Characterizing G-type antiferromagnetism quantitatively with optical second harmonic generation

Shuai Xu; Cheng Ma; Kui-juan Jin; Qinghua Zhang; Sisi Huang; Yiru Wang; Xu He; Jiesu Wang; Donggang Xie; Qiulin Zhang; Er-Jia Guo; Chen Ge; Can Wang; Xiulai Xu; Lin Gu; Meng He; Guozhen Yang

doi:10.1038/s41377-025-01849-3

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Characterizing G-type antiferromagnetism quantitatively with optical second harmonic generation

Original Articles

- Characterizing G-type antiferromagnetism quantitatively with optical second harmonic generation
- Light: Science & Applications Vol. 14, Issue 6, Pages: 1718-1726(2025)
- Affiliations：
  
  1.Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
  2.University of Chinese Academy of Sciences, Beijing 100049, China
  3.Theoretical Materials Physics, Q-MAT, Université de Liège, Liège B-4000, Belgium
  4.Beijing Academy of Quantum Information Sciences, Beijing 100193, China
  5.State Key Laboratory for Mesoscopic Physics and Frontiers Science Center for Nano-optoelectronics, School of Physics, Peking University, Beijing 100871, China
  6.Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials, Department of Materials Science and Engineering, Tsinghua University, 100084 Beijing, China
- Author bio：
  
  Kui-juan Jin (kjjin@iphy.ac.cn)
- Funds：
- DOI：10.1038/s41377-025-01849-3
  CLC：
- Received：03 December 2024，
  
  Revised：08 March 2025，
  
  Accepted：24 March 2025，
  
  Published Online：22 April 2025，
  
  Published：30 June 2025
- Accepted：
Scan QR Code
Xu, S. et al. Characterizing G-type antiferromagnetism quantitatively with optical second harmonic generation. Light: Science & Applications, 14, 1718-1726 (2025).
DOI：

Xu, S. et al. Characterizing G-type antiferromagnetism quantitatively with optical second harmonic generation. Light: Science & Applications, 14, 1718-1726 (2025). DOI： 10.1038/s41377-025-01849-3.

摘要

Abstract

Antiferromagnetism has become a promising candidate for the next generation electronic devices due to its thermal stability

low energy consumption

and fast switching speed. However

the canceling of the net magnetic moment in antiferromagnetic order presents great challenge on quantitative characterization and modulation

hindering its investigation and application. In this work

utilizing the optical second harmonic generation (SHG) in a wide temperature range

the integrated differential phase contrast scanning transmission electron microscopy

and first-principles calculations

we performed a quantitative study on the evolution of non-collinear antiferromagnetic order in BiFeO

films with a series of strains. We found that the antiferromagnetic coupling was significantly enhanced

featured by the increase of Néel temperature from 428 K to 646 K

and by one order of enhancement of SHG intensity contributed from the G-type antiferromagnetic order by strain manipulation from -2.4% to +0.6%. We attributed the enhancement of the antiferromagnetic coupling to the enhancement of the superexchange interaction as the Fe-O-Fe bond angle approaches 180° when the in-plane lattice co

nstants increase

which might also result in a tendency from a non-collinear antiferromagnetic order to a collinear one. Our work not only bridges the antiferromagnetic order and the strain manipulation in epitaxial multiferroics

more importantly

also paves a way for quantitative characterization by SHG technology and the precise manipulation of antiferromagnetism.

关键词

Keywords

references

Němec, P. et al. Antiferromagnetic opto-spintronics. Nat. Phys. 14 , 229–241 (2018)..

Manchon, A. et al. Current-induced spin-orbit torques inferromagnetic and antiferromagnetic systems. Rev. Mod. Phys. 91 , 035004 (2019)..

Yang, H. et al. Two-dimensional materials prospects for non-volatile spintronic memories. Nature 606 , 663–673 (2022)..

Zhang, Y. et al. Ferrimagnets for spintronic devices: from materials to applications. Appl. Phys. Rev. 10 , 011301 (2023)..

Mostufa, S. et al. Spintronic devices for biomedical applications. npj Spintronics 2 , 26 (2024)..

Spaldin, N. A. & Ramesh, R. Advances in magnetoelectric multiferroics. Nat. Mater. 18 , 203–212 (2019)..

Srihari, N. V., Vinayakumar, K. B. & Nagaraja, K. K. Magnetoelectric coupling in bismuth ferrite—challenges and perspectives. Coatings 10 , 1221 (2020)..

Liu, Y. Q. et al. Cont rollable electrical, magnetoelectric and optical properties of BiFeO 3 via domain engineering. Prog. Mater. Sci. 127 , 100943 (2022)..

Fiebig, M., et al. The evolution of multiferroics. Nat. Rev. Mater. 1 , 16046 (2016)..

Bousquet, E. & Cano, A. Non-collinear magnetism & multiferroicity: the perovskite case. Phys. Sci. Rev. 8 , 479–508 (2023)..

Ortega, N. et al. Multifunctional magnetoelectric materials for device applications. J. Phys.: Condens. Matter 27 , 504002 (2015)..

Wang, N. et al. Structure, performance, and application of BiFeO 3 nanomaterials. Nano Micro Lett. 12 , 81 (2020)..

Fiebig, M., Pavlov, V. V. & Pisarev, R. V. Second-harmonic generation as a tool for studying electronic and magnetic structures of crystals: review. J. Opt. Soc. Am. B 22 , 96–118 (2005)..

