Fine-structure Manifold Research Articles

Exciton Fine Structure in 2D Perovskites: The Out‐of‐Plane Excitonic State

Abstract2D Ruddlesden‐Popper metal‐halide perovskites feature particularly strong excitonic effects, making them a fascinating playground for studying exciton physics. A complete understanding of the properties of this quasi‐particle is crucial to fully exploit the tremendous potential of 2D perovskites (2DP) in light emission applications. Despite intense investigations, some of the exciton properties remain elusive to date, for example, the energy‐ordering of the exciton states within the so‐called fine structure manifold. Using optical spectroscopy, it demonstrates that in the archetypical 2DP (PEA)2PbI4, in contradiction to theoretical predictions, the energy of the bright out‐of‐plane exciton state is higher than that of two in‐plane states. Having elucidated the order of exciton fine structure, it determines the g‐factor of the dark exciton transition, together with the values of the electron and hole g‐factors in the direction parallel to the c‐axis of the crystal. In this way, it provides for the first time, a complete picture of the exciton fine structure in (PEA)2PbI4 2DP.

High-accuracy optical clocks based on group-16-like highly charged ions

We identify laser-accessible transitions in group 16-like highly charged ions as candidates for high-accuracy optical clocks, including S-, Se-, and Te-like systems. For this class of ions, the ground $^{3}P_{J}$ fine structure manifold exhibits irregular (nonmonotonic in $J$) energy ordering for large enough ionization degree. We consider the $|^3P_2\rangle \longleftrightarrow |^3P_0\rangle$ (ground to first-excited state) electric quadrupole transition, performing relativistic many-body calculations of several atomic properties important for optical clock development. All ions discussed are suitable for production in small-scale ion sources and lend themselves to sympathetic cooling and quantum-logic readout with singly charged ions.

Dynamics of atomic spin-orbit-state wave packets produced by short-pulse laser photodetachment

We analyse the experiment by Hultgren et al. [Phys. Rev. A {\bf 87}, 031404 (2013)] on orbital alignment and quantum beats in coherently excited atomic fine-structure manifolds produced by short-pulse laser photodetachment of C$^-$, Si$^-$ and Ge$^-$ negative ions, and derive a formula that describes the beats. Analysis of the experimental data enables us to extract the non-coherent background contribution for each species, and indicates the need for a full density matrix treatment of the problem.

Anisotropy induced Feshbach resonances in mixture of

We theoretically explore the scattering properties in collisions between in the ground state and fermionic in the metastable state. Unlike the role of the electronic spin degree of freedom in collisions of two alkali-metal atoms, the orbital degrees of freedom from the p electron of the metastable atoms, which induce not only mixings between different partial waves but also couplings between channels in different fine-structure manifolds, introduce the anisotropic interactions for producing broad-enough Feshbach resonances. Our closed-coupling calculation shows that this mechanism is similar to that in highly magnetic atoms, but the resonances also suffer from a large inelastic rate at the magnitude of to lower-lying fine-structure states or Zeeman sublevels, which will be an obstacle for associating ultracold polar molecules with both electron spin and electric dipole momentum. However, such a rich mixture of inelastic processes, and the experimental advantage of immunity from intraspecies inelastic collisions for metastable fermionic allow for precise investigations on the interspecies scattering properties for systems with excited-state atoms included.

Few-body bound states of dipole-dipole-interacting Rydberg atoms

We show that the resonant dipole-dipole interaction can give rise to bound states between two and three Rydberg atoms with non-overlapping electron clouds. The dimer and trimer states arise from avoided level crossings between states converging to different fine structure manifolds in the limit of separated atoms. We analyze the angular dependence of the potential wells, characterize the quantum dynamics in these potentials and discuss methods for their production and detection. Typical distances between the atoms are of the order of several micrometers which can be resolved in state-of-the-art experiments. The potential depths and typical oscillation frequencies are about one order of magnitude larger as compared to the dimer and trimer states investigated in [PRA $\textbf{86}$ 031401(R) (2012)] and [PRL $\textbf{111}$ 233003 (2014)], respectively. We find that the dimer and trimer molecules can be aligned with respect to the axis of a weak electric field.

Sensitivity of rotational transitions in CH and CD to a possible variation of fundamental constants

The sensitivity of rotational transitions in CH and CD to a possible variation of fundamental constants has been investigated. Largely enhanced sensitivity coefficients are found for specific transitions which are due to accidental degeneracies between the different fine-structure manifolds. These degeneracies occur when the spin-orbit coupling constant is close to four times the rotational constant. CH and particularly CD match this condition closely. Unfortunately, an analysis of the transition strengths shows that the same condition that leads to an enhanced sensitivity suppresses the transition strength, making these transitions too weak to be of relevance for testing the variation of fundamental constants over cosmological time scales. We propose a test in CH based on the comparison between the rotational transitions between the e and f components of the Omega'=1/2,J=1/2 and Omega'=3/2,J=3/2 levels at 532 and 536 GHz and other rotational or Lambda-doublet transitions in CH involving the same absorbing ground levels. Such a test, to be performed by radioastronomy of highly redshifted objects, is robust against systematic effects.

