Two-dimensional THz spectroscopy of liquids: non-linear vibrational response to a series of THz laser pulses

Abstract We propose a non-linear experiment using the non-linear interaction with THz pulses, the generation of which has recently become well established. In the lowest non-linear process, we have two controllable delay times. This is another optical analogue of two-dimensional (2D) NMR as the recently developed 2D Raman spectroscopy. Our model calculation for liquid water demonstrates the striking capability of the proposed technique, clearly distinguishing two types of anharmonicity in the low-frequency modes.

[1]  Steffen,et al.  Femtosecond two-dimensional spectroscopy of molecular motion in liquids. , 1996, Physical review letters.

[2]  Y. Tanimura,et al.  Interplay of inhomogeneity and anharmonicity in 2D Raman spectroscopy of liquids , 1997 .

[3]  K. Nelson,et al.  Time-resolved vibrational spectroscopy in the impulsive limit , 1994 .

[4]  S. Mukamel,et al.  Two-Dimensional Raman Spectroscopy of Vibrational Interactions in Liquids , 1997 .

[5]  Y. Tanimura,et al.  The (2n+1)th-order off-resonant spectroscopy from the (n+1)th-order anharmonicities of molecular vibrational modes in the condensed phase , 1997 .

[6]  K. Wynne,et al.  Ultrafast Dipole Solvation Measured in the Far Infrared , 1997 .

[7]  S. Mukamel,et al.  Two-dimensional femtosecond vibrational spectroscopy of liquids , 1993 .

[8]  Klaas Wynne,et al.  Femtosecond far-infrared pump-probe spectroscopy: A new tool for studying low-frequency vibrational dynamics in molecular condensed phases , 1997 .

[9]  C. Schmuttenmaer,et al.  FAR-INFRARED DIELECTRIC PROPERTIES OF POLAR LIQUIDS PROBED BY FEMTOSECOND TERAHERTZ PULSE SPECTROSCOPY , 1996 .

[10]  D. Mittleman,et al.  Terahertz spectroscopy of water in inverse micelles , 1997 .

[11]  J. Fourkas,et al.  Polarization selectivity of nonresonant spectroscopies in isotropic media , 1997 .

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

[13]  Tominaga,et al.  Fifth order optical response of liquid CS2 observed by ultrafast nonresonant six-wave mixing. , 1995, Physical review letters.

[14]  Norbert F. Scherer,et al.  Pulsed Terahertz Transmission Spectroscopy of Liquid CHCl3, CCl4, and their Mixtures , 1996 .

[15]  Y. Tanimura,et al.  Femtosecond two-dimensional spectroscopy from anharmonic vibrational modes of molecules in the condensed phase , 1997 .

[16]  A. Tokmakoff,et al.  Two-dimensional Raman spectroscopy of the intermolecular modes of liquid CS2 , 1997 .

[17]  S. Saito,et al.  Off-resonant fifth-order nonlinear response of water and CS2: Analysis based on normal modes , 1998 .

[18]  S. Mukamel,et al.  Off-resonant transient birefringence in liquids , 1993 .