Direct Observation of Photoinduced Tautomerization in Single Molecules at a Metal Surface

Nano Letters
Hannes BöckmannTakashi Kumagai

Abstract

Molecular switches are of fundamental importance in nature, and light is an important stimulus to selectively drive the switching process. However, the local dynamics of a conformational change in these molecules remain far from being completely understood at the single-molecule level. Here, we report the direct observation of photoinduced tautomerization in single porphycene molecules on a Cu(111) surface by using a combination of low-temperature scanning tunneling microscopy and laser excitation in the near-infrared to ultraviolet regime. It is found that the thermodynamically stable trans configuration of porphycene can be converted to the metastable cis configuration in a unidirectional fashion by photoirradiation. The wavelength dependence of the tautomerization cross section exhibits a steep increase around 2 eV and demonstrates that excitation of the Cu d-band electrons and the resulting hot carriers play a dominant role in the photochemical process. Additionally, a pronounced isotope effect in the cross section (∼100) is observed when the transferred hydrogen atoms are substituted with deuterium, indicating a significant contribution of zero-point energy in the reaction. Combined with the study of inelastic tunneling el...Continue Reading

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Jul 29, 2016·Chemical Reviews·Jacek Waluk
Aug 10, 2016·ACS Nano·Szymon GodlewskiMark Saeys
Feb 16, 2017·The Journal of Physical Chemistry Letters·Dino NovkoJean Christophe Tremblay
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May 26, 2021·ACS Nano·Aleš CahlíkPavel Jelínek
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Nov 9, 2021·The Journal of Physical Chemistry Letters·Yongfeng TongAmandine Bellec

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