Epitaxial films including bulk-like cubic and wurtzite polymorphs of MnSb have been grown by molecular beam epitaxy on GaAs via careful control of the Sb4/Mn flux ratio. Nonzero-temperature density functional theory was used to predict ab initio the spin polarization as a function of reduced magnetization for the half-metals NiMnSb and cubic MnSb. In both cases, half-metallicity is lost at a threshold magnetization reduction, corresponding to a temperature T * < TC . This threshold is far higher for cubic MnSb compared to NiMnSb and corresponds to T * > 350K, making epitaxial cubic MnSb a promising candidate for room temperature spin injection into semiconductors.Efficient electrical spin injection is crucial for the development of semiconductor (SC) spintronics, in which spin-polarized charge carriers flow from a ferromagnetic (FM) material into a non-magnetic SC structure. An ideal FM material would provide a fully spin polarized current [1] and should possess "engineering compatibility" with its SC host, which includes controllable epitaxy and interfaces, and suitability for device processing. Certain half-metallic ferromagnetic (HMF) materials have a density-of-states (DOS) spin polarisation at the Fermi level of P DOS = 100% due to the presence of a band gap straddling the Fermi energy E F for one spin channel only [2]. Density functional theory (DFT) has predicted this property in several classes of materials [1], including Heusler alloys and transition metal pnictides (TMPs), at temperature T = 0K. On this basis, half-metallicity was first envisaged in NiMnSb, which has a minority spin gap E g ≈ 0.5 eV [3]. However, there is presently no HMF candidate with SC engineering compatibility which clearly maintains P DOS ≈ 100% at room temperature.Experimental verification of P DOS is not straightforward and after more than two decades' study, P DOS (T ) for NiMnSb is not known. Positron annihilation experiments on bulk NiMnSb at T = 27K support P DOS ≈ 100% [4]. Spin polarized photoemission spectroscopy (SPPES) can, in principle, measure P DOS more directly but it is strongly affected by the magnetic, chemical and structural conditions of the surface, which may differ from those of the bulk. Threshold SPPES measured [20]. It is crucial to address the intrinsic limitations on P DOS . It has been realised that HMF band structures change as T increases, even well below the Curie temperature T C [21][22][23][24]. The DOS in the minority spin gap becomes nonzero as the thermal fluctuations produce disorder in the local spin moment alignment. In fact, beyond a threshold temperature T * < T C , the value of P DOS collapses far more rapidly than the reduction of magnetisation M (T ) [22].We report here the successful stabilization of bulklike c-MnSb and w-MnSb crystallites within fully relaxed n-MnSb films grown by molecular beam epitaxy (MBE) on GaAs(111). We confirm by DFT that these are HMF materials at T = 0K. However, we also calculate P DOS as a function of magnetization M (T ) using nonzero-temperature DFT, and...