Switchable Two‐Photon Pumped Polarized Lasing Performance in Composition‐Graded MOFs Based Heterostructures

Abstract The manipulation on dual‐/multi‐band multiphoton pumped lasing in a single microcrystal is critically essential and technologically needed, which still faces difficulties such as the lack of effective approaches to integrate various multiphoton gain media while avoiding undesirable energy transfer processes. Herein, for the first time, the switchable dual‐band two‐photon pumped (TPP) lasing is realized by constructing composition‐graded metal–organic frameworks (MOFs) heterostructures. The epitaxial growth strategy is adopted for the development of heterostructures, which achieves the hierarchical encapsulation of different linear dye molecules along the 1D channels, thereby effectively restraining unnecessary intermolecular interactions. Strong position dependence of emission response in such deliberately designed heterostructures is observed, enabling a switchable dual‐band TPP polarized lasing through precise selection on excited positions. Furthermore, the excitation wavelength dependence of emission also endows such heterostructures with switchable optical behaviors (two‐photon fluorescence or lasing) via controlling the incident wavelength. The novel heterostructures for switchable dual‐band TPP lasing with uniquely position‐dependent and excitation wavelength‐dependent features open an avenue to develop controllable miniaturized lasers and make such MOFs based micro‐lasers promising for practical applications in future optoelectronic devices.