arXiv subjects

Manuel Barranco

Publications and source records attributed to Manuel Barranco.

At least 19 recordsLinked to original sources

arXiv2025

Tracking Microhydration of the NaCl Rocksalt Molecule in Helium Nanodroplets by Penning Ionization Electron Spectroscopy

The microhydration of rock salt (NaCl) molecules was investigated using high-resolution Penning ionization electron spectroscopy (PIES) in helium nanodroplets. Although model calculations predict that NaCl molecules are fully submerged inside the droplets, PIES of NaCl are highly resolved, in stark contrast to other molecular species. Co-doping the droplets with a controlled number of $n=5$--10 water molecules leads to efficient quenching of the NaCl Penning ionization signal and to its full suppression for $n\gtrsim 30$. Accompanying density-functional theory (DFT) and force field calculations reveal a transition from contact ion pair structures to solvent-separated ion pairs at $n=12$--15. However, it takes $n\approx 17$ water molecules to form a complete solvation shell around the Cl$^-$ anion and as many as $n\approx 34$ to fully hydrate the Na$^+$ cation, thus the entire NaCl molecule, which rationalizes the experimental findings.

physics.chem-ph↗

arXiv2025

Time-resolved solvation of alkali ions in superfluid helium nanodroplets: Theoretical simulation of a pump-probe study

The solvation process of an alkali ion (Na$^+$, K$^+$, Rb$^+$, Cs$^+$) inside a superfluid $^4$He$_{2000}$ nanodroplet is investigated theoretically using liquid $^4$He time-dependent density functional theory at zero temperature. We simulate both steps of the pump-probe experiment conducted on Na$^+$ [Albrechtsen et al., Nature 623, 319 (2023)], where the alkali atom residing at the droplet surface is ionized by the pump pulse and its solvation is probed by ionizing a central xenon atom and detecting the expulsed Na$^+$He$_n$ ions. Our results confirm the Poissonian model for the binding of the first five He atoms for the lighter Na$^+$ and K$^+$ alkalis, with a rate in good agreement with the more recent experimental results on Na$^+$ [Albrechtsen et al., J. Chem. Phys. 162, 174309 (2025)]. For the probe step we show that the ion takes several picoseconds to get out of the droplet. During this rather long time, the solvation structure around it is very hot and far from equilibrium, and it can gain or lose more He atoms. Surprisingly, analysing the Na$^+$ solvation structure energy reveals that it is not stable by itself during the first few picoseconds of the solvation process. After that, energy relaxation follows a Newton behavior, as found experimentally, but with a longer time delay, $5.0\leq t_0\leq 6.5$ ps vs. $0.23\pm0.06$ ps, and characteristic decay time, $7.3\le\tau\le 16.5$ ps vs. $2.6\pm 0.4$ ps. We conclude that the first instants of the solvation process are highly turbulent and that the solvation structure is stabilized only by the surrounding helium ``solvent''.

physics.atm-clus↗

arXiv2024

Revisiting Thomson's model with multiply charged superfluid helium nanodroplets

We study superfluid helium droplets multiply charged with ions. When stable, the charges are found to reside in equilibrium close to the droplet surface, thus representing a physical realization of Thomson's model. We find the minimum radius of the helium droplet that can host a given number of ions using a model whose physical ingredients are the solvation energy of the cations, calculated within the He-DFT approach, and their mutual Coulomb repulsion energy. Our model goes beyond the often used liquid drop model, where charges are smeared out either within the droplet or on its surface, and which neglects the solid-like helium shell around the ions. We find that below a threshold droplet radius R_0, the total energy of the system becomes higher than that of the separated system of the pristine helium droplet and the charges embedded in their solvation microcluster ("snowball"). However, the ions are still kept within the droplet by the presence of energy barriers which hinder Coulomb explosion. A further reduction of the droplet radius below a value R_expl eventually results in the disappearance of such barrier, leading to Coulomb explosion. Surprisingly, our results are rather insensitive to the ion atomic species. This makes room to discuss them in the context of intrinsic multicharged helium droplets, where the charges are triatomic He3+ ions. Our calculated values for R_expl display the correct scaling with the number of cations compared to available experimental results, at variance with other estimates for the critical radii.

cond-mat.mes-hall↗

arXiv2023

Quantized vortex nucleation in collisions of superfluid nanoscopic helium droplets at zero temperature

