Light-emitting Quantum Research Articles

Plexcitonic Quantum Light Emission from Nanoparticle-on-Mirror Cavities.

We investigate the quantum-optical properties of the light emitted by a nanoparticle-on-mirror cavity filled with a single quantum emitter. Inspired by recent experiments, we model a dark-field setup and explore the photon statistics of the scattered light under grazing laser illumination. Exploiting analytical solutions to Maxwell’s equations, we quantize the nanophotonic cavity fields and describe the formation of plasmon–exciton polaritons (or plexcitons) in the system. This way, we reveal that the rich plasmonic spectrum of the nanocavity offers unexplored mechanisms for nonclassical light generation that are more efficient than the resonant interaction between the emitter natural transition and the brightest optical mode. Specifically, we find three different sample configurations in which strongly antibunched light is produced. Finally, we illustrate the power of our approach by showing that the introduction of a second emitter in the platform can enhance photon correlations further.

Reduction in the Photoluminescence Intensity Caused by Ultrathin GaN Quantum Barriers in InGaN/GaN Multiple Quantum Wells

The optical properties of InGaN/GaN violet light-emitting multiple quantum wells with different thicknesses of GaN quantum barriers are investigated experimentally. When the barrier thickness decreases from 20 to 10 nm, the photoluminescence intensity at room temperature increases, which can be attributed to the reduced polarization field in the thin-barrier sample. However, with a further reduction in the thickness to 5 nm, the sample’s luminescence intensity decreases significantly. It is found that the strong nonradiative loss process induced by the deteriorated crystal quality and the quantum-tunneling-assisted leakage of carriers may jointly contribute to the enhanced nonradiative loss of photogenerated electrons and holes, leading to a significant reduction in photoluminescence intensity of the sample with nanoscale ultrathin GaN quantum barriers.

Broadband, efficient extraction of quantum light by a photonic device comprised of a metallic nano-ring and a gold back reflector

To implement quantum light sources based on quantum emitters in applications, it is desirable to improve the extraction efficiency of single photons. In particular, controlling the directionality and solid angle of the emission are key parameters, for instance, to couple single photons into optical fibers and send the information encoded in quantum light over long distances, for quantum communication applications. In addition, fundamental studies of the radiative behavior of quantum emitters, including studies of coherence and blinking, benefit from such improved photon collection. Quantum dots grown via Stranski–Krastanov technique have shown to be good candidates for bright, coherent, indistinguishable quantum light emission. However, one of the challenges associated with these quantum light sources arises from the fact that the emission wavelengths can vary from one emitter to the other. To this end, broadband light extractors that do not rely on high-quality factor optical cavities would be desirable, so that no tuning between the quantum dot emission wavelength and the resonator used to increase the light extraction is needed. Here, we show that metallic nano-rings combined with gold back reflectors increase the collection efficiency of single photons, and we study the statistics of this effect when quantum dots are spatially randomly distributed within the nano-rings. We show an average increase in the brightness of about a factor 7.5, when comparing emitters within and outside the nano-rings, in devices with a gold back reflector, and we measure count rates exceeding 7 × 106 photons per second and single photon purities as high as 85% ± 1%. These results are important steps toward the realization of scalable, broadband, easy to fabricate sources of quantum light for quantum communication applications.

Quantum emission of light with densely packed driven dipoles

Collective excitations in regular structures of strongly interacting driven dipoles have been found to lead to strongly antibunched statistics of the emitted photons $[{g}^{(2)}(0)\ensuremath{\ll}0.5]$, but precise control of the number of emitters and their spatial distribution is in general a complex experimental task. We overcome this limitation by showing quantum light emission from densely packed driven dipoles does not require their arrangement in any specific structure, pointing strongly towards possible single-photon sources based on hot thermal vapors confined within nanocells, or on irregular quantum dot ensembles.

Vibronic effect and influence of aggregation on the photophysics of graphene quantum dots.

