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Physics Physics Atomic and Molecular Clusters

physics.atm-clus Watch Atomic and Molecular Clusters

Thursday 8 October

Atomic and Molecular Clusters

Multiple photoelectron inelastic scattering in large He nanodroplets

Niklas Scheel, Narcis Silviu Blaj, Rajni Rajni et al. (+7 more)

Helium nanodroplets are ideal testbeds for elucidating secondary processes induced by ionizing radiation in condensed matter. Here we study photoionization electron spectra of large He nanodroplets in the extreme ultraviolet region, where photoelectrons undergo multiple inelastic collisions with He atoms in the nanodroplets. The resulting characteristic electron energy-loss features are identified by their dependence on photon energy and nanodroplet size and by comparison with a simple numerical simulation. Conditions for minimizing electron scattering with the He nanodroplets are discussed.
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All authors Niklas Scheel, Narcis Silviu Blaj, Rajni Rajni, Asbjørn Ørnemark Lægdsmand, Jayesh Sadasivan, Subhendu De, Sivarama Krishnan, John Bozek, Aleksandar R. Milosavljevic, Marcel Mudrich

Wednesday 7 October

Atomic and Molecular Clusters · Cross-listed from physics.chem-ph

Nonuniform Screening Reshapes Collective Excitons in Molecular Aggregates from Stochastic Bethe-Salpeter Theory

Barry Y. Li, Chern Chuang, Tim Duong et al. (+3 more)

We build and apply an $\textit{ab initio}$ stochastic Bethe-Salpeter Equation (sBSE) approach to planar cyanine dye aggregate clusters containing up to 2,856 valence electrons. Using a transferable, parameterized screened exchange kernel, we resolve dielectric response, exciton delocalization, and optical spectra within a unified many-body framework. Remarkably, the sBSE transition densities validate the Frenkel exciton picture in real space and provide a practical first-principles route to its screened couplings. The calculations reproduce $\textit{H}$-, $\textit{I}$-, and $\textit{J}$-like spectral evolution and reveal that spatially dependent screening does not merely shift excitonic bands, but reshapes their dispersion, leading to changes in the relative energies of bright and dark exciton states. These results establish sBSE as a predictive framework for large molecular aggregates.
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All authors Barry Y. Li, Chern Chuang, Tim Duong, Tucker Allen, Justin R. Caram, Daniel Neuhauser

Atomic and Molecular Clusters · Cross-listed from hep-ph

Tensor-structure sum rules for spin-1 targets at all $Q^2$

Vladimir Pascalutsa and Marc Vanderhaeghen

We derive a family of sum rules for the tensor structure functions of targets with spin one or higher, rooted in exact Siegert relations. The mixed rank-two $TT$–$LT$ degeneracy combines amplitudes of opposite crossing parity and, under the superconvergence assumption, gives $\int_0^1\! d x\,[b_2(x,Q^2)-3b_4(x,Q^2)]=0$ in the Hoodbhoy–Jaffe–Manohar (HJM) basis. At large $Q^2$, the protected moment agrees with Detmold's target-mass-complete twist-two OPE; in the strict Bjorken projection, and if $b_4$ is neglected, it reduces to the Efremov–Teryaev (ET)-type condition $\int_0^1\! d x\,x\,b_1(x)=0$, whose measured-range footprint is consistent with the HERMES data. Two further rank-two combinations connect crossing-even amplitudes and determine the corresponding subtraction functions through weighted HJM moments. The protected combination can be isolated through separated tensor $LT$ and $TT$ responses, providing a direct experimental strategy for JLab and, ultimately, a future EIC.
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Sunday 4 October

Atomic and Molecular Clusters · Cross-listed from quant-ph

Long-lived Coherent Phonons Reveal Competing Thermal and Many-Body Dynamics in $\alpha$-In$_{2}$Se$_{3}$

Xuanchao Zhang, Dehao Yuan, Junhua Zhou et al. (+4 more)

