Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning

Samarakoon, Anjana M.; Laurell, Pontus; Balz, Christian; Banerjee, Arnab; Lampen-Kelley, Paula; Mandrus, David; Nagler, Stephen E.; Okamoto, Satoshi; Tennant, D. Alan

doi:10.1103/PhysRevResearch.4.L022061

Title: Extraction of interaction parameters for $α − {RuCl}_{3}$ from neutron data using machine learning

Abstract

Single-crystal inelastic neutron-scattering (INS) data contain rich information about the structure and dynamics of a material. Yet the challenge of matching sophisticated theoretical models with large data volumes is compounded by computational complexity and the ill-posed nature of the inverse scattering problem. Here we utilize a novel machine-learning (ML)-assisted framework featuring multiple neural network architectures to address this via high-dimensional modeling and numerical methods. A comprehensive data set of diffraction and INS measured on the Kitaev material α-RuCl₃ is processed to extract its Hamiltonian. Semiclassical Landau-Lifshitz dynamics and Monte-Carlo simulations were employed to explore the parameter space of an extended Kitaev-Heisenberg Hamiltonian. A ML-assisted iterative algorithm was developed to map the uncertainty manifold to match experimental data, a nonlinear autoencoder was used to undertake information compression, and radial basis networks were utilized as fast surrogates for diffraction and dynamics simulations to predict potential spin Hamiltonians with uncertainty. Exact diagonalization calculations were employed to assess the impact of quantum fluctuations on the selected parameters around the best prediction.

Authors:

;

; Balz, Christian; Banerjee, Arnab; Lampen-Kelley, Paula; Mandrus, David;

; Okamoto, Satoshi; Tennant, D. Alan

Publication Date:: Tue Jun 21 00:00:00 EDT 2022

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) and Oak Ridge Leadership Computing Facility (OLCF); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC)

OSTI Identifier:: 1873436

Alternate Identifier(s):: OSTI ID: 1873526; OSTI ID: 1883884

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

Resource Type:: Published Article

Journal Name:: Physical Review Research

Additional Journal Information:: Journal Name: Physical Review Research Journal Volume: 4 Journal Issue: 2; Journal ID: ISSN 2643-1564

Publisher:: American Physical Society

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; quantum spin liquid; strongly correlated systems; data analysis; deep learning; exact diagonalization; hybrid Monte Carlo algorithm; inelastic neutron scattering; Kitaev-Heisenberg model; Landau-Lifshitz model; machine learning; neutron diffraction; neutron scattering; simulated annealing

Citation Formats


                    Samarakoon, Anjana M., Laurell, Pontus, Balz, Christian, Banerjee, Arnab, Lampen-Kelley, Paula, Mandrus, David, Nagler, Stephen E., Okamoto, Satoshi, and Tennant, D. Alan. Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning.  United States: N. p., 2022. 
Web.  doi:10.1103/PhysRevResearch.4.L022061.

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                    Samarakoon, Anjana M., Laurell, Pontus, Balz, Christian, Banerjee, Arnab, Lampen-Kelley, Paula, Mandrus, David, Nagler, Stephen E., Okamoto, Satoshi, & Tennant, D. Alan. Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning.  United States.  https://doi.org/10.1103/PhysRevResearch.4.L022061

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                    Samarakoon, Anjana M., Laurell, Pontus, Balz, Christian, Banerjee, Arnab, Lampen-Kelley, Paula, Mandrus, David, Nagler, Stephen E., Okamoto, Satoshi, and Tennant, D. Alan. Tue .  
"Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning".  United States.  https://doi.org/10.1103/PhysRevResearch.4.L022061.

