Super-bandgap light stimulated reversible transformation and laser-driven mass transport at the surface of As2S3 chalcogenide nanolayers studied in situ

R. Holomb, O. Kondrat, V. Mitsa, M. Veres, A. Czitrovszky, A. Feher, N. Tsud, M. Vondráček, K. Veltruská, V. Matolín, K. C. Prince

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

The super-bandgap laser irradiation of the in situ prepared As-S chalcogenide films was found to cause drastic structural transformations and unexpected selective diffusion processes, leading to As enrichment on the nanolayer surface. Excitation energy dependent synchrotron radiation photoelectron spectroscopy showed complete reversibility of the molecular transformations and selective laser-driven mass transport during "laser irradiation"-"thermal annealing" cycles. Molecular modeling and density functional theory calculations performed on As-rich cage-like clusters built from basic structural units indicate that the underlying microscopic mechanism of laser induced transformations is connected with the realgar-pararealgar transition in the As-S structure. The detected changes in surface composition as well as the related local and molecular structural transformations are analyzed and a model is proposed and discussed in detail. It is suggested that the formation of a concentration gradient is a result of bond cleavage and molecular reorientation during transformations and anisotropic molecular diffusion.

Original languageEnglish
Article number214702
JournalJournal of Chemical Physics
Volume149
Issue number21
DOIs
Publication statusPublished - Dec 7 2018

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Fingerprint Dive into the research topics of 'Super-bandgap light stimulated reversible transformation and laser-driven mass transport at the surface of As<sub>2</sub>S<sub>3</sub> chalcogenide nanolayers studied in situ'. Together they form a unique fingerprint.

  • Cite this

    Holomb, R., Kondrat, O., Mitsa, V., Veres, M., Czitrovszky, A., Feher, A., Tsud, N., Vondráček, M., Veltruská, K., Matolín, V., & Prince, K. C. (2018). Super-bandgap light stimulated reversible transformation and laser-driven mass transport at the surface of As2S3 chalcogenide nanolayers studied in situ. Journal of Chemical Physics, 149(21), [214702]. https://doi.org/10.1063/1.5053228