Population inversion in a single InGaAs quantum dot using the method of adiabatic rapid passage

Preparation of a specific quantum state is a required step for a variety of proposed quantum applications. We report an experimental demonstration of optical quantum state inversion in a single semiconductor quantum dot using adiabatic rapid passage. This method is insensitive to variation in the optical coupling in contrast with earlier work based on Rabi oscillations. We show that when the pulse power exceeds a threshold for inversion, the final state is independent of power. This provides a new tool for preparing quantum states in semiconductor dots and has a wide range of potential uses.     

Optically gated resonant emission of single quantum dots

We report on the resonant emission in coherently driven single semiconductor quantum dots. We demonstrate that an ultraweak nonresonant laser acts as an optical gate for the quantum dot resonant response. We show that the gate laser suppresses Coulomb blockade at the origin of a resonant emission quenching, and that the optically gated quantum dots systematically behave as ideal two-level systems in both regimes of coherent and incoherent resonant emission.     

Excitonic absorption of spherical PbS nanoparticles in zeolite A

We report the optical and structural properties of PbS nanoparticles in zeolite A. The samples were obtained by sulfidation of the Pb²⁺ ion-exchanged zeolite in a thiourea solution at 50 °C. The optical properties of the samples were studied by diffuse reflectance spectroscopy. Their crystalline structure and morphology were studied by electron diffraction and by transmission and scanning electron microscopy. The results show that the nanoparticles are not inside the zeolite cages but outside, embedded in the zeolite matrix. Exciton absorption peaks at much higher energy than the fundamental absorption edge of bulk PbS indicate quantum confinement effects in the spherical shape nanoparticles as a consequence of their small size.     

Plasmonic Dicke effect

We study cooperative emission by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, near a metal nanoparticle. The primary mechanism of cooperative emission is resonant energy transfer between emitters and plasmons rather than Dicke radiative coupling between emitters. The emission is dominated by three superradiant states with the same quantum yield as a single emitter, leading to a drastic reduction of ensemble radiated energy down to just thrice of that by a single emitter, the remaining energy being dissipated in the metal through subradiant states. We perform numerical calculations of system eigenstates and find that the plasmonic Dicke effect interactions affect is not impacted by the interactions between emitters or non-radiative losses in the metal.     

Recent Advances of Light Propagation in Surface Plasmon Enhanced Quantum Dot Devices

Surface plasmons are of particular interest recently as their performance is approaching the enhancement of light emission efficiencies, after synthesized close to the vicinity of solid state materials, i.e., semiconductor structure. As other scientific works have been proposed to improve the light-emitting efficiency, such as the use of resonant cavities, photon recycling, and thin-light emitting layers with periodic surface texturing, surface plasmon possesses a promising way to the light enhancement, due to the energy coupling effect between the emitted photons from the semiconductor and the metallic nanoparticles fabricated by nanotechnology. The usual pathway of plasmon enhanced light emitting devices is the use of Ag/Au nanoparticles coating the surface of semiconductor quantum dot (QD) or quantum well (QW) structures. However, apart from efforts to extract as much light as possible from single-driven surface plasmon-QD/QW, it is possible to enhance the light emission rate with double optical-excitations. This approach is based on the quantum interference between the external lasers and the localized quantum light, and promised to stimulate the development of plasmon-enhanced optical sensors. In this review, we describe the quantum properties of light propagation in hybrid nanoparticle and semiconductor materials, i.e., quantum dot or nanomechanical resonator coupled to Ag/Au nanoparticles, driven by two optical fields. Distinct with single excitation, plasmon-assisted complex driven by two optical fields, exhibit specific quantum interference characteristics that can be used as sensitive all-optical devices, such as the slow light switch, nonlinear optical Kerr modulator, and ultra-sensitive mass sensing. We summarize the recent advances of light propagation in surface plasmon-enhanced quantum dot devices, driven by two optical fields, which would stimulate the development of novel optical materials, deeper theoretical insights, innovative new devices, and plasmonic applications with potential for significant technological and societal impact.     