Shen, Y. R. The Principles of Nonlinear Optics 1st edn, Vol. 576 (New York: Wiley, 1984).

Wang, Y. et al. Structural phase transition in monolayer MoTe 2 driven by electrostatic doping. Nature 550 , 487–491 (2017)..

Sun, Z. Y. et al. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI 3 . Nature 572 , 497–501 (2019)..

Zhang, X. S. et al. Light-induced electronic polarization in antiferromagnetic Cr 2 O 3 . Nat. Mater. 23 , 790–795 (2024)..

Huang, S. S. et al. Ferroelectric order evolution in freestanding PbTiO 3 films monitored by optical second harmonic generation. Adv. Sci. 11 , 2307571 (2024)..

Dähn, A., Hübner, W. & Bennemann, K. H. Symmetry analysis of the nonlinear optical response: second harmonic generation at surfaces of antiferromagnets. Phys. Rev. Lett. 77 , 3929–3932 (1996)..

Lim, S. C. Magnetic second-harmonic generation of an antiferromagnetic film. J. Opt. Soc. Am. B 19 , 1401–1410 (2002)..

Chauleau, J. Y. et al. Multi-stimuli manipulation of antiferromagnetic domains assessed by second-harmonic imaging. Nat. Mater. 16 , 803–807 (2017)..

Xu, S. et al. Magnetoelectric coupling in multiferroics probed by optical second harmonic generation. Nat. Commun. 14 , 2274 (2023)..

Nývlt, M., Bisio, F. & Kirschner, J. Second harmonic generation study of the antiferromagnetic NiO(001) surface. Phys. Rev. B 77 , 014435 (2008)..

Ni, Z. L. et al. Observation of giant surface second-harmonic generation coupled to nematic orders in the van der waals antiferromagnet FePS 3 . Nano Lett. 22 , 3283–3288 (2022)..

Infante, I. C. et al. Bridging multiferroic phase transitions by epitaxial strain in BiFeO 3 . Phys. Rev. Lett. 105 , 057601 (2010)..

Infante, I. C. et al. Multiferroic phase tr ansition near room temperature in BiFeO 3 films. Phys. Rev. Lett. 107 , 237601 (2011)..

Seo, J. W. et al. Antiferromagnetic LaFeO 3 thin films and their effect on exchange bias. J. Phys. Condens. Matter 20 , 264014 (2008)..

Park, J. G. et al. Structure and spin dynamics of multiferroic BiFeO 3 . J. Phys. Condens. Matter 26 , 433202 (2014)..

Tamilselvan, A. et al. Role of oxygen vacancy and Fe–O–Fe bond angle in compositional, magnetic, and dielectric relaxation on Eu-substituted BiFeO 3 nanoparticles. Dalton Trans. 43 , 5731–5738 (2014)..

Modak, P., Lahiri, D. & Sharma, S. M. Correlation between structure and ferromagnetism in nano-BiFeO 3 . J. Phys. Chem. C. 120 , 8411–8416 (2016)..

Yang, X. et al. Single-crystal BiFeO 3 nanoplates with robust antiferromagnetism. ACS Appl. Mater. Interfaces 10 , 5785–5792 (2018)..

Chu, H. et al. Linear magnetoelectric phase in ultrathin MnPS 3 probed by optical second harmonic generation. Phys. Rev. Lett. 124 , 027601 (2020)..

Gross, I. et al. Real-space imaging of non-collinear antiferromagnetic order with a single-spin magnetometer. Nature 549 , 252–256 (2017)..

Finco, A. et al. Imaging topological defects in a noncollinear antiferromagnet. Phys. Rev. Lett. 128 , 187201 (2022)..

Goodenough, J. B. Goodenough-kanamori rule. Scholarpedia 3 , 7382 (2008)..

Lazić, I., Bosch, E. G. T. & Lazar, S. Phase contrast STEM for thin samples: integrated differential phase contrast. Ultramicroscopy 160 , 265–280 (2016)..

Li, Z. B. et al. Integrated differential phase contrast (IDPC)-STEM utilizing a multi-sector detector for imaging thick samples. Microsc. Microanal. 28 , 611–621 (2022)..

Perdew, J. P. et al. Restoring the density-gradient expansion for exchange in solids and surfaces. Phys. Rev. Lett. 100 , 039902 (2008)..

Soler, J. M. et al. The SIESTA method for ab initio order- N materials simulation. J. Phys. Condens. Matter 14 , 2745–2779 (2002)..

García, A. et al. SIESTA: recent developments and applications. J. Chem. Phys. 152 , 204108 (2020)..

Liechtenstein, A. I., Anisimov, V. I. & Zaanen, J. Density-functional theory and strong interactions: orbital ordering in mott-hubbard insulators. Phys. Rev. B 52 , R5467–R5470 (1995)..

Gómez-Ortiz, F. et al. Compatibility of DFT+U with non-collinear magnetism and spin-orbit coupling within a framework of numerical atomic orbitals. Comput. Phys. Commun. 286 , 108684 (2023)..

Kornev, I. A. et al. Finite-temperature properties of multiferroic BiFeO 3 . Phys. Rev. Lett. 99 , 227602 (2007)..

Xu, B. et al. First-principles study of spin spirals in the multiferroic BiFeO 3 . Phys. Rev. B 103 , 214423 (2021)..

Van Setten, M. J. et al. The PseudoDojo: training and grading a 85 element optimized norm-conserving pseudopotential table. Comput. Phys. Commun. 226 , 39–54 (2018)..

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