In this talk, I will review the field of fullerene-based quantum information processing. I will present progress on the synthesis, chemical functionalization and alignment of N@C60 and N@C70 in different matrices. Recently, we were able to align N@C60 and N@C70 derivatives in a liquid crystal matrix with ordering parameter Ozz = 0.61. With the aligned samples, we were able to achieve addressability of the available 4-electron spin levels in endohedral nitrogen by coherent manipulations.
Furthermore, these functionalized molecules give rise to endohedral fullerene qudits: multi-level computational units alternative to the conventional 2-level qubits. Qudits offer a larger state space for encoding information and thus can offer enhancement of quantum algorithm efficiency. Indeed, we were able to demonstrate the first ever geometric phase using pulsed EPR; something that was first proposed over 30 years ago!