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

Ranhili, Jayajeewana N.; Khadka, Sumit; Li, Junjie; Cenker, John; Ruiz, Alberto M.; Shumilin, Andrei; Baldoví, José J.; Shen, Ka; Fedurin, Mikhail; Palmer, Mark; Chica, Daniel G.; Byaruhanga, Paul; Chen, Shuo; Xu, Xiaodong; Roy, Xavier; Freelon, Byron

doi:10.1063/4.0000266

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

Journal Article · Thu Mar 20 00:00:00 EDT 2025 · Structural Dynamics

DOI:https://doi.org/10.1063/4.0000266· OSTI ID:2533591

; ; ; ; ; Shumilin, Andrei; ; ; ; ; ; Byaruhanga, Paul; ; ; ;

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0012704

OSTI ID:: 2533591

Alternate ID(s):: OSTI ID: 2555699

Journal Information:: Structural Dynamics, Journal Name: Structural Dynamics Journal Issue: 2 Vol. 12; ISSN 2329-7778

Publisher:: American Institute of PhysicsCopyright Statement

Country of Publication:: United States

Language:: English

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