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Within this study, we investigate the intrinsic photostability of thin‐film solar cells, here organic photovoltaic cells. Since degradation under natural sun light proceeds within the timeframe of months and years, the process needs to be speeded up for fast material analysis and screening, using high‐concentration accelerated lifetime testing (high‐C ALT). For this purpose, we established setups allowing irradiances of up to 730 sun equivalents (SE). One key finding of our study is that accelerating the testing procedure by such large intensities is possible but a precise measurement and control of the solar cell temperature is absolutely essential. Accordingly, we developed an innovative method of determining the temperature of the active layer which offers significant advantages over commonly used measurement methods. Furthermore, it was found that the degradation process under high illumination densities can be well described by a stretched exponential law. We demonstrate that the temperature kinetics of P3HT:PCBM was found to be Arrhenius governed with an activation energy of 27.2 kJ/mol under continuous illumination of 300 SE. Finally, it was shown that the velocity of light‐induced degradation of short‐circuit current depends linearly on the used irradiance dose at a given temperature starting from normal illumination conditions up to at least 300 SE. This makes high‐C ALT a very valuable tool for swift screening of the lifetime of novel thin‐film solar cells and materials.

Although ternary organic solar cells (OSCs) have unique advantages in improving device performance, the morphology assembly in the ternary-phase would be more uncertain or complex than that in the binary-phase. Here, we propose a new concept of oligomer-assisted photoactive layers for high-performance OSCs. The formed alloy-like phase of the oligomer : host polymer blend enabled the oligomer-assisted OSCs to fuse the advantages of both binary and ternary devices, exhibiting substantially enhanced performance and stability compared to the control devices. With the addition of oligomers, outstanding efficiencies of 17.33 % for a PM6 : Y6 device, 18.32 % for a PM6 : BTP-eC9 device, and 17.13 % for a PM6/Y6 pseudo-bilayer device were achieved, all of which are one of the highest values in their corresponding fields. The improved performance originated from the downshift energy levels, enhanced light absorption, optimized blend morphology, favorable charge dynamics, and reduced non-radiative energy loss.

While power conversion efficiencies (PCEs) of bulk heterojunction (BHJ) organic solar cells (OSCs) continue increasing towards the 20% milestone, important factors for industrial application are mostly neglected, such as photostability and the cost potential. Single-component organic solar cells (SCOSCs) employing materials with donor and acceptor moieties chemically bonded, successfully overcome the immiscibility between donor and acceptor as well as the resultant self-aggregation under external stress. To inspire a broader interest, the industrial figure of merit (i-FoM) of BHJ OSCs and the corresponding SCOSCs are calculated and analyzed, which includes PCE, photostability, and synthetic complexity (SC) index. Despite slightly more complex synthesis, all SCOSCs exhibit increased i-FoM values than the corresponding BHJ OSCs, and with the increase of efficiency, SCOSCs possess the further potential to a higher i-FoM value. With the excellent photostability for nearly all investigated single component semiconductors, SCOSCs are coming into the focus of attention for industrial utilization.

Rational design and engineering of top interface layers with combined properties of effective passivation, high thermal‐ and photo‐stability are effective methods to advance the commercialization of perovskite photovoltaics. Here, an innovative anode interface combination is developed based on alcohol‐dispersed poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) nanoparticles as the hole transport material and chlorobenzene‐dissolved trioctylphosphine oxide (TOPO) as the passivation agent. It is shown that instead of the commonly used 2D passivation ligands, TOPO‐passivated perovskite films exhibit greatly improved thermal stability. Furthermore, the passivation contributes to an enhanced carrier lifetime and reduced surface trap density, yielding an improvement in the quasi‐fermi‐level splitting of 57 meV. To maintain surface passivation during solution processing of further layers, it is necessary to develop a hole transport layer that can be processed from orthogonal solvents. P3HT nanoparticles formulated in alcoholic media fully meet this requirement, clearly benefitting from their high vertical conductivity and extremely low contact resistance with carbon electrodes. Based on this configuration, device efficiency of up to 18.4% is demonstrated for perovskite solar cells with fully solution‐processed carbon electrodes, along with significantly improved device stability and reproducibility.

