ABSTRACT
The design of magnetic molecular materials exhibiting multiple functions has garnered significant interest owing to their potential applications in molecular switches, sensors, and data storage devices. In this study, we synthesized a two-dimensional (2D) FeII-based Hofmann-type coordination polymer, namely {Fe(DPPE)2[Ag(CN)2]2}·2EtOH (1), using a luminescent ligand 1,1-diphenyl-2,2-di(4-pyridylbiphenyl)ethylene (DPPE). Single-crystal structural analyses and magnetic measurements revealed a thermally induced spin crossover (SCO) with the transition temperature T1/2 = 231 K. Variable-temperature fluorescence emission spectra indicated the coexistence of spin crossover and fluorescence properties. Moreover, a pronounced dielectric change (Δε' = 1.2 at 0.5 kHz) was observed during the SCO process, confirming the simultaneous magnetic and dielectric switching arising from the rearrangement of 3d electrons and deformation of the FeII-centered coordination sphere. This work provides an approach to explore the interplay between magnetic, dielectric, and fluorescence properties, and holds significance for developing multifunctional molecular materials.
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Ferroptosis regulators have been found to affect tumor progression. However, studies focusing on ferroptosis and soft tissue sarcoma (STS) are rare. Somatic mutation, copy number variation, reverse transcription-quantitative polymerase chain reaction (RT-qPCR) analysis, consensus clustering, differentially expressed genes analysis (DEGs), principal component analysis (PCA) and gene set enrichment analysis (GSEA) were used to identify and explore different ferroptosis modifications in STS. A nomogram was constructed to predict the prognosis of STS. Moreover, three immunotherapy datasets were used to assess the Fescore. Western blotting, siRNA transfection, EdU assay and reactive oxygen species (ROS) measurement were performed. 16 prognostic ferroptosis regulators were screened and significant differences were observed in somatic mutation, copy number variation (CNV) and RT-qPCR among these ferroptosis regulators. 2 different ferroptosis modification patterns were found (Fe cluster A and B). Fe cluster A with higher Fescore was correlated with p53 pathway and had better prognosis of STS (p = 0.002) while Fe cluster B with lower Fescore was correlated with angiogenesis and MYC pathway and showed a poorer outcome. Besides, the nomogram effectively predicted the outcome of STS and the Fescore could also well predict the prognosis of other 16 tumors and immunotherapy response. Downregulation of LOX also inhibited growth and increased ROS production in sarcoma cells. The molecular characterization of ferroptosis regulators in STS was explored and an Fescore was constructed. The Fescore quantified ferroptosis modification in STS patients and effectively predicted the prognosis of a variety of tumors, providing novel insights for precision medicine.
Subject(s)
Ferroptosis , Sarcoma , Humans , Prognosis , DNA Copy Number Variations , Ferroptosis/genetics , Reactive Oxygen Species , Sarcoma/genetics , Sarcoma/therapy , Computational Biology , ImmunotherapyABSTRACT
OBJECTIVE: To observe the effects of acupuncture on swallowing function and quality of life for patients with dysphagia in Parkinson's disease (PD). METHODS: A total of 60 patients of PD with dysphagia were randomly divided into an observation group (30 cases, 2 cases dropped off) and a control group (30 cases, 3 cases dropped off). The control group was given conventional medication therapy and rehabilitation training. On the basis of the treatment as the control group, the observation group was given acupuncture at Fengfu (GV 16), Baihui (GV 20), Shenting (GV 24), Yintang (GV 24+), Yansanzhen and bilateral Fengchi (GB 20), 30 min each time, once a day, 6 times a week for 4 weeks. Before and after treatment, the Kubota water swallowing test, standardized swallowing assessment (SSA) and swallowing quality of life (SWAL-QOL) were used to evaluate the swallowing function and quality of life of the two groups. RESULTS: After treatment, the Kubota water swallowing test grade, SSA scores in the two groups were decreased compared with those before treatment (P<0.05, P<0.001)ï¼the SWAL-QOL scores were increased compared with those before treatment (P<0.001); in the observation groupï¼the Kubota water swallowing test grade and SSA score were lower than those in the control group (P<0.05)ï¼the SWAL-QOL score was higher than that in the control group (P<0.001). CONCLUSION: On the basis of conventional medication therapy and rehabilitation trainingï¼acupuncture could improve the swallowing function and quality of life for patients of PD with dysphagia.
