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Peller, Dominik ; Kastner, Lukas Z. ; Buchner, Thomas ; Roelcke, Carmen ; Albrecht, Florian ; Moll, Nikolaj ; Huber, Rupert ; Repp, Jascha

Sub-cycle atomic-scale forces coherently control a single-molecule switch

Peller, Dominik, Kastner, Lukas Z., Buchner, Thomas , Roelcke, Carmen , Albrecht, Florian, Moll, Nikolaj , Huber, Rupert and Repp, Jascha (2020) Sub-cycle atomic-scale forces coherently control a single-molecule switch. Nature 585 (7823), pp. 58-62.

Date of publication of this fulltext: 03 Sep 2020 09:48
Article
DOI to cite this document: 10.5283/epub.43676


Abstract

Scanning probe techniques can leverage atomically precise forces to sculpt matter at surfaces, atom by atom. These forces have been applied quasi-statically to create surface structures(1-7)and influence chemical processes(8,9), but exploiting local dynamics(10-14)to realize coherent control on the atomic scale remains an intriguing prospect. Chemical reactions(15-17), conformational ...

Scanning probe techniques can leverage atomically precise forces to sculpt matter at surfaces, atom by atom. These forces have been applied quasi-statically to create surface structures(1-7)and influence chemical processes(8,9), but exploiting local dynamics(10-14)to realize coherent control on the atomic scale remains an intriguing prospect. Chemical reactions(15-17), conformational changes(18,19)and desorption(20)have been followed on ultrafast timescales, but directly exerting femtosecond forces on individual atoms to selectively induce molecular motion has yet to be realized. Here we show that the near field of a terahertz wave confined to an atomically sharp tip provides femtosecond atomic-scale forces that selectively induce coherent hindered rotation in the molecular frame of a bistable magnesium phthalocyanine molecule. Combining lightwave-driven scanning tunnelling microscopy(21-24)with ultrafast action spectroscopy(10,13), we find that the induced rotation modulates the probability of the molecule switching between its two stable adsorption geometries by up to 39 per cent. Mapping the response of the molecule in space and time confirms that the force acts on the atomic scale and within less than an optical cycle (that is, faster than an oscillation period of the carrier wave of light). We anticipate that our strategy might ultimately enable the coherent manipulation of individual atoms within single molecules or solids so that chemical reactions and ultrafast phase transitions can be manipulated on their intrinsic spatio-temporal scales. The near field of a terahertz wave confined to a scanning probe tip provides femtosecond atomic-scale forces that coherently modulate the switching probability of a molecule between two stable adsorption geometries.



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    Peller, Dominik, Kastner, Lukas Z., Buchner, Thomas , Roelcke, Carmen , Albrecht, Florian, Moll, Nikolaj , Huber, Rupert and Repp, Jascha (2020) Sub-cycle atomic-scale forces coherently control a single-molecule switch. Nature 585 (7823), pp. 58-62. [Currently displayed]

Details

Item typeArticle
Journal or Publication TitleNature
Publisher:Nature
Open Access Type:No Open Access
Place of Publication:LONDON
Volume:585
Number of Issue or Book Chapter:7823
Page Range:pp. 58-62
Date2 September 2020
InstitutionsPhysics > Institute of Experimental and Applied Physics > Group Jascha Repp
Physics > Institute of Experimental and Applied Physics > Chair Professor Huber > Group Rupert Huber
Identification Number
ValueType
10.1038/s41586-020-2620-2DOI
KeywordsCHEMICAL-REACTION; MOTION; TAUTOMERIZATION; ISOMERIZATION;
Dewey Decimal Classification500 Science > 530 Physics
500 Science > 540 Chemistry & allied sciences
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgYes
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-436764
Item ID43676

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