Slow geminate-charge-pair recombination dynamics at polymer: Fullerene heterojunctions in efficient organic solar cells

We explore charge recombination dynamics at electron donor‐acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative (PC70BM), by means of combined time‐resolved photoluminescence and transient absorption spectroscopies. Following prompt exciton dissociatio...

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Published in:	Journal of polymer science. Part B, Polymer physics Vol. 50; no. 20; pp. 1395 - 1404
Main Authors:	Provencher, Françoise, Sakowicz, Maciej, Brosseau, Colin-Nadeau, Latini, Gianluca, Beaupré, Serge, Leclerc, Mario, Reynolds, Luke X., Haque, Saif A., Leonelli, Richard, Silva, Carlos
Format:	Journal Article
Language:	English
Published:	Hoboken Wiley Subscription Services, Inc., A Wiley Company 15.10.2012 Wiley
Subjects:	Application fields Applied sciences Charge charge-transfer excitons Derivatives Dynamics Energy Exact sciences and technology Excitation Fullerenes Heterojunctions materials science Natural energy organic solar cells Pathways Photovoltaic conversion physical chemistry physics polaron-pair recombination dynamics Polymer industry, paints, wood polymer science & technology semiconductor polymers Semiconductors Solar cells. Photoelectrochemical cells Solar energy Technology of polymers Terpolymer Fullerene compounds Solid solid interface Photoluminescence Organic solar cells Modeling Excitonic process Charge carrier recombination Optical properties Nitrogen heterocycle copolymer physics Aromatic copolymer Heterojunction physical chemistry materials science Carbazole derivative copolymer charge-transfer excitons Thiophene copolymer Experimental study polymer science & technology Luminescence decay semiconductor polymers Conjugated copolymer Kinetics polaron-pair recombination dynamics
ISSN:	0887-6266, 1099-0488
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Abstract	We explore charge recombination dynamics at electron donor‐acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative (PC70BM), by means of combined time‐resolved photoluminescence and transient absorption spectroscopies. Following prompt exciton dissociation across the heterojunction, a subset of bound electron‐hole pairs recombines with a temperature‐independent rate distribution spanning submicrosecond timescales to produce luminescent charge‐transfer excitons (CTX). At 14 K, this slow mechanism is the dominant geminate charge recombination pathway, whereas we also observe CTX emission on subnanosecond timescales at 293 K. We thus find that at these temperatures, a fraction of the initial charge‐pair population is trapped deeply such that they only recombine slowly over a broad distribution of timescales by quantum tunneling. We identify geminate polaron pairs (GPP) as a reservoir of long‐lived localized states that repopulate the CTX up to microsecond timescales. The observation of such distributed geminate‐charge recombination highlights the importance of the molecular nature of specific donor–acceptor electronic interactions in defining the relaxation pathways of trapped GPP. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012 Charge‐transfer‐exciton recombination dynamics are probed over timescales orders of magnitude longer than has been previously reported for PCDTBT:PC70BM donor‐acceptor heterostructures. Delayed photoluminescence is attributed to slow generation of charge‐transfer excitons via tunneling from deeply trapped geminate polaron pairs. Using time‐resolved spectroscopic measurements at various temperatures and photophysical modeling, it is estimated that 16% of geminate recombination at room temperature originate from this slow mechanism.
AbstractList	We explore charge recombination dynamics at electron donor‐acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative (PC70BM), by means of combined time‐resolved photoluminescence and transient absorption spectroscopies. Following prompt exciton dissociation across the heterojunction, a subset of bound electron‐hole pairs recombines with a temperature‐independent rate distribution spanning submicrosecond timescales to produce luminescent charge‐transfer excitons (CTX). At 14 K, this slow mechanism is the dominant geminate charge recombination pathway, whereas we also observe CTX emission on subnanosecond timescales at 293 K. We thus find that at these temperatures, a fraction of the initial charge‐pair population is trapped deeply such that they only recombine slowly over a broad distribution of timescales by quantum tunneling. We identify geminate polaron pairs (GPP) as a reservoir of long‐lived localized states that repopulate the CTX up to microsecond timescales. The observation of such distributed geminate‐charge recombination highlights the importance of the molecular nature of specific donor–acceptor electronic interactions in defining the relaxation pathways of trapped GPP. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012 Charge‐transfer‐exciton recombination dynamics are probed over timescales orders of magnitude longer than has been previously reported for PCDTBT:PC70BM donor‐acceptor heterostructures. Delayed photoluminescence is attributed to slow generation of charge‐transfer excitons via tunneling from deeply trapped geminate polaron pairs. Using time‐resolved spectroscopic measurements at various temperatures and photophysical modeling, it is estimated that 16% of geminate recombination at room temperature originate from this slow mechanism. We explore charge recombination dynamics at electron donor‐acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative (PC 70 BM), by means of combined time‐resolved photoluminescence and transient absorption spectroscopies. Following prompt exciton dissociation across the heterojunction, a subset of bound electron‐hole pairs recombines with a temperature‐independent rate distribution spanning submicrosecond timescales to produce luminescent charge‐transfer excitons (CTX). At 14 K, this slow mechanism is the dominant geminate charge recombination pathway, whereas we also observe CTX emission on subnanosecond timescales at 293 K. We thus find that at these temperatures, a fraction of the initial charge‐pair population is trapped deeply such that they only recombine slowly over a broad distribution of timescales by quantum tunneling. We identify geminate polaron pairs (GPP) as a reservoir of long‐lived localized states that repopulate the CTX up to microsecond timescales. The observation of such distributed geminate‐charge recombination highlights the importance of the molecular nature of specific donor–acceptor electronic interactions in defining the relaxation pathways of trapped GPP. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012 We explore charge recombination dynamics at electron donor-acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative (PC(70)BM), by means of combined time-resolved photolumi-nescence and transient absorption spectroscopies. Following prompt exciton dissociation across the heterojunction, a subset of bound electron-hole pairs recombines with a temperature-independent rate distribution spanning submi-crosecond timescales to produce luminescent charge-transfer excitons (CTX). At 14K, this slow mechanism is the dominant geminate charge recombination pathway, whereas we also observe CTX emission on subnanosecond timescales at 293 K. We thus find that at these temperatures, a fraction of the initial charge-pair population is trapped deeply such that they only recombine slowly over a broad distribution of timescales by quantum tunneling. We identify geminate polaron pairs (GPP) as a reservoir of long-lived localized states that repopulate the CTX up to microsecond timescales. The observation of such distributed geminate-charge recombination highlights the importance of the molecular nature of specific donor-acceptor electronic interactions in defining the relaxation pathways of trapped GPP.
