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Author

Guy Allan

Other affiliations: Ghent University
Bio: Guy Allan 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 39, co-authored 84 publications receiving 9349 citations. Previous affiliations of Guy Allan include Ghent University.


Papers
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TL;DR: 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 as discussed by the authors.
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.

1,793 citations

Journal ArticleDOI
25 Sep 2009-ACS Nano
TL;DR: 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 Q dot dielectric function.
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.

1,022 citations

Journal ArticleDOI
TL;DR: The luminescence in the visible range of porous silicon is analyzed in the hypothesis of quantum confinement and it is concluded that experimental nonradiative processes in porous silicon are more efficient than calculated radiative ones at T=300 K.
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.

860 citations

Journal ArticleDOI
TL;DR: In this article, inductively coupled plasma mass spectrometry (ICP-MS) was combined with UV-vis−NIR spectrophotometry and transmission electron microscopy to determine the nanocrystal composition and molar extinction coefficient ϵ of colloidal PbSe quantum dot (Q-PbSe) suspensions.
Abstract: Inductively coupled plasma mass spectrometry (ICP-MS) was combined with UV–vis−NIR spectrophotometry and transmission electron microscopy to determine the nanocrystal composition and molar extinction coefficient ϵ of colloidal PbSe quantum dot (Q-PbSe) suspensions. The ICP-MS results show a nonstoichiometric Pb/Se ratio, with a systematic excess of lead for all samples studied. The observed ratio is consistent with a faceted spherical Q-PbSe model, composed of a quasi stoichiometric Q-PbSe core terminated by a Pb surface shell. At high photon energies, we find that ϵ scales with the nanocrystal volume, irrespective of the Q-PbSe size. From ϵ, we calculated a size-independent absorption coefficient. Its value is in good agreement with the theoretical value for bulk PbSe. At the band gap, ϵ is size-dependent. The resulting absorption coefficient increases quadratically with decreasing Q-PbSe size. Calculations of the oscillator strength of the first optical transition are in good agreement with theoretical ...

514 citations

Journal ArticleDOI
TL;DR: In this article, the electronic structure of spherical silicon crystallites containing up to 2058 Si atoms was calculated and a variation of the optical band gap with respect to the size of the crystallites was predicted in very good agreement with available experimental results.
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.

419 citations


Cited by
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TL;DR: Recent advances at the intersection of plasmonics and photovoltaics are surveyed and an outlook on the future of solar cells based on these principles is offered.
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.

8,028 citations

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TL;DR: In this article, a review of the properties of the Al x Ga1−x As/GaAs heterostructure system is presented, which can be classified into sixteen groups: (1) lattice constant and crystal density, (2) melting point, (3) thermal expansion coefficient, (4), lattice dynamic properties, (5) lattices thermal properties,(6) electronic-band structure, (7) external perturbation effects on the bandgap energy, (8) effective mass, (9) deformation potential, (10) static and
Abstract: The Al x Ga1−x As/GaAs heterostructure system is potentially useful material for high‐speed digital, high‐frequency microwave, and electro‐optic device applications Even though the basic Al x Ga1−x As/GaAs heterostructure concepts are understood at this time, some practical device parameters in this system have been hampered by a lack of definite knowledge of many material parameters Recently, Blakemore has presented numerical and graphical information about many of the physical and electronic properties of GaAs [J S Blakemore, J Appl Phys 5 3, R123 (1982)] The purpose of this review is (i) to obtain and clarify all the various material parameters of Al x Ga1−x As alloy from a systematic point of view, and (ii) to present key properties of the material parameters for a variety of research works and device applications A complete set of material parameters are considered in this review for GaAs, AlAs, and Al x Ga1−x As alloys The model used is based on an interpolation scheme and, therefore, necessitates known values of the parameters for the related binaries (GaAs and AlAs) The material parameters and properties considered in the present review can be classified into sixteen groups: (1) lattice constant and crystal density, (2) melting point, (3) thermal expansion coefficient, (4) lattice dynamic properties, (5) lattice thermal properties, (6) electronic‐band structure, (7) external perturbation effects on the band‐gap energy, (8) effective mass, (9) deformation potential, (10) static and high‐frequency dielectric constants, (11) magnetic susceptibility, (12) piezoelectric constant, (13) Frohlich coupling parameter, (14) electron transport properties, (15) optical properties, and (16) photoelastic properties Of particular interest is the deviation of material parameters from linearity with respect to the AlAs mole fraction x Some material parameters, such as lattice constant, crystal density, thermal expansion coefficient, dielectric constant, and elastic constant, obey Vegard’s rule well Other parameters, eg, electronic‐band energy, lattice vibration (phonon) energy, Debye temperature, and impurity ionization energy, exhibit quadratic dependence upon the AlAs mole fraction However, some kinds of the material parameters, eg, lattice thermal conductivity, exhibit very strong nonlinearity with respect to x, which arises from the effects of alloy disorder It is found that the present model provides generally acceptable parameters in good agreement with the existing experimental data A detailed discussion is also given of the acceptability of such interpolated parameters from an aspect of solid‐state physics Key properties of the material parameters for use in research work and a variety of Al x Ga1−x As/GaAs device applications are also discussed in detail

