Excitation spectra in fluids: How to analyze them properly

Abstract

Although the understanding of excitation spectra in fluids is of great importance, it is still unclear how different methods of spectral analysis agree with each other and which of them is suitable in a wide range of parameters. Here, we show that the problem can be solved using a two-oscillator model to analyze total velocity current spectra, while other considered methods, including analysis of the spectral maxima and single mode analysis, yield rough results and become unsuitable at high temperatures and wavenumbers. To prove this, we perform molecular dynamics (MD) simulations and calculate excitation spectra in Lennard-Jones and inverse-power-law fluids at different temperatures, both in 3D and 2D cases. Then, we analyze relations between thermodynamic and dynamic features of fluids at (Frenkel) crossover from a liquid- to gas-like state and find that they agree with each other in the 3D case and strongly disagree in 2D systems due to enhanced anharmonicity effects. The results provide a significant advance in methods for detail analysis of collective fluid dynamics spanning fields from soft condensed matter to strongly coupled plasmas.