A phase-sensitive detection method using diffractive optics for polarization-selective femtosecond Raman spectroscopy

被引：45

作者：

Khalil, M ^{[1
]}

Demirdöven, N ^{[1
]}

Golonzka, O ^{[1
]}

Fecko, CJ ^{[1
]}

Tokmakoff, A ^{[1
]}

机构：

[1] MIT, Dept Chem, Cambridge, MA 02139 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2000年 / 104卷 / 24期

关键词：

D O I：

10.1021/jp994455q

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A phase-sensitive detection method that uses two diffractive optics for femtosecond nonresonant Raman spectroscopy is demonstrated. One diffractive optic is used for generating the three input pulses for the third-order nonlinear experiment, and the second is used for recombining the signal with a passively phase-locked local oscillator derived from the probe pulse. This approach allows for phase-sensitive detection, direct phase calibration, control over all field polarizations, and removal of unwanted two-pulse signal contributions. Experiments on the intermolecular dynamics of CS2 and CH3CN demonstrate that the birefringent (in-quadrature) signal amplitude is significantly greater than the dichroic tin-phase) contribution. Polarization selective measurements are used to project the isotropic birefringent response for CS2, which suppresses reorientational dynamics and allows interaction-induced effects to be observed.

引用

页码：5711 / 5715

页数：5

共 34 条

[1] Fifth-order two-dimensional Raman spectra of CS2 are dominated by third-order cascades [J].