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Third-harmonic generation (THG) experiments on superconductors can be used to investigate collective excitations like the amplitude mode of the order parameter known as Higgs mode. These modes are visible due to resonances in the THG signal if the driving frequency matches the energy of the mode. In real materials multiple modes can exist giving rise to additional THG contributions, such that it is difficult to unambiguously interpret the results. In this paper, we additionally analyze the phase of the THG signal, which contains microscopic details beyond classical resonances as well as signatures of couplings between modes which are difficult to observe in the amplitude alone. We investigate how the Higgs mode, impurities or Coulomb interaction affects the phase response and consider exemplary two systems with additional modes. We argue that extracting this phase information could be valuable in future experiments., Comment: 22 pages, 10 figures

Higgs oscillations in nonequilibrium superconductors provide an unique tool to obtain information about the underlying order parameter. Several properties like the absolute value, existence of multiple gaps and the symmetry of the order parameter can be encoded in the Higgs oscillation spectrum. Studying Higgs oscillations with time-resolved angle-resolved photoemission spectroscopy (ARPES) has the advantage over optical measurements that a momentum-resolved analysis of the condensate dynamic is possible. In this paper, we investigate the time-resolved spectral function measured in ARPES for different quench protocols. We find that analyzing amplitude oscillations of the ARPES intensity in the whole Brillouin zone allows to understand how the condensate dynamic contributes to the emerging of collective Higgs oscillations. Furthermore, by evaluating the phase of these oscillations the symmetry deformation dynamic of the condensate can be revealed, which gives insight about the ground state symmetry of the system. With such an analysis, time-resolved ARPES experiments might be used in future as a powerful tool in the field of Higgs spectroscopy., 15 pages, 9 figures, updated and extended

The Higgs mode in superconductors is a scalar mode without electric or magnetic dipole moment. Thus, it is commonly believed that its excitation is restricted to a nonlinear two-photon Raman process. However, recent efforts have shown that a linear excitation in the presence of a supercurrent is possible, resulting in a new resonant enhancement at $\Omega=2\Delta$ with the driving light frequency $\Omega$ and the energy of the Higgs mode $2\Delta$. This is in contrast to the usual $2\Omega = 2\Delta$ resonance condition found in nonlinear third-harmonic generation experiments. In this communication, we show that such a linear excitation can still be described as an effective Raman two-photon process, with one photon at $\omega=2\Delta$ and one virtual photon at $\omega=0$ which represents the dc supercurrent. At the same time we demonstrate that a straightforward infrared activation with a single photon excitation is negligible. Moreover, we give a general context to our theory, providing an explanation for how the excitation of the Higgs mode in both THz quench and drive experiments can be understood within a conventional difference-frequency generation or sum-frequency generation process, respectively. In such a picture, the observed new resonance condition $\Omega = 2\Delta$ is just a special case. With the same approach, we further discuss another recent experiment, where we find a suppression of odd order higher harmonics in the presence of a dc supercurrent., Comment: 6 pages, 4 figures + supplement