Emission Quantum Research Articles

Local Droplet Etching with Indium Droplets on InP(100) by Metal-Organic Vapor Phase Epitaxy.

The local droplet etching (LDE) by using indium droplets on bare InP(100) surfaces is demonstrated in a metal-organic vapor phase epitaxy (MOVPE) environment for the first time. The role of an arsenic flow applied to self-assembled metallic indium droplets is systematically studied. Increasing the arsenic supply leads to the formation of ring-like nanostructures and nanoholes. The results are analyzed with reference to LDE in a molecular beam epitaxy environment, where such a technique is well established, particularly for arsenide-based III-V semiconductors, and where only one group-V material is involved. Here, As-P exchange reactions at droplet sites are identified as the drivers for the formation of nanoholes. Such nanoholes can serve as nucleation sites for subsequent fabrication of highly symmetric QDs by nanohole-infilling or as a means for in situ surface nanopatterning. LDE on InP by MOVPE can thus be considered as a promising approach for the cost-effective fabrication of novel quantum emitters at the telecom C-band.

Probing the limits for coherent optical control of a mechanically decoupled defect center in hexagonal boron nitride

The coherent control of a two-level system is among the most essential challenges in modern quantum optics. Understanding its fundamental limitations is crucial, also for the realization of next generation quantum devices. The quantum coherence of a two-level system is fragile in particular, when the two levels are connected via an optical transition, which, at the same time, enables the manipulation of the system. When such quantum emitters are located in solids the coherence suffers from the interaction of the optical transition with the solid state environment, which requires the sample to be cooled to temperatures of a few Kelvin or below. Here, we use a mechanically isolated quantum emitter in hexagonal boron nitride to explore the individual mechanisms which affect the coherence of an optical transition under resonant drive. We operate the system at the threshold where the mechanical isolation collapses in order to study the onset and temperature-dependence of dephasing and independently of spectral diffusion. The insights on the underlying physical decoherence mechanisms reveal a limit in temperature until which coherent driving of the system is possible. This study enables to increase the operation temperature of hBN-based quantum devices, therefore reducing the need for cryogenic cooling.

Synthesis, structure, photo- and electroluminescent properties of methyl- and alkoxy-substituted 4-methyl-N-[2-(phenyliminomethyl)phenyl]benzenesulfamides and their zinc(II) complexes

A series of novel Zn(II) bischelate complexes based on azomethines of 2-(N-tosylamino)benzaldehyde and aromatic amines (aniline, 4-methylaniline, 4-methoxyaniline, 2-methoxylaniline, and 4-ethoxylanine) were designed and synthesized with the aim of studying their photo- and electro-luminescent properties. The structures of the synthesized azomethines and their complexes were studied by elemental analysis, infrared (IR) and proton nuclear magnetic resonance (1H NMR) spectroscopy. The structure of the Zn(II)-complexes was determined using X-ray diffraction analysis. In the solid state, azomethines exhibit bright luminescence in the yellow part of the spectrum with high emission efficiency and quantum yields of approximately 50%. Zinc complexes based on them exhibit noticeable luminescence in the solid state and in solutions of methylene chloride. Compared to azomethines, the luminescence maxima of Zn(II) complexes are hypsochromically shifted, and they exhibit pronounced blue-green luminescence. The OLED devices based on zinc(II) complexes emit strong bluish-green light with a peak maximum at 478-490 nm. The device with the best parameters has a maximum luminance of 2103 cd/m2, a current efficiency of 14.0 cd/A, and an overall efficiency of 4.8%, with a turn-on voltage of 3.6 V.

Efficient coupling between photonic waveguides and III-nitride quantum emitters in the UV-visible spectral range

Efficient coupling between photonic waveguides and III-nitride quantum emitters in the UV-visible spectral range

Mono-/multi-fluorination of 1,8-naphthalimides for developing AIE/AIEE fluorophores with tuning emission wavelength

Aggregation-induced emission/aggregation-induced emission enhancement (AIE/AIEE) luminogens provides amount of highly emissive materials in density states for versatile applications. Most of the AIE/AIEEgens were designed with the multiply rotation unit, in which the additional rotation units not only extend the molecular structure but also suffer from low atom economy. Herein, a fluorination strategy was introduced to construct ten AIE/AIEEgens with 1∼3 fluorine (F) atoms at different position of phenyl ring at previous developed AIEgen, 4-phenyl-1,8-naphthalimide, which can output tuning emissive wavelength and high quantum yields in both aqueous solutions and solids. In these compounds, five AIEgens with ortho-F atom and five AIEEgens without ortho-F atom were obtained. All compounds show bright blue emissions centered at 430–485 nm in aqueous solutions and wide emissions covering visible region in solid states. We calculated the ratio of quantum yields between their aqueous solution and THF solution (Φwater/ΦTHF). The AIE luminogens show the higher ratios between 10.19 and 24.89 and the AIEEgens show the lower ratios between 1.89 and 6.40. This strategy based on changing the substituent positions of F atoms provides an efficient and convenient method for construction of novel AIE-active materials with variable photophysical properties in density states.

