Lars Christiansen

Laser-Induced Rotation of Iodine Molecules in Helium Nanodroplets: Revivals and Breaking Free

Rotation of molecules embedded in helium nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear-instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its helium shell. Our results open novel opportunities for studying nonequilibrium solute-solvent dynamics and quantum thermalization.

Strongly aligned molecules inside helium droplets in the near-adiabatic regime

Iodine (I2) molecules embedded in He nanodroplets are aligned by a 160 ps long laser pulse. The highest degree of alignment, occurring at the peak of the pulse and quantified by ⟨cos2𝜃2D⟩, is measured as a function of the laser intensity. The results are well described by ⟨cos2𝜃2D⟩ calculated for a gas of isolated molecules each with an effective rotational constant of 0.6 times the gas-phase value and at a temperature of 0.4 K. Theoretical analysis using the angulon quasiparticle to describe rotating molecules in superfluid helium rationalizes why the alignment mechanism is similar to that of isolated molecules with an effective rotational constant. A major advantage of molecules in He droplets is that their 0.4 K temperature leads to stronger alignment than what can generally be achieved for gas phase molecules-here demonstrated by a direct comparison of the droplet results to measurements on a ∼1 K supersonic beam of isolated molecules. This point is further illustrated for a more complex system by measurements on 1,4-diiodobenzene and 1,4-dibromobenzene. For all three molecular species studied, the highest values of ⟨cos2𝜃2D⟩ achieved in He droplets exceed 0.96.

Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules

The gas-phase structures of four difluoroiodobenzene and two dihydroxybromobenzene isomers were identified by correlating the emission angles of atomic fragment ions created, following femtosecond laser-induced Coulomb explosion. The structural determinations were facilitated by confining the most polarizable axis of each molecule to the detection plane prior to the Coulomb explosion event using one-dimensional laser-induced adiabatic alignment. For a molecular target consisting of two difluoroiodobenzene isomers, each constituent structure could additionally be singled out and distinguished.

Communication: Switched wave packets with spectrally truncated chirped pulses

A new technique for obtaining switched wave packets using spectrally truncated chirped laser pulses is demonstrated experimentally and numerically by one-dimensional alignment of both linear and asymmetric top molecules. Using a simple long-pass transmission filter, a pulse with a slow turn-on and a rapid turn-off is produced. The degree of alignment, characterized by ⟨cos2 θ2D⟩, rises along with the pulse intensity and reaches a maximum at the peak of the pulse. After truncation, ⟨cos2 θ2D⟩ drops sharply but exhibits pronounced half and full revivals. The experimental alignment dynamics trace agrees very well with a numerically calculated trace based on the solution of the time-dependent Schrödinger equation. However, the extended periods of field-free alignment of asymmetric tops following pulse truncation reported previously are not reproduced in our work.

Velocity map imaging with non-uniform detection: Quantitative molecular axis alignment measurements via Coulomb explosion imaging

We present a method for inverting charged particle velocity map images which incorporates a non-uniform detection function. This method is applied to the specific case of extracting molecular axis alignment from Coulomb explosion imaging probes in which the probe itself has a dependence on molecular orientation which often removes cylindrical symmetry from the experiment and prevents the use of standard inversion techniques for the recovery of the molecular axis distribution. By incorporating the known detection function, it is possible to remove the angular bias of the Coulomb explosion probe process and invert the image to allow quantitative measurement of the degree of molecular axis alignment.

Femtosecond laser induced Coulomb explosion imaging of aligned OCS oligomers inside helium nanodroplets

Dimers and trimers of carbonyl sulfide (OCS) molecules embedded in helium nanodroplets are aligned by a linearly polarized 160 ps long moderately intense laser pulse and Coulomb exploded with an intense 40 fs long probe pulse in order to determine their structures. For the dimer, recording of 2D images of OCS+ and S+ ions and covariance analysis of the emission directions of the ions allow us to conclude that the structure is a slipped-parallel shape similar to the structure found for gas phase dimers. For the trimer, the OCS+ ion images and the corresponding covariance maps reveal the presence of a barrel-shaped structure (as in the gas phase) but also other structures not present in the gas phase, most notably a linear chain structure.