Fluorescence‐detected wave packet interferometry: Time resolved molecular spectroscopy with sequences of femtosecond phase‐locked pulses

We introduce a novel spectroscopic technique which utilizes a two‐pulse sequence of femtosecond duration phase‐locked optical laser pulses to resonantly excite vibronic transitions of a molecule. In contrast with other ultrafast pump–probe methods, in this experiment a definite optical phase angle between the pulses is maintained while varying the interpulse delay with interferometric precision. For the cases of in‐phase, in‐quadrature, and out‐of‐phase pulse pairs, respectively, the optical delay is controlled to positions that are integer, integer plus one quarter, and integer plus one half multiples of the wavelength of a selected Fourier component. In analogy with a double slit optical interference experiment, the two the two pulse experiments reported herein involve the preparation and quantum interference of two nuclear wave packet amplitudes state of a molecule.These experiments are designed to be sensitive to the total phase evolution of the wave packet prepared by the initial pulse. The direct de...

[1]  E L Green,et al.  Active stabilization of a Michelson interferometer by an electrooptically tuned laser. , 1980, Applied optics.

[2]  A. Zewail,et al.  Femtosecond temporal spectroscopy and direct inversion to the potential: Application to iodine , 1990 .

[3]  B. Garside.  Optical Resonance and Two-level Atoms , 1975 .

[4]  E. Heller.  Quantum corrections to classical photodissociation models , 1978 .

[5]  Samuel H. Tersigni,et al.  Wavepacket dancing: Achieving chemical selectivity by shaping light pulses , 1989 .

[6]  K. Freed,et al.  ENHANCEMENT OF QUANTUM INTERFERENCE EFFECTS. , 1976 .

[7]  M. Shapiro,et al.  Coherent radiative control of unimolecular reactions: Selective bond breaking with picosecond pulses , 1989 .

[8]  A. Siegman,et al.  Ultrafast Phenomena V , 1986 .

[9]  R. Leroy.  Spectroscopic reassignment and ground-state dissociation energy of molecular iodine , 1970 .

[10]  H. Avramopoulos,et al.  Bandwidth limitation and distinct operating regimes of passively mode-locked dye lasers using strong phase shaping , 1991 .

[11]  Stuart A. Rice,et al.  Control of selectivity of chemical reaction via control of wave packet evolution , 1985 .

[12]  J. Jortner,et al.  Some features of coherent optical effects in large molecules , 1978 .

[13]  Andrew M. Weiner,et al.  Analysis of picosecond pulse shape synthesis by spectral masking in a grating pulse compressor , 1986 .

[14]  C. cohen-tannoudji,et al.  Quantum Mechanics: , 2020, Fundamentals of Physics II.

[15]  Jean-Claude Diels,et al.  Multiphoton coherent excitation of molecules , 1986 .

[16]  A. H. Zewail,et al.  Femtosecond laser observations of molecular vibration and rotation , 1990, Nature.

[17]  K. Freed,et al.  Intramolecular vibrational energy redistribution and the time evolution of molecular fluorescence , 1980 .

[18]  Y. P. Zhang,et al.  Depolarization ratios of resonance Raman scattering in the gas phase , 1989 .

[19]  J. Ferraro,et al.  Fourier Transform Infrared Spectroscopy: Applications to Chemical Systems , 1978 .

[20]  R. Keller,et al.  Photon-induced ionization changes in a neon discharge , 1978 .

[21]  D. Haar,et al.  Statistical Physics , 1971, Nature.

[22]  Robert R. Alfano,et al.  Picosecond characteristics of a spectrograph measured by a streak camera/video readout system , 1980 .

[23]  M. Salour.  Quantum interference effects in two-photon spectroscopy , 1978 .

[24]  Marlan O. Scully,et al.  Theory of Optical Free-Induction Decay and Two-Photon Superradiance , 1973 .

[25]  A. Zewail,et al.  Femtosecond selective control of wave packet population , 1990 .

[26]  Warren S. Warren,et al.  The Art of Pulse Crafting: Applications to Magnetic Resonance and Laser Spectroscopy , 1988 .

[27]  Stuart A. Rice,et al.  Coherent pulse sequence induced control of selectivity of reactions , 1986, International Laser Science Conference.

[28]  J. Cina,et al.  Optical impulsive excitation of molecular pseudorotation in Jahn–Teller systems , 1990 .

[29]  A. Marshall,et al.  High-resolution multiple-ion simultaneous monitoring by means of multiple-foldover Fourier transform ion cyclotron resonance mass spectrometry. , 1988, Analytical chemistry.

[30]  W. Wilson,et al.  Picosecond time-scale phase-related optical pulses: measurement of sodium optical coherence decay by observation of incoherent fluorescence , 1989 .

[31]  Graham R. Fleming,et al.  Time resolved dynamics of isolated molecular systems studied with phase‐locked femtosecond pulse pairs , 1990 .

[32]  Shenghua Shi,et al.  Optimal control of selective vibrational excitation of harmonic molecules: Analytic solution and restricted forms for the optimal fields , 1990 .

[33]  D A Wiersma,et al.  Picosecond Holographic-Grating Spectroscopy , 1987, Science.