[{"isi":1,"title":"Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance","external_id":{"pmid":["37310395"],"isi":["001008564800001"]},"doi":"10.1021/acsnano.3c03541","year":"2023","pmid":1,"_id":"13235","publication_identifier":{"issn":["1936-0851"],"eissn":["1936-086X"]},"acknowledgement":"Y.L. acknowledges funding from the National Natural Science Foundation of China (NSFC) (Grants No. 22209034), the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province (Grant No. 2022LCX002). K.H.L. acknowledges financial support from the National Natural Science Foundation of China (Grant No. 22208293). Y.Z. acknowledges support from the SBIR program NanoOhmics. J.L. is grateful for the project supported by the Natural Science Foundation of Sichuan (2022NSFSC1229). M.I. acknowledges financial support from ISTA and the Werner Siemens Foundation.","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","quality_controlled":"1","project":[{"name":"HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of Semiconductors for Waste Heat Recovery","_id":"9B8F7476-BA93-11EA-9121-9846C619BF3A"}],"oa_version":"None","volume":17,"date_updated":"2023-08-02T06:29:55Z","article_processing_charge":"No","abstract":[{"text":"AgSbSe2 is a promising thermoelectric (TE) p-type material for applications in the middle-temperature range. AgSbSe2 is characterized by relatively low thermal conductivities and high Seebeck coefficients, but its main limitation is moderate electrical conductivity. Herein, we detail an efficient and scalable hot-injection synthesis route to produce AgSbSe2 nanocrystals (NCs). To increase the carrier concentration and improve the electrical conductivity, these NCs are doped with Sn2+ on Sb3+ sites. Upon processing, the Sn2+ chemical state is conserved using a reducing NaBH4 solution to displace the organic ligand and anneal the material under a forming gas flow. The TE properties of the dense materials obtained from the consolidation of the NCs using a hot pressing are then characterized. The presence of Sn2+ ions replacing Sb3+ significantly increases the charge carrier concentration and, consequently, the electrical conductivity. Opportunely, the measured Seebeck coefficient varied within a small range upon Sn doping. The excellent performance obtained when Sn2+ ions are prevented from oxidation is rationalized by modeling the system. Calculated band structures disclosed that Sn doping induces convergence of the AgSbSe2 valence bands, accounting for an enhanced electronic effective mass. The dramatically enhanced carrier transport leads to a maximized power factor for AgSb0.98Sn0.02Se2 of 0.63 mW m–1 K–2 at 640 K. Thermally, phonon scattering is significantly enhanced in the NC-based materials, yielding an ultralow thermal conductivity of 0.3 W mK–1 at 666 K. Overall, a record-high figure of merit (zT) is obtained at 666 K for AgSb0.98Sn0.02Se2 at zT = 1.37, well above the values obtained for undoped AgSbSe2, at zT = 0.58 and state-of-art Pb- and Te-free materials, which makes AgSb0.98Sn0.02Se2 an excellent p-type candidate for medium-temperature TE applications.","lang":"eng"}],"author":[{"first_name":"Yu","full_name":"Liu, Yu","last_name":"Liu","orcid":"0000-0001-7313-6740","id":"2A70014E-F248-11E8-B48F-1D18A9856A87"},{"first_name":"Mingquan","last_name":"Li","full_name":"Li, Mingquan"},{"first_name":"Shanhong","last_name":"Wan","full_name":"Wan, Shanhong"},{"first_name":"Khak Ho","last_name":"Lim","full_name":"Lim, Khak Ho"},{"first_name":"Yu","full_name":"Zhang, Yu","last_name":"Zhang"},{"first_name":"Mengyao","full_name":"Li, Mengyao","last_name":"Li"},{"last_name":"Li","full_name":"Li, Junshan","first_name":"Junshan"},{"first_name":"Maria","orcid":"0000-0001-5013-2843","full_name":"Ibáñez, Maria","last_name":"Ibáñez","id":"43C61214-F248-11E8-B48F-1D18A9856A87"},{"full_name":"Hong, Min","last_name":"Hong","first_name":"Min"},{"first_name":"Andreu","last_name":"Cabot","full_name":"Cabot, Andreu"}],"publication_status":"published","citation":{"short":"Y. Liu, M. Li, S. Wan, K.H. Lim, Y. Zhang, M. Li, J. Li, M. Ibáñez, M. Hong, A. Cabot, ACS Nano 17 (2023) 11923–11934.","ista":"Liu Y, Li M, Wan S, Lim KH, Zhang Y, Li M, Li J, Ibáñez M, Hong M, Cabot A. 2023. Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. ACS Nano. 17(12), 11923–11934.","mla":"Liu, Yu, et al. “Surface Chemistry and Band Engineering in AgSbSe₂: Toward High Thermoelectric Performance.” <i>ACS Nano</i>, vol. 17, no. 12, American Chemical Society, 2023, pp. 11923–11934, doi:<a href=\"https://doi.org/10.1021/acsnano.3c03541\">10.1021/acsnano.3c03541</a>.","ama":"Liu Y, Li M, Wan S, et al. Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. <i>ACS Nano</i>. 2023;17(12):11923–11934. doi:<a href=\"https://doi.org/10.1021/acsnano.3c03541\">10.1021/acsnano.3c03541</a>","chicago":"Liu, Yu, Mingquan Li, Shanhong Wan, Khak Ho Lim, Yu Zhang, Mengyao Li, Junshan Li, Maria Ibáñez, Min Hong, and Andreu Cabot. “Surface Chemistry and Band Engineering in AgSbSe₂: Toward High Thermoelectric Performance.” <i>ACS Nano</i>. American Chemical Society, 2023. <a href=\"https://doi.org/10.1021/acsnano.3c03541\">https://doi.org/10.1021/acsnano.3c03541</a>.","ieee":"Y. Liu <i>et al.</i>, “Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance,” <i>ACS Nano</i>, vol. 17, no. 12. American Chemical Society, pp. 11923–11934, 2023.","apa":"Liu, Y., Li, M., Wan, S., Lim, K. H., Zhang, Y., Li, M., … Cabot, A. (2023). Surface chemistry and band engineering in AgSbSe₂: Toward high thermoelectric performance. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.3c03541\">https://doi.org/10.1021/acsnano.3c03541</a>"},"date_created":"2023-07-16T22:01:11Z","department":[{"_id":"MaIb"}],"publisher":"American Chemical Society","scopus_import":"1","language":[{"iso":"eng"}],"month":"06","date_published":"2023-06-13T00:00:00Z","article_type":"original","issue":"12","publication":"ACS Nano","page":"11923–11934","intvolume":"        17","status":"public","day":"13","type":"journal_article"},{"page":"275-287","issue":"1","publication":"ACS Nano","status":"public","intvolume":"        17","type":"journal_article","day":"10","date_created":"2023-08-01T09:30:29Z","language":[{"iso":"eng"}],"publisher":"American Chemical Society","scopus_import":"1","article_type":"original","date_published":"2023-01-10T00:00:00Z","month":"01","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","quality_controlled":"1","oa_version":"Published Version","_id":"13346","extern":"1","publication_identifier":{"issn":["1936-0851"],"eissn":["1936-086X"]},"volume":17,"date_updated":"2023-08-02T06:51:15Z","oa":1,"article_processing_charge":"No","author":[{"first_name":"Chiara","last_name":"Lionello","full_name":"Lionello, Chiara"},{"full_name":"Perego, Claudio","last_name":"Perego","first_name":"Claudio"},{"full_name":"Gardin, Andrea","last_name":"Gardin","first_name":"Andrea"},{"id":"8e84690e-1e48-11ed-a02b-a1e6fb8bb53b","first_name":"Rafal","last_name":"Klajn","full_name":"Klajn, Rafal"},{"first_name":"Giovanni M.","last_name":"Pavan","full_name":"Pavan, Giovanni M."