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L. S. Cederbaum

Publications and source records attributed to L. S. Cederbaum.

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Fragmentation of a trapped multiple-species bosonic mixture

We consider a multiple-species mixture of interacting bosons, $N_1$ bosons of mass $m_1$, $N_2$ bosons of mass $m_2$, and $N_3$ bosons of mass $m_3$ in a harmonic trap of frequency $ω$. The corresponding intraspecies interaction strengths are $λ_{11}$, $λ_{22}$, and $λ_{33}$, and the interspecies interaction strengths are $λ_{12}$, $λ_{13}$, and $λ_{23}$. When the shape of all interactions are harmonic, this is the generic multiple-species harmonic-interaction model which is exactly solvable. We start by solving the many-particle Hamiltonian and concisely discussing the ground-state wavefunction and energy in explicit forms as functions of all parameters, the masses, numbers of particles, and the intraspecies and interspecies interaction strengths. We then move to compute explicitly the reduced one-particle density matrices for all the species and diagonalize them, thus generalizing the treatment in [J. Chem. Phys. {\bf 161}, 184307 (2024)]. The respective eigenvalues determine the degree of fragmentation of each species. As applications, we focus on aspects that do not appear for the respective single-species and two-species systems. For instance, placing a mixture of two kinds of bosons in a bath made by a third kind, and controlling the fragmentation of the former by coupling to the latter. Another example exploits the possibility of different connectivities (i.e., which species interacts with which species) in the mixture, and demonstrates how the fragmentation of species $3$ can be manipulated by the interaction between species $1$ and species $2$, when species $3$ and $1$ do not interact with each other. We thereby highlight properties of fragmentation that only appear in the multiple-species mixture. Further applications are briefly discussed.

cond-mat.quant-gas

Properties of a trapped multiple-species bosonic mixture at the infinite-particle-number limit: A solvable model

We investigate a trapped mixture of Bose-Einstein condensates consisting of a multiple number of P species using an exactly-solvable many-body model, the $P$-species harmonic-interaction model. The solution is facilitated by utilizing a double set of Jacoby coordinates. A scheme to integrate the all-particle density matrix is derived and implemented. Of particular interest is the infinite-particle-number limit, which is obtained when the numbers of bosons are taken to infinity while keeping the interaction parameters fixed. We first prove that at the infinite-particle-number limit {\it all} the species are $100\%$ condensed. The mean-field solution of the $P$-species mixture is also obtained analytically, and is used to show that the energy per particle and densities per particle computed at the many-body level of theory boil down to their mean-field counterparts. Despite these, correlations in the mixture exist at the infinite-particle-number limit. To this end, we obtain closed-form expressions for the correlation energy and the depletion of the species at the infinite-particle-number limit. The depletion and the correlation energy per species are shown to critically depend on the number of species. Of separate interest is the entanglement between one species of bosons and the other $P-1$ species. Interestingly, there is an optimal number of species, here $P=3$, where the entanglement is maximal. Importantly, the manifestation of this interspecies entanglement in an observable is possible. It is the position-momentum uncertainty product of one species in the presence of the other $P-1$ species which is derived and demonstrated to correlate with the interspecies entanglement. All in all, we show and explain how correlations at the infinite-particle-number limit of a trapped multiple-species bosonic mixture depend on the interactions, and how they evolve with the number of species.

cond-mat.quant-gas

Effects Beyond Center-of-Mass Separability in a Trapped Bosonic Mixture: Exact Results

An exactly solvable model mimicking demixing of two Bose-Einstein condensates at the many-body level of theory is devised. Various properties are expressed in closed form along the demixing pathway and investigated. The connection between the center-of-mass coordinate and in particular the relative center-of-mass coordinate and demixing is explained. The model is also exactly solvable at the mean-field level of theory, allowing thereby comparison between many-body and mean-field properties. Applications are briefly discussed.

cond-mat.quant-gas

Time-resolved observation of interatomic Coulombic decay induced by two-photon double excitation of Ne$_{2}$

The hitherto unexplored two-photon doubly-excited states [Ne$^{*}$($2p^{-1}3s$)]$_{2}$ were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD) which predominantly produces singly-ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne$_{2}^{+}$ ions was recorded as a function of delay between the XUV pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly-excited states, 390 (-130 / +450} fs, and of the short-lived ones, less than 150~fs, are in good agreement with \emph{ab initio} quantum mechanical calculations.

physics.atom-ph

First Observation of Electron Transfer Mediated Decay in Aqueous Solutions: A Novel Probe of Ion Pairing

A major goal of many spectroscopic techniques is to provide comprehensive information on the local chemical environment. Electron transfer mediated decay (ETMD) is a sensitive probe of the environment since it is actively involved in this non-local radiationless decay process through electron and energy transfer steps. We report the first experimental observation of ETMD in the liquid phase. Using liquid-jet X-ray photoelectron spectroscopy we explore LiCl aqueous solution, and detect low-energy electrons unambiguously emerging from the ETMD processes of core-ionized Li+. We interpret the experimental results with molecular dynamics and high-level ab initio calculations. By considering various solvation-structure models we show that both water molecules and Cl- anions can participate in ETMD, with each process having its characteristic spectral fingerprint. Different ion associations lead to different spectral shapes. The potential application of the unique sensitivity of the ETMD spectroscopy to the local hydration structure and ion pairing is discussed.

