Showing 1–28 of 28 results for author: Manni, S

Probing the magnetic ground state and magnetoelastic coupling in double perovskite ruthenate: Ca2ScRuO6

Authors: Asha Ann Abraham, Anjali Kumari, Md Aktar Hossain, Sanjoy Kr Mahatha, Saikat Das, A. K. Bera, Soham Manni

Abstract: Ruthenates, materials with a single magnetic Ruthenium (Ru) atom, often display an exotic array of ground states ranging from superconductivity to altermagnetism. In this work, we investigated the magnetic ground state of a least explored member of the 4d3 double perovskite ruthenate series A2ScRuO6 (A = Ca, Sr, Ba): Ca2ScRuO6. Interestingly, temperature-dependent bulk susceptibility curve shows f… ▽ More Ruthenates, materials with a single magnetic Ruthenium (Ru) atom, often display an exotic array of ground states ranging from superconductivity to altermagnetism. In this work, we investigated the magnetic ground state of a least explored member of the 4d3 double perovskite ruthenate series A2ScRuO6 (A = Ca, Sr, Ba): Ca2ScRuO6. Interestingly, temperature-dependent bulk susceptibility curve shows ferrimagnetic-like behaviour above the magnetic ordering at around 40 K, which were corroborated by the identification of the mixed valence states, Ru5+ and Ru4+ via X-ray absorption spectroscopy. Structural analysis further revealed atomic-site exchange between the Ru and Sc sites, which results in the Ru mixed valence states. Neutron powder diffraction measurements detected the presence of magnetic Bragg peaks at a low temperature near 4 K and a moderate magnetoelastic coupling near the ordering temperature of 40 K. However, the corresponding symmetry analysis shows a weak Type I antiferromagnetic ground state with a reduced magnetic moment of 1.1μB/Ru atom. Our findings establish an unusual magnetic ground state in the Mott insulating Ca2ScRuO6, where a long range ordered antiferromagnet coexists with small magnetic clusters, which manifests a ferrimagnetic-like high temperature inverse magnetic susceptibility. This system presents a unique platform to study long-range magnetic order in the presence of antisite disorder. △ Less

Submitted 31 December, 2025; originally announced January 2026.

Comments: 11 pages, including appendix

Disorder mediated fully compensated ferrimagnetic spin-gapless semiconducting behaviour in Cr3Al Heusler alloy

Authors: Reshna Elsa Philip, Pooja Vyas, Nikhil Joseph Joy, Sandip Kumar Kuila, Sonia Beniwal, Akshata Magar, Dinesh Kumar Shukla, Partha Pratim Jana, Amit Kumar, Aftab Alam, Jayakumar Balakrishnan, Soham Manni

Abstract: Spin-gapless semiconductors (SGSs) that simultaneously host fully compensated ferrimagnetism are highly sought for energy-efficient and stray-field-free spintronic technologies, yet their realization in chemically disordered systems has remained elusive. Here, we demonstrate that the binary Heusler alloy Cr3Al despite adopting a fully A2-disordered structure exhibits a rare coexistence of SGS tran… ▽ More Spin-gapless semiconductors (SGSs) that simultaneously host fully compensated ferrimagnetism are highly sought for energy-efficient and stray-field-free spintronic technologies, yet their realization in chemically disordered systems has remained elusive. Here, we demonstrate that the binary Heusler alloy Cr3Al despite adopting a fully A2-disordered structure exhibits a rare coexistence of SGS transport and a fully compensated ferrimagnetic (FCF) ground state. Single-crystalline and polycrystalline Cr3Al samples were synthesized, and comprehensive structural analyses using single crystal XRD, synchrotron powder XRD, and neutron powder diffraction reveal complete Cr/Al site mixing. Remarkably, this chemical disorder does not disrupt magnetic order; instead, magnetization, X-ray magnetic circular dichroism (XMCD), and temperature-dependent neutron diffraction establish a robust compensated ferrimagnetic state with a vanishingly small ordered moment of 0.1(1) muB/f.u and a high Curie temperature of 773(2) K. Electrical and thermal transport measurements uncover clear SGS characteristics, including weak temperature-dependent conductivity, very low Seebeck coefficients, and electron-hole compensated transport. Hall measurements show unusual temperature-dependent carrier concentrations consistent with disorder-modified electronic states. First-principles calculations on an A2-disordered SQS structure reproduce the experimentally observed negligibly small magnetization (0.0072 muB/f.u) and reveal a vanishing spin-up band gap unambiguously supporting SGS behavior driven by chemical disorder. Our results identify Cr3Al as the first experimentally verified A2-disordered Heusler alloy exhibiting both fully compensated ferrimagnetism and spin-gapless semiconducting transport, positioning it as a robust and disorder-tolerant platform for next-generation, high-temperature spintronic devices. △ Less

Submitted 11 December, 2025; originally announced December 2025.

Comments: 18 Pages including SI

Cavity based sensing of antiferromagnetic canting and nonzero-momentum spin waves in a van der Waals cavity-magnon-polariton system

Authors: Supriya Mandal, Krishnendu Maji, Lucky N. Kapoor, Souvik Sasmal, Soham Manni, John Jesudasan, Pratap Raychaudhuri, Arumugam Thamizhavel, Mandar M. Deshmukh

