Time-resolved THz Stark spectroscopy
Abstract
We introduce THz Stark spectroscopy by using intense single-cycle terahertz pulses as the electric field source and monitoring the induced spectral response of an isotropic molecular ensemble with a coincident femtosecond supercontinuum pulse. THz Stark spectroscopy offers several advantages over conventional Stark spectroscopy and opens previously inaccessible perspectives. Most importantly, THz pulses oscillate faster than typical molecular rotations and consequently eliminate the requirement to freeze the samples to prevent poling effects. Hence, THz Stark spectroscopy allows for time-resolved studies at arbitrary temperatures, specifically ambient conditions more relevant to physiological or operative conditions. Moreover, dynamical field effects, e.g., higher order Stark contributions or hysteresis effects (non-Markovian behavior), can be studied on the time scales of molecular vibrations or rotations. We demonstrate THz Stark spectroscopy for two judiciously selected molecular systems and compare the results to conventional Stark spectroscopy and first principle calculations.
Cite
@article{arxiv.2212.10333,
title = {Time-resolved THz Stark spectroscopy},
author = {Bong Joo Kang and Egmont J. Rohwer and David Rohrbach and Maryam Akbarimoosavi and Zoltan Ollmann and Elnaz Zyaee and Raymond F. Pauszek and Gleb Sorohhov and Alex Borgoo and Michele Cascella and Andrea Cannizzo and Silvio Decurtins and Robert J. Stanley and Shi-Xia Liu and Thomas Feurer},
journal= {arXiv preprint arXiv:2212.10333},
year = {2022}
}