Mechanism of femtosecond laser ablation revealed by THz emission spectroscopy

We investigated femtosecond laser ablation dynamics using THz time-domain spectroscopy. To clarify the breakdown dynamics of materials, we focused on the motion of charged particles and measured the terahertz waves emitted during laser ablation. We revealed that the Coulomb force dominated the ablation process. Furthermore, comparisons of the experimental results with theoretical models showed that material breakdown occurs within a few hundred femtoseconds. Our experimental results indicate that electrostatic ablation is the most likely ablation mechanism for metals

Probing thermal dissipation dimensionality to laser ablation in the pulse duration range from 300 fs to 1 μs.pdf

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Coherent control of acoustic phonons in a silica fiber using a multi-GHz optical frequency comb

Multi-gigahertz mechanical vibrations stemming from interactions between light fields and matter, also known as acoustic phonons, have long been a subject of study. In recent years, specially designed functional devices have been developed to enhance the light-matter interaction strength, since the excitation of acoustic phonons by a continuous wave laser alone is insufficient. However, with such structure-dependent enhancements, the strength of the interaction cannot be aptly and instantly controlled. We propose a new technique to control the effective interaction strength, which is not via the material structure in the spatial domain, as with the above-mentioned specially designed functional devices, but through the structure of light in the time domain. Here we show the effective excitation and coherent control of acoustic phonons in a single-mode fiber using an optical frequency comb by tailoring the optical pulse train. We believe this work represents an important step towards "comb-matter interactions.

Ultrafast Excited State Dynamics of Forward and Reverse <i>trans</i>-<i>cis</i> Photoisomerization of Red-Light-Absorbing Indigo Derivatives

Femtosecond time-resolved transient absorption (TRTA) spectroscopy was carried out to investigate the ultrafast excited state dynamics of both trans → cis and trans ← cis photoisomerization of red-light-absorbing indigo derivatives. For N,N′-bis­(tert-butyloxycarbonylmethyl)­indigo (tBOMI), the excited state lifetime of the trans-form was measured to be 41 ps while that of the cis-form was as short as 730 fs in acetonitrile (Acn). The excited state lifetime of trans-N,N′-dimethylindigo (DMI) in Acn was also measured to be as short as 10 ps. These values are much shorter than those of the blue-light-absorbing trans-forms of indigo derivatives such as N,N′-diacetylindigo (DAI) and thioindigo (ThI). The chromophore of indigo is composed of two pairs of electron donor and acceptor substituents conjugated in the shape of a letter “H” (so-called “H-chromophore”), although DFT and TDDFT calculations suggest that the charge transfer (CT) character is not very significant. Nevertheless, when a weak CT within the H-chromophore is promoted, the absorption band shifts to longer wavelengths and the excited state lifetime shortens. For the photoisomerization of DAI and ThI, a relatively long excited state lifetime is required for the photoisomerization, while for tBOMI and DMI, a vibrationally hot ground state that overcomes the energy barrier in the ground state is produced by rapid nonradiative decay through conical intersection. In the case of cis-tBOMI, the repulsion between the two adjacent negatively charged carbonyl groups and the weakening of the central CC double bond in the S1 state twist the molecule, shorten the excited state lifetime, and increase the quantum yield of the trans ← cis photoisomerization

Selective excitation of multipolar spoof plasmons using orbital angular momentum of light

The nature of light-matter interaction is governed by the spatial-temporal structures of a light field and material wavefunctions. The emergence of the light beam with transverse phase vortex, or equivalently orbital angular momentum (OAM) has been providing intriguing possibilities to induce unconventional optical transitions beyond the framework of the electric dipole interaction. The uniqueness stems from the OAM transfer from light to material, as demonstrated using the bound electron of a single trapped ion. However, many aspects of the vortex light-matter interaction are still unexplored especially in solids with extended electronic states. Here, we unambiguously visualized dipole-forbidden multipolar excitations in a solid-state electron system; spoof localized surface plasmon, selectively induced by the terahertz vortex beam. The results obey the selection rules governed by the conservation of the total angular momentum, which is numerically confirmed by the electromagnetic field analysis. Our results show light's OAM can be efficiently transferred to an elementary excitation in solids

Supplementary document for Real-time high-spectral-resolution mid-infrared spectroscopy with a signal-to-noise ratio of ten thousand - 6046806.pdf

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