@article{LeCorreDiekmannPenaCamargoetal.2022, author = {Le Corre, Vincent M. and Diekmann, Jonas and Pe{\~n}a-Camargo, Francisco and Thiesbrummel, Jarla and Tokmoldin, Nurlan and Gutierrez-Partida, Emilio and Peters, Karol Pawel and Perdig{\´o}n-Toro, Lorena and Futscher, Moritz H. and Lang, Felix and Warby, Jonathan and Snaith, Henry J. and Neher, Dieter and Stolterfoht, Martin}, title = {Quantification of efficiency losses due to mobile ions in Perovskite solar cells via fast hysteresis measurements}, series = {Solar RRL}, volume = {6}, journal = {Solar RRL}, number = {4}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202100772}, pages = {10}, year = {2022}, abstract = {Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1\% and 3\% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments.}, language = {en} } @article{HosseiniTokmoldinLeeetal.2020, author = {Hosseini, Seyed Mehrdad and Tokmoldin, Nurlan and Lee, Young Woong and Zou, Yingping and Woo, Han Young and Neher, Dieter and Shoaee, Safa}, title = {Putting order into PM6:Y6 solar cells to reduce the langevin recombination in 400 nm thick junction}, series = {Solar RRL}, volume = {4}, journal = {Solar RRL}, number = {11}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202000498}, pages = {7}, year = {2020}, abstract = {Increasing the active layer thickness without sacrificing the power conversion efficiency (PCE) is one of the great challenges faced by organic solar cells (OSCs) for commercialization. Recently, PM6:Y6 as an OSC based on a non-fullerene acceptor (NFA) has excited the community because of its PCE reaching as high as 15.9\%; however, by increasing the thickness, the PCE drops due to the reduction of the fill factor (FF). This drop is attributed to change in mobility ratio with increasing thickness. Furthermore, this work demonstrates that by regulating the packing and the crystallinity of the donor and the acceptor, through volumetric content of chloronaphthalene (CN) as a solvent additive, one can improve the FF of a thick PM6:Y6 device (approximate to 400 nm) from 58\% to 68\% (PCE enhances from 12.2\% to 14.4\%). The data indicate that the origin of this enhancement is the reduction of the structural and energetic disorders in the thick device with 1.5\% CN compared with 0.5\% CN. This correlates with improved electron and hole mobilities and a 50\% suppressed bimolecular recombination, such that the non-Langevin reduction factor is 180 times. This work reveals the role of disorder on the charge extraction and bimolecular recombination of NFA-based OSCs.}, language = {en} } @article{AldiyarovSokolovAkylbayevaetal.2020, author = {Aldiyarov, Abdurakhman and Sokolov, Dmitriy and Akylbayeva, Aigerim and Nurmukan, Assel and Tokmoldin, Nurlan}, title = {On thermal stability of cryovacuum deposited CH4+H2O films}, series = {Low temperature physics}, volume = {46}, journal = {Low temperature physics}, number = {11}, publisher = {American Institute of Physics}, address = {Melville}, issn = {1063-777X}, doi = {10.1063/10.0002156}, pages = {1121 -- 1124}, year = {2020}, abstract = {Whereas stable homogenous states of aqueous hydrocarbon solutions are typically observed at high temperatures and pressures far beyond the critical values corresponding to individual components, the stability of such system may be preserved upon transition into the region of metastable states at low temperatures and low pressures. This work is dedicated to the study of the thermal stability of a water-methane mixture formed by cryogenic vapor phase deposition. The obtained thin films were studied using vibrational spectroscopy in the temperature range of 16-180 K. During thermal annealing of the samples, characteristic vibrational C-H modes of methane were monitored alongside the chamber pressure to register both structural changes and desorption of the film material. The obtained results reveal that upon the co-deposition of methane and water, methane molecules appear both in non-bound and trapped states. The observed broadening of the characteristic C-H stretching mode at 3010 cm(-1) upon an increase in temperature of the sample from 16 to 90 K, followed by narrowing of the peak as the temperature is reduced back to 16 K, indicates localization of methane molecules within the water matrix at lower temperatures.