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Abstract Thermoelectric materials offer a unique solution for active cooling or conversion of heat to electricity within a thermal protection system due to their solid-state nature. Yet, the integration of thermoelectrics into thermal protection systems is hindered by conventional manufacturing processes, which limit the material’s shape. Laser additive manufacturing can enable freeform shapes that allow integration of thermoelectrics into systems that are favorable for thermoelectric energy conversion. Through modeling and experimentation, this work presents single melt line processing and structures of silicon germanium, a high-temperature thermoelectric material, for laser powder bed fusion. Experiments consisted of single melt lines with an Nd-YAG laser and 50-µm spot size on Si₅₀Ge₅₀and Si₈₀Ge₂₀powder compacts. We found that laser processing of silicon germanium alloys causes oxidation and processing defects that are resolved through rescanning strategies. Rapid cooling results in a microstructure with silicon-rich grains and germanium entrapped near grain boundaries for Si₈₀Ge₂₀and dendritic structures in Si₅₀Ge₅₀which are linked to the degree of undercooling during solidification. Laser-processed silicon germanium contains crystalline defects, nanoscale precipitates, and an average grain size of 24 µm. This work informs laser additive manufacturing of silicon germanium parts and uncovers process-structure relationships of laser-processed silicon germanium alloys. 

Abstract Laser processing of thermoelectric materials provides an avenue to influence the nano‐ and micro‐structure of the material and enable additive manufacturing processes that facilitate freeform device shapes, a capability that is lacking in thermoelectric materials processing. This paper describes the multiscale structures formed in selenium‐doped bismuth telluride, an n‐type thermoelectric material, from laser‐induced rapid melting and solidification. Macroscale samples are fabricated in a layer‐by‐layer technique using laser powder bed fusion (also known as selective laser melting). Laser processing results in highly textured columnar grains oriented in the build direction, nanoscale inclusions, and a shift in the primary charge carriers. Sparse oxide inclusions and tellurium segregation shift the material to p‐type behavior with a Seebeck coefficient that peaks at 143 µV K^–1at 95 °C. With an average relative density of 74%, fabricated parts have multiscale porosity and microscale cracking that likely resulted from low powder layer packing density and processing parameters near the transition threshold between conduction and keyhole mode processing. These results provide insights regarding the pathways for influencing carrier transport in thermoelectric materials via laser melting‐induced nanoscale structuring and the laser processing parameters required to achieve effective powder consolidation and hierarchical structuring in thermoelectric parts. 

Additive manufacturing allows fabrication of custom-shaped thermoelectric materials while minimizing waste, reducing processing steps, and maximizing integration compared to conventional methods. Establishing the process-structure-property relationship of laser additive manufactured thermoelectric materials facilitates enhanced process control and thermoelectric performance. This research focuses on laser processing of bismuth telluride (Bi 2 Te 3 ), a well-established thermoelectric material for low temperature applications. Single melt tracks under various parameters (laser power, scan speed and number of scans) were processed on Bi 2 Te 3 powder compacts. A detailed analysis of the transition in the melting mode, grain growth, balling formation, and elemental composition is provided. Rapid melting and solidification of Bi 2 Te 3 resulted in fine-grained microstructure with preferential grain growth along the direction of the temperature gradient. Experimental results were corroborated with simulations for melt pool dimensions as well as grain morphology transitions resulting from the relationship between temperature gradient and solidification rate. Samples processed at 25 W, 350 mm/s with 5 scans resulted in minimized balling and porosity, along with columnar grains having a high density of dislocations. 

Additive manufacturing offers several opportunities for thermoelectric energy harvesting systems. This new manufacturing approach enables customized leg geometries, minimized thermal boundary resistances, less retooling, reduced thermoelectric material waste, and strong potential to manipulate microstructure for higher values of figure of merit. Although additive manufacturing has been used to fabricate thin thermoelectric films, there has been comparatively limited demonstrations of additive manufacturing for bulk thermoelectric structures. This review provides insights about the current progress of bulk thermoelectric material and device additive manufacturing. Each additive manufacturing technique used to produce bulk thermoelectric structures is discussed in detail along with future directions and challenges. 

The ability of thermoelectric (TE) materials to convert thermal energy to electricity and vice versa highlights them as a promising candidate for sustainable energy applications. Despite considerable increases in the figure of merit zT of thermoelectric materials in the past two decades, there is still a prominent need to develop scalable synthesis and flexible manufacturing processes to convert high-efficiency materials into high-performance devices. Scalable printing techniques provide a versatile solution to not only fabricate both inorganic and organic TE materials with fine control over the compositions and microstructures, but also manufacture thermoelectric devices with optimized geometric and structural designs that lead to improved efficiency and system-level performances. In this review, we aim to provide a comprehensive framework of printing thermoelectric materials and devices by including recent breakthroughs and relevant discussions on TE materials chemistry, ink formulation, flexible or conformable device design, and processing strategies, with an emphasis on additive manufacturing techniques. In addition, we review recent innovations in the flexible, conformal, and stretchable device architectures and highlight state-of-the-art applications of these TE devices in energy harvesting and thermal management. Perspectives of emerging research opportunities and future directions are also discussed. While this review centers on thermoelectrics, the fundamental ink chemistry and printing processes possess the potential for applications to a broad range of energy, thermal and electronic devices.