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Layered metal phosphorus trichalcogenides (MPX3) feature bandgaps spanning the visible to ultraviolet range and exhibit a complex interplay between excitons, phonons, and defects. Here we use static and time-resolved photoluminescence and femtosecond broadband transient reflectivity to investigate the temperature-dependent ultrafast carrier dynamics in layered HgPSe3, a semiconductor with a quasi-direct bandgap near 2 eV. We identify distinct sub-bandgap photoluminescence features that become prominent at low temperature. Their temperature and fluence dependence strongly indicate radiative recombination involving localized states. The transient reflectivity map displays three features associated with interband optical transitions in the visible range, as corroborated by density functional theory band structure calculations. These features exhibit fluence-dependent decay dynamics, indicating a competition between carrier localization into sub-bandgap states, state-filling effects that limit the available electronic phase space for hot-carrier relaxation, and phonon-bottleneck-limited carrier cooling. Our results provide new insights into the ultrafast carrier dynamics of HgPSe3 and establish a framework for understanding the role of sub-bandgap states in MPX3 semiconductors, with potential implications for broadband optoelectronic and photodetection applications.<\/jats:p>","DOI":"10.1021\/acs.jpcc.6c03448","type":"journal-article","created":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T00:01:22Z","timestamp":1790899282000},"page":"14220-14229","source":"Crossref","is-referenced-by-count":0,"title":["The Interplay of\nPhonons and Subgap States Governs\nUltrafast Carrier Dynamics in Layered HgPSe3"],"prefix":"10.1021","volume":"130","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2567-3335","authenticated-orcid":true,"given":"Alessandro","family":"Baserga","sequence":"first","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2331-3088","authenticated-orcid":true,"given":"Mi\u0142osz","family":"Rybak","sequence":"additional","affiliation":[{"name":"Wroc\u0142aw University of Science and Technology , , Wybrzez\u0307e Wyspian\u0301skiego 27 , ,","place":["Wroc\u0142aw, Poland, 50-370"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-3243-8666","authenticated-orcid":true,"given":"Micol","family":"Bertolotti","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8610-8028","authenticated-orcid":true,"given":"Antonella","family":"Treglia","sequence":"additional","affiliation":[{"name":"Istituto Italiano di Tecnologia , ,","place":["Milano, Italy, 20134"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1783-6974","authenticated-orcid":true,"given":"Samim","family":"Sardar","sequence":"additional","affiliation":[{"name":"Istituto Italiano di Tecnologia , ,","place":["Milano, Italy, 20134"]},{"name":"National Institute of Technology Warangal , , ,","place":["Telangana, India, 506004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-7563-1022","authenticated-orcid":true,"given":"Valentino","family":"Jadris\u030cko","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-1822-7945","authenticated-orcid":true,"given":"Matteo","family":"Ghezzi","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2349-566X","authenticated-orcid":true,"given":"Giuseppe Maria","family":"Paterno\u0300","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cosimo","family":"D\u2019Andrea","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]},{"name":"Istituto Italiano di Tecnologia , ,","place":["Milano, Italy, 20134"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6914-4537","authenticated-orcid":true,"given":"Annamaria","family":"Petrozza","sequence":"additional","affiliation":[{"name":"Istituto Italiano di Tecnologia , ,","place":["Milano, Italy, 20134"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1391-4448","authenticated-orcid":true,"given":"Zdenek","family":"Sofer","sequence":"additional","affiliation":[{"name":"University of Chemistry and Technology Prague , , Technicka\u0301 5 , ,","place":["Prague 6, Czech Republic, 166 28"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1393-0317","authenticated-orcid":true,"given":"Artur P.","family":"Herman","sequence":"additional","affiliation":[{"name":"Wroc\u0142aw University of Science and Technology , , Wybrzez\u0307e Wyspian\u0301skiego 27 , ,","place":["Wroc\u0142aw, Poland, 50-370"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2593-9172","authenticated-orcid":true,"given":"Robert","family":"Kudrawiec","sequence":"additional","affiliation":[{"name":"Wroc\u0142aw