4H silicon carbide (SiC) polytype is preferred over other SiC polytypes for high-power, high-voltage, and high-frequency applications due to its superior electrical, thermal, and structural characteristics. In this manuscript, we provide a comprehensive study of the spin coupling dynamics between conduction electrons and nitrogen (N) donors in monocrystalline 4H SiC with various concentrations of uncompensated N donors from 1017 to 5 × 1019 cm−3 by continuous wave, pulsed electron paramagnetic resonance (EPR), and microwave perturbation techniques at T = 4.2–300 K. At low temperatures, two triplets due to N donors in cubic (Nk) hexagonal (Nh) positions and triplet arisen from spin-interaction between Nh and Nk were observed in 4H SiC having Nd − Na ≈ 1017 cm−3. A single S-line (S = 1/2) dominates the EPR spectra in all investigated 4H SiC monocrystals at high temperatures. It was established that this line occurs due to the exchange coupling of localized electrons (dominate at low temperatures) and non-localized electrons (dominate at high temperatures). The localized electrons were attributed to Nh for Nd − Na ≈ 1017 cm−3 and Nk donors for Nd − Na ≥ 5 × 1018 cm−3. We have concluded that the conduction electrons in 4H SiC monocrystals are characterized by g|| = 2.0053(3) and g = 2.0011(3) for Nd − Na ≤ 5 × 1018 cm−3 and g|| = 2.0057(3) and g = 2.0019(3) for Nd – Na ≈ 5 × 1019 cm−3. Using the theoretical fitting of the temperature variation of S-line EPR linewidth in 4H SiC having Nd – Na ≤ 5 × 1018 cm−3, the energy levels of 57–65 meV that correlate with the valley-orbit splitting values for Nk donors in 4H SiC monocrystals were obtained.

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