Coarse-grained simulations of polyelectrolyte complexes: MARTINI models for poly(styrene sulfonate) and poly(diallyldimethylammonium)

Vögele, Martin; Holm, Christian; Smiatek, Jens

doi:10.1063/1.4937805

Cited by 80 publications

(113 citation statements)

References 57 publications

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“…37 Developed initially for biomolecules, 37,61−64 this CG force field has been later extended to nonbiological systems, including various polymers 65−68 and carbon-based nanostructures. 69−72 As a general rule, four heavy atoms are coarse-grained to one interaction site (bead).…”

Section: Methodsmentioning

confidence: 99%

Bulk Heterojunction Morphologies with Atomistic Resolution from Coarse-Grain Solvent Evaporation Simulations

Alessandri¹,

Uusitalo²,

Vries³

et al. 2017

J. Am. Chem. Soc.

160

270

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Control over the morphology of the active layer of bulk heterojunction (BHJ) organic solar cells is paramount to achieve high-efficiency devices. However, no method currently available can predict morphologies for a novel donor–acceptor blend. An approach which allows reaching relevant length scales, retaining chemical specificity, and mimicking experimental fabrication conditions, and which is suited for high-throughput schemes has been proven challenging to find. Here, we propose a method to generate atom-resolved morphologies of BHJs which conforms to these requirements. Coarse-grain (CG) molecular dynamics simulations are employed to simulate the large-scale morphological organization during solution-processing. The use of CG models which retain chemical specificity translates into a direct path to the rational design of donor and acceptor compounds which differ only slightly in chemical nature. Finally, the direct retrieval of fully atomistic detail is possible through backmapping, opening the way for improved quantum mechanical calculations addressing the charge separation mechanism. The method is illustrated for the poly(3-hexyl-thiophene) (P3HT)–phenyl-C61-butyric acid methyl ester (PCBM) mixture, and found to predict morphologies in agreement with experimental data. The effect of drying rate, P3HT molecular weight, and thermal annealing are investigated extensively, resulting in trends mimicking experimental findings. The proposed methodology can help reduce the parameter space which has to be explored before obtaining optimal morphologies not only for BHJ solar cells but also for any other solution-processed soft matter device.

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Section: Methodsmentioning

confidence: 99%

Bulk Heterojunction Morphologies with Atomistic Resolution from Coarse-Grain Solvent Evaporation Simulations

Alessandri¹,

Uusitalo²,

Vries³

et al. 2017

J. Am. Chem. Soc.

160

270

View full text Add to dashboard Cite

show abstract

“…The latter was originally developed for biomolecular systems 35,36 and later on extended for polymer systems. [37][38][39][40][41][42] The Martini model categorizes the beads into polar (P), nonpolar (N), apolar (C), and charged (Q) ones. For each kind of bead, there are subgroups which give more freedom for choosing the appropriate bead type.…”

Section: The Coarse-grained Model For Pedotmentioning

confidence: 99%

“…35 Recently, the Martini model was successfully applied to polymers like poly(3-hexyl-thiophene) (P3HT), [37][38][39]43 phenyl-C61-butyric acid methyl ester (PCBM), 37 polystyrene 40,41 and PSS. 42 Also, a polarizable CG model for water is developed based on one neutral and two charged beads. 44 The validity of the Martini polarizable water model for application to systems with charges is confirmed for the ionic conductivity of Na + and Cl À ions in pure water.…”

Section: The Coarse-grained Model For Pedotmentioning

confidence: 99%

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Morphology and ion diffusion in PEDOT:Tos. A coarse grained molecular dynamics simulation

Modarresi

Franco-González

Zozoulenko

2018

Phys. Chem. Chem. Phys.

126

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A Martini coarse-grained Molecular Dynamics (MD) model for the doped conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) is developed. The morphology of PEDOT:Tos (i.e. PEDOT doped with molecular tosylate) and its crystallization in aqueous solution for different oxidation levels were calculated using the developed method and compared with corresponding all atomistic MD simulations. The diffusion coefficients of Na+ and Cl- ions in PEDOT:Tos are studied using the developed coarse-grained MD approach. It is shown that the diffusion coefficients decrease exponentially as the hydration level is reduced. It is also predicted that the diffusion coefficients decrease when the doping level of PEDOT is increased. The observed behavior is related to the evolution of water clusters and trapping of ions around the polymer matrix as the hydration level changes. The predicted behavior of the ionic diffusion coefficients can be tested experimentally, and we believe that molecular picture of ionic diffusion in PEDOT unraveled in the present study is instrumental for the design of polymeric materials and devices for better and enhanced performance.

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“…CGMD simulations are employed using the recently improvised Martini force field where P3HT, PCBM, and chlorobenzene (CB) molecules are modeled with the CG beads extended to polymers, fullerene, and benzene rings, as shown in Figure . Solvent evaporation and thermal annealing of solvent‐free mixture are simulated under an isothermal–isobaric (NPT) ensemble with the pressure constrained at 1 atm and temperature at 298 K following the approach similar to our earlier work (briefly discussed in the Computational Method section) .…”

Section: Introductionmentioning

confidence: 99%

Effect of polydispersity on the bulk‐heterojunction morphology of P3HT:PCBM solar cells

Munshi

Ghumman

Iyer

et al. 2019

J Polym Sci B Polym Phys

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Bulk heterojunctions (BHJs) based on semiconducting electron–donor polymer and electron–acceptor fullerene have been extensively investigated as potential photoactive layers for organic solar cells (OSCs). In the experimental studies, poly‐(3‐hexyl‐thiophene) (P3HT) polymers are hardly monodisperse as the synthesis of highly monodisperse polymer mixture is a near impossible task to achieve. However, the majority of the computational efforts on P3HT: phenyl‐C61‐butyric acid methyl ester (P3HT:PCBM)‐based OSCs, a monodisperse P3HT is usually considered. Here, results from coarse‐grained molecular dynamics simulations of solvent evaporation and thermal annealing process of the BHJ are shared describing the effect of variability in molecular weight (also known as polydispersity) on the morphology of the active layer. Results affirm that polydispersity is beneficial for charge separation as the interfacial area is observed to increase with higher dispersity. Calculations of percolation and orientation tensors, on the other hand, reveal that a certain polydispersity index ranging between 1.05 and 1.10 should be maintained for optimal charge transport. Most importantly, these results point out that the consideration of polydispersity should be considered in computational studies of polymer‐based OSCs. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019, 57, 895–903

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Coarse-grained simulations of polyelectrolyte complexes: MARTINI models for poly(styrene sulfonate) and poly(diallyldimethylammonium)

Cited by 80 publications

References 57 publications

Bulk Heterojunction Morphologies with Atomistic Resolution from Coarse-Grain Solvent Evaporation Simulations

Bulk Heterojunction Morphologies with Atomistic Resolution from Coarse-Grain Solvent Evaporation Simulations

Morphology and ion diffusion in PEDOT:Tos. A coarse grained molecular dynamics simulation

Effect of polydispersity on the bulk‐heterojunction morphology of P3HT:PCBM solar cells

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