Solitons, particle-like excitations ubiquitous in many fields of physics, have been shown to exhibit bound states akin to molecules. The formation of such temporal soliton bound states and their internal dynamics have escaped direct experimental observation. By means of an emerging time-stretch technique, we resolve the evolution of femtosecond soliton molecules in the cavity of a few-cycle mode-locked laser. We track two- and three-soliton bound states over hundreds of thousands of consecutive cavity roundtrips, identifying fixed points and periodic and aperiodic molecular orbits. A class of trajectories acquires a path-dependent geometrical phase, implying that its dynamics may be topologically protected. These findings highlight the importance of real-time detection in resolving interactions in complex nonlinear systems, including the dynamics of soliton bound states, breathers, and rogue waves.

Real-time spectral interferometry probes the internal dynamics of femtosecond soliton molecules

Coherent Raman imaging techniques have evolved to become powerful tools for biomedical imaging without the need for labelling.

Chemically sensitive bioimaging with coherent Raman scattering

A topical review of numerical and experimental studies of supercontinuum generation in photonic crystal fiber is presented over the full range of experimentally reported parameters, from the femtosecond to the continuous-wave regime. Results from numerical simulations are used to discuss the temporal and spectral characteristics of the supercontinuum, and to interpret the physics of the underlying spectral broadening processes. Particular attention is given to the case of supercontinuum generation seeded by femtosecond pulses in the anomalous group velocity dispersion regime of photonic crystal fiber, where the processes of soliton fission, stimulated Raman scattering, and dispersive wave generation are reviewed in detail. The corresponding intensity and phase stability properties of the supercontinuum spectra generated under different conditions are also discussed.

Supercontinuum generation, photonic crystal fiber

Photonic time-stretch techniques and their applications are reviewed. The approach enables the observation of signals that are otherwise too short or rapid for conventional measurement. Observing non-repetitive and statistically rare signals that occur on short timescales requires fast real-time measurements that exceed the speed, precision and record length of conventional digitizers. Photonic time stretch is a data acquisition method that overcomes the speed limitations of electronic digitizers and enables continuous ultrafast single-shot spectroscopy, imaging, reflectometry, terahertz and other measurements at refresh rates reaching billions of frames per second with non-stop recording spanning trillions of consecutive frames. The technology has opened a new frontier in measurement science unveiling transient phenomena in nonlinear dynamics such as optical rogue waves and soliton molecules, and in relativistic electron bunching. It has also created a new class of instruments that have been integrated with artificial intelligence for sensing and biomedical diagnostics. We review the fundamental principles and applications of this emerging field for continuous phase and amplitude characterization at extremely high repetition rates via time-stretch spectral interferometry.

Time stretch and its applications

The interaction of light and matter in metallic nanosystems is mediated by the collective oscillation of surface electrons, called plasmons. After excitation, plasmons are absorbed by the metal electrons through inter- and intraband transitions, creating a highly non-thermal distribution of electrons. The electron population then decays through electron-electron interactions, creating a hot electron distribution within a few hundred femtoseconds, followed by a further relaxation via electron-phonon scattering on the timescale of a few picoseconds. In the spectral domain, hot plasmonic electrons induce changes to the plasmonic resonance of the nanostructure by modifying the dielectric constant of the metal. Here, we report on the observation of anomalously strong changes to the ultrafast temporal and spectral responses of these excited hot plasmonic electrons in hybrid metal/oxide nanostructures as a result of varying the geometry and composition of the nanostructure and the excitation wavelength. In particular, we show a large ultrafast, pulsewidth-limited contribution to the excited electron decay signal in hybrid nanostructures containing hot spots. The intensity of this contribution correlates with the efficiency of the generation of highly excited surface electrons. Using theoretical models, we attribute this effect to the generation of hot plasmonic electrons from hot spots. We then develop general principles to enhance the generation of energetic electrons through specifically designed plasmonic nanostructures that could be used in applications where hot electron generation is beneficial, such as in solar photocatalysis, photodetectors and nonlinear devices.

