Plastic Solar Cells Lightweight, flexible and rugged!

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1 NSF ONR Workshop Alan Heeger University of California, Santa Barbara Santa Barbara, CA Plastic Solar Cells Lightweight, flexible and rugged!

2 Plastic Solar Cells The ultrafast electron transfer in polymer BHJ Materials and in small molecule BHJ Materiials is enabled by the Uncertainty Principle Excited state and charge transfer hν Interfacial traps and Interfacial excitons Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s Ground state Recombination --- Mostly bimolecular

3 The Initial Discovery (1992): Ultrafast Photo-induced electron transfer B. Kraabel, C.H. Lee, D. McBranch, D. Moses, N. S. Sariciftci and AJH Chem. Phys. Lett. 1993, 213, <100 fs * hn + e- * n Electron Acceptor LUMO LUMO HOMO HOMO 50 fs Electron Donor Brabec et al Chem Phys Lett 2001

4 Phase separation morphology is critical to OPV solar cell performance Need connected pathways Need relatively high mobility to get charges out prior to recombination Need self-assembly to form phase separated morphology at the nm length scale Ultrafast carrier generation does not suffer the recombination losses expected from regions of low phase purity (e.g.intermixed systems or intercalated systems). Why phase separation? Polymers always want to phase separate --- no entropy of mixing for high polymers Crystallinity: Strong driver of phase separation

5 Time Resolved Charge Transfer Photo-induced absorption measurements in the sub-ps to sub-ns time regime. Excited state and charge transfer hν 50fs Interfacial traps and Interfacial excitons Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s Ground state Recombination --- Mostly bimolecular But first, in order to understand the importance of the ultrafast electron transfer, we must understand the morphology.

6 P3HT:PCBM Cross-section TEM: Column-like Morphology slice with Focused Ion Beam Jisun Moon et al Nano-Letters 2009

7 S n O OMe P3HT:PCBM Cross-section TEM: Column-like Morphology Good morphology --- relatively direct pathways to the electrodes Nano-scale solar cells: ALL CONNECTED IN PARALLEL!

8 Spatial FT 2 1 L i xf x x PSD( f x) I( x) e dx L 0 x Autocorrelation function 2 ACR( x) 1 L x 0 L x I( x) I( x x ' ) dx Period nm (Ave. Domain size)

9 TEM Tomography 1:2 Polymer:PC 70 BM (η=6.0%) Polymer James Rogers Ed Kramer UCSB

10 Reality Concept New Material Organic Nano-photovoltaics

11 Time Resolved Charge Transfer Photo-induced absorption measurements in the sub-ps to sub-ns time regime. Excited state and charge transfer hν t < 50 fs Interfacial traps and Interfacial excitons Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s Ground state Recombination --- mostly bimolecular Photoinduced charge transfer over approx. 20 nm in 50 fs!

12 Current conventional wisdom describes the charge transfer process as occurring in four steps: Photo-generation of Frenkel excitons Exciton migration to a donor-acceptor interface Interfacial charge transfer into a bound state (charge transfer (CT) exciton) at the donor-acceptor interface Field induced dissociation of the CT exciton 50 fs much too fast for exciton diffusion to interface ---- of order ps would be required!

13 Absorbance A (au) A (au) Esign and synthesis by Bazan and Welch S S S N N N S Si S N p-dts(ptth 2 ) 2 N S N S S 5,5'-bis{(4-(7-hexylthiophen-2-yl)thiophen-2-yl)-[1,2,5]thiadiazolo [3,4-c]pyridine-3,3'-di-2-ethylhexylsilylene-2,2'-bithiophene O OMe S N N H 17 C 8 C 8 H 17 Design and synthesis Mario Leclerc U of Laval S S PCDTBT N n PC 70 BM Wudl poly[n-9 -heptadecanyl-2,7 carbazole-alt-5,5-(4,7 -di2-thienyl- 2,1,3 -benzothiadiazole [6,6]-phenyl C 70 -butyric acid methyl ester p-dts(ptth 2 ) 2 :PC 70 BM PCDTBT:PC 70 BM wavelength (nm) ps 23 ps 200 ps 1500 ps wavelength (nm) ps 20 ps 200 ps 1500 ps wavelength (nm)

14 Current density (ma/cm 2 ) IPCE (%) BHJ solar Cells fabricated from small Molecules Design and synthesis: G. Bazan and G. Welch Voltage (V) % 0.2% 0.6% 1.0% Wavelength (nm) Performance of solar cells with a DTS(PTTh 2 ) 2 :PC 70 BM active layer as a function of DIO content (as processing additive) Solution-Processed Small-Molecule Solar Cells with 7% Efficiency: Nat Mater 2012, 11, 44.

