Synergistic Effects in Two‐Photon Absorption: the Quantum Electrodynamics of Bimolecular Mean‐Frequency Absorption

Andrews, Davıd L.; Hopkins, Kevin

doi:10.1002/9780470141267.ch2

Cited by 18 publications

(3 citation statements)

References 111 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This mechanism results in entirely new features in the absorption spectrum, allowing for transitions that are forbidden without any such mutual interaction between molecules. Here, the effect was subsequently experimentally observed in matrixisolated solids, liquids, gases, and molecular beams [196][197][198][199][200][201][202]. Attention has recently been drawn to the connection between providing accurate descriptions of short-range interactions and making due allowance for causality, the latter emerging again, naturally, through the retarded field formulation that is intrinsic to QED [203].…”

Section: B Original Predictions Of Qedmentioning

confidence: 96%

Quantum electrodynamics in modern optics and photonics: tutorial

et al. 2020

Self Cite

View full text Add to dashboard Cite

One of the key frameworks for developing the theory of light-matter interactions in modern optics and photonics is quantum electrodynamics (QED). Contrasting with semiclassical theory, which depicts electromagnetic radiation as a classical wave, QED representations of quantized light fully embrace the concept of the photon. This tutorial review is a broad guide to cutting-edge applications of QED, providing an outline of its underlying foundation and an examination of its role in photon science. Alongside the full quantum methods, it is shown how significant distinctions can be drawn when compared to semiclassical approaches. Clear advantages in outcome arise in the predictive capacity and physical insights afforded by QED methods, which favors its adoption over other formulations of radiation-matter interaction.

show abstract

Section: B Original Predictions Of Qedmentioning

confidence: 96%

Quantum electrodynamics in modern optics and photonics: tutorial

et al. 2020

Self Cite

View full text Add to dashboard Cite

show abstract

“…The excitation energy is generally provided by the absorption of one or two simultaneously absorbed photons. Both experiment and theory are well developed, and the two-photon case has been reviewed recently (Andrews and Hopkins 1990). It has also recently been suggested that one-photon processes of this type might account for features in the water vapour absorption continuum (Hudis et a1 1991(Hudis et a1 , 1992.…”

Section: Introductionmentioning

confidence: 99%

Three-photon bimolecular absorption

Andrews¹,

Bittner²

1993

J. Phys. B: At. Mol. Opt. Phys.

View full text Add to dashboard Cite

Abstract. Three-photon bimolecular absorption is a process which, through the simultaneous absorption of three laser photons, resulrs in the demonic excitation of two molecules or atoms. Following a recent treatment of the selection rules, a quantum electrodynamical treatment is employed to describe the main features associated with the process and to produce an equation for the excitation rate. The dependence on photon polarization is investigated, and the magnitude of the excitation rate is estimated. It is shown that two different mechanisms operate, each with different selection rules and different dependences on intermolecular separation. In each case an energy mismatch is conveyed from one molecule to the other by means of virtual photon coupling. Some possible schemes for experimental study of the process are outlined.

show abstract

“…27 Although ostensibly similar in nature to ASERIT and TIDQE, respectively, they significantly differ in the constraints they impose on laser wavelength. Moreover, all the intermediate molecular states that participate in those mechanisms are virtual in nature; accordingly, the overall mechanisms are likely to occur with significantly lower levels of efficiency.…”

Section: Relative Efficiency Of Each Mechanismmentioning

confidence: 99%

Energy migration in molecular assemblies: the characterisation and differentiation of two-photon mechanisms

Andrews

2006

SPIE Proceedings

Self Cite

View full text Add to dashboard Cite

Energy migration between chromophores plays a prominent role in a range of energy harvesting assemblies. Recent advances in the design and production of light-harvesting polymers have led to the synthesis of novel two-photon absorbing dendrimers. To construct increasingly efficient multifunctional macromolecules of this type, understanding the inherent optical processes and disentangling them has become imperative. This paper explores the fundamental processes by means of which energy transfers from a donor chromophore to an acceptor through two-photon absorption from an input laser beam. It is determined that three distinct classes of mechanism can operate: (i) two-photon absorption by individual chromophores is followed by transfer of the energy to an acceptor group; (ii) a singly excited chromophore is excited to a virtual state by the additional absorption of a photon from the pump radiation field, coupled with resonance energy transfer to the acceptor, or; (iii) two-photon excitation of the acceptor results from acquisition of one quantum of energy from a singly excited neighbour group and another from the throughput radiation. These mechanisms may compete and, in certain cases, lead to manifestations of quantum interference. Generally, the most favoured mechanism is determined by a balance of factors and constraints. Principal amongst the latter are the choice of wavelength (connected with the possibility of exploiting certain electronic resonances, whilst judiciously avoiding others) and the precise chromophore architecture (taking account of geometric factors concerned with the relative orientation of transition moments). As the relative importance of each mechanism determines the key nanophotonic characteristics of the assembly, the principles and results reported here afford the means for expediting highly efficient two-photon energy migration.

show abstract

Synergistic Effects in Two‐Photon Absorption: the Quantum Electrodynamics of Bimolecular Mean‐Frequency Absorption

Cited by 18 publications

References 111 publications

Quantum electrodynamics in modern optics and photonics: tutorial

Quantum electrodynamics in modern optics and photonics: tutorial

Three-photon bimolecular absorption

Energy migration in molecular assemblies: the characterisation and differentiation of two-photon mechanisms

Contact Info

Product

Resources

About