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Register a new userDetection of squeezed phonons in pump-probe spectroscopy
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Robust engineering of phonon squeezed states in optically excited solids has emerged as a promising tool to control and manipulate their properties. However, in contrast to quantum optical systems, detection of phonon squeezing is subtle and elusive, and an important question is what constitutes an unambiguous signature of it. The state of the art involves observing oscillations at twice the phonon frequency in time resolved measurements of the out of equilibrium phonon fluctuation. Using Keldysh formalism we show that such a signal is a necessary but not a sufficient signature of a squeezed phonon, since we identify several mechanisms that do not involve squeezing and yet which produce similar oscillations. We show that a reliable detection requires a time and frequency resolved measurement of the phonon spectral function.
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Time-resolved spectroscopies using intense THz pulses appear as a promising tool to address collective electronic excitations in condensed matter. In particular recent experiments showed the possibility to selectively excite collective modes emerging across a phase transition, as it is the case for superconducting and charge-density-wave (CDW) systems. One possible signature of these excitations is the emergence of coherent oscillations of the differential probe field in pump-probe protocols. While the analogy with the case of phonon modes suggests that the basic underlying mechanism should be a sum-frequency stimulated Raman process, a general theoretical scheme able to describe the experiments and to define the relevant optical quantity is still lacking. Here we provide this scheme by showing that coherent oscillations as a function of the pump-probe time delay can be linked to the convolution in the frequency domain between the squared pump field and a Raman-like non-linear optical kernel. This approach is applied and discussed in few paradigmatic examples: ordinary phonons in an insulator, and collective charge and Higgs fluctuations across a superconducting and a CDW transition. Our results not only account very well for the existing experimental data in a wide variety of systems, but they also offer an useful perspective to design future experiments in emerging materials.
In high-resolution core-valence-valence (CVV) Auger electron spectroscopy from the surface of a solid at thermal equilibrium, the main correlation satellite, visible in the case of strong valence-electron correlations, corresponds to a bound state of the two holes in the final state of the CVV Auger process. We discuss the physical significance of this satellite in nonequilibrium pump-probe Auger spectroscopy by numerical analysis of a single-band Hubbard-type model system including core states and a continuum of high-energy scattering states. It turns out that the spectrum of the photo-doped system, due to the increased double occupancy, shares features with the equilibrium spectrum at higher fillings. The pumping of doublons can be watched when working with overlapping pulses at short $Delta t$. For larger pump-probe delays $Delta t$ and on the typical femtosecond time scale for electronic relaxation processes, spectra are hardly $Delta t$-dependent, reflecting the high stability of bound two-hole states for strong Hubbard-$U$. We argue that taking into account the spatial expansion of single-particle orbitals when these are doubly occupied, as described by the dynamical Hubbard model, produces an oscillation of the barycenter of the satellite as a function of $Delta t$. Pump-probe Auger-electron spectroscopy is thus highly sensitive to dynamical screening of the Coulomb interaction.
We study the role of excited phonon populations in the relaxation rates of nonequilibrium electrons using a nonequilibrium Greens function formalism. The transient modifications in the phononic properties are accounted for by self-consistently solving the Dyson equation for the electron and phonon Greens functions. The pump induced changes manifest in both the electronic and phononic spectral functions. We find that the excited phonon populations suppress the decay rates of nonequilibrium electrons due to enhanced phonon absorption. The increased phonon occupation also sets the nonequilibrium decay rates and the equilibrium scattering rates apart. The decay rates are found to be time-dependent, and this is illustrated in the experimentally observed population decay of photoexcited $mathrm{Bi}_{1.5}mathrm{Sb}_{0.5} mathrm{Te}_{1.7}mathrm{Se}_{1.3}$.
We report the detection of a magnetic resonance mode in multiferroic Ba0.6Sr1.4Zn2Fe12O22 using time domain pump-probe reflectance spectroscopy. Magnetic sublattice precession is coherently excited via picosecond thermal modification of the exchange energy. Importantly, this precession is recorded as a change in reflectance caused by the dynamic magnetoelectric effect. Thus, transient reflectance provides a sensitive probe of magnetization dynamics in materials with strong magnetoelectric coupling, such as multiferroics, revealing new possibilities for application in spintronics and ultrafast manipulation of magnetic moments.
Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some technical details related to the perturbative derivation of the photoemission spectra, which involve processes where the pump pulse photoexcites electrons due to nonequilibrium effects.
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