Tamper resistance in optical excitation transfer based on optical near-field interactions

We present tamper resistance in optical excitation transfer via optical near-field interactions based on the energy dissipation process occurring locally in nanometric devices such as quantum dots. A theoretical comparison with electrical systems is also shown, focusing on the required environmental conditions. Numerical simulations based on virtual photon models demonstrate high tamper resistance.     

Nanometric summation architecture based on optical near-field interaction between quantum dots

A nanoscale data summation architecture is proposed and experimentally demonstrated based on the optical near-field interaction between quantum dots. Based on local electromagnetic interactions between a few nanometric elements via optical near fields, we can combine multiple excitations at a certain quantum dot, which allows construction of a summation architecture. Summation plays a key role for content-addressable memory, which is one of the most important functions in optical networks.     

Optical pulsation mechanism based on optical near-field interactions

We theoretically demonstrate optical pulsation based on optical near-field interactions between quantum nanostructures. It is composed of two quantum dot systems, each of which consists of a combination of smaller and larger quantum dots, so that optical excitation transfer occurs. With an architecture in which the two systems take the role of a timing delay and frequency up-conversion, we observe pulsation in populations pumped by continuous-wave light irradiation. The pulsation is induced with suitable setting of parameters associated with the optical near-field interactions. This will provide critical insights toward the design and implementation of experimental nanophotonic pulse generating devices.     

Fixed-distance coupling and encapsulation of heterogeneous quantum dots using phonon-assisted photo-curing

We propose a novel method of coupling heterogeneous quantum dots at fixed distances and capsulating the coupled quantum dots by utilizing nanometric local curing of a photo-curable polymer caused by multistep electronic transitions based on a phonon-assisted optical near-field process between quantum dots. Because the coupling and the capsulating processes are triggered only when heterogeneous quantum dots floating in a solution closely approach each other to induce optical near-field interactions between them, the distances between the coupled quantum dots are physically guaranteed to be equal to the scale of the optical near fields. To experimentally verify our idea, we fabricated coupled quantum dots, consisting of CdSe and ZnO quantum dots and a UV-curable polymer. We also measured the photoluminescence properties due to the quantum-dot coupling and showed that the individual photoluminescences from the CdSe and ZnO quantum dots exhibited a trade-off relationship.     

Demonstration of nanophotonic NOT gate using near-field optically coupled quantum dots

We propose and demonstrate the operation of a nanometric optical NOT gate using CuCl quantum dots coupled via an optical near-field interaction. The device was smaller than 20 nm and its repeated operation was verified. The operating energy of this device was much lower than that of a conventional photonic device. We also introduce all-optical NAND and NOR gates using coupled quantum dots. Toward an actual nanophotonic device, we discuss the possibility of coupled InAlAs quantum dots. A double layer of InAlAs quantum dots for nanophotonic device operation was prepared using molecular beam epitaxial growth. We obtained a near-field spectroscopy signal, indicating that the InAlAs quantum dots coupled with the optical near field acted as a NOT gate. The experimental results show that the sample has great potential as an actual nanophotonic device. PACS 78.67.Hc; 07.79.Fc; 42.79.Ta     

Nanophotonic droplet: a nanometric optical device consisting of size- and number-selective coupled quantum dots

Although recent advances in fabrication technologies have allowed the realization of highly accurate nanometric devices and systems, most approaches still lack uniformity and mass-production capability sufficient for practical use. We have previously demonstrated a novel technique for autonomously coupling heterogeneous quantum dots to induce particular optical responses based on a simple phonon-assisted photocuring method in which a mixture of quantum dots and photocurable polymer is irradiated with light. The cured polymer sequentially encapsulates coupled quantum dots, forming what we call a nanophotonic droplet. Recently, we found that each quantum dot in the mixture is preferably coupled with other quantum dots of similar size due to a size resonance effect of the optical near-field interactions between them. Moreover, every nanophotonic droplet is likely to contain the same number of coupled quantum dots. In this paper, we describe the basic mechanisms of autonomously fabricating nanophotonic droplets, and we examine the size- and number-selectivity of the quantum dots during their coupling process. The results from experiments show the uniformity of the optical properties of mass-produced nanophotonic droplets, revealed by emission from the contained coupled quantum dots, due to the fundamental characteristics of our method.     

