Modeling of resonant excitation of ferroelectric lattice subsystem by terahertz radiation under nonequilibrium conditions

Objectives. The search for a fundamentally new, fast, and least dissipative method for controlling the ferroic order parameter is a pressing and ambitious task of basic and applied research on the development of low-dissipation and high-speed functional elements of information systems operating at terahertz (THz) frequencies for 6G network technologies. The aim of the work is to study the conditions for modulating ferroelectric polarization using a short THz pulse. This will also include the influence of additional factors on the efficiency of the THz-induced dynamics of the ferroic order parameter, such as stationary heating and the application of an additional electric field to the ferroelectric.

Methods. The numerical simulation of resonant excitation of the lattice subsystem by THz radiation was performed for a Ba_0.8Sr_0.2TiO₃ ferroelectric film using the Landau–Khalatnikov equation system, and the equation of phonon mode oscillations with the phonon–phonon interaction as a driving force. The novelty of the proposed approach lies in the interaction of the THz pulse with a previously coherently excited phonon mode with a significant amplitude.

Results. The time dependencies were presented for the polarization and the effective amplitude of infrared-active mode oscillations with varying THz field parameters. The results also included constants of expansion of the thermodynamic potential of the nonequilibrium state in powers of order parameter in various exposure modes, including temperature changes and the application of an additional external electric field.

Conclusions. The approach proposed herein describes polarization switching under the action of a THz pulse with preliminary excitation of a coherent phonon by a femtosecond optical pulse. The most important parameter when determining the threshold effect of a THz pulse on phonon excitation is pulse energy (amplitude). In the region of small amplitudes, an increase in temperature does not exacerbate switching conditions.

1. Leitenstorfer A., Moskalenko A.S., Kampfrath T., Kono J., Castro-Camus E., Peng K., Qureshi N., Turchinovich D., Tanaka K., Markelz A.G., Havenith M., Hough C., Joyce H.J., Padilla W.J., Zhou B., Kim K-Y., Zhang X.-C., Uhd Jepsen P., Dhillon S., Vitiello M., Linfield E., Davies A.G., Hoffmann M.C., Lewis R., Tonouchi M., Klarskov P., Seifert T.S., Gerasimenko Y.A., Mihailovic D., Huber R., Boland J.L., Mitrofanov O., Dean P., Ellison B.N., Huggard P.G., Rea S.P., Walker C., Leisawitz D.T., Gao J.R., Li C., Chen Q., Valûsis G., Wallace V.P., Pickwell-MacPherson E., Shang X., Hesler J., Ridler N., Renaud C.C., Kallfass I., Nagatsuma T., Zeitler J.A., Arnone D., Johnston M.B., Cunningham J. The 2023 terahertz science and technology roadmap. J. Phys. D: Appl. Phys. 2023;56:223001(67 p.). https://doi.org/10.1088/1361-6463/acbe4c

2. Brekhov K., Bilyk V., Ovchinnikov A., Chefonov O., Mukhortov V., Mishina E. Resonant Excitation of the Ferroelectric Soft Mode by a Narrow-Band THz Pulse. Nanomaterials. 2023;13(13):1961. https://doi.org/10.3390/nano13131961

3. Monnai Y., Lu X., Sengupta K. Terahertz Beam Steering: from Fundamentals to Applications. J. Infrared, Milli. Terahz Waves. 2023;44(3):169–211. https://doi.org/10.1007/s10762-022-00902-1

4. Quy V.K., Chehri A., Quy N.M., Han N.D., Ban N.T. Innovative Trends in the 6G Era: A Comprehensive Survey of Architecture, Applications, Technologies, and Challenges. IEEE Access. 2023;11:39824–39844. https://doi.org/10.1109/ACCESS.2023.3269297

5. Katayama I., Aoki H., Takeda J., Shimosato H., Ashida M., Kinjo R., Kawayama I., Tonouchi M., Nagai M., Tanaka K. Ferroelectric Soft Mode in a SrTiO3 Thin Film Impulsively Driven to the Anharmonic Regime Using Intense Picosecond Terahertz Pulses. Phys. Rev. Lett. 2012;108(9):097401(5 p.). https://doi.org/10.1103/PhysRevLett.108.097401

6. Hoffmann M.C., Hwang H.Y., Brandt N.C., et al. Terahertz-induced Kerr-effect in Relaxor Ferroelectrics. MRS Online Proceedings Library. 2009;1230:408. https://doi.org/10.1557/PROC-1230-MM04-08

7. Yamakawa H., Miyamoto T., Morimoto T., Takamura N., Liang S., Yoshimochi H., Terashige T., Kida N., Suda M., Yamamoto H.M., Mori H., Miyagawa K., Kanoda K., Okamoto H. Terahertz-field-induced polar charge order in electronic type dielectrics. Nat. Commun. 2021;12:953(11 p.). https://doi.org/10.1038/s41467-021-20925-x

8. Hamm P., Meuwly M., Johnson S.L., Beaud P., Staub U. Perspective: THz-driven nuclear dynamics from solids to molecules. Struct. Dyn. 2017;4(6):061601(19 p.). https://doi.org/10.1063/1.4992050

