Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III2-VI4 Colloidal Nanocrystals

Pavel, Md Sarkar; Chen, Yunhua; Santhiran, Anuluxan; Gi, Eunbyeol; Ochoa-Romero, Kerly; Miller, Gordon J.; Guirado, Gonzalo; Rossini, Aaron J.; Vela, Javier

doi:10.1021/acsenergylett.4c02032

Title: Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III₂-VI₄ Colloidal Nanocrystals

Journal Article · 20 September 2024 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.4c02032 · OSTI ID:2448470

Pavel, Md Sarkar ^[1]; Chen, Yunhua ^[2]; Santhiran, Anuluxan ^[2];

^[2]; Ochoa-Romero, Kerly ^[3];

^[1]; Guirado, Gonzalo ^[3];

^[2];

^[2]

Iowa State Univ., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States); Ames Laboratory (AMES), Ames, IA (United States)
Univ. Autonoma de Barcelona (Spain)

Ternary tetrahedral II-III₂-VI₄ semiconductors, where II is Zn or Cd, III In or Ga, and VI S, Se, or Te, are of interest in UV radiation detectors in medicine and space physics as well as CO₂ photoreduction under visible light. We synthesize colloidal II-III₂-VI₄ semiconductor nanocrystals from readily available precursors and ascertain their ternary nature by structural and spectroscopic methods, including ⁷⁷Se solid-state NMR spectroscopy. The pyramidally shaped nanocrystals range between 2 and 12 nm and exhibit optical gaps of 2–3.9 eV. In the presence of excess anions on the particle surface, treatment with Lewis acidic, Z-type ligands results in better passivation and enhanced photoluminescence. Electronic structure calculations reveal the most stable, lowest energy polymorphs and coloring patterns. This work will pave the way toward more environmentally friendly, ternary semiconductors for optoelectronics and electrocatalysis.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 2448470

Report Number(s):: IS-J--11,443

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 10 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (53)

