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Lattice vibration in solids may carry angular momentum. But unlike theintrinsic spin of electrons, the lattice vibration is rarely rotational. Toinduce angular momentum, one needs to find a material that can accommodate atwisted normal mode, two orthogonal modes or excitation of magnons. Ifexcitation is too strong, one may exceed the Lindemann limit, so the materialmelts. Therefore these methods are not ideal. Here, we theoretically propose anew route to phonon angular momentum in a molecular crystal $\rm C_{60}$. Wefind that a single laser pulse is able to inject a significant amount ofangular momentum to $\rm C_{60}$, and the momentum transfer ishelicity-dependent. Changing from right-circularly polarized light toleft-circularly polarized light switches the direction of phonon angularmomentum. On the ultrafast time scale, the orbital angular momentum changeclosely resembles the displacive excitation of coherent phonons, with acosine-function dependence on time, different from the spin counterpart. Atomicdisplacements, even under strong laser excitation, remain far below theLindemann criterion. Under thermal excitation, spinning $\rm C_{60}$ even atroom temperature generates a huge angular momentum close to several hundred$\hbar$. Our finding opens the door to a large group of fullerenes, from $\rmC_{60}$, C$_{70}$ to their endohedral derivatives, where angular momentum canbe generated through light or temperature. This paves the way to the phononiccontrol electronic spin and harvesting thermal energy through phonon angularmomentum.

Optically- and thermally-driven huge lattice orbital and spin angular momenta from spinning fullerenes