{"id":"https://openalex.org/W4254883545","doi":"https://doi.org/10.26434/chemrxiv.13003490","title":"Measuring Theoretical Descriptors of Water Oxidation: Free Energy Differences Between Intermediates Using Time-Resolved Optical Spectroscopy","display_name":"Measuring Theoretical Descriptors of Water Oxidation: Free Energy Differences Between Intermediates Using Time-Resolved Optical Spectroscopy","publication_year":2020,"publication_date":"2020-09-25","ids":{"openalex":"https://openalex.org/W4254883545","doi":"https://doi.org/10.26434/chemrxiv.13003490"},"language":"en","primary_location":{"id":"doi:10.26434/chemrxiv.13003490","doi":"https://doi.org/10.26434/chemrxiv.13003490","is_oa":true,"landing_page_url":"https://doi.org/10.26434/chemrxiv.13003490","pdf_url":null,"source":{"id":"https://openalex.org/S4393918830","display_name":"ChemRxiv","issn_l":"2573-2293","issn":["2573-2293"],"is_oa":false,"is_in_doaj":false,"is_core":false,"listed_in":[],"host_organization":null,"host_organization_name":null,"host_organization_lineage":[],"host_organization_lineage_names":[],"type":"repository"},"license":"cc-by-nc-nd","license_id":"https://openalex.org/licenses/cc-by-nc-nd","version":"submittedVersion","is_accepted":false,"is_published":false,"raw_source_name":null,"raw_type":"posted-content"},"parent_works":[],"lineage":["https://openalex.org/W4254883545"],"child_works_count":0,"type":"preprint","is_traditional":true,"indexed_in":["crossref"],"open_access":{"is_oa":true,"oa_status":"green","oa_url":"https://doi.org/10.26434/chemrxiv.13003490","any_repository_has_fulltext":true},"authorships":[{"author_position":"first","author":{"id":null,"display_name":"Ilya Vinogradov","orcid":null,"observed_orcids":[]},"institutions":[{"id":"https://openalex.org/I188538660","display_name":"University of Colorado Boulder","ror":"https://ror.org/02ttsq026","country_code":"US","type":"education","lineage":["https://openalex.org/I188538660"]}],"countries":["US"],"is_corresponding":false,"raw_author_name":"Ilya Vinogradov","raw_affiliation_strings":["Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303"],"raw_orcid":null,"affiliations":[{"raw_affiliation_string":"Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]},{"raw_affiliation_string":"\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]}]},{"author_position":"middle","author":{"id":"https://openalex.org/A5082056990","display_name":"Suryansh Singh","orcid":"https://orcid.org/0009-0000-1415-1692","observed_orcids":["https://orcid.org/0009-0000-1415-1692"]},"institutions":[{"id":"https://openalex.org/I188538660","display_name":"University of Colorado Boulder","ror":"https://ror.org/02ttsq026","country_code":"US","type":"education","lineage":["https://openalex.org/I188538660"]}],"countries":["US"],"is_corresponding":false,"raw_author_name":"Suryansh Singh","raw_affiliation_strings":["Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303"],"raw_orcid":null,"affiliations":[{"raw_affiliation_string":"Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]},{"raw_affiliation_string":"\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]}]},{"author_position":"middle","author":{"id":"https://openalex.org/A5011141281","display_name":"Hanna Lyle","orcid":null,"observed_orcids":[]},"institutions":[{"id":"https://openalex.org/I188538660","display_name":"University of Colorado Boulder","ror":"https://ror.org/02ttsq026","country_code":"US","type":"education","lineage":["https://openalex.org/I188538660"]}],"countries":["US"],"is_corresponding":false,"raw_author_name":"Hanna Lyle","raw_affiliation_strings":["Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303"],"raw_orcid":null,"affiliations":[{"raw_affiliation_string":"Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]},{"raw_affiliation_string":"\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]}]},{"author_position":"middle","author":{"id":null,"display_name":"Aritra