Rotation of molecules embedded in He nanodroplets is explored by a combination of fs laserinduced 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 He shell. Our results open novel opportunities for studying non-equilibrium solute-solvent dynamics and quantum thermalization.

We present a new high-resolution global renewable energy atlas (REatlas) that can be used to calculate customised hourly time series of wind and solar PV power generation. In this paper, the atlas is applied to produce 32-year-long hourly model wind power time series for Denmark for each historical and future year between 1980 and 2035. These are calibrated and validated against real production data from the period 2000 to 2010. The high number of years allows us to discuss how the characteristics of Danish wind power generation varies between individual weather years. As an example, the annual energy production is found to vary by ±10% from the average. Furthermore, we show how the production pattern change as small onshore turbines are gradually replaced by large onshore and offshore turbines. Finally, we compare our wind power time series for 2020 to corresponding data from a handful of Danish energy system models. The aim is to illustrate how current differences in model wind may result in significant differences in technical and economical model predictions. These include up to 15% differences in installed capacity and 40% differences in system reserve requirements.

Iodine (I 2 ) 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 cos 2 θ2D , is measured as a function of the laser intensity. The results are well described by cos 2 θ2D 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 more complex system by measurements on 1,4-diiodobenzene and 1,4-dibromobenzene. For all three molecular species studied the highest values of cos 2 θ2D achieved in He droplets exceed 0.96.

A moderately intense 450 fs laser pulse is used to create rotational wave packets in gas phase I_{2} molecules. The ensuing time-dependent alignment, measured by Coulomb explosion imaging with a delayed probe pulse, exhibits the characteristic revival structures expected for rotational wave packets but also a complex nonperiodic substructure and decreasing mean alignment not observed before. A quantum mechanical model attributes the phenomena to coupling between the rotational angular momenta and the nuclear spins through the electric quadrupole interaction. The calculated alignment trace agrees very well with the experimental results.

The nonadiabatic alignment dynamics of weakly bound molecule-atom complexes, induced by a moderately intense 300 fs nonresonant laser pulse, is calculated by direct numerical solution of the time-dependent Schrödinger equation. Our method propagates the wave function according to the coupled channel equations for the complex, which can be done in a very efficient and stable manner out to large times. We present results for two van der Waal complexes, CS-He and HCCH-He, as respective examples of linear molecules with large and small moments of inertia. Our main result is that at intensities typical of nonadiabatic alignment experiments, these complexes rapidly dissociate. In the case of the CS-He complex, the ensuing rotational dynamics resembles that of isolated molecules, whereas for the HCCH-He complex, the detachment of the He atom severely perturbs and essentially quenches the subsequent rotational motion. At intensities of the laser pulse ≲2.0 × 10 W/cm, it is shown that the molecule-He complex can rotate and align without breaking apart. We discuss the implications of our findings for recent experiments on iodine molecules solvated in helium nanodroplets.

We present an efficient, noise-robust method based on Fourier analysis for reconstructing the three-dimensional measure of the alignment degree, ⟨cosθ⟩, directly from its two-dimensional counterpart, ⟨cosθ⟩. The method applies to nonadiabatic alignment of linear molecules induced by a linearly polarized, nonresonant laser pulse. Our theoretical analysis shows that the Fourier transform of the time-dependent ⟨cosθ⟩ trace over one molecular rotational period contains additional frequency components compared to the Fourier transform of ⟨cosθ⟩. These additional frequency components can be identified and removed from the Fourier spectrum of ⟨cosθ⟩. By rescaling of the remaining frequency components, the Fourier spectrum of ⟨cosθ⟩ is obtained and, finally, ⟨cosθ⟩ is reconstructed through inverse Fourier transformation. The method allows the reconstruction of the ⟨cosθ⟩ trace from a measured ⟨cosθ⟩ trace, which is the typical observable of many experiments, and thereby provides direct comparison to calculated ⟨cosθ⟩ traces, which is the commonly used alignment metric in theoretical descriptions. We illustrate our method by applying it to the measurement of nonadiabatic alignment of I molecules. In addition, we present an efficient algorithm for calculating the matrix elements of cosθ and any other observable in the symmetric top basis. These matrix elements are required in the rescaling step, and they allow for highly efficient numerical calculation of ⟨cosθ⟩ and ⟨cosθ⟩ in general.

Moderately intense, nonresonant laser pulses can be used to accurately control how gas phase molecules are oriented in space. This topic, driven by intense experimental and theoretical efforts, has been ever growing and developed for more than 20 years, and laser-induced alignment methods are used routinely in a number of applications in physics and chemistry. Starting in 2013, we have demonstrated that laser-induced alignment also applies to molecules dissolved in helium nanodroplets. Here we present an overview of this new work discussing alignment in both the nonadiabatic (short-pulse) and adiabatic (long-pulse) limit. We show how femtosecond or picosecond pulses can set molecules into coherent rotation that lasts for a long time and reflects the rotational structure of the helium-solvated molecules, provided the pulses are weak or, conversely, results in desolvation of the molecules when the pulses are strong. For long pulses we show that the 0.4 K temperature of the droplets, shared with the molecules or molecular complexes, leads to exceptionally high degrees of alignment. Upon rapid truncation of the laser pulse, the strong alignment can be made effectively field-free, lasting for about 10 ps thanks to slowing of molecular rotation by the helium environment. Finally, we discuss how the combination of strongly aligned molecular dimers and laser-induced Coulomb explosion imaging enables determination of the structure of the dimers. As a background and reference point, the first third of the article introduces some of the central concepts of laser-induced alignment for isolated molecules, illustrated by numerical and experimental examples.

No abstract