Long-range Magnetic Order Research Articles

Hubbard Bands and Exotic States in Doped and Undoped Mott Systems: The Kotliar–Ruckenstein Representation

The slave–particle representation is a promising method to treat the properties of exotic strongly correlated systems. We develop a unified approach to describe both the paramagnetic state with possible spin–liquid features and states with strong long-range or short-range magnetic order. Combining the Kotliar–Ruckenstein representation and fractionalized spin–liquid deconfinement picture, the Mott transition and Hubbard subbands are considered. The spectrum in the insulating state is significantly affected by the presence of the spinon spin–liquid spectrum and a hidden Fermi surface. Presenting a modification of the Kotliar–Ruckenstein representation in the spin–wave region, we treat the case of magnetic order, with special attention being paid to the half-metallic ferromagnetic state. The formation of small and large Fermi surfaces for doped current carriers in the antiferromagnetic state is also discussed.

Magnetic ordering in the layered oxyhalide Sr2NiO2Cl2

The full characterisation of the high-pressure-synthesised, metastable layered oxyhalide Sr2NiO2Cl2 is reported. It is comprised of infinite NiO2 layers along with double rock salt Sr2Cl2 layers and is closely related to the n = 1 Ruddlesden-Popper phases. At ambient temperature, it crystallises in the tetragonal space group I4/mmm with 2 formula units per unit cell with the basal lattice parameters a = b = 4.03417(2) Å and the stacking direction lattice parameter, c = 15.1058(1) Å. A tiny cusp in the temperature dependence of the magnetic susceptibility in a previous report suggested that this oxyhalide underwent long-range magnetic order and therefore contained high-spin Ni2+ ions. Powder neutron diffraction has confirmed that Sr2NiO2Cl2 is a localised-moment oxyhalide, adopting the high-spin S = 1 configuration with fully occupied dxz, dyz and dxy orbitals and partially occupied dz2 and dx2-y2 orbitals. The Ni2+ magnetic moments order antiferromagnetically below ≈ 180 K in a G-type arrangement on a √2a × √2a × c expansion of the nuclear cell with the propagation vector (½, ½, 0) and with a saturated long-range ordered magnetic moment of 1.57(7) μB per Ni2+ cation which is in line with previously calculated computational results and showing that the ligand field around the Ni2+ cation is not sufficiently anisotropic to drive it into the low-spin, diamagnetic configuration found for this d8 cation in square planar or highly elongated octahedral coordination.

Long-range magnetic order in the quasicrystals and approximants

Long-range magnetic order in the quasicrystals and approximants

Uncommon Magnetism in Rare-Earth Intermetallic Compounds with Strong Electronic Correlations

Rare-earth intermetallic compounds are characterised by the presence of a long-range magnetic order due to the interaction of local magnetic moments periodically located within the crystal lattice. This paper considers the possibility of forming an ordered state in cases where there is no opportunity to observe the local moment of the f-electronic shell in a traditional sense. These are, first of all, systems with a singlet ground state, as well as systems with fast spin fluctuations caused by a homogeneous intermediate-valence state of a rare-earth ion. Extensive experimental studies of these effects using neutron diffraction, neutron spectroscopy, and high-pressure studies of the magnetic phase diagram are presented and analysed, and the corresponding microscopic model representations are discussed. In particular, the possible origin of long-range magnetic order in mixed-valence compounds is analysed.

Magnetic properties of V[formula omitted]MnGa, V[formula omitted]MnAl, V[formula omitted]FeGa and V[formula omitted]FeAl

The investigated materials belong to Heusler compounds and are similar in composition to titanium-based analogs, like Ti2MnAl, which was suspected of exhibiting Spin Gapless Semiconductor (SGS) or Weyl semimetal state in some earlier papers. The vanadium-based materials are not well known in earlier reports. We show the results of our XRD analysis of the synthesized samples, their magnetic properties, and their resistivity measured vs. temperature as well as magnetic field. Heusler compounds can crystallize in simple or inverted structures, here we try to resolve which one is more probable in these materials and whether the SGS state can exist in them or not. From our measurements it is clear that in these samples both of those crystal structures coexist, and they do not show signs of long range magnetic ordering. The ground state obtained from our ab-initio calculations should be magnetic for both structural models, which means that the disorder induced by the coexistence of those two structures at the same time eliminates the long-range magnetic ordering.

