Details

Autor(en) / Beteiligte

• Hoffman, Anna N.
• Gu, Yiyi
• Liang, Liangbo
• Fowlkes, Jason D.
• Xiao, Kai
• Rack, Philip D.

Titel

Exploring the air stability of PdSe2 via electrical transport measurements and defect calculations

Ist Teil von

• NPJ 2D materials and applications, 2019-12, Vol.3 (1), Article 50

Ort / Verlag

London: Nature Publishing Group UK

Erscheinungsjahr

2019

Quelle

EZB Free E-Journals

Beschreibungen/Notizen

• In this work we investigate the effects of ambient exposure on CVD grown PdSe 2 and correlate density functional theory calculations of various physisorption and chemisorption binding energies and band structures to the observed changes in the electrical transport. Pristine PdSe 2 is n-type due to intrinsic selenium vacancies, but shows increased p-type conduction and decreased n-type conduction as a function of ambient aging during which various aging mechanisms appear to be operative. Short term aging (<160 h) is ascribed to an activated chemisorption of molecular O 2 at selenium vacancies; first-principles calculations suggest a ~0.85 eV activation energy and adsorption geometries with binding energies varying between 1.3–1.6 eV, in agreement with experimental results. Importantly, this chemisorption is reversible with a low temperature anneal. At long term aging (>430 h), there is a total suppression of n-type conduction, which is attributed to a dissociative adsorption/reaction of the O 2 molecules to atomic O and subsequent PdO 2 formation. XPS confirms the presence of PdO 2 in long term aged flakes. At these extended aging times, the low temperature anneal restores low n-type conduction and suppresses p-type conduction due to the low thermal stability of PdO 2 which, in agreement with XPS measurements, sublimates during the anneal. Thus PdSe 2 devices can be processed into device architectures in standard laboratory environments if atmospheric exposure times are limited to on the order of 1 week.