Response theory for time-resolved second-harmonic generation and two-photon photoemission: Dependence on the pulse shape of the exciting light field

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  • 27 February 2001
Abstract
A unifying response theory for the time-resolved nonlinear light generation and two-photon photoemission (2PPE) from flat metal surfaces is presented. The theory describes the dependence of the nonlinear optical response and the photoelectron yield, respectively, on the pulse shape of the exciting laser. While our theory works for arbitrary pulse shapes, we mostly focus on the case of two pulses of the same mean frequency. The interplay between pulse shape, relaxation times of excited electrons, and band structure is analyzed directly in the time domain. The theory allows to discuss when the frequently used optical Bloch equations are valid and how collective excitations affect the nonlinear optical response and 2PPE.

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