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  1. Book ; Online: Efficient Thermal Transport across Molecular Chains in Hybrid 2D Lead Bromide Perovskites

    Dahod, Nabeel S. / Paritmongkol, Watcharaphol / Tisdale, William A.

    2023  

    Abstract: We report measurements of the heat capacity and cross-plane thermal conductivity of 2D (CxH2x+1NH3)2[MAPbBr3]n-1PbBr4 (MA = methylammonium) lead bromide perovskites (2D LHPs) at room temperature as a function of both the octahedral layer thickness (n = 1, ...

    Abstract We report measurements of the heat capacity and cross-plane thermal conductivity of 2D (CxH2x+1NH3)2[MAPbBr3]n-1PbBr4 (MA = methylammonium) lead bromide perovskites (2D LHPs) at room temperature as a function of both the octahedral layer thickness (n = 1,2,3) and the organic spacer chain length (x=4,5,6,7,8) using differential scanning calorimetry (DSC) and frequency domain thermoreflectance (FDTR) respectively. We observe ultralow thermal conductivities (0.18-0.51 W/m K) for all 2D LHPs studied, but surprisingly minimal suppression of thermal conductivity with respect to bulk MAPbBr3 (0.5 W/m K). Cross-plane thermal conductivity is found to increase monotonically as a function of both the octahedral layer thickness (0.18-0.26 W/m K for n=1-3) and the organic chain length (0.18-0.51 W/m K for x=4-8). Additionally, we measure heat capacities that are well described by composite theory, suggesting bulk-like phonon density-of-states within the separate organic and inorganic subphases of the layered structure. The striking observation of increasing thermal conductivity with increasing organic phase fraction (i.e. increasing organic chain length) indicates efficient thermal transport along the ordered alkyl chain backbone. Our experimental results agree most closely with a predictive model of ballistic phonon transport with diffuse interface scattering - rather than normal thermal conduction within each phase. This study indicates the potential for synthesizing 2D LHPs with thermal conductivity that exceeds the bulk perovskite phase, while also shedding light on relevant phonon transport pathways in 2D LHPs.
    Keywords Physics - Applied Physics ; Condensed Matter - Materials Science
    Publishing date 2023-03-30
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  2. Article: Size and Quality Enhancement of 2D Semiconducting Metal–Organic Chalcogenolates by Amine Addition

    Paritmongkol, Watcharaphol / Sakurada, Tomoaki / Lee, Woo Seok / Wan, Ruomeng / Müller, Peter / Tisdale, William A.

    Journal of the American Chemical Society. 2021 Nov. 21, v. 143, no. 48

    2021  

    Abstract: The use of two-dimensional (2D) materials in next-generation technologies is often limited by small lateral size and/or crystal defects. Here, we introduce a simple chemical strategy to improve the size and overall quality of 2D metal–organic ... ...

    Abstract The use of two-dimensional (2D) materials in next-generation technologies is often limited by small lateral size and/or crystal defects. Here, we introduce a simple chemical strategy to improve the size and overall quality of 2D metal–organic chalcogenolates (MOCs), a new class of hybrid organic–inorganic 2D semiconductors that can exhibit in-plane anisotropy and blue luminescence. By inducing the formation of silver–amine complexes during a solution growth method, we increase the average size of silver phenylselenolate (AgSePh) microcrystals from <5 μm to >1 mm, while simultaneously extending the photoluminescence lifetime and suppressing mid-gap emission. Mechanistic studies using ⁷⁷Se NMR suggest dual roles for the amine in promoting the formation of a key reactive intermediate and slowing down the final conversion to AgSePh. Finally, we show that amine addition is generalizable to the synthesis of other 2D MOCs, as demonstrated by the growth of single crystals of silver 4-methylphenylselenolate (AgSePhMe), a novel member of the 2D MOC family.
    Keywords anisotropy ; photoluminescence ; semiconductors ; silver
    Language English
    Dates of publication 2021-1121
    Size p. 20256-20263.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c09106
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  3. Article ; Online: Bright Excitonic Fine Structure in Metal-Halide Perovskites: From Two-Dimensional to Bulk.

