Model-free reconstruction of magnetic correlations in frustrated magnets

Frustrated magnetic systems exhibit extraordinary physical properties but quantification of their magnetic correlations poses a serious challenge to experiment and theory. Current insight into frustrated magnetic correlations relies on modelling techniques such as reverse Monte Carlo methods, which require knowledge about the exact ordered atomic structure. Here we present a method for direct reconstruction of magnetic correlations in frustrated magnets by three-dimensional difference pair distribution function analysis of neutron total scattering data. The methodology is applied to the disordered frustrated magnet bixbyite, (Mn1-xFex)2O3, which reveals nearest-neighbor antiferromagnetic correlations for the metal sites up to a range of approximately 15 {\AA}. Importantly, this technique allows for magnetic correlations to be determined directly from the experimental data without any assumption about the atomic structure

Unusual Phase Transitions and Magnetoelastic Coupling in TlFe1.6Se2 Single Crystals

Structural, magnetic, electrical transport, and heat capacity data are reported for single crystals of TlFe1.6Se2. This compound crystallizes in a tetragonal structure similar to the ThCr2Si2 structure, but with vacancies in the Fe layer. The vacancies can be ordered or disordered depending on temperature and thermal history. If the vacancies are ordered, the basal plane lattice constant increases from a to \sqrt{5}a. Antiferromagnetic order with the Fe spins along the c-axis occurs below T_N ~ 430K as shown by single crystal neutron diffraction and the magnetic structure is reported. In addition, for the vacancy ordered crystal, two other phase transitions are found at T_1 ~ 140K, and T_2 ~ 100K. The phase transitions at T_1 and T_2 are evident in heat capacity, magnetic susceptibility, resistivity data, a and c lattice parameters, and in the unusual temperature dependence of the magnetic order parameter determined from neutron scattering. The phase transitions at T_1 and T_2 result in significant changes in the magnetic moment per iron, with 1.72(6)\mu_B observed at 300K, 2.07(9)\mu_B at 140\,K, 1.90(9)\,\mu_B at 115\,K, and 1.31(8)\mu_B for 5\,K if the same "block checkerboard" magnetic structure is used at all temperatures. The phase transitions appear to be driven by small changes in the c lattice constant, large magnetoelastic coupling, and the localization of carriers with decreasing temperature.Comment: Accepted for publication in Physical Review

The magnetic and crystal structures of Sr2IrO4: A neutron diffraction study

We report a single-crystal neutron diffraction study of the layered $\rm Sr_2IrO_4$. This work unambiguously determines the magnetic structure of the system and reveals that the spin orientation rigidly tracks the staggered rotation of the $\rm IrO_6$ octahedra in $\rm Sr_2IrO_4$. The long-range antiferromagnetic order has a canted spin configuration with an ordered moment of 0.208(3) $\mu_B$/Ir site within the basal plane; a detailed examination of the spin canting yields 0.202(3) and 0.049(2) $\mu_B$/site for the a axis and the b axis, respectively. It is intriguing that forbidden nuclear reflections of space group $I4_1/acd$ are also observed in a wide temperature range from 4 K to 600 K, which suggests a reduced crystal structure symmetry. This neutron-scattering work provides a direct, well-refined experimental characterization of the magnetic and crystal structures that are crucial to the understanding of the unconventional magnetism exhibited in this unusual magnetic insulator.Comment: the version appeared in PR

Spin reorientation in TlFe1.6Se2 with complete vacancy ordering

The relationship between vacancy ordering and magnetism in TlFe1.6Se2 has been investigated via single crystal neutron diffraction, nuclear forward scattering, and transmission electron microscopy. The examination of chemically and structurally homogenous crystals allows the true ground state to be revealed, which is characterized by Fe moments lying in the ab-plane below 100K. This is in sharp contrast to crystals containing regions of order and disorder, where a competition between c-axis and ab-plane orientations of the moments is observed. The properties of partially-disordered TlFe1.6Se2 are therefore not associated with solely the ordered or disordered regions. This contrasts the viewpoint that phase separation results in independent physical properties in intercalated iron selenides, suggesting a coupling between ordered and disordered regions may play an important role in the superconducting analogues.Comment: Minor changes; updated references and funding acknowledgemen

Structure symmetry determination and magnetic evolution in Sr2Ir1−xRhxO4\rm Sr_2Ir_{1-x}Rh_{x}O_4

We use single-crystal neutron diffraction to determine the crystal structure symmetry and the magnetic evolution in the rhodium doped iridates $\rm Sr_2Ir_{1-x}Rh_{x}O_4$ ($0\leq x \leq 0.16$). Throughout this doping range, the crystal structure retains a tetragonal symmetry (space group $I4_1/a$) with two distinct magnetic Ir sites in the unit cell forming staggered $\rm IrO_6$ rotation. Upon Rh doping, the magnetic order is suppressed and the magnetic moment of Ir$^{4+}$ is reduced from 0.21 $\rm \mu_B$/Ir for $x=0$ to 0.18 $\rm \mu_B$/Ir for $x=0.12$. The magnetic structure at $x=0.12$ is different from that of the parent compound while the moments remain in the basal plane.Comment: Accepted for publication in Phys. Rev.

Direct evidence of a zigzag spin chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation on single crystal Na2IrO3\rm Na_2IrO_3

We have combined single crystal neutron and x-ray diffractions to investigate the magnetic and crystal structures of the honeycomb lattice $\rm Na_2IrO_3$. The system orders magnetically below $18.1(2)$ K with Ir$^{4+}$ ions forming zigzag spin chains within the layered honeycomb network with ordered moment of $\rm 0.22(1) \mu_B$/Ir site. Such a configuration sharply contrasts the N{\'{e}}el or stripe states proposed in the Kitaev-Heisenberg model. The structure refinement reveals that the Ir atoms form nearly ideal 2D honeycomb lattice while the $\rm IrO_6$ octahedra experience a trigonal distortion that is critical to the ground state. The results of this study provide much-needed experimental insights into the magnetic and crystal structure crucial to the understanding of the exotic magnetic order and possible topological characteristics in the 5$d$-electron based honeycomb lattice.Comment: Revised version as that to appear in PR

Magnetic and Crystal Structures of Sr\u3csub\u3e2\u3c/sub\u3eIrO\u3csub\u3e4\u3c/sub\u3e: A Neutron Diffraction Study

We report a single-crystal neutron diffraction study of the layered Sr2IrO4. This work unambiguously determines the magnetic structure of the system and reveals that the spin orientation rigidly tracks the staggered rotation of the IrO6 octahedra in Sr2IrO4. The long-range antiferromagnetic order has a canted spin configuration with an ordered moment of 0.208(3) μB/Ir site within the basal plane; a detailed examination of the spin canting yields 0.202(3) and 0.049(2) μB/site for the a axis and the b axis, respectively. It is intriguing that forbidden nuclear reflections of space group I41/acd are also observed in a wide temperature range from 4 K to 600 K, which suggests a reduced crystal structure symmetry. This neutron-scattering work provides a direct, well-refined experimental characterization of the magnetic and crystal structures that are crucial to the understanding of the unconventional magnetism exhibited in this unusual magnetic insulator