Spin-orbit coupling and dimensionality at the heart of quantum magnetism of heavy transition metal oxides
Lead Research Organisation:
Science and Technology Facilities Council
Department Name: ISIS Pulsed Neutron & Muon Source
Abstract
This proposal is focused on the study of quantum materials with competing interactions. Measurements of the various quantum-mechanical phases provide the most direct manifestation of the underlying abstract physics, such as quantum spin liquid, topological behaviour and quantum entanglement. The in-depth experimental and theoretical investigations of emergent phenomena of the candidate quantum materials have been serving as a major theme of recent condensed matter physics research. Understanding the complex magnetic interactions in these novel quantum materials is crucial for the development of fundamental science in the form of modern theory of higher d transition metal oxides, as well as for the strong foundation of alternative pathways towards the design of new and exotic materials and functional devices, which hold true promise for future generation of technological applications. The investigations on the novel 5d Iridates and 4d rhodates reveal a burgeoning list of theoretical proposals as well as predictions of unusual states, such as Jeff half Mott-insulating state, the quantum spin liquid phase, Kitaev quantum magnetism, unconventional superconductivity, Weyl semimetals, correlated topological insulators, etc., which are indeed truly remarkable and stimulating. The physics of iridates, ruthenates and rhodates clearly warrants serious intellectual challenges both theoretically and experimentally, and hence, in this proposal we focus on design, synthesis and characterisation of the new candidate quantum materials within 4d Rh/Ru- and 5d Ir-based oxides. Quantum spin liquid (QSL) is a novel state of quantum magnetism where long range magnetic order is suppressed due to strong quantum fluctuations down to the lowest temperature. The gapless QSLs exhibit long-range quantum-entanglement and fractionalised spin excitations named as Majorana Fermions. Such fractionalised spin excitations are different from conventional magnons observed in compounds with long-range magnetic ordering. The present proposal is therefore aimed to investigate the exotic and unconventional magnetic ground states of iridates, ruthenates and rhodates within a variety of crystal structures and lattice geometries by implementing detailed experimental study (both laboratory based and state-of-art neutron, muon and x-ray synchrotron based advanced measurements) and ab-initio electronic structure calculations. These in-depth investigations will help in understanding the importance of various competing interactions, e.g. spin-orbit interaction, on-site Coulomb U, crystal field, Hund's coupling, hopping and electronic bandwidth. The nature of the extraordinary structural sensitivity of quantum materials also calls for extraordinarily high-quality single crystals and we are planning to synthesise such single crystals using UCL crystal growth lab at Harwell and investigate them using various central facilities.
Organisations
- Science and Technology Facilities Council (Lead Research Organisation)
- Max Planck Society (Collaboration)
- University of Warwick (Collaboration)
- Tohoku University (Collaboration)
- Institut Laue–Langevin (Collaboration)
- University of Johannesburg (Project Partner)
- University of Warwick (Project Partner)
Publications
Adroja D
(2024)
Magnetic and Magnetoelectric Materials
in Magnetochemistry
Amorese A
(2022)
Metamagnetism and crystal-field splitting in pseudohexagonal CeRh 3 Si 2
in Physical Review B
Anand V
(2022)
Thermal conductivity, thermoelectric power and Mössbauer investigations on atiferromagnetic CeFe1.7Ir0.3Al10
in Journal of Magnetism and Magnetic Materials
Anand V
(2023)
Time-reversal symmetry breaking and s - wave superconductivity in CaPd 2 Ge 2 : A µ SR study
in Physical Review B
Anand V
(2023)
Role of crystal-field ground state in the classical spin-liquid behavior of the quasi-one-dimensional spin-chain system Sr 3 NiPtO 6
in Physical Review B
Anand V
(2023)
Magnetic structure and crystal field states of Pr 2 Pd 3 Ge 5 : µ SR and neutron scattering investigations
in Physical Review B
Bhattacharyya A
(2022)
Nodeless time-reversal symmetry breaking in the centrosymmetric superconductor Sc 5 Co 4 Si 10 probed by muon-spin spectroscopy
in Physical Review Materials
Bhattacharyya A
(2023)
µSR Study of Unconventional Pairing Symmetry in the Quasi-1D Na2Cr3As3 Superconductor
in Magnetochemistry
Bhattacharyya A
(2023)
Superconducting Gap Structure of Filled Skutterudite LaOs4As12 Compound through µSR Investigations
in Magnetochemistry
Bhattacharyya A
(2024)
Exploring superconductivity in Ba3Ir4Ge16: Experimental and theoretical insights
in Journal of Alloys and Compounds
