Müller, Marcus

[["dc.bibliographiccitation.artnumber","024903"],["dc.bibliographiccitation.issue","2"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","128"],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.date.accessioned","2018-11-07T11:19:08Z"],["dc.date.available","2018-11-07T11:19:08Z"],["dc.date.issued","2008"],["dc.description.abstract","We discuss a method for calculating free energy differences between disordered and ordered phases of self-assembling systems utilizing computer simulations. Applying an external, ordering field, we impose a predefined structure onto the fluid in the disordered phase. The structure in the presence of the external, ordering field closely mimics the structure of the ordered phase (in the absence of an ordering field). Self-consistent field theory or density functional theory provides an accurate estimate for choosing the strength of the ordering field. Subsequently, we gradually switch off the external, ordering field and, in turn, increase the control parameter that drives the self-assembly. The free energy difference along this reversible path connecting the disordered and the ordered state is obtained via thermodynamic integration or expanded ensemble simulation techniques. Utilizing Single-Chain-in-Mean-Field simulations of a symmetric diblock copolymer melt we illustrate the method and calculate the free energy difference between the disordered phase and the lamellar structure at an intermediate incompatibility chi N=20. Evidence for the first-order character of the order-disorder transition at fixed volume is presented. The transition is located at chi(ODT)N=13.65 +/- 0.10 for an invariant degree of polymerization of ($) over barN=14 884. The magnitude of the shift of the transition from the mean field prediction qualitatively agrees with other simulations. (c) 2008 American Institute of Physics."],["dc.identifier.doi","10.1063/1.2818565"],["dc.identifier.isi","000252450100038"],["dc.identifier.pmid","18205471"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/55199"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","0021-9606"],["dc.title","Calculating the free energy of self-assembled structures by thermodynamic integration"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","4097"],["dc.bibliographiccitation.issue","15"],["dc.bibliographiccitation.journal","Soft Matter"],["dc.bibliographiccitation.lastpage","4102"],["dc.bibliographiccitation.volume","9"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.date.accessioned","2018-11-07T09:30:10Z"],["dc.date.available","2018-11-07T09:30:10Z"],["dc.date.issued","2013"],["dc.description.abstract","The prospects of compressible Self-Consistent Field (SCF) theory schemes for describing structures in amphiphilic membranes are illustrated by considering the thermodynamic stability of hourglass-shaped, hydrophobic connections (stalks) between apposed bilayers. The membranes are represented by a coarse-grained, solvent-free model. We represent the chain architecture by a Gaussian-thread representation of the chain architecture and capture the non-bonded interactions with a functional, which is of third-order in the densities of the hydrophilic and the hydrophobic segments. Using a three dimensional real-space scheme, we study the thermodynamic stability of the stalk with respect to two planar apposing bilayers as a function of membrane tension and molecular asymmetry. The structure and thermodynamics predicted by SCF theory agree very well with particle-based simulations, which include fluctuations. We discuss how the longer-range perturbations of the membrane induced by the stalk can affect thermodynamic properties."],["dc.description.sponsorship","DFG [SFB 803/B03]"],["dc.identifier.doi","10.1039/c3sm00098b"],["dc.identifier.fs","592377"],["dc.identifier.isi","000316573400021"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/10827"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/31237"],["dc.notes","This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively."],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1744-683X"],["dc.relation.orgunit","Fakultät für Physik"],["dc.title","Exploring thermodynamic stability of the stalk fusion-intermediate with three-dimensional self-consistent field theory calculations"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","168"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","ACS Nano"],["dc.bibliographiccitation.lastpage","175"],["dc.bibliographiccitation.volume","1"],["dc.contributor.author","Stoykovich, Mark P."],["dc.contributor.author","Kang, Huiman"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Liu, Guoliang"],["dc.contributor.author","Liu, Chi-Chun"],["dc.contributor.author","de Pablo, Juan J."],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Nealey, Paul F."],["dc.date.accessioned","2018-11-07T10:57:51Z"],["dc.date.available","2018-11-07T10:57:51Z"],["dc.date.issued","2007"],["dc.description.abstract","Self-assembling block copolymers are of interest for nanomanufacturing due to the ability to realize sub-100 nm dimensions, thermodynamic control over the size and uniformity and density of features, and inexpensive processing. The insertion point of these materials in the production of integrated circuits, however, is often conceptualized in the short term for niche applications using the dense periodic arrays of spots or lines that characterize bulk block copolymer morphologies, or in the long term for device layouts completely redesigned into periodic arrays. Here we show that the domain structure of block copolymers in thin films can be directed to assemble into nearly the complete set of essential dense and isolated patterns as currently defined by the semiconductor industry. These