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000908349 1001_ $$0P:(DE-HGF)0$$aGe, Zhen-Hua$$b0
000908349 245__ $$aAtomic‐Scale Observation of Off‐Centering Rattlers in Filled Skutterudites
000908349 260__ $$aWeinheim$$bWiley-VCH$$c2022
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000908349 520__ $$aAs one of the most fundamental order parameters, the coordinate order of atoms is a cornerstone in determining the physical and chemical properties of materials. Off-centering shifts of atoms from their centrosymmetric positions, a phenomenon that is closely related to symmetry breaking and structural transitions in crystals, is of key importance in modifying a broad range of fundamental properties, such as ferroelectricity, antiferroelectricity, and piezoelectricity. In thermoelectric materials, which can be used to directly interconvert heat to electricity, off-centering has been proposed in, e.g., lead tellurides, halide perovskites, type I and II clathrates, and filled skutterudites, to be the physical origin of the experimentally measured exceptionally low thermal conductivity, but only indirectly supported from structural refinements and experimental/theoretical vibration mode analyses. In this work, Yb partially filled and Ce fully filled skutterudite is taken as a model system for directly measuring the off-centering shifts of filler atoms, i.e., rattlers, with picometer precision in real space, by means of atomic-resolution negative spherical aberration imaging transmission electron microscopy. This finding allows an in-depth understanding of the relationship between the off-centering and the thermoelectric performance, and the presented methodology here is also applicable to investigate the off-centering phenomena in other functional materials, e.g., ferroelectrics and solar cells.
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000908349 7001_ $$0P:(DE-HGF)0$$aLi, Wen-Jie$$b1
000908349 7001_ $$0P:(DE-HGF)0$$aFeng, Jing$$b2
000908349 7001_ $$0P:(DE-Juel1)165965$$aZheng, Fengshan$$b3
000908349 7001_ $$0P:(DE-Juel1)130736$$aJia, Chun-Lin$$b4
000908349 7001_ $$0P:(DE-HGF)0$$aWu, Di$$b5$$eCorresponding author
000908349 7001_ $$0P:(DE-Juel1)145711$$aJin, Lei$$b6$$eCorresponding author
000908349 773__ $$0PERI:(DE-600)2594556-7$$a10.1002/aenm.202103770$$gVol. 12, no. 15, p. 2103770 -$$n15$$p2103770 -$$tAdvanced energy materials$$v12$$x1614-6832$$y2022
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