We report on an example of confined magnetic ions with long spin coherence near room temperature. This was achieved by confining single Mn2+ spins in colloidal semiconductor quantum dots (QDs) and by dispersing the QDs in a proton-spin free matrix. The controlled suppression of Mn–Mn interactions and minimization of Mn–nuclear spin dipolar interactions result in unprecedentedly long phase memory (TM ~ 8 μs) and spin–lattice relaxation (T1 ~ 10 ms) time constants for Mn2+ ions at T = 4.5 K, and in electron spin coherence observable near room temperature (TM ~ 1 μs).
The nanoscale design of quantum dots (QDs) requires advanced analytical techniques. However, those that are commonly used do not have sufficient sensitivity or spatial resolution. Here, we use magnetic resonance techniques combined with paramagnetic Mn impurities in PbS QDs for sensitive probing of the QD surface and environment. In particular, we reveal inequivalent proton spin relaxations of the capping ligands and solvent molecules, strengths and anisotropies of the Mn nuclear spin interactions, and Mn nuclei distances with ∼1 Å sensitivity. These findings demonstrate the potential of magnetically doped QDs as sensitive magnetic nanoprobes and the use of electron spins for surface sensing.
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