Direct bandgap optical transitions in Si nanocrystals

JETP Letters - The effect of quantum confinement on the direct bandgap of spherical Si nanocrystals has been modelled theoretically. We conclude that the energy of the direct bandgap at the...     

Multiphoton transitions and the resonant optical Stark effect in AgBr nanocrystals

Nonlinear absorption of 30-ps light pulses with λ = 560 nm in AgBr nanocrystals is experimentally studied in the range of intensities 10⁸–10¹⁰ W/cm². The results of a theoretical analysis show that the absorption is related to direct interband n-photon transitions. With increasing light intensity j, the number n increases and the region of the k-space changes for the transitions predominantly contributing to the absorption. It is shown that, due to specific features of the AgBr electronic band structure, the probabilities of two-photon transitions for the light at λ = 560 nm are anomalously low, while those of four-photon transitions are anomalously high. In addition, the increase in the two-photon transition rate with increasing intensity is blocked at j ? 10⁸ W/cm² due to the resonant optical Stark effect and due to a gap arising in the band spectrum, rearranged because of the interaction with light.     

Erbium-doped Si nanocrystals: optical properties and electroluminescent devices

In the last decade, a strong effort has been devoted towards the achievement of efficient light emission from silicon. Among the different approaches, rare-earth doping and quantum confinement in Si nanostructures have shown great potentialities. In the present work, the synthesis and properties of low-dimensional silicon structures in SiO₂ will be analyzed. All of these structures present a strong room temperature optical emission, tunable in the visible by changing the crystal size. Moreover, Si nanocrystals (nc) embedded in SiO₂ together with Er ions show a strong coupling with the rare earth. Indeed each Si nc absorbs energy which is then preferentially transferred to the nearby Er ions. The signature of this interaction is the strong increase of the excitation cross section for an Er ion in the presence of Si nc with respect to a pure oxide host. We will show the properties of Er-doped Si nc embedded within Si/SiO₂ Fabry–Pérot microcavities. Very narrow, intense and highly directional luminescence peaks can be obtained. Moreover, the electroluminescence (EL) properties of Si nc and Er-doped Si nc in MOS devices are investigated. It is shown that an efficient carrier injection at low voltages and quite intense room temperature EL signals can be achieved, due to the sensitizing action of Si nc for the rare earth. These data will be presented and the impact on future applications discussed.     

Temperature dependent optical properties of Si nanocrystals embedded in SiO2 matrix

The optical properties of Si nanocrystals (nc-Si) with different sizes (2～5 nm) embedded in a SiO₂ matrix synthesized by the SiO _x /SiO₂ superlattice approach were studied in a temperature range from room temperature to 600 K by spectroscopic ellipsometry. The Maxwell–Garnett effective medium approximation and Lorentz oscillator model were employed to extract the dielectric function of nc-Si. The results show that the temperature dependence of optical properties of nc-Si is sensitive to its size. An empirical expression of Varshni approximation was obtained to characterize the band-gap energy change of nc-Si at different temperatures.     

Excitons in Si nanocrystals

The states of electron-hole pairs in spherical silicon nanocrystals are theoretically studied using the “multiband” effective-mass approximation in the limit of an infinitely high potential barrier at the boundary. The degeneracy of the states at the top of the valence band is taken into account in the spherical approximation, and the ellipsoidal character of the electronic spectrum in the conduction band is allowed for. Coulomb interaction-induced corrections to the energy of an electron-hole pair are found.     

Frequency domain studies of intersubband optical transitions in Si inversion layers

Fourier Transform Spectroscopic studies of inter-electric-field subband transitions in Silicon inversion layers are compared with optical properties calculated with a 5 media model and a classical dielectric function representation of the inversion layer. Qualitative discrepancies in relative intensities of the subband transitions are interpreted in terms of many-body effects.     

Enhancement of optical switching parameter and third-order optical nonlinearities in embedded Si nanocrystals: A theoretical assessment

Third-order bound-charge electronic nonlinearities of Si nanocrystals (NCs) embedded in a wide band-gap matrix representing silica are theoretically studied using an atomistic pseudopotential approach. Nonlinear refractive index, two-photon absorption and optical switching parameter are examined from small clusters to NCs up to a size of 3 nm. Compared to bulk values, Si NCs show higher third-order optical nonlinearities and much wider two-photon absorption-free energy gap which gives rise to enhancement in the optical switching parameter.     

Effect of photonic bandgap on luminescence from silicon nanocrystals

The modification of the luminescence of silicon nanocrystals experiencing the effect of a photonic bandgap in a 2D photonic crystal was investigated. The time-integrated photoluminescence spectra detected in the plane of the photonic crystal revealed a dip in the light emission corresponding to the wavelength of the bandgap, whose position changes according to the geometry of the prepatterned pillar array. The calculated emission pattern for a pointlike dipole placed in such a structure suggests an inhibition of the spontaneous emission rate at certain directions as a physical reason for the observed modification of luminescence.     

Homogeneous broadening and k-vector conservation in direct bandgap transitions

k-vector conservation is studied in direct bandgap optical transitions by examining edge emitted photoluminescent and electroluminescent spectra. Inhomogeneously and homogeneously broadened spectra are identified in tensile strained, single quantum well, broad stripe laser diode structures. In low excitation conditions, the molecular beam epitaxy (MBE) deposited test structures showed Urbach-tail like inhomogeneous broadening with small Urbach parameter values, typical for high quality materials. At high excitation conditions, significant deviations from Lorentzian line shape were observed and concluded to arise from k-vector conservation within the line broadening process.     

