Permanent Electric Dipole Research Articles

Hydrogenated Silicon Nanoclusters with a Permanent Electric Dipole Moment for the Controlled Assembly of Silicon-Based Nanostructures

Centre National de la Recherche Scientifique (Innovation Prematuration 2020 program); Hariri Foundation for Sustainable Human Development (Scholarship)

Van der Waals molecules consisting of a zinc or cadmium atom interacting with an alkali-metal or alkaline-earth-metal atom

Alkaline-earth-like transition-metal atoms such as Zn and Cd are promising candidates for precision measurements and quantum many-body physics experiments. Here, we theoretically investigate the properties of diatomic molecules containing these closed-shell atoms. We calculate potential energy curves, permanent electric dipole moments, and spectroscopic constants for molecules consisting of either a Zn or Cd atom interacting with an alkali-metal (Li, Na, K, Rb, Cs, Fr) or alkaline-earth-metal (Be, Mg, Ca, Sr, Ba, Ra) atom. We use the ab initio electronic structure coupled cluster method with single, double, and triple excitations combined with large Gaussian basis sets and small-core relativistic energy-consistent pseudopotentials for heavier atoms. We predict that the studied molecules in the ground electronic state are chemically reactive weakly bound van der Waals complexes with small permanent electric dipole moments. The present results may be useful for spectroscopy and application of the studied molecules in modern ultracold physics and chemistry experiments.

Electric field induced tuning of electronic correlation in weakly confining quantum dots

We conduct a combined experimental and theoretical study of the quantum-confined Stark effect in GaAs/AlGaAs quantum dots obtained with the local droplet etching method. In the experiment, we probe the permanent electric dipole and polarizability of neutral and positively charged excitons weakly confined in GaAs quantum dots by measuring their light emission under the influence of a variable electric field applied along the growth direction. Calculations based on the configuration-interaction method show excellent quantitative agreement with the experiment and allow us to elucidate the role of Coulomb interactions among the confined particles and -- even more importantly -- of electronic correlation effects on the Stark shifts. Moreover, we show how the electric field alters properties such as built-in dipole, binding energy, and heavy-light hole mixing of multiparticle complexes in weakly confining systems, underlining the deficiencies of commonly used models for the quantum-confined Stark effect.

Investigation of the Stark Effect on a Centrosymmetric Quantum Emitter in Diamond.

Quantum emitters in diamond are leading optically accessible solid-state qubits. Among these, Group IV-vacancy defect centers have attracted great interest as coherent and stable optical interfaces to long-lived spin states. Theory indicates that their inversion symmetry provides first-order insensitivity to stray electric fields, a common limitation for optical coherence in any host material. Here we experimentally quantify this electric field dependence via an external electric field applied to individual tin-vacancy (SnV) centers in diamond. These measurements reveal that the permanent electric dipole moment and polarizability are at least 4 orders of magnitude smaller than for the diamond nitrogen vacancy (NV) centers, representing the first direct measurement of the inversion symmetry protection of a Group IV defect in diamond. Moreover, we show that by modulating the electric-field-induced dipole we can use the SnV as a nanoscale probe of local electric field noise, and we employ this technique to highlight the effect of spectral diffusion on the SnV.

Two-dimensional beam profile monitor for the detection of alpha-emitting radioactive isotope beam

Ions with similar charge-to-mass ratios cannot be separated from existing beam profile monitors (BPMs) in nuclear facilities in which low-energy radioactive ions are produced due to nuclear fusion reactions. In this study, we developed a BPM using a microchannel plate and a charge-coupled device to differentiate the beam profiles of alpha-decaying radioactive isotopes from other ions (reaction products) produced in a nuclear reaction. This BPM was employed to optimize the low-energy radioactive francium ion (Fr+) beam developed at the Cyclotron and Radioisotope Center (CYRIC), Tohoku University, for electron permanent electric dipole moment (e-EDM) search experiments using Fr atoms. We demonstrated the performance of the BPM by separating the Fr+ beam from other reaction products produced during the nuclear fusion reaction of an oxygen (18O) beam and gold (197Au) target. However, as the mass of Au is close to that of Fr, separating the ions of these elements using a mass filter is a challenge, and a dominant number of Au+ renders the Fr+ beam profile invisible when using a typical BPM. Therefore, by employing the new BPM, we could successfully observe the Fr+ beam and other ion beams distinctly by measuring the alpha decay of Fr isotopes. This novel technique to monitor the alpha-emitting radioactive beam covers a broad range of lifetimes, for example, from approximately 1 s to 10 min, and can be implemented for other alpha-emitter beams utilized for medical applications.

