Optimal Control of Nonadiabatic Alignment of Rotationally Cold<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">N</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>Molecules with the Feedback of Degree of Alignment

Suzuki, Takayuki; Sugawara, Y.; Minemoto, Shinichirou; Sakai, Hirofumi

doi:10.1103/physrevlett.100.033603

Cited by 44 publications

(29 citation statements)

References 33 publications

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“…This is desirable for applications where the presence of a strong laser field interferes. The impulsive alignment that can be achieved using a single laser pulse is intrinsically limited 13 but can be improved by applying a laser-pulse sequence 13,19 or an appropriately tailored laser-pulse profile 20,21 .The availability of aligned molecules has sparked the emergence of new techniques such as tomographic imaging of electronic orbitals 11 , and the observation of multicentre interference in highharmonic generation as a tool for structural determination 12 . Further improvements in the alignment of molecules are likely to enable new applications, such as diffractive imaging at emerging X-ray free-electron lasers such as LCLS at Stanford, XFEL at Hamburg and SCSS at 23 .…”

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Impulsive orientation and alignment of quantum-state-selected NO molecules

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Manipulation of the molecular-axis distribution is an important ingredient in experiments aimed at understanding and controlling molecular processes 1-6 . Samples of aligned or oriented molecules can be obtained following the interaction with an intense laser field 7-9 , enabling experiments in the molecular rather than the laboratory frame 10-12 . However, the degree of impulsive molecular orientation and alignment that can be achieved using a single laser field is limited 13 and crucially depends on the initial states, which are thermally populated. Here we report the successful demonstration of a new technique for laser-field-free orientation and alignment of molecules that combines an electrostatic field, non-resonant femtosecond laser excitation 14 and the preparation of state-selected molecules using a hexapole 2 . As a unique quantum-mechanical wavepacket is formed, a large degree of orientation and alignment is observed both during and after the femtosecond laser pulse, which is even further increased (to cos θ = −0.74 and cos 2 θ = 0.82, respectively) by tailoring the shape of the femtosecond laser pulse. This work should enable new applications such as the study of reaction dynamics or collision experiments in the molecular frame, and orbital tomography 11 of heteronuclear molecules.The outcome of molecular collision experiments is strongly affected by the angular anisotropies in the initial molecular axis distribution. In bimolecular and molecule-surface collisions, collision cross-sections sensitively depend on the relative arrangement of the collision partners 1,2 . Likewise, photon-molecule collisions such as X-ray diffraction and photodissocation experiments aimed at the elucidation of molecular structure or photochemical activity depend on and can benefit from angular confinement of the sample 3,4 . The two most important moments of the molecular axis distribution are the 'alignment' ( cos 2 θ ) and 'orientation' ( cosθ ), where θ is the angle between the molecular axis and a reference axis.First attempts to orient and align molecules relied on electrostatic fields. A hexapole electric field can be used to stateselect polar molecules and orient them through their first-order Stark effect 2,5 using a moderate field strength. The orientation is limited by the selected state. 'Brute-force orientation' uses a strong homogeneous electrostatic field and relies on the second-and higher-order Stark effect 6 . It requires molecules with a large dipole moment and extremely high electric-field strengths.As a part of extensive efforts aimed at achieving laser-controlled chemistry 15-17 , laser-controlled alignment 8 has attracted considerable attention. Suitably chosen laser fields can exert torques on molecules, exploiting the interaction of the laser field with the molecular polarizability. Both adiabatic alignment, where molecules are exposed to a slowly varying laser field 18 , and non-adiabatic (impulsive) alignment, where molecules align after receiving a kick by a short laser pulse 7 , have been succe...

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Impulsive orientation and alignment of quantum-state-selected NO molecules

et al. 2009

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“…Different from the sample molecules at room temperature, the alignment is optimized by doubly peaked pulses with approximately equal intensities for rotationally cold molecules. 80 Based on the considerations in both temporal and frequency domains, it is found that the double-peaked pulse with an appropriate interval can induce nonadiabatic molecular alignment virtually equivalent to that induced by a single pulse with an appropriate duration.…”

Section: Enhancement Of Molecular Alignmentmentioning

confidence: 98%

Field-Free Molecular Alignment by Two Femosecond Laser Pulses

Hong-bing

Gong

2011

Advances in Multi-Photon Processes and Spectroscopy

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Field-free molecular alignment can be achieved by nonadiabatic rotational excitation of molecules with strong femtosecond laser pulses. We reviewed our recent progresses in controling the rotational wavepacket of molecules created by two strong femtosecond laser pulses. Through adjusting the time delay between the two laser pulses, we can control the rotational population as well as the alignment structures. The potential application of aligned molecules is also included in tuning the frequency of few cycle pulses.

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“…The shaped femtosecond laser pulses have been widely used in the coherent control of the molecular ensembles. [20][21][22][23][24] Also, these phase-shaped laser pulses have been used in the rotational and vibrational control and further molecular alignment manipulation. [25][26][27] It has been demonstrated that the degree of the molecular alignment could be greatly enhanced by the phase-shaped laser pulses.…”

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confidence: 99%

Manipulation of the Molecular Orientation by Combined Electrostatic and Phase-Shaped Laser Fields

Huang

2012

J. Nonlinear Optic. Phys. Mat.

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We theoretically show that the field-free molecular orientation induced by the combined electrostatic and laser fields can be manipulated through shaping the femtosecond laser pulse with periodic phase step modulation. By adjusting the modulation time τ or the modulation depth δ, the maximum degree of the molecular orientation can be fully suppressed or reconstructed by the combined electrostatic and the transform-limited laser fields. The relations between the maximum degree of the field-free molecular orientation and the laser intensity, the amplitude of the electrostatic field, as well as the rotational temperature are also investigated.

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Optimal Control of Nonadiabatic Alignment of Rotationally ColdN2Molecules with the Feedback of Degree of Alignment

Cited by 44 publications

References 33 publications

Impulsive orientation and alignment of quantum-state-selected NO molecules

Impulsive orientation and alignment of quantum-state-selected NO molecules

Field-Free Molecular Alignment by Two Femosecond Laser Pulses

Manipulation of the Molecular Orientation by Combined Electrostatic and Phase-Shaped Laser Fields

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