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1.
J Phys Chem Lett ; 11(9): 3582-3588, 2020 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-32302138

RESUMO

Organic guest/host systems with long persistent luminescence benefiting from the formation of a long-lived charge-separated state have recently been demonstrated. However, the photogeneration mechanism of such key charge-separated states remains elusive. Here, we report the identification of intermediate triplet states with mixed local excitation and charge-transfer character that connect the initial photoexcited singlet states and the long-lived charge-separated states. Using time-resolved optical spectroscopy, we observe the intersystem crossing from photoexcited singlet charge-transfer states to triplet intermediate states on a time scale of ∼52 ns. Temperature-dependent measurements reveal that the long-lived triplet intermediate states ensure a relatively high efficiency of diffusion-driven charge separation to form the charge-separated state responsible for LPL emission. The findings in this work provide a rationale for the development of new LPL materials that may also improve our understanding of the mechanism of photon-to-charge conversion in many organic optoelectronic devices.

2.
Adv Mater ; 31(44): e1904319, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31532872

RESUMO

Compared to efficient green and near-infrared light-emitting diodes (LEDs), less progress has been made on deep-blue perovskite LEDs. They suffer from inefficient domain [various number of PbX6 - layers (n)] control, resulting in a series of unfavorable issues such as unstable color, multipeak profile, and poor fluorescence yield. Here, a strategy involving a delicate spacer modulation for quasi-2D perovskite films via an introduction of aromatic polyamine molecules into the perovskite precursor is reported. With low-dimensional component engineering, the n1 domain, which shows nonradiative recombination and retarded exciton transfer, is significantly suppressed. Also, the n3 domain, which represents the population of emission species, is remarkably increased. The optimized quasi-2D perovskite film presents blue emission from the n3 domain (peak at 465 nm) with a photoluminescence quantum yield (PLQY) as high as 77%. It enables the corresponding perovskite LEDs to deliver stable deep-blue emission (CIE (0.145, 0.05)) with an external quantum efficiency (EQE) of 2.6%. The findings in this work provide further understanding on the structural and emission properties of quasi-2D perovskites, which pave a new route to design deep-blue-emissive perovskite materials.

3.
Nat Commun ; 10(1): 4247, 2019 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-31534166

RESUMO

Long-lived room temperature phosphorescence (LRTP) is an attractive optical phenomenon in organic electronics and photonics. Despite the rapid advance, it is still a formidable challenge to explore a universal approach to obtain LRTP in amorphous polymers. Based on the traditional polyethylene derivatives, we herein present a facile and concise chemical strategy to achieve ultralong phosphorescence in polymers by ionic bonding cross-linking. Impressively, a record LRTP lifetime of up to 2.1 s in amorphous polymers under ambient conditions is set up. Moreover, multicolor long-lived phosphorescent emission can be procured by tuning the excitation wavelength in single-component polymer materials. These results outline a fundamental principle for the construction of polymer materials with LRTP, endowing traditional polymers with fresh features for potential applications.

4.
Nanoscale ; 11(3): 1451, 2019 01 17.
Artigo em Inglês | MEDLINE | ID: mdl-30604819

RESUMO

Correction for 'Direct Z scheme-fashioned photoanode systems consisting of Fe2O3 nanorod arrays and underlying thin Sb2Se3 layers toward enhanced photoelectrochemical water splitting performance' by Yong Zhou et al., Nanoscale, 2019, DOI: 10.1039/c8nr08292h.

5.
Nanoscale ; 11(1): 109-114, 2018 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-30534720

RESUMO

An elegant Z-scheme-fashioned photoanode consisting of Fe2O3 nanorod arrays and underlying thin Sb2Se3 layers was rationally constructed. The photocurrent density of the Sb2Se3-Fe2O3 Z-scheme photoanode reached 3.07 mA cm-2 at 1.23 V vs. RHE, three times higher than that of pristine Fe2O3 at 1.03 mA cm-2. An obvious cathodic shift of the photocurrent onset potential of about 200 mV was also observed. The transient photovoltage response demonstrates that the suitable band edges (ECB ∼ -0.4 eV and EVB ∼ 0.8 eV) of Sb2Se3, match well with Fe2O3 (ECB ∼ 0.29 eV and EVB ∼ 2.65 eV), permitting the photoexcited electrons on the conduction band of the Fe2O3 to transfer to the valence band of Sb2Se3, and recombine with the holes therein, thus allowing a high concentration of holes to collect in the Fe2O3 for water oxidation. The transient absorption spectra further corroborate that the built-in electric field in the p-n heterojunction leads to a more effective separation and a longer lifetime of the charge carriers.

6.
Chem Commun (Camb) ; 54(98): 13817-13820, 2018 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-30460938

RESUMO

Integration of FexS electrocatalysts and simultaneously generated interfacial oxygen vacancies (VO) was designed to promote the water splitting performance of Fe2O3 photoanodes, in which a synergistic effect remarkably reduces the carrier recombination, increases the number of active sites, and facilitates the photogenerated holes to participate in water oxidation.

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