Direct observation of optical excitation transfer based on resonant optical near-field interaction

This article reports the direct observation of long-distance optical excitation transfer based on resonant optical near-field interactions in randomly distributed quantum dots (QDs). We fabricated optical excitation transfer paths based on randomly distributed QDs by using CdSe/ZnS core?Cshell QDs and succeeded for the first time in obtaining output signals resulting from a unidirectional optical excitation transfer length of 2.4???m. Furthermore, we demonstrate that the optical excitation transfer occurs via the resonant excited levels of the QDs with a comparative experiment using non-resonant QDs. This excitation-transfer mechanism allows for intersecting, non-interacting nano-optical wires.     

Pressure-induced modulation of the confinement in self-organized quantum dots produced and detected by a near-field optical probe

Near-field optical probing, or nanoprobing, achieves spatial resolution that surpasses the diffraction limit of light and makes possible the luminescence imaging and spectroscopy of single quantum dots in dense arrays of dots. We use optical nanoprobing to study self-organized InGaAs quantum dots grown on (3 1 1)B oriented GaAs substrates. Here, we emphasize a new feature of nanoprobing: pressure-induced strain modulation near the surface. Operating in near-field optical excitation–collection mode, the probe makes contact with the surface and exerts direct pressure whose main effect is a compressive uniaxial strain under the probe. By adjusting the applied pressure, we modulate the local strain environment in and around a quantum dot, but still preserve the capability to capture its near-field luminescence. Nanoprobe pressure effects modify the confinement potential and radiative emission of single quantum dots, and the coupling strength between dots. This opens new possibilities for the study and control of the optical and electronic properties of single- and coupled-quantum dots.     

Controlling the energy transfer between near-field optically coupled ZnO quantum dots

We performed time-resolved spectroscopy of ZnO quantum dots (QD), and observed exciton energy transfer and dissipation between QD via an optical near-field interaction. Two different sizes of ZnO QD with resonant energy levels were mixed to test the energy transfer and dissipation using time-resolved photoluminescence spectroscopy. The estimated energy transfer time was 144 ps. Furthermore, we demonstrated that the ratio of energy transfer between the resonant energy states could be controlled.     

Second-harmonic generation of semiconductor quantum dots studied by near-field optical microscopy

We present a theoretical study of optical second-harmonic generation(SHG) of symmetric semiconductor quantum dots (QDs) excited by the near field of the tip in a near-field scanning optical microscope. We show that the usual optical transition selection rules for the SH nonlinear interaction between the tip field and the QD are broken when the tip is scanned over the QD, because the tip field varies rapidly over the QD domain. It is also demonstrated that the tip-position dependence of the SH signal essentially maps the spatial distribution of the tip field.     

Optical characterization of quantum dots entrained in microstructured optical fibers

We present a study of the basic optical properties of colloidal CdSe/ZnS core/shell quantum dots entrained in a microstructured optical fiber. Quantum dots suspended in heptane were pulled into the holes surrounding the solid core of a microstructured optical fiber of the holey fiber class via capillary action and are found to remain in the fiber. In this experiment, a laser coupled into the fiber photoexcited quantum dots along the length of the fiber. Quantum dot emission was observed to couple into the fiber core and propagate along the fiber. To investigate the use of such a system in fiber-based light generation or amplification, a second laser overlapping the low-energy portion of the quantum dot emission was simultaneously coupled into the fiber. We observed apparent amplification of this light when photoexciting the quantum dots well above their bandedge.     

Direct observation of variations of optical properties in single quantum dots by using time-resolved near-field scanning optical microscope

We study the variations of optical properties of self-assembled In_0.5Ga_0.5As single quantum dots (QDs) in the spatial and time domains by combining a near-field scanning optical microscope with an ultrafast pulsed laser. Through the examinations of several tens of QDs, we find that the variations of photoluminescence (PL) intensity strongly depend on the condition of the initial carrier creation. The differences in quantum efficiency and those in the carrier flow rate into QDs cause the large distribution of PL intensity when the carriers are excited in the barrier layers. From the results of time-resolved PL decay measurements, we find that there are two types of QDs exhibiting quite different PL decay profiles.     

