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Register a new userDynamical resonance quench and Fano interference in spontaneous Raman scattering from quasiparticle and collective excitations
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Time-resolved spontaneous Raman spectroscopy serves as a probe for incoherent quasiparticle and collective excitation dynamics, and allows to distinguish symmetry changes across a photoinduced phase transition through the inelastic light scattering selection rules. Largely unexplored is the role of the Raman resonance enhancement in the time-domain, and the transient interaction between scattering from quasiparticles and collective excitations, with the latter interaction leading to a Fano interference. In this work, we report on the observation of a phonon Raman tensor quench and Fano interference after strong photoexcitation of an intrinsic semiconductor. We observed a dynamic phonon scattering rate asymmetry and spectral asymmetry through simultaneous detection of both the anti-Stokes and Stokes response. The asymmetric phonon scattering rate is ascribed to the combined effect of the transient phonon population and the reduction of the phonon Raman tensor resulting from the photoexcited hole population. This same hole population results in a strong enhancement of the Fano spectral asymmetry.
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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.
The temperature effect on the Raman scattering efficiency is investigated in $varepsilon$-GaSe and $gamma$-InSe crystals. We found that varying the temperature over a broad range from 5 K to 350 K permits to achieve both the resonant conditions and the antiresonance behaviour in Raman scattering of the studied materials. The resonant conditions of Raman scattering are observed at about 270 K under the 1.96 eV excitation for GaSe due to the energy proximity of the optical band gap. In the case of InSe, the resonant Raman spectra are apparent at about 50 K and 270 K under correspondingly the 2.41 eV and 2.54 eV excitations as a result of the energy proximity of the mbox{so-called} B transition. Interestingly, the observed resonances for both materials are followed by an antiresonance behaviour noticeable at higher temperatures than the detected resonances. The significant variations of phonon-modes intensities can be explained in terms of electron-phonon coupling and quantum interference of contributions from different points of the Brillouin zone
A valley degree of freedom (DOF) in transition metal dichalcogenides with broken inversion symmetry can be controlled through spin and orbital DOFs owing to their valley-contrasting characters. Another important aspect of the spin and orbital DOFs is that they affect quasiparticle scattering processes that govern the valley lifetime. Here we combine quasiparticle-interference (QPI) imaging experiments and theoretical simulations to study the roles of the spin and orbital DOFs in 3R-NbS2. We find that the QPI signal arising from an inter-valley scattering is noticeably weaker than that caused by an intra-valley scattering. We show that this behavior is predominantly associated with the orbital DOF, signifying the different spin and orbital structures of spin-split bands at each valley. These findings provide important insights into understanding the valley-related transport properties.
The nanofabrication technology has taught us that an $m$-dimensional confining potential imposed upon an $n$-dimensional electron gas paves the way to a quasi-($n-m$)-dimensional electron gas, with $m le n$ and $1le n, m le 3$. This is the road to the (semiconducting) quasi-$n$ dimensional electron gas systems we have been happily traversing on now for almost three decades. Achieving quasi-one dimensional electron gas (Q-1DEG) [or quantum wire(s) for more practical purposes] led us to some mixed moments in this journey: while the reduced phase space for the scattering led us believe in the route to the faster electron devices, the proximity to the 1D systems left us in the dilemma of describing it as a Fermi liquid or as a Luttinger liquid. No one had ever suspected the potential of the former, but it took quite a while for some to convince the others on the latter. A realistic Q-1DEG system at the low temperatures is best describable as a Fermi liquid rather than as a Luttinger liquid. In the language of condensed matter physics, a critical scrutiny of Q-1DEG systems has provided us with a host of exotic (electronic, optical, and transport) phenomena revealing their unparallel behavior characteristics unseen in their higher or lower dimensional counterparts. Here, we embark on the systematic investigation of the inelastic electron scattering (IES) and of inelastic light scattering (ILS) from the elementary electronic excitations in quantum wires in the absence of an applied magnetic field. To that end, we begin with the Kubos correlation functions to derive the generalized nonlocal, dynamic dielectric function, the inverse dielectric function, and the Dyson equation for the dynamic screened potential in the framework of Bohm-Pines full and famous random-phase approximation...
The cuprate high-temperature superconductors are known to host a wide array of effects due to interactions and disorder. In this work, we look at some of the consequences of these effects which can be visualized by scanning tunneling spectroscopy. These interaction and disorder effects can be incorporated into a mean-field description by means of a self-energy appearing in the Greens function. We first examine the quasiparticle scattering interference spectra in the superconducting state at optimal doping as temperature is increased. Assuming agreement with angle-resolved photoemission experiments which suggest that the scattering rate depends on temperature, resulting in the filling of the $d$-wave gap, we find that the peaks predicted by the octet model become progressively smeared as temperature is increased. When the scattering rate is of the same order of magnitude as the superconducting gap, the spectral function shows Fermi-arc-like patterns, while the power spectrum of the local density of states shows the destruction of the octet-model peaks. We next consider the normal state properties of the optimally-doped cuprates. We model this by adding a marginal Fermi liquid self-energy to the normal-state propagator, and consider the dependence of the QPI spectra on frequency, temperature, and doping. We demonstrate that the MFL self-energy leads to a smearing of the caustics appearing in the normal-state QPI power spectrum as either temperature or frequency is increased at fixed doping. The smearing is found to be more prominent in the MFL case than in an ordinary Fermi liquid. We also consider the case of a marginal Fermi liquid with a strongly momentum-dependent self-energy which gives rise to a visible nodal-antinodal dichotomy at the normal state, and discuss how the spectra as seen in ARPES and STS differ from both an isotropic metal and a broadened $d$-wave superconductor.
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