Shaped and feedback-controlled excitation of single molecules in the weak-field limit
Coherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can...
| Main Authors: | , , |
|---|---|
| Format: | Journal article |
| Language: | English |
| Published: |
American Chemical Society
2015
|
| _version_ | 1826264402427379712 |
|---|---|
| author | Weigel, A Sebesta, A Kukura, P |
| author_facet | Weigel, A Sebesta, A Kukura, P |
| author_sort | Weigel, A |
| collection | OXFORD |
| description | Coherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can be influenced by the pulse shape, even if only a single photon is absorbed. Most such experiments are performed on many molecules simultaneously, so that ensemble averaging reduces the access to quantum effects. Here, we demonstrate systematic coherent control experiments on the fluorescence intensity of a single molecule in the weak-field limit. We demonstrate that a delay scan of interfering pulses reproduces the excitation spectrum of the molecule upon Fourier transformation, but that the spectral phase of a pulse sequence does not affect the transition probability. We generalize this result to arbitrary pulse shapes by performing the first closed-loop coherent control experiments on a single molecule. |
| first_indexed | 2024-03-06T20:07:13Z |
| format | Journal article |
| id | oxford-uuid:294ae360-145c-4a86-abd1-2d401ec73d8a |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T20:07:13Z |
| publishDate | 2015 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:294ae360-145c-4a86-abd1-2d401ec73d8a2022-03-26T12:18:21ZShaped and feedback-controlled excitation of single molecules in the weak-field limitJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:294ae360-145c-4a86-abd1-2d401ec73d8aEnglishSymplectic Elements at OxfordAmerican Chemical Society2015Weigel, ASebesta, AKukura, PCoherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can be influenced by the pulse shape, even if only a single photon is absorbed. Most such experiments are performed on many molecules simultaneously, so that ensemble averaging reduces the access to quantum effects. Here, we demonstrate systematic coherent control experiments on the fluorescence intensity of a single molecule in the weak-field limit. We demonstrate that a delay scan of interfering pulses reproduces the excitation spectrum of the molecule upon Fourier transformation, but that the spectral phase of a pulse sequence does not affect the transition probability. We generalize this result to arbitrary pulse shapes by performing the first closed-loop coherent control experiments on a single molecule. |
| spellingShingle | Weigel, A Sebesta, A Kukura, P Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title | Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title_full | Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title_fullStr | Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title_full_unstemmed | Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title_short | Shaped and feedback-controlled excitation of single molecules in the weak-field limit |
| title_sort | shaped and feedback controlled excitation of single molecules in the weak field limit |
| work_keys_str_mv | AT weigela shapedandfeedbackcontrolledexcitationofsinglemoleculesintheweakfieldlimit AT sebestaa shapedandfeedbackcontrolledexcitationofsinglemoleculesintheweakfieldlimit AT kukurap shapedandfeedbackcontrolledexcitationofsinglemoleculesintheweakfieldlimit |