The search for the neutron electric dipole moment at PSI

The existence of a nonzero permanent electric dipole moment (EDM) of the neutron would reveal a new source of CP violation and shed light on the origin of the matter–antimatter asymmetry of the Universe. The sensitivity of current experiments using stored ultracold neutrons (UCN) probe new physics beyond the TeV scale. Using the UCN source at the Paul Scherrer Institut, the nEDM collaboration has performed the most sensitive measurement of the neutron EDM to date, still compatible with zero (|d_n|<1.8\times 10^{-26} \, e {cm}|dn|<1.8×10−26ecm, C.L.,90%). A new experiment designed to improve the sensitivity by an order of magnitude, n2EDM, is currently under construction.

FCI calculations of the adiabatic electronic structure of KRb highlighting the K−Rb+ ionic limit effect

A non-relativistic description of the electronic structure for the heteronuclear molecule KRb was developed through the Full Configuration Interaction (FCI) and pseudo-potential method. Below the ionic limit K−Rb+, the ground and all excited singlet and triplet states of different symmetries Σ+, Π and Δ (in the Hund's case (a): 2s + 1Λ±) were intensively investigated. Several adiabatic results including potential energy curves (PECs), permanent and transition electric dipole moments (PEDM, TEDM) were analyzed in short and long-range of internuclear distances. Tables of these properties as functions of separation are presented. The spectroscopic constants with the vibrational levels were derived using the “Numerov” algorithm. These molecular parameters were compared with those published in the literature, feature a good agreement. In the adiabatic representation, strong couplings between successive 1Σ+ states were reached by series of avoided crossing, yielding to the appearance of the ionic character and the good illustration of charge transfer. This description of the KRb molecule was helpful in the design of the prospect photo-association experiments and the obtaining of the quantum-degenerate gas of the polar molecule.

Ab initio calculations of electric dipole moments of light nuclei

In any finite system, the presence of a non-zero permanent electric dipole moment (EDM) would indicate CP violation beyond the small violation predicted in the Standard Model. Here, we use the ab initio no-core shell model (NCSM) framework to theoretically investigate the magnitude of the nuclear EDM. We calculate EDMs of several light nuclei using chiral two- and three-body interactions and a PT-violating Hamiltonian based on a one-meson-exchange model. We present a benchmark calculation for $^3$He, as well as results for the more complex nuclei $^{6,7}$Li, $^9$Be, $^{10,11}$B, $^{13}$C, $^{14,15}$N, and $^{19}$F. Our results suggest that different nuclei can be used to probe different terms of the PT violating interaction. These calculations allow us to suggest which nuclei may be good candidates in the search for a measurable permanent electric dipole moment.

Interaction potentials, electric moments, polarizabilities, and chemical reactions of YbCu, YbAg, and YbAu molecules

Ultracold YbAg molecules have been recently proposed as promising candidates for electron electric dipole moment searches Verma et al (2020 Phys. Rev. Lett. 125 153201). Here, we calculate potential energy curves, permanent electric dipole and quadrupole moments, and static electric dipole polarizabilities for the YbCu, YbAg, and YbAu molecules in their ground electronic states. We use the coupled cluster method restricted to single, double, and noniterative triple excitations with large Gaussian basis sets, while the scalar relativistic effects are included within the small-core energy-consistent pseudopotentials. We find that the studied molecules are relatively strongly bound with the well depths of 5708 cm−1, 5253 cm−1, and 13349 cm−1 and equilibrium distances of 5.50 bohr, 5.79 bohr, and 5.55 bohr for YbCu, YbAg, and YbAu, respectively. They have large permanent electric dipole moments of 3.2D, 3.3D, and 5.3D at equilibrium distances, respectively. We also calculate equilibrium geometries and energies of corresponding trimers. The studied molecules are chemically reactive unless they are segregated in an optical lattice or shielded with external fields. The investigated molecules may find application in ultracold controlled chemistry, dipolar many-body physics, or precision measurement experiments.