Graphene quantum dots, atomically precise nanopieces of graphene, are promising nano-objects with potential applications in various domains such as photovoltaics, quantum light emitters and bio-imaging. Despite their interesting prospects, precise reports on their photophysical properties remain scarce. Here, we report on a study of the photophysics of C96H24(C12H25) graphene quantum dots. A combination of optical studies down to the single molecule level with advanced molecular modelling demonstrates the importance of coupling to vibrations in the emission process. Optical fingerprints for H-like aggregates are identified. Our combined experimental-theoretical investigations provide a comprehensive description of the light absorption and emission properties of nanographenes, which not only represents an essential step towards precise control of sample production but also paves the way for new exciting physics focused on twisted graphenoids.

Cathodoluminescence in Ultrafast Electron Microscopy.

Implementing the modern technologies of light-emitting devices, light harvesting, and quantum information processing requires the understanding of the structure-function relations at spatial scales below the optical diffraction limit and time scales of energy and information flows. Here, we distinctively combine cathodoluminescence (CL) with ultrafast electron microscopy (UEM), termed CL-UEM, because CL and UEM synergetically afford the required spectral and spatiotemporal sensitivities, respectively. For color centers in nanodiamonds, we demonstrate the measurement of CL lifetime with a local sensitivity of 50 nm and a time resolution of 100 ps. It is revealed that the emitting states of the color centers can be populated through charge transfer among the color centers across diamond lattices upon high-energy electron beam excitation. The technical advance achieved in this study will facilitate the specific control over energy conversion at nanoscales, relevant to quantum dots and single-photon sources.

Understanding the Luminescence Characteristics of Ultraviolet InGaN/AlGaN Multiple Quantum Wells with Different In Gradients

The electroluminescence (EL) properties of InGaN/AlGaN ultraviolet light-emitting multiple quantum wells (MQWs) with identical average In content but different In gradients (In content increases linearly, along the growth direction) are investigated numerically. It is found that the luminescence efficiency is improved, and the EL spectral peak wavelength becomes longer for the MQW sample with a larger In gradient. Since the influence of In gradient is different for the conduction and valence bands in InGaN layers, the distribution of electrons and holes in QWs may be changed, leading to a redshift of EL spectra. In particular, when the In gradient increases, the overlap integral of electron-hole wavefunction in InGaN QWs increases, resulting in a higher radiative recombination rate and an enhanced EL intensity.

Research on Innovation Experiment and Practice Teaching Reform of "Semiconductor Physics and Devices"

Professional innovation experiment and practice is the key link to broaden students' vision, exercise their thinking, and improve their practical skills in the process of university teaching. It is an important way to increase students' interest in learning, deepen the understanding of esoteric and obscure theoretical knowledge, and catch up with the frontiers of international science. However, due to the limitations of school funding resources, laboratory conditions, and traditional teaching mode, there are many problems during the experimental teaching of "Semiconductor Physics and Devices", such as the insufficient proportion of comprehensive and innovative experiments, outdated experimental contents, and single limited teaching methods that cannot stimulate students' learning interests of students. In response to the abovementioned situation, combined with many years of experience in learning and teaching semiconductor courses and drawing lessons from the advanced teaching modes of international applied technology universities, we creatively adopt the new experimental and practical teaching mode of "in school experiment + out of school practice" and "in-class experiment + extracurricular innovation project expansion". Network interesting experiments and international cutting-edge research topics (such as organic optoelectronic materials) are introduced into our innovative experiments and practical teaching, such as preparing new organic light-emitting pn junction diodes and quantum dot light-emitting diodes, and perovskite thin-film solar cells. Students deeply love these teaching reform measures, stimulate their interest in learning and scientific research, and significantly improve their ability to solve practical problems or scientific research innovation ability, which have achieved preliminary results. The accumulated teaching experience will provide a reference for developing semiconductor physics and devices experimental courses for semiconductor or optoelectronics and microelectronics majors in application-oriented universities.

A hybrid coupler for directing quantum light emission with high radiative Purcell enhancement to a dielectric metasurface lens

Quantum photonic technologies such as quantum sensing, metrology, and simulation could be transformatively enabled by the availability of integrated single photon sources with high radiative rates and photon collection efficiencies. We address these challenges for quantum emitters formed from color center defect sites such as those in hexagonal boron nitride, which are promising candidates as single photon sources due to their bright, stable, polarized, and room temperature emission. We report design of a nanophotonic coupler from color center quantum emitters to a dielectric metasurface lens. The coupler is comprised of a hybrid plasmonic–dielectric resonator that achieves a large radiative Purcell enhancement and partial control of far-field radiation. We report radiative Purcell factors up to 285 and photon collection efficiencies up to 89% for a lossless metasurface, applying a continuous hyperboloidal phase-front. Our hybrid plasmonic–dielectric coupler interfacing two nanophotonic elements is a compound optical element, analogous to those found in microscope objective lenses, which combine multiple optical functions into a single component for improved performance.

