High‐Quality Whispering‐Gallery‐Mode Lasing from Cesium Lead Halide Perovskite Nanoplatelets

Semiconductor micro/nano‐cavities with high quality factor (Q) and small modal volume provide critical platforms for exploring strong light‐matter interactions and quantum optics, enabling further development of coherent and quantum photonic devices. Constrained by exciton binding energy and thermal fluctuation, only a handful of wide‐band semiconductors such as ZnO and GaN have stable excitons at room temperature. Metal halide perovskite with cubic lattice and well‐controlled exciton may provide solutions. In this work, high‐quality single‐crystalline cesium lead halide CsPbX₃ (X = Cl, Br, I) whispering‐gallery‐mode (WGM) microcavities are synthesized by vapor‐phase van der Waals epitaxy method. The as‐grown perovskites show strong emission and stable exciton at room temperature over the whole visible spectra range. By varying the halide composition, multi‐color (400–700 nm).WGM excitonic lasing is achieved at room temperature with low threshold (~ 2.0 μJ cm^?2) and high spectra coherence (~0.14–0.15 nm). The results advocate the promise of inorganic perovskites towards development of optoelectronic devices and strong light‐matter coupling in quantum optics.     

Platelet‐in‐Box Colloidal Quantum Wells: CdSe/CdS@CdS Core/Crown@Shell Heteronanoplatelets

Here, the CdSe/CdS@CdS core/crown@shell heterostructured nanoplatelets (NPLs) resembling a platelet‐in‐box structure are developed and successfully synthesized. It is found that the core/crown@shell NPLs exhibit consistently substantially improved photoluminescence quantum yield compared to the core@shell NPLs regardless of their CdSe‐core size, CdS‐crown size, and CdS‐shell thickness. This enhancement in quantum yield is attributed to the passivation of trap sites resulting from the critical peripheral growth with laterally extending CdS‐crown layer before the vertical shell growth. This is also verified with the disappearance of the fast nonradiative decay component in the core/crown NPLs from the time‐resolved fluorescence spectroscopy. When compared to the core@shell NPLs, the core/crown@shell NPLs exhibit relatively symmetric emission behavior, accompanied with suppressed lifetime broadening at cryogenic temperatures, further suggesting the suppression of trap sites. Moreover, constructing both the CdS‐crown and CdS‐shell regions, significantly enhanced absorption cross‐section is achieved. This, together with the suppressed Auger recombination, enables the achievement of the lowest threshold amplified spontaneous emission (≈20 μJ cm^?2) from the core/crown@shell NPLs among all different architectures of NPLs. These findings indicate that carefully heterostructured NPLs will play a critical role in building high‐performance colloidal optoelectronic devices, which may even possibly challenge their traditional epitaxially grown thin‐film based counterparts.     

Coupled Whispering Gallery Mode Resonators via Template‐Assisted Assembly of Photoluminescent Microspheres

This study reports a facile method for the assembly of large, array style, coupled dye‐doped microsphere resonators by template‐assisted, in which an aqueous suspension of colloidal microspheres assemble on a patterned template. By exploiting the high resolution of 3D (two‐photon) lithography derived templates, closely packed large arrays, hundreds to thousands of dimers with controlled gap spacing, only limited by the size of the substrate can be achieved. Dye‐doped emissive microspheres with Q‐factors >2.5 × 10² can be achieved and trapped into predetermined cavity positions, thereby controlling the distance between adjacent microspheres. This design allows to scale down dimer spacing from usual 400 nm for traditional photolithography to very small spacing of 50 nm. It is found that exciting individual microspheres in the ensemble shows intense optical cavity modes, whereas closely coupled pairs show controlled mode splitting. Coupling between photoluminescent microspheres is strongly influenced by the gap distance, with strong coupling, equating to normal mode splitting, arising as the gap distance is reduced below traditional sub‐micrometer scale. The coupled dimer assemblies are promising candidates for advancing the development of large‐area coupled nanophotonic structures, beyond the spatial resolution‐limited photolithographical derived arrays.     

