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Article: Spatio-Temporal Dynamics of Free and Bound Carriers in Photovoltaic Materials.

Fish, George / Moser, Jacques-E

2022 Volume 76, Issue 6, Page(s) 552–557

Abstract: Charge transfer and subsequent separation into free carriers are key processes that govern the efficiencies of third generation solar cell technologies based on donor-acceptor heterojunctions. As these processes typically occur on picosecond to ... ...

Abstract	Charge transfer and subsequent separation into free carriers are key processes that govern the efficiencies of third generation solar cell technologies based on donor-acceptor heterojunctions. As these processes typically occur on picosecond to femtosecond timescales, it is necessary to employ ultrafast spectroscopic techniques to further our understanding of these processes in order to provide vital information that can aide in furthering material design. Within the framework of the National Centre of Competence in Research "Molecular Ultrafast Science and Technology" (NCCR MUST), we have developed and utilized a suite of different ultrafast spectroscopic techniques to study charge generation, separation and recombination in a variety of small molecule based organic solar cells and lead halide perovskites. Here, we provide an overview of the main techniques used in our laboratory and the recent results obtained using these spectroscopic techniques.
Language	English
Publishing date	2022-06-29
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	1516-7
ISSN	0009-4293
ISSN	0009-4293
DOI	10.2533/chimia.2022.552
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Perovskite photovoltaics: Slow recombination unveiled.

Moser, Jacques-E

Nature materials

2016 Volume 16, Issue 1, Page(s) 4–6

Language	English
Publishing date	2016-12-20
Publishing country	England
Document type	Journal Article
ZDB-ID	2088679-2
ISSN	1476-4660 ; 1476-1122
ISSN (online)	1476-4660
ISSN	1476-1122
DOI	10.1038/nmat4796
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Photogenerated charge transfer in Dion-Jacobson type layered perovskite based on naphthalene diimide.

Nussbaum, Simon / Socie, Etienne / Fish, George C / Diercks, Nicolas J / Hempel, Hannes / Friedrich, Dennis / Moser, Jacques-E / Yum, Jun-Ho / Sivula, Kevin

Chemical science

2023 Volume 14, Issue 22, Page(s) 6052–6058

Abstract: Incorporating organic semiconducting spacer cations into layered lead halide perovskite structures provides a powerful approach to mitigate the typical strong dielectric and quantum confinement effects by inducing charge-transfer between the organic and ... ...

Abstract	Incorporating organic semiconducting spacer cations into layered lead halide perovskite structures provides a powerful approach to mitigate the typical strong dielectric and quantum confinement effects by inducing charge-transfer between the organic and inorganic layers. Herein we report the synthesis and characterization of thin films of novel DJ-phase organic-inorganic layered perovskite semiconductors using a naphthalene diimide (NDI) based divalent spacer cation, which is shown to accept photogenerated electrons from the inorganic layer. With alkyl chain lengths of 6 carbons, an NDI-based thin film exhibited electron mobility (based on space charge-limited current for quasi-layered 〈
Language	English
Publishing date	2023-05-15
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/d3sc00783a
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Tailoring p-Type Behavior in ZnO Quantum Dots through Enhanced Sol-Gel Synthesis: Mechanistic Insights into Zinc Vacancies.

Kahraman, Abdullah / Socie, Etienne / Nazari, Maryam / Kazazis, Dimitrios / Buldu-Akturk, Merve / Kabanova, Victoria / Biasin, Elisa / Smolentsev, Grigory / Grolimund, Daniel / Erdem, Emre / Moser, Jacques E / Cannizzo, Andrea / Bacellar, Camila / Milne, Christopher

The journal of physical chemistry letters

2024 Volume 15, Issue 6, Page(s) 1755–1764

Abstract: The synthesis and control of properties of p-type ZnO is crucial for a variety of optoelectronic and spintronic applications; however, it remains challenging due to the control of intrinsic midgap (defect) states. In this study, we demonstrate a ... ...

