Budding of crystalline domains in fluid membranes T. Kohyama, 1, * D. M. Kroll, 2 and G. Gompper 1 1 Institut fu ¨r Festko ¨rperforschung, Forschungszentrum Ju ¨lich, D-52425 Ju ¨lich, Germany 2 Supercomputing Institute, University of Minnesota, 599 Walter Library, 117 Pleasant Street S.E., Minneapolis, Minnesota 55455, USA Received 25 July 2003; published 17 December 2003 Crystalline domains embedded in fluid membrane vesicles are studied by Monte Carlo simulations of dynamically triangulated surfaces and by scaling arguments. A budding transition from a caplike state to a budded shape is observed for increasing spontaneous curvature C 0 of the crystalline domain as well as increasing line tension . The location of the budding transition is determined as a function of C 0 , , and the radius R A of the crystalline domain. In contrast to previous theoretical predictions, it is found that budding occurs at a value of the spontaneous curvature C 0 , that is always a decreasing function of the domain size R A . Several characteristic scaling regimes are predicted. The distribution of five- and sevenfold disclinations as the budding transition is approached is determined, and the dynamics of the generation of defects is studied. DOI: 10.1103/PhysRevE.68.061905 PACS numbers: 87.16.Dg, 64.70.Dv, 82.70.-y I. INTRODUCTION The primary new feature in two-component—compared to single-component—fluids is the possibility of phase sepa- ration. Canonically, mixtures have a lower miscibility gap, that is, the system is homogeneously mixed at high tempera- tures, but demixes at low temperatures into two coexisting phases that are enriched in one of the two components. How- ever, upper miscibility gaps and closed coexistence loops also exist, typically in systems in which the hydrophobic effect is important. The inverted phase behavior of these sys- tems is due to the orientational degrees of freedom of the water molecules, which are distributed isotropically at high temperatures, but have a preferred orientation in the neigh- borhood of polar solutes. It is therefore natural to expect phase separation in two- component amphiphilic membranes. Indeed, phase separa- tion in Langmuir monolayers at the water-air interface has been well documented for many years, and has been inves- tigated in considerable detail 1,2. However, in bilayer membranes, phase separation turns out to be much more dif- ficult to observe. Initial evidence showed gel-fluid coexist- ence in some systems 3, while fluid-fluid coexistence re- mained elusive for a long time. Only very recently have experiments using three-component membranes revealed very clear and convincing evidence for both gel-fluid 4,5 and fluid-fluid 6,7coexistence. The coupling of phase separation and membrane shape in flexible bilayer membranes opens the possibility for the bud- ding of domains 8,9. The physical mechanism of this phe- nomenon is the competition between the line tension energy of the phase boundary and the curvature energy of the mem- brane. Since the curvature energy is scale invariant, so that the curvature energy of a spherical vesicle is independent of the vesicle radius, and the line tension energy is proportional to the domain perimeter, i.e., to the domain radius, it is im- mediately clear that a budding transition occurs when the domain radius R is on the order of /, where is the bend- ing rigidity and is the line tension. Similarly, a membrane patch with spontaneous curvature C 0 has a budding transi- tion at R 1/C 0 . The coexistence of two phases in biological membranes has also received considerable attention recently. The exis- tence of ‘‘lipid rafts’’ 10may indeed play an important role in the control of the activity of membrane proteins. Another kind of two-phase coexistence in biological membranes oc- curs when domains of adsorbed proteins form spontaneously. A famous, and biologically very important, example is the adsorption of clathrin molecules on the plasma membrane 11. Clathrin molecules assemble to form a regular hexago- nal network on the membrane surface 12–14. By forming first a coated pit and then a complete bud see Fig. 1, these clathrin coats control endo- and exocytosis, i.e., the forma- tion and detachment of small transport vesicles from the cell membrane. The formation of clathrin cages is therefore an example of the budding of crystalline membrane patches em- bedded in a fluid lipid membrane. *Permanent and present address: Department of Physics, Faculty of Education, Shiga University, Hiratsu 2-5-1, Otsu, Shiga 520- 0862, Japan. FIG. 1. Rounded clathrin-coated pits in normal chick fibroblasts adand coated pits on membrane fragments derived from cells that have been broken open and left in p H 7 buffer for 10 min at 25 °C before fixation and freeze drying ef. The width of the field of view of the individual pictures is 0.4 m. Reproduced from Ref. 14by copyright permission of The Rockefeller University Press. PHYSICAL REVIEW E 68, 061905 2003 1063-651X/2003/686/06190515/$20.00 ©2003 The American Physical Society 68 061905-1