| 1. |
- Andersson, Mattias, et al.
(author)
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Unified Study of Recombination in Polymer:Fullerene Solar Cells Using Transient Absorption and Charge-Extraction Measurements
- 2013
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In: Journal of Physical Chemistry Letters. - : American Chemical Society. - 1948-7185 .- 1948-7185. ; 4:12, s. 2069-2072
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Journal article (peer-reviewed)abstract
- Recombination in the well-performing bulk heterojunction solar cell blend between the conjugated polymer TQ-1 and the substituted fullerene PCBM has been investigated with pump-probe transient absorption and charge extraction of photo-generated carriers (photo-CELIV). Both methods are shown to generate identical and overlapping data under appropriate experimental conditions. The dominant type of recombination is bimolecular with a rate constant of 7 x 10(-12) cm(-3) s(-1). This recombination rate is shown to be fully consistent with solar cell performance. Deviations from an ideal bimolecular recombination process, in this material system only observable at high pump fluences, are explained with a time-dependent charge-carrier mobility, and the implications of such a behavior for device development are discussed.
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| 2. |
- Bian, Qingzhen, 1988-, et al.
(author)
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Vibronic coherence contributes to photocurrent generation in organic semiconductor heterojunction diodes
- 2020
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In: Nature Communications. - : NATURE PUBLISHING GROUP. - 2041-1723. ; 11:1
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Journal article (peer-reviewed)abstract
- Charge separation dynamics after the absorption of a photon is a fundamental process relevant both for photosynthetic reaction centers and artificial solar conversion devices. It has been proposed that quantum coherence plays a role in the formation of charge carriers in organic photovoltaics, but experimental proofs have been lacking. Here we report experimental evidence of coherence in the charge separation process in organic donor/acceptor heterojunctions, in the form of low frequency oscillatory signature in the kinetics of the transient absorption and nonlinear two-dimensional photocurrent spectroscopy. The coherence plays a decisive role in the initial 200 femtoseconds as we observe distinct experimental signatures of coherent photocurrent generation. This coherent process breaks the energy barrier limitation for charge formation, thus competing with excitation energy transfer. The physics may inspire the design of new photovoltaic materials with high device performance, which explore the quantum effects in the next-generation optoelectronic applications.
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| 3. |
- De, Swati, et al.
(author)
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Exciton Dynamics in Alternating Polyfluorene/Fullerene Blends
- 2008
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In: Journal of Chemical Physics. - College Park, MD, United States : American Institute of Physics (AIP). - 0021-9606 .- 1089-7690. ; 350:1-3, s. 14-22
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Journal article (peer-reviewed)abstract
- Exciton dynamics in alternating copolymer/fullerene solar cell blends have been investigated using femtosecond transient absorption spectroscopy. The acceptor concentrations have been varied over a wide range. Experimental data, kinetic modeling and simulations, all indicate that the efficiency of exciton conversion to charges is 100% even at acceptor concentrations as low as 20 wt%. The reported dependence of solar cell efficiency on fullerene concentration may thus arise from other factors. However, there exists an acceptor concentration threshold (5 wt%) below which a substantial fraction of the excitations remain unquenched. The results, we believe are very relevant to optimization of performance efficiency by clever manipulation of morphology. We have also observed exciton–exciton energy transfer in these blends at low acceptor concentrations.
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| 4. |
- De, Swati, et al.
(author)
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Geminate charge recombination in alternating polyfluorene copolymer/fullerene blends
- 2007
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 129:27, s. 8466-8472
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Journal article (peer-reviewed)abstract
- By measuring excited state and charge dynamics in blends of an alternating polyfluorene copolymer and fullerene derivative over nine orders in time and two orders in light intensity, we have monitored the light-induced processes from ultrafast charge photogeneration to much slower decay of charges by recombination. We find that at low light intensities relevant to solar cell operation relatively fast (∼30 ns) geminate recombination is the dominating charge decay process, while nongeminate recombination has a negligible contribution. The conclusion of our work is that under solar illumination conditions geminate recombination of charges may be directly competing with efficient charge collection in polymer/fullerene solar cells. © 2007 American Chemical Society.
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| 5. |
- Infahsaeng, Yingyot, et al.
