  Magnetic doping of semiconductor nanostructures is actively pursued for
applications in magnetic memory and spin-based electronics. Central to these
efforts is a drive to control the interaction strength between carriers
(electrons and holes) and the embedded magnetic atoms. In this respect,
colloidal nanocrystal heterostructures provide great flexibility via
growth-controlled `engineering' of electron and hole wavefunctions within
individual nanocrystals. Here we demonstrate a widely tunable magnetic sp-d
exchange interaction between electron-hole excitations (excitons) and
paramagnetic manganese ions using `inverted' core-shell nanocrystals composed
of Mn-doped ZnSe cores overcoated with undoped shells of narrower-gap CdSe.
Magnetic circular dichroism studies reveal giant Zeeman spin splittings of the
band-edge exciton that, surprisingly, are tunable in both magnitude and sign.
Effective exciton g-factors are controllably tuned from -200 to +30 solely by
increasing the CdSe shell thickness, demonstrating that strong quantum
confinement and wavefunction engineering in heterostructured nanocrystal
materials can be utilized to manipulate carrier-Mn wavefunction overlap and the
sp-d exchange parameters themselves.