Abstract: Cavity-magnon-polaritons are hybrid excitations from the interaction between cavity photons and magnons, the quanta of collective spin oscillations. Along with the tunability of the magnon-photon coupling strength, fast information transfer and conversion speed are desired in hybrid devices. This can be achieved utilizing the propagating nature of spin waves with non-zero momentum for their ultra-… ▽ More Cavity-magnon-polaritons are hybrid excitations from the interaction between cavity photons and magnons, the quanta of collective spin oscillations. Along with the tunability of the magnon-photon coupling strength, fast information transfer and conversion speed are desired in hybrid devices. This can be achieved utilizing the propagating nature of spin waves with non-zero momentum for their ultra-fast time dynamics and reduced ohmic dissipation. Antiferromagnets are particularly interesting as hosts for magnons since stray-field interactions are minimized, and they support multiple modes with distinctive magnetic-field behavior across the phase diagram. CrCl3 is a van der Waals antiferromagnet having a strong easy-plane anisotropy and a weak in-plane easy-axis anisotropy. Despite some magnetic resonance studies, the impact of magnetic reorientation of spins in CrCl3 on cavity-magnon-polariton interaction strength as a function of magnetic field remains largely unexplored. In this study, we investigate the coupling between magnons in CrCl3 and photons in a coplanar waveguide resonator as a function of magnetic field. In particular, we find that the magnon-photon coupling strength varies nonmonotonically and distinctly with the magnetic field for both acoustic and optical magnons, enabling tuning of the coupling strength with an external magnetic field as a knob. We find the signature of spin-flop transition in two harmonics of the cavity due to a stronger dispersive coupling between optical magnons and cavity photons at lower fields. Additionally, we find standing modes formed by spin waves with nonzero momentum associated with the two hybrid magnons when the external field is applied at an angle with the crystal plane. These modes do not undergo substantial coupling with the cavity mode unlike the antiferromagnetic modes and can be used as low-loss propagation channels in hybrid devices. △ Less

Submitted 4 December, 2025; originally announced December 2025.

Comments: 24 pages, 8 figures

Journal ref: Phys. Rev. B 112, 214443 (2025)

Electron doping in single crystalline BaBiO$_3$: BaBiO$_{3-x}$F$_{x}$

Authors: Sathishkumar M, Asha Ann Abrahama, Rajesh Kumar Sahu, Soma Banik, Soham Manni

Abstract: Topological insulators are a new class of insulators with conducting surface state. Most of the topological insulators are chalcogenides, where a tiny amount of chalcogen vacancy destroys the predicted bulk insulating state and results in a metallic or semimetallic bulk electrical transport. BaBiO$_3$ (BBO) is an interesting large bandgap (0.7 eV) insulator that upon hole doping becomes a supercon… ▽ More Topological insulators are a new class of insulators with conducting surface state. Most of the topological insulators are chalcogenides, where a tiny amount of chalcogen vacancy destroys the predicted bulk insulating state and results in a metallic or semimetallic bulk electrical transport. BaBiO$_3$ (BBO) is an interesting large bandgap (0.7 eV) insulator that upon hole doping becomes a superconductor and is theoretically predicted to show a topological insulating state under electron doping. We have explored electron doping through the chemical substitution of fluorine atoms at the oxygen site. The single crystals of BBO and fluorine doped BBO were synthesized via a one-step solid-state technique. The single crystals of pure BBO and 10 % F -doped BBO (BaBiO$_{2.7}$F$_{0.3}$) are chemically single-phase samples and crystallize in monoclinic I2/m crystal structure. The core level and valence band X-ray photoelectron spectra confirm electron doping in the 10% fluorine-doped BBO. 20 % F-doped BBO appears to be a multiphase sample, confirmed by back-scattered electron (BSE) imaging and X-ray diffraction. This article reports on the successful growth of pure and F-doped BBO using a one-step solid-state technique and discusses the effect of F-doping on structural and electronic properties. △ Less

Submitted 22 July, 2025; originally announced July 2025.

Comments: 5 pages, 5 figures, 2 tables

Investigation of competing magnetic orders and the associated spin-phonon coupling effect in quasi-2D Cr1+xTe2 (x = 0.22) single crystal

Authors: Gayathri V, Sathishkumar M, Sandip Kumar Kuila, Vikash Kumar, Abhidev B, Reshna Elsa Philip, Partha Pratim Jana, Soham Manni

Abstract: Single crystals of quasi-2D chromium telluride system represented by Cr1+xTe2 (x = 0.22), which crystallizes in the trigonal structure with the c-axis as the growth direction, are synthesized by the flux method. The magnetization measurements revealed the coexistence and competition between ferromagnetic and antiferromagnetic exchange interactions due to the presence of the intercalated Cr-layers.… ▽ More Single crystals of quasi-2D chromium telluride system represented by Cr1+xTe2 (x = 0.22), which crystallizes in the trigonal structure with the c-axis as the growth direction, are synthesized by the flux method. The magnetization measurements revealed the coexistence and competition between ferromagnetic and antiferromagnetic exchange interactions due to the presence of the intercalated Cr-layers. A series of diverse magnetic transitions is exhibited by the crystal. While cooling the crystal, it undergoes a paramagnetic to antiferromagnetic transition at 190 K, followed by a transition into a ferromagnetic state at around 160 K, and a spin-canting at a lower temperature of 75 K. A possible lack of inversion symmetry in the crystal structure, along with the observance of an unusual jump and loop opening in the isothermal magnetization suggests that the crystals Cr1+xTe2 (x = 0.22) may host skyrmions. Furthermore, concomitant to their magnetic transitions, anomalies were observed in the derived Breit-Wigner-Fano fit parameters obtained from the asymmetric temperature-dependent Raman spectra, evidencing a strong spin-phonon coupling effect, intrinsic to the grown crystals. A strong perpendicular magnetic anisotropy along with the robust spin-phonon coupling, makes the system a promising candidate for prospective spintronics applications. △ Less

Submitted 18 July, 2025; originally announced July 2025.

Comments: 5 pages + Supplimentary material

Electronic and magnetic ground state of 4$d^3$ double perovskite ruthenates A$_2$LaRuO$_6$ (A $=$ Ca, Sr, Ba)

Authors: Asha Ann Abraham, Roumita Roy, Ruta Kulkarni, Sudipta Kanungo, Soham Manni

Abstract: 4$d$ transition metal oxide (TMO) offers an intriguing puzzle for their electronic and magnetic ground state. They are in the cross-over regime of strong spin orbit interaction (SOI) and electron-electron correlation ($U$) with quenched orbital angular momentum. Our work unravels the electronic and magnetic ground state of the less investigated 4$d^{3}$ double perovskite ruthenates A$_{2}$LaRuO… ▽ More 4$d$ transition metal oxide (TMO) offers an intriguing puzzle for their electronic and magnetic ground state. They are in the cross-over regime of strong spin orbit interaction (SOI) and electron-electron correlation ($U$) with quenched orbital angular momentum. Our work unravels the electronic and magnetic ground state of the less investigated 4$d^{3}$ double perovskite ruthenates A$_{2}$LaRuO$_6$ (A = Ca, Ba). The negligible effect of SOI is evident from the bulk magnetic, specific heat measurements and density functional theory (DFT) calculations, indicating a classical spin-only magnetic ground state (${S}$ = 3/2) for the materials. Magnetization measurements show that both materials have long range antiferromagnetic order with high degree of magnetic frustration ($f$ $\approx$13 -15). Interestingly, a near $T^2$- behavior is observed in low-$T$ magnetic heat capacity measurement, indicating the presence of low-dimensional spin-wave exciation and magnetic frustration in both materials. The temperature dependent resistivity measurements and electronic band structure calculations confirm a conventional Mott insulating ground state in these two systems. Moreover, our experimental investigation and DFT calculations highlight the reason for the nonexistence of Sr$_2$LaRuO$_6$. △ Less

Submitted 13 June, 2024; originally announced June 2024.

