Self-organization mechanism in Bridgman-grown MnBi2Te4/(Bi2Te3)n: influence on layer sequence and magnetic properties

Abstract

The growth of high-quality magnetic topological insulator crystals by the Bridgman method remains challenging due to thermodynamic limitations inherent to this technique. Nevertheless, this approach continues to provide bulk materials with significantly reduced free carrier concentrations compared to epitaxial methods. Here, we investigate the Inverted Vertical Bridgman growth of MnBi₂Te₄/(Bi₂Te₃)_n crystals, with particular emphasis on the structural ordering of MnBi₂Te₄ septuple layers within the Bi₂Te₃ quintuple-layer matrix and its influence on magnetic properties. Through a detailed analysis of growth dynamics, we identify four distinct stages, including a turbulent flow regime promoting pure MnBi₂Te₄ phase, rapid MnTe precipitation reducing Mn content in the melt, a stationary growth phase supporting ordered stacking of septuple and quintuple layers, and a final stage marked by flow cessation and defect formation. We demonstrate that septuple layer spacing is inversely correlated with MnTe supersaturation due to the diffusion-limited incorporation of Mn in stationary growth phase. Magnetic characterization reveals antiferromagnetic ordering in pure MnBi₂Te₄ phase and in MnBi₂Te₄/Bi₂Te₃ heterostructure, with ferromagnetism emerging for wider septuple layer spacing. We determine critical temperatures for observed antiferromagnetic and ferromagnetic phase transitions and magnetic anisotropy constants for ferromagnetic samples. Our findings highlight key growth parameters governing magnetic and structural quality, offering a pathway to scalable synthesis of layered topological insulators with tunable magnetic properties.