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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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Balancing Light Absorption and Charge Transport in Vertical SnS 2 Nanoflake Photoanodes with Stepped Layers and Large Intrinsic Mobility
Abstract Significant optical absorption in the blue–green spectral range, high intralayer carrier mobility, and band alignment suitable for water splitting suggest tin disulfide (SnS2) as a candidate material for photo‐electrochemical applications. In this work, vertically aligned SnS2nanoflakes are synthesized directly on transparent conductive substrates using a scalable close space sublimation (CSS) method. Detailed characterization by time‐resolved terahertz and time‐resolved photoluminescence spectroscopies reveals a high intrinsic carrier mobility of 330 cm2V−1s−1and photoexcited carrier lifetimes of 1.3 ns in these nanoflakes, resulting in a long vertical diffusion length of ≈1 µm. The highest photo‐electrochemical performance is achieved by growing SnS2nanoflakes with heights that are between this diffusion length and the optical absorption depth of ≈2 µm, which balances the competing requirements of charge transport and light absorption. Moreover, the unique stepped morphology of these CSS‐grown nanoflakes improves photocurrent by exposing multiple edge sites in every nanoflake. The optimized vertical SnS2nanoflake photoanodes produce record photocurrents of 4.5 mA cm−2for oxidation of a sulfite hole scavenger and 2.6 mA cm−2for water oxidation without any hole scavenger, both at 1.23 VRHEin neutral electrolyte under simulated AM1.5G sunlight, and stable photocurrents for iodide oxidation in acidic electrolyte.
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- PAR ID:
- 10460223
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Energy Materials
- Volume:
- 9
- Issue:
- 31
- ISSN:
- 1614-6832
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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