25 research outputs found
Multiexcitons confined within a sub-excitonic volume: Spectroscopic and dynamical signatures of neutral and charged biexcitons in ultrasmall semiconductor nanocrystals
The use of ultrafast gating techniques allows us to resolve both spectrally
and temporally the emission from short-lived neutral and negatively charged
biexcitons in ultrasmall (sub-10 nm) CdSe nanocrystals (nanocrystal quantum
dots). Because of forced overlap of electronic wave functions and reduced
dielectric screening, these states are characterized by giant interaction
energies of tens (neutral biexcitons) to hundreds (charged biexcitons) of meV.
Both types of biexcitons show extremely short lifetimes (from sub-100
picoseconds to sub-picosecond time scales) that rapidly shorten with decreasing
nanocrystal size. These ultrafast relaxation dynamics are explained in terms of
highly efficient nonradiative Auger recombination.Comment: 5 pages, 4 figures, to be published in Phys. Rev.
Exciton states and optical properties of CdSe nanocrystals
The optical spectra of CdSe nanocrystals up to 55 A in diameter are analyzed
in a wide range of energies from the fine structure of the low-energy
excitations to the so-called high-energy transitions. We apply a symmetry-based
method in two steps. First we take the tight-binding (TB) parameters from the
bulk sp^{3}s^{*} TB model, extended to include the spin-orbit interaction. The
full single-particle spectra are obtained from an exact diagonalization by
using a group-theoretical treatment. The electron-hole interaction is next
introduced: Both the Coulomb (direct) and exchange terms are considered. The
high-energy excitonic transitions are studied by computing the electric dipole
transition probabilities between single-particle states, while the transition
energies are obtained by taking into account the Coulomb interaction. The fine
structure of the lowest excitonic states is analyzed by including the
electron-hole exchange interaction and the wurtzite crystal-field terms in the
exciton Hamiltonian. The latter is diagonalized in the single electron-hole
pair excitation subspace of progressively increasing size until convergence.
The peaks in the theoretical transition spectra are then used to deduce the
resonant and nonresonant Stokes shifts, which are compared with their measured
values in photoluminescence experiments. We find that the final results depend
on the crystal-field term, the relative size of the surface and the degree of
saturation of the dangling bonds. The results show a satisfactory agreement
with the available experimental data.Comment: Revtex, 24 pages, 7 Postscript figure
Large-Scale Synthesis of Highly Luminescent InP@ZnS Quantum Dots Using Elemental Phosphorus Precursor
Department of Chemical EngineeringColloidal quantum dots can control the bandgap by controlling the particle size, and are capable of solution processing, which is cost competitive, and has a narrow half width of the emission wavelength. Using these characteristics, it is possible to utilize various kinds of LED, solar cell, and bio imaging. Among them, indium phosphide (InP) quantum dots have a bandgap capable of emitting light in the near-infrared region from the visible light region, and are less toxic to humans and the environment than cadmium-based quantum dots, and are attracting attention as next generation light emitting materials.
However, the limited choice and high cost of P precursors have a negative impact on their practical applicability. In this work, I report the large-scale synthesis of highly luminescent InP@ZnS QDs from an elemental P precursor (P4), which was simply synthesized via the sublimation of red P powder. The size of the InP QDs was controlled by varying the reaction parameters such as the reaction time and temperature, and the type of In precursors. This way, the photoluminescence properties of the synthesized InP@ZnS QDs could be easily tuned across the entire visible range, while their quantum yield could be increased up to 60% via the optimization of reaction conditions. Furthermore, possible reaction pathways for the formation of InP QDs using the P4 precursor have been investigated with nuclear magnetic resonance spectroscopy and it was demonstrated that the direct reaction of P4 precursor with In precursor produces InP structures without the formation of intermediate species. The large-scale production of InP@ZnS QDs was demonstrated by yielding more than 6 g of QDs per one-batch reaction.
In the case of InP using different precursor P except the Tris(Trimethylsilyl) phosphine ((TMS)3P) there has been a problem that the size distribution is poor. Two kinds of P precursors with different reactivities were used to separate the nucleation and growth processes and to induce growth along the Lamer mechanism to produce uniform particles. For this, (TMS)3P and DEAP were used as fast reacting P precursors, and P4 was used as a slow reacting P precursor. Through this, the possibility of uniform particle formation was observed. I strongly believe that the newly developed approach bears the potential to be widely used for manufacturing inexpensive high-quality QD emitters.ope