- The ability for optically active media to rotate the polarization of light is the basis of polarimetry, a prominent technique responsible for many breakthroughs in fields as varied as astronomy, medicine, and material science. Here, we recast the primary mechanism for spin readout in semiconductor-based quantum computers, Pauli spin-blockade (PSB), as the natural extension of polarimetry to the third dimension. We perform polarimetry with spins through a silicon quantum dot exchanging a hole with a boron acceptor, demonstrating the role of spin–orbit coupling in creating spin misalignment. Perfect spin alignment may be recovered by means of rotating the applied magnetic-field orientation. This work shows how spin misalignment sets a fundamental upper limit for the spin readout fidelity in quantum-computing systems based on PSB.