results suggest that block copolymer materials, with their intrinsically advantageous self-assembling properties, may be amenable for broad application in advanced lithography, including device layouts used in existing nanomanufacturing processes."],["dc.identifier.doi","10.1021/nn700164p"],["dc.identifier.isi","000252145100006"],["dc.identifier.pmid","19206647"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/50347"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1936-0851"],["dc.title","Directed self-assembly of block copolymers for nanolithography: Fabrication of isolated features and essential integrated circuit geometries"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","164906"],["dc.bibliographiccitation.issue","16"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","129"],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.date.accessioned","2018-11-07T11:09:56Z"],["dc.date.available","2018-11-07T11:09:56Z"],["dc.date.issued","2008"],["dc.description.abstract","We investigate the ability of Monte-Carlo algorithms to describe the single-chain dynamics in a dense homogeneous melt and a lamellar phase of a symmetric diblock copolymer. A minimal, coarse-grained model is employed that describes connectivity of effective segments by harmonic springs and where segments interact via soft potentials, which do not enforce noncrossability of the chain molecules. Studying the mean-square displacements, the dynamic structure factor, and the stress relaxation, we show that local, unconstraint displacements of segments via a Smart Monte Carlo algorithm give rise to Rouse dynamics for all but the first Monte Carlo steps. Using the slithering-snake algorithm, we observe a dynamics that is compatible with the predictions of the tube model of entangled melts for long times, but the dynamics inside the tube cannot be resolved. Using a slip-link model, we can describe the effect of entanglements and follow the different regimes of the single-chain dynamics over seven decades in time. Applications of this simulation scheme to spatially inhomogeneous systems are illustrated by studying the lamellar phase of a symmetric diblock copolymer. For the local, unconstraint dynamics, the single-chain motions parallel and perpendicular to the interfaces decouples; the perpendicular dynamics is slowed down but the parallel dynamics is identical to that in a homogeneous melt. Both the slithering-snake dynamics and the slip-link dynamics give rise to a coupling of parallel and perpendicular directions and a significant slowing down of the dynamics in the lamellar phase. (C) 2008 American Institute of Physics. [DOI: 10.1063/1.2997345]"],["dc.description.sponsorship","VW-foundation; DFG Priority Programme, Polymer solid [Mu 1674/9]"],["dc.identifier.doi","10.1063/1.2997345"],["dc.identifier.isi","000260572300076"],["dc.identifier.pmid","19045313"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/53107"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.title","Single-chain dynamics in a homogeneous melt and a lamellar microphase: A comparison between Smart Monte Carlo dynamics, slithering-snake dynamics, and slip-link dynamics"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","2334"],["dc.bibliographiccitation.issue","5"],["dc.bibliographiccitation.journal","Macromolecules"],["dc.bibliographiccitation.lastpage","2342"],["dc.bibliographiccitation.volume","43"],["dc.contributor.author","Stoykovich, Mark P."],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Kang, Huiman"],["dc.contributor.author","de Pablo, Juan J."],["dc.contributor.author","Nealey, Paul F."],["dc.date.accessioned","2018-11-07T08:45:06Z"],["dc.date.available","2018-11-07T08:45:06Z"],["dc.date.issued","2010"],["dc.description.abstract","Block copolymer Structures have been directed to assemble oil chemically patterned surfaces with the domain interfaces oriented perpendicular to the substrate. Such methods have been pursued for lithographic applications to achieve long-range order in the assembled structures and, potentially more important, provide nanometer-level control over the interfaces between Structures. The chemically striped surfaces used for the directed assembly of lamellae are patterned by top-down lithographic techniques and thus often have rough edges between the regions of different chemistry. Here we quantitatively characterize, using experiments and molecular-level simulations, the propagation of line edge roughness from the chemically patterned surfaces into the interfaces between domains of block copolymer lamellae as a function of the wavelength, amplitude, and geometry of the roughness. Two geometries of surface pattern roughness are considered with oscillatory neighboring interfaces that are either in-phase or out-of-phase. Block copolymer lamellae of poly(styrene-b/ock-methyl methacrylate) effectively self-corrected surface patterns with small wavelength in-phase and out-of-phase roughness such that little or no memory of the Substrate pattern roughness could be observed at the top surface of a 40 nm thin film. Larger wavelength in-phase roughness, and to a lesser extent larger wavelength out-of-phase roughness, propagated farther from the surface pattern such that the domain interfaces between block copolymer lamellae maintained the roughness throughout the film. These self-healing capabilities of block copolymers will be essential for lithographic applications with tight tolerances on line edge roughness and line width control, e.g., in patterning transistor gates."],["dc.identifier.doi","10.1021/ma902494v"],["dc.identifier.isi","000274928400032"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/20353"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0024-9297"],["dc.title","Remediation