Thermodynamic Limit for Excitonic Light-Emitting Diodes

Giebink, Noel C.; Forrest, Stephen R.

doi:10.1103/physrevlett.130.267002

Thermodynamic Limit for Excitonic Light-Emitting Diodes

Journal Article · Thu Jun 29 00:00:00 EDT 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.130.267002· OSTI ID:2418099

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Univ. of Michigan, Ann Arbor, MI (United States); Pennsylvania State Univ., University Park, PA (United States); OSTI
Univ. of Michigan, Ann Arbor, MI (United States)

Here, we derive the thermodynamic limit for organic light-emitting diodes (OLEDs), and show that strong exciton binding in these devices requires a higher voltage to achieve the same luminance as a comparable inorganic LED. The OLED overpotential, which does not reduce the power conversion efficiency, is minimized by having a small exciton binding energy, a long exciton lifetime, and a large Langevin coefficient for electron-hole recombination. Based on these results, it seems likely that the best phosphorescent and thermally activated delayed fluorescence OLEDs reported to date approach their thermodynamic limit. The framework developed here is broadly applicable to other excitonic materials, and should therefore help guide the development of low voltage LEDs for display and solid-state lighting applications.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0009694

OSTI ID:: 2418099

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 26 Vol. 130; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (42)

Extremely Low Operating Voltage Green Phosphorescent Organic Light-Emitting Devices Sasabe, Hisahiro; Nakanishi, Hiromi; Watanabe, Yuichiro Advanced Functional Materials, Vol. 23, Issue 44 https://doi.org/10.1002/adfm.201301069	journal	June 2013
Tuning Energy Levels of Electron‐Transport Materials by Nitrogen Orientation for Electrophosphorescent Devices with an ‘Ideal’ Operating Voltage Su, Shi‐Jian; Sasabe, Hisahiro; Pu, Yong‐Jin Advanced Materials, Vol. 22, Issue 30 https://doi.org/10.1002/adma.200904249	journal	August 2010
Factors Limiting Device Efficiency in Organic Photovoltaics Janssen, René A. J.; Nelson, Jenny Advanced Materials, Vol. 25, Issue 13 https://doi.org/10.1002/adma.201202873	journal	December 2012
Low-Driving-Voltage Blue Phosphorescent Organic Light-Emitting Devices with External Quantum Efficiency of 30% Udagawa, Kazuo; Sasabe, Hisahiro; Cai, Cao Advanced Materials, Vol. 26, Issue 29 https://doi.org/10.1002/adma.201401621	journal	June 2014
Ultrahigh Power Efficiency Thermally Activated Delayed Fluorescent OLEDs by the Strategic Use of Electron‐Transport Materials Sasabe, Hisahiro; Sato, Ryo; Suzuki, Katsuaki Advanced Optical Materials, Vol. 6, Issue 17 https://doi.org/10.1002/adom.201800376	journal	June 2018
Universal Electroluminescence at Voltages below the Energy Gap in Organic Light‐Emitting Diodes Li, Yungui; Sachnik, Oskar; van der Zee, Bas Advanced Optical Materials, Vol. 9, Issue 21 https://doi.org/10.1002/adom.202101149	journal	August 2021
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
Origin of Sub-Bandgap Electroluminescence in Organic Light-Emitting Diodes Xiang, Chaoyu; Peng, Cheng; Chen, Ying Small, Vol. 11, Issue 40 https://doi.org/10.1002/smll.201501355	journal	August 2015
Exciton binding energies in organic semiconductors Knupfer, M. Applied Physics A, Vol. 77, Issue 5 https://doi.org/10.1007/s00339-003-2182-9	journal	October 2003
