Developing multidimensional electronic spectroscopy: lessons from NMR

Dr Jonathan Tollerud

Centre for Quantum and Optical Science, Swinburne University of Technology

Over the last decade, much effort has gone into the development of multidimensional electronic spectroscopy, in part due to conceptual similarities to multidimensional nuclear magnetic resonance (NMR). NMR has a nearly half century head start, and as a result many incisive variants have been developed. In fact, modern techniques and equipment allow for complete structural determination of complex molecules (including proteins). Due to the conceptual similarities in the techniques, there is much to be gained by translating some of these specialized experiments into multidimensional spectroscopy of electronic transitions. In this talk, I will discuss how the experimental approach underlying one particular technique (heteronuclear multi-quantum NMR) can be translated from 'nuclear' to 'electronic'.
Furthermore, I will describe some of the physical insights we have gained using more traditional variants of multidimensional electronic spectroscopy, including coupling of bright and dark states in semiconductor quantum wells and the appearance of what may be a superradiant state when extremely low excitation levels are used. I will also describe the multidimensional spectroscopy experiment we have implemented here at Swinburne, whose flexibility and stability have made these observations possible.

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