TY - JOUR
T1 - Coherent-to-Incoherent Transition of Molecular Fluorescence Controlled by Surface Plasmon Polaritons
AU - Wang, Siwei
AU - Scholes, Gregory D.
AU - Hsu, Liang Yan
PY - 2020/8/6
Y1 - 2020/8/6
N2 - We investigate the coherent-to-incoherent transition of molecular fluorescence of a chromophore above a silver surface (including bulk and thin-film systems) and explore the distance dependence of fluorescence rate enhancement. In the framework of macroscopic quantum electrodynamics, we generalize our previous theory to include multiple vibrational modes. The present theory can accurately describe quantum dynamics from the coherent limit to the incoherent limit. Moreover, we introduce a new concept Incoherent Index to quantify the degree of quantum coherence and demonstrate that the coherent-to-incoherent transition can be controlled by the dielectric environment and the molecule-silver distance. In addition, our theory indicates that strong molecule-photon (polariton) coupling can be achieved by virtue of small Huang-Rhys factors, large transition dipole moments, and appropriate dielectric material design. The present study provides a new direction for engineering light-matter interactions in polaritonic chemistry.
AB - We investigate the coherent-to-incoherent transition of molecular fluorescence of a chromophore above a silver surface (including bulk and thin-film systems) and explore the distance dependence of fluorescence rate enhancement. In the framework of macroscopic quantum electrodynamics, we generalize our previous theory to include multiple vibrational modes. The present theory can accurately describe quantum dynamics from the coherent limit to the incoherent limit. Moreover, we introduce a new concept Incoherent Index to quantify the degree of quantum coherence and demonstrate that the coherent-to-incoherent transition can be controlled by the dielectric environment and the molecule-silver distance. In addition, our theory indicates that strong molecule-photon (polariton) coupling can be achieved by virtue of small Huang-Rhys factors, large transition dipole moments, and appropriate dielectric material design. The present study provides a new direction for engineering light-matter interactions in polaritonic chemistry.
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U2 - 10.1021/acs.jpclett.0c01680
DO - 10.1021/acs.jpclett.0c01680
M3 - Article
C2 - 32619095
AN - SCOPUS:85089617234
VL - 11
SP - 5948
EP - 5955
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 15
ER -