Comments: 11 pages, 12 figures, 5 tables

Observation of superconductivity in the noncentrosymmetric nodal chain semimetal Ba5In4Bi5

Authors: Yuzhe Ma, Yulong Wang, Yuxin Wang, Soham Manni, Qisheng Lin, Linlin Wang, Kun Jiang, Sergey L. Bud'ko, Paul C. Canfield, Gang Wang

Abstract: The combination with superconductivity and topological nontrivial band structure provides a promising route towards novel quantum states such as topological superconductivity. Here, we report the first observation of superconductivity (4.1 K) in Ba5In4Bi5 single crystal, a noncentrosymmetric topological semimetal featuring nodal chain loops at the high-symmetry points R and X. The magnetization, r… ▽ More The combination with superconductivity and topological nontrivial band structure provides a promising route towards novel quantum states such as topological superconductivity. Here, we report the first observation of superconductivity (4.1 K) in Ba5In4Bi5 single crystal, a noncentrosymmetric topological semimetal featuring nodal chain loops at the high-symmetry points R and X. The magnetization, resistivity, and specific heat capacity measurements reveal that Ba5In4Bi5 is a moderately coupled type-II Bardeen-Cooper-Schrieffer superconductor. Bulk superconductivity is suggested from the magnetic susceptibility and specific heat measurements. The results show that Ba5In4Bi5 provides a new platform for exploring the relationship of superconductivity and topological nontrivial band topology. △ Less

Submitted 8 October, 2022; originally announced October 2022.

Effects of magnetic and non-magnetic doping on the vortex lattice in MgB$_2$

Authors: E. R. Louden, S. Manni, J. E. Van Zandt, A. W. D. Leishman, V. Taufour, S. L. Bud'ko, L. DeBeer-Schmitt, D. Honecker, C. D. Dewhurst, P. C. Canfield, M. R. Eskildsen

Abstract: Using small-angle neutron scattering we have studied the vortex lattice in superconducting MgB$_2$ with the magnetic field applied along the $c$-axis, doped with either manganese or carbon to achieve a similar suppression of the critical temperature. For Mn-doping, the vortex lattice phase diagram remains qualitatively similar to that of pure MgB$_2$, undergoing a field-and temperature-driven… ▽ More Using small-angle neutron scattering we have studied the vortex lattice in superconducting MgB$_2$ with the magnetic field applied along the $c$-axis, doped with either manganese or carbon to achieve a similar suppression of the critical temperature. For Mn-doping, the vortex lattice phase diagram remains qualitatively similar to that of pure MgB$_2$, undergoing a field-and temperature-driven $30^{\circ}$ rotation transition, indicating only a modest effect on the vortex-vortex interaction. In contrast, the vortex lattice rotation transition is completely suppressed in the C-doped case, likely due to a change in the electronic structure which affects the two-band/two-gap nature of superconductivity in MgB2. The vortex lattice longitudinal correlation length shows the opposite behavior, remaining roughly unchanged between pure and C-doped MgB$_2$ while it is significantly reduced in the Mn-doped case. However, the extensive vortex lattice metastability and related activated behavior, observed in conjunction with the vortex lattice transition in pure MgB$_2$, is also seen in the Mn doped sample. This shows that the vortex lattice disordering is not associated with a substantially increased vortex pinning. △ Less

Submitted 2 May, 2022; v1 submitted 21 February, 2022; originally announced February 2022.

Comments: To appear in the Journal of Applied Crystallography for the special issue "Magnetic Small-Angle Neutron Scattering - from nanoscale magnetism to long-range magnetic structures"

Journal ref: J. Appl. Cryst. 55, 693 (2022)

Coplanar cavity for strong coupling between photons and magnons in van der Waals antiferromagnet

Authors: Supriya Mandal, Lucky N. Kapoor, Sanat Ghosh, John Jesudasan, Soham Manni, A. Thamizhavel, Pratap Raychaudhuri, Vibhor Singh, Mandar M. Deshmukh

Abstract: We investigate the performance of niobium nitride superconducting coplanar waveguide resonators towards hybrid quantum devices with magnon-photon coupling. We find internal quality factors ~ 20000 at 20 mK base temperature, in zero magnetic field. We find that by reducing film thickness below 100 nm internal quality factor greater than 1000 can be maintained up to parallel magnetic field of ~ 1 T… ▽ More We investigate the performance of niobium nitride superconducting coplanar waveguide resonators towards hybrid quantum devices with magnon-photon coupling. We find internal quality factors ~ 20000 at 20 mK base temperature, in zero magnetic field. We find that by reducing film thickness below 100 nm internal quality factor greater than 1000 can be maintained up to parallel magnetic field of ~ 1 T and perpendicular magnetic field of ~ 100 mT. We further demonstrate strong coupling of microwave photons in these resonators, with magnons in chromium trichloride, a van der Waals antiferromagnet, which shows that these cavities serve as a good platform for studying magnon-photon coupling in 2D magnonics based hybrid quantum systems. We demonstrate strong magnon-photon coupling for both optical and acoustic magnon modes of an antiferromagnet. △ Less

Submitted 20 January, 2021; v1 submitted 1 February, 2020; originally announced February 2020.

