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arXiv:1812.09222 · Physical review. B./Physical review. B

Noise correlations in time- and angle-resolved photoemission spectroscopy

Christopher Stahl, Martin Eckstein

Published Jun 20, 2019• 19 citations
arXivHTMLPDF

Abstract

In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultrashort pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent two-particle correlations in the solid. This can extend the scope of time- and angle-resolved photoemission spectroscopy to probe superconducting and charge density fluctuations in systems without long-range order, and to reveal their dynamics independent of the electronic gap and thus unrestricted by the energy-time uncertainty. The proposal is illustrated for superconductivity in a BCS model. An impulsive perturbation can quench the gap on ultrafast timescales, while nonequilibrium pairing correlations persist much longer, even when electron-electron scattering beyond mean-field theory is taken into account. There is thus a clear distinction between a dephasing of the Cooper pairs and the thermalization into the normal state. While a measurement of the gap would be blind to such pairing correlations, they can be revealed by the angular correlations in photoemission.

DOI
10.1103/physrevb.99.241111

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In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultrashort pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent two-particle correlations in the solid. This can extend the scope of time- and angle-resolved photoemission spectroscopy to probe superconducting and charge density fluctuations in systems without long-range order, and to reveal their dynamics independent of the electronic gap and thus unrestricted by the energy-time uncertainty. The proposal is illustrated for superconductivity in a BCS model. An impulsive perturbation can quench the gap on ultrafast timescales, while nonequilibrium pairing correlations persist much longer, even when electron-electron scattering beyond mean-field theory is taken into account. There is thus a clear distinction between a dephasing of the Cooper pairs and the thermalization into the normal state. While a measurement of the gap would be blind to such pairing correlations, they can be revealed by the angular correlations in photoemission.
Time-resolved photoemission experiments can reveal fascinating quantum dynamics of correlated electrons. However, the thermalization of the electronic system is typically so fast that very short probe pulses are necessary to resolve the time evolution of the quantum state, and this leads to poor energy resolution due to the energy-time uncertainty relation. Although the photoemission intensity can be calculated from the nonequilibrium electronic Green's functions, the converse procedure is therefore difficult. We analyze a hypothetical time-resolved photoemission experiment on a correlated electronic system, described by the Falicov-Kimball model in dynamical mean-field theory, which relaxes between metallic and insulating phases. We find that the real-time Green's function which describes the transient behavior during the buildup of the metallic state cannot be determined directly from the photoemission signal. On the other hand, the characteristic collapse-and-revival oscillations of an excited Mott insulator can be observed as oscillating weight in the center of the Mott gap in the time-dependent photoemission spectrum.
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This thesis is about unconventional superconductors out of equilibrium. More precisely, it summarizes our theoretical efforts in addressing a few questions related to the real-time evolution in models displaying unconventional superconductivity. Apart from the purely theoretical interest, the motivation for these studies comes from the recent achievement in the field of ultrafast time-resolved spectroscopy on correlated materials, such as the high-temperature copper-oxide superconductors. The task of describing such systems in nonequilibrium is a very difficult one. In this thesis we attack the problem from two different points of view: • the anisotropic unconventional d-wave symmetry, • the strong electron-electron correlations. The thesis is organized as follows: The first part introduces the basic concepts which lay at the foundation of the work presented in the other two parts. In Chapter 1, the concept of unconventional superconductivity is briefly introduced. This mainly includes the high-temperature copper-oxide superconductors and their phenomenology: d-wave symmetry of the super- conducting gap and strong electron-electron interaction. Chapter 2 is devoted to a review of the recent experimental advances in the field of ultrafast spectroscopy of high temperature superconductors and correlated materials, with a particular focus on time- and angle- resolved photoemission spectroscopy. Finally, Chapter 3 is a short review of some works in the field of cold-atom Fermi gases. In the second part we address the physics of the d-wave superconductor after a sudden excitation. First, in Chapter 4 we introduce in some detail a model of mean-field superconductor with a d-wave symmetry. The principal