Intermittent Defect Fluctuations in Oxide Heterostructures

Zhang, Qingteng; Wan, Gang; Starchenko, Vitalii; Hu, Guoxiang; Dufresne, Eric M.; Zhou, Hua; Jeen, Hyoungjeen; Almazan, Irene Calvo; Dong, Yongqi; Liu, Huajun; Sandy, Alec R.; Sterbinsky, George E.; Lee, Ho Nyung; Ganesh, P.; Fong, Dillon D.

doi:10.1002/adma.202305383

Title: Intermittent Defect Fluctuations in Oxide Heterostructures

Journal Article · 14 August 2023 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202305383 · OSTI ID:1999315

^[1]; Wan, Gang ^[2]; Starchenko, Vitalii ^[3]; Hu, Guoxiang ^[4];

^[1]; Zhou, Hua ^[1]; Jeen, Hyoungjeen ^[5]; Almazan, Irene Calvo ^[1]; Dong, Yongqi ^[1]; Liu, Huajun ^[6];

^[1]; Sterbinsky, George E. ^[1]; Lee, Ho Nyung ^[3]; Ganesh, P. ^[4]; Fong, Dillon D. ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Pusan National Univ., Busan (Korea, Republic of)
Argonne National Laboratory (ANL), Argonne, IL (United States); Agency for Science, Technology and Research (A*STAR) (Singapore). Institute of Materials Research and Engineering (IMRE)

The heterogeneous nature, local presence, and dynamic evolution of defects typically govern the ionic and electronic properties of a wide variety of functional materials. While the last 50 years have seen considerable efforts into development of new methods to identify the nature of defects in complex materials, such as the perovskite oxides, very little is known about defect dynamics and their influence on the functionality of a material. Here, the discovery of the intermittent behavior of point defects (oxygen vacancies) in oxide heterostructures employing X-ray photon correlation spectroscopy is reported. Local fluctuations between two ordered phases in strained SrCoO_x with different degrees of stability of the oxygen vacancies are observed. Ab-initio-informed phase-field modeling reveals that fluctuations between the competing ordered phases are modulated by the oxygen ion/vacancy interaction energy and epitaxial strain. The results demonstrate how defect dynamics, evidenced by measurement and modeling of their temporal fluctuations, give rise to stochastic properties that now can be fully characterized using coherent X-rays, coupled for the first time to multiscale modeling in functional complex oxide heterostructures. The study and its findings open new avenues for engineering the dynamical response of functional materials used in neuromorphic and electrochemical applications.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE

Grant/Contract Number:: AC02-06CH11357; AC02-05CH11231; BES-ERCAP0024097

OSTI ID:: 1999315

Alternate ID(s):: OSTI ID: 2203015; OSTI ID: 2397270

Journal Information:: Advanced Materials, Vol. 35, Issue 42; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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