A method for organic solar cell (OSC) stability testing is presented that aims to provide more unique insight into the causes of degradation patterns of OSCs. The method involves using monochromatic light at high irradiation doses to accelerate isolated degradation mechanisms while monitoring the device with a series of in‐situ steady‐state and transient electrical measurements. The experimental results are accompanied by drift‐diffusion simulations to localize degradation pathways. PM6:Y6‐based OSCs are tested, which are known to show a rather broad range of lifetimes as a function of device architecture, material batches, or degradation conditions. The experiments reveal a degradation mechanism that causes an increased trap‐state density inside the PM6:Y6 layer. The transient simulations suggest that these states are formed at or around the interface between the PM6:Y6 and the electron transport layer. Furthermore, the surprisingly dominant impact of the illuminating wavelength on the degradation pattern is evidenced. Lastly, the degradation rate of the devices scales linearly with light intensity, making high intensity and spectrally selective degradation the most promising way to accelerate stability testing for the faster development of stable OSCs.

The incorporation of solid additive has been considered as an effective strategy for developing organic photovoltaics with multi-components, which is independent of dynamics, playing unique roles in morphology adjustment. However, their complex working mechanisms involving specific chemical structures are selective to material systems, hence limiting their university and flexibility in application. Herein, we introduce an inert small-molecular compound naphtho[1,2-c:5,6-c′]bis[1,2,5]thiadiazole (NT) into the bulk-heterojunction blend as the solid additive, which can function with various material systems and solvents, depending on its simple π-conjugated structure and S···N interaction for adjusting molecular alignment. It is interesting to note that the introduced NT can not only improve device performance, but also simplify complicated pre- or post-processing methods, reduce impact from batch-to-batch differences, construct sufficient energy transfer channel as well as improve device stability. The resulting devices based on PTzBI-dF:Y6-BO system show an impressive power conversion efficiency of 17.4% with obviously enhanced T80 lifetime of >1200 h. These findings provide useful guidelines for exploring potential universal solid additives benefitting toward commercial application.

Organic solar cells are composed of electron donating and accepting organic semiconductors. Whilst a significant palette of donors has been developed over three decades, until recently only a small number of acceptors have proven capable of delivering high power conversion efficiencies. In particular the fullerenes have dominated the landscape. In this perspective, the emergence of a family of materials-the non-fullerene acceptors (NFAs) is described. These have delivered a discontinuous advance in cell efficiencies, with the significant milestone of 20% now in sight. Intensive international efforts in synthetic chemistry have established clear design rules for molecular engineering enabling an ever-expanding number of high efficiency candidates. However, these materials challenge the accepted wisdom of how organic solar cells work and force new thinking in areas such as morphology, charge generation and recombination. This perspective provides a historical context for the development of NFAs, and also addresses current thinking in these areas plus considers important manufacturability criteria. There is no doubt that the NFAs have propelled organic solar cell technology to the efficiencies necessary for a viable commercial technology-but how far can they be pushed, and will they also deliver on equally important metrics such as stability? The work was supported by the Ser Cymru II Program through the Welsh Government, European Regional Development Fund, Welsh European Funding Office, and Swansea University strategic initiative in Sustainable Advanced Materials. A.A. is a Ser Cymru II Rising Star Fellow and P.M. is a Ser Cymru II National Research Chair. T.W. acknowledges financial support from the National Natural Science Foundation of China (21774097). Z.X. and L.D. thank National Key Research and Development Program of China (2017YFA0206600) and National Natural Science Foundation of China (51773045, 21772030, 51922032, 21961160720) for financial support. J.N. thanks the European Research Council for support under the European Union's Horizon 2020 research and innovation program (grant agreement No 742708). Armin, A; Meredith, P (corresponding author), Swansea Univ, Dept Phys, Sustainable Adv Mat Ser SAM, Singleton Pk, Swansea SA2 8PP, W Glam, Wales. ardalan.armin@swansea.ac.uk; paul.meredith@swansea.ac.uk

There is a strong market driven need for processing organic photovoltaics from eco-friendly solvents. Water-dispersed organic semiconducting nanoparticles (NPs) satisfy these premises convincingly. However, the necessity of surfactants, which are inevitable for stabilizing NPs, is a major obstacle towards realizing competitive power conversion efficiencies for water-processed devices. Here, we report on a concept for minimizing the adverse impact of surfactants on solar cell performance. A poloxamer facilitates the purification of organic semiconducting NPs through stripping excess surfactants from aqueous dispersion. The use of surfactant-stripped NPs based on poly(3-hexylthiophene) / non-fullerene acceptor leads to a device efficiency and stability comparable to the one from devices processed by halogenated solvents. A record efficiency of 7.5% is achieved for NP devices based on a low-band gap polymer system. This elegant approach opens an avenue that future organic photovoltaics processing may be indeed based on non-toxic water-based nanoparticle inks., Water-based semiconducting polymer nanoparticles are eco-friendly and non-toxic but their performance suffers from the surfactants. Here Xie et al. design an approach to minimize the amount of residual surfactant in these nanoparticles and make high-efficiency and stability solar cells.