Label‐Free Bioanalysis Based on Low‐Q Whispering Gallery Modes: Rapid Preparation of Microsensors by Means of Layer‐by‐Layer Technology

Low‐Q‐whispering gallery modes (low‐Q‐WGM) can be used for label‐free detection of interactions between biomolecules, measuring their binding and release kinetics or for analysis of changes in the medium in real‐time. The main advantage of the low‐Q‐WGM approach over other label‐free methods is the possibility of measurements in small cavities as the method uses microparticles down to 6 µm as sensors. Commercially available dye‐doped microparticles that are used as low‐Q‐WGM sensors exhibit several drawbacks. Therefore, alternative particle types are developed and optimized as low‐Q‐WGM sensors. First, dye‐doped particles made of different materials are screened. The most critical parameter for WGM performance is the refractive index (RI) of sensor particles. Furthermore, surface roughness of particles, determined by scanning electron microscopy and atomic force microscopy, affects their performance as WGM microsensors. In the second test, fluorescent dyes immobilized on nonfluorescent particles by means of nanometer thick layer‐by‐layer (LbL) films are shown to generate a strong WGM signal. The LbL‐coated particles show remarkably less background fluorescence than dye‐doped particles and are easier to prepare. Finally, this article proposes rapid preparation methods for WGM microparticle sensors based on various parameters such as material type, RI, surface roughness, and number of coated polymer layers.     

Electro‐Optics of Colloidal Quantum Dot Solids for Thin‐Film Solar Cells

The electro‐optics of thin‐film stacks within photovoltaic devices plays a critical role for the exciton and charge generation and therefore the photovoltaic performance. The complex refractive indexes of each layer in heterojunction colloidal quantum dot (CQD) solar cells are measured and the optical electric field is simulated using the transfer matrix formalism. The exciton generation rate and the photocurrent density as a function of the quantum dot solid thickness are calculated and the results from the simulations are found to agree well with the experimentally determined results. It can therefore be concluded that a quantum dot solid may be modeled with this approach, which is of general interest for this type of materials. Optimization of the CQD solar cell is performed by using the optical simulations and a maximum solar energy conversion efficiency of 6.5% is reached for a CQD solid thickness of 300 nm.     

Remote Biosensing with Polychromatic Optical Waveguide Using Blue Light‐Emitting Organic Nanowires Hybridized with Quantum Dots

Nanometer‐scale optical waveguides are attractive due to their potential applicability in photonic integration, optoelectronic communication, and optical sensors. Nanoscale white light‐emitting and/or polychromatic optical waveguides are desired for miniature white‐light generators in microphotonic circuits. Here, polychromatic (i.e., blue, green, and red) optical waveguiding characteristics are presented using a novel hybrid composite of highly crystalline blue light‐emitting organic nanowires (NWs) combined with blue, green, and red CdSe/ZnS quantum dots (QDs). Near white‐color waveguiding is achieved for organic NWs hybridized with green and red QDs. Light, emitted from QDs, can be transferred to the organic NW and then optically waveguided through highly packed π‐conjugated organic molecules in the NW with different decay characteristics. Remote biosensing using dye‐attached biomaterials is presented by adapting the transportation of QD‐emitted light through the organic NW.     

Facet Control for Trap‐State Suppression in Colloidal Quantum Dot Solids

Trap states in colloidal quantum dot (QD) solids significantly affect the performance of QD solar cells, because they limit the open‐circuit voltage and short circuit current. The {100} facets of PbS QDs are important origins of trap states due to their weak or missing passivation. However, previous investigations focused on synthesis, ligand exchange, or passivation approaches and ignored the control of {100} facets for a given dot size. Herein, trap states are suppressed from the source via facet control of PbS QDs. The {100} facets of ≈3 nm PbS QDs are minimized by tuning the balance between the growth kinetics and thermodynamics in the synthesis. The PbS QDs synthesized at a relatively low temperature with a high oversaturation follow a kinetics‐dominated growth, producing nearly octahedral nanoparticles terminated mostly by {111} facets. In contrast, the PbS QDs synthesized at a relatively high temperature follow a thermodynamics‐dominated growth. Thus, a spherical shape is preferred, producing truncated octahedral nanoparticles with more {100} facets. Compared to PbS QDs from thermodynamics‐dominated growth, the PbS QDs with less {100} facets show fewer trap states in the QD solids, leading to a better photovoltaic device performance with a power conversion efficiency of 11.5%.     

Laser‐Induced In‐Fiber Fluid Dynamical Instabilities for Precise and Scalable Fabrication of Spherical Particles

Scalable fabrication of spherical particles at both the micro‐ and nanoscales is of significant importance for applications spanning optical devices, electronics, targeted drug delivery, biodevices, sensors, and cosmetics. However, current top‐down and bottom‐up fabrication methods are unable to provide the full spectrum of uniformly sized, well‐ordered, and high‐quality spheres due to their inherent restrictions. Here, a generic, scalable, and precisely controllable fabrication method is demonstrated for generating spherical particles in a full range of diameters from microscale to nanoscale. This method begins with a macroscopic composite multimaterial solid‐state preform drawn into a fiber that defines precisely the initial conditions for the process. It is then followed by CO₂ laser heating to enable the transformation from a continuous fiber core into a series of homogeneous spheres via Plateau–Rayleigh capillary instability inside the fiber. This physical breakup method applies to a wide range of functional materials with different melting temperatures from 400 to 2400 K and 10 orders of difference in fiber core/cladding viscosity ratio. Furthermore, an ordered array of silicon‐based whispering‐gallery mode resonators with the Q factor as high as 7.1 × 10⁵ is achieved, owing to the process induced ultrasmooth surface and highly crystalline nature.     

