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Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glassinto the dynamics of molecular systems. In particular two-dimensionalelectronic spectroscopy (2DES) provides a probe of coherence and the flow ofenergy within quantum systems which is not possible with more conventionaltechniques. While heterodyne-detected (HD) 2DES is increasingly common, morerecently fluorescence-detected (FD) 2DES offers new opportunities, includingsingle-molecule experiments. However in both techniques it can be difficult tounambiguously identify the pathways which dominate the signal. Therefore theuse of numerically modelling of 2DES is vitally important, which in turnrequires approximating the pulsing scheme to some degree. Here we employnon-pertubative time evolution to investigate the effects of finite pulse widthand amplitude on 2DES signals. In doing so we identify key differences in theresponse of HD and FD detection schemes, as well as the regions of parameterspace where the signal is obscured by unwanted artefacts in either technique.Mapping out parameter space in this way provides a guide to choosingexperimental conditions and also shows in which limits the usual theoreticalapproximations work well and which limits more sophisticated approaches arerequired.

Two-dimensional spectroscopy beyond the perturbative limit: the influence of finite pulses and detection modes