15 7:3 G24:PC G24:PC 70 BM (η=6.7%) 70 BM (η=6.7%) Note: Ratio only 70:30 30% Fullerene Top View 100 nm SideView James Rogers Ed Kramer

16 DTS(PTTh 2 ) 2 BHJ on MoOx (no DIO ) (163 nm per side) False Color Raw Image In-plane stacking of DTS(PTTh 2 ) 2 at 0.31 Å -1. (approx. 2 nm d-spacing) Regions of solid color indicate the spatial extent and direction of the crystal lattice fringes. (50 nm scale bar) TEM: Chris Takacs

17 Fabricated with 0.25% DIO additive (Optimum) Crystallinity remains very high; crystallite size decreases

18 A (au) CT (fs) absorbance (au) p-dts(ptth 2 ) 2 :PC 70 BM Ultrafast charge separation is enhanced by DIO additive Absorption spectrum d-dts(ptth 2 ) 2 PC 70 BM blend Photo-induced absorption Ground state bleaching plus polaron formation Loren Kaake wavelength (nm) ( a ) ( b ) DIO (% v/v) time (ps) DIO (% v/v) 0.6 J. Chem. Phys. Lett. 3, 1253 (2012)

19 Ultrafast Electron Transfer in Bulk Heterojunction Solar Cells: The Mechanism A (au) A (au) DTS(PTTh 2 ) 2 : PC 70 BM PCDTBT:PC 70 BM pump power ( J cm -2 ) Bimolecular recombination at high power densities pump power ( J cm -2 ) time (ps) time (ps) Ultrafast component is linear in the pump intensity. Ultrafast charge transfer is observed at all pump power levels.

20 A (au) A (au) t lower pump powers, when the excitation density is close to that of one sun, the carrier density decreases to the point where the bimolecular decay is no longer observable DTS(PTTh 2 ) 2 PC 70 BM pump power ( J cm -2 ) PCDTBT: PC 70 BM pump power ( J cm -2 ) time (ps) time (ps) Under these conditions, a slow increase emerges over much longer time scales!

21 The two very different characteristics of the charge transfer dynamics unambiguously imply two mechanisms: One consistent with ultrafast charge transfer via delocalized states, and A second, slower contribution from excitons diffusing to a donor-acceptor interface.

22 A (au) A (au) A (au) A (au) ( a ) ( J cm -2 ) time (ps) ( c ) PCDTBT:PC 70 BM ( d ) p-dts(ptth 2 ) 2 :PC 70 BM C 0.6 ( J cm -2 ) C ( b ) C time (ps) C No change in dynamics when pump power decreased by another factor of two where excitation densities are comparable to those generated under illumination by 1 sun time (ps) time (ps) The exciton diffusion contribution to the charge transfer contributes approx. 30% of the mobile charges. The Ultrafast contribution contributes approx. 70%.

23 The Charge Transfer Exciton E exciton hopping Donor E CT > 0 Acceptor ultrafast CT direct carrier production ( a ) Resonance state (degenerate with the continuum; comprised of mobile electrons in the acceptor domain and mobile holes in the donor domain) Donor x Acceptor ( b ) or ultrafast CT E exciton hopping direct carrier production E CT < 0 Charge transfer exciton (Bound State) x If the CT exciton is a bound state, it serves as the pathway for recombination (both radiant and non-radiant). If the conditions are such that the CT exciton is a bound state, it will serve as a principal route for bimolecular recombination.