2,671 citations

Journal ArticleDOI
23 Nov 2000-Nature
TL;DR: It is demonstrated that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix, which opens a route to the fabrication of a silicon laser.
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.

2,204 citations

Journal ArticleDOI
TL;DR: UV-Visible ار راد ن .د TiO2 ( تیفرظ راون مان هب نورتکلا یاراد لماش VB و ) رگید اب لاقتنا VB (CO2) .
Abstract: UV-Visible ار راد ن .د TiO2 ( تیفرظ راون مان هب نورتکلا یاراد یژرنا زارت لماش VB و ) رگید زارت ی یژرنا اب ( ییاناسر راون مان هب نورتکلا زا یلاخ و رتلااب VB یم ) .دشاب ت ود نیا نیب یژرنا توافت یژرنا فاکش زار ، پگ دناب هدیمان یم .دوش هک ینامز زا نورتکلا لاقتنا VB هب VB یم ماجنا دریگ ، TiO2 اب ودح یژرنا بذج د ev 2 / 3 ، نورتکلا تفج کی دیلوت یم هرفح .دیامن و نورتکلا هرفح ی نا اب هدش دیلوت یم کرتشم حطس هب لاقت ثعاب دناوت شنکاو ماجنا اه یی ددرگ . TiO2 دربراک ،دراد یدایز یاه هلمج زا یم ناوت اوه یگدولآ هیفصت یارب (CO2) و بآ و ... نآ زا هدافتسا درک .

2,055 citations

Journal ArticleDOI
TL;DR: The lifetime of a photophysical process is the time required by a population of N electronically excited molecules to be reduced by a factor of e via the loss of energy through fluorescence and other non-radiative processes and the average length of time τ is called the mean lifetime, or simply lifetime.
Abstract: When a molecule absorbs a photon of appropriate energy, a chain of photophysical events ensues, such as internal conversion or vibrational relaxation (loss of energy in the absence of light emission), fluorescence, intersystem crossing (from singlet state to a triplet state) and phosphorescence, as shown in the Jablonski diagram for organic molecules (Fig. 1). Each of the processes occurs with a certain probability, characterized by decay rate constants (k). It can be shown that the average length of time τ for the set of molecules to decay from one state to another is reciprocally proportional to the rate of decay: τ = 1/k. This average length of time is called the mean lifetime, or simply lifetime. It can also be shown that the lifetime of a photophysical process is the time required by a population of N electronically excited molecules to be reduced by a factor of e. Correspondingly, the fluorescence lifetime is the time required by a population of excited fluorophores to decrease exponentially to N/e via the loss of energy through fluorescence and other non-radiative processes. The lifetime of photophycal processes vary significantly from tens of femotoseconds for internal conversion1,2 to nanoseconds for fluorescence and microseconds or seconds for phosphorescence.1 Open in a separate window Figure 1 Jablonski diagram and a timescale of photophysical processes for organic molecules.

1,829 citations