Resonance Energy Transfer in Arbitrary Media

Beyond the Point Dipole Approximation

K. Nasiri Avanaki, Wendu Ding, George C Schatz

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

In this work, we present a comprehensive theoretical and computational study of donor/acceptor resonance energy transfer (RET) beyond the dipole approximation, in arbitrary inhomogeneous and dispersive media. The theoretical method extends Förster theory for RET between particles (molecules or nanoparticles) to the case where higher multipole transitions in the donor and/or acceptor play a significant role in the energy transfer process. In our new formulation, the energy transfer matrix element is determined by a fully quantum electrodynamic expression, but its evaluation requires only classical electrodynamics calculations. By means of a time domain electrodynamical approach (TED), the matrix element evaluation involves the electric and magnetic fields generated by the donor and evaluated at the position of the acceptor, including fields associated with transition electric dipoles, electric quadrupoles, and magnetic dipoles in the donor, and the acceptor response to the electric and magnetic fields and to the electric field gradient. As an illustration of the benefits of the new formalism, we tested our method with a 512 atom lead sulfide (PbS) quantum dot as the donor/acceptor in vacuum, and with spherical nanoparticles (toy model) possessing designed transition multipoles. This includes an analysis of the effects of interferences between multipoles in the energy transfer rate. The results show important deviations from the conventional Förster dipole theory that are important even in vacuum but that can be amplified by interaction with a plasmonic nanoparticle.

Original languageEnglish
Pages (from-to)29445-29456
Number of pages12
JournalJournal of Physical Chemistry C
Volume122
Issue number51
DOIs
Publication statusPublished - Dec 27 2018

Fingerprint

Energy transfer
energy transfer
dipoles
multipoles
approximation
Electrodynamics
Electric fields
Nanoparticles
nanoparticles
electric fields
transferred electron devices
Vacuum
Magnetic fields
lead sulfides
vacuum
evaluation
quantum electrodynamics
magnetic dipoles
magnetic fields
electrodynamics

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Resonance Energy Transfer in Arbitrary Media : Beyond the Point Dipole Approximation. / Nasiri Avanaki, K.; Ding, Wendu; Schatz, George C.

In: Journal of Physical Chemistry C, Vol. 122, No. 51, 27.12.2018, p. 29445-29456.

Research output: Contribution to journalArticle

@article{dd98c5d5374f46d39172a2effbefda86,
title = "Resonance Energy Transfer in Arbitrary Media: Beyond the Point Dipole Approximation",
abstract = "In this work, we present a comprehensive theoretical and computational study of donor/acceptor resonance energy transfer (RET) beyond the dipole approximation, in arbitrary inhomogeneous and dispersive media. The theoretical method extends F{\"o}rster theory for RET between particles (molecules or nanoparticles) to the case where higher multipole transitions in the donor and/or acceptor play a significant role in the energy transfer process. In our new formulation, the energy transfer matrix element is determined by a fully quantum electrodynamic expression, but its evaluation requires only classical electrodynamics calculations. By means of a time domain electrodynamical approach (TED), the matrix element evaluation involves the electric and magnetic fields generated by the donor and evaluated at the position of the acceptor, including fields associated with transition electric dipoles, electric quadrupoles, and magnetic dipoles in the donor, and the acceptor response to the electric and magnetic fields and to the electric field gradient. As an illustration of the benefits of the new formalism, we tested our method with a 512 atom lead sulfide (PbS) quantum dot as the donor/acceptor in vacuum, and with spherical nanoparticles (toy model) possessing designed transition multipoles. This includes an analysis of the effects of interferences between multipoles in the energy transfer rate. The results show important deviations from the conventional F{\"o}rster dipole theory that are important even in vacuum but that can be amplified by interaction with a plasmonic nanoparticle.",
author = "{Nasiri Avanaki}, K. and Wendu Ding and Schatz, {George C}",
year = "2018",
month = "12",
day = "27",
doi = "10.1021/acs.jpcc.8b07407",
language = "English",
volume = "122",
pages = "29445--29456",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "51",

}

TY - JOUR

T1 - Resonance Energy Transfer in Arbitrary Media

T2 - Beyond the Point Dipole Approximation

AU - Nasiri Avanaki, K.

AU - Ding, Wendu

AU - Schatz, George C

PY - 2018/12/27

Y1 - 2018/12/27

N2 - In this work, we present a comprehensive theoretical and computational study of donor/acceptor resonance energy transfer (RET) beyond the dipole approximation, in arbitrary inhomogeneous and dispersive media. The theoretical method extends Förster theory for RET between particles (molecules or nanoparticles) to the case where higher multipole transitions in the donor and/or acceptor play a significant role in the energy transfer process. In our new formulation, the energy transfer matrix element is determined by a fully quantum electrodynamic expression, but its evaluation requires only classical electrodynamics calculations. By means of a time domain electrodynamical approach (TED), the matrix element evaluation involves the electric and magnetic fields generated by the donor and evaluated at the position of the acceptor, including fields associated with transition electric dipoles, electric quadrupoles, and magnetic dipoles in the donor, and the acceptor response to the electric and magnetic fields and to the electric field gradient. As an illustration of the benefits of the new formalism, we tested our method with a 512 atom lead sulfide (PbS) quantum dot as the donor/acceptor in vacuum, and with spherical nanoparticles (toy model) possessing designed transition multipoles. This includes an analysis of the effects of interferences between multipoles in the energy transfer rate. The results show important deviations from the conventional Förster dipole theory that are important even in vacuum but that can be amplified by interaction with a plasmonic nanoparticle.

AB - In this work, we present a comprehensive theoretical and computational study of donor/acceptor resonance energy transfer (RET) beyond the dipole approximation, in arbitrary inhomogeneous and dispersive media. The theoretical method extends Förster theory for RET between particles (molecules or nanoparticles) to the case where higher multipole transitions in the donor and/or acceptor play a significant role in the energy transfer process. In our new formulation, the energy transfer matrix element is determined by a fully quantum electrodynamic expression, but its evaluation requires only classical electrodynamics calculations. By means of a time domain electrodynamical approach (TED), the matrix element evaluation involves the electric and magnetic fields generated by the donor and evaluated at the position of the acceptor, including fields associated with transition electric dipoles, electric quadrupoles, and magnetic dipoles in the donor, and the acceptor response to the electric and magnetic fields and to the electric field gradient. As an illustration of the benefits of the new formalism, we tested our method with a 512 atom lead sulfide (PbS) quantum dot as the donor/acceptor in vacuum, and with spherical nanoparticles (toy model) possessing designed transition multipoles. This includes an analysis of the effects of interferences between multipoles in the energy transfer rate. The results show important deviations from the conventional Förster dipole theory that are important even in vacuum but that can be amplified by interaction with a plasmonic nanoparticle.

UR - http://www.scopus.com/inward/record.url?scp=85058810398&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85058810398&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.8b07407

DO - 10.1021/acs.jpcc.8b07407

M3 - Article

VL - 122

SP - 29445

EP - 29456

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 51

ER -