Pulse Shaping and Coherent Control

Shaped femtosecond pulses to steer molecular dynamics

Shaped femtosecond pulses steer molecular dynamics, for example by restricting intramolecular vibrational relaxation.

Question

Can the phase and amplitude of an ultrafast laser pulse decide where the energy of an excited molecule goes? Prof. Goswami’s early work on restricting intramolecular vibrational relaxation (IVR) [1] showed, through model calculations, that appropriate frequency sweeps can lock excitation over a well-defined range of resonance frequencies and so stop IVR.

Technique

The lab programs the spectral phase and amplitude of femtosecond pulses (the research overview describes the pulse shaper) and applies this to gaseous and liquid-phase molecular dynamics, including coherent control of multiphoton transitions [2].

Representative papers

• Control of Chemical Dynamics by Restricting Intramolecular Vibrational Relaxation, The Journal of Chemical Physics, 1993. doi:10/bjh64b
• Coherent Control of Multiphoton Transitions with Femtosecond Pulse Shaping, Physical Review A, 2001. doi:10/ffjx3v
• Optical Pulse Shaping Approaches to Coherent Control, Physics Reports, 2003. doi:10/fwwrc5

Related topics: quantum computing and thermal effects and sensing. Full list of papers here.

Publications

1. Coherent Control of Multiphoton Transitions with Femtosecond Pulse Shaping. S. A. Hosseini and D. Goswami, Physical Review A 64(3), 033410 (2001)

   BibTeX: @article{hosseiniCoherentControlMultiphoton2001,
     title = {Coherent Control of Multiphoton Transitions with Femtosecond Pulse Shaping},
     author = {Hosseini, S. Abbas and Goswami, Debabrata},
     year = {2001},
     month = aug,
     journal = {Physical Review A},
     volume = {64},
     number = {3},
     pages = {033410},
     doi = {10/ffjx3v},
     urldate = {2019-08-14},
     annotation = {GSCC: 0000066 \\
     31 citations (Crossref) [2024-05-28]\\
     00000}
   }
   

2. Control of Chemical Dynamics by Restricting Intramolecular Vibrational Relaxation. D. Goswami and W. S. Warren, The Journal of Chemical Physics 99(6), 4509–4517 (1993)

   BibTeX: @article{goswamiControlChemicalDynamics1993,
     title = {Control of Chemical Dynamics by Restricting Intramolecular Vibrational Relaxation},
     author = {Goswami, Debabrata and Warren, Warren S.},
     year = {1993},
     month = sep,
     journal = {The Journal of Chemical Physics},
     volume = {99},
     number = {6},
     pages = {4509--4517},
     issn = {0021-9606},
     doi = {10/bjh64b},
     urldate = {2019-08-14},
     annotation = {GSCC: 0000036 \\
     26 citations (Crossref) [2024-05-28]\\
     00000}
   }