Argon plasma modeling with detailed fine-structure cross sections

Our recently reported fully relativistic distorted-wave electron-impact cross sections from the ground and metastable states of argon to various excited fine-structure levels are incorporated in a collisional-radiative model to obtain the population densities for the 3p54s and 3p54p (1s and 2p) fine-structure manifolds for low temperature argon plasmas. Excitation cross sections from the two 3p54s J = 1 resonance levels, 1s2 and 1s4, to the higher lying 2p fine-structure manifold as well as for transitions among individual levels of the 1s and 2p manifolds are also calculated and included in the present model which were not fully considered in any earlier model. Our results for the population densities of the 1s and 2p levels show good agreement with recent measurements. The variation of population densities of all the 1s and 2p levels with electron temperature and density are presented. We have also calculated and compared the intensities for the 750.38 nm (2p1 → 1s2) and 696.54 nm (2p2 → 1s5) lines with recently reported experimental results. The present work suggests that the inclusion of a complete fine-structure description of the electronic processes occurring in the plasma is important for a collisional radiative model, which includes separate 1s and 2p levels.

Nuclear magnetic octupole moment and the hyperfine structure of the5D3/2,5/2states of theBa+ion

The hyperfine structure of the long-lived $5{D}_{3/2}$ and $5{D}_{5/2}$ levels of ${\text{Ba}}^{+}$ ion is analyzed. A procedure for extracting relatively unexplored nuclear magnetic moments $\ensuremath{\Omega}$ is presented. The relevant electronic matrix elements are computed in the framework of the ab initio relativistic many-body perturbation theory. Both the first- and the second-order (in the hyperfine interaction) corrections to the energy levels are analyzed. It is shown that a simultaneous measurement of the hyperfine structure of the entire $5{D}_{J}$ fine-structure manifold allows one to extract $\ensuremath{\Omega}$ without contamination from the second-order corrections. Measurements to the required accuracy should be possible with a single trapped barium ion using sensitive techniques already demonstrated in ${\text{Ba}}^{+}$ experiments.

Laser fluorescence study of the S( 1D) + CD 4 reaction: determination of the SD product internal state distribution

The dynamics of the S( 1D) + CD 4 → SD + CD 3 reaction has been studied in a photolysis-probe experiment. S( 1D) reagent was prepared by laser photolysis of CS 2, and the SD(X 2Π) product was detected by laser fluorescence excitation. The nascent rotational/fine-structure state distribution of the SD(X 2Π) product was determined. The experimentally determined rotational state distribution within each fine-structure manifold agrees well with the predictions of a statistical ‘prior’ distribution, while the F 1 to F 2 fine-structure branching ratio is higher than predicted statistically. The product state distribution is consistent with reaction through the formation and decay of an energized CD 3SD complex.

Determination of the internal state distribution of the SD product from the S(1D)+D2 reaction

The S(1D)+D2-->SD+D reaction has been studied through a photolysis-probe experiment in a cell. S(1D) reagent was prepared by 193 nm photolysis of CS2, and the SD(X 2Pi) product was detected by laser fluorescence excitation. The nascent rotational/fine-structure state distribution of the SD(X 2Pi) product was determined. This reaction, previously studied theoretically and in a crossed molecular beam experiment, is known to proceed through formation and decay of a long-lived collision complex involving the deep well in the H2S ground electronic state. The determined SD rotational state distribution in the v=0 vibrational level was found to be approximately statistical, with a small preference for formation of the F1 (Omega=3/2) fine-structure manifold over F2 (Omega=1/2). The branching into the Lambda doublet levels was also investigated, and essentially equal populations of levels of A' and A" symmetry were found. The present results are compared with previous investigations of this reaction and the analogous O(1D)+D2 reaction.

Control of the spin polarization of photoelectrons/photoions using short laser pulses

We present a generic pump-probe scheme to control spin polarization of photoelectrons/photoions by short laser pulses. By coherently exciting fine structure manifolds of a multi-valence-electron system by the pump laser, a superposition of fine structure states is created. Since each fine structure state can be further decomposed into a superposition of various spin states of valence electrons, each spin component evolves differently in time. This means that varying the time delay between the pump and probe lasers leads to the control of spin states. Specific theoretical results are presented for two-valence-electron atoms, in particular for Mg, which demonstrate that not only the degree of spin polarization but also its sign can be manipulated through time delay. Since the underline physics is rather general and transparent, the presented idea may be potentially applied to nanostructures such as quantum wells and quantum dots.