}, language = {en} } @article{FritschKurpiersRolandetal.2022, author = {Fritsch, Tobias and Kurpiers, Jona and Roland, Steffen and Tokmoldin, Nurlan and Shoaee, Safa and Ferron, Thomas and Collins, Brian A. and Janietz, Silvia and Vandewal, Koen and Neher, Dieter}, title = {On the interplay between CT and singlet exciton emission in organic solar cells with small driving force and its impact on voltage loss}, series = {Advanced energy materials}, volume = {12}, journal = {Advanced energy materials}, number = {31}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202200641}, pages = {11}, year = {2022}, abstract = {The interplay between free charge carriers, charge transfer (CT) states and singlet excitons (S-1) determines the recombination pathway and the resulting open circuit voltage (V-OC) of organic solar cells. By combining a well-aggregated low bandgap polymer with different blend ratios of the fullerenes PCBM and ICBA, the energy of the CT state (E-CT) is varied by 130 meV while leaving the S-1 energy of the polymer (ES1\[{E_{{{\rm{S}}_1}}}\]) unaffected. It is found that the polymer exciton dominates the radiative properties of the blend when ECT\[{E_{{\rm{CT}}}}\] approaches ES1\[{E_{{{\rm{S}}_1}}}\], while the V-OC remains limited by the non-radiative decay of the CT state. It is concluded that an increasing strength of the exciton in the optical spectra of organic solar cells will generally decrease the non-radiative voltage loss because it lowers the radiative V-OC limit (V-OC,V-rad), but not because it is more emissive. The analysis further suggests that electronic coupling between the CT state and the S-1 will not improve the V-OC, but rather reduce the V-OC,V-rad. It is anticipated that only at very low CT state absorption combined with a fairly high CT radiative efficiency the solar cell benefit from the radiative properties of the singlet excitons.}, language = {en} } @article{OmarovaYerezhepAldiyarovetal.2022, author = {Omarova, Zhansaya and Yerezhep, Darkhan and Aldiyarov, Abdurakhman and Tokmoldin, Nurlan}, title = {In Silico Investigation of the Impact of Hole-Transport Layers on the Performance of CH3NH3SnI3 Perovskite Photovoltaic Cells}, series = {Crystals}, volume = {12}, journal = {Crystals}, number = {5}, publisher = {MDPI}, address = {Basel}, issn = {2073-4352}, doi = {10.3390/cryst12050699}, pages = {17}, year = {2022}, abstract = {Perovskite solar cells represent one of the recent success stories in photovoltaics. The device efficiency has been steadily increasing over the past years, but further work is needed to enhance the performance, for example, through the reduction of defects to prevent carrier recombination. SCAPS-1D simulations were performed to assess efficiency limits and identify approaches to decrease the impact of defects, through the selection of an optimal hole-transport material and a hole-collecting electrode. Particular attention was given to evaluation of the influence of bulk defects within light-absorbing CH3NH3SnI3 layers. In addition, the study demonstrates the influence of interface defects at the TiO2/CH3NH3SnI3 (IL1) and CH3NH3SnI3/HTL (IL2) interfaces across the similar range of defect densities. Finally, the optimal device architecture TiO2/CH3NH3SnI3/Cu2O is proposed for the given absorber layer using the readily available Cu2O hole-transporting material with PCE = 27.95\%, FF = 84.05\%, V-OC = 1.02 V and J(SC) = 32.60 mA/cm(2), providing optimal performance and enhanced resistance to defects.}, language = {en} } @article{TokmoldinHosseiniRaoufietal.2020, author = {Tokmoldin, Nurlan and Hosseini, Seyed Mehrdad and Raoufi, Meysam and Phuong, Le Quang and Sandberg, Oskar J. and Guan, Huilan and Zou, Yingping and Neher, Dieter and Shoaee, Safa}, title = {Extraordinarily long diffusion length in PM6:Y6 organic solar cells}, series = {Journal of materials chemistry : A, materials for energy and sustainability}, volume = {8}, journal = {Journal of materials chemistry : A, materials for energy and sustainability}, number = {16}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7488}, doi = {10.1039/d0ta03016c}, pages = {7854 -- 7860}, year = {2020}, abstract = {The PM6:Y6 bulk-heterojunction (BHJ) blend system achieves high short-circuit current (J(SC)) values in thick photovoltaic junctions. Here we analyse these solar cells to understand the observed independence of the short-circuit current upon photoactive layer thickness. We employ a range of optoelectronic measurements and analyses, including Mott-Schottky analysis, CELIV, photoinduced absorption spectroscopy, mobility measurements and simulations, to conclude that, the invariant photocurrent for the devices with different active layer thicknesses is associated with the Y6's diffusion length exceeding 300 nm in case of a 300 nm thick cell. This is despite unintentional doping that occurs in PM6 and the associated space-charge effect, which is expected to be even more profound upon photogeneration. This extraordinarily long diffusion length - which is an order of magnitude larger than typical values for organics - dominates transport in the flat-band region of thick junctions. Our work suggests that the performance of the doped PM6:Y6 organic solar cells resembles that of inorganic devices with diffusion transport playing a pivotal role. Ultimately, this is expected to be a key requirement for the fabrication of efficient, high-photocurrent, thick organic solar cells.