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Synopsis
Femtosecond time-resolved photoelectron spectroscopy on liquid microjets (LPES) is used to study the ultrafast dynamics of solutes in high vapor pressure solvents. By monitoring the time-evolving kinetic energy of the detached electron, we are able to record transient lifetimes, solvation timescales, and binding energies of a wide variety of species. Recent upgrades to the experiment have extended probe energies into the extreme ultraviolet (XUV), drastically expanding the photophysics accessible for study using this method.
Our current focus is on the photophysics of DNA. In particular, we are interested in building a molecular-level understanding of the short-time dynamics present in nucleic acid constituents (NACs) subsequent to absorbing ultraviolet radiation. Working from simpler systems like solvated nucleobases to the more complex oligonucleotides, we aim to construct a more complete model of DNA photophysics by tracking the complete relaxation dynamics present in these systems.
Molecules studied:
Nucleobases, nucleosides, nucleotides
Solvated electrons
Project members:
Jaydeep Basu
Do Hyung Kang
Neal Haldar
Recent publications:
"Dynamics of photoexcited 5-bromouracil and 5-bromo-2'-deoxyuridine studied by extreme ultraviolet time-resolved photoelectron spectroscopy in liquid flat jets" D. H. Kang, M. Koga, N. Haldar, D. M. Neumark, Chem. Sci., 15, 17245–17255 (2024). pdf
"Extreme ultraviolet time-resolved photoelectron spectroscopy of adenine, adenosine and adenosine monophosphate in a liquid flat jet" M. Koga, D. H. Kang, Z. N. Heim, P. Meyer, B. A. Erickson, N. Haldar, N. Baradaran, M. Havenith, D. M. Neumark, Phys. Chem. Chem. Phys., 26, 13106 (2024). pdf
"Nonadiabatic Dynamics Studied by Liquid-Jet Time-Resolved Photoelectron Spectroscopy" Z. N. Heim, D. M. Neumark, Acc. Chem. Res., 55, 3652 (2022). pdf
"Relaxation Dynamics of Hydrated Thymine, Thymidine, and Thymidine Monophosphate Probed by Liquid Jet Time-Resolved Photoelectron Spectroscopy" B. A. Erickson, Z. N. Heim, E. Pieri, E. Liu, T. J. Martinez, D. M. Neumark, J. Phys. Chem. A 123, 10676 (2019). pdf
"Time-resolved photoelectron spectroscopy of adenosine and adenosine monophosphate photodeactivation dynamics in water microjets" H. L. Williams, B. A. Erickson, D. M. Neumark, J. Chem. Phys. 148, 194303 (2018). pdf
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