A tunable time-resolved spontaneous Raman spectroscopy setup for probing ultrafast collective excitation and quasiparticle dynamics in quantum materials

Abstract

We present a flexible and efficient ultrafast time-resolved spontaneous Raman spectroscopy setup to study collective excitation and quasi-particle dynamics in quantum matter. The setup has a broad energy tuning range extending from the visible to near infrared spectral regions for both the pump excitation and Raman probe pulses. Additionally, the balance between energy and time-resolution can be controlled. A high light collecting efficiency is realized by high numerical aperture collection optics and a high-throughput flexible spectrometer. We demonstrate the functionality of the setup with a study of the zone-center longitudinal optical phonon and hole continuum dynamics in silicon, and discuss the role of the Raman tensor in time-resolved Raman scattering. In addition, we show evidence for unequal phonon softening rates at different high symmetry points in the Brillouin zone of silicon by means of detecting pump-induced changes in the two-phonon overtone spectrum. Demagnetization dynamics in the helimagnet Cu2OSeO3 is studied by observing softening and broadening of a magnon after photo-excitation, underlining the unique power of measuring transient dynamics in the frequency domain, and the feasibility to study phase transitions in quantum matter.

16 pages, 6 figures, accepted for publication in AIP Publishing/ACA Structural Dynamics

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• Accessing Excited State Molecular Vibrations by Femtosecond Stimulated Raman Spectroscopy
• Incoherent phonon population and exciton-exciton annihilation in monolayer WS2 revealed by time-resolved spontaneous Raman scattering
• Dynamical resonance quench and Fano interference in spontaneous Raman scattering from quasiparticle and collective excitations
• Relaxation timescales and electron-phonon coupling in optically-pumped YBa${}_2$Cu${}_3$O${}_{6+x}$ revealed by time-resolved Raman scattering
• Time-domain study of coupled collective excitations in quantum materials
• Fingerprints of hot-phonon physics in time-resolved correlated quantum lattice dynamics
• Nonequilibrium dynamics of $\alpha$-RuCl${}_3$ -- a time-resolved magneto-optical spectroscopy study
• Ultrafast Raman thermometry in driven YBa${}_2$Cu${}_3$O${}_{6.48}$
• Coupled dynamics of long-range and internal spin cluster order in Cu${}_2$OSeO${}_3$
• A set-up for Hard X-ray Time-resolved Resonant Inelastic X-ray Scattering at SwissFEL
• Ultrafast Raman probe of the photoinduced superconducting to normal state transition in the cuprate Bi${}_2$Sr${}_2$CaCu${}_2$O${}_{8+\delta }$