The blinking statistics of numerous single silicon quantum dots fabricated by electron-beam lithography, plasma etching, and oxidation have been analyzed. Purely exponential on- and off-time distributions were found consistent with the absence of statistical aging. This is in contrast to blinking reports in the literature where power-law distributions prevail as well as observations of statistical aging in nanocrystal ensembles. A linear increase of the switching frequency with excitation power density indicates a domination of single-photon absorption processes, possibly through a direct transfer of charges to trap states without the need for a bimolecular Auger mechanism. Photoluminescence saturation with increasing excitation is not observed; however, there is a threshold in excitation (coinciding with a mean occupation of one exciton per nanocrystal) where a change from linear to square-root increase occurs. Finally, the statistics of blinking of single quantum dots in terms of average on-time, blinking frequency and blinking amplitude reveal large variations (several orders) without any significant correlation demonstrating the individual microscopic character of each quantum dot.
We measured the exciton lifetime of single silicon quantum dots, fabricated by electron beam lithography, reactive ion etching and oxidation. The observed photoluminescence decays are of mono-exponential character with a large variation (5-45 μs) from dot to dot, even for the same emission energy. We show that this lifetime variation may be the origin of the heavily debated non-exponential (stretched) decays typically observed for ensemble measurements.
Single silicon nanowires (Si-NWs) prepared by electron-beam lithography and reactive-ion etching are investigated by imaging optical spectroscopy under variable temperatures and laser pumping intensities. Spectral images of individual Si-NWs reveal a large variability of photoluminescence (PL) along a single Si-NW. The weaker broad emission band asymmetrically extended to the high-energy side is interpreted to be due to recombination of quasi-free 1D excitons while the brighter localized emission features (with significantly variable peak position, width, and shape) are due to localization of electron-hole pairs in surface protrusions acting like quasi-0D centers or quantum dots (QDs). Correlated PL and scanning electron microscopy images indicate that the efficiently emitting QDs are located at the Si-NW interface with completely oxidized neck of the initial Si wall. Theoretical fitting of the delocalized PL emission band explains its broad asymmetrical band to be due to the Gaussian size distribution of the Si-NW diameter and reveals also the presence of recombination from the Si-NW excited state which can facilitate a fast capture of excitons into QD centers.
Blinking is a phenomenon observed in single quantum emitters, which reduces their overall light emission. Even though it seems to be a fundamental property of quantum dots (QDs), substantial differences can be found in the blinking statistics of different nanocrystals. This work compares the blinking of numerous single, oxide-capped Si nanocrystals with that of CdSe/ZnS core-shell nanocrystals, measured under the same conditions in the same experimental system and over a broad range of excitation power densities. We find that ON-and OFF-times can be described by exponential statistics in Si QDs, as opposed to power-law statistics for the CdSe nanocrystals.The type of blinking (power-law or mono-exponential) does not depend on excitation, but seems to be an intrinsic property of the material system. Upon increasing excitation power, the duty 2 cycle of Si quantum dots remains constant, whereas it decreases for CdSe nanocrystals, which is readily explained by blinking statistics. Both ON-OFF and OFF-ON transitions can be regarded as light-induced in Si/SiO 2 QDs, while the OFF-ON transition in CdSe/ZnS nanocrystals is not stimulated by photons. The differences in blinking behavior in these systems will be discussed.3
Starting from the hydrodynamic equations describing the positive column of glow discharges in oxygen, the stability of the homogeneous state is investigated. The model contains electrons, positive and negative ions as well as the metastable molecule O2(a1Δg) as a detachment partner. It is shown that the transition from the H-mode to the T-mode of a dc-driven oxygen discharge is caused by an attachment-induced ionization instability. The stability boundaries are calculated for selected values of the plasma parameters. The comparison of experimental data and theoretical predictions shows satisfactory agreement.
A fabrication method for a matrix pattern of laterally separated silicon quantum rods was developed, consisting of a three‐step recipe utilizing electron beam lithography (EBL), reactive ion etching (RIE), and oxidation. Photoluminescence (PL) measurements – images, spectra, and blinking – verified that the presented method results in a high number of luminescing single silicon quantum rods in well defined positions on the sample. These are suitable for single dot spectroscopy and repeatable measurements, even using different measurement methods and instruments. Colorized scanning electron microscope images of undulating silicon nanowalls for controlled single quantum rod fabrication.
We demonstrate that nonradiative recombination in semiconductor nanocrystals can be described by a rapid luminescence intermittency, based on carrier tunneling to resonant traps. Such process, we call it “rapid trapping (blinking)”, leads to delayed luminescence and promotes Auger recombination, thus lowering the quantum efficiency. To prove our model, we probed oxide- (containing static traps) and ligand- (trap-free) passivated silicon nanocrystals emitting at similar energies and featuring monoexponential blinking statistics. This allowed us to find analytical formulas and to extract characteristic trapping/detrapping rates, and quantum efficiency as a function of temperature and excitation power. Experimental single-dot temperature-dependent decays, supporting the presence of one or few resonant static traps, and ensemble saturation curves were found to be very well described by this effect. The model can be generalized to other semiconductor nanocrystals, although the exact interplay of trapping/detrapping, radiative, and Auger processes may be different, considering the typical times of the processes involved.
Elongated silicon quantum dots (also referred to as rods) were fabricated using a lithographic process which reliably yields sufficient numbers of emitters. These quantum rods are perfectly aligned and the vast majority are spatially separated well enough to enable single-dot spectroscopy. Not only do they exhibit extraordinarily high linear polarization with respect to both absorption and emission, but the silicon rods also appear to luminesce much more brightly than their spherical counterparts. Significantly increased quantum efficiency and almost unity degree of linear polarization render these quantum rods perfect candidates for numerous applications.
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