The “Coloring Problem” in Solids: How It Affects Structure, Composition and Properties Miller, Gordon J. European Journal of Inorganic Chemistry, Vol. 1998, Issue 5 https://doi.org/10.1002/(SICI)1099-0682(199805)1998:5<523::AID-EJIC523>3.0.CO;2-L	journal	May 1998
Optical and Dynamic Properties of ZnGa₂S₄ Asadullayeva, Saida G.; Jahangirli, Zakir A.; Naghiyev, Tural G. physica status solidi (b), Vol. 258, Issue 8 https://doi.org/10.1002/pssb.202100101	journal	June 2021
Bulk Modulus, Elastic Constants, and Force Constants of Interatomic Bonds of II–III₂–VI₄ Compounds Mamedova, Irada A.; Jahangirli, Zakir A.; Kerimova, Taira G. physica status solidi (b), Vol. 260, Issue 6 https://doi.org/10.1002/pssb.202200441	journal	April 2023
Anomalous dependence of photoluminescence properties on composition x in Cd _{1– x} Mn _x Ga ₂ S ₄ mixed crystals Park, Hyun; Kim, Young‐San; Hyun, Seung‐Cheol physica status solidi c, Vol. 3, Issue 8 https://doi.org/10.1002/pssc.200669622	journal	August 2006
QCPMG-MAS NMR of Half-Integer Quadrupolar Nuclei Larsen, Flemming H.; Jakobsen, Hans J.; Ellis, Paul D. Journal of Magnetic Resonance, Vol. 131, Issue 1 https://doi.org/10.1006/jmre.1997.1341	journal	March 1998
Solid-State NMR of Inorganic Semiconductors Yesinowski, James P. Topics in Current Chemistry https://doi.org/10.1007/128_2011_208	book	January 2011
Photoluminescence study of chemical bath deposited ZnIn2Se4 thin films Babu, Pejjai; Reddy, Minnam Reddy Vasudeva; Reddy, Kotte Tulasi Ramakrishna Electronic Materials Letters, Vol. 10, Issue 4 https://doi.org/10.1007/s13391-013-3207-y	journal	July 2014
Photocatalytic degradable polymer precursor production and C–C bond synthesis with CO2 over sulfur vacancies enriched ZnIn2S4 nanosheets Sheng, Meilin; Gan, Chuan; Li, Yue Chemical Engineering Journal, Vol. 446 https://doi.org/10.1016/j.cej.2022.136919	journal	October 2022
29Si NMR in solid state with CPMG acquisition under MAS Wiench, J. W.; Lin, V. S. -Y.; Pruski, M. Journal of Magnetic Resonance, Vol. 193, Issue 2 https://doi.org/10.1016/j.jmr.2008.05.007	journal	August 2008
Optical activity in []ZnGa2S4 Joshi, N. V.; Luengo, Jorge; Vera, Fatima Materials Letters, Vol. 61, Issue 8-9 https://doi.org/10.1016/j.matlet.2006.07.177	journal	April 2007
Diorganyl Dichalcogenides as Useful Synthons for Colloidal Semiconductor Nanocrystals Brutchey, Richard L. Accounts of Chemical Research, Vol. 48, Issue 11 https://doi.org/10.1021/acs.accounts.5b00362	journal	October 2015
Expanding the I–II–V Phase Space: Soft Synthesis of Polytypic Ternary and Binary Zinc Antimonides White, Miles A.; Baumler, Katelyn J.; Chen, Yunhua Chemistry of Materials, Vol. 30, Issue 17 https://doi.org/10.1021/acs.chemmater.8b02910	journal	August 2018
Ligand-Mediated Phase Control in Colloidal AgInSe ₂ Nanocrystals Tappan, Bryce A.; Horton, Matthew K.; Brutchey, Richard L. Chemistry of Materials, Vol. 32, Issue 7 https://doi.org/10.1021/acs.chemmater.9b05163	journal	March 2020
Colloidal Semiconductor Nanocrystal Lasers and Laser Diodes Ahn, Namyoung; Livache, Clément; Pinchetti, Valerio Chemical Reviews, Vol. 123, Issue 13, p. 8251-8296 https://doi.org/10.1021/acs.chemrev.2c00865	journal	June 2023
Wide Band Gap Chalcogenide Semiconductors Woods-Robinson, Rachel; Han, Yanbing; Zhang, Hanyu Chemical Reviews, Vol. 120, Issue 9 https://doi.org/10.1021/acs.chemrev.9b00600	journal	April 2020
Molecular Decomposition Routes of Diaryl Diselenide Precursors in Relation to the Phase Determination of Copper Selenides Koziel, Alexandra C.; Goldfarb, Ralston B.; Endres, Emma J. Inorganic Chemistry, Vol. 61, Issue 37 https://doi.org/10.1021/acs.inorgchem.2c02042	journal	September 2022
Toward Bright Colloidal Near-Infrared Emitters: Surface Passivation of 2D PbSe Nanoplatelets by Metal Halides Biesterfeld, Leon; Klepzig, Lars F.; Niebur, André The Journal of Physical Chemistry C, Vol. 126, Issue 45 https://doi.org/10.1021/acs.jpcc.2c05850	journal	November 2022
Corrosion of Late- and Post-Transition Metals into Metal–Organic Chalcogenolates and Implications for Nanodevice Architectures Yeung, Matthew; Popple, Derek C.; Schriber, Elyse A. ACS Applied Nano Materials, Vol. 3, Issue 4 https://doi.org/10.1021/acsanm.0c00057	journal	March 2020
