38 results on '"Tkachenko, A. V."'
Search Results
2. Symmetry-specific characterization of bond orientation order in DNA-assembled nanoparticle lattices
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Logan, Jack A., Michelson, Aaron, Pattammattel, Ajith, Yan, Hanfei, Gang, Oleg, and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Disordered Systems and Neural Networks ,Condensed Matter - Statistical Mechanics - Abstract
Bond-orientational order in DNA-assembled nanoparticle lattices is explored with the help of recently introduced Symmetry-specific Bond Order Parameters (SymBOPs). This approach provides a more sensitive analysis of local order than traditional scalar Bond Order Parameters, facilitating the identification of coherent domains at the single bond level. The present study expands the method initially developed for assemblies of anisotropic particles to the isotropic ones or cases where particle orientation information is unavailable. The SymBOP analysis was applied to experiments on DNA-frame-based assembly of nanoparticle lattices. It proved highly sensitive in identifying coherent crystalline domains with different orientations, as well as detecting topological defects, such as dislocations. Furthermore, the analysis distinguishes individual sublattices within a single crystalline domain, such as pair of interpenetrating FCC lattices within a cubic diamond. The results underscore the versatility and robustness of SymBOPs in characterizing ordering phenomena, making them valuable tools for investigating structural properties in various systems., Comment: 12 pages, 12 figures
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- 2023
3. Controlling morphology in hybrid isotropic/patchy particle assemblies
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Mushnoori, Srinivas, Logan, Jack A., Tkachenko, Alexei V., and Dutt, Meenakshi
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
Brownian Dynamics is used to study self-assembly in a hybrid system of istotropic particles (IPs), combined with anisotropic building blocks that represent special "designer particles". Those are modeled as spherical patchy particles (PPs) with binding only allowed between their patches and IPs. In this study, two types of PPs are considered: Octahedral PPs (Oh-PPs) and Square PPs (Sq-PPs), with octahedral and square arrangements of patches, respectively. The self-assembly is additionally facilitated by the simulated annealing procedure. The resultant structures are characterized by a combination of local correlations in cubatic ordering, and a symmetry-specific variation of bond orientation order parameters (SymBOPs). By varying the PP/IP size ratio, we detected a sharp crossover between two distinct morphologies, in both types of systems. High symmetry phases, NaCl crystal for Oh-PP and square lattice for Sq-PP, are observed for larger size ratios. For smaller ones, the dominant morphologies are significantly different, e.g., Oh-PPs form a compact amorphous structure with predominantly Face-to-Face orientation of neighboring PPs. Unusually for a morphology without a long range order, it is still possible to identify well organized coherent clusters of this structure, thanks to the adoption of our SymBOP-based characterization., Comment: 9 pages, 14 figures
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- 2021
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4. Symmetry-specific orientational order parameters for complex structures
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Logan, Jack A., Mushnoori, Srinivas, Dutt, Meenakshi, and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
A comprehensive framework of characterizing complex self-assembled structures with a set of orientational order parameters is presented. It is especially relevant in the context of using anisotropic building blocks with various symmetries. Two classes of tensor order parameters are associated with polyhedral nematic, and bond orientational order, respectively. For the latter, a variation of classical bond order parameters is introduced that takes advantage of the symmetry of constituent particles, and/or expected crystalline phases. These Symmetrized Bond Order Parameters (SymBOPs) can be averaged over an entire system, or assigned locally to an individual bond. By combining that with bond percolation procedure, one is able to identify coherent domains within a self-assembled structure. As a demonstration of the proposed framework, we apply it to a simulated hybrid system that combines isotropic and patchy particles with octahedral symmetry. Not only does the methodology allow one to identify individual crystalline domains, but it also detects coherent clusters of a peculiar compact amorphous structure that is not space-filling and lacks any long-range order., Comment: 8 pages, 4 figures
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- 2021
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5. Geometric and Topological Entropies of Sphere Packing
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Logan, Jack A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Disordered Systems and Neural Networks ,Condensed Matter - Statistical Mechanics - Abstract
We present a statistical mechanical description of randomly packed spherical particles, where the average coordination number is treated as a macroscopic thermodynamic variable. The overall packing entropy is shown to have two contributions: geometric, reflecting statistical weights of individual configurations, and topological, which corresponds to the number of topologically distinct states. Both of them are computed in the thermodynamic limit for isostatic packings in 2D and 3D, and the result is further expanded to the case of "floppy" particle clusters. The theory is directly applicable to sticky colloids, and in addition, generalizes concepts of granular and glassy configurational entropies for the case of non-jammed systems., Comment: 8 pages, 7 figures
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- 2021
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6. Comment on 'Colossal Pressure-Induced Softening in Scandium Fluoride'
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Zaliznyak, I. A., Bozin, E., and Tkachenko, A. V.