Comments: 15 pages, 14 figures

Journal ref: Appl. Phys. Lett. 117, 263101 (2020)

Evidence of standing spin-waves in a van der Waals magnetic material

Authors: Lucky N. Kapoor, Supriya Mandal, Meghan Patankar, Soham Manni, A. Thamizhavel, Mandar M. Deshmukh

Abstract: Spin-waves have been studied for data storage, communication and logic circuits in the field of spintronics based on their potential to substitute electrons. Recent discovery of magnetism in two-dimensional (2D) systems such as monolayer CrI$_3$ and Cr$_2$Ge$_2$Te$_6$ has led to a renewed interest in such applications of magnetism in the 2D limit. Here we present direct evidence of standing spin-w… ▽ More Spin-waves have been studied for data storage, communication and logic circuits in the field of spintronics based on their potential to substitute electrons. Recent discovery of magnetism in two-dimensional (2D) systems such as monolayer CrI$_3$ and Cr$_2$Ge$_2$Te$_6$ has led to a renewed interest in such applications of magnetism in the 2D limit. Here we present direct evidence of standing spin-waves along with the uniform precessional resonance modes in van der Waals magnetic material, CrCl$_3$. Our experiment is the first direct observation of standing spin-wave modes, set up across a thickness of 20 $μ$m, in a van der Waals material. We detect standing spin-waves in the vicinity of both, optical and acoustic, branches of the antiferromagnetic resonance. We also observe magnon-magnon coupling, softening of resonance modes with temperature and extract the evolution of interlayer exchange field as a function of temperature. △ Less

Submitted 16 January, 2020; originally announced January 2020.

Comments: 11 pages, 10 figures

Beyond freezing: amorphous water in biomimetic soft nanoconfinement

Authors: Livia Salvati Manni, Salvatore Assenza, Michael Duss, Jijo J. Vallooran, Fanni Juranyi, Simon Jurt, Oliver Zerbe, Ehud M. Landau, Raffaele Mezzenga

Abstract: Water is a ubiquitous liquid with unique physico-chemical properties, whose nature has shaped our planet and life as we know it. Water in restricted geometries has different properties than in bulk. Confinement can prevent low-temperature crystallization into a hexagonal structure, thus creating a state of amorphous water. In this work we introduce a family of synthetic lipids with designed cyclop… ▽ More Water is a ubiquitous liquid with unique physico-chemical properties, whose nature has shaped our planet and life as we know it. Water in restricted geometries has different properties than in bulk. Confinement can prevent low-temperature crystallization into a hexagonal structure, thus creating a state of amorphous water. In this work we introduce a family of synthetic lipids with designed cyclopropyl modification in the hydrophobic chains that exhibit unique liquid-crystalline behaviour at low temperature, enabling maintenance of amorphous water down to 10 K due to nanoconfinement in a bio-mimetic milieu. Small and Wide Angle X-ray Scattering, Elastic and Inelastic Neutron Scattering, Nuclear Magnetic Resonance Spectroscopy and Differential Scanning Calorimetry, complemented by Molecular Dynamics Simulations, unveil a complex lipid/water phase diagram, in which bicontinuous cubic and lamellar liquid crystalline phases containing sub-zero liquid, glassy, or ice water emerge as a competition between the two components, each pushing towards its thermodynamically favoured state. △ Less

Submitted 16 October, 2018; originally announced October 2018.

Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet $α$-Li$_2$IrO$_3$

Authors: Sungkyun Choi, S. Manni, J. Singleton, C. V. Topping, T. Lancaster, S. J. Blundell, D. T. Adroja, V. Zapf, P. Gegenwart, R. Coldea

Abstract: The layered honeycomb iridate $α$-Li$_2$IrO$_3$ displays an incommensurate magnetic structure with counterrotating moments on nearest-neighbor sites, proposed to be stabilized by strongly-frustrated anisotropic Kitaev interactions between spin-orbit entangled Ir$^{4+}$ magnetic moments. Here we report powder inelastic neutron scattering measurements that observe sharply dispersive low-energy magne… ▽ More The layered honeycomb iridate $α$-Li$_2$IrO$_3$ displays an incommensurate magnetic structure with counterrotating moments on nearest-neighbor sites, proposed to be stabilized by strongly-frustrated anisotropic Kitaev interactions between spin-orbit entangled Ir$^{4+}$ magnetic moments. Here we report powder inelastic neutron scattering measurements that observe sharply dispersive low-energy magnetic excitations centered at the magnetic ordering wavevector, attributed to Goldstone excitations of the incommensurate order, as well as an additional intense mode above a gap $Δ\simeq2.3$ meV. Zero-field muon-spin relaxation measurements show clear oscillations in the muon polarization below the Néel temperature $T_{\rm N}\simeq15$ K with a time-dependent profile consistent with bulk incommensurate long-range magnetism. Pulsed field magnetization measurements observe that only about half the saturation magnetization value is reached at the maximum field of 64 T. A clear anomaly near 25 T indicates a transition to a phase with reduced susceptibility. The transition field has a Zeeman energy comparable to the zero-field gapped mode, suggesting gap suppression as a possible mechanism for the field-induced transition. △ Less

Submitted 7 October, 2018; originally announced October 2018.

Comments: 8 pages, 6 figures

Journal ref: Phys. Rev. B 99, 054426 (2019)

Effect of pressure on the physical properties of the superconductor NiBi3

Authors: Elena Gati, Li Xiang, Lin-Lin Wang, Soham Manni, Paul C. Canfield, Sergey L. Bud'ko

Abstract: We present an experimental study of the superconducting properties of NiBi3 as a function of pressure by means of resistivity and magnetization measurements and combine our results with DFT calculations of the band structure under pressure. We find a moderate suppression of the critical temperature Tc from ~ 4.1K to ~ 3K by pressures up to 2GPa. By taking into account the change of the band struct… ▽ More We present an experimental study of the superconducting properties of NiBi3 as a function of pressure by means of resistivity and magnetization measurements and combine our results with DFT calculations of the band structure under pressure. We find a moderate suppression of the critical temperature Tc from ~ 4.1K to ~ 3K by pressures up to 2GPa. By taking into account the change of the band structure as a function of pressure, we argue that the decrease in Tc is consistent with conventional, electron-phonon-mediated BCS-type superconductivity. △ Less

Submitted 13 December, 2018; v1 submitted 20 September, 2018; originally announced September 2018.

