{"article_number":"023101","publication_identifier":{"issn":["2469-9926"],"eissn":["2469-9934"]},"article_processing_charge":"No","intvolume":"       109","title":"Modeling laser pulses as δ kicks: Reevaluating the impulsive limit in molecular rotational dynamics","citation":{"mla":"Karle, Volker, and Mikhail Lemeshko. “Modeling Laser Pulses as δ Kicks: Reevaluating the Impulsive Limit in Molecular Rotational Dynamics.” <i>Physical Review A</i>, vol. 109, no. 2, 023101, American Physical Society, 2024, doi:<a href=\"https://doi.org/10.1103/PhysRevA.109.023101\">10.1103/PhysRevA.109.023101</a>.","ista":"Karle V, Lemeshko M. 2024. Modeling laser pulses as δ kicks: Reevaluating the impulsive limit in molecular rotational dynamics. Physical Review A. 109(2), 023101.","ieee":"V. Karle and M. Lemeshko, “Modeling laser pulses as δ kicks: Reevaluating the impulsive limit in molecular rotational dynamics,” <i>Physical Review A</i>, vol. 109, no. 2. American Physical Society, 2024.","short":"V. Karle, M. Lemeshko, Physical Review A 109 (2024).","apa":"Karle, V., &#38; Lemeshko, M. (2024). Modeling laser pulses as δ kicks: Reevaluating the impulsive limit in molecular rotational dynamics. <i>Physical Review A</i>. American Physical Society. <a href=\"https://doi.org/10.1103/PhysRevA.109.023101\">https://doi.org/10.1103/PhysRevA.109.023101</a>","chicago":"Karle, Volker, and Mikhail Lemeshko. “Modeling Laser Pulses as δ Kicks: Reevaluating the Impulsive Limit in Molecular Rotational Dynamics.” <i>Physical Review A</i>. American Physical Society, 2024. <a href=\"https://doi.org/10.1103/PhysRevA.109.023101\">https://doi.org/10.1103/PhysRevA.109.023101</a>.","ama":"Karle V, Lemeshko M. Modeling laser pulses as δ kicks: Reevaluating the impulsive limit in molecular rotational dynamics. <i>Physical Review A</i>. 2024;109(2). doi:<a href=\"https://doi.org/10.1103/PhysRevA.109.023101\">10.1103/PhysRevA.109.023101</a>"},"scopus_import":"1","quality_controlled":"1","volume":109,"date_published":"2024-02-01T00:00:00Z","year":"2024","oa":1,"abstract":[{"lang":"eng","text":"The impulsive limit (the “sudden approximation”) has been widely employed to describe the interaction between molecules and short, far-off-resonant laser pulses. This approximation assumes that the timescale of the laser-molecule interaction is significantly shorter than the internal rotational period of the molecule, resulting in the rotational motion being instantaneously “frozen” during the interaction. This simplified description of the laser-molecule interaction is incorporated in various theoretical models predicting rotational dynamics of molecules driven by short laser pulses. In this theoretical work, we develop an effective theory for ultrashort laser pulses by examining the full time-evolution operator and solving the time-dependent Schrödinger equation at the operator level. Our findings reveal a critical angular momentum, lcrit, at which the impulsive limit breaks down. In other words, the validity of the sudden approximation depends not only on the pulse duration but also on its intensity, since the latter determines how many angular momentum states are populated. We explore both ultrashort multicycle (Gaussian) pulses and the somewhat less studied half-cycle pulses, which produce distinct effective potentials. We discuss the limitations of the impulsive limit and propose a method that rescales the effective matrix elements, enabling an improved and more accurate description of laser-molecule interactions."}],"main_file_link":[{"open_access":"1","url":"https://doi.org/10.48550/arXiv.2307.07256"}],"language":[{"iso":"eng"}],"day":"01","author":[{"first_name":"Volker","orcid":"0000-0002-6963-0129","last_name":"Karle","full_name":"Karle, Volker","id":"D7C012AE-D7ED-11E9-95E8-1EC5E5697425"},{"orcid":"0000-0002-6990-7802","last_name":"Lemeshko","first_name":"Mikhail","id":"37CB05FA-F248-11E8-B48F-1D18A9856A87","full_name":"Lemeshko, Mikhail"}],"user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","type":"journal_article","date_updated":"2024-02-26T09:45:20Z","oa_version":"Preprint","doi":"10.1103/PhysRevA.109.023101","department":[{"_id":"MiLe"}],"project":[{"name":"Angulon: physics and applications of a new quasiparticle","_id":"2688CF98-B435-11E9-9278-68D0E5697425","grant_number":"801770","call_identifier":"H2020"}],"acknowledgement":"We thank Bretislav Friedrich, Marjan Mirahmadi, Artem Volosniev, and Burkhard Schmidt for insightful discussions. M.L. acknowledges support by the European Research Council (ERC) under Starting Grant No. 801770 (ANGULON).","ec_funded":1,"_id":"15004","article_type":"original","status":"public","external_id":{"arxiv":["2307.07256"]},"publisher":"American Physical Society","publication_status":"published","date_created":"2024-02-18T23:01:01Z","month":"02","issue":"2","publication":"Physical Review A"}