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1.
Nano Lett ; 24(5): 1746-1752, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38286024

RESUMO

Bright, polarized, and high-purity single-photon sources in telecom wavelengths are crucial components in long-distance quantum communication, optical quantum computation, and quantum networks. Semiconductor InAs/InP quantum dots (QDs) combined with photonic cavities provide a competitive path, leading to optimal single-photon sources in this range. Here, we demonstrate a bright and polarized single-photon source operating in the telecom C-band based on an elliptical Bragg grating (EBG) cavity. With a significant Purcell enhancement of 5.25 ± 0.05, the device achieves a polarization ratio of 0.986, a single-photon purity of g2(0) = 0.078 ± 0.016, and a single-polarized photon collection efficiency of ∼24% at the first lens (NA = 0.65) without blinking. These findings suggest that C-band QD-based single-photon sources are potential candidates for advancing quantum communication.

2.
Nano Lett ; 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38620181

RESUMO

Advancements in photonic quantum information systems (QIS) have driven the development of high-brightness, on-demand, and indistinguishable semiconductor epitaxial quantum dots (QDs) as single photon sources. Strain-free, monodisperse, and spatially sparse local-droplet-etched (LDE) QDs have recently been demonstrated as a superior alternative to traditional Stranski-Krastanov QDs. However, integration of LDE QDs into nanophotonic architectures with the ability to scale to many interacting QDs is yet to be demonstrated. We present a potential solution by embedding isolated LDE GaAs QDs within an Al0.4Ga0.6As Huygens' metasurface with spectrally overlapping fundamental electric and magnetic dipolar resonances. We demonstrate for the first time a position- and size-independent, 1 order of magnitude increase in the collection efficiency and emission lifetime control for single-photon emission from LDE QDs embedded within the Huygens' metasurfaces. Our results represent a significant step toward leveraging the advantages of LDE QDs within nanophotonic architectures to meet the scalability demands of photonic QIS.

3.
Nano Lett ; 23(22): 10228-10235, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37930320

RESUMO

Achieving pure single-photon emission is essential for a range of quantum technologies, from quantum computing to quantum key distribution to quantum metrology. Among solid-state quantum emitters, colloidal lead halide perovskite (LHP) nanocrystals (NCs) have attracted considerable interest due to their structural and optical properties, which make them attractive candidates for single-photon sources (SPSs). However, their practical utilization has been hampered by environment-induced instabilities. In this study, we fabricate and characterize in a systematic manner Zn-treated CsPbBr3 colloidal NCs obtained through Zn2+ ion doping at the Pb-site, demonstrating improved stability under dilution and illumination. The doped NCs exhibit high single-photon purity, reduced blinking on a submillisecond time scale, and stability of the bright state even at excitation powers well above saturation. Our findings highlight the potential of this synthesis approach to optimize the performance of LHP-based SPSs, opening up interesting prospects for their integration into nanophotonic systems for quantum technology applications.

4.
Nano Lett ; 22(15): 6402-6408, 2022 08 10.
Artigo em Inglês | MEDLINE | ID: mdl-35875900

RESUMO

Optical antennas are nanostructures designed to manipulate light-matter interactions by interfacing propagating light with localized optical fields. In recent years, numerous devices have been realized to efficiently tailor the absorption and/or emission rates of fluorophores. By contrast, modifying the spatial characteristics of their radiation fields remains challenging. Successful phased array nanoantenna designs have required the organization of several elements over a footprint comparable to the operating wavelength. Here, we report unidirectional emission of a single fluorophore using an ultracompact optical antenna. The design consists of two side-by-side gold nanorods self-assembled via DNA origami, which also controls the positioning of the single-fluorophore. Our results show that when a single fluorescent molecule is positioned at the tip of one nanorod and emits at a frequency capable of driving the antenna in the antiphase mode, unidirectional emission with a forward to backward ratio of up to 9.9 dB can be achieved.


