Conformational behavior of linear DNA in the presence of dodecyldimethylami
ne oxide (DDAO), an amphiphile that exists either in a neutral or cationic
protonated form depending on the pH of aqueous solution, was examined. DNA
phase behavior in the presence of free DDAO and DDAO/dioleoyl phosphatidyle
thanolamine (DOPE) mixed vesicles was found to be strongly pH-dependent. Us
ing the fluorescence microscopy technique for the real-time visualization o
f DNA compaction process at the single-molecule level, a dramatic increase
in the surfactant concentration needed for the collapsing coil-globule tran
sition in individual DNAs was noticed as amphiphilic DDAO molecules are dep
rotonated by increasing the pH of an aqueous solution. A similar, but less
pronounced, effect was detected for DNA condensation in the presence of DDA
O-containing pH-sensitive mixed vesicles. In general, positively charged DD
AO ions in vesicular form behave as a more efficient DNA-condensing agent t
han those in the micellar form. The structures of corresponding DNA-lipid c
omplexes were studied by small-angle X-ray scattering (SAXS) and cryogenic
transmission electron microscopy (cryo-TEM) techniques and found to be hexa
gonal for the DNA-DDAO system and lamellar for the DNA-DDAO/DOPE mixed-vesi
cle system. When DNA was introduced to vesicular DDAO/DOPE solutions under
acidic conditions, it induced the disintegration of vesicles and formation
of multilamellar structures. Under alkaline conditions DNA showed no intera
ction with the neutral vesicles but induced their aggregation and flocculat
ion.