Nonreciprocal Transport with Quantum Geometric Origin in Layered Hybrid Perovskite

Abstract: Quantum geometry quantifies how the electron wavefunction evolves distinctly from conventional transport theory. In noncentrosymmetric materials, nonreciprocal transport with quantum geometric origin remains prominent with localized charge independent of vanished group velocity. The discovery of such nonreciprocal and nonlinear responses was realized by recent advances in two-dimensional materials. As a promising candidate, the electronic structure and symmetry of layered hybrid perovskites can be deliberately designed and manipulated by incorporating selected organic ligands. Despite the observation of exotic photogalvanic effects and chiral optical effects, the underlying mechanism how these nonlinear responses are enabled in the multi-quantum well structures remained unclear. Here we demonstrated the quantum geometric origin for interlayer spontaneous photocurrent in (PEA)2PbI4. Contrary to assumptions that charge transport across the 2D planes is limited, we observed a spontaneous photocurrent along this crystalline orientation. Theoretical analysis using a tight-binding model identifies shift current as the microscopic origin. This quantum geometric effect is enabled by ionic displacements from centrosymmetric coordinates and enhanced by multiband transition high-density bands of the layered hybrid crystal. We anticipate that such unique low-dimensional systems with structure can provide fertile ground for discovering novel optoelectronic functionalities.