Assuntos
Nanoestruturas , Nanotecnologia , DNA/química , Corantes Fluorescentes , Ouro/química , Nanoestruturas/química
5.
Nanotechnology ; 33(21)2022 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-35105827

RESUMO

Atomic force microscopy (AFM) nanoxerography was successfully used to direct the assembly of colloidal nanodiamonds (NDs) containing nitrogen-vacancy (NV) centres on electrostatically patterned surfaces. This study reveals that the number of deposited NDs can be controlled by tuning the surface potentials of positively charged dots on a negatively charged background written by AFM in a thin PMMA electret film, yielding assemblies down to a unique single-photon emitter with very good selectivity. The mechanisms of the ND directed assembly are attested by numerical simulations. This robust deterministic nano-positioning of quantum emitters thus offers great opportunities for ultimate applications in nanophotonics for quantum technologies.

6.
Sensors (Basel) ; 22(3)2022 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-35161882

RESUMO

Fluorescent biomarkers are used to detect target molecules within inhomogeneous populations of cells. When these biomarkers are found in trace amounts it becomes extremely challenging to detect their presence in a flow cytometer. Here, we present a framework to draw a detection baseline for single emitters and enable absolute calibration of a flow cytometer based on quantum measurements. We used single-photon detection and found the second-order autocorrelation function of fluorescent light. We computed the success of rare-event detection for different signal-to-noise ratios (SNR). We showed high-accuracy identification of the events with occurrence rates below 10-5 even at modest SNR levels, enabling early disease diagnostics and post-disease monitoring.


Assuntos
Fótons , Calibragem , Citometria de Fluxo , Razão Sinal-Ruído
7.
Nano Lett ; 21(1): 323-329, 2021 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-33338376

RESUMO

Telecom-wavelength single photons are essential components for long-distance quantum networks. However, bright and pure single photon sources at telecom wavelengths remain challenging to achieve. Here, we demonstrate a bright telecom-wavelength single photon source based on a tapered nanobeam containing InAs/InP quantum dots. The tapered nanobeam enables directional and Gaussian-like far-field emission of the quantum dots. As a result, using above-band excitation we obtain an end-to-end brightness of 4.1 ± 0.1% and first-lens brightness of 27.0 ± 0.1% at the ∼1300 nm wavelength. Furthermore, we adopt quasi-resonant excitation to reduce both multiphoton emission and decoherence from unwanted charge carriers. As a result, we achieve a coherence time of 523 ± 16 ps and postselected Hong-Ou-Mandel visibility of 0.91 ± 0.09 along with a comparable first-lens brightness of 21.0 ± 0.1%. These results represent a major step toward a practical fiber-based single photon source at telecom wavelengths for long-distance quantum networks.

8.
Nano Lett ; 18(8): 4710-4715, 2018 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-29932664

RESUMO

Single-photon emitters play an essential role in quantum technologies, including quantum computing and quantum communications. Atomic defects in hexagonal boron nitride ( h-BN) have recently emerged as new room-temperature single-photon emitters in solid-state systems, but the development of scalable and tunable h-BN single-photon emitters requires external methods that can control the emission energy of individual defects. Here, by fabricating van der Waals heterostructures of h-BN and graphene, we demonstrate the electrical control of single-photon emission from atomic defects in h-BN via the Stark effect. By applying an out-of-plane electric field through graphene gates, we observed Stark shifts as large as 5.4 nm per GV/m. The Stark shift generated upon a vertical electric field suggests the existence of out-of-plane dipole moments associated with atomic defect emitters, which is supported by first-principles theoretical calculations. Furthermore, we found field-induced discrete modification and stabilization of emission intensity, which were reversibly controllable with an external electric field.

9.
Nano Lett ; 16(9): 5785-91, 2016 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-27574953

RESUMO

Elastic strain fields based on single crystal piezoelectric elements represent an effective way for engineering the quantum dot (QD) emission with unrivaled precision and technological relevance. However, pioneering researches in this direction were mainly based on bulk piezoelectric substrates, which prevent the development of chip-scale devices. Here, we present a monolithically integrated Microelectromechanical systems (MEMS) device with great potential for on-chip quantum photonic applications. High-quality epitaxial PMN-PT thin films have been grown on SrTiO3 buffered Si and show excellent piezoelectric responses. Dense arrays of MEMS with small footprints are then fabricated based on these films, forming an on-chip strain tuning platform. After transferring the QD-containing nanomembranes onto these MEMS, the nonclassical emissions (e.g., single photons) from single QDs can be engineered by the strain fields. We envision that the strain tunable QD sources on the individually addressable and monolithically integrated MEMS pave the way toward complex quantum photonic applications on chip.

