论文标题
非共振相干振幅转移在Attsond四波混合光谱中
Non-resonant Coherent Amplitude Transfer in Attosecond Four-Wave Mixing Spectroscopy
论文作者
论文摘要
使用XUV脉冲和两种非共线近红外脉冲的Attsond四波混合光谱谱法被用于测量由Atomic Argon中的3S电子激发产生的Rydberg Wavepacket动力学,使原子量的紫外线激发成一系列自动离子化的3S-1NP Rydberg States of 29 ev。来自单个Rydberg州的发射信号表现出振荡结构,并持续超出了发射的Rydberg国家的预期寿命。这些结果反映了寿命较长的Rydberg状态对每个单独检测状态的四个波混合发射信号的实质性贡献。波袋分解分析表明,相干振幅转移主要是从光激发的3S-1(n+1)p状态到观察到的3S-1NP Rydberg状态的。实验观察结果是通过使用电子结构和过渡矩计算的时间依赖性的Schrödinger方程模拟来重现的。该理论强调,在四波混合过程中,通过3S-1(n+1)S和3S-1(N+1)S和3S-1(N+1)S和3S-1(N-1)D黑暗状态通过近红外光线将连贯的振幅转移驱动到3S-1NP状态。
Attosecond four-wave mixing spectroscopy using an XUV pulse and two noncollinear near-infrared pulses is employed to measure Rydberg wavepacket dynamics resulting from extreme ultraviolet excitation of a 3s electron in atomic argon into a series of autoionizing 3s-1np Rydberg states around 29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the four wave mixing emission signals of each individually detected state. A wavepacket decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s-1(n+1)p states to the observed 3s-1np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. The theory highlights that coherent amplitude transfer is driven non-resonantly to the 3s-1np states by the near-infrared light through 3s-1(n+1)s and 3s-1(n-1)d dark states during the four-wave mixing process.