Abstract
Two-dimensional correlation spectroscopy (2DCOS) without a priori knowledge of meaningful spectral sampling order is considered. Construction of synchronous 2D correlation spectrum does not require the knowledge of sampling order, and disrelation spectrum derived from synchronous spectrum possesses useful features similar to those of asynchronous spectrum. Disrelation analysis may provide enhanced spectral resolution and distinction of bands arising from different sources but not the sequential order of intensity variations. Dataset sampled in an arbitrary or scrambled order may be reassembled into a more structured form by rank ordering the spectra with the intensity of a select band. If there is no meaningful data structure, asynchronous 2D correlation should not be attempted, although synchronous and disrelation spectra may still be useful. The intrinsic ambiguity in the direction of sampling order may sometimes be resolved using additional physical information known about the sample system.
Published Version
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