Angle-resolved photoemission spectroscopy (ARPES)

Experiment track

In plain words

A measurement that shines light on a crystal, catches the electrons it knocks out and records the direction and energy of each one. From that it reconstructs how the electrons were moving inside – the closest thing there is to a photograph of a material’s .

Going deeper

Left: a photon strikes a sample in vacuum and an electron leaves at an angle θ from the surface normal towards an analyser that measures its energy and angle; below, the relations E_kin = hν − φ − E_B and k∥ = √(2m·E_kin)/ħ · sin θ. Right: energy against in-plane momentum, with a parabolic band crossing a dashed Fermi level; the part below the Fermi level is drawn as bright measured intensity and the part above it as a faint dashed line labelled not seen by ARPES. light in, electrons out photon, energy hν sample, in vacuum θ analyser: energy, angle E_kin = hν − φ − E_B k∥ = √(2m·E_kin)/ħ · sin θ what it maps: filled bands only energy in-plane momentum k∥ E_F k_F above E_F: empty, not seen by ARPES filled states
ARPES turns each emitted electron’s energy and angle into the energy and in-plane momentum it had inside the crystal. It sees only filled states, so the part of a band above the Fermi level – including the conduction band of an undoped semiconductor – stays invisible unless electrons are put there first.

From emitted electrons to bands

A of known energy hν frees an electron from the crystal. Energy conservation gives the electron’s binding energy from its kinetic energy and the φ. Momentum parallel to the surface is conserved as the electron leaves, so the emission angle gives its in-plane momentum inside the crystal. Recording electrons over a range of angles and energies builds up a map of energy against momentum – the occupied band structure.

Momentum perpendicular to the surface is not conserved, which complicates ARPES on three-dimensional crystals. A has almost no dispersion in that direction, which makes it a natural subject. Light sources range from lasers of about 6 eV and helium lamps at 21.2 eV to synchrotrons, whose tunable photon energy selects different parts of the Brillouin zone and different orbitals.

What the maps show

The bright lines are band dispersions: their curvature gives , their crossings and gaps the band , and a cut at the the . Line widths and kinks carry the effects of interactions – a kink where electrons couple to , a broadening from electron–electron scattering. In ARPES measures directly the of the at K.

Only filled states are seen. The conduction band of an undoped , and so its band gap, needs electrons put there first, by depositing potassium on the surface or by a pump pulse in ARPES. A gap read this way is the , which exceeds the optical gap by the – although the added electrons also screen the layer and shrink it somewhat.

Practical limits

The emitted electrons come from the top few atomic layers, so the surface must be clean and the measurement is done in ultrahigh vacuum; crystals are cleaved inside the chamber, or grown there. The sample must be electrically grounded, or it charges up and the spectra shift. A buried layer is out of reach: in a , the layer of interest has to be on top or covered by no more than a single sheet or so.

Exfoliated are usually tens of micrometres across, smaller than the spot of a conventional beamline. Micro- and nano-ARPES focus the beam down to around a micrometre or below, at the cost of photon flux and resolution, and have made single-domain twisted and few-layer samples measurable.

For specialists

Photoemission with energy and momentum resolution, giving the occupied band structure, Fermi surface and self-energy directly. It needs a clean, flat, conducting surface in ultrahigh vacuum; focused micro- and nano-ARPES beamlines bring the spot down to the size of an exfoliated flake, which is what makes single-domain twisted and few-layer samples measurable at all.

Where this comes from

  1. Angle-resolved photoemission studies of the cuprate superconductors Damascelli et al. · Reviews of Modern Physics 75, 473 (2003) cited by 3,783
  2. A perspective on the application of spatially resolved ARPES for 2D materials Cattelan and Fox · Nanomaterials 8, 284 (2018) cited by 78