Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 138, Issue 30, Pages 9393-9396Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b05208
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Funding
- Block Allocation Grant
- European Research Council [279705]
- Alexander von Humboldt Foundation
- European Union (EU) [641887]
- Marie Curie Actions (MSCA) [641887] Funding Source: Marie Curie Actions (MSCA)
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We study the compositional dependence of molecular orientation (multipolar) and orbital (quadrupolar) order in the perovskite-like metal organic frameworks [C(NH2)(3)]CuxCd1-x(HCOO)(3). Upon increasing the fraction x of Jahn-Teller-active Cu2+, we observe an orbital disorder/order transition and a multipolar reorientation transition, each occurring at distinct critical compositions x(o) = 0.45(5) and x(m), = 0.55(5). We attribute these transitions to a combination of size, charge distribution, and percolation effects. Our results establish the accessibility in formate perovskites of novel structural degrees of freedom beyond the familiar dipolar terms responsible for (anti)ferroelectric order. We discuss the implications of cooperative quadrupolar and multipolar states for the design of relaxor-like hybrid perovskites.
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