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Christophe Testelin

Publications and source records attributed to Christophe Testelin.

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Magnetic interactions and origin of high Curie temperatures in high Mn content (MnSb2Te4)x(Sb2Te3)1-x quantum materials

Understanding the magnetic interactions that promote high TC in topological quantum materials is essential to effectively design materials whose magnetic configuration persists at high temperatures and are thus practical to integrate into commercial spintronic devices. Here we provide evidence of the origin of the high TC observed in mixed Mn1+ySb2-yTe4 septuple layers and Sb2-yMnyTe3 quintuple layer structures. Analysis of the quintuple layer/septuple layer structures explored their magnetic behavior through different models of Mn-incorporation in the crystal, evidenced as Mn spin S = 5/2, and provided an explanation for the low magnetization per Mn atom observed, signature of competing ferromagnetic and antiferromagnetic interactions between Mn2+ ions. Our studies provide insight to better understand and control the Mn incorporation in our samples to optimize their properties.

cond-mat.mtrl-sci

Hyperfine driven spin relaxation of charge carriers in metal-halide perovskites

Spin relaxation of localized charge carriers in semiconductors is primarily governed by hyperfine interaction with the surrounding nuclear spin bath. While this mechanism is well-established in III-V bulk materials and quantum dots, its critical role in metal halide perovskites (MHPs) has only recently emerged. Their inverted band structure induces an unusual hierarchy of hyperfine couplings, with hole interactions dominating electron interactions, particurlaly in Pb-based perovskites. Here, we adapt a spin relaxation model - originally developed for muon spin spectroscopy - to provide an exact description of longitudinal spin relaxation for localized carriers across arbitrary hyperfine correlation times. This approach is motivated by recent experimental evidence in MAPbI3, which places carrier spins in an intermediate correlation regime, where conventional mono-exponential approximations fail. Our analysis reveals distinct hyperfine relaxation channels: electrons couple primarily to halogen nuclei, whereas holes are governed by metal nuclei. This leads to a key prediction - perovskites with lighter halogens and metal cations exhibit significantly extended spin lifetimes. Applied to time-resolved Faraday rotation data obtained from two perovskite samples, our model extracts key microscopic parameters - including the carrier localization volume and hyperfine correlation time - demonstrating the necessity of the exact dynamical solution over a single-exponential approximation. These findings provide microscopic insight into hyperfine-driven spin relaxation in MHPs and establish a robust framework for characterizing carrier localization and spin dynamics.

cond-mat.mtrl-sci

Structural and magnetic properties of molecular beam epitaxy (MnSb2Te4)x(Sb2Te3)1-x topological materials with exceedingly high Curie temperature

Tuning magnetic properties of magnetic topological materials is of interest to realize elusive physical phenomena such as quantum anomalous hall effect (QAHE) at higher temperatures and design topological spintronic devices. However, current topological materials exhibit Curie temperature (TC) values far below room temperature. In recent years, significant progress has been made to control and optimize TC, particularly through defect engineering of these structures. Most recently we showed evidence of TC values up to 80K for (MnSb2Te4)x(Sb2Te3)1-x, where x is greater than or equal to 0.7 and less than or equal to 0.85, by controlling the compositions and Mn content in these structures. Here we show further enhancement of the TC, as high as 100K, by maintaining high Mn content and reducing the growth rate from 0.9 nm/min to 0.5 nm/min. Derivative curves reveal the presence of two TC components contributing to the overall value and propose TC1 and TC2 have distinct origins: excess Mn in SLs and Mn in Sb2-yMnyTe3QLs alloys, respectively. In pursuit of elucidating the mechanisms promoting higher Curie temperature values in this system, we show evidence of structural disorder where Mn is occupying not only Sb sites but also Te sites, providing evidence of significant excess Mn and a new crystal structure:(Mn1+ySb2-yTe4)x(Sb2-yMnyTe3)1-x. Our work shows progress in understanding how to control magnetic defects to enhance desired magnetic properties and the mechanism promoting these high TC in magnetic topological materials such as (Mn1+ySb2-yTe4)x(Sb2-yMnyTe3)1-x.

cond-mat.mtrl-sci

Compositional Control and Optimization of Molecular Beam Epitaxial Growth of (Sb2Te3)x(MnSb2Te4)y Magnetic Topological Insulators

Magnetic topological insulators such as MnBi2Te4 and MnSb2Te4 are promising hosts of novel physical phenomena such as quantum anomalous Hall effect and intrinsic axion insulator state, both potentially important for the implementation in topological spintronics and error-free quantum computing. In the bulk, the materials are antiferromagnetic but appropriate stacking with non-magnetic layers or excess Mn in the crystal lattice can induce a net ferromagnetic alignment. In this work we report the growth of (Sb2Te3)x(MnSb2Te4)y layers with varying Mn content by molecular beam epitaxy. The Mn flux fraction provided during growth controls the percent of MnSb2Te4 that is formed in the resulting layers by a self-assembly process. Highly crystalline layers with compositions varying between Sb2Te3 (y=0) and MnSb2Te4 (x=0) were obtained. The results show that Mn incorporates as a structural component to form MnSb2Te4, and as an impurity element both in Sb2Te3 and in MnSb2Te4. Two modifications of the growth conditions were implemented to enhance the incorporation of Mn as a structural element to form MnSb2Te4. Annealing of a thin portion of the layer at the beginning of growth (pre-anneal step), and increasing the growth temperature, both result in a larger percent of MnSb2Te4 for similar Mn flux fractions during growth. Samples having at least a few percent of MnSb2Te4 layers exhibit ferromagnetic behavior likely due to the excess Mn in the system which stabilizes on Sb sites as MnSb antisite defects.

cond-mat.mtrl-sci

Designer topological insulator with enhanced gap and suppressed bulk conduction in Bi2Se3/Sb2Te3 ultra-short period superlattices

A novel approach to reduce bulk conductance by the use of short period superlattices (SL) of two alternating topological insulator layers is presented. Evidence for a superlattice gap enhancement (SGE) was obtained from the observed reduction of bulk background doping by more than one order of magnitude, from 1.2x1020 cm-3 to 8.5x1018 cm-3 as the period of Bi2Se3/Sb2Te3 SLs is decreased from 12 nm to 5 nm, respectively. Tight binding calculations show that in the very thin period regime, a significant SGE can be achieved by the appropriate choice of materials. The ultrathin SL of alternating Bi2Se3 and Sb2Te3 layers behaves as a new designer material with a bulk bandgap as much as 60% larger than the bandgap of the constituent layer with the largest bandgap, while retaining topological surface features. Analysis of the weak antilocalization (WAL) cusp evident in the low temperature magneto-conductance of a very thin period SL sample grown confirms that the top and bottom surfaces of the SL structure behave as Dirac surface states. This approach represents a promising and yet to be explored platform for building truly insulating bulk TIs.

cond-mat.mtrl-sci

Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr$_3$ Single Crystal

Exciton fine structure splitting in semiconductors reflects the underlying symmetry of the crystal and quantum confinement. Since the latter factor strongly enhances the exchange interaction, most work has focused on nanostructures. Here, we report on the first observation of the bright exciton fine structure splitting in a bulk semiconductor crystal, where the impact of quantum confinement can be specifically excluded, giving access to the intrinsic properties of the material. Detailed investigation of the exciton photoluminescence and reflection spectra of a bulk methylammonium lead tribromide single crystal reveals a zero magnetic field splitting as large as $\sim 200\mu$eV. This result provides an important starting point for the discussion of the origin of the large bright exciton fine structure observed in perovskite nanocrystals.

cond-mat.mes-hall