Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2.

The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties such as valence, spin, and orbital degrees of freedom as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultra-high conductivity, non-magnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce emergence of a net moment on the surrounding transition metal octahedral sites. These highly-localized moments communicate through the itinerant metal states which triggers the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultra-high conductivity film and will be critical to applications across spintronics.

[1]  D. Schlom,et al.  Growth of PdCoO2 films with controlled termination by molecular-beam epitaxy and determination of their electronic structure by angle-resolved photoemission spectroscopy , 2022, APL Materials.

[2]  T. Harada,et al.  Metallic delafossite thin films for unique device applications , 2022, APL Materials.

[3]  Yiting Liu,et al.  Anomalous Hall effect in electrolytically reduced PdCoO2 thin films , 2022, Thin Solid Films.

[4]  T. Ward,et al.  The structural modification and magnetism of many-layer epitaxial graphene implanted with low-energy light ions , 2022, Carbon.

[5]  Timur K. Kim,et al.  Tuneable electron–magnon coupling of ferromagnetic surface states in PdCoO2 , 2021, npj Quantum Materials.

[6]  O. Heinonen,et al.  A combined first principles study of the structural, magnetic, and phonon properties of monolayer CrI3. , 2021, The Journal of chemical physics.

[7]  W. Chueh,et al.  Layer-resolved many-electron interactions in delafossite PdCoO2 from standing-wave photoemission spectroscopy , 2021, Communications Physics.

[8]  M. Arnold,et al.  Epitaxy, exfoliation, and strain-induced magnetism in rippled Heusler membranes , 2021, Nature Communications.

[9]  L. Feldman,et al.  Effective reduction of PdCoO2 thin films via hydrogenation and sign tunable anomalous Hall effect , 2021, Physical Review Materials.

[10]  A. Barnard,et al.  Directional ballistic transport in the two-dimensional metal PdCoO2 , 2021, Nature Physics.

[11]  A. Herklotz,et al.  PHYSICAL REVIEW B 103, 085121 (2021) Post-synthesis control of Berry phase driven magnetotransport in SrRuO3 films , 2021 .

[12]  Y. Tokura,et al.  Giant anomalous Hall effect from spin-chirality scattering in a chiral magnet , 2020, Nature communications.

[13]  F. Giustino,et al.  The 2021 quantum materials roadmap , 2020, Journal of Physics: Materials.

[14]  B. Diény,et al.  Review on spintronics: Principles and device applications , 2020, Journal of Magnetism and Magnetic Materials.

[15]  Stephen D. Wilson,et al.  Giant, unconventional anomalous Hall effect in the metallic frustrated magnet candidate, KV3Sb5 , 2020, Science Advances.

[16]  A. Tsukazaki,et al.  Control of Schottky barrier height in metal/β-Ga2O3 junctions by insertion of PdCoO2 layers , 2020 .

[17]  Edgar Josué Landinez Borda,et al.  QMCPACK: Advances in the development, efficiency, and application of auxiliary field and real-space variational and diffusion quantum Monte Carlo. , 2020, The Journal of chemical physics.

[18]  Kevin M. Roccapriore,et al.  Pulsed-laser epitaxy of metallic delafossite PdCrO2 films , 2020, APL Materials.

[19]  C. Melton,et al.  Many-body electronic structure of LaScO3 by real-space quantum Monte Carlo , 2020, 2001.04359.

[20]  D. Schlom,et al.  Growth of CuFeO2 single crystals by the optical floating-zone technique , 2019, Journal of Crystal Growth.

[21]  D. Ralph,et al.  Probing and controlling magnetic states in 2D layered magnetic materials , 2019, Nature Reviews Physics.

[22]  Z. Liao,et al.  Metal-insulator transition in (111) SrRuO3 ultrathin films , 2019, APL Materials.

[23]  M. Kitamura,et al.  Anomalous Hall effect at the spontaneously electron-doped polar surface of PdCoO2 ultrathin films , 2019, Physical Review Research.

[24]  D. Ralph,et al.  Local Photothermal Control of Phase Transitions for On‐Demand Room‐Temperature Rewritable Magnetic Patterning , 2019, Advanced materials.

[25]  R. Unocic,et al.  Growth of metallic delafossite PdCoO2 by molecular beam epitaxy , 2019, Physical Review Materials.

[26]  R. Cabeza,et al.  Present and Future , 2008 .

[27]  A. Fontcuberta i Morral,et al.  Rational strain engineering in delafossite oxides for highly efficient hydrogen evolution catalysis in acidic media , 2019, Nature Catalysis.

[28]  D. Muller,et al.  Controlled Introduction of Defects to Delafossite Metals by Electron Irradiation , 2019, Physical Review X.

[29]  Ying Wai Li,et al.  QMCPACK: an open source ab initio quantum Monte Carlo package for the electronic structure of atoms, molecules and solids , 2018, Journal of physics. Condensed matter : an Institute of Physics journal.

