Hybrid organic/inorganic lead halide perovskites (LHPs) have recently emerged as extremely promising photonic materials. However, the exploration of their optical nonlinearities has been mainly focused on the third- and higher-order nonlinear optical (NLO) effects. Strong second-order NLO responses are hardly expected from ordinary LHPs due to their intrinsic centrosymmetric structures, but are highly desirable for advancing their applications in the next generation integrated photonic circuits. Here we demonstrate the fabrication of a novel noncentrosymmetric LHP material by introducing chiral amines as the organic component. The nanowires grown from this new LHP material crystallize in a noncentrosymmetric P1 space group and demonstrate highly efficient second harmonic generation (SHG) with high polarization ratios and chiroptical NLO effects. Such a chiral perovskite skeleton could provide a new platform for future engineering of optoelectronic functionalities of hybrid perovskite materials.

Conjugated organic molecules are interesting materials because of their structures and their electronic, electrical, magnetic, optical, biological, and chemical properties. However, researchers continue to face great challenges in the construction of well-defined organic compounds that aggregate into larger molecular materials such as nanowires, tubes, rods, particles, walls, films, and other structural arrays. Such nanoscale materials could serve as direct device components. In this Account, we describe our recent progress in the construction of nanostructures formed through the aggregation of organic conjugated molecules and in the investigation of the optical, electrical, and electronic properties that depend on the size or morphology of these nanostructures. We have designed and synthesized functional conjugated organic molecules with structural features that favor assembly into aggregate nanostructures via weak intermolecular interactions. These large-area ordered molecular aggregate nanostructures are based on a variety of simpler structures such as fullerenes, perylenes, anthracenes, porphyrins, polydiacetylenes, and their derivatives. We have developed new methods to construct these larger structures including organic vapor-solid phase reaction, natural growth, association via self-polymerization and self-organization, and a combination of self-assembly and electrochemical growth. These methods are both facile and reliable, allowing us to produce ordered and aligned aggregate nanostructures, such as large-area arrays of nanowires, nanorods, and nanotubes. In addition, we can synthesize nanoscale materials with controlled properties. Large-area ordered aggregate nanostructures exhibit interesting electrical, optical, and optoelectronic properties. We also describe the preparation of large-area aggregate nanostructures of charge transfer (CT) complexes using an organic solid-phase reaction technique. By this process, we can finely control the morphologies and sizes of the organic nanostructures on wires, tubes, and rods. Through field emission studies, we demonstrate that the films made from arrays of CT complexes are a new kind of cathode materials, and we systematically investigate the effects of size and morphology on electrical properties. Low-dimension organic/inorganic hybrid nanostructures can be used to produce new classes of organic/inorganic solid materials with properties that are not observed in either the individual nanosize components or the larger bulk materials. We developed the combined self-assembly and templating technique to construct various nanostructured arrays of organic and inorganic semiconductors. The combination of hybrid aggregate nanostructures displays distinct optical and electrical properties compared with their individual components. Such hybrid structures show promise for applications in electronics, optics, photovoltaic cells, and biology. In this Account, we aim to provide an intuition for understanding the structure-function relationships in organic molecular materials....

Halide perovskites provide an ideal platform for engineering highly promising semiconductor materials for a wide range of applications in optoelectronic devices, such as photovoltaics, light‐emitting diodes, photodetectors, and lasers. More recently, increasing research efforts have been directed toward the nonlinear optical properties of halide perovskites because of their unique chemical and electronic properties, which are of crucial importance for advancing their applications in next‐generation photonic devices. Here, the current state of the art in the field of nonlinear optics (NLO) in halide perovskite materials is reviewed. Halide perovskites are categorized into hybrid organic/inorganic and pure inorganic ones, and their second‐, third‐, and higher‐order NLO properties are summarized. The performance of halide perovskite materials in NLO devices such as upconversion lasers and ultrafast laser modulators is analyzed. Several potential perspectives and research directions of these promising materials for nonlinear optics are presented.

