Dimension Evolution of Self‐Assembled Organic Microcrystal for Laser and Polarization‐Rotation Function

Multidimensional integrated micro/nanostructures are vitally important for the implementation of versatile photonic functionalities, whereas current material structures still suffer undesired surface defects and contaminations in either multistep micro/nanofabrications or extreme synthetic conditions. Herein, the dimension evolution of organic self‐assembled structures 2D microrings and 3D microhelixes for multidimensional photonic devices is realized via a protic/aprotic solvent‐directed molecular assembly method based on a multiaxial confined‐assisted growth mechanism. The 2D microrings with consummate circle boundaries and molecular‐smooth surfaces function as high‐quality whispering‐gallery‐mode microcavities for dual‐wavelength energy‐influence‐dependent switchable lasing. Moreover, the 3D microhelixes with smooth surfaces and natural twistable characteristics act as active photon‐transport materials and polarization rotators. These results will broaden the horizon of constructing multidimensional microstructures for integrated photonic circuits. The dimension evolution of organic microcrystals is realized via a protic/aprotic solvent directed assembly method based on multiaxial confined‐assisted growth mechanism. Multidimensional structures exhibit the dimension‐dependent photonic properties: 2D microrings as dual‐wavelength lasing, 3D microhelixes as active photon‐transport materials and polarization rotators.