}],"keyword":["General Physics and Astronomy","General Engineering","General Materials Science"],"abstract":[{"text":"The self-assembly of nanoparticles driven by small molecules or ions may produce colloidal superlattices with features and properties reminiscent of those of metals or semiconductors. However, to what extent the properties of such supramolecular crystals actually resemble those of atomic materials often remains unclear. Here, we present coarse-grained molecular simulations explicitly demonstrating how a behavior evocative of that of semiconductors may emerge in a colloidal superlattice. As a case study, we focus on gold nanoparticles bearing positively charged groups that self-assemble into FCC crystals via mediation by citrate counterions. In silico ohmic experiments show how the dynamically diverse behavior of the ions in different superlattice domains allows the opening of conductive ionic gates above certain levels of applied electric fields. The observed binary conductive/nonconductive behavior is reminiscent of that of conventional semiconductors, while, at a supramolecular level, crossing the “band gap” requires a sufficient electrostatic stimulus to break the intermolecular interactions and make ions diffuse throughout the superlattice’s cavities.","lang":"eng"}],"publication_status":"published","citation":{"mla":"Lionello, Chiara, et al. “Supramolecular Semiconductivity through Emerging Ionic Gates in Ion–Nanoparticle Superlattices.” <i>ACS Nano</i>, vol. 17, no. 1, American Chemical Society, 2023, pp. 275–87, doi:<a href=\"https://doi.org/10.1021/acsnano.2c07558\">10.1021/acsnano.2c07558</a>.","ama":"Lionello C, Perego C, Gardin A, Klajn R, Pavan GM. Supramolecular semiconductivity through emerging ionic gates in ion–nanoparticle superlattices. <i>ACS Nano</i>. 2023;17(1):275-287. doi:<a href=\"https://doi.org/10.1021/acsnano.2c07558\">10.1021/acsnano.2c07558</a>","ista":"Lionello C, Perego C, Gardin A, Klajn R, Pavan GM. 2023. Supramolecular semiconductivity through emerging ionic gates in ion–nanoparticle superlattices. ACS Nano. 17(1), 275–287.","short":"C. Lionello, C. Perego, A. Gardin, R. Klajn, G.M. Pavan, ACS Nano 17 (2023) 275–287.","apa":"Lionello, C., Perego, C., Gardin, A., Klajn, R., &#38; Pavan, G. M. (2023). Supramolecular semiconductivity through emerging ionic gates in ion–nanoparticle superlattices. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.2c07558\">https://doi.org/10.1021/acsnano.2c07558</a>","ieee":"C. Lionello, C. Perego, A. Gardin, R. Klajn, and G. M. Pavan, “Supramolecular semiconductivity through emerging ionic gates in ion–nanoparticle superlattices,” <i>ACS Nano</i>, vol. 17, no. 1. American Chemical Society, pp. 275–287, 2023.","chicago":"Lionello, Chiara, Claudio Perego, Andrea Gardin, Rafal Klajn, and Giovanni M. Pavan. “Supramolecular Semiconductivity through Emerging Ionic Gates in Ion–Nanoparticle Superlattices.” <i>ACS Nano</i>. American Chemical Society, 2023. <a href=\"https://doi.org/10.1021/acsnano.2c07558\">https://doi.org/10.1021/acsnano.2c07558</a>."},"main_file_link":[{"url":"https://doi.org/10.1021/acsnano.2c07558","open_access":"1"}],"title":"Supramolecular semiconductivity through emerging ionic gates in ion–nanoparticle superlattices","doi":"10.1021/acsnano.2c07558","year":"2023"},{"article_processing_charge":"No","date_updated":"2023-10-04T11:29:22Z","volume":17,"oa_version":"None","quality_controlled":"1","acknowledgement":"The authors acknowledge support from the projects ENE2016-77798-C4-3-R and NANOGEN (PID2020-116093RB-C43) funded by MCIN/AEI/10.13039/501100011033/and by “ERDF A way of making Europe”, and by the “European Union”. K.X. and B.N. thank the China Scholarship Council (CSC) for scholarship support. The authors acknowledge funding from Generalitat de Catalunya 2017 SGR 327 and 2017 SGR 1246. ICN2 is supported by the Severo Ochoa program from the Spanish MCIN/AEI (Grant No.: CEX2021-001214-S). IREC and ICN2 are funded by the CERCA Programme/Generalitat de Catalunya. J.L. acknowledges support from the Natural Science Foundation of Sichuan province (2022NSFSC1229). Part of the present work was performed in the frameworks of Universitat de Barcelona Nanoscience Ph.D. program and Universitat Autònoma de Barcelona Materials Science Ph.D. program. Y.L. acknowledges funding from the National Natural Science Foundation of China (Grant No. 22209034) and the Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province (Grants No. 2022LCX002). K.H.L. acknowledges the financial support of the National Natural Science Foundation of China (Grant No. 22208293).","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"_id":"12915","pmid":1,"citation":{"short":"C. Xing, Y. Zhang, K. Xiao, X. Han, Y. Liu, B. Nan, M.G. Ramon, K.H. Lim, J. Li, J. Arbiol, B. Poudel, A. Nozariasbmarz, W. Li, M. Ibáñez, A. Cabot, ACS Nano 17 (2023) 8442–8452.","ista":"Xing C, Zhang Y, Xiao K, Han X, Liu Y, Nan B, Ramon MG, Lim KH, Li J, Arbiol J, Poudel B, Nozariasbmarz A, Li W, Ibáñez M, Cabot A. 2023. Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. ACS Nano. 17(9), 8442–8452.","mla":"Xing, Congcong, et al. “Thermoelectric Performance of Surface-Engineered Cu1.5–XTe–Cu2Se Nanocomposites.” <i>ACS Nano</i>, vol. 17, no. 9, American Chemical Society, 2023, pp. 8442–52, doi:<a href=\"https://doi.org/10.1021/acsnano.3c00495\">10.1021/acsnano.3c00495</a>.","ama":"Xing C, Zhang Y, Xiao K, et al. Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. <i>ACS Nano</i>. 2023;17(9):8442-8452. doi:<a href=\"https://doi.org/10.1021/acsnano.3c00495\">10.1021/acsnano.3c00495</a>","chicago":"Xing, Congcong, Yu Zhang, Ke Xiao, Xu Han, Yu Liu, Bingfei Nan, Maria Garcia Ramon, et al. “Thermoelectric Performance of Surface-Engineered Cu1.5–XTe–Cu2Se Nanocomposites.” <i>ACS Nano</i>. American Chemical Society, 2023. <a href=\"https://doi.org/10.1021/acsnano.3c00495\">https://doi.org/10.1021/acsnano.3c00495</a>.","ieee":"C. Xing <i>et al.</i>, “Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites,” <i>ACS Nano</i>, vol. 17, no. 9. American Chemical Society, pp. 8442–8452, 2023.","apa":"Xing, C., Zhang, Y., Xiao, K., Han, X., Liu, Y., Nan, B., … Cabot, A. (2023). Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.3c00495\">https://doi.org/10.1021/acsnano.3c00495</a>"},"publication_status":"published","author":[{"full_name":"Xing, Congcong","last_name":"Xing","first_name":"Congcong"},{"full_name":"Zhang, Yu","last_name":"Zhang","first_name":"Yu"},{"full_name":"Xiao, Ke","last_name":"Xiao","first_name":"Ke"},{"first_name":"Xu","last_name":"Han","full_name":"Han, Xu"},{"id":"2A70014E-F248-11E8-B48F-1D18A9856A87","first_name":"Yu","last_name":"Liu","full_name":"Liu, Yu","orcid":"0000-0001-7313-6740"},{"first_name":"Bingfei","full_name":"Nan, Bingfei","last_name":"Nan"},{"full_name":"Ramon, Maria Garcia","last_name":"Ramon","first_name":"Maria Garcia","id":"1ffff7cd-ed76-11ed-8d5f-be5e7c364eb9"},{"full_name":"Lim, Khak Ho","last_name":"Lim","first_name":"Khak Ho"},{"last_name":"Li","full_name":"Li, Junshan","first_name":"Junshan"},{"first_name":"Jordi","full_name":"Arbiol, Jordi","last_name":"Arbiol"},{"first_name":"Bed","last_name":"Poudel","full_name":"Poudel, Bed"},{"first_name":"Amin","full_name":"Nozariasbmarz, Amin","last_name":"Nozariasbmarz"},{"first_name":"Wenjie","last_name":"Li","full_name":"Li, Wenjie"},{"first_name":"Maria","full_name":"Ibáñez, Maria","last_name":"Ibáñez","orcid":"0000-0001-5013-2843","id":"43C61214-F248-11E8-B48F-1D18A9856A87"},{"first_name":"Andreu","full_name":"Cabot, Andreu","last_name":"Cabot"}],"abstract":[{"text":"Cu2–xS and Cu2–xSe have recently been reported as promising thermoelectric (TE) materials for medium-temperature applications. In contrast, Cu2–xTe, another member of the copper chalcogenide family, typically exhibits low Seebeck coefficients that limit its potential to achieve a superior thermoelectric figure of merit, zT, particularly in the low-temperature range where this material could be effective. To address this, we investigated the TE performance of Cu1.5–xTe–Cu2Se nanocomposites by consolidating surface-engineered Cu1.5Te nanocrystals. This surface engineering strategy allows for precise adjustment of Cu/Te ratios and results in a reversible phase transition at around 600 K in Cu1.5–xTe–Cu2Se nanocomposites, as systematically confirmed by in situ high-temperature X-ray diffraction combined with differential scanning calorimetry analysis. The phase transition leads to a conversion from metallic-like to semiconducting-like TE properties. Additionally, a layer of Cu2Se generated around Cu1.5–xTe nanoparticles effectively inhibits Cu1.5–xTe grain growth, minimizing thermal conductivity and decreasing hole concentration. These properties indicate that copper telluride based compounds have a promising thermoelectric potential, translated into a high dimensionless zT of 1.3 at 560 K.","lang":"eng"}],"isi":1,"doi":"10.1021/acsnano.3c00495","year":"2023","title":"Thermoelectric performance of surface-engineered Cu1.5–xTe–Cu2Se nanocomposites","external_id":{"pmid":["37071412"],"isi":["000976063200001"]},"page":"8442-8452","publication":"ACS Nano","issue":"9","type":"journal_article","day":"09","status":"public","intvolume":"        17","department":[{"_id":"MaIb"}],"date_created":"2023-05-07T22:01:04Z","article_type":"original","date_published":"2023-05-09T00:00:00Z","month":"05","language":[{"iso":"eng"}],"scopus_import":"1","publisher":"American Chemical Society"},{"has_accepted_license":"1","department":[{"_id":"MaIb"}],"file":[{"date_updated":"2022-03-02T16:17:29Z","access_level":"open_access","file_name":"2022_ACSNano_Liu.pdf","file_size":9050764,"date_created":"2022-03-02T16:17:29Z","checksum":"74f9c1aa5f95c0b992a4328e8e0247b4","content_type":"application/pdf","relation":"main_file","creator":"cchlebak","file_id":"10808","success":1}],"date_created":"2021-09-24T07:55:12Z","month":"01","date_published":"2022-01-25T00:00:00Z","article_type":"original","publisher":"American Chemical Society ","scopus_import":"1","language":[{"iso":"eng"}],"issue":"1","publication":"ACS Nano","file_date_updated":"2022-03-02T16:17:29Z","page":"78-88","day":"25","type":"journal_article","intvolume":"        16","status":"public","tmp":{"image":"/images/cc_by.png","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","short":"CC BY (4.0)"},"isi":1,"related_material":{"record":[{"status":"public","id":"12885","relation":"dissertation_contains"}]},"ddc":["540"],"doi":"10.1021/acsnano.1c06720","year":"2022","ec_funded":1,"external_id":{"pmid":["34549956"],"isi":["000767223400008"]},"title":"Defect engineering in solution-processed polycrystalline SnSe leads to high thermoelectric performance","date_updated":"2023-08-02T14:41:05Z","volume":16,"oa":1,"article_processing_charge":"Yes (via OA deal)","pmid":1,"_id":"10042","publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","acknowledgement":"This work was financially supported by IST Austria and the Werner Siemens Foundation. Y.L. acknowledges funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 754411. S.L. and M.C. received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement No. 665385. J.D. acknowledges funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 665919 (P-SPHERE) cofunded by Severo Ochoa Programme. C.C. acknowledges funding from the FWF “Lise Meitner Fellowship” grant agreement M 2889-N. Y.Y. and O.C.-M. acknowledge the financial support from DFG within the project SFB 917: Nanoswitches. M.C.S. received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 754510 (PROBIST) and the Severo Ochoa programme. J.D. received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 665919 (P-SPHERE) cofunded by Severo Ochoa Programme. The ICN2 is funded by the CERCA Program/Generalitat de Catalunya and by the Severo Ochoa program of the Spanish Ministry of Economy, Industry, and Competitiveness (MINECO, grant no. SEV-2017-0706). ICN2 acknowledges funding from Generalitat de Catalunya 2017 SGR 327 and the Spanish MINECO project NANOGEN (PID2020-116093RB-C43). This project received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 823717-ESTEEM3. The FIB sample preparation was conducted in the LMA-INA-Universidad de Zaragoza.","oa_version":"Published Version","project":[{"grant_number":"754411","call_identifier":"H2020","name":"ISTplus - Postdoctoral Fellowships","_id":"260C2330-B435-11E9-9278-68D0E5697425"},{"call_identifier":"H2020","name":"International IST Doctoral Program","_id":"2564DBCA-B435-11E9-9278-68D0E5697425","grant_number":"665385"},{"_id":"9B8F7476-BA93-11EA-9121-9846C619BF3A","name":"HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of Semiconductors for Waste Heat Recovery"},{"_id":"9B8804FC-BA93-11EA-9121-9846C619BF3A","name":"Bottom-up Engineering for Thermoelectric Applications","grant_number":"M02889"}],"quality_controlled":"1","publication_status":"published","citation":{"chicago":"Liu, Yu, Mariano Calcabrini, Yuan Yu, Seungho Lee, Cheng Chang, Jérémy David, Tanmoy Ghosh, et al. “Defect Engineering in Solution-Processed Polycrystalline SnSe Leads to High Thermoelectric Performance.” <i>ACS Nano</i>. American Chemical Society , 2022. <a href=\"https://doi.org/10.1021/acsnano.1c06720\">https://doi.org/10.1021/acsnano.1c06720</a>.","ieee":"Y. Liu <i>et al.</i>, “Defect engineering in solution-processed polycrystalline SnSe leads to high thermoelectric performance,” <i>ACS Nano</i>, vol. 16, no. 1. American Chemical Society , pp. 78–88, 2022.","apa":"Liu, Y., Calcabrini, M., Yu, Y., Lee, S., Chang, C., David, J., … Ibáñez, M. (2022). Defect engineering in solution-processed polycrystalline SnSe leads to high thermoelectric performance. <i>ACS Nano</i>. American Chemical Society . <a href=\"https://doi.org/10.1021/acsnano.1c06720\">https://doi.org/10.1021/acsnano.1c06720</a>","ista":"Liu Y, Calcabrini M, Yu Y, Lee S, Chang C, David J, Ghosh T, Spadaro MC, Xie C, Cojocaru-Mirédin O, Arbiol J, Ibáñez M. 2022. Defect engineering in solution-processed polycrystalline SnSe leads to high thermoelectric performance. ACS Nano. 16(1), 78–88.","short":"Y. Liu, M. Calcabrini, Y. Yu, S. Lee, C. Chang, J. David, T. Ghosh, M.C. Spadaro, C. Xie, O. Cojocaru-Mirédin, J. Arbiol, M. Ibáñez, ACS Nano 16 (2022) 78–88.","ama":"Liu Y, Calcabrini M, Yu Y, et al. Defect engineering in solution-processed polycrystalline SnSe leads to high thermoelectric performance. <i>ACS Nano</i>. 