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Maxence Lepers

Publications and source records attributed to Maxence Lepers.

At least 19 recordsLinked to original sources

Revisiting the luminescence properties of Pr3+: YAG within the framework of an extended approach of Judd-Ofelt theory

We show in this article the improvements which can be obtained in the description of the luminescence properties of Pr3+ doped materials by using an extension of the Judd-Ofelt theory in order to relax some strong selection rules and approximations of the standard formalism and to better account for the influence of the 4f5d excited electronic configuration. The demonstration is made by re-examining the case of Pr3+:YAG, a well known luminescent and laser crystal with a very low energy 4f5d absorption band. Our extension thus provides a better agreement between calculated and measured absorption intensities, especially for the hypersensitive 3 H4 $\rightarrow$ 3 P2 transition. A comparison is made with the results obtained in the case of Pr3+:ZBLAN, a laser fluoride glass with much higher 4f5d absorption levels. Our investigation also gives the opportunity, in the case of Pr3+:YAG, to provide more complete and more reliable absorption and emission data than reported in the past literature and to exploit these data to better address the question of laser operation at various emission wavelengths. It is thus demonstrated that laser operation should be possible with improved laser performance at 488 nm, 616 nm and 744 nm, as it was already achieved in the past, but also at 566 nm and 931 nm by using appropriate laser cavities and laser mirrors.

physics.atom-ph

Determination of the ground state polarizability of $^{162}$Dy near 530 nm

Open-shell lanthanide atoms, and dysprosium in particular, combine a large ground-state angular momentum with dense electronic spectra, making their dynamical polarizability strongly dependent on wavelength and internal state and therefore particularly challenging to characterize accurately. This issue has become especially relevant with the recent development of single-atom trapping of dysprosium in optical-tweezer arrays, where precise knowledge of the polarizability is needed to design optimized trapping architectures. Here, we exploit the strong spin-dependent light shift near the $J'=J-1$ intercombination line at 530.306 nm to determine the background scalar and vector polarizabilities of $^{162}$Dy in its ground state near this wavelength. Our measurements quantitatively agree with atomic-structure calculations and provide new insight into the contributions of nearby transitions in a spectral region relevant to emerging dysprosium tweezer platforms.

cond-mat.quant-gas

Two-photon-assisted collisions in ultracold gases of polar molecules II : Optical shielding of ultracold polar molecular collisions

We theoretically investigate the collisions between ultracold polar molecules in the presence of two lasers ensuring a Raman resonant transition on individual molecules to suppress photon scattering, taking the example of bosonic $^{23}$Na$^{39}$K molecules. By varying laser detunings and intensities, we enable a repulsive long-range interaction potential between molecules. After solving a set of coupled Schr\"odinger equations with the Hamiltonian written in the basis of laser-dressed states of the molecule pair at infinite distance, we identify quasi-resonant conditions under which elastic collisions are favored over inelastic and reactive ones, by a factor of about 2, thus demonstrating a promising pathway for efficient two-photon optical shielding of ultracold molecular collisions. The results are analyzed in terms of scattering length of the colliding laser-dressed molecules, which exhibit prominent resonances assigned to the interaction of the entrance channel with other specific channels, consistent with the existence of a quasi-bound level of the long-range molecular pair induced by the lasers.

cond-mat.quant-gas

Structure and interactions of atoms and diatomic molecules: from ultracold gases to doped solids

This is the manuscript of my "Habilitation \`a diriger des recherches", where I present the research work that I have done after my PhD, defended in 2009. The manuscript is divided in two parts. The first one is dedicated to atomic-structure calculations with neutral and trivalent lanthanides, in the contexts of ultracold gases and rare-earth doped solids. The second part deals with long-range interactions in ultracold gases of alkali-metal atoms and diatomic molecules, as well as lanthanide atoms. The detailed description of long-range interactions serves to characterize ultralow-temperature phenomena, like photoassociation and collisional shielding.

cond-mat.quant-gas

Two-photon-assisted collisions in ultracold gases of polar molecules

We present a theoretical formalism to treat the ultracold dynamics of a pair of colliding polar molecules submitted to two laser fields. We express the dressed Hamiltonian including the dipole-dipole interaction of the colliding molecular pair, both in their ground and electronic excited states, as well as their interaction with the two laser fields. We apply adiabatic elimination of the electronic excited state to reduce the size of the dressed-state basis in which the dressed Hamiltoninan is expressed. In an application, we investigate the feasibility of two-photon collisional shielding between two \NaK molecules, which could be favored by the Raman resonance condition suppressing unwanted spontaneous emission and photon scattering. We demonstrate the influence of the laser Rabi frequencies on the dynamics through the computation of elastic, inelastic, and reactive collision rates.