Properties of metastable alkaline-earth-metal atoms calculated using an accurate effective core potential

The first three electronically excited states in the alkaline-earth-metal atoms magnesium, calcium, and strontium comprise the (nsnp) triplet P^o_J (J=0,1,2) fine-structure manifold. All three states are metastable and are of interest for optical atomic clocks as well as for cold-collision physics. An efficient technique--based on a physically motivated potential that models the presence of the ionic core--is employed to solve the Schroedinger equation for the two-electron valence shell. In this way, radiative lifetimes, laser-induced clock shifts, and long-range interaction parameters are calculated for metastable Mg, Ca, and Sr.

Electron spin-polarized alkaline-earth ions produced by multiphoton ionization

We propose two realistic schemes for producing electron spin-polarized alkaline-earth ions. One of the schemes is based on one-photon resonant two-photon ionization via fine structure manifolds of triplet states, while the other is based on one-photon resonant one-photon ionization. For both schemes we find that the ionization must take place from a triplet state to produce spin-polarized photoions. Photoions produced from a singlet state are always unpolarized regardless of the laser polarization and a magnetic sublevel from which ionization takes place. We carry out specific analysis for both schemes with Sr atoms, and find 85%–90% and 66% polarizations for the former and the latter schemes, respectively, if the wavelengths and polarizations of lasers are judiciously chosen. In particular, if all the produced photoions are in the ground s state, we find an exact one-to-one correspondence between the spin-polarization of photoions and ejected photoelectrons.

Fine structure of neutral and charged excitons in self-assembled In(Ga)As/(Al)GaAs quantum dots

The fine structure of excitons is studied by magnetophotoluminescence spectroscopy of single self-assembled In(Ga)As/(Al)GaAs quantum dots. Both strength and orientation of the magnetic field are varied. In a combination with a detailed theoretical analysis, these studies allow us to develop a comprehensive picture of the exciton fine structure. Symmetry of the dot structures as well as its breaking cause characteristic features in the optical spectra, which are determined by the electron-hole exchange and the Zeeman interaction of the carriers. The symmetry breaking is either inherent to the dot due to geometry asymmetries, or it can be obtained by applying a magnetic field with an orientation different from the dot symmetry axis. From data on spin splitting and on polarization of the emission we can identify neutral as well as charged exciton complexes. For dots with weakly broken symmetry, the angular momentum of the neutral exciton is no longer a good quantum number and the exchange interaction lifts degeneracies within the fine-structure manifold. The symmetry can be restored by a magnetic field due to the comparatively strong Zeeman interactions of electron and hole. For dots with a strongly broken symmetry, bright and dark excitons undergo a strong hybridization, as evidenced by pronounced anticrossings when states within the manifold are brought into resonance. The fine structure can no longer be described within the frame developed for structures of higher dimensionality. In particular, the hybridization cannot be broken magnetically. For charged excitons, the exchange interaction vanishes, demonstrating that the exchange splitting of a neutral exciton can be switched off by injecting an additional carrier.

Band structure effects in ejection of Ni atoms in fine structure states.

Kinetic energy distributions of Ni atoms in six electronic fine structure states ejected from a single crystal Ni{001} surface due to bombardment with 5 keV ${\mathrm{Ar}}^{+}$ ions have been measured. These states arise from two different electronic configurations, $3{d}^{8}4{s}^{2}{a^{3}F_{4,3,2}}$ and $3{d}^{9}4{s}^{1}{a^{3}D_{3,2} or a^{1}D_{2}}$, which form three distinct fine structure manifolds within 0.422 eV of the $^{3}F_{4}$ ground state. We find that the band structure effects dominate leading to larger populations in the excited $^{3}D_{3,2}$ states than found for the ground state.

Analysis of the Fourier transform and diode laser spectra of the ν3 fundamental of PuF 6

A detailed analysis of the ν 3 band of PuF 6 is presented. The P, Q, and R branches of the fundamental transition and of several hot bands have been observed for a cooled gas sample of PuF 6 at very low pressure in a long path length cell. Both a Fourier transform spectrometer (resolution 6 × 10 −3 cm −1) and a diode laser (resolution 4 × 10 −4 cm −1) have been used. Wavenumbers of the rotational transitions, measured on the diode spectra, have led to accurate values for the band origin and the rotational line spacing constant. Octahedral fine-structure manifolds in the P and R branches, for low to moderate values of J, have yielded a value of the splitting parameter. However, in the high- J manifolds and throughout the entire Q branch, the fine structure deviates substantially from theory. These discrepancies are apparently the result of accidental resonances with rotational levels of one or two neighboring vibrational states.