2022;16(1):78-88. doi:<a href=\"https://doi.org/10.1021/acsnano.1c06720\">10.1021/acsnano.1c06720</a>","mla":"Liu, Yu, et al. “Defect Engineering in Solution-Processed Polycrystalline SnSe Leads to High Thermoelectric Performance.” <i>ACS Nano</i>, vol. 16, no. 1, American Chemical Society , 2022, pp. 78–88, doi:<a href=\"https://doi.org/10.1021/acsnano.1c06720\">10.1021/acsnano.1c06720</a>."},"abstract":[{"lang":"eng","text":"SnSe has emerged as one of the most promising materials for thermoelectric energy conversion due to its extraordinary performance in its single-crystal form and its low-cost constituent elements. However, to achieve an economic impact, the polycrystalline counterpart needs to replicate the performance of the single crystal. Herein, we optimize the thermoelectric performance of polycrystalline SnSe produced by consolidating solution-processed and surface-engineered SnSe particles. In particular, the SnSe particles are coated with CdSe molecular complexes that crystallize during the sintering process, forming CdSe nanoparticles. The presence of CdSe nanoparticles inhibits SnSe grain growth during the consolidation step due to Zener pinning, yielding a material with a high density of grain boundaries. Moreover, the resulting SnSe–CdSe nanocomposites present a large number of defects at different length scales, which significantly reduce the thermal conductivity. The produced SnSe–CdSe nanocomposites exhibit thermoelectric figures of merit up to 2.2 at 786 K, which is among the highest reported for solution-processed SnSe."}],"author":[{"id":"2A70014E-F248-11E8-B48F-1D18A9856A87","first_name":"Yu","full_name":"Liu, Yu","last_name":"Liu","orcid":"0000-0001-7313-6740"},{"first_name":"Mariano","last_name":"Calcabrini","full_name":"Calcabrini, Mariano","id":"45D7531A-F248-11E8-B48F-1D18A9856A87"},{"full_name":"Yu, Yuan","last_name":"Yu","first_name":"Yuan"},{"first_name":"Seungho","orcid":"0000-0002-6962-8598","last_name":"Lee","full_name":"Lee, Seungho","id":"BB243B88-D767-11E9-B658-BC13E6697425"},{"id":"9E331C2E-9F27-11E9-AE48-5033E6697425","full_name":"Chang, Cheng","last_name":"Chang","orcid":"0000-0002-9515-4277","first_name":"Cheng"},{"full_name":"David, Jérémy","last_name":"David","first_name":"Jérémy"},{"first_name":"Tanmoy","last_name":"Ghosh","full_name":"Ghosh, Tanmoy","id":"a5fc9bc3-feff-11ea-93fe-e8015a3c7e9d"},{"first_name":"Maria Chiara","full_name":"Spadaro, Maria Chiara","last_name":"Spadaro"},{"last_name":"Xie","full_name":"Xie, Chenyang","first_name":"Chenyang"},{"first_name":"Oana","last_name":"Cojocaru-Mirédin","full_name":"Cojocaru-Mirédin, Oana"},{"first_name":"Jordi","full_name":"Arbiol, Jordi","last_name":"Arbiol"},{"id":"43C61214-F248-11E8-B48F-1D18A9856A87","full_name":"Ibáñez, Maria","last_name":"Ibáñez","orcid":"0000-0001-5013-2843","first_name":"Maria"}],"keyword":["tin selenide","nanocomposite","grain growth","Zener pinning","thermoelectricity","annealing","solution processing"]},{"date_published":"2021-03-01T00:00:00Z","article_type":"original","month":"03","language":[{"iso":"eng"}],"publisher":"American Chemical Society ","scopus_import":"1","department":[{"_id":"MaIb"}],"date_created":"2021-03-10T20:12:45Z","type":"journal_article","day":"01","status":"public","intvolume":"        15","page":"4967–4978","issue":"3","publication":"ACS Nano","year":"2021","doi":"10.1021/acsnano.0c09866","title":"Effect of the annealing atmosphere on crystal phase and thermoelectric properties of copper sulfide","external_id":{"pmid":["33645986"],"isi":["000634569100106"]},"isi":1,"main_file_link":[{"open_access":"1","url":"https://upcommons.upc.edu/bitstream/handle/2117/363528/Pb%20mengyao.pdf?sequence=1&isAllowed=y"}],"publication_status":"published","citation":{"short":"M. Li, Y. Liu, Y. Zhang, X. Han, T. Zhang, Y. Zuo, C. Xie, K. Xiao, J. Arbiol, J. Llorca, M. Ibáñez, J. Liu, A. Cabot, ACS Nano 15 (2021) 4967–4978.","ista":"Li M, Liu Y, Zhang Y, Han X, Zhang T, Zuo Y, Xie C, Xiao K, Arbiol J, Llorca J, Ibáñez M, Liu J, Cabot A. 2021. Effect of the annealing atmosphere on crystal phase and thermoelectric properties of copper sulfide. ACS Nano. 15(3), 4967–4978.","ama":"Li M, Liu Y, Zhang Y, et al. Effect of the annealing atmosphere on crystal phase and thermoelectric properties of copper sulfide. <i>ACS Nano</i>. 2021;15(3):4967–4978. doi:<a href=\"https://doi.org/10.1021/acsnano.0c09866\">10.1021/acsnano.0c09866</a>","mla":"Li, Mengyao, et al. “Effect of the Annealing Atmosphere on Crystal Phase and Thermoelectric Properties of Copper Sulfide.” <i>ACS Nano</i>, vol. 15, no. 3, American Chemical Society , 2021, pp. 4967–4978, doi:<a href=\"https://doi.org/10.1021/acsnano.0c09866\">10.1021/acsnano.0c09866</a>.","chicago":"Li, Mengyao, Yu Liu, Yu Zhang, Xu Han, Ting Zhang, Yong Zuo, Chenyang Xie, et al. “Effect of the Annealing Atmosphere on Crystal Phase and Thermoelectric Properties of Copper Sulfide.” <i>ACS Nano</i>. American Chemical Society , 2021. <a href=\"https://doi.org/10.1021/acsnano.0c09866\">https://doi.org/10.1021/acsnano.0c09866</a>.","ieee":"M. Li <i>et al.</i>, “Effect of the annealing atmosphere on crystal phase and thermoelectric properties of copper sulfide,” <i>ACS Nano</i>, vol. 15, no. 3. American Chemical Society , pp. 4967–4978, 2021.","apa":"Li, M., Liu, Y., Zhang, Y., Han, X., Zhang, T., Zuo, Y., … Cabot, A. (2021). Effect of the annealing atmosphere on crystal phase and thermoelectric properties of copper sulfide. <i>ACS Nano</i>. American Chemical Society . <a href=\"https://doi.org/10.1021/acsnano.0c09866\">https://doi.org/10.1021/acsnano.0c09866</a>"},"author":[{"full_name":"Li, Mengyao","last_name":"Li","first_name":"Mengyao"},{"orcid":"0000-0001-7313-6740","last_name":"Liu","full_name":"Liu, Yu","first_name":"Yu","id":"2A70014E-F248-11E8-B48F-1D18A9856A87"},{"last_name":"Zhang","full_name":"Zhang, Yu","first_name":"Yu"},{"full_name":"Han, Xu","last_name":"Han","first_name":"Xu"},{"last_name":"Zhang","full_name":"Zhang, Ting","first_name":"Ting"},{"full_name":"Zuo, Yong","last_name":"Zuo","first_name":"Yong"},{"first_name":"Chenyang","full_name":"Xie, Chenyang","last_name":"Xie"},{"full_name":"Xiao, Ke","last_name":"Xiao","first_name":"Ke"},{"last_name":"Arbiol","full_name":"Arbiol, Jordi","first_name":"Jordi"},{"full_name":"Llorca, Jordi","last_name":"Llorca","first_name":"Jordi"},{"first_name":"Maria","full_name":"Ibáñez, Maria","last_name":"Ibáñez","orcid":"0000-0001-5013-2843","id":"43C61214-F248-11E8-B48F-1D18A9856A87"},{"first_name":"Junfeng","full_name":"Liu, Junfeng","last_name":"Liu"},{"last_name":"Cabot","full_name":"Cabot, Andreu","first_name":"Andreu"}],"keyword":["General Engineering","General Physics and Astronomy","General Materials Science"],"abstract":[{"lang":"eng","text":"Cu2–xS has become one of the most promising thermoelectric materials for application in the middle-high temperature range. Its advantages include the abundance, low cost, and safety of its elements and a high performance at relatively elevated temperatures. However, stability issues limit its operation current and temperature, thus calling for the