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@article{osti_1873436,

  title        = {Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning},

  author       = {Samarakoon, Anjana M. and Laurell, Pontus and Balz, Christian and Banerjee, Arnab and Lampen-Kelley, Paula and Mandrus, David and Nagler, Stephen E. and Okamoto, Satoshi and Tennant, D. Alan},

  abstractNote = {Single-crystal inelastic neutron-scattering (INS) data contain rich information about the structure and dynamics of a material. Yet the challenge of matching sophisticated theoretical models with large data volumes is compounded by computational complexity and the ill-posed nature of the inverse scattering problem. Here we utilize a novel machine-learning (ML)-assisted framework featuring multiple neural network architectures to address this via high-dimensional modeling and numerical methods. A comprehensive data set of diffraction and INS measured on the Kitaev material α-RuCl3 is processed to extract its Hamiltonian. Semiclassical Landau-Lifshitz dynamics and Monte-Carlo simulations were employed to explore the parameter space of an extended Kitaev-Heisenberg Hamiltonian. A ML-assisted iterative algorithm was developed to map the uncertainty manifold to match experimental data, a nonlinear autoencoder was used to undertake information compression, and radial basis networks were utilized as fast surrogates for diffraction and dynamics simulations to predict potential spin Hamiltonians with uncertainty. Exact diagonalization calculations were employed to assess the impact of quantum fluctuations on the selected parameters around the best prediction.},

  doi          = {10.1103/PhysRevResearch.4.L022061},

  journal      = {Physical Review Research},

  number       = 2,

  volume       = 4,

  place        = {United States},

  year         = {Tue Jun 21 00:00:00 EDT 2022},

  month        = {Tue Jun 21 00:00:00 EDT 2022}

}

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Jackeli, G.; Khaliullin, G.
Physical Review Letters, Vol. 102, Issue 1
DOI: 10.1103/PhysRevLett.102.017205

Interpretable, calibrated neural networks for analysis and understanding of inelastic neutron scattering data
journal, April 2021

Butler, Keith T.; Le, Manh Duc; Thiyagalingam, Jeyan
Journal of Physics: Condensed Matter, Vol. 33, Issue 19
DOI: 10.1088/1361-648X/abea1c

Spin-Wave Excitations Evidencing the Kitaev Interaction in Single Crystalline $α − {RuCl}_{3}$
journal, March 2017

Ran, Kejing; Wang, Jinghui; Wang, Wei
Physical Review Letters, Vol. 118, Issue 10
DOI: 10.1103/PhysRevLett.118.107203

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Title: Extraction of interaction parameters for α − RuCl 3 from neutron data using machine learning

Abstract

Citation Formats

Breakdown of magnons in a strongly spin-orbital coupled magnet journal, October 2017

Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3 journal, June 2021

Field-induced quantum criticality in the Kitaev system α − RuCl 3 journal, July 2017

Quantum lattice model solver H Φ journal, August 2017

Erratum: Effective model with strong Kitaev interactions for α − RuCl 3 [Phys. Rev. B 97 , 134424 (2018)] journal, June 2019

Field-induced intermediate ordered phase and anisotropic interlayer interactions in α − RuCl 3 journal, May 2021

2D proximate quantum spin liquid state in atomic-thin α -RuCl 3 journal, November 2018

Proximate ferromagnetic state in the Kitaev model material α-RuCl3 journal, July 2021

Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales journal, June 2016

Excitations in the field-induced quantum spin liquid state of α-RuCl3 journal, February 2018

Finite field regime for a quantum spin liquid in α − RuCl 3 journal, August 2019

Phase diagram of α − RuCl 3 in an in-plane magnetic field journal, May 2017

Time-Domain Anyon Interferometry in Kitaev Honeycomb Spin Liquids and Beyond journal, April 2021

Observation of two types of fractional excitation in the Kitaev honeycomb magnet journal, May 2018

Magnetic field-dependent low-energy magnon dynamics in α – RuCl 3 journal, August 2019

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS journal, November 2010

Quantum spin liquids: a review journal, November 2016

Sample dependence of half-integer quantized thermal Hall effect in the Kitaev spin-liquid candidate α − RuCl 3 journal, December 2020

Thermodynamic evidence of fractionalized excitations in α − RuC l 3 journal, March 2019

Models and materials for generalized Kitaev magnetism journal, November 2017

Evidence for a Field-Induced Quantum Spin Liquid in α - RuCl 3 journal, July 2017

Probing α − RuCl 3 Beyond Magnetic Order: Effects of Temperature and Magnetic Field journal, February 2018

