arXiv subjects

A. A. Milner

Publications and source records attributed to A. A. Milner.

11 recordsLinked to original sources

arXiv2025

An optical centrifuge with zero rotational acceleration

An optical centrifuge is a laser pulse which enables controlled rotational excitation of molecules. Centrifuged molecules rotating with well-defined angular frequencies are ideal candidates to probe many-body quantum systems at the nanoscale. Because the interaction with the quantum environment increases the effective moment of inertia of the embedded molecular probes, the required rotational acceleration of the optical centrifuge must be lowered to accommodate adiabatic spinning. We demonstrate a new design of an optical centrifuge, based on the method of spectral focusing, which enables extremely low, down to zero, rotational accelerations. We discuss the potential of using such constant frequency centrifuge to investigate molecular rotation inside helium nanodroplets.

physics.chem-ph↗

arXiv2022

Ultrafast non-equilibrium dynamics of rotons in superfluid helium

Superfluid 4He, the first superfluid ever discovered, is in some ways the least well understood. Unlike 3He superfluid, or the variety of Bose-Einstein condensates of ultracold gases, superfluid 4He is a very dense liquid of strongly interacting quasiparticles. The theory is then necessarily phenomenological: the quasiparticle properties are found from experiment, and controversies over their description still remain, notably regarding vortex dynamics and the nature of rotons and roton pair creation. It is therefore important to develop new experimental tools for probing the system far from equilibrium. Here we describe a method for locally perturbing the density of superfluid helium through the excitation of roton pairs with ultrashort laser pulses. By measuring the time dependence of this perturbation, we track the non-equilibrium evolution of the two-roton states on a picosecond timescale. Our results reveal an ultrafast cooling of hot roton pairs as they thermalize with the colder gas of other quasiparticles. We anticipate that these findings, as well as future applications of the introduced ultrafast laser technique to different temperature and pressure regimes in bulk liquid 4He, will stimulate further experimental and theoretical investigations towards better understanding of superfluidity.

cond-mat.quant-gas↗

arXiv2021

State- and molecule-selective rotational control in gas mixtures with a shaped optical centrifuge

We demonstrate experimentally a method of all-optical selective rotational control in gas mixtures. Using an optical centrifuge - an intense laser pulse whose linear polarization rotates at an accelerated rate, we simultaneously excite two different molecular species to two different rotational frequencies of choice. The new level of control is achieved by shaping the centrifuge spectrum according to the rotational spectra of the centrifuged molecules. The shaped optical centrifuge releases one molecular species earlier than the other, therefore separating their target rotational frequencies and corresponding rotational states. The technique will expand the utility of rotational control in the studies of the effects of molecular rotation on collisions and chemical reactions.

physics.chem-ph↗

arXiv2017

Probing molecular potentials with an optical centrifuge

We use an optical centrifuge to excite coherent rotational wave packets in N$_2$O, CS$_2$ and OCS molecules with rotational quantum numbers reaching up to J=465, 690 and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high levels of rotational excitation can be used as a sensitive tool to probe the molecular potential energy surface at inter-nuclear distances far from their equilibrium values. Significant bond stretching in the centrifuged molecules results in the growing period of the rotational revivals, which are experimentally detected using coherent Raman scattering. We measure the revival period as a function of the centrifuge-induced rotational frequency and compare it with the numerical calculations based on the known Morse-cosine potentials.

physics.chem-ph↗

arXiv2016

Ultrafast magnetization of a dense molecular gas with an optical centrifuge

Strong laser-induced magnetization of oxygen gas at room temperature and atmospheric pressure is achieved experimentally on the sub-nanosecond time scale. The method is based on controlling the electronic spin of paramagnetic molecules by means of manipulating their rotation with an optical centrifuge. Spin-rotational coupling results in high degree of spin polarization on the order of one Bohr magneton per centrifuged molecule. Owing to the non-resonant interaction with the laser pulses, the demonstrated technique is applicable to a broad class of paramagnetic rotors. Executed in a high-density gas, it may offer an efficient way of generating macroscopic magnetic fields remotely (as shown in this work), producing large amount of polarized electrons and converting electronic to nuclear spin polarization.