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Condensed Matter - Materials Science ,Condensed Matter - Soft Condensed Matter - Abstract
The results reported by Wei et al. [Phys. Rev. Lett. 124, 255502 (2020)] can be confronted with predictive, quantitative theories of negative thermal expansion (NTE) and pressure-induced softening, allowing to corroborate, or invalidate certain approaches. Motivated to corroborate the quantitative predictions of the recent Coulomb Floppy Network (CFN) microscopic theory of vibrational and thermomechanical properties of empty perovskite crystals [Tkachenko and Zaliznyak, arXiv:1908.11643 (2019)], we compared theory prediction for the mean-squared transverse displacement of the F atoms, U$_{perp}$, with that reported in Fig. 5 of Wei et al. and observed a marked discrepancy (an order-of-magnitude larger than the error bar). We then compared these results with the previously published Xray diffraction data of Greve, et al. [JACS 132, 15496 (2010)] and the neutron diffraction data of Wendt, et al. [Science Advances 5 (2019), 10.1126/sciadv.aay2748]. We found the latter two data sets to be in a good agreement with each other, as well as with the prediction of CFN theory. We thus conclude that U$_{perp}$ values reported in Fig. 5 of Wei et al. are substantially incorrect. The purpose of this Comment is twofold: (i) to caution the researchers against using the U$_{perp}$ data of Wei et al. for quantitative comparisons with theory, and (ii) to encourage Wei et al. to reconsider their analysis and obtain a reliable U$_{perp}$ data by better accounting for the beam transmission and attenuation effects., Comment: 1 page, 1 figure
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- 2020
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7. Empty perovskites as Coulomb floppy networks: entropic elasticity and negative thermal expansion
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Tkachenko, Alexei V. and Zaliznyak, Igor A.
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Condensed Matter - Materials Science ,Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
Floppy Networks (FNs) provide valuable insight into the origin of anomalous mechanical and thermal properties in soft matter systems, from polymers, rubber, and biomolecules to glasses and granular materials. Here, we use the very same FN concept to construct a quantitative microscopic theory of empty perovskites, a family of crystals with ReO$_3$ structure, which exhibit a number of unusual properties. One remarkable example is ScF$_3$, which shows a near-zero-temperature structural instability and large negative thermal expansion (NTE). We trace these effects to an FN-like crystalline architecture formed by strong nearest-neighbor bonds, which is stabilized by net electrostatic repulsion that plays a role similar to osmotic pressure in polymeric gels. NTE in these crystalline solids, which we conceptualize as Coulomb Floppy Networks, emerges from the tension effect of Coulomb repulsion combined with the FN's entropic elasticity, and has the same physical origin as in gels and rubber. Our theory provides an accurate, quantitative description of phonons, thermal expansion, compressibility, and structural phase diagram, all in excellent agreement with experiments. The entropic stabilization of critical soft modes, which play only a secondary role in NTE, explains the observed phase diagram. Significant entropic elasticity resolves the puzzle of a marked, $\approx$50\% discrepancy between the experimentally observed bulk modulus and ab initio calculations. The Coulomb FN approach is potentially applicable to other important materials with markedly covalent bonds, from perovskite oxides to iron chalcogenides, whose anomalous vibrational and structural properties are still poorly understood., Comment: Manuscript with appendices, 12 pages, 3 figures
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- 2019
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8. Compact interaction potential for van der Waals nanorods
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Logan, Jack A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Mesoscale and Nanoscale Physics - Abstract
We studied the van der Waals interactions of two finite, solid, cylindrical rods at arbitrary angle and position with respect to each other. An analytic interpolative formula for the interaction potential energy is constructed, based on various asymptotic cases. The potential can be readily used for numerical and analytic description of multi-wall carbon nanotubes, metallic nanorods, rod-shaped colloids, or any other similar objects with significant van der Waals interactions.
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- 2018
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9. Onset of natural selection in auto-catalytic heteropolymers
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Tkachenko, Alexei V. and Maslov, Sergei
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Quantitative Biology - Populations and Evolution ,Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics ,Quantitative Biology - Biomolecules - Abstract
Reduction of information entropy along with ever-increasing complexity are among the key signatures of living matter. Understanding the onset of such behavior in early prebiotic world is essential for solving the problem of origins of life. To elucidate this transition, we study a theoretical model of information-storing heteropolymers capable of template-assisted ligation and subjected to cyclic non-equilibrium driving forces. We discover that this simple physical system undergoes a spontaneous reduction of the information entropy due to the competition of chains for constituent monomers. This natural-selection-like process ultimately results in the survival of a limited subset of polymer sequences. Importantly, the number of surviving sequences remains exponentially large, thus opening up the possibility of further increase in complexity due to Darwinian evolution. We also propose potential experimental implementations of our model using either biopolymers or artificial nano-structures.
