arXiv subjects

Safa Shoaee

Publications and source records attributed to Safa Shoaee.

7 recordsLinked to original sources

arXiv2025

The contribution of electron and hole conductivity to the transport loss in organic solar cells

The effective conductivity determines the reciprocal of the transport resistance, the dominant loss of fill factor in organic solar cells. We experimentally determine the dependence of effective conductivity on its electron and hole contributions. Using PM6:Y12 blends with tunable morphological and energetic disorder, we show that the effective conductivity follows a harmonic mean of electron and hole conductivities even across nearly three orders of magnitude in conductivity imbalance. We also validate the method for directly extracting effective conductivity from current-voltage measurements, eliminating the need to rely on indirect mobility and charge carrier density-based proxies. Our findings challenge the widespread use of geometric mean approximations and offer a more accurate framework for analysing and modelling transport in disordered organic semiconductors.

cond-mat.mtrl-sci↗

arXiv2025

Understanding the fill-factor limit of organic solar cells

Although the power conversion efficiencies of organic solar cells (OSCs) have surpassed 20%, they still lag behind commercial inorganic solar cells and emerging perovskite solar cells. To bridge this efficiency gap, improving the fill factor (FF) is critical, provided other photovoltaic parameters are not compromised. However, the fundamental understanding of the FF in OSCs remains incomplete. In this work, we systematically investigate a wide range of OSCs with the FF values spanning 0.27 to 0.80, and analyse the effect of free charge generation and recombination on the FF in OSCs. To explain our observations, we developed an analytical model that quantitatively correlates the applied electric field with the energetics of excited states in donor-acceptor blends. By combining device characterisation, spectroscopy, and theoretical modelling, we reveal that the Stark effect and the field-dependent charge transfer significantly impact the FF in state-of-the-art OSCs with low voltage losses. Our findings highlight that suppressing geminate decay by increasing exciton lifetime is a promising strategy for boosting the FF and achieving future efficiency gains in OSCs.

cond-mat.mtrl-sci↗

arXiv2025

Triplet Excitons Reconcile Charge Generation and Recombination in Low-Offset Organic Solar Cells: Efficiency Limits from a 5-State Model

The power conversion efficiency of organic solar cells has recently improved beyond 20%. The active layers of these devices comprise of at least two organic semiconductors, forming a type II heterojunction. Hereby, the device performance is determined by the kinetic interplay of various species, including localized excitons, charge transfer states as well as charge-separated states. However, a model which describes all relevant photovoltaic measures has yet to be developed. Herein, we present a comprehensive 5-state rate model which includes both singlet and triplet charge transfer states and takes into account the formation, re-splitting and decay of the local triplet state, parametric in the respective energy offset. We show that this model not only describes key device properties such as charge generation efficiency, photoluminescence, electroluminescence and Langevin reduction factor simultaneously but also elucidate how these vary across material combinations based on the D:A interfacial energy offset alone. We find that the electroluminescence and Langevin reduction factor depend strongly on the triplet properties and that the triplet decay becomes the dominant charge recombination pathway for systems with moderate offset, in full agreement to previous experimental results. Validation against literature data demonstrates the model's ability to predict the device efficiency accurately. Subsequently, we identify material combinations with singlet exciton to charge transfer state energetic offset of roughly 150meV as particularly promising. Our model explains further why recent certified efficiency records for binary blends remain at ca. 20% if no further means to improve photon and charge carrier harvesting are taken.

cond-mat.mtrl-sci↗

arXiv2023

Whats special about Y6; the working mechanism of neat Y6 organic solar cell

Non-fullerene acceptors (NFA) have delivered advance in bulk heterojunction organic solar cell efficiencies, with the significant milestone of 20% now in sight. However, these materials challenge the accepted wisdom of how organic solar cells work. In this work we present neat Y6 device with efficiency above 4.5%. We thoroughly investigate mechanisms of charge generation and recombination as well as transport in order to understand what is special about Y6. Our data suggest Y6 generates bulk free charges, with ambipolar mobility, which can be extracted in the presence of transport layers

cond-mat.mtrl-sci↗

arXiv2023

Anticorrelated Photoluminescence and Free Charge Generation Proves Field-Assisted Exciton Dissociation in Low-Offset PM6:Y5 Organic Solar Cells

Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high performance donor-acceptor systems. Here, we probe the origin of field-dependent free charge generation and photoluminescence in non-fullerene acceptor (NFA) based organic solar cells using the polymer PM6 and NFA Y5 - a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of samples with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artefacts from non-geminate recombination of photogenerated- and dark charge carriers near the electrodes. We then correlate free charge generation with steady state photoluminescence intensity, and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low offset system is entirely controlled by the field dependent exciton dissociation into charge transfer states.

cond-mat.mtrl-sci↗

arXiv2022

Structural order promotes efficient separation of delocalized charges at molecular heterojunctions

The energetic landscape at the interface between electron donating and accepting molecular materials favors efficient conversion of intermolecular charge-transfer states (CTS) into free charge carriers in high-performance organic solar cells. Here, we elucidate how interfacial energetics, charge generation and radiative recombination are affected by structural ordering. We experimentally determine the CTS binding energy of a series of model, small molecule donor-acceptor blends, where the used acceptors (B2PYMPM, B3PYMPM and B4PYMPM) differ only in the nitrogen position of their lateral pyridine rings. We find that the formation of an ordered, face-on molecular packing in B4PYMPM is beneficial to efficient, field-independent charge separation, leading to fill factors over 70% in photovoltaic devices. This is rationalized by a comprehensive computational protocol showing that, compared to the more amorphous and isotropically oriented B2PYMPM, the higher order of the B4PYMPM molecules provides more delocalized CTS. Furthermore, we find no correlation between the quantum efficiency of radiative free charge carrier recombination and the bound or unbound nature of the CTS. This work highlights the importance of structural ordering at donor-acceptor interfaces for efficient free carrier generation and shows that more ordering and less bound CT states do not preclude efficient radiative recombination.

physics.app-ph↗

arXiv2021

General Rules for the Impact of Energetic Disorder and Mobility on Nongeminate Recombination in Phase-Separated Organic Solar Cells

State of the art organic solar cells exhibit power conversion efficiencies of 18 % and above. These devices benefit from the suppression of free charge recombination with regard to the Langevin-limit of charge encounter in a homogeneous medium. It has been recognized that the main cause of suppressed free charge recombination is the reformation and resplitting of charge transfer states at the interface between donor and acceptor domains. Here, we use kinetic Monte Carlo simulations to understand the interplay between free charge motion and recombination in an energetically-disordered phase-separated donor-acceptor blend. We identify conditions for encounter-dominated and resplitting-dominated recombination. In the former regime, recombination is proportional to mobility for all parameters tested and only slightly reduced with respect to the Langevin limit. In contrast, mobility is not the decisive parameter determining the non-geminate recombination coefficient k_2in the latter case where k_2 is a sole function of the morphology, CT and CS energetics and CT states decay properties. Our simulations also show that free charge encounter in the phase-separated disordered blend is determined by the average mobility of all carriers, while CT reformation and resplitting involves mostly states near the transport energy. Therefore, charge encounter is more affected by increased disorder than the resplitting of the CT state. As a consequence, for a given mobility, larger energetic disorder in combination with a higher hopping rate is preferred. These findings have important implications for the understanding of suppressed recombination in solar cells with non-fullerene acceptors which are known to exhibit lower energetic disorder than fullerenes.

physics.app-ph↗