Control over molecular crystal growth modes requires control over grow
th rates. Improvements in crystal size, morphology and defects due to
improved control over growth rates have been reported using a modifica
tion of the standard constant current method of electrocrystallization
. This modified method seeks to maintain a constant current density at
the crystal surface, using a theoretical approximation of the actual
time-dependence of the crystal surface area. In this paper, we present
direct experimental observations of the time dependence of the crysta
l surface area (and the location and rate of new growth) for single cr
ystals of (BEDT-TTF)(2)Cu(SCN)(2). Contrary to theory, we find that gr
owth at crystal faces normal to the high conductivity plane does not o
ccur uniformly but instead occurs primarily along electric field lines
. Our results illustrate the need for in-situ measurements to control
the current density at the crystal surface. The change in the effectiv
e surface area for oxidation due to the anisotropic conductivity of mo
lecular crystals is also discussed.