Kondo interaction in FeTe and its potential role in the magnetic order

Finding d-electron heavy fermion states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator. Yet, obtaining direct spectroscopic evidence for a d-electron heavy fermion system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy, scanning tunneling spectroscopy and transport property measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle and Fano-type tunneling spectra at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order.

On the magnetic structures of 1:1:1 stoichiometric topological phases LnSbTe (Ln = Pr, Nd, Dy and Er)

LnSbTe (Ln – lanthanide) group of materials, belonging to ZrSiS/PbFCl (P4/nmm) structure type, is a platform to study the phenomena originating from the interplay between the electronic correlations, magnetism, structural instabilities and topological electronic structure. Here we report a systematic study of magnetic properties and magnetic structures of LnSbTe materials. The studied materials undergo antiferromagnetic ordering at TN = 2.1 K (Ln = Er), 6.7 K (Ln = Dy), 3.1 K (Ln = Nd). Neutron powder diffraction reveals ordering with k1 = (½ + δ 0 0) in ErSbTe, k2 = (½ 0 ¼) in NdSbTe. DySbTe features two propagation vectors k2 and k4 = (0 0 ½). No long-range magnetic order is observed in PrSbTe down to 1.8 K. We propose the most probable models of magnetic structures, discuss their symmetry and possible relation between the electronic structure and magnetic ordering.

Resonant Elastic X-Ray Scattering of Antiferromagnetic Superstructures in EuPtSi_{3}.

We report resonant elastic x-ray scattering of long-range magnetic order in EuPtSi_{3}, combining different scattering geometries with full linear polarization analysis to unambiguously identify magnetic scattering contributions. At low temperatures, EuPtSi_{3} stabilizes type A antiferromagnetism featuring various long-wavelength modulations. For magnetic fields applied in the hard magnetic basal plane, well-defined regimes of cycloidal, conical, and fanlike superstructures may be distinguished that encompass a pocket of commensurate type A order without superstructure. For magnetic field applied along the easy axis, the phase diagram comprises the cycloidal and conical superstructures only. Highlighting the power of polarized resonant elastic x-ray scattering, our results reveal a combination of magnetic phases that suggest a highly unusual competition between antiferromagnetic exchange interactions with Dzyaloshinsky-Moriya spin-orbit coupling of similar strength.

Magnetic properties of S=12 distorted J1−J2 honeycomb lattice compound NaCuIn(PO4)2

The subtle interplay between low-dimensionality and spin correlations can lead to exotic ground states with unconventional excitations in two-dimensional honeycomb-lattice-based quantum magnets. Herein, we present the structural, magnetic, and heat capacity measurements; density functional theory $+$ Hubbard $U$ ($\mathrm{DFT}+U$) based electronic structure calculations; and quantum Monte Carlo simulations for $\mathrm{NaCuIn}{({\mathrm{PO}}_{4})}_{2}$. The structure of $\mathrm{NaCuIn}{({\mathrm{PO}}_{4})}_{2}$ consists of a well-separated, $\mathit{S}=\frac{1}{2}$ distorted ${\mathit{J}}_{1}\text{\ensuremath{-}}{\mathit{J}}_{2}$ honeycomb layer which is a combination of the magnetic couplings ${\mathit{J}}_{1}$ (forming spin dimers) and ${\mathit{J}}_{2}$ (constituting spin chains). At high temperatures, the magnetic susceptibility $\ensuremath{\chi}(T)$ follows paramagnetic behavior with a Curie-Weiss temperature ${\ensuremath{\theta}}_{\mathrm{CW}}\ensuremath{\approx}\ensuremath{-}16$ K, implying the presence of antiferromagnetic interactions. A broad maximum is observed at about $13\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ in $\ensuremath{\chi}(T)$, indicating the presence of short-range spin correlations. The quantum Monte Carlo simulations using the $\mathit{S}=\frac{1}{2}\phantom{\rule{4pt}{0ex}}{\mathit{J}}_{1}\text{\ensuremath{-}}{\mathit{J}}_{2}$ Heisenberg model on a distorted honeycomb lattice are in good agreement with the measured magnetic susceptibility data. The obtained ratio of the exchange couplings ($\frac{{\mathit{J}}_{2}}{{\mathit{J}}_{1}}$) is 2.63, which is consistent with the value obtained from our $\mathrm{DFT}+U$ calculations. The title material undergoes a magnetic long-range order at 0.4 K in the heat capacity, which is suppressed with an applied magnetic field of 10 kOe. The magnetic heat capacity data follow a linear temperature-dependent behavior well above the transition temperature, suggesting the presence of gapless excitations. The observed behavior can be attributed to the presence of low connectivity and weak magnetic frustration in this two-dimensional distorted honeycomb lattice.