10.
Nano Lett ; 16(11): 7061-7066, 2016 11 09.
Artigo em Inglês | MEDLINE | ID: mdl-27749076

RESUMO

Interactions between solid-state quantum emitters and cavities are important for a broad range of applications in quantum communication, linear optical quantum computing, nonlinear photonics, and photonic quantum simulation. These applications often require combining many devices on a single chip with identical emission wavelengths in order to generate two-photon interference, the primary mechanism for achieving effective photon-photon interactions. Such integration remains extremely challenging due to inhomogeneous broadening and fabrication errors that randomize the resonant frequencies of both the emitters and cavities. In this Letter, we demonstrate two-photon interference from independent cavity-coupled emitters on the same chip, providing a potential solution to this long-standing problem. We overcome spectral mismatch between different cavities due to fabrication errors by depositing and locally evaporating a thin layer of condensed nitrogen. We integrate optical heaters to tune individual dots within each cavity to the same resonance with better than 3 µeV of precision. Combining these tuning methods, we demonstrate two-photon interference between two devices spaced by less than 15 µm on the same chip with a postselected visibility of 33%, which is limited by timing resolution of the detectors and background. These results pave the way to integrate multiple quantum light sources on the same chip to develop quantum photonic devices.

11.
ACS Nano ; 2024 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-39058675

RESUMO

Single-photon sources are essential for advancing quantum technologies with scalable integration being a crucial requirement. To date, deterministic positioning of single-photon sources in large-scale photonic structures remains a challenge. In this context, colloidal quantum dots (QDs), particularly core/shell configurations, are attractive due to their solution processability. However, traditional QDs are typically small, about 3 to 6 nm, which restricts their deterministic placement and utility in large-scale photonic devices, particularly within optical cavities. The largest existing core/shell QDs are a family of giant CdSe/CdS QDs, with total diameters ranging from about 20 to 50 nm. Pushing beyond this size limit, we introduce a synthesis strategy for colossal CdSe/CdS QDs, with sizes ranging from 30 to 100 nm, using a stepwise high-temperature continuous injection method. Electron microscopy reveals a consistent hexagonal diamond morphology composed of 12 semipolar {101̅1} facets and one polar (0001) facet. We also identify conditions where shell growth is disrupted, leading to defects, islands, and mechanical instability, which suggest synthetic requirements for growing crystalline particles beyond 100 nm. The stepwise growth of thick CdS shells on CdSe cores enables the synthesis of emissive QDs with long photoluminescence lifetimes of a few microseconds and suppressed blinking at room temperature. Notably, QDs with 80 and 100 CdS monolayers exhibit high single-photon emission purity with second-order photon correlation g(2)(0) values below 0.2.

12.
ACS Nano ; 18(16): 10807-10817, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38598660

RESUMO

Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr3 QDs. However, this also increases the fluorescence intermittency. Achieving high SP purity and blinking mitigation simultaneously remains a significant challenge. Here, we transcend this limitation with room-temperature synthesized weakly confined hybrid organic-inorganic perovskite (HOIP) QDs. Superior single photon purity with a low g(2)(0) < 0.07 ± 0.03 and a nearly blinking-free behavior (ON-state fraction >95%) in 11 nm FAPbBr3 QDs are achieved at room temperature, attributed to their long exciton lifetimes (τX) and short biexciton lifetimes (τXX). The significance of the organic A-cation is further validated using the mixed-cation FAxCs1-xPbBr3. Theoretical calculations utilizing a combination of the Bethe-Salpeter (BSE) and k·p approaches point toward the modulation of the dielectric constants by the organic cations. Importantly, our findings provide valuable insights into an additional lever for engineering facile-synthesized room-temperature PQD single photon sources.

13.
Chemphyschem ; 14(11): 2393-402, 2013 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-23784791

RESUMO

The efficient feeding of spontaneous emission (SE) into a controlled optical mode lies at the heart of a new generation of advanced optoelectronic devices, such as low-threshold microlasers and bright sources of quantum light. In the solid state, single-mode emission was first demonstrated by using the Purcell effect that arises in a resonant microcavity. Recently, the need to relax the constraints inherent to such a narrow-band approach has motivated large effort to develop structures ensuring broadband and efficient SE control. This minireview deals with fiber-like photonic nanowires, a class of high-index waveguides that features key assets in this context. Combining theoretical predictions and experimental results, the paper details the SE dynamics in such tiny wires. In addition, it shows how the far-field emission of a single wire can be tailored through proper engineering of the two wire ends. As an application in the field of quantum optics, we review the realization of an ultrabright single-photon source. This first device was based on a self-assembled quantum dot embedded in a wire antenna realized with a top-down fabrication process. Considering recent advances in the direct growth of tapered photonic wires, we also propose a bottom-up fabrication route to realize a complete device. In particular, this proposal ensures the optimal 3D positioning of a single emitter inside the antenna. Finally, future research and application prospects are also reviewed.

