Abstract
With rational designability, versatile tunability, and quantum
coherence, molecular electron spin qubits could offer new opportunities
for quantum information science, enabling simplified implementation of
quantum algorithms and chemical-specific quantum sensing. The
development of these transformative technologies relies on coherent
addressing of single molecular electron spin qubits with high
initialization, manipulation, and readout fidelities. This is formidable
to conventional electron spin resonance spectroscopy, which is widely
used for coherent addressing of ensemble electron spins, due to its low
initialization efficiency and readout sensitivity. Taking advantage of
single spin detectability of single-molecule spectroscopy, scanning
tunneling microscopy, atomic force microscopy, and quantum metrology,
several strategies have been developed to empower electron spin
resonance spectroscopy with single qubit addressability. In this
Emerging Topic, we introduce principles and technical implementation of
strategies for coherently addressing single molecular electron spin
qubits and point out their challenges in molecular design and/or
decoherence suppression. We discuss future directions to overcome these
challenges and to improve single qubit addressing technologies, which
will facilitate the advancement of molecular quantum information
science.