We present a flexible and efficient ultrafast time-resolved spontaneous Raman spectroscopy setup to study collective excitation and quasi-particle dynamics in quantum materials. 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 an 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 materials.

Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications in nano-electronics. In this work, we study the incoherent optical phonon and exciton population dynamics in monolayer WS2 by timeresolved spontaneous Raman scattering spectroscopy. Upon excitation of the exciton transition, both the Stokes and anti-Stokes optical phonon scattering strength exhibit a large reduction. Based on the detailed balance, the optical phonon population is retrieved, which shows an instant buildup and a relaxation lifetime of ~4 ps at an exciton density ~10 12 cm -2 . The corresponding optical phonon temperature rises by 25 K, eventually, after some 10's of picoseconds, leading to a lattice heating by only ~3 K. The exciton relaxation dynamics extracted from the transient vibrational Raman response shows a strong excitation density dependence, signaling an important bimolecular contribution to the decay. The exciton relaxation rate is found to be ~ (70 ps) -1 and exciton-exciton annihilation rate ~0.1 cm 2 s -1 . These results provide valuable insight into the thermal dynamics after optical excitation and enhance the understanding of the fundamental exciton dynamics in two-dimensional transition metal materials.

Cu4 triplet clusters form the relevant spin entity for the formation of long-range magnetic order in the cluster magnet Cu2OSeO3. Using time-resolved Raman spectroscopy, we probed photoinduced spin and lattice dynamics in this Mott insulator. Multiple ps-decade spin-lattice relaxation dynamics is observed, evidencing a separation of the order parameter dynamics into disordering of long-range and internal spin cluster order. Our study exemplifies the double order parameter dynamics of generalized molecular crystals of charge, spin, and orbital nature.

Clusters of single spins form the relevant spin entities in the formation of long-range magnetic order in spin cluster Mott insulators. Such type of spin order bears resemblance to molecular crystals, and we therefore may expect a prototypical spin wave spectrum which can be divided into low-energy external and high-energy internal cluster spin wave modes. Here, we study high-energy spin cluster excitations in the spin cluster Mott insulator Cu2OSeO3 by means of spontaneous Raman scattering. Multiple high-energy optical magnon modes are observed, of which the Raman-activity is shown to originate in the Elliot-Loudon scattering mechanism. Upon crossing the long-range ordering transition temperature the magnetic modes significantly broaden, corresponding to scattering from localized spin excitations within the spin clusters. Different optical phonon modes show a strong temperature dependence, evidencing a strong magnetoelectric coupling between optical phonons and the high-energy spin cluster excitations. Our results support the picture that Cu2OSeO3 can be regarded as a solid-state molecular crystal of spin nature.