Sunovian. He is/has been involved in clinical trials conducted by Lilly & Shire. The present work is unrelated to the above grants and relationships. Jonna Kuntsi has given talks at educational events sponsored by Medice; all funds are received by King's College London and used for studies of ADHD. Theo Van Erp consulted for Roche Pharmaceuticals and has a contract with Otsuka Pharmaceutical, Ltd. Anders Dale is a Founder of CorTechs Labs, Inc. He serves on the Scientific Advisory Boards of CorTechs Labs and Human Longevity, Inc., and receives research funding through a Research Agreement with General Electric Healhcare. Paulo Mattos was on the speakers' bureau and/or acted as consultant for Janssen-Cilag, Novartis, and Shire in the previous five years; he also received travel awards to participate in scientific meetings from those companies. The ADHD outpatient program (Grupo de Estudos do Déficit de Atenção/Institute of Psychiatry) chaired by Dr. Mattos has also received research support from Novartis and Shire.The funding sources had no role in the design and conduct of the study; collection, management, analysis, or interpretation of the data; or preparation, review, or approval of the manuscript. Tobias Banaschewski served in an advisory or consultancy role for Actelion,
The evolution of the optical phonon spectra of colloidal core/shell CdSe/ZnS quantum dots with an increase of the shell thickness from 0.5 to 3.4 monolayers has been studied by resonant Raman spectroscopy. The results obtained suggest that the ZnS shell changes its structure from amorphous to partly crystalline as the thickness increases. Simultaneously, an increase in Raman scattering by surface ͑core/shell interface͒ phonons and the redshift of the corresponding phonon band have been observed and assigned to variations in the shell structure. The disorder present in the shell provides a major contribution to the line shape of the Raman spectra at higher ZnS coverage. A method to control the quality of quantum dots based on Raman spectroscopy is proposed.
We demonstrate that the nanoscale assemblies of water-solubilized, oppositely charged CdSe/ZnS core/shell quantum dots and of quantum dots and nanogold particles make it possible to develop FRET-based sensors with a donor quenching efficiency close to 100%. The cw and time-resolved photoluminescence analysis of nanoassemblies with different donor-to-acceptor ratios demonstrates a prevalence of 1:1 complexes. Experimental data perfectly fit the mathematical simulation based on long-range FRET and a static model of the assembling of the oppositely charged nanoparticles. These assemblies are stable in biological fluids, suggesting new applications.
A new class of chiral nanoparticles is of great interest not only for nanotechnology, but also for many other fields of scientific endeavor. Normally the chirality in semiconductor nanocrystals is induced by the initial presence of chiral ligands/stabilizer molecules. Here we report intrinsic chirality of ZnS coated CdSe quantum dots (QDs) and quantum rods (QRs) stabilized by achiral ligands. As-prepared ensembles of these nanocrystals have been found to be a racemic mixture of d- and l-nanocrystals which also includes a portion of nonchiral nanocrystals and so in total the solution does not show a circular dichroism (CD) signal. We have developed a new enantioselective phase transfer technique to separate chiral nanocrystals using an appropriate chiral ligand and obtain optically active ensembles of CdSe/ZnS QDs and QRs. After enantioselective phase transfer, the nanocrystals isolated in organic phase, still capped with achiral ligands, now display circular dichroism (CD). We propose that the intrinsic chirality of CdSe/ZnS nanocrystals is caused by the presence of naturally occurring chiral defects.
We report on an anomalous size dependence of the room-temperature photoluminescence decay time from the lowest-energy state of PbS quantum dots in colloidal solution, which was found using the transient luminescence spectroscopy. The observed 10-fold reduction in the decay time (from ~2.5 to 0.25 μs) with the increase in the quantum dots' diameter is explained by the existence of phonon-induced transitions between the in-gap state-whose energy drastically depends on the diameter-and the fundamental state of the quantum dots.
Carbon
dots (CDots) are a promising biocompatible nanoscale source
of light, yet the origin of their emission remains under debate. Here,
we show that all the distinctive optical properties of CDots, including
the giant Stokes shift of photoluminescence and the strong dependence
of emission color on excitation wavelength, can be explained by the
linear optical response of the partially sp2-hybridized
carbon domains located on the surface of the CDots’ sp3-hybridized amorphous cores. Using a simple quantum chemical
approach, we show that the domain hybridization factor determines
the localization of electrons and the electronic bandgap inside the
domains and analyze how the distribution of this factor affects the
emission properties of CDots. Our calculation data fully agree with
the experimental optical properties of CDots, confirming the overall
theoretical picture underlying the model. It is also demonstrated
that fabrication of CDots with large hybridization factors of carbon
domains shifts their emission to the red side of the visible spectrum,
without a need to modify the size or shape of the CDots. Our theoretical
model provides a useful tool for experimentalists and may lead to
extending the applications of CDots in biophysics, optoelectronics,
and photovoltaics.
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