Quantum systems can provide outstanding performance in various sensing applications, ranging from bioscience to nanotechnology. Atomic-scale defects in silicon carbide are very attractive in this respect because of the technological advantages of this material and favorable optical and radio frequency spectral ranges to control these defects. We identified several, separately addressable spin-3/2 centers in the same silicon carbide crystal, which are immune to nonaxial strain fluctuations. Some of them are characterized by nearly temperature independent axial crystal fields, making these centers very attractive for vector magnetometry. Contrarily, the zero-field splitting of another center exhibits a giant thermal shift of −1.1 MHz/K at room temperature, which can be used for thermometry applications. We also discuss a synchronized composite clock exploiting spin centers with different thermal response.
Several systems in the solid state have been suggested as promising candidates for spin-based quantum information processing. In spite of significant progress during the last decade, there is a search for new systems with higher potential [D. DiVincenzo, Nature Mat. 9, 468 (2010)]. We report that silicon vacancy defects in silicon carbide comprise the technological advantages of semiconductor quantum dots and the unique spin properties of the nitrogen-vacancy defects in diamond. Similar to atoms, the silicon vacancy qubits can be controlled under the double radio-optical resonance conditions, allowing for their selective addressing and manipulation. Furthermore, we reveal their long spin memory using pulsed magnetic resonance technique. All these results make silicon vacancy defects in silicon carbide very attractive for quantum applications.PACS numbers: 61.72. Hh, 76.70.Hb, 61.72.jd The double radio-optical resonance in atoms [1] constitutes the basis for a unprecedented level of coherent quantum control. Atomic time standards [2] and multiqubit quantum logic gates [3] are among the most known examples. In the solid state, semiconductor quantum dots (QDs) and the nitrogen-vacancy (NV) defects in diamond, frequently referred to as artificial atoms, are considered as the most promising candidates for quantum information processing [4,5]. Nevertheless, such a high degree of quantum control, as achieved in atoms,has not yet been demonstrated in these systems so far. Therefore, there is a search for quantum systems with even more potential [6].Recently, intrinsic defects in silicon carbide (SiC) have been proposed as eligible candidates for qubits [7,8]. Indeed, they reveal quantum spin coherence even at room temperature [9][10][11]. All of these experiments have been carried out under non-resonant optical excitation where all spins are controlled simultaneously. However, for spinbased information processing it is necessary to perform manipulations of selected spins, while the rest should remain unaffected. This demonstration in SiC is still an outstanding task.The selective spin control can be realized using a resonant optical excitation. As a rule, inhomogeneous broadening is much larger than the natural spectral linewidth, and such resonant addressing can be done on single centers only. To avoid this problem, we applied a special procedure to "freeze" silicon vacancy (V Si ) defects during their growth, allowing to preserve a high homogeneity inherent to Lely crystals. This is confirmed by the extremely sharp optical resonances in our samples. The spectral width of the V Si absorption lines is several µeV (ca. 1 GHz), which comparable with that of a single QD or a single NV center in diamond.We then demonstrate the selective spin initialization and readout by tuning the laser wavelength together with the spin manipulation by means of electron spin resonance (ESR). Such a double radio-optical resonance control indicates that the V Si defects strongly interact with light and are well decoupled from lattice vibr...
We demonstrate that silicon carbide (SiC) with natural isotope abundance can preserve a coherent spin superposition in silicon vacancies over unexpectedly long time approaching 0.1 seconds. The spin-locked subspace with drastically reduced decoherence rate is attained through the suppression of heteronuclear spin cross-talking by applying a moderate magnetic field in combination with dynamic decoupling from the nuclear spin baths. We identify several phonon-assisted mechanisms of spin-lattice relaxation, ultimately limiting quantum coherence, and find that it can be extremely long at cryogenic temperature, equal or even longer than 8 seconds. Our approach may be extended to other polyatomic compounds and open a path towards improved qubit memory for wafer-scale quantum techmologies.PACS numbers: 76.30. Mi, 42.50.Dv, 76.70.Hb Introduction -Long electron quantum coherence in solid-state systems is the ultimate prerequisite for new technologies based on quantum phenomena [1,2]. Particularly, the sensitivity of quantum sensors scales with the electron spin coherence time T 2 [3,4]. One of the common sources of decoherence is the interaction with fluctuating nuclear spins, and the usual way to prolong spin coherence is to perform isotope purification of the crystal. Indeed, the longest electron T 2 times of about 1 s and 0.6 s have been reported for spin-free silicon 28 Si and diamond 12 C crystals, respectively [5,6]. However, isotope purification is a technologically demanding procedure, which is not always possible. Therefore, one of the key challenges in quantum information science is to achieve long-lived spin coherence in natural materials.To address this goal, we combine two approaches. First, we exploit the suppression of mutual spin flip-flop processes between different types of nuclei in binary compounds, which occur in strong enough magnetic fields according to the theoretical simulations of Ref. [7]. Second, we use a periodic train of radiofrequency (RF) pulses to refocus spin coherence and decouple electron spins from inhomogeneous environment, similar to that applied for color centers [6] and quantum dots (QDs) [8].In recent years, SiC is attracting continuously growing interest as a technologically perspective platform for quantum spintronics [9][10][11][12][13][14][15][16][17] with the ability for single spin engineering and control [18][19][20][21]. The longest T 2 in SiC reported to date is 1 ms at cryogenic temperature [19]. We observe that in a finite magnetic field, a coherent spin superposition can be locked over longer time, which continuously increases up to about 75 ms with the number of decoupling pulses. The absence of saturation indicates that the longest possible spin locking time T
Understanding of degradation mechanisms in polymer:fullerene bulk-heterojunctions on the microscopic level aimed at improving their intrinsic stability is crucial for the breakthrough of organic photovoltaics. These materials are vulnerable to exposure to light and/or oxygen, hence they involve electronic excitations. To unambiguously probe the excited states of various multiplicities and their reactions with oxygen, we applied combined magneto-optical methods based on multifrequency (9 and 275 GHz) electron paramagnetic resonance (EPR), photoluminescence (PL), and PL-detected magnetic resonance (PLDMR) to the conjugated polymer poly(3-hexylthiophene) (P3HT) and polymer:fullerene bulk heterojunctions (P3HT:PCBM; PCBM = [6,6]-phenyl-C(61)-butyric acid methyl ester). We identified two distinct photochemical reaction routes, one being fully reversible and related to the formation of polymer:oxygen charge transfer complexes, the other one, irreversible, being related to the formation of singlet oxygen under participation of bound triplet excitons on the polymer chain. With respect to the blends, we discuss the protective effect of the methanofullerenes on the conjugated polymer bypassing the triplet exciton generation.
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