Laser transitions under resonant optical pumping of donor centres in Si:P

Terahertz stimulated emission of phosphorus donors in silicon optically excited by radiation from the free-electron laser FELIX has been studied. It is found that a spectral line of the Si:P laser emission depends on pump frequency. Stimulated emission arises on the 2p₀→1s(E) intra-centre transition (21.2 meV) under resonant pumping of the 2p₀ state and on the 2p₀→1s(T₂) transition (22.3 meV) under pumping of the 2p_± or higher odd-parity donor states. The line shift is attributed to the Auger redistribution of the 1s(E)- and 1s(T₂)-state populations. Received: 7 November 2002 / Revised version: 7 April 2003 / Published online: 14 May 2003 RID="*" ID="*"Corresponding author. Fax: +49-30/6705-55-07, E-mail: sergeij.pavlov@dlr.de RID="**" ID="**"On leave from: The Institute for Physics of Microstructures, Nizhny Novgorod, Russia     

Structural phase transitions in niobium oxide nanocrystals

Niobium oxide nanocrystals were successfully synthesized employing the green synthesis method. Phase formation, microstructure and compositional properties of 1, 4 and 7 days incubation treated samples after calcinations at 450 °C were examined using X-ray diffraction, Raman, photoluminescence (PL), infrared, X-ray photoelectron spectra and transmission electron microscopic characterizations. It was observed that phase formation of Nb₂O₅ nanocrystals was dependent upon the incubation period required to form stable metal oxides. The characteristic results clearly revealed that with increasing incubation and aging, the transformation of cubic, orthorhombic and monoclinic phases were observed. The uniform heating at room temperature (32 °C) and the ligation of niobium atoms due to higher phenolic constituents of utilized rambutan during aging processing plays a vital role in structural phase transitions in niobium oxide nanocrystals. The defects over a period of incubation and the intensities of the PL spectra changing over a period of aging were related to the amount of the defects induced by the phase transition.     

Photoluminescence studies of Si nanocrystals

Summary We report room temperature time-resolved photoluminescence (PL) and temperature dependence of continuous wave (cw) PL studies of high fluence (from 3·10¹⁶ to 3·10¹⁷ cm⁻²) Si⁺-implanted thermal SiO₂ layers after annealing at high temperature (T=1000°C). Such measurements were related to TEM analysis of samples. Nancocrystals were observed at TEM only a samples implanted at higher fluence. In these samples a near infrared PL signal peaked at approximately 1.5 eV with decay time of about 100 μs is present. Besides, in all samples a light emission is present in the green region of the spectrum. The intensity of the emission shows large variations with ion fluence, and is characterized by 0.4, 2 and 7 ns decay times. Paper presented at the III INSEL (Incontro Nazionale sul Silicio Emettitore di Luce) Torino, 12–13 October 1995.     

Electronic and optical properties of Si and Ge nanocrystals: An ab initio study

First-principles calculations within density functional theory and many-body perturbation theory have been carried out in order to investigate the structural, electronic and optical properties of undoped and doped silicon nanostructures. We consider Si nanoclusters co-doped with B and P. We find that the electronic band gap is reduced with respect to that of the undoped crystals, suggesting the possibility of impurity based engineering of electronic and optical properties of Si nanocrystals. Finally, motivated by recent suggestions concerning the chance of exploiting Ge dots for photovoltaic nanodevices, we present calculations of the electronic and optical properties of a Ge₃₅H₃₆ nanocrystal, and compare the results with those for the corresponding Si₃₅H₃₆ nanocrystals and the co-doped Si₃₃BPH₃₆.     

Compensation-induced optical transitions within the ground state of shallow donors in Ge and Si

An approximate formula for integral intensity of the compensation-induced parity-forbidden optical transition within the ground state of shallow donors in Ge and Si is derived in the limit of small compensations. The lineshapes for absorptions in Ge(Sb), Ge(P), Ge(As) and Si(As) are also calculated.     

Density of states measured by scanning-tunneling spectroscopy sheds new light on the optical transitions in PbSe nanocrystals

The density-of-states function of individual colloidal PbSe nanocrystals varying in diameter between 3 and 7 nm is measured by resonant tunneling spectroscopy. It is in semiquantitative agreement with tight-binding calculations, but the energy separation between electron (hole) levels of S and P symmetry is systematically smaller than predicted by the theory. These results provide an explanation for the second and third excitonic optical transitions, which have been debated for a long time.     

Excitonic and quasiparticle gaps in Si nanocrystals

We present calculations of the one- and two-particle excitations in silicon nanocrystals. The one-particle properties are handled in the GW approximation, and the excitonic gap is obtained from the Bethe-Salpeter equation. We develop a tight binding version of these methods to treat clusters up to 275 atoms. The self-energy and Coulomb corrections almost exactly cancel each other for crystallites with radius larger than 0.6 nm. The result of this cancellation is that one-particle calculations give quite accurate values for the excitonic gap of crystallites in the most studied range of sizes.