物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2014年
5期
836-844
,共9页
冯海冉%李鹏%郑雨军%王德华
馮海冉%李鵬%鄭雨軍%王德華
풍해염%리붕%정우군%왕덕화
多光子%分子%激发%控制%李代数
多光子%分子%激髮%控製%李代數
다광자%분자%격발%공제%리대수
Multiphoton%Molecule%Excitation%Control%Lie-algebra
用解析代数方法研究了分子转动和激光脉冲对双原子分子多光子激发控制的影响并推导得到不同转动通道下的分子振动激发几率的解析表达式。为了考察转动能级和考虑分子转动后与激光场夹角的变化对分子多光子振动激发和振动激发控制的影响,我们计算并比较了分子纯振动和加入分子转动两种情况,并分别给出了分子与极化激光场在不同取向角下三光子选择激发的图像。研究发现分子的转动能级对多光子非共振激发有修正作用,但是分子转动会降低多光子激发的选择性,而选择合适的激光脉冲形状有利于目标多光子激发控制的实现。文中还进一步讨论了激光脉冲初相位对分子多光子激发控制的影响,发现脉冲初相位对多光子激发过程有明显的调制作用。
用解析代數方法研究瞭分子轉動和激光脈遲對雙原子分子多光子激髮控製的影響併推導得到不同轉動通道下的分子振動激髮幾率的解析錶達式。為瞭攷察轉動能級和攷慮分子轉動後與激光場夾角的變化對分子多光子振動激髮和振動激髮控製的影響,我們計算併比較瞭分子純振動和加入分子轉動兩種情況,併分彆給齣瞭分子與極化激光場在不同取嚮角下三光子選擇激髮的圖像。研究髮現分子的轉動能級對多光子非共振激髮有脩正作用,但是分子轉動會降低多光子激髮的選擇性,而選擇閤適的激光脈遲形狀有利于目標多光子激髮控製的實現。文中還進一步討論瞭激光脈遲初相位對分子多光子激髮控製的影響,髮現脈遲初相位對多光子激髮過程有明顯的調製作用。
용해석대수방법연구료분자전동화격광맥충대쌍원자분자다광자격발공제적영향병추도득도불동전동통도하적분자진동격발궤솔적해석표체식。위료고찰전동능급화고필분자전동후여격광장협각적변화대분자다광자진동격발화진동격발공제적영향,아문계산병비교료분자순진동화가입분자전동량충정황,병분별급출료분자여겁화격광장재불동취향각하삼광자선택격발적도상。연구발현분자적전동능급대다광자비공진격발유수정작용,단시분자전동회강저다광자격발적선택성,이선택합괄적격광맥충형상유리우목표다광자격발공제적실현。문중환진일보토론료격광맥충초상위대분자다광자격발공제적영향,발현맥충초상위대다광자격발과정유명현적조제작용。
The influence of molecular rotation, laser pulse shape and initial phase on controlling the infrared multiphoton excitation of diatomic molecules has been studied using an analytical algebraic approach, which involved the derivation of analytic transition probabilities with various rotational channels. To observe the correctional functions of the rotational energy and the relationship between the molecular orientation and the polarized direction of the laser field in terms of their impact on control ing multiphoton excitation, we calculated the probabilities in the purely vibrational and ro-vibrational cases. The maximum transition probabilities were determined as a function of the time and molecular orientation angle in both cases for comparison, which al owed for the target multiphoton excitations to be achieved. However, oscil ations appeared in the population of the ro-vibrational case which denoted rotational interference can decrease the selectivity of the molecular vibrational excitation. Furthermore, the rotational energy had a corrected action on multiphoton non-resonant excitation and the power of actions was dependent on the molecular anharmonicity. We have also provided a discussion of the influences of laser pulse shape and initial phase. We found that the use of an appropriate laser pluse shape afforded the target multiphoton excitation event, and that the initial phase of the chirped laser pulse had an obvious modulatory function on the multiphoton processes.