Theory of multi-exciton states in semiconductor nanocrystals

In this article, the fundamental physics of multi-exciton states in semiconductor nano-crystals is reviewed focusing on the mesoscopic enhancement of the excitonic radiative decay rate and the excitonic optical nonlinearity and the mechanism of their saturation with increase of the nanocrystal size. In the case of the radiative decay rate the thermal excitation of excited exciton states having small oscillator strength within the homogeneous linewidth of the exciton ground state is essential in determining the saturation behavior. The weakly correlated exciton pair states are found to cause a cancellation effect in the third-order nonlinear optical susceptibility at the exciton resonance, providing the first consistent understanding of the experimentally observed saturation of the mesoscopic enhancement of the excitonic optical nonlinearity. The presence of the weakly correlated exciton pair states is confirmed convincingly from the good correspondence between theory and experiments on the induced absorption spectra from the exciton state in CuCl nanocrystals. Furthermore, ultrafast relaxation processes of biexcitons are discussed in conjunction with the observed very fast rise of the biexciton gain in nanocrystals. In prospect of future progress in research, the theoretical formulation to calculate the triexciton states as one of the multi-exciton states beyond the biexciton is presented for the first time including the electron-hole exchange interaction.     

渐变折射率光量子阱对束缚态能级的调整

在对称的均匀电介质材料光子晶体体系中插入另一折射率渐变的光子晶体可构成光量子阱结构.利用时域有限差分法计算了不同折射率分布光量子阱结构的传输谱.研究表明：束缚态是对处于垒光子晶体禁带中的阱光子晶体导通带的离散化,束缚态能级个数等于阱光子晶体结构单元的重复周期数；以渐变方式调整阱区折射率分布,可在特定频率范围内得到新的互不交叠的束缚态.这样在有限的禁带区域可以成倍增加光子束缚态而无需增大光量子阱结构的尺寸,使信道密度最大化、光波有效带宽的使用最优化.这种量子阱结构可用于制作超窄带滤波器和多通道窄带滤波器,有望在光通信超密集波分复用和光学精密测量技术中获得广泛应用. 关键词： 光量子阱 光子束缚态 渐变折射率 光子晶体     

Heavy photon states in photonic chains of resonantly coupled cavities with supermonodispersive microspheres

We propose and demonstrate a "bottom-up" approach to constructing photonic structures for photon manipulation. Supermonodispersive polymer microspheres are used as building blocks and a size uniformity better than 0.05% could be obtained by sorting the spheres using spectroscopic methods. The spheres are positioned in a V groove on a silicon substrate and form a photonic chain with resonant coupling of the optical whispering-gallery modes. Photonic band modes are clearly observed in fluorescence and resonant scattering spectra, and an excellent agreement with a tight-binding model calculation is found. Heavy photon states and a group index as high as 40 are obtained.     

Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals

We report room-temperature ordered multiphoton emission from multiexciton states of single CdSe(CdZnS) core(-shell) colloidal nanocrystals (NCs) that are synthesized by wet chemical methods. Spectrally and temporally resolved measurements of biexciton and triexciton emission from single NCs are also presented. A simple four level system models the results accurately and provides estimates for biexciton and triexciton radiative lifetimes and quantum yields.     

Efficient generation of cluster states with semiconductor double-dot molecules on a chip

We propose an efficient scheme for the generation of the cluster states directly using the iSWAP gate, with semiconductor double-dot molecules on a chip. The implementation of an iSWAP gate only requires resonant interaction between a molecule and a transmission line resonator, which results in considerable improvement for gate speed comparing to conventional dispersive techniques. Meanwhile, the fast generation speed is also very important in view of decoherence. Therefore, our approach makes one-way quantum computation more feasible via this on chip architecture.     

Quasi-nanowires from fluorescent semiconductor nanocrystals on the surface of oriented DNA molecules

Ordered structures in the form of quasi-nanowires were obtained from CdSe/ZnS fluorescent semiconductor nanoparticles of spherical (quantum dots) or rodlike (quantum rods) form by their electrostatic deposition on DNA molecules with subsequent stretching of the molecules on a solid substrate. Positively charged nanoparticles were fixed along the negatively charged backbones of DNA molecules by electrostatic interactions in an aqueous solution of a mixture of DNA with quantum particles at different stoichiometric ratios. Strands of single DNA molecules with quantum particles fixed along them were immobilized and stretched on hydrophobic surfaces using the molecular combing technique. It is shown that, by varying the nanoparticle charge and the stoichiometry of complexes of DNA with particles, it is possible to create fluorescent structures with predetermined morphology and properties.     

