Low temperature-grown GaAs carrier lifetime evaluation by double optical pump terahertz time-domain emission spectroscopy.

We present the use of a "double optical pump" technique in terahertz time-domain emission spectroscopy as an alternative method to investigate the lifetime of photo-excited carriers in semiconductors. Compared to the commonly employed optical pump-probe transient photo-reflectance, this non-contact and room temperature characterization technique allows relative ease in achieving optical alignment. The technique was implemented to evaluate the carrier lifetime in low temperature-grown gallium arsenide (LT-GaAs). The carrier lifetime values deduced from "double optical pump" THz emission decay curves show good agreement with data obtained from standard transient photo-reflectance measurements on the same LT-GaAs samples grown at 250 °C and 310 °C.

A matter of symmetry: terahertz polarization detection properties of a multi-contact photoconductive antenna evaluated by a response matrix analysis.

While terahertz time domain spectroscopy (THz-TDS) is a well-established technique, polarization sensitive measurements are challenging due to the need of broadband polarization devices. Here, we characterize our recently introduced multi-contact photoconductive detector antenna with a response matrix analysis. We show that the lead lines attached to electrodes reduce the antenna symmetry and thereby influence the properties of the response matrices. With a wire grid polarizer, we simulate a sample influencing the polarization angle and the intensity of the incident THz pulse. Evaluating the measurements with the response matrix analysis, our results show a well agreement of the adjusted and measured polarization angles and intensities over a frequency range from 0.25 to 0.8 THz.

Dissecting the THz spectrum of liquid water from first principles via correlations in time and space.

Solvation of molecules in water is at the heart of a myriad of molecular phenomena and of crucial importance to understanding such diverse issues as chemical reactivity or biomolecular function. Complementing well-established approaches, it has been shown that laser spectroscopy in the THz frequency domain offers new insights into hydration from small solutes to proteins. Upon introducing spatially-resolved analyses of the absorption cross section by simulations, the sensitivity of THz spectroscopy is traced back to characteristic distance-dependent modulations of absorption intensities for bulk water. The prominent peak at approximately 200 cm(-1) is dominated by first-shell dynamics, whereas a concerted motion involving the second solvation shell contributes most significantly to the absorption at about 80 cm(-1) approximately 2.4 THz. The latter can be understood in terms of an umbrella-like motion of two hydrogen-bonded tetrahedra along the connecting hydrogen bond axis. Thus, a modification of the hydrogen bond network, e.g., due to the presence of a solute, is expected to affect vibrational motion and THz absorption intensity at least on a length scale that corresponds to two layers of solvating water molecules. This result provides a molecular mechanism explaining the experimentally determined sensitivity of absorption changes in the THz domain in terms of distinct, solute-induced dynamical properties in solvation shells of (bio)molecules--even in the absence of well-defined resonances.

Revealing the dynamics of ultrarelativistic non-equilibrium many-electron systems with phase space tomography.

The description of physical processes with many-particle systems is a key approach to the modeling of numerous physical systems. For example in storage rings, where ultrarelativistic particles are agglomerated in dense bunches, the modeling and measurement of their phase-space distribution is of paramount importance: at any time the phase-space distribution not only determines the complete space-time evolution but also provides fundamental performance characteristics for storage ring operation. Here, we demonstrate a non-destructive tomographic imaging technique for the 2D longitudinal phase-space distribution of ultrarelativistic electron bunches. For this purpose, we utilize a unique setup, which streams turn-by-turn near-field measurements of bunch profiles at MHz repetition rates. To demonstrate the feasibility of our method, we induce a non-equilibrium state and show that the phase-space distribution microstructuring as well as the phase-space distribution dynamics can be observed in great detail. Our approach offers a pathway to control ultrashort bunches and supports, as one example, the development of compact accelerators with low energy footprints.

Watching the low-frequency motions in aqueous salt solutions: the terahertz vibrational signatures of hydrated ions.

The details of ion hydration still raise fundamental questions relevant to a large variety of problems in chemistry and biology. The concept of water "structure breaking" and "structure making" by ions in aqueous solutions has been invoked to explain the Hofmeister series introduced over 100 years ago, which still provides the basis for the interpretation of experimental observations, in particular the stabilization/destabilization of biomolecules. Recent studies, using state-of-the-art experiments and molecular dynamics simulations, either challenge or support some key points of the structure maker/breaker concept, specifically regarding long-ranged ordering/disordering effects. Here, we report a systematic terahertz absorption spectroscopy and molecular dynamics simulation study of a series of aqueous solutions of divalent salts, which adds a new piece to the puzzle. The picture that emerges from the concentration dependence and assignment of the observed absorption features is one of a limited range of ion effects that is confined to the first solvation shell.