Description | We have identified new quantum spin-liquid (QSL) material based on heavy transition metal using muon spin rotation and relaxation measurements. In this material magnetic frustration plays important role, which enhances quantum fluctuations and prevents a long-range magnetic ordering of the strongly correlated spins down to lowest temperature. Investigations of materials hosting QSL ground states are of immense importance in the context of understanding the mechanism of high-temperature superconductivity, as well as for possible applications in data storage, memory devices, and future generation quantum computation. |
Exploitation Route | Investigations of materials hosting QSL ground states are of immense importance in the context of understanding the mechanism of high-temperature superconductivity, as well as for possible applications in data storage, memory devices, and future generation quantum computation. |
Sectors | Chemicals Digital/Communication/Information Technologies (including Software) Education |
URL | https://arxiv.org/pdf/2403.06446.pdf |
Title | CCDC 2221970: Experimental Crystal Structure Determination |
Description | Related Article: Marta Roman, Maria Fritthum, Berthold Stöger, Devashibhai T. Adroja, Herwig Michor|2023|Physical Review B: covering condensed matter and materials physics|107||doi:10.1103/PhysRevB.107.125137 |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
URL | http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2dl4gm&sid=DataCite |
Title | CCDC 2221971: Experimental Crystal Structure Determination |
Description | Related Article: Marta Roman, Maria Fritthum, Berthold Stöger, Devashibhai T. Adroja, Herwig Michor|2023|Physical Review B: covering condensed matter and materials physics|107||doi:10.1103/PhysRevB.107.125137 |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
URL | http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2dl4hn&sid=DataCite |
Title | CCDC 2221972: Experimental Crystal Structure Determination |
Description | Related Article: Marta Roman, Maria Fritthum, Berthold Stöger, Devashibhai T. Adroja, Herwig Michor|2023|Physical Review B: covering condensed matter and materials physics|107||doi:10.1103/PhysRevB.107.125137 |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
URL | http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2dl4jp&sid=DataCite |
Title | Strain control of a bandwidth-driven spin reorientation in Ca3Ru2O7 |
Description | Here, we provide data for the manuscript "Strain control of a bandwidth-driven spin reorientation in Ca3Ru2O7" by C. D. Dashwood, A. H. Walker, M. P. Kwasigroch, L. S. I. Veiga, Q. Faure, J. G. Vale, D. G. Porter, P. Manuel, D. D. Khalyavin, F. Orlandi, C. V. Colin, O. Fabelo, F. Kruger, R. S. Perry, R. D. Johnson, A. G. Green, and D. F. McMorrow. |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
URL | https://springernature.figshare.com/articles/dataset/Strain_control_of_a_bandwidth-driven_spin_reori... |
Title | Strain control of a bandwidth-driven spin reorientation in Ca3Ru2O7 |
Description | Here, we provide data for the manuscript "Strain control of a bandwidth-driven spin reorientation in Ca3Ru2O7" by C. D. Dashwood, A. H. Walker, M. P. Kwasigroch, L. S. I. Veiga, Q. Faure, J. G. Vale, D. G. Porter, P. Manuel, D. D. Khalyavin, F. Orlandi, C. V. Colin, O. Fabelo, F. Kruger, R. S. Perry, R. D. Johnson, A. G. Green, and D. F. McMorrow. |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
URL | https://springernature.figshare.com/articles/dataset/Strain_control_of_a_bandwidth-driven_spin_reori... |
Description | Hard X-ray Photoelectron Spectroscopy (HAXPES) and X-ray absorption (XAS) investigations on transition metal oxides |
Organisation | Max Planck Society |
Department | Max Planck Institute for Chemical Physics of Solids |
Country | Germany |
Sector | Academic/University |
PI Contribution | Our research team prepared the samples in collaboration with Korean group. We performed the bulk characterisation and muon spin rotation measurements. My team was leading the writing the research paper, which has been submitted for publication to Phys. Rev. B. |
Collaborator Contribution | Dr Takegami Daisuke works in our partner group lead by Prof. Liu Hao Tjeng Director Max Planck Institute for Chemical Physics of Solids, Nöthnitzerstr. 40, 01187, Dresden Germany. Dr Daisuke performed HAXPES measurements on Ba4NbRu3O12 and also carried out DFT calculation. Dr Z. Hu also works in Prof. Liu Hao Tjeng groups and he carried our X-ray absorption study on on Ba4NbRu3O12. |
Impact | Novel quantum spin liquid ground state in the trimer rhodate Ba4NbRh3O12 Abhisek Bandyopadhyay, S. Lee, D. T. Adroja, G. B. G. Stenning, Adam Berlie, M. R. Lees, R. A. Saha, D. Takegami, A. Melendez-Sans, G. Poelchen, M. Yoshimura, K. D. Tsuei, Z. Hu, Cheng-Wei Kao, Yu-Cheng Huang, Ting-Shan Chan, Kwang-Yong Cho https://arxiv.org/abs/2403.06446 (2024) |
