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Physical Review

Ground-State Modulation Using Optical Double Resonance in Trivalent Rare-Earth-Doped Single Crystals

L. Esterowitz, Evan P. Chicklis

Published Oct 10, 1968• 5 citations
Publisher

Abstract

We report a double-resonance technique that can substantially increase our knowledge of the many complex and competitive processes operative in materials such as the trivalent rare-earth-doped single crystals. This technique, which modulates the ground-state population, is similar in many respects to the Bloembergen quantum counter and the Varsanyi infrared-optical double-resonance experiment. The similarity and differences of the three techniques are analyzed and discussed. Ground-state modulation has been observed in single crystals of CaW${\mathrm{O}}_{4}$: 2% ${\mathrm{Tm}}^{3+}$ and Cd${\mathrm{F}}_{2}$: 5% ${\mathrm{Ho}}^{3+}$. The applications of this technique to determine the dominant process of competing mechanisms are discussed. This technique may also be used to resolve ambiguities present in optical spectra of the trivalent rare-earth-doped single crystals and as a possible negative \ensuremath{\leftrightarrow} positive image converter.

DOI
10.1103/physrev.174.463

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Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. 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Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. 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•Jan 1, 2016•1 citation
We report a double-resonance technique that can substantially increase our knowledge of the many complex and competitive processes operative in materials such as the trivalent rare-earth-doped single crystals. This technique, which modulates the ground-state population, is similar in many respects to the Bloembergen quantum counter and the Varsanyi infrared-optical double-resonance experiment. The similarity and differences of the three techniques are analyzed and discussed. Ground-state modulation has been observed in single crystals of CaWO4{\mathrm{O}}_{4}O4​: 2% Tm3+{\mathrm{Tm}}^{3+}Tm3+ and CdF2{\mathrm{F}}_{2}F2​: 5% Ho3+{\mathrm{Ho}}^{3+}Ho3+. The applications of this technique to determine the dominant process of competing mechanisms are discussed. This technique may also be used to resolve ambiguities present in optical spectra of the trivalent rare-earth-doped single crystals and as a possible negative \ensuremath{\leftrightarrow} positive image converter.
In this paper, we report the first laser-excited optical double-resonance experiments in rare-earth-doped crystals. Infrared upconversion in LaCl3 : Pr3+ and LaF3 : Pr3+ has been achieved by means of a tunable cw dye laser pump. The quantum efficiency of the upconversion process at 2.03 μ in LaCl3 : Pr3+ is 1.2×10−3, which is an improvement of 4×105 over the highest efficiency found previously with incoherent sources. It is shown that an efficiency of 1 can be easily obtained with higher fluxes and improved crystal quality. Direct excitation of the output fluorescence from the 3P0 level is observed in both LaCl3 : Pr3+ and LaF3 : Pr3+ when the dye laser frequency is resonant with the states of the lower-lying 1D2 manifold in the absence of the infrared input. Detailed assignments of the observed double-resonance transitions have been made from wavelength and polarization measurements.
To study the role of stepwise and relaxation processes under effective excitation of anti-Stokes luminescence of rare-earth (RE) ions in crystals the time-shifted pulse method is used. It is shown that direct comparison of measured single- and two-photon luminescence excitation spectra often enables one to make immediate conclusions on the position and classification of electron levels of RE ions. The Tb3+ and Eu3− level structures (crystal CaF2) in the near ultraviolet are considered as an example. The peculiarities connected with the polarization characteristics of the two-photon absorption of radiation by the trivalent RE ions in a crystal matrix are discussed. To obtain the two-photon spectra a frequency-tunable organic dye solution laser (ODSL) is used.
Abstract : Quantum counter action has been observed in divalent rare earth doped ions lattices. The report presents the experimental work that has been done on Sm(2+) and Tm(2+) singly doped and Sm(2+) : Tm(2+) double doped systems in order to investigate the nature and efficiency of the schemes. The results show that while these systems are more efficient per ion than the trivalent rare earth doped systems the lower concentrations possible bring the overall efficiency back to the same level. (Author)