    Posmyk, Katarzyna / Zawadzka, Natalia / Łucja Kipczak / Dyksik, Mateusz / Surrente, Alessandro / Maude, Duncan K / Kazimierczuk, Tomasz / Babiński, Adam / Molas, Maciej R / Bumrungsan, Wakul / Chooseng, Chanisara / Paritmongkol, Watcharaphol / Tisdale, William A / Baranowski, Michał / Plochocka, Paulina

    Journal of the American Chemical Society

    2024  Volume 146, Issue 7, Page(s) 4687–4694

    Abstract: The optical response of two-dimensional (2D) perovskites, often referred to as natural quantum wells, is primarily governed by excitons, whose properties can be readily tuned by adjusting the perovskite layer thickness. We have investigated the exciton ... ...

    Abstract The optical response of two-dimensional (2D) perovskites, often referred to as natural quantum wells, is primarily governed by excitons, whose properties can be readily tuned by adjusting the perovskite layer thickness. We have investigated the exciton fine structure splitting in the archetypal 2D perovskite (PEA)
    Language English
    Publishing date 2024-02-07
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.3c11957
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: Two Origins of Broadband Emission in Multilayered 2D Lead Iodide Perovskites.

    Paritmongkol, Watcharaphol / Powers, Eric R / Dahod, Nabeel S / Tisdale, William A

    The journal of physical chemistry letters

    2020  Volume 11, Issue 20, Page(s) 8565–8572

    Abstract: Broadband emission in lead iodide 2D perovskites has been alternately attributed to self-trapped excitons (STEs) or permanent structural defects and/or impurities. Here, we investigate six different multilayered ( ...

    Abstract Broadband emission in lead iodide 2D perovskites has been alternately attributed to self-trapped excitons (STEs) or permanent structural defects and/or impurities. Here, we investigate six different multilayered (
    Language English
    Publishing date 2020-09-25
    Publishing country United States
    Document type Journal Article
    ISSN 1948-7185
    ISSN (online) 1948-7185
    DOI 10.1021/acs.jpclett.0c02214
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Power-Dependent Photoluminescence Efficiency in Manganese-Doped 2D Hybrid Perovskite Nanoplatelets.

    Ha, Seung Kyun / Shcherbakov-Wu, Wenbi / Powers, Eric R / Paritmongkol, Watcharaphol / Tisdale, William A

    ACS nano

    2021  Volume 15, Issue 12, Page(s) 20527–20538

    Abstract: Substitutional metal doping is a powerful strategy for manipulating the emission spectra and excited state dynamics of semiconductor nanomaterials. Here, we demonstrate the synthesis of colloidal manganese ( ... ...

    Abstract Substitutional metal doping is a powerful strategy for manipulating the emission spectra and excited state dynamics of semiconductor nanomaterials. Here, we demonstrate the synthesis of colloidal manganese (Mn
    Language English
    Publishing date 2021-11-18
    Publishing country United States
    Document type Journal Article
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/acsnano.1c09103
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Size and Quality Enhancement of 2D Semiconducting Metal-Organic Chalcogenolates by Amine Addition.

    Paritmongkol, Watcharaphol / Sakurada, Tomoaki / Lee, Woo Seok / Wan, Ruomeng / Müller, Peter / Tisdale, William A

    Journal of the American Chemical Society

    2021  Volume 143, Issue 48, Page(s) 20256–20263

    Abstract: The use of two-dimensional (2D) materials in next-generation technologies is often limited by small lateral size and/or crystal defects. Here, we introduce a simple chemical strategy to improve the size and overall quality of 2D metal-organic ... ...