University of Science and Technology , , Wybrzez\u0307e Wyspian\u0301skiego 27 , ,","place":["Wroc\u0142aw, Poland, 50-370"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9534-2702","authenticated-orcid":true,"given":"Giulio","family":"Cerullo","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Giulia","family":"Folpini","sequence":"additional","affiliation":[{"name":"Istituto Italiano di Tecnologia , ,","place":["Milano, Italy, 20134"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2563-9970","authenticated-orcid":true,"given":"Nikolas","family":"Antonatos","sequence":"additional","affiliation":[{"name":"Wroc\u0142aw University of Science and Technology , , Wybrzez\u0307e Wyspian\u0301skiego 27 , ,","place":["Wroc\u0142aw, Poland, 50-370"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6613-9644","authenticated-orcid":true,"given":"Christoph","family":"Gadermaier","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8582-3185","authenticated-orcid":true,"given":"Stefano","family":"Dal Conte","sequence":"additional","affiliation":[{"name":"Politecnico di Milano , , ,","place":["Milan, Italy, 20133"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,1]]},"reference":[{"key":"2026101508085944100_cit1","first-page":"1","volume-title":"Two-Dimensional Metal\nPhosphorus Trichalcogenide Nanostructure for Sustainable Energy Conversion","author":"Wang","year":"2022"},{"key":"2026101508085944100_cit2","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.94.184428","article-title":"Electronic and magnetic\nproperties\nof single-layer MPX3 metal\nphosphorous trichalcogenides","volume":"94","author":"Chittari","year":"2016","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit3","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201802151","article-title":"New Frontiers on van der Waals Layered\nMetal Phosphorous\nTrichalcogenides","volume":"28","author":"Wang","year":"2018","journal-title":"Adv. Funct. Mater."},{"key":"2026101508085944100_cit4","doi-asserted-by":"publisher","DOI":"10.3389\/fmats.2024.1362744","article-title":"MPX3 van\nder Waals magnets under pressure (M = Mn, Ni, V, Fe, Co, Cd; X = S,\nSe)","volume":"11","author":"Matsuoka","year":"2024","journal-title":"Front. Mater."},{"key":"2026101508085944100_cit5","doi-asserted-by":"publisher","first-page":"851","DOI":"10.1039\/C9RA09030D","article-title":"Electronic,\nmagnetic and optical properties of MnPX3 (X = S, Se) monolayers\nwith and without chalcogen defects: a first-principles study","volume":"10","author":"Yang","year":"2020","journal-title":"RSC Adv."},{"key":"2026101508085944100_cit6","doi-asserted-by":"publisher","DOI":"10.1038\/s41535-020-00259-5","article-title":"Piezochromism in the magnetic chalcogenide\nMnPS3","volume":"5","author":"Harms","year":"2020","journal-title":"npj Quantum Mater."},{"key":"2026101508085944100_cit7","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adn6216","article-title":"Giant nonlinear optical\nwave mixing\nin a van der Waals correlated insulator","volume":"10","author":"Yue","year":"2024","journal-title":"Sci.\nAdv."},{"key":"2026101508085944100_cit8","doi-asserted-by":"publisher","first-page":"2560","DOI":"10.1039\/D0TA09752G","article-title":"Two-dimensional\ntransition metal phosphorous trichalcogenides (MPX3): a\nreview on emerging trends, current state and future perspectives","volume":"9","author":"Samal","year":"2021","journal-title":"J. Mater. Chem. A"},{"key":"2026101508085944100_cit9","doi-asserted-by":"publisher","first-page":"1738","DOI":"10.1021\/acsnano.5b05927","article-title":"Weak Van der Waals\nStacking, Wide-Range Band Gap, and Raman Study on Ultrathin Layers\nof Metal Phosphorus Trichalcogenides","volume":"10","author":"Du","year":"2016","journal-title":"ACS Nano"},{"key":"2026101508085944100_cit10","doi-asserted-by":"publisher","first-page":"2836","DOI":"10.1021\/acsami.0c19530","article-title":"High-Performance Phototransistors\nBased on MnPSe3 and Its Hybrid Structures with Au Nanoparticles","volume":"13","author":"Han","year":"2021","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026101508085944100_cit11","doi-asserted-by":"publisher","first-page":"8834","DOI":"10.1039\/D2TC00904H","article-title":"Layered selenophosphate\nHgPSe3 single crystals: a new candidate for X-ray to visible\nlight photodetectors","volume":"10","author":"Liao","year":"2022","journal-title":"J. Mater. Chem. C"},{"key":"2026101508085944100_cit12","doi-asserted-by":"publisher","first-page":"3053","DOI":"10.1021\/acs.nanolett.4c04945","article-title":"Unraveling the Nanosecond\nPhotoresponse\nof Layered HgPSe3","volume":"25","author":"Antonatos","year":"2025","journal-title":"Nano Lett."