Abstract	The synthesis and control of properties of p-type ZnO is crucial for a variety of optoelectronic and spintronic applications; however, it remains challenging due to the control of intrinsic midgap (defect) states. In this study, we demonstrate a synthetic route to yield colloidal ZnO quantum dots (QD) via an enhanced sol-gel process that effectively eliminates the residual intermediate reaction molecules, which would otherwise weaken the excitonic emission. This process supports the creation of ZnO with p-type properties or compensation of inherited n-type defects, primarily due to zinc vacancies under oxygen-rich conditions. The in-depth analysis of carrier recombination in the midgap across several time scales reveals microsecond carrier lifetimes at room temperature which are expected to occur via zinc vacancy defects, supporting the promoted p-type character of the synthesized ZnO QDs.
Language	English
Publishing date	2024-02-07
Publishing country	United States
Document type	Journal Article
ISSN	1948-7185
ISSN (online)	1948-7185
DOI	10.1021/acs.jpclett.3c03519
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Article: Resonant Band-Edge Emissive States in Strongly Confined CsPbBr₃ Perovskite Nanoplatelets

Socie, Etienne / Vale, Brener R. C. / Terpstra, Aaron T. / Schiavon, Marco A. / Moser, Jacques-E.

Journal of physical chemistry. 2021 June 27, v. 125, no. 26

2021

Abstract: Strongly confined, fully inorganic cesium lead halide perovskite nanocrystals are of great promise for light-emitting devices in the blue spectral range owing to their high photoluminescence quantum yields. A combination of broadband fluorescence up- ... ...

Abstract	Strongly confined, fully inorganic cesium lead halide perovskite nanocrystals are of great promise for light-emitting devices in the blue spectral range owing to their high photoluminescence quantum yields. A combination of broadband fluorescence up-conversion and transient absorption spectroscopies was used to study early exciton dynamics in quasi-1D CsPbBr₃ nanoplatelets (3 × 4 × 23 nm³, NPls). This allowed to reveal emitting band-edge states in the NPls that form instantaneously upon photoexcitation and then relax within the first picosecond to lower energy confined hole states (CHSs). The influence of the pump excitation intensity on the latter process was further scrutinized. The band-edge population lifetime was found to increase with the rise of the photon fluence due to CHS filling. When the concentration of NPls in solution becomes very high, nanoparticles overlap, resulting in a decrease in their external absorption cross-section and an increase in the emission Stokes shift due to photon reabsorption.
Keywords	absorption ; cesium ; energy ; fluorescence ; lead ; nanocrystals ; photochemical reactions ; photoluminescence ; photons ; resorption
Language	English
Dates of publication	2021-0627
Size	p. 14317-14325.
Publishing place	American Chemical Society
Document type	Article
ISSN	1932-7455
DOI	10.1021/acs.jpcc.1c01353
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Exciton and Carrier Dynamics in Two-Dimensional Perovskites.

Burgos-Caminal, Andrés / Socie, Etienne / Bouduban, Marine E F / Moser, Jacques-E

The journal of physical chemistry letters

2020 Volume 11, Issue 18, Page(s) 7692–7701

Abstract: Two-dimensional Ruddlesden-Popper hybrid lead halide perovskites have become a major topic in perovskite optoelectronics. Here, we aim to unravel the ultrafast dynamics governing the evolution of charge carriers and excitons in these materials. Using a ... ...