Understanding the Role of NHC Ditopic Ligand Substituents in the Molecular Diversity and Emissive Properties of Silver Complexes.

Silver bis(carbene) complexes featuring ditopic N-heterocyclic carbene (NHC) ligands have been synthesized which enable the assembly of supramolecular architectures via reaction with silver triflate. Through a systematic exploration of crystal structures and emissive properties, this study investigates the impact of the substituents on the NHC ditopic ligands [R-Im-2-Z-py], where R = Me, benzyl (Bz), or 2-naphthylmethyl (NaphCH2), and Z = H or Cl in the structural framework and emissive properties observed in the silver bis(carbene) or polynuclear species. Remarkably diverse structural motifs emerge in both of them, predominantly influenced by the choice of R wingtip and second by the Z substituent. Also the emissive quantum yield of the complexes is mostly governed by the selection of the R wingtip and further modulated by the Z substituent. Several of the mono and polynuclear complexes exhibit complex emissive profiles, including the observation of dual emission phenomena. Particularly noteworthy is the complex [Ag(NHC)]2]OTf (R = Bz, Z = Cl), which demonstrates an exceptionally intense single blue emission with a remarkable solid-state quantum yield (Φ) of 24%.

Recent Advances of Organic-Inorganic Hybrid Fluorescent Hyperbranched Polymer: Synthesis, Performance Regulation Strategies and Applications.

The organic-inorganic hybrid fluorescent hyperbranched polymer, including hyperbranched polysiloxane and hyperbranched polyborate, have attracted much attention due to their excellent optical properties and wide range of applications. Hyperbranched polysiloxane and polyborates, prepared by introducing Si or B elements into organic polymer chains at the molecular level through rational molecular design and novel synthesis methods, exhibit outstanding photophysical properties as an indispensable branch of organic-inorganic hybrid fluorescent materials. Herein, this review highlights the recent research progress on hyperbranched polysiloxanes and hyperbranched polyborates, including strategies for regulating their emission wavelengths, quantum yields, and fluorescence lifetimes, potential emission mechanisms, and various applications. Finally, some challenges and promising future directions in the field of organic-inorganic hybrid fluorescent polymers are summarized.

Computationally Driven Discovery of T Center-like Quantum Defects in Silicon.

Quantum technologies would benefit from the development of high-performance quantum defects acting as single-photon emitters or spin-photon interfaces. Finding such a quantum defect in silicon is especially appealing in view of its favorable spin bath and high processability. While some color centers in silicon have been emerging in quantum applications, there remains a need to search for and develop new high-performance quantum emitters. By searching a high-throughput computational database of more than 22,000 charged complex defects in silicon, we identify a series of defects formed by a group III element combined with carbon ((A-C)Si with A = B, Al, Ga, In, Tl) and substituting on a silicon site. These defects are analogous structurally, electronically, and chemically to the well-known T center in silicon ((C-C-H)Si), and their optical properties are mainly driven by an unpaired electron on the carbon p orbital. They all emit in the telecom, and some of these color centers show improved properties compared to the T center in terms of computed radiative lifetime, emission efficiency, or smaller optical linewidth. The kinetic barrier computations and previous experimental evidence show that these T center-like defects can be formed through the capture of a diffusing carbon by a substitutional group III atom. We also show that the synthesis of hydrogenated T center-like defects followed by a dehydrogenation annealing step could facilitate the formation of these defects. Our work motivates further studies on the synthesis and control of this new family of quantum defects and demonstrates the use of high-throughput computational screening to discover new color center candidates.

