Experimental Physical Chemistry
Biography
- 2019–present: Chemist, Argonne National Laboratory
- 2015–2019: Assistant Chemist, Argonne National Laboratory
- Postdoctoral researcher (2013–2014) with Prof. Arthur. G. Suits, Wayne State University
- Postdoctoral researcher (2007–2012) with Prof. Robert W. Field, Massachusetts Institute of Technology
- Ph.D. (2007) and M.S. (2003) in Chemistry from University of Southern California under the guidance of Prof. Andrey F. Vilesov
- M.S. (2000) and B.S. (1998) in Applied Mathematics and Physics from the Moscow Institute of Physics and Technology
Research interests
I am interested in discovering fundamental mechanisms of chemical reactions in the gas phase. How and why do molecules react? What are the ways of steering the outcome of their reactions? Can we rationally design new fuels or improve the biomass conversion processes? These questions can be answered by a combination of the experiments that I am conducting using the chirped-pulse Fourier transform millimeter-wave (CP-FTmmW) spectroscopy and the theoretical support I am receiving from my colleagues. In particular, we are investigating the contributions from the roaming radicals dynamics, non-thermal effects, quantum tunneling, and H-atom addition/elimination to the outcomes of chemical reactions in different experimental environments.
Pyrolysis reactions
In this research effort, complex networks of chemical reactions are thermally initiated in the micro-tubular pyrolysis reactor (Chen nozzle) heated to 800–1900 K. The reaction products are cooled in the supersonic expansion to ~10 K where they are observed and quantified using CP-FTmmW spectroscopy. Based on these measurements, and with the help of kinetic modeling, reaction networks are built and new chemical pathways are discovered.
Time-Resolved Kinetic Chirped-Pulse spectroscopy
In this novel experimental approach, chemistry in my room temperature flow-tube reactor is initiated by UV laser pulses. Subsequent reactions and thermalization of energized photo-products are observed with a time- and vibrational quantum state-resolved chirped-pulse rotational spectroscopy. Vibrational population distributions of reaction products are a key to discovering new reaction mechanisms.
Assignment of rotational spectra using artificial neural networks
Increasing throughput of spectroscopic data from broadband chirped-pulse rotational experiments opens new opportunities for chemical research. At the same time, assignment of broadband rotational spectra and identification of chemical species becomes a bottleneck. We have demonstrated the potential of machine learning for sorting through these spectroscopic data and eventually converting them to chemical information.
Recent publications
Daniel P. Zaleski, Raghu Sivaramakrishnan, Hailey R. Weller, Nathan A. Seifert, David H. Bross, Branko Ruscic, Kevin B. Moore III, Sarah N. Elliott, Andreas V. Copan, Lawrence B. Harding, Stephen J. Klippenstein, Robert W. Field, and Kirill Prozument, “Substitution Reactions in the Pyrolysis of Acetone Revealed through a Modeling, Experiment, Theory Paradigm”, J. Am. Chem. Soc. 143, 3124–3142 (2021)
Kirill Prozument, Boris G. Sartakov, and Andrey F. Vilesov, “Mixed ortho-H2 and para-H2 clusters studied by vibrational coherent anti-Stokes Raman spectroscopy”, Phys. Rev. B 101, 184507 (2020)
Kirill Prozument, Joshua H. Baraban, P. Bryan Changala, G. Barratt Park, Rachel G. Shaver, John S. Muenter, Stephen J. Klippenstein, Vladimir Y. Chernyak, and Robert W. Field, “Photodissociation transition states characterized by chirped pulse millimeter wave spectroscopy”, Proc. Natl. Acad. Sci. U.S.A. 117, 146−151 (2020)
Daniel P. Zaleski and Kirill Prozument, “Automated assignment of rotational spectra using artificial neural networks”, J. Chem. Phys. 149, 104106 (2018)
Peter J. Weddle, Canan Karakaya, Huayang Zhu, Raghu Sivaramakrishnan, Kirill Prozument, Robert J. Kee, “Boundary-layer model to predict chemically reacting flow within heated, high-speed, micro-tubular reactors”, Int. J. Chem. Kinet., 50, 473−480 (2018)
Daniel P. Zaleski, Lawrence B. Harding, Stephen J. Klippenstein, Branko Ruscic, and Kirill Prozument, “Time-Resolved Kinetic Chirped-Pulse Rotational Spectroscopy in a Room Temperature Flow Reactor“, J. Phys. Chem. Lett. 8, 6180−6188 (2017)
Daniel P. Zaleski and Kirill Prozument, “Pseudo-equilibrium geometry of HNO determined by an E-Band CP-FTmmW spectrometer”, Phys. Chem. Lett. 680, 101−108 (2017)
Daniel P. Zaleski, Chuanxi Duan, Miguel Carvajal, Isabelle Kleiner, and Kirill Prozument, “The Broadband Rotational Spectrum of Fully Deuterated Acetaldehyde (CD3CDO) in a CW Supersonic Expansion”, J. Mol. Spectrosc. 342, 17−24 (2017)