Christoph Lienau

Exciton binding energies in carbon nanotubes from two-photon photoluminescence

Excitonic effects in the linear and nonlinear optical properties of single-walled carbon nanotubes are manifested by photoluminescence excitation experiments and ab initio calculations. One- and two-photon spectra showed a series of exciton states; their energy splitting is the fingerprint of excitonic interactions in carbon nanotubes. By ab initio calculations we determine the energies, wave functions, and symmetries of the excitonic states. Combining experiment and theory we find binding energies of

Coherent ultrafast charge transfer in an organic photovoltaic blend

0.3\char21{}0.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV}

Apertureless near-field optical microscopy: Tip–sample coupling in elastic light scattering

for nanotubes with diameters between 6.8 and

Ultrafast Manipulation of Strong Coupling in Metal−Molecular Aggregate Hybrid Nanostructures

9.0\phantom{\rule{0.3em}{0ex}}\mathrm{\AA{}}

Toward Plasmonics with Nanometer Precision: Nonlinear Optics of Helium-Ion Milled Gold Nanoantennas

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Shape resonance omni-directional terahertz filters with near-unity transmittance

Pull, pull, pulling electrons along Organic photovoltaics operate by transferring charge from a light-absorbing donor material to a nearby acceptor. Falke et al. show that molecular vibrations smooth the way for this charge transfer to proceed. A combination of ultrafast spectroscopy and theoretical simulations revealed an oscillatory signal in a model donor/acceptor blend that implicates carbon-carbon bond stretching in concert with the electronic transition. This vibrational/electronic, or vibronic, process maintains a quantum-mechanical phase relationship that guides the charge more rapidly and directly than an incoherent migration from donor to acceptor. Science, this issue p. 1001 Oscillations in ultrafast spectra implicate assistance from molecular vibrations in the operation of organic photovoltaics. Blends of conjugated polymers and fullerene derivatives are prototype systems for organic photovoltaic devices. The primary charge-generation mechanism involves a light-induced ultrafast electron transfer from the light-absorbing and electron-donating polymer to the fullerene electron acceptor. Here, we elucidate the initial quantum dynamics of this process. Experimentally, we observed coherent vibrational motion of the fullerene moiety after impulsive optical excitation of the polymer donor. Comparison with first-principle theoretical simulations evidences coherent electron transfer between donor and acceptor and oscillations of the transferred charge with a 25-femtosecond period matching that of the observed vibrational modes. Our results show that coherent vibronic coupling between electronic and nuclear degrees of freedom is of key importance in triggering charge delocalization and transfer in a noncovalently bound reference system.

Carrier-envelope phase effects on the strong-field photoemission of electrons from metallic nanostructures

For linear light scattering in apertureless scanning near-field optical microscopy, we have studied the correlations between the tip radius of the probe, signal strength, spatial resolution, and sample material. Pronounced variations of the near-field distance dependence on tip shape and dielectric function of the sample are observed. For very sharp metal tips, the scattered near-field signal decays on a 5 nm length scale. Despite this highly localized tip–sample coupling, the contrast is found to depend sensitively on the vertical composition of the sample on a length scale given by the penetration depth of the incident light. The resulting implications on the use of the technique as an analytic probe method are discussed.

Bethe-hole polarization analyser for the magnetic vector of light

We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.

Adiabatic Nanofocusing Scattering-Type Optical Nanoscopy of Individual Gold Nanoparticles

Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.

Ultrafast Electron Emission from a Sharp Metal Nanotaper Driven by Adiabatic Nanofocusing of Surface Plasmons

Terahertz transmission filters have been manufactured by perforating metal films with various geometric shapes using femtosecond laser machining. Two dimensional arrays of square, circular, rectangular, c-shaped, and epsilon-shaped holes all support over 99% transmission at specific frequencies determined by geometric shape, symmetry, polarization, and lattice constant. Our results show that plasmonic structures with different geometric shaped holes are extremely versatile, dependable, easy to control and easy to make terahertz filters.