Anomalous ultrafast dynamics of hot plasmonic electrons in nanostructures with hot spots

Spontaneous Raman (SR) microscopy allows label-free chemically specific imaging based on the vibrational response of molecules; however, due to the low Raman scattering cross section, it is intrinsically slow. Coherent Raman scattering (CRS) techniques, by coherently exciting all the vibrational oscillators in the focal volume, increase signal levels by several orders of magnitude. In its single-frequency version, CRS microscopy has reached very high imaging speeds, up to the video rate; however, it provides an information which is not sufficient to distinguish spectrally overlapped chemical species within complex heterogeneous systems, such as cells and tissues. Broadband CRS combines the acquisition speed of CRS with the information content of SR, but it is technically very demanding. This paper reviews the current state of the art in broadband CRS microscopy, both in the coherent anti-Stokes Raman scattering (CARS) and the stimulated Raman scattering (SRS) versions. Different technical solutions for broadband CARS and SRS, working both in the frequency and in the time domains, are compared and their merits and drawbacks assessed.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/lpor.201800020

Broadband Coherent Raman Scattering Microscopy

A highly simplified architecture for stimulated-Raman-scattering microscopy is demonstrated, where multiple tunable narrowband picosecond pulses are generated by spectral compression of femtosecond pulses emitted by a single compact Er-fiber oscillator. The system provides high sensitivity (2×10−7) and spectral resolution (sub-15 cm−1), and it offers an unprecedented flexibility for multicolor imaging.

Fiber-format stimulated-Raman-scattering microscopy from a single laser oscillator

We study by femtosecond pump–probe microscopy the transient plasmonic response of individual gold nanoantennas fabricated by electron-beam lithography on a glass substrate. By exploiting the capability of the fabrication technique to control geometrical parameters at the nanoscale, we tuned the plasmonic resonance in a broad wavelength range, from the visible to the infrared. Numerical simulations based on a three-temperature model (3TM) for the electrons and lattice dynamics, combined with full-wave numerical analysis and semiclassical theory of optical transitions in the solid state, are compared with the measurements on a single gold nanoantenna probed at different wavelengths. The agreement between the experiment and the prediction of the 3TM turns out to be comparable to that achievable with the more sophisticated Boltzmann equation formalism. We also investigate the influence of the plasmon detuning with respect to the pump and probe wavelengths on the nonlinear optical response using different nano...

/pdf/transient-optical-response-of-a-single-gold-nanoantenna-the-f5rt9fx8l5.pdf

Transient Optical Response of a Single Gold Nanoantenna: The Role of Plasmon Detuning

We demonstrate an approach to coherent anti-Stokes Raman scattering (CARS) spectroscopy/microscopy based on spectral compression of femtosecond pulses emitted by a compact Er-fiber oscillator. Spectral compression is achieved by group-velocity mismatched second-harmonic generation in periodically poled nonlinear crystals, and it allows efficient synthesis of synchronized narrow-bandwidth (less than 10 cm−1) pump and Stokes pulses with the frequency difference continuously tunable up to ~3000 cm−1. CARS signal enhancement by up to 3 orders of magnitude is obtained by interferometric superposition with a phase-coherent local oscillator field, also synthesized by spectral compression.

Fiber-format CARS spectroscopy by spectral compression of femtosecond pulses from a single laser oscillator

We propose a new approach to broadband Stimulated Raman Scattering (SRS) spectroscopy and microscopy based on time-domain Fourier transform (FT) detection of the stimulated Raman gain (SRG) spectrum. We generate two phase-locked replicas of the Stokes pulse after the sample using a passive birefringent interferometer and measure by the FT technique both the Stokes and the SRG spectra. Our approach blends the very high sensitivity of single-channel lock-in balanced detection with the spectral coverage and resolution afforded by FT spectroscopy. We demonstrate our method by measuring the SRG spectra of different compounds and performing broadband SRS imaging on inorganic blends.

/pdf/broadband-stimulated-raman-scattering-with-fourier-transform-2bmpz3ki4n.pdf

Vikas Kumar

Papers

Broadband Coherent Raman Scattering Microscopy

Fiber-format stimulated-Raman-scattering microscopy from a single laser oscillator

Transient Optical Response of a Single Gold Nanoantenna: The Role of Plasmon Detuning

Fiber-format CARS spectroscopy by spectral compression of femtosecond pulses from a single laser oscillator

Broadband stimulated Raman scattering with Fourier-transform detection.