$^{63/65}$Cu- and $^{35/37}$Cl-NMR Studies of Triplet Localization in the Quantum Spin System NH$_4$CuCl$_3$

TL;DR

This study uses $^{63/65}$Cu- and $^{35/37}$Cl-NMR to investigate triplet localization in NH$_4$CuCl$_3$, revealing temperature-dependent localization behavior and triplet distribution at different magnetic phases.

Contribution

It provides detailed NMR evidence of triplet localization and distribution in NH$_4$CuCl$_3$, clarifying the low-temperature magnetic structure and constraining theoretical models.

Findings

Triplet localization occurs below 6 K.

Triplets are equally distributed among dimers at high fields.

Cl NMR reveals different hyperfine interactions at singlet and triplet sites.

Abstract

$^{63/65}$Cu- and $^{35/37}$Cl-NMR experiments were performed to investigate triplet localization in the $S=1/2$ dimer compound NH$_4$CuCl$_3$, which shows magnetization plateaus at one-quarter and three-quarters of the saturation magnetization. In $^{63/65}$Cu-NMR experiments, signal from only the singlet Cu site was observed, because that from the triplet Cu site was invisible due to the strong spin fluctuation of onsite 3$d$-spins. We found that the temperature dependence of the shift of $^{63/65}$Cu-NMR spectra at the singlet Cu site deviated from that of macroscopic magnetization below T=6 K. This deviation is interpreted as the triplet localization in this system. From the $^{35/37}$Cl-NMR experiments at the 1/4-plateau phase, we found the two different temperature dependences of Cl-shift, namely the temperature dependence of one deviates below T=6 K from that of the macroscopic magnetization as observed in the $^{63/65}$Cu-NMR experiments, whereas the other corresponds well with that of the macroscopic magnetization in the entire experimental temperature region. We interpreted these dependences as reflecting the transferred hyperfine field at the Cl site located at a singlet site and at a triplet site, respectively. This result also indicates that the triplets are localized at low temperatures. $^{63/65}$Cu-NMR experiments performed at high magnetic fields between the one-quarter and three-quarters magnetization plateaus have revealed that the two differently oriented dimers in the unit cell are equally occupied by triplets, the fact of which limits the theoretical model on the periodic structure of the localized triplets.