The fate of quantum coherence following photoexcitation is a central problem in nonequilibrium condensed-matter physics, especially in low-dimensional solids where electronic, structural and many-body energy scales are strongly coupled. Here, we investigate this interplay in ferroelectric $\alpha$-In$_{2}$Se$_{3}$ using broadband transient-grating spectroscopy with $\sim$5 fs laser pulses. Photoexcitation launches pronounced oscillations dominated by a $\sim$104 cm$^{-1}$ mode that persists for several picoseconds. Measurements from 10 to 300 K show that its frequency remains nearly unchanged while its coherence is progressively suppressed, distinguishing the lattice coordinate from thermally activated dephasing. Varying excitation energy reveals a distinct crossover in which increasing photoexcitation progressively modifies and damps the coherent response. First-principles calculations assign the dominant oscillation to a 101.47 cm$^{-1}$ $\Gamma$-point optical phonon involving collective In-Se displacement, while quantum-dynamical simulations reproduce the main transient-grating oscillations. These results establish $\alpha$-In$_{2}$Se$_{3}$ as a model system for independently probing lattice coherence, thermal fluctuations and carrier-density-dependent interactions, revealing how a polar van der Waals semiconductor evolves from coherent lattice motion toward an incoherent many-body state after ultrafast excitation.
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All authors Xuanchao Zhang, Dehao Yuan, Junhua Zhou, Vandana Tiwari, Fulu Zheng, Ajay Jha, Hong-Guang Duan

Tuesday 29 September

Atomic and Molecular Clusters · Cross-listed from cond-mat.quant-gas

Finite-momentum trimers and Cooper quartets in a one-dimensional Fermi gas with coexistent $s$- and $p$-wave interactions

Yixin Guo

We study finite-momentum trimers and Cooper quartets in a one-dimensional two-component Fermi gas with coexistent $s$- and $p$-wave interactions, regularized in the relative momentum of each pair so that they remain Galilean invariant. Pauli blocking alone then makes the trimer dispersion deviate from free center-of-mass motion, so the trimer energy can be lowest at finite total momentum. Allowing this motion expands the $abb$ region among pairs and trimers and removes the region where an odd-wave pair is lowest. The $aabb$ quartet lies below all these branches at every sampled coupling, and in a strip starting on the crossing of the two dimer-pair channels its lowest breakup channel is a moving $abb$ trimer and an atom. At weak interspecies attraction, a variational bound shows that two odd-wave Cooper pairs bind into a quartet, whose binding exceeds that of the coexisting trimer by orders of magnitude as the attraction weakens. At stronger interspecies attraction, the quartet binding relative to two unlike-species dimers disappears when the odd-wave interaction is switched off, although the even-wave interaction dominates the interaction energy. Relative to the in-vacuum case, the Fermi sea enhances the weak-coupling quartet binding, and at fixed scattering lengths the quartet binding grows with density while the coexisting trimer becomes much shallower. These results show that neither the most strongly bound pair nor the dominant interaction energy alone determines whether the quartet binds.
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Monday 28 September

Atomic and Molecular Clusters

Model potential based estimation of positron bound states with polar molecules

Snigdha Sharma and Dhanoj Gupta

Positron forming a bound state with molecules is an area of meticulous research and remains open to simpler techniques for estimating the binding energy. Correlation between the incoming positron and the molecular electrons plays a crucial role even for polar molecules, where binding is also possible at the static-potential level. In this work, we have used a model correlation potential, which accounts for the virtual positronium formation, in the single-center expansion scattering calculations for polar oxygen-containing molecules. The thus determined S-matrix is continued into the complex momentum plane by fitting it to the Pade approximant. The positron bound state is estimated using the calculated pole position of the S-matrix. The results, compared with the latest experimental and ab initio findings, look quite promising.
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Thursday 17 September

Atomic and Molecular Clusters

Hydrogen isotope mixing entropy in ammonia clusters

Klavs Hansen, Åke Andersson, Johannes Reichegger et al. (+2 more)

Measured evaporation branching ratios of partially deuterated isotopologues of protonated ammonia clusters (NH$_3$)$_N$ H$^+$ ($N \geq 8$) show ratios that depend only on the clusters' deuterium mole fraction. This demonstrates randomly distributed protium and deuterium in the molecules and can be used to determine free energy differences in the product cluster. The entropy thus determined is exclusively the deuterium-protium mixing entropy. The relative dissociation energies of the four isotopologues are determined and with the support of quantum chemistry calculations, their absolute values are estimated.
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All authors Klavs Hansen, Åke Andersson, Johannes Reichegger, Siegfried Kollotzek, Paul Scheier

Wednesday 16 September

Atomic and Molecular Clusters · Cross-listed from physics.chem-ph

Spectroscopy of deprotonated anions of cold chlorophyll pigments, an approach to their photosynthetic properties

