Colloidally stable suspensions of lead halide perovskite nanocrystals are prepared from high-quality lead halide nanocrystal seeds. Perovskite nanocrystals with different layered crystal structures are reported. These systems are well suited for investigations of the intrinsic photophysics and spectroscopy of organic-inorganic metal halide perovskites.
We report a novel photochromic molecular system, phenoxyl-imidazolyl radical complex (PIC), in which both a phenoxyl radical site and an imidazolyl radical site are reversibly and simultaneously generated upon UV light irradiation. PIC consists of the three parts: an aromatic linker, a diarylimidazole moiety, and a 4H-cyclohexadienone ring. Upon UV light irradiation, the C-N bond between the 4H-cyclohexadienone ring and the imidazole ring in the colorless closed-ring isomer of PIC undergoes a homolytic cleavage, leading to the formation of the transient colored open-ring isomer. Based on the substituents on the imidazoyl/4H-cyclohexadienone rings and the nature of the aromatic linker, the half-life of the colored open-ring isomer can be varied between tens of nanoseconds and seconds. PIC derivatives containing a 1,2-phenylene linker exhibit high fatigue resistance toward repeated photochromic reactions. Analysis using laser flash photolysis reveals that the absorption spectra of the open-ring isomers are not readily rationalized by a straightforward superposition of the spectra of the two component radical fragments and the photogenerated radicals are electronically coupled through the aromatic linker. Furthermore, the open-ring isomer can be treated as a hybrid of the pure open-shell biradical and closed-shell quinoid resonance structures.
Infrared (IR) light represents an untapped energy source accounting for almost half of all solar energy. Thus, there is a need to develop systems to convert IR light to fuel and make full use of this plentiful resource. Herein, we report photocatalytic H 2 evolution driven by near-to shortwave-IR light (up to 2500 nm) irradiation, based on novel CdS/Cu 7 S 4 heterostructured nanocrystals. The apparent quantum yield reached 3.8% at 1100 nm, which exceeds the highest efficiencies achieved by IR light energy conversion systems reported to date. Spectroscopic results revealed that plasmon-induced hotelectron injection at p−n heterojunctions realizes exceptionally long-lived charge separation (>273 μs), which results in efficient IR light to hydrogen conversion. These results pave the way for the exploration of undeveloped low-energy light for solar fuel generation.
CdTe quantum dots (QDs) were synthesized using oleic acid (OA) and thioglycolic acid (HS-CH 2 COOH, TGA) as capping reagents. Biexciton Auger recombination of CdTe QDs was examined by femtosecond transient absorption spectroscopy by changing excitation intensity. The lifetime of biexciton Auger recombination τ Auger was analyzed as a function of QD diameter D and capping reagents. It was found that τ Auger is proportional to D R , and that the scaling index R is dependent on capping reagents and/or surface conditions. For TGA capped CdTe QDs, R is determined to be 4.6, whereas it is 7.0 for OA capped CdTe QDs with high luminescence quantum yields Φ of 60-85%. This relationship did not hold for small size OA capped CdTe QDs with rather low Φ of 15-30%, in which τ Auger became as short as 2∼3 ps irrespective of the diameter. These results suggest that biexciton Auger recombination of CdTe QDs is strongly dependent on the QD surface trapping and capping reagents.
Benzo-annulated chromenes, i.e., naphthopyrans, are well-known photochromic molecules that undergo photochemical ring-opening reactions to form two colored open-ring isomers, the transoid-cis and transoid-trans forms, upon light irradiation. Though the transoid-cis form returns thermally to the uncolored closed form, the fading rate of the transoid-trans form is extremely slow because of its higher thermal stability. This slow fading behavior of the transoid-trans form is responsible for the persistence of residual color for several minutes to hours, and prevents the application of such molecules to fast photoswitching materials. We have found a new simple and versatile strategy to substantially reduce the amount of the undesirable long-lived colored transoid-trans form by introducing an alkoxy group at the 1-position of azino-fused chromenes, i.e., 8H-pyranoquinazolines. The alkoxy group effectively reduces the formation of the transoid-trans form due to C-H···O intramolecular hydrogen bonding in the transoid-cis form. Moreover, the introduction of a condensed aromatic ring at the 3-position was found to be effective to increase the photosensitivity of the ring-opening reaction. This strategy can also be applied for naphthopyran derivatives and is useful for the development of fast photoresponsive photochromic lenses and fast photoswitching applications such as dynamic holographic materials and molecular actuators.
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