Mandal","orcid":null,"observed_orcids":[]},"institutions":[{"id":"https://openalex.org/I188538660","display_name":"University of Colorado Boulder","ror":"https://ror.org/02ttsq026","country_code":"US","type":"education","lineage":["https://openalex.org/I188538660"]}],"countries":["US"],"is_corresponding":false,"raw_author_name":"Aritra Mandal","raw_affiliation_strings":["Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303"],"raw_orcid":null,"affiliations":[{"raw_affiliation_string":"Renewable and Sustainable Energy Institute (RASEI), University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]},{"raw_affiliation_string":"\u03b3 Materials Science and Engineering Program, University of Colorado, Boulder, Boulder, 80303","institution_ids":["https://openalex.org/I188538660"]}]},{"author_position":"middle","author":{"id":"https://openalex.org/A5083668074","display_name":"Jan Rossmeisl","orcid":"https://orcid.org/0000-0001-7749-6567","observed_orcids":["https://orcid.org/0000-0001-7749-6567"]},"institutions":[],"countries":[],"is_corresponding":false,"raw_author_name":"Jan Rossmeisl","raw_affiliation_strings":[],"raw_orcid":null,"affiliations":[]},{"author_position":"last","author":{"id":"https://openalex.org/A5066895569","display_name":"Tanja Cuk","orcid":"https://orcid.org/0000-0002-1635-2946","observed_orcids":["https://orcid.org/0000-0002-1635-2946"]},"institutions":[{"id":"https://openalex.org/I188538660","display_name":"University of Colorado Boulder","ror":"https://ror.org/02ttsq026","country_code":"US","type":"education","lineage":["https://openalex.org/I188538660"]}],"countries":["US"],"is_corresponding":false,"raw_author_name":"Tanja Cuk","raw_affiliation_strings":["University of Colorado, Boulder"],"raw_orcid":null,"affiliations":[{"raw_affiliation_string":"University of Colorado, Boulder","institution_ids":["https://openalex.org/I188538660"]}]}],"institutions":[],"countries_distinct_count":1,"institutions_distinct_count":1,"corresponding_author_ids":[],"corresponding_institution_ids":[],"apc_list":null,"apc_paid":null,"fwci":null,"has_fulltext":false,"cited_by_count":0,"citation_normalized_percentile":null,"cited_by_percentile_year":null,"biblio":{"volume":null,"issue":null,"first_page":null,"last_page":null},"is_retracted":false,"is_paratext":false,"is_xpac":false,"primary_topic":{"id":"https://openalex.org/T10078","display_name":"Advanced Photocatalysis Techniques","score":0.5336999893188477,"subfield":{"id":"https://openalex.org/subfields/2105","display_name":"Renewable Energy, Sustainability and the Environment"},"field":{"id":"https://openalex.org/fields/21","display_name":"Energy"},"domain":{"id":"https://openalex.org/domains/3","display_name":"Physical Sciences"}},"topics":[{"id":"https://openalex.org/T10078","display_name":"Advanced Photocatalysis Techniques","score":0.5336999893188477,"subfield":{"id":"https://openalex.org/subfields/2105","display_name":"Renewable Energy, Sustainability and the Environment"},"field":{"id":"https://openalex.org/fields/21","display_name":"Energy"},"domain":{"id":"https://openalex.org/domains/3","display_name":"Physical Sciences"}},{"id":"https://openalex.org/T10030","display_name":"Electrocatalysts for Energy Conversion","score":0.392300009727478,"subfield":{"id":"https://openalex.org/subfields/2105","display_name":"Renewable Energy, Sustainability and the Environment"},"field":{"id":"https://openalex.org/fields/21","display_name":"Energy"},"domain":{"id":"https://openalex.org/domains/3","display_name":"Physical Sciences"}},{"id":"https://openalex.org/T10024","display_name":"TiO2 Photocatalysis and Solar Cells","score":0.028999999165534973,"subfield":{"id":"https://openalex.org/subfields/2105","display_name":"Renewable Energy, Sustainability and the