Center for Interface Science: Solar Electric Materials
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1 Center for Interface Science: Solar Electric Materials The Interface Science of Emerging Thin Film Solar Energy Conversion Technologies: Learning to Understand, Deal With and (Occasionally) Love Recombination and All That It Implies Scialog 2012 Biosphere II Neal Armstrong Center for Interface Science: Solar Electric Materials Research supported as part of the Center for Interface Science: Solar Electric Materials (CISSEM), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE SC
2 Generation III PVs What are they? Where are they headed? Solarinterface.org 2
3 New Thin Film PV Technologies e.g. Solarmer, Polyera, Heliatek.. Nearly 7% module efficiency
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5 Roll to roll vacuum processing?? Solarinterface.org
6 Where are solar cell efficiencies going? Solarinterface.org December 2011 Heliatek 6
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8 DOE SunShot Forum, June 2012 Can we make PV competitive without subsidy?
9 The motivation for interface science active layer contact nano laminate barrier layers contact light management top contact Interlayer ca nm) charge selective interlayer active layer Ratcliff, Zacher et al. JPC Letters Perspective 2011 Images: Kai Lin Ou, Xerxes Steirer, Delvin Tadytin charge selective interlayer bottom contact contact Interlayer nano laminate barrier layers/substrate 9
10 Solarinterface.org The motivation for interface science Layer by layer assembly Semiconductor Nanocrystal Active Layers NC polymer hybrids Ratcliff, Zacher et al. JPC Letters Perspective
11 What makes a good contact? Transparency, conductivity, low cost, earth abundant, scalable Other issues: Heterogeneity in electrical properties Interfacial compatibility with organic or inorganic active layers Selective interlayer ITO
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13 CISSEM Identity Principal Investigators David Ginger David Ginley Associate Director Dana Olson Joseph Berry Antoine Kahn Neal Armstrong Director Jeanne Pemberton Associate Director S. Scott Saavedra Associate Director Dominic McGrath Oliver Monti Seth Marder Associate Director Bernard Kippelen Associate Director Jean Luc Brédas Samuel Graham, Jr. Chemistry, Electrical & Mechanical Engineering, Materials Science, Optical Sciences, Physics 13
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15 (A) (B) FF = V OC J ph (C) J RS A Jo n RP A + V - J SC P MAX P TH (D) V JR S V JRS J Jo exp 1 J nkt o B e RP ph (E) V OC n ok BT J ph ln 1 e J o (F) J SC P * V OC SOLAR * FF
16 Component Materials and Interfaces in OPVs and Thin Film PVs Contacts (oxides and metals) Charge selective interlayers (both oxide and molecular materials) Substrates and barrier layers (often materials which are complementary to the contacts and interlayers) 16
17 Component Materials and Interfaces in OPVs and Thin Film PVs Contacts (oxides and metals) Charge selective interlayers (both oxide and molecular materials) Substrates and barrier layers (often materials which are complementary to the contacts and interlayers) Facile and selective charge harvesting 17
18 Contacts (oxides and metals) Solarinterface.org Component Materials and Interfaces in OPVs and Thin Film PVs Charge selective interlayers (both oxide and molecular materials) Substrates and barrier layers (often materials which are complementary to the contacts and interlayers) Oxide and metal contacts, and oxide interlayers 18
19 Contacts (oxides and metals) Solarinterface.org Component Materials and Interfaces in OPVs and Thin Film PVs Charge selective interlayers (both oxide and molecular materials) Substrates and barrier layers (often materials which are complementary to the contacts and interlayers) Dipolar and redox active interface modifiers 19
