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1. Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi 2 Te 4

   https://doi.org/10.1002/adma.202202841  

   Padmanabhan, Hari ; Stoica, Vladimir A. ; Kim, Peter K. ; Poore, Maxwell ; Yang, Tiannan ; Shen, Xiaozhe ; Reid, Alexander H. ; Lin, Ming‐Fu ; Park, Suji ; Yang, Jie ; et al ( November 2022 , Advanced Materials)

   Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi₂Te₄, a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi‐Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto‐optic measurements show that the p states demagnetize via electron‐phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X‐ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. By quantifying this exchange coupling, this study validates the materials‐by‐design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

    

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2. A generic dual d-band model for interlayer ferromagnetic coupling in a transition-metal doped MnBi 2 Te 4 family of materials

   https://doi.org/10.1039/D2NR03283J  

   Zhang, Huisheng ; Zhang, Jingjing ; Zhang, Yaling ; Yang, Wenjia ; Wang, Yingying ; Xu, Xiaohong ; Liu, Feng ( September 2022 , Nanoscale)

   Realization of ferromagnetic (FM) interlayer coupling in magnetic topological insulators (TIs) of the MnBi 2 Te 4 family of materials (MBTs) may pave the way for realizing the high-temperature quantum anomalous Hall effect (high- T QAHE). Here we propose a generic dual d-band (DDB) model to elucidate the energy difference (Δ E = E AFM − E FM ) between the AFM and FM coupling in transition-metal (TM)-doped MBTs, where the valence of TMs splits into d-t 2g and d-e g sub-bands. Remarkably, the DDB shows that Δ E is universally determined by the relative position of the dopant (X) and Mn d-e g / t 2g bands, . If Δ E d > 0, then Δ E > 0 and the desired FM coupling is favored. This surprisingly simple rule is confirmed by first-principles calculations of hole-type 3d and 4d TM dopants. Significantly, by applying the DDB model, we predict the high- T QAHE in the V-doped Mn 2 Bi 2 Te 5 , where the Curie temperature is enhanced by doubling of the MnTe layer, while the topological order mitigated by doping can be restored by strain. 

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3. Electrically and magnetically switchable nonlinear photocurrent in РТ-symmetric magnetic topological quantum materials

   https://doi.org/10.1038/s41524-020-00462-9  

   Wang, Hua ; Qian, Xiaofeng ( December 2020 , npj Computational Materials)

   Nonlinear photocurrent in time-reversal invariant noncentrosymmetric systems such as ferroelectric semimetals sparked tremendous interest of utilizing nonlinear optics to characterize condensed matter with exotic phases. Here we provide a microscopic theory of two types of second-order nonlinear direct photocurrents, magnetic shift photocurrent (MSC) and magnetic injection photocurrent (MIC), as the counterparts of normal shift current (NSC) and normal injection current (NIC) in time-reversal symmetry and inversion symmetry broken systems. We show that MSC is mainly governed by shift vector and interband Berry curvature, and MIC is dominated by absorption strength and asymmetry of the group velocity difference at time-reversed ±kpoints. Taking$${\cal{P}}{\cal{T}}$$$PT$-symmetric magnetic topological quantum material bilayer antiferromagnetic (AFM) MnBi₂Te₄as an example, we predict the presence of large MIC in the terahertz (THz) frequency regime which can be switched between two AFM states with time-reversed spin orderings upon magnetic transition. In addition, external electric field breaks$${\cal{P}}{\cal{T}}$$$PT$symmetry and enables large NSC response in bilayer AFM MnBi₂Te₄, which can be switched by external electric field. Remarkably, both MIC and NSC are highly tunable under varying electric field due to the field-induced large Rashba and Zeeman splitting, resulting in large nonlinear photocurrent response down to a few THz regime, suggesting bilayer AFM-zMnBi₂Te₄as a tunable platform with rich THz and magneto-optoelectronic applications. Our results reveal that nonlinear photocurrent responses governed by NSC, NIC, MSC, and MIC provide a powerful tool for deciphering magnetic structures and interactions which could be particularly fruitful for probing and understanding magnetic topological quantum materials.

    

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4. Systemic consequences of disorder in magnetically self-organized topological MnBi 2 Te 4 /(Bi 2 Te 3 ) n superlattices

   https://doi.org/10.1088/2053-1583/ac3cc6  

   Sitnicka, Joanna ; Park, Kyungwha ; Skupiński, Paweł ; Grasza, Krzysztof ; Reszka, Anna ; Sobczak, Kamil ; Borysiuk, Jolanta ; Adamus, Zbigniew ; Tokarczyk, Mateusz ; Avdonin, Andrei ; et al ( December 2021 , 2D Materials)

   Abstract MnBi 2 Te 4 /(Bi 2 Te 3 ) n materials system has recently generated strong interest as a natural platform for the realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic (FM) MnBi 2 Te 4 /(Bi 2 Te 3 ) n it is found that migration of Mn between MnBi 2 Te 4 septuple layers (SLs) and otherwise non-magnetic Bi 2 Te 3 quintuple layers (QLs) has systemic consequences—it induces FM coupling of Mn-depleted SLs with Mn-doped QLs, seen in ferromagnetic resonance as an acoustic and optical resonance mode of the two coupled spin subsystems. Even for a large SL separation ( n ≳ 4 QLs) the structure cannot be considered as a stack of uncoupled two-dimensional layers. Angle-resolved photoemission spectroscopy and density functional theory studies show that Mn disorder within an SL causes delocalization of electron wave functions and a change of the surface band structure as compared to the ideal MnBi 2 Te 4 /(Bi 2 Te 3 ) n . These findings highlight the critical importance of inter- and intra-SL disorder towards achieving new QAH platforms as well as exploring novel axion physics in intrinsic topological magnets. 

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5. Tunable layered-magnetism–assisted magneto-Raman effect in a two-dimensional magnet CrI 3

   https://doi.org/10.1073/pnas.2012980117  

   Jin, Wencan ; Ye, Zhipeng ; Luo, Xiangpeng ; Yang, Bowen ; Ye, Gaihua ; Yin, Fangzhou ; Kim, Hyun Ho ; Rojas, Laura ; Tian, Shangjie ; Fu, Yang ; et al ( October 2020 , Proceedings of the National Academy of Sciences)

   null (Ed.)

   We used a combination of polarized Raman spectroscopy experiment and model magnetism–phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet CrI 3 . We reveal a layered-magnetism–assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in N -layer CrI 3 . We resolve in data and by calculations that the first-order A g phonon of the monolayer splits into an N -fold multiplet in N -layer CrI 3 due to the interlayer coupling ( N ≥ 2 ) and that the phonons within the multiplet show distinct magnetic field dependence because of their different layered-magnetism–phonon coupling. We further find that such a layered-magnetism–phonon coupled Raman scattering mechanism extends beyond first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higher-order multiphonons in N -layer CrI 3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin–phonon physics in van der Waals layered magnets. 

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