Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms

Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms Haowen Zhou, William Perreault, Nandini Mukherjee, Richard Zare This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-356225/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 02 May, 2022 Read the published version in Nature Chemistry → Version 1 posted You are reading this latest preprint version Abstract The dynamics of a resonant oriented scattering process dominated by a single partial wave provide the most sensitive probe of the long-range anisotropic forces important to chemical reactions. Here, we control the collision temperature and geometry to probe the dynamics of the cold (<2 K) rotationally inelastic scattering of a pair of optically state-prepared D2 molecules. The collision temperature is manipulated by combining the strobing action of laser state preparation and detection with the velocity dispersion of the molecular beam. When the bond axes are aligned parallel to the collision velocity, the scattering rate drops by nearly an order of magnitude when collision energies >1 K are removed, demonstrating a clear geometry-dependent resonance. Using partial wave analysis of the measured scattering angular distribution, we determine that an l = 2 shape resonance originates from the collisions between a pair of aligned D2 molecules. Our experiment illustrates the strong anisotropy of the long-range quadrupole-quadrupole interaction that controls the dynamic resonance for diatom-diatom collisions. Physical Chemistry anisotropic resonant dynamics chemical physics Figures Figure 1 Figure 2 Figure 3 Figure 4 Full Text Due to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the manuscript can be downloaded and accessed as a PDF. Additional Declarations There is NO Competing Interest. Cite Share Download PDF Status: Published Journal Publication published 02 May, 2022 Read the published version in Nature Chemistry → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-356225","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":18273903,"identity":"8e0a9764-761a-4c48-af7c-32ad0227df95","order_by":0,"name":"Haowen Zhou","email":"","orcid":"https://orcid.org/0000-0001-5068-6758","institution":"Department of Chemistry, Stanford University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Haowen","middleName":"","lastName":"Zhou","suffix":""},{"id":18273904,"identity":"265ce320-8d83-46e9-b8e9-b40a6b051cc9","order_by":1,"name":"William Perreault","email":"","orcid":"https://orcid.org/0000-0003-0639-5800","institution":"Stanford University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"William","middleName":"","lastName":"Perreault","suffix":""},{"id":18273905,"identity":"715fe160-3be0-49da-b334-c578cf40f959","order_by":2,"name":"Nandini Mukherjee","email":"","orcid":"https://orcid.org/0000-0003-1486-8508","institution":"Stanford University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Nandini","middleName":"","lastName":"Mukherjee","suffix":""},{"id":18273906,"identity":"5ac98591-c0f1-42c1-aa68-e26c4af395fa","order_by":3,"name":"Richard Zare","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAx0lEQVRIiWNgGAWjYLCCDyCC+QADAw8DA2MDMToYZzAYMDCwJZCghZmHJC3y7WcfPrb580fenI352Ic3DDayGw4QclRPurFxbpuB4c42tuSZcxjSjAlqYWZIY5PObTBg3HC/xxjowsOJBLWw8T9j/23xx8B+wzEekJb/hLXwSKSxMTOwGSRCtRwgrEVC4hmzZG+bcfKGY2zJjHMMko1nEtIi35/G+OHHHznbDceYDzO8qbCT7SOkBQ0YkKZ8FIyCUTAKRgEOAADQbTyHQlpLYgAAAABJRU5ErkJggg==","orcid":"https://orcid.org/0000-0001-5266-4253","institution":"Stanford University","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Richard","middleName":"","lastName":"Zare","suffix":""}],"badges":[],"createdAt":"2021-03-23 22:30:52","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-356225/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-356225/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41557-022-00926-z","type":"published","date":"2022-05-02T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":7848203,"identity":"9c53b82d-b9e0-4765-a02e-6aca080a4687","added_by":"auto","created_at":"2021-04-09 18:30:11","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":60247,"visible":true,"origin":"","legend":"Measured time-of-flight distributions of scattered D2 (v = 2, j' = 0) for the HSARP (a) and VSARP (b) alignments at delays of 100 ns (red dots) and 500 ns (blue dots) after SARP preparation. In HSARP, the total number of counts drops by ~90%, while for VSARP it drops by only ~40%. (See Table I) The negative points for HSARP at 500 ns result from the signal level falling below the stochastic fluctuations of the background noise and should be taken only as a demonstration of the dramatic reduction in relaxation rate. Schematic at top shows the SARP preparation of a defined region of the molecular beam (orange spot). As the delay is increased, this spot propagates downstream and spreads out. As described in the text, only those scattering products within the small REMPI volume (purple spots) are detected","description":"","filename":"1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1/7c815f494d769a883d803067.jpg"},{"id":7847949,"identity":"16b9d93c-d60d-4991-b0ee-d271ae0342c0","added_by":"auto","created_at":"2021-04-09 18:27:11","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":72188,"visible":true,"origin":"","legend":"(a) The velocity distributions of the prepared D2 (v = 2, j = 2) (green curve) and unprepared D2 (v = 0, j = 1, 2) (black dotted curve) at 100 ns delay. (b) The velocity distributions of the prepared D2 (v = 2, j = 2) (cyan curve) and unprepared D2 (v = 0, j = 1, 2) (black dotted curve) at 500 ns delay. All velocities are determined by fitting the time-of-flight distribution taking into account the electron recoil, which gives a measurement error of less than 3 m/s. (c) Collision speeds for both the aligned-aligned (red and blue curves) and aligned-unaligned (black and magenta dashed curves) collision pairs at the two delays. As described in the Methods section, these curves are generated by convoluting the velocity distributions given in (a) and (b). The only substantial change is in the collision speed for the