Structural evolution of millisecond laser-induced metastable crystalline GeTe
Discovering new inorganic materials using solid-state synthesis in an accelerated fashion is difficult due their sluggish diffusion coefficients and long diffusion distances. Furthermore, high temperatures used in these reactions generally produce thermodynamically stable products, which provides li...
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sg-ntu-dr.10356-1806732024-10-18T15:48:11Z Structural evolution of millisecond laser-induced metastable crystalline GeTe Recatala-Gomez, Jose Li, Yun Nur Qalishah Adanan Ghosh, Biplab Dai, Haiwen Bai, Yang Zhang, Chenguang Morris, Samuel Alexander Jin, Zavier Goh You Zhai, Wenhao Mass, Tobias W. W. Kumar, Pawan Wei, Fengxia Thway, Maung Rafikul Ali Saha Solano, Eduardo Rosenthal, Martin Roeffaers, Maarten Kirby, Nigel Miłogrodzka, Izabela Simpson, Robert E. Tan, Kwan Wee Hippalgaonkar, Kedar School of Materials Science and Engineering Engineering High-throughput experiments Laser heating Discovering new inorganic materials using solid-state synthesis in an accelerated fashion is difficult due their sluggish diffusion coefficients and long diffusion distances. Furthermore, high temperatures used in these reactions generally produce thermodynamically stable products, which provides limited control on the reaction and prevents access to functional metastable phases. Herein, we report the use of a millisecond laser annealing technique to regulate the crystallographic phases of germanium telluride films of varying thicknesses. After laser heating, we combine temperature-dependent synchrotron grazing incidence measurements and transmission electron microscopy to study the structural evolution of the post-laser-heated GeTe. On average, we observe that millisecond laser heating induced the transformation of amorphous GeTe samples up to a ∼40% to 60% mixture of cubic β-GeTe (Fm3̅m) and rhombohedral α-GeTe (R3m) for GeTe films (thicknesses between 100 nm and 2 μm) deposited on thermally conducting substrates (such as Si), as opposed to phase-pure α-GeTe, which is obtained on low thermal conductivity substrates (quartz). Further, a room-temperature thermoelectric power factor of 6.10 μV cm-1 K-2 was measured for a laser-heated film on quartz. These findings suggest that conformal interfaces on substrates with high thermal conductivity facilitate accelerated rates of heat extraction at the sample-substrate interface to achieve phase control. We believe our strategy opens new avenues for the development of materials that are stabilized far from their equilibrium conditions. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Research Foundation (NRF) Submitted/Accepted version K.H. acknowledges financial support from the AcceleratedMaterials Development for Manufacturing Program atA*STAR via the AME Programmatic Fund by the Agencyfor Science, Technology and Research under Grant No.A1898b0043. K.H. also acknowledges funding from the NRFFellowship NRF-NRFF13-2021-0011. K.W.T. and Y.L. ac-knowledge financial support from the Singapore Ministry ofEducation AcRF Tier 2 grant (MOET2EP 50221-0017). R.E.S.and N.Q.A. are grateful for funding from the A*STAR IRGGrant No. A20E5c0093. B.G. would like to thank KU Leuvenfor a PDM scholarship (PDMT1/22/011). 2024-10-18T08:22:54Z 2024-10-18T08:22:54Z 2024 Journal Article Recatala-Gomez, J., Li, Y., Nur Qalishah Adanan, Ghosh, B., Dai, H., Bai, Y., Zhang, C., Morris, S. A., Jin, Z. G. Y., Zhai, W., Mass, T. W. W., Kumar, P., Wei, F., Thway, M., Rafikul Ali Saha, Solano, E., Rosenthal, M., Roeffaers, M., Kirby, N., ...Hippalgaonkar, K. (2024). Structural evolution of millisecond laser-induced metastable crystalline GeTe. ACS Applied Electronic Materials, 6(7), 4977-4987. https://dx.doi.org/10.1021/acsaelm.4c00511 2637-6113 https://hdl.handle.net/10356/180673 10.1021/acsaelm.4c00511 2-s2.0-85198528579 7 6 4977 4987 en A1898b0043 NRF-NRFF13-2021-0011 MOET2EP 50221-0017 ACS Applied Electronic Materials © 2024 American Chemical Society. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1021/acsaelm.4c00511. application/pdf |
