Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes, or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a route to phonon angular momentum in a molecular crystal ${\mathrm{C}}_{60}$. We find that a single laser pulse is able to inject a significant amount of angular momentum to ${\mathrm{C}}_{60}$, and the momentum transfer is helicity dependent. Changing from right-circularly polarized light to left-circularly polarized light switches the direction of phonon angular momentum. On the ultrafast timescale, the orbital angular momentum change closely resembles the displacive excitation of coherent phonons, with a cosine-function dependence on time, different from the spin counterpart. Atomic displacements, even under strong laser excitation, remain far below the Lindemann criterion. Under thermal excitation, spinning ${\mathrm{C}}_{60}$ even at room temperature generates a huge angular momentum close to several hundred $\hslash$. Our finding opens the door to a large group of fullerenes, from ${\mathrm{C}}_{60},{\mathrm{C}}_{70}$ to their endohedral derivatives, where angular momentum can be generated through light or temperature. This paves the way to the phononic control electronic spin and harvesting thermal energy through phonon angular momentum.

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• Lattice dynamics
• Phonons
• Polarization of light
• Fullerenes
• Nanoparticles
• Optical absorption spectroscopy
• Ultrafast pump-probe spectroscopy