期刊
GEOCHIMICA ET COSMOCHIMICA ACTA
卷 312, 期 -, 页码 44-56出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.gca.2021.07.034
关键词
Biomarker; Molecular dynamic simulations; brGDGT; MBT; Terrestrial; Membrane; Bacteria
资金
- Royal Society Tata University Research Fellowship (URF)
- EPSRC [EP/M022609/1]
- BrisSynBio, a BBSRC/EPSRC Synthetic Biology Research Centre [BB/L01386X/1]
Branched glycerol dialkyl glycerol tetraethers (brGDGTs) are bacterial membrane lipids that are ubiquitous in the environment, and their degree of methylation is correlated with temperature, forming the basis of the brGDGT paleothermometer. Molecular dynamics simulations show that increasing the degree of methylation modulates membrane order and packing, making the membrane less rigid and more fluid. These findings support the hypothesis that the brGDGT paleothermometer is based on homeoviscous adaptation.
Branched glycerol dialkyl glycerol tetraethers (brGDGTs) are bacterial membrane lipids that are ubiquitous in the environment. Although the exact source organism is unknown, the distribution of brGDGTs in mineral soils, peats, and lake sediments is correlated with temperature through a decrease in the degree of methylation with increasing temperature. This empirical observation forms the basis of the brGDGT paleothermometer, one of the most important and widely used organic proxies to reconstruct terrestrial temperatures in the past. However, a mechanistic understanding to underpin this empirical correlation between the degree of methylation of brGDGT lipids and temperature is lacking, hindering a holistic understanding of the brGDGT paleothermometer as well as the membrane dynamics of their bacterial producers. To address this, here we present the first molecular dynamics simulations of membranes consisting of brGDGTs. Using intact polar lipid (IPL) brGDGTs with two sugar headgroups, our simulations demonstrate that increasing the degree of methylation modulates membrane order and packing, rendering the membrane less rigid and more fluid. These results indicate that the empirically observed correlation between the degree of methylation and temperature allows brGDGT-producing bacteria to maintain adequate membrane fluidity. Our simulations provide the first molecular simulation data to support the hypothesis that the brGDGT paleothermometer is based on homeoviscous adaptation. (C) 2021 The Authors. Published by Elsevier Ltd.
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