Abstract

In antiferromagnetic spintronics where manipulation of the antiferromagnetic spins is a central technological challenge[1], it is important to understand the dynamic properties, especially their THz spin dynamics and the magnetic damping. While both experimental and theoretical investigations of the antiferromagnetic resonance began in 1950s[2], they have been recently revisited with more advanced experimental techniques [3,4] as well as with more rigorous theoretical treatments[5] in the context of emerging antiferromagnetic spintronics. In the early stage of the investigations, the state-of-art spectroscopy with a rather inefficient and weak far-infrared source[1] was employed to investigate various antiferromagnets, such as NiO, CoO, MnO, and Cr2O3. Although their high resonant frequencies have been experimentally confirmed, the experimental technique at the time was not sufficiently sensitive to withstand detail analyses of the spin dynamics and the magnetic damping. However, thanks to the recent development of the THz technologies, frequency-domain THz spectroscopies with much better sensitivity than before has now became accessible and affordable for investigating in more detail the spin dynamics in antiferromagnets.In this work, a frequency domain continuous wave THz spectroscopy system capable of scanning up to ω = 2 THz with the frequency resolution <10 MHz is employed to investigate the antiferromagnetic resonances. NiO-based materials are used to demonstrate controllability of the antiferromagnetic resonance properties, such as resonance frequency and linewidth, or Q-factor.First, we investigated temperature dependence of antiferromagnetic resonance and the damping in poly- and mono-crystalline NiO. The resonant frequency (~ 1THz at room temperature) was found to decrease with increasing temperature, which was nicely explained by the temperature dependence of the anisotropy with a power of the sublattice magnetization with the exponent n = 0.72. We also found the damping parameters to be α = 5.0 ± 0.4 x 10-4 and 7.4 ± 0.4 x 10-4 for the mono- and poly-crystalline samples, respectively. The remarkable difference in α depending on the crystallinity manifests the significance of the extrinsic damping in antiferromagnet[6].Second, we investigated the antiferromagnetic resonance in the cation-substituted NiO of Ni1-xMxO (M = Mn, Li, or Mg). We show the wide range tunability of the resonant frequency as well as the Q-factor by the magnetic doping (Mn2+ substitute), the non-magnetic doping (Mg2+ substitute), and the hole doping (Li+ substitute). We discuss the trends of how those different doping impact the antiferromagnetic resonance properties, which will be appreciated as a design guideline for THz materials adapting to various types of applications such as THz microwave absorbers and filters where the control of resonant frequency and Q-factor is important[7].Lastly, we investigated the spin pumping enhanced antiferromagnetic damping in the (NiO)1-xHMx (HM = Pt and Pd) granular systems (Fig. 1 (a)). The spin pumping effect due to antiferromagnetic dynamics at the THz frequency was quantitatively elucidated by characterizing the linewidth Δω of the (NiO)1-xHMx granular systems as a function of x (Fig. 1(b) and (c)). The mixing conductance of the NiO/Pt and NiO/Pd interface was found to be g↑↓= 12 nm-2 and 5 nm-2, respectively. Our experimental results resolved the missing part of the spin interaction physics in antiferromagnets at THz, i.e. the spin pumping effect. The experimental manifestation of the value of g↑↓ helps understanding various spin current transfer phenomena with antiferromagnets, and would further motivate and promote the antiferromagnetic spintronics[8].In summary, we explored frequency-domain THz spectroscopies of antiferromagnetic NiO and showed detail quantitative analysis of the antiferromagnetic damping, observation of the THz spin pumping effect in NiO/Pt and NiO/Pd and determination of the spin mixing conductance, and control of the antiferromagnetic resonance properties by various cation substations of NiO. These results are important milestone for future THz antiferromagnetic spintronicsThis work was supported in part by JSPS KAKENHI Grant Numbers 17H04924, 15H05702, 17H04795, 17H05181 (“Nano Spin Conversion Science”), by the Collaborative Research Program of Institute for Chemical Research, Kyoto University (grant # 2018-61 and 2019-87), and by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering under Award No. DE-SC0012190. **

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