Physikalische und Theoretische Chemie, Institut für Chemie und Biochemie, Freie Universität Berlin, Takustr. 3, 14195 Berlin, Germany.
Faraday Discuss. 2011;153:361-73; discussion 395-413. doi: 10.1039/c1fd00032b.
Coherent excitation of a superposition of Rydberg states in neon by the 13th harmonic of an intense 804 nm pulse and the formation of a wave packet is reported. Pump-probe experiments are performed, where the 3d-manifold of the 2p6-->2p5 (2P3/2) 3d [1/2]1- and 2p6-->2p5 (2P3/2) 3d [3/2]1-transitions are excited by an extreme ultraviolet (XUV) radiation pulse, which is centered at 20.05 eV photon energy. The temporal evolution of the excited state population is probed by ionization with a time-delayed 804 nm pulse. Control of coherent transient excitation and wave packet dynamics in the XUV-regime is demonstrated, where the spectral phase of the 13th harmonic is used as a control parameter. Modulation of the phase is achieved by propagation of the XUV-pulse through neon of variable gas density. The experimental results indicate that phase-shaped high-order harmonics can be used to control fundamental coherent excitation processes in the XUV-regime.
报道了通过强 804nm 脉冲的 13 次谐波相干激发氖的里德堡态叠加,并形成波包。进行了泵浦-探测实验,其中通过极紫外(XUV)辐射脉冲激发 2p6-->2p5(2P3/2)3d [1/2]1-和 2p6-->2p5(2P3/2)3d [3/2]1-跃迁的 3d 态。通过延迟的 804nm 脉冲进行电离来探测激发态种群的时间演化。在 XUV 区域中证明了相干瞬态激发和波包动力学的控制,其中 13 次谐波的光谱相位用作控制参数。通过在不同气体密度的氖中传播 XUV 脉冲来实现相位调制。实验结果表明,相位整形的高次谐波可用于控制 XUV 区域中的基本相干激发过程。