physics.chem-ph

Fano Resonances observed in Helium Nanodroplets

Doubly-excited Rydberg states of helium (He) nanodroplets have been studied using synchrotron radiation. We observed Fano resonances related to the atomic N = 2,0 series as a function of droplet size. Although similar qualitatively to their atomic counterparts, the resonance lines are broader and exhibit a shift in energy which increases for the higher excited states. Furthermore, additional resonances are observed which are not seen in atomic systems. We discuss these features in terms of delocalized atomic states perturbed by the surrounding He atoms and compare to singly excited droplets.

physics.chem-ph

Enhanced ionization of embedded clusters by Electron Transfer Mediated Decay in helium nanodroplets

Here, we report the observation of electron transfer mediated decay (ETMD) involving Mg clusters embedded in helium nanodroplets which is initiated by the ionization of helium followed by removal of two electrons from the Mg clusters of which one is transferred to the He environment neutralizing it while the other electron is emitted into the continuum. The process is shown to be the dominant ionization mechanism for embedded clusters for photon energies above the ionization potential of He. The photoelectron spectrum reveals a low energy ETMD peak. For Mg clusters larger than 5 atoms we observe stable doubly-ionized clusters. We argue that ETMD provides a new pathway to the formation of doubly-ionized cold species.

physics.chem-ph

Overcoming blockade in producing doubly-excited dimers by a single intense pulse and their decay

Excitation of two identical species in a cluster by the absorption of two photons of the same energy is strongly suppressed since the excitation of one subunit blocks the excitation of the other one due to the binding Coulomb interaction. Here, we propose a very efficient way to overcome this blockade in producing doubly-excited homoatomic clusters by a single intense laser pulse. For Ne$_2$ it is explicitly demonstrated that the optimal carrier frequency of the pulse is given by half of the energy of the target state, which allows one to doubly excite more than half of the dimers at moderate field intensities. These dimers then undergo ultrafast interatomic decay bringing one Ne to its ground state and ionizing the other one. The reported \emph{ab initio} electron spectra present reliable predictions for future experiments by strong laser pulses.

physics.atm-clus

Build-up of coherence between initially-independent subsystems: The case of Bose-Einstein condensates

When initially-independent subsystems are made to contact, {\it coherence} can develop due to interaction between them. We exemplify and demonstrate this paradigm through several scenarios of two initially-independent Bose-Einstein condensates which are allowed to collide. The build-up of coherence depends strongly on time, interaction strength and other parameters of each condensate. Implications are discussed.

cond-mat.other

Interferences in the density of two initially independent Bose-Einstein condensates

It is shown that the density of two {\it initially independent} condensates which are allowed to expand and overlap can show interferences as a function of time due to interparticle interaction. Using many-body theory, explicit expressions for the density are given which are exact in the weak interaction limit. General working equations are discussed which reproduce exactly the density in this limit. Illustrative examples are presented.

cond-mat.other

Time-dependent multi-orbital mean-field for fragmented Bose-Einstein condensates

The evolution of Bose-Einstein condensates is usually described by the famous time-dependent Gross-Pitaevskii equation, which assumes all bosons to reside in a single time-dependent orbital. In the present work we address the evolution of fragmented condensates, for which two (or more) orbitals are occupied, and derive a corresponding time-dependent multi-orbital mean-field theory. We call our theory TDMF($n$), where $n$ stands for the number of evolving fragments. Working equations for a general two-body interaction between the bosons are explicitly presented along with an illustrative numerical example.

cond-mat.other

Best mean-field for condensates

The Gross-Pitaevskii equation assumes that all (identical) bosons of a condensate reside in a single one-particle function. Here, we raise the question whether it always provides the best mean-field ansatz for condensates, leading to the lowest mean-field ground state energy. To this end, we derive a mean-field approach allowing for bosons to reside in several different one-particle functions. The number of bosons in each of these functions is a variational parameter minimizing the energy. The energy and one-particle functions at these optimal numbers can be determined directly. A numerical example is presented demonstrating that the mean-field energy of trapped bosons can be below that provided by the Gross-Pitaevskii equation. Implications are discussed.

cond-mat

Self-consistent fragmented excited states of trapped condensates

Self-consistent excited states of condensates are solutions of the Gross-Pitaevskii (GP) equation and have been amply discussed in the literature and related to experiments. By introducing a more general mean-field which includes the GP one as a special case, we find a new class of self-consistent excited states. In these states macroscopic numbers of bosons reside in different one-particle functions, i.e., the states are fragmented. Still, a single chemical potential is associated with the condensate. A numerical example is presented, illustrating that the energies of the new, fragmented, states are much lower than those of the GP excited states, and that they are stable to variations of the particle number and shape of the trap potential.

