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Abstract X-ray photoelectron spectroscopy and high-resolution transmission electron microscopy have been used to determine interfacial properties of HfO2 and HfAlO gate dielectrics grown on InP by atomic layer deposition. An undesirable interfacial InPxOy layer is easily formed at the HfO2/InP interface, which can severely degrade the electrical performance. However, an abrupt interface can be achieved when the growth of the HfAlO dielectric on InP starts with an ultrathin Al2O3 layer. The valence and conduction band offsets for HfAlO/InP heterojunctions have been determined to be 1.87 ± 0.1 and 2.83 ± 0.1 eV, respectively. These advantages make HfAlO a potential dielectric for InP MOSFETs.