Charge-order phase transition in the quasi one-dimensional organic conductor (TMTTF)$_2$NO$_3$

TL;DR

This study uses ESR measurements to identify a charge-order phase transition in (TMTTF)$_2$NO$_3$ at around 250 K, revealing anisotropic spin behavior linked to charge ordering in this quasi-one-dimensional organic conductor.

Contribution

First ESR evidence of charge-order phase transition in (TMTTF)$_2$NO$_3$, demonstrating anisotropic spin relaxation associated with charge ordering.

Findings

Charge-order phase develops below ~250 K.

ESR linewidth anisotropy indicates magnetically inequivalent sites.

No such ESR behavior in non-charge-ordered analogs.

Abstract

Low-dimensional organic conductors show a rich phase diagram, which has, despite all efforts, still some unexploed regions. Charge ordered phases present in many compounds of the (TMTTF)$_2 X$ family are typically studied with their unique electronic properties in mind. An influence on the spin arrangement is, however, not expected at first glance. Here, we report temperature and angle dependent electron spin resonance (ESR) measurements on the quasi one-dimensional organic conductor (TMTTF)$_2$NO$_3$. We found that the (TMTTF)$_2$NO$_3$ compound develops a peculiar anisotropy with a doubled periodicity ($ab'$-plane) of the ESR linewidth below about $T_\text{CO}=250\pm 10$ K. This behavior is similar to observations in the related compounds (TMTTF)$_2 X$ ($X$ = PF$_6$, SbF$_6$ and AsF$_6$), where it has been attributed to relaxation processes of magnetically inequivalent sites in the charge-ordered state. For the structural analogous (TMTTF)$_2$ClO$_4$, known for the absence of charge order, such angular dependence of the ESR signal is not observed. Therefore, our ESR measurements lead us to conclude that a charge-order phase is stabilized in the title compound below $T_\text{CO} \approx 250$ K.