cond-mat.quant-gas

Anisotropic polarizability of Dy at 532 nm on the intercombination transition

We report experimental measurements of the dynamical polarizability of dysprosium, at a wavelength of 532 nm. We measure all three components (scalar, vector, tensor) of the anisotropic polarizability for the ground and the excited manifolds of the intercombination transition of Dy at 626 nm. The apparatus on which the measurements are performed is first presented. We obtain with this setup imaging of single Dy atoms with fidelity above 99 % and losses below 2.5 % induced by imaging. We then describe the methods used to extract the polarizability. In particular, we combine a measurement of trap frequency and trap depth on single atoms in optical tweezers, allowing us to obtain a measurement of the ground state polarizability free of errors in trap waist calibration. The obtained values give a magic condition between two Zeeman states in the ground and excited manifolds, which was used to image single atoms in optical tweezer arrays. The scalar polarizability of the ground state is in disagreement with theoretical expectations, calling for future investigations to resolve the discrepancy.

physics.atom-ph

Van der Waals coefficients for interactions of dysprosium and erbium atoms with alkali-metal and alkaline-earth-metal atoms

The long-range part of the interatomic interactions plays a substantial role in the collisional dynamics of ultracold gases. Here, we report on the calculation of the isotropic and anisotropic $C_6$ coefficients characterizing the van der Waals interaction between dysprosium or erbium atoms in the two lowest energy levels and the ground-state alkali-metal (Li, Na, K, Rb, Cs, Fr) or alkaline-earth-metal (Be, Mg, Ca, Sr, Ba) atoms. The calculations are done using the integral of dynamic dipole polarizabilities at so-called imaginary frequencies of the two interacting atoms. For all atom pairs, we find that the isotropic $C_6$ coefficients are two or three orders of magnitude larger than the anisotropic ones. Those coefficients are essential for modeling collisional properties of heteronuclear quantum mixtures containing highly magnetic dysprosium or erbium atoms and alkali-metal or alkaline-earth-metal atoms.

physics.atom-ph

Extension of Judd-Ofelt theory: Application on Eu$^{3+}$, Nd$^{3+}$ and Er$^{3+}$

We present a modified version of the Judd-Ofelt theory, which describes the intensities of f-f transitions for trivalent lanthanide ions (Ln$^{3+}$) in solids. In our model, the properties of the dopant are calculated with well-established atomic-structure techniques, while the influence of the crystal-field potential is described as a perturbation, by three adjustable parameters. Compared to our previous work [G. Hovhannesyan \textit{et al.}, J. Lumin. \textbf{241}, 118456 (2022)], the spin-orbit interaction within the first excited configuration 4f$^{w-1}$5d is described in a perturbative way, whereas it is exactly taken into account in the ground configuration 4f$^w$, using all the eigenvector components of the free-ion levels. Moreover, the wavelength-dependence of the refractive index of the host material is also accounted for. We test the validity of our model on three ions: Eu$^{3+}$, Nd$^{3+}$ and Er$^{3+}$. The results of the extension are satisfactory, we are able to give a physical insight into all the transitions within the ground electronic configuration, and also to reproduce quantitatively experimental absorption oscillator strengths. We also performed calculations of standard JO parameters, and the results are in good agreement with the values reported in the literature. The code used to make the calculations is available on GitLab.

physics.atom-ph

Improving the spectroscopic knowledge of neutral Neodymium

Laser cooling and trapping of lanthanides has opened the possibility to carry out new experiments with ultracold dipolar gases, for example for quantum simulation of solid state physics. To identify new suitable candidates for laser-cooling, it is important to have a precise spectroscopic knowledge of the atom under consideration. Along this direction, we present here a detailed modeling of the energy levels of neutral neodymium (Nd), an element belonging to the left part of the lanthanide row, which has not yet been considered for laser-cooling. Using the semi-empirical method implemented in the Cowan suite of codes, we are in particular able to interpret more than 200 experimental levels of the NIST database belonging to both parities. The optimal set of atomic parameters obtained after the least-square fitting step can serve to calculate radiative transition probabilities in the future.

physics.atom-ph

FitAik: a package to calculate least-square fitted atomic transitions probabilities. Application to the Er+ lanthanide ion

