Spectroscopic signatures of phonons in high pressure superconducting hydrides

TL;DR

This paper discusses how optical spectroscopy reveals phonon-related signatures in high-pressure hydride superconductors, confirming electron-phonon interactions as the mechanism behind their high critical temperatures.

Contribution

It provides a detailed analysis of phonon signatures in optical spectra, linking them to the superconducting order parameter and confirming electron-phonon coupling as the key mechanism.

Findings

Optical reflectance shows anomalous temperature dependence in SH3.

Phonon structures in optics encode information about $T_c$ and the order parameter.

Comparison with LaH10 highlights the relevance of high-energy phonons in high-$T_c$ superconductivity.

Abstract

The discovery of superconductivity at 203K in SH$_3$ is an important step toward higher values of $T_c$. Predictions based on state-of-the-art DFT for the electronic structure, including one preceding experimental confirmation, showed the mechanism to be the electron-phonon interaction. This was confirmed in optical spectroscopy measurements. For photon energies between $\sim 450$ and 600 meV in SH$_3$, the reflectance in the superconducting state is below that in its normal state. This difference decreases as $T$ approaches $T_c$. Decreasing absorption with increasing $T$ is opposite to what is expected in ordinary metals. Such an anomalous behavior can be traced back to the energy dependence of the superconducting density of states which is highly peaked at the energy gap value $\Delta$ but decays back to the constant normal state value as energy is increased, on a scale of a few $\Delta$, or by increasing $T$ towards $T=T_c$. The process of phonon-assisted optical absorption is encoded with a knowledge of the $T$-dependence of $\Delta$, the order parameter of the superconducting state. Should the energy of the phonon involved be very large, of order 200 meV or more, this process offers the possibility of observing the closing of the superconducting order parameter with $T$ at correspondingly very large energies. The very recent experimental observation of a $T_c\simeq 250$ K in LaH$_{10}$ has further heightened interest in the hydrides. We compare the relevant phonon structure seen in optics with related features in the real and imaginary part of the frequency dependent gap, quasiparticle density of states, reflectance, absorption, and optical scattering rate. The phonon structures all carry information on the $T_c$ value and the $T$-dependence of the order parameter, and can be used to confirm that the mechanism involved in superconductivity is the electron-phonon interaction.