Vacancy-Driven Disorder and Elevated Dielectric Response in the Pyrochlore Pb1.5Nb2O6.5

Dang, Uyen; O’Hara, Jake; Evans, Hayden A.; Olds, Daniel; Chamorro, Juan; Hickox-Young, Daniel; Laurita, Geneva; Macaluso, Robin T.

doi:10.1021/acs.inorgchem.2c03031

Vacancy-Driven Disorder and Elevated Dielectric Response in the Pyrochlore Pb_1.5Nb₂O_6.5

Journal Article · Tue Nov 08 00:00:00 EST 2022 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.2c03031· OSTI ID:2446650

Dang, Uyen ^[1]; ^[2]; ^[3]; Olds, Daniel ^[4]; Chamorro, Juan ^[5]; ^[6]; ^[2]; ^[1]

Univ. of Texas, Arlington, TX (United States)
Bates College, Lewiston, ME (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Univ. of California, Santa Barbara, CA (United States)
Roanoke College, Salem, VA (United States)

Lone pair-driven distortions are a hallmark of many technologically important lead (Pb)-based materials. Here, the role of Pb²⁺ in polar perovskites is well understood and easily manipulated for applications in piezo- and ferroelectricity, but the control of ordered lone pair behavior in Pb-based pyrochlores is less clear. Crystallographically and geometrically more complex than the perovskite structure, the pyrochlore structure is prone to geometric frustration of local dipoles due to a triangular arrangement of cations on a diamond lattice. The role of vacancies on the O' site of the pyrochlore network has been implicated as an important driver for the expression and correlation of stereochemically active lone pairs in pyrochlores such as Pb₂Ru₂O_6.5 and Pb₂Sn₂O₆. In this work we report on the structural, dielectric, and heat capacity behavior of the cation- and anion-deficient pyrochlore Pb_1.5Nb₂O_6.5 upon cooling. We find that local distortions are present at all temperatures that can be described by cristobalite-type cation ordering, and this ordering persists to longer length scales upon cooling. From a crystallographic perspective, the material remains disordered and does not undergo an observable phase transition. In combination with density function calculations, we propose that the stereochemical activity of the Pb²⁺ lone pairs is driven by proximity to O' vacancies, and the crystallographic site disorder of the O' vacancies prohibits long range correlation of lone pair-driven distortions. This in turn prevents a low-temperature phase transition and results in an elevated dielectric permittivity across a broad temperature range.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2446650

Report Number(s):: BNL--226127-2024-JAAM

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 46 Vol. 61; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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