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- 2017
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10. Layer-by-layer assembly of patchy particles as a route to non-trivial structures
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Patra, Niladri and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter - Abstract
We propose a new strategy for robust high-quality self-assembly of non-trivial periodic structures out of patchy particles, and investigate it with Brownian Dynamics (BD) simulations. Its first element is the use of specific patch-patch and shell-shell interactions between the particles, that can be implemented through differential functionalization of patched and shell regions with specific DNA strands. The other key element of our approach is the use of layer-by-layer protocol that allows to avoid a formations of undesired random aggregates. As an example, we design and self-assemble in silico a version of a Double Diamond (DD) lattice in which four particle types are arranged into BCC crystal made of four FCC sub-lattices. The lattice can be further converted to Cubic Diamond (CD) by selective removal of the particles of certain types. Our results demonstrate that by combining the directionality, selectivity of interactions and the layer-by-layer protocol, a high-quality robust self-assembly can be achieved., Comment: 18 pages, 14 figures
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- 2017
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11. Chromatic patchy particles: effects of specific interactions on liquid structure
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Vasilyev, Oleg A., Klumov, Boris A., and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter - Abstract
We study the structural and thermodynamic properties of patchy particle liquids, with a special focus on the role of "color", i.e. specific interactions between individual patches. A possible experimental realization of such "chromatic" interactions is by decorating the particle patches with single-stranded DNA linkers. The complementarity of the linkers can promote selective bond formation between predetermined pairs of patches. By using MD simulations, we compare the local connectivity, the bond orientation order, and other structural properties of the aggregates formed by the "colored" and "colorless" systems. The analysis is done for spherical particles with two different patch arrangements (tetrahedral and cubic). It is found that the aggregated (liquid) phase of the "colorless" patchy particles is better connected, denser and typically has stronger local order than the corresponding "colored" one. This, in turn, makes the colored liquid less stable thermodynamically. Specifically, we predict that in a typical case the chromatic interactions should increase the relative stability of the crystalline phase with respect to the disordered liquid, thus expanding its region in the phase diagram., Comment: 22 pages, 11 figures
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- 2014
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12. Onset of autocatalysis of information-coding polymers
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Tkachenko, Alexei V. and Maslov, Sergei
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Mesoscale and Nanoscale Physics ,Condensed Matter - Statistical Mechanics ,Quantitative Biology - Biomolecules ,Quantitative Biology - Populations and Evolution - Abstract
Self-replicating systems based on information-coding polymers are of crucial importance in biology. They also recently emerged as a paradigm in material design on nano- and micro-scales. We present a general theoretical and numerical analysis of the problem of spontaneous emergence of autocatalysis for heteropolymers capable of template-assisted ligation driven by cyclic changes in the environment. Our central result is the existence of the first order transition between the regime dominated by free monomers and that with a self-sustaining population of sufficiently long chains. We provide a simple, mathematically tractable model supported by numerical simulations, which predicts the distribution of chain lengths and the onset of autocatalysis in terms of the overall monomer concentration and two fundamental rate constants. Another key result of our study is the emergence of the kinetically-limited optimal overlap length between a template and each of its two substrates. The template-assisted ligation allows for heritable transmission of the information encoded in chain sequences thus opening up the possibility of long-term memory and evolvability in such systems., Comment: 20 pages, 4 figures
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- 2014
13. Precursors of order in aggregates of patchy particles
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Vasilyev, Oleg A., Klumov, Boris A., and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter - Abstract
We study computationally the local structure of aggregated systems of patchy particles. By calculating the probability distribution functions of various rotational invariants we can identify the precursors of orientation order in amorphous phase. Surprisingly, the strongest signature of local order is observed for 4-patch particles with tetrahedral symmetry, not for 6-patch particles with the cubic one. This trend is exactly opposite to their known ability to crystallize. We relate this anomaly to the observation that a generic aggregate of patchy systems has coordination number close to 4. Our results also suggest a significant correlation between rotational order in the studied liquids with the corresponding crystalline phases, making this approach potentially useful for a broader range of patchy systems., Comment: 12 pages, 3 figures
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- 2013
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14. DNA-Programmed Mesoscopic Architecture
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Halverson, Jonathan D. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science - Abstract
