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DOE OSTI · 3024016

Polaronic Quasiparticles in the Valence-Transition Compound TmSe 1−𝑥⁢ Te 𝑥

Min, Chul H. [Christian-Albrechts-Univ. zu Kiel (Germany); Norwegian Univ. of Science and Technology, Trondheim (Norway)] (ORCID:0000000227328773)·Müller, S. [Univ. of Wurzburg (Germany)] (ORCID:0000000240025005)·Choi, W. J. [Daegu Gyeongbuk Institute of Science and Technology (DGIST) (Korea, Republic of)]·Dudy, L. [Synchrotron SOLEIL, Gif-sur-Yvette (France)] (ORCID:0000000242045405)·Zabolotnyy, V. [Univ. of Wurzburg (Germany)] (ORCID:0000000276327312)·Heber, M. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)]·Denlinger, J. D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000176451631)·Kang, C.-J. [Chungnam National Univ., Daejeon (Korea, Republic of)] (ORCID:0000000328954888)·Kalläne, M. [Christian-Albrechts-Univ. zu Kiel (Germany)]·Wind, N. [Christian-Albrechts-Univ. zu Kiel (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)] (ORCID:0000000277580678)·Scholz, M. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000156699912)·Lee, T. L. [Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.]·Schlueter, C. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000287453074)·Gloskovskii, A. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000222915207)·Rienks, E. D. L. [Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy] (ORCID:0000000291920552)·Hinkov, V. [Univ. of Wurzburg (Germany)] (ORCID:0000000266021002)·Bentmann, H. [Norwegian Univ. of Science and Technology, Trondheim (Norway)]·Kwon, Y. S. [Daegu Gyeongbuk Institute of Science and Technology (DGIST) (Korea, Republic of)] (ORCID:0000000160151183)·Reinert, F. [Univ. of Wurzburg (Germany)] (ORCID:0000000179931171)·Kim, H.-D. [Pohang Accelerator Laboratory (PAL) (Korea, Republic of)]·Rossnagel, K. [Christian-Albrechts-Univ. zu Kiel (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000151070090)

Abstract

Exotic quasiparticle states have been proposed in mixed-valent compounds exhibiting valence transitions. However, clear spectroscopic evidence identifying these states has remained elusive. Here, using synchrotron-based hard x-ray and extreme ultraviolet photoemission spectroscopy, we have probed the Tm 3⁢𝑑 and 4⁢𝑓 emissions in TmSe 1−𝑥 ⁢Te 𝑥 , where a Te concentration-dependent semimetal–insulator transition occurs alongside the valence transition. Our photoemission results, which are characteristic of the bulk, track this combined transition across the critical concentration (𝑥 𝑐 = 0.29). Notably, our results reveal a noninteger valence for the insulating phase and a novel quasiparticle excitation in the semimetallic phase: a Holstein polaron that extends beyond the standard periodic Anderson model.

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Min, Chul H. [Christian-Albrechts-Univ. zu Kiel (Germany); Norwegian Univ. of Science and Technology, Trondheim (Norway)] (ORCID:0000000227328773), Müller, S. [Univ. of Wurzburg (Germany)] (ORCID:0000000240025005), Choi, W. J. [Daegu Gyeongbuk Institute of Science and Technology (DGIST) (Korea, Republic of)], Dudy, L. [Synchrotron SOLEIL, Gif-sur-Yvette (France)] (ORCID:0000000242045405), Zabolotnyy, V. [Univ. of Wurzburg (Germany)] (ORCID:0000000276327312), Heber, M. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)], Denlinger, J. D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000176451631), Kang, C.-J. [Chungnam National Univ., Daejeon (Korea, Republic of)] (ORCID:0000000328954888), Kalläne, M. [Christian-Albrechts-Univ. zu Kiel (Germany)], Wind, N. [Christian-Albrechts-Univ. zu Kiel (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)] (ORCID:0000000277580678), Scholz, M. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000156699912), Lee, T. L. [Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.], Schlueter, C. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000287453074), Gloskovskii, A. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000222915207), Rienks, E. D. L. [Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy] (ORCID:0000000291920552), Hinkov, V. [Univ. of Wurzburg (Germany)] (ORCID:0000000266021002), Bentmann, H. [Norwegian Univ. of Science and Technology, Trondheim (Norway)], Kwon, Y. S. [Daegu Gyeongbuk Institute of Science and Technology (DGIST) (Korea, Republic of)] (ORCID:0000000160151183), Reinert, F. [Univ. of Wurzburg (Germany)] (ORCID:0000000179931171), Kim, H.-D. [Pohang Accelerator Laboratory (PAL) (Korea, Republic of)], Rossnagel, K. [Christian-Albrechts-Univ. zu Kiel (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)] (ORCID:0000000151070090). 2025-10-29. Polaronic Quasiparticles in the Valence-Transition Compound TmSe 1−𝑥⁢ Te 𝑥. https://doi.org/10.1103/72dv-ynm2

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