We have performed muon spin rotation/relaxation (muSR) measurements on single crystals of the chiral helimagnet Cr1/3NbS2 at zero to low magnetic field. The transition from the paramagnetic to helical magnetically ordered phase at zero field is marked by the onset of a coherent oscillation of the zero-field muon spin polarization below a critical temperature Tc. An enhancement of the muon spin precession frequency is observed below T ~ 50K, where anomalous behavior has been observed in bulk transport measurements. The enhanced precession frequency indicates a low-temperature modification of the helical magnetic structure. A Landau free energy analysis suggests that the low-temperature change in the magnetic structure is caused by a structural change, whereas the magnetic order above Tc is the result of an attractive interaction between the ferromagnetic moment induced by the applied field and the magnetic moments of the helical structure. We also suggest a longer periodicity of helicity below T ~ 50K, which can be verified by neutron scattering.
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