Fuller Franklin D, Ogilvie Jennifer P
Department of Physics, University of Michigan, Ann Arbor, Michigan 48109; email:
Annu Rev Phys Chem. 2015 Apr;66:667-90. doi: 10.1146/annurev-physchem-040513-103623. Epub 2015 Feb 4.
Two-dimensional electronic spectroscopy (2DES) reveals connections between an optical excitation at a given frequency and the signals it creates over a wide range of frequencies. These connections, manifested as cross-peak locations and their lineshapes, reflect the underlying electronic and vibrational structure of the system under study. How these spectroscopic signatures evolve in time reveals the system dynamics and provides a detailed picture of coherent and incoherent processes. 2DES is rapidly maturing and has already found numerous applications, including studies of photosynthetic energy transfer and photochemical reactions and many-body interactions in nanostructured materials. Many systems of interest contain electronic transitions spanning the ultraviolet to the near infrared and beyond. Most 2DES measurements to date have explored a relatively small frequency range. We discuss the challenges of implementing 2DES and compare and contrast different approaches in terms of their information content, ease of implementation, and potential for broadband measurements.
二维电子光谱（2DES）揭示了给定频率的光激发与其在很宽频率范围内产生的信号之间的联系。这些联系表现为交叉峰位置及其线形，反映了所研究系统的潜在电子和振动结构。这些光谱特征如何随时间演变揭示了系统动力学，并提供了相干和非相干过程的详细图景。2DES正在迅速成熟，并且已经有了许多应用，包括对光合作用能量转移、光化学反应以及纳米结构材料中的多体相互作用的研究。许多感兴趣的系统包含跨越紫外到近红外及更远范围的电子跃迁。迄今为止，大多数2DES测量都探索了相对较小的频率范围。我们讨论了实施2DES的挑战，并在信息内容、实施难易程度和宽带测量潜力方面对不同方法进行了比较和对比。
