Time-Resolved Photoemission Spectroscopy

Angle-resolved photoemission spectroscopy (ARPES) is used to analyze the electronic band structure in momentum and energy space for superconductors, topological insulators, transition metal dichalcogenides, and other crystalline materials. In ARPES, a deep-UV laser beam is sent onto the surface. The electrons are emitted by the photoelectric effect above the vacuum level and then collected by a detector, scanned around the sample. Analyzing the energy and momentum of the emitted electron provides the required information for a complete electronic bandstructure mapping.

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) extends and complements conventional ARPES by adding femtosecond temporal resolution. TR-ARPES resolves elementary scattering processes directly in the electronic band structure as a function of energy and electron momentum due to the simultaneous measurement of the spectral and dynamic information. In such a pump-probe scheme, a femtosecond infrared laser pulse excites the sample by electron-hole pair creation, and a delayed UV pulse probes momentum and energy of electrons in the conduction band.

The ideal laser source for TR-ARPES produces deep UV photons at a high repetition rate (hundreds of kHz or higher). Intermediate pulse energy is also advantageous because high pulse energies can cause parasitic space charge effects at the measured surface. Typically, the UV photon is generated by high harmonic generation (HHG) in solids or gases.

Optical parametric amplifiers (OPAs), such as ORPHEUS-MIR and ORPHEUS-N, and optical parametric chirped-pulse amplifiers (OPCPAs) provide state-of-the-art solutions for TR-ARPES.

  • < 6 fs transform-limited pulse duration
  • Up to 1 MHz repetition rate
  • Up to 320 W pump power
  • Up to 8 mJ pump pulse energy
  • CEP stabilization option
  • Compact footprint
  • Up to 800 cm-1 spectral bandwidth
  • 2500 – 15 000 nm tuning range
  • < 100 fs pulse duration
  • Up to 400 kHz repetition rate
  • CEP-stable option
  • < 30 fs pulse duration
  • Single-shot – 1 MHz repetition rate
  • Integrated prism compressor
  • Adjustable spectral bandwidth and pulse duration
  • Wavelength feedback with internal spectrometer
  • 190 – 16000 nm tuning range
  • Single-shot – 2 MHz repetition rate
  • Up to 80 W pump power
  • Up to 2 mJ pump pulse energy
  • Completely automated
  • 100 fs – 20 ps tunable pulse duration
  • 4 mJ maximum pulse energy
  • 20 W maximum output power
  • Single-shot – 1 MHz repetition rate
  • BiBurst
  • Automated harmonic generators (up to 5th harmonic)
  • 190 fs – 20 ps tunable pulse duration
  • 2 mJ maximum pulse energy
  • 80 W maximum output power
  • Single-shot – 2 MHz repetition rate
  • BiBurst
  • Air-cooled version
  • 515 nm, 343 nm, 258 nm, and 206 nm outputs
  • Simple selection of active harmonic
  • Simultaneous or switchable outputs
  • Customizable or high-power and -energy models

Investigation of the non-equilibrium state of strongly correlated materials by complementary ultrafast spectroscopy techniques

H. Hedayat, C. J. Sayers, A. Ceraso, J. van Wezel, S. R. Clark, C. Dallera, G. Cerullo, E. D. Como, and E. Carpene, New Journal of Physics 3 (23), 033025 (2021).

Spatially heterogeneous ultrafast interfacial carrier dynamics of 2D-MoS2 flakes

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Ultrafast generation and decay of a surface metal

L. Gierster, S. Vempati, and J. Stähler, Nature Communications 1 (12) (2021).

A combined laser-based angle-resolved photoemission spectroscopy and two-photon photoemission spectroscopy study of Td–WTe2

P. Hein, S. Jauernik, H. Erk, L. Yang, Y. Qi, Y. Sun, C. Felser, and M. Bauer, Journal of Physics: Condensed Matter 34 (32), 345503 (2020).

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Extreme ultraviolet time- and angle-resolved photoemission setup with 21.5 meV resolution using high-order harmonic generation from a turn-key Yb:KGW amplifier

Y. Liu, J. E. Beetar, M. M. Hosen, G. Dhakal, C. Sims, F. Kabir, M. B. Etienne, K. Dimitri, S. Regmi, Y. Liu et al., Review of Scientific Instruments 1 (91), 013102 (2020).

High resolution time- and angle-resolved photoemission spectroscopy with 11 eV laser pulses

C. Lee, T. Rohwer, E. J. Sie, A. Zong, E. Baldini, J. Straquadine, P. Walmsley, D. Gardner, Y. S. Lee, I. R. Fisher et al., Review of Scientific Instruments 4 (91), 043102 (2020).

Spontaneous Exciton Dissociation at Organic Semiconductor Interfaces Facilitated by the Orientation of the Delocalized Electron–Hole Wavefunction

T. R. Kafle, B. Kattel, S. Wanigasekara, T. Wang, and W. Chan, Advanced Energy Materials 10 (10), 1904013 (2020).

Femtosecond time-resolved spectroscopic photoemission electron microscopy for probing ultrafast carrier dynamics in heterojunctions

B. Li, G. Zhang, Y. Liang, Q. Hao, J. Sun, C. Zhou, Y. Tao, X. Yang, and Z. Ren, 4 (32), 399-405 (2019).

Evidence for topological defects in a photoinduced phase transition

A. Zong, A. Kogar, Y. Bie, T. Rohwer, C. Lee, E. Baldini, E. Ergeçen, M. B. Yilmaz, B. Freelon, E. J. Sie et al., Nature Physics 1 (15), 27-31 (2018).

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