A monolayer of Se is deposited on Si(100) before high-k deposition. HfO2 and Al2O3 are deposited by 'gentle' methods of evaporation/oxidation, CVD and ALD. Significant improvement in interface and high-k properties are observed with Se, including suppression of interfacial oxide above 400C, reduction in leakage current by over an order of magnitude, reduction in C-V hysteresis by a factor of 2 and reduction in interface trap density by a factor of 5. Further improvement in thermal stability above 1,000C and EOT below 1 nm requires 1) a non-oxide high-k dielectric to prevent interfacial oxide and 2) an in-situ ultrahigh vacuum process for surface preparation and high-k deposition to prevent surface contamination.