Publication

Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems

Kunsel, T., Tiwari, V., Matutes, Y. A., Gardiner, A. T., Cogdell, R. J., Ogilvie, J. P. & Jansen, T. L. C., 17-Jan-2019, In : Journal of Physical Chemistry B. 123, 2, p. 394-406 13 p.

Research output: Contribution to journalArticleAcademicpeer-review

APA

Kunsel, T., Tiwari, V., Matutes, Y. A., Gardiner, A. T., Cogdell, R. J., Ogilvie, J. P., & Jansen, T. L. C. (2019). Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems. Journal of Physical Chemistry B, 123(2), 394-406. https://doi.org/10.1021/acs.jpcb.8b10176

Author

Kunsel, Tenzin ; Tiwari, Vivek ; Matutes, Yassel Acosta ; Gardiner, Alastair T. ; Cogdell, Richard J. ; Ogilvie, Jennifer P. ; Jansen, Thomas L. C. / Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems. In: Journal of Physical Chemistry B. 2019 ; Vol. 123, No. 2. pp. 394-406.

Harvard

Kunsel, T, Tiwari, V, Matutes, YA, Gardiner, AT, Cogdell, RJ, Ogilvie, JP & Jansen, TLC 2019, 'Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems' Journal of Physical Chemistry B, vol. 123, no. 2, pp. 394-406. https://doi.org/10.1021/acs.jpcb.8b10176

Standard

Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems. / Kunsel, Tenzin; Tiwari, Vivek; Matutes, Yassel Acosta; Gardiner, Alastair T.; Cogdell, Richard J.; Ogilvie, Jennifer P.; Jansen, Thomas L. C.

In: Journal of Physical Chemistry B, Vol. 123, No. 2, 17.01.2019, p. 394-406.

Research output: Contribution to journalArticleAcademicpeer-review

Vancouver

Kunsel T, Tiwari V, Matutes YA, Gardiner AT, Cogdell RJ, Ogilvie JP et al. Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems. Journal of Physical Chemistry B. 2019 Jan 17;123(2):394-406. https://doi.org/10.1021/acs.jpcb.8b10176


BibTeX

@article{7c6c307881d842bca8bcede8757b8c0a,
title = "Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems",
abstract = "We present a theory for modeling fluorescence-detected two-dimensional electronic spectroscopy of multichromophoric systems. The theory is tested by comparison of the predicted spectra of the light-harvesting complex LH2 with experimental data. A qualitative explanation of the strong cross-peaks as compared to conventional two-dimensional electronic spectra is given. The strong cross-peaks are attributed to the clean ground-state signal that is revealed when the annihilation of exciton pairs created on the same LH2 complex cancels oppositely signed signals from the doubly excited state. This annihilation process occurs much faster than the nonradiative relaxation. Furthermore, the line shape difference is attributed to slow dynamics, exciton delocalization within the bands, and intraband exciton-exciton annihilation. This is in line with existing theories presented for model systems. We further propose the use of time-resolved fluorescence-detected two-dimensional spectroscopy to study state-resolved exciton-exciton annihilation.",
keywords = "LIGHT-HARVESTING COMPLEX, EXCITON-EXCITON ANNIHILATION, LH2 ANTENNA COMPLEX, ENERGY-TRANSFER, RHODOPSEUDOMONAS-ACIDOPHILA, RHODOBACTER-SPHAEROIDES, PERIPHERAL ANTENNA, SPECTRAL VARIANTS, CRYSTAL-STRUCTURE, IR-SPECTROSCOPY",
author = "Tenzin Kunsel and Vivek Tiwari and Matutes, {Yassel Acosta} and Gardiner, {Alastair T.} and Cogdell, {Richard J.} and Ogilvie, {Jennifer P.} and Jansen, {Thomas L. C.}",
year = "2019",
month = "1",
day = "17",
doi = "10.1021/acs.jpcb.8b10176",
language = "English",
volume = "123",
pages = "394--406",
journal = "The Journal of Physical Chemistry. B: Materials, Surfaces, Interfaces, & Biophysical",
issn = "1520-6106",
publisher = "AMER CHEMICAL SOC",
number = "2",

}

RIS

TY - JOUR

T1 - Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems

AU - Kunsel, Tenzin

AU - Tiwari, Vivek

AU - Matutes, Yassel Acosta

AU - Gardiner, Alastair T.

AU - Cogdell, Richard J.

AU - Ogilvie, Jennifer P.

AU - Jansen, Thomas L. C.

PY - 2019/1/17

Y1 - 2019/1/17

N2 - We present a theory for modeling fluorescence-detected two-dimensional electronic spectroscopy of multichromophoric systems. The theory is tested by comparison of the predicted spectra of the light-harvesting complex LH2 with experimental data. A qualitative explanation of the strong cross-peaks as compared to conventional two-dimensional electronic spectra is given. The strong cross-peaks are attributed to the clean ground-state signal that is revealed when the annihilation of exciton pairs created on the same LH2 complex cancels oppositely signed signals from the doubly excited state. This annihilation process occurs much faster than the nonradiative relaxation. Furthermore, the line shape difference is attributed to slow dynamics, exciton delocalization within the bands, and intraband exciton-exciton annihilation. This is in line with existing theories presented for model systems. We further propose the use of time-resolved fluorescence-detected two-dimensional spectroscopy to study state-resolved exciton-exciton annihilation.

AB - We present a theory for modeling fluorescence-detected two-dimensional electronic spectroscopy of multichromophoric systems. The theory is tested by comparison of the predicted spectra of the light-harvesting complex LH2 with experimental data. A qualitative explanation of the strong cross-peaks as compared to conventional two-dimensional electronic spectra is given. The strong cross-peaks are attributed to the clean ground-state signal that is revealed when the annihilation of exciton pairs created on the same LH2 complex cancels oppositely signed signals from the doubly excited state. This annihilation process occurs much faster than the nonradiative relaxation. Furthermore, the line shape difference is attributed to slow dynamics, exciton delocalization within the bands, and intraband exciton-exciton annihilation. This is in line with existing theories presented for model systems. We further propose the use of time-resolved fluorescence-detected two-dimensional spectroscopy to study state-resolved exciton-exciton annihilation.

KW - LIGHT-HARVESTING COMPLEX

KW - EXCITON-EXCITON ANNIHILATION

KW - LH2 ANTENNA COMPLEX

KW - ENERGY-TRANSFER

KW - RHODOPSEUDOMONAS-ACIDOPHILA

KW - RHODOBACTER-SPHAEROIDES

KW - PERIPHERAL ANTENNA

KW - SPECTRAL VARIANTS

KW - CRYSTAL-STRUCTURE

KW - IR-SPECTROSCOPY

U2 - 10.1021/acs.jpcb.8b10176

DO - 10.1021/acs.jpcb.8b10176

M3 - Article

VL - 123

SP - 394

EP - 406

JO - The Journal of Physical Chemistry. B: Materials, Surfaces, Interfaces, & Biophysical

JF - The Journal of Physical Chemistry. B: Materials, Surfaces, Interfaces, & Biophysical

SN - 1520-6106

IS - 2

ER -

ID: 75559647