Environment"},"field":{"id":"https://openalex.org/fields/21","display_name":"Energy"},"domain":{"id":"https://openalex.org/domains/3","display_name":"Physical Sciences"}}],"keywords":[{"id":"https://openalex.org/keywords/water-oxidation","display_name":"water oxidation","score":0.9459999799728394},{"id":"https://openalex.org/keywords/free-energy-difference","display_name":"free energy difference","score":0.9309999942779541},{"id":"https://openalex.org/keywords/photoelectrochemical-water-splitting","display_name":"photoelectrochemical water splitting","score":0.6639999747276306},{"id":"https://openalex.org/keywords/time-resolved-spectroscopy","display_name":"time-resolved spectroscopy","score":0.7990000247955322},{"id":"https://openalex.org/keywords/srtio3","display_name":"SrTiO3","score":0.7689999938011169},{"id":"https://openalex.org/keywords/langmuir-isotherm","display_name":"Langmuir isotherm","score":0.8519999980926514},{"id":"https://openalex.org/keywords/ph-dependence","display_name":"pH dependence","score":0.5580000281333923},{"id":"https://openalex.org/keywords/electrocatalysis","display_name":"electrocatalysis","score":0.45500001311302185}],"concepts":[{"id":"https://openalex.org/C185592680","wikidata":"https://www.wikidata.org/wiki/Q2329","display_name":"Chemistry","level":0,"score":0.7042125463485718},{"id":"https://openalex.org/C32891209","wikidata":"https://www.wikidata.org/wiki/Q483666","display_name":"Spectroscopy","level":2,"score":0.5912639498710632},{"id":"https://openalex.org/C2908647359","wikidata":"https://www.wikidata.org/wiki/Q2625603","display_name":"Population","level":2,"score":0.5484344959259033},{"id":"https://openalex.org/C161790260","wikidata":"https://www.wikidata.org/wiki/Q82264","display_name":"Catalysis","level":2,"score":0.4825443625450134},{"id":"https://openalex.org/C181500209","wikidata":"https://www.wikidata.org/wiki/Q215328","display_name":"Excited state","level":2,"score":0.4787939488887787},{"id":"https://openalex.org/C135473242","wikidata":"https://www.wikidata.org/wiki/Q4147614","display_name":"Oxygen evolution","level":4,"score":0.4783310890197754},{"id":"https://openalex.org/C93391505","wikidata":"https://www.wikidata.org/wiki/Q658700","display_name":"Reaction rate constant","level":3,"score":0.46420177817344666},{"id":"https://openalex.org/C55904794","wikidata":"https://www.wikidata.org/wiki/Q82682","display_name":"Redox","level":2,"score":0.45497795939445496},{"id":"https://openalex.org/C10710636","wikidata":"https://www.wikidata.org/wiki/Q857809","display_name":"Equilibrium constant","level":2,"score":0.4263645112514496},{"id":"https://openalex.org/C147789679","wikidata":"https://www.wikidata.org/wiki/Q11372","display_name":"Physical chemistry","level":1,"score":0.4170268476009369},{"id":"https://openalex.org/C113196181","wikidata":"https://www.wikidata.org/wiki/Q485223","display_name":"Analytical Chemistry (journal)","level":2,"score":0.3683859705924988},{"id":"https://openalex.org/C148898269","wikidata":"https://www.wikidata.org/wiki/Q1108792","display_name":"Kinetics","level":2,"score":0.34524670243263245},{"id":"https://openalex.org/C75473681","wikidata":"https://www.wikidata.org/wiki/Q188651","display_name":"Photochemistry","level":1,"score":0.3371598422527313},{"id":"https://openalex.org/C52859227","wikidata":"https://www.wikidata.org/wiki/Q7877","display_name":"Electrochemistry","level":3,"score":0.3259727954864502},{"id":"https://openalex.org/C179104552","wikidata":"https://www.wikidata.org/wiki/Q11165","display_name":"Inorganic chemistry","level":1,"score":0.1773970127105713},{"id":"https://openalex.org/C184779094","wikidata":"https://www.wikidata.org/wiki/Q26383","display_name":"Atomic