PERMANENT DIPOLE-MOMENTS AND 2-COLOR MULTIPHOTON RESONANCES IN THE 2-LEVEL MOLECULE - THE ROTATING WAVE APPROXIMATION VERSUS EXACT RESULTS

被引:31
作者
KONDO, AE
BLOKKER, VM
MEATH, WJ
机构
[1] Department of Chemistry, University of Western Ontario, London
[2] Department of Applied Mathematics, University of Waterloo, Waterloo
关键词
D O I
10.1063/1.462006
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
The interaction of two continuous wave electric fields (lasers) with a two-level molecule, that has a nonzero difference d, between the permanent dipoles of the two states involved in a multiphoton two-color transition, is studied in the rotating wave approximation and by using exact methods. Analytical rotating wave approximation results for the time-dependent populations of the molecular states and for the resonance profiles are derived and used to help discuss the effects of permanent dipole moments in the two-color absorption problem. Several examples of multiphoton, two-color, two-level resonance profiles calculated in the rotating wave approximation and by using exact techniques, are employed for illustrative purposes. They are used to help quantify the conditions for the validity of the two-color rotating wave approximation, which are considerably more restrictive than the analogous conditions for the one-color rotating wave approximation with d not-equal 0, and to illustrate the interpretive and predictive nature of the rotating wave approximation results. For example, there are many multiphoton, two-color transitions that are available if a molecule possesses permanent dipoles (not-equal-to 0). The analytic rotating wave approximation expression for the molecule-two laser coupling can often be used to reliably estimate the field parameters of the two lasers that are required to optimize a given transition relative to others.
引用
收藏
页码:2544 / 2555
页数:12
相关论文
共 44 条
[1]   MULTIPHOTON TRANSITIONS IN MOLECULES WITH PERMANENT DIPOLE-MOMENTS [J].
BAND, YB ;
BAVLI, R ;
HELLER, DF .
CHEMICAL PHYSICS LETTERS, 1989, 156 (04) :405-410
[2]   NONLINEAR-OPTICAL PROPERTIES OF 2-LEVEL SYSTEMS WITH PERMANENT DIPOLE-MOMENTS [J].
BAVLI, R ;
HELLER, DF ;
BAND, YB .
PHYSICAL REVIEW A, 1990, 41 (07) :3960-3968
[3]   SEMICLASSICAL THEORY OF 2-PHOTON ABSORPTION - ABSORPTION AND LEVEL SHIFTS IN A MODEL SYSTEM [J].
BURROWS, MD ;
SALZMAN, WR .
PHYSICAL REVIEW A, 1977, 15 (04) :1636-1639
[4]   RECENT DEVELOPMENTS IN SEMICLASSICAL FLOQUET THEORIES FOR INTENSE-FIELD MULTIPHOTON PROCESSES [J].
CHU, SI .
ADVANCES IN ATOMIC AND MOLECULAR PHYSICS, 1985, 21 :197-253
[5]   THE PERMANENT MOMENT CONTRIBUTION TO 2-PHOTON ABSORPTION [J].
CRAIG, DP ;
THIRUNAMACHANDRAN, T .
CHEMICAL PHYSICS LETTERS, 1988, 148 (01) :97-100
[6]   IMPORTANCE OF INITIAL AND FINAL-STATES AS INTERMEDIATE STATES IN 2-PHOTON SPECTROSCOPY OF POLAR-MOLECULES [J].
DICK, B ;
HOHLNEICHER, G .
JOURNAL OF CHEMICAL PHYSICS, 1982, 76 (12) :5755-5760
[7]   STOCHASTIC-THEORY OF INTRAMOLECULAR ENERGY-TRANSFER IN THE PRESENCE OF RADIATION [J].
DOUGHERTY, EP ;
AUGUSTIN, SD ;
RABITZ, H .
JOURNAL OF CHEMICAL PHYSICS, 1981, 74 (02) :1175-1185
[8]   MICROWAVE IONIZATION OF HYDROGENLIKE LI AND NA ATOMS [J].
GALLAGHER, TF ;
MAHON, CR ;
PILLET, P ;
FU, PM ;
NEWMAN, JB .
PHYSICAL REVIEW A, 1989, 39 (09) :4545-4549
[9]   2-LEVEL SYSTEM IN A BICHROMATIC FIELD [J].
GUCCIONEGUSH, R ;
GUSH, HP .
PHYSICAL REVIEW A, 1974, 10 (05) :1474-1487
[10]  
Hirschfelder J. O., 1976, ADV CHEM PHYS, V35, P265