DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Recent Advances on Carrier and Exciton Self-Trapping in Strontium Titanate: Understanding the Luminescence Emissions

Abstract

An up-to-date review on recent results for self-trapping of free electrons and holes, as well as excitons, in strontium titanate (STO), which gives rise to small polarons and self-trapped excitons (STEs) is presented. Special attention is paid to the role of carrier and exciton self-trapping on the luminescence emissions under a variety of excitation sources with special emphasis on experiments with laser pulses and energetic ion-beams. In spite of the extensive research effort, a definitive identification of such localized states, as well as a suitable understanding of their operative light emission mechanisms, has remained lacking or controversial. However, promising advances have been recently achieved and are the objective of the present review. In particular, significant theoretical advances in the understanding of electron and hole self-trapping are discussed. Also, relevant experimental advances in the kinetics of light emission associated with electron-hole recombination have been obtained through time-resolved experiments using picosecond (ps) laser pulses. The luminescence emission mechanisms and the light decay processes from the self-trapped excitons are also reviewed. Recent results suggest that the blue emission at 2.8 eV, often associated with oxygen vacancies, is related to a transition from unbound conduction levels to the ground singlet state of the STE.more » The stabilization of small electron polarons by oxygen vacancies and its connection with luminescence emission are discussed in detail. Through ion-beam irradiation experiments, it has recently been established that the electrons associated with the vacancy constitute electron polaron states (Ti3+) trapped in the close vicinity of the empty oxygen sites. These experimental results have allowed for the optical identification of the oxygen vacancy center through a red luminescence emission centered at 2.0 eV. Ab-initio calculations have provided strong support for those experimental findings. Finally, the use of Cr-doped STO has offered a way to monitor the interplay between the chromium centers and oxygen vacancies as trapping sites for the electron and hole partners resulting from the electronic excitation.« less

Authors:
 [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Missouri University of Science and Technology, Rolla, MO (United States)
  3. Centro de Microanálisis de Materiales, CMAM-UAM, Cantoblanco, Madrid (Spain)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1495953
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Crystals
Additional Journal Information:
Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 2073-4352
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; wide-bandgap semiconductors; strontium titanate; defects; oxygen vacancies; polarons; self-trapped excitons; ionoluminescence

Citation Formats

Crespillo, Miguel, Graham, Joseph, Agulló-López, Fernando, Zhang, Yanwen, and Weber, William. Recent Advances on Carrier and Exciton Self-Trapping in Strontium Titanate: Understanding the Luminescence Emissions. United States: N. p., 2019. Web. doi:10.3390/cryst9020095.
Crespillo, Miguel, Graham, Joseph, Agulló-López, Fernando, Zhang, Yanwen, & Weber, William. Recent Advances on Carrier and Exciton Self-Trapping in Strontium Titanate: Understanding the Luminescence Emissions. United States. https://doi.org/10.3390/cryst9020095
Crespillo, Miguel, Graham, Joseph, Agulló-López, Fernando, Zhang, Yanwen, and Weber, William. Wed . "Recent Advances on Carrier and Exciton Self-Trapping in Strontium Titanate: Understanding the Luminescence Emissions". United States. https://doi.org/10.3390/cryst9020095. https://www.osti.gov/servlets/purl/1495953.
@article{osti_1495953,
title = {Recent Advances on Carrier and Exciton Self-Trapping in Strontium Titanate: Understanding the Luminescence Emissions},
author = {Crespillo, Miguel and Graham, Joseph and Agulló-López, Fernando and Zhang, Yanwen and Weber, William},
abstractNote = {An up-to-date review on recent results for self-trapping of free electrons and holes, as well as excitons, in strontium titanate (STO), which gives rise to small polarons and self-trapped excitons (STEs) is presented. Special attention is paid to the role of carrier and exciton self-trapping on the luminescence emissions under a variety of excitation sources with special emphasis on experiments with laser pulses and energetic ion-beams. In spite of the extensive research effort, a definitive identification of such localized states, as well as a suitable understanding of their operative light emission mechanisms, has remained lacking or controversial. However, promising advances have been recently achieved and are the objective of the present review. In particular, significant theoretical advances in the understanding of electron and hole self-trapping are discussed. Also, relevant experimental advances in the kinetics of light emission associated with electron-hole recombination have been obtained through time-resolved experiments using picosecond (ps) laser pulses. The luminescence emission mechanisms and the light decay processes from the self-trapped excitons are also reviewed. Recent results suggest that the blue emission at 2.8 eV, often associated with oxygen vacancies, is related to a transition from unbound conduction levels to the ground singlet state of the STE. The stabilization of small electron polarons by oxygen vacancies and its connection with luminescence emission are discussed in detail. Through ion-beam irradiation experiments, it has recently been established that the electrons associated with the vacancy constitute electron polaron states (Ti3+) trapped in the close vicinity of the empty oxygen sites. These experimental results have allowed for the optical identification of the oxygen vacancy center through a red luminescence emission centered at 2.0 eV. Ab-initio calculations have provided strong support for those experimental findings. Finally, the use of Cr-doped STO has offered a way to monitor the interplay between the chromium centers and oxygen vacancies as trapping sites for the electron and hole partners resulting from the electronic excitation.},
doi = {10.3390/cryst9020095},
journal = {Crystals},
number = 2,
volume = 9,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 23 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Optical Gap of Strontium Titanate (Deviation from Urbach Tail Behavior)
journal, November 1970