},{"key":"2026101508085944100_cit13","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.106.035137","article-title":"Proximity effects in\ngraphene on monolayers of transition-metal\nphosphorus trichalcogenides MPX3 (M: Mn, Fe, Ni, Co, andX: S, Se)","volume":"106","author":"Zollner","year":"2022","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit14","doi-asserted-by":"publisher","first-page":"8853","DOI":"10.1039\/D5NR05417F","article-title":"Pressure-induced phase transition\non layered HgPSe3 revealed by optical, structural and vibrational\nstudies","volume":"18","author":"de Simoni","year":"2026","journal-title":"Nanoscale"},{"key":"2026101508085944100_cit15","doi-asserted-by":"publisher","first-page":"409","DOI":"10.1016\/j.cjph.2024.12.016","article-title":"Raman spectroscopy\nof HgPSe3 thin flakes and its application to near UV-to-visible\nphotodetectors","volume":"93","author":"Chuang","year":"2025","journal-title":"Chin. J. Phys."},{"key":"2026101508085944100_cit16","doi-asserted-by":"publisher","first-page":"15","DOI":"10.1016\/0927-0256(96)00008-0","article-title":"Efficiency\nof ab-initio total energy calculations for\nmetals and semiconductors using a plane-wave basis set","volume":"6","author":"Kresse","year":"1996","journal-title":"Comput. Mater. Sci."},{"key":"2026101508085944100_cit17","doi-asserted-by":"publisher","DOI":"10.1063\/1.1926272","article-title":"The Perdew\u2013Burke\u2013Ernzerhof\nexchange-correlation functional applied to the G2\u20131 test set\nusing a plane-wave basis set","volume":"122","author":"Paier","year":"2005","journal-title":"J. Chem. Phys."},{"key":"2026101508085944100_cit18","doi-asserted-by":"publisher","first-page":"329","DOI":"10.1016\/S0010-4655(00)00244-7","article-title":"A Projector Augmented Wave (PAW)\ncode for electronic structure calculations, Part I: atompaw for generating\natom-centered functions","volume":"135","author":"Holzwarth","year":"2001","journal-title":"Comput. Phys. Commun."},{"key":"2026101508085944100_cit19","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.13.5188","article-title":"Special points for\nBrillouin-zone integrations","volume":"13","author":"Monkhorst","year":"1976","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit20","doi-asserted-by":"publisher","DOI":"10.1063\/1.3382344","article-title":"A consistent and accurate\nab initio parametrization of density functional dispersion correction\n(DFT-D) for the 94 elements H-Pu","volume":"132","author":"Grimme","year":"2010","journal-title":"J. Chem. Phys."},{"key":"2026101508085944100_cit21","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.73.045112","article-title":"Linear optical properties in the projector-augmented\nwave methodology","volume":"73","author":"Gajdos\u030c","year":"2006","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit22","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevResearch.2.032019","article-title":"Accurate optical spectra through\ntime-dependent density functional theory based on screening-dependent\nhybrid functionals","volume":"2","author":"Tal","year":"2020","journal-title":"Phys. Rev. Res."},{"key":"2026101508085944100_cit23","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.92.045209","article-title":"Beyond the\nTamm-Dancoff approximation\nfor extended systems using exact diagonalization","volume":"92","author":"Sander","year":"2015","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit24","doi-asserted-by":"publisher","first-page":"2338","DOI":"10.1021\/acs.jpclett.8b00919","article-title":"Doubly Screened\nHybrid Functional: An Accurate First-Principles Approach for Both\nNarrow- and Wide-Gap Semiconductors","volume":"9","author":"Cui","year":"2018","journal-title":"J. Phys.\nChem. Lett."},{"key":"2026101508085944100_cit25","doi-asserted-by":"publisher","DOI":"10.1088\/1361-648X\/ab4150","article-title":"Assessing model-dielectric-dependent\nhybrid functionals on the antiferromagnetic transition-metal monoxides\nMnO, FeO, CoO, and NiO","volume":"32","author":"Liu","year":"2020","journal-title":"J. Phys.: Condens. Matter"},{"key":"2026101508085944100_cit26","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevMaterials.2.073803","article-title":"Nonempirical\ndielectric-dependent hybrid functional with range separation for semiconductors\nand insulators","volume":"2","author":"Chen","year":"2018","journal-title":"Phys. Rev. Mater."},{"key":"2026101508085944100_cit27","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.112.096401","article-title":"Ionization Potentials\nof Solids: The Importance of Vertex Corrections","volume":"112","author":"Gru\u0308neis","year":"2014","journal-title":"Phys. Rev. Lett."