The polypyrrole (PPy) films were electrochemically deposited on roughened gold substrates with different
predominant crystalline orientations of (111) and (220), respectively. Gold was roughened via a cyclic
voltammetry procedure. The result indicates that the (220) crystalline orientation of gold was partially changed
into (111) one after gold was roughened with oxidation−reduction cycles (ORC) treatment. The surface-enhanced Raman scattering (SERS) spectroscopy of PPy deposited on gold with predominant (111) orientation
exhibits higher intensity and more excellent resolution. Meanwhile, the redox behavior of gold and the resulting
complex in ORC were strongly sensitive to the crystalline orientation. A mechanism of the roughening
procedure on gold was also proposed to illustrate the resulting complex and its effect on the SERS enhancement.
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