Distinguishing Resonant from Non-Resonant Nonlinear Optical Processes Using Intensity–Intensity Correlation Analyses

Three-color coherent anti-Stokes Raman scattering (CARS) represents non-degenerate four wave mixing that includes both non-resonant and resonant processes, the contributions of which depend upon how the molecular vibrational modes are being excited by the input laser pulses. The scattering signal due to resonant processes builds up progressively. An advanced analytical tool to reveal this deferred resonant signal buildup phenomenon is in need. In this work, we adapt a quantitative analytical tool by introducing one-dimensional and two-dimensional intensity–intensity correlation functions in terms of a new variable (probe pulse delay) and a new perturbation parameter (probe pulse linewidth). In particular, discrete diagonal directional sums are defined here as a tool to reduce both synchronous and asynchronous two-dimensional correlation spectroscopy (2D-COS) maps down to one-dimensional plots while maintaining the valuable analytical information. Detailed analyses using the all-Gaussian coherent Raman scattering closed-form solutions and the representative experimental data for resonant and non-resonant processes are presented and compared. The present work holds a promising potential for industrial application, e.g., by extractive industries to distinguish hydrocarbons (chemically resonant substance) from water (non-resonant contaminant) by utilizing the one- and two-dimensional correlation analyses.

External Modulation Optical Coherent Domain Reflectometry with Long Measurement Range

Optical coherent domain reflectometry (OCDR) can achieve a high spatial resolution that is independent of the bandwidth of the receiver, but the measurement range is usually very limited. Here we propose an external modulation OCDR system, in which a pair of linear frequency-modulated pulses generated by one modulator are employed as the probe pulse and the reference, respectively. The spatial resolution is determined by the frequency modulation range of the pulse, and the measurement speed is boosted by orders because the proposed technology can simultaneously diagnose a section of fiber with each pair of pulses, while only a single point can be accessed at a time in typical OCDR. In the demonstrational experiment, a measurement range of up to 50 km is achieved with a spatial resolution of 1.4 m and a measuring time of less than 30 s.

In-situ diagnostic of femtosecond laser probe pulses for high resolution ultrafast imaging

Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack of characterization of weak probe beams. For pump–probe experiments realized within solids or liquids, because of the difference in group velocities between pump and probe, the determination of the absolute pump–probe delay depends on the sample position. In addition, pulse-front tilt is a widespread issue, unacceptable for ultrafast imaging, but which is conventionally very difficult to evaluate for the low-intensity probe pulses. Here we show that a pump-induced micro-grating generated from the electronic Kerr effect provides a detailed in-situ characterization of a weak probe pulse. It allows solving the two issues of absolute pump–probe delay determination and pulse-front tilt detection. Our approach is valid whatever the transparent medium with non-negligible Kerr index, whatever the probe pulse polarization and wavelength. Because it is nondestructive and fast to perform, this in-situ probe diagnostic can be repeated to calibrate experimental conditions, particularly in the case where complex wavelength, spatial frequency or polarization encoding is used. We anticipate that this technique will enable previously inaccessible spatiotemporal imaging in a number of fields of ultrafast science at the micro- and nanoscale.

Relativistic cavity, possibilities, and advantages

The relativistic mirror (RM) is an interesting subject which introduced in the nonlinear regime of the laser–plasma interaction. Reflection of counter-propagating probe pulse from relativistic flying mirror has some excellent features, such as frequency up-shifting and compressing by a factor of 4γ2. In the high-intensity laser–plasma interaction, sometimes a sequence of RMs creates. For example, electron density cusps generate in the nonlinear laser wakefield generation or flying electron sheaths create in the blown-out regime of the laser foil interaction. Under these circumstances, the second counter-propagated seed (probe) pulse can be reflected back and forth between two or more successive RMs. This structure may be used as a relativistic cavity (RECA). Amplification and threshold conditions for the gain medium and pumping rate in the RECA are obtained, and it is shown that amplification can be started from background simultaneous emission (without seed pulse). A new feature of RECA is it's bidirectional (two frequencies) characteristic. Thereupon, the gain process can be implemented on the two different transitions in this bidirectional gain structure. In the RECA, driver pulse may be assembled as a pumping operation, and background plasma medium with high degree ionized substances is a good candidate for gain medium in the UV or X-ray regions. In this paper, we propose a new all-optical cavity for the generation of the ultrashort laser pulse in the UV or X-ray regions.