Christophe Delerue

Bio: Christophe Delerue is an academic researcher from Centre national de la recherche scientifique. The author has contributed to research in topics: Quantum dot & Band gap. The author has an hindex of 54, co-authored 241 publications receiving 12185 citations. Previous affiliations of Christophe Delerue include university of lille & Utrecht University.

Electronic States and Luminescence in Porous Silicon Quantum Dots: The Role of Oxygen

Abstract: Depending on the size, the photoluminescence (PL) of silicon quantum dots present in porous silicon can be tuned from the near infrared to the ultraviolet when the surface is passivated with Si-H bonds. After exposure to oxygen, the PL shifts to the red by as much as 1 eV. This shift and the changes in PL intensity and decay time, show that both quantum confinement and surface passivation determine the electronic states of silicon quantum dots. A theoretical model in which new electronic states appear in the band gap of the smaller quantum dots when a Si-O bond is formed, is in good agreement with experiments. This result clarifies the controversy regarding the PL mechanisms in porous silicon.

Size-dependent optical properties of colloidal PbS quantum dots.

Abstract: We quantitatively investigate the size-dependent optical properties of colloidal PbS nanocrystals or quantum dots (Qdots), by combining the Qdot absorbance spectra with detailed elemental analysis of the Qdot suspensions. At high energies, the molar extinction coefficient epsilon increases with the Qdot volume d(3) and agrees with theoretical calculations using the Maxwell-Garnett effective medium theory and bulk values for the Qdot dielectric function. This demonstrates that quantum confinement has no influence on epsilon in this spectral range, and it provides an accurate method to calculate the Qdot concentration. Around the band gap, epsilon only increases with d(1.3), and values are comparable to the epsilon of PbSe Qdots. The data are related to the oscillator strength f(if) of the band gap transition and results agree well with theoretical tight-binding calculations, predicting a linear dependence of f(if) on d. For both PbS and PbSe Qdots, the exciton lifetime tau is calculated from f(if). We find values ranging between 1 and 3 mus, in agreement with experimental literature data from time-resolved luminescence spectroscopy. Our results provide a thorough general framework to calculate and understand the optical properties of suspended colloidal quantum dots. Most importantly, it highlights the significance of the local field factor in these systems.

Theoretical aspects of the luminescence of porous silicon.

Abstract: The luminescence in the visible range of porous silicon is analyzed in the hypothesis of quantum confinement. We calculate the electronic and optical properties of silicon crystallites and wires with sizes between 0 and 4.5 nm. The band-gap energies of such confined systems are in agreement with the photon energies observed in luminescence. We calculate the radiative recombination times of the confined excitons. We conclude that experimental nonradiative processes in porous silicon are more efficient than calculated radiative ones at T=300 K. The high photoluminescence efficiency of porous silicon is due to the small probability of finding a nonradiative recombination center in silicon nanocrystallites. Recently, it has been proposed that the low-temperature dependence of the experimental radiative decay time of the luminescence of porous silicon could be explained by the exchange splitting in the fundamental exciton. We show that the influence of the valley-orbit splitting cannot be excluded. The sharp optical-absorption edge above 3.0 eV is not proof of the molecular origin of the properties of porous silicon because silicon nanostructures present a similar absorption spectrum. We calculate the nonradiative capture of electrons or holes on silicon dangling bonds and show that it is very dependent on the confinement. We find that the presence of one dangling bond at the surface of a crystallite in porous silicon must destroy its luminescent properties above 1.1 eV but can produce a luminescence below 1.1 eV due to a radiative capture on the dangling bond.

Electronic structure and optical properties of silicon crystallites: Application to porous silicon

Abstract: We have calculated the electronic structure of spherical silicon crystallites containing up to 2058 Si atoms. We predict a variation of the optical band gap with respect to the size of the crystallites in very good agreement with available experimental results. We also calculate the electron‐hole recombination time which is of the order of 10−4–10−6 s for crystallites with diameters of 2.0–3.0 nm. We conclude that small silicon crystallites can have interesting optical properties in the visible range. These results are applied to porous silicon for which we confirm that a possible origin of the luminescence is the quantum confinement.

Quantum confinement in germanium nanocrystals

Abstract: The electronic structure of Ge nanocrystals is studied using a sp3 tight binding description. Analytical laws for the confinement energies, valid over the whole range of sizes, are derived. We validate our results with ab initio calculations in the local density approximation for smaller clusters. Comparing to experimental data, we conclude that, similar to the case of silicon: (a) the blue-green photoluminescence (PL) of Ge nanocrystals comes from defects in the oxide and (b) the size dependent PL in the near infrared probably involves a deep trap in the gap of the nanocrystals. We predict that the radiative lifetimes remain long in spite of the small difference (0.14 eV) between direct and indirect gaps of bulk Ge.

Plasmonics for improved photovoltaic devices

Abstract: The emerging field of plasmonics has yielded methods for guiding and localizing light at the nanoscale, well below the scale of the wavelength of light in free space. Now plasmonics researchers are turning their attention to photovoltaics, where design approaches based on plasmonics can be used to improve absorption in photovoltaic devices, permitting a considerable reduction in the physical thickness of solar photovoltaic absorber layers, and yielding new options for solar-cell design. In this review, we survey recent advances at the intersection of plasmonics and photovoltaics and offer an outlook on the future of solar cells based on these principles.

Band parameters for III–V compound semiconductors and their alloys

Abstract: We present a comprehensive, up-to-date compilation of band parameters for the technologically important III–V zinc blende and wurtzite compound semiconductors: GaAs, GaSb, GaP, GaN, AlAs, AlSb, AlP, AlN, InAs, InSb, InP, and InN, along with their ternary and quaternary alloys. Based on a review of the existing literature, complete and consistent parameter sets are given for all materials. Emphasizing the quantities required for band structure calculations, we tabulate the direct and indirect energy gaps, spin-orbit, and crystal-field splittings, alloy bowing parameters, effective masses for electrons, heavy, light, and split-off holes, Luttinger parameters, interband momentum matrix elements, and deformation potentials, including temperature and alloy-composition dependences where available. Heterostructure band offsets are also given, on an absolute scale that allows any material to be aligned relative to any other.

Optical gain in silicon nanocrystals

Abstract: Adding optical functionality to a silicon microelectronic chip is one of the most challenging problems of materials research. Silicon is an indirect-bandgap semiconductor and so is an inefficient emitter of light. For this reason, integration of optically functional elements with silicon microelectronic circuitry has largely been achieved through the use of direct-bandgap compound semiconductors. For optoelectronic applications, the key device is the light source--a laser. Compound semiconductor lasers exploit low-dimensional electronic systems, such as quantum wells and quantum dots, as the active optical amplifying medium. Here we demonstrate that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix. Net optical gain is seen in both waveguide and transmission configurations, with the material gain being of the same order as that of direct-bandgap quantum dots. We explain the observations using a model based on population inversion of radiative states associated with the Si/SiO2 interface. These findings open a route to the fabrication of a silicon laser.