DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Magnetically propagating Hund’s exciton in van der Waals antiferromagnet NiPS3

Journal Article · · Nature Communications
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [1];  [3]; ORCiD logo [3]; ORCiD logo [2];  [4]; ORCiD logo [5]; ORCiD logo [3]; ORCiD logo [6]; ORCiD logo [1]
  1. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  2. Univ. of Warsaw (Poland)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. Univ. of Tennessee, Knoxville, TN (United States)
  5. Univ. of Texas, Austin, TX (United States)
  6. Harvard Univ., Cambridge, MA (United States)

Magnetic van der Waals (vdW) materials have opened new frontiers for realizing novel many-body phenomena. Recently NiPS3 has received intense interest since it hosts an excitonic quasiparticle whose properties appear to be intimately linked to the magnetic state of the lattice. Despite extensive studies, the electronic character, mobility, and magnetic interactions of the exciton remain unresolved. Here we address these issues by measuring NiPS3 with ultra-high energy resolution resonant inelastic x-ray scattering (RIXS). We find that Hund’s exchange interactions are primarily responsible for the energy of formation of the exciton. Measuring the dispersion of the Hund’s exciton reveals that it propagates in a way that is analogous to a double-magnon. We trace this unique behavior to fundamental similarities between the NiPS3 exciton hopping and spin exchange processes, underlining the unique magnetic characteristics of this novel quasiparticle.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); US Army Research Office (ARO); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704
OSTI ID:
2331227
Alternate ID(s):
OSTI ID: 2340941; OSTI ID: 2370324
Report Number(s):
BNL--225384-2024-JAAM; BNL--225675-2024-JAAM
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (46)

Spin-correlated exciton–polaritons in a van der Waals magnet journal September 2022
Magnon gap excitations and spin-entangled optical transition in the van der Waals antiferromagnet NiPS3 journal September 2023
Effective Hamiltonian for the superconducting Cu oxides journal March 1988
Multiferroic‐Enabled Magnetic‐Excitons in 2D Quantum‐Entangled Van der Waals Antiferromagnet NiI 2 journal January 2022
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 April 2017
Colloquium : Excitons in atomically thin transition metal dichalcogenides journal April 2018
Magnetic structure of the quasi-two-dimensional antiferromagnet NiPS 3 journal December 2015
Nickel L-Edge Soft X-ray Spectroscopy of Nickel−Iron Hydrogenases and Model CompoundsEvidence for High-Spin Nickel(II) in the Active Enzyme journal November 2000
The determining factor for interstitial oxygen formation in Ruddlesden–Popper type La 2 NiO 4 -based oxides journal January 2016
EDRIXS: An open source toolkit for simulating spectra of resonant inelastic x-ray scattering dataset January 2019
Exciton-magnon structure of the optical absorption spectrum of antiferromagnetic MnPS3 journal February 2011
Soft X-Ray Spectroscopy of Low-Valence Nickelates journal December 2021
Coherent many-body exciton in van der Waals antiferromagnet NiPS3 journal July 2020
Local spin-flip spectral distribution obtained by resonant x-ray Raman scattering journal June 1998
Magnetic dynamics of NiPS3 journal November 2022
mpmdean/He2024magnetically: v1.0.0 software March 2024
Electronic Raman scattering in the 2D antiferromagnet NiPS 3 journal January 2022
High-temperature charge density wave correlations in La 1.875 Ba 0.125 CuO 4 without spin–charge locking journal November 2017
Excitonic quasiparticles in a spin–orbit Mott insulator journal July 2014
Magnetism in two-dimensional van der Waals materials journal October 2018
Spin-mediated Mott excitons journal February 2023
Spin Dynamics of the 2D Spin 1 2 Quantum Antiferromagnet Copper Deuteroformate Tetradeuterate (CFTD) journal June 2001
Highly anisotropic excitons and multiple phonon bound states in a van der Waals antiferromagnetic insulator journal March 2021
Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4 journal May 2016
Exciton-magnon splitting in the van der Waals antiferromagnet MnPS3 unveiled by second-harmonic generation journal November 2023
Electron-hole excitations and optical spectra from first principles journal August 2000
Nature of Excitons and Their Ligand-Mediated Delocalization in Nickel Dihalide Charge-Transfer Insulators journal July 2024
Charge-Spin Correlation in van der Waals Antiferromagnet NiPS 3 journal March 2018
Three-dimensional dispersion of spin waves measured in NiO by resonant inelastic x-ray scattering journal July 2017
Lattice dynamics of layered MP X 3 ( M= Mn,Fe,Ni,Zn; X= S,Se) compounds journal December 1988
EDRIXS: An open source toolkit for simulating spectra of resonant inelastic x-ray scattering journal October 2019
Resonant inelastic x-ray scattering studies of elementary excitations journal June 2011
Many-Body Physics of Single and Double Spin-Flip Excitations in NiO journal February 2020
Towards 10 meV resolution: The design of an ultrahigh resolution soft X-ray RIXS spectrometer journal November 2016
Quantum dynamics of the square-lattice Heisenberg model journal October 2018
Controlling the anisotropy of a van der Waals antiferromagnet with light journal June 2021
Spin wave Hamiltonian and anomalous scattering in NiPS3 journal September 2023
Observation of Two Nondispersive Magnetic Excitations in NiO by Resonant Inelastic Soft-X-Ray Scattering journal January 2009
The Magnetic Genome of Two-Dimensional van der Waals Materials journal April 2022
Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS3 journal January 2024
Exciton-driven antiferromagnetic metal in a correlated van der Waals insulator journal August 2021
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies journal October 1986
Two-dimensional magnetic crystals and emergent heterostructure devices journal February 2019
Spatially Resolved Photogenerated Exciton and Charge Transport in Emerging Semiconductors journal April 2020
Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet journal March 2023
Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals journal April 2021