We study the problem of the self-assembly of nanoparticles (NPs) into finite mesoscopic structures with a programmed local morphology and complex overall shape. Our proposed building blocks are NPs directionally-functionalized with DNA. The combination of directionality and selectivity of interactions allows one to avoid unwanted metastable configurations which have been shown to lead to slow self-assembly kinetics even in much simpler systems. With numerical simulations, we show that a variety of target mesoscopic objects can be designed and self-assembled in near perfect yield. They include cubes, pyramids, boxes and even an Empire State Building model. We summarize our findings with a set of design strategies that lead to the successful self-assembly of a wide range of mesostructures., Comment: 5 pages, 7 figures, published version
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- 2013
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15. A simple analytical formula for the free-energy of ligand-receptor mediated interactions
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Angioletti-Uberti, Stefano, Varilly, Patrick, Mognetti, Bortolo Matteo, Tkachenko, Alexei V., and Frenkel, Daan
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics ,Physics - Biological Physics - Abstract
Recently \1, we presented a general theory for calculat- ing the strength and properties of colloidal interactions mediated by ligand-receptor bonds (such as those that bind DNA-coated colloids). In this communication, we derive a surprisingly simple analytical form for the inter- action free energy, which was previously obtainable only via a costly numerical thermodynamic integration. As a result, the computational effort to obtain potentials of in- teraction is significantly reduced. Moreover, we can gain insight from this analytic expression for the free energy in limiting cases. In particular, the connection of our general theory to other previous specialised approaches is now made transparent. This important simplification will significantly broaden the scope of our theory., Comment: 4 pages, 3 Figures
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- 2012
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16. Transition from single-file to two-dimensional diffusion of interacting particles in a quasi-one-dimensional channel
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Lucena, D., Tkachenko, D. V., Nelissen, K., Misko, V. R., Ferreira, W. P., Farias, G. A., and Peeters, F. M.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
Diffusive properties of a monodisperse system of interacting particles confined to a \textit{quasi}-one-dimensional (Q1D) channel are studied using molecular dynamics (MD) simulations. We calculate numerically the mean-squared displacement (MSD) and investigate the influence of the width of the channel (or the strength of the confinement potential) on diffusion in finite-size channels of different shapes (i.e., straight and circular). The transition from single-file diffusion (SFD) to the two-dimensional diffusion regime is investigated. This transition (regarding the calculation of the scaling exponent ($\alpha$) of the MSD $<\Delta x^{2}(t)>$ $\propto t^{\alpha}$) as a function of the width of the channel, is shown to change depending on the channel's confinement profile. In particular the transition can be either smooth (i.e., for a parabolic confinement potential) or rather sharp/stepwise (i.e., for a hard-wall potential), as distinct from infinite channels where this transition is abrupt. This result can be explained by qualitatively different distributions of the particle density for the different confinement potentials., Comment: 13 pages, 11 figures
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- 2010
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17. The dynamics of colloids in a narrow channel driven by a non-uniform force
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Tkachenko, D. V., Misko, V. R., and Peeters, F. M.
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Condensed Matter - Soft Condensed Matter - Abstract
Using Brownian dynamics simulations, we investigate the dynamics of colloids confined in two-dimensional narrow channels driven by a non-uniform force F(y). We considered linear-gradient, parabolic and delta-like driving-force profiles. This driving force induces melting of the colloidal solid (i.e., shear-induced melting), and the colloidal motion experiences a transition from elastic to plastic regime with increasing F. For intermediate F (i.e., in the transition region) the response of the system, i.e., the distribution of the velocities of the colloidal chains, in general does not coincide with the profile of the driving force F(y), and depends on the magnitude of F, the width of the channel and the density of colloids. For example, we show that the onset of plasticity is first observed near the boundaries while the motion in the central region is elastic. This is explained by: (i) (in)commensurability between the chains due to the larger density of colloids near the boundaries, and (ii) the gradient in F. Our study provides a deeper understanding of the dynamics of colloids in channels and could be accessed in experiments on colloids (or in dusty plasma) with, e.g., asymmetric channels or in the presence of a gradient potential field., Comment: 10 pages, 7 figures
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- 2009
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18. Self-assembling DNA-caged particles: nanoblocks for hierarchical self-assembly
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science ,Condensed Matter - Statistical Mechanics - Abstract