Subject(s)
Acupuncture Therapy , Deglutition Disorders , Parkinson Disease , Humans , Deglutition Disorders/etiology , Deglutition Disorders/therapy , Deglutition , Quality of Life , Parkinson Disease/complications , Parkinson Disease/therapy , WaterABSTRACT
Manipulating fluorescence by photo-switched spin-state conversions is an attractive prospect for applications in smart magneto-optical materials and devices. The challenge is how to modulate the energy transfer paths of the singlet excited state by light-induced spin-state conversions. In this work, a spin crossover (SCO) FeII-based fluorophore was embedded into a metal-organic framework (MOF) to tune the energy transfer paths. Compound 1 {Fe(TPA-diPy)[Ag(CN)2]2}·2EtOH (1) has an interpenetrated Hofmann-type structure, wherein the FeII ion is coordinated by a bidentate fluorophore ligand (TPA-diPy) and four cyanide nitrogen atoms and acts as the fluorescent-SCO unit. Magnetic susceptibility measurements revealed that 1 underwent an incomplete and gradual spin crossover with T1/2 = 161 K. Photomagnetic studies confirmed photo-induced spin state conversions between the low-spin (LS) and high-spin (HS) states, where the irradiation of 532 and 808 nm laser lights converted the LS and HS states to the HS and LS states, respectively. Variable-temperature fluorescence spectra study revealed an anomalous decrease in emission intensity upon the HS â LS transition, confirming the synergetic coupling between the fluorophore and SCO units. Alternating irradiation of 532 and 808 nm laser lights resulted in reversible fluorescence intensity changes, confirming spin state-controlled fluorescence in the SCO-MOF. Photo-monitored structural analyses and UV-vis spectroscopic studies demonstrated that the photo-induced spin state conversions changed energy transfer paths from the TPA fluorophore to the metal-centered charge transfer bands, ultimately leading to the switching of fluorescence intensities. This work represents a new prototype compound showing bidirectional photo-switched fluorescence by manipulating the spin states of iron(ii).
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Cyano-bridged 4d-4f molecular nanomagnets have re-called increasing research interests in molecular magnetism since they offer more possibilities in achieving novel nanomagnets with versatile structures and magnetic interactions. In this work, four ß-diketone ligands bearing different substitution N-sites were designed and synthesized, namely 1-(2-pyridyl)-3-(3-pyridyl)-1,3-propanedione (HL1 ), 1,3-Bis (3-pyridyl)-1,3-propanedione (HL2 ), 1-(4-pyridyl)-3-(3-pyridyl)-1,3-propanedione (HL3 ), and 1,3-Bis (4-pyridyl)-1,3-propanedione (HL4 ), to tune the magnetic relaxation behaviors of cyano-bridged {DyIII MoV } systems. By reacting with DyCl3 â 6H2 O and K4 Mo(CN)8 â 2H2 O, four cyano-bridged complexes, namely {[Dy[MoV (CN)8 ](HL1 )2 (H2 O)3 ]} â 6H2 O (1), {[Dy[MoV (CN)8 ](HL2 )(H2 O)3 (CH3 OH)]}2 â 2CH3 OH â 3H2 O (2), {[Dy[MoV (CN)8 ](HL3 )(H2 O)2 (CH3 OH)] â H2 O}n (3), and {[Dy[MoV (CN)8 ](HL4 )2 (H2 O)3 ]} â 2H2 Oâ CH3 OH (4) were obtained. Structural analyses revealed that 1 and 4 are binuclear complexes, 2 has a tetragonal structure, and 3 exhibits a stair-like polymer chain structure. The DyIII ions in all complexes have eight-coordinated configurations with the coordination spheres DyO7 N1 for 1 and 4, DyO6 N2 for 2, and DyO5 N3 for 3. Magnetic measurements indicate that 1 is a zero-field single-molecule magnet (SMM) and complexes 2-4 are field-induced SMMs, with complex 4 featuring a two-step relaxation process. The magnetic characterizations and ab initio calculations revealed that changing the N-sites in the ß-diketone ligands can effectively alter the structures and magnetic properties of cyano-bridged 4d-4f nanomagnets by adjusting the coordination environments of the DyIII centers.
