Abstract

The exchange of molecules between different physical or chemical environments due to diffusion or chemical transformations has a crucial role in a plethora of fundamental processes such as breathing, protein folding, chemical reactions and catalysis. Here, we introduce a method for a single-scan, ultrafast NMR analysis of molecular exchange based on the diffusion coefficient contrast. The method shortens the experiment time by one to four orders of magnitude. Consequently, it opens the way for high sensitivity quantification of important transient physical and chemical exchange processes such as in cellular metabolism. As a proof of principle, we demonstrate that the method reveals the structure of aggregates formed by surfactants relevant to aerosol research.

Highlights

  • The exchange of molecules between different physical or chemical environments due to diffusion or chemical transformations has a crucial role in a plethora of fundamental processes such as breathing, protein folding, chemical reactions and catalysis

  • Ultrafast (UF) Nuclear magnetic resonance (NMR) spectroscopy relies on spatial encoding of incremented evolution times into the layers of a sample by exploiting the principles of magnetic resonance imaging (MRI)[4,5]

  • The UF approach is capable of delivering any kind of 2D NMR spectra in a single scan[6], and spatial encoding in discrete layers by using frequency selective pulses along with gradients have been exploited in the measurement of single-scan exchange spectroscopy (EXSY) spectrum[7]

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Summary

Introduction

The exchange of molecules between different physical or chemical environments due to diffusion or chemical transformations has a crucial role in a plethora of fundamental processes such as breathing, protein folding, chemical reactions and catalysis. We introduce a method for a single-scan, ultrafast NMR analysis of molecular exchange based on the diffusion coefficient contrast. Ultrafast (UF) NMR spectroscopy relies on spatial encoding of incremented evolution times into the layers of a sample by exploiting the principles of magnetic resonance imaging (MRI)[4,5]. We have demonstrated that the principles of spatial encoding can be extended to multidimensional relaxation and diffusion correlation experiments under the concept of ultrafast Laplace NMR (UF LNMR)[9,10]. We show that UF LNMR allows single-scan exchange measurements via a Laplace NMR contrast (in this case molecular diffusion coefficient D). Contrary to the single-scan EXSY methods described above, the method introduced here is based on continuous spatial encoding and non-under-sampled data

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