of Line Edge Roughness in Chemical Nanopatterns by the Directed Assembly of Overlying Block Copolymer Films"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","197"],["dc.bibliographiccitation.lastpage","233"],["dc.bibliographiccitation.seriesnr","224"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.date.accessioned","2018-11-07T08:48:30Z"],["dc.date.available","2018-11-07T08:48:30Z"],["dc.date.issued","2010"],["dc.description.abstract","An overview of molecular models and computer simulation techniques for amphiphilic vesicles formed either by lipid or block copolymer molecules is presented. First, system-specific, atomistic or coarse-grained representations of amphiphilic vesicles, which account for the detailed, chemical structure of the system, are briefly considered. The common features of collective phenomena on the mesoscale (e.g., the self-assembly into vesicles, their rupture or fusion), observed in a broad class of amphiphilic systems, suggest a universal underlying mechanism. This observation forms the basis for modeling large-scale properties of amphiphilic vesicles by minimal models. These coarse-grained models describe the underlying atomistic structure through a few relevant interactions, whose strength is characterized by coarse-grained parameters. The discussion of these coarse-grained models particularly focuses on how their parameterization can be related to the material properties of specific systems. In this context, the concept of combining density functional representations of amphiphilic systems with particle-based simulation techniques is introduced. As an illustration, a solvent-free model based on a virial expansion functional is elaborated and applied to investigate the behavior of polymersomes loaded with long homopolymers. Although the interactions are cast in a density functional language, the model is a particle-based one and its equilibrium properties are obtained from a straightforward Monte-Carlo scheme. The mechanical properties of the vesicles are established and compared to the properties of a planar bilayer. Selected results concerning the effect of loading on vesicle stability and mechanical properties of its bilayer shell are presented."],["dc.identifier.doi","10.1007/12_2008_7"],["dc.identifier.isi","000274503000006"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/21226"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Springer"],["dc.publisher.place","Berlin"],["dc.relation.crisseries","Advances in Polymer Science"],["dc.relation.isbn","978-3-642-10478-7"],["dc.relation.ispartof","POLYMER MEMBRANES/BIOMEMBRANES"],["dc.relation.ispartofseries","Advances in Polymer Science; 224"],["dc.relation.issn","0065-3195"],["dc.title","Comparison of Simulations of Lipid Membranes with Membranes of Block Copolymers"],["dc.type","review"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","1284"],["dc.bibliographiccitation.issue","4"],["dc.bibliographiccitation.journal","Langmuir"],["dc.bibliographiccitation.lastpage","1295"],["dc.bibliographiccitation.volume","24"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Stoykovich, Mark P."],["dc.contributor.author","Kang, Huiman"],["dc.contributor.author","de Pablo, Juan J."],["dc.contributor.author","Nealey, Paul F."],["dc.date.accessioned","2018-11-07T11:18:16Z"],["dc.date.available","2018-11-07T11:18:16Z"],["dc.date.issued","2008"],["dc.description.abstract","The directed assembly of lamella-forming copolymer systems on substrates chemically patterned with rough stripes has been studied using a Helfrich-type, phenomenological theory and Single-Chain-in-Mean-Field (SCMF) simulations. The stripe period matches that of the lamellar spacing in the bulk. The effect of the line edge roughness (LER) of the substrate pattern on the microphase-separated morphology was investigated considering two generic types of substrate LER with a single characteristic wavelength imposed on the edges of the stripes: undulation and peristaltic LER. In both cases, the domain interfaces are pinned to the rough stripe boundary at the substrate and, thus, are deformed. We study how this deformation decays as a function of the distance from the substrate. The simple theory and the SCMF simulations demonstrate that one of the basic factors determining the decay of the roughness transferred into the self-assembled morphology is the characteristic LER wavelength of the substrate pattern; i.e., the distance over which the roughness propagates away from the substrate increases with wavelength. However, both approaches reveal that, for a quantitative understanding of the consequences of substrate LER, it is important to consider the interplay of the pattern wavelength with the other characteristic length scales of the system, such as the film thickness and the bulk lamellar spacing. For instance, in thin films, the induced deformation of the lamellar interface decays slower with distance from the patterned surface than in thicker films. It is shown that the phenomenological theory can capture many of the same qualitative results as the SCMF simulations for copolymer assembly on substrate patterns with LER, but, at the same time, is limited by an incomplete description of the constraints on the polymer chain conformations imposed by the substrate."],["dc.identifier.doi","10.1021/la702482z"],["dc.identifier.isi","000253130900022"],["dc.identifier.pmid","18067336"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/54999"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0743-7463"],["dc.title","Directed copolymer assembly on chemical substrate patterns: A phenomenological and single-chain-in-mean-field simulations study of the influence of roughness in the substrate