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Rational design of all organic polymer dielectrics

Nature Communications volume 5, Article number: 4845 (2014) | Download Citation

Abstract

To date, trial and error strategies guided by intuition have dominated the identification of materials suitable for a specific application. We are entering a data-rich, modelling-driven era where such Edisonian approaches are gradually being replaced by rational strategies, which couple predictions from advanced computational screening with targeted experimental synthesis and validation. Here, consistent with this emerging paradigm, we propose a strategy of hierarchical modelling with successive downselection stages to accelerate the identification of polymer dielectrics that have the potential to surpass ‘standard’ materials for a given application. Successful synthesis and testing of some of the most promising identified polymers and the measured attractive dielectric properties (which are in quantitative agreement with predictions) strongly supports the proposed approach to material selection.

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Acknowledgements

This paper is based on the work supported by a Multidisciplinary University Research Initiative (MURI) grant (N00014-10-1-0944) from the Office of Naval Research (ONR). Computational support was provided by the Extreme Science and Engineering Discovery Environment (XSEDE) and the National Energy Research Scientific Computing Center (NERSC). A.R.O. thanks the National Science Foundation (grants EAR-1114313, DMR-1231586), DARPA (Grants No. W31P4Q1310005, and No. W31P4Q1210008), grant of the Government of the Russian Federation (No. 14.A12.31.0003) and CRDF Global (UKE2-7034-KV-11). Ms JoAnne Ronzello and Dr Yang Cao are gratefully acknowledged for assistance with electrical characterization of the polymer samples. Dr Kenny Lipkowitz, Dr Paul Armistead and Ms Patricia Irwin are acknowledged for support, discussions and general guidance.

Author information

Affiliations

  1. Department of Materials Science and Engineering, University of Connecticut, Storrs, Connecticut 06269, USA

    • Vinit Sharma
    • , Chenchen Wang
    •  & Rampi Ramprasad
  2. Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06269, USA

    • Vinit Sharma
    • , Chenchen Wang
    • , Robert G. Lorenzini
    • , Rui Ma
    • , Gregory A. Sotzing
    • , Steven A. Boggs
    •  & Rampi Ramprasad
  3. Department of Chemistry, Institute of Materials Science, University of Connecticut, Storrs, Connecticut 06226, USA

    • Robert G. Lorenzini
    • , Rui Ma
    •  & Gregory A. Sotzing
  4. Department of Geosciences and Center for Materials by Design, Stony Brook University, Stony Brook, New York 11794, USA

    • Qiang Zhu
    •  & Artem R. Oganov
  5. Department of Chemical Engineering, Columbia University, New York, New York 10027, USA

    • Daniel W. Sinkovits
    •  & Sanat Kumar
  6. Materials Science and Technology Division (MST-8), Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA

    • Ghanshyam Pilania
  7. Moscow Institute of Physics and Technology, 9 Institutskiy lane, Moscow 141700, Russia

    • Artem R. Oganov
  8. Northwestern Polytechnical University, Xi’an 710072, China

    • Artem R. Oganov

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Contributions

R.R. designed and supervised the study. The high-throughput computations and combinatorial screening were performed by C.W. and G.P. (guided by R.R.). Structure prediction using the evolutionary structure search scheme was performed by V.S. and Q.Z. (guided by A.R.O.) and using the melt-and-quench approach by D.W.S. (guided by S.K.). Synthesis, characterization and testing of the polymers were performed by R.G.L. and R.M. (guided by G.A.S. and S.A.B.). R.R., V.S., S.K. and S.A.B. wrote and shaped the manuscript. All authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Rampi Ramprasad.

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DOI

https://doi.org/10.1038/ncomms5845

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