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Physical Review

Symmetry Selection Rules of Electric-Dipole Transitions of Eu3+ and Sm2+ in Crystals: A Solid-State Infrared Quantum Counter-Amplifier

Francis K. Fong, Lawrence A. Vredevoe, Roger E. De Wames

Published Jun 10, 1968• 14 citations
Publisher

Abstract

A practical scheme for a 10-\ensuremath{\mu} infrared quantum counter-amplifier is proposed, where the infrared frequency is converted into an easily detectable optical frequency. Detailed analysis of the electric-dipole transitions within the $4{f}^{6}$ ground configuration of ${\mathrm{Eu}}^{3+}$ and ${\mathrm{Sm}}^{2+}$ ions in various symmetries reveals that these ions have selection rules in ${C}_{3h}$, ${D}_{3h}$, and ${D}_{3}$ symmetries which allow for significant amplification. This scheme could provide a means of detecting the 10-\ensuremath{\mu} photons generated by the C${\mathrm{O}}_{2}$ laser.

DOI
10.1103/physrev.170.412

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IRQC parameters for Er3+ occupying sites of C2v and C3v symmetry in CdF2

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Measurements have been made of the optical parameters relevant to the operation of the Er3+ infrared quantum counter (IRQC) proposed recently to detect 1.5-μm radiation. The CdF2:Er3+ crystals used for this purpose were prepared under specific conditions selected to provide different local site symmetries at the Er3+ ions. EPR measurements were employed to determine the site symmetries and the relative concentration of ions at the various sites. In particular, high concentrations of C2v sites were generated by double doping with NaF prior to crystalline growth [CdF2: (Er3+,Na+)], whereas C3v sites were generated preferentially by oxygen firing sodium-free crystals subsequent to growth [CdF2: (Er3+,O2−)]. Selective generation of these two sites permitted the unambiguous determination of their characteristic optical absorption, emission, and excitation spectra, as well as the lifetimes and radiative efficiencies of relevant excited states. In addition, double excitation using two ir sources simultaneously, was used to determine the cross section for transitions between the 4I13/2 and 4S3/2 excited states and the lifetime of the former state. The optical properties of the Er3+ ion were observed to be sensitive to the local environment associated with each site and, in particular, to the magnitude of the noncubic component of the crystalline field. Phase-lag measurements confirmed the successive-excitation model proposed to explain the conversion of 1.5-μm radiation to 540- or 660-nm radiation in the presence of an 840-nm pump. Cooperative-excitation processes, on the other hand, were observed to produce 660-nm emission when 790- or 970-nm pumps were employed. The dependence of the over-all IRQC quantum efficiency on pump flux and on the optical parameters of Er3+ is derived from solutions to the appropriate rate equations. The analysis indicates that the performance of the 1.5-μm Er:IRQC, utilizing an 840-nm pump, is nearly optimized for CdF2: (Er3+,O2−).