Electronic and optical properties of InAs/InP self-assembled quantum dots on patterned substrates

We present atomistic theory of electronic and optical properties of a single InAs quantum dot grown on a pyramidal InP nanotemplate. The shape and size of the dot is assumed to follow the nanotemplate shape and size. The electron and valence hole single particle states are calculated using atomistic effective–bond–orbital model with second nearest-neighbor interactions. The electronic calculations are coupled to separately calculated strain distribution via Bir–Pikus Hamiltonian. The optical properties of InAs dots embedded in InP pyramids are calculated by solving the many-exciton Hamiltonian for interacting electron and hole complexes using the configuration–interaction method. The effect of quantum-dot geometry on the optical spectra is investigated by a comparison between dots of different shapes.     

Surface plasmon mediated near-field imaging and optical addressing in nanoscience

We present an overview of recent progress in "plasmonics". We focus our study on the observation and excitation of surface plasmon polaritons (SPPs) with optical near-field microscopy. We discuss in particular recent applications of photon scanning tunnelling microscope (PSTM) for imaging of SPP propagating in metal and dielectric wave guides. We show how near-field scanning optical microscopy (NSOM) can be used to optically and actively address remote nano objects such as quantum dots. Additionally we compare results obtained with near-field microcopy to those obtained with other optical far-field methods of analysis such as leakage radiation microscopy (LRM).     

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.     

Coherent nonlinear optical response of single quantum dots studied by ultrafast near-field spectroscopy

The nonlinear response of single GaAs quantum dots is studied in femtosecond near-field pump-probe experiments. At negative time delays, transient reflectivity spectra show pronounced oscillatory structure around the quantum dot exciton line, providing the first evidence for a perturbed free induction decay of the excitonic polarization. Phase-disturbing Coulomb interactions between the excitonic polarization and continuum excitations dominate the optical nonlinearity on ultrafast time scales. A theoretical analysis based on the semiconductor Bloch equations accounts for this behavior.     

Carrier-diffusion-limited remote optical addressing of single quantum dots

We present a scheme for remotely addressing single quantum dots (QDs) by means of near-field optical microscopy that simply makes use of the polarization of light. A structure containing self-assembled CdTe QDs is covered with a thin metal film presenting sub-wavelength holes. When the optical tip is positioned some distance away from a hole, surface plasmons in the metal coating are generated which, by turning the polarization plane of the excitation light, transfer the excitation towards a chosen hole and induce emission from the underlying dots. In addition, our procedure gives valuable insight into the diffusion of photo-excited carriers in the QD plane that can put limits to the addressing scheme.     

边界对石墨烯量子点非线性光学性质的影响

石墨烯作为一种新型非线性光学材料,在光子学领域具有重要的应用前景,引起研究人员的极大兴趣.本文运用量子化学计算方法研究了边界引入碳碳双键(C=C)和掺杂环硼氮烷(B₃N₃)环对石墨烯量子点非线性光学性质和紫外-可见吸收光谱的影响.研究发现,扶手椅边界上引入C=C双键后,六角形石墨烯量子点分子结构对称性降低,电荷分布对称性发生破缺,导致分子二阶非线性光学活性增强.石墨烯量子点在从扶手椅型边界向锯齿型边界过渡的过程中,随着边界C=C双键数目的增加,六角形石墨烯量子点和B3N3掺杂六角形石墨烯量子点的极化率和第二超极化率分别呈线性增加.此外,边界对石墨烯量子点的吸收光谱也有重要影响.无论是石墨烯量子点还是B₃N₃掺杂石墨烯量子点,扶手椅型边界上引入C=C双键导致最高占据分子轨道能级升高,最低未占分子轨道能级的降低,前线分子轨道能级差减小,因而最大吸收波长发生了红移.中心掺杂B₃N₃环后会增大石墨烯量子点的分子前线轨道能级差,导致B3N3掺杂后的石墨烯量子点紫外-可见吸收光谱发生蓝移.本文研究为边界修饰调控石墨烯量子点非线性光学响应提供了一定的理论指导.     

Direct observation of optically forbidden energy transfer between CuCl quantum cubes via near-field optical spectroscopy

We report, for the first time, evidence of near-field energy transfer among CuCl quantum cubes using an ultrahigh-resolution near-field optical microscopy and spectroscopy in the near UV region at 15 K. The sample was high-density CuCl quantum cubes embedded in a NaCl matrix. Measured spatial distributions of the luminescence intensities from 4.6-nm and 6.3-nm quantum cubes clearly established anticorrelation features. This is thought to be a manifestation of the energy transfer from the lowest state of exciton in 4.6-nm quantum cubes to the first dipole-forbidden excited state of exciton in 6.3-nm quantum cubes, which is attributed to the resonant optical near-field interaction.