Implementation of continuous fast scanning detection in femtosecond Fourier-transform two-dimensional vibrational-electronic spectroscopy to decrease data acquisition time.

Femtosecond Fourier transform two-dimensional vibrational-electronic (2D VE) spectroscopy is a recently developed third-order nonlinear spectroscopic technique to measure coupled electronic and vibrational motions in the condensed phase. The viability of femtosecond multidimensional spectroscopy as an analytical tool requires improvements in data collection and processing to enhance the signal-to-noise ratio and increase the amount of data collected in these experiments. Here a continuous fast scanning technique for the efficient collection of 2D VE spectroscopy is described. The resulting 2D VE spectroscopic method gains sensitivity by reducing the effect of laser drift, as well as decreasing the data collection time by a factor of 10 for acquiring spectra with a high signal-to-noise ratio within 3 dB of the more time intensive step scanning methods. This work opens the door to more comprehensive studies where 2D VE spectra can be collected as a function of external parameters such as temperature, pH, and polarization of the input electric fields.

[1]  P. Hamm,et al.  Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy. , 2017, Chemical reviews.

[2]  S. Mosquera-Vázquez,et al.  Ultrabroadband 2D electronic spectroscopy with high-speed, shot-to-shot detection. , 2017, Optics express.

[3]  Martin T Zanni,et al.  Broadband 2D electronic spectrometer using white light and pulse shaping: noise and signal evaluation at 1 and 100 kHz. , 2017, Optics express.

[4]  Daniele M. Monahan,et al.  Rapid and economical data acquisition in ultrafast frequency-resolved spectroscopy using choppers and a microcontroller. , 2016, Optics express.

[5]  Caitlin C. Bannan,et al.  Investigating vibrational relaxation in cyanide-bridged transition metal mixed-valence complexes using two-dimensional infrared and infrared pump-probe spectroscopies , 2016, Structural dynamics.

[6]  Amber T. Krummel,et al.  2D IR spectroscopy at 100 kHz utilizing a Mid-IR OPCPA laser source. , 2016, Optics express.

[7]  Trevor L. Courtney,et al.  Two-dimensional vibrational-electronic spectroscopy. , 2015, The Journal of chemical physics.

[8]  Jennifer P Ogilvie,et al.  Two-Color Nonlinear Spectroscopy for the Rapid Acquisition of Coherent Dynamics. , 2015, The journal of physical chemistry letters.

[9]  Laura Estergreen,et al.  Measuring Coherently Coupled Intramolecular Vibrational and Charge-Transfer Dynamics with Two-Dimensional Vibrational-Electronic Spectroscopy. , 2015, The journal of physical chemistry letters.

[10]  Thomas A A Oliver,et al.  Correlating the motion of electrons and nuclei with two-dimensional electronic–vibrational spectroscopy , 2014, Proceedings of the National Academy of Sciences.

[11]  Caitlin C. Bannan,et al.  Investigating vibrational anharmonic couplings in cyanide-bridged transition metal mixed valence complexes using two-dimensional infrared spectroscopy. , 2014, The Journal of chemical physics.

[12]  Trevor L. Courtney,et al.  Enhanced interferometric detection in two-dimensional spectroscopy with a Sagnac interferometer. , 2014, Optics letters.

[13]  Josef A. Dunbar,et al.  Accelerated 2D-IR Using Compressed Sensing , 2013 .

[14]  Amber T. Krummel,et al.  Active Bragg angle compensation for shaping ultrafast mid-infrared pulses. , 2012, Optics express.

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

[16]  J. Loparo,et al.  A fast-scanning Fourier transform 2D IR interferometer , 2011 .

[17]  M. Cho.  Two-Dimensional Optical Spectroscopy , 2009 .

[18]  J. Ogilvie,et al.  Two-dimensional Fourier transform electronic spectroscopy with a pulse-shaper , 2009 .

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

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

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

[22]  Andrei Tokmakoff,et al.  Two-dimensional Fourier transform spectroscopy in the pump-probe geometry. , 2007, Optics letters.

[23]  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.

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

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

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

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

[28]  Andrei Tokmakoff,et al.  Coherent 2D IR Spectroscopy: Molecular Structure and Dynamics in Solution , 2003 .

[29]  J. Asbury,et al.  Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics , 2003 .

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

[31]  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.

[32]  G. Walker,et al.  Ultrafast Infrared Spectroscopy of Vibrational States Prepared by Photoinduced Electron Transfer in (CN)5FeCNRu(NH3)5 , 2000 .

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

[34]  J. Hupp,et al.  Solvent control of vibronic coupling upon intervalence charge transfer excitation of (CN)5FeCNRru(NH3)5- as revealed by resonance raman and near-infrared absorption spectroscopies [22] , 1998 .

[35]  K. W. Raine,et al.  An Unmodulated Bi-Directional Fringe-Counting Interferometer System for Measuring Displacement , 1979 .

[36]  Peter Hamm,et al.  Compact implementation of Fourier transform two-dimensional IR spectroscopy without phase ambiguity , 2011 .

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