(author)
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Transient photocurrent of bulk heterojunction solar cell characterized by ns-laser and sub-ms LED
- 2015
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In: Proceedings of SPIE. - : SPIE. - 0277-786X .- 1996-756X. ; 9659
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Conference paper (peer-reviewed)abstract
- We measure the transient photocurrent of APFO3:PCBM bulk heterojunction solar cells illuminated with ns-laser and sub-ms LED light sources. The ratio of the number of collective charges to the number of excited photon (external quantum efficiency, EQE) and the transient photocurrent fall times have been carried out with difference pulse durations and fluences. The EQEs characterized by ns-laser source are shown to obey the bimolecular recombination at high excitation fluences. The increasing of transient photocurrent fall times suggests that the fall times of free charge carriers are effected by deep trap density of state (DoS) and thus the free charge carriers have a sufficient time for bimolecular recombination at short circuit condition. At the same fluences, however, the EQEs characterized by sub-ms LED sources exhibit an excitation fluences independence of EQE. The transient photocurrent fall times with sub-ms LED sources are rather constant when the excitation fluences increases indicating that the deep trap DoS has less effect at short circuit condition for longer pulse duration.
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| 6. |
- Jespersen, Kim, et al.
(author)
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Charge formation and transport in bulk-heterojunction solar cells based on alternating polyfluorene copolymers blended with fullerenes
- 2006
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In: Organic Electronics. - : Elsevier BV. - 1566-1199 .- 1878-5530. ; 7:4, s. 235-242
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Journal article (peer-reviewed)abstract
- We investigate charge formation in bulk-heterojunction solar cells based on conjugated polymers in the form of alternating polyfluorene copolymers and the methanofullerene PCBM. Using transient absorption spectroscopy we show that optimal charge formation is obtained with 20-50 wt% PCBM. This is in contrast to the maximum short circuit current density obtained at similar to 80 wt% PCBM as determined by steady state current density-voltage characterization. Hence, we show explicitly that the solar cell performance of these interpenetrating polymer networks containing PCBM is limited by charge transport rather than by formation of charges. (c) 2006 Elsevier B.V. All rights reserved.
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| 7. |
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| 8. |
- Nemec, Hynek, et al.
(author)
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Charge carrier dynamics in alternating polyfluorene copolymer : Fullerene blends probed by terahertz spectroscopy
- 2008
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In: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 112:16, s. 6558-6563
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Journal article (peer-reviewed)abstract
- Time-resolved terahertz spectroscopy is used for investigation of photoinduced charge carrier dynamics in blends of a polyfluorene copolymer (poly[2,7-(9,9-dioctyl-fluorene)-alt-5,5-(4',7'-di-2-thienyl- 2',1',3-benzo-thiadiazole)]) and an electron acceptor ([6,6]-phenyl-C61-butyric acid methyl ester). The transient far-infrared response appears instantaneously after photoexcitation. We show that the transient conductivity spectrum is dominated by two major contributions: response of separated charge carriers and response of coupled polaron pairs. © 2008 American Chemical Society.
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| 9. |
- Pal, S. K., et al.
(author)
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Geminate Charge Recombination in Polymer/Fullerene Bulk Heterojunction Films and Implications for Solar Cell Function
- 2010
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 1520-5126 .- 0002-7863. ; 132:35, s. 12440-12451
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Journal article (peer-reviewed)abstract
- We have studied the influence of three different fullerene derivatives on the charge generation and recombination dynamics of polymer/fullerene bulk heterojunction (BHJ) solar cell blends. Charge generation in APFO3/[70]PCBM and APFO3/[60]PCBM is very similar and somewhat slower than charge generation in APFO3/[70]BTPF. This difference qualitatively matches the trend in free energy change of electron transfer estimated from the LUMO energies of the polymer and fullerene derivatives. The first order (geminate) charge recombination rate is significantly different for the three fullerene derivatives studied and increases in the order APFO3/[70]PCBM
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| 10. |
- Pranculis, Vytenis, et al.
(author)
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Charge Carrier Generation and Transport in Different Stoichiometry APFO3:PC61BM Solar Cells
- 2014
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In: Journal of the American Chemical Society. - : American Chemical Society. - 0002-7863 .- 1520-5126. ; 136:32, s. 11331-11338
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Journal article (peer-reviewed)abstract
- In this paper we studied carrier drift dynamics in APFO3:PC61BM solar cells of varied stoichiometry (2:1, 1:1, and 1:4 APFO3:PC61BM) over a wide time range, from subpicoseconds to microseconds with a combination of ultrafast optical electric field probing and conventional transient integrated photocurrent techniques. Carrier drift and extraction dynamics are strongly stoichiometry dependent: the speed of electron or hole drift increases with higher concentration of PC61BM or polymer, respectively. The electron extraction from a sample with 80% PC61BM takes place during hundreds of picoseconds, but slows down to sub-microseconds in a sample with 33% PC61BM. The hole extraction is less stoichiometry dependent: it varies form sub-nanoseconds to tens of nanoseconds when the PC61BM concentration changes from 33% to 80%. The electron extraction rate correlates with the conversion efficiency of solar cells, leading to the conclusion that fast electron motion is essential for efficient charge carrier separation preventing their geminate recombination.
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