 Supporting Information               Matthias Schade, Andrea Knoll, Alexander Vogel, Oliver Seitz, Jürgen Liebscher, Daniel Huster, Andreas Herrmann, and Anna Arbuzova 303K 308K 313K 318K 323K PNA-d 62 frequency / kHz PSM-d 31 –60 –40 –20 0 20 40 60 –60 –40 –20 0 20 40 60 –60 –40 –20 0 20 40 60 frequency / kHz frequency / kHz POPC-d 31     ! "    # $%$&’$"’’$ Spectra were recorded for temperatures between 303 K (30°C) and 323 K (50°C) in 5 K intervals. Three samples were prepared, in which either POPC, PSM, or the PNA_C16 were deuterated allowing the determination of the order parameters for each individual species. The spectra show the typical superposition of Pake doublets originating from the individual carbon positions. As expected, the spectra became narrower with increasing temperature due to a reduction in acyl chain order. Also the spectra of POPC are always narrower than those of PSM and PNA_C16 indicating that PSM and PNA_C16 have similar high order while the order of POPC is lower.   $%$&’$"’ (()*+ , - ./0 1 &*!2!$&  $3&*’3       . ,- At 16 °C the vesicle reveals phase separation with ld and lo domains indicated by the partitioning of C66NBD6PC into the ld domain (green fluorescence) and the partitioning of the PNA_C16/DNAc1_Rh hybrid into the lo domain of the vesicle (red fluorescence). ,2- Increasing the temperature to 40 °C induces mixing of all membrane components and an equal distribution of the PNA_C16/DNAc1_Rh hybrid. The dots with increased red fluorescence are presumably aggregates of PNA_C16 stuck to the membranes; such aggregates were observed in aging stocks of PNA_C16. Ratios between the fluorescence intensities lo/ld are given (see Material and Methods) only for 16 °C. Scale bars correspond to 10 =m.