Sub-5-fs transform-limited visible pulse source and its application to real-time spectroscopy

Transform-limited (TL) visible pulses with as short a duration as 4.7 fs with a 5-/spl mu/J pulse energy have been generated for the first time from a novel noncollinear optical parametric amplifier. Both signal-idler group-velocity matching and pulse-front matching are essential to generate coherent down-converted pulses compressible to the TL pulse with more than 150 THz bandwidth. Tunable operation with bandwidth-limited sub-10-fs pulses in the visible (550-700 nm) and near-infrared (900-1300 nm) ranges, achieved by increasing the seed chirp, is also a marked property. Applications for ultrafast spectroscopy of the sub-5-fs pulse source to the real-time spectroscopy of conjugated polymer, a dye molecule, and J-aggregates are also described.

[1]  D. Erni,et al.  Noncollinear parametric generation in LiIO(3) and beta-barium borate by frequency-doubled femtosecond Ti:sapphire laser pulses. , 1995, Optics letters.

[2]  Algis S. Piskarskas,et al.  Traveling-wave parametric generation of widely tunable, highly coherent femtosecond light pulses , 1993 .

[3]  D Yelin,et al.  Adaptive femtosecond pulse compression. , 1997, Optics letters.

[4]  S. Okada,et al.  Synthesis of Polydiacetylene-Based Ladder Polymer , 1997 .

[5]  Uwe Stamm,et al.  Relaxation dynamics of photoexcitations in polydiacetylenes and polythiophene , 1990 .

[6]  Audrius Dubietis,et al.  Powerful femtosecond pulse generation by chirped and stretched pulse parametric amplification in BBO crystal , 1992 .

[7]  Villeneuve,et al.  Observation of fractional revivals of a molecular wave packet. , 1996, Physical review. A, Atomic, molecular, and optical physics.

[8]  Akira Shirakawa,et al.  Noncollinear Phase- and Group-Velocity Matching of Optical Parametric Amplifier for Ultrashort Pulse Generation , 1998 .

[9]  L Gallmann,et al.  Semiconductor saturable-absorber mirror assisted Kerr-lens mode-locked Ti:sapphire laser producing pulses in the two-cycle regime. , 1999, Optics letters.

[10]  D. Akins,et al.  Fluorescence Decay Kinetics and Structure of Aggregated Tetrakis(p-Sulfonatophenyl)Porphyrin , 1996 .

[11]  Robert L. Byer,et al.  Optical parametric amplification , 1979 .

[12]  Ian N. Ross,et al.  The prospects for ultrashort pulse duration and ultrahigh intensity using optical parametric chirped pulse amplifiers , 1997 .

[13]  Róbert Szipőcs,et al.  All-solid-state cavity-dumped sub-5-fs laser , 1997 .

[14]  M M Fejer,et al.  High-energy femtosecond pulse amlification in a quasi-phase-matched parametric amplifier. , 1998, Optics letters.

[15]  J G Fujimoto,et al.  Sub-two-cycle pulses from a Kerr-lens mode-locked Ti:sapphire laser. , 1999, Optics letters.

[16]  Generation of 11-fs pulses tunable across the visible by optical parametric amplification , 1997 .

[17]  E. Riedle,et al.  Sub-20-fs pulses tunable across the visible from a blue-pumped single-pass noncollinear parametric converter. , 1997, Optics letters.

[18]  Akira Shirakawa,et al.  Sub-5-fs visible pulse generation by pulse-front-matched noncollinear optical parametric amplification , 1999 .

[19]  J. Gordon,et al.  Dynamics of spectral hole burning , 1988 .

[20]  Takayoshi Kobayashi,et al.  Real-time vibrational mode-coupling associated with ultrafast geometrical relaxation in polydiacetylene induced by sub-5-fs pulses , 2000 .

[21]  M. Cavallari,et al.  Broad-bandwidth parametric amplification in the visible: femtosecond experiments and simulations , 1998 .

[22]  Oscar E. Martínez,et al.  Achromatic phase matching for second harmonic generation of femtosecond pulses , 1989 .

[23]  Takashi Kobayashi,et al.  Broadband near‐infrared pulse generation in KTiOPO4 , 1994 .

[24]  R. Mathies,et al.  Theory of dynamic absorption spectroscopy of nonstationary states. 4. Application to 12-fs resonant impulsive Raman spectroscopy of bacteriorhodopsin , 1992 .

[25]  D. Wiersma,et al.  Amplitude and phase characterization of 4.5-fs pulses by frequency-resolved optical gating. , 1998, Optics letters.

[26]  Takayoshi Kobayashi,et al.  Femtosecond spectroscopy of a polydiacetylene with extended conjugation to acetylenic side groups , 1997 .

[27]  F Hache,et al.  Sub-20-fs tunable pulses in the visible from an 82-MHz optical parametric oscillator. , 1995, Optics letters.

[28]  Takao Fuji,et al.  Dynamical observation of Duschinsky rotation by sub-5-fs real-time spectroscopy , 2000 .

[29]  Bela Racz,et al.  Group velocity dispersion in prisms and its application to pulse compression and travelling-wave excitation , 1985 .

[30]  J. Bigot,et al.  Quantum-mechanical theory for 6 fs dynamic absorption spectroscopy and its application to nile blue , 1990 .

[31]  A. Piskarskas,et al.  Matching of group velocities in three-wave parametric interaction with femtosecond pulses and application to traveling-wave generators , 1995 .

[32]  N. Scherer,et al.  Ultrafast Pump−Probe Studies of Excited-State Charge-Transfer Dynamics in Blue Copper Proteins , 1998 .

[33]  S. Silvestri,et al.  Sub-8-fs pulses from an ultrabroadband optical parametric amplifier in the visible. , 1998, Optics letters.

[34]  Takayoshi Kobayashi,et al.  Noncollinearly phase-matched femtosecond optical parametric amplification with a 2000 cm -1 bandwidth , 1998 .

[35]  Satoshi Hirayama,et al.  Steady‐state and time‐resolved fluorescence study of some dyes in polymer microspheres showing morphology dependent resonances , 1996 .

[36]  Takayoshi Kobayashi,et al.  Pulse-front-matched optical parametric amplification for sub-10-fs pulse generation tunable in the visible and near infrared. , 1998, Optics letters.

[37]  Ulrich A. Russek,et al.  Pulse compression by use of deformable mirrors. , 1999, Optics letters.

[38]  A. Piskarskas,et al.  Matching of group velocities by spatial walk-off in collinear three-wave interaction with tilted pulses. , 1996, Optics letters.

[39]  R. Byer,et al.  Power and bandwidth of spontaneous parametric emission , 1968 .

[40]  O. Svelto,et al.  A novel-high energy pulse compression system: generation of multigigawatt sub-5-fs pulses , 1997 .

[41]  J. Fujimoto,et al.  Sub-two-cycle pulses from a Kerr-lens mode-locked Ti:sapphire laser: addenda. , 1999, Optics Letters.

[42]  S. Mukamel.  Principles of Nonlinear Optical Spectroscopy , 1995 .

[43]  G. Mourou,et al.  Wave-front correction of femtosecond terawatt lasers by deformable mirrors. , 1998, Optics letters.

[44]  Oscar E. Martínez,et al.  Pulse distortions in tilted pulse schemes for ultrashort pulses , 1986 .