Abstract
Future information technologies, such as ultrafast data recording, quantum computation or spintronics, call for ever faster spin control by light1,2,3,4,5,6,7,8,9,10,11,12,13,14,15,16. Intense terahertz pulses can couple to spins on the intrinsic energy scale of magnetic excitations5,11. Here, we explore a novel electric dipole-mediated mechanism of nonlinear terahertz-spin coupling that is much stronger than linear Zeeman coupling to the terahertz magnetic field5,10. Using the prototypical antiferromagnet thulium orthoferrite (TmFeO3), we demonstrate that resonant terahertz pumping of electronic orbital transitions modifies the magnetic anisotropy for ordered Fe3+ spins and triggers large-amplitude coherent spin oscillations. This mechanism is inherently nonlinear, it can be tailored by spectral shaping of the terahertz waveforms and its efficiency outperforms the Zeeman torque by an order of magnitude. Because orbital states govern the magnetic anisotropy in all transition-metal oxides, the demonstrated control scheme is expected to be applicable to many magnetic materials.
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Acknowledgements
The authors thank M. Furthmeier for technical assistance, R.V. Pisarev and A.M. Balbashov for providing samples, T.L. Cocker for discussions and Th. Rasing for continuous support. S.B., M.H. and R.H. were supported by the European Research Council through ERC grant no. 305003 (QUANTUMsubCYCLE) and the Deutsche Forschungsgemeinschaft (DFG) through Collaborative Research Centre SFB 689. A.V.K., R.V.M. and A.K.Z. were supported by the European Community Seventh Framework Programme FP7-NMP-2011-SMALL-281043 (FEMTOSPIN), the European Research Council ERC (grant agreement no. 257280, Femtomagnetism), the Foundation for Fundamental Research on Matter (FOM) as well as the Netherlands Organization for Scientific Research (NWO) and the programme ‘Leading Scientist’ of the Russian Ministry of Education and Science (14.z50.31.0034). T.K. acknowledges the Deutsche Forschungsgemeinschaft and ERC for support through priority programme SPP 1538 and the ERC grant no. 681917 (TERAMAG), respectively.
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S.B., A.V.K., R.H. and R.V.M. conceived the study, carried out the experiments and analysed the data. A.K.Z. and R.V.M. developed the theoretical model. S.B., M.H., A.V.K., R.H. and R.V.M. wrote the manuscript with feedback from T.K. and A.K.Z. All authors discussed the results.
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Baierl, S., Hohenleutner, M., Kampfrath, T. et al. Nonlinear spin control by terahertz-driven anisotropy fields. Nature Photon 10, 715–718 (2016). https://doi.org/10.1038/nphoton.2016.181
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DOI: https://doi.org/10.1038/nphoton.2016.181
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