High-quality, large (10 cm long and 2.5 cm diameter), nuclear spectrometer grade Cd 0.9 Zn 0.1 Te (CZT) single crystals have been grown by a controlled vertical Bridgman technique using in-house zone refined precursor materials (Cd, Zn, and Te). A state-of-the-art computer model, multizone adaptive scheme for transport and phase-change processes (MASTRAP), is used to model heat and mass transfer in the Bridgman growth system and to predict the stress distribution in the as-grown CZT crystal and optimize the thermal profile. The model accounts for heat transfer in the multiphase system, convection in the melt, and interface dynamics. The grown semi-insulating (SI) CZT crystals have demonstrated promising results for high-resolution roomtemperature radiation detectors due to their high dark resistivity (r % 2.8 3 10 11 V cm), good charge-transport properties [electron and hole mobility-lifetime product, mt e % (2-5) 3 10 ÿ 3 and mt h % (3-5) 3 10 ÿ 5 respectively, and low cost of production. Spectroscopic ellipsometry and optical transmission measurements were carried out on the grown CZT crystals using two-modulator generalized ellipsometry (2-MGE). The refractive index n and extinction coefficient k were determined by mathematically eliminating the ;3-nm surface roughness layer. Nuclear detection measurements on the single-element CZT detectors with 241 Am and 137 Cs clearly detected 59.6 and 662 keV energies with energy resolution (FWHM) of 2.4 keV (4.0%) and 9.2 keV (1.4%), respectively.