Gouy phase effects on photocurrents in plasmonic nanogaps driven by single-cycle pulses.

The investigation of optical phenomena in the strong-field regime requires few-cycle laser pulses at field strengths exceeding gigavolts per meter (GV/m). Surprisingly, such conditions can be reached by tightly focusing pJ-level pulses with nearly octave spanning optical bandwidth onto plasmonic nanostructures, exploiting the field-enhancement effect. In this situation, the Gouy phase of the focused beam can deviate significantly from the monochromatic scenario.

Sub-8-fs pulses in the visible to near-infrared by a degenerate optical parametric amplifier.

This work presents a single-stage optical parametric amplifier (OPA) operating at degeneracy (DOPA) and pumped by the third harmonic of a Yb:KGW laser system. This DOPA exploits the broad amplification bandwidth that occurs with type-I phase-matching in β-barium borate (BBO) when signal and idler overlap in the spectrum. The output pulses span from 590 to 780 nm (1.

Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas.

Molecular polaritons are hybrid light-matter states that emerge when a molecular transition strongly interacts with photons in a resonator. At optical frequencies, this interaction unlocks a way to explore and control new chemical phenomena at the nanoscale. Achieving such control at ultrafast timescales, however, is an outstanding challenge, as it requires a deep understanding of the dynamics of the collectively coupled molecular excitation and the light modes.

Ultrafast Thermionic Electron Injection Effects on Exciton Formation Dynamics at a van der Waals Semiconductor/Metal Interface.

Inorganic van der Waals bonded semiconductors such as transition metal dichalcogenides are the subject of intense research due to their electronic and optical properties which are promising for next-generation optoelectronic devices. In this context, understanding the carrier dynamics, as well as charge and energy transfer at the interface between metallic contacts and semiconductors, is crucial and yet quite unexplored. Here, we present an experimental study to measure the effect of mutual interaction between thermionically injected and directly excited carriers on the exciton formation dynamics in bulk WS.

Passively phase-locked Er:fiber source of single-cycle pulses in the near infrared with electro-optic timing modulation for field-resolved electron control.

A single-cycle light source in the near infrared is demonstrated enabling sensitive applications of ultrafast optical field control of electronic transport. The compact Er:fiber system generates passively phase-locked pulses with broadband spectra covering 150 THz to 350 THz at a duration of 4.2 fs and 40 MHz repetition rate.

Magneto-Optical Activity in Nonmagnetic Hyperbolic Nanoparticles.

Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical activity in nonmagnetic hyperbolic nanoparticles. We demonstrate that the magneto-optical response is driven by the hyperbolic dispersion via the coupling of metallic-induced electric and dielectric-induced magnetic dipolar optical modes with static magnetic fields.

Dynamics of electron-emission currents in plasmonic gaps induced by strong fields.

The dynamics of ultrafast electron currents triggered by femtosecond laser pulse irradiation of narrow gaps in a plasmonic dimer is studied using quantum mechanical Time-Dependent Density Functional Theory (TDDFT). The electrons are injected into the gap due to the optical field emission from the surfaces of the metal nanoparticles across the junction. Further evolution of the electron currents in the gap is governed by the locally enhanced electric fields.

Plasmonic mid-infrared third harmonic generation in germanium nanoantennas.

We demonstrate third harmonic generation in plasmonic antennas consisting of highly doped germanium grown on silicon substrates and designed to be resonant in the mid-infrared frequency range that is inaccessible with conventional nonlinear plasmonic materials. Owing to the near-field enhancement, the result is an ultrafast, subdiffraction, coherent light source with a wavelength tunable between 3 and 5 µm, and ideally overlapping with the fingerprint region of molecular vibrations. To observe the nonlinearity in this challenging spectral window, a high-power femtosecond laser system equipped with parametric frequency conversion in combination with an all-reflective confocal microscope setup is employed.

Switchable dissociation of excitons bound at strained CdTe/CdS interfaces.

Charge carrier dynamics of semiconductor nano-heterostructures are determined by band alignment and lattice mismatch of the adjacent materials. However, quantum efficiencies for the separation of excited charge carriers at such an interface are hard to predict and cannot yet be easily controlled. In this work we examine nanorods with a severely strained, axial CdTe/CdS interface using femtosecond transient absorption spectroscopy.

Incoherent Pathways of Charge Separation in Organic and Hybrid Solar Cells.

In this work, we investigate the exciton dissociation dynamics occurring at the donor:acceptor interface in organic and hybrid blends employed in the realization of photovoltaic cells. Fundamental differences in the charge separation process are studied with the organic semiconductor polymer poly(3-hexylthiophene) (P3HT) and either [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) or titanium dioxide (TiO) acting as the acceptor. By using ultrafast broad-band transient absorption spectroscopy with few-fs temporal resolution, we observe that in both cases the incoherent formation of free charges dominates the charge generation process.

Coherent field transients below 15 THz from phase-matched difference frequency generation in 4H-SiC.

We experimentally demonstrate tunable, phase-matched difference frequency generation covering the spectral region below 15 THz using 4H-SiC as a nonlinear crystal. This material combines a non-centrosymmetric lattice and strong birefringence with broadband transparency at low optical frequencies. Thorough refractive index measurements in the terahertz spectral range allow us to calculate phase-matching conditions for any near-infrared pump laser source.

Stimulated Raman scattering microscopy by Nyquist modulation of a two-branch ultrafast fiber source.

