Interfacial electronic states and charge transfer play an important role in many organic devices, but it has been
technically challenging to probe surface electronic states under ambient conditions or at buried interfaces. Developments
in two-dimensional (2D) IR-visible sum frequency generation (SFG) spectroscopy have made it possible to study the
optical and electronic properties of organic molecules located at a buried interface. We present studies of poly[2-
methoxy, 5-ethyl (2'-hexyloxy) para-phenylenevinylene] (MEH-PPV) surfaces using 2D SFG. Surface SFG electronic
spectra were obtained by scanning the frequencies of both incident visible and IR beams, and used to study the electronic
transitions associated with the C-C stretching of benzene rings. Assuming an oligomer model and a Gaussian
conjugation-length distribution, the average conjugation lengths were estimated to be 5.8 monomer units at the MEHPPV/
solid interface and 5.1 monomer units at the air/polymer interface.
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