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Repeated injection of spin polarized carriers in a quantum dot leads to thepolarization of nuclear spins, a process known as dynamic nuclear spinpolarization (DNP). Here, we report the first observation of p-shell carrierassisted DNP in single QDs at zero external magnetic field. The nuclear field -measured by using the Overhauser shift of the singly charged exciton state ofthe QDs - continues to increase, even after the carrier population in thes-shell saturates. This is also accompanied by an abrupt increase in nuclearspin buildup time as p-shell emission overtakes that of the s-shell. Weattribute the observation to p-shell electrons strongly altering the nuclearspin dynamics in the QD, supported by numerical simulation results based on arate equation model of coupling between electron and nuclear spin system. DNPwith p-shell carriers could open up avenues for further control to increase thedegree of nuclear spin polarization in QDs.

P-shell carriers assisted dynamic nuclear spin polarization in single quantum dots at zero external magnetic field