Utilizing Site Disorder in the Development of New Energy-Relevant Semiconductors Schnepf, Rekha R.; Cordell, Jacob J.; Tellekamp, M. Brooks ACS Energy Letters https://doi.org/10.1021/acsenergylett.0c00576	journal	June 2020
Colloidal Quantum Dot Photovoltaics: Current Progress and Path to Gigawatt Scale Enabled by Smart Manufacturing Kirmani, Ahmad R.; Luther, Joseph M.; Abolhasani, Milad ACS Energy Letters, Vol. 5, Issue 9 https://doi.org/10.1021/acsenergylett.0c01453	journal	August 2020
Surface Chemistry and Quantum Dot Luminescence: Shell Growth, Atomistic Modification, and Beyond Eagle, Forrest W.; Park, Nayon; Cash, Melanie ACS Energy Letters, Vol. 6, Issue 3 https://doi.org/10.1021/acsenergylett.0c02697	journal	February 2021
Silicon as Emerging Anode in Solid-State Batteries Huo, Hanyu; Janek, Jürgen ACS Energy Letters, Vol. 7, Issue 11 https://doi.org/10.1021/acsenergylett.2c01950	journal	October 2022
Development of Group III–V Colloidal Quantum Dots for Optoelectronic Applications Kim, Taewan; Shin, Daekwon; Kim, Meeree ACS Energy Letters, Vol. 8, Issue 1, p. 447-456 https://doi.org/10.1021/acsenergylett.2c02489	journal	December 2022
Prospects of Chalcopyrite-Type Nanocrystals for Energy Applications Sandroni, Martina; Wegner, K. David; Aldakov, Dmitry ACS Energy Letters, Vol. 2, Issue 5 https://doi.org/10.1021/acsenergylett.7b00003	journal	April 2017
High-Performance CuInS ₂ Quantum Dot Laminated Glass Luminescent Solar Concentrators for Windows Bergren, Matthew R.; Makarov, Nikolay S.; Ramasamy, Karthik ACS Energy Letters, Vol. 3, Issue 3 https://doi.org/10.1021/acsenergylett.7b01346	journal	January 2018
Development of InP Quantum Dot-Based Light-Emitting Diodes Wu, Zhenghui; Liu, Pai; Zhang, Wenda ACS Energy Letters, Vol. 5, Issue 4 https://doi.org/10.1021/acsenergylett.9b02824	journal	March 2020
Morphological Control of 2D Hybrid Organic–Inorganic Semiconductor AgSePh Paritmongkol, Watcharaphol; Lee, Woo Seok; Shcherbakov-Wu, Wenbi ACS Nano, Vol. 16, Issue 2 https://doi.org/10.1021/acsnano.1c07498	journal	January 2022
2D Material Infrared Photonics and Plasmonics Elbanna, Ahmed; Jiang, Hao; Fu, Qundong ACS Nano, Vol. 17, Issue 5 https://doi.org/10.1021/acsnano.2c10705	journal	February 2023
Studies of Organically Functionalized Mesoporous Silicas Using Heteronuclear Solid-State Correlation NMR Spectroscopy under Fast Magic Angle Spinning Trebosc, Julien; Wiench, Jerzy W.; Huh, Seong Journal of the American Chemical Society, Vol. 127, Issue 20 https://doi.org/10.1021/ja0509127	journal	May 2005
Synthesis and Shape Control of CuInS ₂ Nanoparticles Kruszynska, Marta; Borchert, Holger; Parisi, Jürgen Journal of the American Chemical Society, Vol. 132, Issue 45 https://doi.org/10.1021/ja103828f	journal	November 2010
Phase Selection and Site-Selective Distribution by Tin and Sulfur in Supertetrahedral Zinc Gallium Selenides Wu, Tao; Bu, Xianhui; Zhao, Xiang Journal of the American Chemical Society, Vol. 133, Issue 24 https://doi.org/10.1021/ja203143q	journal	June 2011
Solution-Grown Sodium Bismuth Dichalcogenides: Toward Earth-Abundant, Biocompatible Semiconductors Rosales, Bryan A.; White, Miles A.; Vela, Javier Journal of the American Chemical Society, Vol. 140, Issue 10 https://doi.org/10.1021/jacs.7b12873	journal	February 2018
Finding and Fixing Traps in II–VI and III–V Colloidal Quantum Dots: The Importance of Z-Type Ligand Passivation Kirkwood, Nicholas; Monchen, Julius O. V.; Crisp, Ryan W. Journal of the American Chemical Society, Vol. 140, Issue 46 https://doi.org/10.1021/jacs.8b07783	journal	October 2018
Shape-Programmed Nanofabrication: Understanding the Reactivity of Dichalcogenide Precursors Guo, Yijun; Alvarado, Samuel R.; Barclay, Joshua D. ACS Nano, Vol. 7, Issue 4 https://doi.org/10.1021/nn400596e	journal	April 2013
Excitonic effects in absorption spectra of carbon dioxide reduction photocatalysts Biswas, Tathagata; Singh, Arunima K. npj Computational Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41524-021-00640-3	journal	November 2021
Silicon heterojunction solar cells with up to 26.81% efficiency achieved by electrically optimized nanocrystalline-silicon hole contact layers Lin, Hao; Yang, Miao; Ru, Xiaoning Nature Energy, Vol. 8, Issue 8 https://doi.org/10.1038/s41560-023-01255-2	journal	May 2023