We present a new method implemented in our new package \textit{FitAik}, to perform least-squares fitting of calculated and experimental atomic transition probabilities, by using the mono-electronic transition integrals $\langle n\ell |r| n'\ell' \rangle$ (with $r$ the electronic radial coordinate) as adjustable quantities. \textit{FitAik} is interfaced to the Cowan suite of codes, for which it automatically writes input files and reads output files. We illustrate our procedure with the example of Er$^{+}$ ion, for which the agreement between calculated and experimental Einstein coefficients is found to be very good. The source code of \emph{FitAik} can be found on GitLab, and the calculated Einstein coefficients are stored in our new database CaDDiACs. They are also used to calculate the dynamic dipole polarizability of Er$^+$.

physics.atom-ph

Two-photon optical shielding of collisions between ultracold polar molecules

We propose a method to engineer repulsive long-range interactions between ultracold ground-state molecules using optical fields, thus preventing short-range collisional losses. It maps the microwave coupling recently used for collisional shielding onto a two-photon transition, and takes advantage of optical control techniques. In contrast to one-photon optical shielding [Phys. Rev. Lett. 125, 153202 (2020)], this scheme avoids heating of the molecular gas due to photon scattering. The proposed protocol, exemplified for 23Na39K, should be applicable to a large class of polar diatomic molecules.

quant-ph

Transition intensities of trivalent lanthanide ions in solids: Revisiting the Judd-Ofelt theory

We present a modified version of the Judd-Ofelt theory, which describes the intensities of f-f transitions by trivalent lanthanide ions (Ln$^{3+}$) in solids. In our model, the properties of the dopant are calculated with well-established atomic-structure techniques, while the influence of the crystal-field potential is described by three adjustable parameters. By applying our model to europium (Eu$^{3+}$), well-known to challenge the standard Judd-Ofelt theory, we are able to give a physical insight into all the transitions within the ground electronic configuration, and also to reproduce quantitatively experimental absorption oscillator strengths. Our model opens the possibility to interpret polarized-light transitions between individual levels of the ion-crystal system.

cond-mat.mtrl-sci

Purely long-range polar molecules composed of identical lanthanide atoms

Doubly polar molecules, possessing an electric dipole moment and a magnetic dipole moment, can strongly couple to both an external electric field and a magnetic field, providing unique opportunities to exert full control of the system quantum state at ultracold temperatures. We propose a method for creating a purely long-range doubly polar homonuclear molecule from a pair of strongly magnetic lanthanide atoms, one atom being in its ground level and the other in a superposition of quasi-degenerate opposite-parity excited levels [Phys.~Rev.~Lett.~\textbf{121}, 063201 (2018)]. The electric dipole moment is induced by coupling the excited levels with an external electric field. We derive the general expression of the long-range, Stark, and Zeeman interaction energies in the properly symmetrized and fully-coupled basis describing the diatomic complex. Taking the example of holmium, our calculations predict shallow long-range wells in the potential energy curves that may support vibrational levels accessible by direct photoassociation from pairs of ground-level atoms.

physics.atom-ph

Quantum mechanical study of the high-temperature $\mathrm{H}^+ + \mathrm{HD} \to \mathrm{D}^+ + \mathrm{H}_2$ reaction for the primordial universe chemistry

We use the time-independent quantum-mechanical formulation of reactive collisions in order to investigate the state-to-state $\mathrm{H}^+ + \mathrm{HD} \to \mathrm{D}^+ + \mathrm{H}_2$ chemical reaction. We compute cross sections for collision energies up to 1.8 electron-volts and rate coefficients for temperatures up to 10000 kelvin. We consider HD in the lowest vibrational level $v=0$ and rotational levels $j=0$ to 4, and H$_2$ in vibrational levels $v'=0$ to 3 and rotational levels $j'=0$ to 9. For temperatures below 4000 kelvin, the rate coefficients strongly vary with the initial rotational level $j$, depending on whether the reaction is endothermic ($j\le 2$) or exothermic ($j\ge 3$). The reaction is also found less and less probable as the final vibrational quantum number $v'$ increases. Our results illustrate the importance of studying state-to-state reactions, in the context of the chemistry of the primordial universe.

astro-ph.CO

Anisotropic light-shift and magic-polarization of the intercombination line of Dysprosium atoms in a far-detuned dipole trap