On the relation between absorption and emission spectra of molecules in solution van Metter, R. L.; Knox, R. S. Chemical Physics, Vol. 12, Issue 3 https://doi.org/10.1016/0301-0104(76)87103-0	journal	February 1976
Device physics of organic light-emitting diodes based on molecular materials Brütting, Wolfgang; Berleb, Stefan; Mückl, Anton G. Organic Electronics, Vol. 2, Issue 1 https://doi.org/10.1016/S1566-1199(01)00009-X	journal	March 2001
Electron affinities of organic materials used for organic light-emitting diodes: A low-energy inverse photoemission study Yoshida, Hiroyuki; Yoshizaki, Kei Organic Electronics, Vol. 20 https://doi.org/10.1016/j.orgel.2015.01.037	journal	May 2015
Modeling of photoluminescence spectra and quasi-Fermi level splitting in μc-Si:H solar cells Pieters, B. E.; Kirchartz, T.; Merdzhanova, T. Solar Energy Materials and Solar Cells, Vol. 94, Issue 11 https://doi.org/10.1016/j.solmat.2010.06.005	journal	November 2010
Exciplex-Based Electroluminescence: Over 21% External Quantum Efficiency and Approaching 100 lm/W Power Efficiency Liang, Baoyan; Wang, Jiaxuan; Cheng, Zong The Journal of Physical Chemistry Letters, Vol. 10, Issue 11 https://doi.org/10.1021/acs.jpclett.9b01140	journal	May 2019
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
Excitons versus free charges in organo-lead tri-halide perovskites D’Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4586	journal	April 2014
Emissive and charge-generating donor–acceptor interfaces for organic optoelectronics with low voltage losses Ullbrich, Sascha; Benduhn, Johannes; Jia, Xiangkun Nature Materials, Vol. 18, Issue 5 https://doi.org/10.1038/s41563-019-0324-5	journal	April 2019
Triazine-phosphine oxide electron transporter for ultralow-voltage-driven sky blue PHOLEDs Jia, Jilin; Zhu, Liping; Wei, Ying Journal of Materials Chemistry C, Vol. 3, Issue 19 https://doi.org/10.1039/C4TC02993C	journal	January 2015
Highly efficient blue thermally activated delayed fluorescent OLEDs with record-low driving voltages utilizing high triplet energy hosts with small singlet–triplet splittings Zhang, Dongdong; Cai, Minghan; Bin, Zhengyang Chemical Science, Vol. 7, Issue 5 https://doi.org/10.1039/C5SC04755B	journal	January 2016
Temperature dependence of the radiative recombination coefficient of intrinsic crystalline silicon Trupke, T.; Green, M. A.; Würfel, P. Journal of Applied Physics, Vol. 94, Issue 8 https://doi.org/10.1063/1.1610231	journal	January 2003
Efficient, deep-blue organic electrophosphorescence by guest charge trapping Holmes, R. J.; D’Andrade, B. W.; Forrest, S. R. Applied Physics Letters, Vol. 83, Issue 18, p. 3818-3820 https://doi.org/10.1063/1.1624639	journal	November 2003
Very high-efficiency and low voltage phosphorescent organic light-emitting diodes based on a p-i-n junction He, Gufeng; Schneider, Oliver; Qin, Dashan Journal of Applied Physics, Vol. 95, Issue 10 https://doi.org/10.1063/1.1702143	journal	May 2004
Upconversion injection in rubrene/perylene-diimide-heterostructure electroluminescent diodes Pandey, Ajay K.; Nunzi, Jean-Michel Applied Physics Letters, Vol. 90, Issue 26 https://doi.org/10.1063/1.2752540	journal	June 2007
Intrinsic luminance loss in phosphorescent small-molecule organic light emitting devices due to bimolecular annihilation reactions Giebink, N. C.; D’Andrade, B. W.; Weaver, M. S. Journal of Applied Physics, Vol. 103, Issue 4 https://doi.org/10.1063/1.2884530	journal	February 2008
