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Title: Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La 2 - x Sr x NiO 4 Observed by X Rays

Abstract

Here, we report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to collective magnetic excitations in S=1 systems by probing the Ni L 3 edge of La 2$$-$$xSr xNiO 4 (x=0, 0.33, 0.45). The magnetic excitation peak is asymmetric, indicating the presence of single and multi-spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. Lastly, this work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultrafast pump-probe experiments.

Authors:
 [1];  [1];  [2];  [2];  [2];  [3];  [4];  [4];  [5];  [6];  [6];  [1];  [7];  [7];  [2];  [8];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  2. Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany)
  3. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics and Inst. of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
  4. National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Synchotron Radiation and Nanotechnology Research Dept.
  6. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Condensed Matter Theory Group
  7. Univ. of Oxford (United Kingdom). Clarendon Lab., Dept. of Physics
  8. National Synchrotron Radiation Research Center, Hsinchu (Taiwan); National Tsing Hua Univ., Hsinchu (Taiwan). Dept. of Physics
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1351735
Alternate Identifier(s):
OSTI ID: 1351704
Report Number(s):
BNL-113724-2017-JA
Journal ID: ISSN 0031-9007; PRLTAO; R&D Project: PO011; KC0201060; TRN: US1700539
Grant/Contract Number:  
SC00112704; 104747; 2015CB92130; XDB07020200; 1047478
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 15; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Fabbris, G., Meyers, D., Xu, L., Katukuri, V. M., Hozoi, L., Liu, X., Chen, Z. -Y., Okamoto, J., Schmitt, T., Uldry, A., Delley, B., Gu, G. D., Prabhakaran, D., Boothroyd, A. T., van den Brink, J., Huang, D. J., and Dean, M. P. M. Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La2-xSrxNiO4 Observed by X Rays. United States: N. p., 2017. Web. doi:10.1103/PhysRevLett.118.156402.
Fabbris, G., Meyers, D., Xu, L., Katukuri, V. M., Hozoi, L., Liu, X., Chen, Z. -Y., Okamoto, J., Schmitt, T., Uldry, A., Delley, B., Gu, G. D., Prabhakaran, D., Boothroyd, A. T., van den Brink, J., Huang, D. J., & Dean, M. P. M. Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La2-xSrxNiO4 Observed by X Rays. United States. https://doi.org/10.1103/PhysRevLett.118.156402
Fabbris, G., Meyers, D., Xu, L., Katukuri, V. M., Hozoi, L., Liu, X., Chen, Z. -Y., Okamoto, J., Schmitt, T., Uldry, A., Delley, B., Gu, G. D., Prabhakaran, D., Boothroyd, A. T., van den Brink, J., Huang, D. J., and Dean, M. P. M. Wed . "Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La2-xSrxNiO4 Observed by X Rays". United States. https://doi.org/10.1103/PhysRevLett.118.156402. https://www.osti.gov/servlets/purl/1351735.
@article{osti_1351735,
title = {Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La2-xSrxNiO4 Observed by X Rays},
author = {Fabbris, G. and Meyers, D. and Xu, L. and Katukuri, V. M. and Hozoi, L. and Liu, X. and Chen, Z. -Y. and Okamoto, J. and Schmitt, T. and Uldry, A. and Delley, B. and Gu, G. D. and Prabhakaran, D. and Boothroyd, A. T. and van den Brink, J. and Huang, D. J. and Dean, M. P. M.},
abstractNote = {Here, we report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to collective magnetic excitations in S=1 systems by probing the Ni L3 edge of La2$-$xSrxNiO4 (x=0, 0.33, 0.45). The magnetic excitation peak is asymmetric, indicating the presence of single and multi-spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. Lastly, this work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultrafast pump-probe experiments.},
doi = {10.1103/PhysRevLett.118.156402},
url = {https://www.osti.gov/biblio/1351735}, journal = {Physical Review Letters},
issn = {0031-9007},
number = 15,
volume = 118,
place = {United States},
year = {2017},
month = {4}
}

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Cited by: 2 works
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Works referenced in this record:

Persistence of High-Frequency Spin Fluctuations in Overdoped Superconducting La 2 x Sr x CuO 4 ( x = 0.22 )
journal, August 2007


Multiplet effects in X-ray spectroscopy
journal, January 2005


Spin–orbital separation in the quasi-one-dimensional Mott insulator Sr2CuO3
journal, April 2012


Spin dynamics in stripe-ordered La 5 / 3 Sr 1 / 3 NiO 4
journal, March 2003


Two energy scales in the spin excitations of the high-temperature superconductor La2−xSrxCuO4
journal, February 2007


A combination of quasirelativistic pseudopotential and ligand field calculations for lanthanoid compounds
journal, June 1993


Comparison of x-ray absorption with x-ray photoemission of nickel dihalides and NiO
journal, March 1986


Spin dynamics of half-doped La 3 2 Sr 1 2 Ni O 4
journal, May 2005


Multiplet structure in the L 2 , 3 x-ray-absorption spectra: A fingerprint for high- and low-spin Ni 2 + compounds
journal, April 1988


Collective Nature of Spin Excitations in Superconducting Cuprates Probed by Resonant Inelastic X-Ray Scattering
journal, May 2015


Theory of Resonant Inelastic X-Ray Scattering by Collective Magnetic Excitations
journal, October 2010


Doping dependence of the magnetic excitations in La 2 x Sr x CuO 4
journal, February 2017


Asymmetry of collective excitations in electron- and hole-doped cuprate superconductors
journal, October 2014


Resonant inelastic x-ray scattering studies of elementary excitations
journal, June 2011


Ab Initio determination of Cu 3d orbital energies in layered copper oxides
journal, August 2011


Excitonic quasiparticles in a spin–orbit Mott insulator
journal, July 2014


Spin-Wave Excitations in Two Dimensional Antiferromagnet of Stoichiometric La 2 NiO 4
journal, December 1993


Spin Correlations among the Charge Carriers in an Ordered Stripe Phase
journal, December 2003


Specific CI calculation of energy differences: Transition energies and bond energies
journal, May 1993


Ab initio calculation of d - d excitations in quasi-one-dimensional Cu d 9 correlated materials
journal, December 2011


Highly efficient beamline and spectrometer for inelastic soft X-ray scattering at high resolution
journal, January 2014


Systematic computation of crystal-field multiplets for x-ray core spectroscopies
journal, March 2012


Energy‐adjusted a b i n i t i o pseudopotentials for the first row transition elements
journal, January 1987


NiO as a test case for high resolution resonant inelastic soft x-ray scattering
journal, August 2005


Oxygen and strontium codoping of La 2 Ni O 4 : Room-temperature phase diagrams
journal, August 2004


Spin excitations in a single La2CuO4 layer
journal, September 2012


Towards 10 meV resolution: The design of an ultrahigh resolution soft X-ray RIXS spectrometer
journal, November 2016


Polarization-dependent nickel 2 p x-ray-absorption spectra of La 2 NiO 4 + δ
journal, January 1998


Persistent spin excitations in doped antiferromagnets revealed by resonant inelastic light scattering
journal, February 2014


Local spin-flip spectral distribution obtained by resonant x-ray Raman scattering
journal, June 1998


Simultaneous Ordering of Holes and Spins in La 2 Ni O 4.125
journal, August 1994


Systematically convergent basis sets for transition metals. I. All-electron correlation consistent basis sets for the 3d elements Sc–Zn
journal, August 2005


Neutron diffraction study on structural and magnetic properties of La 2 NiO 4
journal, May 1991


Optical spectroscopy of the charge-ordering transition in La 1.67 Sr 0.33 NiO 4
journal, November 1996


Raman and fluorescence characteristics of resonant inelastic X-ray scattering from doped superconducting cuprates
journal, January 2016


Localized Electronic Excitations in NiO Studied with Resonant Inelastic X-Ray Scattering at the Ni M Threshold: Evidence of Spin Flip
journal, October 2005


Magnetic and ligand field properties of copper at the interfaces of (CaCuO 2 ) n /(SrTiO 3 ) n superlattices
journal, June 2012