Beyond the Rabi model: Light interactions with polar atomic systems in a cavity

The Rabi Hamiltonian, describing the interaction between a two-level atomic system and a single-cavity mode of the electromagnetic field, is one of the fundamental models in quantum optics. The model becomes exactly solvable by considering an atom without permanent dipole moments, whose excitation energy is quasiresonant with the cavity photon energy, and by neglecting the nonresonant (counter-rotating) terms. In this case, after including the decay of either the atom or the cavity mode to a continuum, one can derive the well-known phenomenology of quasiresonant transitions, including the fluorescence triplets. In this work we consider the most general Rabi model, incorporating the effects of permanent atomic electric dipole moments. Based on a perturbative analysis, we compare the intensities of emission lines induced by rotating terms, counter-rotating terms, and parity-symmetry-breaking terms in order to identify the parameter regimes in which these different contributions play a significant role. The analysis reveals that the emission strength related to the existence of permanent dipoles may surpass the one due to the counter-rotating interaction terms but is usually much weaker than the emission due to the main, resonant coupling. This ratio can be modified in systems with a reduced dimensionality or by engineering the energy spectral density of the continuum.

Anionic dependency of electronic and nonlinear optical properties of ionic liquids

Nonlinear optical phenomena play significant roles in the bulk properties and responsive characteristics of ionic liquids, especially when used under strong electric fields. The variability of the anion-cation pair in ionic liquids makes them designer solvents; thus, the anion or cation dependency of the physicochemical properties should be understood in depth. Accordingly, the electric field-induced characteristics of eight ionic liquids with [Br]−, [BF4]−, [PF6]−, [Ac]−, [TFAc]−, [MS]−, [NTf2]−, and [Tos]− anions paired with the 1-butyl-3-methyl imidazolium cation were investigated using density functional theory modeling at four theoretical levels: B3LYP-6-31G(d), M06-2X 6-31G(d), M06-2X 6-311++G(d,p), and M06-2X aug-cc-PVTZ. The frontier molecular orbitals, electrostatic potential surface, and electron density difference maps were obtained to visualize the electrostatic characteristics. The permanent electric dipole moment, linear electric polarizability, and first-order and second-order hyperpolarizabilities were also determined. While the static dipole moment and dipole polarizabilities could be obtained using low-level quantum chemistry at a satisfactory level, the functionalization of more intensive methods was required to accurately obtain the nonlinear optical properties.

Fabrication and dielectric performance of RGO-PANI reinforced PVDF/BaTiO3 composite for energy harvesting

Today’s techno savvy world demands smart devices which are light-weight, flexible, and scalable. Functional polymers and their composites are suitable candidates that can fulfill the requirements in flexible device applications. Polyvinylidene fluoride (PVDF) is one kind of functional polymers possessing a large dielectric strength as well as permanent electrical dipole. To improve the dielectric and ferroelectric performance of the PVDF polymer, it can be hybridized with an inorganic/organic inclusion phase, usually ferroelectric ceramic particles or nano-sized low dimensional carbon. In this work, reduced- graphene oxide (RGO) and RGO-PANI were chosen as the inclusion phase (filler). The present work focuses towards enhancing the dielectric and ferroelectric properties of PVDF-BaTiO3 (P/BT) nanocomposites impregnated with RGO and RGO/PANI(Polyaniline) nanofillers. In-situ polymerization method was adapted to fabricate the RGO/PANI nanocomposite and spin coating method for P/BT composites. X-ray diffractograms and FTIR corroborate the presence of ferroelectric phases in P/BT matrix. Wayne Kerr precision impedance analyzer was used in the frequency frame of 1 Hz to 1 MHz and temperature window from 30 °C to 160 °C to study the dielectric properties. The P-E hysteresis loops were obtained using Radiant Ferroelectric Tester at different voltage cycles. The dielectric constant of P/BT matrix with 0.03% RGO loading exhibited the highest dielectric constant 2 × 105. Remarkable increase in the energy density of composites with filler loading was observed. P/BT with 1 wt% loading of RGO-PANI achieved the maximum value of polarization 3.6 µC/cm2 and discharge energy density 0.76 J/cm3 (under the electric field of 170 kV/cm) with 55% efficiency. This contribution provides a potential route to design and fabricate high energy density flexible capacitor for microelectronic devices.

Rotational Dynamics of an Amphidynamic Zirconium Metal-Organic Framework Determined by Dielectric Spectroscopy.