Self-purification in semiconductor nanocrystals

Doping of nanocrystals is an important and very difficult task. "Self-purification" mechanisms are often claimed to make this task even more difficult, as the distance a defect or impurity must move to reach the surface of a nanocrystal is very small. We show that self-purification can be explained through energetic arguments and is an intrinsic property of defects in semiconductor nanocrystals. We find the formation energies of defects increases as the size of the nanocrystal decreases. We analyze the case of Mn-doped CdSe nanocrystals and compare our results to experimental findings.     

Photoinduced relaxation processes in complexes based on semiconductor CdSe nanocrystals and organic molecules

Possible pathways and mechanisms of photoinduced relaxation processes in CdSe and CdSe/ZnS nanocrystals that are surface-passivated (as a result of two-point interactions) by nitrogen-containing ligands of different nature (pyridyl-substituted porphyrin molecules and their derivatives, 2,2′-dipyridyl, and 1,10-phenanthroline) are studied in toluene at 295 K by the methods of steady-state and time-resolved spectroscopy. In nanocrystal-organic ligand composites, a high luminescence-quenching efficiency of nanocrystals by molecules of tetrapyrrole compounds compared to 2,2′-dipyridyl, 1,10-shenanthroline, and pyridine can be associated with the electronic properties of a π conjugated macrocycle and anchor groups. The fundamental role that mesomeric effects and the partial overlap of HOMOs and LUMOs of porphyrin and meso-pyridyl rings play in the enhancement of nonradiative recombination of charges in a surface interface layer is substantiated.     

Tunable photon lifetime in photonic molecules: a concept for delaying an optical signal

We experimentally and theoretically studied the photon lifetime spectral distribution in two coherently coupled spherical microcavities of 3-16 microm diameter forming a photonic molecule, which shows a multipeak narrowband modal structure resulting from lifting of the mode degeneracy with respect to the azimuthal quantum number. The results demonstrate the feasibility of photonic molecules as a basis for a multichannel, wavelength-tunable optical delay-line device, which can be used for delay times in the range 10 ps to 1 ns.     

Photoluminescence polarization of semiconductor nanocrystals

We review the polarization properties of photoluminescence (PL) in nanocrystals (NCs) from both theoretical and experimental points of view. We show that, under linearly polarized excitation, NCs emit partly polarized light owing to their uniaxial structure or their anisotropic shape. In elongated NCs, the anisotropy may have two origins, the electronic confinement or the effect of depolarizing field created by the light-induced charges on the interfaces. Results of polarization studies in porous silicon are presented. They are explained by the shape of the Si NCs. Experiments in CdSe NCs reveal the fine structure of the excitonic levels and show evidence of the enhancement of the electron-hole exchange energy with decreasing NC size. Spin orientation in wurtzite-type NCs is achieved by optical pumping with circularly polarized light. The effect of a magnetic field on the degree of circular polarization and the mechanisms of spin relaxation are discussed. Results in large-size NCs are presented.     

Optical activity of semiconductor nanocrystals with ionic impurities

The strength of the enantioselective interaction of chiral semiconductor nanocrystals with circularly polarized light can be varied over a wide range, which finds a series of important applications in modern nanophotonics. As a rule, this interaction is relatively weak, because the dimension of nanocrystals is much smaller than the wavelength of the optical radiation, and the optical activity of nanocrystals is rather low. In this work, we show theoretically that, by applying ion doping, one can significantly enhance the optical activity of nanocrystals and to vary its magnitude over a wide range of values and over a wide range of frequencies. We show that, by precisely arranging impurities inside nanocrystals, one can optimize the rotatory strengths of intraband transitions, making them 100 times stronger than typical rotatory strengths of small chiral molecules.     

