Femtosecond Phase-Coherent Two-Dimensional Spectroscopy

Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.

[1]  M. Fayer,et al.  Two-dimensional time-frequency ultrafast infrared vibrational echo spectroscopy. , 2001, Physical review letters.

[2]  R. R. Ernst,et al.  Two‐dimensional spectroscopy. Application to nuclear magnetic resonance , 1976 .

[3]  D. Wiersma,et al.  Heterodyne-detected stimulated photon echo : applications to optical dynamics in solution , 1998 .

[4]  R. Hochstrasser,et al.  STRUCTURE OF THE AMIDE I BAND OF PEPTIDES MEASURED BY FEMTOSECOND NONLINEAR-INFRARED SPECTROSCOPY , 1998 .

[5]  P. Hamm,et al.  Subpicosecond conformational dynamics of small peptides probed by two-dimensional vibrational spectroscopy , 2001, Proceedings of the National Academy of Sciences of the United States of America.

[6]  O. Golonzka,et al.  Vibrational anharmonicities revealed by coherent two-dimensional infrared spectroscopy. , 2001, Physical review letters.

[7]  S. Mukamel,et al.  Design strategies for pulse sequences in multidimensional optical spectroscopies , 2001 .

[8]  A. Weiner.  Femtosecond pulse shaping using spatial light modulators , 2000 .

[9]  David M. Jonas,et al.  Two-dimensional Fourier transform electronic spectroscopy , 2001 .

[10]  D. Goswami,et al.  Rapid ultrafine-tunable optical delay line at the 1.55-mum wavelength. , 1998, Optics letters.

[11]  A. Zewail,et al.  Optical analogs of NMR phase coherent multiple pulse spectroscopy , 1981 .

[12]  R. Hochstrasser,et al.  Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes. , 2000, Proceedings of the National Academy of Sciences of the United States of America.

[13]  G. Bodenhausen,et al.  Principles of nuclear magnetic resonance in one and two dimensions , 1987 .

[14]  R. Hochstrasser,et al.  Two-dimensional IR spectroscopy can be designed to eliminate the diagonal peaks and expose only the crosspeaks needed for structure determination , 2001, Proceedings of the National Academy of Sciences of the United States of America.

[15]  Peter Hamm,et al.  Nonlinear two-dimensional vibrational spectroscopy of peptides , 2002 .

[16]  S. Mukamel,et al.  Ultrafast Phenomena XII , 2001 .

[17]  Graham R. Fleming,et al.  Fluorescence‐detected wave packet interferometry: Time resolved molecular spectroscopy with sequences of femtosecond phase‐locked pulses , 1991 .

[18]  Warren S. Warren,et al.  Role of Pulse Phase and Direction in Two-Dimensional Optical Spectroscopy , 1999 .

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

[20]  S. Mukamel,et al.  Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations. , 2000, Annual review of physical chemistry.