Journal ref: J. Phys.: Condens. Matter 31 035701 (2019)

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling

Authors: Dahlia R. Klein, David MacNeill, Jose L. Lado, David Soriano, Efrén Navarro-Moratalla, Kenji Watanabe, Takashi Taniguchi, Soham Manni, Paul Canfield, Joaquín Fernández-Rossier, Pablo Jarillo-Herrero

Abstract: Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic… ▽ More Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%, 300%, and 550% for bilayer, trilayer, and tetralayer CrI3 barriers, respectively. We further measure inelastic tunneling spectra for our junctions, unveiling a rich spectrum of collective magnetic excitations (magnons) in CrI3. Our results establish vertical tunneling as a versatile probe of magnetism in atomically thin insulators. △ Less

Submitted 26 January, 2018; originally announced January 2018.

Journal ref: Science 360, 1218-1222 (2018)

Extremely large magnetoresistance and Kohler's rule in PdSn4: a complete study of thermodynamic, transport and band structure properties

Authors: Na Hyun Jo, Yun Wu, Lin-Lin Wang, Peter P. Orth, Savannah S. Downing, Soham Manni, Dixiang Mou, Duane D. Johnson, Adam Kaminski, Sergey L. Bud'ko, Paul C. Canfield

Abstract: The recently discovered material PtSn$_4$ is known to exhibit extremely large magnetoresistance (XMR) that also manifests Dirac arc nodes on the surface. PdSn$_4$ is isostructure to PtSn$_4$ with same electron count. We report on the physical properties of high quality single crystals of PdSn$_4$ including specific heat, temperature and magnetic field dependent resistivity and magnetization, and e… ▽ More The recently discovered material PtSn$_4$ is known to exhibit extremely large magnetoresistance (XMR) that also manifests Dirac arc nodes on the surface. PdSn$_4$ is isostructure to PtSn$_4$ with same electron count. We report on the physical properties of high quality single crystals of PdSn$_4$ including specific heat, temperature and magnetic field dependent resistivity and magnetization, and electronic band structure properties obtained from angle resolved photoemission spectroscopy (ARPES). We observe that PdSn$_4$ has physical properties that are qualitatively similar to those of PtSn$_4$, but find also pronounced differences. Importantly, the Dirac arc node surface state of PtSn$_4$ is gapped out for PdSn$_4$. By comparing these similar compounds, we address the origin of the extremely large magnetoresistance in PdSn$_4$ and PtSn$_4$; based on detailed analysis of the magnetoresistivity, $ρ(H,T)$, we conclude that neither carrier compensation nor the Dirac arc node surface state are primary reason for the extremely large magnetoresistance. On the other hand, we find that surprisingly Kohler's rule scaling of the mangnetoresistance, which describes a self-similarity of the field induced orbital electronic motion across different length scales and is derived for a simple electronic response of metals to applied in a magnetic field is obeyed over the full range of temperatures and field strengths that we explore. △ Less

Submitted 31 October, 2017; v1 submitted 18 July, 2017; originally announced July 2017.

Journal ref: Phys. Rev. B 96, 165145 (2017)

Growth and characterization of BaZnGa

Authors: Na Hyun Jo, Qisheng Lin, Manh Cuong Nguyen, Udhara S. Kaluarachchi, Wiliam R. Meier, Soham Manni, Savannah S. Downing, Anna E. Böhmer, Tai Kong, Yang Sun, Valentin Taufour, Cai-Zhuang Wang, Kai-Ming Ho, Sergey L. Bud'ko, Paul C. Canfield

Abstract: We report the growth, structure and characterization of BaZnGa, identifying it as the sole known ternary compound in the Ba-Zn-Ga system. Single crystals of BaZnGa can be grown out of excess Ba-Zn and adopt a tI36 structure type. There are three unique Ba sites and three M\,=\,Zn/Ga sites. Using DFT calculations we can argue that whereas one of these three M sites is probably solely occupied by Ga… ▽ More We report the growth, structure and characterization of BaZnGa, identifying it as the sole known ternary compound in the Ba-Zn-Ga system. Single crystals of BaZnGa can be grown out of excess Ba-Zn and adopt a tI36 structure type. There are three unique Ba sites and three M\,=\,Zn/Ga sites. Using DFT calculations we can argue that whereas one of these three M sites is probably solely occupied by Ga, the other two M sites, most likely, have mixed Zn/Ga occupancy. Temperature dependent resistivity and magnetization measurements suggest that BaZnGa is a poor metal with no electronic or magnetic phase transitions between 2\,K and 300\,K. △ Less

Submitted 11 July, 2017; v1 submitted 29 June, 2017; originally announced June 2017.

Journal ref: Philos. Mag. 97 (2017) 3317-3324

GdPtPb: A non collinear antiferromagnet with distorted Kagomé lattice

Authors: S. Manni, Sergey L. Bud'ko, Paul C. Canfield

Abstract: In the spirit of searching for Gd-based, frustrated, rare earth magnets, we have found antiferomagnetism (AF) in GdPtPb which crystallizes in the ZrNiAl-type structure that has a distorted Kagomé lattice of Gd-triangles. Single crystals were grown and investigated using structural, magnetic, transport and thermodynamic measurements. GdPtPb orders antiferromagnetically at 15.5 K arguably with a pla… ▽ More In the spirit of searching for Gd-based, frustrated, rare earth magnets, we have found antiferomagnetism (AF) in GdPtPb which crystallizes in the ZrNiAl-type structure that has a distorted Kagomé lattice of Gd-triangles. Single crystals were grown and investigated using structural, magnetic, transport and thermodynamic measurements. GdPtPb orders antiferromagnetically at 15.5 K arguably with a planar, non-collinear structure. The high temperature magnetic susceptibility data reveal an "anti-frustration" behavior having a frustration parameter, $|f|$ = $|Θ|$/ $T_N$ = 0.25, which can be explained by mean field theory (MFT) within a two sub-lattice model. Study of the magnetic phase diagram down to $T$ = 1.8 K reveals a change of magnetic structure through a metamagnetic transition at around 20 kOe and the disappearance of the AF ordering near 140 kOe. In total, our work indicates that, GdPtPb can serve as an example of a planar, non collinear, AF with a distorted Kagomé magnetic sub-lattice. △ Less

Submitted 1 June, 2017; originally announced June 2017.