9. Chen F., Zhu Y., Liu S., Qi Y., Hwang H.Y., Brandt N.C., Lu J., Quirin F., Enquist H., Zalden P., Hu T., Goodfellow J., Sher M.-J., Hoffmann M.C., Zhu D., Lemke H., Glownia J., Chollet M., Damodaran, Park J., Cai Z., Jung I.W., Highland M.J., Walko D.A., Freeland J.W., Evans P.G., Vailionis A., Larsson J., Nelson K.A., Rappe A.M., Sokolowski-Tinten K., Martin L.W., Wen H., Lindenberg A.M. Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3. Phys. Rev. B. 2016;94(18):180104(6 p.). https://doi.org/10.1103/PhysRevB.94.180104

10. Kozina M., Pancaldi M., Bernhard C., van Driel T., Glownia J.M., Marsik P., Radovic M., Vaz C.A.F., Zhu D., Bonetti S., Staub U., Hoffmann M.C. Local terahertz field enhancement for time-resolved x-ray diffraction. Appl. Phys. Lett. 2017;110(8):081106. https://doi.org/10.1063/1.4977088

11. Kozina M., van Driel T., Chollet M., Sato T., Glownia J.M., Wandel S., Radovic M., Staub U., Hoffmann M.C. Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO3. Struct. Dyn. 2017;4(5):054301(7 p.). https://doi.org/10.1063/1.4983153

12. Grishunin K.A., Ilyin N.A., Sherstyuk N.E., Mishina E.D., Kimel A., Mukhortov V.M., Ovchinnikov A.V., Chefonov O.V., Agranat M.B. THz Electric Field-Induced Second Harmonic Generation in Inorganic Ferroelectric. Sci. Rep. 2017;7(1):687. https://doi.org/10.1038/s41598-017-00704-9

13. Mankowsky R., von Hoegen A., Först M., Cavalleri A. Ultrafast Reversal of the Ferroelectric Polarization. Phys. Rev. Lett. 2017;118:197601(5 p.). https://doi.org/10.1103/PhysRevLett.118.197601

14. Bilyk V., Mishina E., Sherstyuk N., Bush A., Ovchinnikov A., Agranat M. Transient polarization reversal using intense THz pulse in silicon-doped lead germinate. Physica Status Solidi (RRL). Rapid Research Letters. 2021;15(1):2000460(5 p.). https://doi.org/10.1002/pssr.202000460

15. Landau L.D., Khalatnikov I.M. On anomalous absorption of sound near a second order phase transition point. Doklady Akademii Nauk SSSR. 1954;96:469–472 (in Russ.).

16. Juraschek D.M., Fechner M., Spaldin N.A. Ultrafast Structure Switching through Nonlinear Phononics. Phys. Rev. Lett. 2017;118:054101(5 p.). https://doi.org/10.1103/PhysRevLett.118.054101

17. Radaelli P.G. Breaking symmetry with light: Ultrafast ferroelectricity and magnetism from three-phonon coupling. Phys. Rev. B. 2018;97:085145(9 p.). https://doi.org/10.1103/PhysRevB.97.085145

18. Subedi А. Proposal for ultrafast switching of ferroelectrics using midinfrared pulses. Phys. Rev. B. 2015;92:214303(6 p.). https://doi.org/10.1103/PhysRevB.92.214303

19. Mertelj T., Kabanov V.V. Comment on “Ultrafast Reversal of the Ferroelectric Polarization”. Phys. Rev. Lett. 2019;123:129701. https://doi.org/10.1103/physrevlett.123.129701

20. Blinc R., Žekš B. Soft Modes in Ferroelectrics and Antiferroelectrics. Amsterdam: North–Holland Publishing Company; 1974, 317 p.

21. Abalmasov V.A. Ultrafast reversal of the ferroelectric polarization by a midinfrared pulse. Phys. Rev. B. 2020;101:014102(8 p.). https://doi.org/10.1103/PhysRevB.101.014102

22. Shirokov V.B., Yuzyuk Yu.I., Kalinchuk V.V., Lemanov V.V. Material constants of (Ba,Sr)TiO3 solid solutions. Fizika tverdogo tela. 2013;55(4):709–714 (in Russ.). https://elibrary.ru/rcsvjh ] [Shirokov V.B., Yuzyuk Yu.I., Kalinchuk V.V., Lemanov V.V. Material constants of (Ba,Sr)TiO3 solid solutions. Phys. Solid State. 2013;55:773–779. https://doi.org/10.1134/S1063783413040276 ]

23. Anokhin A.S., Yuzyuk Yu.I., Lyanguzov N.V., Razumnaya A.G., Stryukov D.V., Bunina O.A., Golovko Yu.I., Shirokov V.B., Mukhortov V.M., El Marssi M. Direct transition from the rhombohedral ferroelectric to the paraelectric phase in a (Ba,Sr)TiO3 thin film on a (111)MgO substrate. Europhysics Letters. 2015;112(4):47001(6 p). https://doi.org/10.1209/0295-5075/112/47001

24. Kwaaitaal M., Lourens D.G., Davies C.S., Kirilyuk A. Disentangling thermal birefringence and strain in the all-optical switching of ferroelectric polarization. Sci. Rep. 2024;14:24956(9 p.). https://doi.org/10.1038/s41598-024-75670-0