Spontaneous Emission Of Quantum Dots Research Articles

Controlling of spontaneous emission of quantum dots based on hyperbolic metamaterials

The study of spontaneous emission has basic and supporting significance for enhancing the interaction between light and matter, solid-state lighting and biosensors. Hyperbolic metamaterials (HMMs) can support high k modes due to their hyperbolic dispersion characteristics, resulting in extremely high photon density, which affects spontaneous emission. Therefore, here we study the effect of HMMs on the spontaneous emission of quantum dots (QDs), and the Purcell factor reaches 20 times. At the same time, the structure of HMMs with gold nanoantennas is studied. The addition of gold nanoantennas further increases the Purcell factor to 120 times. In addition, the effects of the metal filling rate, the position and polarization direction of QDs on spontaneous emission enhancement and radiation power peak position are also studied. This provides a new perspective for enhancing and controlling spontaneous emission of QDs based on HMMs.

Controlling exciton spontaneous emission of quantum dots by Au nanoparticles

As an ideal single-photon source, quantum dots (QDs) can play a unique role in the field of quantum information. Controlling QD exciton spontaneous emission can be achieved by anti-phase coupling between QD exciton dipole field and Au dipole field after QD film has been transferred onto the Si substrate covered by Au nanoparticles. In experiment, the studied InAs/GaAs QDs are grown by molecular beam epitaxy (MBE) on a (001) semi-insulation substrate. The films containing QDs with different GaAs thickness values are separated from the GaAs substrate by etching away the AlAs sacrificial layer and transferring the QD film to the silicon wafer covered by Au nanoparticles with a diameter of 50 nm. The distance <i>D</i> (thickness of GaAs) from the surface of the Au nanoparticles to the QD layer is 10, 15, 19, 25, and 35 nm, separately. A 640-nm pulsed semiconductor laser with a 40-ps pulse length is used to excite the QD samples for measuring QD exciton photoluminescence and time-resolved photoluminescence spectra at 5 K. It is found that when the distance <i>D</i> is 15–35 nm the spontaneous emission rate of exciton is suppressed. And when <i>D</i> is close to 19 nm, the QD spontaneous emission rate decreases to <inline-formula><tex-math id="M2">\begin{document}$ ~{10}^{-3} $\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20211863_M2.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20211863_M2.png"/></alternatives></inline-formula>, which is consistent with the theoretical calculations. The physical mechanism of long-lived exciton luminescence observed in experiment lies in the fact that Au nanoparticles scatter the light field of the exciton radiation in the QD wetting layer, and the phase of the scattered field is opposite to the phase of the exciton radiation field. Therefore, the destructive interference between the exciton radiation field and scattering field of Au nanoparticles results in long-lived exciton emission observed in experiment.

Laser-controlled projection of quantum dot dipoles using metal-oxide plasmonic metastructures: maintaining spin polarization memory

A plasmonic meta-structure is used to control the polarization and intensity of spontaneous emission of quantum dots via polarization of an off-resonant laser. Spin polarization memory transfer occurs in quantum dots with symmetrical structures.

Controlling Exciton Spontaneous Emission of Quantum Dots by Au nanoparticles

摘要 将InAs/GaAs量子点样品薄膜置于覆盖有直径为50 nm的金（Au）纳米颗粒的硅衬底上，可以调控量子点激子的自发辐射速率．实验发现，当量子点浸润层距离Au纳米颗粒表面15-35 nm时，激子自发辐射速率受到抑制，且距离为19 nm时抑制作用最大，导致量子点激子的自发辐射速率减小到没有Au纳米颗粒时自发辐射速率的~10^(-3)．基于经典的偶极辐射模型模拟计算的激子自发辐射速率与实验结果一致． 关键词: 量子点 / 自发辐射速率 / 金属纳米颗粒 / 长寿命激子 文章全文 施引文献

Controlling amplified spontaneous emission of quantum dots by polymerized nanostructure interfaces.

