Laser Control of Chemical Reactions

The control of reactions is a key subject in chemistry. Apart from varying the conventional parameters, such as temperature, concentration or catalyst, the outcome of a chemical reaction can also be influenced by a light source. With specifically shaped laser pulses, a coherent control of the reaction can be achieved.

We use a control scheme with a short time resonant few cycle carrier-envelope phase (CEP) laser pulse that generates a phase-dependent superposition in the vicinity of a conical intersection. The phase-dependency of this superposition is defined by the waveform of the applied laser pulse, which strongly varies due to the few cycles. The interference between the phase of the generated superposition and the geometric phase induced by the conical intersection is decisive for the control mechanism.

Research Highlights

The Effect of a Mobile Solvent Environment on Quantum Control of Chemical Reactions
WATOC 2017, Munich

Observing and Controlling the Coupled Nuclear and Electron Dynamics in the Nucleobase Uracil
STC 2021, Würzburg

Key Publications

• F. Schüppel, T. Schnappinger, L. Bäuml, and R. de Vivie-Riedle
  Waveform control of molecular dynamics close to a conical intersection
  J. Chem. Phys. 153 (2020), 224307.
• D. Keefer, and R. Vivie-Riedle
  Theoretical Quantum Control of Fluctuating Molecular Energy Levels in Complex Chemical Environments
  Adv. Quantum Technol. 2 (2019), 1800099.
• D. Keefer, and R. de Vivie-Riedle
  Pathways to New Applications for Quantum Control
  Acc. Chem. Res. 51 (2018), 2279-2286.
• S. Thallmair, D. Keefer, F. Rott, and R. de Vivie-Riedle
  Simulating the control of molecular reactions via modulated light fields: From gas phase to solution
  J. Phys. B: At., Mol. Opt. Phys. 50 (2017), 082001.
• D. Keefer, S. Thallmair, S. Matsika, and R. de Vivie-Riedle
  Controlling Photorelaxation in Uracil with Shaped Laser Pulses: A Theoretical Assessment
  J. Am. Chem. Soc. 139 (2017), 5061-5066.
• C. Gollub, M. Kowalewski and R. de Vivie-Riedle
  Monotonic convergent optimal control theory with strict limitations on the spectrum of optimized laser fields.
  Phys. Rev. Lett. 101 (2008), 073002.
• Regina de Vivie-Riedle, Lukas Kurtz, and Angelika Hofmann
  Coherent Control for ultrafast photchemical reactions
  Pure Appl. Chem. 73 (2001), 525-528.