Coupled Rotary and Oscillatory Motion in a Second-Generation Molecular Motor Pd Complex

[Image: see text] Molecular machines offer many opportunities for the development of responsive materials and introduce autonomous motion in molecular systems. While basic molecular switches and motors carry out one type of motion upon being exposed to an external stimulus, the development of molecular systems capable of performing coupled motions is essential for the development of more advanced molecular machinery. Overcrowded alkene-based rotary molecular motors are an ideal basis for the design of such systems as they undergo a controlled rotation initiated by light allowing for excellent spatio-temporal precision. Here, we present an example of a Pd complex of a second-generation rotary motor whose Pd center undergoes a coupled oscillatory motion relative to the motor core upon rotation of the motor. We have studied this phenomenon by UV–vis, NMR, and density functional theory calculations to support our conclusions. With this demonstration of a coupled rotation–oscillation motion powered by a light-driven molecular motor, we provide a solid basis for the development of more advanced molecular machines integrating different types of motion in their operation.