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arXiv:2005.00647 · Science Advances

Optically pumped spin polarization as a probe of many-body thermalization

Daniela Pagliero, Pablo R. Zangara, Jacob Henshaw, Ashok Ajoy, Rodolfo Hector Acosta, Jeffrey A. Reimer, Alexander Pines, Carlos A. Meriles

Published May 1, 2020• 25 citations
arXivHTMLPDF

Abstract

C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings.

DOI
10.1126/sciadv.aaz6986

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C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings.
We study the role of dipolar interactions in the standard protocol used to achieve dynamic nuclear polarization (DNP). We point out that a critical strength of interactions is required to obtain significant nuclear hyperpolarization. Otherwise, the electron spins do not thermalize among each other, due to the incipient many-body localization transition in the electron spin system. Only when the interactions are sufficiently strong, in the so-called spin-temperature regime, they establish an effective thermodynamic behavior in the out-of-equilibrium stationary state. The highest polarization is reached at a point where the spin temperature is just not able to establish itself anymore. We provide numerical predictions for the level of nuclear hyperpolarization and present an analytical technique to estimate the spin temperature as a function of interaction strength and quenched disorder. We show that, at sufficiently strong coupling, nuclear spins perfectly equilibrate to the spin temperature that establishes among the spins of radicals.
Collision experiments employing a preparation and/or an analysis of spin polarization provide a powerful tool to study individual interaction mechanisms. For atoms or ions with nonvanishing nuclear moments the hyperfine interaction before and after the collision may affect the spin polarization and any collision-induced orientation and alignment, thereby substantially reducing experimentally observable effects. This disturbance can be avoided by applying an external magnetic field, as is demonstrated here for the inelastic collision process He+{\mathrm{He}}^{+}He++Na(\ensuremath{\uparrow}) \ensuremath{\rightarrow}He+{\mathrm{He}}^{+}He++Na∗{\mathrm{Na}}^{\mathrm{*}}Na∗(3p). Easily attainable magnetic field strengths are sufficient to decouple electronic and nuclear spins whereby the figure of merit for both, orientation and alignment, is increased by more than one order of magnitude.
We numerically study the hyperfine induced nuclear spin dynamics in a system of two coupled quantum dots in zero magnetic field. Each of the electron spins is considered to interact with an individual bath of nuclear spins via homogeneous coupling constants (all coupling coefficients being equal). In order to lower the dimension of the problem, the two baths are approximated by two single long spins. We demonstrate that the hyperfine interaction allows to utilize the nuclear baths for quantum information purposes. In particular, we show that it is possible to swap the nuclear ensembles on time scales of seconds and indicate that it might even be possible to fully entangle them. As a key result, it turns out that the larger the baths are, the more useful they become as a resource of quantum information. Interestingly, the nuclear spin dynamics strongly benefits from combining two quantum dots of different geometry to a double-dot setup.
We numerically study the hyperfine induced nuclear spin dynamics in a system of two coupled quantum dots in zero magnetic field. Each of the electron spins is considered to interact with an individual bath of nuclear spins via homogeneous coupling constants (all coupling coefficients being equal). In order to lower the dimension of the problem, the two baths are approximated by two single long spins. We demonstrate that the hyperfine interaction allows to utilize the nuclear baths for quantum information purposes. In particular, we show that it is possible to swap the nuclear ensembles on time scales of seconds and indicate that it might even be possible to fully entangle them. As a key result, it turns out that the larger the baths are, the more useful they become as a resource of quantum information. Interestingly, the nuclear spin dynamics strongly benefits from combining two quantum dots of different geometry to a double-dot setup.