ABSTRACT
Colossal and anisotropic thermal expansion is a key function for microscale or nanoscale actuators in material science. Herein, we present a hexanuclear compound of [(Tp*)FeIII (CN)3 ]4 [FeII (Ppmp)]2 â 2 CH3 OH (1, Tp*=hydrotris(3,5-dimethyl-pyrazol-1-yl)borate and Ppmp=2-[3-(2'-pyridyl)pyrazol-1-ylmethyl]pyridine), which has a rhombic core structure abbreviated as {FeIII 2 FeII 2 }. Magnetic susceptibility measurements and single-crystal X-ray diffraction analyses revealed that 1 underwent thermally-induced spin transition with the thermal hysteresis. The FeII site in 1 behaved as a spin crossover (SCO) unit, and significant deformation of its octahedron was observed during the spin transition process. Moreover, the distortion of the FeII centers actuated anisotropic deformation of the rhombic {FeIII 2 FeII 2 } core, which was spread over the whole crystal through the subsequent molecular rearrangements, leading to the colossal anisotropic thermal expansion. Our results provide a rational strategy for realizing the colossal anisotropic thermal expansion and shape memory effects by tuning the magnetic bistability.
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In recent years, spin defects in silicon carbide have become promising platforms for quantum sensing, quantum information processing and quantum networks. It has been shown that their spin coherence times can be dramatically extended with an external axial magnetic field. However, little is known about the effect of magnetic-angle-dependent coherence time, which is an essential complement to defect spin properties. Here, we investigate the optically detected magnetic resonance (ODMR) spectra of divacancy spins in silicon carbide with a magnetic field orientation. The ODMR contrast decreases as the off-axis magnetic field strength increases. We then study the coherence times of divacancy spins in two different samples with magnetic field angles, and both of the coherence times decrease with the angle. The experiments pave the way for all-optical magnetic field sensing and quantum information processing.
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BACKGROUND: Intrahepatic cholangiocarcinoma (iCCA) is the second most common primary hepatic malignancy worldwide. However, currently available systemic therapies are of limited effectiveness, and the median overall survival of patients treated with first-line standard chemotherapy is less than one year. Immune checkpoint inhibitors have been used to treat solid tumors. Clinical studies recently explored the combination of chemotherapy and immunotherapy for CCA. However, the clinical significance of predictive biomarkers for chemo-immunotherapy in CCA remains unclear. It is also worth exploring whether a combination of chemotherapeutic agents can increase the sensitivity of CCA immunotherapy. CASE SUMMARY: This study reports a case of advanced iCCA in which clinical complete remission had been achieved using a programmed death 1 (PD-1) inhibitor and paclitaxel without known predictive biomarkers, but with BRCA1, KRAS, and NTRK3 mutations after rapid progression to first-line chemotherapy, and has remained in clinical complete remission for more than two years. This case suggests that chemo-immunotherapy is a potential therapeutic option for patients with iCCA and few known predictive biomarkers for immunotherapies as well as synergistic effect of the combination of paclitaxel and PD-1 monoclonal antibody. CONCLUSION: The combination of paclitaxel and PD-1 monoclonal antibodyr can be explored in patients with advanced iCCA.
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Hexagonal boron nitride (hBN) has recently been demonstrated to contain optically polarized and detected electron spins that can be utilized for implementing qubits and quantum sensors in nanolayered-devices. Understanding the coherent dynamics of microwave driven spins in hBN is of crucial importance for advancing these emerging new technologies. Here, we demonstrate and study the Rabi oscillation and related phenomena of a negatively charged boron vacancy (V[Formula: see text]) spin ensemble in hBN. We report on different dynamics of the V[Formula: see text] spins at weak and strong magnetic fields. In the former case the defect behaves like a single electron spin system, while in the latter case it behaves like a multi-spin system exhibiting multiple-frequency dynamical oscillation as beat in the Ramsey fringes. We also carry out theoretical simulations for the spin dynamics of V[Formula: see text] and reveal that the nuclear spins can be driven via the strong electron nuclear coupling existing in V[Formula: see text] center, which can be modulated by the magnetic field and microwave field.
