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Probing Ordered Lipid Assemblies with Polarized Third-Harmonic-Generation Microscopy
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DOI：10.1103/PhysRevX.3.011002.png)
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Abstract
En 中文
Ordered lipid assemblies are responsible for important physiological functions including skin barrier and axon conductivity. However, techniques commonly used to probe molecular order such as X-ray scattering and nuclear magnetic resonance are not suited for in-situ tissue studies. Here, we identify and characterize a novel contrast mechanism in nonlinear optical microscopy which is sensitive to molecular ordering in multilamellar lipid vesicles (MLVs) and in samples obtained from human skin biopsy: polarized third-harmonic generation (P-THG). We develop a multiscale theoretical framework to calculate the anisotropic, nonlinear optical response of lipid arrays as a function of molecular order. This analysis reveals that conserved carbon-carbon bond and aliphatic tail directionality are the atomic-and molecular-scale sources of the observed P-THG response, respectively. Agreement between calculations and experiments on lipid droplets and MLVs validates the use of P-THG as a probe of lipid ordering. Finally, we show that P-THG can be used to map molecular ordering in the multilamellar, intercorneocyte lipid matrix of the stratum corneum of human skin. These results provide the foundation for the use of P-THG in probing molecular order and highlight a novel biomedical application of multiphoton microscopy in an optically accessible tissue relevant to monitoring lipid-related disorder. DOI: 10.1103/PhysRevX.3.011002
Keywords:
BOND-CHARGE CALCULATION
2ND-HARMONIC GENERATION
RAMAN-SCATTERING
IN-VIVO
BILAYERS
ORIENTATION
MOLECULES
VESICLES
COLLAGEN
DENSITY
Journal
IF:
15.7
Papers:
2.7K
Citations:
3.4W