Determining the local symmetry of luminescent centers in crystals is critical for understanding and controlling their optical transitions, yet current methods are limited by stringent experimental requirements and ambiguous symmetry assignments. Here, we develop a robust computational electromagnetics framework that directly connect the local symmetry and chirality of rare-earth-doped single crystals to the polarization states of their emitted light. This framework is experimentally validated through the precise determination of point and space group symmetries using high-resolution, polarization-resolved micro-photoluminescence (μ-PL) spectra. Unlike conventional approaches that usually rely on analyzing multiple transitions at cryogenic temperatures, our technique operates at room temperature, requires only a single optical transition, and enables accurate orientation of symmetry axes. This enables deterministic polarization control of nano-emitters by tailoring symmetry groups and selecting appropriate transition dipoles, eliminating the need for bulky or complex photonic structures. Additionally, we demonstrate the function of bio-sensing, via determining single particle orientations in complex cellular environments using minimal polarization measurements. These results pave the way for advances in energy transfer systems, ultra-bright rare-earth nanocrystals, nanophotonic materials, and real-time single-particle tracking in biological contexts.
Determining the local symmetry of luminescent centers in crystals is critical for understanding and controlling their optical transitions, yet current methods are limited by stringent experimental requirements and ambiguous symmetry assignments. Here, we develop a robust computational electromagnetics framework that directly connect the local symmetry and chirality of rare-earth-doped single crystals to the polarization states of their emitted light. This framework is experimentally validated through the precise determination of point and space group symmetries using high-resolution, polarization-resolved micro-photoluminescence (μ-PL) spectra. Unlike conventional approaches that usually rely on analyzing multiple transitions at cryogenic temperatures, our technique operates at room temperature, requires only a single optical transition, and enables accurate orientation of symmetry axes. This enables deterministic polarization control of nano-emitters by tailoring symmetry groups and selecting appropriate transition dipoles, eliminating the need for bulky or complex photonic structures. Additionally, we demonstrate the function of bio-sensing, via determining single particle orientations in complex cellular environments using minimal polarization measurements. These results pave the way for advances in energy transfer systems, ultra-bright rare-earth nanocrystals, nanophotonic materials, and real-time single-particle tracking in biological contexts.
Rare-earth ion doped crystals are of great significance for microsensing and quantum information, while the ions in the crystals emit light with spontaneous partial polarization, which is, though believed to be originated from the crystal lattice structure, still lacking a deterministic explanation that can be tested with quantitative accuracy. We report experimental evidence showing the profound physical relation between the polarization degree of light emitted by the doped ion and the lattice symmetry by demonstrating, with high precision, that the lattice constant ratio c / a directly quantifies the macroscopic effective polar angle of the electric and magnetic dipoles, which essentially determines the linear polarization degree of the emission. Based on this result, we further propose a pure optical technology to identify the three-dimensional orientation of a rod-shaped single microcrystal using the polarization-resolved microspectroscopy. Our results, demonstrating the physical origin of light polarization in ion-doped crystals, allow work toward on-demand polarization control with crystallography and provide a versatile platform for polarization-based microscale sensing in dynamical systems.
Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the ${}^{5}{D}_{0}{\ensuremath{\rightarrow}}^{7}{F}_{1}$ transition dipole vector in individual NaYF4:Eu3+ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of NaYF4:Eu3+ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.
Spin-photon interfaces based on solid-state defects are key building blocks for scalable quantum networks and hybrid quantum platforms. Optimizing light-matter coupling in these systems requires precise knowledge of the optical transition dipole polarization, yet for many promising quantum emitters this quantity is hard to determine and therefore remains poorly characterized. Here, we develop a framework for reconstructing electric transition dipole polarization in spin-1/2 solid-state defects directly from ensemble spectroscopy. The approach combines the response of photoluminescence spectra to magnetic field, optical polarization, and strain. Applied to erbium ions in silicon, a particularly challenging system containing multiple crystallographic subsites, the framework identifies strain-induced shifts as the origin of asymmetric ensemble spectra and enables simultaneous determination of the optical dipole polarization and strain-orbital coupling tensor. The resulting model predicts how cavity-ion coupling depends on crystallographic orientation and magnetic-field direction, which we verify using single erbium ions coupled to a nanophotonic cavity. Together, these results establish a broadly applicable route for extracting microscopic properties of solid-state quantum emitters from ensemble spectroscopy and for engineering optimized spin-photon and spin-phonon interfaces.
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.
Quantum emitters in solid-state crystals have recently attracted a lot of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that play a crucial role in the applications, such as quantum computation that uses the indistinguishability of photons. However, the degree of single photon polarization is typically quantified using time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single photon sources to reveal the origin and the temporal evolution of dipole orientation in solid-state quantum emitters. The angle of excitation and emission dipoles relative to the crystal axes are determined experimentally and then calculated using density functional theory, which results in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics reveal a strongly modified linear polarization visibility that depends on the excited state decay time of individual excitation. This effect can be traced back potentially to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further be used to improve the performance of polarization-sensitive experiments, in particular that of quantum communication with single photon emitters.
Quantum emitters in solid-state crystals have recently attracted a great deal of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single-photon sources to reveal the origin and temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.