A. Muheddine, B. Robert, N. Shafizadeh et al. (+1 more)

We introduce here a new approach to the study of isolated chlorophyll pigments with the electronic spectroscopy of their deprotonated anions in a cold environment at 9K. These anions are isoelectronic to the corresponding neutral molecules, therefore their electronic properties are comparable. This comparison is pursued through this article. The electronic spectrum of the Q bands of deprotonated pheophorbide and methyl pheophorbide are recorded by resonant two photon electron detachment with vibrational resolution and show well-resolved bands extending through the visible spectrum in a very similar fashion to their neutral counterparts in solution. The results are compared with data of neutral pheophytin obtained by fluorescence line narrowing spectroscopy at 4K and resonance Raman spectroscopy and found very similar. The theoretical analysis is achieved by density functional (ground state DFT WB97XD, hybrid exchange-correlation functionals and 6-311++G(d,p) basis sets) and time dependent density functional (TDDFT) calculations. The comparison of the active orbitals in the Q transitions shows a great similarity between neutral and anionic forms together with some orbital and related level inversions. The vibronic spectra are simulated by Franck-Condon calculations to assign the dominant transitions of the electronic spectrum. Globally, this is a new perspective in the electronic spectroscopy of chlorophyll pigments that has been opened.
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All authors A. Muheddine, B. Robert, N. Shafizadeh, B. Soep

Tuesday 15 September

Atomic and Molecular Clusters

Electron scattering from polar hydrides using relativistic optical potential method

Sudhanshu Arya and Bobby Antony

We extend the relativistic spherical complex optical-potential method with group additivity developed in our recent work [S. Arya and B. Antony, RSC Adv. 16, 13548–13558 (2026)] to molecules with permanent dipole moments. The short-range electronic collision is described by a central Dirac partial-wave calculation, while the missing anisotropic long-range dipole interaction is restored through a rotationally resolved first-Born contribution. The rotational thresholds, state-to-state transition-dipole strengths, and thermal populations are obtained from the HITRAN2024 spectroscopic database and thermally reweighted at the adopted rotational temperature. Both excitation and superelastic de-excitation channels are included. Electron scattering from benchmark polar hydrides ($\rm H_2O$, $\rm H_2S$, $\rm NH_3$, and $\rm PH_3$) is investigated over the incident-energy range 0.1–10,000 eV. We report vibrationally elastic, differential, integral, and momentum-transfer cross sections, together with a total cross section that also contains electronically inelastic loss from the quasifree absorption potential. The calculations reproduce the broad experimental and recommended trends over a wide energy range. The largest deviations are confined mainly to the low-energy and resonance-sensitive regions. Overall, the agreement improves substantially from the tens-of-eV region upward. The method therefore retains the low computational cost and wide energy coverage of the optical-potential approach while adding the long-range rotational physics needed for polar molecules.
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Monday 7 September

Atomic and Molecular Clusters · Cross-listed from physics.chem-ph

Strong Evidence for Formation of Hydroxyl Anion via 2-Particle-1-Hole Feshbach Resonances

Siddique Ali, Meenakshi Rana, Soumya Ghosh et al. (+3 more)

This study investigates the formation of the hydroxyl anion (OH$^-$) via dissociative electron attachment in 2-propanol as a model system for studying both organic and inorganic molecules. Using high-level CAP-EOM-EA-CCSD calculations and advanced ToF mass spectrometry, we demonstrate that OH$^-$ formation at electron energies between 7 and 11 eV is dominated by two-particle-one-hole (2p-1h) Feshbach resonances. The potential-energy curves reveal a dense manifold of anionic states coupled through numerous avoided crossings, facilitating nonadiabatic population transfer during C-OH bond dissociation. Survival-probability analysis identifies a subset of six long-lived resonances that persist long enough to drive fragmentation, with states 25 and 28 acting as primary drivers by funneling the attached electron into the localized $\sigma^*(\mathrm{C{-}OH})$ antibonding orbital. These theoretical predictions are confirmed by experimental observations of a prominent OH$^-$ yield peaking at 8.6 eV, supporting a site-specific fragmentation mechanism that generalizes to the broader class of molecules.
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All authors Siddique Ali, Meenakshi Rana, Soumya Ghosh, Narayan Kundu, Aryya Ghosh, Dhananjay Nandi

