The liquid and supercooled states of water show a series of anomalies whose nature is debated. A key role is attributed to the formation of structural aggregates induced by critical phenomena occurring deep in the supercooled region; the nature of the water anomalies and of the hidden critical processes remains elusive. Here we report a time-resolved optical Kerr effect investigation of the vibrational dynamics and relaxation processes in supercooled bulk water. The experiment measures the water intermolecular vibrations and the structural relaxation process in an extended temperature range, and with unprecedented data quality. A mode-coupling analysis of the experimental data enables to characterize the intermolecular vibrational modes and their interplay with the structural relaxation process. The results bring evidence of the coexistence of two local configurations, which are interpreted as high-density and low-density water forms, with an increasing weight of the latter at low temperatures.

The major development recently undergone by quantum cascade lasers has effectively extended frequency comb emission to longer-wavelength spectral regions, i.e. the mid and far infrared. Unlike classical pulsed frequency combs, their mode-locking mechanism relies on four-wave mixing nonlinear processes, with a temporal intensity profile different from conventional short-pulses trains. Measuring the absolute phase pattern of the modes in these combs enables a thorough characterization of the onset of mode-locking in absence of shortpulses emission, as well as of the coherence properties.Here, by combining dual-comb multi-heterodyne detection with Fourier-transform analysis, we show how to simultaneously acquire and monitor over a wide range of timescales the phase pattern of a generic frequency comb. The technique is applied to characterize a mid-infrared and a terahertz quantum cascade laser frequency comb, conclusively proving the high degree of coherence and the remarkable long-term stability of these sources. Moreover, the technique allows also the reconstruction of electric field, intensity profile and instantaneous frequency of the emission. IntroductionThe optical frequency comb (FC) is a peculiar multi-frequency coherent photonic state made of a series of evenly-spaced modes in the frequency domain, typically generated by frequency-stabilized and controlled femtoseconds mode-locked lasers [1][2][3][4]. In the visible and near infrared (IR) such technology is nowadays well established [5]. The miniaturization of these sources, together with the expansion of their operation range towards other spectral regions (e.g. mid and far IR), is crucial for broadening their application range.In this direction, the most interesting results have recently been achieved with quantum cascade lasers (QCLs), current-driven semiconductor lasers based on intersubband transitions in quantum wells, emitting high-power coherent radiation in the mid IR and terahertz (THz) [6][7][8][9][10][11]. In

The time-resolved optical Kerr effect spectroscopy (OKE) is a powerful experimental tool enabling accurate investigations of the dynamic phenomena in molecular liquids. We introduced innovative experimental and fitting procedures, that permit a safe deconvolution of sample response function from the instrumental function. This is a critical issue in order to measure the dynamics of sample presenting weak signal, e.g. liquid water. We report OKE data on water measuring intermolecular vibrations and the structural relaxation processes in an extended temperature range, inclusive of the supercooled states. The unpreceded data quality makes possible a solid comparison with few theoretical models; the multi-mode Brownian oscillator model, the Kubo's discrete random jump model and the schematic mode-coupling model. All these models produce reasonable good fits of the OKE data of stable liquid water, i.e. over the freezing point. The features of water dynamics in the OKE data becomes unambiguous only at lower temperatures, i.e. for water in the metastable supercooled phase. Hence this data enable a valid comparison between the model fits. We found that the schematic mode-coupling model provides the more rigorous and complete model for water dynamics, even if is intrinsic hydrodynamic approach hide the molecular informations.

We present an experiment where Ramsey-type spectroscopy is applied to autoionizing states of krypton by using the ninth harmonic (88 nm) of a femtosecond Ti:sapphire laser. The ionization process, detected by an electron-energy spectrometer, shows the characteristic quantum interference pattern. The behavior of the fringe contrast compares favorably with a simple essential-state model, whose parameters have been taken from the literature. The experiment shows the feasibility of high-resolution spectroscopy in the extreme ultraviolet by using high-order laser harmonics.