Quantum oscillations in magnetically doped colloidal nanocrystals

Progress in the synthesis of colloidal quantum dots has recently provided access to entirely new forms of diluted magnetic semiconductors, some of which may find use in quantum computation. The usefulness of a spin qubit is defined by its Rabi frequency, which determines the operation time, and its coherence time, which sets the error correction window. However, the spin dynamics of magnetic impurity ions in colloidal doped quantum dots remain entirely unexplored. Here, we use pulsed electron paramagnetic resonance spectroscopy to demonstrate long spin coherence times of ∼0.9 µs in colloidal ZnO quantum dots containing the paramagnetic dopant Mn(2+), as well as Rabi oscillations with frequencies ranging between 2 and 20 MHz depending on microwave power. We also observe electron spin echo envelope modulations of the Mn(2+) signal due to hyperfine coupling with protons outside the quantum dots, a situation unique to the colloidal form of quantum dots, and not observed to date.