Journal of Physical Chemistry p. 6231 - 6237 (1990)
Update date:2022-08-16
Topics:
Veregin, Richard P.
Harbour, John R.
Electron spin resonance (ESR) spectra have been obtained for the radical cation of N,N'-diphenyl-N,N'-bis(3-methylphenyl)-4,4'-diamine (TPD) in dichloromethane solution, in solid amorphous films, and in TPD/polycarbonate films doped with tris(p-bromophenyl)ammonium hexachloroantimonate or HNO3.By use of ESR the mediation of electronic charge (hole) transport via the TPD+ radical cation has been observed in the TPD films in the absence of an applied field.Arrhenius activation parameters were calculated for charge transport from the ESR data, giving EA = 10 +/- 2 kJ/mol Α = (1.7 +/- 1) * 1010 s-1, and a rate constant at 300 K of (3.1 +/-1) * 108 s-1.The value of EA is one-half that from time-of-flight (TOF) measurements extrapolated to zero field, while the rate constant is a factor of 10 smaller, and Α is a factor of 1000 smaller.The differences can be understood in terms of the compensation effect due to the presence of residual solvent, and the ion pairing of an TPD+ ions with dopant counterions.In TPD/polycarbonate films the rate of hole transport is too slow to produce significant changes in the ESR spectrum.The rate of charge transport is thus less than 2*108 s-1 in these films, consistent with TOF data.In dichloromethane solution, an EA of 9.8 kJ/mol was observed with ESR.Extrapolating the solution data to solid TPD gives a hole transport rate of 9.75 * 109 s-1, a factor of 3 higher than that from TOF data.The lower Ea and higher rate in dichloromethane solution are consistent with the effect of the higher dielectric constant compared to an TPD film.This suggests that the rate-determing step for hole transport is the same in solution as it is in the solid state.
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