Accelerated 2D-IR Using Compressed Sensing

Abstract

A fundamental aspect of Fourier transform (FT) spectroscopy is the inverse relationship between frequency resolution and the maximum scanned time delay. In situations where essential chemical information is contained in spectral peak amplitudes rather than in their detailed shapes, it is possible to dramatically reduce the experimental acquisition time of time domain methods such as two-dimensional infrared (2D-IR) spectroscopy. By introducing compressed sensing to the analysis and experimental design of 2D-IR spectroscopy, we show that waiting-time-dependent 2D peak amplitudes reproduce conventional FT acquisition and analysis but can be recorded in a fraction of the time. Peak amplitude data are often sufficient for measuring intramolecular vibrational redistribution, vibrational coherence, chemical exchange, population, and orientational relaxation, as well as spectral diffusion.

Optimizing sparse sampling for 2D electronic spectroscopy

“…45 Furthermore, it was shown that CS reconstruction can also be used to retrieve the 2D spectrum from a uniformly sampled subset of the full signal. 46 Other non-uniform sampling protocols, such as exponentially biased, radial, or Poisson-gap sampling, are successfully applied in multidimensional NMR. [47][48][49][50] They benefit from a priori assumptions on the approximate signal characteristics and use a dense sampling close to the origin of the time domain where the signal amplitudes are still large.…”

Less is More: How Compressed Sensing is Transforming Metrology in Chemistry

“…Compressed sensing provides a mathematical framework to unify signal reconstruction techniques across a variety of disciplines and hence will enable algorithms that have been established as robust in applications such as astronomy to be readily implemented in, e.g., NMR spectroscopy. We can therefore expect sparse sampling techniques to become commonplace in all areas of spectroscopy research, indeed compressed sensing has recently been demonstrated for 2D Fourier transform infrared spectroscopy 71…”

Light-powered molecular logic goes nonlinear

“…The time needed to scan the laser pulses and acquire sufficient signal-to-noise can sometimes present an issue. This might be alleviated to some extent by using cutting edge techniques such as compressed sensing (15,16). One of the requirements for capitalizing fully on the 2DES method for implementing molecular logic is that signal generation pathways need to be deconvolved.…”