Summary
This study utilized muon spin rotation spectroscopy to investigate the effect of oxygen isotope substitution (16O/18O) on the spin density wave (SDW) transition in the trilayer Ruddlesden-Popper nickelate Pr4Ni3O10. Under ambient pressure, the SDW transition temperatures for the 16O and 18O samples were 158.04 K and 159.81 K, respectively, exhibiting a finite isotope shift. Under hydrostatic pressure, the transition temperatures for both isotopes decreased linearly at nearly identical rates (approximately -4.9 K/GPa), resulting in an essentially pressure-independent isotope shift. This pressure-independent isotope effect indicates that the SDW transition primarily originates from electronic correlations rather than lattice dynamics. Combined with recent inelastic X-ray scattering results that revealed no phonon softening, this study supports a novel mechanism of intertwined charge density wave and spin density wave order stabilized by strong spin interactions in trilayer Ruddlesden-Popper nickelates. This finding contrasts with the doping-enhanced isotope effect observed in cuprates and provides critical constraints for understanding the electronic origin of density wave order and its relationship with superconductivity in nickelates.
Materials
Methods
- Muon-spin rotation (μSR)
- Raman spectroscopy
- Oxygen isotope substitution
- High-pressure measurements
Keywords
- oxygen isotope effect
- spin density wave
- intertwined order
- electronically driven
- charge density wave
- pressure invariant
Highlights
- First pressure-dependent isotope effect study in trilayer RP nickelates.
- Provides evidence that the intertwined CDW/SDW transition is electronically driven.
- Contrasts with cuprate isotope effect behavior.
Conclusions
- The SDW transition shows a finite oxygen-isotope shift at ambient pressure (ΔT_SDW = 1.77 K).
- Under hydrostatic pressure, T_SDW decreases linearly at nearly identical rates for both isotope compositions, making the isotope shift pressure-independent.
- The absence of pressure enhancement indicates a predominantly electronic origin of the SDW transition.
- This is consistent with recent inelastic X-ray scattering results showing no phonon softening, suggesting a new regime of intertwined order stabilized by strong spin interactions.
Main claims
- The SDW transition shows a finite oxygen-isotope shift at ambient pressure (ΔT_SDW ≈ 1.77 K).
- Evidence: Abstract,Full text: At ambient pressure, 16T_SDW=158.04(5) K and 18T_SDW=159.81(6) K.
- Under pressure, T_SDW decreases linearly at nearly identical rates for both isotopes, so the isotope shift remains constant.
- Evidence: Abstract,Full text: d16T_SDW/dp=-4.93(5) K/GPa and d18T_SDW/dp=-4.90(7) K/GPa.
- The absence of pressure enhancement of the isotope effect points to a predominantly electronic origin of the SDW transition.
- Evidence: Abstract,Full text: The absence of pressure enhancement… points to a predominantly electronic origin of the SDW transition.
Workflow
- sample_preparation
- Materials: Pr4Ni3O10; 16O/18O isotope substitution
- Methods: oxygen-isotope exchange
- Observations: 18O enrichment ≈70%
- muon_SR_measurement
- Methods: weak-transverse-field μSR; hydrostatic pressure cell
- Observations: SDW transition temperatures for both isotopes
- Raman_measurement
- Methods: Raman spectroscopy
- Observations: oxygen participation in phonon modes
- data_analysis
- Methods: Fermi function fit to paramagnetic fraction; linear fit of T_SDW vs pressure
- Observations: dT_SDW/dp nearly identical for both isotopes; isotope shift constant under pressure
- interpretation — The pressure-independent isotope effect indicates an electronic origin of the SDW transition.