Spin-liquid state with precursor ferromagnetic clusters interacting antiferromagnetically in frustrated glassy tetragonal spinel Zn0.8Cu0.2FeMnO4

Spinels (AB 2O4) with magnetic ions occupying only the octahedral B sites have inherent magnetic frustration which inhibits magnetic long-range order (LRO) but may lead to exotic states. Here we report on the magnetic properties of the tetragonal spinel Zn0.8Cu0.2FeMnO4, the tetragonality resulting from the Jahn–Teller active Mn3+ ions. X-ray diffraction and x-ray photoelectron spectroscopy of the sample yielded the composition () A [] B O4‒δ . Analysis of the temperature dependence of magnetization (M), ac magnetic susceptibilities (χ′ and χ′′), dc susceptibility (χ), heat capacity Cp , and neutron diffraction (ND) measurements show complex temperature-dependent short-range order (SRO) but without LRO. The data of χ vs. T fits the Curie–Weiss law: χ = C/(T ‒ θ) from T = 250 K to 400 K with θ ≃ 185 K signifying dominant ferromagnetic (FM) coupling with the FM exchange constant J/k B = 17 K, and C = 3.29 emu K mol‒1 Oe‒1 yielding an effective magnetic moment µ eff = 5.13 µ B resulting from the high-spin states of Cu2+ (A site) and Fe2+ (B site), while the B site trivalent ions Mn3+ and Fe3+ are in their low-spin states. The extrapolated saturation magnetization obtained from the M vs. H data at T = 2 K is explained using the spin arrangement (Cu2+↓) A [Fe2+↑, Fe3+↓, Mn3+↑] B leading to FM clusters interact antiferromagnetically at low temperatures. Temperature dependence of d(χT)/dT shows the onset of ferrimagnetism below ∼100 K and peaks near 47 K and 24 K. The relaxation time τ obtained from temperature and frequency dependence of χ″ when fit to the power law and Vogel–Fulcher laws confirm the cluster spin-glass (SG) state. The magnetic field dependence of the SG temperature follows the equation: with T SG (0) = 46.6 K, A = 8.6 × 10‒3 Oe‒0.593 and = 3.37. The temperature dependence of hysteresis loops yields coercivity HC ∼ 3.8 kOe at 2 K without exchange-bias, but HC decreases with increase in T becoming zero above 24 K, the T SG(H) for H = 800 Oe. Variations of Cp vs. T from 2 K to 200 K in H = 0 and H = 90 kOe do not show any peak characteristic of LRO. However, after correcting for the lattice contribution, a broad weak peak typically of SRO becomes evident centered around 40 K. For T < 9 K, Cp varies as T2 ; a typical signature of spin-liquids (SLs). Comparison of the ND measurements at 1.7 K and 79.4 K shows absence of LRO. Time dependence of thermo-remanent magnetization M TRM(t) studies below 9 K reveal weakening of the inter-cluster interaction with increase in temperature. A summary of these results is that in Zn0.8Cu0.2FeMnO4, ferromagnetic clusters interact antiferromagnetically without LRO but producing a cluster SG state at T SG(0) = 46.6 K, followed by SL behavior below 9 K.

