“…The increase in E SA band intensity with increasing magnetic field for NaCrF 3 at 2 K is not observed for KCrF 3 or other related Cr 2+ fluorides, e.g. Rb 2 CrCl 4 in which the E SF transitions decline in intensity with increasing magnetic field [22,23]. The increase could be related to the orbital structure and spin ordering correlations described in the Kugel-Khomskii Hamiltonian [24].…”
Chromium (II) fluoroperovskites ACrF3(A= Na + , K + ) are strongly correlated Jahn-Teller active materials at low temperatures. In this paper, we examine the role that the A-site ion plays in this family of fluoroperovskites using both experimental methods (XRD, optical absorption spectroscopy and magnetic fields) and DFT simulations. Temperature-dependent optical absorption experiments show that the spin-allowed transitions E2 and E3 only merge completely for A= Na at 2 K. Fielddependent optical absorption measurements at 2 K show that the oscillating strength of the spinallowed transitions in NaCrF3 increases with increasing applied field. Direct magneto-structural correlations which suppress the spin-flip transitions are observed for KCrF3 below its Neél temperature. In NaCrF3 the spin-flip transitions vanish abruptly below 9 K revealing magneto-optical correlations not linked to crystal structure changes. This suggests that as the long range ordering is reduced local JT effects in the individual CrF 4− 6 octahedra take control of the observed behavior. Our results show clear deviation from the pattern found for the isoelectronic AxMnF3+x system. The size of the A-site cation is shown to be central in dictating the physical properties and phase transitions in ACrF3, opening up the possibility of varying the composition to create novel states of matter with tuneable properties.
“…The increase in E SA band intensity with increasing magnetic field for NaCrF 3 at 2 K is not observed for KCrF 3 or other related Cr 2+ fluorides, e.g. Rb 2 CrCl 4 in which the E SF transitions decline in intensity with increasing magnetic field [22,23]. The increase could be related to the orbital structure and spin ordering correlations described in the Kugel-Khomskii Hamiltonian [24].…”
Chromium (II) fluoroperovskites ACrF3(A= Na + , K + ) are strongly correlated Jahn-Teller active materials at low temperatures. In this paper, we examine the role that the A-site ion plays in this family of fluoroperovskites using both experimental methods (XRD, optical absorption spectroscopy and magnetic fields) and DFT simulations. Temperature-dependent optical absorption experiments show that the spin-allowed transitions E2 and E3 only merge completely for A= Na at 2 K. Fielddependent optical absorption measurements at 2 K show that the oscillating strength of the spinallowed transitions in NaCrF3 increases with increasing applied field. Direct magneto-structural correlations which suppress the spin-flip transitions are observed for KCrF3 below its Neél temperature. In NaCrF3 the spin-flip transitions vanish abruptly below 9 K revealing magneto-optical correlations not linked to crystal structure changes. This suggests that as the long range ordering is reduced local JT effects in the individual CrF 4− 6 octahedra take control of the observed behavior. Our results show clear deviation from the pattern found for the isoelectronic AxMnF3+x system. The size of the A-site cation is shown to be central in dictating the physical properties and phase transitions in ACrF3, opening up the possibility of varying the composition to create novel states of matter with tuneable properties.
“…(12) and (13) have been used for Rb 2 CrCl 4 and related systems in, e.g. [64][65][66][67][68][69][70][71]. Below only a few selected examples are explicitly provided.…”
“…These very weak lines are associated with electronic origins and they have a magnetic dipole character because the approximate symmetry at each Cr2+ site is centrosymmetric Z)4h. The bands in the two selected spectral regions have been discussed (Janke et al 1982) as pure spin-flips and it is now believed that the appropriate assign ments with tetragonal (octahedral) notations are 5B lg (5Eg)-> 3B lg (3Eg(3H)) and N ___ E/cm 1 F ig u r e 7. Influence of a magnetic field .£?//[ 100] in region I at 1.4 K. The magnon occupation number nk is the average value (otk a.ky or (P£ fiP).…”
Section: (B) Experimental Study Of Absorption Profilesmentioning
confidence: 99%
“…The result of the competition between the ferromagnetic exchange and the anisotropy terms is a structure with spins on neighbouring ions canted at an angle + 6 from the easy [110] direction (Janke et al 1983) and the occurrence of a small gap in the acoustic spin-wave branch. Applying a magnetic field along one of the relatively hard [100] or hard [001] axes, this gap should first decrease to zero at a critical field B& or Bc and then rise again (Elliott et al 1980; Harrop The unusual temperature dependence of the visible absorption bands in Rb2CrCl4 has been the subject of several experimental studies (Day 1979 ;Janke et al 1982). Attention has concentrated on two regions, near 631 an 530 nm.…”
Section: Introductionmentioning
confidence: 99%
“…Although the main features of the temperature-and field-dependence of intensity of the hot magnon sidebands are reasonably well understood (Gregson et al 1976;Janke et al 1982), the method of simulating the band profiles (Elliott et al 1980) has not been given in detail. Harrop (1981) calculated band shapes by numerical methods involving a mesh of points throughout the Brillouin zone, in the absence or presence of a relatively large (greater than 1 T) magnetic field.…”
Eigenvalues and eigenfunctions of the spin waves in Rb
2
CrCl
4
, in the absence or presence of a magnetic field oriented along (or slightly off) one of the major crystallographic axes, are given in detail for the first time. We present a simple model to simulate the profiles of exchange induced exciton-magnon combination bands in canted ferromagnets, under various experimental conditions of temperature and magnetic field. This model is used to analyse new high-resolution magneto-optical data at low and very low (0.35 K) temperatures and to derive precise anisotropy parameters. It can be applied with only slight modifications to metamagnets showing axial or planar anisotropy.
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