Force-induced tautomerization in a single molecule
Heat transfer, electrical potential and light energy are common ways to activate chemical reactions. Applied force is another way, but dedicated studies for such a mechanical activation are limited, and this activation is poorly understood at the single-molecule level. Here, we report force-induced tautomerization in a single porphycene molecule on a Cu(110) surface at 5 K, which is studied by scanning probe microscopy and density functional theory calculations. Force spectroscopy quantifies the force needed to trigger tautomerization with submolecular spatial resolution. The calculations show how the reaction pathway and barrier of tautomerization are modified in the presence of a copper tip and reveal the atomistic origin of the process. Moreover, we demonstrate that a chemically inert tip whose apex is terminated by a xenon atom cannot induce the reaction because of a weak interaction with porphycene and a strong relaxation of xenon on the tip as contact to the molecule is formed.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2016 |
|---|---|
| Erschienen: |
2016 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:8 |
|---|---|
| Enthalten in: |
Nature chemistry - 8(2016), 10 vom: 22. Okt., Seite 935-40 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Ladenthin, Janina N [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
|---|
| Anmerkungen: |
Date Completed 16.08.2018 Date Revised 13.11.2018 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1038/nchem.2552 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM264594193 |
|---|
| LEADER | 01000naa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM264594193 | ||
| 003 | DE-627 | ||
| 005 | 20231224210433.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 231224s2016 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1038/nchem.2552 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n0882.xml |
| 035 | |a (DE-627)NLM264594193 | ||
| 035 | |a (NLM)27657869 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Ladenthin, Janina N |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Force-induced tautomerization in a single molecule |
| 264 | 1 | |c 2016 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Completed 16.08.2018 | ||
| 500 | |a Date Revised 13.11.2018 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Heat transfer, electrical potential and light energy are common ways to activate chemical reactions. Applied force is another way, but dedicated studies for such a mechanical activation are limited, and this activation is poorly understood at the single-molecule level. Here, we report force-induced tautomerization in a single porphycene molecule on a Cu(110) surface at 5 K, which is studied by scanning probe microscopy and density functional theory calculations. Force spectroscopy quantifies the force needed to trigger tautomerization with submolecular spatial resolution. The calculations show how the reaction pathway and barrier of tautomerization are modified in the presence of a copper tip and reveal the atomistic origin of the process. Moreover, we demonstrate that a chemically inert tip whose apex is terminated by a xenon atom cannot induce the reaction because of a weak interaction with porphycene and a strong relaxation of xenon on the tip as contact to the molecule is formed | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Research Support, Non-U.S. Gov't | |
| 700 | 1 | |a Frederiksen, Thomas |e verfasserin |4 aut | |
| 700 | 1 | |a Persson, Mats |e verfasserin |4 aut | |
| 700 | 1 | |a Sharp, John C |e verfasserin |4 aut | |
| 700 | 1 | |a Gawinkowski, Sylwester |e verfasserin |4 aut | |
| 700 | 1 | |a Waluk, Jacek |e verfasserin |4 aut | |
| 700 | 1 | |a Kumagai, Takashi |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Nature chemistry |d 2009 |g 8(2016), 10 vom: 22. Okt., Seite 935-40 |w (DE-627)NLM192571583 |x 1755-4349 |7 nnns |
| 773 | 1 | 8 | |g volume:8 |g year:2016 |g number:10 |g day:22 |g month:10 |g pages:935-40 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1038/nchem.2552 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 8 |j 2016 |e 10 |b 22 |c 10 |h 935-40 | ||