Adaptive multiscale simulation for organic electronics

• Applicant: Dr. Denis Andrienko
• Subject Area: Experimental and Theoretical Physics of Polymers
• Term: from 2007 to 2011
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 33852402

• Final Report Year: 2011

Final Report Abstract

To assist rational compound design of organic semiconductors, two problems need to be addressed. First, the material morphology has to be known at an atomistic level. Second, with the morphology at hand, an appropriate charge transport model needs to be developed in order to link charge carrier mobility to structure. The former can be addressed by generating atomistic morphologies using molecular dynamics simulations. However, the accessible range of time- and length-scales is limited. To overcome these limitations, systematic coarse-graining methods can be used. The developed Versatile Object-oriented Toolkit for Coarse-graining Applications provides a platform for the implementation of coarse-graining methods. Tools to perform Boltzmann inversion, iterative Boltzmann inversion, inverse Monte Carlo, and force-matching are available and have been tested on a set of model systems. In partially disordered systems, the second issue is closely connected to constructing appropriate diabatic states between which charge transfer occurs. Here, charge transport is modeled by introducing conjugated segments on which charge carriers are localized. Inter-chain transport is then treated within a high temperature non-adiabatic Marcus theory while an adiabatic rate expression is used for intra-chain transport. The charge dynamics is simulated using the kinetic Monte Carlo method. The developed framework was implemented in a software package (www.votca.org). The package is written in C++, has a scripting flow control, test-suite, tutorials, manual, bug-trucker, and wiki-pages. It was employed to establish a relation between the morphology and the charge mobility of several discotic liquid crystals, small-molecule self-assembled monolayers, amorphous metal-coordinated semiconductors and conjugated oligomers.

Publications

• “Charge mobility of discotic mesophases: a multiscale quantum/classical study”, Phys. Rev. Lett., 98, 227402, 2007
  J. Kirkpatrick, V. Marcon, J. Nelson, K. Kremer, D. Andrienko
  
• “Columnar mesophases of hexabenzocoronene derivatives. I. Phase transitions” J. Chem. Phys., 129, 094505, 2008
  V. Marcon, T. Vehoff, J. Kirkpatrick, Ch. Jeong, Do. Y. Yoon, K. Kremer, D. Andrienko
  
• “Columnar mesophases of hexabenzocoronene derivatives: II. Charge carrier mobility”, J. Chem. Phys., 129, 094506, 2008
  J. Kirkpatrick, V. Marcon, K. Kremer, J. Nelson, D. Andrienko
  
• “Charge transport in semiconductors with multiscale conformational dynamics” Phys. Rev. Lett., 102, 116602, 2009
  A. Troisi, D. L. Cheung, D. Andrienko
  
• “Towards high charge-carrier mobilities by rational design of the shape and periphery of discotics” Nature Materials, 8, 421 - 426, 2009
  X. Feng, V. Marcon, W. Pisula, M. R. Hansen, J. Kirkpatrick, F. Grozema, D. Andrienko, K. Kremer, K. Müllen
  
• “Understanding structure-mobility relations for perylene tetracarboxdiimide derivatives” J. Am. Chem. Soc., 131, 11426-11432, 2009
  V. Marcon, W. Pisula, J. Dahl, D. W. Breiby, J. Kirkpatrick, S. Patwardhan, F. Grozema, D. Andrienko
  
• “Charge transport in organic crystals: role of disorder and topological connectivity” J. Am. Chem. Soc., 132, 11702-11708, 2010
  T. Vehoff, B. Baumeier, A. Troisi, D. Andrienko
  
• “Extracting nondispersive charge carrier mobilities of organic semiconductors from simulations of small systems”, Phys. Rev. B, 82, 193202, 2010
  A. Lukyanov, D. Andrienko