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Horst Weller

Publications and source records attributed to Horst Weller.

At least 19 recordsLinked to original sources
PubMed2006

Electrical control of Förster energy transfer.

Bringing together compounds of intrinsically different functionality, such as inorganic nanostructures and organic molecules, constitutes a particularly powerful route to creating novel functional devices with synergetic properties found in neither of the constituents. We introduce nanophotonic functional elements combining two classes of materials, semiconductor nanocrystals and dyes, whose physical nature arises as a superposition of the properties of the individual components. The strongly absorbing rod-like nanocrystals focus the incident radiation by photopumping the weakly absorbing dye via energy transfer. The CdSe/CdS nanorods exhibit a large quantum-confined Stark effect on the single-particle level, which enables direct control of the spectral resonance between donor and acceptor required for nanoscopic Förster-type energy transfer in single nanorod-dye couples. With this far-field manipulation of a near-field phenomenon, the emission from single dye molecules can be controlled electrically. We propose that this effect could lead to the design of single-molecule optoelectronic switches providing building blocks for more complex nanophotonic circuitry.

Journal Article↗
PubMed2006

Semiconductor nanocrystals photosensitize C60 crystals.

Semiconductor nanocrystals (SCNCs) made of CdSe, CdTe, and InP are used to photosensitize needlelike C(60) crystals. The photocurrent is increased by up to 3 orders of magnitude as compared with C(60) crystals without SCNCs. The photocurrent spectrum can be tuned precisely by the SCNC size and material, rendering the SCNC-functionalized C(60) crystals an excellent material for spectrally tuneable photodetectors. We explain the increased photocurrent as a result of photoexcited electrons transferring from the SCNCs to the C(60) crystals and causing photoconductivity, while the complementary holes remain trapped in the SCNCs.

Cadmium Compounds↗
PubMed2005

Electrostatic and covalent interactions in CdTe nanocrystalline assemblies.

This paper focuses on the interactions between cysteamine-stabilized CdTe nanocrystals [CdTe(CA) NCs] and thioglycolic-acid-stabilized CdTe nanocrystals [CdTe(TGA) NCs]. These interactions were examined by the absorption, continuous, and time-resolved photoluminescence (PL) spectra of the electrostatically mixed and the covalently linked NCs assemblies comprised of the oppositely surface charged CdTe(CA) and CdTe(TGA) NCs and by a comparison with those of the corresponding pristine NCs. The CdTe(CA)-CdTe(TGA) coupling is dictated by the surfactant spacer, ranging between 0.93 and 1.14 nm and by electrostatic and covalent interactions, enabling a Förster resonance energy transfer (FRET) process among the NCs. The results revealed an excellent spectral overlap between the emission of the CdTe(TGA) NCs and the absorption of the CdTe(CA) NCs as well as a PL spectral red shift on the formation of electrostatic and covalent interactions. Furthermore, the measurements showed a lifetime ranging between 1.2 and 3 ns for the electrostatically mixed and the covalently linked assemblies, shorter than those of the pristine CdTe(CA) NCs and CdTe(TGA) NCs, both of which measured as approximately 5.5 ns. When CdTe(TGA) NCs performed as the most efficient donors, FRET rates of 10(10)-10(11) s(-1) were calculated for the electrostatically mixed NCs or covalently linked NCs.

Cadmium↗
PubMed2005

Interplay between Auger and ionization processes in nanocrystal quantum dots.

We study the interplay between Auger effects and ionization processes in the limit of strong electronic confinement in core/shell CdSe/ZnS semiconductor nanocrystal quantum dots. Spectrally resolved fluorescence decay measurements reveal a monotonic increase of the photoluminescence decay rate on excitation density. Our results suggest that Auger recombination accelerates ionization processes that lead to the occupation of dark, nonemissive nanocrystal states. A model is proposed in the quantized Auger regime describing these experimental observations and providing an estimate of the Auger assisted ionization rates.

Journal Article↗
PubMed2005

Density of states measured by scanning-tunneling spectroscopy sheds new light on the optical transitions in PbSe nanocrystals.

The density-of-states function of individual colloidal PbSe nanocrystals varying in diameter between 3 and 7 nm is measured by resonant tunneling spectroscopy. It is in semiquantitative agreement with tight-binding calculations, but the energy separation between electron (hole) levels of S and P symmetry is systematically smaller than predicted by the theory. These results provide an explanation for the second and third excitonic optical transitions, which have been debated for a long time.

Journal Article↗
PubMed2005

Determination of nanocrystal sizes: a comparison of TEM, SAXS, and XRD studies of highly monodisperse CoPt3 particles.

