Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells
Abstract
Here, we investigate the nature of occupation and relaxation within the charge transfer density of states (CT DOS) for bulk heterojunction organic solar cells consisting of the donor boron subphthalocyanine chloride and the acceptor C60. We observe relaxation of geminate CT states on a sub-ns timescale via an approximately 70-meV dynamic redshift in their photoluminescence, whereas free carrier relaxation at longer times leads to the formation of nongeminate CT states at even lower energy. In steady state, we find that thermalization within the DOS is incomplete, resulting in a Boltzmann-like CT state distribution characterized by an effective temperature above that of the ambient. These findings confirm that electron and hole populations can be far from equilibrium in organic solar cells and may prompt a reassessment of analyses that assume the same temperature for their charge-carrier distributions in the dark and under illumination.
- Authors:
-
- Pennsylvania State Univ., University Park, PA (United States)
- Princeton Univ., NJ (United States)
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States); Pennsylvania State Univ., University Park, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1595576
- Alternate Identifier(s):
- OSTI ID: 1546137
- Grant/Contract Number:
- SC0012458; SC0012365
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Applied
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 2331-7019
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 14 SOLAR ENERGY; Organic semiconductors; nonequilibrium; photovoltaics
Citation Formats
Brigeman, A. N., Fusella, M. A., Rand, B. P., and Giebink, N. C. Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells. United States: N. p., 2018.
Web. doi:10.1103/PhysRevApplied.10.034034.
Brigeman, A. N., Fusella, M. A., Rand, B. P., & Giebink, N. C. Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells. United States. https://doi.org/10.1103/PhysRevApplied.10.034034
Brigeman, A. N., Fusella, M. A., Rand, B. P., and Giebink, N. C. Tue .
"Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells". United States. https://doi.org/10.1103/PhysRevApplied.10.034034. https://www.osti.gov/servlets/purl/1595576.
@article{osti_1595576,
title = {Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells},
author = {Brigeman, A. N. and Fusella, M. A. and Rand, B. P. and Giebink, N. C.},
abstractNote = {Here, we investigate the nature of occupation and relaxation within the charge transfer density of states (CT DOS) for bulk heterojunction organic solar cells consisting of the donor boron subphthalocyanine chloride and the acceptor C60. We observe relaxation of geminate CT states on a sub-ns timescale via an approximately 70-meV dynamic redshift in their photoluminescence, whereas free carrier relaxation at longer times leads to the formation of nongeminate CT states at even lower energy. In steady state, we find that thermalization within the DOS is incomplete, resulting in a Boltzmann-like CT state distribution characterized by an effective temperature above that of the ambient. These findings confirm that electron and hole populations can be far from equilibrium in organic solar cells and may prompt a reassessment of analyses that assume the same temperature for their charge-carrier distributions in the dark and under illumination.},
doi = {10.1103/PhysRevApplied.10.034034},
journal = {Physical Review Applied},
number = 3,
volume = 10,
place = {United States},
year = {Tue Sep 18 00:00:00 EDT 2018},
month = {Tue Sep 18 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Role of the Charge Transfer State in Organic Donor-Acceptor Solar Cells
journal, August 2010
- Deibel, Carsten; Strobel, Thomas; Dyakonov, Vladimir
- Advanced Materials, Vol. 22, Issue 37
Ultrafast Long-Range Charge Separation in Organic Semiconductor Photovoltaic Diodes
journal, December 2013
- Gelinas, S.; Rao, A.; Kumar, A.
- Science, Vol. 343, Issue 6170
Entropy and Disorder Enable Charge Separation in Organic Solar Cells
journal, October 2016
- Hood, Samantha N.; Kassal, Ivan
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 22
Low-Temperature Behaviour of Charge Transfer Excitons in Narrow-Bandgap Polymer-Based Bulk Heterojunctions
journal, May 2011
- Jarzab, Dorota; Cordella, Fabrizio; Gao, Jio
- Advanced Energy Materials, Vol. 1, Issue 4
Nanoscale transport of charge-transfer states in organic donor–acceptor blends
journal, September 2015
- Deotare, P. B.; Chang, W.; Hontz, E.
- Nature Materials, Vol. 14, Issue 11
Charge-Transfer States and Upper Limit of the Open-Circuit Voltage in Polymer:Fullerene Organic Solar Cells
journal, November 2010
- Vandewal, Koen; Tvingstedt, Kristofer; Manca, Jean V.
