Abstract
Interatomic Coulombic decay (ICD) is a very efficient process by which high-energy radiation is redistributed between molecular systems, often producing a slow electron, which can be damaging to biological tissue. During ICD, an initially-ionised and highly-excited donor species undergoes a transition where an outer-valence electron moves to a lower-lying vacancy, transmitting a photon with sufficient energy to ionise an acceptor species placed close by. Traditionally the ICD process has been described via ab initio quantum chemistry based on electrostatics in free space, which cannot include the effects of retardation stemming from the finite speed of light, nor the influence of a dispersive, absorbing, discontinuous environment. Here we develop a theoretical description of ICD based on macroscopic quantum electrodynamics in dielectrics, which fully incorporates all these effects, enabling the established power and broad applicability of macroscopic quantum electrodynamics to be unleashed across the fast-developing field of ICD.
Highlights
Interatomic Coulombic decay (ICD) is a very efficient process by which high-energy radiation is redistributed between molecular systems, often producing a slow electron, which can be damaging to biological tissue
Its origin is the coupling of the atom to the quantum electrodynamical vacuum field that permeates all of space, so while being originally thought of as a fundamental atomic property, spontaneous emission can be tuned by placing the emitter in an environment that modifies the vacuum state—between mirrors, for example
The explanation of a previously known effect in terms of a more fundamental theory, quantum electrodynamics (QED), led to the prediction of new physics, later verified in experiments. This is the blueprint we wish to follow in the present study of interatomic Coulombic decay (ICD)
Summary
Interatomic Coulombic decay (ICD) is a very efficient process by which high-energy radiation is redistributed between molecular systems, often producing a slow electron, which can be damaging to biological tissue. For donor and acceptor situated near a macroscopic body, we predict that the ICD rate can be enhanced or suppressed due to resonant interactions with surface plasmons.
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