    Abstract The use of two-dimensional (2D) materials in next-generation technologies is often limited by small lateral size and/or crystal defects. Here, we introduce a simple chemical strategy to improve the size and overall quality of 2D metal-organic chalcogenolates (MOCs), a new class of hybrid organic-inorganic 2D semiconductors that can exhibit in-plane anisotropy and blue luminescence. By inducing the formation of silver-amine complexes during a solution growth method, we increase the average size of silver phenylselenolate (AgSePh) microcrystals from <5 μm to >1 mm, while simultaneously extending the photoluminescence lifetime and suppressing mid-gap emission. Mechanistic studies using
    Language English
    Publishing date 2021-11-21
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c09106
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article ; Online: Light Emission in 2D Silver Phenylchalcogenolates.

    Lee, Woo Seok / Cho, Yeongsu / Powers, Eric R / Paritmongkol, Watcharaphol / Sakurada, Tomoaki / Kulik, Heather J / Tisdale, William A

    ACS nano

    2022  

    Abstract: Silver phenylselenolate (AgSePh, also known as "mithrene") and silver phenyltellurolate (AgTePh, also known as "tethrene") are two-dimensional (2D) van der Waals semiconductors belonging to an emerging class of hybrid organic-inorganic materials called ... ...

    Abstract Silver phenylselenolate (AgSePh, also known as "mithrene") and silver phenyltellurolate (AgTePh, also known as "tethrene") are two-dimensional (2D) van der Waals semiconductors belonging to an emerging class of hybrid organic-inorganic materials called metal-organic chalcogenolates. Despite having the same crystal structure, AgSePh and AgTePh exhibit a strikingly different excitonic behavior. Whereas AgSePh exhibits narrow, fast luminescence with a minimal Stokes shift, AgTePh exhibits comparatively slow luminescence that is significantly broadened and red-shifted from its absorption minimum. Using time-resolved and temperature-dependent absorption and emission microspectroscopy, combined with subgap photoexcitation studies, we show that exciton dynamics in AgTePh films are dominated by an intrinsic self-trapping behavior, whereas dynamics in AgSePh films are dominated by the interaction of band-edge excitons with a finite number of extrinsic defect/trap states. Density functional theory calculations reveal that AgSePh has simple parabolic band edges with a direct gap at Γ, whereas AgTePh has a saddle point at Γ with a horizontal splitting along the Γ-N
    Language English
    Publishing date 2022-11-23
    Publishing country United States
    Document type Journal Article
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/acsnano.2c06204
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  8. Article ; Online: Morphological Control of 2D Hybrid Organic-Inorganic Semiconductor AgSePh.

    Paritmongkol, Watcharaphol / Lee, Woo Seok / Shcherbakov-Wu, Wenbi / Ha, Seung Kyun / Sakurada, Tomoaki / Oh, Soong Ju / Tisdale, William A

    ACS nano

    2022  Volume 16, Issue 2, Page(s) 2054–2065

    Abstract: Silver phenylselenolate (AgSePh) is a hybrid organic-inorganic two-dimensional (2D) semiconductor exhibiting narrow blue emission, in-plane anisotropy, and large exciton binding energy. Here, we show that the addition of carefully chosen solvent vapors ... ...

    Abstract Silver phenylselenolate (AgSePh) is a hybrid organic-inorganic two-dimensional (2D) semiconductor exhibiting narrow blue emission, in-plane anisotropy, and large exciton binding energy. Here, we show that the addition of carefully chosen solvent vapors during the chemical transformation of metallic silver to AgSePh allows for control over the size and orientation of AgSePh crystals. By testing 28 solvent vapors (with different polarities, boiling points, and functional groups), we controlled the resulting crystal size from <200 nm up to a few μm. Furthermore, choice of solvent vapor can substantially improve the orientational homogeneity of 2D crystals with respect to the substrate. In particular, solvents known to form complexes with silver ions, such as dimethyl sulfoxide (DMSO), led to the largest lateral crystal dimensions and parallel crystal orientation. We perform systematic optical and electrical characterizations on DMSO vapor-grown AgSePh films demonstrating improved crystalline quality, lower defect densities, higher photoconductivity, lower dark conductivity, suppression of ionic migration, and reduced midgap photoluminescence at low temperature. Overall, this work provides a strategy for realizing AgSePh films with improved optical properties and reveals the roles of solvent vapors on the chemical transformation of metallic silver.
    Language English
    Publishing date 2022-01-31
    Publishing country United States
    Document type Journal Article
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/acsnano.1c07498
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  9. Article ; Online: Efficient Homojunction Tin Perovskite Solar Cells Enabled by Gradient Germanium Doping.