We report a new polymer/colloidal-quantum-dot (CQD) film with a nanostructured interface, which is fabricated through a template-assisted photopolymerization method, toward the use of amplified spontaneous emission. It is experimentally demonstrated that the amplified spontaneous emission of CQDs is able to be manipulated by changing the nanostructured polymeric interface with a weak scattering ability. The dependences of emission wavelength and threshold on the size of the nanostructure and CQD layer thickness are investigated.

Enhancement of spontaneous emission of semiconductor quantum dots inside one-dimensional porous silicon photonic crystals.

Controlling spontaneous emission by modifying the local electromagnetic environment is of great interest for applications in optoelectronics, biosensing and energy harvesting. Although the development of devices based on one-dimensional porous silicon photonic crystals with embedded luminophores is a promising approach for applications, the efficiency of the embedded luminophores remains a key challenge because of the strong quenching of the emission due to the contact of the luminophores with the surface of porous silicon preventing the observation of interesting light-matter coupling effects. Here, we experimentally demonstrate an increase in the quantum dot (QD) spontaneous emission rate inside a porous silicon microcavity and almost an order of magnitude enhancement of QD photoluminescence intensity in the weak light-matter coupling regime. Furthermore, we have demonstrated drastic alteration of the QD spontaneous emission at the edge of the photonic band gap in porous silicon distributed Bragg reflectors and proved its dependence on the change in the density of photonic states.

Enhanced quantum dots spontaneous emission with metamaterial perfect absorbers

Metamaterial perfect absorbers (PAs) made of a hexagonal array of holes on Ag-SiO2-Ag thin films have been realized and utilized to enhance the spontaneous emission rate and photoluminescence intensity of CdSe/ZnS quantum dots (QDs) spin-coated on the absorber top surface. Perfect absorption of incoming light occurs at the wavelength where the impedance is matched to that of the free space. When QDs strongly excite both the electric and magnetic resonances at this perfect absorption wavelength, a significant Purcell effect on the spontaneous emission process and enhanced radiative outcoupling of photoluminescence intensity are expected. For perfect absorbers with near-unity absorption at the QD emission wavelength of 620 nm, 5-fold Purcell enhancement of the spontaneous emission rate and 3.6-fold enhancement of photoluminescence intensity are demonstrated in the time-resolved photoluminescence experiments, which are in good agreement with three-dimensional finite-difference time-domain simulation. These results will advance the understanding and applications of metamaterial PA-based light harvesting and emitting devices.

Reduction of the fluorescence lifetime of quantum dots in presence of plasmonic nanostructures

Developing a single photon source in the near infrared spectrum for optical fibre communications implies the control of the spontaneous emission of quantum dots. In this paper we show that the fluorescence lifetime of lead sulphide quantum dots can be drastically decreased due to the presence of plasmonic nanostructures specially designed to confine the electromagnetic field to which the emitted photons could decay at λ = 1550nm. To demonstrate this, we first measured the fluorescence lifetime of colloidal quantum dots in toluene solution and took this as a reference measurement. Then, we compared this value with the fluorescence lifetime of quantum dots in two different plasmonic nanostructures. The measurement of lifetime was made using the Time-Correlated Single Photon Counting technique. We obtained for the quantum dots in solution a fluorescence lifetime of 0.98084μs and for the quantum dots in the nanostructures, fluorescence lifetimes of 0.06227μs and 0.11789μs. We also numerically calculated the distribution of the electromagnetic field near the plasmonic nanostructures. These results demonstrate that the plasmonic nanostructures modified the fluorescence lifetime of the quantum dots, and that these plasmonic nanostructures with the lead sulphide quantum dots could work as a single photon source that could be integrated in a photonic circuit for infrared optical fibre communications.