Energy-adjusted pseudopotentials for the rare earth elements
journal, January 1989


O 1 s near-edge x-ray absorption of La 2 x Sr x NiO 4 + δ : Holes, polarons, and excitons
journal, April 1996


SAXES, a high resolution spectrometer for resonant x-ray emission in the 400–1600eV energy range
journal, November 2006


Direct observation of dynamic charge stripes in La2–xSrxNiO4
journal, March 2014


The CTM4XAS program for EELS and XAS spectral shape analysis of transition metal L edges
journal, October 2010


Insights into the high temperature superconducting cuprates from resonant inelastic X-ray scattering
journal, February 2015


Dispersive spin excitations in highly overdoped cuprates revealed by resonant inelastic x-ray scattering
journal, July 2013


Intense paramagnon excitations in a large family of high-temperature superconductors
journal, July 2011


Complete Two-Dimensional Antiferromagnetic Spin-Wave Dispersion Relation of La 2 NiO 4 Determined by Chopper Spectrometer Installed at the Pulsed Neutron Source
journal, April 1991


Magnetic spectrum of the two-dimensional antiferromagnet La 2 CoO 4 studied by inelastic neutron scattering
journal, November 2010


Evidence for Short-Range-Ordered Charge Stripes Far above the Charge-Ordering Transition in La 1.67 Sr 0.33 NiO 4
journal, August 2013


Melting of Quasi-Two-Dimensional Charge Stripes in La 5 / 3 Sr 1 / 3 NiO 4
journal, September 1997


Density matrix averaged atomic natural orbital (ANO) basis sets for correlated molecular wave functions: IV. Medium size basis sets for the atoms H-Kr
journal, January 1995


Variational calculation of small energy differences. The singlet-triplet gap in [Cu2Cl6]2−
journal, October 1992


d d excitations and charge ordering in La 5 / 3 Sr 1 / 3 NiO 4
journal, May 2010


Isotropic O 1s prepeak as evidence for polarons in La2NiO4 + δ
journal, March 1995


Mapping spin-wave dispersions in stripe-ordered La 2 x Sr x Ni O 4 ( x = 0.275 , 0.333)
journal, August 2005


Magnetic Correlations in La 2 Ni O 4 + δ
journal, July 1988


Quenched Magnon excitations by oxygen sublattice reconstruction in (SrCuO2)n/(SrTiO3)2 superlattices
journal, September 2016


Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates
journal, October 2016


Growth of large La2–xSrxNiO4+δ single crystals by the floating-zone technique
journal, April 2002


Electronic states in La 2 x Sr x CuO 4 + δ probed by soft-x-ray absorption
journal, January 1991


Spin Waves and Electronic Interactions in La 2 CuO 4
journal, June 2001


Observation of Two Nondispersive Magnetic Excitations in NiO by Resonant Inelastic Soft-X-Ray Scattering
journal, January 2009


High-Energy Spin Dynamics in L a 1.69 S r 0.31 N i O 4
journal, April 2003


Structure of the interstitial oxygen defect in La 2 NiO 4 + δ
journal, August 1989


    Works referencing / citing this record:

    Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective
    journal, April 2019

    • Cao, Y.; Mazzone, D. G.; Meyers, D.
    • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
    • https://doi.org/10.1098/rsta.2017.0480

    Measurement of the Resonant Magneto-Optical Kerr Effect Using a Free Electron Laser
    journal, June 2017


    Emergent c -axis magnetic helix in manganite-nickelate superlattices
    journal, November 2018


    Continuum Charge Excitations in High-Valence Transition-Metal Oxides Revealed by Resonant Inelastic X-Ray Scattering
    journal, September 2018


    Low-energy orbital excitations in strained LaCoO 3 films
    journal, October 2019


    Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective
    journal, April 2019

    • Cao, Y.; Mazzone, D. G.; Meyers, D.
    • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
    • https://doi.org/10.1098/rsta.2017.0480

    Ab‐Initio Real‐Time Magnon Dynamics in Ferromagnetic and Ferrimagnetic Systems
    journal, January 2020