Graphene-enhanced Raman scattering (GERS) spectra and coherent anti-Stokes Raman scattering (CARS) of thymine molecules adsorbed on a single-layer graphene were studied. The enhancement factor was shown to depend on the molecular groups of thymine. In the GERS spectra of thymine, the main bands are shifted with respect to those for molecules adsorbed on a glass surface, indicating charge transfer for thymine on graphene. The probable mechanism of the GERS enhancement is discussed. CARS spectra are in accord with the GERS results, which indicates similar benefit from the chemical enhancement.

Theranostics is the emerging field of medicine that uniquely combines diagnostic techniques and active agents to diagnose and treat medical conditions simultaneously or sequentially. Finding a theranostic agent capable to cure the affected cells and being safe for the healthy ones is the key for successful treatment. Here, we demonstrate that agglomerated single-walled carbon nanotubes (SWCNTs) are promising theranostic agent that enables photo-activated ‘cold’ destruction of the cancer cells keeping their environment alive. The absorption of picosecond pulses by SWCNT agglomerates results in the mechanical (due to photoacoustic effect) rather than photothermal cancer cell destruction, which was visualized by micro-Raman and ultrafast near-infrared CARS. The developed theoretical model allows us to distinguish photothermal, photoacoustic, and photothermoacoustic regimes of the cancer cell destruction, and also to optimize SWCNT-based theranostics recipe.

Identification of chemically homologous microcrystals in a polycrystal sample is a big challenge and requires developing specific highly sensitive tools. Second harmonic (SHG) and coherent anti-Stokes Raman scattering (CARS) spectroscopy can be used to reveal arrangement of thymine molecules, one of the DNA bases, in microcrystalline sample. Strong dependence of CARS and SHG intensity on the orientation of the linear polarization of the excitation light allows to obtain high resolution images of thymine microcrystals by additionally utilizing the scanning microscopy technique. Experimental findings and theoretical interpretation of the results are compared. Presented experimental data together with quantum chemistry-based theoretical interpretation allowed us to determine the most probable organization of the thymine molecules.

The shape of coherent anti-Stokes Raman scattering (CARS) spectral line depends on the ratio of the vibrational and electronic contributions to the third-order susceptibility of the material. The G-mode (1590 cm⁻¹) of graphene and carbon nanotubes (CNTs) exhibits opposite features in the CARS spectrum, showing “dip” and “peak,” respectively. Here, we consider the CARS spectra of graphene and carbon nanotubes in terms of Fano formalism describing the line shapes of CARS resonances. We show that imaging at only 1590 cm⁻¹ is not sufficient to separate the constituents of a composite material consisting of both graphene and CNTs. We propose an algorithm to map the graphene and CNTs in a composite material.

We employed polarization-sensitive nonlinear optical microscopy to assess crystallinity of diamond microneedles. In the experiment, we mapped the coherent anti-Stokes Raman spectroscopy (CARS) signal in the vicinity of 1332 cm−1 diamond Raman peak over the needle length and demonstrated that the third-order nonlinear optical susceptibility remains the same at both micrometer-sized base and the nanoscale thin apex of the needle. This indicated the single-crystal nature of the diamond needle and allowed us to describe the results of the polarization CARS measurements in terms of the third-order nonlinear susceptibility of diamond. High crystallinity of the needle was also confirmed by measuring the linewidth of the zero-phonon line of the silicon-vacancy centers in diamond.