Perturbative Transfer Matrix Method for optical-pump-THz-probe of ultrafast dynamics

TL;DR

This paper introduces the Perturbative Transfer Matrix Method (PTMM), a new theoretical framework to accurately model ultrafast THz interactions with dynamically changing multilayer materials, enabling improved analysis of ultrafast processes and spintronics mechanisms.

Contribution

The paper develops PTMM to model THz interactions with time-dependent multilayers, allowing for precise analysis of ultrafast dynamics and spintronic THz emitters.

Findings

PTMM accurately models THz interactions with ultrafast changing multilayers.

Time-resolved spectra can measure sub-picosecond processes.

Delay-resolved spectra reveal spin current dynamics.

Abstract

Ultrafast optical excitations trigger in materials a range of dynamics. An interesting range of dynamics is the ones that unfold within the picosecond timescale, corresponding to the THz frequency range. Within this short timescale, the material's properties, and therefore its response to electromagnetic fields, dynamically change. For this reason, any THz radiation used to probe the material will interact with the multilayer undergoing time-dependent modifications of the dielectric responses within a single optical cycle (a very similar situation arises for THz radiation produced in spintronics THz emitters). Such interaction goes beyond typical quasistatic approaches. It is, therefore paramount to be able to describe accurately all the interaction of THz radiation with out-of-equilibrium multilayers. We develop here a theoretical framework called PTMM (Perturbative Transfer Matrix Method) to model the production of THz accurately and its interaction with multilayers undergoing ultrafast changes in their dielectric properties. That analysis allows us to propose two novel ways to utilize Terahertz time-domain spectroscopy. We will first show that a simple analysis of the time resolved Optical-Pump-Terahertz-Probe spectra can provide not only the time scale of processes that are slower than the THz pulse time-width, but it can accurately measure the timescale of sub-picosecond and faster processes as well. Further, we will apply our method to THz probed spintronics THz emitters, and compute the interference between the produced THz and the THz probe. We will show that an analysis of the delay-resolved transmission spectra allows for a direct measurement of the time distance between the laser excitation and the peak of the spin current, allowing an unprecedented insight into the ultrafast spin-to-charge conversion mechanism.