Exciton Fission & Solar energy conversion beyond the limit. Xiaoyang Zhu, Columbia University 1
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1 Exciton Fission & Solar energy conversion beyond the limit 1
2 Acknowledgement Dr. Wai-lun Chan (U. Kansas) Dr. John Tritsch (Intel) Dr. M. Tuan Trinh Mr. Tim Berkelbach, Dr. Mark Hybertsen, Prof. David Reichman, Prof. Jiali Gao, Dr. M. Sfeir, Dr. M. Steigerwald, Prof. Colin Nuckolls Drs. Manuel Ligges, Askat Jailaubekov, Loren Kaake, Luis Miaja-Avila, Mr. Nick Monahan, Mr. Kris Williams, Dr. Felix Leyssner, Dr. Manuel Marks, Dr. Martin Gustaffson, Ms. Xiaoxi Wu, Mr. Cory Nelson, Mr. Tim Attalah NSF-DMR ( & ) DOE-EFRC Columbia (DE-SC ) 2
3 Exceeding the Shockley-Queisser Limit η 31% η 44 % η 66% h The SQ limit: Shockley & Queisser, JAP 1961 Multiple excitons Science 2011, 334, 1541 Nature Chem. 2012, 4, 840 JACS 2012, 134, Nature Com. 2013, 4, Hot carrier cell 3
4 Singlet fission & solar cell efficiency Large exchange energy à E T1 ½ E S1 Spin conserved S o + S 1 ME T 1 + T 1 Two chromophores? S 1 T 1 + hv 1 hv2 S o Chromophore 1 Chromophore 2 Hanna & Nozik, JAP (2006) 4
5 Seeing the multiexciton state in pentacene 2x E T1 - E S1 = 2x = ev 4.65 ev 2.15 ev Time-resolved two-photon photoemission Science 334, (2011). 5
6 Coherent population of the dark multiexciton state via electronic coupling to the singlet. It s forbidden to generate 2 e-h pairs from 1 photon. S 1? ME S 0 hv 2e - + Red curve: simulation from the Liouville von Neumann eqn. 6
7 Schrödinger's cat dies from thinking outside-of-the-box Pump-probe delay (ps) S1 ME Hot ME cools down by 0.11 ev, in agreement with theory. 2xT1 Nature Chem. 2 (2010) 649. JACS 133 (2011) [ S 1 ME] ME * T 1 + T 1 7
8 The lifespan of Schrödinger's cat depends on energetics Tetracene S ME 2T 1 1 Interaction with environment: the bath. Pentacene S 1 ME 2T 1 Science 334, 1541 (2011) Nature Chem. 4, 840 (2012) 8
9 Evidence for the quantum coherent mechanism in transient absorption: perfluoro-pentacene Kolata, K., Breuer, T., Witte, G., & Chatterjee, S. (2014). ACS Nano. DOI: /nn502544d 9
10 The critical role of inter-molecular charge transfer state in singlet fission FE CT ME Eric C. Greyson, Josh Vura-Weis, Josef Michl, Mark A. Ratner, J. Phys. Chem. B 114, 14168, 2010 Smith & Michl, Chem. Rev. 110, 6891 (2010) 10
11 Theoretical analysis suggests the critical role of inter-molecular charge transfer (CT) state in mediating efficient singlet fission S 1 -CT & CT-ME coupling strong: ~100 mev < Φ ( S ) ˆ uv 1 H Φuv( CT ) > 2 body integrals < Φ ( CT ) Hˆ Φ ( ME) > uv uv Direct S 1 -ME coupling is weak: 0 2 mev 3 body integrals < Φ ( S ) ˆ 1 H Φ ( ME) > uv uv FE CT ME i ˆρ t = Ĥ ME, ˆρ i ˆD Tetracene lattice Acct. Chem. Res. 46, (2013) 11
12 The dominance of CT character in S 1 J. Phys. Chem. Lett. 2013, 4, Phys. Rev. Lett. 110, (2013) S 1 S 1 ab ac T 1 T 1 ab ac 12
13 Where is the CT state in time-resolved twophoton photoemission (TR-2PPE) spectra? FE hν 2 Vac e ME e hν 1 CT e CT e Nature Chem. 6,492 (2014) SOI 13
14 CT state mediated S 1 -ME coupling FE+CT ME+CT S 1 CT ME S 0 [ FE + CT + ME] ME * T 1 + T 1 Nuclear localization 14
15 Charge transfer state in singlet fission FE CT ME 15
16 A designer polymer with 175% intra-molecular SF quantum yield A D A - + hv Erik Busby Jianlong Xia Luis Campos Matt Sfeir + - T 1 T 1 S 1 with CT character T 1 localized on A Tune D-A to control S 1 energy, with E T1 fixed Erik Busby, Jianlong Xia, Qin Wu, Jonathan Z. Low, Rui Song, John R. Miller, X-Y. Zhu, Luis M. Campos, Matthew Y. Sfeir, Xiaoyang Nature Zhu, Mater.. Columbia University 16
17 Evidence for efficient singlet fission Annihilation 70 ps. cf: Intrinsic T 1 lifetime 1 µs QY = 175% (n=1), 50-60% (n=2) QY = 20-30% (n=1), 30-70% (n=2) 17
18 Annihilation of the intra-molecular triplet pair Black: Single triplet from pulse radiolysis Fast 1 (TT)à S 2 à S 0 Slow T 1 à S 0 18
19 From intra to inter-molecular singlet fission: a new mechanism ME 2x T 1 M. T. Trinh, Y. Zhong, T. Schiros, Q. Chen, S. Jockusch, M.Y. Sfeir, M. Steigerwald, C. Nuckolls, and X-Y. Zhu, Under review 19
20 A class of modified oligoenes: DPDC n Chem. Sci. 2012, 3, 1007 Prof. Colin Nuckolls DPDC 7 has the smallest singlet triplet pair gap. 20
21 Transient absorption establishes multiexciton state in DPDC 7 solution DPDC 7 Transient absorption pump probe Evidences for SF in solid DPDC 7 film: Fast singlet decay Long lived bleaching Phosphorescence 21
22 Transient absorption establishes singlet fission in DPDC 7 films DPDC 7 Transient absorption pump probe Evidences for SF in solid DPDC 7 film: Long lived bleaching Phosphorescence 22
23 Delayed bleaching of ground state molecules reveals intra- to inter-molecular fission Pump-probe delay (ps) ME 2x T 1 23
24 Activated singlet fission t = 0 S 2 ME S 0 S 2 t > 0 ME 2x T 1 S 1 Picosecond acoustics S 0 S 0 24
25 Harvesting singlet fission for solar energy conversion: 1e, 2e or energy transfer Science 334, (2011) ; JACS 134, (2012); Nature Commun. 4, 2679 (2013) 25
26 Summary Singlet fission from coherent coupling between S 1 & ME. The critical role of CT states in efficient singlet fission. Intra- to inter-molecular fission in oligoenes (DPDCs) 1 vs. 2 electron transfer from the S 1 -ME state Triplet energy transfer & the need to minimize D 2 /D 1 area. Exceeding the SQ limit. June
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