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From colloidal CdSe quantum dots to microscale optically anisotropic supercrystals through bottom-up self-assembly
摘要： The development of fabrication techniques for novel nanostructured materials is one of the key tasks of modern materials science. One pathway to successfully complete this task is the bottom-up assembly of colloidal nanoparticles into ordered superstructures, possessing both the properties of individual nanoparticles and further novel properties resulting from their interactions. However, nanoparticle self-assembly depends on a variety of parameters, which makes the precise control of this process a complicated problem. Here, the time course of quantum dot (QD) self-assembly into ordered superstructures has been analyzed, along with the evolution of their morphological and optical properties. QD self-assembly occurs through two distinct stages (homo- and hetero-geneous), leading to the formation of supercrystals with a layered morphology. Analysis of the optical properties throughout the superstructures’ growth has shown that the absorption and photoluminescence (PL) bands are blue shifted, retaining almost the same PL lifetimes as in the initial QD solution. The supercrystals formed possess a further unique optical property caused by their layered morphology; namely, a four-fold symmetry characterized by strong birefringence. Such supercrystals may be used for the fabrication of microscale optical paths with high extinction coefficients and specific polarization properties for novel optoelectronic devices.
关键词： optical anisotropy,nanostructured materials,birefringence,self-assembly,quantum dots,supercrystals
更新于2025-11-21 11:08:12
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Plasmon-enhanced inelastic scattering by 2D and 3D superlattices made of silver nanocrystals
摘要： The lattice dynamics of natural crystals, artificial superlattices, or self‐organized nanocrystals intimately mix confinement, coupling, periodicity, and dissipative effects. The low wavenumber vibrational response of the new class of nanomaterials called “supercrystals” does contain relevant information concerning finite size effects on atomic movements inside each nanocrystal, mechanical coupling between adjacent nanocrystals, coherent behavior of the total assembly due to its superperiodicity, and finally finite‐time effects due to damping. All these aspects concerning the dynamical behavior of silver supercrystals has been analyzed using plasmon resonance Raman scattering. Owing to the highly uniform size and chemical environment of the nanocrystals, the confinement and homogeneous damping of their fundamental vibrations are carefully analyzed. The signature of their internal atomic arrangements, as a reminiscence of bulk phonons, is also explored. It is shown that for low particles diameter (?5 nm), deviations from the continuum elastic approximation occur and that the vibrational response is more sensitive to atomic arrangements and surface effects inside the nanocrystals than to spatial coherence effects between them.
关键词： atomistic simulations,supercrystals,damping,low wavenumber,metallic nanocrystals
更新于2025-09-23 15:21:01