Fluctuating magnetic droplets immersed in a sea of quantum spin liquid

The search of quantum spin liquid (QSL), an exotic magnetic state with strongly fluctuating and highly entangled spins down to zero temperature, is a main theme in current condensed matter physics. However, there is no smoking gun evidence for deconfined spinons in any QSL candidate so far. The disorders and competing exchange interactions may prevent the formation of an ideal QSL state on frustrated spin lattices. Here we report comprehensive and systematic measurements of the magnetic susceptibility, ultralow-temperature specific heat, muon spin relaxation (μSR), nuclear magnetic resonance (NMR), and thermal conductivity for NaYbSe2 single crystals, in which Yb3+ ions with effective spin-1/2 form a perfect triangular lattice. All these complementary techniques find no evidence of long-range magnetic order down to their respective base temperatures. Instead, specific heat, μSR, and NMR measurements suggest the coexistence of quasi-static and dynamic spins in NaYbSe2. The scattering from these quasi-static spins may cause the absence of magnetic thermal conductivity. Thus, we propose a scenario of fluctuating ferrimagnetic droplets immersed in a sea of QSL. This may be quite common on the way pursuing an ideal QSL, and provides a brand new platform to study how a QSL state survives impurities and coexists with other magnetically ordered states.

Point defects in two-dimensional RuCl3

Defects are crucial in determining a variety of material properties especially in low dimensions. In this work, we study point defects in monolayer \ensuremath{\alpha}-phase Ruthenium (III) chloride $(\ensuremath{\alpha}-\mathrm{Ru}{\mathrm{Cl}}_{3})$, a promising candidate to realize quantum spin liquid with nearly degenerate magnetic states. Our first-principles simulations reveal that Cl vacancies, Ru vacancies, and oxygen substitutional defects are the most energetically stable point defects. Besides, these point defects break the magnetic degeneracy: Cl vacancies and oxygen substitutional defects energetically favor the zigzag-antiferromagnetic configuration while Ru vacancies favor the ferromagnetic configuration, shedding light on understanding the observed magnetic structures and further defect engineering of magnetism in monolayer $\ensuremath{\alpha}-\mathrm{Ru}{\mathrm{Cl}}_{3}$. We further calculated their electronic structures and optical absorption spectra. The polarization symmetry of optical responses provides a convenient signature to identify the point defect types and long-range magnetic orders.

Low-temperature antiferromagnetic order in orthorhombic CePdAl3

We report the magnetization, ac susceptibility, and specific heat of optically float-zoned single crystals of ${\mathrm{CePdAl}}_{3}$. In comparison to the properties of polycrystalline ${\mathrm{CePdAl}}_{3}$ reported in the literature, which displays a tetragonal crystal structure and no long-range magnetic order, our single crystals exhibit an orthorhombic structure ($Cmcm$) and antiferromagnetic order below a N\'eel temperature ${T}_{1}=5.6$ K. The specific heat at zero field shows two anomalies, namely, a broad transition at ${T}_{1}=5.6$ K followed by a $\ensuremath{\lambda}$-anomaly at ${T}_{2}=5.4$ K. A conservative estimate of the Sommerfeld coefficient of the electronic specific heat, $\ensuremath{\gamma}=121\phantom{\rule{0.28em}{0ex}}\mathrm{mJ}\phantom{\rule{0.16em}{0ex}}{\mathrm{K}}^{\ensuremath{-}2}\phantom{\rule{0.16em}{0ex}}{\mathrm{mol}}^{\ensuremath{-}1}$, indicates a moderately enhanced heavy-fermion ground state. A twin microstructure evolves in the family of planes spanned by the basal plane lattice vectors ${\mathbf{a}}_{\mathrm{o}}$ and ${\mathbf{c}}_{\mathrm{o}}$ , with the magnetic hard axis ${\mathbf{b}}_{\mathrm{o}}$ common to all twins. The antiferromagnetic state is characterized by a strong a${}_{\mathrm{o}}$, c${}_{\mathrm{o}}$ easy-plane magnetic anisotropy where the a${}_{\mathrm{o}}$ direction is the easy axis in the easy plane. A spin-flop transition induced under magnetic field along the easy directions, results in complex magnetic phase diagrams. Taken together, our results reveal a high sensitivity of the magnetic and electronic properties of ${\mathrm{CePdAl}}_{3}$ to its structural modifications.

