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The physics of interacting nuclear spins arranged in a crystalline lattice istypically described using a thermodynamic framework: a variety of experimentalstudies in bulk solid-state systems have proven the concept of a spintemperature to be not only correct but also vital for the understanding ofexperimental observations. Using demagnetization experiments we demonstratethat the mesoscopic nuclear spin ensemble of a quantum dot (QD) can in generalnot be described by a spin temperature. We associate the observed deviationsfrom a thermal spin state with the presence of strong quadrupolar interactionswithin the QD that cause significant anharmonicity in the spectrum of thenuclear spins. Strain-induced, inhomogeneous quadrupolar shifts also lead to acomplete suppression of angular momentum exchange between the nuclear spinensemble and its environment, resulting in nuclear spin relaxation timesexceeding an hour. Remarkably, the position dependent axes of quadrupolarinteractions render magnetic field sweeps inherently non-adiabatic, therebycausing an irreversible loss of nuclear spin polarization.

Demagnetization of Quantum Dot Nuclear Spins: Breakdown of the Nuclear Spin Temperature Approach