Electronic and nuclear dynamics of alkali atoms adsorbed on noble metal surfaces are investigated in real time by the interferometric time-resolved two-photon photoemission technique.@footnote 1@ Photoinduced charge transfer with a <20 fs laser pulse turns on repulsive Coulomb force between alkali atoms and the substrate, thereby initiating desorption from the surface. The resulting nuclear wave packet motion is detected through changes in the surface electronic structure. In the extreme case of Cs/Cu(111), the alkali atom desorptive motion can be observed for up to 200 fs, which according to a Newton's law model corresponds to stretching of the Cu-Cs bond by ~0.3 Å.@footnote 2@ Furthermore, the coherent polarization created by the charge-transfer excitation persists for up to 60 fs. Demonstration of quantum control, whereby it is possible to generate displaced ground and excited state wave packets, is accomplished by interference between the pump and probe excited polarization in the sample.@footnote 3@ However, the photodesorption process is frustrated by the wave packet spreading and decay through recoil-induced phonon generation, reverse charge transfer, and electron inelastic scattering, which induce the phase and energy relaxation.@footnote 4@ Prospects of controlling the electronic and nuclear motion of atoms and molecules at surfaces will be discussed. @FootnoteText@ @footnote 1@S. Ogawa, H. Nagano, and H. Petek, Phys. Rev. Lett. 82, 1931 (1999). @footnote 2@H. Petek, H. Nagano, M. J. Weida, and S. Ogawa, Science 288, 1402 (2000). @footnote 3@H. Petek, M. J. Weida, H. Nagano, and S. Ogawa, J. Phys. Chem. A 104, 10234 (2000). @footnote 4@H. Petek, H. Nagano, M. J. Weida, and S. Ogawa, J. Phys. Chem. (Feature Article; in press). .