    Zhao, Zhenzhu / Sun, Mulin / Ji, Yuyang / Mao, Kaitian / Huang, Zongming / Yuan, Chengjian / Yang, Yuqian / Ding, Honghe / Yang, Yingguo / Li, Yu / Chen, Wenjing / Zhu, Junfa / Wei, Jing / Xu, Jixian / Paritmongkol, Watcharaphol / Abate, Antonio / Xiao, Zhengguo / He, Lixin / Hu, Qin

    Nano letters

    2024  Volume 24, Issue 18, Page(s) 5513–5520

    Abstract: P-type self-doping is known to hamper tin-based perovskites for developing high-performance solar cells by increasing the background current density and carrier recombination processes. In this work, we propose a gradient homojunction structure with ... ...

    Abstract P-type self-doping is known to hamper tin-based perovskites for developing high-performance solar cells by increasing the background current density and carrier recombination processes. In this work, we propose a gradient homojunction structure with germanium doping that generates an internal electric field across the perovskite film to deplete the charge carriers. This structure reduces the dark current density of perovskite by over 2 orders of magnitude and trap density by an order of magnitude. The resultant tin-based perovskite solar cells exhibit a higher power conversion efficiency of 13.3% and excellent stability, maintaining 95% and 85% of their initial efficiencies after 250 min of continuous illumination and 3800 h of storage, respectively. We reveal the homojunction formation mechanism using density functional theory calculations and molecular level characterizations. Our work provides a reliable strategy for controlling the spatial energy levels in tin perovskite films and offers insights into designing intriguing lead-free perovskite optoelectronics.
    Language English
    Publishing date 2024-04-18
    Publishing country United States
    Document type Journal Article
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.4c00646
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  10. Article ; Online: Dicarboxylic Acid-Assisted Surface Oxide Removal and Passivation of Indium Antimonide Colloidal Quantum Dots for Short-Wave Infrared Photodetectors.

    Zhang, Yangning / Xia, Pan / Rehl, Benjamin / Parmar, Darshan H / Choi, Dongsun / Imran, Muhammad / Chen, Yiqing / Liu, Yanjiang / Vafaie, Maral / Li, Chongwen / Atan, Ozan / Pina, Joao M / Paritmongkol, Watcharaphol / Levina, Larissa / Voznyy, Oleksandr / Hoogland, Sjoerd / Sargent, Edward H

    Angewandte Chemie (International ed. in English)

    2024  Volume 63, Issue 8, Page(s) e202316733

    Abstract: Heavy-metal-free III-V colloidal quantum dots (CQDs) are promising materials for solution-processed short-wave infrared (SWIR) photodetectors. Recent progress in the synthesis of indium antimonide (InSb) CQDs with sizes smaller than the Bohr exciton ... ...

    Abstract Heavy-metal-free III-V colloidal quantum dots (CQDs) are promising materials for solution-processed short-wave infrared (SWIR) photodetectors. Recent progress in the synthesis of indium antimonide (InSb) CQDs with sizes smaller than the Bohr exciton radius enables quantum-size effect tuning of the band gap. However, it has been challenging to achieve uniform InSb CQDs with band gaps below 0.9 eV, as well as to control the surface chemistry of these large-diameter CQDs. This has, to date, limited the development of InSb CQD photodetectors that are sensitive to
    Language English
    Publishing date 2024-01-16
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.202316733
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