Abstract
We present a new data acquisition concept using optimized non-uniform sampling and compressed sensing reconstruction in order to substantially decrease the acquisition times in action-based multidimensional electronic spectroscopy. For this we acquire a regularly sampled reference data set at a fixed population time and use a genetic algorithm to optimize a reduced non-uniform sampling pattern. We then apply the optimal sampling for data acquisition at all other population times. Furthermore, we show how to transform two-dimensional (2D) spectra into a joint 4D time-frequency von Neumann representation. This leads to increased sparsity compared to the Fourier domain and to improved reconstruction. We demonstrate this approach by recovering transient dynamics in the 2D spectrum of a cresyl violet sample using just 25% of the originally sampled data points.
Highlights
Coherent two-dimensional (2D) electronic spectroscopy1–5 has become an established method to study, among others, energy transfer in light harvesting complexes,6–8 electronic dynamics in semiconductors,9–13 plasmonic coherences,14 and photochemical reactions.15 Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal
The rephasing signal is of particular interest in coherent 2D spectroscopy since it allows to observe molecular couplings and to extract the homogenous and inhomogeneous linewidths of the sample under study
We have suggested and implemented a new scheme for employing compressed sensing reconstruction in coherent two-dimensional (2D) spectroscopy
Summary
Coherent two-dimensional (2D) electronic spectroscopy has become an established method to study, among others, energy transfer in light harvesting complexes, electronic dynamics in semiconductors, plasmonic coherences, and photochemical reactions. Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal. Coherent two-dimensional (2D) electronic spectroscopy has become an established method to study, among others, energy transfer in light harvesting complexes, electronic dynamics in semiconductors, plasmonic coherences, and photochemical reactions.. Most of the experimental realizations rely on the non-collinear box geometry and heterodyned detection of a coherent optical signal. Another option that has been developed is action-based 2D spectroscopy using a train of four (often collinear) laser pulses and a phase-modulation, or phase-cycling scheme.. The action-based ansatz employs the detection of incoherent signals, e.g., fluorescence (see Fig. 1(a)), (photo)electrons, or (photo)-ions.. One advantage of detecting incoherent signals is that it permits the study of lowdensity samples, even down to the single-molecule limit.. Another option that has been developed is action-based 2D spectroscopy using a train of four (often collinear) laser pulses and a phase-modulation, or phase-cycling scheme. The action-based ansatz employs the detection of incoherent signals, e.g., fluorescence (see Fig. 1(a)), (photo)electrons, or (photo)-ions. One advantage of detecting incoherent signals is that it permits the study of lowdensity samples, even down to the single-molecule limit. A detailed comparison of various experimental 2D spectroscopy approaches can be found in a recent review.
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