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Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

Watching a single molecule move on its intrinsic time scale—one of the central goals of modern nanoscience—calls for measurements that combine ultrafast temporal resolution1–8 with atomic spatial resolution9–30. Steady-state experiments achieve the requisite spatial resolution, as illustrated by dir...

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Autores principales: Cocker, Tyler L., Peller, Dominik, Yu, Ping, Repp, Jascha, Huber, Rupert
Formato: Online Artículo Texto
Lenguaje:English
Publicado: 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5597038/
https://www.ncbi.nlm.nih.gov/pubmed/27830788
http://dx.doi.org/10.1038/nature19816
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author Cocker, Tyler L.
Peller, Dominik
Yu, Ping
Repp, Jascha
Huber, Rupert
author_facet Cocker, Tyler L.
Peller, Dominik
Yu, Ping
Repp, Jascha
Huber, Rupert
author_sort Cocker, Tyler L.
collection PubMed
description Watching a single molecule move on its intrinsic time scale—one of the central goals of modern nanoscience—calls for measurements that combine ultrafast temporal resolution1–8 with atomic spatial resolution9–30. Steady-state experiments achieve the requisite spatial resolution, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy9–11 or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution27–29. But tracking the dynamics of a single molecule directly in the time domain faces the challenge that single-molecule excitations need to be confined to an ultrashort time window. A first step towards overcoming this challenge has combined scanning tunnelling microscopy with so-called ‘lightwave electronics”1–8, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on time scales faster even than that of a single cycle of light. Here we use such ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state and thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record ~100 fs snapshot images of the structure of the orbital involved, and to reveal through pump-probe measurements coherent molecular vibrations at terahertz frequencies directly in the time domain and with sub-angstrom spatial resolution. We anticipate that the combination of lightwave electronics1–8 and atomic resolution of our approach will open the door to controlling electronic motion inside individual molecules at optical clock rates.
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spelling pubmed-55970382017-09-13 Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging Cocker, Tyler L. Peller, Dominik Yu, Ping Repp, Jascha Huber, Rupert Nature Article Watching a single molecule move on its intrinsic time scale—one of the central goals of modern nanoscience—calls for measurements that combine ultrafast temporal resolution1–8 with atomic spatial resolution9–30. Steady-state experiments achieve the requisite spatial resolution, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy9–11 or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution27–29. But tracking the dynamics of a single molecule directly in the time domain faces the challenge that single-molecule excitations need to be confined to an ultrashort time window. A first step towards overcoming this challenge has combined scanning tunnelling microscopy with so-called ‘lightwave electronics”1–8, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on time scales faster even than that of a single cycle of light. Here we use such ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state and thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record ~100 fs snapshot images of the structure of the orbital involved, and to reveal through pump-probe measurements coherent molecular vibrations at terahertz frequencies directly in the time domain and with sub-angstrom spatial resolution. We anticipate that the combination of lightwave electronics1–8 and atomic resolution of our approach will open the door to controlling electronic motion inside individual molecules at optical clock rates. 2016-11-10 /pmc/articles/PMC5597038/ /pubmed/27830788 http://dx.doi.org/10.1038/nature19816 Text en Users may view, print, copy, and download text and data-mine the content in such documents, for the purposes of academic research, subject always to the full Conditions of use:http://www.nature.com/authors/editorial_policies/license.html#terms
spellingShingle Article
Cocker, Tyler L.
Peller, Dominik
Yu, Ping
Repp, Jascha
Huber, Rupert
Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title_full Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title_fullStr Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title_full_unstemmed Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title_short Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
title_sort tracking the ultrafast motion of a single molecule by femtosecond orbital imaging
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5597038/
https://www.ncbi.nlm.nih.gov/pubmed/27830788
http://dx.doi.org/10.1038/nature19816
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