Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells

Brigeman, A. N.; Fusella, M. A.; Rand, B. P.; Giebink, N. C.

doi:10.1103/PhysRevApplied.10.034034

Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells

Journal Article · Tue Sep 18 00:00:00 EDT 2018 · Physical Review Applied

DOI:https://doi.org/10.1103/PhysRevApplied.10.034034· OSTI ID:1595576

Brigeman, A. N. ^[1]; Fusella, M. A. ^[2]; Rand, B. P. ^[2]; Giebink, N. C. ^[3]

Pennsylvania State Univ., University Park, PA (United States); Princeton University
Princeton Univ., NJ (United States)
Pennsylvania State Univ., University Park, PA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Pennsylvania State Univ., University Park, PA (United States); Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012365; SC0012458

OSTI ID:: 1595576

Alternate ID(s):: OSTI ID: 1540693
OSTI ID: 1546137

Journal Information:: Physical Review Applied, Journal Name: Physical Review Applied Journal Issue: 3 Vol. 10; ISSN 2331-7019; ISSN PRAHB2

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (42)

Efficient Organic Photovoltaic Cells Based on Nanocrystalline Mixtures of Boron Subphthalocyanine Chloride and C60 Pandey, Richa; Gunawan, Aloysius A.; Mkhoyan, K. Andre Advanced Functional Materials, Vol. 22, Issue 3 https://doi.org/10.1002/adfm.201101948	journal	December 2011
Dispersion-Dominated Photocurrent in Polymer:Fullerene Solar Cells Melianas, Armantas; Pranculis, Vytenis; Devižis, Andrius Advanced Functional Materials, Vol. 24, Issue 28 https://doi.org/10.1002/adfm.201400404	journal	April 2014
Role of the Charge Transfer State in Organic Donor-Acceptor Solar Cells Deibel, Carsten; Strobel, Thomas; Dyakonov, Vladimir Advanced Materials, Vol. 22, Issue 37 https://doi.org/10.1002/adma.201000376	journal	August 2010
Recombination Dynamics as a Key Determinant of Open Circuit Voltage in Organic Bulk Heterojunction Solar Cells: A Comparison of Four Different Donor Polymers Maurano, Andrea; Hamilton, Rick; Shuttle, Chris G. Advanced Materials, Vol. 22, Issue 44 https://doi.org/10.1002/adma.201002360	journal	August 2010
Increased Open-Circuit Voltage of Organic Solar Cells by Reduced Donor-Acceptor Interface Area Vandewal, Koen; Widmer, Johannes; Heumueller, Thomas Advanced Materials, Vol. 26, Issue 23 https://doi.org/10.1002/adma.201400114	journal	March 2014
Electronic Structure and Properties of Organic Bulk-Heterojunction Interfaces Street, Robert A. Advanced Materials, Vol. 28, Issue 20 https://doi.org/10.1002/adma.201503162	journal	November 2015
Low-Temperature Behaviour of Charge Transfer Excitons in Narrow-Bandgap Polymer-Based Bulk Heterojunctions Jarzab, Dorota; Cordella, Fabrizio; Gao, Jio Advanced Energy Materials, Vol. 1, Issue 4 https://doi.org/10.1002/aenm.201100083	journal	May 2011
Beyond Langevin Recombination: How Equilibrium Between Free Carriers and Charge Transfer States Determines the Open-Circuit Voltage of Organic Solar Cells Burke, Timothy M.; Sweetnam, Sean; Vandewal, Koen Advanced Energy Materials, Vol. 5, Issue 11 https://doi.org/10.1002/aenm.201500123	journal	April 2015
Understanding Open-Circuit Voltage Loss through the Density of States in Organic Bulk Heterojunction Solar Cells Collins, Samuel D.; Proctor, Christopher M.; Ran, Niva A. Advanced Energy Materials, Vol. 6, Issue 4 https://doi.org/10.1002/aenm.201501721	journal	November 2015
Photogenerated Carrier Mobility Significantly Exceeds Injected Carrier Mobility in Organic Solar Cells Melianas, Armantas; Pranculis, Vytenis; Xia, Yuxin Advanced Energy Materials, Vol. 7, Issue 9 https://doi.org/10.1002/aenm.201602143	journal	January 2017
Charge Carrier Extraction in Organic Solar Cells Governed by Steady-State Mobilities Le Corre, Vincent M.; Chatri, Azadeh Rahimi; Doumon, Nutifafa Y. Advanced Energy Materials, Vol. 7, Issue 22 https://doi.org/10.1002/aenm.201701138	journal	September 2017
Verification of a generalized Planck law for luminescence radiation from silicon solar cells Schick, K.; Daub, E.; Finkbeiner, S. Applied Physics A Solids and Surfaces, Vol. 54, Issue 2 https://doi.org/10.1007/BF00323895	journal	February 1992