Abstract	Two-dimensional Ruddlesden-Popper hybrid lead halide perovskites have become a major topic in perovskite optoelectronics. Here, we aim to unravel the ultrafast dynamics governing the evolution of charge carriers and excitons in these materials. Using a combination of ultrabroadband time-resolved THz (TRTS) and fluorescence upconversion spectroscopies, we find that sequential carrier cooling and exciton formation best explain the observed dynamics, while exciton-exciton interactions play an important role in the form of Auger heating and biexciton formation. We show that the presence of a longer-lived population of carriers is due to the latter processes and not to a Mott transition. Therefore, excitons still dominate at laser excitation densities. We use kinetic modeling to compare the phenethylammonium and butylammonium organic cations while investigating the stability of the resulting films. In addition, we demonstrate the capability of using ultrabroadband TRTS to study excitons in large binding energy semiconductors through spectral analysis at room temperature.
Language	English
Publishing date	2020-08-31
Publishing country	United States
Document type	Journal Article
ISSN	1948-7185
ISSN (online)	1948-7185
DOI	10.1021/acs.jpclett.0c02425
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Article ; Online: The Impact of Spacer Size on Charge Transfer Excitons in Dion-Jacobson and Ruddlesden-Popper Layered Hybrid Perovskites.

Fish, George C / Terpstra, Aaron T / Dučinskas, Algirdas / Almalki, Masaud / Carbone, Loï C / Pfeifer, Lukas / Grätzel, Michael / Moser, Jacques-E / Milić, Jovana V

The journal of physical chemistry letters

2023 Volume 14, Issue 27, Page(s) 6248–6254

Abstract: Organic materials can tune the optical properties in layered (2D) hybrid perovskites, although their impact on photophysics is often overlooked. Here, we use transient absorption spectroscopy to probe the Dion-Jacobson (DJ) and Ruddlesden-Popper (RP) 2D ... ...

Abstract	Organic materials can tune the optical properties in layered (2D) hybrid perovskites, although their impact on photophysics is often overlooked. Here, we use transient absorption spectroscopy to probe the Dion-Jacobson (DJ) and Ruddlesden-Popper (RP) 2D perovskite phases. We show the formation of charge transfer excitons in DJ phases, resulting in a photoinduced Stark effect which is shown to be dependent on the spacer size. By using electroabsorption spectroscopy, we quantify the strength of the photoinduced electric field, while temperature-dependent measurements demonstrate new features in the transient spectra of RP phases at low temperatures resulting from the quantum-confined Stark effect. This study reveals the impact of spacer size and perovskite phase configuration on charge transfer excitons in 2D perovskites of interest to their advanced material design.
Language	English
Publishing date	2023-06-30
Publishing country	United States
Document type	Journal Article
ISSN	1948-7185
ISSN (online)	1948-7185
DOI	10.1021/acs.jpclett.3c01125
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Article ; Online: Critical role of H-aggregation for high-efficiency photoinduced charge generation in pristine pentamethine cyanine salts.

Fish, George C / Moreno-Naranjo, Juan Manuel / Billion, Andreas / Kratzert, Daniel / Hack, Erwin / Krossing, Ingo / Nüesch, Frank / Moser, Jacques-E

Physical chemistry chemical physics : PCCP

2021 Volume 23, Issue 41, Page(s) 23886–23895

Abstract: The mechanism of photoinduced symmetry-breaking charge separation in solid cyanine salts at the base of organic photovoltaic and optoelectronic devices is still debated. Here, we employ femtosecond transient absorption spectroscopy (TAS) to monitor the ... ...

Abstract	The mechanism of photoinduced symmetry-breaking charge separation in solid cyanine salts at the base of organic photovoltaic and optoelectronic devices is still debated. Here, we employ femtosecond transient absorption spectroscopy (TAS) to monitor the charge transfer processes occurring in thin films of pristine pentamethine cyanine (Cy5). Oxidized dye species are observed in Cy5-hexafluorophosphate salts upon photoexcitation, resulting from electron transfer from monomer excited states to H-aggregates. The charge separation proceeds with a quantum yield of 86%, providing the first direct proof of high efficiency intrinsic charge generation in organic salt semiconductors. The impact of the size of weakly coordinating anions on charge separation and transport is studied using TAS alongside electroabsorption spectroscopy and time-of-flight techniques. The degree of H-aggregation decreases with increasing anion size, resulting in reduced charge transfer. However, there is little change in carrier mobility, as despite the interchromophore distance increasing, the decrease in energetic disorder helps to alleviate the trapping of charges by H-aggregates.
Language	English
Publishing date	2021-10-27
Publishing country	England
Document type	Journal Article
ZDB-ID	1476244-4
ISSN	1463-9084 ; 1463-9076
ISSN (online)	1463-9084
ISSN	1463-9076
DOI	10.1039/d1cp03251h
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Article: Solar cells: later rather than sooner.