Comments: 8 Pages, 9 figures

Journal ref: Phys. Rev. B 96, 054435 (2017)

BaSn$_2$: A new, wide-gap, strong topological insulator

Authors: Steve M Young, S. Manni, Junping Shao, Paul C. Canfield, Aleksey N. Kolmogorov

Abstract: BaSn$_2$ has been shown to form as layers of buckled stanene intercalated by barium ions~\cite{Kim_2008}. However, despite an apparently straightforward synthesis and significant interest in stanene as a topological material, BaSn$_2$ has been left largely unexplored, and has only recently been recognized as a potential topological insulator. Belonging to neither the lead nor bismuth chalcogenide… ▽ More BaSn$_2$ has been shown to form as layers of buckled stanene intercalated by barium ions~\cite{Kim_2008}. However, despite an apparently straightforward synthesis and significant interest in stanene as a topological material, BaSn$_2$ has been left largely unexplored, and has only recently been recognized as a potential topological insulator. Belonging to neither the lead nor bismuth chalcogenide families, it would represent a unique manifestation of the topological insulating phase. Here we present a detailed investigation of BaSn$_2$, using both {\it ab initio} and experimental methods. First-principles calculations demonstrate that this overlooked material is a indeed strong topological insulator with a bulk band gap of 360meV, among the largest observed for topological insulators. We characterize the surface state dependence on termination chemistry, providing guidance for experimental efforts to measure and manipulate its topological properties. Additionally, through {\it ab initio} modeling and synthesis experiments we explore the stability and accessibility of this phase, revealing a complicated phase diagram that indicates a challenging path to obtaining single crystals. △ Less

Submitted 21 September, 2016; v1 submitted 18 July, 2016; originally announced July 2016.

Journal ref: Phys. Rev. B 95, 085116 (2017)

Incommensurate Counterrotating Magnetic Order Stabilized by Kitaev Interactions in the Layered Honeycomb $α$-Li$_2$IrO$_3$

Authors: S. C. Williams, R. D. Johnson, F. Freund, Sungkyun Choi, A. Jesche, I. Kimchi, S. Manni, A. Bombardi, P. Manuel, P. Gegenwart, R. Coldea

Abstract: The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate ma… ▽ More The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counter-rotating on nearest-neighbour sites. This type of magnetic structure has not been reported experimentally before in honeycomb magnets and cannot be explained by a spin Hamiltonian with dominant isotropic (Heisenberg) couplings. The magnetic structure shares many key features with the magnetic order in the structural polytypes $β$ and $γ$-Li$_2$IrO$_3$, understood theoretically to be stabilized by dominant Kitaev interactions between Ir moments located on the vertices of three-dimensional hyperhoneycomb and stripyhoneycomb lattices, respectively. Based on this analogy and a theoretical soft-spin analysis of magnetic ground states for candidate spin Hamiltonians, we propose that Kitaev interactions also dominate in $α$-Li$_2$IrO$_3$, indicative of universal Kitaev physics across all three members of the harmonic honeycomb family of Li$_2$IrO$_3$ polytypes. △ Less

Submitted 25 February, 2016; originally announced February 2016.

Comments: 13 pages, 8 figures

Journal ref: Phys. Rev. B 93, 195158 (2016)

Isotope Effect on Electron-Phonon Interaction in Multiband Superconductor MgB2

Authors: Daixiang Mou, Soham Manni, Valentin Taufour, Yun Wu, Lunan Huang, S. L. Bud'ko, P. C. Canfield, Adam Kaminski

Abstract: We investigate the effect of isotope substitution on the electron-phonon interaction in the multi-band superconductor MgB2 using tunable laser based Angle Resolved Photoemission Spectroscopy. The kink structure around 70 meV in the $σ$ band, which is caused by electron coupling to the E2g phonon mode, is shifted to higher binding energy by ~3.5 meV in Mg(10)B2 and the shift is not affected by supe… ▽ More We investigate the effect of isotope substitution on the electron-phonon interaction in the multi-band superconductor MgB2 using tunable laser based Angle Resolved Photoemission Spectroscopy. The kink structure around 70 meV in the $σ$ band, which is caused by electron coupling to the E2g phonon mode, is shifted to higher binding energy by ~3.5 meV in Mg(10)B2 and the shift is not affected by superconducting transition. These results serve as the benchmark for investigations of isotope effects in known, unconventional superconductors and newly discovered superconductors where the origin of pairing is unknown. △ Less

Submitted 9 February, 2016; originally announced February 2016.

Comments: 5 pages, 4 figures

Journal ref: Phys. Rev. B 93, 144504 (2016)

Local Magnetism and Spin Dynamics of the Frustrated Honeycomb Rhodate Li2RhO3

Authors: P. Khuntia, S. Manni, F. R. Foronda, T. Lancaster, S. J. Blundell, P. Gegenwart, M. Baenitz

Abstract: We report magnetization, heat capacity, 7Li - nuclear magnetic resonance (NMR), and muSR (muon spin roration) measurements on the honeycomb 4d5 spin liquid candidate Li2RhO3. The magnetization in small magnetic fields provides evidence of the partial spin-freezing of a small fraction of Rh4+ -moments at 6 K, whereas the Curie-Weiss behavior above 100 K suggests a pseudo-spin-1/2 paramagnet with a… ▽ More We report magnetization, heat capacity, 7Li - nuclear magnetic resonance (NMR), and muSR (muon spin roration) measurements on the honeycomb 4d5 spin liquid candidate Li2RhO3. The magnetization in small magnetic fields provides evidence of the partial spin-freezing of a small fraction of Rh4+ -moments at 6 K, whereas the Curie-Weiss behavior above 100 K suggests a pseudo-spin-1/2 paramagnet with a moment of about 2.2 muB. The magnetic specific heat (Cm) exhibits no field dependence and demonstrates the absence of long range magnetic order down to 0.35 K. Cm/T passes through a broad maximum at about 10 K and Cm=T^2 at low temperatures. Measurements of the spin-lattice relaxation rate (1/T1) reveal a gapless slowing down of spin fluctuations upon cooling with 1/T1=T^2.2. The results from NMR and muSR are consistent with a scenario in which a minority of Rh4+ moments are in a ahort-range correlated frozen state and coexist with a majority of moments in a liquid-like state that continue to fluctuate at low temperatures. △ Less

Submitted 26 September, 2017; v1 submitted 15 December, 2015; originally announced December 2015.

