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Semiconducting WTe<jats:sub>2<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>S<jats:sub>2(1\u2010<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic><jats:sub>)<\/jats:sub> monolayer possesses two inequivalent valleys in the Brillouin zone, each valley coupling selectively with circularly polarized light (CPL). The degree of valley polarization (DVP) under the excitation of CPL represents the purity of valley polarized photoluminescence (PL), a critical parameter for opto\u2010valleytronic applications. Here, new strategies to efficiently tailor the valley\u2010polarized PL from semiconducting monolayer WTe<jats:sub>2<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic>S<jats:sub>2(1\u2010<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic><jats:sub>)<\/jats:sub> at room temperature (RT) through alloying and back\u2010gating are presented. The DVP at RT is found to increase drastically from &lt; 5% in WS<jats:sub>2<\/jats:sub> to 40% in WTe<jats:sub>0.12<\/jats:sub>S<jats:sub>1.88<\/jats:sub> by Te\u2010alloying to enhance the spin\u2010orbit coupling. Further enhancement and control of the DVP from 40% up to 75% is demonstrated by electrostatically doping the monolayer WTe<jats:sub>0.12<\/jats:sub>S<jats:sub>1.88<\/jats:sub> via metallic 1T\u2032\u2010WTe<jats:sub>2<\/jats:sub> electrodes, where the use of 1T\u2032\u2010WTe<jats:sub>2<\/jats:sub> substantially lowers the Schottky barrier height (SBH) and weakens the Fermi\u2010level pinning of the electrical contacts. The demonstration of drastically enhanced DVP and electrical tunability in the valley\u2010polarized emission from 1T\u2032\u2010WTe<jats:sub>2<\/jats:sub>\/WTe<jats:sub>0.12<\/jats:sub>S<jats:sub>1.88<\/jats:sub> heterostructures paves new pathways towards harnessing valley excitons in ultrathin valleytronic devices for RT applications.<\/jats:p>","DOI":"10.1002\/advs.202304890","type":"journal-article","created":{"date-parts":[[2023,11,17]],"date-time":"2023-11-17T03:35:03Z","timestamp":1700192103000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Dramatically Enhanced Valley\u2010Polarized Emission by Alloying and Electrical Tuning of Monolayer WTe<sub>2<\/sub><i><sub>x<\/sub><\/i>S<sub>2(1\u2010<\/sub><i><sub>x<\/sub><\/i><sub>)<\/sub> Alloys at Room Temperature with 1T\u2032\u2010WTe<sub>2<\/sub>\u2010Contact"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0037-1277","authenticated-orcid":false,"given":"Wei\u2010Hsiang","family":"Lin","sequence":"first","affiliation":[{"name":"Department of Applied Physics California Institute of Technology  Pasadena CA 91125 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chia\u2010Shuo","family":"Li","sequence":"additional","affiliation":[{"name":"Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering National Taiwan University  Taipei Taiwan 106 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chih\u2010I","family":"Wu","sequence":"additional","affiliation":[{"name":"Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering National Taiwan University  Taipei Taiwan 106 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"George R.","family":"Rossman","sequence":"additional","affiliation":[{"name":"Department of Geological and Planetary Sciences California Institute of Technology  Pasadena CA 91125 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9435-0201","authenticated-orcid":false,"given":"Harry A.","family":"Atwater","sequence":"additional","affiliation":[{"name":"Department of Applied Physics California Institute of Technology  Pasadena CA 91125 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1826-419X","authenticated-orcid":false,"given":"Nai\u2010Chang","family":"Yeh","sequence":"additional","affiliation":[{"name":"Department of Physics California Institute of Technology  Pasadena CA 91125 USA"},{"name":"Kavli Nanoscience Institute California Institute of Technology  Pasadena CA 91125 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