optimization of the material performance in the middle temperature range. Here, we present a synthetic protocol for large scale production of covellite CuS nanoparticles at ambient temperature and atmosphere, and using water as a solvent. The crystal phase and stoichiometry of the particles are afterward tuned through an annealing process at a moderate temperature under inert or reducing atmosphere. While annealing under argon results in Cu1.8S nanopowder with a rhombohedral crystal phase, annealing in an atmosphere containing hydrogen leads to tetragonal Cu1.96S. High temperature X-ray diffraction analysis shows the material annealed in argon to transform to the cubic phase at ca. 400 K, while the material annealed in the presence of hydrogen undergoes two phase transitions, first to hexagonal and then to the cubic structure. The annealing atmosphere, temperature, and time allow adjustment of the density of copper vacancies and thus tuning of the charge carrier concentration and material transport properties. In this direction, the material annealed under Ar is characterized by higher electrical conductivities but lower Seebeck coefficients than the material annealed in the presence of hydrogen. By optimizing the charge carrier concentration through the annealing time, Cu2–xS with record figures of merit in the middle temperature range, up to 1.41 at 710 K, is obtained. We finally demonstrate that this strategy, based on a low-cost and scalable solution synthesis process, is also suitable for the production of high performance Cu2–xS layers using high throughput and cost-effective printing technologies."}],"date_updated":"2023-10-03T09:59:55Z","volume":15,"oa":1,"article_processing_charge":"No","acknowledgement":"This work was supported by the European Regional Development Funds. M.Y.L., X.H., T.Z., and K.X. thank the China Scholarship Council for scholarship support. M.I. acknowledges financial support from IST Austria. J.L. acknowledges support from the National Natural Science Foundation of China (No. 22008091), the funding for scientific research startup of Jiangsu University (No. 19JDG044), and Jiangsu Provincial Program for High-Level Innovative and Entrepreneurial Talents Introduction. J.L. is a Serra Húnter fellow and is grateful to the ICREA Academia program and projects MICINN/FEDER RTI2018-093996-B-C31 and GC 2017 SGR 128. ICN2 acknowledges funding from Generalitat de Catalunya 2017 SGR 327 and the Spanish MINECO ENE2017-85087-C3. ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. Part of the present work has been performed in the framework of Universitat Autònoma de Barcelona Materials Science PhD program. T.Z. has received funding from the CSC-UAB PhD scholarship program.","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","quality_controlled":"1","oa_version":"Submitted Version","_id":"9235","pmid":1,"publication_identifier":{"issn":["1936-0851"],"eissn":["1936-086X"]}},{"title":"Exclusive electron transport in Core@Shell PbTe@PbS colloidal semiconductor nanocrystal assemblies","external_id":{"isi":["000526301400057"],"pmid":["32073817"]},"doi":"10.1021/acsnano.9b08687","year":"2020","isi":1,"abstract":[{"lang":"eng","text":"Assemblies of colloidal semiconductor nanocrystals (NCs) in the form of thin solid films leverage the size-dependent quantum confinement properties and the wet chemical methods vital for the development of the emerging solution-processable electronics, photonics, and optoelectronics technologies. The ability to control the charge carrier transport in the colloidal NC assemblies is fundamental for altering their electronic and optical properties for the desired applications. Here we demonstrate a strategy to render the solids of narrow-bandgap NC assemblies exclusively electron-transporting by creating a type-II heterojunction via shelling. Electronic transport of molecularly cross-linked PbTe@PbS core@shell NC assemblies is measured using both a conventional solid gate transistor and an electric-double-layer transistor, as well as compared with those of core-only PbTe NCs. In contrast to the ambipolar characteristics demonstrated by many narrow-bandgap NCs, the core@shell NCs exhibit exclusive n-type transport, i.e., drastically suppressed contribution of holes to the overall transport. The PbS shell that forms a type-II heterojunction assists the selective carrier transport by heavy doping of electrons into the PbTe-core conduction level and simultaneously strongly localizes the holes within the NC core valence level. This strongly enhanced n-type transport makes these core@shell NCs suitable for applications where ambipolar characteristics should be actively suppressed, in particular, for thermoelectric and electron-transporting layers in photovoltaic devices."}],"author":[{"full_name":"Miranti, Retno","last_name":"Miranti","first_name":"Retno"},{"first_name":"Daiki","full_name":"Shin, Daiki","last_name":"Shin"},{"first_name":"Ricky Dwi","full_name":"Septianto, Ricky Dwi","last_name":"Septianto"},{"id":"43C61214-F248-11E8-B48F-1D18A9856A87","first_name":"Maria","full_name":"Ibáñez, Maria","last_name":"Ibáñez","orcid":"0000-0001-5013-2843"},{"first_name":"Maksym V.","last_name":"Kovalenko","full_name":"Kovalenko, Maksym V."},{"first_name":"Nobuhiro","full_name":"Matsushita, Nobuhiro","last_name":"Matsushita"},{"first_name":"Yoshihiro","last_name":"Iwasa","full_name":"Iwasa, Yoshihiro"},{"full_name":"Bisri, Satria Zulkarnaen","last_name":"Bisri","first_name":"Satria Zulkarnaen"}],"citation":{"chicago":"Miranti, Retno, Daiki Shin, Ricky Dwi Septianto, Maria Ibáñez, Maksym V. Kovalenko, Nobuhiro Matsushita, Yoshihiro Iwasa, and Satria Zulkarnaen Bisri. “Exclusive Electron Transport in Core@Shell PbTe@PbS Colloidal Semiconductor Nanocrystal Assemblies.” <i>ACS Nano</i>. American Chemical Society, 2020. <a href=\"https://doi.org/10.1021/acsnano.9b08687\">https://doi.org/10.1021/acsnano.9b08687</a>.","ieee":"R. Miranti <i>et al.</i>, “Exclusive electron transport in Core@Shell PbTe@PbS colloidal semiconductor nanocrystal assemblies,” <i>ACS Nano</i>, vol. 14, no. 3. American Chemical Society, pp. 3242–3250, 2020.","apa":"Miranti, R., Shin, D., Septianto, R. D., Ibáñez, M., Kovalenko, M. V., Matsushita, N., … Bisri, S. Z. (2020). Exclusive electron transport in Core@Shell PbTe@PbS colloidal semiconductor nanocrystal assemblies. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.9b08687\">https://doi.org/10.1021/acsnano.9b08687</a>","short":"R. Miranti, D. Shin, R.D. Septianto, M. Ibáñez, M.V. Kovalenko, N. Matsushita, Y. Iwasa, S.Z. Bisri, ACS Nano 14 (2020) 3242–3250.","ista":"Miranti R, Shin D, Septianto RD, Ibáñez M, Kovalenko MV, Matsushita N, Iwasa Y, Bisri SZ. 2020. Exclusive electron transport in Core@Shell PbTe@PbS colloidal semiconductor nanocrystal assemblies. ACS Nano. 14(3), 3242–3250.","ama":"Miranti R, Shin D, Septianto RD, et al. Exclusive electron transport in Core@Shell PbTe@PbS colloidal semiconductor nanocrystal assemblies. <i>ACS Nano</i>. 