Effect of Dual-Organic Cations on the Structure and Properties of 2D Hybrid Perovskites as Scintillators.

Two-dimensional (2D) hybrid organic-inorganic perovskite (HOIP) crystals show promise as scintillating materials for wide-energy radiation detection, outperforming their three-dimensional counterparts. In this study, we synthesized single crystals of (PEA2-xBZAx)PbBr4 (x ranging from 0.1 to 2), utilizing phenethylammonium (C6H5CH2CH2NH3+) and benzylammonium (C6H5CH2NH3+) cations. These materials exhibit favorable optical and scintillation properties, rendering them suitable for high light yield (LY) and fast-response scintillators. Our investigation, employing various techniques such as X-ray diffraction (XRD), photoluminescence (PL), time-resolved (TR) PL, Raman spectroscopy, radioluminescence (RL), thermoluminescence (TL), and scintillation measurements, unveiled lattice strain induced by dual-organic cations in powder X-ray diffraction. Density functional theory analysis demonstrated a maximal 0.13 eV increase in the band gap with the addition of BZA cation addition. Notably, the largest Stokes shift of 0.06 eV was observed in (BZA)2PbBr4. The dual-organic cation crystals displayed >80% fast component scintillation decay time, which is advantageous for the scintillating process. Furthermore, we observed a dual-organic cations-induced enhancement of electron-hole transfer efficiency by up to 60%, with a contribution of >70% to the fast component of scintillation decay. The crystal with the lowest BZA concentration, (PEA1.9BZA0.1)PbBr4, demonstrated the highest LYs of 14.9 ± 1.5 ph/keV at room temperature. Despite a 55-70% decrease in LY for BZA concentrations >5%, simultaneous reductions in scintillation decay time (12-32%) may work for time-of-flight positron emission tomography and photon-counting computed tomography. Our work underscores the crucial role of dual-organic cations in advancing our understanding of 2D-HOIP crystals for materials science and radiation detection applications.

Strain-induced topological phase transition in ferromagnetic Janus monolayer MnSbBiS2Te2.

We investigate a strain-induced topological phase transition in the ferromagnetic Janus monolayer MnSbBiS2Te2 using first-principles calculations. The electronic, magnetic, and topological properties are studied under biaxial strain within the range of -8 to +8%. The ground state of monolayer MnSbBiS2Te2 is metallic with an out-of-plane magnetic easy axis. A band gap is opened when a compressive strain between -4% and -7% is applied. We observe a topological phase transition at a biaxial strain of -5%, where the material becomes a Chern insulator exhibiting a quantum anomalous hall (QAH) effect. We find that biaxial strain and spin-orbit coupling (SOC) are responsible for the topological phase transition in MnSbBiS2Te2. In addition, we find that biaxial strain can alter the direction of the magnetic easy axis of MnSbBiS2Te2. The Curie temperature is calculated using the Heisenberg model and is found to be 24 K. This study could pave the way to the design of topological materials with potential applications in spintronics, quantum computing, and dissipationless electronics.

Anisotropic optical properties of single Si2Te3 nanoplates.

We report a combined experimental and computational study of the optical properties of individual silicon telluride (Si2Te3) nanoplates. The p-type semiconductor Si2Te3 has a unique layered crystal structure with hexagonal closed-packed Te sublattices and Si-Si dimers occupying octahedral intercalation sites. The orientation of the silicon dimers leads to unique optical and electronic properties. Two-dimensional Si2Te3 nanoplates with thicknesses of hundreds of nanometers and lateral sizes of tens of micrometers are synthesized by a chemical vapor deposition technique. At temperatures below 150 K, the Si2Te3 nanoplates exhibit a direct band structure with a band gap energy of 2.394 eV at 7 K and an estimated free exciton binding energy of 150 meV. Polarized reflection measurements at different temperatures show anisotropy in the absorption coefficient due to an anisotropic orientation of the silicon dimers, which is in excellent agreement with theoretical calculations of the dielectric functions. Polarized Raman measurements of single Si2Te3 nanoplates at different temperatures reveal various vibrational modes, which agree with density functional perturbation theory calculations. The unique structural and optical properties of nanostructured Si2Te3 hold great potential applications in optoelectronics and chemical sensing.

Predicting a Novel Phase of 2D SiTe2.

Layered IV-VI2 compounds often exist in a CdI2 structure. Using the evolution algorithm and first-principles calculations, we predict a novel layered structure of silicon ditelluride (SiTe2) that is more stable than the CdI2 phase. The structure has a triclinic unit cell in its bulk form. The atomic arrangement indicates the competition between the Si atoms' tendency to form tetrahedral bonds and the Te atoms' tendency to form hexagonal close-packing. The electronic and vibrational properties of the predicted phase are investigated. The effective mass of an electron is small among two-dimensional (2D) semiconductors, which is beneficial for applications such as field-effect transistors. The vibrational Raman and IR spectra are calculated to facilitate future experimental investigations.