We address the collision of two superfluid 4 He droplets at non-zero initial relative velocities and impact parameters within the framework of liquid 4 He time-dependent density functional theory at zero temperature. In spite of the small size of these droplets (1000 He atoms in the merged droplet) imposed by computational limitations, we have found that quantized vortices may be readily nucleated for reasonable collision parameters. At variance with head-on collisions, where only vortex rings are produced, collisions with non-zero impact parameter produce linear vortices which are nucleated at indentations appearing on the surface of the deformed merged droplet. Whereas for equal-size droplets vortices are produced in pairs, an odd number of vortices can appear when the colliding droplet sizes are different. In all cases vortices coexist with surface capillary waves. The possibility for collisions to be at the origin of vortex nucleation in experiments involving very large droplets is discussed. An additional surprising result is the observation of the drops coalescence even for grazing and distal collisions at relative velocities as high as 80 m/s and 40 m/s, respectively, induced by the long-range Van der Waals attraction between the droplets.

physics.atm-clus↗

arXiv2023

Breakup of quantum liquid filaments into droplets

We have investigated how the Rayleigh-Plateau instability of a filament made of a 41K-87Rb self-bound mixture may lead to an array of identical quantum droplets, with typical breaking times which are shorter than the lifetime of the mixture. If the filament is laterally confined -- as it happens in a toroidal trap -- and atoms of one species are in excess with respect to the optimal, equilibrium ratio, the droplets are immersed into a superfluid background made by the excess species which provides global phase coherence to the system, suggesting that the droplets array in the unbalanced system may display supersolid character. This possibility has been investigated by computing the non-classical translational inertia coefficient. The filament may be a reasonable representation of a self-bound mixture subject to toroidal confinement when the bigger circle radius of the torus is much larger than the filament radius.

cond-mat.quant-gas↗

arXiv2023

Nanoscopic jets and filaments of superfluid He-4 at zero temperature: a DFT study

Helium droplets produced by the instability of a cryogenic helium jet exiting a source chamber leads to the formation of He drops which are considered as ideal matrices for spectroscopic studies of embedded atoms and molecules. Here, we present a He-DFT description of droplet formation resulting from jet breaking and contraction of superfluid He-4 filaments. Whereas the fragmentation of long jets closely follows the predictions of linear theory for inviscid fluids, leading to droplet trains interspersed with smaller satellite droplets, the contraction of filaments with an aspect ratio larger than a threshold value leads to the nucleation of vortex rings which hinder their breakup into droplets.

cond-mat.mes-hall↗

arXiv2023

Self-sustained deformable rotating liquid He cylinders: The pure normal fluid $^3$He and superfluid $^4$He cases

We have studied self-sustained, deformable, rotating liquid He cylinders of infinite length. In the normal fluid $^3$He case, we have employed a classical model where only surface tension and centrifugal forces are taken into account, as well as the Density Functional Theory (DFT) approach in conjunction with a semi-classical Thomas-Fermi approximation for the kinetic energy. In both approaches, if the angular velocity is sufficiently large, it is energetically favorable for the $^3$He cylinder to undergo a shape transition, acquiring an elliptic-like cross section which eventually becomes two-lobed. In the $^4$He case, we have employed a DFT approach that takes into account its superfluid character, limiting the description to vortex-free configurations where angular momentum is exclusively stored in capillary waves on a deformed cross section cylinder. The calculations allow us to carry out a comparison between the rotational behavior of a normal, rotational fluid ($^3$He) and a superfluid, irrotational fluid ($^4$He).

cond-mat.mes-hall↗

arXiv2021

Dynamics of photo-excited Cs atoms attached to helium nanodroplets

We present an experimental study of the dynamics following the photo-excitation and subsequent photo-ionization of single Cs atoms on the surface of helium nanodroplets. The dynamics of excited-Cs-atom desorption and re-adsorption as well as CsHe exciplex formation are measured using femtosecond pump-probe velocity-map-imaging spectroscopy and ion-time-of-flight spectrometry. The timescales for the desorption of excited Cs atoms off helium nanodroplets as well as the timescales for CsHe exciplex formation are experimentally determined for the 6p states of Cs. For the 6p $^2Π_ {1/2}$ state, our results confirm that the excited Cs atoms only desorb from the nanodroplet when the excitation wavenumber is blue-shifted from the $6p\,^2Π_ {1/2} \leftarrow 6s\,^2Σ_ {1/2}$ resonance. Our results suggest that the dynamics following excitation to the 6p $^2Π_ {3/2}$ state can be described by an evaporation-like desorption mechanism, whereas the dynamics arising from excitation to the 6p $^2Σ_ {1/2}$ state is indicative for a more impulsive desorption process. Furthermore, our results suggest a helium-induced spin-orbit relaxation from the the 6p $^2Σ_ {1/2}$ state to the 6p $^2Π_ {1/2}$ state. Our findings largely agree with the results of time-dependent $^4$He-density-functional theory (DFT) simulations published earlier [Coppens et al., Eur. Phys. J. D 73, 94 (2019)].

