We employ dynamical mean-field theory to identify the materials properties that optimize Tc for a generalized double-exchange (DE) model. We reach the surprising conclusion that Tc achieves a maximum when the band angular momentum j equals 3/2 and when the masses in the mj = ±1/2 and ±3/2 sub-bands are equal. However, we also find that Tc is significantly reduced as the ratio of the masses decreases from one. Consequently, the search for dilute magnetic semiconductors (DMS) materials with high Tc should proceed on two fronts. In semiconductors with p bands, such as the currently studied Mn-doped Ge and GaAs semiconductors, Tc may be optimized by tuning the band masses through strain engineering or artificial nanostructures. On the other hand, semiconductors with s or d bands with nearly equal effective masses might prove to have higher Tc's than p-band materials with disparate effective masses.The discovery of dilute-magnetic semiconductors (DMS) with current transition temperatures above 170 K[1-3] initiated an active search for the optimal material for spintronic device applications [4]. However, the ferromagnetic transition temperature of magnetic semiconductors involves many parameters that are difficult to control experimentally. To facilitate the search for new magnetic semiconductors with high transition temperatures, we evaluate T c for a double-exchange system with general angular momentum j using dynamical mean-field theory (DMFT). Surprisingly, T c is found to reach a maximum for j = 3/2 and for equal light and heavy hole masses. However, we also find that T c decreases significantly when the ratio of the masses is reduced.The notion of using magnetic semiconductors in spintronic devices dates back to the 1960's, when europium chalcogenides [5] and chromium spinels [6] were extensively studied. Before the appearance of the latest generation of III-V DMS grown by molecular beam epitaxy techniques [1,2], II-VI [7] and IV-VI [8] DMS were developed by alloying non-magnetic semiconductors with magnetic ions. Improvement in growth techniques has pushed the T c of Ga 1−x Mn x As to values above 170 K [3]. As we discuss later, the large value of T c in deltadoped GaAs [9] might be associated with the reduced magnetic frustration when the Mn ions are restricted to two-dimensional planes.In our calculation we employ the DMFT, which was formulated in the late 1980's by and Metzner and Vollhardt [11]. It has since developed into one of the most powerful many-body techniques for studying electronic models such as the Hubbard [12,13] and DE [14-19] models. Since DMFT becomes exact in the dilute limit, it is a good starting point for studying DMS. Recent work on DMS materials has used DMFT to study variants of the DE model [20,21] with less than one local moment per site. A DE model with one local moment per site and large coupling constant J c provides an upper limit to the transition temperature for a system with exchange coupling between the local moments and charge carriers. Perhaps more importantly, the behavi...