Effect of spin-orbit coupling on magnetoresistance in organic semiconductors Y. Sheng, 1 T. D. Nguyen, 1 G. Veeraraghavan, 2 Ö. Mermer, 1 and M. Wohlgenannt 1, * 1 Department of Physics and Astronomy and Optical Science and Technology Center, University of Iowa, Iowa City, Iowa 52242-1479, USA 2 Department of Electrical and Computer Engineering and Optical Science and Technology Center, University of Iowa, Iowa City, Iowa 52242-1595, USA Received 17 July 2006; revised manuscript received 2 October 2006; published 2 January 2007 We study the recently discovered organic magnetoresistance OMAReffect in a pair of materials that have similar chemical structures except that one contains a heavy atom to enhance spin-orbit coupling. We use photoluminescence spectroscopy to estimate the spin-orbit coupling strength. In the material with weak spin- orbit coupling the characteristic magnetic field scale is comparable to the hyperfine coupling strength. In the material with strong spin-orbit coupling we find that the OMAR is strongly reduced in size and the OMAR traces clearly exhibit a second, higher field scale which we identify with the spin-orbit coupling strength. We model our results using the standard spin-dynamics Hamiltonian. DOI: 10.1103/PhysRevB.75.035202 PACS numbers: 73.50.-h, 73.43.Qt I. INTRODUCTION There has been growing interest in magnetoelectronic effects 16 in organic semiconductors. We recently discovered 1 a large, low-field up to 10% at 10 mT and 300 Kmagnetoresistive effect in organic light-emitting di- odes OLEDs, which we dubbed organic magnetoresistance OMAR. The effect has also been observed by others. 6 In addition to its potential applications, OMAR poses a signifi- cant scientific puzzle since it is, to the best of our knowledge, the only known example of large room-temperature magne- toresistance in nonmagnetic materials with the exception of high-mobility materials. 7,8 To the best of our knowledge the mechanism causing OMAR is currently not known with certainty, although two theories based on spin dynamics have been suggested very recently. 6,9 In general, magnetoresistance in nonmagnetic de- vices can be caused by several different physical principles: iLorentz force deflection, causing effects like Hall volt- ages, classical magnetoresistance, and extraordinary magnetoresistance, 10 iiquantum-mechanical diamagnetism, such as effects associated with Landau levels or hopping magnetoresistance, 11 iiiinterference phenomena such as weak localization 12 that are sensitive to magnetic fields be- cause the vector potential enters the Schrödinger equation in a way that leads to phase shifts, and finally ivspin dynam- ics. In our opinion, we have been able to exclude iiiiin our earlier work 3 as possible explanations for OMAR. How- ever, spin dynamics could be the cause of OMAR. Prior work 6,13 has shown that OMAR is substantially reduced upon introduction of spin-orbit coupling. No attempt was made, however, to examine on a quantitative level whether this observation can actually be derived from the spin-orbit coupling Hamiltonian. In any case, a detailed comparison between theory and experiment would not have been pos- sible, because experimental OMAR traces in Refs. 6 and 13 in materials with strong spin-orbit coupling were below the experimental noise level. In the present work we remedy these shortcomings by using a modulation technique to record OMAR traces in materials with strong spin-orbit coupling. For the benefit of the reader, we will briefly summarize some of the main experimental results regarding OMAR. We have shown 13,14 that iOMAR is a bulk effect rather than an interface effect; iithe functional form of OMAR is accurately described by the laws B 2 / B 2 + B 0 2 or B 2 / |B | + B 0 2 dependent on the material, where B 0 5 mT in all materials we have studied; iiithe effect is indepen- dent of the magnetic field direction; ivthe magnitude of the OMAR effect is only weakly dependent on the minority car- rier density; and vOMAR can be of positive or negative sign, dependent on material and/or operating conditions of the devices. II. EXPERIMENT The device fabrication steps were described in detail in our earlier publications 13 and follow the standard OLED fabrication recipe. The -conjugated small molecules tris8- hydroxyquinolinealuminium Alq 3 and tris2- phenylpyridineiridium Irppy 3 were purchased from H. W. Sands corporation. The samples were mounted on the cold finger of a closed-cycle helium cryostat located between the poles of an electromagnet. The magnetoconductance ratio I / I, for the Alq 3 devices was determined by measuring the current I at a constant applied voltage V for different mag- netic fields, B. Due to the much smaller magnetoresistance effect in Irppy 3 devices, I / I could not be measured in the same way. Instead, a modulation method was required: for each constant voltage and B, Itpulses are recorded as the applied magnetic field is switched on and off multiple times at a frequency of approximately 1 Hz. The ratio I / I for that certain magnetic field is calculated using fast fourier trans- form LABVIEWfrom the current pulses. By varying the ap- plied magnetic field, I / I as a function of B is obtained. The number of pulses was chosen such that a sufficient signal-to- noise ratio was achieved. The modulation technique em- ployed required the usage of a relatively small magnet B 300 mTsince larger magnets have large self-inductance, severely limiting the achievable modulation frequency. For PHYSICAL REVIEW B 75, 035202 2007 1098-0121/2007/753/0352026©2007 The American Physical Society 035202-1