Oscillations of the thermal conductivity in the spin-liquid state of α-RuCl3 journal, May 2021

Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α − RuCl 3 journal, December 2017

Machine learning for neutron scattering at ORNL * journal, January 2021

Machine-learned phase diagrams of generalized Kitaev honeycomb magnets journal, September 2021

Spin-wave analysis of the low-temperature thermal Hall effect in the candidate Kitaev spin liquid α − RuCl 3 journal, August 2018

Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 journal, April 2015

α − RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice journal, July 2014

Unveiling magnetic interactions of ruthenium trichloride via constraining direction of orbital moments: Potential routes to realize a quantum spin liquid journal, August 2017

Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3 journal, January 2020

Antiferromagnetic Resonance and Terahertz Continuum in α − RuCl 3 journal, November 2017

Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in α − RuCl 3 journal, November 2017

Thermodynamic Perspective on Field-Induced Behavior of α − RuCl 3 journal, August 2020

Thermal Pure Quantum States at Finite Temperature journal, June 2012

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3 journal, November 2016

Crystal structure and magnetism in α − RuCl 3 : An ab initio study journal, April 2016

Equation of State Calculations by Fast Computing Machines journal, June 1953

Deriving models for the Kitaev spin-liquid candidate material α − RuCl 3 from first principles journal, August 2019

Polarization-resolved Raman spectroscopy of α − RuCl 3 and evidence of room-temperature two-dimensional magnetic scattering journal, October 2019

Nesting instability of gapless U(1) spin liquids with spinon Fermi pockets in two dimensions journal, October 2021

Effective model with strong Kitaev interactions for α − RuCl 3 journal, April 2018

Thermodynamic evidence for a field-angle-dependent Majorana gap in a Kitaev spin liquid journal, January 2022

Theoretical investigation of magnetic dynamics in α − RuCl 3 journal, September 2017

Low-temperature crystal and magnetic structure of α − RuCl 3 journal, April 2016

Rethinking α − RuCl 3 journal, July 2020

Electrical Probes of the Non-Abelian Spin Liquid in Kitaev Materials journal, July 2020

Terahertz excitations in α − RuC l 3 : Majorana fermions and rigid-plane shear and compression modes journal, September 2019

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet journal, April 2016

Spin liquids in frustrated magnets journal, March 2010

Concept and realization of Kitaev quantum spin liquids journal, March 2019

Anyons in an exactly solved model and beyond journal, January 2006

Monoclinic crystal structure of α − RuCl 3 and the zigzag antiferromagnetic ground state journal, December 2015

Fermionic response from fractionalization in an insulating two-dimensional magnet journal, July 2016

The range of non-Kitaev terms and fractional particles in α-RuCl3 journal, March 2020

The Spallation Neutron Source in Oak Ridge: A powerful tool for materials research journal, November 2006

Unusual Thermal Hall Effect in a Kitaev Spin Liquid Candidate α − RuCl 3 journal, May 2018

Magnetic order in α − RuCl 3 : A honeycomb-lattice quantum magnet with strong spin-orbit coupling journal, April 2015

Machine learning for magnetic phase diagrams and inverse scattering problems journal, November 2021

Evidence for Magnetic Fractional Excitations in a Kitaev Quantum-Spin-Liquid Candidate α-RuCl 3 journal, February 2022

Physics of the Kitaev Model: Fractionalization, Dynamic Correlations, and Material Connections journal, March 2018

Half-integer quantized anomalous thermal Hall effect in the Kitaev material candidate α-RuCl 3 journal, July 2021

Neutron scattering in the proximate quantum spin liquid α-RuCl 3 journal, June 2017

Magnetic thermal conductivity far above the Néel temperature in the Kitaev-magnet candidate α − RuCl 3 journal, June 2017

Revealing the phase diagram of Kitaev materials by machine learning: Cooperation and competition between spin liquids journal, April 2021

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Corelli: Efficient single crystal diffraction with elastic discrimination journal, October 2008

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Machine-learning-assisted insight into spin ice Dy2Ti2O7 journal, February 2020

Majorana fermions in the Kitaev quantum spin system α-RuCl3 journal, September 2017

