arXiv subjects

Ian MacPhail-Bartley

Publications and source records attributed to Ian MacPhail-Bartley.

6 recordsLinked to original sources

arXiv2026

Optical centrifuge as a probe of strong dissipative coupling between a molecular rotor and superfluid helium

A macroscopic manifestation of superfluidity is that objects moving through liquid helium experience negligible friction below the Landau critical velocity. How this frictionless motion breaks down at the nanoscale remains an open question. Molecules embedded in helium nanodroplets represent a well-controlled system for studying this breakdown, yet none has reached the regime of strong dissipative coupling, when energy transfer from the molecule to the superfluid dominates the observed dynamics. Molecular rotation, induced by short laser pulses, offer a suitable probe to reach rotational energies in the range of the roton gap, where superfluid helium supports a large number of elementary excitations. However, the solvation shell around a rotating molecule caps the energy reachable by a free rotor after impulsive excitation well below the roton excitation energy. Here we show that continuous driving with an ultraslow optical centrifuge overcomes this limitation: the strong field dresses the molecule into pendular states whose energies fall within the spectrum of the collective excitations of the superfluid, placing the system in the strong-dissipation regime. The resulting rapid thermalization locks the molecule to the rotating field until the rotation-induced level splittings overtake the thermalization rate, beyond which the molecular alignment is progressively lost. Our approach offers a direct measurement of the molecule-bath coupling in a quantum fluid.

quant-ph↗

arXiv2026

Ultraslow optical centrifuge with arbitrarily low rotational acceleration

We outline the design and characterization of a laser pulse shaper, which creates an ``ultraslow optical centrifuge'' - a linearly polarized field whose polarization vector rotates with arbitrarily low angular acceleration. By directly recording this rotation in time with nonlinear cross-correlation, we demonstrate the tunability of such centrifuge (both in terms of its initial and its final rotational frequencies) in the range of accelerations which are three orders of magnitude lower than those available with a conventional centrifuge design. We showcase the functionality of the ultraslow centrifuge by spinning CS$_2$ molecules in a molecular jet. Utilizing the extremely low angular acceleration to control molecular rotation inside viscous media is a promising application for this unique optical tool.

physics.chem-ph↗

arXiv2025

Control of molecular rotation in helium nanodroplets with an optical centrifuge

We experimentally demonstrate that the rotation of molecules embedded in helium nanodroplets can be controlled with an optical centrifuge, allowing for the study of molecular dynamics inside the strongly interacting many-body environment of superfluid helium at variable levels of rotational excitation. By doping the droplets with dimers of nitric oxide, (NO)$_2$, and measuring the degree of their centrifuge-induced alignment as a function of time, we show both the forced in-field rotation of molecules in a continuous range of frequencies, as well as the field-free resonant rotation with a long nanosecond-scale decay. The ability to control and monitor the rotational dynamics of molecular rotors inside the superfluid medium may shed new light on superfluidity and the interaction of superfluids with defects at the atomic level.

quant-ph↗

arXiv2023

Coherent control of molecular rotation in superfluid helium

We experimentally demonstrate control of molecular rotation in bulk superfluid $^4\mathrm{He}$. Metastable helium dimers, $\mathrm{He}_2^*$, are rotationally excited by a periodic train of linearly polarized femtosecond laser pulses. We show that the degree of rotational excitation of $\mathrm{He}_2^*$ can be enhanced or suppressed by varying the period of the pulse train, whereas the directionality of molecular rotation can be controlled by the relative angle between the polarization vectors of pulses in the train. The experimental results are in agreement with numerical calculations, based on a simple model, in which $\mathrm{He}_2^*$ molecules do not interact with the superfluid.

quant-ph↗

arXiv2020

Laser control of molecular rotation: Expanding the utility of an optical centrifuge

Since its invention in 1999, optical centrifuge has become a powerful tool for controlling molecular rotation and studying molecular dynamics and molecular properties at extreme levels of rotational excitation. The technique has been applied to a variety of molecular species, from simple linear molecules to symmetric and asymmetric tops, to molecular ions and chiral enantiomers. Properties of isolated ultrafast rotating molecules, so-called molecular superrotors, have been investigated, as well as their collisions with one another and interaction with external fields. The ability of an optical centrifuge to spin a particular molecule of interest depends on both the molecular structure and the parameters of the centrifuge laser pulse. An interplay between these two factors dictates the utility of an optical centrifuge in any specific application. Here, we discuss the strategy of assessing and adjusting the properties of the centrifuge to those of the molecular rotors, and describe two practical examples of optical centrifuges with very different characteristics, implemented experimentally in our laboratory.

physics.ins-det↗

arXiv2019

Controlled enantioselective orientation of chiral molecules with an optical centrifuge

We report on the first experimental demonstration of enantioselective rotational control of chiral molecules with a laser field. In our experiments, two enantiomers of propylene oxide are brought to accelerated unidirectional rotation by means of an optical centrifuge. Using Coulomb explosion imaging, we show that the centrifuged molecules acquire preferential orientation perpendicular to the plane of rotation, and that the direction of this orientation depends on the relative handedness of the enantiomer and the rotating centrifuge field. The observed effect is in agreement with theoretical predictions and is reproduced in numerical simulations of the centrifuge excitation followed by Coulomb explosion of the centrifuged molecules. The demonstrated technique opens new avenues in optical enantioselective control of chiral molecules with a plethora of potential applications in differentiation, separation and purification of chiral mixtures.

physics.chem-ph↗