Field-free Three-Dimensional Orientation of Asymmetric-Top Molecules

Abstract

Alignment and orientation of molecules by intense, ultrashort laser fields are crucial for a variety of applications in physics and chemistry. These include control of high harmonics generation, molecular orbitals tomography, control of molecular photoionization and dissociation processes, production of "molecular movies" with the help of X-ray free-electron laser sources and ultrafast electron diffraction of relativistic electrons. While the dynamics of laser-induced molecular alignment has been extensively studied and demonstrated, molecular orientation is a much more challenging task, especially for asymmetric-top molecules. Here we report the first experimental demonstration of a field-free, all-optical three-dimensional orientation of asymmetric-top molecules by means of phase-locked cross-polarized two-color laser pulses. In addition to the conventional integrated orientation factor, we report the differential degree of orientation which is not amenable to optical measurements, but is readily accessible in our angle-resolved imaging technique. Our scheme applies to a wide class of asymmetric molecules and opens new ways towards controlling their orientation, eventually leading to direct imaging of structure of gas-phase molecules using advanced free electron laser beams with extremely high spatiotemporal resolution.

References in corpus (16)

• Laser-induced alignment and orientation of quantum-state-selected large molecules
• Molecular Orientation by Intense Single Cycle THz Pulses
• Discovery of the Interstellar Chiral Molecule Propylene Oxide (CH${}_3$CHCH${}_2$O)
• Manipulation of Molecules with Electromagnetic Fields
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
• Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
• Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion
• Oriented rotational wave-packet dynamics studies via high harmonic generation
• Efficient and long-lived field-free orientation of molecules by a single hybrid short pulse
• Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization
• Detecting chirality in molecules by linearly polarized laser fields
• Rotational control of asymmetric molecules: dipole- vs. polarizability- driven rotational dynamics
• Orientation of molecules via laser-induced anti-alignment
• Orienting Asymmetric Molecules by Laser Fields with Skewed Polarization
• Transition between mechanisms of laser-induced field-free molecular orientation

Cited by in corpus (17)

• Quantum control of molecular rotation
• Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules
• Molecular rotation movie filmed with high-harmonic generation
• Quantum Coherent Control of a Single Molecular-Polariton Rotation
• Observation of persistent orientation of chiral molecules by laser field with twisted polarization
• Optimal three-state field-free molecular orientation with terahertz pulses
• Orientational quantum revivals induced by a single-cycle terahertz pulse
• Long-lasting Molecular Orientation Induced by a Single Terahertz Pulse
• Molecular Frame Photoelectron Angular Distributions in Polyatomic Molecules from Lab Frame Coherent Rotational Wavepacket Evolution
• Laser-induced dynamics of molecules with strong nuclear quadrupole coupling
• Three Dimensional Orientation of Complex Molecules Excited by Two-Color Femtosecond Pulses
• Molecular Orientation-Induced Second Harmonic Generation: deciphering different contributions apart
• Echo-enhanced molecular orientation at high temperatures
• Controlling rotation in the molecular-frame with an optical centrifuge
• Long-Lasting Orientation of Symmetric-top Molecules Excited by Two-Color Femtosecond Pulses
• Visualizing coherent molecular rotation in a gaseous medium
• Ionization-induced Long-lasting Orientation of Symmetric-top Molecules