Role of oxygen vacancies on light emission mechanisms in SrTiO3 induced by high-energy particles

Crespillo, M. L.; Graham, J. T.; Agulló-López, F.; Zhang, Y.; Weber, W. J.

doi:10.1088/1361-6463/aa627f

Role of oxygen vacancies on light emission mechanisms in SrTiO₃ induced by high-energy particles

Journal Article · Thu Feb 23 00:00:00 EST 2017 · Journal of Physics. D, Applied Physics

DOI:https://doi.org/10.1088/1361-6463/aa627f· OSTI ID:1348342

Crespillo, M. L. ^[1]; Graham, J. T. ^[2]; Agulló-López, F. ^[3]; Zhang, Y. ^[4]; Weber, W. J. ^[4]

Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States); Missouri Univ. of Science and Technology, Rolla, MO (United States)
Centro de Microanalisis de Materiales, Madrid (Spain)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Light emission under MeV hydrogen and oxygen ions in stoichiometric SrTiO₃ are identified at temperatures of 100 K, 170 K and room-temperature. MeV ions predominately deposit their energies to electrons in SrTiO₃ with energy densities orders of magnitude higher than from UV or x-ray sources but comparable to femtosecond lasers. The ionoluminescence (IL) spectra can be resolved into three main Gaussian bands at 2.0 eV, 2.5 eV and 2.8 eV, whose relative contributions strongly depend on irradiation temperature, electronic energy loss and irradiation fluence. Two main bands, observed at 2.5 eV and 2.8 eV, are intrinsic and associated with electron–hole recombination in the perfect SrTiO₃ lattice. The 2.8 eV band is attributed to recombination of free (conduction) electrons with an in-gap level, possibly related to self-trapped holes. Self-trapped excitons (STEs) are considered suitable candidates for the 2.5 eV emission band, which implies a large energy relaxation in comparison to the intrinsic edge transition. The dynamics of electronic excitation, governs a rapid initial rise of the intensity; whereas, accumulated irradiation damage (competing non-radiative recombination channels) accounts for a subsequent intensity decrease. The previously invoked role of isolated oxygen vacancies for the blue luminescence (2.8 eV) does not appear consistent with the data. An increasing well-resolved band at 2.0 eV dominates at 170 K and below. It has been only previously observed in heavily strained and amorphous SrTiO₃, and is, here, attributed to transitions from d(t 2g) conduction band levels to d(e g) levels below the gap. In accordance with ab initio theoretical calculations they are associated to trapped electron states in relaxed Ti³⁺ centers at an oxygen vacancy within distorted TiO₆ octahedra. The mechanism of defect evolution monitored during real-time IL experiments is presented. In conclusion, the light emission data confirm that IL is a useful tool to investigate lattice disorder in irradiated SrTiO₃.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1348342

Journal Information:: Journal of Physics. D, Applied Physics, Journal Name: Journal of Physics. D, Applied Physics Journal Issue: 15 Vol. 50; ISSN 0022-3727

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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The blue emission at 2.8 eV in strontium titanate: evidence for a radiative transition of self-trapped excitons from unbound states Crespillo, M. L.; Graham, J. T.; Agulló-López, F. Materials Research Letters, Vol. 7, Issue 7 https://doi.org/10.1080/21663831.2019.1604444	journal	April 2019
DFT + DMFT study of oxygen vacancies in a Mott insulator Souto-Casares, Jaime; Spaldin, Nicola A.; Ederer, Claude Physical Review B, Vol. 100, Issue 8 https://doi.org/10.1103/physrevb.100.085146	journal	August 2019
Resistance Switching Behavior in Rectangle-Nano-Pattern SrTiO3 Induced by Simple Annealing Liao, Xiaxia; Zhang, Yufeng; Wang, Jiaou Materials, Vol. 12, Issue 22 https://doi.org/10.3390/ma12223698	journal	November 2019

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74 ATOMIC AND MOLECULAR PHYSICS
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