In summary, we have demonstrated that the concept of selective deposition can be applied not only to polyelectrolyte adsorption, but also to the deposition of charged particles on surfaces. By manipulating adsorption conditions, it is possible to direct two different sets of particles to different surface re- gions based on the manipulation of secondary interactions such as hydrophobicity and hydrogen bonding. This approach requires a balance between the use of interactions that can prevent deposition, such as steric and hydration forces or elec- trostatic repulsion, and those that encourage it. 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Soc. 2001, 123, 1101. [59] H. Zheng, M. F. Rubner, P. T. Hammond, Langmuir 2002, in press. Controlled Cluster Size in Patterned Particle Arrays via Directed Adsorption on Confined Surfaces** By Ilsoon Lee, Haipeng Zheng, Michael F. Rubner, and Paula T.Hammond* The precise positioning of colloidal particles in complex two- and three-dimensional (2D/3D) structures has attracted a great deal of attention for potential applications, such as opto- electronic devices, [1] photonic bandgap materials, [2] and bio- chip devices and sensors. [3] A number of methods have been successfully used to direct the assembly of colloidal particles onto patterned surfaces, including flow-induced packing into cavities of controlled dimensions and shape [4] to create highly 572 Ó WILEY-VCH Verlag GmbH, D-69469 Weinheim, 2002 0935-9648/02/0804-0572 $ 17.50+.50/0 Adv.Mater. 2002, 14, No. 8, April 18 COMMUNICATIONS ± [*] Prof. P. T. Hammond, Dr. I. Lee, Dr. H. Zheng Department of Chemical Engineering Massachusetts Institute of Technology Cambridge, Massachusetts 02139 (USA) E-mail: hammond@mit.edu Prof. M. F. Rubner Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge, Massachusetts 02139 (USA) [**] The authors acknowledge Felice Frankel at MIT for the optical micro- graph image of colloidal assembly (Fig. 3a) and general discussion on cap- turing meaningful images for science. Thanks also go to Dr. Insung Choi and Dr. Yongwoo Lee for the synthesis of EG-thiol and helpful discus- sions on alkanethiolate SAMs, and to Dr. Gyoo yul Jung for micro-filtra- tion of the colloidal solutions and for invaluable discussions on the poten- tial application of patterned arrays to biological application. Funding for this work is provided by the Microphotonics Research Center and the Center for Materials Science and Engineering at MIT.