Single-component organic solar cells (SCOSCs) have witnessed great improvement during the last few years with the champion efficiency jumping from the previous 2–3% to currently 6–11% for the representative material classes. However, the photophysics in many of these materials has not been sufficiently investigated, lacking essential information regarding charge-carrier dynamics as a function of microstructure, which is highly demanded for a better understanding and potential guidance for further improvements. In this work, for the first time, the charge-carrier dynamics of a representative double-cable polymer, which achieves efficiencies of over 6% as an active layer in SCOSCs, is investigated across seven orders of magnitude in time scale, from fs–ps charge generation to ns–µs charge recombination processes. Specific emphasis is placed on understanding the impact of thermal post-treatment on the charge dissociation and recombination dynamics. Annealing the photoactive layer at 230 °C results in the highest photovoltaic performance because of efficient charge generation in parallel to suppressed recombination. This work intends to present a complete picture of the charge-carrier dynamics in SCOSCs using the representative double-cable polymer PBDBPBICl.

Simultaneously enhancing device performance and longevity, as well as balancing the requirements on cost, scalability, and simplification of processing, is the goal of interface engineering of organic solar cells (OSCs). In our work, we strategically introduce antimony (Sb3+) cations into an efficient and generic n-type SnO2 nanoparticles (NPs) host during the scalable flame spray pyrolysis synthesis. Accordingly, a significant switch of conduction property from an n-type character to a p-type character is observed, with a corresponding shift in the work function (WF) from 4.01 ± 0.02 eV for pristine SnO2 NPs to 5.28 ± 0.02 eV for SnO2 NPs with 20 mol. % Sb content (ATO). Both pristine SnO2 and ATO NPs with fine-tuned optoelectronic properties exhibit remarkable charge carrier extraction properties, excellent UV resistance and photo-stability being compatible with various state-of-the-art OSCs systems. The reliable and scalable pristine SnO2 and ATO NPs processed by doctor-blading in air demand no complex post-treatment. Our work offers a simple but unique approach to accelerate the development of advanced interfacial materials, which could circumvent the major existing interfacial problems in solution-processed OSCs.

Numerous articles on thermal annealing (TA) and solvent vapor annealing (SVA) treatments have shown that both strategies effectively improve bulk morphology, reduce carrier recombination and thus improve photovoltaic performance of bulk heterojunction (BHJ) organic solar cells (OSCs). In previous work, we found that both TA and SVA treated devices based on a blend composed of a 3-ethyl-2-thioxothiazolidin-4-one containing molecule as donor (named DRCN5T) and [6,6]-phenyl-C71-butyric acid methyl ester (PC70BM) as acceptor show the similar photovoltaic performance, but their bulk microstructures are difference. Here employing in situ photoluminescence (PL) setup and X-ray scattering technologies, we found that the early stages of SVA remarkably affect the surface of film, and in contrast TA affects the whole bulk. Meanwhile, a plurality of experimental results all further confirm the different thermodynamics and kinetics of morphology evolution processed either by TA treatment or SVA treatment. Importantly, it was found that the SVA-treated film showed the increased photo-degradation in devices as compared to the TA-treated layer, resulting from obvious bulk morphology changes under illumination over 500 hours. The aim is to provide comprehensive insight into the influence of TA and SVA on time morphological evolution and degradation in OSCs.

Solution‐processed organic solar cells (OSCs) are promising low‐cost, flexible, portable renewable sources for future energy supply. The state‐of‐the‐art OSCs are typically fabricated from a bulk‐heterojunction (BHJ) active layer containing well‐mixed donor and acceptor molecules in the nanometer regime. However, BHJ solar cells suffer from stability problems caused by the severe morphological changes upon thermal or illumination stress. In comparison, single‐component organic solar cells (SCOSCs) based on a double‐cable conjugated polymer with a covalently stabilized microstructure is suggested to be a key strategy for superior long‐term stability. Here, the thermal‐ and photostability of SCOSCs based on a model double‐cable polymer is systematically investigated. It is encouraging to find that under 90 °C & 1 sun illumination, the performance of SCOSCs remains substantially stable. Transport measurements show that charge generation and recombination (lifetime and recombination order) hardly change during the aging process. Particularly, the SCOSCs exhibit ultrahigh long‐term thermal stability with 100% PCE remaining after heating at temperature up to 160 °C for over 400 h, indicating an excellent candidate for extremely rugged applications.

