Molecular Picture of the Transient Nature of Lipid Rafts.

In biological membranes, lipid rafts are now thought to be transient and nanoscopic. However, the mechanism responsible for these nanoscopic assemblies remains poorly understood, even in the case of model membranes. As a result, it has proven extremely challenging to probe the physicochemical properties of lipid rafts at the molecular level. Here, we use all-atom molecular dynamics (MD) simulations and inelastic X-ray scattering (IXS), an intrinsically nanoscale technique, to directly probe the energy transfer and collective short-wavelength dynamics (phonons) of biologically relevant model membranes. We show that the nanoscale propagation of stress in lipid rafts takes place in the form of collective motions made up of longitudinal (compression waves) and transverse (shear waves) molecular vibrations. Importantly, we provide a molecular picture for the so-called van der Waals mediated "force from lipid" [Anishkin, A. et al. Proc. Natl. Acad. Sci. U.S.A. 2014, 111, 7898], a key parameter for the ionic channel mechano-transduction and the mechanism for the lipid transfer of molecular level stress [Aponte-Santamaría, C. et al. J. Am. Chem. Soc. 2017, 139, 13588]. Specifically, we describe how lipid rafts are formed and maintained through the propagation of molecular stress, lipid raft rattling dynamics, and a relaxation process. Eventually, the rafts dissipate through the self-diffusion of lipids making up the rafts. We also show that the molecular stress and viscoelastic properties of transient lipid rafts can be modulated through the use of hydrophobic biomolecules such as melatonin and tryptophan. Ultimately, the herein proposed mechanism describing the molecular interactions for the formation and dissolution of lipid rafts may offer insights as to how lipid rafts enable biological function.

Functional lipid pairs as building blocks of phase-separated membranes.

Biological membranes exhibit a great deal of compositional and phase heterogeneity due to hundreds of chemically distinct components. As a result, phase separation processes in cell membranes are extremely difficult to study, especially at the molecular level. It is currently believed that the lateral membrane heterogeneity and the formation of domains, or rafts, are driven by lipid-lipid and lipid-protein interactions. Nevertheless, the underlying mechanisms regulating membrane heterogeneity remain poorly understood. In the present work, we combine inelastic X-ray scattering with molecular dynamics simulations to provide direct evidence for the existence of strongly coupled transient lipid pairs. These lipid pairs manifest themselves experimentally through optical vibrational (a.k.a. phononic) modes observed in binary (1,2-dipalmitoyl-sn-glycero-3-phosphocholine [DPPC]-cholesterol) and ternary (DPPC-1,2-dioleoyl-sn-glycero-3-phosphocholine/1-palmitoyl-2-oleoyl-glycero-3-phosphocholine [DOPC/POPC]-cholesterol) systems. The existence of a phononic gap in these vibrational modes is a direct result of the finite size of patches formed by these lipid pairs. The observation of lipid pairs provides a spatial (subnanometer) and temporal (subnanosecond) window into the lipid-lipid interactions in complex mixtures of saturated/unsaturated lipids and cholesterol. Our findings represent a step toward understanding the lateral organization and dynamics of membrane domains using a well-validated probe with a high spatial and temporal resolution.

Emergent Optical Phononic Modes upon Nanoscale Mesogenic Phase Transitions.

The investigation of phononic collective excitations in soft matter systems at the molecular scale has always been challenging due to limitations of experimental techniques in resolving low-energy modes. Recent advances in inelastic X-ray scattering (IXS) enabled the study of such systems with unprecedented spectral contrast at meV excitation energies. In particular, it has become possible to shed light on the low-energy collective motions in materials whose morphology and phase behavior can easily be manipulated, such as mesogenic systems. The understanding of collective mode behavior with a Q-dependence is the key to implement heat management based on the control of a sample structure. The latter has great potential for a large number of energy-inspired innovations. As a first step toward this goal, we carried out high contrast IXS measurements on a liquid crystal sample, D7AOB, which exhibits solid-like dynamic features, such as the coexistence of longitudinal and transverse phononic modes. For the first time, we found that these terahertz phononic excitations persist in the crystal, smectic A, and isotropic phases. Furthermore, the intermediate smectic A phase is shown to support a van der Waals-mediated nonhydrodynamic mode with an optical-like phononic behavior. The tunability of the collective excitations at nanometer-terahertz scales via selection of the sample mesogenic phase represents a new opportunity to manipulate optomechanical properties of soft metamaterials.

Ultrahigh energy resolution focusing monochromator for inelastic x-ray scattering spectrometer.

A further development of a focusing monochromator concept for X-ray energy resolution of 0.1 meV and below is presented. Theoretical analysis of several optical layouts based on this concept was supported by numerical simulations performed in the "Synchrotron Radiation Workshop" software package using the physical-optics approach and careful modeling of partially-coherent synchrotron (undulator) radiation. Along with the energy resolution, the spectral shape of the energy resolution function was investigated. It was shown that under certain conditions the decay of the resolution function tails can be faster than that of the Gaussian function.

Performance of a collimating L-shaped laterally graded multilayer mirror for the IXS analyzer system at NSLS-II.

The L-shaped laterally graded multilayer mirror is a vital part of the ultrahigh-energy and momentum-resolution inelastic X-ray scattering spectrometer at the National Synchrotron Light Source II. This mirror was designed and implemented as a two-dimensional collimating optic for the analyzer system. Its performance was characterized using a secondary large-divergence source at the 30-ID beamline of the Advanced Photon Source, which yielded an integrated reflectivity of 47% and a collimated beam divergence of 78 µrad with a source size of 10 µm. Numerical simulations of the mirror performance in tandem with the analyzer crystal optics provided details on the acceptance sample volume in forward scattering and defined the technical requirements on the mirror stability and positioning precision. It was shown that the mirror spatial and angular stability must be in the range <8.4 µm and <21.4 µrad, respectively, for reliable operation of the analyzer.

The landscape of Y chromosome polymorphisms in Russia.

BACKGROUND: The pattern of diversity for the Y chromosome provides a view of male-driven processes of dispersal and settlement. By virtue of the broad geographic continuity, the genetic signature of movements from Asia to Europe can be detected in populations of north-eastern Europe. AIM: To directly test previous hypotheses on the peopling of Russia, by considering a broader spectrum of potential diversity. SUBJECTS AND METHODS: A total of 636 unrelated males (24 samples) from geographically and ethnically defined populations of Russia, Belarus, Azerbaijan and Georgia were analysed for 16 Y-STR loci. Some of the populations represent more or less distinct isolates. RESULTS: Microsatellites alone can have the power of detecting Asian contributions to the gene pool of populations now residing in Europe. Within Europe, a greater heterogeneity among populations sharing the same language than between populations sharing the same ethnic affiliation was found. There was low diversity and marked population differentiation in some Altaic speakers. Sympatry eroded inter-ethnic differentiation. No regular decline in genetic similarity with geography was seen. CONCLUSION: Two layers of overall diversity represent a main feature of the genetic landscape of the population of the European portion of Russia.