Quantum Dot Research: Current State and Future Prospects

This article reviews the current state of research involving semiconductor quantum dots, provides a brief review of the theory behind their unique properties, and an introduction explaining the importance of quantum dot research. The characteristic shifting of the band gap energy with quantum dot size, as predicted from the density of states for low-dimensional structures, allows experimental measurements to determine the extent to which quantum confinement effects play a role in the resulting properties. A few of the current techniques used to measure the presence and physical characteristics of quantum dots and their energy levels is reviewed, including transmission electron microscopy, optical transmission, and Raman and photoluminescence spectroscopy. Finally, some of the more exciting applications for quantum dots currently being researched for use in the field of optoelectronics are reviewed, including quantum dot infrared photodetectors, quantum dot lasers, and quantum dot solar cells. Comments are made on the current progress and the future prospects of quantum dot research and device applications.     

Robust quantum dot exciton generation via adiabatic passage with frequency-swept optical pulses

The energy states in semiconductor quantum dots are discrete as in atoms, and quantum states can be coherently controlled with resonant laser pulses. Long coherence times allow the observation of Rabi flopping of a single dipole transition in a solid state device, for which occupancy of the upper state depends sensitively on the dipole moment and the excitation laser power. We report on the robust population inversion in a single quantum dot using an optical technique that exploits rapid adiabatic passage from the ground to an excited state through excitation with laser pulses whose frequency is swept through the resonance. This observation in photoluminescence experiments is made possible by introducing a novel optical detection scheme for the resonant electron hole pair (exciton) generation.     

Surface enhanced Raman scattering by CdS quantum dots

Surface enhanced Raman scattering is studied in nanostructures with CdS quantum dots formed using the Langmuir-Blodgett technology. Features due to quantum dot longitudinal optical phonons are observed in the Raman spectra of both free CdS quantum dots and such dots distributed in an organic matrix. The surface enhanced Raman scattering by nanostructures with CdS quantum dots covered by an Ag cluster film is observed experimentally. Applying Ag clusters onto the nanostructure surfaces results in a sharp (40-fold) increase in the intensity of Raman scattering by optical phonons in the quantum dots. It is shown that the dependence of surface enhanced Raman scattering on the excitation energy is resonant with a maximum at the energy corresponding to the maximum absorption coefficient of Ag clusters.     

Electrical and optical properties of colloidal semiconductor nanocrystals in aqueous environments

Microscale and larger semiconductor crystals have electronic and optical properties that depend on their bulk band structures. When these crystals are reduced into the nanoscale, they enter a new regime in which the electrical and optical properties are no longer influenced solely by their bulk band structures, but are influenced by the crystallite size and shape. In this paper, dimensional confinement and proximity phenomena are examined for colloidal semiconductor nanocrystals in several cases of practical importance. Specifically, we determine the effective binding potentials of selected quantum dots in aqueous environments in various colloidal semiconductor nanocrystals and correlate them with experimentally obtained absorption spectra. We also study fluorescence resonance energy transfer (FRET) between semiconductor crystals connected by short peptide chains as well as the shift in photoluminescence spectra of CdTe nanowires made from a chain of CdTe quantum dots.     

Controlled positioning of self-assembled InAs quantum dots on (1 1 0) GaAs

We report on a new approach for positioning of self-assembled InAs quantum dots on (1 1 0) GaAs with nanometer precision. By combining self-assembly of quantum dots with molecular beam epitaxy on in situ cleaved surfaces (cleaved-edge overgrowth) we have successfully fabricated arrays of long-range ordered InAs quantum dots. Both atomic force microscopy and micro-photoluminescence measurements demonstrate the ability to control position and ordering of the quantum dots with epitaxial precision as well as size and size homogeneity. Furthermore, photoluminescence investigations on dot ensembles and on single dots confirm the high homogeneity and the excellent optical quality of the quantum dots fabricated.     

