Year: 2022
Type: preprint
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.
Source: arXiv (Cornell University)
Authors: Kang, Bong Joo, Rohwer, Egmont J., Rohrbach, David, Akbarimoosavi, Maryam, Ollmann, Zoltan, Zyaee, Elnaz, Pauszek, Raymond F., Sorohhov, Gleb, Borgoo, Alex, Cascella, Michele, Cannizzo, Andrea, Decurtins, Silvio, Stanley, Robert J., Liu, Shi-Xia, Feurer, Thomas
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: green
Awards: G1765324173, Fellowship Program of the NCCR MUST (National Competence Center for Research in Molecular Ultrafast Science and Technology) and the Cluster of Excellence RESOLV, G481740877, Nitrogenated Polycyclic Aromatic Hydrocarbons (N-PAHs): Nanostructures, Functionalization and Electronic Properties (NanoFun), G993971353
OpenAlex ID: W4312091284