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Bulletin of the American Physical Society

Theory of Time-Resolved Raman Scattering in Correlated Systems: Ultrafast Engineering of Spin Dynamics and Detection of Thermalization

Cheng-Chien Chen, Yao Wang, Thomas Devereaux

Published Mar 5, 2019• 0 citations
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Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics, especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes and anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. Time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.
Memory-assisted quantum networks require photon sources with controllable temporal and correlation properties. The Duan-Lukin-Cirac-Zoller (DLCZ) protocol provides a platform based on spontaneous Raman scattering in atomic ensembles, but a unified predictive theory connecting control parameters to correlations under realistic propagation and noise conditions remains lacking. Here we present a propagation-inclusive open-system quantum theory that retains write-induced population redistribution while combining Heisenberg-Langevin dynamics with Maxwell-Schrödinger propagation. We experimentally validate its key predictions. The theory predicts time-dependent Stokes generation, spin-wave evolution, retrieved anti-Stokes wavepackets, and time-resolved cross-correlations. Experiments confirm robust correlations under retrieval tuning and enhanced correlations for shorter write pulses, consistent with the different scaling of correlated coincidences and accidental backgrounds with the mean spin-wave excitation number. Classically controlled retrieval enables temporal gating and slicing of the anti-Stokes wavepacket, establishing a quantitative framework for correlation engineering in memory-compatible DLCZ photon sources.
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $\sim$50fs. The heterodyne-detected Raman signal is further developed to capture the phases of electronic coherence and emission in real-time domain.