Centrifugation-Mediated Crystal Growth of Attractive Colloids for Band Edge Lasing.

Attractive depletion interactions are utilized to organize colloidal particles into crystalline arrays with high crystallinity through spontaneous phase separation. However, uncontrolled nucleation frequently leads to the formation of crystalline grains with varied crystal orientations, which hampers the optical performance of photonic crystals. Here, colloidal crystals have been engineered with uniform orientation and high surface coverage by applying centrifugal force during the depletion-induced assembly of polystyrene particles. The centrifugal force encourages the particles to move toward the bottom surface, which fosters heterogeneous nucleation and supports rapid crystal growth, yielding densely-packed and uniformly-arranged crystal grains with high reflectivity. This study has observed that the nucleation and crystal growth behavior is significantly influenced by the salt concentration. Based on the pair potentials, the transition boundary has been quantitatively analyzed between fluid and crystal phases and identified the threshold for homogeneous nucleation. Utilizing the high-reflectivity colloidal crystals, band-edge lasing is achieved by dissolving the water-soluble dye into the aqueous suspensions. Upon optical excitation, a lasing emission characterized is observed by a narrow spectral width at the short-wavelength band edge. Notably, the laser wavelength can be adjusted by altering the salt concentration or particle diameter, offering a versatile approach to tuning the optical properties.

Microstructure-Assisted Wafer-Scale Fabrication of Perovskite Microlaser Arrays.

All inorganic lead halide perovskites exhibit fascinating optical and optoelectronic characteristics for on-chip lasing, but the lack of precise control of wafer-scale fabrication for perovskite microstructure arrays restricts their potential applications in on-chip-integrated devices. In this work, a microstructure-template assisted crystallization method is demonstrated via a designed chemical vapor deposition process, achieving the controllable fabrication of homogeneous perovskite micro-hemispheroid (PeMH) arrays spanning the entire surface area of a 4-inch wafer. Benefiting from the low-loss whispering gallery resonance and plasmon-enhanced light-matter interactions in well-confined hybrid cavities, this CsPbX3/Ag (X = Cl, Br) plasmonic microlasers exhibit quite low thresholds below 10 µJ cm-2. Interestingly, these thresholds can be efficiently modulated through the manipulation of plasmonic resonance and electromagnetic field mode in PeMHs owning various diameters. This strategy not only provides a valuable methodology for the large-scale fabrication of perovskite microstructures but also endorses the potential of all-inorganic perovskite nanostructures as promising candidates for on-chip-integrated light sources.

Architecture for Surface-Emitting Lasers with On-Demand Lasing Wavelength by Nanowire Optical Cavities.

Despite the importance and exciting progress of surface-emitting (SE) semiconductor lasers, we have limited choices of lasing wavelength even today. From an application viewpoint, it is desirable to have an architecture that can allow SE lasing in a wide spectral range, based on the need of applications. Herein, we demonstrate a path for SE lasers with lasing wavelength on demand by exploiting III-nitride nanowire optical cavities formed by low-temperature selective area epitaxy (SAE), combined with fine-tuning of substrate patterns and photonic bands. Moreover, in this study, we focus on the device demonstration in the ultraviolet (UV) spectral range, considering the severe lag in developing SE lasers in the UV wavelength range compared to longer wavelengths, e.g., near-infrared (NIR), as well as the potential applications enabled by UV lasers such as solar blind optical wireless communications. Ultralow threshold wavelength-tunable SE UV lasing is achieved by optical pumping. Moreover, SE UV lasing under direct electric current injection is also achieved. This study not only represents an important step in the journey of SE UV laser development but, more importantly, it lays the ground for SE lasers with lasing wavelength on demand, broadly from NIR to UV.

Two-Dimensional Electron-Hole Plasma in Colloidal Quantum Shells Enables Integrated Lasing Continuously Tunable in the Red Spectrum.

Combining integrated optical platforms with solution-processable materials offers a clear path toward miniaturized and robust light sources, including lasers. A limiting aspect for red-emitting materials remains the drop in efficiency at high excitation density due to non-radiative quenching pathways, such as Auger recombination. Next to this, lasers based on such materials remain ill characterized, leaving questions about their ultimate performance. Here, we show that colloidal quantum shells (QSs) offer a viable solution for a processable material platform to circumvent these issues. We first show that optical gain in QSs is mediated by a 2D plasma state of unbound electron-hole pairs, opposed to bound excitons, which gives rise to broad-band and sizable gain across the full red spectrum with record gain lifetimes and a low threshold. Moreover, at high excitation density, the emission efficiency of the plasma state does not quench, a feat we can attribute to an increased radiative recombination rate. Finally, QSs are integrated on a silicon nitride platform, enabling high spectral contrast, surface emitting, and TE-polarized lasers with ultranarrow beam divergence across the entire red spectrum from a small surface area. Our results indicate QS materials are an excellent materials platform to realize highly performant and compact on-chip light sources.

