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

Matthew Brahlek; Alessandro R. Mazza; Abdulgani Annaberdiyev; Michael Chilcote; Gaurab Rimal; Gábor B. Halász; Anh Pham; Yun Yi Pai; Jaron T. Krogel; Jason Lapano; Benjamin J. Lawrie; Gyula Eres; Jessica McChesney; Thomas Prokscha; Andreas Suter; Seongshik Oh; John W. Freeland; Yue Cao; Jason S. Gardner; Zaher Salman; Robert G. Moore; Panchapakesan Ganesh; T. Zac Ward

doi:10.1021/acs.nanolett.3c01065

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

Matthew Brahlek, Alessandro R. Mazza, Abdulgani Annaberdiyev, Michael Chilcote, Gaurab Rimal, Gábor B. Halász, Anh Pham, Yun Yi Pai, Jaron T. Krogel, Jason Lapano, Benjamin J. Lawrie, Gyula Eres, Jessica McChesney, Thomas Prokscha, Andreas Suter, Seongshik Oh, John W. Freeland, Yue Cao, Jason S. Gardner, Zaher SalmanRobert G. Moore, Panchapakesan Ganesh, T. Zac Ward

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

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 can be 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 ultrahigh-conductivity, nonmagnetic layered oxide PdCoO₂ where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

Original language	English
Pages (from-to)	7279-7287
Number of pages	9
Journal	Nano Letters
Volume	23
Issue number	16
DOIs	https://doi.org/10.1021/acs.nanolett.3c01065
State	Published - Aug 23 2023

Funding

Processing, electronic characterization and manuscript were supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Spectroscopy was supported by the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Quantum Science Center. Part of the theory work (quantum Monte Carlo and density functional theory using Quantum ESPRESSO) has been supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. Initial theory screening (density functional theory using VASP) that formed the basis of current theory-work was supported by the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. Part of this research (quantum Monte Carlo) used resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC05-00OR22725. Part of this research (quantum Monte Carlo) used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC02-06CH11357. Part of this research (density functional theory) used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. The use of the Advanced Photon Source, Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The use of the Swiss Muon Source (SμS) and Swiss Light Source (SLS), Paul Scherrer Institute, Villigen, Switzerland. Muon spectroscopy was partially supported by Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. Synthesis was supported by National Science Foundation (NSF) Grant No. DMR2004125 and Army Research Office (ARO) Grant No. W911NF2010108. Work at CINT, an Office of Science User Facility operated for the U.S. Department of Energy Office of Science through the Los Alamos National Laboratory. Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy (Contract No. 89233218CNA000001).

Keywords

anomalous Hall effect
delafossite
implantation
magnetism
molecular beam epitaxy
spintronics

Access to Document

10.1021/acs.nanolett.3c01065

Cite this

Brahlek, M., Mazza, A. R., Annaberdiyev, A., Chilcote, M., Rimal, G., Halász, G. B., Pham, A., Pai, Y. Y., Krogel, J. T., Lapano, J., Lawrie, B. J., Eres, G., McChesney, J., Prokscha, T., Suter, A., Oh, S., Freeland, J. W., Cao, Y., Gardner, J. S., ... Ward, T. Z. (2023). Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO₂. Nano Letters, 23(16), 7279-7287. https://doi.org/10.1021/acs.nanolett.3c01065

@article{0280bc2bacd944f4a2f622057472ae03,

title = "Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2",

abstract = "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 can be 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 ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.",

keywords = "anomalous Hall effect, delafossite, implantation, magnetism, molecular beam epitaxy, spintronics",

author = "Matthew Brahlek and Mazza, {Alessandro R.} and Abdulgani Annaberdiyev and Michael Chilcote and Gaurab Rimal and Hal{\'a}sz, {G{\'a}bor B.} and Anh Pham and Pai, {Yun Yi} and Krogel, {Jaron T.} and Jason Lapano and Lawrie, {Benjamin J.} and Gyula Eres and Jessica McChesney and Thomas Prokscha and Andreas Suter and Seongshik Oh and Freeland, {John W.} and Yue Cao and Gardner, {Jason S.} and Zaher Salman and Moore, {Robert G.} and Panchapakesan Ganesh and Ward, {T. Zac}",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = aug,

day = "23",

doi = "10.1021/acs.nanolett.3c01065",

language = "English",

volume = "23",

pages = "7279--7287",

journal = "Nano Letters",

issn = "1530-6984",

publisher = "American Chemical Society",

number = "16",

}

Brahlek, M, Mazza, AR, Annaberdiyev, A, Chilcote, M, Rimal, G, Halász, GB, Pham, A, Pai, YY, Krogel, JT, Lapano, J, Lawrie, BJ , Eres, G, McChesney, J, Prokscha, T, Suter, A, Oh, S, Freeland, JW, Cao, Y, Gardner, JS, Salman, Z, Moore, RG , Ganesh, P & Ward, TZ 2023, 'Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO₂', Nano Letters, vol. 23, no. 16, pp. 7279-7287. https://doi.org/10.1021/acs.nanolett.3c01065

TY - JOUR

T1 - Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2

AU - Brahlek, Matthew

AU - Mazza, Alessandro R.

AU - Annaberdiyev, Abdulgani

AU - Chilcote, Michael

AU - Rimal, Gaurab

AU - Halász, Gábor B.

AU - Pham, Anh

AU - Pai, Yun Yi

AU - Krogel, Jaron T.

AU - Lapano, Jason

AU - Lawrie, Benjamin J.

AU - Eres, Gyula

AU - McChesney, Jessica

AU - Prokscha, Thomas

AU - Suter, Andreas

AU - Oh, Seongshik

AU - Freeland, John W.

AU - Cao, Yue

AU - Gardner, Jason S.

AU - Salman, Zaher

AU - Moore, Robert G.

AU - Ganesh, Panchapakesan

AU - Ward, T. Zac

PY - 2023/8/23

Y1 - 2023/8/23

N2 - 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 can be 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 ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

AB - 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 can be 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 ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

KW - anomalous Hall effect

KW - delafossite

KW - implantation

KW - magnetism

KW - molecular beam epitaxy

KW - spintronics

UR - http://www.scopus.com/inward/record.url?scp=85167805716&partnerID=8YFLogxK

U2 - 10.1021/acs.nanolett.3c01065

DO - 10.1021/acs.nanolett.3c01065

M3 - Article

C2 - 37527431

AN - SCOPUS:85167805716

SN - 1530-6984

VL - 23

SP - 7279

EP - 7287

JO - Nano Letters

JF - Nano Letters

IS - 16

ER -