5,237 research outputs found
Measurement of the dynamic charge response of materials using low-energy, momentum-resolved electron energy-loss spectroscopy (M-EELS)
One of the most fundamental properties of an interacting electron system is
its frequency- and wave-vector-dependent density response function, . The imaginary part, , defines the
fundamental bosonic charge excitations of the system, exhibiting peaks wherever
collective modes are present. quantifies the electronic compressibility
of a material, its response to external fields, its ability to screen charge,
and its tendency to form charge density waves. Unfortunately, there has never
been a fully momentum-resolved means to measure at the
meV energy scale relevant to modern elecronic materials. Here, we demonstrate a
way to measure with quantitative momentum resolution by applying
alignment techniques from x-ray and neutron scattering to surface
high-resolution electron energy-loss spectroscopy (HR-EELS). This approach,
which we refer to here as "M-EELS," allows direct measurement of with meV resolution while controlling the momentum with an accuracy
better than a percent of a typical Brillouin zone. We apply this technique to
finite-q excitations in the optimally-doped high temperature superconductor,
BiSrCaCuO (Bi2212), which exhibits several phonons
potentially relevant to dispersion anomalies observed in ARPES and STM
experiments. Our study defines a path to studying the long-sought collective
charge modes in quantum materials at the meV scale and with full momentum
control.Comment: 26 pages, 10 sections, 7 figures, and an appendi
Response theory for time-resolved second-harmonic generation and two-photon photoemission
A unified response theory for the time-resolved nonlinear light generation
and two-photon photoemission (2PPE) from metal surfaces is presented. The
theory allows to describe the dependence of the nonlinear optical response and
the photoelectron yield, respectively, on the time dependence of the exciting
light field. Quantum-mechanical interference effects affect the results
significantly. Contributions to 2PPE due to the optical nonlinearity of the
surface region are derived and shown to be relevant close to a plasmon
resonance. The interplay between pulse shape, relaxation times of excited
electrons, and band structure is analyzed directly in the time domain. While
our theory works for arbitrary pulse shapes, we mainly focus on the case of two
pulses of the same mean frequency. Difficulties in extracting relaxation rates
from pump-probe experiments are discussed, for example due to the effect of
detuning of intermediate states on the interference. The theory also allows to
determine the range of validity of the optical Bloch equations and of
semiclassical rate equations, respectively. Finally, we discuss how collective
plasma excitations affect the nonlinear optical response and 2PPE.Comment: 27 pages, including 11 figures, version as publishe
Electron Energy-Loss Spectroscopy: A versatile tool for the investigations of plasmonic excitations
The inelastic scattering of electrons is one route to study the vibrational
and electronic properties of materials. Such experiments, also called electron
energy-loss spectroscopy, are particularly useful for the investigation of the
collective excitations in metals, the charge carrier plasmons. These plasmons
are characterized by a specific dispersion (energy-momentum relationship),
which contains information on the sometimes complex nature of the conduction
electrons in topical materials. In this review we highlight the improvements of
the electron energy-loss spectrometer in the last years, summarize current
possibilities with this technique, and give examples where the investigation of
the plasmon dispersion allows insight into the interplay of the conduction
electrons with other degrees of freedom
Random-phase approximation and its applications in computational chemistry and materials science
The random-phase approximation (RPA) as an approach for computing the
electronic correlation energy is reviewed. After a brief account of its basic
concept and historical development, the paper is devoted to the theoretical
formulations of RPA, and its applications to realistic systems. With several
illustrating applications, we discuss the implications of RPA for computational
chemistry and materials science. The computational cost of RPA is also
addressed which is critical for its widespread use in future applications. In
addition, current correction schemes going beyond RPA and directions of further
development will be discussed.Comment: 25 pages, 11 figures, published online in J. Mater. Sci. (2012
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