To enable cutting edge science, the lab develops state of the art tabletop spectroscopy and microscopy techniques
and collaborates with
programs at LBNL's Advanced Light Source and the Molecular Foundry.
Angle-Resolved Photoemission Spectroscopy (ARPES) is an experimental technique
based on several refinements of the photoelectric effect initially observed by Heinrich Hertz
in 1887. When a monochromatic beam of photons of energy hν are incident upon a sample,
measurement of the electron's kinetic energy and exit angle gives information about the momentum and
energy ("band structure") of the electron state in the studied material.
Directly, ARPES gives the binding energy (Eb) of the emitted electrons and the
components of momentum parallel to the sample surface (k∥).
Crystalline translational symmetry is broken by the vacuum interface, so less
information is available for the out of plane momentum (kz)
without varying the incident photon energy.
Experiment
From simple energy and momentum conservation arguments, we can explain the process by which ARPES
makes available the electronic band structure. In typical ARPES experiments, a hemispherical energy analyzer
simultaneously measures the intensity distribution of photoelectrons along a one dimensional linecut
of angle—defined by an entrance slit on the analyzer—and resolved by the photoelectron kinetic energy.
Briefly, photoelectrons emitted from different angles (green, blue, and orange in the above depiction) are
incident at different locations on the entrance slit and follow different circular trajectories between
the analyzer plates. Meanwhile, more and less energetic electrons follow longer and shorter paths
(depicted as a spread in blue, green, and orange curves) due to their different bend radii in the constant E-field
produced by the analyzer. The analyzer therefore spatially filters the electrons to produce an image of the
photoemitted beam. A final electron sensitive detector, typically a channel plate paired with a phosphor
screen + CCD or delay line + timing hardware, turns the spatially filtered electron signal into a digital one.
If a photoemitted electron leaves the sample with an energy Ekin at
an angle (θ,ϕ) to the sample normal, z^, the
binding energy and k∥ are given by conservation:
Eb=knownhν−φ−measuredEkinp∥=2mEkinsinθ(cosϕx^+sinϕy^).
The sample workfunction φ, giving the different between the
Fermi and vacuum levels, may or may not be known. The Fermi edge of a metallic sample (actual or reference),
nevertheless links the kinetic energy to the electron binding energy.
By turning the sample, z^ can be rastered perpendicular
to the analyzer entrance, making available the photoemission intensity over all values
of k∥. Consideration must be given
to the difference between experimentally measured angles and the spherical polar angles relative to
z^.
To obtain high-quality data, ARPES experiments are conducted in an ultra-high vacuum
chamber which minimizes surface contamination and interactions between the photoemitted
electrons and any potential interference between the emission and detection processes.
Additionally, ARPES experiments are often performed at cryogenic temperatures to minimize
thermal broadening of the data. This capability also allows for the study of
high-temperature superconductors below their critical temperatures, where the electrons
take on a fundamentally different structure.
## Single + Many Body Physics
ARPES provides a direct measurement of the angle resolved photocurrent
I(k,ω). This can be expressed in terms of a
dipole interaction matrix element M, the Fermi-Dirac
distribution for state occupancy, and the single-particle spectral function A(k,ω):
I(k,ω)=M(k,ω,k⋅A)f(ω)A(k,ω).
Although matrix element contribution can in general be difficult to disentangle, it is typically
slowly varying in momentum and photon energy, and therefore ARPES can be thought of as measuring also
A(k,ω).
A(k,ω)=−π1[ω−Bare bandϵ0(k)−E-renormalizationΣ′(k,ω)]2+[LifetimesΣ′′(k,ω)]2Σ′′(k,ω)
From this quantity much can be extracted, including single-particle
band structure,
energy renormalization by interaction, and measurement
of the
quasiparticle lifetimes.
ARPES therefore makes available momentum resolved information on electron-electron and electron-boson
interaction in real material systems.
## Laser ARPES
From the conservation equations, we can see that given a fixed angular resolution of Δθ
of our analyzer, we may obtain a higher momentum resolution for smaller photoelectron kinetic energy,
Δk∝EkinΔθ.