半导体红外量子点发展现状与前景

半导体量子点具有独特的光学与电学性质,特别是红外量子点良好的光稳定性和生物相容性等优点使其在光电器件、生物医学等领域受到广泛关注。综述了吸收或发射光谱位于红外波段的量子点在激光、能源、光电探测以及生物医学等方面的应用现状与前景,归纳了适用于红外量子点材料的制备方法,并对比了不同方法在应用中的优势。半导体红外量子点材料选择丰富、应用形式多样:InAs量子点被动锁模激光器在1.3 μm波长处产生7.3 GHz的近衍射极限脉冲输出;InAs/GaAs量子点双波长激光器可泵浦产生0.6 nW的THz波;PbS量子点掺杂光纤放大器可在1.53 μm中心波长处实现10.5 dB光增益,带宽160 nm;CdSeTe量子点敏化太阳能电池、异质结Si基量子点太阳能电池的总转换效率可达8%和14.8%;胶质HgTe量子点制成的量子点红外探测器(QDIP)可实现3 μm~5 μm中波红外探测,Ge/Si量子点可实现3 μm~7 μm红外探测;CdTe/ZnSe核壳量子点可用于检测DNA序列的损伤与突变。半导体红外量子点上述应用形式的发展,将进一步促进红外光电系统向高效、快速、大规模集成的方向演进,也将极大地促进临床医学中活体成像检测的应用推广。     

Effects of increasing number of rings on the ion sensing ability of CdSe quantum dots: a theoretical study

A computational study on the structural and electronic properties of a special class of artificial atoms, known as quantum dots, has been carried out. These are semiconductors with unique optical and electronic properties and have been widely used in various applications, such as bio-sensing, bio-imaging, and so on. We have considered quantum dots belonging to II–VI types of semiconductors, due to their wide band gap, possession of large exciton binding energies and unique optical and electronic properties. We have studied their applications as chemical ion sensors by beginning with the study of the ion sensing ability of (CdSe) _n (n?=?3, 6, 9 which are in the size range of ~?0.24, 0.49, 0.74 nm, respectively) quantum dots for cations of the zinc triad, namely Zn²⁺, Cd²⁺, Hg²⁺, and various anions of biological and environmental importance, and studied the effect of increasing number of rings on their ion sensing ability. The various structural, electronic, and optical properties, their interaction energies, and charge transfer on interaction with metal ions and anions have been calculated and reported. Our studies indicate that the CdSe quantum dots can be employed as sensors for both divalent cations and anions, but they can sense cations better than anions.     

Surface-plasmon-assisted electromagnetic field enhancement in semiconductor quantum dots

The temporal development of incident electromagnetic plane waves across semiconductor quantum dots (QDs) is analyzed by the finite-difference time-domain method. By coating the QDs using thin metal films, surface plasmon polaritons (SPPs) can be created. As illustration, our modeling approach is applied to fluorescent multiphoton quantum dots made of cadmium sulphide of particular size (3.7 nm) and energy band gap (2.67 eV). When such a QD is coated by a metal film, a dipole-formed SPP is generated at the external surface of the coated QD by the incident electromagnetic wave with a photon energy of 1.34 eV corresponding to a two-photon process. When the thickness of the metal film is 0.37 nm, the peak intensity of the SPP oscillates through both the thin metal film and the core QD, resulting in an electromagnetic field inside the QD enhanced by a factor of 10, and thus an increased two-photon excitation that can be useful for bioimaging applications. Further increasing the metal film thickness blockades the SPP initially generated at the external surface of the coated QD from penetrating through the metal film, reducing the electromagnetic field inside the QD. PACS 73.22.-f; 78.67.Hc     

限域量子态调控研究

电子、激子和声子等量子态在固体中的行为早已被人们所熟知. 然而，当体系的尺寸只有纳米量级的时候，已有的固体理论常常不能适用，需要新的低维物理理论的建立. 我们系统研究了低维体系限域量子态（包括电子、激子和声子）的行为对环境、应力、压力及光的响应和性质的调控. 较早认识到低维体系之显著的表面-体积比对量子态性质调控之有效性，系统地揭示了低维体系的一系列由表面和应力决定的新颖性质，证明了低维体系的表面和应力效应同量子限域效应同等重要. 本文概况了如下五个方面的结果：（1）一种使用应力效应调控电子能带结构的方法和（2）一种使用表面效应调控电子能带结构的方法（这两个方法都可将低维体系能带从间接能隙调控至直接能隙能带结构）；（3）一种低维体系表面掺杂方法，该方法将在低维体系掺杂中取代传统方法；（4）量子点表面诱导的光致异构现象；（5）基于表面自催化半导体低维结构的形成机理. 希望我们的研究工作有助于促进低维体系在光电子、纳电子、环境、能源、生物和医学等领域的应用.     

