{"doi":"10.1101/2022.03.31.486235","title":"Temporal and Spatial Resolution of a Protein Quake that Activates Hydrogen Tunneling in Soybean Lipoxygenase","abstract":"Abstract The enzyme soybean lipoxygenase (SLO) provides a prototype for deep tunneling mechanisms in hydrogen transfer catalysis. This work combines room temperature X-ray studies with extended hydrogen deuterium exchange experiments to detect a radiating cone of aliphatic side chains that extends from the iron active site of SLO to the protein-solvent interface. Employing eight variants of SLO, nanosecond fluorescence Stokes shifts have been measured using a probe appended to the identified surface loop. We report a remarkable identity of the enthalpies of activation for the Stokes shifts decay rates and the millisecond C-H bond cleavage step that is restricted to side chain mutants within the identified thermal network. While the role of dynamics in enzyme function has been predominantly attributed to a distributed protein conformational landscape, these new data implicate a thermally initiated, cooperative protein quake as the source of the activation of SLO. These findings indicate a direct coupling of distal protein motions surrounding the exposed fluorescent probe to active site motions controlling catalysis.","journal":"bioRxiv (Cold Spring Harbor Laboratory)","year":2022,"id":299091,"datarank":0.0,"base_score":0.0,"endowment":0.0,"self_citation_contribution":0.0,"citation_network_contribution":0.0,"self_endowment_contribution":0.0,"citer_contribution":0.0,"corpus_percentile":null,"corpus_rank":null,"citation_count":4,"citer_count":0,"citers_with_citation_signal":0,"citers_with_endowment":0,"datacite_reuse_total":0,"is_dataset":false,"is_dataset_confidence":0.959,"is_data_producer":false,"deposit_databanks":null,"is_oa":true,"file_count":0,"downloads":0,"has_version_chain":false,"published_date":"2022-01-01","fair_score":null,"fair_percentile":null,"algorithm_id":"datarank_citation_only_1hop_v6","ranking_scope":"data_only","authors":[{"id":702349,"name":"Adam R. Offenbacher","orcid":"0000-0001-6990-7178","position":1,"is_corresponding":false},{"id":988959,"name":"Shenshen Hu","orcid":null,"position":2,"is_corresponding":false},{"id":344885,"name":"Christine L. Gee","orcid":"0000-0002-2632-6418","position":3,"is_corresponding":false},{"id":988960,"name":"Zachary M. Firestein","orcid":null,"position":4,"is_corresponding":false},{"id":988551,"name":"Natalie Minnetian","orcid":"0000-0002-1817-184X","position":5,"is_corresponding":false},{"id":988552,"name":"Zhenyu Deng","orcid":"0000-0001-8781-3140","position":6,"is_corresponding":false},{"id":988961,"name":"Flora Fan","orcid":null,"position":7,"is_corresponding":false},{"id":261600,"name":"Anthony T. Iavarone","orcid":null,"position":8,"is_corresponding":false},{"id":480717,"name":"Judith P. Klinman","orcid":"0000-0001-5734-2843","position":9,"is_corresponding":false},{"id":501565,"name":"Jan Paulo T. Zaragoza","orcid":"0000-0002-2583-6571","position":0,"is_corresponding":true}],"reference_count":134,"raw_metadata":null,"created_at":"2026-07-19T00:31:40.528568Z","pmid":null,"pmcid":null,"fwci":null,"citation_percentile":null,"influential_citations":0,"oa_status":null,"license":null,"views":0,"total_file_size_bytes":0,"version_count":0,"fair_f":null,"fair_a":null,"fair_i":null,"fair_r":null,"fair_zscore":null,"fair_rationale":null,"fair_model":null,"fair_agent_version":null,"fair_fulltext_source":null,"fair_has_llm":null,"fair_computed_at":null,"clinical_trials":[],"software_tools":[],"db_accessions":[],"linked_datasets":[],"topics":[]}