One of the most fundamental tasks in nanoscience is the accurate determination of particle sizes. Various methods have been developed to elucidate the mean particle diameter and the standard deviation for an ensemble of nanocrystals. However, good agreement between the results from different methods is not always encountered in the literature. In this study, we investigate colloidally prepared, highly monodisperse CoPt3 nanoparticles by transmission electron microscopy (TEM), small-angle X-ray scattering (SAXS), and powder X-ray diffraction (XRD). The results are compared in order to examine to which extent agreement is obtained by the different techniques when applied to small nanocrystals in the size range below 10 nm. In particular, the applicability of the simple Scherrer formula for size determination from the broadening of XRD reflections is checked. When the different techniques are correctly applied, the results from all methods are in good agreement.

Journal Article↗
PubMed2005

Colloidal synthesis of organic-capped ZnO nanocrystals via a sequential reduction-oxidation reaction.

A nonhydrolytic route to quantum-sized (d < 9 nm) ZnO nanocrystals in homogeneous organic solutions is presented. Nearly spherical ZnO nanocrystals were grown in a surfactant mixture of hexadecylamine and oleic acid (OLEA) by means of a two-step chemical process, based on the hot reduction (at 180-250 degrees C) of a zinc halide by superhydride (LiBEt3H) followed by oxidation of the resulting product. The experimental results suggested that the controlled growth of ZnO in the nanosized regime depended both on the OLEA-assisted generation of intermediate metallic nanoparticles and on the adjustment of their oxidation conditions by using a mild oxidant, trimethylamine-N-oxide, rather than molecular oxygen. The present synthetic approach demonstrates to be particularly suitable to prepare organic-soluble ultra-small ZnO nanocrystals of low size dispersion and of stable size, which are appealing for optoelectronic, catalytic, and sensing purposes.

Journal Article↗
PubMed2004

CdSe and CdSe/CdS nanorod solids.

We demonstrate the self-organization of CdSe nanorods into nematic, smectic, and crystalline solids. Layered colloidal crystals of CdSe nanorods grow by slow destabilization of a nanocrystal solution upon allowing the diffusion of a nonsolvent into the colloidal solution of nanocrystals. The colloidal crystals of nanorods show characteristic birefringence, which we assign to specific spherulite-like texture of each nanorod assembly. To demonstrate the general character of nanorod self-assembly technique, CdSe/CdS heterostructure nanorods were organized into highly luminescent superlattices.

Journal Article↗
PubMed2004

Optical and electrical properties of three-dimensional interlinked gold nanoparticle assemblies.

The optical and electrical properties of 11-20 nm thick films composed of approximately 4 nm gold nanoparticles (Au-NPs) interlinked by six organic dithiol or bis-dithiocarbamate derivatives were compared to investigate how these properties depend on the core of the linker molecule (benzene or cyclohexane) and its metal-binding substituents (thiol or dithiocarbamate). Films prepared with the thiol-terminated linker molecules, (1,4-bis(mercaptomethyl)benzene, 1,4-bis(mercaptomethyl)cyclohexane, 1,4-bis(mercaptoacetamido)benzene, and 1,4-bis(mercaptoacetamido)cyclohexane), exhibit thermally activated charge transport. The activation energies lie between 59 and 71 meV. These films show distinct plasmon absorption bands with maxima between 554 and 589 nm. In contrast, the film prepared with 1,4-cyclohexane-bis(dithiocarbamate) has a significantly red-shifted plasmon band ( approximately 626 nm) and a pronounced absorbance in the near infrared. The activation energy for charge transport is only 14 meV. These differences are explained in terms of the formation of a resonant state at the interface due to overlap of the molecular orbital and metal wave function, leading to an apparent increase in NP diameter. The film prepared with 1,4-phenylene-bis(dithiocarbamate) exhibits metallic properties, indicating the full extension of the electron wave function between interlinked NPs. In all cases, the replacement of the benzene ring with a cyclohexane ring in the center of the linker molecule leads to a 1 order of magnitude decrease in conductivity. A linear relationship is obtained when the logarithm of conductivity is plotted as a function of the number of nonconjugated bonds in the linker molecules. This suggests that nonresonant tunneling along the nonconjugated parts of the molecule governs the electron tunneling decay constant (beta(N)(-)(CON)), while the contribution from the conjugated parts of the molecule is weak (corresponding to resonant tunneling). The obtained value for beta(N)(-)(CON) is approximately 1.0 (per non-conjugated bond) and independent of the nanoparticle-binding group. Hence, the molecules can be viewed as consisting of serial connections of electrically insulating (nonconjugated) and conductive (conjugated) parts.