physics","level":1,"score":0.12748226523399353},{"id":"https://openalex.org/C17525397","wikidata":"https://www.wikidata.org/wiki/Q176140","display_name":"Electrode","level":2,"score":0.12014180421829224},{"id":"https://openalex.org/C121332964","wikidata":"https://www.wikidata.org/wiki/Q413","display_name":"Physics","level":0,"score":0.09530067443847656},{"id":"https://openalex.org/C43617362","wikidata":"https://www.wikidata.org/wiki/Q170050","display_name":"Chromatography","level":1,"score":0.0},{"id":"https://openalex.org/C144024400","wikidata":"https://www.wikidata.org/wiki/Q21201","display_name":"Sociology","level":0,"score":0.0},{"id":"https://openalex.org/C149923435","wikidata":"https://www.wikidata.org/wiki/Q37732","display_name":"Demography","level":1,"score":0.0},{"id":"https://openalex.org/C62520636","wikidata":"https://www.wikidata.org/wiki/Q944","display_name":"Quantum mechanics","level":1,"score":0.0},{"id":"https://openalex.org/C55493867","wikidata":"https://www.wikidata.org/wiki/Q7094","display_name":"Biochemistry","level":1,"score":0.0}],"mesh":[],"locations_count":1,"locations":[{"id":"doi:10.26434/chemrxiv.13003490","doi":"https://doi.org/10.26434/chemrxiv.13003490","is_oa":true,"landing_page_url":"https://doi.org/10.26434/chemrxiv.13003490","pdf_url":null,"source":{"id":"https://openalex.org/S4393918830","display_name":"ChemRxiv","issn_l":"2573-2293","issn":["2573-2293"],"is_oa":false,"is_in_doaj":false,"is_core":false,"listed_in":[],"host_organization":null,"host_organization_name":null,"host_organization_lineage":[],"host_organization_lineage_names":[],"type":"repository"},"license":"cc-by-nc-nd","license_id":"https://openalex.org/licenses/cc-by-nc-nd","version":"submittedVersion","is_accepted":false,"is_published":false,"raw_source_name":null,"raw_type":"posted-content"}],"best_oa_location":{"id":"doi:10.26434/chemrxiv.13003490","doi":"https://doi.org/10.26434/chemrxiv.13003490","is_oa":true,"landing_page_url":"https://doi.org/10.26434/chemrxiv.13003490","pdf_url":null,"source":{"id":"https://openalex.org/S4393918830","display_name":"ChemRxiv","issn_l":"2573-2293","issn":["2573-2293"],"is_oa":false,"is_in_doaj":false,"is_core":false,"listed_in":[],"host_organization":null,"host_organization_name":null,"host_organization_lineage":[],"host_organization_lineage_names":[],"type":"repository"},"license":"cc-by-nc-nd","license_id":"https://openalex.org/licenses/cc-by-nc-nd","version":"submittedVersion","is_accepted":false,"is_published":false,"raw_source_name":null,"raw_type":"posted-content"},"sustainable_development_goals":[],"study_designs":[],"awards":[{"id":"https://openalex.org/G1394502702","display_name":null,"funder_award_id":"Contract No. DE-SC0018939","funder_id":"https://openalex.org/F4320337480","funder_display_name":"Basic Energy Sciences"},{"id":"https://openalex.org/G5033002523","display_name":null,"funder_award_id":"DE-SC0018939","funder_id":"https://openalex.org/F4320337480","funder_display_name":"Basic Energy Sciences"},{"id":"https://openalex.org/G7815593317","display_name":"OBSERVING THE MOLECULAR AND DYNAMIC PATHWAY OF WATER OXIDATION ON TITANIA SURFACES","funder_award_id":"DESC0018939","funder_id":"https://openalex.org/F4320306084","funder_display_name":"U.S. Department of Energy"}],"funders":[{"id":"https://openalex.org/F4320306084","display_name":"U.S. Department of Energy","ror":"https://ror.org/01bj3aw27"},{"id":"https://openalex.org/F4320332359","display_name":"Office of Science","ror":"https://ror.org/00mmn6b08"},{"id":"https://openalex.org/F4320337480","display_name":"Basic Energy