Persistent hole burning in semiconductor nanocrystals

The persistent spectral hole burning (PSHB) phenomenon was found to occur in many kinds of nanocrystalline semiconductors, such as CdSe, CdS, CuCl, CuBr and CuI, embedded in crystals, glass or polymers. In inhomogeneously broadened exciton absorption spectra of these nanocrystals, the spectral hole and its associated structure were created by the narrow-band laser excitation and were conserved for more than several hours at 2 K. Hole depth grew in proportion to the logarithm of the burning fluence. Thermally-annealing and light-induced hole-filling phenomena were observed. The hole burning takes place by the tunneling process through potential barriers with broadly distributed barrier height and thickness. Unusual luminescence behaviors related to the PSHB phenomena were also observed. They are luminescence elongation with increase of the light exposure and hole burning in the luminescence spectrum. The observed PSHB phenomena are explained by the exciton localization and the succeeding ionization of nanocrystals. The energy of the photoionized nanocrystal is released from the original energy and the new energies depend on the spatial arrangement of the trapped carriers. Quantum confinement of carriers and resulting strong Coulomb interaction between confined carriers and trapped carriers are essential for the energy change. Possible applications of the PSHB phenomenon is discussed.     

用不同密度分布的发光分子探测光子晶体的全态密度

单一原子（分子）的自发辐射衰变的动力学性质强烈地依赖于其在光子晶体中的位置及其辐射偶极矩与所处位置场的相对方向.测量单一原子（分子）的自发辐射衰变特性只能反映光子晶体的局域态密度特征，而不能反映光子晶体的全态密度特征.理论上研究发现，通过引入含不同密度分布的发光分子可以探测到光子晶体的全态密度的部分细节甚至全部信息.按来源首次将全态密度分为两个部分，证明了特定的发光分子分布可以完善地反映其中的一部分或者全部，这为解释、设计加速或抑制原子（分子）自发辐射的实验提供了有益的指导. 关键词： 光子晶体 自发辐射 态密度 密度分布     

Single photon sources with single semiconductor quantum dots

In t.his contribution, we briefly recall the basic concepts of quantum optics and properties of semicon- ductor quantum clot. （QD） which a.re necessary to the nnderstanding of the physics of single-photon generation with single QDs. Firstly, we address the theory of quantmn emitter-cavity system, the fluorescence and optical properties of semiconductor QDs, and the photon statistics as well as opti- cal properties of the QDs. We then review the localizatioll of single semiconductor QDs in quantum confined optical microcavity systems to achieve their overall optical properties and perfornances in terms of strong coupling regime, elfieiency, directionality, and polarization control. Furthermore, we will discuss the recenl, progress on the fabrication of single photon sources, and various a.pproaehes for embedding single QDs into mieroca,vities or photonic crystal nanoeavities and show how to ex- tend the wavelength range. We focus in part;icular on new generations of electrically driven QD single photon source leading to high repetition rates, efficiencies at elevated temperature operation. Besides strong eoupling regime, and high collection new development;s of room temperature sin- gle photon emission in the strong coupling regime are reviewed. The generation of indistinguishable photons and remaining challenges for pract ical single-photon sources are also discussed.     

Photo-modification and synthesis of semiconductor nanocrystals

Both photo-oxidation and photosynthesis manifest a strong interaction between nanoparticles and photons due to the large surface area-to-volume ratio. The final sizes of the semiconductor nanocrystals are determined by the photon energy during these phenomena. The photosynthesis is demonstrated in a Si-rich oxide and is similar to thermal synthesis, which involves the decomposition of SiO_x into Si and SiO₂, that is well known and often employed to form Si or Ge nanocrystals embedded in SiO₂ by annealing SiO_x at high temperature. However, photosynthesis is much faster, and allows the low-temperature growth of Si nanocrystals and is found to be pronounced in the SiO nanopowder, which is made by thermal CVD using SiH₄ and O₂. The minimum laser power required for the photosynthesis in the SiO nanopowder is much lower than in the Si-rich oxide formed by the co-sputtering of Si and SiO₂. This is attributed to the weak bond strength of Si-Si and Si-O in the SiO nanopowder. Photosynthesis, which can control the size and position of Si nanocrystals, is a novel nanofabrication technique making the best use of the strong interaction between photons and nanoparticles.