Time-resolved absorption and UV resonance Raman spectra reveal stepwise formation of T quaternary contacts in the allosteric pathway of hemoglobin

Journal of Molecular Biology
Gurusamy BalakrishnanThomas G Spiro

Abstract

Hemoglobin undergoes a series of molecular changes on the nanosecond and microsecond time-scale following photodissociation of CO ligands. We have monitored these processes with a combination of transient absorption and resonance Raman (RR) spectroscopy. The latter have been acquired at higher data rates than previously available, thanks to kilohertz Ti:sapphire laser technology, with frequency-quadrupling into the ultraviolet. As a result of improved resolution of the UVRR time-course, a new intermediate has been identified in the pathway from the R (HbCO) to the T (deoxyHb) state. This intermediate is not detected via absorption transients, since the change in heme absorption is insignificant, but its lifetime agrees with a reported magnetic circular dichroism transient, which has been attributed to a quaternary tryptophan interaction. The new UVRR data allow elaboration of the allosteric pathway by establishing that the T-state quaternary contacts are formed in two well-separated steps, with time constants of 2.9 micros and 21 micros, instead of a single 20 micros process. The first step involves the "hinge" region contacts, as monitored by the Trp beta 37...Asp alpha 94 H-bond, while the second involves the "switch" region,...Continue Reading

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Citations

Mar 17, 2009·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Gurusamy BalakrishnanThomas G Spiro
Nov 15, 2007·Inorganic Chemistry·Thomas G Spiro
Mar 19, 2011·Proceedings of the National Academy of Sciences of the United States of America·Stefan FischerMartin Karplus
Aug 29, 2012·Proceedings of the National Academy of Sciences of the United States of America·Matteo LevantinoAntonio Cupane
Sep 27, 2013·PLoS Computational Biology·Martin D Vesper, Bert L de Groot
Aug 25, 2009·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Yayoi AkiTeizo Kitagawa
Sep 12, 2007·Journal of Pharmaceutical Sciences·Zai-Qing Wen
Jul 3, 2010·Journal of Molecular Biology·M CammarataA Cupane
Jun 18, 2010·Journal of Molecular Biology·Thomas G Spiro, Gurusamy Balakrishnan
Jun 5, 2014·Protein Science : a Publication of the Protein Society·Eric M JonesThomas G Spiro
Jul 9, 2008·Current Opinion in Structural Biology·Gurusamy BalakrishnanThomas G Spiro
May 7, 2013·Biochimica Et Biophysica Acta·Takashi Yonetani, Kenji Kanaori
Jun 30, 2016·Biochemistry·Raymond M EsquerraRobert A Goldbeck
Dec 22, 2005·Journal of Molecular Biology·Janina KneippThomas G Spiro
Aug 15, 2015·Physical Chemistry Chemical Physics : PCCP·Cheolhee YangHyotcherl Ihee
Nov 21, 2018·International Journal of Molecular Sciences·Cheolhee YangHyotcherl Ihee
Dec 21, 2017·Physical Chemistry Chemical Physics : PCCP·Shanyan ChangYasuhisa Mizutani
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Jun 17, 2021·The Journal of Physical Chemistry. B·Takeo YamawakiYasuhisa Mizutani
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Jan 22, 2015·Chemical Reviews·Yue YuanChien Ho
Apr 25, 2014·The Journal of Physical Chemistry Letters·Key Young OangHyotcherl Ihee

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