Nature of Magnetic Excitations in the High-Field Phase of α − RuCl 3 journal, July 2020

Kitaev magnetism in honeycomb RuCl 3 with intermediate spin-orbit coupling journal, June 2015

Machine learning on neutron and x-ray scattering and spectroscopies journal, September 2021

Magnetic anisotropy in the Kitaev model systems Na 2 IrO 3 and RuCl 3 journal, August 2016

Efficient Global Optimization of Expensive Black-Box Functions journal, January 1998

Machine learning for quantum matter journal, January 2020

Title: Extraction of interaction parameters for $α − {RuCl}_{3}$ from neutron data using machine learning

Breakdown of magnons in a strongly spin-orbital coupled magnet
journal, October 2017

Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3
journal, June 2021

Field-induced quantum criticality in the Kitaev system $α - {RuCl}_{3}$
journal, July 2017

Quantum lattice model solver $H Φ$
journal, August 2017

Erratum: Effective model with strong Kitaev interactions for $α − {RuCl}_{3}$ [Phys. Rev. B 97 , 134424 (2018)]
journal, June 2019

Field-induced intermediate ordered phase and anisotropic interlayer interactions in $α − {RuCl}_{3}$
journal, May 2021

2D proximate quantum spin liquid state in atomic-thin α -RuCl ₃
journal, November 2018

Proximate ferromagnetic state in the Kitaev model material α-RuCl3
journal, July 2021

Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
journal, June 2016

Excitations in the field-induced quantum spin liquid state of α-RuCl3
journal, February 2018

Finite field regime for a quantum spin liquid in $α − {RuCl}_{3}$
journal, August 2019

Phase diagram of $α - {RuCl}_{3}$ in an in-plane magnetic field
journal, May 2017

Time-Domain Anyon Interferometry in Kitaev Honeycomb Spin Liquids and Beyond
journal, April 2021

Observation of two types of fractional excitation in the Kitaev honeycomb magnet
journal, May 2018

Magnetic field-dependent low-energy magnon dynamics in $α - {RuCl}_{3}$
journal, August 2019

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010

Quantum spin liquids: a review
journal, November 2016

Sample dependence of half-integer quantized thermal Hall effect in the Kitaev spin-liquid candidate $α − {RuCl}_{3}$
journal, December 2020

Thermodynamic evidence of fractionalized excitations in $α - RuC l_{3}$
journal, March 2019

Models and materials for generalized Kitaev magnetism
journal, November 2017

Evidence for a Field-Induced Quantum Spin Liquid in $α$ - ${RuCl}_{3}$
journal, July 2017

Probing $α - {RuCl}_{3}$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field
journal, February 2018

Oscillations of the thermal conductivity in the spin-liquid state of α-RuCl3
journal, May 2021

Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of $α − {RuCl}_{3}$
journal, December 2017

Machine learning for neutron scattering at ORNL ^*
journal, January 2021

Machine-learned phase diagrams of generalized Kitaev honeycomb magnets
journal, September 2021

Spin-wave analysis of the low-temperature thermal Hall effect in the candidate Kitaev spin liquid $α - {RuCl}_{3}$
journal, August 2018

Scattering Continuum and Possible Fractionalized Excitations in $α − {RuCl}_{3}$
journal, April 2015

$α - {RuCl}_{3}$ : A spin-orbit assisted Mott insulator on a honeycomb lattice
journal, July 2014

Unveiling magnetic interactions of ruthenium trichloride via constraining direction of orbital moments: Potential routes to realize a quantum spin liquid
journal, August 2017

Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3
journal, January 2020

Antiferromagnetic Resonance and Terahertz Continuum in $α − {RuCl}_{3}$
journal, November 2017

Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in $α − {RuCl}_{3}$
journal, November 2017

Thermodynamic Perspective on Field-Induced Behavior of $α − {RuCl}_{3}$
journal, August 2020

Thermal Pure Quantum States at Finite Temperature
journal, June 2012

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016

Crystal structure and magnetism in $α - {RuCl}_{3}$ : An ab initio study
journal, April 2016

