Physiological Calcium Concentrations Slow Dynamics at the Lipid-Water Interface

Valentine, Mason L.; Cárdenas, Alfredo E.; Elber, Ron; Baiz, Carlos R.

doi:10.1016/j.bpj.2018.08.044

Cited by 37 publications

(45 citation statements)

References 80 publications

(157 reference statements)

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“…Recently, a 2D IR study on the effects of Ca 2+ at nearphysiological concentrations showed that interfacial dynamics were slowed down by Ca 2+ but only in membranes containing anionic lipids. 1 Absorption spectra recorded with isotopelabeled anionic lipids indicated that the spectroscopic changes observed were largely localized to the anionic lipids. Similarly, water SFG spectra revealed that NaCl-dependent changes in H-bonding occurred with anionic lipids.…”

Section: Transmembrane Peptides Modulate H-bond Structure and Dynamicsmentioning

confidence: 97%

“…R. Valentine, M. L. Cardenas, A. E. Elber, R. Baiz, C. R. Biophys. J.20181151541–1551 This investigation used isotope-edited ultrafast two-dimensional infrared spectroscopy to probe the lipid–water interface of lipid bilayers with and without Ca 2+ in solution. Results indicated a dependence of interfacial dynamics on the Ca 2+ concentration in anionic lipid species.…”

Section: Key Referencesmentioning

confidence: 99%

“…One prominent example is cations, which often accumulate near lipid membranes due to the presence of anionic lipid species. Recently, a 2D IR study on the effects of Ca 2+ at near-physiological concentrations showed that interfacial dynamics were slowed down by Ca 2+ but only in membranes containing anionic lipids . Absorption spectra recorded with isotope-labeled anionic lipids indicated that the spectroscopic changes observed were largely localized to the anionic lipids.…”

Section: Model Systems and Case Studiesmentioning

confidence: 99%

“…Where vibrational probes access different components of the membrane environment, the studies discussed here converge on several key conclusions: (1) Water dynamics near the interface are slow compared to those in bulk water; (2) Interfacial dynamics are sensitive to headgroup structure and membrane composition; (3) Ions, osmolytes, and transmembrane peptides all affect lipid interfacial dynamics; however the nature of the effect is difficult to predict as its origin depends on multiple factors. Ultrafast spectroscopy, interpreted through the lens of MD simulations, allows an atomistic interpretation of the membrane environment that is not accessible by either technique alone. − , …”

Section: Future Prospectsmentioning

confidence: 99%

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Ultrafast Dynamics at Lipid–Water Interfaces

2020

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Metrics & MoreArticle Recommendations * sı Supporting Information CONSPECTUS: Lipid membranes are more than just barriers between cell compartments; they provide molecular environments with a finely tuned balance between hydrophilic and hydrophobic interactions that enable proteins to dynamically fold and self-assemble to regulate biological function. Characterizing dynamics at the lipid−water interface is essential to understanding molecular complexities from the thermodynamics of liquid−liquid phase separation down to picosecond-scale reorganization of interfacial hydrogen-bond networks. Ultrafast vibrational spectroscopy, including two-dimensional infrared (2D IR) and vibrational sum-frequency generation (VSFG) spectroscopies, is a powerful tool to examine picosecond interfacial dynamics. Two-dimensional IR spectroscopy provides a bond-centered view of dynamics with subpicosecond time resolutions, as vibrational frequencies are highly sensitive to the local environment. Recently, 2D IR spectroscopy has been applied to carbonyl and phosphate vibrations intrinsically located at the lipid−water interface. Interface-specific VSFG spectroscopy probes the water vibrational modes directly, accessing H-bond strength and water organization at lipid headgroup positions. Signals in VSFG arise from the interfacial dipole contributions, directly probing headgroup ordering and water orientation to provide a structural view of the interface.In this Account we discuss novel applications of ultrafast spectroscopy to lipid membranes, a field that has experienced significant growth over the past decade. In particular, ultrafast experiments now offer a molecular perspective on increasingly complex membranes. The powerful combination of ultrafast, interface-selective spectroscopy and simulations opens up new routes to understanding multicomponent membranes and their function. This Account highlights key prevailing views that have emerged from recent experiments: (1) Water dynamics at the lipid−water interface are slow compared to those of bulk water as a result of disrupted H-bond networks near the headgroups. (2) Peptides, ions, osmolytes, and cosolvents perturb interfacial dynamics, indicating that dynamics at the interface are affected by bulk solvent dynamics and vice versa.(3) The interfacial environment is generally dictated by the headgroup structure and orientation, but hydrophobic interactions within the acyl chains also modulate interfacial dynamics. Ultrafast spectroscopy has been essential to characterizing the biophysical chemistry of the lipid−water interface; however, challenges remain in interpreting congested spectra as well as designing appropriate model systems to capture the complexity of a membrane environment.

