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A unified response theory for the time-resolved nonlinear light generationand two-photon photoemission (2PPE) from metal surfaces is presented. Thetheory allows to describe the dependence of the nonlinear optical response andthe photoelectron yield, respectively, on the time dependence of the excitinglight field. Quantum-mechanical interference effects affect the resultssignificantly. Contributions to 2PPE due to the optical nonlinearity of thesurface region are derived and shown to be relevant close to a plasmonresonance. The interplay between pulse shape, relaxation times of excitedelectrons, and band structure is analyzed directly in the time domain. Whileour theory works for arbitrary pulse shapes, we mainly focus on the case of twopulses of the same mean frequency. Difficulties in extracting relaxation ratesfrom pump-probe experiments are discussed, for example due to the effect ofdetuning of intermediate states on the interference. The theory also allows todetermine the range of validity of the optical Bloch equations and ofsemiclassical rate equations, respectively. Finally, we discuss how collectiveplasma excitations affect the nonlinear optical response and 2PPE.Comment: 27 pages, including 11 figures, version as publishe

Response theory for time-resolved second-harmonic generation and two-photon photoemission