Atomic and Molecular Clusters

Core-Level Spectroscopy Decodes Bond-Alternation Dynamics of Cyclo[18]Carbon

Minrui Wei, Zeyu Liu, Sheng-Yu Wang et al. (+4 more)

The advent of X-ray free-electron lasers and high-harmonic generation has made time-resolved X-ray spectroscopy a powerful tool for probing local atomic environments, yet whether localized core excitations can report on global collective distortions remains open. Cyclo[18]carbon (C$_{18}$), with its polyynic ground state (D$_\text{9h}$) and cumulenic transition state (D$_\text{18h}$), provides an ideal model to address this long-standing issue in bond-length alternation (BLA) dynamics. Mapping two-dimensional potential energy surfaces by first-principles simulations, we find that core ionization symmetrizes the ground-state double-well potential along the BLA coordinate. Our calculated X-ray spectra reveal remarkable sensitivity to bond-length variations: C1s ionization potentials vary by up to 2.4~eV across the BLA coordinate (1.1–1.4~Å), with a 0.9~eV variation for minima predicted by different functionals, while NEXAFS $\pi^*$ peaks shift by up to 4~eV across the same coordinate. These predicted signatures provide a quantitative spectroscopy–structure dictionary for decoding transient structures in future ultrafast X-ray experiments and monitoring bond-alternation dynamics in real time.
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All authors Minrui Wei, Zeyu Liu, Sheng-Yu Wang, Jun-Rong Zhang, Lu Zhang, Guoyan Ge, Weijie Hua

Sunday 6 September

Atomic and Molecular Clusters · Cross-listed from physics.optics

Energy-scalable single-burst attosecond emission at kiloelectronvolt photon energies

Kaito Nishimiya and Eiji J. Takahashi

Attosecond soft-X-ray pulses at kiloelectronvolt photon energies would provide direct access to the L-edges of transition metals, enabling element-specific studies of charge, spin, and orbital dynamics on their intrinsic timescales. However, attosecond emission in this spectral region has remained elusive because the only phase-matched keV high-harmonic source demonstrated to date employed multicycle driving pulses without carrier-envelope-phase (CEP) control. A long-standing gap has therefore persisted between keV photon energies and CEP-controlled attosecond emission. Here, we bridge this gap using a CEP-stabilized mid-infrared laser system with pulse durations tunable to the sub-cycle regime. Through phase-matched highharmonic generation in low-pressure neutral helium under meter-scale loose-focusing conditions, we generate coherent soft-X-ray continua reaching 1.2 keV. Crucially, we observe CEP-dependent spectral modulation that reaches into the transition-metal L-edge region, providing experimental evidence consistent with the generation of isolated attosecond pulses. To demonstrate the capabilities of our source, we perform broadband soft-X-ray absorption spectroscopy spanning the Ti, Fe, Co, and Ni L-edges, as well as the O K-edge, and resolve near-edge fine structures. By combining meter-scale loose focusing with low-pressure phase matching, our approach addresses key energy-scaling limitations of previous keV high-harmonic sources and establishes a phase-matched, CEP-controlled keV soft-X-ray platform for attosecond spectroscopy of magnetic, quantum, and strongly correlated materials.
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Thursday 3 September

Atomic and Molecular Clusters

X-ray photoelectron spectroscopy of Ar and Kr clusters formed in He nanodroplets

N. S. Blaj, N. Scheel, R. Rajni et al. (+7 more)

We report the first soft x-ray photoelectron spectroscopy (XPS) measurements of Ar and Kr clusters formed inside superfluid helium nanodroplets (HNDs) through consecutive pickup of dopant atoms. Ar and Kr atoms and clusters are selectively inner-shell ionized (Ar 2p, Kr 3d) using monochromatic soft x-ray synchrotron radiation. In the regime of strong doping, the electron spectra exhibit features characteristic of free Ar and Kr atoms as well as their clusters. The Kr cluster spectra agree well with literature data for bare Kr clusters. Backed by detailed simulations of the pickup process, this agreement indicates that the observed spectra originate from nearly bare Ar and Kr clusters, from which most or all He has evaporated in the course of cluster aggregation. These results establish HNDs as a platform for XPS of various types of molecular complexes and nanostructures.
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All authors N. S. Blaj, N. Scheel, R. Rajni, A. Ø. Lægdsmand, J. Sadasivan, S. De, S. R. Krishnan, J. Bozek, A. R. Milosavljević, M. Mudrich