A zirconium metal-organic framework with a difluorophenylene rotator bearing a permanent electric dipole of ∼3.2 D was synthesized, and its rotational motion was analyzed by temperature- and frequency-dependent broadband dielectric spectroscopy. While solid-state NMR confirms fast rotation qualitatively, the dissipation factors measured between 113 and 153 K suggested an activation energy Ea = 2.6 kcal/mol, but deviations from a single Debye relaxation suggested a dynamic process that cannot be accounted for by a well-defined potential with a single activation barrier. The dynamic heterogeneity of the dipolar rotor was confirmed by analysis in terms of a Cole-Cole relaxation, which suggested a mean barrier of ∼1.9 kcal/mol, with a heterogeneity that decreases as temperature increases. Based on the single-crystal structure, we propose that the kinetic heterogeneity results from a temperature-dependent potential where rotation motion is mediated by the escape of the rotator from an energy well created by a double Ph-H···F-Ph hydrogen bond.

Ab initio investigation of ground and excited states of ScH molecule

The theoretical study of the electronic structure of Scandium Hydride ScH has been carried out using ab-initio methods. By employing (MRCI-SD/SA-CASSCF) and by using basis sets involving contribution of all electrons of both Scandium and Hydrogen atoms, 18 singlet and 15 triplet low-lying electronic states have been calculated below 28803 cm−1. Potential energy curves have been plotted and the term values at equilibrium Te, the vibrational constants ωe and ωeχe of ScH electronic states have been fitted. In addition, we calculated the permanent electric dipole moments for all these predicted states, the transition dipole moments TDMs within states at a range of internuclear distance around the equilibrium, the vibronic intensities FCF and the radiative lifetime. The calculated spectroscopic constants are in excellent consistency with the available experimental results and with other previous theoretical works. These calculations also predicted many excited states unobserved experimentally. The observed perturbations in D1Π and C1Σ+ have been investigated in this work.

Evidence of ideal excitonic insulator in bulk MoS2 under pressure

Spontaneous condensation of excitons is a long-sought phenomenon analogous to the condensation of Cooper pairs in a superconductor. It is expected to occur in a semiconductor at thermodynamic equilibrium if the binding energy of the excitons-electron (e) and hole (h) pairs interacting by Coulomb force-overcomes the band gap, giving rise to a new phase: the "excitonic insulator" (EI). Transition metal dichalcogenides are excellent candidates for the EI realization because of reduced Coulomb screening, and indeed a structural phase transition was observed in few-layer systems. However, previous work could not disentangle to which extent the origin of the transition was in the formation of bound excitons or in the softening of a phonon. Here we focus on bulk [Formula: see text] and demonstrate theoretically that at high pressure it is prone to the condensation of genuine excitons of finite momentum, whereas the phonon dispersion remains regular. Starting from first-principles many-body perturbation theory, we also predict that the self-consistent electronic charge density of the EI sustains an out-of-plane permanent electric dipole moment with an antiferroelectric texture in the layer plane: At the onset of the EI phase, those optical phonons that share the exciton momentum provide a unique Raman fingerprint for the EI formation. Finally, we identify such fingerprint in a Raman feature that was previously observed experimentally, thus providing direct spectroscopic confirmation of an ideal excitonic insulator phase in bulk [Formula: see text] above 30 GPa.

Highly efficient electromagnetic absorption on ZnN4-based MOFs-derived carbon composites

Rapid expansion in microelectronic devices has accelerated considerable attention on the development of high-performance electromagnetic wave absorption materials. We herein reported a nitrogen-anchored Zn single atom microwave absorber derived from zeolitic imidazolate frameworks with high Zn–N4 content (18.4%) and defect concentration (2.43 × 1011 cm−2), thus featuring with remarkable dielectric loss tangent ∼5.6. Theoretical calculations revealed that this significant enhancement was originated from the coordination structure of single zinc atoms localized within carbon matrix, associated with a high density of permanent electric dipoles that act as atomic-scale polarization sites under the alternating electromagnetic field. This work has important significance in understanding the physical origin of electromagnetic wave absorption for the MOFs and provides an alternative for designing the excellent electromagnetic wave absorption materials.

