Abstract:The photoemission spectrum of graphite is still debated. To help resolve this issue, we present photoemission measurements at high photon energy and analyze the results using a Green's function approach that takes into account the full complexity of the loss spectrum. Our measured data show multiple satellite replicas. We demonstrate that these satellites are of intrinsic origin, enhanced by extrinsic losses. The dominating satellite is due to the π + σ plasmon of graphite, whereas the π plasmon creates a tail… Show more
“…If now the spectral width is still smaller than the spacing to socalled satellite peaks at lower energies, e.g., ( − , ), the plasmon-loss peaks displaced by ( ), the energy of the bulk (surface) plasmon excitation, relative timing information on the emission of the main line and the satellite lines becomes accessible. One of the still widely open issues is as to what extent theses satellite features are intrinsic or extrinsic (Aryasetiawan et al, 1996;Guzzo et al, 2014). The notion of plasmon excitation, intrinsically linked to the photoemission, can be viewed as the direct condensed-matter analogue to the atomic shakeup correlation satellites (Section V).…”
Section: Time-resolved Photoemission From Surfacesmentioning
Recent advances in the generation of well characterized sub-femtosecond laser pulses have opened up unpredicted opportunities for the real-time observation of ultrafast electronic dynamics in matter. Such attosecond chronoscopy allows a novel look at a wide range of fundamental photophysical and photochemical processes in the time domain, including Auger and autoionization processes, photoemission from atoms, molecules, and surfaces, complementing conventional energy-domain spectroscopy. Attosecond chronoscopy raises fundamental conceptual and theoretical questions as which novel information becomes accessible and which dynamical processes can be controlled and steered. These questions are currently a matter of lively debate which we address in this review. We will focus on one prototypical case, the chronoscopy of the photoelectric effect by attosecond streaking. Is photoionization instantaneous or is there a finite response time of the electronic wavefunction to the photoabsorption event? Answers to this question turn out to be far more complex and multi-faceted than initially thought. They touch upon fundamental issues of time and time delay as observables in quantum theory. We review recent progress of our understanding of time-resolved photoemission from atoms, molecules, and solids. We will highlight the unresolved and open questions and we point to future directions aiming at the observation and control of electronic motion in more complex nanoscale structures and in condensed matter.
“…If now the spectral width is still smaller than the spacing to socalled satellite peaks at lower energies, e.g., ( − , ), the plasmon-loss peaks displaced by ( ), the energy of the bulk (surface) plasmon excitation, relative timing information on the emission of the main line and the satellite lines becomes accessible. One of the still widely open issues is as to what extent theses satellite features are intrinsic or extrinsic (Aryasetiawan et al, 1996;Guzzo et al, 2014). The notion of plasmon excitation, intrinsically linked to the photoemission, can be viewed as the direct condensed-matter analogue to the atomic shakeup correlation satellites (Section V).…”
Section: Time-resolved Photoemission From Surfacesmentioning
Recent advances in the generation of well characterized sub-femtosecond laser pulses have opened up unpredicted opportunities for the real-time observation of ultrafast electronic dynamics in matter. Such attosecond chronoscopy allows a novel look at a wide range of fundamental photophysical and photochemical processes in the time domain, including Auger and autoionization processes, photoemission from atoms, molecules, and surfaces, complementing conventional energy-domain spectroscopy. Attosecond chronoscopy raises fundamental conceptual and theoretical questions as which novel information becomes accessible and which dynamical processes can be controlled and steered. These questions are currently a matter of lively debate which we address in this review. We will focus on one prototypical case, the chronoscopy of the photoelectric effect by attosecond streaking. Is photoionization instantaneous or is there a finite response time of the electronic wavefunction to the photoabsorption event? Answers to this question turn out to be far more complex and multi-faceted than initially thought. They touch upon fundamental issues of time and time delay as observables in quantum theory. We review recent progress of our understanding of time-resolved photoemission from atoms, molecules, and solids. We will highlight the unresolved and open questions and we point to future directions aiming at the observation and control of electronic motion in more complex nanoscale structures and in condensed matter.
“…Moreover, strong modulation of the carrier density through ultrafast optical excitation and the ensuing hot carrier multiplication drives the electron and hole distributions to different chemical potentials, enabling applications in energy harvesting, ultrafast electronics, and coherent optics [1,3,[16][17][18][19][20]. These novel properties derive from graphene's Dirac fermion band structure, weak screening, and strong, moleculelike electron correlation [21][22][23][24][25][26][27][28][29][30][31], which distinguish it from conventional metals and semiconductors [22,32,33].…”
Electronic heating of cold crystal lattices in nonlinear multiphoton excitation can transiently alter their physical and chemical properties. In metals where free electron densities are high and the relative fraction of photoexcited hot electrons is low, the effects are small, but in semimetals, where the free electron densities are low and the photoexcited densities can overwhelm them, the intense femtosecond laser excitation can induce profound changes. In semimetal graphite and its derivatives, strong optical absorption, weak screening of the Coulomb potential, and high cohesive energy enable extreme hot electron generation and thermalization to be realized under femtosecond laser excitation. We investigate the nonlinear interactions within a hot electron gas in graphite through multiphoton-induced thermionic emission. Unlike the conventional photoelectric effect, within about 25 fs, the memory of the excitation process, where resonant dipole transitions absorb up to eight quanta of light, is erased to produce statistical Boltzmann electron distributions with temperatures exceeding 5000 K; this ultrafast electronic heating causes thermionic emission to occur from the interlayer band of graphite. The nearly instantaneous thermalization of the photoexcited carriers through Coulomb scattering to extreme electronic temperatures characterized by separate electron and hole chemical potentials can enhance hot electron surface femtochemistry, photovoltaic energy conversion, and incandescence, and drive graphite-to-diamond electronic phase transition.
“…This is achieved by the GW plus cumulant (GW+C) approach [13,14], where the cumulant expansion of the electron Green's function G is truncated at second order in the screened Coulomb interaction W . GW+C calculations yielded good agreement with experimental photoemission and tunneling spectra in a wide range of physical systems [6][7][8][15][16][17] and also with highly accurate coupled-cluster Green's function calculations [18]. While Green's function methods, such as the GW+C approach, often produce highly accurate results, gaining intuition and insights into the underlying manybody processes can be difficult.…”
mentioning
confidence: 77%
“…Such plasmon satellites have long been known in core-electron photoemission spectra [4,5]. In recent years, valence band plasmon satellites, which were observed experimentally in three-dimensional metals and semiconductors [6][7][8][9], but also in two-dimensional systems, such as doped graphene and semiconductor quantum-well electron gases [10][11][12], received much attention.…”
Using state-of-the-art many-body Green's function calculations based on the "GW plus cumulant" approach, we analyze the properties of plasmon satellites in the electron spectral function resulting from electron-plasmon interactions in one-, two-and three-dimensional systems. Specifically, we show how their dispersion relation, lineshape and linewidth are related to the properties of the constituent electrons and plasmons. To gain insight into the many-body processes giving rise to the formation of plasmon satellites, we connect the "GW plus cumulant" approach to a many-body wavefunction picture of electron-plasmon interactions and introduce the coupling-strength weighted electron-plasmon joint-density states as a powerful concept for understanding plasmon satellites.
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