Robust Fabrication of Quantum Dots on Few‐Layer MoS2 by Soft Hydrogen Plasma and Post‐Annealing

Apart from unique properties of layered transition‐metal dichalcogenide nanosheets like MoS₂, quantum dots (QDs) from these layered materials promise novel science and applications due to their quantum confinement effect. However, the reported fabrication techniques for such QDs all involve the use of liquid organic solvents and the final material extraction from such liquid dispersions. Here a novel and convenient dry method for the synthesis of MoS₂ quantum dots interspersed on few‐layer MoS₂ using soft hydrogen plasma treatment followed by post‐annealing is demonstrated. The size of MoS₂ nanodots can be well controlled by adjusting the working pressure of hydrogen plasma and post‐thermal annealing. This method relies on the cumulative hydrogen ion bombardment effect which can destroy the hexagonal structure of the top MoS₂ layer and disintegrate the top layer into MoS₂ nanodots and even QDs. Post‐thermal annealing can further reduce the size. Such MoS₂ quantum dots interspersed on few‐layer MoS₂ exhibit two new photoluminescence peaks at around 575 nm because of the quantum confinement effect. This dry method is versatile, scalable, and compatible with the semiconductor manufacturing processes, and can be extended to other layered materials for applications in hydrogen evolution reaction, catalysis, and energy devices.     

反射式无孔径近场Raman研究(英文)

近场扫描光学显微技术与Raman光谱技术的结合能够在纳米尺度下提供化学 /结构信息 ,这对很多应用都是至关重要的 ,比如硅器件 ,纳米器件 ,量子点及生物样品单分子研究。本文报导了采用无孔径探针的近场Raman研究。我们的系统有两大特征 :1 近场Raman的增强是通过金属探针上的银镀层实现的 ,无需样品准备 ;2 系统在反射模式下工作 ,适用于任何样品。这两点对实际应用是至关重要的。我们首次在实际硅器件上用 1秒积分时间获得了 1维近场Raman映射和 2维近场Raman图象。我们首次展示了由于积分时间短 ,该技术可用于成象用途。因此 ,这是近场扫描Raman研究中的一次巨大进步。此外 ,我们系统中采用的金属探针可同时用于AFM及电学特性成象 ,比如电阻 ,电容 ,这些是器件应用中的重要参数。     

半导体微结构物理效应及其应用讲座第三讲半导体的激子效应及其在光电子器件中的应用

人们对半导体中的电子空穴对在库仑互作用下形成的激子态及其有关的物理性质进行了深入研究.激子效应对半导体中的光吸收、发光、激射和光学非线性作用等物理过程具有重要影响,并在半导体光电子器件的研究和开发中得到了重要的应用.与半导体体材料相比,在量子化的低维电子结构中,激子的束缚能要大得多,激子效应增强,而且在较高温度或在电场作用下更稳定.这对制作利用激子效应的光电子器件非常有利.近年来量子阱、量子点等低维结构研究获得飞速的进展,已大大促进了激子效应在新型半导体光源和半导体非线性光电子器件领域的应用.     

Single quantum dots as scanning tunneling microscope tips

We report the use of single quantum dot structures as tips on a scanning tunneling microscope (STM). A single quantum dot structure with a diameter of less than 200 nm and a height of 2 μm was fabricated by reactive ion etching. This dot was placed on a 40 μm-high mesa and mounted on the tip of a STM. The topography of large structures such as quantum wires or gold test substrates is clearly resolved with such a tip. To check the transport properties of the tip, quantum dot arrays were fabricated on resonant tunneling double barrier structures using the same process parameters. Conventional tunneling spectroscopy clearly resolved the 0D states in our samples. Using a metal substrate as second electrode such STM tips can be used to perform high resolution energy spectroscopy on single dots and free standing wire structures.     

Optical Stark effect in a quantum dot: ultrafast control of single exciton polarizations

We report the first experimental study of the optical Stark effect in single semiconductor quantum dots (QD). For below band gap excitation, two-color pump-probe spectra show dispersive line shapes caused by a light-induced blueshift of the excitonic resonance. The line shape depends strongly on the excitation field strength and is determined by the pump-induced phase shift of the coherent QD polarization. Transient spectral oscillations can be understood as rotations of the QD polarization phase with negligible population change. Ultrafast control of the QD polarization is demonstrated.