Sciences","ror":"https://ror.org/05mg91w61"}],"has_content":{"pdf":false,"grobid_xml":false},"content_urls":null,"referenced_works_count":32,"referenced_works":["https://openalex.org/W1480171480","https://openalex.org/W1906682345","https://openalex.org/W1910980698","https://openalex.org/W1968076335","https://openalex.org/W1972949070","https://openalex.org/W1979665920","https://openalex.org/W1982153238","https://openalex.org/W2031611994","https://openalex.org/W2048252048","https://openalex.org/W2076807032","https://openalex.org/W2080681961","https://openalex.org/W2084628727","https://openalex.org/W2133406747","https://openalex.org/W2148667390","https://openalex.org/W2159742564","https://openalex.org/W2165801834","https://openalex.org/W2171613439","https://openalex.org/W2274701321","https://openalex.org/W2312771340","https://openalex.org/W2329051406","https://openalex.org/W2337261154","https://openalex.org/W2342986122","https://openalex.org/W2468442926","https://openalex.org/W2557471635","https://openalex.org/W2573377826","https://openalex.org/W2761424377","https://openalex.org/W2899973458","https://openalex.org/W2924161339","https://openalex.org/W2955991791","https://openalex.org/W2956312175","https://openalex.org/W2970727831","https://openalex.org/W4256474636"],"related_works":["https://openalex.org/W3209223443","https://openalex.org/W4309811456","https://openalex.org/W2970727831","https://openalex.org/W4412703094","https://openalex.org/W4401698547","https://openalex.org/W7169035066","https://openalex.org/W3168793616","https://openalex.org/W2521376370","https://openalex.org/W7052006396"],"abstract_inverted_index":{"Theoretical":[0],"descriptions":[1],"differentiate":[2],"catalytic":[3,182],"activity":[4],"of":[5,16,32,49,62,81,91,119,138,180,219],"material":[6,143],"surfaces":[7],"for":[8,156],"the":[9,14,17,33,50,57,77,82,92,109,172,177,181,191,194,201,217],"water":[10,53,220],"oxidation":[11,54,221],"reaction":[12,55,100,140,159],"by":[13,37,96,169,213],"stability":[15],"reactive":[18],"oxygen":[19],"(O*)":[20],"intermediate.":[21],"The":[22,130],"underlying":[23,78],"conjecture":[24],"is":[25],"that":[26,87,155,193],"there":[27,66],"are":[28,184],"several":[29],"meta-stable":[30],"steps":[31,141],"reaction,":[34],"each":[35],"connected":[36],"free":[38,178],"energy":[39],"differences":[40],"critically":[41],"dependent":[42],"on":[43,142,160],"O*.":[44],"Recently":[45],"in-situ,":[46],"time-resolved":[47,188],"spectroscopy":[48],"(photo":[51],")-electrochemical":[52],"identified":[56],"vibrational":[58],"and":[59,76,206,211,222],"optical":[60,89],"signatures":[61],"O*":[63,93,174],"time-evolution.":[64],"However,":[65],"has":[67],"been":[68,148],"little":[69],"connection":[70,208],"between":[71,209],"these":[72],"inherently":[73],"kinetic":[74],"experiments":[75],"thermodynamic":[79],"parameters":[80],"theory.":[83],"Here,":[84],"we":[85,153],"discover":[86],"picosecond":[88],"spectra":[90],"population":[94],"modulated":[95],"a":[97,117,125,157,161,166,187,204],"shift":[98],"in":[99],"equilibria":[101],"defines":[102],"an":[103],"effective":[104],"equilibrium":[105,136,199],"constant":[106],"(Keff)":[107],"containing":[108],"relevant":[110],"free-energy":[111],"differences.":[112],"A":[113],"Langmuir":[114],"isotherm":[115],"as":[116],"function":[118],"electrolyte":[120],"pH":[121,167],"extracts":[122],"Keff":[123,170],"using":[124],"model":[126],"titania":[127],"system":[128],"(SrTiO3).":[129],"results":[131],"show":[132],"how":[133],"to":[134,215],"obtain":[135],"constants":[137],"individual":[139],"surfaces,":[144],"which":[145,214],"had":[146],"not":[147],"experimentally":[149],"accessible":[150],"previously.":[151],"Further,":[152],"find":[154],"photo-excited":[158],"semiconductor":[162],"surface":[163,183,195,224],"tuning":[164],"past":[165],"defined":[168],"doubles":[171],"initial":[173],"population.":[175],"That":[176],"energies":[179],"definable":[185],"through":[186],"spectroscopy,":[189],"alongside":[190],"finding":[192],"recollects":[196],"its":[197],"explicit":[198],"with":[200],"electrolyte,":[202],"provides":[203],"new":[205],"critical":[207],"theory":[210],"experiment":[212],"tailor":[216],"pathway":[218],"other":[223],"reactions.":[225]},"counts_by_year":[],"updated_date":"2026-11-14T11:04:58.165337","created_date":"2022-05-12T00:00:00"}
