TY - JOUR
T1 - Subterahertz collective dynamics of polar vortices
AU - Li, Qian
AU - Stoica, Vladimir A.
AU - Paściak, Marek
AU - Zhu, Yi
AU - Yuan, Yakun
AU - Yang, Tiannan
AU - McCarter, Margaret R.
AU - Das, Sujit
AU - Yadav, Ajay K.
AU - Park, Suji
AU - Dai, Cheng
AU - Lee, Hyeon Jun
AU - Ahn, Youngjun
AU - Marks, Samuel D.
AU - Yu, Shukai
AU - Kadlec, Christelle
AU - Sato, Takahiro
AU - Hoffmann, Matthias C.
AU - Chollet, Matthieu
AU - Kozina, Michael E.
AU - Nelson, Silke
AU - Zhu, Diling
AU - Walko, Donald A.
AU - Lindenberg, Aaron M.
AU - Evans, Paul G.
AU - Chen, Long Qing
AU - Ramesh, Ramamoorthy
AU - Martin, Lane W.
AU - Gopalan, Venkatraman
AU - Freeland, John W.
AU - Hlinka, Jirka
AU - Wen, Haidan
N1 - Funding Information:
Acknowledgements We acknowledge discussions with M. Trigo, D. Xiao, Z. Hong, I. Luk’yanchuk and V. M. Vinokur. This work was primarily supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division: experimental design, data collection, data analysis, and part of simulations by Q.L. and H.W. were supported under the DOE Early Career Award; ultrafast measurements and sample synthesis by V.A.S., Y.Y., S.P., L.W.M., C.D., S.Y., A.L., L.-Q.C., V.G., J.W.F. and H.W. were supported under award no. DE-SC-0012375; ancillary ultrafast X-ray measurements by H.L., S.M., Y.A. and P.E. were supported under award no. DE-FG02-04ER46147. M.M., S.D., and R.R. acknowledge support for part of sample synthesis through the Quantum Materials programme (KC 2202) funded by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences Division under contract no. DE-AC02-05-CH11231. J.H. and M.P. were supported by the Czech Science Foundation (project no. 19-28594X) and acknowledge the access to computing facilities owned by parties and projects contributing to the National Grid Infrastructure MetaCentrum, provided under programme no. Cesnet LM2015042. T.Y. and L.-Q.C. acknowledge partial support from the US Department of Energy, Office of Science, Basic Energy Sciences, under award n0. DE-SC0020145 as part of the Computational Materials Sciences Program and from NSF under award DMR-1744213. Y.Z. and H.W. acknowledge support by ANL-LDRD for preliminary X-ray measurements. Q.L. acknowledges support by the Basic Science Center Project of NSFC under grant no. 51788104 for completing phase-field simulations at Tsinghua University. S.M. acknowledges support from the Office of Science Graduate Student Research (SCGSR) programme (DOE contract no. DE‐SC0014664) and from the UW-Madison Materials Research Science and Engineering Center (NSF DMR-1720415). H.L. acknowledges support by the National Research Foundation of Korea under grant 2017R1A6A3A11030959. Use of the Linac Coherent Light Source is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. Use of the Advanced Photon Source is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02– 06CH11357.
Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2021/4/15
Y1 - 2021/4/15
N2 - The collective dynamics of topological structures1–6 are of interest from both fundamental and applied perspectives. For example, studies of dynamical properties of magnetic vortices and skyrmions3,4 have not only deepened our understanding of many-body physics but also offered potential applications in data processing and storage7. Topological structures constructed from electrical polarization, rather than electron spin, have recently been realized in ferroelectric superlattices5,6, and these are promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics underlying the functionality of such complex extended nanostructures. Here, using terahertz-field excitation and femtosecond X-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders-of-magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices3. A previously unseen tunable mode, hereafter referred to as a vortexon, emerges in the form of transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond timescales. Its frequency is considerably reduced (softened) at a critical strain, indicating a condensation (freezing) of structural dynamics. We use first-principles-based atomistic calculations and phase-field modelling to reveal the microscopic atomic arrangements and corroborate the frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens opportunities for electric-field-driven data processing in topological structures with ultrahigh speed and density.
AB - The collective dynamics of topological structures1–6 are of interest from both fundamental and applied perspectives. For example, studies of dynamical properties of magnetic vortices and skyrmions3,4 have not only deepened our understanding of many-body physics but also offered potential applications in data processing and storage7. Topological structures constructed from electrical polarization, rather than electron spin, have recently been realized in ferroelectric superlattices5,6, and these are promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics underlying the functionality of such complex extended nanostructures. Here, using terahertz-field excitation and femtosecond X-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders-of-magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices3. A previously unseen tunable mode, hereafter referred to as a vortexon, emerges in the form of transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond timescales. Its frequency is considerably reduced (softened) at a critical strain, indicating a condensation (freezing) of structural dynamics. We use first-principles-based atomistic calculations and phase-field modelling to reveal the microscopic atomic arrangements and corroborate the frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens opportunities for electric-field-driven data processing in topological structures with ultrahigh speed and density.
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UR - http://www.scopus.com/inward/citedby.url?scp=85104264753&partnerID=8YFLogxK
U2 - 10.1038/s41586-021-03342-4
DO - 10.1038/s41586-021-03342-4
M3 - Article
C2 - 33854251
AN - SCOPUS:85104264753
SN - 0028-0836
VL - 592
SP - 376
EP - 380
JO - Nature
JF - Nature
IS - 7854
ER -