New ion beam materials laboratory for materials modification and irradiation effects research
journal, November 2014

  • Zhang, Y.; Crespillo, M. L.; Xue, H.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 338
  • DOI: 10.1016/j.nimb.2014.07.028

X‐Ray Diffractometry of Low‐Temperature Phase Transformations in Strontium Titanate
journal, July 1964

  • Lytle, Farrel W.
  • Journal of Applied Physics, Vol. 35, Issue 7
  • DOI: 10.1063/1.1702820

Oxygen vacancies shine blue
journal, November 2005


In-Gap States in Wide-Band-Gap SrTiO3 Analyzed by Cathodoluminescence: In-Gap States in Wide-Band-Gap SrTiO3
journal, March 2011


Photoluminescence and reversible photo-induced spectral change of SrTiO 3
journal, January 2005

  • Mochizuki, Shosuke; Fujishiro, Fumito; Minami, Seiko
  • Journal of Physics: Condensed Matter, Vol. 17, Issue 6
  • DOI: 10.1088/0953-8984/17/6/011

Defect Studies Using Advances with Ion Beam Excited Luminescence
journal, January 2013


Time-resolved spectroscopy of the visible emission band in strontium titanate
journal, June 1986


Localizing nature of photo-excited states in SrTiO3
journal, May 2000


Trapping, self-trapping and the polaron family
journal, May 2007


Drift mobility measurements of small-polaron transport in SrTiO 3
journal, February 1984

  • Keroack, D.; Lepine, Y.; Brebner, J. L.
  • Journal of Physics C: Solid State Physics, Vol. 17, Issue 5
  • DOI: 10.1088/0022-3719/17/5/013

Superconducting Transition Temperatures of Semiconducting SrTi O 3
journal, November 1967


Band-edge luminescence from SrTiO3: No polaron effect
journal, March 2012


Common Fermi-liquid origin of T 2 resistivity and superconductivity in n -type SrTiO 3
journal, November 2011


Epitaxial SrTiO3 films with electron mobilities exceeding 30,000 cm2 V-1 s-1
journal, April 2010

  • Son, Junwoo; Moetakef, Pouya; Jalan, Bharat
  • Nature Materials, Vol. 9, Issue 6, p. 482-484
  • DOI: 10.1038/nmat2750