Wednesday 2 September

Atomic and Molecular Clusters · Cross-listed from cond-mat.mtrl-sci

A Wannier-first approach for extended chiral systems

Yashpal Singh, Juan E. Peralta, Koblar A. Jackson et al. (+1 more)

We present a real-space formulation of DFT for extended systems in which localized Wannier-like functions are constructed directly from localized Gaussian basis functions without explicitly computing canonical Bloch-like states during the self-consistent cycle. Building on the formalism of Pederson and Lin [Phys. Rev. B 35, 2273 (1987)], a variational set of Wannier-like functions is generated self-consistently within a finite Wannier domain and used to construct the charge density, electrostatic potential, and per cell total energy of the extended system. The occupied space can be determined entirely from the Wannier-like functions. Electronic band structures can be recovered in a post-processing step by solving the full Hamiltonian in a Bloch-like basis constructed from Gaussian orbitals. A key feature of the method is that it can incorporate combined translation–rotation, or screw, symmetries, enabling efficient simulations of chiral and helical systems with finite twist angles at essentially the same computational cost as systems described by pure translational symmetry. The approach is validated through calculations on linear and twisted $\mathrm{{-}C{\equiv}C{-}}$ and $\mathrm{{-}Li{-}F{-}}$ chains, as well as graphene, where total energies and band structures show excellent agreement with reference periodic calculations. To illustrate the ability of the method to treat three-dimensional systems, it is further applied to AA graphite, in which carbon atoms in adjacent graphene layers are aligned directly above one another, as well as helically stacked AA graphite structures. The Wannier-first framework provides a practical route for treating extended systems with nontrivial translational, rotational, and screw symmetries, and provides a natural foundation for the implementation of orbital-dependent functionals such as the Perdew–Zunger self-interaction correction.
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All authors Yashpal Singh, Juan E. Peralta, Koblar A. Jackson, Mark R. Pederson

Wednesday 26 August

Atomic and Molecular Clusters · Cross-listed from physics.chem-ph

Core-valence double ionization of SF6 involving S2p, F1s and S1s inner shells

Veronica Daver Ideböhn, Daniel M. Pereira, Lucas M. Cornetta et al. (+11 more)

Core-valence double ionization electron spectra near the S2p, F1s and S1s edges of SF6 are presented, analyzed and compared with conventional valence photoelectron spectra and quantum chemical calculations. The core-valence spectra are energetically stretched out, revealing salient structures between 15 and 40 eV that are sufficiently separated for molecular orbital analysis. The spectra offer new insights into the electronic structure, showing that the core hole substantially rearranges the molecular orbital order. This effect can be traced to orbital localization and nodal structure, as well as to valence-to-core penetration. The singlet and triplet splittings of the dicationic states progressively decrease in all three core-valence spectra towards deeper core levels, with larger splittings for S2p than S1s, reflecting greater valence-to-core penetration and exchange interaction for S2p. By large, the MO interpretation holds in frozen or self-consistent-field representations, except for the inner parts of the F1s spectra, which require analysis in terms of MO breakdown effects. An intensity model for CV spectra is derived using an independent-channel approach, where primary core ionization is treated by dipolar coupling to a continuum and the valence electron is promoted to a second continuum through shake-off. Full spin coupling and spin selectivity between the discrete doubly ionized states and the two continuum electrons are maintained. The primary molecular photoelectron intensity is expressed as a weighted sum of atomic subshell cross sections using a one-center atomic orbital projection of the relevant molecular orbital. The calculated spectra agree well with experiment and allow detailed assignment. In particular, symmetry breaking at the F1s core-ionization site is identified and discussed.
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All authors Veronica Daver Ideböhn, Daniel M. Pereira, Lucas M. Cornetta, Richard J. Squibb, Andreas Hult Roos, Emelie Olsson, Måns Wallner, Marco Parriani, Nihar Ranjan Behera, Gunnar Öhrwall, Florian Trinter, John H.D. Eland, Hans Ågren, Raimund Feifel

