Background-free nonlinear microspectroscopy with vibrational molecular interferometry

We demonstrate a method for performing nonlinear microspectroscopy that provides an intuitive and unified description of the various signal contributions, and allows the direct extraction of the vibrational response. Three optical fields create a pair of Stokes Raman pathways that interfere in the same vibrational state. Frequency modulating one of the fields leads to amplitude modulations on all of the fields. This vibrational molecular interferometry (VMI) technique allows imaging at high speed free of non-resonant background, and is able to distinguish between electronic and vibrational contributions to the total signal.

[1]  Mischa Bonn,et al.  Quantitative CARS spectroscopy using the maximum entropy method: the main lipid phase transition. , 2007, Chemphyschem : a European journal of chemical physics and physical chemistry.

[2]  Andreas Volkmer,et al.  Time-resolved coherent anti-Stokes Raman scattering microscopy: Imaging based on Raman free induction decay , 2002 .

[3]  J P Korterik,et al.  Background free CARS imaging by phase sensitive heterodyne CARS. , 2008, Optics express.

[4]  S. A. Akhmanov,et al.  Coherent ellipsometry of Raman scattering of light , 1977 .

[5]  Application of spectral phase shaping to high resolution CARS spectroscopy. , 2008, Optics express.

[6]  S. Mukamel,et al.  Stimulated coherent anti-Stokes Raman spectroscopy (CARS) resonances originate from double-slit interference of two-photon Stokes pathways , 2010, Proceedings of the National Academy of Sciences.

[7]  Origin of spectral interferences in femtosecond stimulated Raman microscopy , 2011 .

[8]  J. Lindsey,et al.  PhotochemCAD ‡ : A Computer‐Aided Design and Research Tool in Photochemistry , 1998 .

[9]  Alfred Leitenstorfer,et al.  Ultrabroadband background-free coherent anti-Stokes Raman scattering microscopy based on a compact Er:fiber laser system. , 2010, Optics letters.

[10]  Yaron Silberberg,et al.  Quantum control of coherent anti-Stokes Raman processes , 2002 .

[11]  J P Korterik,et al.  Vibrational phase contrast microscopy by use of coherent anti-Stokes Raman scattering. , 2009, Physical review letters.

[12]  R. Glauber Coherent and incoherent states of the radiation field , 1963 .

[13]  H. Offerhaus,et al.  Exploring, tailoring, and traversing the solution landscape of a phase-shaped CARS process. , 2010, Optics express.

[14]  Andrew G. Glen,et al.  APPL , 2001 .

[15]  J Greve,et al.  Polarization sensitive coherent anti-Stokes Raman scattering spectroscopy of the amide I band of proteins in solutions. , 1992, Biophysical journal.

[16]  Yuexin Liu,et al.  Broadband CARS spectral phase retrieval using a time-domain Kramers-Kronig transform. , 2009, Optics letters.

[17]  O. Katz,et al.  Single-pulse stimulated Raman scattering spectroscopy. , 2010, Optics letters.

[18]  Herman L. Offerhaus,et al.  High‐resolution narrowband CARS spectroscopy in the spectral fingerprint region , 2008 .

[19]  Conor L Evans,et al.  Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging. , 2006, Optics letters.

[20]  T. Greenhalgh 42 , 2002, BMJ : British Medical Journal.

[21]  X. Xie,et al.  Polarization coherent anti-Stokes Raman scattering microscopy. , 2001, Optics letters.

[22]  Stephen R. Leone,et al.  Single pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy (CARS) , 2005 .

[23]  M. Shapiro,et al.  Laser control of molecular processes. , 1992, Annual review of physical chemistry.

[24]  Delong Zhang,et al.  Highly Sensitive Vibrational Imaging by Femtosecond Pulse Stimulated Raman Loss. , 2011, The journal of physical chemistry letters.