Effects of NaB<sub>2</sub>O<sub>4</sub>:Mn<sup>2+</sup> and Ba<sub>2</sub>Li<sub>2</sub>Si<sub>2</sub>O<sub>7</sub>:Sn<sup>3+</sup>,Mn<sup>2+</sup> phosphors and remote structure organizations on the white light-emitting diodes with quantum dots and phosphors

In order to increase the optical features of white light-emitting diodes (WLEDs), quantum dots (QDs) and phosphor materials have been proposed because of outstanding performance. The configuration of WLEDs with QDs layer and phosphor-silicone layer suggested placing these components separately to limit light loss, and enhance consistency at contact surface of QDs. In this research, the effects of QDs and phosphor on the performance of WLEDs are concluded through experiments. The emitted light and PL spectra were examined thoroughly, and infrared thermal imagers were applied to simulate the heat generation of an actual WLED device. The results show that with the configuration of 60 mA energy source, WLEDs which has the QDs-on-phosphor form attained luminous efficiency (LE) of 110 lm/W, with color rendering index (CRI) of Ra=92 and R9=80, whereas the WLEDs which has the phosphor-on-QDs form only has 68 lm/W in LE, Ra=57 and R9=24. Furthermore, WLEDs which has the QDs-on-phosphor form has less high temperature generated at the components’ conjunction in comparison to the counterpart, the peak generated heat in QDs-on-phosphor WLEDs is also lower and the heating capacity gap between 2 structures can go up to 12.3°C.

Controlling quantum numbers and light emission of Rydberg states via the laser pulse duration

High Harmonic Generation (HHG) creates coherent high frequency radiation via the process of strong field ionization followed by recombination. Recently, a complementary approach based on Frustrated Tunnel Ionization (FTI) was demonstrated (Nature Photonics 12, 620 (2018)). It uses spectrally separated peaks created by lower quantum number Rydberg states to produce coherent extreme ultraviolet (EUV) light. While much is understood about enhancing emission from HHG by controlling recombining electron trajectories, relatively little is known about controlling the quantum number distribution of Rydberg states. This distribution is generally believed to be determined primarily by field strength and laser frequency. We show that, in fact, it also changes significantly with the duration of the laser pulse: increasing pulse duration depletes lower-lying Rydberg states, thereby substantially decreasing EUV yield. Using electron trajectory analysis, we identify elastic recollision as the underlying cause. Our results open a door to greater control over production of coherent high frequency radiation, by combining FTI and HHG mechanisms, and also improved the interpretation of molecular imaging experiments that rely on elastic electron recollision.

Single quantum emitters detection with amateur CCD: Comparison to a scientific-grade camera

Fluorescence imaging of single quantum light emitters (atoms, molecules, quantum dots, color centers in crystals) is an inherent experimental problem of modern photonics and its numerous applications. In these measurements, highly sensitive cameras are of the key significance. Recent progress in technologies of charge-coupling devices (CCD) and complementary metal-oxide semiconductor (CMOS) sensors opens up possibilities for detection of extreme low light signals up to a single photon counting. Here, we investigate the parameters of high-professional scientific- and amateur-grade cameras in the view of their use in the fluorescence nanoscopy with the detection of single molecules and, in general, quantum emitters of different nature. A series of photoluminescence imaging experiments have been conducted with single colloidal semiconductor core-shell nanocrystals CdSeS/ZnS (quantum dots, QD), which are usually considered as a basis of various sensors and actuators technologies. We find parameters of the experiment for the amateur-grade camera to obtain images of single QDs with signal-to-noise ratio compared to the scientific-grade camera at exposure times ranging from 1s to 1000s.

