Effect of oxidation on excited state dynamics of neutral TinO2n-x(n < 10, x < 4) clusters

Jacob M. Garcia, Lauren F. Heald, Ryan E. Shaffer, Scott G. Sayres

Research output: Contribution to journalArticlepeer-review

Abstract

Excited state lifetimes of neutral titanium oxide clusters (TinO2n-x, n < 10, x < 4) were measured using a sequence of 400 nm pump and 800 nm probe femtosecond laser pulses. Despite large differences in electronic properties between the closed shell stoichiometric TinO2n clusters and the suboxide TinO2n-x (x = 1-3) clusters, the transient responses for all clusters contain a fast response of 35 fs followed by a sub-picosecond (ps) excited state lifetime. In this non-scalable size regime, subtle changes in the sub-ps lifetimes are attributed to variations in the coordination of Ti atoms and localization of charge carriers following UV photoexcitation. In general, clusters exhibit longer lifetimes with increased size and also with the addition of O atoms. This suggests that the removal of O atoms develops stronger Ti-Ti interactions as the system transitions from a semiconducting character to a fast metallic electronic relaxation mechanism.

Original languageEnglish (US)
Article number211102
JournalJournal of Chemical Physics
Volume155
Issue number21
DOIs
StatePublished - Dec 7 2021
Externally publishedYes

ASJC Scopus subject areas

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

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