Time-resolved THz Stark spectroscopy of molecules in solution

Bong Joo Kang, Egmont J. Rohwer, David Rohrbach, Elnaz Zyaee, Maryam Akbarimoosavi, Zoltan Ollmann, Gleb Sorohhov, Alex Borgoo, Michele Cascella, Andrea Cannizzo, Silvio Decurtins, Robert J. Stanley, Shi-Xia Liu and Thomas Feurer ()
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Bong Joo Kang: University of Bern
Egmont J. Rohwer: University of Bern
David Rohrbach: University of Bern
Elnaz Zyaee: University of Bern
Maryam Akbarimoosavi: University of Bern
Zoltan Ollmann: University of Bern
Gleb Sorohhov: University of Bern
Alex Borgoo: University of Oslo
Michele Cascella: University of Oslo
Andrea Cannizzo: University of Bern
Silvio Decurtins: University of Bern
Robert J. Stanley: Temple University
Shi-Xia Liu: University of Bern
Thomas Feurer: University of Bern

Nature Communications, 2024, vol. 15, issue 1, 1-7

Abstract: Abstract For decades, it was considered all but impossible to perform Stark spectroscopy on molecules in a liquid solution, because their concomitant orientation to the applied electric field results in overwhelming background signals. A way out was to immobilize the solute molecules by freezing the solvent. While mitigating solute orientation, freezing removes the possibility to study molecules in liquid environments at ambient conditions. Here we demonstrate time-resolved THz Stark spectroscopy, utilizing intense single-cycle terahertz pulses as electric field source. At THz frequencies, solute molecules have no time to orient their dipole moments. Hence, dynamic Stark spectroscopy on the time scales of molecular vibrations or rotations in both non-polar and polar solvents at arbitrary temperatures is now possible. We verify THz Stark spectroscopy for two judiciously selected molecular systems and compare the results to conventional Stark spectroscopy and first principle calculations.

Date: 2024
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DOI: 10.1038/s41467-024-48164-w

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