PMID- 16208734
OWN - NLM
STAT- PubMed-not-MEDLINE
DCOM- 20070212
LR  - 20051017
IS  - 1439-4235 (Print)
IS  - 1439-4235 (Linking)
VI  - 6
IP  - 10
DP  - 2005 Oct 14
TI  - Systematic control of nonlinear optical processes using optimally shaped 
      femtosecond pulses.
PG  - 1970-2000
AB  - This article reviews experimental efforts to control multiphoton transitions 
      using shaped femtosecond laser pulses, and it lays out the systematic study being 
      followed by us for elucidating the effect of phase on nonlinear optical 
      laser-molecule interactions. Starting with a brief review of nonlinear optics and 
      how nonlinear optical processes depend on the electric field inducing them, a 
      number of conclusions can be drawn directly from analytical solutions of the 
      equations. From a Taylor expansion of the phase in the frequency domain, we learn 
      that nonlinear optical processes are affected only by the second- and 
      higher-order terms. This simple result has significant implications on how 
      pulse-shaping experiments are to be designed. If the phase is allowed to vary 
      arbitrarily as a continuous function, then an infinite redundancy that arises 
      from the addition of a linear phase function across the spectrum with arbitrary 
      offset and slope could prevent us from carrying out a closed-loop optimization 
      experiment. The early results illustrate how the outcome of a nonlinear optical 
      transition depends on the cooperative action of all frequencies in the bandwidth 
      of a laser pulse. Maximum constructive or destructive interference can be 
      achieved by programming the phase using only two phase values, 0 and pi. This 
      assertion has been confirmed experimentally, where binary phase shaping (BPS) was 
      shown to outperform other alternative functions, sometimes by at least on order 
      of magnitude, in controlling multiphoton processes. Here we discuss the solution 
      of a number of nonlinear problems that range from narrowing the second harmonic 
      spectrum of a laser pulse to optimizing the competition between two- and 
      three-photon transitions. This Review explores some present and future 
      applications of pulse shaping and coherent control.
FAU - Lozovoy, Vadim V
AU  - Lozovoy VV
AD  - Department of Chemistry, Michigan State University, East Lansing, MI 48824, USA.
FAU - Dantus, Marcos
AU  - Dantus M
LA  - eng
PT  - Journal Article
PL  - Germany
TA  - Chemphyschem
JT  - Chemphyschem : a European journal of chemical physics and physical chemistry
JID - 100954211
EDAT- 2005/10/07 09:00
MHDA- 2005/10/07 09:01
CRDT- 2005/10/07 09:00
PHST- 2005/10/07 09:00 [pubmed]
PHST- 2005/10/07 09:01 [medline]
PHST- 2005/10/07 09:00 [entrez]
AID - 10.1002/cphc.200400342 [doi]
PST - ppublish
SO  - Chemphyschem. 2005 Oct 14;6(10):1970-2000. doi: 10.1002/cphc.200400342.