remarkable optical gain characteristics. While their high-power lasing performance was demonstrated convincingly, the photophysics at low and intermediate powers-where charge-carrier populations are discrete-remain unexplored. Using single-photon avalanche diode (SPAD) array technology, we resolve the dynamics and energetics of six multi-carrier excited states in individual CdSe/CdS core/shell BNCs, containing up to four electrons and two holes. Each state exhibits bimodal emission, indicative of thermal equilibrium between closely spaced electron and hole levels, confirmed via temperature-dependent single-particle measurements. Quantification of radiative and nonradiative decay channels reveals strongly suppressed Auger recombination through both the negative- and positive-trion pathways. We present a model that combines statistical scaling of rate constants with Fermi-Dirac thermal occupations of electron and hole levels, bridging the transitional regime between quantum-confined and bulk nanocrystals, and providing a comprehensive framework for understanding this emerging class of materials.

cond-mat.mtrl-sci

Non-Topological Edge-Localized Yu-Shiba-Rusinov States in CrBr$_3$/NbSe$_2$ Heterostructures

Topological superconductivity is predicted to emerge in certain magnet-superconductor hybrid systems. Here, we revisit the heterostructure of insulating monolayer CrBr$_3$ and NbSe$_2$, for which different conclusions on the presence of topological superconductivity have been reported. Using low-temperature scanning tunneling microscopy and (shot noise) spectroscopy, we find that the superconducting gap well inside the CrBr3 islands is not affected by magnetism. At the island edges, we observe Yu-Shiba-Rusinov (YSR) states at a variety of in-gap positions, including zero energy. The absence of topological superconductivity is verified by extensive dI/dV measurements at the CrBr$_3$ island edges. Our results ask for a more detailed understanding of the interaction between magnetic insulators and superconductors.

cond-mat.supr-con

Topology of Bi$_2$Se$_3$ nanosheets

Recently, the quantum spin-Hall edge channels of two-dimensional colloidal nanocrystals of the topological insulator Bi$_2$Se$_3$ were observed directly. Motivated by this development, we reconsider the four-band effective model which has been traditionally employed in the past to describe thin nanosheets of this material. Derived from a three-dimensional $\boldsymbol{k} \boldsymbol{\cdot} \boldsymbol{p}$ model, it physically describes the top and bottom electronic surface states at the $Γ$ point that become gapped due to the material's small thickness. However, we find that the four-band model for the surface states alone, as derived directly from the three-dimensional theory, is inadequate for the description of thin films of a few quintuple layers and even yields an incorrect topological invariant within a significant range of thicknesses. To address this limitation we propose an eight-band model which, in addition to the surface states, also incorporates the set of bulk states closest to the Fermi level. We find that the eight-band model not only captures most of the experimental observations, but also agrees with previous first-principles calculations of the $\mathbb{Z}_{2}$ invariant in thin films of varying thickness. The band inversion around the $Γ$ point, which endows the surface-like bands with topology, is shown to be enabled by the presence of the additional bulk-like states without requiring any reparametrization of the resulting effective Hamiltonian.

cond-mat.mes-hall

Electronic properties of atomically coherent square PbSe nanocrystal superlattice resolved by STS

Rock-salt lead selenide nanocrystals can be used as building blocks for large scale square superlattices via two-dimensional assembly of nanocrystals at a liquid-air interface followed by oriented attachment. Here we report measurements of the local density of states of an atomically coherent superlattice with square geometry made from PbSe nanocrystals. Controlled annealing of the sample permits the imaging of a clean structure and to reproducibly probe the band gap and the valence hole and conduction electron states. The measured band gap and peak positions are compared to the results of optical spectroscopy and atomistic tight-binding calculations of the square superlattice band structure. In spite of the crystalline connections between nanocrystals that induce significant electronic couplings, the electronic structure of the superlattices remains very strongly influenced by the effects of disorder and variability.

cond-mat.mtrl-sci

Observation of the quantized motion of excitons in CdSe nanoplatelets

We show that the finite lateral sizes of ultrathin CdSe nanoplatelets strongly affect both their photoluminescence and optical absorption spectra. This is in contrast to the situation in quantum wells, in which the large lateral sizes may be assumed to be infinite. The lateral sizes of the nanoplatelets are varied over a range of a few to tens of nanometers. For these sizes excitons experience in-plane quantum confinement, and their center-of-mass motion becomes quantized. Our direct experimental observation of the discretization of the exciton center-of-mass states can be well understood on the basis of the simple particle-in-a-box model.

cond-mat.mes-hall

p Orbital flat band and Dirac cone in the electronic honeycomb lattice

Theory anticipates that the in-plane px, py orbitals in a honeycomb lattice lead to new and potentially useful quantum electronic phases. So far, p orbital bands were only realized for cold atoms in optical lattices and for light and exciton-polaritons in photonic crystals. For electrons, in-plane p orbital physics is difficult to access since natural electronic honeycomb lattices, such as graphene and silicene, show strong s-p hybridization. Here, we report on electronic honeycomb lattices prepared on a Cu(111) surface in a scanning tunneling microscope that, by design, show (nearly) pure orbital bands, including the p orbital flat band and Dirac cone.

cond-mat.mes-hall

Experimental realization and characterization of an electronic Lieb lattice

Geometry, whether on the atomic or nanoscale, is a key factor for the electronic band structure of materials. Some specific geometries give rise to novel and potentially useful electronic bands. For example, a honeycomb lattice leads to Dirac-type bands where the charge carriers behave as massless particles. Theoretical predictions are triggering the exploration of novel 2D geometries, such as graphynes, Kagomé and the Lieb lattice. The latter is the 2D analogue of the 3D lattice exhibited by perovskites; it is a square-depleted lattice, which is characterised by a band structure featuring Dirac cones intersected by a topological flat band. Whereas photonic and cold-atom Lieb lattices have been demonstrated, an electronic equivalent in 2D is difficult to realize in an existing material. Here, we report an electronic Lieb lattice formed by the surface state electrons of Cu(111) confined by an array of CO molecules positioned with a scanning tunneling microscope (STM). Using scanning tunneling microscopy, spectroscopy and wave-function mapping, we confirm the predicted characteristic electronic structure of the Lieb lattice. The experimental findings are corroborated by muffin-tin and tight-binding calculations. At higher energy, second-order electronic patterns are observed, which are equivalent to a super-Lieb lattice.

cond-mat.mes-hall

Non-blinking single-photon emitters in silica

Samples for single-emitter spectroscopy are usually prepared by spin-coating a dilute solution of emitters on a microscope cover slip of silicate based glass (such as quartz). Here, we show that both borosilicate glass and quartz contain intrinsic defect colour centres that fluoresce when excited at 532 nm. In a microscope image the defect emission is indistinguishable from spin-coated emitters. The emission spectrum is characterised by multiple peaks, most likely due to coupling to a silica vibration with an energy of 160-180 meV. The defects are single-photon emitters, do not blink, and have photoluminescence lifetimes of a few nanoseconds. Photoluminescence from such defects may previously have been misinterpreted as originating from single nanocrystal quantum dots.

cond-mat.mtrl-sci