Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr

Magnetism in two-dimensional (2D) van der Waals (vdW) crystals offers promising new directions for low-dimensional physics and devices. In this work, mega-electron volt (MeV) ultrafast electron diffraction was employed to investigate the ultrafast atomic dynamics of a novel, 2D vdW magnetic single-c...

Full description

Saved in:
Bibliographic Details
Main Authors: Jayajeewana N. Ranhili, Sumit Khadka, Junjie Li, John Cenker, Alberto M. Ruiz, Andrei Shumilin, José J. Baldoví, Ka Shen, Mikhail Fedurin, Mark Palmer, Daniel G. Chica, Paul Byaruhanga, Shuo Chen, Xiaodong Xu, Xavier Roy, Byron Freelon
Format: Article
Language:English
Published: AIP Publishing LLC and ACA 2025-03-01
Series:Structural Dynamics
Online Access:http://dx.doi.org/10.1063/4.0000266
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1850205190436683776
author Jayajeewana N. Ranhili
Sumit Khadka
Junjie Li
John Cenker
Alberto M. Ruiz
Andrei Shumilin
José J. Baldoví
Ka Shen
Mikhail Fedurin
Mark Palmer
Daniel G. Chica
Paul Byaruhanga
Shuo Chen
Xiaodong Xu
Xavier Roy
Byron Freelon
author_facet Jayajeewana N. Ranhili
Sumit Khadka
Junjie Li
John Cenker
Alberto M. Ruiz
Andrei Shumilin
José J. Baldoví
Ka Shen
Mikhail Fedurin
Mark Palmer
Daniel G. Chica
Paul Byaruhanga
Shuo Chen
Xiaodong Xu
Xavier Roy
Byron Freelon
author_sort Jayajeewana N. Ranhili
collection DOAJ
description Magnetism in two-dimensional (2D) van der Waals (vdW) crystals offers promising new directions for low-dimensional physics and devices. In this work, mega-electron volt (MeV) ultrafast electron diffraction was employed to investigate the ultrafast atomic dynamics of a novel, 2D vdW magnetic single-crystal CrSBr. Femtosecond (fs) optical pump pulses excited non-equilibrium atomic displacements shown to be coherent acoustic phonons (CAPs). Phonon frequencies were extracted by analyzing oscillations of different Bragg peak (BP) intensities and were determined to be GHz acoustic disturbances that propagated as strain waves. Phonon modes exhibit anisotropy with respect to the a and b crystal axes. Subharmonic phonon frequencies were also observed, and this provided a signature of nonlinear oscillatory coupling between the laser-induced pumping phonon frequency and secondary phonon frequencies. Thus, CrSBr was found to serve as a nonlinear phononic frequency converter. The ultrafast time dependence of the Bragg intensity was simulated by incorporating an oscillating deviation parameter ansatz into expressions for the dynamical scattering intensity yielded excellent modeling of the ultrafast structural dynamics of the photo-excited 2D crystal. Our work provides a foundation for exploring how fs light pulses can influence phonon dynamics in materials with strong spin-lattice coupling. These results suggest that CAPs can match the magnon frequencies and show the promise of CrSBr for use in optical-to-microwave transducers and phononic devices.
format Article
id doaj-art-171ac2fedcb14cae981a98f2bd166d64
institution OA Journals
issn 2329-7778
language English
publishDate 2025-03-01
publisher AIP Publishing LLC and ACA
record_format Article
series Structural Dynamics
spelling doaj-art-171ac2fedcb14cae981a98f2bd166d642025-08-20T02:11:09ZengAIP Publishing LLC and ACAStructural Dynamics2329-77782025-03-01122024501024501-1110.1063/4.0000266Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBrJayajeewana N. Ranhili0Sumit Khadka1Junjie Li2John Cenker3Alberto M. Ruiz4Andrei Shumilin5José J. Baldoví6Ka Shen7Mikhail Fedurin8Mark Palmer9Daniel G. Chica10Paul Byaruhanga11Shuo Chen12Xiaodong Xu13Xavier Roy14Byron Freelon15Physics Department and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204, USAPhysics Department and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204, USAAccelerator Test Facility, Brookhaven National Laboratory, Upton, New York 11973, USAPhysics Department, University of Washington, Seattle, Washington 98195, USAInstituto de Ciencia Molecular (ICMol), University of Valencia, Valencia, SpainInstituto de Ciencia Molecular (ICMol), University of Valencia, Valencia, SpainInstituto de Ciencia Molecular (ICMol), University of Valencia, Valencia, SpainThe Center for Advanced Quantum