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Engineering High-throughput experiments Laser heating Recatala-Gomez, Jose Li, Yun Nur Qalishah Adanan Ghosh, Biplab Dai, Haiwen Bai, Yang Zhang, Chenguang Morris, Samuel Alexander Jin, Zavier Goh You Zhai, Wenhao Mass, Tobias W. W. Kumar, Pawan Wei, Fengxia Thway, Maung Rafikul Ali Saha Solano, Eduardo Rosenthal, Martin Roeffaers, Maarten Kirby, Nigel Miłogrodzka, Izabela Simpson, Robert E. Tan, Kwan Wee Hippalgaonkar, Kedar Structural evolution of millisecond laser-induced metastable crystalline GeTe |
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Discovering new inorganic materials using solid-state synthesis in an accelerated fashion is difficult due their sluggish diffusion coefficients and long diffusion distances. Furthermore, high temperatures used in these reactions generally produce thermodynamically stable products, which provides limited control on the reaction and prevents access to functional metastable phases. Herein, we report the use of a millisecond laser annealing technique to regulate the crystallographic phases of germanium telluride films of varying thicknesses. After laser heating, we combine temperature-dependent synchrotron grazing incidence measurements and transmission electron microscopy to study the structural evolution of the post-laser-heated GeTe. On average, we observe that millisecond laser heating induced the transformation of amorphous GeTe samples up to a ∼40% to 60% mixture of cubic β-GeTe (Fm3̅m) and rhombohedral α-GeTe (R3m) for GeTe films (thicknesses between 100 nm and 2 μm) deposited on thermally conducting substrates (such as Si), as opposed to phase-pure α-GeTe, which is obtained on low thermal conductivity substrates (quartz). Further, a room-temperature thermoelectric power factor of 6.10 μV cm-1 K-2 was measured for a laser-heated film on quartz. These findings suggest that conformal interfaces on substrates with high thermal conductivity facilitate accelerated rates of heat extraction at the sample-substrate interface to achieve phase control. We believe our strategy opens new avenues for the development of materials that are stabilized far from their equilibrium conditions. |
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School of Materials Science and Engineering |
author_facet |
School of Materials Science and Engineering Recatala-Gomez, Jose Li, Yun Nur Qalishah Adanan Ghosh, Biplab Dai, Haiwen Bai, Yang Zhang, Chenguang Morris, Samuel Alexander Jin, Zavier Goh You Zhai, Wenhao Mass, Tobias W. W. Kumar, Pawan Wei, Fengxia Thway, Maung Rafikul Ali Saha Solano, Eduardo Rosenthal, Martin Roeffaers, Maarten Kirby, Nigel Miłogrodzka, Izabela Simpson, Robert E. Tan, Kwan Wee Hippalgaonkar, Kedar |
format |
Article |
author |
Recatala-Gomez, Jose Li, Yun Nur Qalishah Adanan Ghosh, Biplab Dai, Haiwen Bai, Yang Zhang, Chenguang Morris, Samuel Alexander Jin, Zavier Goh You Zhai, Wenhao Mass, Tobias W. W. Kumar, Pawan Wei, Fengxia Thway, Maung Rafikul Ali Saha Solano, Eduardo Rosenthal, Martin Roeffaers, Maarten Kirby, Nigel Miłogrodzka, Izabela Simpson, Robert E. Tan, Kwan Wee Hippalgaonkar, Kedar |
author_sort |
Recatala-Gomez, Jose |
title |
Structural evolution of millisecond laser-induced metastable crystalline GeTe |
title_short |
Structural evolution of millisecond laser-induced metastable crystalline GeTe |
title_full |
Structural evolution of millisecond laser-induced metastable crystalline GeTe |
title_fullStr |
Structural evolution of millisecond laser-induced metastable crystalline GeTe |
title_full_unstemmed |
Structural evolution of millisecond laser-induced metastable crystalline GeTe |
title_sort |
structural evolution of millisecond laser-induced metastable crystalline gete |
publishDate |
2024 |
url |
https://hdl.handle.net/10356/180673 |
_version_ |
1814777784887672832 |