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.

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Ultrafast optical parametric amplifiers (OPAs) can provide, under suitable conditions, ultra-broad gain bandwidths and can thus be used as effective tools for the generation of widely tunable few-optical-cycle light pulses. In this paper we review recent work on the development of ultra-broadband OPAs and experimentally demonstrate pulses with durations approaching the single-cycle limit and almost continuous tunability from the visible to the mid-IR.

The generation of sub-optical-cycle, carrier-envelope phase-stable light pulses is one of the frontiers of ultrafast optics. The two key ingredients for sub-cycle pulse generation are bandwidths substantially exceeding one octave and accurate control of the spectral phase. These requirements are very challenging to satisfy with a single laser beam, and thus intense research activity is currently devoted to the coherent synthesis of pulses generated by separate sources. In this review we discuss the conceptual schemes and experimental tools that can be employed for the generation, amplification, control, and combination of separate light pulses. The main techniques for the spectrotemporal characterization of the synthesized fields are also described. We discuss recent implementations of coherent waveform synthesis: from the first demonstration of a single-cycle optical pulse by the addition of two pulse trains derived from a fiber laser, to the coherent combination of the outputs from optical parametric chirped-pulse amplifiers.

We report on a kHz, mJ-level, carrier-envelope phase (CEP)-stable ultrabroadband optical parametric chirped-pulse amplifier (OPCPA) at 2.1-μm wavelength, pumped by a high-energy, 14 ps, cryogenic Yb:YAG pump laser, and its application to high-order harmonic generation (HHG) with Xe. The pre-amplifier chain is pumped by a 12-ps Nd:YLF pump laser and both pump lasers are optically synchronized to the signal pulse of the OPCPA. An amplified pulse energy of 0.85 mJ was obtained at the final OPCPA stage with good beam profile. The pulse is compressed to 4.5 optical cycles (<32 fs) with a spectral bandwidth of 474 nm supporting 3.5 optical cycles. The CEP stability was measured to be 194 mrad and the super-fluorescence noise is estimated to be ~9%. First HHG results are demonstrated with Xe showing significant cutoff extension to >85 eV with an efficiency of ~10^-10 per harmonic, limited by the maximum gas pressure and flow into the chamber. This demonstrates the potential of this 2.1-μm source for scaling of photon energy and flux in the water-window range when applied to Ne and He at kHz repetition rate.

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

We introduce a simple approach for the efficient generation of tunable narrow-bandwidth picosecond pulses synchronized to broadband femtosecond ones. Second harmonic generation in the presence of large group velocity mismatch between the interacting pulses transfers a large fraction of the energy of a broadband fundamental frequency pulse into a narrowband second harmonic one. Using a periodically poled stoichiometric lithium tantalate crystal coupled to an infrared optical parametric amplifier, we generated 200-nJ pulses with spectral width lower than 8.5 cm(-1) and tunability from 720 to 890 nm. Energy scaling and extension of the tuning range are straightforward.