Journal Article↗
PubMed2003

Low-temperature synthesis of soluble and processable organic-capped anatase TiO2 nanorods.

We demonstrate the controlled growth of high aspect ratio anatase TiO2 nanorods by hydrolysis of titanium tetraisopropoxide (TTIP) in oleic acid (OLEA) as surfactant at a temperature as low as 80 degrees C. Chemical modification of TTIP by OLEA is proven to be a rational strategy to tune the reactivity of the precursor toward water. The most influential factors in shape control of the nanoparticles are investigated by simply manipulating their growth kinetics. The presence of tertiary amines or quaternary ammonium hydroxides as catalysts is essential to promote fast crystallization under mild conditions. The novelty of the present approach relies on the large-scale production of organic-capped TiO2 nanocrystals to which standard processing of colloidal nanocrystals, such as surface ligand exchange, can be applied for the first time. Concentrated colloidal titania dispersions can be prepared for a number of fundamental studies in homogeneous solutions and represent a new source of easily processable oxide material for many technological applications.

Journal Article↗
PubMed2003

Magneto-optical studies of HgTe/HgxCd1-xTe(S) core-shell nanocrystals.

The synthesis and magneto-optical properties of HgTe nanocrystals capped with HgxCd1-xTe(S) alloyed shells have been investigated. The magneto-optical measurements included the use of optically detected magnetic resonance (ODMR) and circular polarized photoluminescence (CP-PL) spectroscopy. The PL spectra suggest the existence of luminescence events from both the core HgTe and the HgxCd1-xTe(S) shells. The continuous-wave (cw) and time-resolved ODMR measurements revealed that the luminescence at the shell regime is associated with a trap-to-band recombination emission. The electron trap is comprised of a Cd-Hg mixed site, confirming the existence of an alloyed HgxCd1-xTe(S) composition. The ODMR data and the CP-PL measurements together revealed the g-values of the trapped electron and the valence band hole.

Journal Article↗
PubMed2003

Study of nucleation and growth in the organometallic synthesis of magnetic alloy nanocrystals: the role of nucleation rate in size control of CoPt3 nanocrystals.

High quality CoPt(3) nanocrystals were synthesized via simultaneous reduction of platinum acetylacetonate and thermodecomposition of cobalt carbonyl in the presence of 1-adamantanecarboxylic acid and hexadecylamine as stabilizing agents. The high flexibility and reproducibility of the synthesis allows us to consider CoPt(3) nanocrystals as a model system for the hot organometallic synthesis of metal nanoparticles. Different experimental conditions (reaction temperature, concentration of stabilizing agents, ratio between cobalt and platinum precursors, etc.) have been investigated to reveal the processes governing the formation of the metal alloy nanocrystals. It was found that CoPt(3) nanocrystals nucleate and grow up to their final size at an early stage of the synthesis with no Ostwald ripening observed upon further heating. In this case, the nanocrystal size can be controlled only via proper balance between the rates for nucleation and for growth from the molecular precursors. Thus, the size of CoPt(3) nanocrystals can be precisely tuned from approximately 3 nm up to approximately 18 nm in a predictable and reproducible way. The mechanism of homogeneous nucleation, evolution of the nanocrystal ensemble in the absence of Ostwald ripening, nanocrystal faceting, and size-dependent magnetic properties are investigated and discussed on the example of CoPt(3) magnetic alloy nanocrystals. The developed approach was found to be applicable to other systems, e.g., FePt and CoPd(2) magnetic alloy nanocrystals.

Journal Article↗
PubMed2003

Synthesis and self-assembly of colloidal nanoparticles.

We describe recent developments in the synthesis of semiconductor nanoparticles, which lead to a substantial improvement of the luminescence quantum efficiency. Concerning a theoretical model for the growth of an ensemble of nanoparticles, the highest quantum efficiencies are achieved in particles that grow under conditions of a rapid exchange of monomers at the particle surface, leading to a smooth surface structure. Selective etching, core-shell formation and doping of nanoparticles are also discussed as fluorescence-enhancing preparative techniques. Examples of self-assembly of almost-uniformly-sized nanoparticles are given, which result in two-dimensional and three-dimensional superlattices, colloidal crystals and crystalline structures built-up from particles of different sizes. Finally, the self-assembled oriented attachment of quasi-spherical ZnO nanoparticles onto single-crystalline nanorods is presented.

Journal Article↗