Accuracies of the empirical theories of the escape probability based on Eigen model and Braun model compared with the exact extension of Onsager theory Wojcik, Mariusz; Tachiya, M. The Journal of Chemical Physics, Vol. 130, Issue 10 https://doi.org/10.1063/1.3082005	journal	March 2009
Numerical simulations of the electrical characteristics and the efficiencies of single-layer organic light emitting diodes Malliaras, G. G.; Scott, J. C. Journal of Applied Physics, Vol. 85, Issue 10 https://doi.org/10.1063/1.369373	journal	May 1999
Electric field assisted dissociation of charge transfer states as a mechanism of photocarrier production Braun, Charles L. The Journal of Chemical Physics, Vol. 80, Issue 9 https://doi.org/10.1063/1.447243	journal	May 1984
Electroluminescent refrigeration by ultra-efficient GaAs light-emitting diodes Xiao, T. Patrick; Chen, Kaifeng; Santhanam, Parthiban Journal of Applied Physics, Vol. 123, Issue 17 https://doi.org/10.1063/1.5019764	journal	May 2018
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
Organic Electronics Forrest, Stephen R. Oxford University Press https://doi.org/10.1093/oso/9780198529729.001.0001	book	August 2020
On The Thermodynamics of Fluorescence Kennard, E. H. Physical Review, Vol. 11, Issue 1 https://doi.org/10.1103/PhysRev.11.29	journal	January 1918
Energy Loss in Organic Photovoltaics: Nonfullerene Versus Fullerene Acceptors Liu, Xiao; Li, Yongxi; Ding, Kan Physical Review Applied, Vol. 11, Issue 2 https://doi.org/10.1103/PhysRevApplied.11.024060	journal	February 2019
Nonequilibrium Steady-State Statistics and Associated Effects for Insulators and Semiconductors Containing an Arbitrary Distribution of Traps Simmons, J. G.; Taylor, G. W. Physical Review B, Vol. 4, Issue 2 https://doi.org/10.1103/PhysRevB.4.502	journal	July 1971
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
Effects of disorder on the current density and recombination profile in organic light-emitting diodes Coehoorn, R.; van Mensfoort, S. L. M. Physical Review B, Vol. 80, Issue 8 https://doi.org/10.1103/PhysRevB.80.085302	journal	August 2009
Electron-hole recombination in disordered organic semiconductors: Validity of the Langevin formula van der Holst, J. J. M.; van Oost, F. W. A.; Coehoorn, R. Physical Review B, Vol. 80, Issue 23 https://doi.org/10.1103/PhysRevB.80.235202	journal	December 2009
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
Trap-assisted and Langevin-type recombination in organic light-emitting diodes Wetzelaer, G. A. H.; Kuik, M.; Nicolai, H. T. Physical Review B, Vol. 83, Issue 16 https://doi.org/10.1103/PhysRevB.83.165204	journal	April 2011
Thermodynamic efficiency limit of excitonic solar cells Giebink, Noel C.; Wiederrecht, Gary P.; Wasielewski, Michael R. Physical Review B, Vol. 83, Issue 19 https://doi.org/10.1103/PhysRevB.83.195326	journal	May 2011
Effects of energy correlations and superexchange on charge transport and exciton formation in amorphous molecular semiconductors: An ab initio study Massé, Andrea; Friederich, Pascal; Symalla, Franz Physical Review B, Vol. 95, Issue 11 https://doi.org/10.1103/PhysRevB.95.115204	journal	March 2017
Photocurrent Generation in Polymer-Fullerene Bulk Heterojunctions Mihailetchi, V. D.; Koster, L. J. A.; Hummelen, J. C. Physical Review Letters, Vol. 93, Issue 21 https://doi.org/10.1103/PhysRevLett.93.216601	journal	November 2004
Thermally-activated Delayed Fluorescence for Light-emitting Devices Nakanotani, Hajime; Tsuchiya, Youichi; Adachi, Chihaya Chemistry Letters, Vol. 50, Issue 5 https://doi.org/10.1246/cl.200915	journal	May 2021

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