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Coherent control of ultrafast nano-optical excitations of a corrugated silver surface is demonstrated by means of predetermined few-parameter scans and adaptive polarization laser pulse shaping. “Hot spots” in the multiphoton photoemission signals are enhanced and manipulated with a high contrast. Switching between separated and closely spaced hot spots is shown. The latter allows controlling the shape of hot spots and yields improved nanofocusing and “purification” of the photoemission signals. Complex pulse shapes were obtained in adaptive optimizations whose features were reproducible in repeated runs. Predetermined few-parameter control scans provide insight into the interpretation of optimal pulse shapes. The results indicate the existence of long coherence lifetimes on a corrugated silver surface. This combination of collective strong nanoplasmonic near-field enhancement and long-lived coherence may be used to achieve an even stronger field enhancement (“superenhancement”) making these hot spots ideal candidates for future nanophotonic, spectroscopic, sensor and quantum information applications. In addition the observation of such long coherence lifetimes is relevant to the understanding of surface-enhanced spectroscopies such as single-molecule Raman spectroscopy. [ABSTRACT FROM PUBLISHER]

The most general investigation and exploitation of light-induced processes require simultaneous control over spatial and temporal properties of the electromagnetic field on a femtosecond time and nanometer length scale. Based on the combination of polarization pulse shaping and time-resolved two-photon photoemission electron microscopy, we demonstrate such control over nanoscale spatial and ultrafast temporal degrees of freedom of an electromagnetic excitation in the vicinity of a nanostructure. The time-resolved cross-correlation measurement of the local photo-emission yield reveals the switching of the nanolocalized optical near-field distribution with a lateral resolution well below the diffraction limit and a temporal resolution on the femtosecond time scale: In addition, successful adaptive spatiotemporal control demonstrates the flexibility of the method. This flexible simultaneous control of temporal and spatial properties of nanophotonic excitations opens new possibilities to tailor and optimize the light-matter interaction in spectroscopic methods as well as in nanophotonic applications. [ABSTRACT FROM AUTHOR]