There are distinct differences in the molecular
packing of phospholipid molecules in the inner and outer membrane
monolayers of small lipid vesicles; a small radius of curvature
imparts an asymmetry to the interface between these two monolayers.
I have used an amphiphilic fluorescent probe, N-[5- (dimethylamino)naphthalenyl-1-sulfonyl]glycine
(dansylglycine), to determine if this asymmetry in molecular packing
leads to the existence of different environments for fluorescent
probes resident in the membrane. Dansylglycine is highly sensitive
to the dielectric constant of its environment, and the fluorescence
signal from membrane-bound dye is distinct from that in the aqueous
medium. When dansylglycine is first mixed with vesicles, it rapidly
partitions into the outer monolayer; the subsequent movement of
dye into the inner monolayer is much slower. Because of the time
lag between the initial partitioning and the subsequent translocation,
it is possible to measure the emission spectrum from membrane-bound
dye before and after translocation, thus distinguishing the two
potential environments for dansylglycine molecules. In the outer
membrane monolayer of small dipalmitoylphosphatidylcholine vesicles,
dye fluorescence emission is maximal at 530 nm, corresponding
to a dielectric constant of 7 for the medium surrounding the fluorophore.
For dye in the inner monolayer, emission is maximal at 519 nm,
corresponding to a dielectric constant of 4.7. The results suggest
that water molecules are excluded more efficiently from the dye
binding sites of the inner membrane monolayer than they are from
those of the outer monolayer.