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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. 

Tuning the properties of magnetic topological materials is of interest to realize exotic physical phenomena, new quantum phases and quasiparticles, and topological spintronic devices. However, current topological materials exhibit Curie temperature (TC) values far below those needed for practical applications. In recent years, significant progress has been made to control and optimize TC, particularly through defect-engineering of these structures. Most recently, we reported TC values up to 80 K for (MnSb2Te4)x(Sb2Te3)1−x when 0.7 ≤ x ≤ 0.85 by controlling the composition x and the Mn content in these structures during molecular beam epitaxy growth. In this study, we show further enhancement of the TC, as high as 100 K, by maintaining high Mn content and reducing the growth rate from 0.9 nm/min to 0.5 nm/min. Derivative curves of the Hall resistance and the magnetization reveal the presence of two TC components contributing to the overall value and suggest TC1 and TC2 have distinct origins: excess Mn in MnSb2Te4 septuple layers (SLs) and high Mn content in Sb2−yMnyTe3 quintuple layer (QL) alloys, respectively. To elucidate the mechanisms promoting higher TC values in this system, we show evidence of enhanced structural disorder due to the excess Mn that occupies not only Sb sites but also Te sites, leading to the formation of a new crystal structure for these materials. Learning to control defects that enhance desired magnetic properties and understanding the mechanisms that promote high TC in magnetic topological materials such as (Mn1+ySb2−yTe4)x(Sb2−yMnyTe3)1−x is of great importance to achieve practical quantum devices.