A versatile ultrastable platform for optical multidimensional Fourier-transform spectroscopy.

The JILA multidimensional optical nonlinear spectrometer (JILA-MONSTR) is a robust, ultrastable platform consisting of nested and folded Michelson interferometers that can be actively phase stabilized. This platform generates a square of identical laser pulses that can be adjusted to have arbitrary time delay between them while maintaining phase stability. The JILA-MONSTR provides output pulses for nonlinear excitation of materials and phase-stabilized reference pulses for heterodyne detection of the induced signal. This arrangement is ideal for performing coherent optical experiments, such as multidimensional Fourier-transform spectroscopy, which records the phase of the nonlinear signal as a function of the time delay between several of the excitation pulses. The resulting multidimensional spectrum is obtained from a Fourier transform. This spectrum can resolve, separate, and isolate coherent contributions to the light-matter interactions associated with electronic excitation at optical frequencies. To show the versatility of the JILA-MONSTR, several demonstrations of two-dimensional Fourier-transform spectroscopy are presented, including an example of a phase-cycling scheme that reduces noise. Also shown is a spectrum that accesses two-quantum coherences, where all excitation pulses require phase locking for detection of the signal.

[1]  Alan D. Bristow,et al.  Polarization dependence of semiconductor exciton and biexciton contributions to phase-resolved optical two-dimensional Fourier-transform spectra , 2008, 0812.2914.

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

[3]  Peifang Tian,et al.  Femtosecond Phase-Coherent Two-Dimensional Spectroscopy , 2003, Science.

[4]  Daniel B. Turner,et al.  Two-Quantum 2D FT Electronic Spectroscopy of Biexcitons in GaAs Quantum Wells , 2009, Science.

[5]  A. Bristow,et al.  Optical two-dimensional fourier transform spectroscopy of semiconductor quantum wells. , 2009, Accounts of chemical research.

[6]  S. Mukamel,et al.  Two-dimensional correlation spectroscopy of two-exciton resonances in semiconductor quantum wells. , 2007, Physical review letters.

[7]  Matthew A. Montgomery,et al.  Facile collection of two-dimensional electronic spectra using femtosecond pulse-shaping Technology. , 2007, Optics express.

[8]  Jennifer P. Ogilvie,et al.  Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes , 2004 .

[9]  Andrew H Marcus,et al.  Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation. , 2007, The Journal of chemical physics.

[10]  P. Hamm,et al.  Active phase stabilization in Fourier-transform two-dimensional infrared spectroscopy. , 2005, Optics Letters.

[11]  N. Ge,et al.  Conformations of N-acetyl-L-prolinamide by two-dimensional infrared spectroscopy. , 2006, The journal of physical chemistry. B.

[12]  M. Joffre,et al.  Two-dimensional nonlinear optics using Fourier-transform spectral interferometry. , 1996, Optics Letters.

[13]  Xingcan Dai,et al.  All-optical retrieval of the global phase for two-dimensional Fourier-transform spectroscopy. , 2008, Optics express.

[14]  David M. Jonas,et al.  TWO-DIMENSIONAL ELECTRONIC SPECTROSCOPY , 1998 .

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

[16]  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.

[17]  Manuel Joffre,et al.  Linear techniques of phase measurement by femtosecond spectral interferometry for applications in spectroscopy , 1995 .

[18]  Martin T Zanni,et al.  Automated 2D IR spectroscopy using a mid-IR pulse shaper and application of this technology to the human islet amyloid polypeptide , 2007, Proceedings of the National Academy of Sciences.

[19]  Igor V. Stiopkin,et al.  Tunable two-dimensional femtosecond spectroscopy. , 2004, Optics letters.

[20]  S. Mukamel,et al.  Ultrafast optical spectroscopy of spectral fluctuations in a dense atomic vapor. , 2008, Physical review letters.

[21]  Steven T Cundiff.  Coherent spectroscopy of semiconductors. , 2008, Optics express.

[22]  Steven T. Cundiff,et al.  Optical two-dimensional Fourier transform spectroscopy of semiconductors , 2005 .

[23]  Tianhao Zhang,et al.  Many-body interactions in semiconductors probed by optical two-dimensional fourier transform spectroscopy. , 2006, Physical review letters.

[24]  Brian Patton,et al.  Heterodyne spectral interferometry for multidimensional nonlinear spectroscopy of individual quantum systems. , 2006, Optics letters.

[25]  Minhaeng Cho,et al.  Coherent two-dimensional optical spectroscopy. , 2008, Chemical reviews.

[26]  T. Kuhn,et al.  Femtosecond spectroscopy in semiconductors: a key to coherences, correlations and quantum kinetics , 2004 .

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

[28]  Tobias Brixner,et al.  Inherently phase-stable coherent two-dimensional spectroscopy using only conventional optics. , 2008, Optics letters.

[29]  Steel Dg,et al.  Observation of the ultrafast two-photon coherent biexciton oscillation in a GaAs/AlxGa1-xAs multiple quantum well. , 1996 .

[30]  Shaul Mukamel,et al.  Isolating excitonic Raman coherence in semiconductors using two-dimensional correlation spectroscopy. , 2008, The Journal of chemical physics.

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

[32]  Tianhao Zhang,et al.  Optical two-dimensional Fourier transform spectroscopy with active interferometric stabilization. , 2005, Optics express.

[33]  Joshua C Vaughan,et al.  Coherently controlled ultrafast four-wave mixing spectroscopy. , 2007, The journal of physical chemistry. A.

[34]  R. Mirin,et al.  Polarization-dependent optical 2D Fourier transform spectroscopy of semiconductors , 2007, Proceedings of the National Academy of Sciences.

[35]  J. Semmlow,et al.  Rapid phase-cycled two-dimensional optical spectroscopy in fluorescence and transmission mode. , 2005, Optics express.