DNA is an ideal candidate to organize matter on the nanoscale, primarily due to the specificity and complexity of DNA based interactions. Recent advances in this direction include the self-assembly of colloidal crystals using DNA grafted particles. In this article we theoretically study the self-assembly of DNA-caged particles. These nanoblocks combine DNA grafted particles with more complicated purely DNA based constructs. Geometrically the nanoblock is a sphere (DNA grafted particle) inscribed inside a polyhedron (DNA cage). The faces of the DNA cage are open, and the edges are made from double stranded DNA. The cage vertices are modified DNA junctions. We calculate the equilibriuim yield of self-assembled, tetrahedrally caged particles, and discuss their stability with respect to alternative structures. The experimental feasability of the method is discussed. To conclude we indicate the usefulness of DNA-caged particles as nanoblocks in a hierarchical self-assembly strategy., Comment: v2: 21 pages, 8 figures; revised discussion in Sec. 2, replaced 2 figures, added new references
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- 2008
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19. How to build nanoblocks using DNA scaffolds
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science ,Condensed Matter - Statistical Mechanics - Abstract
In recent years there have been a number of proposals to utilize the specificity of DNA based interactions for potential applications in nanoscience. One interesting direction is the self-assembly of micro- and nanoparticle clusters using DNA scaffolds. In this letter we consider a DNA scaffold method to self-assemble clusters of "colored" particles. Stable clusters of microspheres have recently been produced by an entirely different method. Our DNA based approach self-assembles clusters with additional degrees of freedom associated with particle permutation. We demonstrate that in the non-equilibrium regime of irreversible binding the self-assembly process is experimentally feasible. These color degrees of freedom may allow for more diverse intercluster interactions essential for hierarchical self-assembly of larger structures., Comment: 4 pages, 2 figures ; epl format
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- 2008
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20. Kinetic limitations of cooperativity based drug delivery systems
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Quantitative Biology - Cell Behavior - Abstract
We study theoretically a novel drug delivery system that utilizes the overexpression of certain proteins in cancerous cells for cell specific chemotherapy. The system consists of dendrimers conjugated with "keys" (ex: folic acid) which "key-lock" bind to particular cell membrane proteins (ex: folate receptor). The increased concentration of "locks" on the surface leads to a longer residence time for the dendrimer and greater incorporation into the cell. Cooperative binding of the nanocomplexes leads to an enhancement of cell specificity. However, both our theory and detailed analysis of in-vitro experiments indicate that the degree of cooperativity is kinetically limited. We demonstrate that cooperativity and hence the specificity to particular cell type can be increased by making the strength of individual bonds weaker, and suggest a particular implementation of this idea. The implications of the work for optimizing the design of drug delivery vehicles are discussed., Comment: 4 pages, 4 figures, v3: minor revisions
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- 2007
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21. Role of boundary constraints in DNA cyclization
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Tkachenko, Alexei V.
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Quantitative Biology - Biomolecules ,Condensed Matter - Soft Condensed Matter - Abstract
We modify the classical Shimada-Yamakawa theory of DNA looping by generalizing the form of boundary constraints. This generalization is important in the context of DNA cyclization experiments since it mimics the reduced local rigidity of the "nicked" DNA loop. Our results indicate that the non-trivial boundary constraints may be responsible for the existing dramatic discrepancy between various DNA cyclization experiments. The developed effective Hamiltonian method may be further extended to a broad class of DNA looping problems., Comment: 4 pages, 3 figures
- Published
- 2007
22. Elasticity of strongly stretched ssDNA
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Tkachenko, Alexei V.
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Quantitative Biology - Biomolecules ,Condensed Matter - Soft Condensed Matter - Abstract
We present a simple model which describes elastic response of single-stranded DNA (ssDNA) to stretching, including the regime of very high force (up to 1000 pN). ssDNA is modelled as a discreet persistent chain, whose ground state is a zigzag rather than a straight line configuration. This mimics the underlying molecular architecture and helps to explain the experimentally observed staturation of the stretching curve at very high force., Comment: 5 pages, 2 figures
- Published
- 2007
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23. Colloids with key-lock interactions: non-exponential relaxation, aging and anomalous diffusion
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
The dynamics of particles interacting by key-lock binding of attached biomolecules are studied theoretically. Experimental realizations of such systems include colloids grafted with complementary single-stranded DNA (ssDNA), and particles grafted with antibodies to cell-membrane proteins. Depending on the coverage of the functional groups, we predict two distinct regimes. In the low coverage localized regime, there is an exponential distribution of departure times. As the coverage is increased the system enters a diffusive regime resulting from the interplay of particle desorption and diffusion. This interplay leads to much longer bound state lifetimes, a phenomenon qualitatively similar to aging in glassy systems. The diffusion behavior is analogous to dispersive transport in disordered semiconductors: depending on the interaction parameters it may range from a finite renormalization of the diffusion coefficient to anomalous, subdiffusive behavior. We make connections to recent experiments and discuss the implications for future studies., Comment: v2: substantially revised version, new treatment of localized regime, 19 pages, 10 figures
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- 2007
