Spin-optotronic Properties of Organometal Halide Perovskites

Spin is an intrinsic quantum mechanical property of fundamental particles including the electron. The spin property is intimately related to electronic and optical properties of molecules and materials. The combination of spin (magnetic), electronic, and optical properties of materials, such as organometal halide perovskites (OMHP), has attracted increasing attention, which has led to a new field termed spin-optotronics based on all three key properties. This growing field has implications in emerging technological applications across disciplines, including photonics, electronics, spintronics, quantum computation, and information storage. This Perspective provides a brief introduction to this field from both experimental and computational aspects, with a focus on the effect of spin on charge carrier dynamics in OMHP, a class of materials with novel properties and promising applications in a number of fields. For instance, recent studies have demonstrated the use of ultrafast laser techniques in probing the fundamental charge carrier dynamics in relation to spin properties. Because of strong spin-orbit coupling (SOC) and broken inversion symmetry that result in Rashba and Dresselhaus effects, OMHP are considered ideal for manipulating spin states for spin-optotronics applications. In the meantime, on the basis of first-principles calculations and effective model Hamiltonians, the Rashba splitting in locally polarized domains can result in spin-forbidden recombination with significantly slow transition rate due to the mismatch of spin and momentum. We summarize the state-of-the-art first-principles methods and their current limitations for ultrafast charge and spin dynamics for realistic solid-state systems in general. To conclude, we note some promising future research and development directions for both experimental and theoretical ultrafast spin dynamics studies of OMHP.