Especially how do I interpret 2-D electronic spectra? What do the absorption and emission axes signify?
Hamm and Zanni. Concepts of and Methods of 2D Infrared Spectroscopy. 2011.
is an indispensable resource here.
Simply put, the excitation axis is obtained by performing a Fourier Transform along an excitation scan performed in the time domain. The "emission" axis is obtained in the conventional sense, by dispersing the probe light in a spectrograph.
So, 2D electronic spectroscopy can circumvent the challenge associated with broad bandwith of short pulses. In other words, performing the 2D ES measurement circumvents the issue that when you compress your pulse your bandwidth increases. Even though your bandwidth increases, you have the ultimate "spectral resolution" because you have spread your spectrum over both "emission" and "excitation" axis.
2D Electronic Spectroscopy
The techniques of multidimensional Fourier transform spectroscopy have revolutionized nuclear magnetic resonance (NMR), making it an invaluable tool for determining high resolution structures of complicated biomolecules. NMR can also study dynamics, but on limited time scales. Two dimensional electronic spectroscopy (2DES) is the optical analog of the simplest multidimensional NMR experiment. In analogy to 2D NMR, the 2DES spectrum reveals the coupling between electronic transitions, which appear as cross-peaks. The underlying lineshapes, describing the system dynamics are also revealed in the 2D spectrum, free from inhomogeneous broadening. Our group has been working to make 2DES a simple and accessible technique, and to expand the information content of 2DES for applications to understanding natural and artificial light-harvesting.
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