24 Dynamics and Time Scales Excited state and charge transfer t < 50 fs t ~ ps Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s hν Interfacial traps and Interfacial excitons Ground state Recombination to ground state mostly bimolecular Bimolecular Recombination and radiative recombination if the CT exciton is a bound state

25 photoconductivity (ns) Carrier generation in pure p-dts(ptth 2 ) photoconductivity absorptance fluorescence (au) absorptance (%) Photoconductive response tracks the absorptance across the entire spectrum despite the fact that the initial absortion is that of an intra-molecular Frenkel exciton wavelength (nm) Selected Area Electron Diffraction from a 200 nm spot Polarization anisotropy measurements: Photo-generated carriers are produced immediately, delocalize and move along the - stacking direction) in p-dts(ptth 2 ) 2 2 nd order reflection 3.5Angstroms E E B S 1 one electron transfer to π band x

26 Ultrafast Electron Transfer in Bulk Heterojunction Solar Cells: The Mechanism One cannot know the location of the photoexcitation to an accuracy greater than about λ/4 > 30 nm. This coherent state (intramolecular excitations plus delocalized carriers) can yield ultrafast electron transfer to a nearby fullerene domain and, after decoherence, produce localized excitons that diffuse incoherently toward a donor/acceptor interface. The ultrafast electron transfer in polymer BHJ Materials and in small molecule BHJ Materiials is enabled by the Uncertainty Principle

27 Origin of V oc and the Built-in Potential *-band LUMO V oc -band HOMO V OC E fullerene (LUMO) E polymer (HOMO)+ k B /e{ln (n e n h /N c2 )} Conclusion: Need Deep HOMO for donor material.

28 COMPETITION between SWEEP OUT and RECOMBINATION Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s Interfacial traps and Interfacial excitons Ground state Recombination Time scale??? When sweep-out is faster than recombination --- high efficiency. Cowan, Street, Cho and AJH Phys. RevB 83, 35205

29 Transient photocurrent in operating solar cell: Competition between Sweep-out and Recombination J / V int (m -1 cm -2 ) PCDTBT OMe O PCDTBT:PC 70 BM T = 300K 0.7V 0.6V 0.5V 0.4V 0.2V 0.0V -0.5V -1.0V PC 70 BM Photoconductance = Current / Internal voltage 10-3 V int = V BI V Time ( s) When sweep-out is faster than recombination --- high efficiency.

30 Caution: Generation of impurity during synthesis Typically less than 1% impurity - Remove impurity via extraction with hexanes and column chromatography - Can avoid methyl transfer by lowering reaction temperature

31 Current density (ma/cm 2 ) Open circuit voltage (V) Earlier work on controlled introduction of impurities: PC 84 BM Traps in PCDTBT:PC 84 BM Introduce first-order (monomolecular) recombination and decrease V OC Reduce mobility Reduce j SC and prevent fast sweep out Result: All parameters adversely affected:v OC j SC FF a S S N N S C 8 H 17 C8 H 17 N n O OMe 2 0 a d m 84 :m 60 = 1:100 m 84 :m 60 = 1:1,000 m 84 :m 60 = 0: m 84 :m 60 = 0:1 m 84 :m 60 = 1:10,000 m 84 :m 60 = 1:1,000 m 84 :m 60 = 1:100 m 84 :m 60 = 1:0 (estimated) Voltage (V) PC 84 BM Concentration

32 Dennler, Scharber and Brabec, Adv. Mater 21, 1323, 2009

33 IPCE (%) What is needed to achieve the predicted high efficiencies? Bandgap 1000 nm High V oc Higher mobility and column-like morphology across the thickness of the film. Sweep-out prior to Recombination! G24 G24 with impurity Wavelength (nm)

34 Efficiency (%) Plastic Solar Cells Efficiency Time evolution of NREL NREL NREL efficiency of plastic NREL solar NREL cells United Solar United Solar OPV single junction 13% Mitsubishi Japan 8 Konarka Solarmer Konarka 9.2% SCUT China UCSB 1995 Cambridge U. Linz 2000 Konarka Konarka Siemens Siemens 2005 Year UCSB Plextronics

