Publications by authors named "Sangmin Chae"

7 Publications

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Resolving Atomic-Scale Interactions in Non-Fullerene Acceptor Organic Solar Cells with Solid-State NMR Spectroscopy, Crystallographic Modelling, and Molecular Dynamics Simulations.

Adv Mater 2021 Nov 24:e2105943. Epub 2021 Nov 24.

University of Lille, CNRS, Centrale Lille Institut, Univ. Artois, UMR 8181, Unité de Catalyse et Chimie du Solide, Lille, F-59000, France.

Fused-ring core non-fullerene acceptors (NFAs), designated "Y-series", have enabled high-performance organic solar cells (OSCs) achieving over 18% power conversion efficiency (PCE). Since the introduction of these NFAs, much effort has been expended to understand the reasons for their exceptional performance. While several studies have identified key optoelectronic properties that govern high PCEs, little is known about the molecular level origins of large variations in performance, spanning from 5 to 18% PCE, e.g., in the case of PM6:Y6 OSCs. Here, we introduce a combined solid-state NMR, crystallography, and molecular modelling approach to elucidate the atomic-scale interactions in Y6 crystals, thin films, and PM6:Y6 bulk heterojunction (BHJ) blends. We show the Y6 morphologies in BHJ blends are not governed by the morphology in neat films or single crystals. Notably, PM6:Y6 blends processed from different solvents self-assemble into different structures and morphologies, whereby the relative orientations of the sidechains and end groups of the Y6 molecules to their fused-ring cores play a crucial role in determining the resulting morphology and overall performance of the solar cells. The molecular-level understanding of BHJs enabled by this approach will guide the engineering of next-generation NFAs for stable and efficient OSCs. This article is protected by copyright. All rights reserved.
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http://dx.doi.org/10.1002/adma.202105943DOI Listing
November 2021

Efficiency of Thermally Activated Delayed Fluorescence Sensitized Triplet Upconversion Doubled in Three-Component System.

Adv Mater 2021 Nov 18:e2103976. Epub 2021 Nov 18.

Center for Polymers and Organic Solids (CPOS) and Department of Chemistry & Biochemistry, University of California, Santa Barbara, CA-93106, USA.

As in many fields, the most exciting endeavors in photon upconversion research focus on increasing the efficiency (upconversion quantum yield) and performance (anti-Stokes shift) while diminishing the cost of production. In this vein, studies employing metal-free thermally activated delayed fluorescence (TADF) sensitizers have garnered increased interest. Here, for the first time, the strategy of ternary photon upconversion was utilized with the TADF sensitizer 4CzIPN, resulting in a doubling of the upconversion quantum yield in comparison to the binary system employing p-terphenyl as the emitter. In this ternary blend, the sensitizer 4CzIPN is paired with an intermediate acceptor, 1-methylnaphthalene, in addition to the emitter molecule, p-terphenyl yielding a normalized upconversion quantum yield of 7.6% while maintaining the 0.83 eV anti-Stokes shift. These results illustrate the potential benefits of utilizing this strategy of energy-funneling, previously used only with heavy-metal based sensitizers, to increase the performance of these photon upconversion systems. This article is protected by copyright. All rights reserved.
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http://dx.doi.org/10.1002/adma.202103976DOI Listing
November 2021

Femtosecond laser irradiation of molecular excitonic films for nanophotonic response control and large-area patterning.

Opt Express 2019 Jun;27(13):18044-18054

Molecular excitonic films such as J-aggregate thin films can show an optically metallic response in the visible region and can be considered as alternative materials for plasmonics. However, there was no direct, top-down method to modify the optical response over a large area. Here, we demonstrate the femtosecond (fs) laser processing of J-aggregate films on the centimeter scale. With proper laser conditions, optically metallic films (Re[ε] < 0) were modified to dielectric ones (Re[ε] > 0) with large changes in optical responses. We performed various optical spectrum measurements to investigate the effect of fs-laser irradiation. Our results demonstrate that the strong modification of the optical response can be induced over a large area by fs-laser processing and this can be useful for novel nanophotonic studies.
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http://dx.doi.org/10.1364/OE.27.018044DOI Listing
June 2019

Manipulating the crystal structure of a conjugated polymer for efficient sequentially processed organic solar cells.

Nanoscale 2018 Dec 14;10(45):21052-21061. Epub 2018 Sep 14.

Department of Organic Material Science and Engineering, Pusan National University, Busan 46241, South Korea.