Highly polar molecules consisting of a copper or silver atom interacting with an alkali-metal or alkaline-earth-metal atom

We theoretically investigate the properties of highly polar diatomic molecules containing $^2S$-state transition-metal atoms. We calculate potential energy curves, permanent electric dipole moments, spectroscopic constants, and leading long-range dispersion-interaction coefficients for molecules consisting of either a Cu or Ag atom interacting with an alkali-metal (Li, Na, K, Rb, Cs, Fr) or alkaline-earth-metal (Be, Mg, Ca, Sr, Ba, Ra) atom. We use ab initio electronic structure methods, such as the coupled cluster and configuration interaction ones, with large Gaussian basis sets and small-core relativistic energy-consistent pseudopotentials. We predict that the studied molecules in the ground electronic state are strongly bound with highly polarized covalent or ionic bonds resulting in very large permanent electric dipole moments. We find that highly excited vibrational levels have maximal electric dipole moments, e.g., exceeding 13$\,$debye for CsAg and 6$\,$debye for BaAg. Results for Cu$_2$, Ag$_2$, and CuAg are also reported. The studied molecules may find application in ultracold dipolar many-body physics, controlled chemistry, or precision measurement experiments.

Ultralong-Range Rydberg Bimolecules.

We predict that ultralong-range Rydberg bimolecules form in collisions between polar molecules in cold and ultracold settings. The interaction of Λ-doublet nitric oxide (NO) with long-lived Rydberg NO(nf, ng) molecules forms ultralong-range Rydberg bimolecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bimolecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bimolecules. Considerable orientation of NO dipole can be achieved. The Rydberg molecules described here hold promise for studies of a special class of long-range bimolecular interactions.

Measurement of the permanent electric dipole moment of ultracold ground state 85Rb133Cs molecules by microwave coherent spectroscopy.

We demonstrate measurement of the permanent electric dipole moment (EDM) of 85Rb133Cs molecules in the absolute vibrational ground state by microwave (MW) coherent spectroscopy. The rotational states of the considered molecules, which are formed from short-range photoassociation of mixed cold atoms, are nondegenerated under external electric field. To measure the EDM based on electric-field-induced shifts of the sublevels of X1Σ+(v = 0, J = 1) rotational state, we utilized a MW coherent spectroscopy, which has a higher resolution than depletion spectroscopy and one-photon MW spectroscopy and can also eliminate the influence from Stark shift of the excited state existing in both spectroscopies above. In order to acquire accurate electric intensity, electromagnetic induced transparency spectroscopy of 85Rb Rydberg atoms is used to implement the calibration. The permanent EDM of 85Rb133Cs molecules is finally determined to be 1.266(15) D, which agrees with the theoretical calculations and is comparable with the value of its isotopic molecule.

Ultra-cold long-range Rydberg-ground molecules

<sec> Ultra-cold long-range Rydberg-ground molecule consisting of a Rydberg atom and one or more ground-state atoms is formed by low-energy scattering between the Rydberg electron and ground-state atoms located inside the Rydberg electron’s wave function. The low-energy scattering interaction, initially investigated by Fermi and Omont, has been predicted to lead to molecular binding in a novel type of Rydberg molecules, including the trilobite and butterfly molecules. Their unconventional binding mechanism, which is unlike covalent, or ionic, or van der Waals bonds, results in loosely bound molecules with bond lengths on the order of thousands of Bohr radius. This kind of molecule with large size and huge permanent electric dipole moment is a good candidate for realizing the certain strongly correlated many-body gases and for quantum information processing, as well as for dipolar quantum gases and spin systems with long-range interactions. Consequently, these molecules have received considerable attention in recent years.</sec><sec>In this paper, we review the recent theoretical and experimental investigations of ultra-cold long-range Rydberg-ground molecules, including the scattering interaction between the Rydberg electron and ground-state atom and the resulting adiabatic potential curves, experimental observations of photo-associated Rydberg-ground molecules spectra, as well as the measurements of permanent electric dipole moment. Ultra-cold long-range Rydberg-ground molecules are prepared by photoassociation in a high-density cold atom sample. Therefore, the Rydberg electron can bind several ground-state atoms to form a polyatomic Rydberg-ground molecule. The permanent molecular electric-dipole moments are revealed by spectral line broadening in the electric fields. The latest research pointed out that the permanent electric dipole moments of the Cs <i>n</i>D<sub><i>J</i></sub> -type Rydberg-ground molecules are negative, which is different from the previous reports (the electric dipole moments are positive). The negative sign reflects a deficiency of Rydberg-electron density near the ground-state perturber, which is caused by electronic configuration mixing. </sec>