Deterministic spatio-temporal control of nano-optical fields in optical antennas and nano transmission lines

We show that pulse shaping techniques can be applied to tailor the ultrafast temporal response of the strongly confined and enhanced optical near fields in the feed gap of resonant optical antennas (ROAs). Using finite-difference time-domain (FDTD) simulations followed by Fourier transformation, we obtain the impulse response of a nano structure in the frequency domain, which allows obtaining its temporal response to any arbitrary pulse shape. We apply the method to achieve deterministic optimal temporal field compression in ROAs with reduced symmetry and in a two-wire transmission line connected to a symmetric dipole antenna. The method described here will be of importance for experiments involving coherent control of field propagation in nanophotonic structures and of light-induced processes in nanometer scale volumes.Comment: 5 pages, 5 figure

Dual-tip-enhanced ultrafast CARS nanoscopy

Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nanooptics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure design provides localized excitation sources for CARS by focusing incident laser pulses into subwavelength hot spots via two self-similar nanolens antennas connected by a waveguide. Hot-spot-selective dual-tip-enhanced CARS (2TECARS) nanospectra of DNA nucleobases are obtained by simulating optimized pump, Stokes and probe near fields using tips, laser polarization- and pulse-shaping. This technique may be used to explore ultrafast energy and electron transfer dynamics in real space with nanometre resolution and to develop novel approaches to DNA sequencing.Comment: 11 pages, 6 figure

Photosynthetic reaction center as a quantum heat engine

Two seemingly unrelated effects attributed to quantum coherence have been reported recently in natural and artificial light-harvesting systems. First, an enhanced solar cell efficiency was predicted and second, population oscillations were measured in photosynthetic antennae excited by sequences of coherent ultrashort laser pulses. Because both systems operate as quantum heat engines (QHEs) that convert the solar photon energy to useful work (electric currents or chemical energy, respectively), the question arises whether coherence could also enhance the photosynthetic yield. Here, we show that both effects arise from the same population–coherence coupling term which is induced by noise, does not require coherent light, and will therefore work for incoherent excitation under natural conditions of solar excitation. Charge separation in light-harvesting complexes occurs in a pair of tightly coupled chlorophylls (the special pair) at the heart of photosynthetic reaction centers of both plants and bacteria. We show the analogy between the energy level schemes of the special pair and of the laser/photocell QHEs, and that both population oscillations and enhanced yield have a common origin and are expected to coexist for typical parameters. We predict an enhanced yield of 27% in a QHE motivated by the reaction center. This suggests nature-mimicking architectures for artificial solar energy devices

Revisiting the optical properties of the FMO protein

We review the optical properties of the FMO complex as found by spectroscopic studies of the Qy band over the last two decades. This article emphasizes the different methods used, both experimental and theoretical, to elucidate the excitonic structure and dynamics of this pigment–protein complex

Coherent Control Protocol for Separating Energy-Transfer Pathways in Photosynthetic Complexes by Chiral Multidimensional Signals

Adaptive optimizations performed using a genetic algorithm are employed to construct optimal laser pulse configurations that separate spectroscopic features associated with the two main energy-transfer pathways in the third-order nonlinear optical response simulated for the Fenna–Matthews–Olson (FMO) photosynthetic complex from the green sulfur bacterium Chlorobium tepidum. Superpositions of chirality-induced tensor components in both collinear and noncollinear pulse configurations are analyzed. The optimal signals obtained by manipulating the ratios of various 2D spectral peaks reveal detailed information about the excitation dynamics. [Image: see text

Morphological fractal analysis of shape in cancer cells treated with combinations of microtubule-polymerizing and -depolymerizing agents

The current prognostic parameters, including tumor volume, biochemistry, or immunohistochemistry, are not sufficient to reflect the properties of cancer cells that distinguish them from normal cells. Our focus is to evaluate the effects of a combination of microtubule-polymerizing Taxol (R) and -depolymerizing colchicine on IAR20 PC1 liver cells by measuring the surface fractal dimension as a descriptor of two-dimensional vascular geometrical complexity. The fractal dimension offers a rapid means of assessing cell shape. Furthermore, we show correlations of fractal dimensions of cell contours with the latent factors from our previously employed cell shape analysis

From aluminum foil to two-dimensional nanocrystals using ultrasonic exfoliation

Al nanostructures have unique optical properties such as widely tunable surface plasmon resonances from deep UV to NIR that can be used for label-free fluorescence enhancement and surface-enhanced Raman scattering. Various Al nanostructures have been fabricated using sophisticated “top-down” lithographic and “bottom-up” colloidal methods. Here, we developed a simple and efficient method of synthesizing two-dimensional (2D) aluminum (Al) nanocrystals from commercially available Al foil using ultrasonic exfoliation under ambient environment. 2D Al nanocrystals with sizes from a few hundred nanometers to several micrometers and thickness in the tens of nanometers were isolated through centrifugation separation. The exfoliated 2D Al nanocrystals are covered with a passivated Al2O3 nanolayer. The determined exfoliation mechanism is a combination of the preferred cleavage along the (111) surface planes and layer-by-layer Al2O3 exfoliation from the surface of the 2D Al nanocrystals. We demonstrate that the 2D Al nanocrystals can be assembled at water/air interface and transferred to different substrates to form 2D Al nanocrystal films. These 2D Al nanocrystal films exhibit surface plasmon resonance in the visible spectral range and show enhanced Raman signals of adenine using a 532 nm excitation. These 2D Al nanocrystal films could be further developed for new optical and sensing applications