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We combined synchrotron-based near field infrared spectroscopy and atomic force microscopy to image the properties of ferroelastic domain walls in Sr3Sn2O7. Although frequency shifts at the walls are near the limit of our sensitivity, we can confirm semiconducting rather than metallic character and widths between 20 and 60 nm. The latter is significantly narrower than in other hybrid improper ferroelectrics like Ca3Ti2O7. We attribute this trend to the softer lattice in Sr3Sn2O7, which may enable the octahedral tilt and rotation order parameters to evolve more quickly across the wall without significantly increased strain. These findings are crucial for the understanding of phononic properties at interfaces and the development of domain wall-based devices.more » « lessFree, publicly-accessible full text available November 13, 2025
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Smith, Kevin A.; Ramkumar, Sriram P.; Du, Kai; Xu, Xianghan; Cheong, Sang-Wook; Gilbert Corder, Stephanie N.; Bechtel, Hans A.; Nowadnick, Elizabeth A.; Musfeldt, Janice L. (, ACS Applied Materials & Interfaces)
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Fan, Shiyu; Singh, Sobhit; Xu, Xianghan; Park, Kiman; Qi, Yubo; Cheong, S. W.; Vanderbilt, David; Rabe, Karin M.; Musfeldt, J. L. (, npj Quantum Materials)Abstract Hafnia (HfO 2 ) is a promising material for emerging chip applications due to its high- κ dielectric behavior, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO 2 crystals stabilized with yttrium (chemical formula HfO 2 : x Y, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO 2 and paves the way for an analysis of mode contributions to high- κ dielectric and ferroelectric properties for chip technologies.more » « less
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