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Spatially selective melting of metal materials by laser irradiation allows for the precise welding as well as the 3D printing of complex metal parts. However, the simple scanning of a conventional Gaussian beam typically results in a melt track with randomly distributed surface features due to the complex and dynamic behavior of the melt pool. In this study, the implications of utilizing a dynamically oscillating energy input on driving melt track fluctuations is investigated. Specifically, the laser intensity and/or intensity distribution is sinusoidally modulated at different scan speeds, and the effect of modulation frequency on the resulting surface features of the melt track is examined. The formation of periodically oriented surface features indicates an evident frequency coupling between the melt pool and the modulation frequency. Moreover, such a frequency coupling becomes most prominent under a specific modulation frequency, suggesting resonant behavior. The insights provided in this study will enable the development of novel methods, allowing for the control and/or mitigation of inherent fluctuations in the melt pool through laser-driven resonances.

The prediction of crystal properties plays a crucial role in the crystal design process. Current methods for predicting crystal properties focus on modeling crystal structures using graph neural networks (GNNs). Although GNNs are powerful, accurately modeling the complex interactions between atoms and molecules within a crystal remains a challenge. Surprisingly, predicting crystal properties from crystal text descriptions is understudied, despite the rich information and expressiveness that text data offer. One of the main reasons is the lack of publicly available data for this task. In this paper, we develop and make public a benchmark dataset (called TextEdge) that contains text descriptions of crystal structures with their properties. We then propose LLM-Prop, a method that leverages the general-purpose learning capabilities of large language models (LLMs) to predict the physical and electronic properties of crystals from their text descriptions. LLM-Prop outperforms the current state-of-the-art GNN-based crystal property predictor by about 4% in predicting band gap, 3% in classifying whether the band gap is direct or indirect, and 66% in predicting unit cell volume. LLM-Prop also outperforms a finetuned MatBERT, a domain-specific pre-trained BERT model, despite having 3 times fewer parameters. Our empirical results may highlight the current inability of GNNs to capture information pertaining to space group symmetry and Wyckoff sites for accurate crystal property prediction., Comment: Code for LLM-Prop can be found at: https://github.com/vertaix/LLM-Prop

Pushing the limits of precision and reproducibility in ultrafast laser-based nanostructuring requires detailed control over the properties of the illumination. Most traditional methods of laser-based manufacturing rely on the simplicity of Gaussian beams for their well-understood propagation behavior and ease of generation. However, a variety of benefits can be obtained by moving beyond Gaussian beams to single or multiple tailored beams working toward optimal spatial and temporal control over the beam profiles. In this chapter, we center our attention on methods to generate and manipulate complex light beams and the resulting material interactions that occur in response to irradiations with these non-traditional sources. We begin with a discussion on the main differences between Gaussian and more complex light profiles, describing the mechanisms of phase and spatial control before narrowing the discussion to approaches for spatial structuring associated with materials processing with ultrashort laser pulses. Such structuring can occur in both far-field propagating architectures, considering rapidly varying spatial profiles generated mechanically or optically, as well as near-field, non-propagating beams associated with plasmonic and dielectric systems. This chapter emphasizes some of the unique abilities of complex light to shape materials at the nanoscale from a fundamental perspective while referencing potential applications of such methods.

Subwavelength periodic confinement can collectively and selectively enhance local light intensity and enable control over the photo-induced phase transformations at the nanometer scale. Standard nanofabrication process can result in geometrical and compositional inhomogeneities in optical phase change materials, especially chalcogenides, as those materials exhibit poor chemical and thermal stability. Here we demonstrate the self-assembled planar chalcogenide nanostructured array with resonance enhanced light emission to create an all-dielectric optical metasurface, by taking advantage of the fluid properties associated with solution processed films. A patterned silicon membrane serves as a template for shaping the chalcogenide metasurface structure. Solution-processed arsenic sulfide metasurface structures are self-assembled in the suspended 250 nm silicon membrane templates. The periodic nanostructure dramatically manifests the local light-matter interaction such as absorption of incident photons, Raman emission, and photoluminescence. Also, the thermal distribution is modified by the boundaries and thus the photo-thermal crystallization process, leading to the formation of anisotropic nano-emitters within the field enhancement area. This hybrid structure shows wavelength selective anisotropic photoluminescence, which is a characteristic behavior of the collective response of the resonant guided modes in a periodic nanostructure. The resonance enhanced Purcell effect could manifest the quantum efficiency of localized light emission.

The low activation energy associated with amorphous chalcogenide structures offers broad tunability of material properties with laser-based or thermal processing. In this paper, we study near-bandgap laser induced anisotropic crystallization in solution processed arsenic sulfide. The modified electronic bandtail states associated with laser irritation lead to a distinctive photoluminescence spectrum, compared to thermally annealed amorphous glass. Laser crystalized materials exhibit a periodic subwavelength ripples structure in transmission electron microscopy experiments and show polarization dependent photoluminescence. Analysis of the local atomic structure of these materials using laboratory-based X-ray pair distribution function analysis indicates that laser irradiation causes a slight rearrangement at the atomic length scale, with a small percentage of S-S homopolar bonds converting to As-S heteropolar bonds. These results highlight fundamental differences between laser and thermal processing in this important class of materials.