Recently, the sequential (Sq) process, which forms nanoscale network structures from quasi-solid-state inter-diffusion through swelling and annealing, is considered to be one of the most efficient methods for fabricating organic solar cells and blend films. Here, we examined the effect of the crystallinity and orientation of poly(3-hexylthiophene) (P3HT) molecules on the formation of the nanostructure by carrying out a Sq process using various solvents with different boiling points. We showed that the moderate crystallinity promoted suitable inter-diffusion between the donor (P3HT) and acceptor ([6,6]-pentadeuterophenyl C61 butyric acid methyl ester, PCBM), and hence was important for achieving high-performance solar cells using Sq processing. Nanostructure formation by inter-diffusion was investigated and visualized by taking a combination of grazing-incidence wide-angle X-ray scattering (GIWAXS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) measurements. In addition, our Sq-processed solar cell yielded a device efficiency as high as 3.25%, and was also impressive because it was made with an eco-friendly solvent and using a short-duration annealing process, in contrast to the conventional BHJ process. The present findings provided advanced insight into the Sq process, and we anticipate this efficacious sequential process to contribute not only to the development of higher-efficiency organic solar cells but also to the fabrication of functional blend films.
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http://dx.doi.org/10.1039/c8nr05407jDOI Listing
December 2018

Control of Crystallinity in PbPc:C Blend Film and Application for Inverted Near-Infrared Organic Photodetector.

ACS Appl Mater Interfaces 2018 Aug 20;10(30):25614-25620. Epub 2018 Jul 20.

Department of Materials Science and Engineering, Research Institute of Advanced Materials , Seoul National University , Seoul 08826 , South Korea.

Inverted near-infrared (NIR) organic photodetectors (OPDs) are required to combine the OPDs with an n-channel silicon-based integrated circuit. NIR absorption in the 930-960 nm range is important because the intensity of solar irradiation is low in this wavelength regime. Here, we controlled the crystallinity of lead(II) phthalocyanine (PbPc) in a PbPc:C blend film to obtain NIR absorption. To form a triclinic phase responsible for NIR light absorption, a substrate was heated during fabrication and C was used as a templating layer, as well as an electron extraction layer, for an inverted structure. NIR absorption near 950 nm was enhanced, and the structural properties of the film changed dramatically. The OPD with enhanced NIR absorption exhibited a responsivity of 244 mA/W and an external quantum efficiency of 31.1% at a reverse bias of -3 V and 970 nm. The OPD detectivity also increased to 9.01 × 10 and 1.36 × 10 cm Hz/W under a zero bias and a reverse bias of -3 V, respectively.
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http://dx.doi.org/10.1021/acsami.8b08803DOI Listing
August 2018

Switchable ferroelectric photovoltaic effects in epitaxial h-RFeO thin films.

Nanoscale 2018 Jul;10(27):13261-13269

Department of Materials Science and Engineering, and Division of Advanced Materials Science, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea.

Ferroelectric photovoltaics (FPVs) have drawn much attention owing to their high stability, environmental safety, and anomalously high photovoltages, coupled with reversibly switchable photovoltaic responses. However, FPVs suffer from extremely low photocurrents, which is primarily due to their wide band gaps. Here, we present a new class of FPVs by demonstrating switchable ferroelectric photovoltaic effects and narrow band-gap properties using hexagonal ferrite (h-RFeO3) thin films, where R denotes rare-earth ions. FPVs with narrow band gaps suggest their potential applicability as photovoltaic and optoelectronic devices. The h-RFeO3 films further exhibit reasonably large ferroelectric polarizations (4.7-8.5 μC cm-2), which possibly reduces a rapid recombination rate of the photo-generated electron-hole pairs. The power conversion efficiency (PCE) of h-RFeO3 thin-film devices is sensitive to the magnitude of polarization. In the case of the h-TmFeO3 (h-TFO) thin film, the measured PCE is twice as large as that of the BiFeO3 thin film, a prototypic FPV. The effect of electrical fatigue on FPV responses has been further investigated. This work thus demonstrates a new class of FPVs towards high-efficiency solar cell and optoelectronic applications.
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http://dx.doi.org/10.1039/c7nr08666kDOI Listing
July 2018

Using Femtosecond Laser Irradiation to Enhance the Vertical Electrical Properties and Tailor the Morphology of a Conducting Polymer Blend Film.

ACS Appl Mater Interfaces 2017 Jul 12;9(29):24422-24427. Epub 2017 Jul 12.

Department of Organic Material Science and Engineering, Pusan National University , Busan 46241, South Korea.

We report femtosecond infrared laser-induced selective tailoring of carrier transport as well as surface morphology on a conducting polymer blend thin film. Maximal 2.4 times enhancement on vertical current transport in poly(3-hexylthiophene):phenyl-C61-butyric acid methyl ester, was achieved by this irradiation. The laser irradiation induced a photo expansion without deteriorating its molecular structure and the film morphology could be customized in the micron scale by adjusting the laser writing parameters. In the photoexpanded region, the face-on populations were about 2.2 times larger in comparison with the pristine region, which was a major contributor to the enhanced carrier transport.
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http://dx.doi.org/10.1021/acsami.7b05937DOI Listing
July 2017
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