Coherent control of single molecules at room temperature

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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...

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Detalles Bibliográficos
Autor principal: Brinks, D.
Otros Autores: Hildner, R., Stefani, F.D, Van Hulst, N.F
Formato: Capítulo de libro
Lenguaje:Inglés
Publicado: 2011
Acceso en línea:Registro en Scopus
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Biblioteca Central Dr. Luis F. Leloir (FCEN) de Universidad de Buenos Aires
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024 7 |2 cas  |a Organic Chemicals 
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100 1 |a Brinks, D. 
245 1 0 |a Coherent control of single molecules at room temperature 
260 |c 2011 
270 1 0 |m Van Hulst, N.F.; ICFO - Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels (Barcelona), Spain; email: Niek.vanHulst@ICFO.es 
506 |2 openaire  |e Política editorial 
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520 3 |a 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.  |l eng 
593 |a ICFO - Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels (Barcelona), Spain 
593 |a Dept. de Física, Fac. de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Buenos Aires, Argentina 
593 |a ICREA - Institució Catalana de Recerca i Estudis Avanats, Barcelona 08015, Spain 
690 1 0 |a ORGANIC COMPOUND 
690 1 0 |a ARTICLE 
690 1 0 |a CHEMISTRY 
690 1 0 |a QUANTUM THEORY 
690 1 0 |a TEMPERATURE 
690 1 0 |a VIBRATION 
690 1 0 |a ORGANIC CHEMICALS 
690 1 0 |a QUANTUM THEORY 
690 1 0 |a TEMPERATURE 
690 1 0 |a VIBRATION 
700 1 |a Hildner, R. 
700 1 |a Stefani, F.D. 
700 1 |a Van Hulst, N.F. 
773 0 |d 2011  |g v. 153  |h pp. 51-60  |p Faraday Discuss.  |x 13596640  |t Faraday Discussions 
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856 4 0 |u https://doi.org/10.1039/c1fd00087j  |y DOI 
856 4 0 |u https://hdl.handle.net/20.500.12110/paper_13596640_v153_n_p51_Brinks  |y Handle 
856 4 0 |u https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_13596640_v153_n_p51_Brinks  |y Registro en la Biblioteca Digital 
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