2020;14(3):3242-3250. doi:<a href=\"https://doi.org/10.1021/acsnano.9b08687\">10.1021/acsnano.9b08687</a>","mla":"Miranti, Retno, et al. “Exclusive Electron Transport in Core@Shell PbTe@PbS Colloidal Semiconductor Nanocrystal Assemblies.” <i>ACS Nano</i>, vol. 14, no. 3, American Chemical Society, 2020, pp. 3242–50, doi:<a href=\"https://doi.org/10.1021/acsnano.9b08687\">10.1021/acsnano.9b08687</a>."},"publication_status":"published","publication_identifier":{"eissn":["1936-086X"]},"pmid":1,"_id":"7634","quality_controlled":"1","oa_version":"None","acknowledgement":"This work is partly supported by Grants-in-Aid for Scientific Research by Young Scientist A (KAKENHI Wakate-A) No. JP17H04802, Grants-in-Aid for Scientific Research No. JP19H05602 from the Japan Society for the Promotion of Science, and RIKEN Incentive Research Grant (Shoreikadai) 2016. M.V.K. and M.I. acknowledge financial support from the European Union (EU) via FP7 ERC Starting Grant 2012 (Project NANOSOLID, GA No. 306733) and ETH Zurich via ETH career seed grant (SEED-18 16-2). Support from Cambridge Display Technology, Ltd., and Sumitomo Chemical Company is also acknowledged. We thank Mrs. T. Kikitsu and Dr. D. Hashizume (RIKEN-CEMS) for access to the transmission electron microscope facility.","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","article_processing_charge":"No","volume":14,"date_updated":"2023-08-18T10:25:40Z","scopus_import":"1","publisher":"American Chemical Society","language":[{"iso":"eng"}],"month":"03","article_type":"original","date_published":"2020-03-24T00:00:00Z","date_created":"2020-04-05T22:00:48Z","department":[{"_id":"MaIb"}],"intvolume":"        14","status":"public","day":"24","type":"journal_article","publication":"ACS Nano","issue":"3","page":"3242-3250"},{"publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"_id":"6566","pmid":1,"project":[{"call_identifier":"H2020","name":"ISTplus - Postdoctoral Fellowships","_id":"260C2330-B435-11E9-9278-68D0E5697425","grant_number":"754411"}],"oa_version":"Published Version","quality_controlled":"1","user_id":"4359f0d1-fa6c-11eb-b949-802e58b17ae8","article_processing_charge":"Yes (in subscription journal)","oa":1,"volume":13,"date_updated":"2023-08-28T12:20:53Z","abstract":[{"text":"Methodologies that involve the use of nanoparticles as “artificial atoms” to rationally build materials in a bottom-up fashion are particularly well-suited to control the matter at the nanoscale. Colloidal synthetic routes allow for an exquisite control over such “artificial atoms” in terms of size, shape, and crystal phase as well as core and surface compositions. We present here a bottom-up approach to produce Pb–Ag–K–S–Te nanocomposites, which is a highly promising system for thermoelectric energy conversion. First, we developed a high-yield and scalable colloidal synthesis route to uniform lead sulfide (PbS) nanorods, whose tips are made of silver sulfide (Ag2S). We then took advantage of the large surface-to-volume ratio to introduce a p-type dopant (K) by replacing native organic ligands with K2Te. Upon thermal consolidation, K2Te-surface modified PbS–Ag2S nanorods yield p-type doped nanocomposites with PbTe and PbS as major phases and Ag2S and Ag2Te as embedded nanoinclusions. Thermoelectric characterization of such consolidated nanosolids showed a high thermoelectric figure-of-merit of 1 at 620 K.","lang":"eng"}],"keyword":["colloidal nanoparticles","asymmetric nanoparticles","inorganic ligands","heterostructures","catalyst assisted growth","nanocomposites","thermoelectrics"],"author":[{"orcid":"0000-0001-5013-2843","last_name":"Ibáñez","full_name":"Ibáñez, Maria","first_name":"Maria","id":"43C61214-F248-11E8-B48F-1D18A9856A87"},{"last_name":"Genç","full_name":"Genç, Aziz","first_name":"Aziz"},{"first_name":"Roger","full_name":"Hasler, Roger","last_name":"Hasler"},{"id":"2A70014E-F248-11E8-B48F-1D18A9856A87","full_name":"Liu, Yu","last_name":"Liu","orcid":"0000-0001-7313-6740","first_name":"Yu"},{"last_name":"Dobrozhan","full_name":"Dobrozhan, Oleksandr","first_name":"Oleksandr"},{"first_name":"Olga","full_name":"Nazarenko, Olga","last_name":"Nazarenko"},{"first_name":"María de la","full_name":"Mata, María de la","last_name":"Mata"},{"first_name":"Jordi","full_name":"Arbiol, Jordi","last_name":"Arbiol"},{"first_name":"Andreu","full_name":"Cabot, Andreu","last_name":"Cabot"},{"full_name":"Kovalenko, Maksym V.","last_name":"Kovalenko","first_name":"Maksym V."}],"citation":{"apa":"Ibáñez, M., Genç, A., Hasler, R., Liu, Y., Dobrozhan, O., Nazarenko, O., … Kovalenko, M. V. (2019). Tuning transport properties in thermoelectric nanocomposites through inorganic ligands and heterostructured building blocks. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.9b00346\">https://doi.org/10.1021/acsnano.9b00346</a>","ieee":"M. Ibáñez <i>et al.</i>, “Tuning transport properties in thermoelectric nanocomposites through inorganic ligands and heterostructured building blocks,” <i>ACS Nano</i>, vol. 13, no. 6. American Chemical Society, pp. 6572–6580, 2019.","chicago":"Ibáñez, Maria, Aziz Genç, Roger Hasler, Yu Liu, Oleksandr Dobrozhan, Olga Nazarenko, María de la Mata, Jordi Arbiol, Andreu Cabot, and Maksym V. Kovalenko. “Tuning Transport Properties in Thermoelectric Nanocomposites through Inorganic Ligands and Heterostructured Building Blocks.” <i>ACS Nano</i>. American Chemical Society, 2019. <a href=\"https://doi.org/10.1021/acsnano.9b00346\">https://doi.org/10.1021/acsnano.9b00346</a>.","mla":"Ibáñez, Maria, et al. “Tuning Transport Properties in Thermoelectric Nanocomposites through Inorganic Ligands and Heterostructured Building Blocks.” <i>ACS Nano</i>, vol. 13, no. 6, American Chemical Society, 2019, pp. 6572–80, doi:<a href=\"https://doi.org/10.1021/acsnano.9b00346\">10.1021/acsnano.9b00346</a>.","ama":"Ibáñez M, Genç A, Hasler R, et al. Tuning transport properties in thermoelectric nanocomposites through inorganic ligands and heterostructured building blocks. <i>ACS Nano</i>. 2019;13(6):6572-6580. doi:<a href=\"https://doi.org/10.1021/acsnano.9b00346\">10.1021/acsnano.9b00346</a>","ista":"Ibáñez M, Genç A, Hasler R, Liu Y, Dobrozhan O, Nazarenko O, Mata M de la, Arbiol J, Cabot A, Kovalenko MV. 2019. Tuning transport properties in thermoelectric nanocomposites through inorganic ligands and heterostructured building blocks. ACS Nano. 13(6), 6572–6580.","short":"M. Ibáñez, A. Genç, R. Hasler, Y. Liu, O. Dobrozhan, O. Nazarenko, M. de la Mata, J. Arbiol, A. Cabot, M.V. Kovalenko, ACS Nano 13 (2019) 6572–6580."