Er3+ -doped oxyfluoroborosilicate glass ceramics with embedded CaF2 nanoparticles for 1.53 μm broad band applications

The CaF2 based oxyfluoroborosilicate glasses and glass ceramics doped with Er3+ ions were prepared via melt quench process followed by heat treatment and characterized for 1.53 μm broadband applications. The optimized glass ceramic sample was obtained at 450oC/1h heat treatment. The Er3+ concentration was optimized as 1.0 mol% for efficient emission at 460 nm excitation through concentration dependent luminescence analysis. The spectroscopic parameters such as Ωλ = 2,4,6 parameters and the radiative parameters such as spontaneous transition probability rates (AR), branching ratios (βR) and decay times (τR) were calculated applying the standard Judd-Ofelt theory. The effective bandwidth (Δλeff), stimulated emission cross-section (σe), gain bandwidth (σe × Δλeff), quantum efficiency (η) and figure of merit (σe × τR) were calculated as 25.78 nm, 13.42 × 10−21 cm2, 3.46 × 10−26 cm3, 82.83% and 5.32 × 10−23 cm2s, respectively for the optimized glass ceramic sample. The exchange type of energy transfer among the excited Er3+ ions results the quenching in luminescence and the non-exponentiality in decay curves. The systematic investigations carried out indicate that the glass ceramic obtained at 450oC/1h heat treatment was proficient for 1.53 μm broadband fiber lasers and optical amplifiers in S and C band communication window.

The bound states in the continuum of coupled resonance modes and multiple-function applications in grating-cavity structures

The bound states in the continuum (BICs) are desired for high-performance optical devices. The structures composed of gratings and cavities were investigated. Grating waveguide modes (GWMs) are excited by the grating in structures. When the symmetry of the structure is broken, the positive and opposite GWMs couple and generate upper- and lower-coupled modes. Two coupled modes show different properties, such as the Fabry-Pérot (F–P) BIC in lower-coupled mode and the symmetry-protected (SP) BICs in upper-coupled mode. The special properties indicate the two coupled modes are desirable for multifunctional applications. The radiation from the quantum emitter (QE) was enhanced 3030 times through the quasi-BIC of lower-coupled mode. The maximal group delay reached 6.1 ps by the quasi-BIC of the lower-coupled mode. The quasi-BIC of the upper-coupled mode generates high-performance absorption. Two coupled resonance modes are sensitive to polarization, which can be used for optical switching with a maximal amplitude modulation depth of up to 99.8% with an insertion loss of less than 0.008 dB. These results offer hope for developing multifunctional and high-performance devices through coupled resonance modes in the grating-cavity structures.

Dynamic control and manipulation of near-fields using direct feedback

Shaping and controlling electromagnetic fields at the nanoscale is vital for advancing efficient and compact devices used in optical communications, sensing and metrology, as well as for the exploration of fundamental properties of light-matter interaction and optical nonlinearity. Real-time feedback for active control over light can provide a significant advantage in these endeavors, compensating for ever-changing experimental conditions and inherent or accumulated device flaws. Scanning nearfield microscopy, being slow in essence, cannot provide such a real-time feedback that was thus far possible only by scattering-based microscopy. Here, we present active control over nanophotonic near-fields with direct feedback facilitated by real-time near-field imaging. We use far-field wavefront shaping to control nanophotonic patterns in surface waves, demonstrating translation and splitting of near-field focal spots at nanometer-scale precision, active toggling of different near-field angular momenta and correction of patterns damaged by structural defects using feedback enabled by the real-time operation. The ability to simultaneously shape and observe nanophotonic fields can significantly impact various applications such as nanoscale optical manipulation, optical addressing of integrated quantum emitters and near-field adaptive optics.

A Multi‐Functional New Acceptor for Ultra‐Broad Multiple Emission, Long‐Persistence Thermally Activated Delayed Fluorescence and Room Temperature Phosphorescence

AbstractAiming to design new efficient organic triplet emitters, here a new electron‐accepting moiety 11,13‐dihydro‐12H‐dibenzo[a,c]imidazo[4,5‐i]phenazin‐12‐one (BIPO) are reported. Three new BIPO derivatives containing long alkyl chains, namely DBIPO (acceptor only), DBIPOBr (acceptor containing bromine atoms), and DBIPOAc with acridan moieties in a donor‐acceptor‐donor configuration, are designed and investigated. Efficient room temperature phosphorescence (RTP) is detected for the three compounds, stemming from a high‐lying (anti‐Kasha type) triplet emission occurring in the acceptor moiety. Additionally, the tetrahydrofuran‐ and dichloromethane DBIPOAc solutions show (i) a dual‐band photoluminescence profile stemming from anti‐Kasha emissions from high‐lying charge‐transfer (1CT) and locally excited (1LE) states, and (ii) a thermally activated delayed fluorescence (TADF) from the same high‐lying 1CT state. Importantly, DBIPOAc doped in rigid nonpolar polymer Zeonex simultaneously exhibits both TADF and RTP, with the emission quantum yield reaching 69.6%. Due to these properties, the BIPO derivatives constitute promising candidates as multi‐functional new emitters for the preparation of active layers of electroluminescent devices and optical oxygen/pressure sensors. The reasons for these interesting properties are discussed in detail.