}, language = {en} } @article{TokmoldinVollbrechtHosseinietal.2021, author = {Tokmoldin, Nurlan and Vollbrecht, Joachim and Hosseini, Seyed Mehrdad and Sun, Bowen and Perdig{\´o}n-Toro, Lorena and Woo, Han Young and Zou, Yingping and Neher, Dieter and Shoaee, Safa}, title = {Explaining the fill-factor and photocurrent losses of nonfullerene acceptor-based solar cells by probing the long-range charge carrier diffusion and drift lengths}, series = {Advanced energy materials}, volume = {11}, journal = {Advanced energy materials}, number = {22}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6840}, doi = {10.1002/aenm.202100804}, pages = {9}, year = {2021}, abstract = {Organic solar cells (OSC) nowadays match their inorganic competitors in terms of current production but lag behind with regards to their open-circuit voltage loss and fill-factor, with state-of-the-art OSCs rarely displaying fill-factor of 80\% and above. The fill-factor of transport-limited solar cells, including organic photovoltaic devices, is affected by material and device-specific parameters, whose combination is represented in terms of the established figures of merit, such as theta and alpha. Herein, it is demonstrated that these figures of merit are closely related to the long-range carrier drift and diffusion lengths. Further, a simple approach is presented to devise these characteristic lengths using steady-state photoconductance measurements. This yields a straightforward way of determining theta and alpha in complete cells and under operating conditions. This approach is applied to a variety of photovoltaic devices-including the high efficiency nonfullerene acceptor blends-and show that the diffusion length of the free carriers provides a good correlation with the fill-factor. It is, finally, concluded that most state-of-the-art organic solar cells exhibit a sufficiently large drift length to guarantee efficient charge extraction at short circuit, but that they still suffer from too small diffusion lengths of photogenerated carriers limiting their fill factor.}, language = {en} } @article{VollbrechtTokmoldinSunetal.2022, author = {Vollbrecht, Joachim and Tokmoldin, Nurlan and Sun, Bowen and Brus, Viktor V. and Shoaee, Safa and Neher, Dieter}, title = {Determination of the charge carrier density in organic solar cells}, series = {Journal of applied physics}, volume = {131}, journal = {Journal of applied physics}, number = {22}, publisher = {American Institute of Physics}, address = {Melville, NY}, issn = {0021-8979}, doi = {10.1063/5.0094955}, pages = {18}, year = {2022}, abstract = {The increase in the performance of organic solar cells observed over the past few years has reinvigorated the search for a deeper understanding of the loss and extraction processes in this class of device. A detailed knowledge of the density of free charge carriers under different operating conditions and illumination intensities is a prerequisite to quantify the recombination and extraction dynamics. Differential charging techniques are a promising approach to experimentally obtain the charge carrier density under the aforementioned conditions. In particular, the combination of transient photovoltage and photocurrent as well as impedance and capacitance spectroscopy have been successfully used in past studies to determine the charge carrier density of organic solar cells. In this Tutorial, these experimental techniques will be discussed in detail, highlighting fundamental principles, practical considerations, necessary corrections, advantages, drawbacks, and ultimately their limitations. Relevant references introducing more advanced concepts will be provided as well. Therefore, the present Tutorial might act as an introduction and guideline aimed at new prospective users of these techniques as well as a point of reference for more experienced researchers. Published under an exclusive license by AIP Publishing.}, language = {en} }