Coherent control of single molecules at room temperature
The detection of individual molecules allows to unwrap the inhomogeneously broadened ensemble and reveal the spatial disorder and temporal dynamics of single entities. During 20 years of increasing sophistication this approach has provided valuable insights into biomolecular interactions, cellular p...
Guardado en:
| Autores principales: | , , , |
|---|---|
| Formato: | JOUR |
| Materias: | |
| Acceso en línea: | http://hdl.handle.net/20.500.12110/paper_13596640_v153_n_p51_Brinks |
| Aporte de: |
| id |
todo:paper_13596640_v153_n_p51_Brinks |
|---|---|
| record_format |
dspace |
| spelling |
todo:paper_13596640_v153_n_p51_Brinks2023-10-03T16:10:40Z Coherent control of single molecules at room temperature Brinks, D. Hildner, R. Stefani, F.D. Van Hulst, N.F. organic compound article chemistry quantum theory temperature vibration Organic Chemicals Quantum Theory Temperature Vibration The detection of individual molecules allows to unwrap the inhomogeneously broadened ensemble and reveal the spatial disorder and temporal dynamics of single entities. During 20 years of increasing sophistication this approach has provided valuable insights into biomolecular interactions, cellular processes, polymer dynamics, etc. Unfortunately the detection of fluorescence, i.e. incoherent spontaneous emission, has essentially kept the time resolution of the single molecule approach out of the range of ultrafast coherent processes. In parallel coherent control of quantum interferences has developed as a powerful method to study and actively steer ultrafast molecular interactions and energy conversion processes. However the degree of coherent control that can be reached in ensembles is restricted, due to the intrinsic inhomogeneity of the synchronized subset. Clearly the only way to overcome spatio-temporal disorder and achieve key control is by addressing individual units: coherent control of single molecules. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a superior degree of control compared to the ensemble approach. Phase reversal does invert the molecular response, confirming the control of quantum coherence. Time-phase maps show a rich diversity in excited state dynamics between different, yet chemically identical, molecules. The presented approach is promising for single-unit coherent control in multichromophoric systems. Especially the role of coherence in the energy transfer of single antenna complexes under physiological conditions is subject of great attention. Now the role of energy disorder and variation in coupling strength can be explored, beyond the inhomogeneously broadened ensemble. © 2011 The Royal Society of Chemistry. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_13596640_v153_n_p51_Brinks |
| institution |
Universidad de Buenos Aires |
| institution_str |
I-28 |
| repository_str |
R-134 |
| collection |
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| topic |
organic compound article chemistry quantum theory temperature vibration Organic Chemicals Quantum Theory Temperature Vibration |
| spellingShingle |
organic compound article chemistry quantum theory temperature vibration Organic Chemicals Quantum Theory Temperature Vibration Brinks, D. Hildner, R. Stefani, F.D. Van Hulst, N.F. Coherent control of single molecules at room temperature |
| topic_facet |
organic compound article chemistry quantum theory temperature vibration Organic Chemicals Quantum Theory Temperature Vibration |
| description |
The detection of individual molecules allows to unwrap the inhomogeneously broadened ensemble and reveal the spatial disorder and temporal dynamics of single entities. During 20 years of increasing sophistication this approach has provided valuable insights into biomolecular interactions, cellular processes, polymer dynamics, etc. Unfortunately the detection of fluorescence, i.e. incoherent spontaneous emission, has essentially kept the time resolution of the single molecule approach out of the range of ultrafast coherent processes. In parallel coherent control of quantum interferences has developed as a powerful method to study and actively steer ultrafast molecular interactions and energy conversion processes. However the degree of coherent control that can be reached in ensembles is restricted, due to the intrinsic inhomogeneity of the synchronized subset. Clearly the only way to overcome spatio-temporal disorder and achieve key control is by addressing individual units: coherent control of single molecules. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a superior degree of control compared to the ensemble approach. Phase reversal does invert the molecular response, confirming the control of quantum coherence. Time-phase maps show a rich diversity in excited state dynamics between different, yet chemically identical, molecules. The presented approach is promising for single-unit coherent control in multichromophoric systems. Especially the role of coherence in the energy transfer of single antenna complexes under physiological conditions is subject of great attention. Now the role of energy disorder and variation in coupling strength can be explored, beyond the inhomogeneously broadened ensemble. © 2011 The Royal Society of Chemistry. |
| format |
JOUR |
| author |
Brinks, D. Hildner, R. Stefani, F.D. Van Hulst, N.F. |
| author_facet |
Brinks, D. Hildner, R. Stefani, F.D. Van Hulst, N.F. |
| author_sort |
Brinks, D. |
| title |
Coherent control of single molecules at room temperature |
| title_short |
Coherent control of single molecules at room temperature |
| title_full |
Coherent control of single molecules at room temperature |
| title_fullStr |
Coherent control of single molecules at room temperature |
| title_full_unstemmed |
Coherent control of single molecules at room temperature |
| title_sort |
coherent control of single molecules at room temperature |
| url |
http://hdl.handle.net/20.500.12110/paper_13596640_v153_n_p51_Brinks |
| work_keys_str_mv |
AT brinksd coherentcontrolofsinglemoleculesatroomtemperature AT hildnerr coherentcontrolofsinglemoleculesatroomtemperature AT stefanifd coherentcontrolofsinglemoleculesatroomtemperature AT vanhulstnf coherentcontrolofsinglemoleculesatroomtemperature |
| _version_ |
1807315603122290688 |