Molecular movie of ultrafast coherent rotational dynamics

Abstract

Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. We present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single-quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, $⟨{\cos }^2{\theta }_{2D}⟩=0.96$ ($⟨{\cos }^2\theta ⟩=0.94$) was achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalised the observed very high degree of alignment.

9 Figures

References in corpus (14)

• Photoelectron angular distributions from strong-field ionization of oriented molecules
• X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
• Imaging an aligned polyatomic molecule with laser-induced electron diffraction
• Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
• Diffractive imaging of a molecular rotational wavepacket with femtosecond Megaelectronvolt electron pulses
• Spatially-controlled complex molecules and their applications
• State- and conformer-selected beams of aligned and oriented molecules for ultrafast diffraction studies
• Stark-selected beam of ground-state OCS molecules characterized by revivals of impulsive alignment
• Bootstrapping to the Molecular Frame with Time-domain Photoionization Interferometry
• Two-state wave packet for strong field-free molecular orientation
• Ultimate field-free molecular alignment by combined adiabatic-impulsive field design
• Strongly driven quantum pendulum of the OCS molecule
• Quantum state tomography of molecular rotation
• Climbing the rotational ladder to chirality

Cited by in corpus (24)

• Electronic State Population Dynamics upon Ultrafast Strong Field Ionization and Fragmentation of Molecular Nitrogen
• Observation of persistent orientation of chiral molecules by laser field with twisted polarization
• Ultrafast molecular orbital tomography of a pentacene thin film using time-resolved momentum microscopy at a free-electron laser
• Atomic-resolution imaging of carbonyl sulfide by laser-induced electron diffraction
• In-situ Imaging of a Single-Atom Wave Packet in Continuous Space
• Optical imaging of coherent molecular rotors
• Bayesian optimization for inverse problems in time-dependent quantum dynamics
• Resolving Multiphoton Processes with High-Order Anisotropy Ultrafast X-ray Scattering
• Laser-induced dynamics of molecules with strong nuclear quadrupole coupling
• Quantum interference and imaging using intense laser fields
• Rotation of polarization of light propagating through a gas of molecular super-rotors
• The effect of nuclear-quadrupole coupling in the laser induced alignment of molecules
• Topological charges of periodically kicked molecules
• CMInject: Python framework for the numerical simulation of nanoparticle injection pipelines
• Controlling rotation in the molecular-frame with an optical centrifuge
• Time-resolving the UV-initiated photodissociation dynamics of OCS
• Simultaneous imaging of vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule
• Laser-induced alignment of nanoparticles and macromolecules for single-particle-imaging applications
• A machine learning model to classify dynamic processes in liquid water
• Laser control of an excited-state vibrational wave packet in neutral H${}_2$
• Visualizing coherent molecular rotation in a gaseous medium
• A novel crossed-molecular-beam experiment for investigating reactions of state- and conformationally selected strong-field-seeking molecules
• Gradient-based reconstruction of molecular Hamiltonians and density matrices from time-dependent quantum observables
• Optimal control for manipulating vibrational wave packets through polarizability interactions induced by non-resonant laser pulses