Equation of State Calculations by Fast Computing Machines
journal, June 1953

Deriving models for the Kitaev spin-liquid candidate material $α − {RuCl}_{3}$ from first principles
journal, August 2019

Polarization-resolved Raman spectroscopy of $α − {RuCl}_{3}$ and evidence of room-temperature two-dimensional magnetic scattering
journal, October 2019

Nesting instability of gapless U(1) spin liquids with spinon Fermi pockets in two dimensions
journal, October 2021

Effective model with strong Kitaev interactions for $α − {RuCl}_{3}$
journal, April 2018

Thermodynamic evidence for a field-angle-dependent Majorana gap in a Kitaev spin liquid
journal, January 2022

Theoretical investigation of magnetic dynamics in $α - {RuCl}_{3}$
journal, September 2017

Low-temperature crystal and magnetic structure of $α - {RuCl}_{3}$
journal, April 2016

Rethinking $α − {RuCl}_{3}$
journal, July 2020

Electrical Probes of the Non-Abelian Spin Liquid in Kitaev Materials
journal, July 2020

Terahertz excitations in $α − RuC l_{3}$ : Majorana fermions and rigid-plane shear and compression modes
journal, September 2019

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016

Spin liquids in frustrated magnets
journal, March 2010

Concept and realization of Kitaev quantum spin liquids
journal, March 2019

Anyons in an exactly solved model and beyond
journal, January 2006

Monoclinic crystal structure of $α - {RuCl}_{3}$ and the zigzag antiferromagnetic ground state
journal, December 2015

Fermionic response from fractionalization in an insulating two-dimensional magnet
journal, July 2016

The range of non-Kitaev terms and fractional particles in α-RuCl3
journal, March 2020

The Spallation Neutron Source in Oak Ridge: A powerful tool for materials research
journal, November 2006

Unusual Thermal Hall Effect in a Kitaev Spin Liquid Candidate $α − {RuCl}_{3}$
journal, May 2018

Magnetic order in $α - {RuCl}_{3}$ : A honeycomb-lattice quantum magnet with strong spin-orbit coupling
journal, April 2015

Machine learning for magnetic phase diagrams and inverse scattering problems
journal, November 2021

Evidence for Magnetic Fractional Excitations in a Kitaev Quantum-Spin-Liquid Candidate α-RuCl ₃
journal, February 2022

Physics of the Kitaev Model: Fractionalization, Dynamic Correlations, and Material Connections
journal, March 2018

Half-integer quantized anomalous thermal Hall effect in the Kitaev material candidate α-RuCl ₃
journal, July 2021

Neutron scattering in the proximate quantum spin liquid α-RuCl ₃
journal, June 2017

Magnetic thermal conductivity far above the Néel temperature in the Kitaev-magnet candidate $α − {RuCl}_{3}$
journal, June 2017

Revealing the phase diagram of Kitaev materials by machine learning: Cooperation and competition between spin liquids
journal, April 2021

Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit
journal, February 2014

Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid
journal, July 2018

Corelli: Efficient single crystal diffraction with elastic discrimination
journal, October 2008

Hunting Majorana Fermions in Kitaev Magnets
journal, January 2020

Machine-learning-assisted insight into spin ice Dy2Ti2O7
journal, February 2020

Majorana fermions in the Kitaev quantum spin system α-RuCl3
journal, September 2017

Nature of Magnetic Excitations in the High-Field Phase of $α − {RuCl}_{3}$
journal, July 2020

Kitaev magnetism in honeycomb ${RuCl}_{3}$ with intermediate spin-orbit coupling
journal, June 2015

Machine learning on neutron and x-ray scattering and spectroscopies
journal, September 2021

Magnetic anisotropy in the Kitaev model systems ${Na}_{2} {IrO}_{3}$ and ${RuCl}_{3}$
journal, August 2016

Efficient Global Optimization of Expensive Black-Box Functions
journal, January 1998

Machine learning for quantum matter
journal, January 2020

SEQUOIA: A fine resolution chopper spectrometer at the SNS
journal, November 2006

Non-Abelian anyons and topological quantum computation
journal, September 2008