pattern"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","4989"],["dc.bibliographiccitation.issue","13"],["dc.bibliographiccitation.journal","Macromolecules"],["dc.bibliographiccitation.lastpage","5001"],["dc.bibliographiccitation.volume","41"],["dc.contributor.author","Detcheverry, Francois A."],["dc.contributor.author","Kang, Huiman"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Nealey, Paul F."],["dc.contributor.author","de Pablo, Juan J."],["dc.date.accessioned","2018-11-07T11:13:02Z"],["dc.date.available","2018-11-07T11:13:02Z"],["dc.date.issued","2008"],["dc.description.abstract","A coarse grain model and a Monte Carlo sampling formalism are proposed for simulations of self-assembly in block copolymer melts and nanoparticle-copolymer composites. Our approach relies on a particle-based representation of the system, it does not invoke a saddle point approximation, and it permits treatment of large three-dimensional systems. We provide a detailed description of the model and methods and discuss their relationship to results from self-consistent-field theory and single chain in mean field simulations. The validity of the proposed approach is addressed by applying it to study systems whose description within existing approaches would be demanding. In particular, we use it to examine the directed assembly of copolymer blends and nanoparticles on nanopatterned substrates. We show that results from Simulations are in good agreement with experiment, and we use our theoretical findings to help explain the experimental observations."],["dc.identifier.doi","10.1021/ma702514v"],["dc.identifier.isi","000257366200062"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/53803"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","0024-9297"],["dc.title","Monte Carlo simulations of a coarse grain model for block copolymers and nanocomposites"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","227801"],["dc.bibliographiccitation.issue","22"],["dc.bibliographiccitation.journal","Physical Review Letters"],["dc.bibliographiccitation.volume","107"],["dc.contributor.author","Mueller, Marcus"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.date.accessioned","2018-11-07T08:49:41Z"],["dc.date.available","2018-11-07T08:49:41Z"],["dc.date.issued","2011"],["dc.description.abstract","The difficulty to study intrinsically slow collective processes by computer simulation of particle models stems from multiple disparate time scales (e.g., stiff bonded interactions versus soft nonbonded interactions). Continuum models, which describe the system by collective variables rather than the coordinates of the individual molecular constituents, often do not suffer from this time-scale problem because the stiff microscopic degrees of freedom have been integrated out. We propose to concurrently couple these two descriptions by a heterogeneous multiscale method. We illustrate the technique by studying the Lifshitz-Slyozov coarsening mechanism in a binary polymer blend using a soft coarse-grained particle model and a Landau-Ginzburg-de Gennes free energy functional, respectively. A speedup of up to two orders of magnitudes is achieved."],["dc.description.sponsorship","Volkswagen-Stiftung; DFG [Mu 1674/11]"],["dc.identifier.doi","10.1103/PhysRevLett.107.227801"],["dc.identifier.isi","000297292400002"],["dc.identifier.pmid","22182041"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/21522"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Physical Soc"],["dc.relation.issn","0031-9007"],["dc.title","Speeding Up Intrinsically Slow Collective Processes in Particle Simulations by Concurrent Coupling to a Continuum Description"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","184904"],["dc.bibliographiccitation.issue","18"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","125"],["dc.contributor.author","Daoulas, Kostas Ch."],["dc.contributor.author","Mueller, Marcus"],["dc.date.accessioned","2018-11-07T08:58:19Z"],["dc.date.available","2018-11-07T08:58:19Z"],["dc.date.issued","2006"],["dc.description.abstract","The description of fluctuations by single chain in mean field (SCMF) simulations is discussed and the results of this particle-based self-consistent field technique are quantitatively compared to Monte Carlo simulations of the same discretized Edwards-Hamiltonian providing exact reference data. In SCMF simulations one studies a large ensemble of noninteracting molecules subjected to real, external fields by Monte Carlo simulations. The external fields approximate nonbonded, instantaneous interactions between molecules. In the self-consistent mean field theory the external fields are static and fluctuation effects are ignored. In SCMF simulations, the external fields fluctuate since they are frequently recalculated from the instantaneous density distribution of the ensemble of molecules. In the limit of infinitely high density or instantaneous update of the external fields, the SCMF simulation method accurately describes long-wavelength fluctuations. At high but finite updating frequency the accuracy depends on the discretization of the model. The accuracy is illustrated by studying the single chain structure and intermolecular correlations in polymer melts, and fluctuation effects on the order-disorder transition of symmetric diblock copolymers."],["dc.identifier.doi","10.1063/1.2364506"],["dc.identifier.isi","000242002400064"],["dc.identifier.pmid","17115792"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/23613"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","0021-9606"],["dc.title","Single chain in mean field simulations: Quasi-instantaneous field approximation and quantitative comparison with Monte Carlo simulations"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]