UV and VUV lasers based on frequency doubling in BBO or KBBF and operating at very high photon fluxes with narrow spectral
linewidths of a few meV allow ARPES studies of materials at a much higher resolution than is possible
at synchrotron sources.
Pulsed laser sources also enable [ARPES studies of materials perturbed out of equilibrium](/tr-arpes) by a strong visible
to IR pulse, at the penalty of larger bandwidth Δν and therefore worse energy
resolution.
Spin-Resolved Photoemission Spectroscopy
In our laboratory we have developed a novel analyzer for Spin-ARPES experiments (see photo
at right). This analyzer employs a new concept for spin detection, based on a Time-of-Flight
analyzer (which is 10 times more efficient than dispersive analyzers) coupled with a
high-efficiency spin detector utilizing exchange scattering (about 50-100 times more
efficient for spin detection than using spin-orbit interaction as in Mott detectors).
Spin-ARPES is the only experimental tool that can directly probe the spin-resolved
bandstructure of materials. Our “Spin-TOF” system allows us to perform experiments with
energy resolution, momentum resolution, and collection efficiency unprecedented for a
Spin-ARPES system. It has been used at the Advanced Light Source for measurements in wide
energy and momentum ranges and with with the tabletop laser in our laboratory for high
resolution measurements.
The high efficiency of data collection allows for experimental scope never before possible
with spin resolution. For example, the spin-TOF system mapped the spin-dependence of the
bandstructure of Au(111) surface states, shown at right. These data, which would take
prohibitively long to accumulate on most spin-ARPES systems, were taken in just two hours.
The Spin-TOF system collects data rapidly enough to test a wide range of experimental
parameters such as sample temperature or photon polarization. It can be a crucial probe for
understanding topological insulators, Rashba systems, and magnetic materials.
Photoemission Microscopy
The technological frontier of our century lies in our ability to deal with very small samples (obtained by various combinations of 2D materials) or with quantum materials, where heterogeneity is the key to many of the novel observed behaviors.
Tools that provide spatial resolution, in addition to energy and are becoming a must to advance the frontier of this field.
In our laboratory we are developing a new ‘momentum space microscope’ that will allow us to measure energy and momentum of electrons in solids with nanometer spatial resolution.
The new spectrometer is based on an entirely new concept for microscopy and is posed to revolutionized our understanding of quantum materials while pushing the frontiers for novel technologies.
AI Driven Analysis and Acquisition
We developed PyARPES, an open data analysis toolkit and framework designed specifically for the workflows of angle-resolved photoemission spectroscopy. With PyARPES, scientists can integrate with industry standard libraries for machine learning and image processing, work with specialized models for ARPES, and automate typical workflows.
Terahertz and Mid-Infrared Spectroscopy
# Time-domain THz Spectroscopy
The THz wavelength regime encompasses the far-infrared range of 0.1-100 THz, or about
3−3300cm−1. The THz regime is especially interesting
for condensed matter physics. This is the energy scale (0.4-400 meV) of many collective
processes, like phonon and magnetic modes, superconducting gaps, and spin and charge
ordering gaps, to name a few. It's also the energy scale of surface states in topological
insulators and the Dirac cones of graphene.
Time-domain THz spectroscopy is an integral tool for optical characterization of solids.
The advantage of using femtosecond-scale pulses for THz generation is the ability to map
the full phase and amplitude information of the THz electric field using electro-optic
sampling. After a THz pulse has passed through or been reflected by the material of
interest, the material's complex optical response can be reconstructed from the THz field,
without requiring a broadband spectrum and Kramers-Kronig transformation.
Our THz probe source relies on frequency conversion from the near-infrared
(800 nm femtosecond pulses output by an amplified Ti:Sapphire laser) into single-cycle
THz pulses via optical rectification in ZnTe. The bandwidth of the resulting THz pulses
can probe between 0.3-2.5 THz (10−85cm−1).
We combine our THz spectroscopy probe with a variable wavelength pump generated by optical
parametric amplification and difference frequency generation (OPA+DFG) of 800 nm light.
Our system has a state-of-the-art pulse energy range in the mid-infrared of 50-150 uJ for
wavelengths between 4-15 um. This translates to large excitation fields, on order 10 MV/cm.