Influence of crystalline order and defects on the absolute work functions and electron affinities of TiO2- and SrO-terminated n-SrTiO3(001)

Chambers, Scott A.; Sushko, Petr V.

doi:10.1103/PhysRevMaterials.3.125803

Title: Influence of crystalline order and defects on the absolute work functions and electron affinities of TiO2- and SrO-terminated n-SrTiO3(001)

Journal Article · Mon Dec 23 00:00:00 EST 2019 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.3.125803· OSTI ID:1582408

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BATTELLE (PACIFIC NW LAB)

We establish how the detailed structure and composition of the terminal layer of n-SrTiO3 (001) determine key surface electronic properties. We have measured and calculated from first principles the absolute work functions and electron affinities of bulk SrNb0.01Ti0.99O3(001) with both TiO2 and nominally SrO terminal planes. The match between theory and experiment is excellent at 4.6(1) eV for the TiO2 termination if an ideal, bulk-truncated surface structure is assumed. In contrast, the ideal SrO-termination leads to a calculated work function that is ~1.3 eV lower than the experimental value of 3.6(1) eV. We show that this discrepancy is associated with defects on the SrO surface that serve as electron scavengers. These defects deplete the concentration of itinerant electrons in the subsurface region and increase the negative charge density on the surface, thus increasing the work function. Several different surface defect configurations were modeled; the ones that yield the best agreement with experiment involve Sr vacancies in the terminal layer along with OH–/H– pairs or O22– occupying anion sites adjacent to the Sr vacancies.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1582408

Report Number(s):: PNNL-SA-148767

Journal Information:: Physical Review Materials, Vol. 3, Issue 12

Country of Publication:: United States

Language:: English

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