Mesoscale-structured materials offer broad opportunities in extremely diverse applications owing to their high surface areas, tunable surface energy, and large pore volume. These benefits may improve the performance of materials in terms of carrier density, charge transport, and stability. Although metal oxides-based mesoscale-structured materials, such as TiO2, predominantly hold the record efficiency in perovskite solar cells, high temperatures (above 400 degrees C) and limited materials choices still challenge the community. A novel route to fabricate organic-based mesoscale-structured interfaces (OMI) for perovskite solar cells using a low-temperature and green solvent-based process is presented here. The efficient infiltration of organic porous structures based on crystalline nanoparticles allows engineering efficient "n-i-p" and "p-i-n" perovskite solar cells with enhanced thermal stability, good performance, and excellent lateral homogeneity. The results show that this method is universal for multiple organic electronic materials, which opens the door to transform a wide variety of organic-based semiconductors into scalable n- or p-type porous interfaces for diverse advanced applications.

Morphological control over the bulk heterojunction (BHJ) microstructure of a high-efficiency small molecule photovoltaic system composed of a quinquethiophene based molecule (DRCN5T) as electron donor and [6,6]-phenyl-C71-butyric acid methyl ester (PC70BM) as electron acceptor is demonstrated using three different post-processing strategies, including thermal annealing (TA), solvent vapor annealing (SVA), and two-step annealing (TA-SVA) treatments. We systematically analyze the processing condition-microstructure-device property relationships, explore the corresponding morphology evolution and their effects on carrier transport and recombination dynamics in BHJs as well as understand the nature of phase-separation process resulting in light-induced degradation mechanisms. Within the investigated results, the causative relations between annealing sequence, photovoltaic parameters, morphology evolution and charge carrier dynamics are for the first time delineated. In addition, the observed trade-offs in device efficiency and stability with respect to the well-defined morphologies are highlighted. The in-depth picture of the bulk microstructure formation and its kinetic evolution as a function of the specific post-processing approaches is a valuable asset for the design of new photovoltaic materials and thin film nanoscale architectures that are more efficient and better aid future commercialization efforts.

Correction for ‘Balancing electrical and optical losses for efficient 4-terminal Si-perovskite solar cells with solution processed percolation electrodes’ by César Omar Ramírez Quiroz et al., J. Mater. Chem. A, 2018, 6, 3583–3592.

Lead halide perovskites often suffer from a strong hysteretic behavior on their j–V response in photovoltaic devices that has been correlated with slow ion migration. The electron extraction layer has frequently been pointed to as the main culprit for the observed hysteretic behavior. In this work three hole transport layers are studied with well‐defined highest occupied molecular orbital (HOMO) levels and interestingly the hysteretic behavior is markedly different. Here it is shown that an adequate energy level alignment between the HOMO level of the extraction layer and the valence band of the perovskite, not only suppresses the hysteresis, avoiding charge accumulation at the interfaces, but also degradation of the hole transport layer is reduced. Numerical simulation suggests that formation of an injection barrier at the organic/perovskite heterointerface could be one mechanism causing hysteresis. The suppression of such barriers may require novel design rules for interface materials. Overall, this work highlights that both external contacts need to be carefully optimized in order to obtain hysteresis‐free perovskite devices.

While perovskite-based semitransparent solar cells deliver competitive levels of transparency and efficiency to be envisioned for urban infrastructures, the complexity and sensitivity of their processing conditions remain challenging. Here, we introduce two robust protocols for the processing of sub-100 nm perovskite films, allowing fine-tuning of the active layer without compromising the crystallinity and quality of the semiconductor. Specifically, we demonstrate that a method based on solvent-induced crystallization with a rapid drying step affords perovskite solar cells with 37% average visible transmittance (AVT) and 7.8% PCE. This process enhances crystallization with a preferential phase orientation presumably at the interface, yielding a high fill factor of 72.3%. The second method is based on a solvent–solvent extraction protocol, enabling active layer films as thin as 40 nm and featuring room-temperature crystallization in an ambient environment on a few second time span. As a result, we demonstrate a maximum AVT of 46% with an efficiency of 3.6%, which is the highest combination of efficiency and transparency for a full device stack to date. By combining the two methods presented here we cover a broad range of thicknesses vs. transparency values and confirm that solvent-induced crystallization represents a powerful processing strategy toward high-efficiency semitransparent solar cells. Optical simulations support our experimental findings and provide a global perspective of the opportunities and limitations of semitransparent perovskite photovoltaic devices.