Analysis of Cavity‐Mode Lasing Characteristics from a Resonator with Broadband Cholesteric Liquid‐Crystal Bragg Reflectors

Detailed optical lasing characteristics in liquid crystal (LC) microlasers consisting of multiple polymer cholesteric LC (PCLC) layers are presented as broadband resonators sandwiching a layer of thick gain media, dye‐containing nematic LC (NLC) or isotropic liquid, in between. Multiple lasing emission peaks due to Fabry‐Perot cavity modes are observed for both gain media, and their polarization characteristics investigated. To analyze lasing characteristics, specified eigen modes are defined, the polarization states of which are maintained before and after passing through the broadband resonator, and obtained for the present full system by using the Berreman 4 × 4 matrix method. Using these specified eigen modes, the optical density for each mode is calculated and compared with the experimental results, and shows good agreement. Finally, lasing characteristics between the resonators with NLC and isotropic gain media are compared, and the advantages of adopting dye‐doped NLC gain medium are shown for tunable red, green, blue lasing in a microlaser system with a broadband resonator.     

Light‐Emitting Electrochemical Cells Based on Color‐Tunable Inorganic Colloidal Quantum Dots

Large‐area, ultrathin light‐emitting devices currently inspire architects and interior and automotive designers all over the world. Light‐emitting electrochemical cells (LECs) and quantum dot light‐emitting diodes (QD‐LEDs) belong to the most promising next‐generation device concepts for future flexible and large‐area lighting technologies. Both concepts incorporate solution‐based fabrication techniques, which makes them attractive for low cost applications based on, for example, roll‐to‐roll fabrication or inkjet printing. However, both concepts have unique benefits that justify their appeal. LECs comprise ionic species in the active layer, which leads to the omission of additional organic charge injection and transport layers and reactive cathode materials, thus LECs impress with their simple device architecture. QD‐LEDs impress with purity and opulence of available colors: colloidal quantum dots (QDs) are semiconducting nanocrystals that show high yield light emission, which can be easily tuned over the whole visible spectrum by material composition and size. Emerging technologies that unite the potential of both concepts (LEC and QD‐LED) are covered, either by extending a typical LEC architecture with additional QDs, or by replacing the entire organic LEC emitter with QDs or perovskite nanocrystals, still keeping the easy LEC setup featured by the incorporation of mobile ions.     

An Integrated Multifunctional Nanoplatform for Deep‐Tissue Dual‐Mode Imaging

The combination of biocompatible superparamagnetic and photoluminescent nanoparticles (NPs) is intensively studied as highly promising multifunctional (magnetic confinement and targeting, imaging, etc.) tools in biomedical applications. However, most of these hybrid NPs exhibit low signal contrast and shallow tissue penetration for optical imaging due to tissue‐induced optical extinction and autofluorescence, since in many cases, their photoluminescent components emit in the visible spectral range. Yet, the search for multifunctional NPs suitable for high photoluminescence signal‐to‐noise ratio, deep‐tissue imaging is still ongoing. Herein, a biocompatible core/shell/shell sandwich structured Fe₃O₄@SiO₂@NaYF₄:Nd³⁺ nanoplatform possessing excellent superparamagnetic and near‐infrared (excitation) to near‐infrared (emission), i.e., NIR‐to‐NIR photoluminescence properties is developed. They can be rapidly magnetically confined, allowing the NIR photoluminescence signal to be detected through a tissue as thick as 13 mm, accompanied by high T₂ relaxivity in magnetic resonance imaging. The fact that both the excitation and emission wavelengths of these NPs are in the optically transparent biological windows, along with excellent photostability, fast magnetic response, significant T₂‐contrast enhancement, and negligible cytotoxicity, makes them extremely promising for use in high‐resolution, deep‐tissue dual‐mode (optical and magnetic resonance) in vivo imaging and magnetic‐driven applications.     