physics.atm-clus↗

arXiv2021

Vortices in the supersolid phase of dipolar Bose-Einstein condensates

Vortices are expected to exist in a supersolid but experimentally their detection can be difficult because the vortex cores are localized at positions where the local density is very low. We address here this problem by performing numerical simulations of a dipolar Bose-Einstein Condensate (BEC) in a pancake confinement at $T=0$ K and study the effect of quantized vorticity on the phases that can be realized depending upon the ratio between dipolar and short-range interaction. By increasing this ratio the system undergoes a spontaneous density modulation in the form of an ordered arrangement of multi-atom "droplets". This modulated phase can be either a "supersolid" (SS) or a "normal solid" (NS). In the SS state droplets are immersed in a background of low-density superfluid and the system has a finite global superfluid fraction resulting in non-classical rotational inertia. In the NS state no such superfluid background is present and the global superfluid fraction vanishes. We propose here a protocol to create vortices in modulated phases of dipolar BEC by "freezing" into such phases a vortex-hosting superfluid (SF) state. The resulting system, depending upon the interactions strengths, can be either a SS or a NS To discriminate between these two possible outcome of a "freezing" experiment, we show that upon releasing of the radial harmonic confinement, the expanding vortex-hosting SS shows tell-tale quantum interference effects which display the symmetry of the vortex lattice of the originating SF, as opposed to the behavior of the NS which shows instead a ballistic radial expansion of the individual droplets. Such markedly different behavior might be used to prove the supersolid character of rotating dipolar condensates.

cond-mat.quant-gas↗

arXiv2021

Dynamics of equilibration and collisions in ultradilute quantum droplets

Employing time-dependent density-functional theory, we have studied dynamical equilibration and binary head-on collisions of quantum droplets made of a $^{39}$K-$^{39}$K Bose mixture. The phase space of collision outcomes is extensively explored by performing fully three-dimensional calculations with effective single-component QMC based and two-components LHY-corrected mean-field functionals. We exhaustively explored the important effect -- not considered in previous studies -- of the initial population ratio deviating from the optimal mean-field value $N_2/N_1 = \sqrt{a_{11} / a_{22}}$. Both stationary and dynamical calculations with an initial non-optimal concentration ratio display good agreement with experiments. Calculations including three-body losses acting only on the $\left|F, m_{F}\right\rangle=|1,0\rangle$ state show dramatic differences with those obtained with the three-body term acting on the total density.

cond-mat.quant-gas↗

arXiv2021

Vortex properties in the extended supersolid phase of dipolar Bose-Einstein condensates

We study the properties of singly-quantized linear vortices in the supersolid phase of a dipolar Bose-Einstein condensate at zero temperature modeling $^{164}$Dy atoms. The system is extended in the $x-y$ plane and confined by a harmonic trap in the the polarization direction $z$. Our study is based on a generalized Gross-Pitaevskii equation. We characterize the ground state of the system in terms of spatial order and superfluid fraction and compare the properties of a single vortex and of a vortex dipole in the superfluid phase (SFP) and in the supersolid phase (SSP). At variance with a vortex in the SFP, which is free to move in the superfluid, a vortex in the SSP is localized at the interstitial sites and does not move freely. We have computed the energy barrier for motion from an equilibrium site to another. The fact that the vortex is submitted to a periodic potential has a dramatic effect on the dynamics of a vortex dipole made of two counter rotating parallel vortices; instead of rigidly translating as in the SFP, the vortex and anti-vortex approach each other by a series of jumps from one site to another until they annihilate in a very short time and their energy is transferred to bulk excitations.

cond-mat.quant-gas↗

arXiv2021

Unravelling the Full Relaxation Dynamics of Superexcited Helium Nanodroplets

The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: Droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product of both droplet autoionization and photoionization is He$_2^+$, whereas the delayed appearance of He$^+$ is indicative of the ejection of excited He atoms from the droplets. The state-resolved time-dependent photoelectron spectra reveal that intermediate excited states of the droplets are populated in the course of the relaxation, terminating in the lowest-lying metastable singlet and triplet He atomic states. The slightly faster relaxation of the triplet state compared to the singlet state is in agreement with the simulation showing faster formation of a bubble around a He atom in the triplet state.

physics.atm-clus↗

arXiv2020

Rotating mixed $^3$He-$^4$He nanodroplets

Mixed $^3$He-$^4$He droplets created by hydrodynamic instability of a cryogenic fluid-jet may acquire angular momentum during their passage through the nozzle of the experimental apparatus. These free-standing droplets cool down to very low temperatures undergoing isotopic segregation, developing a nearly pure $^3$He crust surrounding a very $^4$He-rich superfluid core. Here, the stability and appearance of rotating mixed helium droplets are investigated using Density Functional Theory for an isotopic composition that highlights, with some marked exceptions related to the existence of the superfluid inner core, the analogies with viscous rotating droplets.