35 Plastic Solar Cells Low $ cost manufacturing Low energy cost manufacturing Low carbon footprint manufacturing Technology Energy for production (MJ.Wp -1 ) CO 2 footprint (gr.co 2 -eq.wp -1 ) Energy payback time (years) mc-si CdTe CIS Flex OPV A. L. Roes et al, Progress in Photovoltaics 17, 372 (2009)

36 QUESTIONS? AJH

37

38 anisotropy (r). Polarization Anisotropy Measurements ( a ) nm 395 nm ( b ) time (ps) 2.5 t Assuming carrier generation along the direction of - stacking, predictions for the anisotropy at vanishing timescales are: LUMO LUMO +1 λ calc = 620 nm λ calc = 400 nm HOMO 47 HOMO 90 Results: Consistent with band formation along the - stacking direction

39 A (au) A (au) A (au) A (au) ( a ) p-dts(ptth 2 ) 2 :PC 70 BM ( b ) ( J cm -2 ) C 0.5 C time (ps) ( c ) PCDTBT:PC 70 BM ( d ) time (ps) ( J cm -2 ) C 0.5 C time (ps) time (ps) No change in dynamics when pump power decreased by another factor of two.

40 Dynamics and Time Scales Excited state and charge transfer t < 50 fs t ~ ps Mobile carrier sweep out by the internal voltage (built-in electric field) Energy out ns - s hν Interfacial traps and Interfacial excitons Ground state Recombination to ground state mostly bimolecular Geminate Recombination if the CT exciton is a bound state Exciton diffusion to interface does contribute to the charge transfer, but relatively small amount. If the CT exciton is truly a bound state, then major source of bimolecular recombination.

41 The Idea ---- Typical length scale: ~20 nm Localization length in disordered semiconducting polymers ħ R O O R R O O R R O O R e - R O O R Self-Assembly of Bulk Heterojunction nano-material by Spontaneous Phase Separation Minimum LUMO-LUMO offset ~ 0.1 ev Gong, X. et al. Adv. Mater. 23, (2011).

42 Efficiency (%) Plastic Solar Cells Efficiency Time evolution of NREL NREL NREL efficiency of plastic NREL solar NREL cells United Solar United Solar OPV single junction 13% Mitsubishi Japan 8 Konarka Solarmer Konarka 9.2% SCUT China UCSB 1995 Cambridge U. Linz 2000 Konarka Konarka Siemens Siemens 2005 Year UCSB Plextronics

43 Plastic Solar Cells Low $ cost manufacturing Low energy cost manufacturing Low carbon footprint manufacturing Technology Energy for production (MJ.Wp -1 ) CO 2 footprint (gr.co 2 -eq.wp -1 ) Energy payback time (years) mc-si CdTe CIS Flex OPV A. L. Roes et al, Progress in Photovoltaics 17, 372 (2009)

44 Lightweight, flexible and rugged!

45 Semi-transparent Plastic OPV: Light for greenhouse plants and Power the fans, Pump the water

46 Roof of Bus Shelter San Francisco, USA Konarka EU PVSEC September 9 th 2010

47 TEM Phase Contrast Imaging Useful method for exploring morphology in low contrast materials

48 Cross-section --- Spontaneous Phase Separation (a) (a) Al (b) P3HT PEDOT:PSS TiO x PCBM PEDOT:PSS P3HT:PCBM conventional BHJ PEDOT:PSS P3HT:PCBM layer-evolved BHJ PEDOT:PSS TiO x TiO x Focused SiO 2 (c) (d) Defocused 10 m Defocused 30 m

49 DTS(PTTh 2 ) 2 BHJ on MoOx (no DIO ) (163 nm per side) False Color Raw Image (50 nm scale bar) In-plane stacking of DTS(PTTh 2 ) 2 at 0.31 Å -1. (approx. 2 nm d-spacing) Regions of solid color indicate the spatial extent and direction of the crystal lattice fringes. TEM: Chris Takacs

50 Intensity dependent dynamics At short circuit: Sweep out of photogenerated carriers by internal field (V bi ) At open circuit: Recombination only LUMO n oc /n sc ~ Efficient collection of photo-generated carriers HOMO Band-to-band bimolecular recombination R np Bimolecular n = p ~ I 1/2 and np ~ I

