Förster resonance energy transfer, absorption and emission spectra in multichromophoric systems. I. Full cumulant expansions and system-bath entanglement

The Journal of Chemical Physics
Jian Ma, Jianshu Cao

Abstract

We study the Förster resonant energy transfer rate, absorption and emission spectra in multichromophoric systems. The multichromophoric Förster theory (MCFT) is determined from an overlap integral of generalized matrices related to the donor's emission and acceptor's absorption spectra, which are obtained via a full 2nd-order cumulant expansion technique developed in this work. We calculate the spectra and MCFT rate for both localized and delocalized systems, and calibrate the analytical 2nd-order cumulant expansion with the exact stochastic path integral method. We present three essential findings: (i) The role of the initial entanglement between the donor and its bath is found to be crucial in both the emission spectrum and the MCFT rate. (ii) The absorption spectra obtained by the cumulant expansion method are nearly identical to the exact spectra for both localized and delocalized systems, even when the system-bath coupling is far from the perturbative regime. (iii) For the emission spectra, the cumulant expansion can give reliable results for localized systems, but fail to provide reliable spectra of the high-lying excited states of a delocalized system, when the system-bath coupling is large and the thermal energy is smal...Continue Reading

References

Sep 29, 1999·Proceedings of the National Academy of Sciences of the United States of America·M A BoppR M Hochstrasser
May 10, 2002·Quarterly Reviews of Biophysics·Xiche HuKlaus Schulten
Dec 10, 2002·Annual Review of Physical Chemistry·Gregory D Scholes
Jun 7, 2003·Science·David M Jonas
Jul 13, 2004·Physical Review Letters·Seogjoo JangRobert J Silbey
Jan 7, 2005·The Journal of Chemical Physics·Shilong YangJianshu Cao
Jan 6, 2006·The Journal of Chemical Physics·Mino Yang
Jul 21, 2006·The Journal of Physical Chemistry. B·Minhaeng ChoGraham R Fleming
Mar 28, 2008·Chemical Reviews·Minhaeng Cho
Apr 1, 2009·The Journal of Physical Chemistry. B·David BeljonneRobert J Silbey
Sep 11, 2009·The Journal of Chemical Physics·Liping ChenYijing Yan
Jun 10, 2010·Physical Chemistry Chemical Physics : PCCP·Vladimir I Novoderezhkin, Rienk van Grondelle
Mar 10, 2011·The Journal of Chemical Physics·Johan Strümpfer, Klaus Schulten
May 21, 2011·Physical Chemistry Chemical Physics : PCCP·Benedetta Mennucci, Carles Curutchet
Jun 7, 2012·The Journal of Chemical Physics·Chee Kong LeeJianshu Cao
Jul 5, 2012·The Journal of Chemical Physics·Jun YeJianshu Cao
May 8, 2013·Proceedings of the National Academy of Sciences of the United States of America·Liam ClearyJianshu Cao

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Citations

Aug 27, 2015·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Lipeng ChenYang Zhao
Feb 26, 2016·The Journal of Physical Chemistry Letters·Amrit PoudelMark A Ratner
Aug 25, 2015·The Journal of Chemical Physics·Jianlan WuZhoufei Tang
Apr 24, 2015·The Journal of Chemical Physics·Andrius GelzinisLeonas Valkunas
Sep 10, 2016·The Journal of Physical Chemistry Letters·Sima Baghbanzadeh, Ivan Kassal
May 4, 2017·The Journal of Physical Chemistry Letters·Liang-Yan HsuGeorge C Schatz
Jun 16, 2015·Physical Chemistry Chemical Physics : PCCP·Pengfei Huo, Thomas F Miller
Feb 24, 2016·Physical Chemistry Chemical Physics : PCCP·Sima Baghbanzadeh, Ivan Kassal
Dec 24, 2018·The Journal of Chemical Physics·Mike Reppert, Paul Brumer
Jul 3, 2020·The Journal of Chemical Physics·Eric R Heller, Jeremy O Richardson
Oct 13, 2018·Chemical Science·Matthew DuJoel Yuen-Zhou
Sep 10, 2018·The Journal of Chemical Physics·Xiangji Cai, Yujun Zheng
Jan 11, 2020·Scientific Reports·Xiangji Cai
May 8, 2018·Chemical Science·Natasha B Taylor, Ivan Kassal
Sep 25, 2017·The Journal of Chemical Physics·Andrius GelzinisLeonas Valkunas
Apr 15, 2020·Science Advances·Jianshu CaoDonatas Zigmantas
Dec 16, 2019·The Journal of Chemical Physics·Zhihao Gong, Jianlan Wu
Feb 10, 2020·The Journal of Chemical Physics·Andrius Gelzinis, Leonas Valkunas
Jan 1, 2021·The Journal of Chemical Physics·Veljko Janković, Tomáš Mančal
Sep 10, 2020·The Journal of Physical Chemistry. B·Lorenzo CupelliniJianshu Cao
Apr 10, 2021·The Journal of Chemical Physics·Sangita MondalBiman Bagchi
Jun 29, 2021·The Journal of Physical Chemistry Letters·Stefano TomasiIvan Kassal
Aug 7, 2021·Physical Review Letters·Chern Chuang, Jianshu Cao
Aug 12, 2015·The Journal of Physical Chemistry Letters·Jianlan WuShaul Mukamel
Aug 14, 2020·The Journal of Physical Chemistry Letters·Pei-Yun Yang, Jianshu Cao
Dec 7, 2018·Chemical Reviews·Teresa L MakoMindy Levine
Oct 29, 2019·The Journal of Physical Chemistry. B·Shinji SaitoGraham R Fleming
Oct 8, 2021·Journal of Chemical Theory and Computation·Yakov BraverAndrius Gelzinis

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