- IEEE Journal of Selected Topics in Quantum Electronics, Vol. 16, Issue 6
Light intensity dependence of open-circuit voltage of polymer:fullerene solar cells
journal, March 2005
- Koster, L. J. A.; Mihailetchi, V. D.; Ramaker, R.
- Applied Physics Letters, Vol. 86, Issue 12
Reciprocity relation between photovoltaic quantum efficiency and electroluminescent emission of solar cells
journal, August 2007
- Rau, Uwe
- Physical Review B, Vol. 76, Issue 8
Relating the open-circuit voltage to interface molecular properties of donor:acceptor bulk heterojunction solar cells
journal, March 2010
- Vandewal, Koen; Tvingstedt, Kristofer; Gadisa, Abay
- Physical Review B, Vol. 81, Issue 12
Electroluminescence of the Dye-Sensitized Solar Cell
journal, March 1999
- Trupke, T.; Würfel, P.; Uhlendorf, I.
- The Journal of Physical Chemistry B, Vol. 103, Issue 11
On the origin of the open-circuit voltage of polymer–fullerene solar cells
journal, October 2009
- Vandewal, Koen; Tvingstedt, Kristofer; Gadisa, Abay
- Nature Materials, Vol. 8, Issue 11, p. 904-909
Theory to carrier recombination in organic disordered semiconductors
journal, June 2014
- Hofacker, A.; Oelerich, J. O.; Nenashev, A. V.
- Journal of Applied Physics, Vol. 115, Issue 22
Efficient Organic Photovoltaic Cells Based on Nanocrystalline Mixtures of Boron Subphthalocyanine Chloride and C60
journal, December 2011
- Pandey, Richa; Gunawan, Aloysius A.; Mkhoyan, K. Andre
- Advanced Functional Materials, Vol. 22, Issue 3
Direct Observation of Entropy-Driven Electron-Hole Pair Separation at an Organic Semiconductor Interface
journal, June 2015
- Monahan, Nicholas R.; Williams, Kristopher W.; Kumar, Bharat
- Physical Review Letters, Vol. 114, Issue 24
The chemical potential of radiation
journal, June 1982
- Wurfel, P.
- Journal of Physics C: Solid State Physics, Vol. 15, Issue 18
Influence of energetic disorder on electroluminescence emission in polymer:fullerene solar cells
journal, July 2012
- Gong, Wei; Faist, Mark A.; Ekins-Daukes, Nicholas John
- Physical Review B, Vol. 86, Issue 2
Quasi-Fermi level splitting and sub-bandgap absorptivity from semiconductor photoluminescence
journal, November 2014
- Katahara, John K.; Hillhouse, Hugh W.
- Journal of Applied Physics, Vol. 116, Issue 17
Charge Carrier Extraction in Organic Solar Cells Governed by Steady-State Mobilities
journal, September 2017
- Le Corre, Vincent M.; Chatri, Azadeh Rahimi; Doumon, Nutifafa Y.
- Advanced Energy Materials, Vol. 7, Issue 22
Delocalization and dielectric screening of charge transfer states in organic photovoltaic cells
journal, February 2014
- Bernardo, B.; Cheyns, D.; Verreet, B.
- Nature Communications, Vol. 5, Issue 1
Thermalization and recombination in amorphous semiconductors
journal, October 1981
- Orenstein, J.; Kastner, M. A.
- Solid State Communications, Vol. 40, Issue 1
Reciprocity between Charge Injection and Extraction and Its Influence on the Interpretation of Electroluminescence Spectra in Organic Solar Cells
journal, May 2016
- Kirchartz, Thomas; Nelson, Jenny; Rau, Uwe
- Physical Review Applied, Vol. 5, Issue 5
Relationship between energetic disorder and open-circuit voltage in bulk heterojunction organic solar cells
journal, August 2011
- Blakesley, James C.; Neher, Dieter
- Physical Review B, Vol. 84, Issue 7
Understanding Open-Circuit Voltage Loss through the Density of States in Organic Bulk Heterojunction Solar Cells
journal, November 2015
- Collins, Samuel D.; Proctor, Christopher M.; Ran, Niva A.
- Advanced Energy Materials, Vol. 6, Issue 4
Ideal diode equation for organic heterojunctions. I. Derivation and application
journal, October 2010
- Giebink, N. C.; Wiederrecht, G. P.; Wasielewski, M. R.