Since quantum information technologies are expected to offer communication security and high computational capacities, research in the field is currently attracting a lot of attention. Among the materials studied so far, rare earth doped inorganic insulators are one of the most promising. With the different available trivalent rare earth ions, the visible and the IR range including the telecom wavelength at 1.5 μm can be covered. Transitions are usually narrow, and at low temperatures, long optical and spin coherence times can often be observed. Investigations using bulk single crystals have already led to many promising results. Recently, spectroscopic studies have been extended to other forms of inorganic materials, such as transparent ceramics, thin films, and nanoparticles for single rare‐earth qubits. Progress in these areas is expected to offer many new possibilities for the design of quantum light‐matter interfaces and scalable quantum memories and processors.
Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. They are intensively studied as the most promising candidates for the realization of solid-state quantum bits. However, these systems coupled to a complex environment which can result in rapid loss of spin coherence or optical instability. Finding an alternative solid-state single system with remarkable optical and spin properties is the motivation of this dissertation. Rare earth ions doped in inorganic crystal hosts provide promises not only by the high quality factor 4f-4f optical transitions but also by the well preserved and long-lived spin states, with the applications from solid-state laser spectroscopy to quantum information processing. However, for almost three decades, not being able to identify single rare earth elements in solids is the obstacle to achieve their full potential functionality. We demonstrated the first direct optical detection of single rare earth ions (praseodymium) in solids in 2012. This research was covered in my Master Degree Thesis. This dissertation presents experimental progress in optically detecting other single rare earth species in crystals, understanding their fundamental spectroscopy properties and coherently controlling them, which is mainly focused on single trivalent cerium ions in different host materials. Following the optical detection of single cerium ions in yttrium aluminum garnet (YAG), the optical and spin properties of single Ce ions are investigated. Single Ce ions show good photostability under the pulsed laser excitation. Still, like in other solid emitters, photo-induced dynamics of single Ce ions is observed, however, in a counterintuitive way under the continuous laser irradiation. To understand this behavior, we proposed a charge dynamics model, and developed a novel method to suppress this undesired charge dynamics. With this approach, we obtain the photoluminescence excitation spectrum of single Ce ions in YAG under a CW laser excitation. Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. We show the spin state has a coherence time of 290 ns, which is dominated by the surrounding aluminum nuclear spin bath and impurities induced electron spin bath. The coherence time can be extended to 2 ms through dynamical decoupling method, which approaches closely to the upper limit 4.5 ms due to spin-lattice relaxation. This result indicates single Ce electron spin can be a good solid-state qubit. With the combination of optical and spin manipulations of single Ce ions, a quantum interface between a single spin and a single photon is observed by monitoring the temporal behavior of circularly polarized emission photons from the ion. We obtain the Larmor precession of the excited spin state, indicating the direct mapping of the excited spin states of single Ce ions onto the polarization states of the fluorescence photons. Furthermore, with both optical and spin access, we all-optically demonstrate coherent population trapping of a single Ce spin qubit. To scale up the system for further applications, we present the nano-scale engineering of rare earth species in YAG crystal, with the acquirement of the production yield of Ce and Pr implantation (53 and 91% respectively). The optical and spin properties of single implanted Ce ions show fairly good performance, which paves the way towards coherent coupling of single rare earth qubits in a small volume. Besides the study of single Ce ions, the spectroscopy properties of single praseodymium ions in YAG crystal are investigated. We obtain the photoluminescence excitation spectrum and the hyperfine splitting of a single praseodymium ion. All-optical control of a single praseodymium ion is achieved. In this dissertation, we solve the key problem of optically detecting, spectrally studying and coherently manipulating single rare earth ions in solids. The developed methods including optical detection, initialization, readout, coherent control and nanoscale production of single rare earth elements in crystals offer novel and powerful tools for understanding and exploring the fundamental spectroscopy properties of single rare earth elements in solids. It paves a way towards constructing scalable quantum network based on single rare earth solid-state qubits.