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Title: Distinguishing bulk and surface recombination in CdTe thin films and solar cells using time-resolved terahertz and photoluminescence spectroscopies

Journal Article · · Journal of Applied Physics
DOI: https://doi.org/10.1063/5.0064730 · OSTI ID:1828279

Understanding the nature of recombination and its dependence on defects and interfaces is essential for engineering materials and contacts for higher open circuit voltage (Voc) and power conversion efficiency in photovoltaic (PV) devices. Time-resolved photoluminescence (TRPL) has conventionally been used to evaluate recombination, but carrier redistribution often dominates the response at short times. In this work, we report on the quantification of carrier dynamics and recombination mechanisms by complementary use of both time-resolved terahertz spectroscopy (TRTS) and TRPL combined with numerical modeling of the continuity equations and Poisson’s equation. We have demonstrated this approach using CdTe thin films. A thin film stack with CdTe fabricated by vapor transport deposition and treated with CdCl2 exhibited a bulk lifetime of 1.7 ± 0.1 ns, negligible CdTe/CdS interface recombination velocity, and back surface recombination velocity of 6.3 ± 1.3 x104 cm/s. In contrast, a film stack without CdCl2 treatment had a bulk lifetime of only 68 ± 12 ps and a higher interface recombination velocity of 4 ± 2 x108 cm/s. By determining the locus and mechanisms of performance-limiting recombination, we can accelerate the development of thin-film PVs with higher Voc and efficiency. While the method has been demonstrated here using CdTe, it is also applicable to perovskites, Cu(InGa)Se2, Cu2ZnSn(S,Se)4, and emerging technologies.

Research Organization:
Drexel Univ., Philadelphia, PA (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
Grant/Contract Number:
EE0008986; AC36-08GO28308
OSTI ID:
1828279
Alternate ID(s):
OSTI ID: 1828070; OSTI ID: 1834559
Report Number(s):
NREL/JA-5900-81617; DE-EE0008986; TRN: US2216039
Journal Information:
Journal of Applied Physics, Vol. 130, Issue 16; ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (46)

