期刊
JOURNAL OF CHEMICAL PHYSICS
卷 132, 期 15, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3352553
关键词
excited states; hydrogen compounds; molecular beams; molecular moments; molecule-photon collisions; multiphoton processes; photoexcitation; rotational-vibrational states; stimulated Raman scattering; vibrational states; Zeeman effect
资金
- National Science Foundation [NSF CHE 0650414]
A density matrix treatment is presented for a general process of preparing polarized molecules through their coherent interaction with two or more infrared photons of different frequencies, each tuned to cause a transition between real levels. This process, which might be called infrared stimulated Raman adiabatic passage, allows complete population transfer to selected rotational-vibrational levels and controls the direction of the rotational angular momentum vector J of the molecule with the possibility of preparing higher moments of the J spatial distribution. HCl molecules in a supersonic molecular beam are considered as a candidate system. Theory predicts that under collision-free conditions two infrared laser pulses of microsecond duration and milliwatt power are able to achieve complete population transfer and alignment of HCl (v=2, J=2, and M=0) for mutually parallel excitation and HCl (v=2, J=2, and M=+/- 1) for mutually perpendicular excitation. Orientation of the HCl (v=2, J=2, and M=+/- 2) can also be achieved using two circularly polarized pulses of the same helicity. For simplicity, our treatment ignores nuclear spin depolarization, which would be the case for molecules such as (12)C(16)O and (12)C(16)OO(2). Polarized molecules in higher vibrational levels can be prepared using additional infrared pulses.
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