A highly stable setup for stimulated Raman scattering (SRS) microscopy is presented. It is based on a two-branch femtosecond Er:fiber laser operating at a 40 MHz repetition rate. One of the outputs is directly modulated at the Nyquist frequency with an integrated electro-optic modulator (EOM).

Optical Activation of Germanium Plasmonic Antennas in the Mid-Infrared.

Impulsive interband excitation with femtosecond near-infrared pulses establishes a plasma response in intrinsic germanium structures fabricated on a silicon substrate. This direct approach activates the plasmonic resonance of the Ge structures and enables their use as optical antennas up to the mid-infrared spectral range. The optical switching lasts for hundreds of picoseconds until charge recombination redshifts the plasma frequency.

615 fs pulses with 17 mJ energy generated by an Yb:thin-disk amplifier at 3 kHz repetition rate.

A combination of Er/Yb:fiber and Yb:thin-disk technology produces 615 fs pulses at 1030 nm with an average output power of 72 W. The regenerative amplifier allows variation of the repetition rate between 3 and 5 kHz with pulse energies from 13 to 17 mJ. A broadband and intense seed provided by the compact and versatile fiber front-end minimizes gain narrowing.

The nature of singlet exciton fission in carotenoid aggregates.

Singlet exciton fission allows the fast and efficient generation of two spin triplet states from one photoexcited singlet. It has the potential to improve organic photovoltaics, enabling efficient coupling to the blue to ultraviolet region of the solar spectrum to capture the energy generally lost as waste heat. However, many questions remain about the underlying fission mechanism.

Ultrafast intramolecular relaxation and wave-packet motion in a ruthenium-based supramolecular photocatalyst.

The hydrogen-evolving photocatalyst [(tbbpy)2 Ru(tpphz)Pd(Cl)2 ](2+) (tbbpy=4,4'-di-tert-butyl-2,2'-bipyridine, tpphz=tetrapyrido[3,2-a:2',3'-c:3'',2''-h:2''',3'''-j]phenazine) shows excitation-wavelength-dependent catalytic activity, which has been correlated to the localization of the initial excitation within the coordination sphere. In this contribution the excitation-wavelength dependence of the early excited-state relaxation and the occurrence of vibrational coherences are investigated by sub-20 fs transient absorption spectroscopy and DFT/TDDFT calculations. The comparison with the mononuclear precursor [(tbbpy)2 Ru(tpphz)](2+) highlights the influence of the catalytic center on these ultrafast processes.

Ultrastable fiber amplifier delivering 145-fs pulses with 6-μJ energy at 10-MHz repetition rate.

A high-power femtosecond Yb:fiber amplifier operating with exceptional noise performance and long-term stability is demonstrated. It generates a 10-MHz train of 145-fs pulses at 1.03 μm with peak powers above 36 MW.

Nonlinear photoluminescence spectrum of single gold nanostructures.

We investigate the multiphoton photoluminescence characteristics of gold nanoantennas fabricated from single crystals and polycrystalline films. By exciting these nanostructures with ultrashort pulses tunable in the near-infrared range, we observe distinct features in the broadband photoluminescence spectrum. By comparing antennas of different crystallinity and shape, we demonstrate that the nanoscopic geometry of plasmonic devices determines the shape of the emission spectra.

Coherent ultrafast charge transfer in an organic photovoltaic blend.

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.

2D IR spectroscopy with phase-locked pulse pairs from a birefringent delay line.

We introduce a new scheme for two-dimensional IR spectroscopy in the partially collinear pump-probe geometry. Translating birefringent wedges allow generating phase-locked pump pulses with exceptional phase stability, in a simple and compact setup. A He-Ne tracking scheme permits to scan continuously the acquisition time.

Wavepacket splitting and two-pathway deactivation in the photoexcited visual pigment isorhodopsin.

Isorhodopsin is the visual pigment analogue of rhodopsin. It shares the same opsin environment but it embeds 9-cis retinal instead of 11-cis. Its photoisomerization is three times slower and less effective.

Activated singlet exciton fission in a semiconducting polymer.

Singlet exciton fission is a spin-allowed process to generate two triplet excitons from a single absorbed photon. This phenomenon offers great potential in organic photovoltaics, but the mechanism remains poorly understood. Most reports to date have addressed intermolecular fission within small-molecular crystals.

Utilizing ancillary ligands to optimize the photophysical properties of 4H-imidazole ruthenium dyes.

Correlations between structural features and photophysical properties offer the possibility to design dyes with tailor-made properties. In this respect, the photophysical properties of a series of 4H-imidazole (4H-im) ruthenium dyes with varying chemical and electronic structures of the complex fragments [(tpy)Ru(4H-im)X] {tpy=4,4',4''-tri-tert-butyl-2,2':6',2''-terpyridine; X=Cl(-), NCS(-)} and [(bpy)2Ru(4H-im)](+) {bpy=4,4'-di-tert-butyl-2,2'-bipyridine} were investigated. Variation of the π-donor/acceptor properties of the ancillary ligands offers the possibility to tune the relative energies of the d donor and π* acceptor orbitals of 4H-im, which results in a shift in the Ru→4H-im (1)MLCT (MLCT=metal-to-ligand charge transfer) absorption band in the visible range.

Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system.

The efficient conversion of light into electricity or chemical fuels is a fundamental challenge. In artificial photosynthetic and photovoltaic devices, this conversion is generally thought to happen on ultrafast, femto-to-picosecond timescales and to involve an incoherent electron transfer process. In some biological systems, however, there is growing evidence that the coherent motion of electronic wavepackets is an essential primary step, raising questions about the role of quantum coherence in artificial devices.