In the current work, we have investigated the morphological aspects of the ternary solar cells based on host matrices of P3HT:PCBM and P3HT:ICBA, using the low bandgap polymer analogues of C- and Si-bridged PCPDTBT as near IR sensitizers, which show noticeably different performance. A direct comparison of these well-functional and poorly functional ternary blend systems provides insights into the bottlenecks of device performance and enables us to set up an initial set of design rules for ternary organic solar cells. Our study reveals the importance of surface energy as a driving force controlling sensitizer location and morphology formation of ternary blends. The interfacial surface energy results indicate that Si-PCPDTBT locates at amorphous interfaces and P3HT crystallites, while C-PCPDTBT tends to accumulate at amorphous interfaces and semi-crystalline (or agglomerated) domains of the fullerene derivatives. GIWAXS and SCLC results support this prediction where adding high content of C-PCPDTBT influences mainly the semi-crystallinity (aggregation) of the fullerene and reduces the electron mobility, but Si-PCPDTBT impacts mainly the P3HT ordering and, in turn, deteriorates the hole mobility. These findings show that the disruption of the fullerene semi-crystalline domains is more detrimental to the device performance than the disruption of the polymer domains.

Long-term stability of polymer solar cells is determined by many factors, one of which is thermal stability. Although many thermal stability studies occur far beyond the operating temperature of a solar cell which is almost always less than 65 °C, thermal degradation is studied at temperatures that the solar cell would encounter in real-world operating conditions. At these temperatures, movement of the polymer and fullerenes, along with adhesion of the polymer to the back contact, creates a barrier for electron extraction. The polymer barrier can be removed and the performance can be restored by peeling off the electrode and depositing a new one. X-ray photoelectron spectroscopy measurements reveal a larger amount of polymer adhered to electrodes peeled from aged devices than electrodes peeled from fresh devices. The degradation caused by hole-transporting polymer adhering to the electrode can be suppressed by using an inverted device where instead of electrons, holes are extracted at the back metal electrode. The problem can be ultimately eliminated by choosing a polymer with a high glass transition temperature.

Hybrid organo-metal halide perovskites are an exciting new class of solar absorber materials and have exhibited a rapid increase in solar cell efficiencies throughout the past two years to over 17% in both meso-structured and thin-film device architectures. We observe slow transient effects causing hysteresis in the current–voltage characterization of these devices that can lead to an over- or underestimation of the solar cell device efficiency. We find that the current–voltage (IV) measurement scan direction, measurement delay time, and light and voltage bias conditions prior to measurement can all have a significant impact upon the shape of the measured IV light curves and the apparent device efficiency. We observe that hysteresis-free light IV curves can be obtained at both extremely fast and slow voltage scan rates but only in the latter case are quasi-steady-state conditions achieved for a valid power conversion efficiency measurement. Hysteretic effects are also observed in devices utilizing alternative selective contacts but differ in magnitude and time scale, suggesting that the contact interfaces have a big effect on transients in perovskite-absorber devices. The transient processes giving rise to hysteresis are consistent with a polarization response of the perovskite absorber that results in changes in the photocurrent extraction efficiency of the device. The strong dependence of the hysteresis on light and voltage biasing conditions in thin film devices for a period of time prior to the measurement suggests that photo-induced ion migration may additionally play an important role in device hysteresis. Based on these observations, we provide recommendations for correct measurement and reporting of IV curves for perovskite solar cell devices.

