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1.
Opt Express ; 30(22): 39961-39975, 2022 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-36298937

RESUMO

Optically pumped gas molecular terahertz (THz) lasers are promising for generating high-power and high-beam-quality coherent THz radiation. However, for pulsed gas THz lasers, the temporal behavior of the output THz pulse has rarely been investigated. In this study, the temporal behavior of a pulsed gas THz pumped by a fundamental-mode TEA CO2 laser has been presented for the first time both in simulation and experiment. A modified laser kinetics model based on the density matrix rate equation was used to simulate the temporal behavior and output pulse energy of a pulsed gas THz laser at different gas pressures. The results clearly show that the working gas pressure and pump pulse energy have critical influences on the output THz pulse shape. Three typical pulse shapes were obtained, and the THz pulse splitting caused by gain switching was quantitatively simulated and explained based on the laser dynamic process. Besides, with an incident pump pulse energy of 342 mJ, the maximum output THz pulse energy of 2.31 mJ was obtained at 385 µm, which corresponds to a photon conversion efficiency of approximately 56.1%, and to our knowledge, this is the highest efficiency for D2O gas THz laser. The experimental results agreed well with those of the numerical simulation for the entire working gas pressure range, indicating that our model is a powerful tool and paves the way for designing and optimizing high-power pulsed gas lasers.

2.
Small ; 17(23): e2100132, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33891808

RESUMO

Poor charge separation is the main factor that limits the photocatalytic hydrogen generation efficiency of organic conjugated polymers. In this work, a series of linear donor-acceptor (D-A) type oligomers are synthesized by a palladium-catalyzed Sonogashira-Hagihara coupling of electron-deficient diborane unit and different dihalide substitution sulfur functionalized monomers. Such diborane-based A unit exerts great impact on the resulting oligomers, including distinct semiconductor characters with isolated lowest unoccupied molecular orbital (LUMO) orbits locating in diborane-containing fragment, and elevated LUMO level higher than water reduction potential. Relative to A-A type counterpart, the enhanced dipole polarization effect in D-A oligomers facilitates separation of photogenerated charge carriers, as evidenced by notably prolonged electron lifetime. Owing to π-π stacking of rigid backbone, the oligomers can aggregate into an interesting 2D semicrystalline nanosheet (≈2.74 nm), which is rarely reported in linear polymeric photocatalysts prepared by similar carbon-carbon coupling reaction. Despite low surface area (30.3 m2 g-1 ), such ultrathin nanosheet D-A oligomer offers outstanding visible light (λ > 420 nm) hydrogen evolution rate of 833 µmol g-1 h-1 , 14 times greater than its A-A analogue (61 µmol g-1 h-1 ). The study highlights the great potential of using boron element to construct D-A type oligomers for efficient photocatalytic hydrogen generation.

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