Room temperature colossal superparamagnetic order in aminoferrocene–graphene molecular magnets

Intensive studies are published for graphene-based molecular magnets due to their remarkable electric, thermal, and mechanical properties. However, to date, most of all produced molecular magnets are ligand based and subject to challenges regarding the stability of the ligand(s). The lack of long-range coupling limits high operating temperature and leads to a short-range magnetic order. Herein, we introduce an aminoferrocene-based graphene system with room temperature superparamagnetic behavior in the long-range magnetic order that exhibits colossal magnetocrystalline anisotropy of 8 × 105 and 3 × 107 J/m3 in aminoferrocene and graphene-based aminoferrocene, respectively. These values are comparable to and even two orders of magnitude larger than pure iron metal. Aminoferrocene [C10H11FeN]+ is synthesized by an electrophilic substitution reaction. It was then reacted with graphene oxide that was prepared by the modified Hammers method. The phase structure and functionalization of surface groups were characterized and confirmed by XRD, FT-IR, and Raman spectroscopy. To model the behavior of the aminoferrocene between two sheets of hydroxylated graphene, we have used density functional theory by placing the aminoferrocene molecule between two highly ordered hydroxylated sheets and allowing the structure to relax. The strong bowing of the isolated graphene sheets suggests that the charge transfer and resulting magnetization could be strongly influenced by pressure effects. In contrast to strategies based on ligands surface attachment, our present work that uses interlayer intercalated aminoferrocene opens routes for future molecular magnets as well as the design of qubit arrays and quantum systems.

Tunable coupling in magnetic thin film heterostructures with a magnetic phase transition

The magnetic properties of permalloy-based trilayers of the form Py0.8Cu0.2/Py0.4Cu0.6/Py/IrMn were studied as the spacer layer undergoes a paramagnetic to ferromagnetic phase transition. We find the coupling between the free Py0.8Cu0.2 layer and the exchange bias pinned Py to be strongly temperature-dependent: there is negligible coupling above the Curie temperature of the Py0.4Cu0.6 spacer layer, strong ferromagnetic coupling below that temperature, and a tunable coupling between these extremes. Polarized neutron reflectometry was used to measure the depth profile of the magnetic order in the system, allowing us to correlate the order parameter with the coupling strength. The thickness dependence shows that these are interface effects with an inverse relationship to thickness, and that there is a magnetic proximity effect that enhances the Curie temperature of the spacer layer with characteristic length scale of about 7 nm. As a demonstration of potential functionality of such a system, the structure is shown to spontaneously flip from the antiparallel to parallel magnetic configuration once the spacer layer has developed long-range magnetic order.

Quantum correction to the anomalous Hall effect in PtMnGe thin films

The role of quantum correction such as weak localization in anomalous Hall effects (AHEs) is an important issue. In this work, we have investigated the robust quantum correction to the AHE in magnetic PtMnGe (PMG) thin films of high crystalline quality. The PMG films have not shown long-range magnetic order. The observed temperature and magnetic field dependence of the sheet conductivities in the ultrathin PMG films are explained based on the perturbation theory, where the interplay of spin-dependent scattering and the spin Zeeman splitting effect are taken into consideration. It is found that, as long as the magnetic scattering time is comparable to the spin-orbit scattering time, the conductivity correction due to the Cooperons between antiparallel spins that involves spin-flip scattering can be negligible in the two dimensions. Therefore, even when the spin-dependent scattering exists, the quantum correction to the transport behavior is robust in the two-dimensional PMG system. Our work makes a significant step toward clarifying the role of quantum correction in the AHE of the magnetic materials.

