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300(9) Å. In this case, the mass-dependent method did not permit us to determine reliable intermolecular parameters. The combination of experimental rotational constants and results of ab initio calculations thus proves to be very sensitive to examine the accuracy of structural determinations in intermolecular clusters, offering insight into other aggregates.A statistical method is developed to estimate the maximum amplitude of the base pair fluctuations in a three dimensional mesoscopic model for nucleic acids. The base pair thermal vibrations around the helix diameter are viewed as a Brownian motion for a particle embedded in a stable helical structure. The probability to return to the initial position is computed, as a function of time, by integrating over the particle paths consistent with the physical properties of the model potential. The zero time condition for the first-passage probability defines the constraint to select the integral cutoff for various macroscopic helical conformations, obtained by tuning the twist, bending, and slide motion between adjacent base pairs along the molecule stack. Applying the method to a short homogeneous chain at room temperature, we obtain meaningful estimates for the maximum fluctuations in the twist conformation with ∼10.5 base pairs per helix turn, typical of double stranded DNA helices. Untwisting the double helix, the base pair fluctuations broaden and the integral cutoff increases. The cutoff is found to increase also in the presence of a sliding motion, which shortens the helix contour length, a situation peculiar of dsRNA molecules.Model patchy particles have been shown to be able to form a wide variety of structures, including symmetric clusters, complex crystals, and even two-dimensional quasicrystals. Here, we investigate whether we can design patchy particles that form three-dimensional quasicrystals, in particular targeting a quasicrystal with dodecagonal symmetry that is made up of stacks of two-dimensional quasicrystalline layers. We obtain two designs that are able to form such a dodecagonal quasicrystal in annealing simulations. The first is a one-component system of seven-patch particles but with wide patches that allow them to adopt both seven- and eight-coordinated environments. The second is a ternary system that contains a mixture of seven- and eight-patch particles and is likely to be more realizable in experiments, for example, using DNA origami. One interesting feature of the first system is that the resulting quasicrystals very often contain a screw dislocation.We develop new methods to efficiently propagate the hierarchical equations of motion (HEOM) by using the Tucker and hierarchical Tucker (HT) tensors to represent the reduced density operator and auxiliary density operators. We first show that by employing the split operator method, the specific structure of the HEOM allows a simple propagation scheme using the Tucker tensor. When the number of effective modes in the HEOM increases and the Tucker representation becomes intractable, the split operator method is extended to the binary tree structure of the HT representation. It is found that to update the binary tree nodes related to a specific effective mode, we only need to propagate a short matrix product state constructed from these nodes. Numerical results show that by further employing the mode combination technique commonly used in the multi-configuration time-dependent Hartree approaches, the binary tree representation can be applied to study excitation energy transfer dynamics in a fairly large system including over 104 effective modes. selleck kinase inhibitor The new methods may thus provide a promising tool in simulating quantum dynamics in condensed phases.Carbon nanotube (CNT) bundles are being explored as a support structure for four ionic liquids (ILs) in gas separation. Grand canonical Monte Carlo simulations were performed to investigate the CO2/CH4, H2S/CH4, and N2/CH4 separation performance in CNT bundles and CNT-supported ILs (CNT-ILs) as a function of pressure and IL loading. The results show that by adding ILs to the CNT bundles, the gas separation performance can be significantly increased. Increasing the number of IL molecules in the composites increases the separation performance. Such a phenomenon is more evident for the CO2/CH4 mixture in comparison to H2S/CH4 and N2/CH4. Calculations of isosteric heat of adsorption and selectivities in gas mixtures as a function of pressure show promising gas separation performance for CNT-ILs. Due to the excellent mechanical properties of CNTs, it has been shown that this structure may be used as a strong mechanical support for structures containing ILs with excellent CO2/CH4 separation performance.Protein assembly is often studied in a three-dimensional solution, but a significant fraction of binding events involve proteins that can reversibly bind and diffuse along a two-dimensional surface. In a recent study, we quantified how proteins can exploit the reduced dimensionality of the membrane to trigger complex formation. Here, we derive a single expression for the characteristic timescale of this multi-step assembly process, where the change in dimensionality renders rates and concentrations effectively time-dependent. We find that proteins can accelerate dimer formation due to an increase in relative concentration, driving more frequent collisions, which often win out over slow-downs due to diffusion. Our model contains two protein populations that dimerize with one another and use a distinct site to bind membrane lipids, creating a complex reaction network. However, by identifying two major rate-limiting pathways to reach an equilibrium steady-state, we derive an excellent approximation for the mean first passage time when lipids are in abundant supply. Our theory highlights how the "sticking rate" or effective adsorption coefficient of the membrane is central in controlling timescales. We also derive a corrected localization rate to quantify how the geometry of the system and diffusion can reduce rates of membrane localization. We validate and test our results using kinetic and particle-based reaction-diffusion simulations. Our results establish how the speed of key assembly steps can shift by orders-of-magnitude when membrane localization is possible, which is critical to understanding mechanisms used in cells.