Journal ref: Phys. Rev. B 96, 094432 (2017)

Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in $β$-Li2IrO3: full solution via magnetic resonant x-ray diffraction

Authors: A. Biffin, R. D. Johnson, Sungkyun Choi, F. Freund, S. Manni, A. Bombardi, P. Manuel, P. Gegenwart, R. Coldea

Abstract: The recently-synthesized iridate $β$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic s… ▽ More The recently-synthesized iridate $β$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic structure. We find a complex, incommensurate magnetic order with non-coplanar and counter-rotating Ir moments, which surprisingly shares many of its features with the related structural polytype "stripyhoneycomb" $γ$-Li$_2$IrO$_3$, where dominant Kitaev interactions have been invoked to explain the stability of the observed magnetic structure. The similarities of behavior between those two structural polytypes, which have different global lattice topologies but the same local connectivity, is strongly suggestive that the same magnetic interactions and the same underlying mechanism governs the stability of the magnetic order in both materials, indicating that both $β$- and $γ$-Li$_2$IrO$_3$ are strong candidates to realize dominant Kitaev interactions in a solid state material. △ Less

Submitted 1 August, 2014; originally announced August 2014.

Comments: 14 pages, 9 figures

Journal ref: Phys. Rev. B. 90, 205116 (2014)

Investigation of unconventional reconstruction and electronic properties on the Na2IrO3 surface

Authors: F. Lupke, S. Manni, S. C. Erwin, I. I. Mazin, P. Gegenwart, M. Wenderoth

Abstract: Na2IrO3 is an intriguing material for which spin-orbit coupling plays a key role. Theoretical predictions, so far unverified, have been made that the surface of Na2IrO3 should exhibit a clear signature of the quantum spin Hall effect. We studied the surface of Na2IrO3 using scanning tunneling microscopy and density-functional theory calculations. We observed atomic level resolution of the surface… ▽ More Na2IrO3 is an intriguing material for which spin-orbit coupling plays a key role. Theoretical predictions, so far unverified, have been made that the surface of Na2IrO3 should exhibit a clear signature of the quantum spin Hall effect. We studied the surface of Na2IrO3 using scanning tunneling microscopy and density-functional theory calculations. We observed atomic level resolution of the surface and two types of terminations with different surface periodicity and Na content. By comparing bias-dependent experimental topographic images to simulated images, we determined the detailed atomistic structure of both observed surfaces. One of these reveals a strong relaxation to the surface of Na atoms from the subsurface region two atomic layers below. Such dramatic structural changes at the surface cast doubt on any prediction of surface properties based on bulk electronic structure. Indeed, using spatially resolved tunneling spectroscopy we found no indication of the predicted quantum spin Hall behavior. △ Less

Submitted 17 July, 2014; originally announced July 2014.

Journal ref: Phys. Rev. B 91 (2015) 041405(R)

Effect of nonmagnetic dilution in honeycomb lattice iridates Na$_2$IrO$_3$ and Li$_2$IrO$_3$

Authors: S. Manni, Y. Tokiwa, P. Gegenwart

Abstract: We have synthesized single crystals of Na$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and polycrystals of Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and studied the effect of magnetic depletion on the magnetic properties by measurements of the magnetic susceptibility, specific heat and magnetocaloric effect at temperatures down to 0.1~K. In both systems, the non-magnetic substitution rapidly changes the magnetically ordered gr… ▽ More We have synthesized single crystals of Na$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and polycrystals of Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and studied the effect of magnetic depletion on the magnetic properties by measurements of the magnetic susceptibility, specific heat and magnetocaloric effect at temperatures down to 0.1~K. In both systems, the non-magnetic substitution rapidly changes the magnetically ordered ground state into a spin glass, indicating strong frustration. While for the Li system the Weiss temperature $Θ_{\rm W}$ remains unchanged up to $x=0.55$, a strong decrease $|Θ_{\rm W}|$ is found for the Na system. This suggests that only for the former system magnetic exchange beyond nearest neighbors is dominating. This is also corroborated by the observation of a smeared quantum phase transition in Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ near $x=0.5$, i.e. much beyond the site percolation threshold of the honeycomb lattice. △ Less

Submitted 3 June, 2014; v1 submitted 16 April, 2014; originally announced April 2014.

Comments: 8 pages including supplemental, 12 figures

Journal ref: Phys. Rev. B 89, 241102(R) (2014)

Effect of isoelectronic doping on honeycomb lattice iridate A_2IrO_3

Authors: S. Manni, Sungkyun Choi, I. I. Mazin, R. Coldea, Michaela Altmeyer, Harald O. Jeschke, Roser Valenti, P. Gegenwart

Abstract: We have investigated experimentally and theoretically the series (Na$_{1-x}$Li$_{x}$)$_{2}$IrO$_{3}$. Contrary to what has been believed so far, only for $x\leq0.25$ the system forms uniform solid solutions. For larger Li content, as evidenced by powder X-ray diffraction, scanning electron microscopy and density functional theory calculations, the system shows a miscibility gap and a phase separat… ▽ More We have investigated experimentally and theoretically the series (Na$_{1-x}$Li$_{x}$)$_{2}$IrO$_{3}$. Contrary to what has been believed so far, only for $x\leq0.25$ the system forms uniform solid solutions. For larger Li content, as evidenced by powder X-ray diffraction, scanning electron microscopy and density functional theory calculations, the system shows a miscibility gap and a phase separation into an ordered Na$_{3}$LiIr$_2$O$_{6}$ phase with alternating Na$_3$ and LiIr$_2$O$_6$ planes, and a Li-rich phase close to pure Li$_{2}$IrO$_{3}$. For $x\leq 0.25$ we observe (1) an increase of $c/a$ with Li doping up to $x=0.25$, despite the fact that $c/a$ in pure Li$_{2}$IrO$_{3}$ is smaller than in Na$_{2}$IrO$_{3}$, and (2) a gradual reduction of the antiferromagnetic ordering temperature $T_{N}$ and ordered moment. The previously proposed magnetic quantum phase transition at $x\approx 0.7$ may occur in a multiphase region and its nature needs to be re-evaluated. △ Less

Submitted 15 June, 2014; v1 submitted 3 December, 2013; originally announced December 2013.