Collective quantum dynamics with distant quantum emitters in slow-wave nanoplasmonic waveguides

We consider a slow-wave nanoplasmonic waveguide system with spatially separated (distant) quantum emitters. Based on a nanoplasmonic waveguide quantum electrodynamic theory the emerging non-Markovian collective plasmon-polariton dynamics directly reflects the spatial positioning of the quantum emitters. A phase-space analysis allows us to distinguish between collectivity and cooperativity and the transition between these regimes. For distant emitters, temporal decoherence is reflected in anomalous phase-space evolution. In the spectral domain, collectivity emerges as a resonant single Lorentzian peak with two weak sidebands, while cooperativity manifests as a Fano-like resonance normal-mode splitting. Remarkably, even for distant quantum emitters, we achieve collective multiple quantum emitter dynamics with non-vanishing excitation and vanishing instantaneous emission, establishing an interaction-based quantum nanoplasmonic memory with key relevance in quantum nanoplasmonic networks.

Solvent mediated synthesis of multicolor narrow bandwidth emissive carbon quantum dots and their potential in white light emitting diodes

The development of efficient and environmentally sustainable materials for white light-emitting diodes (WLEDs) is of paramount importance in the field of lighting technology. In this study, we present a solvent-modulated synthesis approach for the fabrication of multicolor narrow-bandwidth emissive carbon quantum dots (CQDs) as a promising solution for constructing WLEDs. The synthesis method involves the controlled reaction of organic precursors in different solvent environments, leading to the formation of CQDs with distinct emission wavelengths with a relatively small full width at half maximum, ranging from 28 to 42 nm. Moreover, these synthesized multicolor CQDs demonstrate a remarkably high fluorescence quantum yield of up to 65%, indicating their potential for constructing efficient WLED when incorporated in polymer matrix and coated on the surface of blue light-emitting diode (LED).

Dissipative stabilization of maximal entanglement between nonidentical emitters via two-photon excitation

Two nonidentical quantum emitters, when placed within a cavity and coherently excited at the two-photon resonance, can reach stationary states of nearly maximal entanglement. In Vivas-Viaña, Martín-Cano, and Sánchez Muñoz [], we introduce a frequency-resolved Purcell effect stabilizing entangled W states among strongly interacting quantum emitters embedded in a cavity. Here we delve deeper into a specific configuration with a particularly rich phenomenology: two interacting quantum emitters under coherent excitation at the two-photon resonance. This scenario yields two resonant cavity frequencies where the combination of two-photon driving and Purcell-enhanced decay stabilizes the system into the subradiant and superradiant states, respectively. By considering the case of nondegenerate emitters and exploring the parameter space of the system, we show that this mechanism is merely one among a complex family of phenomena that can generate both stationary and metastable entanglement when driving the emitters at the two-photon resonance. We provide a global perspective of this landscape of mechanisms and contribute analytical characterizations and insights into these phenomena, establishing connections with previous reports in the literature and discussing how some of these effects can be optically detected. Published by the American Physical Society 2024

Alternative Plasmonic Materials for Fluorescence Enhancement.

Noble metals such as gold and silver have been used extensively for a range of plasmonic applications, including enhancing the fluorescence rate of a dye molecule, as evidenced by numerous experiments over the past two decades. Recently, a variety of doped semiconductors have been proposed as alternative plasmonic materials, exhibiting plasmonic resonances from ultraviolet to far-infrared. In this work, we investigate the suitability of these alternative materials for enhancing the fluorescence of a molecule. Considering nanosized spheres, we study their response under plane wave illumination and the resulting enhancement factors when coupled to a quantum emitter. Comparisons with standard plasmonic metals reveal that semiconductor materials lead to a significantly reduced, and often strongly quenched, emission of light caused by their dominant absorption, which hinders fluorescence enhancement. However, we show that enhancement may be obtained when considering poor emitting dyes and high refractive index environments. Our findings demonstrate that these alternative materials result in weaker fluorescence enhancement compared to their plasmonic counterparts. Nonetheless, there are means to compensate for this, and a reasonable enhancement can be achieved for dyes in the infrared spectrum.

