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Controlling quantum interference between virtual and dipole two-photon optical excitation pathways using phase-shaped laser pulses
- Source :
- J Phys Chem A
- Publication Year :
- 2021
- Publisher :
- arXiv, 2021.
-
Abstract
- Two-photon excitation (TPE) proceeds via a "virtual" pathway, which depends on the accessibility of one or more intermediate states, and, in the case of non-centrosymmetric molecules, an additional "dipole" pathway involving the off-resonance dipole-allowed one-photon transitions and the change in the permanent dipole moment between the initial and final states. Here, we control the quantum interference between these two optical excitation pathways by using phase-shaped femtosecond laser pulses. We find enhancements by a factor of up to 1.75 in the two-photon-excited fluorescence of the photobase FR0-SB in methanol after taking into account the longer pulse duration of the shaped laser pulses. Simulations taking into account the different responses of the virtual and dipole pathways to external fields and the effect of pulse shaping on two-photon transitions are found to be in good agreement with our experimental measurements. The observed quantum control of TPE in condensed phase may lead to enhanced signal at a lower intensity in two-photon microscopy, multiphoton-excited photoreagents, and novel spectroscopic techniques that are sensitive to the magnitude of the contributions from the virtual and dipole pathways to multiphoton excitations.<br />Comment: 27 pages, 6 figures, 1 scheme. This article has been accepted for publication in the Journal of Physical Chemistry A
- Subjects :
- Chemical Physics (physics.chem-ph)
Quantum Physics
Chemistry
Phase (waves)
Pulse duration
FOS: Physical sciences
02 engineering and technology
010402 general chemistry
021001 nanoscience & nanotechnology
Laser
01 natural sciences
Pulse shaping
Article
0104 chemical sciences
law.invention
Dipole
Two-photon excitation microscopy
law
Physics - Chemical Physics
Femtosecond
Physical and Theoretical Chemistry
Atomic physics
0210 nano-technology
Quantum Physics (quant-ph)
Excitation
Subjects
Details
- Database :
- OpenAIRE
- Journal :
- J Phys Chem A
- Accession number :
- edsair.doi.dedup.....467a860e34177af4934b9295affc2efc
- Full Text :
- https://doi.org/10.48550/arxiv.2103.09912