scholarly journals Relaxation Dynamics of Hydrated Thymine, Thymidine, and Thymidine Monophosphate Probed by Liquid Jet Time-Resolved Photoelectron Spectroscopy

2019 ◽  
Vol 123 (50) ◽  
pp. 10676-10684
Author(s):  
Blake A. Erickson ◽  
Zachary N. Heim ◽  
Elisa Pieri ◽  
Erica Liu ◽  
Todd J. Martinez ◽  
...  
2019 ◽  
Author(s):  
Blake Erickson ◽  
Zachary Heim ◽  
Elisa Pieri ◽  
Erica Liu ◽  
Todd J. Martínez ◽  
...  

<p>The relaxation dynamics of thymine and its derivatives thymidine and thymidine monophosphate were studied using time-resolved photoelectron spectroscopy applied to a water microjet. Two absorption bands were studied, the first is a bright ππ* state which was populated using tunable-ultraviolet light in the range of 4.74 – 5.17 eV and probed using a 6.20 eV probe pulse. By reversing the order of these pulses, a band containing multiple ππ* states was populated by the 6.20 eV pulse and the lower energy pulse served as the probe. The lower lying ππ* state was found to decay in ~400 fs in both thymine and thymidine independent of pump photon energy while thymidine monophosphate decays varied from 670-840 fs with some pump energy dependence. </p><p>The application of a computational QM/MM scheme at the XMS-CASPT2//CASSCF/AMBER level of theory suggests that conformational differences existing between thymidine and thymidine monophosphate in solution accounts for this difference. The higher lying ππ* band was found to decay in ~600 fs in all three cases, but was only able to be characterized when using the 5.17 eV probe pulse. Notably, no long-lived signal from an np* state could be identified in either experiment on any of the three molecules.</p>


2019 ◽  
Author(s):  
Blake Erickson ◽  
Zachary Heim ◽  
Elisa Pieri ◽  
Erica Liu ◽  
Todd J. Martínez ◽  
...  

<p>The relaxation dynamics of thymine and its derivatives thymidine and thymidine monophosphate were studied using time-resolved photoelectron spectroscopy applied to a water microjet. Two absorption bands were studied, the first is a bright ππ* state which was populated using tunable-ultraviolet light in the range of 4.74 – 5.17 eV and probed using a 6.20 eV probe pulse. By reversing the order of these pulses, a band containing multiple ππ* states was populated by the 6.20 eV pulse and the lower energy pulse served as the probe. The lower lying ππ* state was found to decay in ~400 fs in both thymine and thymidine independent of pump photon energy while thymidine monophosphate decays varied from 670-840 fs with some pump energy dependence. </p><p>The application of a computational QM/MM scheme at the XMS-CASPT2//CASSCF/AMBER level of theory suggests that conformational differences existing between thymidine and thymidine monophosphate in solution accounts for this difference. The higher lying ππ* band was found to decay in ~600 fs in all three cases, but was only able to be characterized when using the 5.17 eV probe pulse. Notably, no long-lived signal from an np* state could be identified in either experiment on any of the three molecules.</p>


2015 ◽  
Vol 17 (47) ◽  
pp. 31978-31987 ◽  
Author(s):  
Franziska Buchner ◽  
Berit Heggen ◽  
Hans-Hermann Ritze ◽  
Walter Thiel ◽  
Andrea Lübcke

Time-resolved photoelectron spectroscopy is performed on aqueous guanosine solution to study its excited-state relaxation dynamics.


2016 ◽  
Vol 18 (36) ◽  
pp. 25070-25079 ◽  
Author(s):  
Liv B. Klein ◽  
James O. F. Thompson ◽  
Stuart W. Crane ◽  
Lisa Saalbach ◽  
Theis I. Sølling ◽  
...  

Time-resolved photoelectron spectroscopy reveals distinct ionization signatures of Rydberg-to-valence state evolution in the secondary aliphatic amine piperidine.


2014 ◽  
Vol 5 (10) ◽  
pp. 1760-1765 ◽  
Author(s):  
Ayumu Makida ◽  
Hironori Igarashi ◽  
Takehisa Fujiwara ◽  
Taro Sekikawa ◽  
Yu Harabuchi ◽  
...  

2014 ◽  
Vol 5 (10) ◽  
pp. 3963-3975 ◽  
Author(s):  
Adam S. Chatterley ◽  
Christopher W. West ◽  
Vasilios G. Stavros ◽  
Jan R. R. Verlet

Time-resolved photoelectron spectroscopy of deprotonated nucleotides provides new insights into their relaxation dynamics.


2018 ◽  
Vol 212 ◽  
pp. 359-381 ◽  
Author(s):  
Gaurav Kumar ◽  
Anirban Roy ◽  
Ryan S. McMullen ◽  
Shanmukh Kutagulla ◽  
Stephen E. Bradforth

Time-resolved photoelectron spectroscopy (TRPES) in a liquid micro-jet is implemented here to investigate the influence of water on the electronic structure and dynamics of indole, the chromophore of the amino acid tryptophan.


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