20 Contacts (oxides and metals) Solarinterface.org Component Materials and Interfaces in OPVs and Thin Film PVs Charge selective interlayers (both oxide and molecular materials) Substrates and barrier layers (often materials which are complementary to the contacts and interlayers) Unique approaches to interface characterization 20
21 The Tools of CISSEM Waveguide Spectroscopy Transient Waveguide Absorbance Spectroscopy Saavedra Laboratory, University of Arizona Potential modulated ATR Waveguide Spectroscopy W.M. Keck Center, University of Arizona Saavedra Laboratory, University of Arizona New tools have been developed in CISSEM to characterize electron transfer at interfaces on multiple time and length scales in solution (and are being developed for condensed phase environments). 21
22 The Tools of CISSEM trefm trefm Ginger Laboratory, University of Washington New implementations of Atomic Force Microscopy (AFM) to characterize heterogeneous, nano scale electrical properties at interfaces: Time Resolved Electrostatic Force Microscopy (trefm). Non contact trefm can recover sub microsecond transients to characterize formation and migration of photo generated charges. 22
23 The Tools of CISSEM IPES and TPPE fs Angle Resolved Two Photon Photoemission (TPPE) Spectroscopy Monti Laboratory, University of Arizona CISSEM uniquely combines ultrasensitive, high resolution photoemission and inverse photoemission spectroscopies to map electronic structure of excited state levels of interfacial regions of contact and interlayer materials. IPES Kahn Laboratory, Princeton University TPPE spectroscopy characterizes electronic structure of excited state levels of interfaces, and with fsec time resolution, can provide direct insight into electron transfer at interfaces. 23
24 The Tools of CISSEM UHV Surface Raman Surface Raman Spectroscopy Pemberton Laboratory, University of Arizona CISSEM uses unique combinations of ultra sensitive optical and x ray surface spectroscopies to probe molecular composition and orientation at oxide/organic and metal/organic interfaces: vibrational spectroscopies, NEXAFS, and X ray reflectivity 24
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26 REALLY BAD SOLAR CELLS!! Albery, Archer Nature 1977 Albery, Accounts of Chemical Research 1982 Solarinterface.org
27 Example redox couples: Ru(bipy) 3 +2 and Fe +2 /Fe +3 IF all electrochemical processes completely optimized: η 18%
28 Albery, Albery, Archer Archer Nature Nature Albery, Albery, Accounts Accounts of of Chemical Chemical Research Research Need for kinetically selective contacts!
29 Real compositional and energetic asymmetry Grätzel, M., Recent Advances in Sensitized Mesoscopic Solar Cells. Accounts of Chemical Research 2009, 42 (11), see also Science Nov. 2011
30 Type II Organic Heterojunction Devices Solarinterface.org load e VAC = 0 TCO E LUMO D Metal J SC = f(e LUMOD E LUMO A 3.0 E F,TCO Donor h + E HOMO D E A LUMO e Acceptor E F,M V OC = f(v bi ) E HOMOD E LUMO A Energy (ev) E HOMO A Tang, et al. Appl. Phys. Lett 1986, 1987 Two layer OLED and OPVs
31 Factors controlling OPV efficiency
32 Interlayer films are needed to provide both kinetic and thermodynamic selectivity for charge harvesting Solarinterface.org 32
33
34 E vs. (NHE) (volts) ( ) (+) e vac hole selective interlayer + Energy (ev) Transparent contact Top contact IP EA electron selective interlayer Active layer(s) X E F,e E F,h + X
35 Energetics (E CB, E VB of organic & oxide interlayers Active layer materials Electron selective interlayers Hole selecitve interlayers Dopants and high Φ interlayers Tunable interlayers Brabec et al. J. Mater. Chem 2010 Erin Ratcliff, Brian Zacher J. Phys. Chem. Lett. Perspective (2011) Notable absences: interface dipole effects!! 35
36 Energy LUMO A HOMO D 1 e + C 60 C e Photocurrent (extraction) limited by Surface Recombination a comparable event occurs for hole extraction at the opposite electrode J sr qs n S p S p ( p s N VB e q( E k T B E T n VB s ) p s n ) S n 2 i ( n s N CB e q( E k CB B E T T ) )
