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1.
ACS Nano ; 17(3): 2661-2668, 2023 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-36648200

RESUMEN

Circularly polarized luminescence (CPL) is one of the critical chiroptical properties for chiral nanomaterials, which exhibit wide potential applications in many research fields. However, it remains a big challenge for real application, limited by their small luminescence dissymmetry factor or low emission intensity. Here, an upconverted near-infrared circularly polarized luminescence (UC-NIR-CPL) system is constructed based on the chiroptical property of chiral liquid crystals, embedding with the lanthanide-doped upconversion nanoparticles. More importantly, a strategy for improving the overall performance of UC-NIR-CPL was proposed and realized by taking advantage of the "dual-band-edge enhancement effect", wherein the glum value was amplified, while the NIR emission intensity showed dual enhancement and the threshold of excitation was decreased. Based on the improved overall performance of the UC-NIR-CPL, which can be used as a distinctive covert light, a kind of photonic barcode with multiple encryptions was realized. These findings will upgrade the level of information encryption through improving the overall performance of CPL-active materials.

2.
ACS Nano ; 15(2): 2753-2761, 2021 Feb 23.
Artículo en Inglés | MEDLINE | ID: mdl-33559470

RESUMEN

Enormous attention has been paid to upconverted circularly polarized luminescence (UC-CPL). However, so far, chiral species are still needed in UC-CPL materials, either through the covalent or noncovalent bond. Here, we report a general supramolecular coassembly approach for the fabrication of UC-CPL systems from completely achiral components. We have found that an achiral C3-symmetric molecule could form a chiral nanohelix through symmetry breaking, which could serve as a general helical platform to endow achiral guests with induced chirality and CPL activity. Two different photon upconversion systems, namely, triplet-triplet annihilation photon upconversion (TTA-UC) donor/acceptor pairs and inorganic lanthanide upconversion nanoparticles (UCNPs), are selected. When these two systems coassembled with the chiral nanohelix made from an achiral C3-symmetric molecule, hybrid nanohelix structures formed and UC-CPL activity was induced. Through such an approach, we demonstrated that the fabrication of the UC-CPL materials does not require any chiral molecules. Moreover, we have shown that the polarization of UC-CPL can be tuned by the helicity of the nanohelix, which could be controlled through the seeded vortex. Our work provides a general approach for designing tunable UC-CPL materials from completely achiral motifs, which largely expands the research scope of the CPL materials.

3.
Adv Mater ; 32(24): e2000820, 2020 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-32378267

RESUMEN

Circularly polarized luminescent materials with high dissymmetry factor (glum ) have been attracting increasing attention due to their distinctive photonic properties. In this work, by incorporating upconversion nanoparticles (UCNPs) and CsPbBr3 perovskite nanocrystals (PKNCs) into a chiral nematic liquid crystal (N*LC), enhanced upconverted circularly polarized luminescence (UC-CPL) based on a radiative energy transfer (RET) process from UCNPs to CsPbBr3 PKNCs is successfully implemented. By locating the emission peak of CsPbBr3 PKNCs at the center of the photonic bandgap of N*LC, the maximum glum value of UC-CPL can be amplified to an extremely large value of 1.1. Meanwhile, upconverted emission of UCNPs can be significantly enhanced due to the band edge enhancement effect of the N*LC, subsequently enhancing the emission of the CsPbBr3 PKNCs through the RET process. In addition, an applied electric field can switch the upconverted emission of the UCNPs, as well as the RET process, enabling an electric-field-controlled UC-CPL switch.

4.
ACS Appl Mater Interfaces ; 11(26): 23512-23519, 2019 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-31252503

RESUMEN

Integrating chromophores into chiral photonic crystals to fabricate materials that exhibit circularly polarized luminescence (CPL) is promising as this method allows efficient manipulation of the spontaneous emission within photonic bandgaps (PBGs). However, tuning the wavelength of CPL and the dissymmetry factor ( glum) in a convenient and accurate manner remains a significant challenge. Here, right-handed, tunable upconverted CPL (UC-CPL) emission was achieved by integrating multiple emissive, upconverting nanoparticles into cellulose nanocrystal based chiral photonic films that had tunable PBGs. Glycerol was used to tune the PBGs of the chiral photonic films, which yielded tunable UC-CPL emission at 450 and 620 nm with a tailored glum. Moreover, humidity responsive UC-CPL at blue wavelength was obtained from glycerol-composite photonic film, with a glum that ranged from -0.156 to -0.033. It was possible because the PBG and chirality of photonic composite was responded to the relative humidity. This work gives valuable insight into tunable and stimuli-responsive CPL photonic systems.

5.
ACS Nano ; 13(3): 2804-2811, 2019 Mar 26.
Artículo en Inglés | MEDLINE | ID: mdl-30688444

RESUMEN

In this work, lanthanide-doped upconversion nanoparticles (UCNPs) showing upconverted circularly polarized luminescence were demonstrated in an organic-inorganic co-assembled system. Achiral UCNPs (NaYF4:Yb/Er or NaYF4:Yb/Tm) can be encapsulated into chiral helical nanotubes through the procedure of co-gelation. These co-gel systems display intense upconverted circularly polarized luminescence (UC-CPL) ranging from ultraviolet (UV, 300 nm) to near-infrared (NIR, 850 nm) wavelength. In addition, the UV part of UC-CPL can be used to initiate the enantioselective polymerization of diacetylene.

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