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1. Multi-Stage Phase-Segregation of Mixed Halide Perovskites under Illumination: A Quantitative Comparison of Experimental Observations and Thermodynamic Models

Author

Suchan, Klara, Just, Justus, Becker, Pascal, Rehermann, Carolin, Merdasa, Aboma, Mainz, Roland, Scheblykin, Ivan G., and Unger, Eva

Subjects
Condensed Matter - Materials Science, Physics - Applied Physics
Abstract

Photo- and charge-carrier induced ion migration is a major challenge when utilizing metal halide perovskite semiconductors for optoelectronic applications. For mixed iodide/bromide perovskites, the compositional instability due to light- or electrical bias induced phase- segregation restricts the exploitation of the entire bandgap range. Previous experimental and theoretical work suggests that excited states or charge-carriers trigger the process but the exact mechanism is still under debate. To identify the mechanism and cause of light-induced phase-segregation phenomena we investigate the full compositional range of methylammonium lead bromide/iodide samples, MAPb(Br$_x$I$_{1-x}$)$_3$ with $x = 0\ldots 1$, by simultaneous in-situ X-ray diffraction and photoluminescence spectroscopy during illumination. The quantitative comparison of composition-dependent in-situ XRD and PL shows that at excitation densities of 1 sun, only the initial stage of photo-segregation can be rationalized with the previously established thermodynamic models. However, we observe a progression of the phase-segregation that can only be rationalized by considering long-lived accumulative photo-induced material alterations. We suggest that (additional) photo-induced defects, possibly halide vacancies and interstitials, need to be considered to fully rationalize light-induced phase-segregation and anticipate our findings to provide crucial insight for the development of more sophisticated models.

Published
2022

2. Broad Distribution of Local I/Br Ratio in Illuminated Mixed Halide Perovskite Films Revealed by Correlative X-ray Diffraction and Photoluminescence

Author

Suchan, Klara, Just, Justus, Becker, Pascal, Rehermann, Carolin, Merdasa, Aboma, Mainz, Roland, Scheblykin, Ivan G., and Unger, Eva L.

Subjects
Condensed Matter - Materials Science, Physics - Chemical Physics
Abstract

Photo-induced phase-segregation in mixed halide perovskite MAPb(BrxI1-x)3 is investigated in the full compositional range by correlative X-ray diffraction and photo-luminescence experiments., Comment: 18 pages, 4 figures + Supporting Information

Published
2021

3. Influence of molecular structure on the antimicrobial function of phenylenevinylene conjugated oligoelectrolytes.

Author

Yan, Hengjing, Rengert, Zachary D, Thomas, Alexander W, Rehermann, Carolin, Hinks, Jamie, and Bazan, Guillermo C

Subjects
Antimicrobial Resistance, Infectious Diseases, Vaccine Related, Prevention, Biodefense, Emerging Infectious Diseases, Generic health relevance, Chemical Sciences
Abstract

Conjugated oligoelectrolytes (COEs) with phenylenevinylene (PV) repeat units are known to spontaneously intercalate into cell membranes. Twelve COEs, including seven structures reported here for the first time, were investigated for the relationship between their membrane disrupting properties and structural modifications, including the length of the PV backbone and the presence of either a tetraalkylammonium or a pyridinium ionic pendant group. Optical characteristics and interactions with cell membranes were determined using UV-Vis absorption and photoluminescence spectroscopies, and confocal microscopy. Toxicity tests on representative Gram-positive (Enterococcus faecalis) and Gram-negative (Escherichia coli) bacteria reveal generally greater toxicity to E. faecalis than to E. coli and indicate that shorter molecules have superior antimicrobial activity. Increased antimicrobial potency was observed in three-ring COEs appended with pyridinium ionic groups but not with COEs with four or five PV repeat units. Studies with mutants having cell envelope modifications indicate a possible charge based interaction with pyridinium-appended compounds. Fluorine substitutions on COE backbones result in structures that are less toxic to E. coli, while the addition of benzothiadiazole to COE backbones has no effect on increasing antimicrobial function. A weakly membrane-intercalating COE with only two PV repeat units allowed us to determine the synthetic limitations as a result of competition between solubility in aqueous media and association with cell membranes. We describe, for the first time, the most membrane disrupting structure achievable within two homologous series of COEs and that around a critical three-ring backbone length, structural modifications have the most effect on antimicrobial activity.