Communications: Polarity fluctuations of the protic ionic liquid ethylammonium nitrate in the terahertz regime.

We have measured the complex dielectric function of the protic ionic liquid ethylammonium nitrate in the frequency range between 0.15 and 1.8 THz with a terahertz time domain spectrometer. The experiments reveal a terahertz mode which can be described as a damped harmonic oscillator with a central frequency of 1.3 THz. The terahertz mode is assigned to an intermolecular vibration, presumably associated with hydrogen-bond dynamics. The data are combined with microwave data to represent the dielectric spectrum from quasistatic conditions up to 1.8 THz.

Rattling in the cage: ions as probes of sub-picosecond water network dynamics.

We present terahertz (THz) measurements of salt solutions that shed new light on the controversy over whether salts act as kosmotropes (structure makers) or chaotropes (structure breakers), which enhance or reduce the solvent order, respectively. We have carried out precise measurements of the concentration-dependent THz absorption coefficient of 15 solvated alkali halide salts around 85 cm(-1) (2.5 THz). In addition, we recorded overview spectra between 30 and 300 cm(-1) using a THz Fourier transform spectrometer for six alkali halides. For all solutions we found a linear increase of THz absorption compared to pure water (THz excess) with increasing solute concentration. These results suggest that the ions may be treated as simple defects in an H-bond network. They therefore cannot be characterized as either kosmotropes or chaotropes. Below 200 cm(-1), the observed THz excess of all salts can be described by a linear superposition of the water absorption and an additional absorption that is attributed to a rattling motion of the ions within the water network. By providing a comprehensive set of data for different salt solutions, we find that the solutions can all be very well described by a model that includes damped harmonic oscillations of the anions and cations within the water network. We find this model predicts the main features of THz spectra for a variety of salt solutions. The assumption of the existence of these ion rattling motions on sub-picosecond time scales is supported by THz Fourier transform spectroscopy of six alkali halides. Above 200 cm(-1) the excess is interpreted in terms of a change in the wing of the water network librational mode. Accompanying molecular dynamics simulations using the TIP3P water model support our conclusion and show that the fast sub-picosecond motions of the ions and their surroundings are almost decoupled. These findings provide a complete description of the solute-induced changes in the THz solvation dynamics for the investigated salts. Our results show that THz spectroscopy is a powerful experimental tool to establish a new view on the contributions of anions and cations to the structuring of water.

From self-organization in relativistic electron bunches to coherent synchrotron light: observation using a photonic time-stretch digitizer.

In recent and future synchrotron radiation facilities, relativistic electron bunches with increasingly high charge density are needed for producing brilliant light at various wavelengths, from X-rays to terahertz. In such conditions, interaction of electron bunches with their own emitted electromagnetic fields leads to instabilities and spontaneous formation of complex spatial structures. Understanding these instabilities is therefore key in most electron accelerators. However, investigations suffer from the lack of non-destructive recording tools for electron bunch shapes. In storage rings, most studies thus focus on the resulting emitted radiation. Here, we present measurements of the electric field in the immediate vicinity of the electron bunch in a storage ring, over many turns. For recording the ultrafast electric field, we designed a photonic time-stretch analog-to-digital converter with terasamples/second acquisition rate. We could thus observe the predicted link between spontaneous pattern formation and giant bursts of coherent synchrotron radiation in a storage ring.

Urea, a structure breaker? Answers from THz absorption spectroscopy.

There has been a controversial debate of whether urea can be regarded as structure breaker or a structure maker. Here, we present concentration and temperature dependent absorption coefficients of urea-water mixtures in the THz range (1.5-10 THz, 50-350 cm(-1)). Our results are in agreement with the hypothesis that urea adapts ideally into the water network. Using a semi-ideal chemical association model and accompanying MD simulations, the observed spectra could be decomposed in three contributions: one is attributed to bulk water, a second one to rattling modes of weakly solvated urea in the surrounding water cage, and the third part accounts for THz modes describing a doubly hydrogen bonded strong solvent-solute interaction. The bands attributed to the rattling motion of the solute scale linearly with concentration. The intensity of this contribution is temperature independent in contrast to the water and strongly solvated solute absorption. We find that even at high urea concentrations the majority of water retains a bulklike absorption spectrum, whereas only a small number (about 0.5-1.1 per urea on average) are strongly bound in the temperature range between 9 and 36 °C. The THz absorption data provide no evidence for urea aggregation in the concentration range investigated (1-10 M).