An electrohydrodynamic methodology has been developed that makes possi
ble the precise assembly of two- and three-dimensional colloidal cryst
als on electrode surfaces. Electrophoretically deposited colloidal par
ticles were observed to move toward one another over very large distan
ces (greater than five particle diameters) to form two-dimensional col
loidal crystals for both micrometer- and nanometer-size particles, Thi
s coalescence of particles with the same charge is opposite to what is
expected from electrostatic considerations and appears to result from
electrohydrodynamic fluid flow arising from an ionic current flowing
through the solution. The ability to modulate this ''lateral attractio
n'' between particles, by adjusting field strength or frequency, facil
itates the reversible formation of two-dimensional fluid and crystalli
ne colloidal states on the electrode surface. Further manipulation all
ows controlled structures to be assembled.