Polar metals are challenging to identify spectroscopically because the fingerprints of electric polarization are often obscured by the presence of screening charges. Here, we unravel unambiguous signatures of a distortive polar order buried in the Fermi sea by probing the nonlinear optical response of materials driven by tailored terahertz fields. We apply this strategy to investigate the topological crystalline insulator PbSnTe, tracking its soft phonon mode in the time domain and observing the occurrence of inversion symmetry breaking as a function of temperature. By combining measurements across the material's phase diagram with ab initio calculations, we demonstrate the generality of our approach. These results highlight the potential of terahertz driving fields to reveal polar orders coexisting with itinerant electrons, thus opening additional avenues for material discovery.
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http://dx.doi.org/10.1126/sciadv.adn0929 | DOI Listing |
Sci Adv
July 2024
Department of Physics and Center for Complex Quantum Systems, The University of Texas at Austin, Austin, TX 78712, USA.
Polar metals are challenging to identify spectroscopically because the fingerprints of electric polarization are often obscured by the presence of screening charges. Here, we unravel unambiguous signatures of a distortive polar order buried in the Fermi sea by probing the nonlinear optical response of materials driven by tailored terahertz fields. We apply this strategy to investigate the topological crystalline insulator PbSnTe, tracking its soft phonon mode in the time domain and observing the occurrence of inversion symmetry breaking as a function of temperature.
View Article and Find Full Text PDFAdv Sci (Weinh)
July 2023
Department of Chemistry, Sogang University, Seoul, 04107, Republic of Korea.
A polar tetragonal tungsten bronze, Pb K □ Li Nb O (□: vacancies), has been successfully synthesized by a high temperature solid-state reaction. Single crystal and powder X-ray diffraction indicate that the structure of Pb K □ Li Nb O crystallizing in the noncentrosymmetric (NCS) space group, P4bm, consists of 3D framework with highly distorted NbO , LiO , PbO , and (Pb/K)O polyhedra. While NCS Pb K □ Li Nb O undergoes a reversible phase transition between polar (P4bm) and nonpolar (P4/mbm) structure at around 460 °C, the material decomposes to centrosymmetric Pb K Li Nb O (P4/mbm) once heated to 1200 °C.
View Article and Find Full Text PDFJ Phys Chem Lett
February 2023
School of Physics and Electronic Sciences, Key Laboratory of Polar Materials and Devices (MOE), East China Normal University, Shanghai 200241, China.
The defect types in layered semiconductors can be identified by matching the scanning transmission electron microscopy (STEM) images with the structures from first-principles simulations. In a PVD-grown MoS monolayer, the Mo antisite (one Mo replaces two S) is recognized as being dominant, because its calculated structure matches the distortive structure in STEM images. Therefore, Mo has received much attention in MoS-related defect engineering.
View Article and Find Full Text PDFJ Phys Condens Matter
July 2021
Laboratory of Dielectric Materials, School of Materials Science and Engineering, Zhejiang University, Zheda Road 38, 310027, Hangzhou, People's Republic of China.
Currently, active research is aimed at perovskite-based oxides, including rare earth orthochromites, which exhibit magnetoelectric properties owed to intrinsic magnetic interactions in external electric and magnetic fields. Due to a variety of structural instabilities and couplings in these materials, understanding the underlying magnetoelectric mechanisms is a challenge. In this paper, we explore magnetoelectric properties of the rare earth orthochromites in the framework of symmetry analysis.
View Article and Find Full Text PDFNat Commun
December 2019
Department of Materials, ETH Zurich, 8093, Zurich, Switzerland.
The secondary nature of polarization in improper ferroelectrics promotes functional properties beyond those of conventional ferroelectrics. In technologically relevant ultrathin films, however, the improper ferroelectric behavior remains largely unexplored. Here, we probe the emergence of the coupled improper polarization and primary distortive order parameter in thin films of hexagonal YMnO.
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