skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Physical Review Letters
 [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

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC00112704; 104747; 2015CB92130; XDB07020200; 1047478
OSTI ID:
1351735
Alternate ID(s):
OSTI ID: 1351704
Report Number(s):
BNL-113724-2017-JA; PRLTAO; R&D Project: PO011; KC0201060; TRN: US1700539
Journal Information:
Physical Review Letters, Vol. 118, Issue 15; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

References (87)

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
Molecular Electronic-Structure Theory book August 2000
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
Emergence of Coherent Magnetic Excitations in the High Temperature Underdoped La 2 x Sr x CuO 4 Superconductor at Low Temperatures journal April 2009
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
Magnetic Excitation Spectra of Sr 2 IrO 4 Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors journal April 2012
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
Magnetic excitations in stripe-ordered La 1.875 Ba 0.125 CuO 4 studied using resonant inelastic x-ray scattering journal July 2013
Transition Metal Compounds book January 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
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Persistence of magnetic excitations in La2−xSrxCuO4 from the undoped insulator to the heavily overdoped non-superconducting metal journal August 2013
Ab initio calculation of d - d excitations in quasi-one-dimensional Cu d 9 correlated materials journal December 2011
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
High-Energy Magnetic Excitations in the Cuprate Superconductor Bi 2 Sr 2 CaCu 2 O 8 + δ : Towards a Unified Description of Its Electronic and Magnetic Degrees of Freedom journal April 2013
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
Magnetic Excitations and Phase Separation in the Underdoped La 2 x Sr x CuO 4 Superconductor Measured by Resonant Inelastic X-Ray Scattering journal February 2010
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
Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4 journal May 2016
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
High-energy magnetic excitations in overdoped La 2 x Sr x CuO 4 studied by neutron and resonant inelastic x-ray scattering journal May 2015
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
High-resolution soft X-ray beamline ADRESS at the Swiss Light Source for resonant inelastic X-ray scattering and angle-resolved photoelectron spectroscopies journal July 2010
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
Orbital characters of three-dimensional Fermi surfaces in Eu 2 x Sr x NiO 4 as probed by soft-x-ray angle-resolved photoemission spectroscopy journal December 2011
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
Core Level Spectroscopy of Solids book January 2008
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
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
Orbital Engineering in Nickelate Heterostructures Driven by Anisotropic Oxygen Hybridization rather than Orbital Energy Levels journal September 2016
Structure of the interstitial oxygen defect in La 2 NiO 4 + δ journal August 1989
The Theory of Atomic Structure and Spectra book December 1981
Density matrix averaged atomic natural orbital (ANO) basis sets for correlated molecular wave functions journal January 1995
Transition metal compounds journal December 1976
Intense paramagnon excitations in a large family of high-temperature superconductors text January 2011
Dispersive spin excitations in highly overdoped cuprates revealed by resonant inelastic x-ray scattering text January 2013
Persistence of magnetic excitations in La2-xSrxCuO4 from the undoped insulator to the heavily overdoped non-superconducting metal text January 2013
Persistent spin excitations in doped antiferromagnets revealed by resonant inelastic light scattering text January 2013
Asymmetry of collective excitations in electron and hole doped cuprate superconductors text January 2013
Direct observation of dynamic charge stripes in La2-xSrxNiO4 text January 2013
Excitonic quasiparticles in a spin-orbit Mott insulator text January 2014
Collective nature of spin excitations in superconducting cuprates probed by resonant inelastic x-ray scattering preprint January 2015
High-energy magnetic excitations in overdoped La$_{2-x}$Sr$_{x}$CuO$_{4}$ studied by neutron and resonant inelastic X-ray scattering text January 2015
Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels text January 2016

Cited By (8)

Ab‐Initio Real‐Time Magnon Dynamics in Ferromagnetic and Ferrimagnetic Systems journal January 2020
Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective
  • 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
journal April 2019
Low-energy orbital excitations in strained LaCoO 3 films journal October 2019
Measurement of the Resonant Magneto-Optical Kerr Effect Using a Free Electron Laser journal June 2017
Site-Selective Probe of Magnetic Excitations in Rare-Earth Nickelates Using Resonant Inelastic X-ray Scattering text January 2018
Continuum Charge Excitations in High-Valence Transition-Metal Oxides Revealed by Resonant Inelastic X-ray Scattering text January 2018
Emergent c-axis magnetic helix in manganite-nickelate superlattices text January 2018
Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective text January 2018