skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Revealing a distortive polar order buried in the Fermi sea
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 Pb1−xSnxTe, 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.  more » « less
Award ID(s):
2308817
PAR ID:
10587858
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
AAAS
Date Published:
Journal Name:
Science Advances
Volume:
10
Issue:
28
ISSN:
2375-2548
Page Range / eLocation ID:
eadn0929-
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. The recently demonstrated chiral modes of lattice motion carry angular momentum and therefore directly couple to magnetic fields. Notably, their magnetic moments are predicted to be strongly influenced by electronic contributions. Here, we have studied the magnetic response of transverse optical phonons in a set of Pb1−xSnxTe films, which is a topological crystalline insulator forx> 0.32 and has a ferroelectric transition at anx-dependent critical temperature. Polarization-dependent terahertz magnetospectroscopy measurements revealed Zeeman splittings and diamagnetic shifts, demonstrating a large phonon magnetic moment. Films in the topological phase exhibited phonon magnetic moment values that were larger than those in the topologically trivial samples by two orders of magnitude. Furthermore, the sign of the effective phonong-factor was opposite in the two phases, a signature of the topological transition according to our model. These results strongly indicate the existence of interplay between the magnetic properties of chiral phonons and the topology of the electronic band structure. 
    more » « less
  2. Measuring terahertz waveforms in terahertz spectroscopy often relies on electro-optic sampling employing a ZnTe crystal. Although the nonlinearities in such zincblende semiconductors induced by intense terahertz pulses have been studied at optical frequencies, a quantitative study of nonlinearities in the terahertz regime has not been reported. In this work, we investigate the nonlinear response of ZnTe in the terahertz frequency region utilizing time-resolved terahertz-pump terahertz-probe spectroscopy. We find that the interaction of two co-propagating terahertz pulses in ZnTe leads to a nonlinear polarization change which modifies the electro-optic response of the medium at terahertz frequencies. We present a model for this polarization that showcases the second-order nonlinear behavior. We also determine the magnitude of the third-order susceptibility in ZnTe at terahertz frequencies,χ(3)THz). These results clarify the interactions in ZnTe at terahertz frequencies, with implications for measurements of intense terahertz fields using electro-optic sampling. 
    more » « less
  3. Abstract Terahertz spectroscopy of thec‐axis Josephson plasma resonance (JPR) in high‐temperature cuprates is a powerful probe of superconductivity, providing a route to couple to and interact with the condensate. Electromagnetic coupling between metasurface arrays of split ring resonators (SRRs) and the JPR of a La2−xSrxCuO4single crystal (Tc= 32 K) is investigated. The metasurface resonance frequency (ωMM), determined by the SRR geometry, is swept through the JPR frequency (ωJPR= 1.53 THz) using a series of interchangeable tapes applied to the same single crystal. Terahertz reflectivity measurements on the resulting hybrid superconducting metamaterials (HSMMs) reveal anticrossing behavior characteristic of strong coupling. The experimental results, validated with numerical simulations, indicate a normalized Rabi frequency of ΩR= 0.29. Further, it is shown that HSMMs with ωMM> ωJPRprovide a route to couple to hyperbolic waveguide modes inc‐axis cuprate samples. This work informs future possibilities for optimizing the coupling strength of HSMMs and investigating nonlinear superconductivity under high field terahertz excitation. 
    more » « less
  4. Abstract The Rashba effect enables control over the spin degree of freedom, particularly in polar materials where the polar symmetry couples to Rashba‐type spin splitting. The exploration of this effect, however, has been hindered by the scarcity of polar materials exhibiting the bulk‐Rashba effect and rapid spin‐relaxation effects dictated by the D'yakonov–Perel mechanism. Here, a polar LiNbO3‐typeR3cphase of Bi1‐xIn1+xO3withx≈0.15–0.24 is stabilized via epitaxial growth, which exhibits a bulk‐Rashba effect with suppressed spin relaxation as a result of its unidirectional spin texture. As compared to the previously observed non‐polarPnmaphase, this polar phase exhibits higher conductivity, reduced bandgap, and enhanced dielectric and piezoelectric responses. Combining first‐principles calculations and multimodal magnetotransport measurements, which reveal weak (anti)localization, anisotropic magnetoresistance, planar‐Hall effect, and nonreciprocal charge transport, a bulk‐Rashba effect without rapid spin relaxation is demonstrated. These findings offer insights into spin‐orbit coupling physics within polar oxides and suggest potential spintronic applications. 
    more » « less
  5. Abstract The discovery of polar vortices and skyrmions in ferroelectric‐dielectric superlattices [such as (PbTiO3)n/(SrTiO3)n] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non‐polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli. Here, using advanced thin‐film deposition and an array of characterization and simulation approaches, polar vortices are realized in all‐ferroelectric trilayers, multilayers, and superlattices built from the fundamental building block of (PbTiO3)n/(PbxSr1−xTiO3)nwherein in‐plane ferroelectric polarization in the PbxSr1−xTiO3provides the appropriate boundary conditions. These superlattices exhibit substantially enhanced electromechanical and ferroelectric responses in the out‐of‐plane direction that arise from the ability of the polarization in both layers to rotate to the out‐of‐plane direction under field. In the in‐plane direction, the layers are found to be strongly coupled during switching and when heterostructured with ferroelectric‐dielectric building blocks, it is possible to produce multistate switching. This approach expands the realm of systems supporting emergent dipolar texture formation and does so with entirely ferroelectric materials thus greatly improving their responses. 
    more » « less