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Lead halide perovskite nanocrystals (NCs) with bright luminescence and broad spectral tunability are good candidates as smart probes for bioimaging, but suffer from hydrolysis even when exposed to atmosphere moisture. In this paper, a strategy is demonstrated by embedding CsPbX3 (X = Cl, Br, I) NCs into microhemispheres (MHSs) of polystyrene matrix to prepare “water‐resistant” NCs@MHSs hybrids as multicolor multiplexed optical coding agents. First, a facile room‐temperature solution self‐assembly approach to highly luminescent colloidal CsPbX3 NCs is developed by injecting a stock solution of CsX⋅PbX2 in N,N‐dimethylformamide into dichloromethane. Polyvinyl pyrrolidone (PVP) is chosen as the capping ligand, which is physically adsorbed and wrapped on the surface of perovskite NCs to form a protective layer. The PVP protective layer not only leads to composition‐tunable CsPbX3 NCs with high quantum yields and narrow emission linewidths of 12–34 nm but also acts as an interfacial layer, making perovskite NCs compatible with polystyrene polymers and facilitating the next step to embed CsPbX3 NCs into polymer MHSs. CsPbX3 NCs@MHSs are demonstrated as multicolor luminescence probes in live cells with high stability and nontoxicity. Using ten intensity levels and seven‐color NCs@MHSs that show non‐overlapping spectra, it will be possible to individually tag about ten million cells.

In the last 10 years, nanomaterials based on small organic molecules have attracted increasing attention. Such materials have unique optical and electronic properties, which could lead to new applications in nanoscale devices. Zero-dimensional (0D) organic nanoparticles with amorphous structures have been widely studied; however, the systematic investigation of crystalline one-dimensional (1D) organic nanostructures has only emerged in recent years. Researchers have used inorganic 1D nanomaterials, such as wires, tubes, and belts, as building blocks in optoelectronic nanodevices. We expect that their organic counterparts will also play an important role in this field. Because organic nanomaterials are composed of molecular units with weaker intermolecular interactions, they allow for higher structural tunability, reactivity, and processability. In addition, organic materials usually possess higher luminescence efficiency and can be grown on almost any solid substrate. In this Account, we describe recent progress in our group toward the construction of organic 1D nanomaterials and studies of their unique optical and electronic properties. First, we introduce the techniques for synthesizing 1D organic nanostructures. Because this strategy is both facile and reliable, liquid phase synthesis is most commonly used. More importantly, this method allows researchers to produce composite materials, including core/sheath and uniformly doped structures, which allow to investigate the interactions between different components in the nanomaterials, including fluorescent resonance energy transfer and photoinduced electron transfer. Physical vapor deposition allows for the synthesis of organic 1D nanomaterials with high crystallinity. Nanomaterials produced with this method offer improved charge transport properties and better optoelectronic performance in areas including multicolor emission, tunable emission, optical waveguide, and lasing. Although inorganic nanomaterials have developed rapidly, our findings highlight the importance of organic compounds as components of novel 1D nanomaterials.

This article presents a comprehensive review of recent progress of research dedicated to low‐dimensional nanomaterials constructed from functional low‐molecular‐weight organic compounds, whose optoelectronic properties are fundamentally different from those of their inorganic counterparts. After introducing the development of inorganic and organic macromolecular nanomaterials, we begin with a general review of the construction strategies for achieving both zero‐dimensional (0D) and one‐dimensional (1D) nanostructures from small organic functional molecules. We then provide an overview of the unique optoelectronic properties induced by molecular aggregation in the nanostructures. Special emphasis is put on the luminescent properties that are different from those of the corresponding bulk materials, such as aggregation‐induced enhanced emission, fluorescence narrowing, multicolor emission, and tunable and switchable emissions from doped nanostructures. We conclude with a summary and our personal view of the direction of future development of organic opto‐functional nanomaterials and devices.

