Efficient occlusion of guest nanoparticles into host single crystals opens up a straightforward and versatile way to construct functional crystalline nanocomposites. This new technique has attracted increasing research interest because it enables the composition, structure and property of the resulting nanocomposites to be well-controlled. In this review article, we aim to provide a comprehensive summary of nanoparticle occlusion within inorganic crystals. First, we summarize recently-developed strategies for the occlusion of various colloidal particles (e.g., diblock copolymer nanoparticles, polymer-modified inorganic nanoparticles, oil droplets, etc.) within host crystals (e.g., CaCO3 , ZnO or ZIF-8). Second, new results pertaining to spatially-controlled occlusion and the physical mechanism of nanoparticle occlusion are briefly discussed. Finally, we highlight the physicochemical properties and potential applications of various functional nanocomposite crystals constructed via nanoparticle occlusion and we also offer our perspective on the likely future for this research topic. This article is protected by copyright. All rights reserved.

Polymer-Inorganic Crystalline Nanocomposite Materials via Nanoparticle Occlusion.

Inclusion of dyes is efficient for regulating the performance of nonlinear optical (NLO) crystals. The commonly seen anisotropic dyeing of solution-grown crystals, promoted by specific dye–facet interactions, limits their optical applicability. Here, two classic dyes, methylene blue (MLB) and aniline blue (ALB), are each isotropic occluded within single crystals of the widely used NLO material, potassium dihydrogen phosphate (KDP). MLB and ALB, which only partially stain solution-grown KDP crystals, are incorporated isotropically into gel-grown crystals with unspoiled single-crystalline lattices. During the gel crystallization, dye molecules bind to the gel-networks, and both become incorporated into the crystals, leading to efficient isotropic dyeing. Furthermore, enrichment of dye molecules from gels into crystals is achieved in the case of ALB because the ALB molecules bind strongly and accumulate onto the gel-networks. Hence, this work provides a generally applicable strategy to facilitate the isotropic dyeing of single crystals and further optimization of crystal properties. 

Isotropically Dyed Single Crystals Produced via Gel-Incorporation

High-performance X-ray detectors are usually based on single crystals, due to the long-range ordering and hence outstanding electronic properties. On the other hand, bulk heterojunctions (BHJs) that can effectively enhance photogenerated exciton dissociation are widely used for photodetectors. The benefits of both spur investigation into how to combine these two strategies to enhance X-ray detection. Here, TiO2 networks are incorporated into PbI2 crystals to form interpenetrating type II heterojunctions, namely BHJs. These BHJs exhibit long-range ordering in molecular packing similar to that of single crystals. Compared with single crystals, the long-range ordered BHJs facilitate the separation of photogenerated electrons and holes to inhibit recombination, extend the mobility lifetime product by 6.4 times, and consequently improve X-ray sensitivity by 5.8 times. Hence, this work provides a new strategy using gel-grown crystals to fabricate high-performance X-ray detectors as well as a new platform for studying the behavior of X-ray-generated carriers in BHJs with long-range ordering.

PbI2-TiO2 Bulk Heterojunctions with Long-Range Ordering for X-ray Detectors.

The growth of acetaminophen polymorphic crystals and the solution-mediated phase transition from trihydrate to form II in agarose gel were investigated. The form II crystals grown in gels, presumably because of the agarose content, dissolved less rapidly at high temperatures and were more stable than in water. The trihydrate crystals in the gel were also expected to be stabilized by containing agarose, but in fact the fine morphology resulted in reduced stability. The solution-mediated phase transition from trihydrate to form II via form II seeding took longer in the gel because the gel slowed down the dissolution of the trihydrate by hindering the dispersion of the form II seeds and delayed the growth of form II by reducing the diffusion rate of the molecules dissolved from the trihydrate. Delays in solution-mediated phase transition and changes in stability for crystals grown in gels indicate the effectiveness of gels in controlling polymorphisms in pharmaceutical compounds.

Growth of Acetaminophen Polymorphic Crystals and Solution-Mediated Phase Transition from Trihydrate to Form II in Agarose Gel

Incorporating polymers within a single-crystal: From heterogeneous structure to multiple functions

Single crystals have been shown to incorporate guest materials (e.g., gel networks and functional particles) and the incorporated materials endow the crystal hosts with non-intrinsic properties. The acquisition of the non-intrinsic crystal properties impels us to diversify the incorporated guest materials and thus to spread the potential applications of single-crystalline materials. Here, fluorescent NIPAM-based microgels have been selected as the guest materials to be incorporated into the crystal hosts. In the presence of microgels, calcite crystallize from either solution or gel media have been examined. Solution-grown crystals exclude the microgels, while two gel-grown methods have proved effective for incorporating these microgels inside calcite single crystals. On one hand, an additional macroscopic agarose gel-network is introduced to trap the microgels. Crystallization in the agarose gel leads to incorporation of agarose gel-network together with the trapped microgels. The microgel concentration in the crystal reaches 33 mg/mL. On the other hand, dispersions of microgels are concentrated to about 352 mg/mL and the microgels aggregate into non-flowing macroscopic gels (termed as macrogels). Crystallization in a macrogel results in its incorporation. By showing the incorporation of microgels through physical entrapment, this work provides a new platform to functionalize single crystals by the microgels.

Incorporation of fluorescent microgels inside calcite single crystals

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Incorporation of fluorescent microgels inside calcite single crystals