Abstract
For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab initio theory of chalcogen vacancies in monolayer MoS2. Chalcogen vacancies are selectively generated by in-vacuo annealing, but also focused ion beam exposure. The defect generation rate, atomic imaging and the optical signatures support this claim. We discriminate the narrow linewidth photoluminescence signatures of vacancies, resulting predominantly from localized defect orbitals, from broad luminescence features in the same spectral range, resulting from adsorbates. Vacancies can be patterned with a precision below 10 nm by ion beams, show single photon emission, and open the possibility for advanced defect engineering of 2D semiconductors at the ultimate scale.
Highlights
For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials
Combing controlled defect engineering with optical spectroscopy as well as atomic imaging and ab initio theory, we identify the optical signature of pristine chalcogen vacancies in MoS2
Combing controlled defect engineering with optical spectroscopy as well as atomic imaging and ab initio theory, we identify the optical signature of chalcogen vacancies in MoS2
Summary
For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Vacancies can be patterned with a precision below 10 nm by ion beams, show single photon emission, and open the possibility for advanced defect engineering of 2D semiconductors at the ultimate scale. Combing controlled defect engineering with optical spectroscopy as well as atomic imaging and ab initio theory, we identify the optical signature of pristine chalcogen vacancies in MoS2. Comparing annealed vs He-ion treated MoS2, we establish that the recently discovered single-photon emitters in He-ion irradiated MoS2 originate from chalcogen vacancies[3]. The latter can be deterministically created with a precision below 10 nm[9], underscoring the potential of defect engineering for twodimensional (quantum-) optoelectronics. Defect levels deep inside the band gap provide further relaxation pathways at even lower transition energies[10]
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