Comments: 8 pages, 9 figures including supplemental information

Journal ref: Phys. Rev. B 89, 245113 (2014)

Origin of the insulating state in honeycomb iridates and rhodates

Authors: I. I. Mazin, S. Manni, K. Foyevtsova, Harald O. Jeschke, P. Gegenwart, Roser Valenti

Abstract: A burning question in the emerging field of spin-orbit driven insulating iridates, such as Na2IrO3 and Li2IrO3 is whether the observed insulating state should be classified as a Mott-Hubbard insulator derived from a half-filled relativistic j_eff=1/2 band or as a band insulator where the gap is assisted by spin-orbit interaction, or Coulomb correlations, or both. The difference between these two i… ▽ More A burning question in the emerging field of spin-orbit driven insulating iridates, such as Na2IrO3 and Li2IrO3 is whether the observed insulating state should be classified as a Mott-Hubbard insulator derived from a half-filled relativistic j_eff=1/2 band or as a band insulator where the gap is assisted by spin-orbit interaction, or Coulomb correlations, or both. The difference between these two interpretations is that only for the former, strong spin-orbit coupling (lambda >~ W, where W is the band width) is essential. We have synthesized the isostructural and isoelectronic Li2RhO3 and report its electrical resistivity and magnetic susceptibility. Remarkably it shows insulating behavior together with fluctuating effective S=1/2 moments, similar to Na2IrO3 and Li2IrO3, although in Rh4+ (4d5) the spin-orbit coupling is greatly reduced. We show that this behavior has non-relativistic one-electron origin (although Coulomb correlations assist in opening the gap), and can be traced down to formation of quasi-molecular orbitals, similar to those in Na2IrO3. △ Less

Submitted 30 January, 2014; v1 submitted 8 April, 2013; originally announced April 2013.

Comments: 7 pages, 7 figures

Journal ref: Phys. Rev. B 88, 035115 (2013)

Crystal field splitting and correlation effect on the electronic structure of A2IrO3

Authors: H. Gretarsson, J. P. Clancy, X. Liu, J. P. Hill, Emil Bozin, Yogesh Singh, S. Manni, P. Gegenwart, Jungho Kim, A. H. Said, D. Casa, T. Gog, M. H. Upton, Heung-Sik Kim, J. Yu, Vamshi M. Katukuri, L. Hozoi, Jeroen van den Brink, Young-June Kim

Abstract: The electronic structure of the honeycomb lattice iridates Na2IrO3 and Li2IrO3 has been investigated using resonant inelastic x-ray scattering (RIXS). Crystal-field split d-d excitations are resolved in the high-resolution RIXS spectra. In particular, the splitting due to non-cubic crystal fields, derived from the splitting of j_eff=3/2 states, is much smaller than the typical spin-orbit energy sc… ▽ More The electronic structure of the honeycomb lattice iridates Na2IrO3 and Li2IrO3 has been investigated using resonant inelastic x-ray scattering (RIXS). Crystal-field split d-d excitations are resolved in the high-resolution RIXS spectra. In particular, the splitting due to non-cubic crystal fields, derived from the splitting of j_eff=3/2 states, is much smaller than the typical spin-orbit energy scale in iridates, validating the applicability of j_eff physics in A2IrO3. We also find excitonic enhancement of the particle-hole excitation gap around 0.4 eV, indicating that the nearest-neighbor Coulomb interaction could be large. These findings suggest that both Na2IrO3 and Li2IrO3 can be described as spin-orbit Mott insulators, similar to the square lattice iridate Sr2IrO4. △ Less

Submitted 24 September, 2012; originally announced September 2012.

Journal ref: Physical Review Letters 110, 076402 (2013)

Relevance of the Heisenberg-Kitaev model for the honeycomb lattice iridates A_2IrO_3

Authors: Yogesh Singh, S. Manni, J. Reuther, T. Berlijn, R. Thomale, W. Ku, S. Trebst, P. Gegenwart

Abstract: Combining thermodynamic measurements with theoretical density functional and thermodynamic calculations we demonstrate that the honeycomb lattice iridates A2IrO3 (A = Na, Li) are magnetically ordered Mott insulators where the magnetism of the effective spin-orbital S = 1/2 moments can be captured by a Heisenberg-Kitaev (HK) model with Heisenberg interactions beyond nearest-neighbor exchange. Exper… ▽ More Combining thermodynamic measurements with theoretical density functional and thermodynamic calculations we demonstrate that the honeycomb lattice iridates A2IrO3 (A = Na, Li) are magnetically ordered Mott insulators where the magnetism of the effective spin-orbital S = 1/2 moments can be captured by a Heisenberg-Kitaev (HK) model with Heisenberg interactions beyond nearest-neighbor exchange. Experimentally, we observe an increase of the Curie-Weiss temperature from θ= -125 K for Na2IrO3 to θ= -33 K for Li2IrO3, while the antiferromagnetic ordering temperature remains roughly the same T_N = 15 K for both materials. Using finite-temperature functional renormalization group calculations we show that this evolution of θ, T_N, the frustration parameter f = θ/T_N, and the zig-zag magnetic ordering structure suggested for both materials by density functional theory can be captured within this extended HK model. Combining our experimental and theoretical results, we estimate that Na2IrO3 is deep in the magnetically ordered regime of the HK model (α\approx 0.25), while Li2IrO3 appears to be close to a spin-liquid regime (0.6 < α< 0.7). △ Less

Submitted 2 February, 2012; v1 submitted 2 June, 2011; originally announced June 2011.

Comments: Version accepted for publication in PRL. Additional DFT and thermodynamic calculations have been included. 6 pages of supplementary material included

Journal ref: Phys. Rev. Lett. 108, 127203 (2012)