NASA NTRS2004
We measured the growth velocities of the (110) face of tetragonal lysozyme, V (centimeters per second), at four different concentrations, c (milligrams per milliliter), as the solution temperature, T (Centigrade), was reduced. For a broad range of T dependent on c, we find that the growth velocities increased as the solution temperature was reduced. The initial increase in V is well characterized by the 2D nucleation model for crystal growth, yielding the magnitude of an effective barrier for growth, gamma(sub s) = 1.2 plus or minus 0.1 x 10(exp -13) erg/molecule. Below certain temperatures, T(sub cr), dependent on c, however, a kinetic roughening hypothesis that considers the continuous addition of molecules anywhere on the crystal surface better describes the observed growth velocities. The application of the continuous growth model, up to the solution cloud-point temperatures, T(sub cl), enabled the determinations of the crossover concentration, c(sub r), from estimated values of T(sub cr). For all conditions presented, we find that the crossover from growth by 2D nucleation to continuous addition occurs at a supersaturation, sigma (sub c), = 2.0 plus or minus 0.1. Moreover, we find the energy barrier for the continuous addition, E(sub c), within the temperature range T(sub cl) less than T less than T less than T (sub cr), to be 6 plus or minus 1 x 10(exp -13) erg/molecule. Further reduction of T below approximately 2-3 C of T(sub cl), also revealed a rapid slowing of crystal growth velocities. From quasi-elastic light scattering investigations, we find that the rapid diminishment of crystal growth velocities can be accounted for by the phase behavior of lysozyme solutions. Namely, we find the reversible formation of dense fluid proto-droplets comprised of lysozyme molecules to occur below approximately 0.3 C of T(sub cl). Hence, the rapid slowing of growth velocities may occur as a result of the sudden depletion of "mobile" molecules within crystal growth solutions as dense fluid proto-droplets form.