On the linear response and scattering of an interacting molecule-metal system

A many-body Green's function approach to the microscopic theory of plasmon-enhanced spectroscopy is presented within the context of localized surface-plasmon resonance spectroscopy and applied to investigate the coupling between quantum-molecular and classical-plasmonic resonances in monolayer-coated silver nanoparticles. Electronic propagators or Green's functions, accounting for the repeated polarization interaction between a single molecule and its image in a nearby nanoscale metal, are explicitly computed and used to construct the linear-response properties of the combined molecule-metal system to an external electromagnetic perturbation. Shifting and finite lifetime of states appear rigorously and automatically within our approach and reveal an intricate coupling between molecule and metal not fully described by previous theories. Self-consistent incorporation of this quantum-molecular response into the continuum-electromagnetic scattering of the molecule-metal target is exploited to compute the localized surface-plasmon resonance wavelength shift with respect to the bare metal from first principles.Comment: under review at Journal of Chemical Physic

Optical Polarization Analogs in Inelastic Free Electron Scattering

Advances in the ability to manipulate free electron phase profiles within the electron microscope have spurred development of quantum-mechanical descriptions of electron energy loss (EEL) processes involving transitions between phase-shaped transverse states. Here, we elucidate an underlying connection between two ostensibly distinct optical polarization analogs identified in EEL experiments as manifestations of the same conserved scattering flux. Our work introduces a procedure for probing general tensorial target characteristics including global mode symmetries and local polarization

Time-dependent quantum many-body theory of identical bosons in a double well: Early time ballistic interferences of fragmented and number entangled states

A time-dependent multiconfigurational self-consistent field theory is presented to describe the many-body dynamics of a gas of identical bosonic atoms confined to an external trapping potential at zero temperature from first principles. A set of generalized evolution equations are developed, through the time-dependent variational principle, which account for the complete and self-consistent coupling between the expansion coefficients of each configuration and the underlying one-body wave functions within a restricted two state Fock space basis that includes the full effects of the condensate's mean field as well as atomic correlation. The resulting dynamical equations are a classical Hamiltonian system and, by construction, form a well-defined initial value problem. They are implemented in an efficient numerical algorithm. An example is presented, highlighting the generality of the theory, in which the ballistic expansion of a fragmented condensate ground state is compared to that of a macroscopic quantum superposition state, taken here to be a highly entangled number state, upon releasing the external trapping potential. Strikingly different many-body matter-wave dynamics emerge in each case, accentuating the role of both atomic correlation and mean-field effects in the two condensate states.Comment: 16 pages, 5 figure

X-ray white beam topography of self-organized domains in flux-grown BaTiO3 single crystals

The phenomenon of self-organization of domains into a “square-net pattern” in single-crystal, flux-grown BaTiO3 several degrees below the ferroelectric to paraelectric phase transition was investigated using in situ synchrotron x-ray topography. The tetragonal distortion of the crystal was determined by measuring the angular separation between the diffraction images received from 90° a and c domains in the projection topographs, and shows a rapid decrease towards 110 °C, the onset temperature for self-organization. The onset of self-organization is accompanied by bending of the {100} lattice planes parallel to the crystal surface, which produces a strain that persists up to and beyond the Curie temperature, where the crystal becomes cubic and the self-organized domains disappear. At the Curie point, the bending angle α100=8.1(±0.3)mrad is at a maximum and corresponds to the radius of curvature of the surface being 16.3(±0.6) mm

Active Control of Plasmonic–Photonic Interactions in a Microbubble Cavity

Active control of light–matter interactions using nanophotonic structures is critical for new modalities for solar energy production, cavity quantum electrodynamics (QED), and sensing, particularly at the single-particle level, where it underpins the creation of tunable nanophotonic networks. Coupled plasmonic–photonic systems show great promise toward these goals because of their subwavelength spatial confinement and ultrahigh-quality factors inherited from their respective components. Here, we present a microfluidic approach using microbubble whispering-gallery mode cavities to actively control plasmonic–photonic interactions at the single-particle level. By changing the solvent in the interior of the microbubble, control can be exerted on the interior dielectric constant and, thus, on the spatial overlap between the photonic and plasmonic modes. Qualitative agreement between experiment and simulation reveals the competing roles mode overlap and mode volume play in altering coupling strengths.journal articl