▎ 摘　　要

Ultrafast optical spin control allows gate operations to be performed within picosecond time scale, orders of magnitude faster than microwave or electrical control. Here, using high-level quantum chemical computations, we suggest several two-qubit logic gates based on the optically induced ultrafast spin-flip and spin-transfer processes on rhombic graphene nanoflakes (Co4-GNF). It is demonstrated that Co atoms chemisorbed on p-conjugated C atoms can significantly influence the spin properties of the system. The spin density of different energy levels is distributed on different Co atoms, thus opening channels for successful spin-transfer processes between the Co atoms. Reversible local spin-flip processes on each Co atom as well as global spin-transfer processes between the Co atoms are realized. By carefully combining the various spin-dynamics processes achieved in our Co4-GNF structure, both classical (OR, AND, NAND) and quantum (CNOT, SWAP) binary logic gates are constructed. All spin manipulation processes finish at the subpicosecond time scale with fidelities above 96%. This theoretical design, which is exclusively based on laser-induced ultrafast spin dynamics, represents a novel implementation of qubit manipulation and can thus pave the way towards the construction of nano magnetic logic circuits and spintronic devices.