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The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently, it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here, we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse central frequency, which can be determined from an absorption spectrum. Our results suggest that for numerous systems, the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.

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Autor(es)

Johnson, Allan S. -  Yuen -  Zhou, Joel -  Aspuru -  Guzik, Alan -  Krich, Jacob - 

Id.: 69632453

Idioma: inglés (Estados Unidos)  - 

Versión: 1.0

Estado: Final

Tipo de recurso: Journal Article  - 

Tipo de Interactividad: Expositivo

Nivel de Interactividad: muy bajo

Audiencia: Estudiante  -  Profesor  -  Autor  - 

Estructura: Atomic

Coste: no

Copyright: sí

: open

Requerimientos técnicos:  Browser: Any - 

Relación: [References] doi:10.1063/1.4903982
[References] https://arxiv.org/abs/1408.3121
[References] The Journal of Chemical Physics

Fecha de contribución: 11-feb-2017

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Localización:
* Quick submit: 2017-02-03T17:20:53-0500
* Johnson, Allan S., Joel Yuen-Zhou, Alán Aspuru-Guzik, and Jacob J. Krich. 2014. “Practical Witness for Electronic Coherences.” The Journal of Chemical Physics 141 (24) (December 28): 244109. doi:10.1063/1.4903982.
* 0021-9606

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