Michael Heiber and Carsten Deibel Optik und Photonik kondensierter Materie Institut für Physik Technische Universität Chemnitz Charge transport in organic (polymer based) devices
created at donor- acceptor interface in the film • Slow extraction ∝ low mobility leads to greater recombination losses • How does the nanoscale morphology affect the charge carrier mobility? → Kinetic Monte Carlo simulation Fullerene Aluminium Cathode Transparent Anode Polymer
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created at donor- acceptor interface in the film • Slow extraction leads to greater recombination losses • How does the nanoscale morphology affect the charge extraction time? → Kinetic Monte Carlo simulation Fullerene Aluminium Cathode Transparent Anode Polymer
• geometric method (μgeo) overestimates the mobility = expectation value μm of the mobility distribution • deviation more prominent at low electric fields and low temp J. Lorrmann et al. J. Appl. Phys. 115, 183702 (2014) ln f ð Þ Scheme J. Appl. Phys. 115, 183702 (2014) 183702-6 Lorrmann et al. FIG. 2. Upper part: Mobility distributions p l (l) for three different tempera- tures T ¼ 130, 190, 300 K (from left to right) at a fixed electric field of. F ¼ 1:2 Â 108 V m . The vertical straight lines illustrate the four different defi- nitions of mobility ltr,m (dashed-double-dotted), lm (dashed), lgeo (solid), 183702-6 Lorrmann et al. 300 K 190 K 130 K
Electric field dependence predicted to change in a blend • Negative field dependence is often not observed experimentally • What role does morphology play? also c.f. simulations by Koster, Phys. Rev. B. 81, 205318 (2010) and Frost et al, Nano Letters 6, 1674- (2006). conjugated polymers, which show highly dispersive current transients, that mobility is not a well-defined material param- eter as for materials with a well-defined carrier transit time. However, following the practice of the field we use the above approach to facilitate comparison of electron and hole tran- sients in this paper and comparison of these transients with other reports. For the P3HT film, a hole mobility of 6.3 −5 2 10-7 10-6 10-5 10-4 10-5 10-4 Current (A) Time (s) P3HT P3HT:F8TBT 0 1 2 3 4 5 6 2 3 4 5 6 7 8 5 Electric Field (x10 V/cm) TOF Mobility (x10 cm2 /Vs) -5 FIG. 1. ͑Color online͒ Hole TOF transients of P3HT and a P3HT:F8TBT blend. The inset displays the electric field dependence of hole mobility in the blend. 0 5.0x10-3 1.0x10-2 1.5x10-2 2.0x10-2 0 1x10-6 2x10-6 3x10-6 4x10-6 5x10-6 Current (A) Time (s) 10-5 10-4 10-3 10-2 10-8 10-7 10-6 No background With ~ 2 mA/cm2 backgro 10-5 10-4 10-3 10-7 10-6 Current (A) m (a) (b) 203310-2 C. R. McNeill and N. C. Greenham Appl. Phys. Lett. 93, 203310 ͑ McNeill and Greenham, APL 93, 203310 (2008): μ(F) ↑ in neat polymer, μ(F) ↓ in blend (see inset)
used to create cross sectional images • Slices are used to construct a 3D image • Obtaining good contrast between phases is extremely difficult J. D. Roehling, K. J. Batenburg, F. B. Swain, A. J. Moulé, and I. Arslan, Adv. Funct. Mater. 23, 2115 (2013).
of TEM tomography Tortuosity of paths in P3HT and fullerene to resp. electrodes O. Wodo, J. D. Roehling, A. J. Moulé, and B. Ganapathysubramanian, Energy Environ. Sci. 6, 3060 (2013).
Ising model for creating controlled BHJ morphologies • Characterisation of domain size, interfacial area to volume ratio, tortuosity, and more https://github.com/MikeHeiber/Ising_OPV
Medium Tortuosity High Tortuosity M. C. Heiber et al. Phys Rev Applied 8, 054043 (2017) Fit electric-field dependence to normalised Poole-Frenkel eqn µ µ0 = µ00 exp r F F0 ! <latexit sha1_base64="R1tPR+SFktRMBTHbbZbhJwfk62w=">AAADg3icjVJdSxwxFL3raKv2w7U+9iV0KVgKy4wI7Ysg/VgKIljoquDIkozZMex8Ncna2mF/lL+m9K39Hz54EmekrfQjQyYnN+ece+dORJUpY8PwW2cumF+4c3dxafne/QcPV7qrj/ZNOdWJHCZlVupDwY3MVCGHVtlMHlZa8lxk8kBMXrvzgzOpjSqLD/a8ksc5Tws1Vgm3CI26O/FY86SO8+nMvUbhjG0xB+oQMJafKxZncmzXWSyk5Sw2H7Wtr0WDWT2AADSt0lP7bNTthf3QD3YbRA3oUTP2ytVOl2I6oZISmlJOkgqywBlxMniOKKKQKsSOqUZMAyl/LmlGy9BOwZJgcEQneKfYHTXRAnvnabw6QZYMU0PJ6CnmwDsKsF1WCWywXmJ+8bH0jxlq7+wqPMcq4LjkHXcRt3QKxr+UecNsa/kfpYCq5Qv/NSdAKeqWeCbAbT3uzGD/Cd1yrgyereJnzt86aGlML33nFHpR+YjraXJTwxucaJ/ZnTB665kpPITfnyFHgXWIfO6Ptg7Md9fVzv0qvUvROHL4aV+3cvXgTkW/36DbYH+jH4X96P1mb/tVc7sW6TE9oXXcoBe0Te9oD3UkdEFf6Tv9CBaC58FGsHlNnes0mjX6ZQRbV+Rrvc8=</latexit> <latexit sha1_base64="R1tPR+SFktRMBTHbbZbhJwfk62w=">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</latexit> <latexit sha1_base64="R1tPR+SFktRMBTHbbZbhJwfk62w=">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</latexit> <latexit sha1_base64="R1tPR+SFktRMBTHbbZbhJwfk62w=">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</latexit>
on disorder, temperature, and tortuosity; but not on domain size (sim not shown) • Could be used to estimate relative tortuosity changes in different films M. C. Heiber et al. Phys Rev Applied 8, 054043 (2017)
the charge carrier mobility? • tortuosity = actual transport path / ideal transport path • anisotropic domains: higher average tortuosity • tortuosity increases for decreasing blend ratio • combination of high disorder & high tortuosity → negative field dependence of mobility Same principle for neat materials with polymer chains or aggregates having (pretty) different „intramolecular“ and „intermolecular“ mobilities!