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24. Dynamics of particles with 'key-lock' interactions
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Statistical Mechanics - Abstract
The dynamics of particles interacting by key-lock binding of attached biomolecules are studied theoretically. Examples of such systems include DNA-functionalized colloids as well as nanoparticles grafted with antibodies to cell membrane proteins. Depending on the coverage of the functional groups, we predict two distinct regimes separated by a percolation transition. In the localized regime at low coverage, the system exhibits a broad, power law like distribution of particle departure times. At higher coverage, there is an interplay between departure dynamics and particle diffusion. This interplay leads to a sharp increase of the departure times, a phenomenon qualitatively similar to aging in glassy systems. This diffusive regime is analogous to dispersive transport in disordered semiconductors: depending on the interaction parameters, the diffusion behavior ranges from standard diffusion to anomalous, subdiffusive behavior. The connection to recent experiments and implications for future studies are discussed., Comment: 4 pages, 6 figures
- Published
- 2006
25. Statistical Mechanics of DNA-Mediated Colloidal Aggregation
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Statistical Mechanics ,Condensed Matter - Soft Condensed Matter - Abstract
We present a statistical mechanical model of aggregation in colloidal systems with DNA mediated interactions. We obtain a general result for the two-particle binding energy in terms of the hybridization free energy $\Delta G$ of DNA and two model dependent properties: the average number of available DNA bridges $\left< N\right>$ and the effective DNA conccentration $c_{eff}$. We calculate these parameters for a particular DNA bridging scheme. The fraction of all the $n$-mers, including the infinite aggregate, are shown to be universal functions of a single parameter directly related to the two-particle binding energy. We explicitly take into account the partial ergodicity of the problem resulting from the slow DNA binding-unbinding dynamics, and introduce the concept of angular localization of DNA linkers. In this way, we obtain a direct link between DNA thermodynamics and the global aggregation and melting properties in DNA-colloidal systems. The results of the theory are shown to be in quantitative agreement with two recent experiments with particles of micron and nanometer size. PACS numbers: 81.16.Dn, 82.20.Db, 68.65.-k, 87.14.Gg, Comment: 12 pages, 6 figures, v2: added reference, expanded conclusion, added journal ref
- Published
- 2006
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26. Self-assembly of DNA-coded nanoclusters
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science ,Condensed Matter - Statistical Mechanics - Abstract
We present a theoretical discussion of a self-assembly scheme which makes it possible to use DNA to uniquely encode the composition and structure of micro- and nanoparticle clusters. These anisotropic DNA-decorated clusters can be further used as building blocks for hierarchical self-assembly of larger structures. We address several important aspects of possible experimental implementation of the proposed scheme: the competition between different types of clusters in a solution, possible jamming in an unwanted configuration, and the degeneracy due to symmetry with respect to particle permutations., Comment: v2, 4 pages, 7 figures, added journal ref
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- 2006
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27. Effects of Sequence Disorder on DNA Looping and Cyclization
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Popov, Yuri O. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter - Abstract
Effects of sequence disorder on looping and cyclization of the double-stranded DNA are studied theoretically. Both random intrinsic curvature and inhomogeneous bending rigidity are found to result in a remarkably wide distribution of cyclization probabilities. For short DNA segments, the range of the distribution reaches several orders of magnitude for even completely random sequences. The ensemble averaged values of the cyclization probability are also calculated, and the connection to the recent experiments is discussed., Comment: 8 pages, 4 figures, LaTeX; accepted to Physical Review E; v2: a substantially revised version; v3: references added, conclusions expanded, minor editorial corrections to the text; v4: a substantially revised and expanded version (total number of pages doubled); v5: new Figure 4, captions expanded, minor editorial improvements to the text
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- 2005
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28. Error-proof programmable self-assembly of DNA-nanoparticle clusters
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Licata, Nicholas A. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science - Abstract
We study theoretically a new generic scheme of programmable self-assembly of nanoparticles into clusters of desired geometry. The problem is motivated by the feasibility of highly selective DNA-mediated interactions between colloidal particles. By analyzing both a simple generic model and a more realistic description of a DNA-colloidal system, we demonstrate that it is possible to suppress the glassy behavior of the system, and to make the self-assembly nearly error-proof. This regime requires a combination of stretchable interparticle linkers (e.g. sufficiently long DNA), and a soft repulsive potential. The jamming phase diagram and the error probability are computed for several types of clusters. The prospects for the experimental implementation of our scheme are also discussed. PACS numbers: 81.16.Dn, 87.14.Gg, 36.40.Ei, Comment: 6 pages, 4 figures, v2: substantially revised version, added journal ref
- Published
- 2005
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29. Effects of Kinks on DNA Elasticity
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Popov, Yuri O. and Tkachenko, Alexei V.
