Phase-cycling schemes for pump–probe beam geometry two-dimensional electronic spectroscopy

Experimental demonstrations and detailed theoretical explanations are provided for a thorough understanding of the various phase-cycling schemes in an optical pulse shaper assisted two-dimensional electronic spectroscopy (2DES) in a pump–probe beam geometry. We show that two and three-step phase-cycling schemes can be employed to retrieve both rephasing and nonrephasing 2D spectra. The studies were performed on the Qy transition of chlorophyll a.

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

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

[3]  Peter Hamm,et al.  Purely absorptive three-dimensional infrared spectroscopy. , 2009, The Journal of chemical physics.

[4]  H. Tan,et al.  Theory and phase-cycling scheme selection principles of collinear phase coherent multi-dimensional optical spectroscopy. , 2008, The Journal of chemical physics.

[5]  Martin T Zanni,et al.  How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping. , 2009, Physical chemistry chemical physics : PCCP.

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

[7]  Graham R. Fleming,et al.  Two-dimensional electronic spectroscopy and photosynthesis: Fundamentals and applications to photosynthetic light-harvesting , 2011 .

[8]  Justin R. Caram,et al.  Direct evidence of quantum transport in photosynthetic light-harvesting complexes , 2011, Proceedings of the National Academy of Sciences.

[9]  Suxia Yan,et al.  Phase cycling schemes for two-dimensional optical spectroscopy with a pump―probe beam geometry , 2009 .

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

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

[12]  Alán Aspuru-Guzik,et al.  Conformation of self-assembled porphyrin dimers in liposome vesicles by phase-modulation 2D fluorescence spectroscopy , 2011, Proceedings of the National Academy of Sciences.

[13]  Andrew F Fidler,et al.  Single-shot gradient-assisted photon echo electronic spectroscopy. , 2011, The journal of physical chemistry. A.

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

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

[16]  Jeffrey A. Myers,et al.  Two-color two-dimensional Fourier transform electronic spectroscopy with a pulse-shaper. , 2008 .

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