},{"key":"2026101508085944100_cit28","doi-asserted-by":"publisher","first-page":"1272","DOI":"10.1107\/S0021889811038970","article-title":"VESTA3 for three-dimensional visualization of crystal,\nvolumetric and morphology data","volume":"44","author":"Momma","year":"2011","journal-title":"J. Appl. Crystallogr."},{"key":"2026101508085944100_cit29","doi-asserted-by":"publisher","first-page":"17962","DOI":"10.1021\/acsnano.5c19936","article-title":"Defect-Induced\nSingle-Photon Emission in ZnPS3","volume":"20","author":"Zawadzka","year":"2026","journal-title":"ACS Nano"},{"key":"2026101508085944100_cit30","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202523655","article-title":"Functional Indium Vacancies\nin Indium Phosphors Chalcogenides","volume":"38","author":"Li","year":"2026","journal-title":"Adv. Mater."},{"key":"2026101508085944100_cit31","doi-asserted-by":"publisher","DOI":"10.1016\/j.esci.2023.100204","article-title":"Unlocking\npower\nof neighboring vacancies in boosting hydrogen evolution reactions\non two-dimensional NiPS3 monolayer","volume":"4","author":"Han","year":"2024","journal-title":"eScience"},{"key":"2026101508085944100_cit32","doi-asserted-by":"publisher","DOI":"10.1002\/pssa.202000101","article-title":"Mechanisms\nof Thermal Quenching of Defect-Related Luminescence in Semiconductors","volume":"218","author":"Reshchikov","year":"2021","journal-title":"Phys. Status Solidi A"},{"key":"2026101508085944100_cit33","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.64.115205","article-title":"Analysis of the\ntemperature and excitation intensity\ndependencies of photoluminescence in undoped GaN films","volume":"64","author":"Reshchikov","year":"2001","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit34","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.84.075212","article-title":"Tunable and abrupt\nthermal quenching\nof photoluminescence in high-resistivity Zn-doped GaN","volume":"84","author":"Reshchikov","year":"2011","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit35","doi-asserted-by":"publisher","DOI":"10.1143\/JJAP.37.550","article-title":"Negative Thermal\nQuenching Curves in Photoluminescence of Solids","volume":"37","author":"Shibata","year":"1998","journal-title":"Jpn. J. Appl. Phys."},{"key":"2026101508085944100_cit36","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1016\/j.nimb.2017.09.018","article-title":"Negative thermal quenching\nof the defects in GaInP top cell with temperature-dependent photoluminescence\nanalysis","volume":"414","author":"Junling","year":"2018","journal-title":"Nucl. Instrum. Methods Phys. Res.,\nSect. B"},{"key":"2026101508085944100_cit37","doi-asserted-by":"publisher","first-page":"3851","DOI":"10.1021\/acs.chemmater.8b05300","article-title":"Unraveling the Mechanisms of Thermal\nQuenching of Luminescence in Ce3+-Doped Garnet Phosphors","volume":"31","author":"Lin","year":"2019","journal-title":"Chem. Mater."},{"key":"2026101508085944100_cit38","doi-asserted-by":"publisher","first-page":"9270","DOI":"10.1021\/acs.jpcc.4c00562","article-title":"Electronic Band Structure and Optical Properties of\nHgPS3 Crystal and Layers","volume":"128","author":"de Simoni","year":"2024","journal-title":"J. Phys.\nChem. C"},{"key":"2026101508085944100_cit39","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.45.8989","article-title":"Excitation-power dependence of the\nnear-band edge photoluminescence of semiconductors","volume":"45","author":"Schmidt","year":"1992","journal-title":"Phys. Rev. B"},{"key":"2026101508085944100_cit40","doi-asserted-by":"publisher","first-page":"10791","DOI":"10.1002\/anie.201915708","article-title":"Metal Coordination\nSphere Deformation Induced Highly\nStokes-Shifted, Ultra Broadband Emission in 2D Hybrid Lead-Bromide\nPerovskites and Investigation of Its Origin","volume":"59","author":"Febriansyah","year":"2020","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026101508085944100_cit41","doi-asserted-by":"publisher","first-page":"2898","DOI":"10.1021\/acsnano.3c07236","article-title":"Strong Exciton\u2013Phonon\nCoupling as a Fingerprint of Magnetic Ordering in van der Waals Layered\nCrSBr","volume":"18","author":"Lin","year":"2024","journal-title":"ACS Nano"},{"key":"2026101508085944100_cit42","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202413438","article-title":"Intrinsic\nLocalized Excitons in MoSe2\/CrSBr Heterostructure","volume":"37","author":"Huang","year":"2025","journal-title":"Adv. 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