Ultrafast photocarrier dynamics in a 3D Dirac semimetal Cd 3 As 2 film studied with terahertz spectroscopy journal June 2019
The role of drift, diffusion, and recombination in time-resolved photoluminescence of CdTe solar cells determined through numerical simulation: The role of drift, diffusion, and recombination in time-resolved photoluminescence journal February 2013
Measurement of charge carrier mobilities in thin films on metal substrates by reflection time resolved terahertz spectroscopy journal January 2017
Charge-Carrier Dynamics and Mobilities in Formamidinium Lead Mixed-Halide Perovskites journal September 2015
Relating Carrier Dynamics and Photovoltaic Device Performance of Single-Crystalline Cu 2 Zn Sn Se 4 journal March 2019
Chalcogenide Photovoltaics book January 2011
Band structure of α-Sn, InSb and CdTe including spin-orbit effects journal July 1968
Overcoming Carrier Concentration Limits in Polycrystalline CdTe Thin Films with In Situ Doping journal September 2018
Numerical simulation of high-efficiency, scalable, all-back-contact Cd(Se,Te) solar cells journal June 2020
Ultrafast Photoluminescence from the Core and the Shell in CdSe/CdS Dot-in-Rod Heterostructures journal November 2015
Charge-Carrier Trapping Dynamics in Bismuth-Doped Thin Films of MAPbBr 3 Perovskite journal April 2020
Emitter/absorber interface of CdTe solar cells journal June 2016
Theoretical study of time-resolved luminescence in semiconductors. II. Pulsed excitation journal September 2014
Identification of Recombination Losses in CdSe/CdTe Solar Cells from Spectroscopic and Microscopic Time‐Resolved Photoluminescence journal March 2021
The roles of carrier concentration and interface, bulk, and grain-boundary recombination for 25% efficient CdTe solar cells journal June 2017
Charge‐Carrier Dynamics, Mobilities, and Diffusion Lengths of 2D–3D Hybrid Butylammonium–Cesium–Formamidinium Lead Halide Perovskites journal June 2019
Bulk and surface recombination properties in thin film semiconductors with different surface treatments from time-resolved photoluminescence measurements journal March 2019
Slow Electron–Hole Recombination in Lead Iodide Perovskites Does Not Require a Molecular Dipole journal September 2017
Nanosecond carrier lifetimes in solution-processed enargite (Cu 3 AsS 4 ) thin films journal October 2020
Obtaining Large Columnar CdTe Grains and Long Lifetime on Nanocrystalline CdSe, MgZnO, or CdS Layers journal January 2018
Time-resolved photoluminescence studies of CdTe solar cells journal September 2003
Terahertz Spectroscopy journal June 2011
Identifying the Real Minority Carrier Lifetime in Nonideal Semiconductors: A Case Study of Kesterite Materials journal May 2017
Terahertz Spectroscopy journal July 2002
Effects of cation composition on carrier dynamics and photovoltaic performance in Cu2ZnSnSe4 monocrystal solar cells journal February 2020
Hybrid Perovskites for Photovoltaics: Charge-Carrier Recombination, Diffusion, and Radiative Efficiencies journal December 2015
Minority and Majority Charge Carrier Mobility in Cu2ZnSnSe4 revealed by Terahertz Spectroscopy journal September 2018
Design of a vapor transport deposition process for thin film materials
  • Hanket, G. M.; McCandless, B. E.; Buchanan, W. A.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 24, Issue 5 https://doi.org/10.1116/1.2214689
journal September 2006
Solar cell efficiency tables (version 52)
  • Green, Martin A.; Hishikawa, Yoshihiro; Dunlop, Ewan D.
  • Progress in Photovoltaics: Research and Applications, Vol. 26, Issue 7 https://doi.org/10.1002/pip.3040
journal June 2018
Radiative and interfacial recombination in CdTe heterostructures journal December 2014
Properties of the CdCl2 Air-annealed CSS CdTe Thin Films journal January 2014
Exceeding 20% efficiency with in situ group V doping in polycrystalline CdTe solar cells journal August 2019
Employing time-resolved terahertz spectroscopy to analyze carrier dynamics in thin-film Cu2ZnSn(S,Se)4 absorber layers journal June 2014
Terahertz spectroscopy and imaging - Modern techniques and applications journal October 2010
High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites journal December 2013
Optically controlled ultrafast terahertz switching in a CdTe nanostructure thin film journal January 2019
Separating grain-boundary and bulk recombination with time-resolved photoluminescence microscopy journal December 2017
Lifetime, Mobility, and Diffusion of Photoexcited Carriers in Ligand-Exchanged Lead Selenide Nanocrystal Films Measured by Time-Resolved Terahertz Spectroscopy journal January 2015
Correlation Between Measured Minority-Carrier Lifetime and $\hbox{Cu}( \hbox{In}, \hbox{Ga})\hbox{Se}_{2}$ Device Performance journal November 2010
Two dimensional numerical simulations of carrier dynamics during time-resolved photoluminescence decays in two-photon microscopy measurements in semiconductors journal July 2015
Terahertz time domain spectroscopy for carrier lifetime mapping in the picosecond to microsecond regime journal January 2015
Physics and chemistry of CdTe/CdS thin film heterojunction photovoltaic devices: fundamental and critical aspects journal January 2014
Theoretical study of time-resolved luminescence in semiconductors. III. Trap states in the band gap journal September 2015
Analysis of Photocarrier Dynamics at Interfaces in Perovskite Solar Cells by Time-Resolved Photoluminescence journal October 2018
Applicability of the thin-film approximation in terahertz photoconductivity measurements journal December 2018
Impact of In Situ Annealing Time on CdTe Polycrystalline Film and Device Performance journal November 2018