cond-mat.quant-gas↗

arXiv2019

Rotating He-3 droplets

Motivated by recent experiments, we study normal-phase rotating He-3 droplets within Density Functional Theory in a semi-classical approach. The sequence of rotating droplet shapes as a function of angular momentum are found to agree with those of rotating classical droplets, evolving from axisymmetric oblate to triaxial prolate to two-lobed shapes as the angular momentum of the droplet increases. Our results, which are obtained for droplets of nanoscopic size, are rescaled to the mesoscopic size characterizing ongoing experimental measurements, allowing for a direct comparison of shapes. The stability curve in the angular velocity-angular momentum plane shows small deviations from the classical rotating drop model predictions, whose magnitude increases with angular momentum. We attribute these deviations to effects not included in the simplified classical model description of a rotating fluid held together by surface tension, i.e. to surface diffuseness, curvature and finite compressibility, and to quantum effects associated with deformation of the He-3 Fermi surface. The influence of all these effects is expected to diminish as the droplet size increases, making the classical rotating droplet model a quite accurate representation of He-3 rotation.

cond-mat.other↗

arXiv2019

Angular momentum in rotating superfluid droplets

The angular momentum of rotating superfluid droplets originates from quantized vortices and capillary waves, the interplay between which remains to be uncovered. Here, the rotation of isolated sub-micrometer superfluid 4He droplets is studied by ultrafast x-ray diffraction using a free electron laser. The diffraction patterns provide simultaneous access to the morphology of the droplets and the vortex arrays they host. In capsule-shaped droplets, vortices form a distorted triangular lattice, whereas they arrange along elliptical contours in ellipsoidal droplets. The combined action of vortices and capillary waves results in droplet shapes close to those of classical droplets rotating with the same angular velocity. The findings are corroborated by density functional theory calculations describing the velocity fields and shape deformations of a rotating superfluid cylinder.

cond-mat.other↗

arXiv2019

Vorticity and quantum turbulence in the merging of superfluid Helium nanodroplets

We have studied the merging of two $^4$He droplets at zero temperature, caused by their Van der Waals mutual attraction. During the early stages of the merging, density structures appear which closely match the experimental observations by Vicente et al. [J. Low Temp. Phys. 121, 627 (2000)]. When the droplets are merging, quantized vortex-antivortex ring pairs nucleate at the surface and annihilate inside the merged droplet producing a roton burst. We also observe the nucleation of quantized vortex-antivortex rings that wrap the droplet surface and remain localized on the surface until they eventually decay into short-wavelength surface waves. Analysis of the kinetic energy spectrum discloses the existence of a regime where turbulence caused by vortex interaction and annihilation is characterized by a Kolmogorov power law. This is followed by another regime where roton radiation (produced by vortex-antivortex annihilation) dominates, whose hallmark is a weak, turbulent surface dynamics. We suggest that similar processes might appear in superfluid helium droplets after they capture impurities or if they are produced by hydrodynamic instability of a liquid jet. Experiments on collisions between recently-discovered self-bound Bose-Einstein condensates should display a similar phenomenology.

cond-mat.mes-hall↗

arXiv2018

Self-bound ultra dilute Bose mixtures within Local Density Approximation

We have investigated self-bound binary ultra dilute bosonic mixtures at zero temperature within Density Functional Theory using a Local Density Approximation. We provide the explicit expression of the Lee-Huang-Yang correction in the general case of heteronuclear mixtures, and investigate the general thermodynamic conditions which lead to the formation of self-bound systems. We have determined the conditions for stability against the evaporation of one component, as well as the mechanical and diffusive spinodal lines. We have also calculated the surface tension of the self-bound state as a function of the inter-species interaction strength. We find that relatively modest changes of the latter result in order-of-magnitude changes in the calculated surface tension. We suggest experimental realizations which might display the metastability and phase separation of the mixture when entering regions of the phase diagram characterized by negative pressures. Finally, we show that these droplets may sustain stable vortex and vortex dimers.

cond-mat.quant-gas↗

arXiv2018

Spinning superfluid helium-4 nanodroplets

We have studied spinning superfluid $^4$He nanodroplets at zero temperature using Density Functional theory. Due to the irrotational character of the superfluid flow, the shapes of the spinning nanodroplets are very different from those of a viscous normal fluid drop in steady rotation. We show that when vortices are nucleated inside the superfluid droplets, their morphology, which evolves from axisymmetric oblate to triaxial prolate to two-lobed shapes, is in good agreement with experiments. The presence of vortex arrays confers to the superfluid droplets the rigid-body behavior of a normal fluid in steady rotation, and this is the ultimate reason of the surprising good agreement between recent experiments and the classical models used for their description.

cond-mat.mes-hall↗