Abstract
This chapter suggests photoelectron spectroscopy measurement of electron dynamics in molecules on attosecond time scales. It analytically studies the photoionization of a coherent superposition of electronic states and shows that chirped pulses can measure attosecond time scale electron dynamics just as effectively as transform-limited attosecond pulses of the same bandwidth. Molecular interference modulates the time-dependent photoelectron spectrum and asymmetry. The important parameter for attosecond science is not the pulse duration, but the bandwidth of phased radiation. The method is based on broad bandwidth photoionization. Single photon ionization from a stationary state produces photoelectrons that contain information on the optical pulse and the phase and structure of the initial state. If the state is known, measurement of the photoelectron spectra produced in the presence of a phased infrared field fully characterizes the attosecond pulse; if, on the other hand, the attosecond pulse is known, measurement of photoelectron spectra produced from two or more coherently excited states determines all information on the associated bound-state wavepacket.
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