Jan Valenta

Step-like enhancement of luminescence quantum yield of silicon nanocrystals

Carrier multiplication by generation of two or more electron-hole pairs following the absorption of a single photon may lead to improved photovoltaic efficiencies and has been observed in nanocrystals made from a variety of semiconductors, including silicon. However, with few exceptions, these reports have been based on indirect ultrafast techniques. Here, we present evidence of carrier multiplication in closely spaced silicon nanocrystals contained in a silicon dioxide matrix by measuring enhanced photoluminescence quantum yield. As the photon energy increases, the quantum yield is expected to remain constant, or to decrease as a result of new trapping and recombination channels being activated. Instead, we observe a step-like increase in quantum yield for larger photon energies that is characteristic of carrier multiplication. Modelling suggests that carrier multiplication is occurring with high efficiency and close to the energy conservation limit.

Photoluminescence spectroscopy of single silicon quantum dots

Photoluminescence (PL) from single silicon quantum dots have been recorded and spectrally resolved at room temperature. The Si nanocrystals (NCs) were fabricated using electron-beam lithography and ...

Brightly Luminescent Organically Capped Silicon Nanocrystals Fabricated at Room Temperature and Atmospheric Pressure

Silicon nanocrystals are an extensively studied light-emitting material due to their inherent biocompatibility and compatibility with silicon-based technology. Although they might seem to fall behind their rival, namely, direct band gap based semiconductor nanocrystals, when it comes to the emission of light, room for improvement still lies in the exploitation of various surface passivations. In this paper, we report on an original way, taking place at room temperature and ambient pressure, to replace the silicon oxide shell of luminescent Si nanocrystals with capping involving organic residues. The modification of surface passivation is evidenced by both Fourier transform infrared spectroscopy and nuclear magnetic resonance measurements. In addition, single-nanocrystal spectroscopy reveals the occurrence of a systematic fine structure in the emission single spectra, which is connected with an intrinsic property of small nanocrystals since a very similar structure has recently been observed in specially passivated semiconductor CdZnSe nanoparticles. The organic capping also dramatically changes optical properties of Si nanocrystals (resulting ensemble photoluminescence quantum efficiency 20%, does not deteriorate, radiative lifetime 10 ns at 550 nm at room temperature). Optically clear colloidal dispersion of these nanocrystals thus exhibits properties fully comparable with direct band gap semiconductor nanoparticles.

Waveguiding effects in the measurement of optical gain in a layer of Si nanocrystals

We discuss applicability of the variable stripe length method to experimental investigation of optical gain in a luminescent layer that behaves like a planar waveguide. We show that an interplay between the output direction of guided light modes and the numerical aperture of the collection optics may lead to an artifact manifesting itself as an apparent but false gain. We propose a way to circumvent this inconvenience by using a “shifting excitation spot” complementary measurement. The method is demonstrated on a layer of Si nanocrystals embedded into a synthetic silica plate.

On the origin of the fast photoluminescence band in small silicon nanoparticles

Colloidal suspensions of small silicon nanoparticles (diameter around 2nm) with fast and efficient ultraviolet-blue photoluminescence (PL) band are fabricated by enhanced electrochemical etching of Si wafers. The detailed study of photoluminescence excitation spectra in a wide range of excitation photon energies (270-420nm) reveals specific behavior of the Stokes shift of the fast PL band that agrees well with theoretical calculation of optical transitions in small silicon nanocrystals and is distinct from emission of silicon dioxide defects.

Electroluminescence of single silicon nanocrystals

We report on measurements of room-temperature electroluminescence from single silicon nanocrystals. The electrically driven emission reveals typical characteristics of single-nanocrystal luminescence: the peak wavelength variations, narrowing of spectral bands, a high degree of linear polarization, and intensity fluctuations (blinking) observed on a scale of minutes. From the count rate statistics of individual nanocrystals, we conclude that the yield of radiative emission is as high as 19%. These findings may open a route to highly efficient all-silicon light emitters.

Determination of sensoric parameters of porous silicon in sensing of organic vapors

Photoluminescence (PL) properties of as-prepared and surface derivatized porous silicon (PS) in the presence of organic compounds in gas phase were studied. Surface derivatization, aimed at increasing stability of porous silicon properties, was performed by Lewis acid mediated hydrosilylation with methyl 10-undecenoate. We have systematically measured changes in photoluminescence intensity for a set of alcohols from C 1 to C 6 . From the variation of the photoluminescence quenching response as a function of alcohol concentration, we determine the sensitivities and detection limits of our porous silicon sensors and these correlate with physical and chemical properties of studied species. For methyl 10-undecenoate derivatized PS samples, we have observed a remarkable enhancement of the selectivity for C 4 -C 6 alcohols as compared with C 1 -C 3 alcohols.

Luminescence of free-standing versus matrix-embedded oxide-passivated silicon nanocrystals: The role of matrix-induced strain

We collect a large number of experimental data from various sources to demonstrate that free-standing (FS) oxide-passivated silicon nanocrystals (SiNCs) exhibit considerably blueshifted emission, by 200 meV on average, compared to those prepared as matrix-embedded (ME) ones of the same size. This is suggested to arise from compressive strain, exerted on the nanocrystals by their matrix, which plays an important role in the light-emission process; this strain has been neglected up to now as opposed to the impact of quantum confinement or surface passivation. Our conclusion is also supported by the comparison of low-temperature behavior of photoluminescence of matrix-embedded and free-standing silicon nanocrystals.

Origin of green luminescence in hydrothermally grown ZnO single crystals

Combining photoluminescence and positron annihilation studies of hydrothermally grown ZnO crystals with stoichiometry varied by controlled annealing enabled us to clarify the origin of green luminescence. It was found that green luminescence in ZnO has multiple origins and consists of a band at 2.3(1) eV due to recombination of electrons of the conduction band by zinc vacancy acceptors coupled with hydrogen and a band at 2.47(2) eV related to oxygen vacancies. The as-grown ZnO crystals contain zinc vacancies associated with hydrogen and exhibit a green luminescence at 2.3(1) eV. Annealing in Zn vapor removed zinc vacancies and introduced oxygen vacancies. This led to disappearance of the green luminescence band at 2.3(1) eV and appearance of a green emission at higher energy of 2.47(2) eV. Moreover, the color of the crystal was changed from colorless to dark red. In contrast, annealing of the as-grown crystal in Cd vapor did not remove zinc vacancies and did not cause any significant change of green luminescence nor change in coloration.

Electroluminescence microscopy and spectroscopy of silicon nanocrystals in thin SiO2 layers

Stable continuously operable electroluminescent diodes have been fabricated by Sii-ion implantation and annealing of thin SiO2 layers on a silicon substrate. The external quantum efficiency of the ...