The influence of retardation and dielectric environments on interatomic Coulombic decay

Hemmerich, Joshua Leo; Bennett, Robert; Buhmann, Stefan Yoshi

doi:10.1038/s41467-018-05091-x

Cited by 34 publications

(33 citation statements)

References 41 publications

(45 reference statements)

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“…Although ICD has considerable theoretical interest, there is evidence of its practical importance to biological chemistry; in particular, in the understanding of a DNA repair mechanism provided by the enzymes known as photolyases [222,223]. The theoretical developments of ICD often mirror those already established in RET-such as the effects of retardation, dielectric environments, a third body and virtual photons [224,225]. Clearly, more research in this exciting emerging field is required, with much still to learn in terms of its fundamental theory and applications.…”

Section: Energy Transfer At Non-optical Frequenciesmentioning

confidence: 99%

Resonance Energy Transfer: From Fundamental Theory to Recent Applications

2019

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Resonance energy transfer (RET), the transport of electronic energy from one atom or molecule to another, has significant importance to a number of diverse areas of science. Since the pioneering experiments on RET by Cario and Franck in 1922, the theoretical understanding of the process has been continually refined. This review presents a historical account of the post-Förster outlook on RET, based on quantum electrodynamics, up to the present-day viewpoint. It is through this quantum framework that the short-range, R −6 distance dependence of Förster theory was unified with the long-range, radiative transfer governed by the inverse-square law. Crucial to the theoretical knowledge of RET is the electric dipole-electric dipole coupling tensor; we outline its mathematical derivation with a view to explaining some key physical concepts of RET. The higher order interactions that involve magnetic dipoles and electric quadrupoles are also discussed. To conclude, a survey is provided on the latest research, which includes transfer between nanomaterials, enhancement due to surface plasmons, possibilities outside the usual ultraviolet or visible range and RET within a cavity.

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Section: Energy Transfer At Non-optical Frequenciesmentioning

confidence: 99%

Resonance Energy Transfer: From Fundamental Theory to Recent Applications

2019

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“…However, there is no equivalent of the virtual photon approximation for the three-body ICD process. This problem can be solved by making use of a macroscopic quantum electrodynamics (QED) based approach recently put forward in [10] where the effects of the environment near the decaying pair can be accounted for. It should be mentioned that the corresponding situation for Förster resonant energy transfer (FRET) has been investigated previously [11,12].In this Letter we develop the virtual photon approximation for three-body ICD and find agreement with ab initio data in the relevant regimes.…”

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confidence: 99%

“…The new theory allows us to readily investigate retardation and geometrical effects in three-body ICD, providing insight into long-range energy transfer processes and guiding future ab initio calculations. Our method is based on the recently-derived formula for the ICD rate in a generic medium [10];…”

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confidence: 99%

Virtual Photon Approximation for Three-Body Interatomic Coulombic Decay

et al. 2019

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Interatomic Coulombic decay (ICD) is a mechanism which allows microscopic objects to rapidly exchange energy. When the two objects are distant, the energy transfer between the donor and acceptor species takes place via the exchange of a virtual photon. On the contrary, recent ab initio calculations have revealed that the presence of a third passive species can significantly enhance the ICD rate at short distances due to the effects of electronic wave function overlap and charge transfer states [Phys. Rev. Lett. 119, 083403 (2017)]. Here, we develop a virtual photon description of three-body ICD, showing that a mediator atom can have a significant influence at much larger distances. In this regime, this impact is due to the scattering of virtual photons off the mediator, allowing for simple analytical results and being manifest in a distinct geometry-dependence which includes interference effects. As a striking example, we show that in the retarded regime ICD can be substantially enhanced or suppressed depending on the position of the ICD-inactive object, even if the latter is far from both donor and acceptor species.Interatomic Coulombic decay (ICD) is an ultrafast process by which energy can be transferred between microscopic objects (e.g. atoms, ions, clusters, quantum dots). First predicted just over two decades ago [1], it involves an excited donor species which then decays and transmits sufficient energy to a neighbouring acceptor species that the latter can be ionised. Since most of the excess energy of the donor is spent ejecting an electron from the acceptor, a slow electron is left in the continuum [2]. As well as being one of the experimental signatures of ICD [3], it has been shown that such slow electrons can be damaging in a biological context [4].The ICD rate is an important property in characterisation of the process. However, its computation is a challenging task. Most calculations of ICD rates use techniques adapted from computational quantum chemistry, necessitated by the donor and acceptor species being very closely spaced so that orbital overlap has a dramatic effect on the system [5,6]. However, at slightly larger distances it is possible to use a 'virtual photon approximation' [5]. There, the donor and acceptor are considered as separate objects coupled via the quantised electromagnetic field. This results in a simple analytic expression for the rate that depends on the single-body decay rate of the donor, the photoionisation cross-section of the acceptor and their mutual separation. This expression is often used as a consistency check for the large-distance behaviour of a particular quantum chemical calculation. Furthermore, an analytical formula for the ICD rate provides a simple means to investigate large systems based on the decomposition of the clusters into pairs [7,8].Recently, a type of three-body ICD mechanism known as superexchange was proposed [9]. Based on extensive ab initio calculations, it was shown that the rate of energy transfer can be substantially enhanced in the presence...

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“…The 1/ R 6 dependence is characteristic for energy transfer processes via dipole–dipole interaction as leading term; however, it needs to be corrected in the case of large excitation energies or in the presence of polarizable media due to additional quantum electrodynamic effects, usually leading to a considerable increase of the ICD width. 121 …”

Section: Theoretical Approachesmentioning

confidence: 99%

Interatomic and Intermolecular Coulombic Decay

et al. 2020

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Interatomic or intermolecular Coulombic decay (ICD) is a nonlocal electronic decay mechanism occurring in weakly bound matter. In an ICD process, energy released by electronic relaxation of an excited atom or molecule leads to ionization of a neighboring one via Coulombic electron interactions. ICD has been predicted theoretically in the mid nineties of the last century, and its existence has been confirmed experimentally approximately ten years later. Since then, a number of fundamental and applied aspects have been studied in this quickly growing field of research. This review provides an introduction to ICD and draws the connection to related energy transfer and ionization processes. The theoretical approaches for the description of ICD as well as the experimental techniques developed and employed for its investigation are described. The existing body of literature on experimental and theoretical studies of ICD processes in different atomic and molecular systems is reviewed.

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The influence of retardation and dielectric environments on interatomic Coulombic decay

Cited by 34 publications

References 41 publications

Resonance Energy Transfer: From Fundamental Theory to Recent Applications

Resonance Energy Transfer: From Fundamental Theory to Recent Applications

Virtual Photon Approximation for Three-Body Interatomic Coulombic Decay

Interatomic and Intermolecular Coulombic Decay

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