Pulse Shaping and Coherent Control

Shaped femtosecond pulses to steer molecular dynamics

Schematic illustration for Pulse Shaping and Coherent Control

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 that shaped pulses can govern the redistribution of excitation energy.

Technique

A femtosecond pulse shaper converts between the time and frequency domains, so the spectral phase and amplitude of the pulse can be programmed. The lab applies this to gaseous and liquid-phase molecular dynamics, including coherent control of multiphoton transitions [2]. The theoretical and experimental foundations are reviewed in [3].

Representative papers

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

Publications

  1. Optical Pulse Shaping Approaches to Coherent Control. D. Goswami, Physics Reports 374(6), 385–481 (2003)
    BibTeX: @article{goswamiOpticalPulseShaping2003,
      title = {Optical Pulse Shaping Approaches to Coherent Control},
      author = {Goswami, Debabrata},
      year = {2003},
      month = feb,
      journal = {Physics Reports},
      volume = {374},
      number = {6},
      pages = {385--481},
      issn = {0370-1573},
      doi = {10/fwwrc5},
      urldate = {2019-08-14},
      annotation = {GSCC: 0000364 \\
      226 citations (Crossref) [2024-05-28]\\
      00000}
    }
    
  2. 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}
    }
    
  3. 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}
    }