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Condensed Matter - Soft Condensed Matter ,Quantitative Biology - Biomolecules - Abstract
We study the elastic response of a worm-like polymer chain with reversible kink-like structural defects. This is a generic model for (a) the double-stranded DNA with sharp bends induced by binding of certain proteins, and (b) effects of trans-gauche rotations in the backbone of the single-stranded DNA. The problem is solved both analytically and numerically by generalizing the well-known analogy to the Quantum Rotator. In the small stretching force regime, we find that the persistence length is renormalized due to the presence of the kinks. In the opposite regime, the response to the strong stretching is determined solely by the bare persistence length with exponential corrections due to the ``ideal gas of kinks''. This high-force behavior changes significantly in the limit of high bending rigidity of the chain. In that case, the leading corrections to the mechanical response are likely to be due to the formation of multi-kink structures, such as kink pairs., Comment: v1: 16 pages, 7 figures, LaTeX; submitted to Physical Review E; v2: a new subsection on soft kinks added to section Theory, sections Introduction and Conclusions expanded, references added, other minor changes; v3: a reference added
- Published
- 2004
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30. Entropically-Stabilized Self-Compactification in Model Colloidal Systems
- Author
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Park, Juyong and Tkachenko, Alexei V.
- Subjects
Condensed Matter - Soft Condensed Matter - Abstract
We discuss the phenomenon of spontaneous self-compactification in a model colloidal system, proposed in a recent work on DNA-mediated self-assembly. We focus on the effect of thermal fluctuations on the stability of membrane-like self-assembled phase with in-plane square order. Surprisingly, the fluctuations are shown to enhance the stability of this quasi-2D phase with respect to transition to alternative 3D structures., Comment: 4 pages, 2 figures, typo corrected
- Published
- 2003
31. Unfolding and unzipping of single-stranded DNA by stretching
- Author
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Tkachenko, Alexei V.
- Subjects
Condensed Matter - Soft Condensed Matter ,Quantitative Biology - Biomolecules - Abstract
We present a theoretical study of single-stranded DNA under stretching. Within the proposed framework, the effects of basepairing on the mechanical response of the molecule can be studied in combination with an arbitrary underlying model of chain elasticity. In a generic case, we show that the stretching curve of ssDNA exhibits two distinct features: the second-order "unfolding" phase transition, and a sharp crossover, reminiscent of the first-order "unzipping" transition in dsDNA. We apply the theory to the particular cases of Worm-like Chain (WLC) and Freely-Joint Chain (FJC) models, and discuss the universal and model--dependent features of the mechanical response of ssDNA. In particular, we show that variation of the width of the unzipping crossover with interaction strength is very sensitive to the energetics of hairpin loops. This opens a new way of testing the elastic properties of ssDNA., Comment: 7 pages, 4 figures, substantially revised version
- Published
- 2003
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32. Electrostatic effects in DNA stretching
- Author
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Tkachenko, Alexei V.
- Subjects
Condensed Matter - Soft Condensed Matter ,Quantitative Biology - Biomolecules - Abstract
The response of a semiflexible polyelectrolyte chain to stretching in the regimes of moderate and weak screening is studied theoretically, with a special focus on DNA experiments. By using the nonlinear Poisson--Boltzmann description of electrostatic self--interactions of the chain, we explicitly demonstrate the applicability of the concept of effective charge to certain aspects of the problem. This charge can be extracted from the far--field asymptotic behavior of electrostatic potential of the fully aligned chain. Surprisingly, in terms of the effective charge, the electrostatically renormalized persistence length can be formally described by the classical Odijk-Skolnick-Fixman (OSF) formula, whose domain of applicability is limited to linearized Debye Huckel (DH) approximation. However, the short--length behavior of the chain in the nonlinear regime deviates from the of DH--based result, even upon the charge renormalization. This difference is revealed in calculated stretching curves of strongly charged DNA, and our results are in good agreement with the recent experiments. In the limit of weak screening we predict the elastic response to have a distinctive two-stage character, with a peculiar intermediate "unstretchable" regime., Comment: substantially expanded version
- Published
- 2003
33. With a little help of DNA: Morphological diversity of colloidal self-assembly
- Author
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Tkachenko, Alexei V.
- Subjects
Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science ,Condensed Matter - Statistical Mechanics ,Quantitative Biology - Abstract
We study theoretically a binary system in which an attraction of unlike particles is combined with a type-independent soft core repulsion. The possible experimental implementation of the system is a mixture of DNA-covered colloids, in which both the repulsion and the attraction may be induced by DNA solution. The system is shown to exhibit surprisingly diverse and unusual morphologies. Among them are the diamond lattice and the membrane phase with in-plane square order, a striking example of spontaneous compactification., Comment: 5 pages, 3 figures
- Published
- 2001
34. Mesoscopic Physics of Granular Flows
- Author
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Tkachenko, Alexei V. and Putkaradze, Vachtang
- Subjects
Condensed Matter - Soft Condensed Matter ,Condensed Matter - Disordered Systems and Neural Networks - Abstract
We present a description of granular dynamics based on the idea of differentiation between fluid and solid components. First, we construct a model of completely fluidized phase. Then we discuss a shear surface motion on the boundary of the bulk solid phase, induced by a moving wall. Our results include the thickness dependence of the velocity of a developed avalanche, density and velocity profiles in granular Couette flow experiment., Comment: 4 pages, 2 figures
- Published
- 1999
35. Stress in frictionless granular material: Adaptive Network Simulations
- Author
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Tkachenko, Alexei V. and Witten, Thomas A.