Published
2016

4. An open-access database and analysis tool for perovskite solar cells based on the FAIR data principles

Author

Jacobsson, T. Jesper, Hultqvist, Adam, García-Fernández, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, González, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martínez-Denegri, Guillermo, Näsström, Hampus, Michaels, Hannes, Köbler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jerónimo-Rendón, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, Junxin, Sveinbjörnsson, Kári, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud. H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark V., Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schröder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, Unger, Eva, Jacobsson, T. Jesper, Hultqvist, Adam, García-Fernández, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, González, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martínez-Denegri, Guillermo, Näsström, Hampus, Michaels, Hannes, Köbler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jerónimo-Rendón, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, Junxin, Sveinbjörnsson, Kári, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud. H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark V., Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schröder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, and Unger, Eva

Abstract

Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.

Published
2022

5. An open-access database and analysis tool for perovskite solar cells based on the FAIR data principles

Author

Jacobsson, Jesper, Hultqvist, Adam, Garcia-Fernandez, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, Gonzalez, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martinez-Denegri, Guillermo, Nasstrom, Hampus, Michaels, Hannes, Kobler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jeronimo-Rendon, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, JunXin, Sveinbjornsson, Kari, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark, V, Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schroeder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, Unger, Eva, Jacobsson, Jesper, Hultqvist, Adam, Garcia-Fernandez, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, Gonzalez, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martinez-Denegri, Guillermo, Nasstrom, Hampus, Michaels, Hannes, Kobler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jeronimo-Rendon, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, JunXin, Sveinbjornsson, Kari, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark, V, Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schroeder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, and Unger, Eva

Abstract

Making large datasets findable, accessible, interoperable and reusable could accelerate technology development. Now, Jacobsson et al. present an approach to build an open-access database and analysis tool for perovskite solar cells. Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.

Published
2022
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6. Direct Probing of Gap States and Their Passivation in Halide Perovskites by High-Sensitivity, Variable Energy Ultraviolet Photoelectron Spectroscopy

Author

Igal, Levine, Kohei, Shimizu, Lomuscio, Alberto, Kulbak, Michael, Rehermann, Carolin, Zohar, Arava, Abdi-Jalebi, Mojtaba, Zhao, Baodan, Siebentritt, Susanne, Zu, Fengshuo, Koch, Norbert, Kahn, Antoine, Hodes, Gary, Friend, Richard H., Cahen, David, Igal, Levine, Kohei, Shimizu, Lomuscio, Alberto, Kulbak, Michael, Rehermann, Carolin, Zohar, Arava, Abdi-Jalebi, Mojtaba, Zhao, Baodan, Siebentritt, Susanne, Zu, Fengshuo, Koch, Norbert, Kahn, Antoine, Hodes, Gary, Friend, Richard H., and Cahen, David

Published
2022

7. Using Combinatorial Inkjet Printing for Synthesis and Deposition of Metal Halide Perovskites in Wavelength‐Selective Photodetectors

Author

Schröder, Vincent R. F., Hermerschmidt, Felix, Helper, Sabrina, Rehermann, Carolin, Ligorio, Giovanni, Näsström, Hampus, Unger, Eva, and List-Kratochvil, Emil J.W.

Subjects
halide variations, bandgap tunability, 540 Chemie und zugeordnete Wissenschaften, ddc:540, metal halide perovskites, combinatorial inkjet printing, wavelength-selective photodetectors
Abstract

Metal halide perovskites have received great attention in recent years, predominantly due to the high performance of perovskite solar cells. The versatility of the material, which allows the tunability of the bandgap, has led to its use in light-emitting diodes, photo, and X-ray detectors, among other optoelectronic device applications. Specifically in photodetectors, the tunability of the bandgap allows fabrication of spectrally selective devices. Utilizing a combinatorial inkjet printing approach, multiple perovskite compositions absorbing at specific wavelengths in a single printing step are fabricated. The drop-on-demand capabilities of inkjet printing enable the deposition of inks in a precise ratio to produce specific perovskite compositions in the printed thin film. By controlling the halide ratio in the compositions, a mixed halide gradient ranging from pure MAPbI3 via MAPbBr3 to MAPbCl3 is produced. The tunability in the absorption onset from 410 to 790 nm is demonstrated, covering the whole visible spectrum, with a precision of 8 nm steps for MAPb(BrxCl1−x)3 compositions. From this range of mixed halide perovskites, photodetectors which show spectral selectivity corresponding to the measured absorption onset are demonstrated, paving the way for use in a printed visible light spectrometer without the need for a dispersion element.

