Understanding the Dynamic Liquid-Assisted Chemical Vapor Deposition Growth of Copper Telluride and Its Low-Temperature Phase Transition

Yea Shine Lee; Dmitry Lebedev; Eric K. Qian; Paloma Lee; Mercouri G. Kanatzidis; Mark C. Hersam; Vinayak P. Dravid

doi:10.1021/acs.cgd.3c00149

Understanding the Dynamic Liquid-Assisted Chemical Vapor Deposition Growth of Copper Telluride and Its Low-Temperature Phase Transition

Yea Shine Lee, Dmitry Lebedev, Eric K. Qian, Paloma Lee, Mercouri G. Kanatzidis, Mark C. Hersam, Vinayak P. Dravid^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

Copper telluride is an emerging layered material that has been shown to undergo phase transitions with slight modifications in its stoichiometry (Cu_2-xTe) at high temperatures. Using Raman spectroscopy and X-ray diffraction, we complete the spectrum of temperatures and detect a low-temperature phase transition of copper telluride for the first time. Moreover, liquid-assisted chemical vapor deposition (CVD) growth is heavily explored for its potential to grow various crystals at a large scale. However, the role that the liquid precursor plays in these growths remains largely elusive, and a theoretical study is impeded by the bulk amorphous liquid precursor. Here, we experimentally demonstrate how the liquid precursor contributes to the morphological orientations of Cu_0.664Te_0.336 crystals. Based on this, we propose a growth process in which tellurium supersaturation of the liquid precursor yields nucleation sites both on the surface and internally. Etching of Cu_0.664Te_0.336 via H₂ flow is also achieved during CVD to increase the density of exposed sites. Optimal parameters to control H₂ flow to achieve layer-by-layer thinning in geometric crystals are also realized. Our study thereby enhances the understanding of temperature-dependent copper telluride phases and presents liquid-assisted growth as a platform ripe with opportunities for materials engineering.

Original language	English (US)
Pages (from-to)	3769-3777
Number of pages	9
Journal	Crystal Growth and Design
Volume	23
Issue number	5
DOIs	https://doi.org/10.1021/acs.cgd.3c00149
State	Published - May 3 2023

Funding

This work was primarily supported by NSF Division of Material Research Grant DMR-1929356 (V.P.D.) with additional support provided by DMR-2003476 (M.C.H.). Low-temperature Raman characterization was supported by the Northwestern University Materials Research Science and Engineering Center (NSF Grant DMR-1720139). This work made use of the SPID and EPIC facilities of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF Grant ECCS-2025633), Northwestern’s MRSEC program (NSF Grant DMR-1720139), the Keck Foundation, and the State of Illinois through IIN. This work also made use of the Jerome B. Cohen X-ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the SHyNE Resource (NSF ECCS-2025633). This work also made use of the IMSERC Crystallography facility at Northwestern University, which has received support from the SHyNE Resource (NSF ECCS-2025633) and Northwestern University. Y.-S.L. gratefully acknowledges support from the Ryan Fellowship and the IIN at Northwestern University.

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics

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10.1021/acs.cgd.3c00149

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title = "Understanding the Dynamic Liquid-Assisted Chemical Vapor Deposition Growth of Copper Telluride and Its Low-Temperature Phase Transition",

abstract = "Copper telluride is an emerging layered material that has been shown to undergo phase transitions with slight modifications in its stoichiometry (Cu2-xTe) at high temperatures. Using Raman spectroscopy and X-ray diffraction, we complete the spectrum of temperatures and detect a low-temperature phase transition of copper telluride for the first time. Moreover, liquid-assisted chemical vapor deposition (CVD) growth is heavily explored for its potential to grow various crystals at a large scale. However, the role that the liquid precursor plays in these growths remains largely elusive, and a theoretical study is impeded by the bulk amorphous liquid precursor. Here, we experimentally demonstrate how the liquid precursor contributes to the morphological orientations of Cu0.664Te0.336 crystals. Based on this, we propose a growth process in which tellurium supersaturation of the liquid precursor yields nucleation sites both on the surface and internally. Etching of Cu0.664Te0.336 via H2 flow is also achieved during CVD to increase the density of exposed sites. Optimal parameters to control H2 flow to achieve layer-by-layer thinning in geometric crystals are also realized. Our study thereby enhances the understanding of temperature-dependent copper telluride phases and presents liquid-assisted growth as a platform ripe with opportunities for materials engineering.",

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Understanding the Dynamic Liquid-Assisted Chemical Vapor Deposition Growth of Copper Telluride and Its Low-Temperature Phase Transition

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