2,696 research outputs found
Exciton storage in CdSe/CdS tetrapod semiconductor nanocrystals: Electric field effects on exciton and multiexciton states
CdSe/CdS nanocrystal tetrapods are interesting building blocks for excitonic circuits, where the flow of excitation energy is gated by an external stimulus. The physical morphology of the nanoparticle, along with the electronic structure, which favors electron delocalization between the two semiconductors, suggests that all orientations of a particle relative to an external electric field will allow for excitons to be dissociated, stored, and released at a later time. While this approach, in principle, works, and fluorescence quenching of over 95% can be achieved electrically, we find that discrete trap states within the CdS are required to dissociate and store the exciton. These states are rapidly filled up with increasing excitation density, leading to a dramatic reduction in quenching efficiency. Charge separation is not instantaneous on the CdS excitonic antennae in which light absorption occurs, but arises from the relaxed exciton following hole localization in the core. Consequently, whereas strong electromodulation of the core exciton is observed, the core multiexciton and the CdS arm exciton are not affected by an external electric field
CdSe/CdS dot-in-rods nanocrystals fast blinking dynamics
The blinking dynamics of colloidal core-shell CdSe/CdS dot-in-rods is studied
in detail at the single particle level. Analyzing the autocorrelation function
of the fluorescence intensity, we demonstrate that these nanoemitters are
characterized by a short value of the mean duration of bright periods (ten to a
few hundreds of microseconds). The comparison of the results obtained for
samples with different geometries shows that not only the shell thickness is
crucial but also the shape of the dot- in-rods. Increasing the shell aspect
ratio results in shorter bright periods suggesting that surface traps impact
the stability of the fluorescence intensity
Temperature-tuning of near-infrared monodisperse quantum dot solids at 1.5 um for controllable Forster energy transfer
We present the first time-resolved cryogenic observations of Forster energy
transfer in large, monodisperse lead sulphide quantum dots with ground state
transitions near 1.5 um (0.83 eV), in environments from 160 K to room
temperature. The observed temperature-dependent dipole-dipole transfer rate
occurs in the range of (30-50 ns)^(-1), measured with our confocal
single-photon counting setup at 1.5 um wavelengths. By temperature-tuning the
dots, 94% efficiency of resonant energy transfer can be achieved for donor
dots. The resonant transfer rates match well with proposed theoretical models
Proliferation of anomalous symmetries in colloidal monolayers subjected to quasiperiodic light fields
Quasicrystals provide a fascinating class of materials with intriguing
properties. Despite a strong potential for numerous technical applications, the
conditions under which quasicrystals form are still poorly understood.
Currently, it is not clear why most quasicrystals hold 5- or 10-fold symmetry
but no single example with 7 or 9-fold symmetry has ever been observed. Here we
report on geometrical constraints which impede the formation of quasicrystals
with certain symmetries in a colloidal model system. Experimentally, colloidal
quasicrystals are created by subjecting micron-sized particles to
two-dimensional quasiperiodic potential landscapes created by n=5 or seven
laser beams. Our results clearly demonstrate that quasicrystalline order is
much easier established for n = 5 compared to n = 7. With increasing laser
intensity we observe that the colloids first adopt quasiperiodic order at local
areas which then laterally grow until an extended quasicrystalline layer forms.
As nucleation sites where quasiperiodicity originates, we identify highly
symmetric motifs in the laser pattern. We find that their density strongly
varies with n and surprisingly is smallest exactly for those quasicrystalline
symmetries which have never been observed in atomic systems. Since such high
symmetry motifs also exist in atomic quasicrystals where they act as
preferential adsorption sites, this suggests that it is indeed the deficiency
of such motifs which accounts for the absence of materials with e.g. 7-fold
symmetry
Electronic structure of and Quantum size effect in III-V and II-VI semiconducting nanocrystals using a realistic tight binding approach
We analyze the electronic structure of group III-V semiconductors obtained
within full potential linearized augmented plane wave (FP-LAPW) method and
arrive at a realistic and minimal tight-binding model, parameterized to provide
an accurate description of both valence and conduction bands. It is shown that
cation sp3 - anion sp3d5 basis along with the next nearest neighbor model for
hopping interactions is sufficient to describe the electronic structure of
these systems over a wide energy range, obviating the use of any fictitious s*
orbital, employed previously. Similar analyses were also performed for the
II-VI semiconductors, using the more accurate FP-LAPW method compared to
previous approaches, in order to enhance reliability of the parameter values.
