Exciton dissociation in polymer field-effect transistors studied using terahertz spectroscopy

Physical Review B - Condensed Matter and Materials Physics 77:12 (2008)

Authors:

J Lloyd-Hughes, T Richards, H Sirringhaus, MB Johnston, LM Herz

Abstract:

We have used terahertz time-domain spectroscopy to investigate photoinduced charge generation in conjugated polymer field-effect transistors. Our measurements show that excitons dissociate in the accumulation layer under the application of a gate voltage, with a quantum efficiency of ∼0.1 for an average gate field of ∼1× 108 V m-1. The transistor history is found to affect the exciton dissociation efficiency, which decreases as holes are increasingly trapped in the accumulation layer. The quantum efficiency of charge formation from excitons is compared with the two contrasting models proposed by Onsager and Arkhipov based on the assumption that field-induced exciton dissociation is assisted by the Brownian diffusive motion or an initial excess energy supplied by excited vibrational modes, respectively. © 2008 The American Physical Society.

Enhanced pi conjugation around a porphyrin[6] nanoring.

Angew Chem Int Ed Engl 47:27 (2008) 4993-4996

Authors:

Markus Hoffmann, Joakim Kärnbratt, Ming-Hua Chang, Laura M Herz, Bo Albinsson, Harry L Anderson

Monte Carlo simulation of exciton bimolecular annihilation dynamics in supramolecular semiconductor architectures

Journal of Physical Chemistry C 111:51 (2007) 19111-19119

Authors:

C Daniel, S Westenhoff, F Makereel, RH Friend, D Beljonne, LM Herz, C Silva

Abstract:

We present a simulation of exciton dynamics in supramolecular assemblies of an oligo-p-phenylenevinylene derivative monofunctionalised with a quadruple hydrogen-bonding group (MOPV). MOPV molecules form helical stacks in dodecane solution through solvophobic and π-π interactions with thermotropic reversibility. We apply a model of incoherent excitation hopping using a Monte Carlo scheme to extract microscopic physical quantities relevant to energy diffusion and bimolecular annihilation processes within isolated nanostructures. We compare the simulation to ultrafast spectroscopic data, namely photoinduced absorption transients at various excitation fluences, their polarization anisotropy, and the dynamic photoluminescence red-shift. We observe that energy diffusion and bimolecular annihilation processes can be described with the same microscopic model based on a Förster-like model that takes into account the spatial extent of the excited state; these two processes are interconnected via the same underlying physics. We extract a high diffusion coefficient (∼0.08 cm2 s-1) over the first few picoseconds following excitation, which plays an important role in dictating the bimolecular annihilation dynamics. © 2007 American Chemical Society.

Transient terahertz conductivity of GaAs nanowires

Nano Letters 7:7 (2007) 2162-2165

Authors:

P Parkinson, J Lloyd-Hughes, Q Gao, HH Tan, C Jagadish, MB Johnston, LM Herz

Abstract:

The time-resolved conductivity of isolated GaAs nanowires is investigated by optical-pump terahertz-probe time-domain spectroscopy. The electronic response exhibits a pronounced surface plasmon mode that forms within 300 fs before decaying within 10 ps as a result of charge trapping at the nanowire surface. The mobility is extracted using the Drude model for a plasmon and found to be remarkably high, being roughly one-third of that typical for bulk GaAs at room temperature. © 2007 American Chemical Society.

Theory of non-Condon emission from the interchain exciton in conjugated polymer aggregates.

J Chem Phys 126:19 (2007) 191102

Authors:

Eric R Bittner, Stoyan Karabunarliev, Laura M Herz

Abstract:

The authors present here a simple analysis that explains the apparent strengthening of electron phonon interaction upon aggregation in conjugated polymer materials. The overall scheme is that of an intermolecular Herzberg-Teller effect whereby sidebands of a forbidden transition are activated by oppositely phased vibrations. The authors show that upon aggregation, the 0-0 emission becomes symmetry forbidden and the apparent redshift and remaining vibronic structure are due to sideband (0-1,0-2, etc.) emission. At higher temperatures, the 0-0 peak is due to thermal population in a higher lying even-parity vibronic state rather than direct emission from the odd-paritied lowest intermolecular vibronic state.