},"publication_status":"published","ddc":["540"],"isi":1,"title":"Tuning transport properties in thermoelectric nanocomposites through inorganic ligands and heterostructured building blocks","external_id":{"pmid":["31185159"],"isi":["000473248300043"]},"year":"2019","doi":"10.1021/acsnano.9b00346","ec_funded":1,"publication":"ACS Nano","issue":"6","page":"6572-6580","file_date_updated":"2020-07-14T12:47:33Z","intvolume":"        13","status":"public","day":"25","type":"journal_article","date_created":"2019-06-18T13:54:34Z","file":[{"creator":"dernst","file_id":"6644","content_type":"application/pdf","relation":"main_file","date_updated":"2020-07-14T12:47:33Z","access_level":"open_access","date_created":"2019-07-16T14:17:09Z","file_name":"2019_ACSNano_Ibanez.pdf","file_size":8628690}],"has_accepted_license":"1","department":[{"_id":"MaIb"}],"scopus_import":"1","publisher":"American Chemical Society","language":[{"iso":"eng"}],"month":"06","date_published":"2019-06-25T00:00:00Z","article_type":"original"},{"language":[{"iso":"eng"}],"scopus_import":"1","publisher":"American Chemical Society","date_published":"2018-01-19T00:00:00Z","article_type":"original","month":"01","date_created":"2021-11-26T15:15:00Z","status":"public","intvolume":"        12","type":"journal_article","day":"19","page":"1508-1518","publication":"ACS Nano","issue":"2","external_id":{"pmid":["29350911"]},"title":"A Programmable DNA origami platform for organizing intrinsically disordered nucleoporins within nanopore confinement","doi":"10.1021/acsnano.7b08044","year":"2018","author":[{"first_name":"Patrick D. Ellis","last_name":"Fisher","full_name":"Fisher, Patrick D. Ellis"},{"last_name":"Shen","full_name":"Shen, Qi","first_name":"Qi"},{"first_name":"Bernice","last_name":"Akpinar","full_name":"Akpinar, Bernice"},{"first_name":"Luke K.","full_name":"Davis, Luke K.","last_name":"Davis"},{"last_name":"Chung","full_name":"Chung, Kenny Kwok Hin","first_name":"Kenny Kwok Hin"},{"last_name":"Baddeley","full_name":"Baddeley, David","first_name":"David"},{"first_name":"Anđela","full_name":"Šarić, Anđela","last_name":"Šarić","orcid":"0000-0002-7854-2139","id":"bf63d406-f056-11eb-b41d-f263a6566d8b"},{"full_name":"Melia, Thomas J.","last_name":"Melia","first_name":"Thomas J."},{"full_name":"Hoogenboom, Bart W.","last_name":"Hoogenboom","first_name":"Bart W."},{"full_name":"Lin, Chenxiang","last_name":"Lin","first_name":"Chenxiang"},{"first_name":"C. Patrick","last_name":"Lusk","full_name":"Lusk, C. Patrick"}],"keyword":["general physics and astronomy"],"abstract":[{"text":"Nuclear pore complexes (NPCs) form gateways that control molecular exchange between the nucleus and the cytoplasm. They impose a diffusion barrier to macromolecules and enable the selective transport of nuclear transport receptors with bound cargo. The underlying mechanisms that establish these permeability properties remain to be fully elucidated but require unstructured nuclear pore proteins rich in Phe-Gly (FG)-repeat domains of different types, such as FxFG and GLFG. While physical modeling and in vitro approaches have provided a framework for explaining how the FG network contributes to the barrier and transport properties of the NPC, it remains unknown whether the number and/or the spatial positioning of different FG-domains along a cylindrical, ∼40 nm diameter transport channel contributes to their collective properties and function. To begin to answer these questions, we have used DNA origami to build a cylinder that mimics the dimensions of the central transport channel and can house a specified number of FG-domains at specific positions with easily tunable design parameters, such as grafting density and topology. We find the overall morphology of the FG-domain assemblies to be dependent on their chemical composition, determined by the type and density of FG-repeat, and on their architectural confinement provided by the DNA cylinder, largely consistent with here presented molecular dynamics simulations based on a coarse-grained polymer model. In addition, high-speed atomic force microscopy reveals local and reversible FG-domain condensation that transiently occludes the lumen of the DNA central channel mimics, suggestive of how the NPC might establish its permeability properties.","lang":"eng"}],"citation":{"chicago":"Fisher, Patrick D. Ellis, Qi Shen, Bernice Akpinar, Luke K. Davis, Kenny Kwok Hin Chung, David Baddeley, Anđela Šarić, et al. “A Programmable DNA Origami Platform for Organizing Intrinsically Disordered Nucleoporins within Nanopore Confinement.” <i>ACS Nano</i>. American Chemical Society, 2018. <a href=\"https://doi.org/10.1021/acsnano.7b08044\">https://doi.org/10.1021/acsnano.7b08044</a>.","apa":"Fisher, P. D. E., Shen, Q., Akpinar, B., Davis, L. K., Chung, K. K. H., Baddeley, D., … Lusk, C. P. (2018). A Programmable DNA origami platform for organizing intrinsically disordered nucleoporins within nanopore confinement. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.7b08044\">https://doi.org/10.1021/acsnano.7b08044</a>","ieee":"P. D. E. Fisher <i>et al.</i>, “A Programmable DNA origami platform for organizing intrinsically disordered nucleoporins within nanopore confinement,” <i>ACS Nano</i>, vol. 12, no. 2. American Chemical Society, pp. 1508–1518, 2018.","short":"P.D.E. Fisher, Q. Shen, B. Akpinar, L.K. Davis, K.K.H. Chung, D. Baddeley, A. Šarić, T.J. Melia, B.W. Hoogenboom, C. Lin, C.P. Lusk, ACS Nano 12 (2018) 1508–1518.","ista":"Fisher PDE, Shen Q, Akpinar B, Davis LK, Chung KKH, Baddeley D, Šarić A, Melia TJ, Hoogenboom BW, Lin C, Lusk CP. 2018. A Programmable DNA origami platform for organizing intrinsically disordered nucleoporins within nanopore confinement. ACS Nano. 12(2), 1508–1518.","ama":"Fisher PDE, Shen Q, Akpinar B, et al. A Programmable DNA origami platform for organizing intrinsically disordered nucleoporins within nanopore confinement. <i>ACS Nano</i>. 2018;12(2):1508-1518. doi:<a href=\"https://doi.org/10.1021/acsnano.7b08044\">10.1021/acsnano.7b08044</a>","mla":"Fisher, Patrick D. Ellis, et al. “A Programmable DNA Origami Platform for Organizing Intrinsically Disordered Nucleoporins within Nanopore Confinement.” <i>ACS Nano</i>, vol. 12, no. 2, American Chemical Society, 2018, pp. 1508–18, doi:<a href=\"https://doi.org/10.1021/acsnano.7b08044\">10.1021/acsnano.7b08044</a>."},"publication_status":"published","quality_controlled":"1","oa_version":"None","acknowledgement":"We thank J. Edel and members of the Lusk, Lin and Hoogenboom lab for discussion and acknowledge A. Pyne and R. Thorogate for support carrying out the AFM experiments. This work was funded by the NIH (R21GM109466 to CPL, CL and TJM, DP2GM114830 to CL, RO1GM105672 to CPL, and T32GM007223 to PDEF) and the UK Engineering and Physical Sciences Research Council (EP/L015277/1, EP/L504889/1, and EP/M028100/1).","user_id":"8b945eb4-e2f2-11eb-945a-df72226e66a9","publication_identifier":{"issn":["1936-0851"],"eissn":["1936-086X"]},"extern":"1","pmid":1,"_id":"10362","article_processing_charge":"No","date_updated":"2021-11-26T15:57:02Z","volume":12},{"doi":"10.1021/acsnano.6b04787","year":"2016","title":"Impact of heterogeneity and lattice bond strength on DNA triangle crystal growth","external_id":{"pmid":["27583560"]},"publication_status":"published","citation":{"mla":"Stahl, Evi, et al. “Impact of Heterogeneity and Lattice Bond Strength on DNA Triangle Crystal Growth.” <i>ACS Nano</i>, vol. 10, no. 10, American Chemical Society, 2016, pp. 9156–64, doi:<a href=\"https://doi.org/10.1021/acsnano.6b04787\">10.1021/acsnano.6b04787</a>.","ama":"Stahl E, Praetorius FM, de Oliveira Mann CC, Hopfner K-P, Dietz H. Impact of heterogeneity and lattice bond strength on DNA triangle crystal growth. <i>ACS Nano</i>. 2016;10(10):9156-9164. doi:<a href=\"https://doi.org/10.1021/acsnano.6b04787\">10.1021/acsnano.6b04787</a>","short":"E. Stahl, F.M. Praetorius, C.C. de Oliveira Mann, K.