While highly desired in integrated optical circuits, multiresponsive and tunable nonlinear optical (NLO) active 1D (sub)wavelength scale superstructures from organic materials are rarely reported due to the strong tendency of organic molecules to self-assembly in centrosymmetric modes. Here a solution-processed assembly approach is reported to generate non-centrosymmetric single-crystalline organic microfibers with a cumulative dipole moment for anisotropic combined second- and third-order NLO.

Graphdiyne (GDY), a newly emerging 2D carbon allotrope, has been widely explored in various fields owing to its outstanding electronic properties such as the intrinsic bandgap and high carrier mobility. Herein, GDY‐based photoelectrochemical‐type photodetection is realized by spin‐coating ultrathin GDY nanosheets onto flexible poly(ethylene terephthalate) (PET) substrates. The GDY‐based photodetectors (PDs) demonstrate excellent photo‐responsive behaviors with high photocurrent (Pph, 5.98 µA cm‐2), photoresponsivity (Rph, 1086.96 µA W‐1), detectivity (7.31 × 1010 Jones), and excellent long‐term stability (more than 1 month). More importantly, the PDs maintain an excellent Pph after 1000 cycles of bending (4.45 µA cm‐2) and twisting (3.85 µA cm‐2), thanks to the great flexibility of the GDY structure that is compatible with the flexible PET substrate. Density functional theory (DFT) calculations are adopted to explore the electronic characteristics of GDY, which provides evidence for the performance enhancement of GDY in alkaline electrolyte. In this way, the GDY‐based flexible PDs can enrich the fundamental study of GDY and pave the way for the exploration of GDY heterojunction‐based photodetection.

A novel route has been developed for surfactant-free synthesis of highly fluorescent gold quantum dots (GQDs) in N,N-dimethylformamide (DMF). The as-prepared GQDs show instinctive fluorescence and good solubility in water. The formation mechanism and functionalization of GQDs were investigated by UV-vis spectra, fluorescence excitation and emission spectra, mass spectra, and TEM observation. Ligand-dependent optical properties of functionalized GQDs were found to be dramatically different. The approach provides a facile method of functionalization of bare GQDs for further applications, such as fluorescent biolabels, energy transfer units, and light-emitting devices.

Graphdiyne is a new carbon allotrope comprising sp‐ and sp2‐hybridized carbon atoms arranged in a 2D layered structure. In this contribution, 2D graphdiyne is demonstrated to exhibit a strong light–matter interaction with high stability to achieve a broadband Kerr nonlinear optical response, which is useful for nonreciprocal light propagation in passive photonic diodes. Furthermore, advantage of the unique Kerr nonlinearity of 2D graphdiyne is taken and a nonreciprocal light propagation device is proposed based on the novel similarity comparison method. Graphdiyne has demonstrated a large nonlinear refractive index in the order of ≈10−5 cm2 W−1, comparing favorably to that of graphene. Based on the strong Kerr nonlinearity of 2D graphdiyne, a nonlinear photonic diode that breaks time‐reversal symmetry is demonstrated to realize the unidirectional excitation of Kerr nonlinearity, which can be regarded as a significant demonstration of a graphdiyne‐based prototypical application in nonlinear photonics and might suggest an important step toward versatile graphdiyne‐based advanced passive photonics devices in the future.

We report a novel approach to modify the second order nonlinear optical (NLO) susceptibility of organic nanofiber crystals by hybridization with the optical modes of microcavities in the strong coupling regime. The wavelength dependence of the SHG efficiency displays two intense peaks corresponding to the so-formed light-matter hybrid states. Our results demonstrate an enhancement of the resonant SHG efficiency of the lower polariton by 2 orders of magnitude for the collectively coupled molecules as compared to that of the same material outside the microcavity. This study is a proof of principle that opens a new direction for NLO of organic materials in subwavelength resonators.