We generalize the concepts of alignment and 3D alignment by moderately intense laser pulses to control both the overall rotations and the torsional motions of polyatomic molecules. Torsional control is applied to manipulate charge transfer events, hence introducing a potential route to light controlled molecular switches. Potential applications in areas such as molecular assembly, molecular spe...

Laser-induced electron diffraction is an evolving tabletop method that aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolutions. Here we demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes t...

We report a comprehensive study of the quantum-state correlation property of product pairs from reactions of chlorine atoms with both the ground-state and the CH stretch-excited CHD(3). In light of available ab initio theoretical results, this set of experimental data provides a conceptual framework to visualize the energy-flow pattern along the reaction path, to classify the activity of differ...

We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed ( )  = P N 1 branch of the vibronic transition ̃ ( ) ̃ ( ) S « P + X A 000 000 2 2 1 2 . A single repumping laser excites the Sr–O stretching vibrational mode, ...

We demonstrate a method for determining the full three-dimensional molecular-frame photoelectron angular distribution in polyatomic molecules using methane as a prototype. Simultaneous double Auger decay and subsequent dissociation allow measurement of the initial momentum vectors of the ionic fragments and the photoelectron in coincidence, allowing full orientation by observing a three-ion dec...

We present a rigorous theoretical study of low-temperature collisions of polyatomic molecular radicals with (1)S(0) atoms in the presence of an external magnetic field. Accurate quantum scattering calculations based on ab initio and scaled interaction potentials show that collision-induced spin relaxation of the prototypical organic molecule CH(2)(X(3)B(1)) (methylene) and nine other triatomic ...

Controlled step-by-step dissociation of single iodobenzene molecules has been performed at Cu(111) step-edges using tunneling electrons from a scanning tunneling microscope (STM) tip at 12 K. We show that the threshold tunneling electron energies to break a single bond inside a polyatomic molecule can be determined by using I-V spectroscopy of single molecules. Electron energies of 1.5±0.1 eV a...

Recent advances in high sensitivity spectroscopy have made it possible, combination with accurate theoretical predictions, to observe, for the first time, very weak electric quadrupole transitions a polar polyatomic molecule of water. Here, we present predictions complete rovibrational spectrum non-polar CO2, important atmospheric and astrophysical applications. Our are validated by recent cavi...

Although important to heterogeneous catalysis, the ability to accurately model reactions of polyatomic molecules with metal surfaces has not kept pace with developments in gas phase dynamics. Partnering the specific reaction parameter (SRP) approach to density functional theory with ab initio molecular dynamics (AIMD) extends our ability to model reactions with metals with quantitative accuracy...