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  1. Abstract

    A comprehensive experimental study on optical properties and photocarrier dynamics in Bi2O2Se monolayers and nanoplates is presented. Large and uniform Bi2O2Se nanoplates with various thicknesses down to the monolayer limit are fabricated. In nanoplates, a direct optical transition near 720 nm is identified by optical transmission, photoluminescence, and transient absorption spectroscopic measurements and is attributed to the transition between the valence and conduction bands in the Γ valley. Time‐resolved differential reflection measurements reveal ultrafast carrier thermalization and energy relaxation processes and a photocarrier recombination lifetime of about 200 ps in nanoplates. Furthermore, by spatially resolving the differential reflection signal, a photocarrier diffusion coefficient of about 4.8 cm2s−1is obtained, corresponding to a mobility of about 180 cm2V−1s−1. A similar direct transition is also observed in monolayer Bi2O2Se, suggesting that the states in the Γ valley do not change significantly with the thickness. The temporal dynamics of the excitons in the monolayer is quite different from the nanoplates, with a strong saturation effect and fast exciton–exciton annihilation at high densities. Spatially and temporally resolved measurements yield an exciton diffusion coefficient of about 20 cm2s−1.

     
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  2. We fabricated a van der Waals heterostructure of WS 2 –ReSe 2 and studied its charge-transfer properties. Monolayers of WS 2 and ReSe 2 were obtained by mechanical exfoliation and chemical vapor deposition, respectively. The heterostructure sample was fabricated by transferring the WS 2 monolayer on top of ReSe 2 by a dry transfer process. Photoluminescence quenching was observed in the heterostructure, indicating efficient interlayer charge transfer. Transient absorption measurements show that holes can efficiently transfer from WS 2 to ReSe 2 on an ultrafast timescale. Meanwhile, electron transfer from ReSe 2 to WS 2 was also observed. The charge-transfer properties show that monolayers of ReSe 2 and WS 2 form a type-II band alignment, instead of type-I as predicted by theory. The type-II alignment is further confirmed by the observation of extended photocarrier lifetimes in the heterostructure. These results provide useful information for developing van der Waals heterostructure involving ReSe 2 for novel electronic and optoelectronic applications and introduce ReSe 2 to the family of two-dimensional materials to construct van der Waals heterostructures. 
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  3. Charge-transfer excitons are formed by photoexcited electrons and holes following charge transfer across a heterojunction. They are important quasiparticles for optoelectronic applications of semiconducting heterostructures. The newly developed two-dimensional heterostructures provide a new platform to study these excitons. We report spatially and temporally resolved transient absorption measurements on the dynamics of charge-transfer excitons in a MoS 2 /WS 2 /MoSe 2 trilayer heterostructure. We observed a non-classical lateral diffusion process of charge-transfer excitons with a decreasing diffusion coefficient. This feature suggests that hot charge-transfer excitons with large kinetic energies are formed and their cooling process persists for about 100 ps. The long energy relaxation time of excitons in the trilayer compared to its monolayer components is attributed to the reduced carrier and phonon scattering due to the dielectric screening effect in the trilayer. Our results help develop an in-depth understanding of the dynamics of charge-transfer excitons in two-dimensional heterostructures. 
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  4. Due to their atomic thinness with reduced dielectric screening, two-dimensional materials can possess a stable excitonic population at room temperature. This is attractive for future excitonic devices, where excitons are used to carry energy or information. In excitonic devices, controlling transport of the charge-neutral excitons is a key element. Here we show that exciton transport in a MoSe 2 monolayer semiconductor can be effectively controlled by dielectric screening. A MoSe 2 monolayer was partially covered with a hexagonal boron nitride flake. Photoluminescence measurements showed that the exciton energy in the covered region is about 12 meV higher than that in the uncovered region. Spatiotemporally resolved differential reflection measurements performed at the junction between the two regions revealed that this energy offset is sufficient to drive excitons across the junction for about 50 ps over a distance of about 200 nm. These results illustrate the feasibility of using van der Waals dielectric engineering to control exciton transport and contribute to understanding the effects of the dielectric environment on the electronic and optical properties of two-dimensional semiconductors. 
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