Pressure-controlled magnetism in 2D molecular layers

Long-range magnetic ordering of two-dimensional crystals can be sensitive to interlayer coupling, enabling the effective control of interlayer magnetism towards voltage switching, spin filtering and transistor applications. With the discovery of two-dimensional atomically thin magnets, a good platform provides us to manipulate interlayer magnetism for the control of magnetic orders. However, a less-known family of two-dimensional magnets possesses a bottom-up assembled molecular lattice and metal-to-ligand intermolecular contacts, which lead to a combination of large magnetic anisotropy and spin-delocalization. Here, we report the pressure-controlled interlayer magnetic coupling of molecular layered compounds via chromium-pyrazine coordination. Room-temperature long-range magnetic ordering exhibits pressure tuning with a coercivity coefficient up to 4 kOe/GPa, while pressure-controlled interlayer magnetism also presents a strong dependence on alkali metal stoichiometry and composition. Two-dimensional molecular interlayers provide a pathway towards pressure-controlled peculiar magnetism through charge redistribution and structural transformation.

Crystal growth and magnetic properties of the coupled alternating S=1 spin chain Sr2Ni(SeO3)3

The structural, magnetic, and thermodynamic properties of a quasi-one-dimensional (1D) $S=1$ alternating spin chain compound ${\mathrm{Sr}}_{2}\mathrm{Ni}{(\mathrm{Se}{\mathrm{O}}_{3})}_{3}$ are investigated by using synchrotron x-ray powder diffraction, magnetic susceptibility $\ensuremath{\chi}(H,T)$, and heat capacity ${C}_{\mathrm{P}}(H,T)$ measurements together with density functional theory (DFT) calculations. The $\ensuremath{\chi}(H,T)$ and ${C}_{\mathrm{P}}(H,T)$ data reveal long-range antiferromagnetic order at ${T}_{\mathrm{N}}=3.4(3)$ K and short-range order at ${T}_{\mathrm{m}}\ensuremath{\approx}7.8\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. The short-range magnetic order together with 95% of spin entropy release above ${T}_{\mathrm{N}}$ signifies the importance of 1D spin correlations persisting to $\ensuremath{\sim}8{T}_{\mathrm{N}}$. Theoretical DFT calculations with generalized gradient approximation determine leading exchange interactions, suggesting that interchain interactions are responsible for the observed long-range magnetic ordering. In addition, the temperature-field phase diagram of ${\mathrm{Sr}}_{2}\mathrm{Ni}{(\mathrm{Se}{\mathrm{O}}_{3})}_{3}$ is determined based on the $\ensuremath{\chi}(T,H)$ and ${C}_{\mathrm{P}}(T,H)$ data. Interestingly, a nonmonotonic phase boundary of ${T}_{\mathrm{m}}$ is found for an external field applied along a hard axis. Our results suggest that the ground state and magnetic behavior of ${\mathrm{Sr}}_{2}\mathrm{Ni}{(\mathrm{Se}{\mathrm{O}}_{3})}_{3}$ rely on the interplay of single-ion anisotropy, bond alternation, and interchain interactions.

New Nabokoite-like Phases ACu7 TeO4 (SO4 )5 Cl (A=Na, K, Rb, Cs) with Decorated and Distorted Square Kagome Lattices.

A new family of compounds ACu7 TeO4 (SO4 )5 Cl (A=Na, K, Rb, Cs) isostructural to mineral Nabokoite (K species) was synthesized by solid state and gas transport reactions in sealed ampoules and characterized in measurements of magnetization and specific heat in a wide temperature range. These complex compounds are of the utmost interest as a testing playground to study the properties of quasi-two-dimensional magnets with a square kagome lattice geometry. A quantum ground state of such a corner-sharing network is a spin liquid. Unlike idealized grid analyzed in numerous models, the square kagome lattice in nabokoites is wavy and distorted being composed of versatile triangles. Moreover, it contains "excessive" decorating magnetic ions, which makes magnetism of these objects even more complicated. The interaction of these decorating ions through virtual excitations of the square kagome lattice is accompanied by the formation of a long-range magnetic order coexisting with the spin liquid.

Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS$GW$ and QS$G\hat{W}$, respectively). Comparing the quasi-particle band structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of $\approx$ 2.1 eV.