Angle-resolved photoemission study of MX-chain compound [Ni(chxn)$_2$Br]Br$_2$

Abstract

We report on the results of angle-resolved photoemission experiments on a quasi-one-dimensional $MX$-chain compound [Ni(chxn)$_2$Br]Br$_2$ (chxn = 1$R$,2$R$-cyclohexanediamine), a one-dimensional Heisenberg system with $S=1/2$ and $J \sim 3600$ K, which shows a gigantic non-linear optical effect. A &#34;band&#34; having about 500 meV energy dispersion is found in the first half of the Brillouin zone $(0\le kb/π<1/2)$, but disappears at $kb / π\sim 1/2$. Two dispersive features, expected from the spin-charge separation, as have been observed in other quasi-one-dimensional systems like Sr$_2$CuO$_3$, are not detected. These characteristic features are well reproduced by the $d$-$p$ chain model calculations with a small charge-transfer energy $Δ$ compared with that of one-dimensional Cu-O based compounds. We propose that this smaller $Δ$ is the origin of the absence of clear spin- and charge-separation in the photoemission spectra and strong non-linear optical effect in [Ni(chxn)$_2$Br]Br$_2$.