期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 26, 页码 14348-14355出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c03684
关键词
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资金
- European Research Council Advanced Grant ENERGYSURF
- EPSRC (U.K.) [EP/D068673/1]
- EU COST Action [CM1104]
- Royal Society (U.K.) through a Wolfson Research Merit Award
- EPSRC [EP/D068673/1] Funding Source: UKRI
This study focuses on the Ti3+ polaronic states in anatase TiO2(101) and demonstrates the ability to tune the excited state resonance of polarons by controlling the chemical environment. Subsurface polarons in anatase TiO2(101) undergo state changes upon subband-gap photoexcitation, with the binding energy influenced by formic acid adsorption. The behavior observed, including significant changes in photoexcitation oscillator strength resonating with states above the Fermi level, is likely due to surface migration of subsurface oxygen vacancies.
Two polymorphs of TiO2, anatase and rutile, are employed in photocatalytic applications. It is broadly accepted that anatase is the more catalytically active and subsequently finds wider commercial use. In this work, we focus on the Ti3+ polaronic states of anatase TiO2(101), which lie at similar to 1.0 eV binding energy and are known to increase catalytic performance. Using UV-photoemission and two-photon photoemission spectroscopies, we demonstrate the capability to tune the excited state resonance of polarons by controlling the chemical environment. Anatase TiO2(101) contains subsurface polarons which undergo subband-gap photoexcitation to states similar to 2.0 eV above the Fermi level. Formic acid adsorption dramatically influences the polaronic states, increasing the binding energy by similar to 0.3 eV. Moreover, the photoexcitation oscillator strength changes significantly, resonating with states similar to 3.0 eV above the Fermi level. We show that this behavior is likely due to the surface migration of subsurface oxygen vacancies.
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