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• W2945408711 abstract "Charge transport in π-conjugated polymers is characterized by a strong degree of disorder in both the energy of conjugated segments and the electronic coupling between adjacent sites. This disorder arises from variations in the structure and conformation of molecular units, as well as the weak intermolecular binding interactions. Although disorder in molecular conformation can be expected to influence the density of states (DOS) distribution—and hence, optoelectronic properties of the material—until now, there has been no direct study of the relationship between a distinct conformational defect and the charge transport properties of a conjugated polymer. Here, we investigate the impact of introducing an extended, planarized chain geometry, known as the “β-phase,” on hole transport through otherwise amorphous films of poly(9,9-dioctylfluorene) (PFO). We show that while β-phase introduces a striking drop of about a hundredfold in time-of-flight (TOF) hole mobility (μh) at room temperature, it reduces the steady-state μh measured from hole-only devices by a factor of less than about 5. In order to reconcile these observations, we combine high-dynamic-range TOF photocurrent spectroscopy and energy-resolved electrochemical impedance spectroscopy to extract the hole DOS of the conjugated polymer. Both methods show that the effect of the β-phase content is to introduce a sharp sub-bandgap feature into the DOS of glassy PFO lying about 0.3 eV above the highest occupied molecular orbital. The observed energy of the conformational trap is consistent with electronic structure calculations using a tight-binding approach. Using the obtained DOS with a drift-diffusion model capable of resolving charge carriers in both time and energy, we show how the seemingly contradictory transport phenomena obtained via the time-resolved, frequency-resolved, and steady-state methods are reconciled. The results highlight the significance of energetic redistribution of charge carriers in affecting transport behavior. This work demonstrates how charge-carrier mobility in organic semiconductors can be controlled via molecular conformation, and it resolves a long-standing debate over how different (equilibrium versus nonequilibrium) transport techniques reveal electronic properties of disordered solids in a unified manner.18 MoreReceived 4 August 2018Revised 18 February 2019DOI:https://doi.org/10.1103/PhysRevX.9.021038Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasCarrier dynamicsConformation changesDensity of statesElectrical conductivityPhysical SystemsConjugated polymersDisordered systemsOrganic semiconductorsTechniquesTight-binding modelTransport techniquesCondensed Matter, Materials & Applied PhysicsPolymers & Soft Matter" @default.
• W2945408711 created "2019-05-29" @default.
• W2945408711 creator A5016308795 @default.
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• W2945408711 creator A5080398727 @default.
• W2945408711 date "2019-05-24" @default.
• W2945408711 modified "2023-10-18" @default.
• W2945408711 title "Relating Chain Conformation to the Density of States and Charge Transport in Conjugated Polymers: The Role of the <mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML display=inline><mml:mi>β</mml:mi></mml:math> -phase in Poly(9,9-dioctylfluorene)" @default.
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