期刊
PHYSICAL REVIEW LETTERS
卷 125, 期 5, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.125.053201
关键词
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资金
- National Natural Science Foundation of China (NSFC) [61625501, 61427816, 11834004, 11761141004]
- National Key R&D Program of China [2018YFA0306303]
- MEXT (Ministry of Education, Culture, Sports, Science and Technology) [19002006, 15H05696]
- 111 project of China [B12024]
- Shanghai Science and Technology Commission [19JC1412200]
A fine manipulation of population transfer among molecular quantum levels is a key technology for control of molecular processes. When a light field intensity is increased to the TW-PW cm(-2) level, it becomes possible to transfer a population to specific excited levels through nonlinear light-molecule interaction, but it has been a challenge to control the extent of the population transfer. We deplete the population in the X-2 Sigma(+)(g) (v = 0) state of N-2(+) almost completely by focusing a dual-color (800 nm and 1.6 mu m) intense femtosecond laser pulse in a nitrogen gas, and make the intensity of N-2(+) lasing at 391 nm enhanced by 5-6 orders of magnitude. By solving a time-dependent Schrodinger equation describing the population transfer among the three lowest electronic states of N-2(+), we reveal that the X-2 Sigma(+)(g) (v = 0) population is depleted by the vibrational Raman excitation followed by the electronic excitation A(2)Pi(u)(v = 2,3,4) <- X-2 Sigma(+)(g)(v = 1) <- X-2 Sigma(+)(g) (v = 0), resulting in the excessive population inversion between the B-2 Sigma(+)(u) (v = 0) and X-2 Sigma(+)(g) (v = 0) states. Our results offer a promising route to efficient population transfer among vibrational and electronic levels of molecules by a precisely designed intense laser field.
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