This article reviews the historical background and recent advances in molecular vibrational imaging methods. We explain the two primary methods for exciting molecular vibrations: infrared and Raman excitations, coupled with several detection techniques to achieve vibrational imaging. Additionally, we introduce cutting-edge developments in stimulated Raman scattering microscopy and mid-infrared photothermal microscopy, highlighting their importance in this field.
Recent developments in high harmonic generation, seeded free-electron laser and synchrotron radiation have enabled to generate attosecond-precision phase-controlled double pulses in the extreme ultraviolet (XUV) regime. The uses of such double pulses have opened new opportunities in quantum control experiments at short wavelengths that had not been feasible before. We review the current status of the light sources, especially focusing on synchrotron radiation. We also overview recent experiments using phase-controlled XUV double pulses in the field of atomic and molecular physics.
To study potential lattice anomalies coupled to the various interesting properties in organic molecular materials, systematic inelastic neutron scattering studies were conducted on the two molecular dimer-Mott insulators, κ-(BEDT-TTF)2 Cu2(CN)3 and κ-(BEDT-TTF)2 Cu[N (CN)2 ]Cl. By using the state-of-the-art triple-axis-spectrometers and an array of co-aligned single crystals of deuterated organic molecular materials, we succeeded in observing characteristic phonon modes which couple to the intra-dimer degrees of freedom in the dimer-Mott insulators. We consider these inelastic neutron scattering results as an important step that may trigger further systematic studies on the lattice dynamics and its coupling to the electronic degree of freedom in the family of organic charge-transfer salts.