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Combinatorial methodology enables the generation of comprehensive and consistent data sets, compared with the ldquoone-composition-at-a-timerdquo approach. We demonstrate, for the first time, the combinatorial methodology applied to the work function (Phim) extraction for Ta1-xAlxNy alloys as metal gates on HfO2, for complementary metal-oxide-semiconductor applications, by automated measurement of over 2000 capacitor devices. Scanning X-ray microdiffraction indicates that a solid solution exists for the Ta1-xAlxNy libraries for 0.05 les x les 0.50. The equivalent oxide thickness maps offer a snapshot of gate stack thermal stability, which show that Ta1-xAlxNy alloys are stable up to 950degC . The Phim of the Ta1-xAlxNy libraries can be tuned as a function of gate metal composition over a wide (0.05 les x les 0.50) composition range, as well as by annealing. We suggest that Ta0.9Al0.1N1.24 gate metal electrodes may be useful for p-channel metal-oxide-semiconductor applications.