Compressed Sensing for Reconstructing Coherent Multidimensional Spectra

Abstract

We apply two sparse reconstruction techniques, the least absolute shrinkage and selection operator (LASSO) and the sparse exponential mode analysis (SEMA), to two-dimensional (2D) spectroscopy. The algorithms are first tested on model data, showing that both are able to reconstruct the spectra using only a fraction of the data required by the traditional Fourier-based estimator. Through the analysis of a sparsely sampled experimental fluorescence detected 2D spectra of LH2 complexes, we conclude that both SEMA and LASSO can be used to significantly reduce the required data, still allowing to reconstruct the multidimensional spectra. Of the two techniques, it is shown that SEMA offers preferable performance, providing more accurate estimation of the spectral line widths and their positions. Furthermore, SEMA allows for off-grid components, enabling the use of a much smaller dictionary than the LASSO, thereby improving both the performance and lowering the computational complexity for reconstructing coherent multidimensional spectra.

Excited States and Their Dynamics in CdSe Quantum Dots Studied by Two-Color 2D Spectroscopy

“…Recent developments in coherent multidimensional spectroscopy (CMDS) 18 − 27 have opened new possibilities for investigating excited-state dynamics with a very high level of precision in both time and spectral resolution. 28 , 29 The method has demonstrated its capabilities in studies of dynamics, including coherent evolution of both vibrational and electronic origin in both biomaterials and semiconductors.…”

“…Recent developments in coherent multidimensional spectroscopy (CMDS) − have opened new possibilities for investigating excited-state dynamics with a very high level of precision in both time and spectral resolution. , The method has demonstrated its capabilities in studies of dynamics, including coherent evolution of both vibrational and electronic origin in both biomaterials and semiconductors. , It has become increasingly popular to investigate quantum coherence, relaxation, and coupling of excited states by using CMDS. ,,, Numerous studies on excited-state dynamics in QDs have applied coherent 2D spectroscopy. ,,,, …”

High-sensitivity Fluorescence-Detected Multidimensional Electronic Spectroscopy Through Continuous Pump-probe Delay Scan

“…One such method, the spectral projected gradient approach, SPGL1 61 , was employed by Marcus and Aspuru-Guzik et al 22 to reconstruct 2D spectra of rubidium vapor by collecting a dense grid and then non-uniformly sampling the grid to reconstruct the spectrum obtained with the full grid. A similar approach has been demonstrated by Pullerits et al 62 . As a departure from previous approaches, we have used the ES scheme and collected the 15 × 15 grid from an independent experiment conducted on a different day such that the uniform and non-uniform data points do not share correlations.…”

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

“…50 We also sample uniformly, opting for simplicity rather than trying to reduce the computational cost with non-uniform sampling. 51,52 We do not investigate the polarization dependency, which is sometimes exploited to select specific pathways, [53][54][55][56][57] but it is known that the early time dynamics suffer from incorrect pulse-ordering artifacts. 58 We assume non-interacting chromophores in our calculations, although the delocalization of excitation energy in many cases is unexpectedly long-range 59 and its role in energy transfer is a hot topic in the field.…”