Enhancement of the electron spin polarization in a correlated two-layer two-dimensional electron system at a total Landau level filling factor of one is reported. Using resistively detected nuclear magnetic resonance, we demonstrate that the electron spin polarization of two closely-spaced two-dimensional electron systems becomes maximized when inter-layer Coulomb correlations establish spontaneous isospin ferromagnetic order. This correlation-driven polarization dominates over the spin polarizations of competing single-layer fractional Quantum Hall states under electron density imbalances.
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