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We report on observations of spin dynamics in single Yb$^+$ ions immersed ina cold cloud of spin-polarized $^6$Li atoms. This species combination has beenproposed to be the most suitable system to reach the quantum regime in atom-ionexperiments. For $^{174}$Yb$^+$, we find that the atomic bath polarizes thespin of the ion by 93(4)\,\% after a few Langevin collisions, pointing tostrong spin-exchange rates. For the hyperfine ground states of $^{171}$Yb$^+$,we also find strong rates towards spin polarization. However, relaxationtowards the $F=0$ ground state occurs after 7.7(1.5) Langevin collisions. Weinvestigate spin impurity atoms as possible source of apparent spin-relaxationleading us to interpret the observed spin-relaxation rates as an upper limit.Using ab initio electronic structure and quantum scattering calculations, weexplain the observed rates and analyze their implications for the possibleobservation of Feshbach resonances between atoms and ions once the quantumregime is reached.

Dynamics of a single ion spin impurity in a spin-polarized atomic bath