Array of nanoparticles coupling with quantum-dot: Lattice plasmon quantum features

In this study, we analyze the interaction of lattice plasmon with quantum-dot in order to mainly examine the quantum features of the lattice plasmon containing the photonic/plasmonic properties. Despite optical properties of the localized plasmon, the lattice plasmon severely depends on the array geometry, which may influence its quantum features such as uncertainty and the second-order correlation function. To investigate this interaction, we consider a closed system containing an array of the plasmonic nanoparticles and quantum-dot. We analyze this system with full quantum theory by which the array electric far field is quantized and the strength coupling of the quantum-dot array is analytically calculated. Moreover, the system's dynamics are evaluated and studied via the Heisenberg-Langevin equations to attain the system optical modes. We also analytically examine the Purcell factor, which shows the effect of the lattice plasmon on the quantum-dot spontaneous emission. Finally, the lattice plasmon uncertainty and its time evolution of the second-order correlation function at different spatial points are examined. These parameters are dramatically affected by the retarded field effect of the array nanoparticles. We found a severe quantum fluctuation at points where the lattice plasmon occurs, suggesting that the lattice plasmon photons are correlated.

金纳米颗粒对量子点荧光自发辐射的影响

金纳米颗粒对量子点荧光自发辐射的影响

Physics and devices of quanutm light emission from semicoductor self-assembled quantum Dots

Self-assembled semiconductor single quantum dots (QDs), as a good candidate of solid-state real single photon (SP) emitters in high purity and counting rate, have attracted great attention in recent two decades, promising for quantum information, optical quantum computation, quantum storage, and quantum coherent manipulation. To isolate single QD from the other QDs surrounding, 1) dilute QD density is well controlled during epitaxy; 2) micro-pillars or nanowires individually in space as hosts are fabricated. To enhance their uni-directional emission, GaAs/AlAs distributed Bragg reflector (DBR) planar cavity is integrated. To improve the system (i.e. confocal microscope, traditionally) stability and its optical collection efficiency, a near-field fiber coupling by adhering a micro-pillar chip to fiber facets directly is used. To enhance the coherence of QD spontaneous emission, resonant excitation technique is applied. In this article, we review our research progress in self-assembled QD SP emission, including SP emission from InAs or GaAs QDs on Ga droplet-self-catalyzed GaAs nanowires (with g2(0) of 0.031 or 0.18, respectively), SP emission from InAs/GaAs QDs coupled with high-Q (1000-5000) DBR micro-pillar cavities and their fiber-coupled device fabrication with SP fiber output rate ~1.8 MHz, single QD resonant fluorescence with inter-dot coherent visibility of 40%, strain-coupled bilayer InAs QDs to extend their emission wavelength to 1320 nm and parametric down conversion of 775 nm SP emission from single QD in nanowire to realize entangled photon pairs at 1550 nm (entanglement fidelity of 91.8%) for telecomm application, and definite quantum storage of InAs QD SPs at 879 nm in ion-doped solid (at most 100 time-bins). In future, there will be still several urgent things to do, including 1) puring the environment of a single QD (e.g. growing GaAs QDs to avoid the wetting layer, and optimizing QD growth to avoid smaller QDs) to reduce its spectral diffusion and developing a high-symmetric QD (e.g. GaAs QD) to reduce the fine structure splitting of its emission; 2) positioning single QD precisely for a good alignment of single QD to a micro-cavity or fiber cone (single mode with high numerical aperture) to increase optical excitation efficiency and SP collection efficiency; 3) developing optical quantum integrated chip, including hybrid structures of active micro-cavity and passive waveguide, and high-transmission waveguide beamsplitter or Mach-Zender interferometer to improve SP extraction (micro-cavity), collection (optical setup) and counting rate (at avalanched photon detectors and coincidence counting module).

Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure

Emission control of colloidal quantum dots (QDs) is a cornerstone of modern high-quality lighting and display technologies. Dynamic emission control of colloidal QDs in an optoelectronic device is usually achieved by changing the optical pump intensity or injection current density. Here we propose and demonstrate a distinctly different mechanism for the temporal modulation of QD emission intensity at constant optical pumping rate. Our mechanism is based on the electrically controlled modulation of the local density of optical states (LDOS) at the position of the QDs, resulting in the modulation of the QD spontaneous emission rate, far-field emission intensity, and quantum yield. We manipulate the LDOS via field effect-induced optical permittivity modulation of an ultrathin titanium nitride (TiN) film, which is incorporated in a gated TiN/SiO2/Ag plasmonic heterostructure. The demonstrated electrical control of the colloidal QD emission provides a new approach for modulating intensity of light in displays and other optoelectronics.

