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

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 Added by Arthur K Mills
 Publication date 2019
  fields Physics
and research's language is English




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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.



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We describe an approach based on topology optimization that enables automatic discovery of wavelength-scale photonic structures for achieving high-efficiency second-harmonic generation (SHG). A key distinction from previous formulation and designs that seek to maximize Purcell factors at individual frequencies is that our method not only aims to achieve frequency matching (across an entire octave) and large radiative lifetimes, but also optimizes the equally important nonlinear--coupling figure of merit $bar{beta}$, involving a complicated spatial overlap-integral between modes. We apply this method to the particular problem of optimizing micropost and grating-slab cavities (one-dimensional multilayered structures) and demonstrate that a variety of material platforms can support modes with the requisite frequencies, large lifetimes $Q > 10^4$, small modal volumes $sim (lambda/n)^3$, and extremely large $bar{beta} gtrsim 10^{-2}$, leading to orders of magnitude enhancements in SHG efficiency compared to state of the art photonic designs. Such giant $bar{beta}$ alleviate the need for ultra-narrow linewidths and thus pave the way for wavelength-scale SHG devices with faster operating timescales and higher tolerance to fabrication imperfections.
Nano-resonator integrated with two-dimensional materials (e.g. transition metal dichalcogenides) have recently emerged as a promising nano-optoelectronic platform. Here we demonstrate resonatorenhanced second-harmonic generation (SHG) in tungsten diselenide using a silicon photonic crystal cavity. By pumping the device with the ultrafast laser pulses near the cavity mode at the telecommunication wavelength, we observe a near visible SHG with a narrow linewidth and near unity linear polarization, originated from the coupling of the pump photon to the cavity mode. The observed SHG is enhanced by factor of ~200 compared to a bare monolayer on silicon. Our results imply the efficacy of cavity integrated monolayer materials for nonlinear optics and the potential of building a silicon-compatible second-order nonlinear integrated photonic platform.
69 - V. E. Nefedova 2020
High-order harmonic generation (HHG) from crystals offers a new source of coherent extreme ultraviolet (XUV) attosecond radiation.
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