SRIM – The stopping and range of ions in matter (2010)
journal, June 2010

  • Ziegler, James F.; Ziegler, M. D.; Biersack, J. P.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12
  • DOI: 10.1016/j.nimb.2010.02.091

Hole localization, migration, and the formation of peroxide anion in perovskite Sr Ti O 3
journal, July 2014


Optical Properties and Band Structure of SrTi O 3 and BaTi O 3
journal, October 1965


Dielectric spectra and electrical conduction in Fe-doped SrTiO 3
journal, February 2000


Hall Mobility in SrTi O 3
journal, September 1967


Temperature Dependence of Photoluminescence Spectra of Nondoped and Electron-Doped SrTiO 3 : Crossover from Auger Recombination to Single-Carrier Trapping
journal, June 2009


Quantum chemical modelling of electron polarons and excitons in ABO 3 perovskites
journal, August 2000


Photo-induced polaron states in strontium titanate
journal, December 2001


Electronic structure of oxygen vacancies in SrTiO 3 and LaAlO 3
journal, October 2012


Atomic control and characterization of surface defect states of TiO2 terminated SrTiO3 single crystals
journal, August 2008

  • Kareev, M.; Prosandeev, S.; Liu, J.
  • Applied Physics Letters, Vol. 93, Issue 6
  • DOI: 10.1063/1.2971035

Bulk electronic structure of SrTiO3: Experiment and theory
journal, December 2001

  • van Benthem, K.; Elsässer, C.; French, R. H.
  • Journal of Applied Physics, Vol. 90, Issue 12
  • DOI: 10.1063/1.1415766

Correlation between Cr 3+ Luminescence and Oxygen Vacancy Disorder in Strontium Titanate under MeV Ion Irradiation
journal, September 2017

  • Crespillo, M. L.; Graham, J. T.; Agulló-López, F.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 36
  • DOI: 10.1021/acs.jpcc.7b04352

Blue-light emission at room temperature from Ar+-irradiated SrTiO3
journal, October 2005

  • Kan, Daisuke; Terashima, Takahito; Kanda, Ryoko
  • Nature Materials, Vol. 4, Issue 11
  • DOI: 10.1038/nmat1498

Photoluminescence dynamics in strontium titanate
journal, December 2009


Magnetic effects at the interface between non-magnetic oxides
journal, June 2007

  • Brinkman, A.; Huijben, M.; van Zalk, M.
  • Nature Materials, Vol. 6, Issue 7, p. 493-496
  • DOI: 10.1038/nmat1931

Blue luminescence of SrTiO3 under intense optical excitation
journal, November 2009

  • Rubano, A.; Paparo, D.; Granozio, F. Miletto
  • Journal of Applied Physics, Vol. 106, Issue 10
  • DOI: 10.1063/1.3256140

Vacancies and small polarons in SrTiO 3
journal, August 2014


Coexistence of trapped and free excess electrons in SrTiO 3
journal, February 2015


X‐ray induced processes in SrTiO 3
journal, December 1982

  • Aguilar, M.; Agulló‐López, F.
  • Journal of Applied Physics, Vol. 53, Issue 12
  • DOI: 10.1063/1.330408

Role of oxygen vacancies on light emission mechanisms in SrTiO 3 induced by high-energy particles
journal, March 2017

  • Crespillo, M. L.; Graham, J. T.; Agulló-López, F.
  • Journal of Physics D: Applied Physics, Vol. 50, Issue 15
  • DOI: 10.1088/1361-6463/aa627f

Recombination kinetics of a dense electron-hole plasma in strontium titanate
journal, September 2007


Lattice Dynamics and Phase Transitions of Strontium Titanate
journal, May 1964


First-principles study of bulk and surface oxygen vacancies in SrTiO3 crystal
journal, October 2009