- Physical Review B, Vol. 82, Issue 15
Diffusion-limited recombination in polymer-fullerene blends and its influence on photocurrent collection
journal, April 2003
- Nelson, Jenny
- Physical Review B, Vol. 67, Issue 15
On the Dissociation Efficiency of Charge Transfer Excitons and Frenkel Excitons in Organic Solar Cells: A Luminescence Quenching Study
journal, November 2010
- Tvingstedt, Kristofer; Vandewal, Koen; Zhang, Fengling
- The Journal of Physical Chemistry C, Vol. 114, Issue 49
Dispersion-Dominated Photocurrent in Polymer:Fullerene Solar Cells
journal, April 2014
- Melianas, Armantas; Pranculis, Vytenis; Devižis, Andrius
- Advanced Functional Materials, Vol. 24, Issue 28
Charge Photogeneration in Organic Solar Cells
journal, November 2010
- Clarke, Tracey M.; Durrant, James R.
- Chemical Reviews, Vol. 110, Issue 11, p. 6736-6767
Localized state distribution and its effect on recombination in organic solar cells
journal, August 2011
- Street, R. A.
- Physical Review B, Vol. 84, Issue 7
Photo-generated carriers lose energy during extraction from polymer-fullerene solar cells
journal, November 2015
- Melianas, Armantas; Etzold, Fabian; Savenije, Tom J.
- Nature Communications, Vol. 6, Issue 1
Hot charge-transfer excitons set the time limit for charge separation at donor/acceptor interfaces in organic photovoltaics
journal, December 2012
- Jailaubekov, Askat E.; Willard, Adam P.; Tritsch, John R.
- Nature Materials, Vol. 12, Issue 1
Photogenerated Carrier Mobility Significantly Exceeds Injected Carrier Mobility in Organic Solar Cells
journal, January 2017
- Melianas, Armantas; Pranculis, Vytenis; Xia, Yuxin
- Advanced Energy Materials, Vol. 7, Issue 9
Device model for the operation of polymer/fullerene bulk heterojunction solar cells
journal, August 2005
- Koster, L. J. A.; Smits, E. C. P.; Mihailetchi, V. D.
- Physical Review B, Vol. 72, Issue 8
Increased Open-Circuit Voltage of Organic Solar Cells by Reduced Donor-Acceptor Interface Area
journal, March 2014
- Vandewal, Koen; Widmer, Johannes; Heumueller, Thomas
- Advanced Materials, Vol. 26, Issue 23
Beyond Langevin Recombination: How Equilibrium Between Free Carriers and Charge Transfer States Determines the Open-Circuit Voltage of Organic Solar Cells
journal, April 2015
- Burke, Timothy M.; Sweetnam, Sean; Vandewal, Koen
- Advanced Energy Materials, Vol. 5, Issue 11
Open-circuit voltage limit caused by recombination through tail states in bulk heterojunction polymer-fullerene solar cells
journal, March 2010
- Garcia-Belmonte, Germà; Bisquert, Juan
- Applied Physics Letters, Vol. 96, Issue 11
Bimolecular recombination losses in polythiophene: Fullerene solar cells
journal, September 2008
- Shuttle, C. G.; O’Regan, B.; Ballantyne, A. M.
- Physical Review B, Vol. 78, Issue 11
Verification of a generalised Planck law by investigation of the emission from GaAs luminescent diodes
journal, April 1990
- Feuerbacher, B.; Wurfel, P.
- Journal of Physics: Condensed Matter, Vol. 2, Issue 16
Recombination Dynamics as a Key Determinant of Open Circuit Voltage in Organic Bulk Heterojunction Solar Cells: A Comparison of Four Different Donor Polymers
journal, August 2010
- Maurano, Andrea; Hamilton, Rick; Shuttle, Chris G.
- Advanced Materials, Vol. 22, Issue 44
Electronic Structure and Properties of Organic Bulk-Heterojunction Interfaces
journal, November 2015
- Street, Robert A.
- Advanced Materials, Vol. 28, Issue 20
Dispersive and steady-state recombination in organic disordered semiconductors
journal, December 2017
- Hofacker, Andreas; Neher, Dieter
- Physical Review B, Vol. 96, Issue 24
Verification of a generalized Planck law for luminescence radiation from silicon solar cells
journal, February 1992
- Schick, K.; Daub, E.; Finkbeiner, S.
- Applied Physics A Solids and Surfaces, Vol. 54, Issue 2
Works referencing / citing this record:
Reply to: Triplet-triplet annihilation in rubrene/C60 OLEDs with electroluminescence turn-on breaking the thermodynamic limit
journal, October 2019
- Engmann, Sebastian; Barito, Adam J.; Bittle, Emily G.
- Nature Communications, Vol. 10, Issue 1