Author	Reynolds, Luke X. Sakowicz, Maciej Silva, Carlos Provencher, Françoise Leonelli, Richard Latini, Gianluca Beaupré, Serge Brosseau, Colin-Nadeau Leclerc, Mario Haque, Saif A.
Author_xml	– sequence: 1 givenname: Françoise surname: Provencher fullname: Provencher, Françoise organization: Département de physique et Regroupement québécois sur les matériaux de pointe, Université de Montréal, C.P. 6128, Succursale centre-ville, Montréal, Québec, Canada H3C 3J7 – sequence: 2 givenname: Maciej surname: Sakowicz fullname: Sakowicz, Maciej organization: Département de physique et Regroupement québécois sur les matériaux de pointe, Université de Montréal, C.P. 6128, Succursale centre-ville, Montréal, Québec, Canada H3C 3J7 – sequence: 3 givenname: Colin-Nadeau surname: Brosseau fullname: Brosseau, Colin-Nadeau organization: Département de physique et Regroupement québécois sur les matériaux de pointe, Université de Montréal, C.P. 6128, Succursale centre-ville, Montréal, Québec, Canada H3C 3J7 – sequence: 4 givenname: Gianluca surname: Latini fullname: Latini, Gianluca organization: Centre for Biomolecular Nanotechnologies, Istituto Italiano di Tecnologia, Via Barsanti, 73010, Arnesano (Lecce), Italy – sequence: 5 givenname: Serge surname: Beaupré fullname: Beaupré, Serge organization: Département de chimie, Université Laval, Québec (Québec), Canada G1K 7P4 – sequence: 6 givenname: Mario surname: Leclerc fullname: Leclerc, Mario organization: Département de chimie, Université Laval, Québec (Québec), Canada G1K 7P4 – sequence: 7 givenname: Luke X. surname: Reynolds fullname: Reynolds, Luke X. organization: Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom – sequence: 8 givenname: Saif A. surname: Haque fullname: Haque, Saif A. organization: Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom – sequence: 9 givenname: Richard surname: Leonelli fullname: Leonelli, Richard organization: Département de physique et Regroupement québécois sur les matériaux de pointe, Université de Montréal, C.P. 6128, Succursale centre-ville, Montréal, Québec, Canada H3C 3J7 – sequence: 10 givenname: Carlos surname: Silva fullname: Silva, Carlos email: carlos.silva@umontreal.ca organization: Département de physique et Regroupement québécois sur les matériaux de pointe, Université de Montréal, C.P. 6128, Succursale centre-ville, Montréal, Québec, Canada H3C 3J7
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Keywords	Terpolymer Fullerene compounds Solid solid interface Photoluminescence Organic solar cells Modeling Excitonic process Charge carrier recombination Optical properties Nitrogen heterocycle copolymer physics Aromatic copolymer Heterojunction physical chemistry materials science Carbazole derivative copolymer charge-transfer excitons Thiophene copolymer Experimental study polymer science & technology Luminescence decay semiconductor polymers Conjugated copolymer Kinetics polaron-pair recombination dynamics
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SSID	ssj0009959
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Snippet	We explore charge recombination dynamics at electron donor‐acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative... We explore charge recombination dynamics at electron donor-acceptor heterojunctions, formed between a semiconductor polymer (PCDTBT) and a fullerene derivative...
SourceID	proquest pascalfrancis crossref wiley istex
SourceType	Aggregation Database Index Database Enrichment Source Publisher
StartPage	1395
SubjectTerms	Application fields Applied sciences Charge charge-transfer excitons Derivatives Dynamics Energy Exact sciences and technology Excitation Fullerenes Heterojunctions materials science Natural energy organic solar cells Pathways Photovoltaic conversion physical chemistry physics polaron-pair recombination dynamics Polymer industry, paints, wood polymer science & technology semiconductor polymers Semiconductors Solar cells. Photoelectrochemical cells Solar energy Technology of polymers
Title	Slow geminate-charge-pair recombination dynamics at polymer: Fullerene heterojunctions in efficient organic solar cells
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Volume	50
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