14.
Materials (Basel) ; 16(24)2023 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-38138825

RESUMO

Single-photon sources (SPSs) play a crucial role in quantum photonics, and colloidal quantum dots (CQDs) have emerged as promising and cost-effective candidates for such applications due to their high-purity single-photon emission at room temperature. This review focuses on various aspects of CQDs as SPSs. Firstly, a brief overview of the fundamental optical properties of CQDs is provided, including emission wavelength engineering and fluorescence intermittency, and their single-photon emission properties. Subsequently, this review delves into research concerning CQDs as SPSs, covering topics such as the coupling of single CQDs to microcavities, both in weak and strong coupling regimes. Additionally, methods for localizing and positioning CQDs are explored, which are critical for on-chip SPSs devices.

15.
ACS Appl Mater Interfaces ; 15(3): 4294-4302, 2023 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-36507852

RESUMO

Colloidal quantum dots (QDs) are promising candidates for single-photon sources with applications in photonic quantum information technologies. Developing practical photonic quantum devices with colloidal materials, however, requires scalable deterministic placement of stable single QD emitters. In this work, we describe a method to exploit QD size to facilitate deterministic positioning of single QDs into large arrays while maintaining their photostability and single-photon emission properties. CdSe/CdS core/shell QDs were encapsulated in silica to both increase their physical size without perturbing their quantum-confined emission and enhance their photostability. These giant QDs were then precisely positioned into ordered arrays using template-assisted self-assembly with a 75% yield for single QDs. We show that the QDs before and after assembly exhibit antibunching behavior at room temperature and their optical properties are retained after an extended period of time. Together, this bottom-up synthetic approach via silica shelling and the robust template-assisted self-assembly offer a unique strategy to produce scalable quantum photonics platforms using colloidal QDs as single-photon emitters.

16.
Adv Sci (Weinh) ; 10(18): e2300190, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37088736

RESUMO

Focused ion beam implantation is ideally suited for placing defect centers in wide bandgap semiconductors with nanometer spatial resolution. However, the fact that only a few percent of implanted defects can be activated to become efficient single photon emitters prevents this powerful capability to reach its full potential in photonic/electronic integration of quantum defects. Here an industry adaptive scalable technique is demonstrated to deterministically create single defects in commercial grade silicon carbide by performing repeated low ion number implantation and in situ photoluminescence evaluation after each round of implantation. An array of 9 single defects in 13 targeted locations is successfully created-a ≈70% yield which is more than an order of magnitude higher than achieved in a typical single pass ion implantation. The remaining emitters exhibit non-classical photon emission statistics corresponding to the existence of at most two emitters. This approach can be further integrated with other advanced techniques such as in situ annealing and cryogenic operations to extend to other material platforms for various quantum information technologies.


Assuntos
Eletrônica , Fótons , Retroalimentação , Semicondutores
17.
Nanomaterials (Basel) ; 13(1)2023 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-36616105

RESUMO

A yet unresolved challenge in developing quantum technologies based on color centres in high refractive index semiconductors is the efficient fluorescence enhancement of point defects in bulk materials. Optical resonators and antennas have been designed to provide directional emission, spontaneous emission rate enhancement and collection efficiency enhancement at the same time. While collection efficiency enhancement can be achieved by individual nanopillars or nanowires, fluorescent emission enhancement is achieved using nanoresonators or nanoantennas. In this work, we optimise the design of a metal-dielectric nanopillar-based antenna/resonator fabricated in a silicon carbide (SiC) substrate with integrated quantum emitters. Here we consider various color centres known in SiC such as silicon mono-vacancy and the carbon antisite vacancy pair, that show single photon emission and quantum sensing functionalities with optical electron spin read-out, respectively. We model the dipole emission fluorescence rate of these color centres into the metal-dielectric nanopillar hybrid antenna resonator using multi-polar electromagnetic scattering resonances and near-field plasmonic field enhancement and confinement. We calculate the fluorescence collected photon rate enhancement for these solid state vacancy-centers in SiC in these metal-dielectric nanopillar resonators, showing a trade-off effect between the collection efficiency and radiative Purcell factor enhancement. We obtained a collected photon rate enhancement from a silicon monovacancy vacancy center embedded in an optimised hybrid antenna-resonator two orders of magnitude larger compared to the case of the color centres in bulk material.