- Subjects
Condensed Matter - Soft Condensed Matter ,Condensed Matter - Disordered Systems and Neural Networks ,Condensed Matter - Statistical Mechanics - Abstract
We present a minimalistic approach to simulations of force transmission through granular systems. We start from a configuration containing cohesive (tensile) contact forces and use an adaptive procedure to find the stable configuration with no tensile contact forces. The procedure works by sequentially removing and adding individual contacts between adjacent beads, while the bead positions are not modified. In a series of two-dimensional realizations, the resulting force networks are shown to satisfy a linear constraint among the three components of average stress, as anticipated by recent theories. The coefficients in the linear constraint remain nearly constant for a range of shear loadings up to about .6 of the normal loading. The spatial distribution of contact forces shows strong concentration along ``force chains". The probability of contact forces of magnitude f shows an exponential falloff with f. The response to a local perturbing force is concentrated along two characteristic rays directed downward and laterally., Comment: 8 pages, 8 figures
- Published
- 1999
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36. Stress Propagation through Frictionless Granular Material
- Author
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Tkachenko, Alexei V. and Witten, Thomas A.
- Subjects
Condensed Matter - Soft Condensed Matter ,Condensed Matter - Disordered Systems and Neural Networks ,Condensed Matter - Statistical Mechanics - Abstract
We examine the network of forces to be expected in a static assembly of hard, frictionless spherical beads of random sizes, such as a colloidal glass. Such an assembly is minimally connected: the ratio of constraint equations to contact forces approaches unity for a large assembly. However, the bead positions in a finite subregion of the assembly are underdetermined. Thus to maintain equilibrium, half of the exterior contact forces are determined by the other half. We argue that the transmission of force may be regarded as unidirectional, in contrast to the transmission of force in an elastic material. Specializing to sequentially deposited beads, we show that forces on a given buried bead can be uniquely specified in terms of forces involving more recently added beads. We derive equations for the transmission of stress averaged over scales much larger than a single bead. This derivation requires the Ansatz that statistical fluctuations of the forces are independent of fluctuations of the contact geometry. Under this Ansatz, the $d(d+1)/2$-component stress field can be expressed in terms of a d-component vector field. The procedure may be generalized to non-sequential packings. In two dimensions, the stress propagates according to a wave equation, as postulated in recent work elsewhere. We demonstrate similar wave-like propagation in higher dimensions, assuming that the packing geometry has uniaxial symmetry. In macroscopic granular materials we argue that our approach may be useful even though grains have friction and are not packed sequentially.=17, Comment: 15 pages, 4 figures, revised vertion for Phys. Rev. E
- Published
- 1998
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37. Effect of Chain Flexibility on Nematic-Smectic Transition
- Author
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Tkachenko, Alexei V.
- Subjects
Condensed Matter - Soft Condensed Matter ,Condensed Matter - Materials Science ,Condensed Matter - Statistical Mechanics - Abstract
The theory of nematic-smectic phase transition in the system of uniform semi-flexible chains with hard-core repulsion is presented. Both the general density-functional formalism the tube-model calculation show that the flexibility of the chains results in a strong first-order transition, in contrast to the common weak-cristallization scenario of the nematic-smectic transition in rigid rods. The calculated spinodal volume fraction of the uniform nematic phase and the period of the modulation instability are consistent with recent experimental results.
- Published
- 1998
- Full Text
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38. On the Glassy Behavior of Parking Lot Model
- Author
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Kolan, Amy J., Nowak, Edmund R., and Tkachenko, Alexei V.
- Subjects
Condensed Matter - Statistical Mechanics ,Condensed Matter - Disordered Systems and Neural Networks ,Condensed Matter - Soft Condensed Matter - Abstract
We present a theoretical discussion of the reversible parking problem, which appears to be one of the simplest systems exhibiting glassy behavior. The existence of slow relaxation, nontrivial fluctuations, and an annealing effect can all be understood by recognizing that two different time scales are present in the problem. One of these scales corresponds to the fast filling of existing voids, the other is associated with collective processes that overcome partial ergodicity breaking. The results of the theory are in a good agreement with simulation data; they provide a simple qualitative picture for understanding recent granular compaction experiments and other glassy systems., Comment: LaTeX, 19 pages; 6 PostScript figures
- Published
- 1998
- Full Text
- View/download PDF
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