Published
2021

8. Exploring the Precursor-Process-Property Space in Metal Halide Perovskite Thin-Films

Author

Rehermann, Carolin, Unger, Eva, List-Kratochvil, Emil J. W., and Mathur, Sanjay

Subjects
Metall-Halogenid-Perovskit Dünnschichten, Formierungsstudien aus Lösung, in-situ spectroscopy, Metal halide perovskite thin-films, process optimization for high-quality thin-films, formation studies from solution, 541 Physikalische Chemie, ddc:541, In-situ Spektroskopie, Prozessoptimierung für hochqualitative Dünnschichten
Abstract

Die Anpassung der Bandlücke und die Herstellung mittels lösungsbasierter Prozesse charakterisieren Metallhalogenid-Perowskite. Sie sind vielversprechend für die Anwendung in optoelektronischen Bauteilen, die die Abscheidung von hochwertigen Dünnschichten erfordern. Deren Qualität hängt stark vom Kristallisationsverhalten ab, welches durch die Komposition der Lösung bestimmt ist. Ziel dieser Arbeit ist es, Korrelationen im Präkursor-Prozess-Eigenschaftsraum von Metallhalogenid-Perowskit zu bewerten und Formierungsprozesse zu rationalisieren. Phasenreinheit, Morphologie und Absorptionseigenschaften zeichnen die Qualität der Perowskit-Dünnschichten aus. Die Optimierung der Herstellung von hochwertigen Filmen über einen breiten Bandlückenbereich wird zuerst beleuchtet. Die Rationalisierung der Formierungsprozesse erweist sich als fundamental, um reproduzierbare Präparationsroutinen für hochwertige Filme zu entwickeln. Anschließend wird ein optischer in-situ Aufbau zur Rationalisierung von Formierungsprozessen vorgestellt. Abhängig vom Halogenidverhältnis in der MAPb(IxBr1-x)3-Reihe werden verschiedene Formierungswege eingeschlagen. Während sich das reine Bromid direkt und Iodid reiche Perowskite über die intermediäre Solvatphase (MA)2(DMSO)2Pb3I8 bilden, bilden sich gemischte Halogenide zwischen 0.1 ≤ x ≤ 0.6 über beide Wege. Die Formierung über konkurrierende Wege erklärt die kompositorische Heterogenität der gemischten Halogenidproben. Zuletzt werden Formierungsprozesse von Bromid-Perowskiten rationalisiert und Abhängigkeiten der Kinetik von der Lösungskonzentration zeigen sich. Niedrige Konzentrationen führen zu einer beschleunigten Kristallisation und Schichtdickenabnahme des Nassfilms. Dieser Trend wird durch geringere Kolloidwechselwirkungen und niedriger koordinierte Blei-Bromid-Komplexe in verdünnten Lösungen erklärt. Die Korrelation im Präkursor-Prozess-Eigenschaftsraum hebt die Herstellung von Perowskiten aus chemischer Sicht zu einem nicht-trivialen Prozess., Bandgap tunability by ion substitution and the fabrication due to solution-based processes characterize metal halide perovskites. They are promising for application in various thin-film opto-electronic devices, which require the deposition of high-quality thin-films. The quality strongly depends on the crystallization behavior predetermined by the precursors in solution. This thesis aims to evaluate correlations in the vast precursor-process-property space of metal halide perovskite and rationalizes formation processes. Phase purity, morphology, and absorption properties determine the perovskite thin-film quality. The first part focuses on optimizing the perovskite fabrication to obtain high-quality films over a wide bandgap range. From high-quality films, the exciton binding energy is determined. The rationalization of formation processes proves essential to design reproducible preparation routines for high-quality films. The second part presents an optical in-situ setup to rationalize perovskite formation processes. Different formation pathways are taken, depending on the halide ratio in the MAPb(IxBr1-x)3 series. While the pure bromide forms directly and iodide-rich perovskites form via the intermediate solvate phase (MA)2(DMSO)2Pb3I8, mixed halides between 0.1 ≤ x ≤ 0.6 form via both. Such a heterogeneous formation process via two competing pathways rationalizes the compositional heterogeneity of mixed halide samples. The third part focuses on rationalizing the formation process of pure bromide perovskites and reveals a dependency of the formation kinetics on the solution concentration. Lower concentrations lead to accelerated crystallization kinetics and increase wet-film thinning. Lower colloid interaction and lower coordinated lead-bromide complexes in diluted solutions explain this trend. The strong correlation in the precursor-process-property space raises the preparation of perovskites via spin-coating to a non-trivial process from a chemical point of view.

Published
2021

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