[30]  Timur K. Kim,et al.  Itinerant ferromagnetism of the Pd-terminated polar surface of PdCoO2 , 2017, Proceedings of the National Academy of Sciences.

[31]  A. Mackenzie The properties of ultrapure delafossite metals , 2016, Reports on progress in physics. Physical Society.

[32]  D. Ralph,et al.  Interface-Induced Phenomena in Magnetism. , 2016, Reviews of modern physics.

[33]  H. N. Lee,et al.  Controlling Octahedral Rotations in a Perovskite via Strain Doping , 2016, Scientific Reports.

[34]  B. Schmidt,et al.  Evidence for hydrodynamic electron flow in PdCoO2 , 2015, Science.

[35]  E. Dagotto,et al.  Strain Doping: Reversible Single-Axis Control of a Complex Oxide Lattice via Helium Implantation. , 2015, Physical review letters.

[36]  Hideo Ohno,et al.  Control of magnetism by electric fields. , 2015, Nature nanotechnology.

[37]  S. May,et al.  Magnetic Oxide Heterostructures , 2014 .

[38]  G. Galli,et al.  Self-consistent hybrid functional for condensed systems , 2014, 1501.03184.

[39]  R. Hübner,et al.  Printing nearly-discrete magnetic patterns using chemical disorder induced ferromagnetism. , 2014, Nano letters.

[40]  Y. Maeno,et al.  Extremely large magnetoresistance in the nonmagnetic metal PdCoO2. , 2013, Physical review letters.

[41]  Roman Engel-Herbert,et al.  Highly Conductive SrVO3 as a Bottom Electrode for Functional Perovskite Oxides , 2013, Advanced materials.

[42]  Shinill Kang,et al.  Nanoscale patterning of complex magnetic nanostructures by reduction with low-energy protons. , 2012, Nature nanotechnology.

[43]  A. Suter,et al.  Musrfit: A Free Platform-Independent Framework for μSR Data Analysis , 2011, 1111.1569.

[44]  H. Ohno,et al.  A perpendicular-anisotropy CoFeB-MgO magnetic tunnel junction. , 2010, Nature materials.

[45]  K. P. Ong,et al.  Origin of anisotropy and metallic behavior in delafossite PdCoO 2 , 2010 .

[46]  B. Min,et al.  Anisotropic electric conductivity of delafossite PdCoO2 studied by angle-resolved photoemission spectroscopy. , 2009, Physical review letters.

[47]  Stefano de Gironcoli,et al.  QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[48]  J. Sinova,et al.  Anomalous hall effect , 2009, 0904.4154.

[49]  M. Beasley,et al.  Critical thickness for itinerant ferromagnetism in ultrathin films of SrRuO3 , 2008, 0811.0384.

[50]  Konrad Deiters,et al.  The new μE4 beam at PSI: A hybrid-type large acceptance channel for the generation of a high intensity surface-muon beam , 2008 .

[51]  J. Fassbender,et al.  Magnetic patterning by means of ion irradiation and implantation , 2008 .

[52]  L. Tjeng,et al.  Valence, spin, and orbital state of Co ions in one-dimensional Ca3Co2O6 : An x-ray absorption and magnetic circular dichroism study , 2006, cond-mat/0611545.

[53]  A Tanaka,et al.  Spin state transition in LaCoO3 studied using soft x-ray absorption spectroscopy and magnetic circular dichroism. , 2006, Physical review letters.

[54]  M. Casula Beyond the locality approximation in the standard diffusion Monte Carlo method , 2006, cond-mat/0610246.

[55]  M. Toney,et al.  Neutron scattering studies of nanomagnetism and artificially structured materials , 2004 .

[56]  E. M. Forgan,et al.  Implantation studies of keV positive muons in thin metallic layers , 2002 .

[57]  T. Prokscha,et al.  Low-energy μSR at PSI: present and future , 2000 .

[58]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[59]  H. Dreyssé,et al.  Onset of magnetism in palladium slabs , 1990 .

[60]  R. N. West,et al.  Positron annihilation and Fermi surface studies: a new approach , 1973 .

[61]  J. Crangle,et al.  Dilute Ferromagnetic Alloys , 1965 .

[62]  John B. Goodenough,et al.  An interpretation of the magnetic properties of the perovskite-type mixed crystals La1-xSrxCoO3-λ , 1958 .

[63]  C. Melton,et al.  Electronic structure of α − RuCl 3 by fixed-node and fixed-phase diffusion Monte Carlo methods , 2022 .

[64]  J. Walter,et al.  Magnetism in Palladium Experimental Results in View of Theoretic Predictions , 2002 .

[65]  R. Needs,et al.  Quantum Monte Carlo simulations of solids , 2001 .

[66]  Wolfgang Eckstein,et al.  Computer simulation of ion-solid interactions , 1991 .

[67]  H. Redkey,et al.  A new approach. , 1967, Rehabilitation record.

[68]  N. V. Bazhanova,et al.  On the Hall Effect in Ferromagnetics , 1958 .