One‐electron second‐order optical activity of a helix

The second‐order nonlinear‐optical response of a chiral molecule is calculated. We model the optical response classically using a single electron bound to a helical path. The helical motion of the electron causes optical activity in the second‐order response. The hyperpolarizability tensor of a single helix and the susceptibility tensor for a thin film of helices are given. We examine the process of second‐harmonic generation from a chiral surface using the calculated susceptibility tensor. The efficiency of the harmonic generation is different for left‐ and right‐hand circularly polarized fundamental light, which is ascribed to be a form of nonlinear optical activity. The roles of pitch and radius of the helix are readily seen in the microscopic and macroscopic second‐order optical responses and in the surface second‐harmonic generation, which may provide some insight for synthesizing new chiral compounds. Our results also allow us to draw conclusions about the relative strength and importance to second‐...

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