Journal of Applied Physics•Apr 1, 1973•9 citations
A practical scheme for a 10-\ensuremath{\mu} infrared quantum counter-amplifier is proposed, where the infrared frequency is converted into an easily detectable optical frequency. Detailed analysis of the electric-dipole transitions within the 4f64{f}^{6}4f6 ground configuration of Eu3+{\mathrm{Eu}}^{3+}Eu3+ and Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions in various symmetries reveals that these ions have selection rules in C3h{C}_{3h}C3h​, D3h{D}_{3h}D3h​, and D3{D}_{3}D3​ symmetries which allow for significant amplification. This scheme could provide a means of detecting the 10-\ensuremath{\mu} photons generated by the CO2{\mathrm{O}}_{2}O2​ laser.
A survey of the salts of the rare-earth series shows that anhydrous PrCl3 has energy levels and selection rules suitable for use in a solid state infrared quantum counter as proposed by Bloembergen [N. Bloembergen, Phys. Rev. Letters 2, 84 (1959)]. Two suitable schemes are proposed, one for detection at 2.33 μ and a second for detection at 104 μ. Consideration is given to isolation of the final detector from the pumping signal and a suitable experimental arrangement for unambiguously determining proper operation is shown.
We report measurements of discrete excitation-induced frequency shifts on the $^{7}F_{0}\ensuremath{\rightarrow}^{5}D_{0}$ transition of the Eu3+{\mathrm{Eu}}^{3+}Eu3+ center in $\mathrm{La}\mathrm{\text{:}}\mathrm{Lu}\mathrm{\text{:}}{\mathrm{EuCl}}_{3}\ifmmode\cdot\else\textperiodcentered\fi{}6{\mathrm{D}}_{2}\mathrm{O}$ resulting from the optical excitation of neighboring Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions. Shifts of up to $46.081\ifmmode\pm\else\textpm\fi{}0.005\text{ }\text{ }\mathrm{MHz}$ were observed. The magnitude of the interaction between neighboring ions was found to be significantly larger than expected from the electric dipole-dipole mechanism often observed in rare earth systems. We show that a large network of interacting and individually addressable centers can be created by lightly doping crystals otherwise stoichiometric in the optically active rare earth ion, and that this network could be used to implement a quantum processor with more than ten qubits.
Summary form only given. Although it is often assumed that all light-matter interactions at optical frequencies are mediated by electric dipole transitions, strong optical-frequency magnetic dipoles do exist. In fact, we see magnetic dipole emission every day from the many lanthanide ions (such as erbium, europium, and terbium) that help to illuminate everything from fluorescent lighting to telecom fiber amplifiers. Higher-order processes such as magnetic dipole and electric quadrupole transitions also play an important part in the light emission from transition metal ions and semiconductor quantum dots. Nevertheless, most applications have overlooked the device implications of these electric-dipole-forbidden transitions throughout the visible and near-infrared regime, and their contributions to many important emitters have not been fully characterized.In this presentation, we will experimentally characterize the "forbidden" transitions in a range of solid-state emitters and investigate their applications and implications for nanophotonics. We will examine the electric dipole approximation commonly used to describe light-matter interactions and discuss naturally occurring systems that exhibit higher-order magnetic dipole and electric quadrupole emission. We will illustrate how these nanoscale quantum transitions can provide both a new way to probe magnetic light-matter interactions and a new degree of design freedom for active electronic and photonic devices. Specifically, we will demonstrate how the different symmetries of multipolar transitions can be exploited to identify, quantify, and control light emission, even at sub-lifetime scales. Despite similar radiation patterns, magnetic and electric dipole emitters have different symmetries with respect to polarization and phase. Thus, in an inhomogeneous environment, we can tailor interference effects and the local density of optical states to selectively enhance either electric or magnetic dipole emission [1,2]. To examine the scope of such higher-order transitions, we will present quantum mechanical calculations that identify all the magnetic dipole and electric quadrupole emission lines in the trivalent lanthanide series in the visible to near-infrared spectrum [3]. Then, we will present an energyand momentum-resolved spectroscopy technique to directly quantify the electric and magnetic dipole contributions from any mixed transition. [4] Using energy-momentum spectroscopy, we will experimentally examine the higher order transitions in lanthanide ions [4,5], transition metal ions [6], and epitaxial quantum dots [7]. If time permits, we will then show how the symmetry differences between magnetic and electric dipoles can be used to address specific electronic states [6] and to dynamically tune emission spectra at sub-lifetime-scales [8].
Noise arising from strong laser pumping and 77-K internal phonon noise upconversion in the proposed supposedly noiseless 10-μ quantum counters using rare-earth-doped crystals is described. The discussions are specialized to the crystals states of the Eu3+ ion. It is shown that at the pump power (∼50 kW cm−2) necessary for background-limited 10-μ quantum counter upconversion detection at 77 K, all the three major processes of noise generation discussed are insignificant compared to the background thermal (300 K) radiation considered previously in arriving at realistic theoretical quantum efficiencies of the proposed 10-μ quantum counters.
Optical frequency magnetic dipole (MD) transitions follow different selection rules from those invoked by the coupling of light to the electric dipole (ED) moment giving valuable complementary spectral information about the system under investigation. However, MD interactions contribute to the optical spectrum by approximately two orders of magnitude less than the ED transitions, therefore remaining concealed in traditional optical spectroscopy. To allow the unperturbed direct detection of the magnetic-field-MD interactions a novel type of magneto-optical spectroscopy is proposed. To this end, spatial separation of the electric and the magnetic field (EF & MF) components of the light can be achieved by means of azimuthally polarised beams (APB) [1]. Under external focusing, the APB develops a doughnut-shaped intensity profile exhibiting a longitudinal MF component at the centre of the beam while the polarisation of the EF oscillates along the beam perimeter. Another way to discern between ED and MD transitions is through spectral selectivity. For example, Eu3+ ions exhibit a MD-allowed transition at 527.5 nm and an ED-allowed one at 532 nm [2].
Measurements have been made of the optical parameters relevant to the operation of the Er3+ infrared quantum counter (IRQC) proposed recently to detect 1.5-μm radiation. The CdF2:Er3+ crystals used for this purpose were prepared under specific conditions selected to provide different local site symmetries at the Er3+ ions. EPR measurements were employed to determine the site symmetries and the relative concentration of ions at the various sites. In particular, high concentrations of C2v sites were generated by double doping with NaF prior to crystalline growth [CdF2: (Er3+,Na+)], whereas C3v sites were generated preferentially by oxygen firing sodium-free crystals subsequent to growth [CdF2: (Er3+,O2−)]. Selective generation of these two sites permitted the unambiguous determination of their characteristic optical absorption, emission, and excitation spectra, as well as the lifetimes and radiative efficiencies of relevant excited states. In addition, double excitation using two ir sources simultaneously, was used to determine the cross section for transitions between the 4I13/2 and 4S3/2 excited states and the lifetime of the former state. The optical properties of the Er3+ ion were observed to be sensitive to the local environment associated with each site and, in particular, to the magnitude of the noncubic component of the crystalline field. Phase-lag measurements confirmed the successive-excitation model proposed to explain the conversion of 1.5-μm radiation to 540- or 660-nm radiation in the presence of an 840-nm pump. Cooperative-excitation processes, on the other hand, were observed to produce 660-nm emission when 790- or 970-nm pumps were employed. The dependence of the over-all IRQC quantum efficiency on pump flux and on the optical parameters of Er3+ is derived from solutions to the appropriate rate equations. The analysis indicates that the performance of the 1.5-μm Er:IRQC, utilizing an 840-nm pump, is nearly optimized for CdF2: (Er3+,O2−).