We report on the possibility of describing the absorption and emission characteristics of an ensemble of silicon nanocrystals (NCs) with realistic distributions in the NC size, by the sum of the reponses of the single NCs. The individual NC responses are evaluated by means of ab-initio theoretical calculations and the summation is performed by taking into account the trend of the optical properties as a function of NC size and oxidation degree. The comparison with experimental results shows a nice matching of the spectra, also without any tuning of the parameters. Finally, the possibility of adapting the model in order to reproduce the experimental data is explored and discussed.
We develop a phenomenological theory of inhomogeneous broadening in zero-dimensional systems and apply it to study photoluminescence (PL) spectra of silicon nanocrystals measured at helium and room temperatures. The proposed approach allowed us to explain experimentally observed PL peak asymmetry, linear dependence of the peak width on its maximum and anomalous alteration of spectral characteristics with temperature increase.
Tin-containing nanocrystals, embedded in silicon, have been fabricated by growing an epitaxial layer of Si_{1-x-y}Sn_{x}C_{y}, where x = 1.6 % and y = 0.04 %, followed by annealing at various temperatures ranging from 650 to 900 degrees C. The nanocrystal density and average diameters are determined by scanning transmission-electron microscopy to ~ 10^{17} cm^{-3} and ~ 5 nm, respectively. Photoluminescence spectroscopy demonstrates that the light emission is very pronounced for samples annealed at 725 degrees C, and Rutherford back-scattering spectrometry shows that the nanocrystals are predo…
It is widely accepted that the properties of most semiconductor nanocrystals can be tuned by their core size, shape and material. In covalent semiconductor nanocrystal materials, such as silicon, germanium or carbon, certain degree of tunability of the properties can be also achieved by the surface ligands. In particular, covalently bonded ligand species on the surface of such a nanocrystal (i) contribute to the density of states of the core via orbital delocalization; (ii) might introduce strain via ligand-to-ligand steric hindrance and (iii) will cause charge transfer from/to the core. In th…
In most of the realistic ab initio and model calculations which have appeared on the emission of light from Si nanocrystals, the role of surface oxygen has been usually ignored, underestimated or completely ruled out. We investigate theoretically, by density functional theory (DFT/B3LYP) possible modes of oxygen bonding in hydrogen terminated silicon quantum dots using as a representative case of the Si29 nanocrystal. We have considered Bridge-bonded oxygen (BBO), Doubly-bonded oxygen (DBO), hydroxyl (OH) and Mix of these oxidizing agents. Due to stoichiometry, all comparisons performed are un…
We investigate the photon statistics of the light emitted by single self-assembled hybrid gold-CdSe/CdS/CdZnS colloidal nanocrystal supraparticles through the detailed analysis of the intensity autocorrelation function $g^{(2)}(τ)$. We first reveal that, despite the large number of nanocrystals involved in the supraparticle emission, antibunching can be observed. We then present a model based on non-coherent Förster energy transfer and Auger recombination that well captures photon antibunching. Finally, we demonstrate that some supraparticles exhibit a bunching effect at short time scales corr…
Silicon photoluminescence and lasing have been critical issues to breakthrough bottlenecks in the understanding of luminescence mechanisms. Unfortunately, long-standing disputes about the exciton recombination mechanism and fluorescence lifetime remain unresolved, especially about whether silicon nanocrystals (Si NCs) can realize fast direct-bandgap-like optical transitions. Here, using ground-state and excited-state density functional theory (DFT), we obtained intrinsic phonon-free optical transitions at sizes from Si22 to Si705, showing that very small Si NCs can realize a strong direct opti…
Silicon nanocrystals (Si NCs) have shown great promise for electroluminescent and photoluminescent applications. In order to optimize the properties of Si NC devices, however, electronic transport in Si NCs films needs to be thoroughly understood. Here we present a systematic study of the temperature and electric field dependence of conductivity in films of alkyl-ligand-terminated Si NCs, which to date have shown the highest potential for device applications. Our measurements suggest that the conductivity is limited by the ionization of rare NCs containing donor impurities. At low bias, this i…
