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Excited-State Dynamics of Structurally Characterized [Re^I(CO)_3(phen)(HisX)]^+(X = 83, 109) Pseudomonas aeruginosa Azurins in Aqueous Solution

Blanco-Rodríguez, Ana María and Busby, Michael and Grǎdinaru, Cristian and Crane, Brian R. and Di Bilio, Angel J. and Matousek, Pavel and Towrie, Michael and Leigh, Brian S. and Richards, John H. and Vlček, Antonín, Jr. and Gray, Harry B. (2006) Excited-State Dynamics of Structurally Characterized [Re^I(CO)_3(phen)(HisX)]^+(X = 83, 109) Pseudomonas aeruginosa Azurins in Aqueous Solution. Journal of the American Chemical Society, 128 (13). pp. 4365-4370. ISSN 0002-7863. https://resolver.caltech.edu/CaltechAUTHORS:20170405-145213550

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Abstract

The triplet metal-to-ligand charge transfer (^3MLCT) dynamics of two structurally characterized Re^I(CO)_3(phen)(HisX)-modified (phen = 1,10-phenanthroline; X = 83, 109) Pseudomonas aeruginosa azurins have been investigated by picosecond time-resolved infrared (TRIR) spectroscopy in aqueous (D_2O) solution. The ^3MLCT relaxation dynamics exhibited by the two ReI−azurins are very different from those of the sensitizer [Re^I(CO)_3(phen)(im)]^+ (im = imidazole). Whereas the Re^I(CO)_3 intramolecular vibrational relaxation in Re^I(CO)_3(phen)(HisX)Az (4 ps) is similar to that of [Re^I(CO)_3(phen)(im)]^+ (2 ps), the medium relaxation is much slower (∼250 vs 9.5 ps); the 250-ps relaxation is attributable to reorientation of D_2O molecules as well as structural reorganization of the rhenium chromophore and nearby polar amino acids in each of the modified proteins.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja057451+DOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja057451%2BPublisherArticle
ORCID:
AuthorORCID
Gray, Harry B.0000-0002-7937-7876
Alternate Title:Excited-State Dynamics of Structurally Characterized [ReI(CO)3(phen)(HisX)]+(X = 83, 109) Pseudomonas aeruginosa Azurins in Aqueous Solution
Additional Information:© 2006 American Chemical Society. Received November 1, 2005; Publication Date (Web): March 16, 2006. This work was supported by the NIH (DK19038), NSF (MCB:  0133564), EPSRC, CCLRC, and QMUL.
Funders:
Funding AgencyGrant Number
NIHDK19038
NSFMCB-0133564
Engineering and Physical Sciences Research Council (EPSRC)UNSPECIFIED
Council for the Central Laboratory of the Research CouncilsUNSPECIFIED
Queen Mary University of LondonUNSPECIFIED
Issue or Number:13
Record Number:CaltechAUTHORS:20170405-145213550
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170405-145213550
Official Citation:Excited-State Dynamics of Structurally Characterized [ReI(CO)3(phen)(HisX)]+ (X = 83, 109) Pseudomonas aeruginosa Azurins in Aqueous Solution Ana María Blanco-Rodríguez, Michael Busby, Cristian Grǎdinaru, Brian R. Crane, Angel J. Di Bilio, Pavel Matousek, Michael Towrie, Brian S. Leigh, John H. Richards, Antonín Vlček, Jr., and Harry B. Gray Journal of the American Chemical Society 2006 128 (13), 4365-4370 DOI: 10.1021/ja057451+
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:75747
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:05 Apr 2017 22:59
Last Modified:09 Mar 2020 13:19

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