Thermalization and recombination in amorphous semiconductors Orenstein, J.; Kastner, M. A. Solid State Communications, Vol. 40, Issue 1 https://doi.org/10.1016/0038-1098(81)90717-1	journal	October 1981
Entropy and Disorder Enable Charge Separation in Organic Solar Cells Hood, Samantha N.; Kassal, Ivan The Journal of Physical Chemistry Letters, Vol. 7, Issue 22 https://doi.org/10.1021/acs.jpclett.6b02178	journal	October 2016
Charge Photogeneration in Organic Solar Cells Clarke, Tracey M.; Durrant, James R. Chemical Reviews, Vol. 110, Issue 11, p. 6736-6767 https://doi.org/10.1021/cr900271s	journal	November 2010
On the Dissociation Efficiency of Charge Transfer Excitons and Frenkel Excitons in Organic Solar Cells: A Luminescence Quenching Study Tvingstedt, Kristofer; Vandewal, Koen; Zhang, Fengling The Journal of Physical Chemistry C, Vol. 114, Issue 49 https://doi.org/10.1021/jp107587h	journal	November 2010
Electroluminescence of the Dye-Sensitized Solar Cell Trupke, T.; Würfel, P.; Uhlendorf, I. The Journal of Physical Chemistry B, Vol. 103, Issue 11 https://doi.org/10.1021/jp982555a	journal	March 1999
Delocalization and dielectric screening of charge transfer states in organic photovoltaic cells Bernardo, B.; Cheyns, D.; Verreet, B. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4245	journal	February 2014
Photo-generated carriers lose energy during extraction from polymer-fullerene solar cells Melianas, Armantas; Etzold, Fabian; Savenije, Tom J. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9778	journal	November 2015
On the origin of the open-circuit voltage of polymer–fullerene solar cells Vandewal, Koen; Tvingstedt, Kristofer; Gadisa, Abay Nature Materials, Vol. 8, Issue 11, p. 904-909 https://doi.org/10.1038/nmat2548	journal	October 2009
Hot charge-transfer excitons set the time limit for charge separation at donor/acceptor interfaces in organic photovoltaics Jailaubekov, Askat E.; Willard, Adam P.; Tritsch, John R. Nature Materials, Vol. 12, Issue 1 https://doi.org/10.1038/nmat3500	journal	December 2012
Nanoscale transport of charge-transfer states in organic donor–acceptor blends Deotare, P. B.; Chang, W.; Hontz, E. Nature Materials, Vol. 14, Issue 11 https://doi.org/10.1038/nmat4424	journal	September 2015
Light intensity dependence of open-circuit voltage of polymer:fullerene solar cells Koster, L. J. A.; Mihailetchi, V. D.; Ramaker, R. Applied Physics Letters, Vol. 86, Issue 12 https://doi.org/10.1063/1.1889240	journal	March 2005
Open-circuit voltage limit caused by recombination through tail states in bulk heterojunction polymer-fullerene solar cells Garcia-Belmonte, Germà; Bisquert, Juan Applied Physics Letters, Vol. 96, Issue 11 https://doi.org/10.1063/1.3358121	journal	March 2010
Theory to carrier recombination in organic disordered semiconductors Hofacker, A.; Oelerich, J. O.; Nenashev, A. V. Journal of Applied Physics, Vol. 115, Issue 22 https://doi.org/10.1063/1.4883318	journal	June 2014
Quasi-Fermi level splitting and sub-bandgap absorptivity from semiconductor photoluminescence Katahara, John K.; Hillhouse, Hugh W. Journal of Applied Physics, Vol. 116, Issue 17 https://doi.org/10.1063/1.4898346	journal	November 2014
The chemical potential of radiation Wurfel, P. Journal of Physics C: Solid State Physics, Vol. 15, Issue 18 https://doi.org/10.1088/0022-3719/15/18/012	journal	June 1982
Verification of a generalised Planck law by investigation of the emission from GaAs luminescent diodes Feuerbacher, B.; Wurfel, P. Journal of Physics: Condensed Matter, Vol. 2, Issue 16 https://doi.org/10.1088/0953-8984/2/16/010	journal	April 1990
Reciprocity between Charge Injection and Extraction and Its Influence on the Interpretation of Electroluminescence Spectra in Organic Solar Cells Kirchartz, Thomas; Nelson, Jenny; Rau, Uwe Physical Review Applied, Vol. 5, Issue 5 https://doi.org/10.1103/PhysRevApplied.5.054003	journal	May 2016
Diffusion-limited recombination in polymer-fullerene blends and its influence on photocurrent collection Nelson, Jenny Physical Review B, Vol. 67, Issue 15 https://doi.org/10.1103/PhysRevB.67.155209	journal	April 2003
