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| 1 | Optical emission enhancement of bent InSe thin films显示文摘In contrast to the majority of two-dimensional semiconductors such as transition metal dichalcogenides,indium selenide(InSe)possesses an intrinsic large out-of-plane oriented band-edge luminescent dipole.This unique anisotropic feature of band-edge optical emissions can be exploited to achieve enhanced optical signal in bent regions of materials created by geometrical modification.We herein investigate based on first-principle calculations the mechanism of this optical emission enhancement by modelling the photoluminescence processes in bent and flat regions of the InSe thin film.We propose in our model that the shorter-wavelength interband transition,labelled as transition B′,between the second-highest valence band and the bottom of conduction band plays an important role in the enhancing process.Our model robustly describes the dependence of optical emission enhancement in the bent InSe thin films on thickness,incident light orientation,and excitation photon energy.In particular,we found that when excitation photon energy is lower than the energy of transition B′,strong enhancement up to hundreds of times can be obtained by applying an incident light at an angle less than 70°to the InSe layers.Our results provide useful references for modulating luminescent properties of InSe films toward flexible optoelectronic device applications. | Jiahao XIE Lijun ZHANG | 2021 | Science China(Information Sciences)2021，64，4： | 0 |
| 2 | Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis显示文摘In comparison with the developing nano-carbon catalysts,some small organic molecules are also emerging as catalysts with typical features,however,their working mechanism is still unclear.Here,we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange engineering.These viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based H_(2)O_(2) electrosynthesis.Differing from the commonly reported carbon-based electrocatalysts,viologens can produce H_(2)O_(2) in a synergistic manner,which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox mediator.We found that the ring current and H_(2)O_(2) selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent group.As a result,a benzyl-substituted viologen(BV)delivers the best electrocatalytic performance among the samples,including the highest H_(2)O_(2) selectivity of 96.9%at 0.6 V and the largest ring current density of about 13.6 mA·mmol-1.Furthermore,density functional theory(DFT)calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital(HOMO)–lowest unoccupied molecular orbital(LUMO)energy gap of BV is beneficial to the synergistic mechanism for H_(2)O_(2) production.This work sheds new insight into the efficient H_(2)O_(2) production in a synergistic manner for small molecules-based electrocatalysts. | Yang Gao Xiaohui Xu Yue Niu Xinran Hu Zeyu Li Longkun Yang Linjie Zhi Bin Wang | 2023 | Nano Research2023，16，12： | 0 |
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