Due to their interesting properties, research on colloidal nanocrystals has moved in the last few years from fundamental research to first applications in materials science and life sciences. In this review some recent biological applications of colloidal nanocrystals are discussed, without going into biological or chemical details. First, the properties of colloidal nanocrystals and how they can be synthesized are described. Second, the conjugation of nanocrystals with biological molecules is discussed. And third, three different biological applications are introduced: (i) the arrangement of nanocrystal–oligonucleotide conjugates using molecular scaffolds such as single-stranded DNA, (ii) the use of nanocrystal–protein conjugates as fluorescent probes for cellular imaging, and (iii) a motility assay based on the uptake of nanocrystals by living cells.

https://iopscience.iop.org/article/10.1088/0957-4484/14/7/201/pdf

Biological applications of colloidal nanocrystals

Instabilities in semiconductor heterostructure growth can be exploited for the self-organized formation of nanostructures, allowing for carrier confinement in all three spatial dimensions. Beside the description of various growth modes, the experimental characterization of structural properties, such as size and shape, chemical composition, and strain distribution is presented. The authors discuss the calculation of strain fields, which play an important role in the formation of such nanostructures and also influence their structural and optoelectronic properties. Several specific materials systems are surveyed together with important applications.

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Structural properties of self-organized semiconductor nanostructures

The quantum-confined Stark effect in single cadmium selenide (CdSe) nanocrystallite quantum dots was studied. The electric field dependence of the single-dot spectrum is characterized by a highly polarizable excited state (∼10 5 cubic angstroms, compared to typical molecular values of order 10 to 100 cubic angstroms), in the presence of randomly oriented local electric fields that change over time. These local fields result in spontaneous spectral diffusion and contribute to ensemble inhomogeneous broadening. Stark shifts of the lowest excited state more than two orders of magnitude larger than the linewidth were observed, suggesting the potential use of these dots in electro-optic modulation devices.

Quantum Confined Stark Effect in Single CdSe Nanocrystallite Quantum Dots

The quintessence of the hot-injection method, a synthesis route for monodisperse, highly luminescent semiconductor nanocrystals, is reviewed. The separate stages of nucleation and growth of the nanocrystals are discussed in the framework of classical nucleation theory and an equilibrium model proposed by Debye. We also review the numerous adaptations of the original synthesis that currently provide colloidal nanocrystals with well-defined, size-dependent optical, electrical, and magnetic properties. The availability of these remarkable materials is one of the most promising developments in nanoscience and nanotechnology.

/pdf/physicochemical-evaluation-of-the-hot-injection-method-a-4hswsx46ll.pdf

Physicochemical evaluation of the hot-injection method, a synthesis route for monodisperse nanocrystals.

In 1954, Dicke pointed out that the description of a spontaneously radiating gas has to include the fact that all atoms or molecules interact with a common radiation field1. Consequently, the individual particles may not be considered as independent sources of radiation. In this regard, the question arises of whether quantum dot (QD) systems may also exhibit signatures of cooperative radiation and hence have to be considered as coupled quantum systems. Here, we present experimental evidence for a long-range electromagnetic interaction between laterally arranged QDs. The experimental results suggest that the QDs do not behave like independent objects as long as they form an ensemble of QDs. By removing QDs from the sample, we found that the coupling was reduced. The range of interaction is shown to be at least 150 nm. This may therefore provide a mechanism to couple discrete quantum objects on a large scale.

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Superradiance of quantum dots

Zero-dimensional excitons (0DXs) in CdSe/ZnSe nanostructures have been studied by time- and spatially resolved photoluminescence spectroscopy. The three-dimensional confinement is confirmed by an exciton lifetime up to 550 ps, independent of temperature up to 130 K. By preparing mesa structures with diameters down to 50 nm as local probes, an extremely high spatial resolution is achieved, giving experimental access to single 0DXs. A splitting of the ground state into a linearly polarized doublet with an energy spacing up to 1.5 meV is found, varying from dot to dot in sign and magnitude. This indicates a noncircular shape with no preferential orientation of the dots. The dot density is estimated to increase from 5×1010 to 1.5×1011 cm−2, when changing the nominal CdSe layer thickness from 1 to 3 ML, i.e., close to the critical thickness.

Single zero-dimensional excitons in cdse/znse nanostructures

The quantum-confined Stark effect in a single self-assembled CdSe/ZnSe quantum dot was studied by means of highly spatially resolved photoluminescence spectroscopy. A nanotechnological approach making use of a capacitor-like geometry enabled us to apply a well-defined lateral electric field on the quantum dots. Stark shifts of up to 1.1 meV were obtained, which can be well fitted by a purely quadratic dependence on an electric field. In quite good agreement with theoretical calculations, an exciton polarizability of 4.9×10−3 meV/(kV/cm)2 can be extracted, while the permanent dipole moment in the lateral direction is found to be negligible.

Stark effect and polarizability in a single CdSe/ZnSe quantum dot

We report on reversible spectral shifts in the emission spectra of self-organized CdSe single quantum dots on a time scale of seconds. Energy shifts of up to 3.5 meV have been observed and can be attributed to the Stark effect caused by fluctuating local electric fields. Most surprisingly, the energy shift turns out to be quasi-periodic with time constants between 70 and 190 s.

Spectral diffusion of the exciton transition in a single self-organized quantum dot

Migration enhanced epitaxy has been applied to induce the change from two-dimensional growth to formation of self-assembling islands in the growth of CdSe on ZnSe. Transmission electron microscopy images from samples with a ZnSe caplayer show a transition from a flat quantum well to an interrupted layer with pronounced thickness fluctuations when the CdSe exceeds its critical thickness. These results are confirmed by high resolution x-ray diffraction measurements, as only for the former sample the 004 rocking curve can be simulated assuming a flat quantum well with abrupt interfaces. Compared to bulk CdSe, the photoluminescence peak is blueshifted by about 0.5 eV. PL excitation experiments indicate that the interrupted layer consists of CdSe islands embedded in Zn1−xCdxSe with a composition gradient. Atomic force microscopy images of uncapped samples show spherical islands with a height of 20 nm and a diameter-to-height ratio of 4:1.

CdSe/ZnSe quantum structures grown by migration enhanced epitaxy: Structural and optical investigations

The influence of the growth conditions during capping of CdSe/ZnSe quantum structures grown on GaAs(001) by molecular-beam epitaxy (MBE) were systematically investigated by high-resolution x-ray diffraction, transmission electron microscopy, and temperature dependent, partly time-resolved photoluminescence spectroscopy. The results clearly indicate formation of quantum wells with potential fluctuations if conventional MBE is used for capping the CdSe by ZnSe. In contrast, quantum dot formation occurs using migration enhanced epitaxy for this growth step. In the latter case, quantum dots can be obtained without formation of stacking faults.

K. Leonardi

Papers

Single zero-dimensional excitons in cdse/znse nanostructures

Stark effect and polarizability in a single CdSe/ZnSe quantum dot

Spectral diffusion of the exciton transition in a single self-organized quantum dot

CdSe/ZnSe quantum structures grown by migration enhanced epitaxy: Structural and optical investigations

Quantum dot formation by segregation enhanced CdSe reorganization