The understanding and control of nanostructures with regard to transport and recombination mechanisms is of key importance in the optimization of the power conversion efficiency (PCE) of solar cells based on inorganic nanocrystals. Here, the transport properties of solution-processed solar cells are investigated using photo-CELIV (photogenerated charge carrier extraction by linearly increasing voltage) and transient photovoltage techniques; the solar cells are prepared by an in-situ formation of CuInS2 nanocrystals (CIS NCs) at the low temperature of 270 °C. Structural and morphological analyses reveal the presence of a metastable CuIn5S8 phase and a disordered morphology in the CuInS2 nanocrytalline films consisting of polycrystalline grains at the nanoscale range. Consistent with the disordered morphology of the CIS NC thin films, the CIS NC devices are characterized by a low carrier mobility. The carrier density dynamic indicates that the recombination kinetics in these devices follows the dispersive bimolecular recombination model and does not fully behave in a diffusion-controlled manner, as expected by Langevin-type recombination. The mobility–lifetime product of the charge carriers properly explains the performance of the thin (200 nm) CIS NC solar cell with a high fill-factor of 64% and a PCE of over 3.5%.

A new star-shaped D–π–A molecule, tris{4-[5′′-(1,1-dicyanobut-1-en-2-yl)-2,2′-bithiophen-5-yl]phenyl}amine N(Ph-2T-DCN-Et)3, with high efficiency potential for photovoltaic applications was synthesized. As compared to its analogue S(TPA-bT-DCN), it showed stronger absorption in the region of 350–450 nm and a lower lying highest occupied molecular energy level (HOMO). Solution-processed organic solar cells (OSCs) based on a blend of N(Ph-2T-DCN-Et)3 and PC70BM resulted in a high PCE of 3.1% without any post-treatment. The PCE of N(Ph-2T-DCN-Et)3 based solar cells was further improved to 3.6% under simulated AM 1.5 by addition of a new additive 4-bromoanisole (BrAni).

Theoretical and experimental studies suggest that energetic offsets between the charge transport energy levels in different morphological phases of polymer:fullerene bulk heterojunctions may improve charge separation and reduce recombination in polymer solar cells (PSCs). In this work, we use cyclic voltammetry, UV-vis absorption, and ultraviolet photoelectron spectroscopy to characterize hole energy levels in the polymer phases of polymer:fullerene bulk heterojunctions. We observe an energetic offset of up to 150 meV between amorphous and crystalline polymer due to bandgap widening associated primarily with changes in polymer conjugation length. We also observe an energetic offset of up to 350 meV associated with polymer:fullerene intermolecular interactions. The first effect has been widely observed, but the second effect is not always considered despite being larger in magnitude for some systems. These energy level shifts may play a major role in PSC performance and must be thoroughly characterized for a complete understanding of PSC function.

This article presents a smart strategy to successfully tackle two main limitations of organic solar cells (OSCs) in one step: the narrow absorption window of polymers as well as the Voc limitation related to the mono-PCBM. We demonstrate the high OSC performance of >5% in the combination of a fullerene multiadduct, i.e. indene-C60 bisadduct (ICBA) with a low bandgap polymer employing the concept of ternary OSCs. Solar cells achieving a fill factor (FF) of >60% along with high quantum efficiency in the near IR region are demonstrated for ternary composites consisting of P3HT, the fullerene-bisindene adduct of ICBA and a low bandgap copolymer sensitizer. Using P3HT as an efficient transport matrix with non-Langevin recombination dynamics allowed us to limit and overcome the otherwise dominant recombination losses of the indene-C60 bisadduct – low bandgap copolymer blends. The success of this strategy resulted in a relative efficiency improvement of over 25%.

Carbon-based organic electronics are a technology, with the potential of complementing and substituting opto-electronic devices based on inorganic semiconductors and metals. In the group of organic semiconductors, carbon allotropes come with outstanding opto-electric properties and are remarkable candidates for novel applications like printed electronics via solution-processing on mechanically flexible, robust and light weight substrates, while reducing the environmental impact. Carbon allotropes like fullerenes, graphene quantum dots (GQD), carbon nanotubes (CNT), graphene and also diamond are especially interesting for photodetectors due to their tunable bandgap, high absorption coefficients and high charge carrier mobilites. These unique opto-electric properties of the allotropes, which strongly depend on their molecular dimensionality (0D, 1D, 2D and 3D), allow each allotrope to be used in a preferential range. Hence, relying on the intrinsic properties of carbon allotropes or by hybridization, carbon-based photodetectors are built for a spectral bandwidth, reaching from gamma-rays to THz radiation. This review highlights the recent advances in photodetectors based on fullerenes, GQDs, CNTs, graphene and diamond, with the focus on room temperature-operated devices. The versatility of multi-dimensional carbon allotropes is outstanding, and promising results outline the maturing of all carbon-based photodetection across the technologically relevant wavelengths.