Demystifying Multidimensional Electronic Spectroscopy

Howe-Siang Tan
Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore

In recent years, coherent multidimensional electronic spectroscopy has added much to the study in the Light Harvesting processes, in attempting to study if quantum coherences lead to a more efficient and robust excitation energy transfer, and to clarify the various pathways in excitation energy transfer processes. However to many, the technique remains mysterious and difficult to comprehend.

Our research group has been at the forefront of developing the coherent multidimensional electronic spectroscopy techniques [1-3] and have used it to study the excitation energy transfer processes in LHC II [4-6].

This presentation will be an introduction and tutorial of the basics of multidimensional electronic spectroscopy. Multidimensional electronic spectroscopy is an extension of the more widely used pump-probe or transient absorption spectroscopy, and we will use transient absorption spectroscopy as a basis to explain multidimensional electronic spectroscopy.

We will describe the various experimental setup used to perform 2D and 3D electronic spectroscopy and compare their advantages and limitations. We will also briefly introduce the basic formalism and theory used to describe multidimensional electronic spectroscopy, and how it has been applied to study light harvesting systems.

References

[1] H.-S. Tan, J. Chem. Phys., 2008, 129, 124501 (2008).
[2] Z. Zhang, K.L. Wells, and H.-S. Tan, Opt. Lett. 2012, 37, 5058-5060.
[3] Z. Zhang, K.L. Wells, E.W.J. Hyland, and H.-S. Tan. Chem. Phys. Lett., 2012, 550, 156-161.
[4] K.L. Wells, P.H. Lambrev, Z. Zhang, G. Garab and H.-S. Tan, Phys. Chem. Chem. Phys., 2014, 16, 11640-11646.
[5] M.M. Enriquez, P. Ahktar, C. Zhang, G. Garab, P.H. Lambrev and H.-S. Tan, J. Chem. Phys., 2015, 142, 212432.
[6] Z. Zhang, P.H. Lambrev, K.L. Wells, G. Garab, H.-S. Tan, Nat. Comm. 2015, 6, 7194.