aligned-aligned collisions at 500 ns (solid blue curve). All three other curves are within our measurement error.","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1/aa40b2b7f5bd3e003dd18d73.jpg"},{"id":7848201,"identity":"59309e0c-ac6b-4d8f-8a63-83529579faac","added_by":"auto","created_at":"2021-04-09 18:30:11","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":38060,"visible":true,"origin":"","legend":"(a) The collision speed distribution for the D2 (v = 2)/D2 (v = 2) collision pair at 100 ns (solid red) and 500 ns delay (solid blue). The red and blue dashed lines show the collision velocity range containing 85% of the D2 (v = 2)/ D2 (v = 2) collisions at 100 and 500 ns delays, respectively. (b) Contour lines for the orbital angular momenta l = 1 (solid orange), l = 2 (solid purple), l = 3 (solid green) as a function of the collision speed and impact parameter. The red and blue dashed lines give the upper limit of the collision speed range for the delays of 100 ns and 500 ns corresponding to the dashed lines in (a).","description":"","filename":"3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1/004e2f27371388fcfa03c582.jpg"},{"id":7848264,"identity":"7ecbfa59-b937-43d4-adbe-9dbaddf9c5e8","added_by":"auto","created_at":"2021-04-09 18:33:11","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":52547,"visible":true,"origin":"","legend":"Experimentally measured scattering angular distributions and fits using partial wave analysis for HSARP (a) and VSARP (b) bond-axis alignments. The red dots represent experimental data taken at 100 ns delay. The solid and dashed black curves represent fits using partial wave analysis. As described in the main text, the solid black curve gives the fit produced using even outgoing orbitals l' = 0, 2, 4, 6, whereas the dashed curve gives the fit produced using odd outgoing orbitals l' = 1, 3, 5. The error bars represent the standard deviation in each time-of-flight bin.","description":"","filename":"4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1/b5da64cd35f6aae6290ff29c.jpg"},{"id":21007436,"identity":"48021596-9e15-47f3-8874-9a35afe3a9a1","added_by":"auto","created_at":"2022-05-03 07:12:00","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":948769,"visible":true,"origin":"","legend":"","description":"","filename":"D2D23292021Final.pdf","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1_covered.pdf"},{"id":13618992,"identity":"0fba075a-78d0-4dad-85dc-1ee23b989d77","added_by":"auto","created_at":"2021-09-17 06:59:18","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":943872,"visible":true,"origin":"","legend":"","description":"","filename":"D2D23292021Final.pdf","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1_covered.pdf"},{"id":7848320,"identity":"617e75c5-c0a8-47c6-ab10-2226e6843f82","added_by":"auto","created_at":"2021-04-09 18:36:16","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1016905,"visible":true,"origin":"","legend":"","description":"","filename":"D2D23292021Final.pdf","url":"https://assets-eu.researchsquare.com/files/rs-356225/v1_stamped.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms","fulltext":[{"header":"Full Text","content":"\u003cp\u003eDue to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the manuscript can be downloaded and accessed as a PDF.\u003c/p\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"anisotropic resonant dynamics, chemical physics","lastPublishedDoi":"10.21203/rs.3.rs-356225/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-356225/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"The dynamics of a resonant oriented scattering process dominated by a single partial wave provide the most sensitive probe of the long-range anisotropic forces important to chemical reactions. Here, we control the collision temperature and geometry to probe the dynamics of the cold (\u003c2 K) rotationally inelastic scattering of a pair of optically state-prepared D2 molecules. The collision temperature is manipulated by combining the strobing action of laser state preparation and detection with the velocity dispersion of the molecular beam. When the bond axes are aligned parallel to the collision velocity, the scattering rate drops by nearly an order of magnitude when collision energies \u003e1 K are removed, demonstrating a clear geometry-dependent resonance. Using partial wave analysis of the measured scattering angular distribution, we determine that an l = 2 shape resonance originates from the collisions between a pair of aligned D2 molecules. Our experiment illustrates the strong anisotropy of the long-range quadrupole-quadrupole interaction that controls the dynamic resonance for diatom-diatom collisions.","manuscriptTitle":"Highly anisotropic resonant dynamics in the aligned-aligned scattering of cold diatoms","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2021-04-09 18:27:10","doi":"10.21203/rs.3.rs-356225/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-chemistry","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"nchem","sideBox":"Learn more about [Nature Chemistry](http://www.nature.com/nchem/)","snPcode":"","submissionUrl":"","title":"Nature Chemistry","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Research","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"0d67bfa7-7564-497d-a2c0-67fde32e6148","owner":[],"postedDate":"April 9th, 2021","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":3539893,"name":"Physical Chemistry"}],"tags":[],"updatedAt":"2022-05-03T07:11:49+00:00","versionOfRecord":{"articleIdentity":"rs-356225","link":"https://doi.org/10.1038/s41557-022-00926-z","journal":{"identity":"nature-chemistry","isVorOnly":false,"title":"Nature Chemistry"},"publishedOn":"2022-05-02 04:00:00","publishedOnDateReadable":"May 2nd, 2022"},"versionCreatedAt":"2021-04-09 18:27:10","video":"","vorDoi":"10.1038/s41557-022-00926-z","vorDoiUrl":"https://doi.org/10.1038/s41557-022-00926-z","workflowStages":[]},"version":"v1","identity":"rs-356225","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-356225","identity":"rs-356225","version":["v1"]},"buildId":"cBFmMYwuxLRRLfASyISRj","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}