Multiqubit quantum state preparation enabled by topology optimization

Using topology optimization, we inverse-design nanophotonic cavities enabling the preparation of pure states of pairs and triples of quantum emitters. Our devices involve moderate values of the dielectric constant, operate under continuous laser driving, and yield fidelities to the target (Bell and W) states approaching unity for distant qubits (several natural wavelengths apart). In the fidelity optimization procedure, our algorithm generates entanglement by maximizing the dissipative coupling between the emitters, which allows the formation of multipartite pure steady states in the driven-dissipative dynamics of the system. Our findings open the way toward the efficient and fast preparation of multiqubit quantum states with engineered features, with potential applications for nonclassical light generation, and quantum sensing and metrology.

Frequency-Resolved Purcell Effect for the Dissipative Generation of Steady-State Entanglement.

We report a driven-dissipative mechanism to generate stationary entangled W states among strongly interacting quantum emitters placed within a cavity. Driving the ensemble into the highest energy state-whether coherently or incoherently-enables a subsequent cavity-enhanced decay into an entangled steady state consisting of a single deexcitation shared coherently among all emitters, i.e., a W state, well known for its robustness against qubit loss. The nonharmonic energy structure of the interacting ensemble allows this transition to be resonantly selected by the cavity, while quenching subsequent off-resonant decays. Evidence of this purely dissipative mechanism should be observable in state-of-the-art cavity QED systems in the solid state, enabling new prospects for the scalable stabilization of quantum states in dissipative quantum platforms.

Inflated electronic and optical assessment of gC3N4/ZnO nanocomposite as a potential emissive layer material for OLED application

Organo-inorganic nanocomposite materials have been proven to be novel hybrid materials with inflated electronic and optical performance that can be tailored with the judicious selection of the building units or their combinations. Here, hydrothermal, thermal polycondensation, and ultrasonication techniques were used to synthesize pure ZnO, gC3N4, and gC3N4/ZnO with varying weights % such as 10 %, 15 %, 20 %, and 25 % of ZnO inorganic filler elements in gC3N4 matrix. The crystalline phase (hexagonal wurtzite) and crystallite size (10.0 nm, 17.6 nm, and 15.90 nm) of the synthesized materials were examined by X-ray diffractometer. The FESEM and HRTEM characterizations revealed the sheet-like gC3N4 and spherical-type ZnO nanoparticle-like microstructures of the samples. The present functional groups, corresponding vibrational frequency, chemical states, and binding energy were investigated using FTIR and XPS spectroscopic methods. Optical parameters such as optical band gap energy (Eg = 3.24 eV), Urbach energy (Eu = 0.41 eV), refractive index (n = 1.99), emission quantum yield (∼ 69.03 %), and color purity of the nanocomposites were examined using UV visible and photoluminescence spectroscopic techniques. IV and Hall measurements techniques were used to determine the semiconducting parameters of the optimized sample, such as conductivity (∼62.90×10−5 S/cm), carrier mobility (∼ 44.1 cm2/Volt. Sce), carrier concentrations (∼1.825×1014 cm−3), and sheet resistance (∼1.062×103 Ω/cm2). Due to their excellent optical and electrical behavior, the nanocomposite materials were found to be fairly suitable as a potential emissive layer material for OLED applications.

Quantum Physical Unclonable Function Based on Multidimensional Fingerprint Features of Single Photon Emitters in Random AlN Nanocrystals

AbstractPhysical unclonable function (PUF) has emerged as a unique physical'fingerprint' that is inherently difficult to replicate. It shows tremendous application value in various hardware security areas such as identity authentication, chip anticounterfeiting, communication encryption, blockchain, etc. However, with the rapid development of 3D nanoprinting, classical PUFs constructed with disordered micro‐nanostructures face tremendous threats from physical cloning attacks. Herein, this study proposes and demonstrates the utilization of room‐temperature single‐photon emitters derived from atomic defects in randomly distributed pyramidal aluminum nitride (AlN) nanocrystals as a novel quantum PUF to resist physical cloning attacks. The fabrication of this quantum PUF on silicon (Si) wafers enables seamless integration with silicon photonic integrated circuits. The multidimensional fingerprint features of the single‐photon emitters are highly sensitive to the lattice parameters of the uneven AlN nanocrystals. Furthermore, each single photon emitter can work as a quantum random number generator to ensure the fundamental unpredictability of PUFs. The subatomic precision requirement coupled with unpredictable quantum emission behavior makes it practically impossible to attack the proposed quantum PUF, providing a promising solution for information security in the post‐quantum era.