Silicon lasers have been the most challenging element for the monolithic integrated Si photonics. Here we report the first successful all-Si laser at room temperature based on silicon nanocrystals (Si NCs) with high optical gains. The active Si NC layer was made from hydrogen silsesquioxane (HSQ) that had undergone a phase separation annealing, followed by high-pressure hydrogen passivation. Using the nanoimprint technique, a second-order Bragg grating was made on the active layer as the distributed feedback (DFB) laser cavity. This Si NC DFB laser device was optically pumped with femtosecond …
We present a theory of the local field corrections to the spontaneous emission rate for the array of silicon nanocrystals in silicon dioxide. An analytical result for the Purcell factor is obtained. We demonstrate that the local-field corrections are sensitive to the volume fill factor of the nanocrystals in the sample and are suppressed for large values of the fill factor. The local-field corrections and the photonic density of states are shown to be described by two different effective permittivities: the harmonic mean between the nanocrystal and the matrix permittivities and the Maxwell-Gar…
Hierarchical material nanostructuring is considered to be a very promising direction for high performance thermoelectric materials. In this work we investigate thermal transport in hierarchically nanostructured silicon. We consider the combined presence of nanocrystallinity and nanopores, arranged under both ordered and randomized positions and sizes, by solving the Boltzmann transport equation using the Monte Carlo method. We show that nanocrystalline boundaries degrade the thermal conductivity more drastically when the average grain size becomes smaller than the average phonon mean free path…
We present a comprehensive and integrated model-independent ab initio study of the structural, cohesive, electronic, and optical properties of silicon quantum dots of various morphologies and sizes in the framework of all-electron static and time-dependent density functional theory (DFT, TDFT), using the well-tested B3LYP and other properly chosen functional(s). Our raw ab initio results for all these properties for hydrogen passivated nanocrystals of various growth models and sizes from 1 to 32 Angstroms, are subsequently fitted, using power-law dependence with judicially selected exponents, …
Controlling thermal energy transfer at the nanoscale has become critically important in many applications and thermal properties since it often limits device performance. In this work, we study the effects on thermal conductivity arising from the nanoscale structure of free-standing nanocrystalline silicon films and the increasing surface-to-volume ratio when fabricated into suspended optomechanical nanobeams. We characterize thermal transport in structures with different grain sizes and elucidate the relative impact of grain size and geometrical dimensions on thermal conductivity. We use a mi…
We report the observation of room-temperature superradiance from single, highly luminescent diamond nanocrystals with spatial dimensions much smaller than the wavelength of light, and each containing a large number (~10^3) of embedded nitrogen-vacancy (NV) centres. After excitation of the nanodiamonds with an off-resonant, green laser pulse, we observe i) ultrafast radiative lifetimes down to ~ 1 ns, and ii) super-Poissonian photon bunching in the autocorrelation function of the light emitted from the fastest nanodiamonds. We explain our findings with a detailed theoretical model based on coll…
Transition between cooperative emission regimes in giant perovskite nanocrystals
IBM Research Europe – Zurich（IBM欧洲苏黎世研究中心）；Institute of Inorganic Chemistry, Department of Chemistry and Applied Bioscience, ETH Zurich（苏黎世联邦理工学院应用化学与生物科学系无机化学研究所）；Laboratory of Thin Films and Photovoltaics, Empa — Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技与测试研究院薄膜与光伏实验室）
Direct determination of the collective pinning radius in high temperature superconductors
利用硅微振荡器研究了微米级$_2$ CaCuPDMATHABMM O $_{8+δ}$单晶的不可逆磁行为开始时的有限尺寸效应。我们发现一个不可逆性线出现远低于热力学布拉格玻璃熔化线在磁场，增加与样品半径和降低温度。我们发现，这种大小相关的不可逆线可以识别与交叉之间的拉金和随机流形制度的涡晶格横向粗糙度。我们的方法可以用{ \it direct way}确定三维弱集体钉扎Larkin半径。