Friday 21 August

Atomic and Molecular Clusters · Cross-listed from quant-ph

Programmable Doppler real-space pattern formation in cold atoms

Yijun Tang

Red-detuned Doppler cooling decelerates atomic motion toward zero velocity, whereas blue-detuned light produces acceleration that separates a cold cloud into finite-velocity packets. Here we combine these complementary dynamics in a programmable split-stop protocol for real-space pattern formation. During each stage, a blue-detuned pulse splits existing packets and drives them apart, while a subsequent red-detuned pulse returns their center-of-mass velocities close to zero, results in spatially resolved stationary packets. Repeating this process recursively multiplies the number of packets in real space. We model the dynamics using stochastic photon-jump simulations that include absorption and spontaneous-emission recoil in one and two dimensions. Using experimentally realistic parameters for the $689~\mathrm{nm}$ ${}^{1}S_{0}\rightarrow{}^{3}P_{1}$ transition of ${}^{88}\mathrm{Sr}$, we demonstrate an 8-packet one-dimensional array and a 64-packet two-dimensional square array.
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Thursday 20 August

Atomic and Molecular Clusters · Cross-listed from cond-mat.quant-gas

Self-limiting electrostriction of a single ion in an ultracold polar gas: From mesoscopic ions to crystalline molecular rings

Ruiren Shi, Saajid Chowdhury, Leon Karpa et al. (+1 more)

We investigate the self-assembly of polar molecules around a single ion immersed in an ultracold, dilute two-dimensional molecular gas. The ion aligns and attracts the molecules through charge-dipole interactions, producing a strong electrostrictive accumulation around the impurity, while intermolecular repulsion limits further densification and favors spatially extended configurations. By combining global optimization with diffusion Monte Carlo, we calculate the evaporation energy as a function of the number of molecules bound to the ion. In contrast to conventional charged and van der Waals clusters, the evaporation energy exhibits a plateau-like dependence on cluster size, reflecting the sequential formation of concentric molecular rings. These structures are governed by the topology of the ion's electric field and by the competition between attractive ion-molecule interactions, repulsive intra-ring interactions, and attractive correlations between neighboring rings, rather than by conventional coordination or icosahedral packing. In the weak-interaction regime, the resulting structures form extended mesoscopic molecular ions, whereas stronger interactions produce increasingly rigid, crystal-like molecular rings. We further analyze their stability against thermal perturbations and the time-dependent ion trap and find that a broad range of clusters remain stable under experimentally relevant conditions. The intermolecular repulsion and dipolar geometry also suppress close-range ion-molecule encounters, suggesting an intrinsic shielding mechanism. Our results establish ion-bound polar-molecule clusters as a distinct class of mesoscopic molecular ions and open a route to studying charged impurities in quantum baths with anisotropic interactions.
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All authors Ruiren Shi, Saajid Chowdhury, Leon Karpa, Jesús Pérez-Ríos

Wednesday 19 August

Atomic and Molecular Clusters · Cross-listed from cond-mat.mtrl-sci

Dynamic Ensembles of Phosphine-Stabilized Gold Nanoclusters

Caitlin A. McCandler, Disha Sanwal and Jutta Rogal

Atomically precise phosphine-stabilized gold nanoclusters are commonly characterized by single-crystal X-ray diffraction, yet the extent to which these static structures represent finite-temperature behavior remains unclear. To explore the free-energy landscapes, equilibrium populations, and isomerization kinetics of these nanoclusters in the gas phase, we establish a general framework that combines molecular dynamics simulations based on a machine-learned interatomic potential with Markov state models (MSMs). Analysis of the MSMs indicates that experimentally reported crystal structures frequently correspond to minor metastable states or transient configurations rather than the dominant finite-temperature structures. Increasing ligand coverage systematically alters both the thermodynamics and kinetics of structural rearrangements, driving the transition from planar to three-dimensional gold cores while accelerating isomerization dynamics. Moreover, catalytically accessible geometries are often only minor members of the equilibrium ensemble, highlighting a trade-off between structural stability and surface accessibility. These results emphasize that ligand-protected nanoclusters need to be viewed as dynamic ensembles and their finite-temperature behavior cannot be fully captured by their corresponding crystallographic structures alone.
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Atomic and Molecular Clusters · Cross-listed from cond-mat.quant-gas

Electrostriction in a Bose-Einstein Condensate of Dipolar Molecules

Haneul Kwak, Ian Stevenson, Weijun Yuan et al. (+5 more)