Optical quantum technologies with hexagonal boron nitride single photon sources

Single photon quantum emitters are important building blocks of optical quantum technologies. Hexagonal boron nitride (hBN), an atomically thin wide band gap two dimensional material, hosts robust, optically active luminescent point defects, which are known to reduce phonon lifetimes, promises as a stable single-photon source at room temperature. In this Review, we present the recent advances in hBN quantum light emission, comparisons with other 2D material based quantum sources and analyze the performance of hBN quantum emitters. We also discuss state-of-the-art stable single photon emitter’s fabrication in UV, visible and near IR regions, their activation, characterization techniques, photostability towards a wide range of operating temperatures and harsh environments, Density-functional theory predictions of possible hBN defect structures for single photon emission in UV to IR regions and applications of single photon sources in quantum communication and quantum photonic circuits with associated potential obstacles.

Quantum Light Emission from Coupled Defect States in DNA-Functionalized Carbon Nanotubes.

Solid-state single-photon sources are essential building blocks for quantum photonics and quantum information technologies. This study demonstrates promising single-photon emission from quantum defects generated in single-wall carbon nanotubes (SWCNTs) by covalent reaction with guanine nucleotides in their single-stranded DNA coatings. Low-temperature photoluminescence spectroscopy and photon-correlation measurements on individual guanine-functionalized SWCNTs (GF-SWCNTs) indicate that multiple, closely spaced guanine defect sites within a single ssDNA strand collectively form an exciton trapping potential that supports a localized quantum state capable of room-temperature single-photon emission. In addition, exciton traps from adjacent ssDNA strands are weakly coupled to give cross-correlations between their separate photon emissions. Theoretical modeling identifies coupling mechanism as a capture of band-edge excitons. Because the spatial pattern of nanotube functionalization sites can be readily controlled by selecting ssDNA base sequences, GF-SWCNTs should become a versatile family of quantum light emitters with engineered properties.

(Invited) Quantum Light Emission from Coupled Defect-States in DNA-Functionalized Carbon Nanotubes

Solid-state single-photon sources are the essential building block for quantum photonics and quantum information technologies. The report here illustrates an advanced perspective of implanting coupled fluorescent quantum defects in single-wall carbon nanotubes (SWCNTs) through chemical reactions between the nanotube sidewall and the guanine nucleotides in single-stranded DNA (ssDNA) that coats the nanotube. Through low-temperature photoluminescence spectroscopy and photon correlation experiments, we have revealed that multiple guanine defects within a single ssDNA strand couple together to form a cumulative deep trapping potential supporting a localized quantum state that is capable of room-temperature single-photon emission. Helical wrapping of multiple ssDNA strands in single nanotubes allows a series of exciton localization sites to be created along the length of the SWCNTs. Such unique exciton trapping potential landscape gives rise to previously inaccessible intrinsic emission characteristics including coupling of multiple spatially separated quantum emitters. Our joint experimental and computational studies together reveal quantum emission properties from multiple spatially patterned covalent defects in SWCNTs, identify capture of the band-edge exciton as the underlying cause of the cross-correlated photon emission and open a distinctive prospect for tailoring chemically altered nanotubes as quantum light emitters.

Two-Dimensional Gallium Sulfide Nanoflakes for UV-Selective Photoelectrochemical-type Photodetectors.

Two-dimensional (2D) transition-metal monochalcogenides have been recently predicted to be potential photo(electro)catalysts for water splitting and photoelectrochemical (PEC) reactions. Differently from the most established InSe, GaSe, GeSe, and many other monochalcogenides, bulk GaS has a large band gap of ∼2.5 eV, which increases up to more than 3.0 eV with decreasing its thickness due to quantum confinement effects. Therefore, 2D GaS fills the void between 2D small-band-gap semiconductors and insulators, resulting of interest for the realization of van der Waals type-I heterojunctions in photocatalysis, as well as the development of UV light-emitting diodes, quantum wells, and other optoelectronic devices. Based on theoretical calculations of the electronic structure of GaS as a function of layer number reported in the literature, we experimentally demonstrate, for the first time, the PEC properties of liquid-phase exfoliated GaS nanoflakes. Our results indicate that solution-processed 2D GaS-based PEC-type photodetectors outperform the corresponding solid-state photodetectors. In fact, the 2D morphology of the GaS flakes intrinsically minimizes the distance between the photogenerated charges and the surface area at which the redox reactions occur, limiting electron–hole recombination losses. The latter are instead deleterious for standard solid-state configurations. Consequently, PEC-type 2D GaS photodetectors display a relevant UV-selective photoresponse. In particular, they attain responsivities of 1.8 mA W–1 in 1 M H2SO4 [at 0.8 V vs reversible hydrogen electrode (RHE)], 4.6 mA W–1 in 1 M Na2SO4 (at 0.9 V vs RHE), and 6.8 mA W–1 in 1 M KOH (at 1.1. V vs RHE) under 275 nm illumination wavelength with an intensity of 1.3 mW cm–2. Beyond the photodetector application, 2D GaS-based PEC-type devices may find application in tandem solar PEC cells in combination with other visible-sensitive low-band-gap materials, including transition-metal monochalcogenides recently established for PEC solar energy conversion applications.