51 Intensity dependence of V OC probes bimolecular recombination V oc 1 e Fullerene Polymer B e h E ln LUMO EHOMO e Nc 2 where Nc= density of states in the band tails k T n n slope = 1 Universal dependence Seven different Semiconducting polymers V oc s kt e ln I Bimolecular --- s = 1 (np ~ I) Monomolecular --- s=2 (np ~ I 2 )

52 V oc (V) Temperature / intensity dependence probes the HOMO- LUMO difference 1 Fullerene Polymer kbt n enh V ln oc ELUMO EHOMO 2 e e Nc V oc reduced by ~ 0.3 V (k B T/e)ln(I) Fermi statistics: T-dependence of E F Universal dependence Five different Semiconducting polymers E HOMO E LUMO Temperature (K)

53 PEDOT:PSS PCDTBT Introduce PC 84 BM Traps a. 3.6 ev 4.3 ev 4.3 ev b. 4.8 ev ITO 5.0 ev 5.5 ev 4.65 ev 4.3 ev Al 6.1 ev PC 84 BM PC 84 BM PC 60 BM 8.1 ev TiO x PC 60 BM Semiconducting polymer RECOMBINATION VIA INTENTIONALLY INTRODUCED TRAPS

54 Trap-assisted recombination Recombination via the trap state E LUMO V oc s kt e ln I polymer fullerene HOMO First-order (monomolecular) s = 2

55 Current density (ma/cm 2 ) Traps: Introduce first-order (monomolecular) recombination and decrease V OC Open circuit voltage (V) Reduce mobility Reduce j SC and prevent fast sweep out Result: All parameters adversely affected: V OC j SC FF 2 0 a. 0.9 d m 84 :m 60 = 1:100 m 84 :m 60 = 1:1,000 m 84 :m 60 = 0: m 84 :m 60 = 0:1 m 84 :m 60 = 1:10,000 m 84 :m 60 = 1:1,000 m 84 :m 60 = 1:100 m 84 :m 60 = 1:0 (estimated) Voltage (V) PC 84 BM Concentration

56 Mobile carriers are swept out by the internal field V int = V bi -V v drift E int V int /d sw = d 2 /2 V int sw 10-7 s with 10-3 cm 2 /Vs

57 Transient photocurrent in operating solar cell: Competition between Sweep-out and Recombination J / V int (m -1 cm -2 ) PCDTBT OMe O PCDTBT:PC 70 BM T = 300K 0.7V 0.6V 0.5V 0.4V 0.2V 0.0V -0.5V -1.0V PC 70 BM Photoconductance = Current / Internal voltage 10-3 V int = V BI V Time ( s) When sweep-out is faster than recombination --- high efficiency.

58 Photoconductance (mω -1 cm -2 ) J / V int (m -1 cm -2 ) J / V int (m -1 cm -2 ) Internal field is well-defined even in the complex BHJ material Photocurrent normalization by V int = V BI V Charge transport via drift V 0.6V 0.5V 0.4V 0.2V 0.0V -0.5V -1.0V Time ( s) PCDTBT:PC 70 BM 10-2

59 A(t=2 ms) A(t=2 ms) ( a ) p-dts(ptth 2 ) ps 2 ms A(t=2 ps) Comparing lineshapes from 2 ps and 2 ms. (a) Transient absorption spectra of a p-dts(ptth 2 ) 2 :PC 70 BM film. (b) Transient absorption spectra of a PCDTBT:PC 70 BM film Left axis belongs to 2 ms measurements, (blue squares). Right axis belongs to 2 ps measurements, (red line). wavelength (nm) ( b ) 4 PCDTBT ps 2 ms 0-20 A(t=2 ps) Polaron lifetime can be very long when there are no electrodes and no sweep-out wavelength (nm) 1000

60 0% DIO (a) 0.5 % DIO Selected area electron diffraction from a 200 nm area of neat (b) p-dts(ptth 2 ) 2. 1 st and 2 nd order scattering π- π peaks are Visible. - Stacking (d = 3.48 A ) with good inter-molecular overlap. Formation of - and *- bands. Transport dominated by these - bands. Excellent photoconductor. o

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