Using these parameters, we calculate the electronic structure of III-V and
II-VI nanocrystals in real space with sizes ranging upto about 7 nm in
diameter, establishing a quantitatively accurate description of the band-gap
variation with sizes for the various nanocrystals by comparing with available
experimental results from the literature.Comment: 28 pages, 8 figures, Accepted for publication in Phys. Rev.
Bistable states of quantum dot array junctions for high-density memory
We demonstrate that two-dimensional (2D) arrays of coupled quantum dots (QDs)
with six-fold degenerate p orbitals can display bistable states, suitable for
application in high-density memory device with low power consumption. Due to
the inter-dot coupling of and orbitals in these QD arrays, two
dimensional conduction bands can be formed in the x-y plane, while the
orbitals remain localized in the x-y plane such that the inter-dot coupling
between them can be neglected. We model such systems by taking into account the
on-site repulsive interactions between electrons in orbitals and the
coupling of the localized orbitals with the 2D conduction bands formed by
and orbitals. The Green's function method within an extended
Anderson model is used to calculate the tunneling current through the QDs. We
find that bistable tunneling current can exist for such systems due to the
interplay of the on-site Coulomb interactions (U) between the orbitals
and the delocalized nature of conduction band states derived from the
hybridization of / orbitals. This bistable current is not sensitive
to the detailed band structure of the two dimensional band, but depends
critically on the strength of and the ratio of the left and right tunneling
rates. The behavior of the electrical bistability can be sustained when the 2D
QD array reduces to a one-dimensional QD array, indicating the feasibility for
high-density packing of these bistable nanoscale structures
Effect of chemical composition on luminescence of thiol-stabilized CdTe nanocrystals
Judicious selection of the amount of surfactant during synthesis enables a drastic increase in the photoluminescence efficiency of aqueous CdTe nanocrystals (NCs) stabilized by thioglycolic acid (TGA). Elemental determination of the NCs was undertaken to identify the origin of this effect. The molar ratio of (Te + S) to Cd approached unity when the optimum amount of TGA was used during synthesis, whereas the number of S atoms originating from TGA molecules in one NC (2.6 nm of diameter) remained unchanged at 90 ± 3. This indicates that the core lattice composition at the beginning of synthesis, rather than the surface conditions, affects the photoluminescence efficiency of the NCs even after prolonged refluxing
Self Assembly of Soft Matter Quasicrystals and Their Approximants
The surprising recent discoveries of quasicrystals and their approximants in
soft matter systems poses the intriguing possibility that these structures can
be realized in a broad range of nano- and micro-scale assemblies. It has been
theorized that soft matter quasicrystals and approximants are largely
entropically stabilized, but the thermodynamic mechanism underlying their
formation remains elusive. Here, we use computer simulation and free energy
calculations to demonstrate a simple design heuristic for assembling
quasicrystals and approximants in soft matter systems. Our study builds on
previous simulation studies of the self-assembly of dodecagonal quasicrystals
and approximants in minimal systems of spherical particles with complex,
highly-specific interaction potentials. We demonstrate an alternative
entropy-based approach for assembling dodecagonal quasicrystals and
approximants based solely on particle functionalization and shape, thereby
recasting the interaction-potential-based assembly strategy in terms of
simpler-to-achieve bonded and excluded-volume interactions. Here, spherical
building blocks are functionalized with mobile surface entities to encourage
the formation of structures with low surface contact area, including
non-close-packed and polytetrahedral structures. The building blocks also
possess shape polydispersity, where a subset of the building blocks deviate
from the ideal spherical shape, discouraging the formation of close-packed
crystals. We show that three different model systems with both of these
features -- mobile surface entities and shape polydispersity -- consistently
assemble quasicrystals and/or approximants. We argue that this design strategy
can be widely exploited to assemble quasicrystals and approximants on the nano-
and micro- scales. In addition, our results further elucidate the formation of
soft matter quasicrystals in experiment.Comment: 12 pages 6 figure
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