Start Year | 2023 |
Description | Muon spin rotation study on Iridates La3Ir3O11 |
Organisation | Tohoku University |
Country | Japan |
Sector | Academic/University |
PI Contribution | I have started collaboration with Prof. AOYAMA on investigating role of spin-orbital coupling in iridates. He has provided La3Ir3O11 materials and we will submit muon spin rotation and neutron scattering proposals at ISIS Facility, ILL, J-PARC and PSI. His details are given below. Prof. Takuya AOYAMA Department of Physics, Tohoku University 6-3 Aramaki-Aoba, Aobaku, Sendai, Miyagi 980-8578, JAPAN Phone:+81-22-795-6488, Mail:aoyama@tohoku.ac.jp |
Collaborator Contribution | Provided samples. |
Impact | At present we are planning for beam time proposals, which will results in future publications. |
Start Year | 2022 |
Description | Neutron diffraction study of transition metal oxides |
Organisation | Institut Laue–Langevin |
Department | Instutut Laue-Langevin Neutron Scattering Facility (France) |
Country | France |
Sector | Academic/University |
PI Contribution | The projects were started by Prof. Devashi Adroja and Dr Shivani Sharma from ISIS Facility. The papers were written in collaboration with Dr Ritter Clemens. |
Collaborator Contribution | Dr Ritter Clemens from ILL provided leadership role in performing neutron diffraction experiments at ILL, trained Dr Dr Shivani Sharma on data analysis and involved in writing the research papers. (1) Magnetic structure of the double perovskite La2NiIrO6 investigated using neutron diffraction Shivani Sharma , C. Ritter, D. T. Adroja , G. B. Stenning, A. Sundaresan, and S. Langridge PHYSICAL REVIEW MATERIALS 6, 014407 (2022) (2) Magnetic structures of the iridium-based double perovskites Pr2NiIrO6 and Nd2NiIrO6 reinvestigated using neutron diffraction C. Ritter, S. Sharma, and D. T. Adroja PHYSICAL REVIEW MATERIALS 6, 084405 (2022) |
Impact | (1) Magnetic structure of the double perovskite La2NiIrO6 investigated using neutron diffraction Shivani Sharma , C. Ritter, D. T. Adroja , G. B. Stenning, A. Sundaresan, and S. Langridge PHYSICAL REVIEW MATERIALS 6, 014407 (2022) (2) Magnetic structures of the iridium-based double perovskites Pr2NiIrO6 and Nd2NiIrO6 reinvestigated using neutron diffraction C. Ritter, S. Sharma, and D. T. Adroja PHYSICAL REVIEW MATERIALS 6, 084405 (2022) |
Start Year | 2019 |
Description | Single crystal and polycrystalline synthesis of transition metal oxides |
Organisation | Max Planck Society |
Department | Max Planck Institute for Solid State Research |
Country | Germany |
Sector | Academic/University |
PI Contribution | Dr Masahiko Isobe from Max Planck Institute for Solid State Research, Heisenberg Strasse 1, D-70569 Stuttgart, Germany and Dr Arvind Yogi from UGC-DAE Consortium for Scientific Research, University Campus, Khandwa Road, Indore (M.P.) have provided transition metal oxides samples, Ba4NbRu3O12, Ba4TaT3O12 (T=Ir and Ru), ZnCoV2O7, CaCoP2O7 and ZnCoP2O7 for our EPSRC project. We have obtained muon spin rotation and relaxation beam time at FLAME instrument, PSI on ZnCoP2O7 and neutron diffraction at ILL on CaCoP2O7 . Beam time proposals for other materials will be submitted at ISIS Facility, ILL, J-PARC. |
Collaborator Contribution | Leading muon and neutron proposals at PSI, ILL and ISIS Facility. Experiments will be carried out by our group, data will be analysed and papers will be written. |
Impact | Beam time allocated at PSI on FLAME instrument to investigate ZnCoP2O7 using muon spin rotation and relaxation. Beam time allocated at ILL on D20 diffractometer to investigate magnetic structure of CaCoP2O7. |
Start Year | 2023 |
Description | transport magnetic measurements on transition metal oxides |
Organisation | University of Warwick |
Country | United Kingdom |
Sector | Academic/University |
PI Contribution | I and my team were leading the project on transition metal oxides and performed muon spin rotation and relaxation experiments and analysis of the data. We also performed mK heat capacity and magnetic measurements and analysis of these data. Finally the paper was written by my research team and myself. |
Collaborator Contribution | Prof. Martin Lees from Department of Physics, University of Warwick, Coventry CV4 7AL, United Kingdom is performing transport and magnetic measurements on our transition metal oxides based materials. He is also performing SEM-EDX measurements to characterized the composition of the materials. |
Impact | Novel quantum spin liquid ground state in the trimer rhodate Ba4NbRh3O12 Abhisek Bandyopadhyay, S. Lee, D. T. Adroja, G. B. G. Stenning, Adam Berlie, M. R. Lees, R. A. Saha, D. Takegami, A. Melendez-Sans, G. Poelchen, M. Yoshimura, K. D. Tsuei, Z. Hu, Cheng-Wei Kao, Yu-Cheng Huang, Ting-Shan Chan, Kwang-Yong Cho https://arxiv.org/pdf/2403.06446.pdf |
Start Year | 2022 |