Coherent two-dimensional ultraviolet spectroscopy in fully noncollinear geometry.

We introduce fully noncollinear coherent two-dimensional (2D) spectroscopy in the UV domain with an all-reflective and miniaturized setup design. Phase stability is achieved via pairwise beam manipulation, and the concept can be transferred to all wavelength regimes. Here we present results from an implementation that has been optimized for wavelengths between 250 and 375 nm. Interferometric measurements prove phase stability over several hours. We obtained 2D spectra of the nonpolar UV chromophore p-terphenyl in ethanol, excited with 50 fs pulses at 287 nm.

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

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

[3]  Graham R Fleming,et al.  Phase-stabilized two-dimensional electronic spectroscopy. , 2004, The Journal of chemical physics.

[4]  Daniel B. Turner,et al.  Multidimensional coherent spectroscopy made easy , 2007 .

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

[6]  D. Jonas.  Two-dimensional femtosecond spectroscopy. , 2003, Annual review of physical chemistry.

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

[8]  V. Prokhorenko,et al.  Coherently-controlled two-dimensional photon echo electronic spectroscopy. , 2009, Optics express.

[9]  V. Prokhorenko,et al.  Diffractive optics based four-wave, six-wave, ..., nu-wave nonlinear spectroscopy. , 2009, Accounts of chemical research.

[10]  D. Zimdars,et al.  Electronic dephasing in nonpolar room temperature liquids: UV photon echo pulse duration dependent measurements , 1997 .

[11]  S. Matsika,et al.  Two-dimensional ultrafast fourier transform spectroscopy in the deep ultraviolet. , 2009, Optics express.

[12]  T. Elsaesser,et al.  Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O , 2005, Nature.

[13]  A. Tortschanoff,et al.  Photon echo peak shift experiments in the UV: p-terphenyl in different solvents , 2008 .

[14]  Y. Avlasevich,et al.  Weakly chirped pulses in frequency resolved coherent spectroscopy. , 2010, The Journal of chemical physics.

[15]  Jaroslaw Sperling,et al.  Compact phase-stable design for single- and double-quantum two-dimensional electronic spectroscopy. , 2009, Optics letters.

[16]  A. Tortschanoff,et al.  Ultrafast UV photon echo peak shift and fluorescence up conversion studies of non-polar solvation dynamics , 2008 .

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

[18]  S. Mukamel,et al.  Optical coherence and theoretical study of the excitation dynamics of a highly symmetric cyclophane-linked oligophenylenevinylene dimer. , 2006, The Journal of chemical physics.

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

[20]  G. Fleming,et al.  Wavelength-dependent resonant homodyne and heterodyne transient grating spectroscopy with a diffractive optics method: Solvent effect on the third-order signal , 2002 .

[21]  M. Cho,et al.  Ultrafast exciton transfers in DNA and its nonlinear optical spectroscopy. , 2008, The Journal of chemical physics.

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

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