Molecular depth profiling of buried lipid bilayers using C(60)-secondary ion mass spectrometry.
An organic delta layer system made of alternating Langmuir-Blodgett multilayers of barium arachidate (AA) and barium dimyristoyl phosphatidate (DMPA) was constructed to elucidate the factors that control depth resolution in molecular depth profile experiments. More specifically, one or several bilayers of DMPA (4.4 nm) were embedded in relatively thick (51 to 105 nm) multilayer stacks of AA, resulting in a well-defined delta layer model system closely resembling a biological membrane. 3-D imaging time-of-flight secondary ion mass spectrometry (TOF-SIMS) depth profile analysis was performed on this system using a focused buckminsterfullerene (C(60)) cluster ion beam. The delta layer depth response function measured in these experiments exhibits similar features as those determined in inorganic depth profiling, namely an asymmetric shape with quasi-exponential leading and trailing edges and a central Gaussian peak. The effects of sample temperature, primary ion kinetic energy, and incident angle on the depth resolution were investigated. While the information depth of the acquired SIMS spectra was found to be temperature independent, the depth resolution was found to be significantly improved at low temperature. Ion induced mixing is proposed to be largely responsible for the broadening, rather than topography, as determined by atomic force microscopy (AFM); therefore, depth resolution can be optimized using lower kinetic energy, glancing angle, and liquid nitrogen temperature.
Department of Chemistry, Pennsylvania State University, 104 Chemistry Building, University Park, Pennsylvania 16802, United States.
Caiyan
C
Lu
Andreas
A
Wucher
Nicholas
N
Winograd
D004537:Eicosanoic Acids / Q000737:chemistry; D037741:Fullerenes / Q000737:chemistry*; D020404:Glycerophospholipids / Q000737:chemistry; D008051:Lipid Bilayers / Q000737:chemistry*; D013058:Mass Spectrometry / Q000379:methods*; D057054:Molecular Imaging; D013696:Temperature
D004537:Eicosanoic Acids; D037741:Fullerenes; D020404:Glycerophospholipids; D008051:Lipid Bilayers; C025602:dimyristoylphosphatidic acid; C069837:fullerene C60; C094477:arachidic acid