Room-Temperature Polariton Lasing from CdSe Core-Only Nanoplatelets.

This paper reports how CdSe core-only nanoplatelets (NPLs) coupled with plasmonic Al nanoparticle lattices can exhibit exciton-polariton lasing. By improving a procedure to synthesize monodisperse 4-monolayer CdSe NPLs, we could resolve polariton decay dynamics and pathways. Experiment and theory confirmed that the system is in the strong coupling regime based on anticrossings in the dispersion diagrams and magnitude of the Rabi-splitting values. Notably, polariton lasing is observed only for cavity lattice periodicities that exhibit specific dispersive characteristics that enable polariton accumulation. The threshold of polariton lasing is 25-fold lower than the reported photon lasing values from CdSe NPLs in similar cavity designs. This open-cavity platform offers a simple approach to control exciton polaritons anticipated to benefit quantum information processing, optoelectronics, and chemical reactions.

Continuous-Wave Pumped Monolayer WS2 Lasing for Photonic Barcoding.

Micro/nano photonic barcoding has emerged as a promising technology for information security and anti-counterfeiting applications owing to its high security and robust tamper resistance. However, the practical application of conventional micro/nano photonic barcodes is constrained by limitations in encoding capacity and identification verification (e.g., broad emission bandwidth and the expense of pulsed lasers). Herein, we propose high-capacity photonic barcode labels by leveraging continuous-wave (CW) pumped monolayer tungsten disulfide (WS2) lasing. Large-area, high-quality monolayer WS2 films were grown via a vapor deposition method and coupled with external cavities to construct optically pumped microlasers, thus achieving an excellent CW-pumped lasing with a narrow linewidth (~0.39 nm) and a low threshold (~400 W cm-2) at room temperature. Each pixel within the photonic barcode labels consists of closely packed WS2 microlasers of varying sizes, demonstrating high-density and nonuniform multiple-mode lasing signals that facilitate barcode encoding. Notably, CW operation and narrow-linewidth lasing emission could significantly simplify detection. As proof of concept, a 20-pixel label exhibits a high encoding capacity (2.35 × 10108). This work may promote the advancement of two-dimensional materials micro/nanolasers and offer a promising platform for information encoding and security applications.

Green Light from Red-Emitting Nanocrystals: Broadband, Low-Threshold Lasing from Colloidal Quantum Shells in Optical Nanocavities.

Spherical semiconductor nanoplatelets, known as quantum shells (QSs), have captured significant interest for their strong suppression of Auger recombination, which leads to long multiexciton lifetimes and wide optical gain bandwidth. Yet, the realization of benefits associated with the multiexciton lasing regime using a suitably designed photonic cavity remains elusive. Here, we demonstrate broadly tunable lasing from close-packed films of CdS/CdSe/CdS QSs deposited over nanopillar arrays on Si substrates. Wide spectral tuning of the stimulated emission in QSs with a fixed bandgap value was achieved by engaging single exciton (λX ∼ 634 nm), biexciton (λBX ∼ 627 nm), and multiple exciton (λMX ∼ 615-565 nm) transitions. The ensemble-averaged gain threshold of ∼ 2.6 electron-hole pairs per QS particle and the low photonic cavity fluence threshold of ∼4 µJ/cm2 were attributed to Auger suppression. The tuning of the lasing emission closely aligns with our model predictions achieved by varying the array period while preserving mode confinement and quality (Q) factors. These results mark a notable step toward the development of colloidal nanocrystal lasers.

Unidirectional Lasing from Mirror-Coupled Dielectric Lattices.

This paper reports how a hybrid system composed of transparent dielectric lattices over a metal mirror can produce high-quality lattice resonances for unidirectional lasing. The enhanced electromagnetic fields are concentrated in the cladding of the periodic dielectric structures and away from the metal. Based on a mirror-image model, we reveal that such high-quality lattice resonances are governed by bound states in the continuum resulting from destructive interference. Using hexagonal arrays of titanium dioxide nanoparticles on a silica-coated silver mirror, we observed lattice resonances with quality factors of up to 2750 in the visible regime. With the lattice resonances as optical feedback and dye solution as the gain medium, we demonstrated unidirectional lasing under optical pumping, where the array size was down to 100 µm × 100 µm. Our scheme can be extended to other spectral regimes to simultaneously achieve strongly enhanced surface fields and high quality factors.

