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Effective Temperature and Universal Conductivity Scaling in Organic Semiconductors
Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
Eindhoven University of Technology, Netherlands.
Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering. Eindhoven University of Technology, Netherlands.ORCID iD: 0000-0002-7104-7127
2015 (English)In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 5, article id 16870Article in journal (Refereed) Published
Resource type
Text
Abstract [en]

We investigate the scalability of the temperature-and electric field-dependence of the conductivity of disordered organic semiconductors to universal curves by two different but commonly employed methods; by so-called universal scaling and by using the effective temperature concept. Experimentally both scaling methods were found to be equally applicable to the out-of-plane charge transport in PEDOT: PSS thin films of various compositions. Both methods are shown to be equivalent in terms of functional dependence and to have identical limiting behavior. The experimentally observed scaling behavior can be reproduced by a numerical nearest-neighbor hopping model, accounting for the Coulomb interaction, the high charge carrier concentration and the energetic disorder. The underlying physics can be captured in a simple empirical model, describing the effective temperature of the charge carrier distribution as the outcome of a heat balance between Joule heating and (effective) temperature-dependent energy loss to the lattice.

Place, publisher, year, edition, pages
Nature Publishing Group, 2015. Vol. 5, article id 16870
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:liu:diva-123329DOI: 10.1038/srep16870ISI: 000364933800002PubMedID: 26581975OAI: oai:DiVA.org:liu-123329DiVA, id: diva2:882190
Available from: 2015-12-14 Created: 2015-12-11 Last updated: 2018-03-14
In thesis
1. Charge and Energy Transport in Disordered Organic Semiconductors
Open this publication in new window or tab >>Charge and Energy Transport in Disordered Organic Semiconductors
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Improvement of the performance of organic disordered semiconductors (OSC) is driven by the understanding   of the underlying charge transport mechanisms and systematic exploitation thereof. There exists a multitude of materials and material systems based on polymers and small molecules with promising performance for use in organic light emitting diodes, photovoltaics, organic field-effect transistors and thermoelectrics. However, universal understanding of many classes of these materials has eluded researchers, due to their broad   spectrum of morphologies, molecular structures and electrical properties. Building on the large body of existing models, this thesis deals with charge transport phenomena from the perspective of transport energetics, by studying the interplay between a few but important concepts commonly accepted to play a crucial role in all  OSC materials; energetic disorder, charge carrier hopping and Coulomb interactions. The influence of these concepts on the energetic landscape through which charge carriers move and how this translates to experimentally observed transport phenomena are studied by a combination of experimental work, kinetic Monte Carlo (MC) simulations and empirical and analytical models.

The universal scaling and collapse of the temperature and electric field dependence of the conductivity of PEDOT:PSS to a single curve is shown to be functionally equivalent to the scaling of the effective temperature, which describes the effect of field heating as a broadening of the charge carrier distribution. From numerical investigation of the energy relaxation, an empirical model is developed that relates the physical meaning   behind both concepts to the heat balance between Joule heating of the carrier distribution via the effective temperature and energy loss to the lattice. For this universal description to be applicable a strongly energy- dependent density of states (DOS) as well as Coulomb interactions and large carrier concentrations are needed.

Chemical doping is a common way of improving charge transport in OSC and is also beneficial for energy transport, which combined leads to an increased thermoelectric power factor. The ensuing thermoelectric investigations not only showed the potential of these materials for use in thermoelectric generators, but are  also helpful in unraveling charge transport mechanism as they give direct insight into the energetics of a material. Interestingly, doped OSC exhibit the same universal power-law relationship between thermopower and conductivity, independent of material system or doping method, pointing towards a common energy and charge transport mechanism. In this thesis an analytical model is presented, which reproduces said universal power-law behavior and is able to attribute it to Variable Range Hopping (VRH) or a transition between Nearest Neighbour Hopping (NNH) and VRH at higher concentrations. This model builds on an existing three- dimensional hopping formalism that includes the effect of the attractive Coulomb potential of ionized dopants that leads to a broadening of the DOS. Here, this model is extended by including the energy offset between   host and dopant material and is positively tested against MC simulations and a set of thermoelectric measurements covering different material groups and doping mechanisms.

Organic field effect transistors (OFETs) have become increasingly comparable in electrical mobility to their inorganic (silicon) counterparts. The spatial extent of charge transport in OFETs has been subject to debate since their inception with many experimental, numerical and analytical studies having been undertaken. Here it is shown that the common way of analyzing the dimensionality of charge transport in OFETs may be prone to misinterpretations. Instead, the results in this thesis suggest that charge transport in OFETs is, in fact, quasi- two-dimensional (2D) due to the confinement of the gate field in addition to a morphology-induced preferred in-plane direction of the transport. The inherently large charge carrier concentrations in OFETs in addition to   the quasi-2D confinement leads to increased Coulomb interaction between charge carriers as compared to bulk material, leading to a thermoelectric behavior that deviates from doped organic systems. At very large concentrations interesting charge transport phenomena are observed, including an unexpected simultaneous increase of the concentration dependence and the magnitude of the mobility, the appearance of a negative transconductance, indicating a transition to an insulating Mott-Hubbard phase. The experimental and   numerical results in this thesis relate these phenomena the intricacies of the interplay between Coulomb interactions, energetic disorder and charge carrier hopping.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2018. p. 100
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1909
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-145673 (URN)10.3384/diss.diva-145673 (DOI)9789176853528 (ISBN)
Public defence
2018-04-13, Sal Schrödinger, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
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Supervisors
Available from: 2018-03-14 Created: 2018-03-14 Last updated: 2018-03-20Bibliographically approved

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