Boosting the Non Linear Optical Response of Carbon Nanotube Saturable Absorbers for Broadband Mode‐Locking of Bulk Lasers

Single‐walled carbon‐nanotube absorbers are experimentally demonstrated for laser mode‐locking. A saturable absorber device is used to mode‐lock three different bulk solid‐state lasers in a 500 nm‐wide wavelength interval. The devices exhibit a low saturation fluence of <10 µJ cm^?2, low scattering losses, and an exceptionally rapid relaxation, with time constants reaching <100 fs. The latter two properties are explained by a decreased curling tendency and increased tube‐to‐tube interactions of the nanotubes, respectively. These properties are the result of an optimized manufacturing procedure in combination with the use of a starting material with a higher microscopic order. The decreased scattering enables universal use of these devices in bulk solid‐state lasers, which tend to be highly sensitive against non‐saturable device losses as caused by scattering. The favorable saturable absorption properties are experimentally verified by mode‐locking the three lasers, which all exhibit near transform‐limited performance with about 100 fs pulse duration. The complete and unconditional absence of Q‐switching side bands verifies the small saturation fluence of these devices.     

SOA‐Integrated Dual‐Mode Laser and PIN‐Photodiode for Compact CW Terahertz System

We designed and fabricated a semiconductor optical amplifier‐integrated dual‐mode laser (SOA‐DML) as a compact and widely tunable continuous‐wave terahertz (CW THz) beat source, and a pin‐photodiode (pin‐PD) integrated with a log‐periodic planar antenna as a CW THz emitter. The SOA‐DML chip consists of two distributed feedback lasers, a phase section for a tunable beat source, an amplifier, and a tapered spot‐size converter for high output power and fiber‐coupling efficiency. The SOA‐DML module exhibits an output power of more than 15 dBm and clear four‐wave mixing throughout the entire tuning range. Using integrated micro‐heaters, we were able to tune the optical beat frequency from 380 GHz to 1,120 GHz. In addition, the effect of benzocyclobutene polymer in the antenna design of a pin‐PD was considered. Furthermore, a dual active photodiode (PD) for high output power was designed, resulting in a 1.7‐fold increase in efficiency compared with a single active PD at 220 GHz. Finally, herein we successfully show the feasibility of the CW THz system by demonstrating THz frequency‐domain spectroscopy of an α‐lactose pellet using the modularized SOA‐DML and a PD emitter.     

Low‐Threshold Distributed‐Feedback Lasers Based on Pyrene‐Cored Starburst Molecules with 1,3,6,8‐Attached Oligo(9,9‐Dialkylfluorene) Arms

Here, a detailed characterization of the optical gain properties of sky‐blue‐light‐emitting pyrene‐cored 9,9‐dialkylfluorene starbursts is reported; it is shown that these materials possess encouragingly low laser thresholds and relatively high thermal and environmental stability. The materials exhibit high solid‐state photoluminescence (PL) quantum efficiencies (>90%) and near‐single‐exponential PL decay transients with excited state lifetimes of ～1.4 ns. The thin‐film slab waveguide amplified spontaneous emission (ASE)‐measured net gain reaches 75–78 cm^?1. The ASE threshold energy is found to remain unaffected by heating at temperatures up to 130 °C, 40 to 50 °C above T_g. The ASE remained observable for annealing temperatures up to 170 or 200 °C. 1D distributed feedback lasers with 75% fill factor and 320 nm period show optical pumping thresholds down to 38–65 Wcm^?2, laser slope efficiencies up to 3.9%, and wavelength tuning ranges of ～40 nm around 471–512 nm. In addition, these lasers have relatively long operational lifetimes, with N_1/2 ≥ 1.1 × 10⁵ pulses for unencapsulated devices operated at ten times threshold in air.     

High‐Security Multifunctional Nano‐Bismuth‐Sphere‐Cluster Prepared from Oral Gastric Drug for CT/PA Dual‐Mode Imaging and Chemo‐Photothermal Combined Therapy In Vivo

Multifunctional nanoprobes that can be applied for real‐time monitoring or precision treatment of tumors have received wide interest among researchers. However, most of these nanoprobes are obtained through chemical synthesis, and thereby may contain toxic residues or harmful reagents. In this article, a nano‐bismuth‐sphere‐cluster (Bi) is synthesized via a one‐step method (after an irradiation with ultra‐violet) and is then applied in dual‐mode computed tomography/photoacoustic imaging. Bismuth potassium citrate granules, which is a common gastric drug that is highly safe and has a low price (<1 China Yuan/g), is used as the only raw material. The results show that the Bi cluster has good stability with sizes of about 25–55 nm, and a photothermal conversion efficiency as high as 39.67%. After being adsorbed onto doxorubicin, the Bi cluster can be used directly in animal experiments. Due to the effect of enhanced permeability and retention, the probe can easily enter tumor cells. Drug release can be controlled by a near‐infrared laser and the acidic environment of tumor cells, which indicates that the combined chemo‐photothermal therapy is achieved. This work presents a new dual‐mode bio‐imaging and combined chemo‐photothermal therapeutic nanoprobe that can be applied in theragnostics for tumors.