Tailoring Single-Mode Random Lasing of Tin Halide Perovskites Integrated in a Vertical Cavity.

The development of random lasing (RL) with predictable and controlled properties is an important step to make these cheap optical sources stable and reliable. However, the design of tailored RL characteristics (emission energy, threshold, number of modes) is only obtained with complex photonic structures, while the simplest optical configurations able to tune the RL are still a challenge. This work demonstrates the tuning of the RL characteristics in spin-coated and inkjet-printed tin-based perovskites integrated into a vertical cavity with low quality factor. When the cavity mode is resonant with the photoluminescence (PL) peak energy, standard vertical lasing is observed. More importantly, single mode RL operation with the lowest threshold and a quality factor as high as 1 000 (twenty times the quality factor of the resonator) is obtained if the cavity mode lies above the PL peak energy due to higher gain. These results can have important technological implications toward the development of low-cost RL sources without chaotic behavior.

Engineering of Solid-State Nanoporous Laser through Dendrimer-Encapsulated Fluorophores.

Dendrimers─nanosized macromolecules that can function as hosts for encapsulation of guest molecules─provide new avenues to engineer gain media for lasing systems. In this context, this study investigates the interplay between the geometric features of a model porous scattering medium, nanoporous anodic alumina (NAA), and the chemical features of a model fluorophore-dendrimer encapsulation system to maximize random lasing. The inner surface of the NAA platforms is functionalized with fluorophore molecules encapsulated within dendrimers via an electrostatic interaction. The resulting solid-state composite structures emit well-resolved, intense random lasing when subjected to optical pumping. By engineering fluorophore-dendrimer and geometric features of scattering medium, we can precisely tune the characteristics of random lasing emissions. It is found that lasing structures with low porosity and thickness functionalized with fluorophore molecules encapsulated in second-generation dendrimers provide the best platforms for lasing generation, resulting in a strongly polarized laser at ∼594 nm that has a high quality-gain product of ∼1588 au, a polarization quality of ∼0.86, and a lasing threshold of ∼0.05 mJ pulse-1. Comparative analysis indicates that dendrimers achieve 2.5 times better random lasing than conventional surfactants due to improved encapsulation and minimization of photobleaching. Our results reveal the importance of the fluorophore encapsulation method and design of scattering media in the engineering of random lasing platforms for applications in optical and optoelectrical systems.

Suppression of Randomness in Electrically Pumped Random Lasing from a ZnO Film-Based Light-Emitting Device on Silicon.

We report on the suppressed randomness in electrically pumped random lasing (RL) from a light-emitting device (LED) based on a metal-insulator-semiconductor (MIS) structure of Au/SiOx (x < 2)/ZnO on a silicon substrate, by means of patterning the light-emitting ZnO polycrystalline film into a number of square blocks separated by streets that are filled with the SiOx insulator. It is found that the RL modes can be remarkably reduced by shrinking the blocks in the absence of interblock optical coupling. Meanwhile, with the imposition of interblock optical coupling by shrinking the streets, the RL modes can be further reduced, and more importantly, the strongest mode wavelength is stabilized around 380 nm, where the ZnO film exhibits the largest optical gain.

High Q-Factor Single-Mode Lasing in Inorganic Perovskite Microcavities with Microfocusing Field Confinement.

The realization of high-Q single-mode lasing on the microscale is significant for the advancement of on-chip integrated light sources. It remains a challenging trade-off between Q-factor enhancement and light-field localization to raise the lasing emission rate. Here, we fabricated a zero-dimensional perovskite microcavity integrated with a nondamage pressed microlens to three-dimensionally tailor the intracavity light field and demonstrated linearly and nonlinearly (two-photon) pumped lasing by this microfocusing configuration. Notably, the microlensing microcavity experimentally achieves a high Q-factor (16700), high polarization (99.6%), and high Purcell factor (11.40) single-mode lasing under high-repetition pulse pumping. Three-dimensional light-field confinement formed by the microlens and plate microcavity simultaneously reduces the mode volume (∼3.66 µm3) and suppresses diffraction and transverse walk-off loss, which induces discretization on energy-momentum dispersions and spatial electromagnetic-field distributions. The Q factor and Purcell factor of our lasing come out on top among most of the reported perovskite microcavities, paving a promising avenue toward further studying electrically driven on-chip microlasers.

