Search

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., QC 20210215

We study the effect of X-ray irradiation on the photoluminescence (PL) efficiency and intermittency (blinking) of single Si/SiO2 and CdSe/CdZnS quantum dots (QDs). Our results show that the PL efficiency of Si nanocrystals is not significantly altered up to a cumulative fluence of 10(20) photons/m(2) (corresponding to similar to 300 kGy of absorbed dose in SiO2), while CdSe particles become completely dark already after a 17 times lower fluence. In both types of QDs, the statistical nature of blinking ON- and OFF-times remains unaltered: mono-exponential for Si and power-law for CdSe QDs. However, the evolution of the blinking parameters with absorbed dose depends on the choice of material. On average, both ON- and OFF-time constants do not vary in Si nanocrystals, highlighting their radiation hardness. Instead, the ON-time exponent increases while the OFF-time exponent decreases with the increasing dose for CdSe dots, confirming their efficiency quenching. Ensemble measurements did not show PL spectral changes neither indicated removal of surface ligands in irradiated CdSe dots. Thus, ionization-generated non-radiative centers in the core-shell system modify blinking of CdSe dots and eventually rapidly quench their emission, in contrast to robust Si/SiO2 nanocrystals. Our study is important for the future use of luminescent QDs in harsh environments, such as space, and the engineering of their blinking properties via ionizing radiation., Credit for the Accepted Manuscript: AIP PublishingReference: Federico Pevere, Carl von Treskow, Emanuele Marino, Monib Anwar, Benjamin Bruhn, Ilya Sychugov and Jan Linnros, "X-ray radiation hardness and influence on blinking in Si and CdSe quantum dots," Applied Physics Letters, Volume 113, Issue 25, pp. 25310, Year 2018.QC 20190115

We report two orders of magnitude stronger absorption in silicon nanorods relative to bulk in a wide energy range. The local field enhancement and dipole matrix element contributions were disentangled experimentally by single-dot absorption measurements on differently shaped particles as a function of excitation polarization and photon energy. Both factors substantially contribute to the observed effect as supported by simulations of the light-matter interaction and atomistic calculations of the transition matrix elements. The results indicate strong shape dependence of the quasidirect transitions in silicon nanocrystals, suggesting nanostructure shape engineering as an efficient tool for overcoming limitations of indirect band gap materials in optoelectronic applications, such as solar cells., QC 20170120

Photoluminescence (PL) intermittency (blinking) observed for single silicon nanocrystals (Si-NCs) embedded in oxide is usually attributed to trapping/de-trapping of carriers in the vicinity of the NC. Following this model, we propose that blinking could be modified by introducing new trap sites, for example, via X-rays. In this work, we present a study of the effect of X-ray irradiation (up to 65 kGy in SiO) on the blinking of single Si-NCs embedded in oxide nanowalls. We show that the luminescence characteristics, such as spectrum and life-time, are unaffected by X-rays. However, substantial changes in ON-state PL intensity, switching frequency, and duty cycle emerge from the blinking traces, while the ON- and OFF- time distributions remain of mono-exponential character. Although we do not observe a clear monotonic dependence of the blinking parameters on the absorbed dose, our study suggests that, in the future, Si-NCs could be blinking-engineered via X-ray irradiation., QC 20151001

ON-OFF intermittency or 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 monoexponential) does not depend on excitation but seems to be an intrinsic property of the material system. Upon increasing excitation power, the duty 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/SiO2 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., QC 20140307

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 mu s) 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., QC 20130710

The evolution of the structural and optical properties of a silicon core in oxidized nanowalls is investigated as a function of oxidation time. The same individual nanostructures are characterized after every oxidation step in a scanning electron microscope and by low-temperature photoluminescence, while a representative sample is also imaged in a transmission electron microscope. Analysis of a large number of recorded single-dot spectra and micrographs allows to identify delocalized and localized exciton emission from a nanowire as well as confined exciton emission of a nanocrystal. It is shown how structural transitions from one-to zero-dimensional confinement affect single-nanostructure optical fingerprints., QC 20130204

Direct measurements of the optical absorption cross section (sigma) and exciton lifetime are performed on a single silicon quantum dot fabricated by electron beam lithography (EBL), reactive ion etching (RIE) and oxidation. For this aim, single photon counting using, an avalanche photodiode detector (APD) is applied to record photoluminescence (PL) intensity traces under pulsed excitation. The PL decay is found to be of a mono-exponential character with a lifetime of 6.5 mu s. By recording the photoluminescence rise time at different photon fluxes the absorption cross could be extracted yielding a value of 1.46x10(-14)cm(2) under 405 nm excitation wavelength. The PL quantum efficiency is found to be about 9% for the specified single silicon quantum dot., QC 20130913

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., QC 20120109

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., QC 20110809

Polarization properties of individual silicon nanowires are studied using an optical micro-spectroscopy setup equipped with a Fresnel rhomb to rotate the polarization of the exciting laser and the analyzer to characterize the polarization of emitted photoluminescence. The Si nanowire samples are prepared by electron-beam lithography, plasma etching and oxidation. The fabricated wires are embedded in SiO2 and oriented parallel to the Si substrate. Due to the fluctuating wire diameter (around 5 nm) the very long wires (several tens of μm) are effectively divided into an array of quantum rods (prolate ellipsoids). These structures have strong photoluminescence under UV-blue excitation at room temperature. The degree of photoluminescence linear polarization of both excitation and emission is very high, between 0.9-1, and reveals relatively low fluctuations at different spots of the wires. Experimental results are compared with available theoretical models leading to the conclusion that the high polarization degree is mostly due to surface charges (dielectric confinement) with smaller contribution of quantum confinement effects., QC 20111130

QS 2012

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. [GRAPHICS] Colorized scanning electron microscope images of undulating silicon nanowalls for controlled single quantum rod fabrication., QC 20110407

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., QC 20100525

QS 2012

QS 2015