Enhanced Quantum Dot Spontaneous Emission with Multilayer Metamaterial Nanostructures

The Purcell effect of quantum dot (QD) spontaneous emission with Ag-SiO2 multilayer metamaterial nanostructures has been demonstrated in experiment and simulation. A broadband enhanced spontaneous emission rate of QDs is observed due to large local density of states in the epsilon-near-zero and hyperbolic regions of multilayer structures. Multilayer gratings are utilized to further enhance the QD spontaneous emission as the QDs located inside the grating grooves strongly interact with high-k coupled surface plasmon polariton modes. Photoluminescence decay measurements are in good agreement with both analytical treatment with a nonlocal effect and three-dimensional finite-element simulation. Detailed studies of QD position and polarization effects on emission rate enhancement for multilayer and multilayer grating nanostructures provide important insight for understanding the coupling mechanisms of emitter–multilayer interaction and the engineering of local density of states in metamaterial nanostructures. ...

Control of spontaneous emission of quantum dots using correlated effects of metal oxides and dielectric materials

We study the emission dynamics of semiconductor quantum dots in the presence of the correlated impact of metal oxides and dielectric materials. For this we used layered material structures consisting of a base substrate, a dielectric layer, and an ultrathin layer of a metal oxide. After depositing colloidal CdSe/ZnS quantum dots on the top of the metal oxide, we used spectral and time-resolved techniques to show that, depending on the type and thickness of the dielectric material, the metal oxide can characteristically change the interplay between intrinsic excitons, defect states, and the environment, offering new material properties. Our results show that aluminum oxide, in particular, can strongly change the impact of amorphous silicon on the emission dynamics of quantum dots by balancing the intrinsic near band emission and fast trapping of carriers. In such a system the silicon/aluminum oxide charge barrier can lead to large variation of the radiative lifetime of quantum dots and control of the photo-ejection rate of electrons in quantum dots. The results provide unique techniques to investigate and modify physical properties of dielectrics and manage optical and electrical properties of quantum dots.

Quantum analysis of plasmonic coupling between quantum dots and nanoparticles

In this study, interaction between core-shells nanoparticles and quantum dots is discussed via the full-quantum-theory method. The electromagnetic field of the nanoparticles is derived by the quasistatic approximation method and the results for different regions of the nanoparticles are quantized from the time-harmonic to the wave equation. Utilizing the optical field quantization, the nanoparticles' and quantum dots' deriving amplitudes contributing to the excitation waves are determined. In the current model, two counterpropagating waves with two different frequencies are applied. We derived the Maxwell-Bloch equations from the Heisenberg-Langevin equations; thus the nanoparticles--quantum dots interaction is perused. Moreover, by full quantum analyzing of the analytical expression, the quantum-plasmonic coupling relation and the Purcell factor are achieved. We show that the spontaneous emission of quantum dots can be dramatically manipulated by engineering the plasmon-plasmon interaction in the core-shells nanoparticles. This issue is a very attractive point for designing a wide variety of quantum-plasmonic sensors. Through the investigation of the nanoparticle plasmonic interaction effects on absorbed power, the results show that the nanoparticles' and quantum dots' absorption saturation state can be switched to each other just by manipulation of their deriving amplitudes. In fact, we manage the interference between the two waves' deriving amplitudes just by the plasmonic interactions effect.

Picosecond time of spontaneous emission in plasmonic patch nanoantennas

A significant (to 12 ps) decrease in the lifetime of excited states of quantum emitters in the form of three-layer colloidal quantum dots (CdSe/CdS/ZnS) placed in an aluminum–triangular silver nanoprism cavity (patch nanoantenna) has been experimentally demonstrated. The decrease in the time of spontaneous emission of quantum dots has been explained by the Purcell effect. The Purcell coefficient for an emitter in the resonator has been found to be 625. Such a significant increase in the rate of spontaneous emission in the patch nanoantenna is due to an increase in the local density of photon states in the plasmonic cavity.

