Advanced Functional Materials and Devices (AFMD) Group

Abstract:

Organic solar cells have the potential to become the cheapest form of electricity, beating even silicon photovoltaics. This article summarizes the state of the art in the field, highlighting research challenges, mainly the need for an efficiency increase as well as an improvement in long‐term stability. It discusses possible current and future applications, such as building integrated photovoltaics or portable electronics. Finally, the environmental footprint of this renewable energy technology is evaluated, highlighting the potential to be the energy generation technology with the lowest carbon footprint of all.

Abstract:

The microstructure of organic small molecule (SM) layers in organic solar cells (OSCs) strongly influences device performance by impacting light absorption, charge transport, and recombination. We demonstrate that ellagic acid (EA), a naturally derived templating layer, induces substantial morphological and thus optoelectronic changes in the vacuum thermally evaporated (VTE) donor molecule DCV5T-Me(3,3). Using in situ grazing incidence wide-angle X-ray scattering (GIWAXS) during thin film deposition in the purpose-built MINERVA VTE chamber at Diamond Light Source, we show that a 5 nm EA layer reorients DCV5T-Me from an edge-on to a face-on molecular packing motif. This templating effect persists for up to around 90 nm of film thickness. Through UV–Vis spectrophotometry and photoluminescence (PL) spectroscopy, we observe a shift towards H-aggregation and decreased light absorption in the donor molecule with the EA template. Atomic force microscopy (AFM) shows that the donor morphology changes as a function of thickness from the donor-templating interface. In DCV5T-Me(3,3):C60 bulk heterojunction devices, the EA layer helps retain donor crystallinity and enhances short circuit current (J S C ), despite the lower absorption. Maximum power conversion efficiency in our devices is achieved with a 5 nm templating layer, which provides sufficient structural templating while maintaining partial interfacial contact for efficient charge extraction. We hypothesize that the improvement in J S C is likely driven by enhanced charge carrier dynamics due to the orientation change, shift towards H-aggregation, and change in growth mode.

Abstract:

Abstract Vacuum-deposited organic solar cells (OSCs) have lagged behind their solution-processed counterparts in achieving high power conversion efficiency (PCE), in particular as result of higher voltage losses. In this study, we demonstrate a bulk heterojunction OSC using SubNc as donor and DCV3T as non-fullerene acceptor, achieving a PCE of 2.6% and a remarkably low total voltage loss of 0.64 V, lower than the typical values exceeding 0.7 V observed in vacuum thermally evaporated fullerene-based systems. The device also exhibits non-radiative voltage losses comparable to leading non-fullerene-acceptor (NFA) based OSCs. Transient absorption spectroscopy confirms efficient Förster resonance energy transfer from DCV3T to SubNc, followed by electron transfer for exciton separation. Morphological Grazing Incidence Wide-Angle X-ray Scattering features suggest both blends have a preferential edge-on orientation of DCV3T molecules, and the blends with higher DCV3T content could suffer from suppressed out-of-plane lamellar crystallinity with possible connection with greater non-radiative losses. Our findings demonstrate the potential of designing low-voltage-loss evaporated OSCs by building on strategies from solution-processed NFA systems, while highlighting the continued need for new evaporable acceptors with optimised optoelectronic and morphological properties.

Abstract:

Graphene nanoribbons (GNRs) combine the remarkable optical and electronic properties of graphene with the presence of a tunable band gap, making them promising for optoelectronic applications. Here, we investigate the excitonic properties of individual cove-edge GNRs through microphotoluminescence (micro-PL) spectroscopy. We observe ultranarrow emission lines with full width at half-maximum as low as 24 μeV, demonstrating a reduction of inhomogeneous broadening by 3 orders of magnitude compared to GNR ensembles. Temperature-dependent PL reveals phonon-mediated broadening mechanisms, with electron–phonon coupling parameters in agreement with ensemble studies but with dramatically reduced line widths. Time-resolved PL suggests long-lived excitonic states, while spectral diffusion analysis demonstrates stable emission energies, highlighting the exceptional quality of these GNRs as single-photon emitters. The absence of intensity blinking and low Mandel parameters further support the robustness of the emission properties. Our findings establish cove-edge GNRs as promising candidates for quantum light sources and nanoscale optoelectronic applications.

Abstract:

Vacuum-based deposition is a scalable, solvent-free industrial method ideal for uniform coatings on complex substrates. However, all vacuum-deposited perovskite solar cells fabricated by thermal evaporation trail solution-processed counterparts in efficiency and stability due to film quality challenges, necessitating advancement and improved understanding. Here, we report a co-evaporation route for 1.67-eV wide-bandgap perovskites by introducing a PbCl2 co-source to optimize film quality. We promote perovskite formation with pronounced (100) “face-up” orientation and deliver a certified all vacuum-deposited solar cell with 18.35% efficiency (19.3% in the lab) for 0.25-cm2 devices (18.5% for 1-cm2 cells). These cells retain 80% of peak efficiency after 1,080 hours under the ISOS-L-2 protocol. Leveraging operando hyperspectral imaging, we provide spatiotemporal spectral insight into halide segregation and trap-mediated recombination, correlating microscopic luminescence features with macroscopic device performance while distinguishing radiative from non-ideal recombination channels. We further demonstrate 27.2%-efficient 1-cm2 evaporated perovskite-on-silicon tandems and outdoor stability of all vacuum-deposited tandems in Italy, retaining ~80% initial performance after 8 months.