18.
ACS Appl Mater Interfaces ; 15(21): 25819-25830, 2023 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-37191386

RESUMO

This paper reports on a new strategy for obtaining homogeneous dispersion of grafted quantum dots (QDs) in a photopolymer matrix and their use for the integration of single-photon sources by two-photon polymerization (TPP) with nanoscale precision. The method is based on phase transfer of QDs from organic solvents to an acrylic matrix. The detailed protocol is described, and the corresponding mechanism is investigated and revealed. The phase transfer is done by ligand exchange through the introduction of mono-2-(methacryloyloxy) ethyl succinate (MES) that replaces oleic acid (OA). Infrared (IR) measurements show the replacement of OA on the QD surface by MES after ligand exchange. This allows QDs to move from the hexane phase to the pentaerythritol triacrylate (PETA) phase. The QDs that are homogeneously dispersed in the photopolymer without any clusterization do not show any significant broadening in their photoluminescence spectra even after more than 3 years. The ability of the hybrid photopolymer to create micro- and nanostructures by two-photon polymerization is demonstrated. The homogeneity of emission from 2D and 3D microstructures is confirmed by confocal photoluminescence microscopy. The fabrication and integration of a single-photon source in a spatially controlled manner by TPP is achieved and confirmed by auto-correlation measurements.

19.
Adv Mater ; 35(26): e2210667, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36946467

RESUMO

Among the diverse platforms of quantum light sources, epitaxially grown semiconductor quantum dots (QDs) are one of the most attractive workhorses for realizing quantum photonic technologies owing to their outstanding brightness and scalability. However, the spatial and spectral randomness of most QDs severely hinders the construction of large-scale photonic platforms. In this work, a methodology is presented to deterministically integrate single QDs with tailor-made photonic structures. A nondestructive luminescence picking method termed as nanoscale-focus pinspot (NFP) is applied using helium-ion microscopy to reduce the luminous QD density while retaining the surrounding medium. A single QD emission is only extracted out of the high-density ensemble QDs. Then the tailor-made photonic structure of a circular Bragg reflector (CBR) is designed and deterministically integrated with the selected QD. Given that the microscopy can image with nanoscale resolution and apply NFP in situ, photonic devices can be deterministically fabricated on target QDs. The extraction efficiency of the NFP-selected QD emission is improved by 25 times after the CBR integration. Since the NFP method only controls the luminescence without destroying the medium, it is applicable to various photonic structures such as photonic waveguides or photonic crystal cavities regardless of materials.

20.
ACS Nano ; 17(16): 16080-16088, 2023 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-37523736

RESUMO

Epitaxially grown self-assembled semiconductor quantum dots (QDs) with atom-like optical properties have emerged as the best choice for single-photon sources required for the development of quantum technology and quantum networks. Nondestructive selection of a single QD having desired structural, compositional, and optical characteristics is essential to obtain noise-free, fully indistinguishable single or entangled photons from single-photon emitters. Here, we show that the structural orientations and local compositional inhomogeneities within a single QD and the surrounding wet layer can be probed in a screening fashion by scanning X-ray diffraction microscopy and X-ray fluorescence with a few tens of nanometers-sized synchrotron radiation beam. The presented measurement protocol can be used to cull the best single QD from the enormous number of self-assembled dots grown simultaneously. The obtained results show that the elemental composition and resultant strain profiles of a QD are sensitive to in-plane crystallographic directions. We also observe that lattice expansion after a certain composition-limit introduces shear strain within a QD, enabling the possibility of controlled chiral-QD formation. Nanoscale chirality and compositional anisotropy, contradictory to common assumptions, need to be incorporated into existing theoretical models to predict the optical properties of single-photon sources and to further tune the epitaxial growth process of self-assembled quantum structures.

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