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Register a new userElectron nuclear interactions and electronic structure of spin 3/2 color centers in silicon carbide: A high-field pulse EPR and ENDOR study
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Andrey Anisimov Dr.
Publication date
2020
fields
Physics
and research's language is
English
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High-frequency pulse electron paramagnetic resonance (EPR) and electron nuclear double resonance (ENDOR) were used to clarify the electronic structure of the color centers with an optically induced high-temperature spin-3/2 alignment in hexagonal 4H-, 6H- and rhombic 15R- silicon carbide (SiC) polytypes. The identification is based on resolved ligand hyperfine interactions with carbon and silicon nearest, next nearest and the more distant neighbors and on the determination of the spin state. The ground state and the excited state were demonstrated to have spin S = 3/2. The microscopic model suggested from the EPR and ENDOR results is as follows: a paramagnetic negatively charged silicon vacancy that is noncovalently bonded to a non-paramagnetic neutral carbon vacancy, located on the adjacent site along the SiC symmetry c-axis.
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We discovered uniaxial oriented centers in silicon carbide having unusual performance. Here we demonstrate that the family of silicon-vacancy related centers with $S= 3/2$ in rhombic 15R-SiC crystalline matrix possess unique characteristics such as ODMR contrast and optical spin alignment existing at temperatures up to 250$^circ$C. Thus the concept of optically addressable silicon vacancy related centers with half integer ground spin state is extended to the wide class of SiC rhombic polytypes. The structure of these centers, which is a fundamental problem for quantum applications, has been established using high frequency ENDOR. It has been shown that a family of siliconvacancy related centers is a negatively charged silicon vacancy in the paramagnetic state with the spin $S= 3/2$, V$_textrm{Si}^-$, perturbed by neutral carbon vacancy in non-paramagnetic state, V$_textrm{C}^0$, having no covalent bond with the silicon vacancy and located adjacently to the silicon vacancy on the c crystal axis.
We demonstrate that the spin of optically addressable point defects can be coherently driven with AC electric fields. Based on magnetic-dipole forbidden spin transitions, this scheme enables spatially confined spin control, the imaging of high-frequency electric fields, and the characterization of defect spin multiplicity. While we control defects in SiC, these methods apply to spin systems in many semiconductors, including the nitrogen-vacancy center in diamond. Electrically driven spin resonance offers a viable route towards scalable quantum control of electron spins in a dense array.
Silicon carbide with optically and magnetically active point defects offers unique opportunities for quantum technology applications. Since interaction with these defects commonly happens through optical excitation and de-excitation, a complete understanding of their light-matter interaction in general and optical signatures, in particular, is crucial. Here, we employ quantum mechanical density functional theory calculations to investigate the photoluminescence lineshapes of selected, experimentally observed color centers (including single vacancies, double vacancies, and vacancy impurity pairs) in 4H-SiC. The analysis of zero-phonon lines as well as Huang-Rhys and Debye-Waller factors are accompanied by a detailed study of the underlying lattice vibrations. We show that the defect lineshapes are governed by strong coupling to bulk phonons at lower energies and localized vibrational modes at higher energies. Generally, good agreement to the available experimental data is obtained, and thus we expect our theoretical work to be beneficial for the identification of defect signatures in the photoluminescence spectra and thereby advance the research in quantum photonics and quantum information processing.
In this paper, we study the electron spin decoherence of single defects in silicon carbide (SiC) nuclear spin bath. We find that, although the natural abundance of $^{29}rm{Si}$ ($p_{rm{Si}}=4.7%$) is about 4 times larger than that of $^{13}{rm C}$ ($p_{rm{C}}=1.1%$), the electron spin coherence time of defect centers in SiC nuclear spin bath in strong magnetic field ($B>300~rm{Gauss}$) is longer than that of nitrogen-vacancy (NV) centers in $^{13}{rm C}$ nuclear spin bath in diamond. The reason for this counter-intuitive result is the suppression of heteronuclear-spin flip-flop process in finite magnetic field. Our results show that electron spin of defect centers in SiC are excellent candidates for solid state spin qubit in quantum information processing.
Quantum photonics plays a crucial role in the development of novel communication and sensing technologies. Color centers hosted in silicon carbide and diamond offer single photon emission and long coherence spins that can be scalably implemented in quantum networks. We develop systems that integrate these color centers with photonic devices that modify their emission properties through electromagnetically tailored light and matter interaction.
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