High-Performance Multiwavelength GaNAs Single Nanowire Lasers.

In this study, we report a significant enhancement in the performance of GaNAs-based single nanowire lasers through optimization of growth conditions, leading to a lower lasing threshold and higher operation temperatures. Our analysis reveals that these improvements in the laser performance can be attributed to a decrease in the density of localized states within the material. Furthermore, we demonstrate that owing to their excellent nonlinear optical properties, these nanowires support self-frequency conversion of the stimulated emission through second harmonic generation (SHG) and sum-frequency generation (SFG), providing coherent light emission in the cyan-green range. Mode-specific differences in the self-conversion efficiency are revealed and explained by differences in the light extraction efficiency of the converted light caused by the electric field distribution of the fundamental modes. Our work, therefore, facilitates the design and development of multiwavelength coherent light generation and higher-temperature operation of GaNAs nanowire lasers, which will be useful in the fields of optical communications, sensing, and nanophotonics.

Super-Wide Temperature Lasers Spanning from -180 to 240 °C Based on Fully-Polymerized Blue Phase Superstructures.

Blue phase liquid crystal (BPLC) lasers have potential applications in displays, sensors, and anti-counterfeiting fields owing to their outstanding optical properties. However, there remain challenges on lasing below 0 °C, which significantly limits the potential application of BPLC lasers in low-temperature environments. In this work, BPLC lasing below 0 °C is realized for the first time in a super-wide temperature range of -180-240 °C using a well-designed fully-polymerized BPLC system with a narrow line width of 0.0881 nm and a low lasing threshold of 37 nJ pulse-1. This fully-polymerized BPLC both effectively avoids low-temperature random crystallization and has excellent compatibility with dye molecules that significantly widen the lasing temperature range below 0 °C. Besides, the variations of laser peak and threshold are also revealed below 0 °C, that is, redshifted laser wavelength and increased threshold value with decreasing temperature, which contribute to a blue-shifted laser signal and a U-shaped lasing threshold in -180-240 °C. These unique laser behaviors can be ascribed to the temperature-dependent anisotropically microstructural deformation of the BP lattice. This work not only opens a door to the development of low-temperature BPLC lasers but also sets out important insights in the design of novel organic optical devices.

A Rigid Multiple Resonance Thermally Activated Delayed Fluorescence Core Toward Stable Electroluminescence and Lasing.

The investigation of organic light-emitting diodes (OLEDs) and organic laser devices with thermally activated delayed fluorescence (TADF) molecules is emerging due to the potential of harnessing triplets. In this work, a boron/nitrogen multiple-resonance TADF polycyclic framework fusing carbazole units (CzBNPh) was proposed. CzBNPh exhibited a narrowband emission (<30 nm), a unity photoluminescence quantum yield, and a fast radiative rate. Consequently, CzBNPh demonstrated a low distributed feedback (DFB) lasing threshold of 0.68 µJ cm-2 . Furthermore, the stimulated emission zone of CzBNPh was effectively separated from its singlet and triplet absorption, thereby minimizing the singlet-triplet annihilation under long-pulsed excitation ranging from 20 µs to 2.5 ms. Significantly, the enhanced rigid molecular conformation, thermal stability, and photo-stability resulted in improved lasing and electroluminescence stability compared to that of 5,9-diphenyl-5,9-diaza-13b-boranaphtho[3,2,1-de]anthracene (DABNA)-core. These findings indicate the potential of CzBN-core as a promising framework for achieving long-pulsed wave and electrically-pumped lasing in the future.

Two-Color Amplified Spontaneous Emission from Auger-Suppressed Quantum Dots in Liquids.

Colloidal quantum-dot (QD) lasing is normally achieved in close-packed solid-state films, as a high QD volume fraction is required for stimulated emission to outcompete fast Auger decay of optical-gain-active multiexciton states. Here a new type of liquid optical-gain medium is demonstrated, in which compact compositionally-graded QDs (ccg-QDs) that feature strong suppression of Auger decay are liquefied using a small amount of solvent. Transient absorption measurements of ccg-QD liquid suspensions reveal broad-band optical gain spanning a wide spectral range from 560 (green) to 675 nm (red). The gain magnitude is sufficient to realize a two-color amplified spontaneous emission (ASE) at 637 and 594 nm due to the band-edge (1S) and the excited-state (1P) transition, respectively. Importantly, the ASE regime is achieved using quasicontinuous excitation with nanosecond pulses. Furthermore, the ASE is highly stable under prolonged excitation, which stands in contrast to traditional dyes that exhibit strong degradation under identical excitation conditions. These observations point toward a considerable potential of high-density ccg-QD suspensions as liquid, dye-like optical gain media that feature readily achievable spectral tunability and stable operation under intense photoexcitation.