Device model for the operation of polymer/fullerene bulk heterojunction solar cells Koster, L. J. A.; Smits, E. C. P.; Mihailetchi, V. D. Physical Review B, Vol. 72, Issue 8 https://doi.org/10.1103/PhysRevB.72.085205	journal	August 2005
Reciprocity relation between photovoltaic quantum efficiency and electroluminescent emission of solar cells Rau, Uwe Physical Review B, Vol. 76, Issue 8 https://doi.org/10.1103/PhysRevB.76.085303	journal	August 2007
Bimolecular recombination losses in polythiophene: Fullerene solar cells Shuttle, C. G.; O’Regan, B.; Ballantyne, A. M. Physical Review B, Vol. 78, Issue 11 https://doi.org/10.1103/PhysRevB.78.113201	journal	September 2008
Relating the open-circuit voltage to interface molecular properties of donor:acceptor bulk heterojunction solar cells Vandewal, Koen; Tvingstedt, Kristofer; Gadisa, Abay Physical Review B, Vol. 81, Issue 12 https://doi.org/10.1103/PhysRevB.81.125204	journal	March 2010
Ideal diode equation for organic heterojunctions. I. Derivation and application Giebink, N. C.; Wiederrecht, G. P.; Wasielewski, M. R. Physical Review B, Vol. 82, Issue 15 https://doi.org/10.1103/PhysRevB.82.155305	journal	October 2010
Localized state distribution and its effect on recombination in organic solar cells Street, R. A. Physical Review B, Vol. 84, Issue 7 https://doi.org/10.1103/PhysRevB.84.075208	journal	August 2011
Relationship between energetic disorder and open-circuit voltage in bulk heterojunction organic solar cells Blakesley, James C.; Neher, Dieter Physical Review B, Vol. 84, Issue 7 https://doi.org/10.1103/PhysRevB.84.075210	journal	August 2011
Influence of energetic disorder on electroluminescence emission in polymer:fullerene solar cells Gong, Wei; Faist, Mark A.; Ekins-Daukes, Nicholas John Physical Review B, Vol. 86, Issue 2 https://doi.org/10.1103/PhysRevB.86.024201	journal	July 2012
Dispersive and steady-state recombination in organic disordered semiconductors Hofacker, Andreas; Neher, Dieter Physical Review B, Vol. 96, Issue 24 https://doi.org/10.1103/PhysRevB.96.245204	journal	December 2017
Direct Observation of Entropy-Driven Electron-Hole Pair Separation at an Organic Semiconductor Interface Monahan, Nicholas R.; Williams, Kristopher W.; Kumar, Bharat Physical Review Letters, Vol. 114, Issue 24 https://doi.org/10.1103/PhysRevLett.114.247003	journal	June 2015
Charge-Transfer States and Upper Limit of the Open-Circuit Voltage in Polymer:Fullerene Organic Solar Cells Vandewal, Koen; Tvingstedt, Kristofer; Manca, Jean V. IEEE Journal of Selected Topics in Quantum Electronics, Vol. 16, Issue 6 https://doi.org/10.1109/JSTQE.2010.2043061	journal	November 2010
Ultrafast Long-Range Charge Separation in Organic Semiconductor Photovoltaic Diodes Gelinas, S.; Rao, A.; Kumar, A. Science, Vol. 343, Issue 6170 https://doi.org/10.1126/science.1246249	journal	December 2013

Cited By (1)

Reply to: Triplet-triplet annihilation in rubrene/C60 OLEDs with electroluminescence turn-on breaking the thermodynamic limit Engmann, Sebastian; Barito, Adam J.; Bittle, Emily G. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12598-4	journal	October 2019

Similar Records

Exploring the impact of the local environment on charge transfer states at molecular donor-acceptor heterojunctions

Technical Report · Mon Mar 04 23:00:00 EST 2024 · OSTI ID:2318724

Donor/Acceptor Charge-Transfer States at Two-Dimensional Metal Halide Perovskite and Organic Semiconductor Interfaces

Journal Article · Wed Oct 10 20:00:00 EDT 2018 · ACS Energy Letters · OSTI ID:1595404

Multiple Charge Transfer States in Donor–Acceptor Heterojunctions with Large Frontier Orbital Energy Offsets

Journal Article · Mon Jun 17 20:00:00 EDT 2019 · Chemistry of Materials · OSTI ID:1595398

Related Subjects

14 SOLAR ENERGY
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Organic semiconductors
nonequilibrium
photovoltaics

Nonthermal Site Occupation at the Donor-Acceptor Interface of Organic Solar Cells

Citation Formats

References (42)

Cited By (1)

Similar Records

Related Subjects