quant-ph↗

arXiv2015

Field-free long-lived alignment of molecules in extreme rotational states

We introduce a new optical tool - a "two-dimensional optical centrifuge", capable of aligning molecules in extreme rotational states. Unlike the conventional centrifuge, which confines the molecules in the plane of their rotation, its two-dimensional version aligns the molecules along a well-defined axis, similarly to the effect of a single linearly polarized laser pulse, but at a much higher level of rotational excitation. The increased robustness of ultra-high rotational states with respect to collisions results in a longer life time of the created alignment in dense media, offering new possibilities for studying and utilizing aligned molecular ensembles under ambient conditions.

physics.chem-ph↗

arXiv2015

Magneto-optical properties of paramagnetic superrotors

We study the dynamics of paramagnetic molecular superrotors in an external magnetic field. Optical centrifuge is used to create dense ensembles of oxygen molecules in ultra-high rotational states. It is shown for the first time, that the gas of rotating molecules becomes optically birefringent in the presence of magnetic field. The discovered effect of "magneto-rotational birefringence" indicates preferential alignment of molecular axes along the field direction. We provide an intuitive qualitative model, in which the influence of the applied magnetic field on the molecular orientation is mediated by the spin-rotation coupling. This model is supported by the direct imaging of the distribution of molecular axes, the demonstration of the magnetic reversal of the rotational Raman signal, and by numerical calculations.

quant-ph↗

arXiv2015

From gyroscopic to thermal motion: a crossover in the dynamics of molecular superrotors

Localized heating of a gas by intense laser pulses leads to interesting acoustic, hydrodynamic and optical effects with numerous applications in science and technology, including controlled wave guiding and remote atmosphere sensing. Rotational excitation of molecules can serve as the energy source for raising the gas temperature. Here, we study the dynamics of energy transfer from the molecular rotation to heat. By optically imaging a cloud of molecular superrotors, created with an optical centrifuge, we experimentally identify two separate and qualitatively different stages of its evolution. The first non-equilibrium "gyroscopic" stage is characterized by the modified optical properties of the centrifuged gas - its refractive index and optical birefringence, owing to the ultrafast directional molecular rotation, which survives tens of collisions. The loss of rotational directionality is found to overlap with the release of rotational energy to heat, which triggers the second stage of thermal expansion. The crossover between anisotropic rotational and isotropic thermal regimes is in agreement with recent theoretical predictions and our hydrodynamic calculations.

physics.optics↗

arXiv2015

Sound emission from the gas of molecular superrotors

We use an optical centrifuge to deposit a controllable amount of rotational energy into dense molecular ensembles. Subsequent rotation-translation energy transfer, mediated by thermal collisions, results in the localized heating of the gas and generates strong sound wave, clearly audible to the unaided ear. For the first time, the amplitude of the sound signal is analyzed as a function of the experimentally measured rotational energy. The proportionality between the two experimental observables confirms that rotational excitation is the main source of the detected sound wave. As virtually all molecules, including the main constituents of the atmosphere, are amenable to laser spinning by the centrifuge, we anticipate this work to stimulate further development in the area of photo-acoustic control and spectroscopy.

physics.chem-ph↗

arXiv2012

Directional spinning of molecules with sequences of femtosecond pulses

We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a "double kick" scheme) or a longer pulse sequence (a "chiral pulse train" scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum state selectivity, i.e. predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counter-rotation of molecular nuclear spin isomers (here, ortho- and para-nitrogen) and molecular isotopologues (here, 14N_2 and 15N_2).

physics.optics↗

arXiv2011

Control of molecular rotation with a chiral train of ultrashort pulses

Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train - a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.

quant-ph↗