Hydrazine-free precursor for solution-processed all-inorganic Se and Se1−xTex photovoltaics

Alfieri, Adam D.; Das, Swarnendu; Kisslinger, Kim; Everhart, Brian M.; Leblanc, Chloe; Ford, Jamie; Kagan, Cherie R.; Glavin, Nicholas R.; Stach, Eric A.; Jariwala, Deep

doi:10.1039/d5ta06459g

Hydrazine-free precursor for solution-processed all-inorganic Se and Se_1−xTe_x photovoltaics

Journal Article · Wed Oct 15 00:00:00 EDT 2025 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d5ta06459g· OSTI ID:3000535

^[1]; ^[1]; ^[2]; Everhart, Brian M. ^[3]; ^[1]; Ford, Jamie ^[1]; ^[1]; ^[3]; ^[1]; ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Air Force Research Laboratory (AFRL), Wright-Patterson AFB, OH (United States)

Selenium (Se) has reemerged as a promising absorber material for indoor and tandem photovoltaics (PVs), and its alloys with Te (Se_1−xTe_x) offer a widely tunable bandgap. Solution processing of this materials system offers a route to low-cost fabrication. However, solution processing of Se has, thus far, only used hydrazine, which is an extremely hazardous solvent. In this work, we prepare and isolate propylammonium poly-Se and poly-Se–Te precursors from a safer thiol-amine solvent system. We formulate molecular inks by dissolving the precursor in dimethylformamide (DMF) with a monoethanolamine (EA) additive and process high-quality Se and Se_1−xTe_x films with bandgaps ranging from 1.20 eV to 1.86 eV. We fabricate PVs from these films using TiO₂ and MoO₃ charge transport layers (CTLs) to achieve power conversion efficiencies as high as 2.73% for Se and 2.33% for Se_0.7Te_0.3 under solar simulation. Se devices show excellent stability with no degradation after 1 month in air, enabled by the excellent stability of Se and the use of inorganic CTLs. This work represents an important step towards low-cost solution-phase processing of Se and Se_1−xTe_x alloys for PVs and photodetectors with low toxicity and high bandgap tunability.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 3000535

Report Number(s):: BNL--229098-2025-JAAM

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 43 Vol. 13; ISSN 2050-7488; ISSN 2050-7496

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (29)

