Cavity-enhanced high harmonic generation for XUV time-resolved ARPES

Abstract

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly desirable for many TR-ARPES studies - while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity (fsEC), realizing a practical source for TR-ARPES that achieves a flux of over 10${}^{11}$ photons/s delivered to the sample, operates over a range of 8-40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe${}_2$, as well as TR-ARPES studies on graphite.

11 pages, 5 figures

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• Establishing non-thermal regimes in pump-probe electron-relaxation dynamics
• Time-resolved ARPES on cuprates: Tracking the low-energy electrodynamics in the time domain
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• HHG-laser-based time- and angle-resolved photoemission spectroscopy of quantum materials
• Ultrafast Polarization-Tunable Monochromatic Extreme Ultraviolet Source at High-Repetition-Rate
• Multispectral time-resolved energy-momentum microscopy using high-harmonic extreme ultraviolet radiation
• Spectroscopic data de-noising via training-set-free deep learning method
• A newly-designed femtosecond KBe${}_2$BO${}_3$F${}_2$ device with pulse duration down to 55 fs for time- and angle-resolved photoemission spectroscopy
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• Widely tunable cavity-enhanced frequency combs
• Ubiquitous suppression of the nodal coherent spectral weight in Bi-based cuprates
• Time- and angle-resolved photoemission spectroscopy with wavelength-tunable pump and extreme ultraviolet probe enabled by twin synchronized amplifiers
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• Time-of-Flight Photoelectron Momentum Microscopy at 100-500 MHz Synchrotron Sources: Electron-Optical Chopping or Bandwidth Pre-Selection