Fabrication of semiconductor nanowire laser arrays is very challenging, owing to difficulties in direct monolithic growth and patterning of III-V semiconductors on silicon substrates. Recently, methylammonium lead halide perovskites (MAPbX, X = Cl, Br, I) have emerged as an important class of high-performance solution-processed optoelectronic materials. Here, we combined the "top-down" fabricated polydimethylsiloxane rectangular groove template (RGT) with the "bottom-up" solution self-assembly together to prepare large-scale perovskite nanowire (PNW) arrays. The template confinement effect led to the directional growth of MAPbX along RGTs into PNWs. We achieved precise control over not only the dimensions of individual PNWs (width 460-2500 nm; height 80-1000 nm, and length 10-50 μm) but also the interwire distances. Well-defined dimensions and uniform geometries enabled individual PNWs to function as high-quality Fabry-Perot nanolasers with almost identical optical modes and similarly low-lasing thresholds, allowing them to ignite simultaneously as a laser array. Optical tests demonstrated that PNW laser arrays exhibit good photostabillity with an operation duration exceeding 4 × 10 laser pulses. Precise placement of PNW arrays at specific locations makes our method highly compatible with lithographic techniques, which are important for integrating PNW electronic and photonic circuits.

Charge-transfer (CT) interactions between donor (D) and acceptor (A) groups, as well as CT exciton dynamics, play important roles in optoelectronic devices, such as organic solar cells, photodetectors, and light-emitting sources, which are not yet well understood. In this contribution, the self-assembly behavior, molecular stacking structure, CT interactions, density functional theory (DFT) calculations, and corresponding physicochemical properties of two similar halogen-bonded co-crystals are comprehensively investigated and compared, to construct an "assembly-structure-CT-property" relationship. Bpe-IFB wire-like crystals (where Bpe = 1,2-bis(4-pyridyl)ethylene and IFB = 1,3,5-trifluoro-2,4,6-triiodobenzene), packed in a segregated stacking form with CT ground and excited states, are measured to be quasi-one-dimensional (1D) semiconductors and show strong violet-blue photoluminescence (PL) from the lowest CT1 excitons (ΦPL = 26.1%), which can be confined and propagate oppositely along the 1D axial direction. In comparison, Bpe-F4DIB block-like crystals (F4DIB = 1,4-diiodotetrafluorobenzene), packed in a mixed stacking form without CT interactions, are determined to be insulators and exhibit unique white light emission and two-dimensional optical waveguide property. Surprisingly, it seems that the intrinsic spectroscopic states of Bpe and F4DIB do not change after co-crystallization, which is also confirmed by theoretical calculations, thus offering a new design principle for white light emitting materials. More importantly, we show that the CT interactions in co-crystals are related to their molecular packing and can be triggered or suppressed by crystal engineering, which eventually leads to distinct optoelectronic properties. These results help us to rationally control the CT interactions in organic D-A systems by tuning the molecular stacking, toward the development of a fantastic "optoelectronic world".

3D organic-inorganic hybrid perovskites have featured high gain coefficients through the electron-hole plasma stimulated emission mechanism, while their 2D counterparts of Ruddlesden-Popper perovskites (RPPs) exhibit strongly bound electron-hole pairs (excitons) at room temperature. High-performance solar cells and light-emitting diodes (LEDs) are reported based on 2D RPPs, whereas light-amplification devices remain largely unexplored. Here, it is demonstrated that ultrafast energy transfer along cascade quantum well (QW) structures in 2D RPPs concentrates photogenerated carriers on the lowest-bandgap QW state, at which population inversion can be readily established enabling room-temperature amplified spontaneous emission and lasing. Gain coefficients measured for 2D RPP thin-films (≈100 nm in thickness) are found about at least four times larger than those for their 3D counterparts. High-density large-area microring arrays of 2D RPPs are fabricated as whispering-gallery-mode lasers, which exhibit high quality factor (Q ≈ 2600), identical optical modes, and similarly low lasing thresholds, allowing them to be ignited simultaneously as a laser array. The findings reveal that 2D RPPs are excellent solution-processed gain materials potentially for achieving electrically driven lasers and ideally for on-chip integration of nanophotonics.