Solid-state fluorescent nitrogen doped graphene quantum dots with yellow emission for white light-emitting diodes

Light-emitting graphene quantum dots (GQDs) are widely investigated due to their distinct merits. However, GQDs generally suffer from aggregation-induced luminescence quenching, which means they are highly emissive in a solution state with uniform dispersion but dramatically quenched in a solid or aggregated state. This problem significantly limits the application of GQDs, partially in the solid-state light-emitting devices. In this report, we successfully developed a simple and efficient hydrothermal method for the production of nitrogen doped graphene quantum dots (N-GQDs) with strong solid-state fluorescence (SSF) by using citric acid and o-Phenylenediamine as precursors. Under the 365 nm UV light illumination, the produced N-GQDs in an aqueous state exhibit blue color, with a quantum yield of 58%. As the concentration of N-GQDs increases, the photoluminescence exhibits an obvious red-shift from blue to yellow. For the N-GQDs in solid state, yellow luminescence with a high photoluminescence quantum yield (PLQY) of 28% is achieved under the 405 nm excitation. Finally, via the simple adjustment of thickness and the concentration of N-GQDs in blue emitting InGaN chips, color converter is enabled by constructing white light-emitting diode (WLED) device with improved color rendering index (CRI) and correlated color temperature (CCT).

Enhanced Photoluminescence of Halide Perovskite Nanocrystals Mediated by a Higher-Order Topological Metasurface

Halide perovskite nanocrystals are a family of nanomaterials with a high prospect for use in light-emitting devices, lasers, and quantum optics, which makes their integration into photonic circuits...

Quantum control of entangled photon-pair generation in electron-atom collisions driven by laser-synthesized free-electron wave packets

We propose an extension of coherent control using laser-synthesized free-electron matter waves. In contrast to coherent control schemes exploiting optical coherences to steer the dynamics of matter waves, we analyze the opposite and investigate the control of quantum light emission driven by laser-sculpted coherent free-electron matter waves. We apply this concept to the control of entangled photon-pair emission in electron-atom collisions, in which the incident electron wave packet, colliding with a target atom $B$, is engineered by interferometric resonantly-enhanced multiphoton ionization of a parent atom $A$. Each ionization pathway leads to electron wave packets that coherently interfere during temporal evolution in the continuum. Their mutual coherence can be controlled by adjusting the relative phases or time delays of the frequency components of the ionizing field contributing to the interfering pathways. We report coherent control of entangled photon-pair generation in radiative photo-cascade emission upon decay of the target atom after inelastic excitation triggered by the collision with the synthesized electron wave packet.

Assembly of large hBN nanocrystal arrays for quantum light emission

We fabricate rectangular arrays of hexagonal boron nitride (hBN) nanoplatelet clusters extending over hundreds of microns. Positioning is achieved by capillary assembly of suspended hBN particles into submicron polymer holes, patterned by electron-beam lithography. After removal of the patterned polymer from the SiO2/Si surface, average positioning yields of 74% at the desired locations are routinely achieved. At 10% of the locations, single-photon emitters (SPEs) are found. Thermal post-annealing of the prepared samples at 850 °C increases the number of SPEs by 50%. Our work paves the way for the production of wafer-scale SPE arrays based on commercially available hBN nanocrystals for a systematic statistical analysis of individually addressable SPEs, as well as for deterministic coupling of many emitters to a large number of photonic structures on photonic chips.