Engineering colloidal semiconductor nanocrystals for quantum information processing Almutlaq, Jawaher; Liu, Yuan; Mir, Wasim J. Nature Nanotechnology, Vol. 19, Issue 8, p. 1091-1100 https://doi.org/10.1038/s41565-024-01606-4	journal	March 2024
Low-dimensional wide-bandgap semiconductors for UV photodetectors Li, Ziqing; Yan, Tingting; Fang, Xiaosheng Nature Reviews Materials, Vol. 8, Issue 9 https://doi.org/10.1038/s41578-023-00583-9	journal	August 2023
Gallium – a versatile element for tuning the photoluminescence properties of InP quantum dots Wegner, K. David; Pouget, Stéphanie; Ling, Wai Li Chemical Communications, Vol. 55, Issue 11 https://doi.org/10.1039/C8CC09740B	journal	January 2019
NMR study of InP quantum dots: Surface structure and size effects Tomaselli, M.; Yarger, J. L.; Bruchez, M. The Journal of Chemical Physics, Vol. 110, Issue 18 https://doi.org/10.1063/1.478858	journal	May 1999
Thermally activated cation ordering in ZnGa₂Se₄single crystals studied by Raman scattering, optical absorption, andab initiocalculations Vilaplana, R.; Gomis, O.; Pérez-González, E. Journal of Physics: Condensed Matter, Vol. 25, Issue 16 https://doi.org/10.1088/0953-8984/25/16/165802	journal	April 2013
Trends in the band-gap pressure coefficients and bulk moduli in different structures of ZnGa₂S₄, ZnGa₂Se₄and ZnGa₂Te₄ Xiao-Shu, Jiang; Ying-Ce, Yan; Shi-Min, Yuan Chinese Physics B, Vol. 19, Issue 10 https://doi.org/10.1088/1674-1056/19/10/107104	journal	October 2010
Linear methods in band theory Andersen, O. Krogh Physical Review B, Vol. 12, Issue 8 https://doi.org/10.1103/PhysRevB.12.3060	journal	October 1975
Zinc-blende–wurtzite polytypism in semiconductors Yeh, Chin-Yu; Lu, Z. W.; Froyen, S. Physical Review B, Vol. 46, Issue 16 https://doi.org/10.1103/PhysRevB.46.10086	journal	October 1992
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Atomic Positional Versus Electronic Order in Semiconducting ZnSe Nanoparticles Cadars, S.; Smith, B. J.; Epping, J. D. Physical Review Letters, Vol. 103, Issue 13 https://doi.org/10.1103/PhysRevLett.103.136802	journal	September 2009
NMR Study of Semiconductor Molecular Clusters Thayer, A. M.; Steigerwald, M. L.; Duncan, T. M. Physical Review Letters, Vol. 60, Issue 25 https://doi.org/10.1103/PhysRevLett.60.2673	journal	June 1988
The coordination chemistry of nanocrystal surfaces Owen, Jonathan Science, Vol. 347, Issue 6222 https://doi.org/10.1126/science.1259924	journal	February 2015
Van der Waals Picture of Liquids, Solids, and Phase Transformations Chandler, D.; Weeks, J. D.; Andersen, H. C. Science, Vol. 220, Issue 4599 https://doi.org/10.1126/science.220.4599.787	journal	May 1983
Semiconductor quantum dots: Technological progress and future challenges García de Arquer, F. Pelayo; Talapin, Dmitri V.; Klimov, Victor I. Science, Vol. 373, Issue 6555 https://doi.org/10.1126/science.aaz8541	journal	August 2021
Data-Driven Discovery of Robust Materials for Photocatalytic Energy Conversion Singh, Arunima K.; Gorelik, Rachel; Biswas, Tathagata Annual Review of Condensed Matter Physics, Vol. 14, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031620-100957	journal	March 2023
CRC Handbook of Chemistry and Physics Haynes, W. M.; Lide, David R.; Bruno, Thomas J. CRC press https://doi.org/10.1201/9781315380476	book	June 2016
Defect Engineering in II–III₂–VI₄ and Related Compounds Radautsan, S. I.; Tiginyanu, I. M. Japanese Journal of Applied Physics, Vol. 32, Issue S3 https://doi.org/10.7567/JJAPS.32S3.5	journal	January 1993

Similar Records

Alkaline Earth-Based Ternary Chalcogenide Nanocrystals: Cadmium- and Lead-Free Optical Materials

Journal Article · 2025 · ACS Nano · OSTI ID:2998112

Pavel, Md Riad Sarkar; Santhiran, Anuluxan; Dalberg, Seth; +2 more

Near-Infrared Photoluminescence Enhancement in Ge/CdS and Ge/ZnS Core/Shell Nanocrystals: Utilizing IV/II-VI Semiconductor Epitaxy

Journal Article · 2014 · ACS Nano · OSTI ID:1163923

Guo, Yijun; Rowland, Clare E; Schaller, Richard D; +1 more

Ternary and multinary compounds

Conference · 1987 · OSTI ID:5060378

Deb, S K; Zunger, A

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III2-VI4 Colloidal Nanocrystals

Citation Formats

References (53)

Similar Records

Related Subjects

Title: Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III₂-VI₄ Colloidal Nanocrystals