arXiv subjects

Dale Green

Publications and source records attributed to Dale Green.

8 recordsLinked to original sources

arXiv2026

Transversality Locks Longitudinal Gradients in Structured-Light Quadrupole Transitions

Electric quadrupole absorption is driven by optical field gradients, not by field amplitudes alone. This distinction is crucial for structured light, where a paraxially small longitudinal field can generate a leading-order longitudinal gradient. For fully vectorial Laguerre-Gaussian modes, Maxwell transversality locks this longitudinal gradient to the transverse structured gradient of the leading paraxial field. This locking is therefore a general electromagnetic constraint, not a focusing-dependent correction that can be removed independently. Decomposing the symmetric-traceless optical field-gradient tensor into spherical components reveals a strongly channel-selective response: the $\Delta m=0$ transition requires the longitudinal gradient at the retained order, the $\Delta m=\pm1$ channels receive scalar and vectorial nonparaxial corrections on top of the carrier-scale longitudinal derivative of the transverse field, and the $\Delta m=\pm2$ channels remain transverse at the same order. These results show that longitudinal optical structure can enter structured-light quadrupole transitions as an indispensable leading-gradient contribution, even when the longitudinal field amplitude itself is paraxially small.

physics.optics↗

arXiv2024

Indirect Communication Between Non-Markovian Baths

In this work we develop a model for an undamped vibration in the presence of an overdamped bath. This two-bath model involves a new derivation of the hierarchical equations of motion (HEOM) for an overdamped Lorentz-Drude (LD) environment that is summed together with an undamped oscillator (UO) bath, termed LDUO-HEOM. We show that information transfer occurs between the two baths, even in the absence of a direct coupling between the baths. This bath-system-bath, mediated information transfer leads to intricate non-Markovian dynamics. The model is analysed using expectation values of the bath coordinates and generates 2D electronic spectra that are in qualitative agreement with single-bath models. Furthermore, the model eliminates the additional superfluous damping introduced by the finite spectral width of the underdamped bath in our previous two-bath underdamped-overdamped, `bath vibration model' [J. Chem. Phys. 156, 084103 (2022)].

quant-ph↗

arXiv2024

Vibrational coherences in half-broadband 2D electronic spectroscopy: spectral filtering to identify excited state displacements

Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about displacements of excited state surfaces for key vibrational modes. Half-broadband 2DES (HB2DES) uses a PP configuration with a white light continuum probe to extend the detection range and resolve vibrational coherences in the excited state absorption (ESA). However, interpretation of these spectra is difficult as they are strongly dependent on the spectrum of the pump laser and the relative displacement of the excited states along the vibrational coordinates. We demonstrate the impact of these convoluting factors for a model based upon cresyl violet. Careful consideration of the position of the pump spectrum can be a powerful tool in resolving the ESA coherences to gain insights into excited state displacements. The paper also highlights the need for caution in considering the spectral window of the pulse when interpreting these spectra.

physics.chem-ph↗

arXiv2024

Topological-charge-dependent dichroism and birefringence of optical vortices

Material anisotropy and chirality produce polarization-dependent light-matter interactions. Absorption leads to linear and circular dichroism, whereas elastic forward scattering produces linear and circular birefringence. Here we highlight a form of dichroism and birefringence whereby ordered generic media display locally different absorption and scattering of a focused vortex beam that depends upon the sign of the topological charge $\ell$. The light-matter interactions described in this work manifest purely through dominant electric-dipole coupling mechanisms and depend on the paraxial parameter to first-order. Previous topological-charge-dependent light-matter interactions required the significantly weaker higher-order multipole moments and are proportional to the paraxial parameter to second-order. The result represents a method of probing the nano-optics of advanced materials and the topological properties of structured light.

physics.optics↗

arXiv2023

Customized optical chirality of vortex structured light through state and degree of polarization control

We show how both the ellipticity $\eta$ and degree of polarization $\textit{P}$ influences the extraordinary optical chirality properties of non-paraxial vortex beams. We find that, in stark contrast to paraxial optics and non-vortex modes, extremely rich and tuneable spatial distributions of optical chirality density can be produced by an optical vortex beam under tight focussing. We develop a theoretical description of how the optical chirality can be tailored for purpose by altering both the state $\eta$ and degree of polarization $\textit{P}$ of the input vortex mode, along with the magnitude and sign of optical orbital angular momentum via the pseudoscalar topological charge $\ell$. We expect that the results will have a significant role in both producing novel techniques and improving existing methods in chiral nano-optics and structured light photonics.

physics.optics↗

arXiv2023

Phonon Signatures in Photon Correlations

We show that the second-order, two-time correlation functions for phonons and photons emitted from a vibronic molecule in a thermal bath result in bunching and anti-bunching (a purely quantum effect), respectively. Signatures relating to phonon exchange with the environment are revealed in photon-photon correlations. We demonstrate that cross-correlation functions have a strong dependence on the order of detection giving insight into how phonon dynamics influences the emission of light. This work offers new opportunities to investigate quantum effects in condensed-phase molecular systems.

quant-ph↗

arXiv2021

Enantioselective optical gradient forces using 3D structured vortex light

Here we highlight enantioselective optical gradient forces present in 3D structured optical vortex tweezing systems. One chiral force originates from the circular polarization of the light, while remarkably the other is independent of the input polarization, even occurring for unpolarized light, and is not present in 2D structured light nor propagating plane waves. This latter chiral sorting mechanism allows for the enantioselective trapping of chiral particles into distinct rings in the transverse plane through conservative radial forces.

physics.optics↗

arXiv2020

Relevance of Longitudinal Fields of Paraxial Optical Vortices

Longitudinal electromagnetic fields generally become comparable with the usually dominant transverse components in strongly-focussed, non-paraxial beams. For optical vortex modes it is highlighted here how their angular momentum properties produce longitudinal fields that in general must be accounted for, even within the paraxial regime. First-order longitudinal components of quantized Laguerre-Gaussian modes are derived and numerically studied with respect to the paraxial parameter, highlighting light-matter and spin-orbit interactions that stem from longitudinal fields of weakly-focussed, paraxial beams in free space. New restrictions are cast on the validity of the paraxial approximation for optical vortices interacting with atoms, molecules and other nanostructures.

physics.optics↗