The recent creation of a Bose-Einstein condensate (BEC) of dipolar molecules has opened a new frontier for many-body quantum systems in which dipolar interactions can drive novel self-organization phenomena. Here, we observe electrostriction in a molecular BEC, an elliptical deformation driven by anisotropic dipolar interactions. We use double microwave dressing, involving $\sigma$- and $\pi$-polarized fields, to control non-axially symmetric dipolar interactions. We compare the experimental observations of electrostriction to a model based on an extended Gross-Pitaevskii equation and find excellent agreement in the regime of weak to moderate interactions. Using electrostriction, we demonstrate that the molecular BEC can be torqued by dynamically changing the orientation of the elliptical $\sigma$ microwave field. This provides a route to setting molecular quantum gases into rotation, opening opportunities to probe vorticity, superfluidity, and supersolidity in strongly dipolar matter.
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All authors Haneul Kwak, Ian Stevenson, Weijun Yuan, Siwei Zhang, Asaf Toprakci, Lin Su, Tijs Karman, Sebastian Will

Atomic and Molecular Clusters · Cross-listed from quant-ph

Unified Strong-Field Dynamics Simulations from Atoms to Heterostructures

Zakaria Dahbi and Amelle Zaïr

We present TDSE-Z, a high-performance open-source framework for strong-field quantum dynamics in atomic, molecular, and semiconductor effective-mass systems. The core engine implements a weak-form Galerkin discretisation of the Hermitian BenDaniel-Duke operator, $\hat{T}_{\mathrm{BDD}} = -\frac{1}{2}\nabla\cdot(m^{-1}(\mathbf{r})\nabla)$, on geometry-adapted B-spline meshes, supporting arbitrary potentials and customisable laser configurations in one to three dimensions. We validate the static position-dependent-mass (PDM) eigensolver through two stringent benchmarks: a comparison to the analytical Quesne PDM model and a $\text{GaAs/Al}_{0.3}\text{Ga}_{0.7}\text{As}$ double quantum well, where the exponential decay of computed tunnel splittings follows Wentzel-Kramers-Brillouin (WKB) theory at the sub-percent level. We further demonstrate the time-propagation engine on constant-mass systems, accurately reproducing high-harmonic generation (HHG) spectra in atomic benchmarks and confirming the importance of dimensionality in fully capturing the strong light-matter interaction. Our implementation demonstrates robust strong-scaling efficiency, maintaining performance across hundreds of CPU cores. While the static eigensolver currently supports optional GPU offloading, the time-propagation engine is CPU-optimised, providing a modular architecture for future expansion toward exascale quantum dynamics.
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Monday 17 August

Atomic and Molecular Clusters · Cross-listed from quant-ph

Evidence for cavity-induced metallic phase from entropic electron correlation effects

Jacob Horak and Dominik Sidler

Experiments have revealed that collective strong coupling in optical cavities can drastically alter the conductivity and dielectric properties of molecular ensembles, or even trigger abrupt phase transitions (in Rayleigh scattering or dispersion force driven conformational equilibrium). Until now, the underlying physical mechanism has remained unknown. A recently proposed theory attributes these collective effects to cavity-induced electron correlations that share properties of the known spherical Sherrington-Kirkpatrick model of a spin glass. As a consequence, entropic effects can trigger a phase transition in the inter-molecular electron correlations that could potentially explain the above experiments. In the following work, we derive analytic expressions for the correlation (free-)energy-induced polarizability changes, which reveal that under certain conditions collective strong coupling can even render our molecular ensemble metallic by entropically ionizing collectively degenerate molecular orbitals. Our results are a first major step towards a holistic theory of cavity-mediated electron correlation effects.
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Thursday 13 August

Atomic and Molecular Clusters

What is superatom?

Zhigang Wang

The term "superatom" was introduced over three decades ago to describe clusters that emulate elemental atoms. The field has long been guided by the spherical jellium model, where magic numbers arise from shell closure of delocalized electrons. This Perspective argues that delocalization, not near-sphericity, is what makes a system atom-like. It shows that superatomic shell structure persists under arbitrary point-group symmetry, that superatomicity survives as a tunable quantum state across pressurized, ionized, and chemically precompressed systems, and that the symmetry rules governing superatoms are conditional, deeper than the jellium picture admits. The future of this field lies not in finding more magic numbers, but in exploiting superatomic states as artificial quantum systems at the atomic level.
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Thursday 6 August

Atomic and Molecular Clusters · Cross-listed from physics.chem-ph

X-ray Driven Trihydrogen Formation on Silica Nanosurfaces

Samuel Sahel-Schackis, Adam Summers, Ritika Dagar et al. (+29 more)

