Radiation-molecule and molecule-molecule interactions. A unified viewpoint from quantum electrodynamics

Craig, D. P.; Thirunamachandran, T.

doi:10.1021/ar00121a002

Cited by 82 publications

(162 citation statements)

References 21 publications

(3 reference statements)

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“…To describe them, the interaction Hamiltonian in Eq. (1.1) has to include extra coupling terms of the molecular magnetic dipole and electric quadrupole moments with the electromagnetic wave [4]. As a result, the differences are in the order of 10 2 to 10 5 times smaller than usual responses arising from the electric dipole term in Eq.…”

Section: Sum-frequency Generation As a Probe Of Chiralitymentioning

confidence: 99%

Sum-Frequency Generation from Chiral Media and Interfaces

2006

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Professor Yuen-Ron Shen, Co-chair Professor Richard J. Saykally, Co-chair Sum frequency generation (SFG), a second-order nonlinear optical process, is electric-dipole forbidden in systems with inversion symmetry. As a result, it has been used to study chiral media and interfaces, systems intrinsically lacking inversion symmetry.This thesis describes recent progresses in the applications of and new insights into SFG from chiral media and interfaces.SFG from solutions of chiral amino acids is investigated, and a theoretical model explaining the origin and the strength of the chiral signal in electronic-resonance SFG spectroscopy is discussed. An interference scheme that allows us to distinguish enantiomers by measuring both the magnitude and the phase of the chiral SFG response is described, as well as a chiral SFG microscope producing chirality-sensitive images with sub-micron 2 resolution. Exploiting atomic and molecular parity nonconservation, the SFG process is also used to solve the Ozma problems.Sum frequency vibrational spectroscopy is used to obtain the adsorption behavior of leucine molecules at air-water interfaces. With poly(tetrafluoroethylene) as a model system, we extend the application of this surface-sensitive vibrational spectroscopy to fluorinecontaining polymers.

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Section: Sum-frequency Generation As a Probe Of Chiralitymentioning

confidence: 99%

Sum-Frequency Generation from Chiral Media and Interfaces

2006

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“…Fluctuations in the quantized vacuum field perturb electronic motions so that the antenna excited state is no longer a stationary state of the system, allowing decay transition to occur; the loss of excitation energy appears as a photon added to the field. 23 To implement the dipolar coupling operator (4), we use the following quantum field expansion of d ⊥ over a complete set of radiation modes (k,η):…”

Section: B Single-site Fluorescencementioning

confidence: 99%

“…First, summing over emission modes again using the density of radiation states, assuming A and B have a common orientation, Eqs. (19), (23), and (25) give…”

Section: One-photon Emission From a Pair With Localized Excitationmentioning

confidence: 99%

Optical emission of a molecular nanoantenna pair

Rice

Andrews

2012

The Journal of Chemical Physics

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The optical emission from a pair of nanoantennas is investigated within the theoretical framework of quantum electrodynamics. The analysis of fluorescent emission from a pair of molecular antenna species in close proximity is prompted by experimental work on oriented semiconductor polymer nanostructures. Each physically different possibility for separation-dependent features in photon emission by any such pair is explored in detail, leading to the identification of three distinct mechanisms: emission from a pair-delocalized exciton state, emission that engages electrodynamic coupling through quantum interference, and correlated photon emission from the two components of the pair. Although each mechanism produces a damped oscillatory dependence on the pair separation, each of the corresponding results exhibits an analytically different form. Significant differences in the associated spatial frequencies enable an apparent ambiguity in the interpretation of experiments to be resolved. Other major differences are found in the requisite conditions, the associated selection rules, and the variation with angular disposition of the emitters, together offering grounds for experimental discrimination between the coupling mechanisms. The analysis paves the way for investigations of pair-wise coupling effects in the emission from nanoantenna arrays.

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“…where V is the normalization volume [21]. The polarization vectors are taken to satisfy the and k = ( /c, k) are four-vectors so that their scalar product is k.x = t − k.x .…”

Section: Plane Waves: Quantum Mechanicalmentioning

confidence: 99%