Two-dimensional colloidal nanoplatelets (NPLs), owing to the atomic-level control of their confined direction (i.e., no inhomogeneous broadening), have demonstrated improved photoluminescence (PL) line widths for cadmium chalcogenide-based nanocrystals. Here we use cation exchange to synthesize mercury chalcogenide NPLs. Appropriate control of reaction kinetics enables the 2D morphology of the NPLs to be maintained during the cation exchange. HgTe and HgSe NPLs have significantly improved optical features compared to existing materials with similar band gaps. The PL line width of HgTe NPLs (40 nm full width at half-maximum, centered at 880 nm) is a factor of 2 smaller than typical PbS nanocrystals (NCs) emitting at the same wavelength. The PL has a lifetime of 50 ns, almost 2 orders of magnitude shorter than small PbS colloidal quantum dots (CQDs), and a quantum yield of ∼10%, almost 2 orders of magnitude shorter than small PbS colloidal quantum dots (CQDs). These materials are promising for a large variety of applications spanning from telecommunications to the design of colloidal topological insulators.
We investigate the electronic and transport properties of HgTe 2D colloidal quantum wells. We demonstrate that the material can be made p- or n-type depending on the capping ligands. In addition to the control of majority carrier type, the surface chemistry also strongly affects the photoconductivity of the material. These transport measurements are correlated with the electronic structure determined by high resolution X-ray photoemission. We attribute the change of majority carriers to the strong hybridization of an n-doped HgS layer resulting from capping the HgTe nanoplatelets by S ions. We further investigate the gate and temperature dependence of the photoresponse and its dynamics. We show that the photocurrent rise and fall times can be tuned from 100 μs to 1 ms using the gate bias. Finally, we use time-resolved photoemission spectroscopy as a probe of the transport relaxation to determine if the observed dynamics are limited by a fundamental process such as trapping. These pump probe surface photovoltage measurements show an even faster relaxation in the 100-500 ns range, which suggests that the current performances are rather limited by geometrical factors.
Among colloidal nanocrystals, 2D nanoplatelets (NPL) made of II-VI compounds, appear as a special class of emitters with especially narrow photoluminescence signal. However the PL signal in the case of NPL is only tunable by discrete step. Here we demonstrate that doping is a viable path to finely tune the color of this NPL from green to red, making them extremely interesting as phosphor for wide gamut display. In addition using a combination of luminescence spectroscopy, tight binding simulation, transport and photoemission, we provide a consistent picture for the Ag doped CdSe NPL. The Ag state is strongly bound and located 340 meV above the valence band of the bulk material. The Ag dopant shifts the Fermi level toward the valence by up to 400 meV but preserve the n-type nature of the material.
Colloidal quantum dots (QDs) are now being used as the new generation of phosphor for displays. White light is obtained by combining the blue emission of a diode with green and red population of QDs. Having bicolor emission within a single nanocrystal population can be even more convenient. Here, we demonstrate that bicolor emission can be obtained from 2D nanoplatelets (NPLs) with a core/crown geometry. In CdSe/CdTe NPLs with type II band alignment, only the charge transfer emission was observed so far due to the very fast (
Among semiconductor nanocrystals (NCs), 2D nanoplatelets (NPLs) are a special class of nanomaterials with well controlled optical features. So far most of the efforts have been focused on wide band gap materials such as cadmium chalcogenide semiconductors. However, optical absorption can be pushed toward the Infra-Red (IR) range using narrow band gap materials such as mercury chalcogenides. Here we demonstrate the feasibility of a core/shell structure made of a CdSe core with two HgSe external wells. We demonstrate that the optical spectrum of the heterostructure is set by the HgSe wells and this, despite the quasi type II band alignment which makes the band edge energy independent of the inner core thickness. On the other hand, these core/shell NPLs behave, from a transport point of view, as a wide band gap material. We demonstrate that the introduction of a wide band gap CdSe core makes the material less conductive and with a larger photoresponse. Hence the heterostructure presents an effective electric band gap wider than the optical band gap. This strategy will be of utmost interest to design infrared effective colloidal materials for which the reduction of the carrier density and the associated dark current is a critical property.
II–VI two-dimensional (2D) nanoplatelets (NPLs) exhibit the narrowest optical features among nanocrystals (NCs). This property remains true for Hg-based NPLs, despite a cation exchange procedure to obtain them from Cd-based NPLs, which leads to structural defects (poorly defined edges and voids) inducing inhomogeneous broadening. Here, we propose an optimized procedure for which a solvent, surface chemistry, and reaction conditions are rationally considered. The procedure is applied to the growth of alloyed HgSe1–x Te x NPLs with various compositions. We report a bright photoluminescence for all compositions. Structural properties being now well defined, it is possible to study the electronic properties of these objects. To do so, we combine k·p modeling of quantum-confined structures with X-ray photoemission. In particular, we clarify the origin of the similarity between CdTe and HgTe NPLs absorption spectra despite their vastly differing bulk band structures. Finally, static- and time-resolved photoemission unveil a crossover from n- to p-type behavior in HgSe1–x Te x NPLs while increasing the Te content.
HgTe nanocrystals, thanks to quantum confinement, present a broadly tunable band gap all over the infrared spectral range. In addition, significant efforts have been dedicated to the design of infrared...
Among colloidal nanocrystals, 2D nanoplatelets (NPLs) made of cadmium chalcogenides have led to especially well controlled optical features. However, the growth of core shell heterostructures has so far been mostly focused on CdS shells, while more confined materials will be more promising to decouple the emitting quantum states of the core from their external environment. Using k·p simulation, we demonstrate that a ZnS shell reduces by a factor 10 the leakage of the wavefunction into the surrounding medium. Using X-ray photoemission (XPS), we confirm that the CdSe active layer is indeed unoxidized. Finally, we build an effective electronic spectrum for these CdSe/ZnS NPLs on an absolute energy scale which is a critical set of parameters for the future integration of this material into optoelectronic devices. We determine the work function (WF) to be 4.47 eV while the material is behaving as an n-type semiconductor.
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