The trihydrogen cation ($\mathrm{H_3^+}$) initiates the ion-molecule reactions that build molecular complexity in interstellar space. Whether its canonical formation reaction, $\mathrm{H_2^+ + H_2 \rightarrow H_3^+ + H}$, proceeds on inorganic surfaces under radiation-driven ionization has remained untested. Here we drive $\mathrm{H_3^+}$ formation on hydrated silica nanoparticles using intense 1.88 keV X-ray pulses, combining ion velocity map imaging, electron time-of-flight spectroscopy, and single-particle coherent diffractive imaging to resolve this chemistry on individual particles. The self-induced surface electric field on the V/nm scale drives interfacial charge transfer and water fragmentation. This field is the dominant parameter governing the relative yields of $\mathrm{H^+}$, $\mathrm{H_2^+}$, and $\mathrm{H_3^+}$ across particle size, composition, and aggregation. Density functional theory and nonadiabatic quantum molecular dynamics simulations trace this field-driven charge transfer, directly analogous to band bending at semiconductor photoelectrodes. These results establish surface-field-driven charge transfer as a unifying mechanism between radiation dominated astrophysical environments and field-driven surface catalysis.
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All authors Samuel Sahel-Schackis, Adam Summers, Ritika Dagar, Alexandra Feinberg, Martin Grassl, Simon Dold, Rebecca Boll, Yevheniy Ovcharenko, Chris Aikens, Cesar Costa Vera, Alberto De Fanis, Avijit Duley, Felix Gerke, Daniel Jost, Regina Leiner, Michael Meyer, Ilana J. P. Molesky, Razib Obaid, Jeffrey Powell, Nils Rennhack, Björn Senfftleben, Hendrik Tackenberg, Paul Tuemmler, Sergey Usenko, Christian Peltz, Thomas Fennel, Markus Gallei, Eckart Rühl, Artem Rudenko, Daniel Rolles, Thomas Linker, Matthias F. Kling

Monday 3 August

Atomic and Molecular Clusters · Cross-listed from physics.plasm-ph

Mass Spectrometry Studies of Hydrogen Ions Energy Distributions in an ECR- based Large Volume Plasma Source

Bibekananda Naik, Ramesh Narayanan, Debaprasad Sahu et al. (+2 more)

Plasma is produced in a Large Volume Plasma Source (LVPS; dia. = 1 m, height = 1m) using CW microwaves (= 400 - 600 W, 2.45 GHz), in a compact ECR plasma source (CEPS) attached to LVPS, at hydrogen gas pressures = 1 - 3 mTorr. Plasma expands along the CEPS magnetic field into LVPS. A Hiden Analytical HPR 60 molecular beam mass spectrometer (MBMS) is used to measure the H^- ion energy distribution functions (IEDFs) in the downstream plasma. Previous plasma characterization studies in LVPS indicated favourable downstream plasma conditions for volume production of H^- ions. Measurements conducted with the MBMS probe aligned facing the plasma flow = 80 cm downstream, gave typical H^- count rates = 3 x 10^5 counts /s, at = 400 W, = 1 mTorr, along with a distinct high energy tail (<= 20 eV). These and other results are analyzed in detail. The positive ion spectrum showed the H_3^+ count to be consistently high in all cases (= 60-70 %); the counts for H_2^+ and H^+ were =30-35 % and a =few %. Combining the Langmuir probe (LP) and MBMS data it is possible to determine the approximate densities in front of the MBMS probe aperture. At = 500 W and = 2 mTorr, one finds: n_(H^+) = 9.6 x 10^9 cm^(-3), n_(H_2^+) = 1.7 x 10^10 cm^(-3) and n_(H_3^+) = 4.3 x 10^10 cm^(-3). The corresponding H^- density, = 80 cm downstream is n_(H^-) = 3.9 x 10^8 cm^(-3). Accounting for all H^- losses due to scattering and destruction, one finds the effective mean free path for H^- loss to be = 12.4 cm. Noting that H^- formation takes place about = 10 - 30 cm downstream of the source exit, the approximate average H^- density in the formation zone is determined as = 5.5 x 10^10 cm^(-3). This value is remarkably encouraging for H^- production in volume mode, considering the large chamber volume and area, as well as the very moderate power used for the experiments.
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All authors Bibekananda Naik, Ramesh Narayanan, Debaprasad Sahu, Mainak Bandyopadhyay, Ashish Ganguli