-P. Hopfner, H. Dietz, ACS Nano 10 (2016) 9156–9164.","ista":"Stahl E, Praetorius FM, de Oliveira Mann CC, Hopfner K-P, Dietz H. 2016. Impact of heterogeneity and lattice bond strength on DNA triangle crystal growth. ACS Nano. 10(10), 9156–9164.","ieee":"E. Stahl, F. M. Praetorius, C. C. de Oliveira Mann, K.-P. Hopfner, and H. Dietz, “Impact of heterogeneity and lattice bond strength on DNA triangle crystal growth,” <i>ACS Nano</i>, vol. 10, no. 10. American Chemical Society, pp. 9156–9164, 2016.","apa":"Stahl, E., Praetorius, F. M., de Oliveira Mann, C. C., Hopfner, K.-P., &#38; Dietz, H. (2016). Impact of heterogeneity and lattice bond strength on DNA triangle crystal growth. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/acsnano.6b04787\">https://doi.org/10.1021/acsnano.6b04787</a>","chicago":"Stahl, Evi, Florian M Praetorius, Carina C. de Oliveira Mann, Karl-Peter Hopfner, and Hendrik Dietz. “Impact of Heterogeneity and Lattice Bond Strength on DNA Triangle Crystal Growth.” <i>ACS Nano</i>. American Chemical Society, 2016. <a href=\"https://doi.org/10.1021/acsnano.6b04787\">https://doi.org/10.1021/acsnano.6b04787</a>."},"abstract":[{"text":"One key goal of DNA nanotechnology is the bottom-up construction of macroscopic crystalline materials. Beyond applications in fields such as photonics or plasmonics, DNA-based crystal matrices could possibly facilitate the diffraction-based structural analysis of guest molecules. Seeman and co-workers reported in 2009 the first designed crystal matrices based on a 38 kDa DNA triangle that was composed of seven chains. The crystal lattice was stabilized, unprecedentedly, by Watson–Crick base pairing. However, 3D crystallization of larger designed DNA objects that include more chains such as DNA origami remains an unsolved problem. Larger objects would offer more degrees of freedom and design options with respect to tailoring lattice geometry and for positioning other objects within a crystal lattice. The greater rigidity of multilayer DNA origami could also positively influence the diffractive properties of crystals composed of such particles. Here, we rationally explore the role of heterogeneity and Watson–Crick interaction strengths in crystal growth using 40 variants of the original DNA triangle as model multichain objects. Crystal growth of the triangle was remarkably robust despite massive chemical, geometrical, and thermodynamical sample heterogeneity that we introduced, but the crystal growth sensitively depended on the sequences of base pairs next to the Watson–Crick sticky ends of the triangle. Our results point to weak lattice interactions and high concentrations as decisive factors for achieving productive crystallization, while sample heterogeneity and impurities played a minor role.","lang":"eng"}],"author":[{"last_name":"Stahl","full_name":"Stahl, Evi","first_name":"Evi"},{"first_name":"Florian M","last_name":"Praetorius","full_name":"Praetorius, Florian M","id":"dfec9381-4341-11ee-8fd8-faa02bba7d62"},{"last_name":"de Oliveira Mann","full_name":"de Oliveira Mann, Carina C.","first_name":"Carina C."},{"first_name":"Karl-Peter","last_name":"Hopfner","full_name":"Hopfner, Karl-Peter"},{"full_name":"Dietz, Hendrik","last_name":"Dietz","first_name":"Hendrik"}],"date_updated":"2023-11-07T12:08:46Z","volume":10,"article_processing_charge":"No","_id":"14302","pmid":1,"publication_identifier":{"issn":["1936-0851"],"eissn":["1936-086X"]},"extern":"1","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","quality_controlled":"1","oa_version":"None","month":"09","article_type":"original","date_published":"2016-09-01T00:00:00Z","publisher":"American Chemical Society","scopus_import":"1","language":[{"iso":"eng"}],"date_created":"2023-09-06T12:52:00Z","day":"01","type":"journal_article","intvolume":"        10","status":"public","issue":"10","publication":"ACS Nano","page":"9156-9164"},{"intvolume":"         8","status":"public","day":"23","type":"journal_article","issue":"12","publication":"ACS Nano","page":"11913-11916","publisher":"American Chemical Society","scopus_import":"1","language":[{"iso":"eng"}],"month":"12","date_published":"2014-12-23T00:00:00Z","article_type":"original","date_created":"2023-08-01T09:45:42Z","abstract":[{"lang":"eng","text":"Nature has long inspired scientists with its seemingly unlimited ability to harness solar energy and to utilize it to drive various physiological processes. With the help of man-made molecular photoswitches, we now have the potential to outperform natural systems in many ways, with the ultimate goal of fabricating multifunctional materials that operate at different light wavelengths. An important challenge in developing light-controlled artificial molecular machines lies in attaining a detailed understanding of the photoisomerization-coupled conformational changes that occur in macromolecules and molecular assemblies. In this issue of ACS Nano, Bléger, Rabe, and co-workers use force microscopy to provide interesting insights into the behavior of individual photoresponsive molecules and to identify contraction, extension, and crawling events accompanying light-induced isomerization."}],"keyword":["General Physics and Astronomy","General Engineering","General Materials Science"],"author":[{"first_name":"Pintu K.","last_name":"Kundu","full_name":"Kundu, Pintu K."},{"id":"8e84690e-1e48-11ed-a02b-a1e6fb8bb53b","first_name":"Rafal","full_name":"Klajn, Rafal","last_name":"Klajn"}],"publication_status":"published","citation":{"ista":"Kundu PK, Klajn R. 2014. Watching single molecules move in response to light. ACS Nano. 8(12), 11913–11916.","short":"P.K. Kundu, R. Klajn, ACS Nano 8 (2014) 11913–11916.","mla":"Kundu, Pintu K., and Rafal Klajn. “Watching Single Molecules Move in Response to Light.” <i>ACS Nano</i>, vol. 8, no. 12, American Chemical Society, 2014, pp. 11913–16, doi:<a href=\"https://doi.org/10.1021/nn506656r\">10.1021/nn506656r</a>.","ama":"Kundu PK, Klajn R. Watching single molecules move in response to light. <i>ACS Nano</i>. 2014;8(12):11913-11916. doi:<a href=\"https://doi.org/10.1021/nn506656r\">10.1021/nn506656r</a>","chicago":"Kundu, Pintu K., and Rafal Klajn. “Watching Single Molecules Move in Response to Light.” <i>ACS Nano</i>. American Chemical Society, 2014. <a href=\"https://doi.org/10.1021/nn506656r\">https://doi.org/10.1021/nn506656r</a>.","apa":"Kundu, P. K., &#38; Klajn, R. (2014). Watching single molecules move in response to light. <i>ACS Nano</i>. American Chemical Society. <a href=\"https://doi.org/10.1021/nn506656r\">https://doi.org/10.1021/nn506656r</a>","ieee":"P. K. Kundu and R. Klajn, “Watching single molecules move in response to light,” <i>ACS Nano</i>, vol. 8, no. 12. American Chemical Society, pp. 11913–11916, 2014."},"pmid":1,"_id":"13399","extern":"1","publication_identifier":{"eissn":["1936-086X"],"issn":["1936-0851"]},"user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","oa_version":"None","quality_controlled":"1","volume":8,"date_updated":"2023-08-08T07:18:58Z","article_processing_charge":"No","title":"Watching single molecules move in response to light","external_id":{"pmid":["25474733"]},"year":"2014","doi":"10.1021/nn506656r"}]