Strong field effects in rotational femtosecond degenerate four-wave mixing

被引：12

作者：

Gelin, Maxim F. ^{[1
]}

Riehn, Christoph ^{[2
]}

Kunitski, Maksim ^{[3
]}

Brutschy, Bernhard ^{[3
]}

机构：

[1] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany

[2] Tech Univ Kaiserslautern, Dept Chem, D-67663 Kaiserslautern, Germany

[3] Goethe Univ Frankfurt, Inst Phys & Theoret Chem, D-60438 Frankfurt, Germany

来源：

JOURNAL OF CHEMICAL PHYSICS | 2010年 / 132卷 / 13期

关键词：

heterodyne detection; high-speed optical techniques; multiwave mixing; INDUCED POLARIZATION SPECTROSCOPY; COHERENCE SPECTROSCOPY; NONADIABATIC ALIGNMENT; TOP MOLECULES; GAS-PHASE; DYNAMICS; PULSES;

D O I：

10.1063/1.3367726

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：

We study theoretically strong field effects in rotational femtosecond degenerate four-wave-mixing (DFWM). First, we developed a perturbative approach and calculated the leading correction to the standard (weak field) formula for femtosecond DFWM signal. Second, we constructed a nonperturbative approach for computing femtosecond DFWM signals excited by (short) pulses of arbitrary intensity. Third, we worked out the theory to describe femtosecond DFWM with an extra aligning pulse. We show that the strong-pulse-induced nonadiabatic alignment does explain many experimentally detected features that develop in femtosecond DFWM signals with increasing laser intensity beyond the standard weak field regime. However, we also show that this nonadiabatic alignment cannot solely be responsible for the onset of the heterodyne detection and pronounced constant background in DFWM signals excited by high intensity laser pulses.

引用

页数：9