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First systematic spin probe ESR study of water freezing has been conductedusing TEMPOL and TEMPO as the probes. The spin probe signature of the waterfreezing has been described in terms of the collapse of narrow triplet spectruminto a single broad line. This spin probe signature of freezing has beenobserved at an anomalously low temperature when a milimoler solution of TEMPOLis slowly cooled from room temperature. A systematic observation has revealed aspin probe concentration dependence of these freezing and respective meltingpoints. These results can be explained in terms of localization of spin probeand liquid water, most probably in the interstices of ice grains, in an icematrix. The lowering of spin probe freezing point, along with the secondaryevidences, like spin probe concentration dependence of peak-to-peak width infrozen limit signal, indicates a possible size dependence of theselocalizations/entrapments with spin probe concentration. A weak concentrationdependence of spin probe assisted freezing and melting points, which has beenobserved for TEMPO in comparison to TEMPOL, indicates different natures ofinteractions with water of these two probes. This view is also supported by therelaxation behavior of the two probes.

Spin Probe ESR Signature of Freezing in Water: Is it Global or Local?