Enhancing photoluminescence yields in lead halide perovskites by photon recycling and light out-coupling

In lead halide perovskite solar cells, there is at least one recycling event of electron-hole pair to photon to electron-hole pair at open circuit under solar illumination. This can lead to a significant reduction in the external photoluminescence yield from the internal yield. Here we show that, for an internal yield of 70%, we measure external yields as low as 15% in planar films, where light out-coupling is inefficient, but observe values as high as 57% in films on textured substrates that enhance out-coupling. We analyse in detail how externally measured rate constants and photoluminescence efficiencies relate to internal recombination processes under photon recycling. For this, we study the photo-excited carrier dynamics and use a rate equation to relate radiative and non-radiative recombination events to measured photoluminescence efficiencies. We conclude that the use of textured active layers has the ability to improve power conversion efficiencies for both LEDs and solar cells.We acknowledge financial support from the Engineering and Physical Sciences Research Council of the U.K. (EPSRC). J.M.R. and M.T. thank the Winton Programme for the Physics of Sustainability (University of Cambridge). L.M.P.-O. thanks the Cambridge Home European Scheme for financial support. L.M.P.-O. and J.P.H.R. also thank the Nano Doctoral Training Center (NanoDTC) of the EPSRC for financial support. M.A.-J. thanks Nyak Technology Limited for a PhD scholarship. F.D. acknowledges funding from a Herchel Smith Research Fellowship

Photodoping through local charge carrier accumulation in alloyed hybrid perovskites for highly efficient luminescence

© 2019, The Author(s), under exclusive licence to Springer Nature Limited. Metal halide perovskites have emerged as exceptional semiconductors for optoelectronic applications. Substitution of the monovalent cations has advanced luminescence yields and device efficiencies. Here, we control the cation alloying to enhance optoelectronic performance through alteration of the charge carrier dynamics in mixed-halide perovskites. In contrast to single-halide perovskites, we find high luminescence yields for photoexcited carrier densities far below solar illumination conditions. Using time-resolved spectroscopy we show that the charge carrier recombination regime changes from second to first order within the first tens of nanoseconds after excitation. Supported by microscale mapping of the optical bandgap, electrically gated transport measurements and first-principles calculations, we demonstrate that spatially varying energetic disorder in the electronic states causes local charge accumulation, creating p- and n-type photodoped regions, which unearths a strategy for efficient light emission at low charge-injection in solar cells and light-emitting diodes.S.F. acknowledges funding from the Studienstiftung des deutschen Volkes and EPSRC, as well as support from the Winton Programme for the Physics of Sustainability. S.M. acknowledges funding from an EPSRC studentship. M.A.-J. thanks Nava Technology Limited, Cambridge Materials Limited and EPSRC (grant number: EP/M005143/1) for their funding and technical support. S.P.S. acknowledges funding from the Royal Society Newton Fellowship and EPSRC through a program grant (EP/M005143/1). T.A.S.D. acknowledges the National University of Ireland (NUI) for a Travelling Studentship and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (HYPERION, grant agreement number 756962). K.F. acknowledges funding from a George and Lilian Schiff Foundation Studentship, an EPSRC studentship and a scholarship from the Winton Programme for the Physics of Sustainability. E.R. acknowledges funding from an ERC starting grant (no. 804523). R.H.F. acknowledges support from the Simons Foundation (grant 601946). Research work in Mons was supported by the Fonds de la Recherche Scientifique de Belgique - Fund for Scientific Research (F.R.S.-FNRS) and the EU Marie-Curie IEF project ‘DAEMON’. Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI). D.B. is an FNRS Research Director. S.D.S. acknowledges the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (HYPERION, grant agreement number 756962), the Royal Society and Tata Group (UF150033). F.D. acknowledges funding from the Winton Programme for the Physics of Sustainability

High-performance light-emitting diodes based on carbene-metal-amides

Organic light-emitting diodes (OLEDs) promise highly efficient lighting and display technologies. We introduce a new class of linear donor-bridge-acceptor light-emitting molecules, which enable solution-processed OLEDs with near-100% internal quantum efficiency at high brightness. Key to this performance is their rapid and efficient utilization of triplet states. Using time-resolved spectroscopy, we establish that luminescence via triplets occurs within 350 nanoseconds at ambient temperature, after reverse intersystem crossing to singlets. We find that molecular geometries exist at which the singlet-triplet energy gap (exchange energy) is close to zero, so that rapid interconversion is possible. Calculations indicate that exchange energy is tuned by relative rotation of the donor and acceptor moieties about the bridge. Unlike other systems with low exchange energy, substantial oscillator strength is sustained at the singlet-triplet degeneracy point.D.D. and R.H.F. acknowledge support from the Department of Physics (Cambridge) and the King Abdulaziz City for Science and Technology–Cambridge University Joint Centre of Excellence. L.Y. thanks the Singapore Agency for Science, Technology and Research (A*STAR) for a Ph.D. studentship. J.M.R. acknowledges support from the Winton Program for the Physics of Sustainability. J.P.H.R. acknowledges the Cambridge NanoDTC (grant EP/L015978/1). M.L. acknowledges support by the Academy of Finland (project 251448). The computations were made possible by use of the Finnish Grid and Cloud Infrastructure. This work was supported by the Engineering and Physical Sciences Research Council (grant no. EP/M005143/1) and the European Research Council (ERC). M.B. is an ERC Advanced Investigator Award holder (grant no. 338944-GOCAT). D.C. and S.J. acknowledge support from the Royal Society (grant nos. UF130278 and RG140472)

Research data supporting: Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics

Experimental dat

Research data supporting: Long-lived polarization memory in the electronic states of lead-halide perovskites from local structural dynamics

Experimental dat

Research data supporting "High-performance light-emitting diodes based on carbene-metal-amides"

This dataset includes the experimental results of optical spectroscopy (cryogenic transient photoluminescence, transient absorption, ultrafast transient photoluminescence, transient electroluminescence, steady-state emission/absorption and Raman), OLED device characterization, electrochemistry, as well as data associated with quantum chemical (DFT) calculations

Photodoping through local charge carrier accumulation in alloyed hybrid perovskites for highly efficient luminescence

© 2019, The Author(s), under exclusive licence to Springer Nature Limited. Metal halide perovskites have emerged as exceptional semiconductors for optoelectronic applications. Substitution of the monovalent cations has advanced luminescence yields and device efficiencies. Here, we control the cation alloying to enhance optoelectronic performance through alteration of the charge carrier dynamics in mixed-halide perovskites. In contrast to single-halide perovskites, we find high luminescence yields for photoexcited carrier densities far below solar illumination conditions. Using time-resolved spectroscopy we show that the charge carrier recombination regime changes from second to first order within the first tens of nanoseconds after excitation. Supported by microscale mapping of the optical bandgap, electrically gated transport measurements and first-principles calculations, we demonstrate that spatially varying energetic disorder in the electronic states causes local charge accumulation, creating p- and n-type photodoped regions, which unearths a strategy for efficient light emission at low charge-injection in solar cells and light-emitting diodes