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Register a new userBand engineering of a magnetic thin film rare earth monopnictide
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Realizing quantum materials in few atomic layer morphologies is a key to both observing and controlling a wide variety of exotic quantum phenomena. This includes topological electronic materials, where the tunability and dimensionality of few layer materials have enabled the detection of $Z_2$, Chern, and Majorana phases. Here, we report the development of a platform for thin film correlated, topological states in the magnetic rare-earth monopnictide ($RX$) system GdBi synthesized by molecular beam epitaxy. This material is known from bulk single crystal studies to be semimetallic antiferromagnets with Neel temperature $T_N =$ 28 K and is the magnetic analog of the non-$f$-electron containing system LaBi proposed to have topological surface states. Our transport and magnetization studies of thin films grown epitaxially on BaF$_2$ reveal that semimetallicity is lifted below approximately 8 crystallographic unit cells while magnetic order is maintained down to our minimum thickness of 5 crystallographic unit cells. First-principles calculations show that the non-trivial topology is preserved down to the monolayer limit, where quantum confinement and the lattice symmetry give rise to a $C=2$ Chern insulator phase. We further demonstrate the stabilization of these films against atmospheric degradation using a combination of air-free buffer and capping procedures. These results together identify thin film $RX$ materials as potential platforms for engineering topological electronic bands in correlated magnetic materials.
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The rare-earth monopnictide family is attracting an intense current interest driven by its unusual extreme magnetoresistance (XMR) property and the potential presence of topologically non-trivial surface states. The experimental observation of non-trivial surface states in this family of materials are not ubiquitous. Here, using high-resolution angle-resolved photoemission spectroscopy (ARPES), magnetotransport, and parallel first-principles modeling, we examine the nature of electronic states in HoSb. Although we find the presence of bulk band gaps at the G and X-symmetry points of the Brillouin zone (BZ), we do not find these gaps to exhibit band inversion so that HoSb does not host a Dirac semimetal state. Our magnetotransport measurements indicate that HoSb can be characterized as a correlated nearly-complete electron-hole-compensated semimetal. Our analysis reveals that the nearly perfect electron-hole compensation could drive the appearance of non-saturating XMR effect in HoSb.
Alkali metal rare-earth chalcogenide $ARECh2$ (A=alkali or monovalent metal, RE=rare earth, Ch=O, S, Se, Te), is a large family of quantum spin liquid (QSL) candidates we discovered recently. Unlike $YbMgGaO4$, most members in the family except for the oxide ones, have relatively small crystalline electric-field (CEF) excitation levels, particularly the first ones. This makes the conventional Curie-Weiss analysis at finite temperatures inapplicable and CEF excitations may play an essential role in understanding the low-energy spin physics. Here we considered an effective magnetic Hamiltonian incorporating CEF excitations and spin-spin interactions, to accurately describe thermodynamics in such a system. By taking $NaYbSe2$ as an example, we were able to analyze magnetic susceptibility, magnetization under pulsed high fields and heat capacity in a systematic and comprehensive way. The analysis allows us to produce accurate anisotropic exchange coupling energies and unambiguously determine a crossover temperature ($sim$25 K in the case of $NaYbSe2$), below which CEF effects fade away and pure spin-spin interactions stand out. We further validated the effective picture by successfully explaining the anomalous temperature dependence of electron spin resonance (ESR) spectral width. The effective scenario in principle can be generalized to other rare-earth spin systems with small CEF excitations.
Multiferroic rare earth manganites attracted recent attention because of the coexistence of different types of magnetic and ferroelectric orders resulting in complex phase diagrams and a wealth of physical phenomena. The coupling and mutual interference of the different orders and the large magnetoelectric effect observed in several compounds are of fundamental interest and bear the potential for future applications in which the dielectric (magnetic) properties can be modified by the onset of a magnetic (dielectric) transition or the application of a magnetic (electric) field. The physical mechanisms of the magnetoelectric effect and the origin of ferroelectric order at magnetic transitions have yet to be explored. We discuss multiferroic phenomena in the hexagonal HoMnO3 and show that the strong magneto-dielectric coupling is intimately related to the lattice strain induced by unusually large spin-phonon correlations.
We studied the electronic band structure of pulsed laser deposition (PLD) grown (111)-oriented SrRuO$_3$ (SRO) thin films using textit{in situ} angle-resolved photoemission spectroscopy (ARPES) technique. We observed previously unreported, light bands with a renormalized quasiparticle effective mass of about 0.8$m_{e}$. The electron-phonon coupling underlying this mass renormalization yields a characteristic kink in the band dispersion. The self-energy analysis using the Einstein model suggests five optical phonon modes covering an energy range 44 to 90 meV contribute to the coupling. Besides, we show that the quasiparticle spectral intensity at the Fermi level is considerably suppressed, and two prominent peaks appear in the valance band spectrum at binding energies of 0.8 eV and 1.4 eV, respectively. We discuss the possible implications of these observations. Overall, our work demonstrates that high-quality thin films of oxides with large spin-orbit coupling can be grown along the polar (111) orientation by the PLD technique, enabling textit{in situ} electronic band structure study. This could allow for characterizing the thickness-dependent evolution of band structure of (111) heterostructures$-$a prerequisite for exploring possible topological quantum states in the bilayer limit.
Frustrated quantum magnets are expected to host many exotic quantum spin states like quantum spin liquid (QSL), and have attracted numerous interest in modern condensed matter physics. The discovery of the triangular lattice spin liquid candidate YbMgGaO$_4$ stimulated an increasing attention on the rare-earth-based frustrated magnets with strong spin-orbit coupling. Here we report the synthesis and characterization of a large family of rare-earth chalcogenides AReCh$_2$ (A = alkali or monovalent ions, Re = rare earth, Ch = O, S, Se). The family compounds share the same structure (R$bar{3}$m) as YbMgGaO$_4$, and antiferromagnetically coupled rare-earth ions form perfect triangular layers that are well separated along the $c$-axis. Specific heat and magnetic susceptibility measurements on NaYbO$_2$, NaYbS$_2$ and NaYbSe$_2$ single crystals and polycrystals, reveal no structural or magnetic transition down to 50mK. The family, having the simplest structure and chemical formula among the known QSL candidates, removes the issue on possible exchange disorders in YbMgGaO$_4$. More excitingly, the rich diversity of the family members allows tunable charge gaps, variable exchange coupling, and many other advantages. This makes the family an ideal platform for fundamental research of QSLs and its promising applications.
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