Spin qubits of Cu(II) doped in Zn(II) metal-organic frameworks above microsecond phase memory time

With the aim of creating Cu(II) spin qubits in a rigid metal-organic framework (MOF), this work demonstrates a doping of 5 %, 2 %, 1 %, and 0.1 % mol of Cu(II) ions into a perovskite-type MOF [CH₆ N₃ ][Zn^II (HCOO)₃ ]. The presence of dopant Cu(II) sites are confirmed with anisotropic g-factors (g_x =2.07, g_y =2.12, and g_z =2.44) in the S=1/2 system by experimentally and theoretically. Magnetic dynamics indicate the occurrence of a slow magnetic relaxation via the direct and Raman processes under an applied field, with a relaxation time (τ) of 3.5 ms (5 % Cu), 9.2 ms (2 % Cu), and 15 ms (1 % Cu) at 1.8 K. Furthermore, pulse-ESR spectroscopy reveals spin qubit properties with a spin-spin relaxation (phase memory) time (T₂ ) of 0.21 μs (2 %Cu), 0.39 μs (1 %Cu), and 3.0 μs (0.1 %Cu) at 10 K as well as Rabi oscillation between M_S =±1/2 spin sublevels. T₂ above microsecond is achieved for the first time in the Cu(II)-doped MOFs. It can be observed at submicrosecond around 50 K. These spin relaxations are very sensitive to the magnetic dipole interactions relating with cross-relaxation between the Cu(II) sites and can be tuned by adjusting the dopant concentration.