We propose a spin-density-matrix framework for probing anomalous interactions in top-quark pair production by exploiting the polarizations of the quark and the boson and their spin correlations. The -quark spin is analyzed through angular distributions in semileptonic decay following fragmentation, while the leptonic decay serves as a -polarization analyzer. We derive the spin density matrix in the presence of anomalous couplings and show that its polarization and spin-correlation parameters provide linear sensitivity to these couplings. We construct experimentally accessible angular observables associated with these parameters and evaluate their statistical sensitivities. For the HL-LHC at with an integrated luminosity of , the proposed method yields improved constraints on most anomalous couplings, with the sensitivity to enhanced by a factor of 8 and that to by a factor of about 6.

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