Melanin diagnostics with nonlinear optics: a mini-review

Optical methods are widely used to perform fundamental studies of living systems and solve problems of biomedical diagnostics. Along with the classical spectroscopy, methods of nonlinear optics (e.g., multiphoton microscopy) are also applied in biophotonics. The potential of nonlinear optical methods for visualisation and analysis of the properties of endogenous chromophore molecules are considered in this minireview. Melanin - a pigment with specific spectral features of photophysical properties in the visible and near-IR ranges - is taken as an example. It is discussed what information about its localisation in tissues and structural organisation can be obtained by nonlinear optical methods: multiphoton fluorescence microscopy (including fluorescence lifetime imaging), third harmonic generation, pump - probe spectroscopy, and coherent anti- Stokes Raman spectroscopy.

Study of Impulsive Stimulated Raman Scattering Effects Using the Femtosecond Pump–Probe Z-Scan Technique

Impulsive stimulated Raman scattering (ISRS) is a nonlinear pump–probe spectroscopy technique particularly suitable to study vibrational intermolecular and intramolecular modes in complex systems. For the latter, recent studies of ISRS microscopy with low-energy laser sources have attracted attention for investigation of photosensitive or biological samples. Following this stream of interest, in this paper, we report an investigation on the relationship between femtosecond ISRS data and pump–probe Z-scan measurements, showing that the latter technique is capable of capturing the Kerr nonlinearities induced by the molecular vibrational modes. To this aim, firstly, spectrally filtered and Raman-induced Kerr ISRS signals were simultaneously acquired to determine the sample nonlinear response and to establish the reference data for the Z-scan analysis. Then, by adopting a suitable experimental arrangement to avoid thermo-optical effects, we were able to unambiguously observe the Raman-induced effects in Z-scan measurements, thus obtaining a consistent picture between ISRS and Z-scan for the first time, to the best of our knowledge. Practical applications of the proposed method include calibrated measurements of the contribution of the internal (Raman) and external molecular modes to the nonlinear refractive index.

Suppressed electronic contribution in thermal conductivity of Ge2Sb2Se4Te

Integrated nanophotonics is an emerging research direction that has attracted great interests for technologies ranging from classical to quantum computing. One of the key-components in the development of nanophotonic circuits is the phase-change unit that undergoes a solid-state phase transformation upon thermal excitation. The quaternary alloy, Ge2Sb2Se4Te, is one of the most promising material candidates for application in photonic circuits due to its broadband transparency and large optical contrast in the infrared spectrum. Here, we investigate the thermal properties of Ge2Sb2Se4Te and show that upon substituting tellurium with selenium, the thermal transport transitions from an electron dominated to a phonon dominated regime. By implementing an ultrafast mid-infrared pump-probe spectroscopy technique that allows for direct monitoring of electronic and vibrational energy carrier lifetimes in these materials, we find that this reduction in thermal conductivity is a result of a drastic change in electronic lifetimes of Ge2Sb2Se4Te, leading to a transition from an electron-dominated to a phonon-dominated thermal transport mechanism upon selenium substitution. In addition to thermal conductivity measurements, we provide an extensive study on the thermophysical properties of Ge2Sb2Se4Te thin films such as thermal boundary conductance, specific heat, and sound speed from room temperature to 400 °C across varying thicknesses.

Phase segregation in mixed-halide perovskites affects charge-carrier dynamics while preserving mobility

Mixed halide perovskites can provide optimal bandgaps for tandem solar cells which are key to improved cost-efficiencies, but can still suffer from detrimental illumination-induced phase segregation. Here we employ optical-pump terahertz-probe spectroscopy to investigate the impact of halide segregation on the charge-carrier dynamics and transport properties of mixed halide perovskite films. We reveal that, surprisingly, halide segregation results in negligible impact to the THz charge-carrier mobilities, and that charge carriers within the I-rich phase are not strongly localised. We further demonstrate enhanced lattice anharmonicity in the segregated I-rich domains, which is likely to support ionic migration. These phonon anharmonicity effects also serve as evidence of a remarkably fast, picosecond charge funnelling into the narrow-bandgap I-rich domains. Our analysis demonstrates how minimal structural transformations during phase segregation have a dramatic effect on the charge-carrier dynamics as a result of charge funnelling. We suggest that because such enhanced recombination is radiative, performance losses may be mitigated by deployment of careful light management strategies in solar cells.

Megahertz scan rates enabled by optical sampling by repetition-rate tuning

We demonstrate, for the first time, optical sampling by repetition-rate tuning (OSBERT) at record megahertz scan rates. A low-cost, tunable and extremely compact 2-section passively mode-locked laser diode (MLLD) is used as the pulsed laser source, whose repetition rate can be modulated electronically through biasing of the saturable absorber section. The pulsed output is split into two arms comparable to an imbalanced Michelson interferometer, where one arm is significantly longer than the other (a passive delay line, or PDL). The resulting electronic detuning of the repetition rate gives rise to a temporal delay between pulse pairs at a detector; the basis for time-resolved spectroscopy. Through impedance-matching, we developed a new system whereby a sinusoidal electrical bias could be applied to the absorber section of the MLLD via a signal generator, whose frequency could be instantly increased from sub-hertz through to megahertz modulation frequencies, corresponding to a ground-breaking megahertz optical sampling scan rate, which was experimentally demonstrated by the real-time acquisition of a cross-correlation trace of two ultrashort optical pulses within just 1 microsecond of real time. This represents scan rates which are three orders of magnitude greater than the recorded demonstrations of OSBERT to date, and paves the way for highly competitive scan rates across the field of time-resolved spectroscopy and applications therein which range from pump probe spectroscopy to metrology.

Pump-probe spectroscopy in gold-garnet magnetoplasmonic metasurfaces

Ultrafast modulation of optical response is realized in a multi-resonant magnetoplasmonic metasurface under resonant femtosecond pump. A saturation of resonant probe transient transmission is shown at dielectric quazi-waveguide mode.