This paper demonstrates a new chemically selective method for achieving high-resolution, area-selective atomic layer deposition (ALD) of Pt thin films on dielectrics. By utilizing the intrinsically selective adsorption behavior of 1-octadecene, a monolayer resist is attached only to the hydride-terminated silicon surfaces, but not to the oxide surfaces, of an oxide-patterned silicon substrate. Subsequently, a Pt thin film is selectively deposited only onto the non-deactivated oxide regions by ALD.ALD is a powerful thin-film growth technique that uses sequential self-terminating surface reaction steps to afford subnanometer control of the growth process. [1,2] It has received significant attention recently as a method for depositing highquality thin films of insulators, semiconductors, and metals. The surface-reaction-controlled deposition mechanism ensures precise control of the film thickness, excellent conformality, and very good uniformity over large areas. [2] In addition, many ALD processes are very sensitive to the conditions of the substrate surfaces. As a consequence, the surface functional groups can be manipulated prior to ALD to carry out an area-selective ALD process. Instead of a conventional subtractive-patterning strategy, area-selective ALD is an additive process, in which material is deposited only where needed. Figure 1 illustrates dual pathways for achieving area-selective ALD on a patterned SiO 2 /Si surface. Patterned SiO 2 /Si is an excellent starting substrate, because conventional photolithography can be used to form an oxide pattern of arbitrary design on silicon with a size down to the submicrometer scale. We will show that with the appropriate choice of chemistry, this single patterned substrate can be used to achieve either positive or negative pattern transfer using area-selective ALD. The overall processes of negative and positive patterning require two chemically selective steps. These two methods are complementary.The negative-patterning method shown in Figure 1 has been introduced previously.[3] In the prior work, octadecyltrichlorosilane (ODTS) was selectively attached to a SiO 2 surface as shown, leaving the hydride-terminated silicon surface unreacted. Subsequently, HfO 2 was deposited selectively by using the ALD process only on the hydride regions.[3]In this work, we utilize hydrosilylation chemistry of 1-alkenes on hydride-terminated silicon. The reaction is selective, leading to the adsorption of 1-alkene on the hydride surface but not on the oxide surface of a patterned silicon substrate. Subsequently, a thin film is selectively deposited only onto the oxide regions by ALD.We have focused on the deposition of Pt for the positivepatterning area-selective ALD method presented here. Pt is a promising electrode material for dynamic random-access memories because of its high chemical stability in an oxidizing atmosphere and its excellent electrical properties. [4,5] It is also a promising gate-metal candidate owing to its high work function (5.6 eV) and compatibility with high-...