Organic copolymer lasing from single defect microcavity fabricated using laser patterning

Journal of Materials Chemistry C Materials for optical and electronic devices Royal Society of Chemistry 11:24 (2023) 8204-8213

Authors:

Peter Claronino, Rahul Jayaprakash, Till Jessewitsch, Rachel C Kilbride, Timothy Thornber, Alina Muravitskaya, Robert DJ Oliver, Ullrich Scherf, Jean-Sebastien G Bouillard, Ali M Adawi, David G Lidzey

Abstract:

Reducing the lasing threshold in optically pumped organic lasers is a necessary component of the drive to develop an organic laser diode, as this may help mitigate the losses associated with electrical contacts and charge injection. In this study we show how increasing the binaphthyl (BN) spacer content in polydioctylfluorene (PFO) decreases its amplified spontaneous emission threshold (ASE) through the suppression of intermolecular interactions. Using co-polymers with low lasing thresholds, we use a laser patterning technique to fabricate physical defects (having a diameter of ∼2.5 μm) within a vertical microcavity. Such defects create additional lateral confinement, with this approach allowing us to reduce the lasing threshold from 11 μJ cm−2 to 7 μJ cm−2 and increase cavity Q-factor from 495 (planar cavity) to 2300. The enhanced performance and the stack structure of the defect microcavity show it is a promising architecture for an electrically-pumped laser device

Intermediate-Phase Engineering via Dimethylammonium Cation Additive for Stable Perovskite Solar Cells

Institute of Electrical and Electronics Engineers (IEEE) 00 (2023) 1-1

Authors:

David P McMeekin, Philippe Holzhey, Sebastian O Fürer, Steven P Harvey, Laura T Schelhas, James M Ball, Suhas Mahesh, Seongrok Seo, Nicholas Hawkins, Jianfeng Lu, Michael B Johnston, Joseph J Berry, Udo Bach, Henry J Snaith

Photovoltaic performance of FAPbI3 perovskite is hampered by intrinsic quantum confinement

ACS Energy Letters American Chemical Society 8:6 (2023) 2543-2551

Authors:

Karim A Elmestekawy, Benjamin M Gallant, Adam D Wright, Philippe Holzhey, Nakita K Noel, Michael B Johnston, Henry J Snaith, Laura M Herz

Abstract:

Formamidinium lead trioiodide (FAPbI3) is a promising perovskite for single-junction solar cells. However, FAPbI3 is metastable at room temperature and can cause intrinsic quantum confinement effects apparent through a series of above-bandgap absorption peaks. Here, we explore three common solution-based film-fabrication methods, neat N,N-dimethylformamide (DMF)–dimethyl sulfoxide (DMSO) solvent, DMF-DMSO with methylammonium chloride, and a sequential deposition approach. The latter two offer enhanced nucleation and crystallization control and suppress such quantum confinement effects. We show that elimination of these absorption features yields increased power conversion efficiencies (PCEs) and short-circuit currents, suggesting that quantum confinement hinders charge extraction. A meta-analysis of literature reports, covering 244 articles and 825 photovoltaic devices incorporating FAPbI3 films corroborates our findings, indicating that PCEs rarely exceed a 20% threshold when such absorption features are present. Accordingly, ensuring the absence of these absorption features should be the first assessment when designing fabrication approaches for high-efficiency FAPbI3 solar cells.

Exciton formation dynamics and band-like free charge-carrier transport in 2D metal halide perovskite semiconductors

Advanced Functional Materials Wiley 33:32 (2023) 2300363

Authors:

Silvia G Motti, Manuel Kober-Czerny, Marcello Righetto, Philippe Holzhey, Joel Smith, Hans Kraus, Henry J Snaith, Michael B Johnston, Laura M Herz

Abstract:

Metal halide perovskite (MHP) semiconductors have driven a revolution in optoelectronic technologies over the last decade, in particular for high-efficiency photovoltaic applications. Low-dimensional MHPs presenting electronic confinement have promising additional prospects in light emission and quantum technologies. However, the optimisation of such applications requires a comprehensive understanding of the nature of charge carriers and their transport mechanisms. This study employs a combination of ultrafast optical and terahertz spectroscopy to investigate phonon energies, charge-carrier mobilities, and exciton formation in 2D (PEA)2PbI4 and (BA)2PbI4 (where PEA is phenylethylammonium and BA is butylammonium). Temperature-dependent measurements of free charge-carrier mobilities reveal band transport in these strongly confined semiconductors, with surprisingly high in-plane mobilities. Enhanced charge-phonon coupling is shown to reduce charge-carrier mobilities in (BA)2PbI4 with respect to (PEA)2PbI4. Exciton and free charge-carrier dynamics are disentangled by simultaneous monitoring of transient absorption and THz photoconductivity. A sustained free charge-carrier population is observed, surpassing the Saha equation predictions even at low temperature. These findings provide new insights into the temperature-dependent interplay of exciton and free-carrier populations in 2D MHPs. Furthermore, such sustained free charge-carrier population and high mobilities demonstrate the potential of these semiconductors for applications such as solar cells, transistors, and electrically driven light sources.

The 2023 terahertz science and technology roadmap

Journal of Physics D: Applied Physics IOP Publishing 56:22 (2023) 223001

Authors:

Alfred Leitenstorfer, Andrey S Moskalenko, Tobias Kampfrath, Junichiro Kono, Enrique Castro-Camus, Kun Peng, Naser Qureshi, Dmitry Turchinovich, Koichiro Tanaka, Andrea G Markelz, Martina Havenith, Cameron Hough, Hannah J Joyce, Willie J Padilla, Binbin Zhou, Ki-Yong Kim, Xi-Cheng Zhang, Peter Uhd Jepsen, Sukhdeep Dhillon, Miriam Vitiello, Edmund Linfield, A Giles Davies, Matthias C Hoffmann, Roger Lewis, Masayoshi Tonouchi, Pernille Klarskov, Tom S Seifert, Yaroslav A Gerasimenko, Dragan Mihailovic, Rupert Huber, Jessica L Boland, Oleg Mitrofanov, Paul Dean, Brian N Ellison, Peter G Huggard, Simon P Rea, Christopher Walker, David T Leisawitz, Jian Rong Gao, Chong Li, Qin Chen, Gintaras Valusis, Vincent P Wallace, Emma Pickwell-MacPherson, Xiaobang Shang, Jeffrey Hesler, Nick Ridler, Cyril C Renaud, Ingmar Kallfass, Michael B Johnston

Abstract:

Terahertz (THz) radiation encompasses a wide spectral range within the electromagnetic spectrum that extends from microwaves to the far infrared (100 GHz-∼30 THz). Within its frequency boundaries exist a broad variety of scientific disciplines that have presented, and continue to present, technical challenges to researchers. During the past 50 years, for instance, the demands of the scientific community have substantially evolved and with a need for advanced instrumentation to support radio astronomy, Earth observation, weather forecasting, security imaging, telecommunications, non-destructive device testing and much more. Furthermore, applications have required an emergence of technology from the laboratory environment to production-scale supply and in-the-field deployments ranging from harsh ground-based locations to deep space. In addressing these requirements, the research and development community has advanced related technology and bridged the transition between electronics and photonics that high frequency operation demands. The multidisciplinary nature of THz work was our stimulus for creating the 2017 THz Science and Technology Roadmap (Dhillon et al 2017 J. Phys. D: Appl. Phys. 50 043001). As one might envisage, though, there remains much to explore both scientifically and technically and the field has continued to develop and expand rapidly. It is timely, therefore, to revise our previous roadmap and in this 2023 version we both provide an update on key developments in established technical areas that have important scientific and public benefit, and highlight new and emerging areas that show particular promise. The developments that we describe thus span from fundamental scientific research, such as THz astronomy and the emergent area of THz quantum optics, to highly applied and commercially and societally impactful subjects that include 6G THz communications, medical imaging, and climate monitoring and prediction. Our Roadmap vision draws upon the expertise and perspective of multiple international specialists that together provide an overview of past developments and the likely challenges facing the field of THz science and technology in future decades. The document is written in a form that is accessible to policy makers who wish to gain an overview of the current state of the THz art, and for the non-specialist and curious who wish to understand available technology and challenges. A such, our experts deliver a ‘snapshot’ introduction to the current status of the field and provide suggestions for exciting future technical development directions. Ultimately, we intend the Roadmap to portray the advantages and benefits of the THz domain and to stimulate further exploration of the field in support of scientific research and commercial realisation.