feature of this model is the anisotropy of the gap and the nodal lines along which the gap vanishes. The results concerning the dynamics of the gap after a “quantum quench” are exposed in Chapter 5 where we compare our model to the s-wave superconductor. This comparison allows to identify the consequences of the unconventional symmetry. In Chapter 6 we discuss the spectral features of the transient nonequilibrium state of the d-wave superconductor. This is particularly important to move a first step towards photoemission experiments. In the third part we concentrate on the attractive Hubbard model as a prototype of strongly correlated superconductor. In Chapter 8 we discuss the superconducting state at equilibrium with the use of dynamical mean-field theory. In Chapter 9 we discuss the extension of this technique to systems out of equilibrium. In particular it is described the implementation in the superconducting phase. At the end of the thesis two appendices give some details of the calculations.
The energy-time uncertainty is an intrinsic limit for time-resolved experiments imposing a tradeoff between the duration of the light pulses used in experiments and their frequency content. In standard time-resolved photoemission, this limitation maps directly onto a tradeoff between the time resolution of the experiment and the energy resolution that can be achieved on the electronic spectral function. Here we propose a protocol to disentangle the energy and time resolutions in photoemission. We demonstrate that dynamical information on all time scales can be retrieved from time-resolved photoemission experiments using suitably shaped light pulses of quantum or classical nature. As a paradigmatic example, we study the dynamical buildup of the Kondo peak, a narrow feature in the electronic response function arising from the screening of a magnetic impurity by the conduction electrons. After a quench, the electronic screening builds up on timescales shorter than the inverse width of the Kondo peak and we demonstrate that the proposed experimental scheme could be used to measure the intrinsic time scales of such electronic screening. The proposed approach provides an experimental framework to access the nonequilibrium response of collective electronic properties beyond the spectral uncertainty limit and will enable the direct measurement of phenomena such as excited Higgs modes and, possibly, the retarded interactions in superconducting systems.
In order to understand the effects of electron-phonon coupling and Coulomb interactions in angle-resolved photoemission spectroscopy (ARPES), a spin-1/2 Hubbard-Holstein model at half-filling is theoretically investigated by means of the mean field theory and classical Monte Carlo simulation method. It shows that the spectral shape of the one-dimensional system is significantly modified by the electron-phonon coupling and Coulomb interactions. The suppression of charge-density wave in one-dimensional system has been ascribed to the short-range Coulomb repulsion and thermal lattice fluctuations. The competition between these interactions can induce zero energy gaps in APPES as well as complete cancellation of charge or spin ordering.
The ability to study ultracold atomic Fermi gases holds the promise of significant advances in testing fundamental theories of many-body quantum physics. Of particular interest are strongly interacting Fermi gases in the BCS to BEC crossover that exhibit a transition to a superfluid state at temperatures near 0.2TF , where TF is the Fermi temperature. This transition, as a fraction of TF, is extremely high compared to any known superfluid or superconductor. These gases are also in a universal regime where the physics is independent of the details of the atomic interactions and is therefore relevant to fields as diverse as condensed matter, nuclear physics and astrophysics. In this thesis, I present an experimental probe of atomic gases that uses momentum-resolved RF spectroscopy to realize an analog of angle-resolved photoemission spectroscopy (ARPES) in materials. This measurement reveals the energy and momentum of single-particle states in the strongly interacting Fermi gas. In condensed matter, ARPES has proved to be one of the most powerful experimental techniques for studying the electronic structure of strongly correlated electron materials. The ability to perform analogous measurements in ultracold Fermi gases constitutes a significant advance in our ability to directly connect ultracold atomic gases to strongly correlated electron systems. Taking advantage of this new measurement technique, I investigate a long-standing problem in the field of strongly interacting fermions, namely whether a pseudogap state consisting of incoherent fermion pairs exists at temperatures above the critical temperature for superfluidity. The photoemission data I present provide strong evidence for this state and have implications for fundamental theories of strongly interacting Fermi gases and strongly correlated electron materials. I also discuss the experimental confirmation of recently predicted universal relations for strongly interacting Fermi gases, as well as some of the first experiments involving atomic Fermi gases with p-wave pairing.