摘要
Monolayer transition metal dichalcogenides （TMDCs）, as direct bandgap semiconductors, show promise for applications in ultra-thin flexible optoelec- tronic devices. However, the optical properties and device performance are greatly affected by defects, such as vacancies, present in these materials. Vacancies exist unavoidably in mechanically exfoliated or grown by chemical vapor deposition （CVD） monolayer TMDCs; therefore, their influence on the electric and optical properties of host materials has been widely studied. Here, we report a new defect state located at 1.54 eV, which is 70 meV lower than the neutral exciton energy in as-prepared WSe2 monolayers grown by CVD. This defect state is clearly observed in photoluminescence （PL） and Raman spectra at ambient conditions. PL mapping, Rarnan mapping, and atomic force microscopy analysis indicate a solid-vapor reaction growth mechanism of the defect state formation. During a certain growth stage, nuclei with the composition of WOxSey do not fully react with the Se vapor, leading to the defect formation. This type of defects permits radiative recombination of bound neutral excitons, which can make the PL intensity as strong as the intrinsic excitation. Our findings reveal a new way to tailor the optical properties of two-dimensional TMDCs without any additional processes performed after growth.
Monolayer transition metal dichalcogenides （TMDCs）, as direct bandgap semiconductors, show promise for applications in ultra-thin flexible optoelec- tronic devices. However, the optical properties and device performance are greatly affected by defects, such as vacancies, present in these materials. Vacancies exist unavoidably in mechanically exfoliated or grown by chemical vapor deposition （CVD） monolayer TMDCs; therefore, their influence on the electric and optical properties of host materials has been widely studied. Here, we report a new defect state located at 1.54 eV, which is 70 meV lower than the neutral exciton energy in as-prepared WSe2 monolayers grown by CVD. This defect state is clearly observed in photoluminescence （PL） and Raman spectra at ambient conditions. PL mapping, Rarnan mapping, and atomic force microscopy analysis indicate a solid-vapor reaction growth mechanism of the defect state formation. During a certain growth stage, nuclei with the composition of WOxSey do not fully react with the Se vapor, leading to the defect formation. This type of defects permits radiative recombination of bound neutral excitons, which can make the PL intensity as strong as the intrinsic excitation. Our findings reveal a new way to tailor the optical properties of two-dimensional TMDCs without any additional processes performed after growth.
基金
This research was financiaUy supported by the National Natural Science Foundation of China （No. 11304060） and the Foundation of Harbin Institute of Technology for the Incubation Program of the Development of Basic Research Outstanding Talents （No. 01509321）.
