Field-resolved THz-pump laser-probe measurements with CEP-unstable THz light sources.

Radiation sources with a stable carrier-envelope phase (CEP) are highly demanded tools for field-resolved studies of light-matter interaction, providing access both to the amplitude and phase information of dynamical processes. At the same time, many coherent light sources, including those with outstanding power and spectral characteristics lack CEP stability, and so far could not be used for this type of research. In this work, we present a method enabling linear and non-linear phase-resolved terahertz (THz) -pump laser-probe experiments with CEP-unstable THz sources. THz CEP information for each pulse is extracted using a specially designed electro-optical detection scheme. The method correlates the extracted CEP value for each pulse with the THz-induced response in the parallel pump-probe experiment to obtain an absolute phase-resolved response after proper sorting and averaging. As a proof-of-concept, we demonstrate experimentally field-resolved THz time-domain spectroscopy with sub-cycle temporal resolution using the pulsed radiation of a CEP-unstable infrared free-electron laser (IR-FEL) operating at 13 MHz repetition rate. In spite of the long history of IR-FELs and their unique operational characteristics, no successful realization of CEP-stable operation has been demonstrated yet. Being CEP-unstable, IR-FEL radiation has so far only been used in non-coherent measurements without phase resolution. The technique demonstrated here is robust, operates easily at high-repetition rates and for short THz pulses, and enables common sequential field-resolved time-domain experiments. The implementation of such a technique at IR-FEL user end-stations will facilitate a new class of linear and non-linear experiments for studying coherent light-driven phenomena with increased signal-to-noise ratio.

Inhibition of Neutrophil Elastase and Cathepsin G As a New Approach to the Treatment of Psoriasis: From Fundamental Biology to Development of New Target-Specific Drugs.

Psoriasis therapy remains an extremely relevant area of modern drug design, due to necessity of adverse reaction reduction, inherent for actual methods of therapy. It was established that two serine proteases-neutrophil elastase 1 (HNE1) and cathepsin G (CatG)-are the key agents in psoriasis development. The collected molecular data for the presented targets form the basis for the molecular modeling strategy for the search for and identification of new target-specific inhibitors. The result of this work is a group of high-priority small-molecule compounds with double-targeted affinity, which are able to suppress the pro-psoriatic processes induced by the considered serine proteases at the initial stage of the disease.

Doubly Dressed Bosons: Exciton Polaritons in a Strong Terahertz Field.

We demonstrate the existence of a novel quasiparticle, an exciton in a semiconductor doubly dressed with two photons of different wavelengths: a near infrared cavity photon and terahertz (THz) photon, with the THz coupling strength approaching the ultrastrong coupling regime. This quasiparticle is composed of three different bosons, being a mixture of a matter-light quasiparticle. Our observations are confirmed by a detailed theoretical analysis, treating quantum mechanically all three bosonic fields. The doubly dressed quasiparticles retain the bosonic nature of their constituents, but their internal quantum structure strongly depends on the intensity of the applied terahertz field.

Slow Noncollinear Coulomb Scattering in the Vicinity of the Dirac Point in Graphene.

The Coulomb scattering dynamics in graphene in energetic proximity to the Dirac point is investigated by polarization resolved pump-probe spectroscopy and microscopic theory. Collinear Coulomb scattering rapidly thermalizes the carrier distribution in k directions pointing radially away from the Dirac point. Our study reveals, however, that, in almost intrinsic graphene, full thermalization in all directions relying on noncollinear scattering is much slower. For low photon energies, carrier-optical-phonon processes are strongly suppressed and Coulomb mediated noncollinear scattering is remarkably slow, namely on a ps time scale. This effect is very promising for infrared and THz devices based on hot carrier effects.

Pressure-dependent structural and electronic properties of quasi-one-dimensional (TMTTF)2PF6.

We have performed detailed x-ray investigations of the quasi-one-dimensional organic conductor (TMTTF)(2)PF(6) at room temperature and hydrostatic pressures up to 27 kbar. Based on the pressure-dependent crystal structure, the electronic band structure was calculated by density functional theory (DFT). Our systematic study provides important information on the coupling among the organic molecules but also to the anions. We discuss the consequences for the electronic properties and compare them with optical investigations under pressure. The increasing plasma frequency observed perpendicular to the stacks corresponds to a widening of the bands for the b-direction. Around 20 kbar a dimensional crossover occurs from a one-dimensional Mott insulator to a two-dimensional metal.

Nonperturbative interband response of a bulk InSb semiconductor driven off resonantly by terahertz electromagnetic few-cycle pulses.

Intense multiterahertz pulses are used to study the coherent nonlinear response of bulk InSb by means of field-resolved four-wave mixing spectroscopy. At amplitudes above 5 MV/cm the signals show a clear temporal substructure which is unexpected in perturbative nonlinear optics. Simulations based on a model of a two-level quantum system demonstrate that in spite of the strongly off-resonant character of the excitation the high-field few-cycle pulses drive the interband resonances into a nonperturbative regime of Rabi flopping. The rotating wave approximation breaks down in this case and the system reaches a complete population inversion.

Ultrafast transient generation of spin-density-wave order in the normal state of BaFe2As2 driven by coherent lattice vibrations.

The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing order. Here, we employ few-cycle multi-terahertz pulses to resonantly probe the evolution of the spin-density-wave (SDW) gap of the pnictide compound BaFe(2)As(2) following excitation with a femtosecond optical pulse. When starting in the low-temperature ground state, optical excitation results in a melting of the SDW order, followed by ultrafast recovery. In contrast, the SDW gap is induced when we excite the normal state above the transition temperature. Very surprisingly, the transient ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. Our results attest to a pronounced spin-phonon coupling in pnictides that supports rapid development of a macroscopic order on small vibrational displacement even without breaking the symmetry of the crystal.

Femtosecond response of quasiparticles and phonons in superconducting YBa(2)Cu(3)O(7-δ) studied by wideband terahertz spectroscopy.

We measure the anisotropic midinfrared response of electrons and phonons in bulk YBa(2)Cu(3)O(7-δ) after femtosecond photoexcitation. A line shape analysis of specific lattice modes reveals their transient occupation and coupling to the superconducting condensate. The apex oxygen vibration is strongly excited within 150 fs, demonstrating that the lattice absorbs a major portion of the pump energy before the quasiparticles are thermalized. Our results attest to substantial electron-phonon scattering and introduce a powerful concept probing electron-lattice interactions in a variety of complex materials.

Highly tunable photonic crystal filter for the terahertz range.

By use of an incipient ferroelectric, SrTiO3, as a defect material inserted into a periodic structure of alternating layers of quartz and high-permittivity ceramic, thermal tuning of a single defect mode over the entire lowest forbidden band was obtained. The tunability of this compact structure reached 60%.

Infrared spectroscopy of KTa(1-x)Nb(x)O(3) crystals.

Fourier-transform infrared and time-domain THz dielectric spectroscopy measurements on KTa(1-x)Nb(x)O(3) crystals for x = 0.018 and 0.022 were performed. The temperature behaviour of the soft mode frequency and damping have been determined above the ferroelectric phase transition. No dielectric dispersion in the frequency range below the polar phonon absorption is observed down to kHz frequencies at temperatures from room temperature down to 60 K. At lower temperatures the KTa(1-x)Nb(x)O(3) samples become opaque due to additional losses, which persist down to liquid helium temperatures. This supports the nanoscopic dipolar glassy state rather than macroscopic ferroelectricity at low temperatures.