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.

Recent progress of exciton transport in two-dimensional semiconductors.

Spatial manipulation of excitonic quasiparticles, such as neutral excitons, charged excitons, and interlayer excitons, in two-dimensional semiconductors offers unique capabilities for a broad range of optoelectronic applications, encompassing photovoltaics, exciton-integrated circuits, and quantum light-emitting systems. Nonetheless, their practical implementation is significantly restricted by the absence of electrical controllability for neutral excitons, short lifetime of charged excitons, and low exciton funneling efficiency at room temperature, which remain a challenge in exciton transport. In this comprehensive review, we present the latest advancements in controlling exciton currents by harnessing the advanced techniques and the unique properties of various excitonic quasiparticles. We primarily focus on four distinct control parameters inducing the exciton current: electric fields, strain gradients, surface plasmon polaritons, and photonic cavities. For each approach, the underlying principles are introduced in conjunction with its progression through recent studies, gradually expanding their accessibility, efficiency, and functionality. Finally, we outline the prevailing challenges to fully harness the potential of excitonic quasiparticles and implement practical exciton-based optoelectronic devices.

Single Quantum Dot Selection and Tailor-Made Photonic Device Integration using a Nanoscale-Focus Pinspot.

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

Helmholtz Resonator Applied to Nanocrystal-Based Infrared Sensing.

While the integration of nanocrystals as an active medium for optoelectronic devices progresses, light management strategies are becoming required. Over recent years, several photonic structures (plasmons, cavities, mirrors, etc.) have been coupled to nanocrystal films to shape the absorption spectrum, tune the directionality, and so on. Here, we explore a photonic equivalent of the acoustic Helmholtz resonator and propose a design that can easily be fabricated. This geometry combines a strong electromagnetic field magnification and a narrow channel width compatible with efficient charge conduction despite hopping conduction. At 80 K, the device reaches a responsivity above 1 A·W-1 and a detectivity above 1011 Jones (3 µm cutoff) while offering a significantly faster time-response than vertical geometry diodes.

Data-Enhanced Deep Greedy Optimization Algorithm for the On-Demand Inverse Design of TMDC-Cavity Heterojunctions.

A data-enhanced deep greedy optimization (DEDGO) algorithm is proposed to achieve the efficient and on-demand inverse design of multiple transition metal dichalcogenides (TMDC)-photonic cavity-integrated heterojunctions operating in the strong coupling regime. Precisely, five types of photonic cavities with different geometrical parameters are employed to alter the optical properties of monolayer TMDC, aiming at discovering new and intriguing physics associated with the strong coupling effect. Notably, the traditional rigorous coupled wave analysis (RCWA) approach is utilized to generate a relatively small training dataset for the DEDGO algorithm. Importantly, one remarkable feature of DEDGO is the integration the decision theory of reinforcement learning, which remedies the deficiencies of previous research that focused more on modeling over decision making, increasing the success rate of inverse prediction. Specifically, an iterative optimization strategy, namely, deep greedy optimization, is implemented to improve the performance. In addition, a data enhancement method is also employed in DEDGO to address the dependence on a large amount of training data. The accuracy and effectiveness of the DEDGO algorithm are confirmed to be much higher than those of the random forest algorithm and deep neural network, making possible the replacement of the time-consuming conventional scanning optimization method with the DEDGO algorithm. This research thoroughly describes the universality, interpretability, and excellent performance of the DEDGO algorithm in exploring the underlying physics of TMDC-cavity heterojunctions, laying the foundations for the on-demand inverse design of low-dimensional material-based nano-devices.

High-Order Photonic Cavity Modes Enabled 3D Structural Colors.

It remains a challenge to directly print arbitrary three-dimensional shapes that exhibit structural colors at the micrometer scale. Woodpile photonic crystals (WPCs) fabricated via two-photon lithography (TPL) are elementary building blocks to produce 3D geometries that generate structural colors due to their ability to exhibit either omnidirectional or anisotropic photonic stop bands. However, existing approaches produce structural colors on WPCs when illuminating from the top, requiring print resolutions beyond the limit of commercial TPL, which necessitates postprocessing techniques. Here, we devised a strategy to support high-order photonic cavity modes upon side illumination on WPCs that surprisingly generate prominent reflectance peaks in the visible spectrum. Based on that, we demonstrate one-step printing of 3D photonic structural colors without requiring postprocessing or subwavelength features. Vivid colors with reflectance peaks exhibiting a full width at half-maximum of ∼25 nm, a maximum reflectance of 50%, a gamut of ∼85% of sRGB, and large viewing angles were achieved. In addition, we also demonstrated voxel-level manipulation and control of colors in arbitrary-shaped 3D objects constituted with WPCs as unit cells, which has potential for applications in dynamic color displays, colorimetric sensing, anti-counterfeiting, and light-matter interaction platforms.

Elucidating Energy Pathways through Simultaneous Measurement of Absorption and Transmission in a Coupled Plasmonic-Photonic Cavity.

Control of light-matter interactions is central to numerous advances in quantum communication, information, and sensing. The relative ease with which interactions can be tailored in coupled plasmonic-photonic systems makes them ideal candidates for investigation. To exert control over the interaction between photons and plasmons, it is essential to identify the underlying energy pathways which influence the system's dynamics and determine the critical system parameters, such as the coupling strength and dissipation rates. However, in coupled systems which dissipate energy through multiple competing pathways, simultaneously resolving all parameters from a single experiment is challenging as typical observables such as absorption and scattering each probe only a particular path. In this work, we simultaneously measure both photothermal absorption and two-sided optical transmission in a coupled plasmonic-photonic resonator consisting of plasmonic gold nanorods deposited on a toroidal whispering-gallery-mode optical microresonator. We then present an analytical model which predicts and explains the distinct line shapes observed and quantifies the contribution of each system parameter. By combining this model with experiment, we extract all system parameters with a dynamic range spanning 9 orders of magnitude. Our combined approach provides a full description of plasmonic-photonic energy dynamics in a weakly coupled optical system, a necessary step for future applications that rely on tunability of dissipation and coupling.

Coupling localized plasmonic and photonic modes tailors and boosts ultrafast light modulation by gold nanoparticles.

Plasmonic nanoparticles offer a broad range of functionalities, owing to their ability to amplify light in the near-field or convert it into heat. However, their ultrafast nonlinear optical response remains too low to envisage all-optical high-rate photonic processing applications. Here, we tackle this challenge by coupling the localized plasmon mode in gold nanoparticles with a localized photonic mode in a 1D resonant cavity. Despite the nonradiative losses, we demonstrate that a strong, reversible, and ultrafast optical modulation can be achieved. By using a light pumping fluence of less than 1 mJ cm(-2), a change of signal transmittance of more than 100% is generated within a few picosecond time scale. The nanoparticle transient optical response is enhanced by a factor of 30 to 40 while its spectral profile is strongly sharpened. The large nonlinear response of such plasmonic cavities could open new opportunities for ultrafast light processing at the nanoscale.