We characterize the anisotropic differential ac-Stark shift for the Dy $626$ nm intercombination transition, induced in a far-detuned $1070$ nm optical dipole trap, and observe the existence of a "magic polarization" for which the polarizabilities of the ground and excited states are equal. From our measurements we extract both the scalar and tensorial components of the dynamic dipole polarizability for the excited state, $α_E^\text{s} = 188 (12)\,α_\text{0}$ and $α_E^\text{t} = 34 (12)\,α_\text{0}$, respectively, where $α_\text{0}$ is the atomic unit for the electric polarizability. We also provide a theoretical model allowing us to predict the excited state polarizability and find qualitative agreement with our observations. Furthermore, we utilize our findings to optimize the efficiency of Doppler cooling of a trapped gas, by controlling the sign and magnitude of the inhomogeneous broadening of the optical transition. The resulting initial gain of the collisional rate allows us, after forced evaporation cooling, to produce a quasi-pure Bose-Einstein condensate of $^{162}$Dy with $3\times 10^4$ atoms.

cond-mat.quant-gas

Ultracold rare-earth magnetic atoms with an electric dipole moment

We propose a new method to produce an electric and magnetic dipolar gas of ultracold dysprosium atoms. The pair of nearly degenerate energy levels of opposite parity, at 17513.33 cm$^{-1}$ with electronic angular momentum $J=10$, and at 17514.50 cm$^{-1}$ with $J=9$, can be mixed with an external electric field, thus inducing an electric dipole moment in the laboratory frame. For field amplitudes relevant to current-day experiments, we predict a magnetic dipole moment up to 13 Bohr magnetons, and an electric dipole moment up to 0.22 Debye, which is similar to the values obtained for alkali-metal diatomics. When a magnetic field is present, we show that the electric dipole moment is strongly dependent on the angle between the fields. The lifetime of the field-mixed levels is found in the millisecond range, thus allowing for suitable experimental detection and manipulation.

physics.atom-ph

Anisotropic polarizability of erbium atoms

We report on the determination of the dynamical polarizability of ultracold erbium atoms in the ground and in one excited state at three different wavelengths, which are particularly relevant for optical trapping. Our study combines experimental measurements of the light shift and theoretical calculations. In particular, our experimental approach allows us to isolate the different contributions to the polarizability, namely the isotropic scalar and anisotropic tensor part. For the latter contribution, we observe a clear dependence of the atomic polarizability on the angle between the laser-field-polarization axis and the quantization axis, set by the external magnetic field. Such an angle-dependence is particularly pronounced in the excited-state polarizability. We compare our experimental findings with the theoretical values, based on semi-empirical electronic-structure calculations and we observe a very good overall agreement. Our results pave the way to exploit the anisotropy of the tensor polarizability for spin-selective preparation and manipulation.

cond-mat.quant-gas

Anisotropic optical trapping as a manifestation of the complex electronic structure of ultracold lanthanide atoms: the example of holmium

The efficiency of optical trapping is determined by the atomic dynamic dipole polarizability, whose real and imaginary parts are associated with the potential energy and photon-scattering rate respectively. In this article we develop a formalism to calculate analytically the real and imaginary parts of the scalar, vector and tensor polarizabilities of lanthanide atoms. We assume that the sum-over-state formula only comprises transitions involving electrons in the valence orbitals like $6s$, $5d$, $6p$ or $7s$, while transitions involving $4f$ core electrons are neglected. Applying this formalism to the ground level of configuration $4f^q6s^2$, we restrict the sum to transitions implying the $4f^q6s6p$ configuration, which yields polarizabilities depending on two parameters: an effective transition energy and an effective transition dipole moment. Then, by introducing configuration-interaction mixing between $4f^q6s6p$ and other configurations, we demonstrate that the imaginary part of the scalar, vector and tensor polarizabilities is very sensitive to configuration-interaction coefficients, whereas the real part is not. The magnitude and anisotropy of the photon-scattering rate is thus strongly related to the details of the atomic electronic structure. Those analytical results agree with our detailed electronic-structure calculations of energy levels, Landé $g$-factors, transition probabilities, polarizabilities and van der Waals $C_6$ coefficients, previously performed on erbium and dysprosium, and presently performed on holmium. Our results show that, although the density of states decreases with increasing $q$, the configuration interaction between $4f^q6s6p$, $4f^{q-1}5d6s^2$ and $4f^{q-1}5d^26s$ is surprisingly stronger in erbium ($q=12$), than in holmium ($q=11$), itself stronger than in dysprosium ($q=10$).

physics.atom-ph