skip to main content

Title: Systemic consequences of disorder in magnetically self-organized topological MnBi 2 Te 4 /(Bi 2 Te 3 ) n superlattices
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.  more » « less
Award ID(s):
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
2D Materials
Page Range / eLocation ID:
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. 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. 
    more » « less
  2. Abstract

    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.

    more » « less
  3. Abstract Magnetic topological materials are promising for realizing novel quantum physical phenomena. Among these, bulk Mn-rich MnSb 2 Te 4 is ferromagnetic due to Mn Sb antisites and has relatively high Curie temperatures (T C ), which is attractive for technological applications. We have previously reported the growth of materials with the formula (Sb 2 Te 3 ) 1−x (MnSb 2 Te 4 ) x , where x varies between 0 and 1. Here we report on their magnetic and transport properties. We show that the samples are divided into three groups based on the value of x (or the percent septuple layers within the crystals) and their corresponding T C values. Samples that contain x < 0.7 or x > 0.9 have a single T C value of 15–20 K and 20–30 K, respectively, while samples with 0.7 < x < 0.8 exhibit two T C values, one (T C1 ) at ~ 25 K and the second (T C2 ) reaching values above 80 K, almost twice as high as any reported value to date for these types of materials. Structural analysis shows that samples with 0.7 < x < 0.8 have large regions of only SLs, while other regions have isolated QLs embedded within the SL lattice. We propose that the SL regions give rise to a T C1 of ~ 20 to 30 K, and regions with isolated QLs are responsible for the higher T C2 values. Our results have important implications for the design of magnetic topological materials having enhanced properties. 
    more » « less
  4. Abstract Results are reported for Mn intercalated Zr 2 Te 2 P, where x-ray diffraction , energy dispersive spectroscopy, and transmission electron microscopy measurements reveal that the van der Waals bonded Te–Te layers are partially filled by Zr and Mn ions. This leads to the chemical formulas Zr 0.07 Zr 2 Te 2 P and Mn 0.06 Zr 0.03 Zr 2 Te 2 P for the parent and substituted compounds, respectively. The impact of the Mn ions is seen in the anisotropic magnetic susceptibility, where Curie–Weiss fits to the data indicate that the Mn ions are in the divalent state. Heat capacity and electrical transport measurements reveal metallic behavior, but the electronic coefficient of the heat capacity ( γ Mn ≈ 36.6 mJ (mol·K 2 ) −1 ) is enhanced by comparison to that of the parent compound. Magnetic ordering is seen at T M ≈ 4  K, where heat capacity measurements additionally show that the phase transition is broad, likely due to the disordered Mn distribution. This transition also strongly reduces the electronic scattering seen in the normalized electrical resistance. These results show that Mn substitution simultaneously introduces magnetic interactions and tunes the electronic state, which improves prospects for inducing novel behavior in Zr 2 Te 2 P and the broader family of ternary tetradymites. 
    more » « less
  5. Abstract

    Van der Waals (vdW) heterostructures that pair materials with diverse properties enable various quantum phenomena. However, the direct growth of vdW heterostructures is challenging. Modification of the surface layer of quantum materials to introduce new properties is an alternative process akin to solid state reaction. Here, vapor deposited transition metals (TMs), Cr and Mn, are reacted with Bi2Se3with the goal to transform the surface layer to XBi2Se4(X = Cr, Mn). Experiments and ab initio MD simulations demonstrate that the TMs have a high selenium affinity driving Se diffusion toward the TM. For monolayer Cr, the surface Bi2Se3is reduced to Bi2‐layer and a stable (pseudo) 2D Cr1+δSe2layer is formed. In contrast, monolayer Mn can transform upon mild annealing into MnBi2Se4. This phase only forms for a precise amount of initial Mn deposition. Sub‐monolayer amounts dissolve into the bulk, and multilayers form stable MnSe adlayers. This study highlights the delicate energy balance between adlayers and desired surface modified layers that governs the interface reactions and that the formation of stable adlayers can prevent the reaction with the substrate. The success of obtaining MnBi2Se4points toward an approach for the engineering of other multicomponent vdW materials by surface reactions.

    more » « less