Spectra and color centers of strontium titanate crystals
journal, January 2012


A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004


Information obtainable from ion beam luminescence
journal, August 2007


Superconducting Interfaces Between Insulating Oxides
journal, August 2007


Time-resolved photoluminescence of n-doped SrTiO3
journal, January 2008

  • Rubano, A.; Paparo, D.; Radović, M.
  • Applied Physics Letters, Vol. 92, Issue 2
  • DOI: 10.1063/1.2832666

Isolated oxygen vacancies in strontium titanate shine red: Optical identification of Ti3+ polarons
journal, September 2018


Dynamics of nonlinear blue photoluminescence and Auger recombination in SrTiO 3
journal, May 2008


Photophysical and Photocatalytic Properties of SrTiO 3 Doped with Cr Cations on Different Sites
journal, August 2006

  • Wang, Defa; Ye, Jinhua; Kako, Tetsuya
  • The Journal of Physical Chemistry B, Vol. 110, Issue 32
  • DOI: 10.1021/jp062487p

Study of photoluminescence and electronic states in nanophase strontium titanate
journal, January 2000

  • Zhang, W. F.; Yin, Z.; Zhang, M. S.
  • Applied Physics A: Materials Science & Processing, Vol. 70, Issue 1
  • DOI: 10.1007/s003390050018

First principle electronic, structural, elastic, and optical properties of strontium titanate
journal, March 2012

  • Ekuma, Chinedu E.; Jarrell, Mark; Moreno, Juana
  • AIP Advances, Vol. 2, Issue 1
  • DOI: 10.1063/1.3700433

Room-temperature photoluminescence in amorphous SrTiO 3 - the influence of acceptor-type dopants
journal, November 2002

  • Soledade, L. E. B.; Longo, E.; Leite, E. R.
  • Applied Physics A: Materials Science & Processing, Vol. 75, Issue 5
  • DOI: 10.1007/s003390101140

An Ideal System for Analysis and Interpretation of Ion Beam Induced Luminescence
journal, January 2015


SrTi O 3 : An intrinsic quantum paraelectric below 4 K
journal, April 1979


Electronic structure of a neutral oxygen vacancy in SrTiO 3
journal, December 2003


Symmetry-breaking Ta 4 + centers in KTaO 3
journal, July 1998

  • Laguta, V. V.; Zaritskii, M. I.; Glinchuk, M. D.
  • Physical Review B, Vol. 58, Issue 1
  • DOI: 10.1103/PhysRevB.58.156

Dielectric Constant of Strontium Titanate at Low Temperatures
journal, October 1962

  • Sawaguchi, Etsuro; Kikuchi, Atsushi; Kodera, Yōichi
  • Journal of the Physical Society of Japan, Vol. 17, Issue 10
  • DOI: 10.1143/JPSJ.17.1666

Temperature measurements during high flux ion beam irradiations
journal, February 2016

  • Crespillo, M. L.; Graham, J. T.; Zhang, Y.
  • Review of Scientific Instruments, Vol. 87, Issue 2
  • DOI: 10.1063/1.4941720

Infrared dispersion in SrTi O 3 at high temperature
journal, December 1980


Defect States Induced by Oxygen Vacancies in Cubic SrTiO 3 : First-Principles Calculations
journal, November 2010

  • Hou, Zhufeng; Terakura, Kiyoyuki
  • Journal of the Physical Society of Japan, Vol. 79, Issue 11
  • DOI: 10.1143/JPSJ.79.114704

In-situ luminescence monitoring of ion-induced damage evolution in SiO2 and Al2O3
journal, April 2016


Anti-ferrodistortive-Like Oxygen-Octahedron Rotation Induced by the Oxygen Vacancy in Cubic SrTiO 3
journal, October 2012


Works referencing / citing this record:

Resistance Switching Behavior in Rectangle-Nano-Pattern SrTiO3 Induced by Simple Annealing
journal, November 2019

  • Liao, Xiaxia; Zhang, Yufeng; Wang, Jiaou
  • Materials, Vol. 12, Issue 22
  • DOI: 10.3390/ma12223698