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Time-resolved THz Stark spectroscopy of molecules in solution

Kang, Bong Joo
Rohwer, Egmont J.
Rohrbach, David
Zyaee, Elnaz
Akbarimoosavi, Maryam
Ollmann, Zoltan
Sorohhov, Gleb
Borgoo, Alex
Cascella, Michele
Cannizzo, Andrea
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Journal article
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2024-05-17
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Chemistry
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https://doi.org/10.1038/s41467-024-48164-w
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 demonstratetime-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.
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Kang, B.J., Rohwer, E.J., Rohrbach, D. et al. Time-resolved THz Stark spectroscopy of molecules in solution. Nat Commun 15, 4212 (2024). https://doi.org/10.1038/s41467-024-48164-w
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Springer Science and Business Media
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Nature Communications, Vol. 15, Iss. 1
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