37 0, 10% O 2 sp ZnO interlayers in BHJ devices (TFD ITO/sp ZnO/BHJ/MoOx/Ag) Solarinterface.org Current density (ma/cm 2 ) % O 2 Dark 10% O 2 Light 0% O 2 Dark 0% O 2 Light Current density (ma/cm 2 ) % O 2 Dark 10% O 2 Light 0% O 2 Dark 0% O 2 Light Voltage (V) Voltage (V) 0.8 ETL V OC (V) Jsc (ma/cm 2 ) F.F. PCE (%) 0% O 2 ZnO 0.51± ± ± ±0.2 10% O 2 ZnO 0.49± ± ± ±0.1
38 These same issues are relevant in describing the photoelectrochemical conversion of sunlight to fuels, using planar or nanowire array electrodes
39 Intrinsic defects in Würtzite ZnO Zinc vacancy 10% Oxygen interstitial Oxygen vacancy 12% 23% partially filled band gap states due to broken bonds of O atoms acceptor (V 0 Zn, V 1 Zn,V 2 Zn) O O i bond (O i split) O i 2 (octahedral) acceptor most probable donor for n ZnO Ideal würtzite ZnO O Oxygen antisite Zn O in the position of Zn O O Zn bond Zinc interstitial donor very unstable Zinc antisite Zn in the position of O Zn O O distances 8% loner vs. quilibrium bonds A. Janotti, C.G. Van de Walle, PHYSICAL REVIEW B 76,
40 (a) (b) primary e - secondary e - e - e - e - e - eēprimary e - secondary e - e - e - incident radiation Determination of: Ionization potentials (IP), E VB Local shifts in vacuum level (interface dipoles) Au Au with C16 thiol source energy, 21.2 ev De Frontier orbital energy offsets Organic/organic heterojunctions: Macromol. Rapid Commun. 2009, 30, Appl. Phys. A., 95, (2009) Intensity Au spectrum width (w) E F E vac Self assembled monolayers: Journal of Physical Chemistry C, 113, (2009 Tethered monolayers of SC NCs ACS Applied Materials and Interfaces, 2, , (2010) Kinetic Energy (ev)
41 New Capabilities Layer by Layer OPV and interlayer formation (vacuum deposited small molecules) Solarinterface.org UPS/XPS ++ layer by layer deposition (vacuum and glove box) of organic semiconductors, semiconductor nanocrystals, interlayers, etc.
42 Inverse photoemission spectroscopy (IPES)
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44 e selective oxide interlayers: sol gel (printed) versus CVD or ALD (nanometer control of thickness and electrical properties Kai Lin Ou/Delvin Tadytin/Xerxes Steirer ACS Applied Materials & Interfaces
45 Energetics (E CB, E VB of organic & oxide interlayers Active layer materials Electron selective interlayers Hole selecitve interlayers Dopants and high Φ interlayers Tunable interlayers Brabec et al. J. Mater. Chem 2010 Erin Ratcliff, Brian Zacher J. Phys. Chem. Lett. Perspective (2011) Notable absences: interface dipole effects!! 45
46 New forms of solution processed NiOx interlayers: K. Xerxes Steirer, Paul Ndione, N. Edwin Widjonarko, Matthew T. Lloyd, Jens Meyer, Erin L. Ratcliff, Antoine Kahn, Neal R. Armstrong, Calvin J. Curtis, David S. Ginley, Joseph J. Berry, and Dana C. Olson
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49 K. Xerxes Steirer, et al., Advanced Energy Materials (2011) Performance, scalability and lifetimes are enhanced!
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51 Brian Zacher et al. JPC C 2011
52 Trajectories of some of the charges emanating from the D/A interface: successful transits from one D/A site d Fast pathways
53 Conducting tip AFM: Mapping of electrical properties for contacts and interlayers 10 V Amplifier Current (na) CuPc Bias (V) ITO/glass MacDonald, Veneman, et al. in preparation
54 Conducting tip AFM: Mapping of electrical properties for contacts and interlayers Current (na) Gold OP-ITO HCL+FeCl3 ODPA-ITO Less ohmic Bias (V) Increasing φ Current through CuPc thin films dominated by V 2 dependence if contact is Ohmic (Mott Guerny) MacDonald, Veneman, ACS Nano this week!
55 Gold a) 10 b) Current Density (ma cm -2 ) C6 C8 C14 C18 DSC Bias (V) nm Current Density (ma cm -2 ) O 2 Plasma Cleaned ITO Detergent Solvent Cleaned ITO Bias (V)
56
57 Generation III PVs What are they? Where are they headed? Solarinterface.org 57
58 CISSEM Interface to Face Research Conference, Energy Science Group
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