Plasmonic Control of Spontaneous Emission of Quantum Dots in Sub-Wavelength Photonic Templates

Finite difference time domain (FDTD) simulations were performed on two different plasmonic sub-wavelength photonic templates embedded with CdSe quantum dots. Tunable loading of these templates with plasmonic nano antenna allowed control of the emission from the embedded quantum dots. We discuss how large loading of nano antenna can effectively control the optical density of states for the quantum dots leading to enhancement of their radiative decay rates as observed in experiments. On the other hand, at low level of loading, while FDTD fails to capture the observed enhancement of decay rates in experiment, an alternative mechanism is suggested to exist in such cases. Thus, subtle interplay of multiple mechanisms engineered by appropriate placement and loading of plasmonic nano antenna in such templates is demonstrated as an effective method to control optical density of states and hence spontaneous emission of embedded quantum dots.

Au Microdisk-Size Dependence of Quantum Dot Emission from the Hybrid Metal-Distributed Bragg Reflector Structures Employed for Single Photon Sources**Supported by the National Key Basic Research Program of China under Grant No 2013CB922304, and the National Natural Science Foundation of China under Grant Nos 11474275 and 11464034.

We investigate metallic microdisk-size dependence of quantum dot (QD) spontaneous emission rate and micro-antenna directional emission effect for the hybrid metal-distributed Bragg reflector structures based on a particular single QD emission. It is found that the measured photoluminescence (PL) intensity is very sensitive to the size of metallic disk, showing an enhancement factor of 11 when the optimal disk diameter is 2 μm and the numerical aperture of microscope objective NA=0.5. It is found that for large metal disks, the Purcell effect is dominant for enhanced PL intensity, whereas for small size disks the main contribution comes from plasmon scattering at the disk edge within the light cone collected by the microscope objective.

Self-aligned deterministic coupling of single quantum emitter to nanofocused plasmonic modes

The quantum plasmonics field has emerged and been growing increasingly, including study of single emitter-light coupling using plasmonic system and scalable quantum plasmonic circuit. This offers opportunity for the quantum control of light with compact device footprint. However, coupling of a single emitter to highly localized plasmonic mode with nanoscale precision remains an important challenge. Today, the spatial overlap between metallic structure and single emitter mostly relies either on chance or on advanced nanopositioning control. Here, we demonstrate deterministic coupling between three-dimensionally nanofocused plasmonic modes and single quantum dots (QDs) without any positioning for single QDs. By depositing a thin silver layer on a site-controlled pyramid QD wafer, three-dimensional plasmonic nanofocusing on each QD at the pyramid apex is geometrically achieved through the silver-coated pyramid facets. Enhancement of the QD spontaneous emission rate as high as 22 ± 16 is measured for all processed QDs emitting over ∼150-meV spectral range. This approach could apply to high fabrication yield on-chip devices for wide application fields, e.g., high-efficiency light-emitting devices and quantum information processing.

Quantum dot spontaneous emission control in a ridge waveguide

We investigate the spontaneous emission (SE) of self-assembled InAs quantum dots (QDs) embedded in GaAs ridge waveguides that lay on a low index substrate. In thin enough waveguides, the coupling to the fundamental guided mode is vanishingly small. A pronounced anisotropy in the coupling to non-guided modes is then directly evidenced by normal-incidence photoluminescence polarization measurements. In this regime, a measurement of the QD decay rate reveals a SE inhibition by a factor up to 4. In larger wires, which ensure an optimal transverse confinement of the fundamental guided mode, the decay rate approaches the bulk value. Building on the good agreement with theoretical predictions, we infer from calculations the fraction β of SE coupled to the fundamental guided mode for some important QD excitonic complexes. For a charged exciton (isotropic in plane optical dipole), β reaches 0.61 at maximum for an on-axis QD. In the case of a purely transverse linear optical dipole, β increases up to 0.91. This optimal configuration is achievable through the selective excitation of one of the bright neutral excitons.