Moser, Jacques-E

Nature materials

2005 Volume 4, Issue 10, Page(s) 723–724

MeSH term(s)	Electric Power Supplies ; Electrochemistry/instrumentation ; Electrochemistry/methods ; Electrodes ; Equipment Design ; Equipment Failure Analysis ; Light ; Photochemistry/instrumentation ; Photochemistry/methods ; Solar Energy ; Titanium/chemistry ; Titanium/radiation effects
Chemical Substances	titanium dioxide (15FIX9V2JP) ; Titanium (D1JT611TNE)
Language	English
Publishing date	2005-10
Publishing country	England
Document type	News
ZDB-ID	2088679-2
ISSN	1476-4660 ; 1476-1122
ISSN (online)	1476-4660
ISSN	1476-1122
DOI	10.1038/nmat1504
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Revealing Exciton and Metal–Ligand Conduction Band Charge Transfer Absorption Spectra in Cu-Zn-In-S Nanocrystals

Vale, Brener R. C / Socie, Etienne / Cunha, Leticia R. C / Fonseca, Andre F. V / Vaz, Roberto / Bettini, Jefferson / Moser, Jacques-E / Schiavon, Marco A

Journal of physical chemistry. 2020 Dec. 02, v. 124, no. 50

2020

Abstract: Copper indium sulfide quantum dots (QDs) have attracted substantial attention in recent years due to environmental issues and diverse applications. We report the synthesis and characterization of copper-zinc-indium-sulfide (CZIS) QDs and CZIS treated ... ...

Abstract	Copper indium sulfide quantum dots (QDs) have attracted substantial attention in recent years due to environmental issues and diverse applications. We report the synthesis and characterization of copper-zinc-indium-sulfide (CZIS) QDs and CZIS treated with excess Zn²⁺ at different temperatures, denoted here as CZIS/ZnS 100 and CZIS/ZnS 200. Zn²⁺ can diffuse into the lattice by an exchange-cation reaction, replacing Cu⁺ and In³⁺. We employed transient absorption (TA) spectroscopy to study the role of Zn²⁺ in the lattice. The data were treated by global analysis, which yielded the decay-associated spectra (DAS). Through DAS and second-order derivative absorption spectra, we could for the first time isolate the excitonic contribution from the metal–ligand conduction band charge transfer (MLCBCT) absorption in the TA spectrum, finding the hole localization lifetime by its spectral and dynamical features. The hole localization lifetime increases from 0.3 to 1.7 ps by increasing the Zn²⁺ concentration. We also measured the electron-trapping constants to be dozens of picoseconds and nonradiative recombination larger than 1 ns. Finally, we concluded that suppression of the electron-trapping rate is not the only process responsible for increasing the photoluminescence quantum yield (PLQY); however, suppression of this process is important since it is the first step of the nonradiative recombination pathway. The detailed mechanism was proposed, and our results suggest that the introduction of Zn²⁺ in the lattice of copper indium sulfide (CIS) QDs could be beneficial for charge extraction.
Keywords	absorption ; indium ; nanocrystals ; photoluminescence ; spectroscopy
Language	English
Dates of publication	2020-1202
Size	p. 27858-27866.
Publishing place	American Chemical Society
Document type	Article
Note	NAL-AP-2-clean
ISSN	1932-7455
DOI	10.1021/acs.jpcc.0c09681
Database	NAL-Catalogue (AGRICOLA)

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