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Section: Transmembrane Peptides Modulate H-bond Structure and Dynamicsmentioning

confidence: 97%

Section: Key Referencesmentioning

confidence: 99%

Section: Model Systems and Case Studiesmentioning

confidence: 99%

Section: Future Prospectsmentioning

confidence: 99%

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Ultrafast Dynamics at Lipid–Water Interfaces

2020

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“…Notably, intracellular Ca 2+ can interact with phosphatidylserine in physiological concentration and cause physico-chemical changes, altered hydration in the lipid-water-interface. This in turn alters lipid packing and may slow down interfacial dynamics 56 . Such changes might be useful for the Ca 2+ -dependent desensitization event of wild-type TRPV1.…”

Section: Discussionmentioning

confidence: 99%

Ratio of hydrophobic-hydrophilic and positive-negative residues at lipid-water-interface influences surface expression and channel-gating of TRPV1

Saha

Das

Divyanshi

et al. 2020

Preprint

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During evolution, TRPV1 has lost, retained or selected certain residues at Lipid-Water-Interface (LWI) and formed specific patterns there. The ratio of “hydrophobic-hydrophilic” and “positive-negative charged” residues at the inner LWI remains conserved throughout vertebrate evolution and play important role in regulating TRPV1 trafficking, localization and functions. Arg575 is an important residue as Arg575Asp mutant has reduced Capsaicin-sensitivity, surface expression, colocalization with lipid-raft markers, cell area, and increased cell lethality. This lethality is due to the disruption of the ratio between positive-negative charges there. Such lethality can be rescued by either using TRPV1-specfic inhibitor 5’-IRTX or by restoring the positive-negative charge ratio at that position, i.e. by introducing Asp576Arg mutation in Arg575Asp backbone. We propose that Arg575Asp mutant confers TRPV1 in a “constitutive-open-like” condition. These findings have broader implication in understanding the molecular basis of thermo-gating and channel-gating and the microenvironments involved in such process that goes erratic in different diseases.

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Rapid and Sequential Dual Oxime Ligation Enables De Novo Formation of Functional Synthetic Membranes from Water‐Soluble Precursors

et al. 2022

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Cell membranes define the boundaries of life and primarily consist of phospholipids. Living organisms assemble phospholipids by enzymatically coupling two hydrophobic tails to a soluble polar head group. Previous studies have taken advantage of micellar assembly to couple single-chain precursors, forming non-canonical phospholipids. However, biomimetic nonenzymatic coupling of two alkyl tails to a polar head-group remains challenging, likely due to the sluggish reaction kinetics of the initial coupling step. Here we demonstrate rapid de novo formation of biomimetic liposomes in water using dual oxime bond formation between two alkyl chains and a phosphocholine head group. Membranes can be generated from non-amphiphilic, water-soluble precursors at physiological conditions using micromolar concentrations of precursors. We demonstrate that functional membrane proteins can be reconstituted into synthetic oxime liposomes from bacterial extracts in the absence of detergent-like molecules.

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Physiological Calcium Concentrations Slow Dynamics at the Lipid-Water Interface

Cited by 37 publications

References 80 publications

Ultrafast Dynamics at Lipid–Water Interfaces

Ultrafast Dynamics at Lipid–Water Interfaces

Ratio of hydrophobic-hydrophilic and positive-negative residues at lipid-water-interface influences surface expression and channel-gating of TRPV1

Rapid and Sequential Dual Oxime Ligation Enables De Novo Formation of Functional Synthetic Membranes from Water‐Soluble Precursors

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