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• W3206506908 abstract "The control over material properties attainable through molecular doping is essential to many technological applications of organic semiconductors, such as organic light-emitting diodes or thermoelectrics. These excitonic semiconductors typically reach the degenerate limit only at impurity concentrations of 5-10%, a phenomenon that has been put in relation with the strong Coulomb binding between charge carriers and ionized dopants, and whose comprehension remained elusive so far. This study proposes a general mechanism for the release of carriers at finite doping in terms of collective screening phenomena. A multiscale model for the dielectric properties of doped organic semiconductor is set up by combining first principles and microelectrostatic calculations. The results predict a large nonlinear enhancement of the dielectric constant (tenfold at 8% load) as the system approaches a dielectric instability (catastrophe) upon increasing doping. This can be attributed to the presence of highly polarizable host-dopant complexes, plus a nontrivial leading contribution from dipolar interactions in the disordered and heterogeneous system. The enhanced screening in the material drastically reduces the (free) energy barriers for electron-hole separation, rationalizing the possibility for thermal charge release. The proposed mechanism is consistent with conductivity data and sets the basis for achieving higher conductivities at lower doping loads." @default.
• W3206506908 created "2021-10-25" @default.
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• W3206506908 date "2021-11-07" @default.
• W3206506908 modified "2023-10-15" @default.
• W3206506908 title "Doping‐Induced Dielectric Catastrophe Prompts Free‐Carrier Release in Organic Semiconductors" @default.
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• W3206506908 doi "https://doi.org/10.1002/adma.202105376" @default.
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• W3206506908 hasPublicationYear "2021" @default.
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