Studies and Department of Physics, Beijing Normal University, Beijing 100875, ChinaAccelerator Test Facility, Brookhaven National Laboratory, Upton, New York 11973, USAAccelerator Test Facility, Brookhaven National Laboratory, Upton, New York 11973, USAChemistry Department, Columbia University, New York, New York 10027, USAPhysics Department and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204, USAPhysics Department and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204, USAPhysics Department, University of Washington, Seattle, Washington 98195, USAChemistry Department, Columbia University, New York, New York 10027, USAPhysics Department and Texas Center for Superconductivity, University of Houston, Houston, Texas 77204, USAMagnetism in two-dimensional (2D) van der Waals (vdW) crystals offers promising new directions for low-dimensional physics and devices. In this work, mega-electron volt (MeV) ultrafast electron diffraction was employed to investigate the ultrafast atomic dynamics of a novel, 2D vdW magnetic single-crystal CrSBr. Femtosecond (fs) optical pump pulses excited non-equilibrium atomic displacements shown to be coherent acoustic phonons (CAPs). Phonon frequencies were extracted by analyzing oscillations of different Bragg peak (BP) intensities and were determined to be GHz acoustic disturbances that propagated as strain waves. Phonon modes exhibit anisotropy with respect to the a and b crystal axes. Subharmonic phonon frequencies were also observed, and this provided a signature of nonlinear oscillatory coupling between the laser-induced pumping phonon frequency and secondary phonon frequencies. Thus, CrSBr was found to serve as a nonlinear phononic frequency converter. The ultrafast time dependence of the Bragg intensity was simulated by incorporating an oscillating deviation parameter ansatz into expressions for the dynamical scattering intensity yielded excellent modeling of the ultrafast structural dynamics of the photo-excited 2D crystal. Our work provides a foundation for exploring how fs light pulses can influence phonon dynamics in materials with strong spin-lattice coupling. These results suggest that CAPs can match the magnon frequencies and show the promise of CrSBr for use in optical-to-microwave transducers and phononic devices.http://dx.doi.org/10.1063/4.0000266
spellingShingle Jayajeewana N. Ranhili
Sumit Khadka
Junjie Li
John Cenker
Alberto M. Ruiz
Andrei Shumilin
José J. Baldoví
Ka Shen
Mikhail Fedurin
Mark Palmer
Daniel G. Chica
Paul Byaruhanga
Shuo Chen
Xiaodong Xu
Xavier Roy
Byron Freelon
Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
Structural Dynamics
title Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
title_full Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
title_fullStr Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
title_full_unstemmed Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
title_short Ultrafast-induced coherent acoustic phonons in the two-dimensional magnet CrSBr
title_sort ultrafast induced coherent acoustic phonons in the two dimensional magnet crsbr
url http://dx.doi.org/10.1063/4.0000266
work_keys_str_mv AT jayajeewananranhili ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT sumitkhadka ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT junjieli ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT johncenker ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT albertomruiz ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT andreishumilin ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT josejbaldovi ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT kashen ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT mikhailfedurin ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT markpalmer ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT danielgchica ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT paulbyaruhanga ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT shuochen ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT xiaodongxu ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT xavierroy ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr
AT byronfreelon ultrafastinducedcoherentacousticphononsinthetwodimensionalmagnetcrsbr