The effect of indium tin oxide ͑ITO͒ surface treatment on hole injection in organic light-emitting diode with C60 as a buffer layer on ITO was studied. Double surface dipole layer was induced on oxygen plasma treated ITO surface, while no dipole formation was observed on ITO without surface treatment. Interfacial energy barrier between ITO and hole transport layer was reduced by 0.4 eV by C60 modification on oxygen plasma treated ITO surface, while there was no change of interfacial energy barrier by C60 on ITO without surface treatment. © 2006 American Institute of Physics. ͓DOI: 10.1063/1.2410224͔ C60 has been known as a n-type semiconductor and has long been used as a moderately strong electron acceptor in solar cells.1,2 Charge transfer from inorganic or metal to C60 can be easily induced and it can accept up to six electrons. In addition, it has a high electron mobility of 1 cm 2 / V s even though hole mobility is relatively low compared with other organic hole transport materials. ITO and N,diphenylbenzidine ͑NPB͒ was reduced by 0.5 eV by surface dipole formation.5 Our group applied C60 as a buffer layer on Al electrode and observed 0.9 eV decrease of interfacial energy barrier.6 Current density was increased by C60 buffer layer on Al and current efficiency was also improved by efficient hole injection from Al to light-emitting layer. Other than these, there have been other works about using C60 as a dopant for hole transport layer. 7,8 In this work, we investigated the relationship between ITO surface treatment and hole injection in C60 modified devices. Hole injection from ITO to NPB was correlated with surface treatment and C60 buffer layer and hole injection mechanism in C60 modified devices was clarified.Device configurations of ITO/ NPB͑100 nm͒ / Al and ITO/ C60/ NPB͑100 nm͒ / Al were used to study hole injection from ITO to NPB. C60 was evaporated at a deposition rate of 0.1 Å / s and NPB was evaporated at an evaporation rate of 1 Å / s. ITO substrates were exposed to oxygen plasma at a rf power of 100 W with O 2 flow rate of 50 SCCM ͑SCCM denotes cubic centimeter per minute at STP͒ after cleaning. Devices were encapsulated with glass lid and calcium oxide getter after organic and metal deposition. Current-voltage ͑I-V͒ characteristics of the devices were measured with keithley 0253A.C60 is an intrinsically nonpolar molecule with 60 carbon atoms on the spherical surface. However, it is a strong electron acceptor and can form a charge transfer complex with metals, leading to interfacial dipole formation between metal and C60.9 Hayashi et al. reported that the vacuum level of metals such as Au, Cu, and Ag was affected by deposition of C60 and it induced interfacial dipole formation due to strong interaction between metals and C60. There has been another study about the interaction between oxide and C60, 5 but the study could not give information about the relationship between ITO surface properties and hole injection in C60 modified devices. Therefore, hole injection in C60 modified devices was corre...