We study the X -band EPR spectra of Co 2 + in single crystalline Zn 1-x Co x O (x = 0.001-0.075) thin films grown by plasma-assisted molecular beam epitaxy. By analyzing the EPR linewidth behavior we argue that the exchange-narrowing model, usually applied to Mn-based II-VI DMS, fails here and that a combined effect of exchange and dipolar broadening can explain the linewidth variation with Co content and temperature.PACS: 76.30.Fc Iron group (3d) ions and impurities (Ti-Cu).Keywords: electron paramagnetic resonance, diluted magnetic semiconductors.Diluted magnetic semiconductors (DMS), the magnetic properties of which are due to the substitution of cations by transition-metal (TM) ions, have become a focus of considerable interest in recent years as essential materials for practical semiconductor spintronic devices such as spin filters [1] or spin polarizers [2]. The theoretical predictions based on the local spin density approximation (LSDA), triggered extensive studies of ZnO:TM alloys with a special focus on ZnO:Co as the most promising candidate for a room-temperature ferromagnetic (FM) semiconductor [3]. Many experiments have been reported on this material fabricated by a variety of methods [4][5][6]; however, the magnetic properties of ZnO:Co still remain a controversial issue since the observed magnetic behavior appears to be strongly dependent on the preparation methods and is poorly reproducible. Ferromagnetism was reported for thin films and bulk samples of ZnO:Co with a very large spread of spontaneous magnetic moment from 6.1 m B /Co to 0.01 m B /Co accompanied by a Curie temperature well above room temperature [4][5][6][7][8][9]. At the same time the absence of ferromagnetism and paramagnetic behavior down to helium temperatures in ZnO:Co were claimed by many authors [10][11][12][13][14][15][16].On the theoretical side, LSDA has difficulties when applied to the magnetic state of TM-doped ZnO, since it does not account for correlations between d-electrons and leads to a semimetallic FM ground state. Quite surprisingly, an improved version of LSDA, LSDA + U also leads to controversial results as regards the exchange constant sign between Co 2 + ions in ZnO. Indeed, in their recent paper, Chanier et al. [17] show that the exchange constants, J out and J in , between nearest-neighbor (NN)Co ions in the ZnO wurtzite structure are both negative (AFM) and have the values -9 K and -21 K, respectively. In contrast, Lee and Chang [18] and Sluiter et al. [19] have detected a competition between FM J out and AFMThe EPR offers an interesting alternative to traditional magnetic and optical methods providing complementary information on the electronic properties of transition metals ions. For example, EPR is able to probe the exchange interactions between TM ions by studying the well known phenomenon of the exchange narrowing of an EPR line. In this case a broadened line, say, by the magnetic dipole interaction, H d , is narrowed by a fast dynamics resulting from the exchange coupling, J. This gives finally a lin...