cond-mat

Strong charge transfer effects in the Mg2p^{-1} core-level spectrum of MgB_2

The two available Mg2p^{-1} spectra of the recently discovered high-temperature superconducting MgB_2 crystal exhibit interesting structures, but contradict each other. This motivated us to perform ab initio calculations on the core-level spectra of cluster models. The computed spectra reveal unusual rich and intense structures triggered by a B2p_z->Mg3s,3p charge transfer

cond-mat.str-el

Ab initio calculations with a nonspherical Gaussian basis set: Excited states of the hydrogen molecule

A basis set of generalized nonspherical Gaussian functions (GGTOs) is presented and discussed. As a first example we report on Born-Oppenheimer energies of the hydrogen molecule. Although accurate results have been obtained, we conclude that H_2 is too 'simple' to allow for a substantial gain by using nonspherical functions. We rather expect that these functions may be particularly useful in calculations on large systems. A single basis set of GGTOs was used to simultaneously calculate the potential energy curves of several states within each subspace of {1,3}Σ_{g,u} symmetry. We hereby considerd the entire region of internuclear distances 0.8 < R < 1000 a.u. In particular the results for the fourth up to sixth electronic states show a high accuracy compared to calculations which invoke explicitely correlated functions, e.g. the relative accuracy is at least of the order of magnitude of 10^{-5}a.u. Energies for the 4 ^1Σ_u^+ and 4-6 ^3Σ_u^+ were improved and accurate data for the 6 ^3Σ_g^+, 5 ^1Σ_u^+, and 6 ^1Σ_u^+ state are, to the best of the authors knowledge, presented for the first time. Energy data for the seventh up to the nineth electronic state within each subspace were obtained with an estimated error of the order of magnitude of 10^{-4}a.u. The 7 ^1Σ_g^+ and the 6 ^1Σ_u^+ state were found to exhibit a very broad deep outer well at large internuclear distances.

physics.chem-ph

The hydrogen molecule in magnetic fields: The ground states of the Sigma manifold of the parallel configuration

The electronic structure of the hydrogen molecule is investigated for the parallel configuration. The ground states of the Sigma manifold are studied for ungerade and gerade parity as well as singlet and triplet states covering a broad regime of field strengths from B = 0 up to B = 100a.u. A variety of interesting phenomena can be observed. For the ^1Sigma_g state we found a monotonous decrease of the equilibrium distance and a simultaneously increase of the dissociation energy with growing magnetic field strength. The ^3Σ_g state is shown to develop an additional minimum which has no counterpart in field-free space. The ^1Σ_u state shows a monotonous increase in the dissociation energy with first increasing and than decreasing internuclear distance of the minimum. For this state the dissociation channel is H_2 to H^- + H^+ for magnetic-field strengths B greater than 20a.u. due to the existence of strongly bound H^- states in strong magnetic fields. The repulsive ^3Σ_u state possesses a very shallow van der Waals minimum for magnetic-field strengths smaller than 1.0a.u. within the numerical accuracy of our calculations. The ^1Σ_g and ^3Σ_u states cross as a function of B and the ^3Σ_u state, which is an unbound state, becomes the ground state of the hydrogen molecule in magnetic fields B greater than 0.2a.u. This is of particular interest for the existence of molecular hydrogen in the vicinity of white dwarfs. In superstrong fields the ground state is again a strongly bound state, the ^3Π_u state.

physics.chem-ph

Hydrogen molecule in a magnetic field: The lowest states of the Pi manifold and the global ground state of the parallel configuration

The electronic structure of the hydrogen molecule in a magnetic field is investigated for parallel internuclear and magnetic field axes. The lowest states of the $Π$ manifold are studied for spin singlet and triplet$(M_s = -1) $ as well as gerade and ungerade parity for a broad range of field strengths $0 \leq B \leq 100 a.u.$ For both states with gerade parity we observe a monotonous decrease in the dissociation energy with increasing field strength up to $B = 0.1 a.u.$ and metastable states with respect to the dissociation into two H atoms occur for a certain range of field strengths. For both states with ungerade parity we observe a strong increase in the dissociation energy with increasing field strength above some critical field strength $B_c$. As a major result we determine the transition field strengths for the crossings among the lowest $^1Σ_g$, $^3Σ_u$ and $^3Π_u$ states. The global ground state for $B \lesssim 0.18 a.u.$ is the strongly bound $^1Σ_g$ state. The crossings of the $^1Σ_g$ with the $^3Σ_u$ and $^3Π_u$ state occur at $B \approx 0.18$ and $B \approx0.39 a.u.$, respectively. The transition between the $^3Σ_u$ and $^3Π_u$ state occurs at $B \approx 12.3 a.u.$ Therefore, the global ground state of the hydrogen molecule for the parallel configuration is the unbound $^3Σ_u$ state for $0.18 \lesssim B \lesssim 12.3 a.u.$ The ground state for $B \gtrsim 12.3 a.u.$ is the strongly bound $^3Π_u$ state. This result is of great relevance to the chemistry in the atmospheres of magnetic white dwarfs and neutron stars.

physics.chem-ph