Evaporated Se _x Te _1‐ _x Thin Films with Tunable Bandgaps for Short‐Wave Infrared Photodetectors Tan, Chaoliang; Amani, Matin; Zhao, Chunsong Advanced Materials, Vol. 32, Issue 38 https://doi.org/10.1002/adma.202001329	journal	August 2020
Standing 1D Chains Enable Efficient Wide‐Bandgap Selenium Solar Cells Liu, Qingxiang; Wang, Xia; Li, Zongbao Advanced Materials, Vol. 37, Issue 1 https://doi.org/10.1002/adma.202410835	journal	November 2024
Modern Processing and Insights on Selenium Solar Cells: The World's First Photovoltaic Device Hadar, Ido; Song, Tze‐Bin; Ke, Weijun Advanced Energy Materials, Vol. 9, Issue 16 https://doi.org/10.1002/aenm.201802766	journal	February 2019
Oxygen‐Assisted High‐Temperature Deposition of High‐Efficiency Trigonal Selenium Solar Cells Shen, Kai; Wang, Xinlong; Xiao, Binquan Advanced Energy Materials, Vol. 15, Issue 33 https://doi.org/10.1002/aenm.202501930	journal	June 2025
Photovoltaic Absorber “Glues” for Efficient Bifacial Selenium Photovoltaics An, Xiaoyan; Li, Zongbao; Wang, Xia Angewandte Chemie International Edition, Vol. 64, Issue 24 https://doi.org/10.1002/anie.202505297	journal	April 2025
Raman Effect in Selenium–Tellurium Mixed Crystals Geick, R.; Steigmeier, E. F.; Auderset, H. physica status solidi (b), Vol. 54, Issue 2 https://doi.org/10.1002/pssb.2220540226	journal	December 1972
Fabrication and characterization of ZnO/Se1-xTex solar cells Zheng, Jiajia; Fu, Liuchong; He, Yuming Frontiers of Optoelectronics, Vol. 15, Issue 1 https://doi.org/10.1007/s12200-022-00040-5	journal	September 2022
Analyzing and Tuning the Chalcogen–Amine–Thiol Complexes for Tailoring of Chalcogenide Syntheses Deshmukh, Swapnil D.; Easterling, Leah F.; Manheim, Jeremy M. Inorganic Chemistry, Vol. 59, Issue 12 https://doi.org/10.1021/acs.inorgchem.0c00597	journal	May 2020
Solution Processed Fabrication of Se–Te Alloy Thin Films for Application in PV Devices Deshmukh, Swapnil D.; Miskin, Caleb K.; Pradhan, Apurva A. ACS Applied Energy Materials, Vol. 5, Issue 3 https://doi.org/10.1021/acsaem.1c03896	journal	March 2022
Laser-Annealing and Solid-Phase Epitaxy of Selenium Thin-Film Solar Cells Nielsen, Rasmus; Hemmingsen, Tobias H.; Bonczyk, Tobias G. ACS Applied Energy Materials, Vol. 6, Issue 17 https://doi.org/10.1021/acsaem.3c01464	journal	August 2023
Two-Stage Melt Processing of Phase-Pure Selenium for Printable Triple-Mesoscopic Solar Cells Wu, Jiawen; Zhang, Zhihui; Tong, Changheng ACS Applied Materials & Interfaces, Vol. 11, Issue 37 https://doi.org/10.1021/acsami.9b09572	journal	August 2019
Solution-Processed Air-Stable Mesoscopic Selenium Solar Cells Zhu, Menghua; Hao, Feng; Ma, Lin ACS Energy Letters, Vol. 1, Issue 2 https://doi.org/10.1021/acsenergylett.6b00249	journal	August 2016
Nonlinear Band Gap Tunability in Selenium–Tellurium Alloys and Its Utilization in Solar Cells Hadar, Ido; Hu, Xiaobing; Luo, Zhong-Zhen ACS Energy Letters, Vol. 4, Issue 9 https://doi.org/10.1021/acsenergylett.9b01619	journal	August 2019
Identification of the Molecular Precursors for Hydrazine Solution Processed CuIn(Se,S)₂ Films and Their Interactions Chung, Choong-Heui; Li, Sheng-Han; Lei, Bao Chemistry of Materials, Vol. 23, Issue 4 https://doi.org/10.1021/cm103258u	journal	January 2011
Ultrathin high band gap solar cells with improved efficiencies from the world’s oldest photovoltaic material Todorov, Teodor K.; Singh, Saurabh; Bishop, Douglas M. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00582-9	journal	September 2017
Selenium as a photoabsorber for inorganic–organic hybrid solar cells Wang, Kai; Shi, Yantao; Zhang, Hong Phys. Chem. Chem. Phys., Vol. 16, Issue 42 https://doi.org/10.1039/c4cp02821j	journal	January 2014
Facile dissolution of selenium and tellurium in a thiol–amine solvent mixture under ambient conditions Webber, David H.; Buckley, Jannise J.; Antunez, Priscilla D. Chemical Science, Vol. 5, Issue 6 https://doi.org/10.1039/c4sc00749b	journal	January 2014
A selenium-based “alkahest”: reactive dissolutions of metals and metal compounds with n-alkylammonium polyselenide solutions Turnley, Jonathan W.; Deshmukh, Swapnil D.; Boulos, Victoria M. Inorganic Chemistry Frontiers, Vol. 10, Issue 20, p. 6032-6044 https://doi.org/10.1039/d3qi01632c	journal	August 2023
Solution processed metal chalcogenide semiconductors for inorganic thin film photovoltaics Turnley, Jonathan W.; Agrawal, Rakesh Chemical Communications, Vol. 60, Issue 40, p. 5245-5269 https://doi.org/10.1039/d4cc01057d	journal	December 2023
Intrinsic point defect tolerance in selenium for indoor and tandem photovoltaics Kavanagh, Seán R.; Nielsen, Rasmus S.; Hansen, John L. Energy & Environmental Science, Vol. 18, Issue 9 https://doi.org/10.1039/d4ee04647a	journal	January 2025
Bulk and metastable defects in CuIn1−xGaxSe2 thin films using drive-level capacitance profiling Heath, Jennifer T.; Cohen, J. David; Shafarman, William N. Journal of Applied Physics, Vol. 95, Issue 3 https://doi.org/10.1063/1.1633982	journal	February 2004
Studies on Tellurium‐Selenium Alloys Grison, E. The Journal of Chemical Physics, Vol. 19, Issue 9 https://doi.org/10.1063/1.1748484	journal	September 1951
Preparation of Se-based solar cell using spin-coating method in ambient condition Zhu, Menghua; Deng, Yaxin; Liu, Weiwei Chinese Physics B, Vol. 27, Issue 1 https://doi.org/10.1088/1674-1056/27/1/015202	journal	January 2018
Variable-temperature and carrier-resolved photo-Hall measurements of high-performance selenium thin-film solar cells Nielsen, Rasmus S.; Gunawan, Oki; Todorov, Teodor Physical Review B, Vol. 111, Issue 16 https://doi.org/10.1103/PhysRevB.111.165202	journal	April 2025
Selenium and the role of defects for photovoltaic applications Moustafa, Hadeel; Kangsabanik, Jiban; Bertoldo, Fabian Physical Review Materials, Vol. 8, Issue 1 https://doi.org/10.1103/PhysRevMaterials.8.015402	journal	January 2024
Resolving the trap levels of Se and Se1−xTex via deep-level transient spectroscopy Chen, Xin; Bai, Songxue; Li, Ruiming Physical Review Materials, Vol. 8, Issue 3 https://doi.org/10.1103/PhysRevMaterials.8.033805	journal	March 2024
Monolithic Selenium/Silicon Tandem Solar Cells Nielsen, Rasmus; Crovetto, Andrea; Assar, Alireza PRX Energy, Vol. 3, Issue 1 https://doi.org/10.1103/prxenergy.3.013013	journal	March 2024
Indoor photovoltaics awaken the world’s first solar cells Yan, Bin; Liu, Xinsheng; Lu, Wenbo Science Advances, Vol. 8, Issue 49 https://doi.org/10.1126/sciadv.adc9923	journal	December 2022
On a new form of selenium cell, and some electrical discoveries made by its use Fritts, C. E. American Journal of Science, Vol. s3-26, Issue 156 https://doi.org/10.2475/ajs.s3-26.156.465	journal	December 1883

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