Long-Lived and Bright Biexcitons in Quantum Dots with Parabolic Band Potentials.

Multiple exciton physics in semiconductor nanocrystals play an important role in optoelectronic devices. This work investigates radially alloyed CdZnSe/CdS nanocrystals with suppressed Auger recombination due to the spatial separation of carriers, which also underpins their performance in optical gain and scintillation experiments. Due to suppressed Auger recombination, the biexciton lifetime is greater than 10 ns, much longer than most nanocrystals. The samples show optical gain, amplified spontaneous emission, and lasing at thresholds <2 excitons per particle. They also show broad gain bandwidth (>500 meV) encompassing 4 amplified spontaneous emission bands. Similarly enabled by slowed multiple exciton relaxation, the samples display strong performance in scintillating films under X-ray illumination. The CdZnSe/CdS samples have fast radioluminescence rise (<80 ps) and decay times (<5 ns), light yields up to 6700 photons·MeV-1, and the demonstrated capacity for incorporation into large area films for scintillation imaging.

Random Lasing for Bimodal Imaging and Detection of Tumor.

The interaction of light with biological tissues is an intriguing area of research that has led to the development of numerous techniques and technologies. The randomness inherent in biological tissues can trap light through multiple scattering events and provide optical feedback to generate random lasing emission. The emerging random lasing signals carry sensitive information about the scattering dynamics of the medium, which can help in identifying abnormalities in tissues, while simultaneously functioning as an illumination source for imaging. The early detection and imaging of tumor regions are crucial for the successful treatment of cancer, which is one of the major causes of mortality worldwide. In this paper, a bimodal spectroscopic and imaging system, capable of identifying and imaging tumor polyps as small as 1 mm2, is proposed and illustrated using a phantom sample for the early diagnosis of tumor growth. The far-field imaging capabilities of the developed system can enable non-contact in vivo inspections. The integration of random lasing principles with sensing and imaging modalities has the potential to provide an efficient, minimally invasive, and cost-effective means of early detection and treatment of various diseases, including cancer.

Electrically Tunable Two-Color Cholesteric Laser.

Two-color lasing emission from an asymmetric structure, consisting of two dye-doped cholesteric liquid crystal (DD-CLC) layers separated by a transparent interlayer, is demonstrated. The DD-CLC mixtures have different reflection bands with long-wavelength band edges located at the green and red wavelengths of the visible spectrum, respectively. For the laser action, the CLC hosts provide the feedback, and the fluorescent laser dyes represent the active medium. When the stacked structure is optically pumped above the threshold, two simultaneous laser lines separated by 123 nm are observed at the long-wavelength band edges of the DD-CLC mixtures. The influence of an electric field on lasing behavior is also analyzed and discussed in terms of the reflection spectrum and laser action. The results show a reversible tuning of the reflection band, accompanied by a modification of the lasing characteristics under the application of an external field. Above a specific threshold voltage, one of the emission lines is suppressed and the other is conserved. With a further increase in the voltage, both laser emissions are entirely inhibited. The investigated structure demonstrates a simple technique to obtain an electrically tunable multi-wavelength laser, which might pave the way for a new generation of organic laser sources.

Lasing Effect in Symmetrical van der Waals Heterostructured Metasurfaces Due to Lattice-Induced Multipole Coupling.

New practical ways to reach the lasing effect in symmetrical metasurfaces have been developed and theoretically demonstrated. Our approach is based on excitation of the resonance of an octupole quasi-trapped mode (OQTM) in heterostructured symmetrical metasurfaces composed of monolithic disk-shaped van der Waals meta-atoms featured by thin photoluminescent layers and placed on a substrate. We revealed that the coincidence of the photoluminescence spectrum maximum of these layers with the wavelength of high-quality OQTM resonance leads to the lasing effect. Based on the solution of laser rate equations and direct full-wave simulation, it was shown that lasing is normally oriented to the metasurface plane and occurs from the entire area of metasurface consisting of MoS2/hBN/MoTe2 disks with line width of generated emission of only about 1.4 nm near the wavelength 1140 nm. This opens up new practical possibilities for creating surface emitting laser devices in subwavelength material systems.