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Spin defects in silicon carbide (SiC) with mature wafer-scale fabrication and micro/nano-processing technologies have recently drawn considerable attention. Although room-temperature single-spin manipulation of colour centres in SiC has been demonstrated, the typically detected contrast is less than 2[Formula: see text], and the photon count rate is also low. Here, we present the coherent manipulation of single divacancy spins in 4H-SiC with a high readout contrast ([Formula: see text]) and a high photon count rate (150 kilo counts per second) under ambient conditions, which are competitive with the nitrogen-vacancy centres in diamond. Coupling between a single defect spin and a nearby nuclear spin is also observed. We further provide a theoretical explanation for the high readout contrast by analysing the defect levels and decay paths. Since the high readout contrast is of utmost importance in many applications of quantum technologies, this work might open a new territory for SiC-based quantum devices with many advanced properties of the host material.
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BACKGROUND: Immune checkpoint inhibitors (ICIs) targeting the programmed death (PD)-1 pathway have substantially changed the clinical management of metastatic urothelial carcinoma (mUC); however, the response rate remains low. There are ongoing efforts to identify robust biomarkers that can effectively predict the treatment response to ICIs. Previous studies have suggested that ERBB2/3 mutations are associated with the efficacy of ICIs in gallbladder carcinoma. CASE SUMMARY: We present a 59-year-old man with mUC harboring ERBB2/3 mutations (in-frame insertion of ERBB2 and ERBB3 amplification), negative PD-ligand 1 expression, and low tumor mutation burden. He received anti-PD-1 antibodies and paclitaxel as second-line treatment. After two cycles of treatment, the lung metastases had significantly shrunk, achieving good partial remission. After six cycles of combination therapy, the patient received sindilimab 200 mg once every 3 wk as maintenance monotherapy. At the last follow-up, the patient continued to exhibit a partial response and progression-free survival for as long as 19 mo. CONCLUSION: ERBB2/3 mutations may represent a predictive biomarker for selecting a subgroup of mUC patients who will benefit from ICIs.
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Optically addressable spin defects in wide-band-gap semiconductors as promising systems for quantum information and sensing applications have recently attracted increased attention. Spin defects in two-dimensional materials are expected to show superiority in quantum sensing due to their atomic thickness. Here, we demonstrate that an ensemble of negatively charged boron vacancies (VB -) with good spin properties in hexagonal boron nitride (hBN) can be generated by ion implantation. We carry out optically detected magnetic resonance measurements at room temperature to characterize the spin properties of ensembles of VB - defects, showing a zero-field splitting frequency of â¼3.47 GHz. We compare the photoluminescence intensity and spin properties of VB - defects generated using different implantation parameters, such as fluence, energy, and ion species. With the use of the proper parameters, we can successfully create VB - defects with a high probability. Our results provide a simple and practicable method to create spin defects in hBN, which is of great significance for realizing integrated hBN-based devices.
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The elevation of ambient temperature beyond the thermoneutral zone leads to heat stress, which is a growing health and welfare issue for homeothermic animals aiming to maintain relatively constant reproducibility and survivability. Particularly, global warming over the past decades has resulted in more hot days with more intense, frequent, and long-lasting heat waves, resulting in a global surge in animals suffering from heat stress. Heat stress causes pathophysiological changes in animals, increasing stress sensitivity and immunosuppression, consequently leading to increased intestinal permeability (leaky gut) and related neuroinflammation. Probiotics, as well as prebiotics and synbiotics, have been used to prevent or reduce stress-induced negative effects on physiological and behavioral homeostasis in humans and various animals. The current data indicate dietary supplementation with a Bacillus subtilis-based probiotic has similar functions in poultry. This review highlights the recent findings on the effects of the probiotic Bacillus subtilis on skeletal health of broiler chickens exposed to heat stress. It provides insights to aid in the development of practical strategies for improving health and performance in poultry.
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BACKGROUND: Osteosarcoma is one of the most common bone tumors among children. Tumor-associated macrophages have been found to interact with tumor cells, secreting a variety of cytokines about tumor growth, metastasis, and prognosis. This study aimed to identify macrophage-associated genes (MAGs) signatures to predict the prognosis of osteosarcoma. METHODS: Totally 384 MAGs were collected from GSEA software C7: immunologic signature gene sets. Differential gene expression (DGE) analysis was performed between normal bone samples and osteosarcoma samples in GSE99671. Kaplan-Meier survival analysis was performed to identify prognostic MAGs in TARGET-OS. Decision curve analysis (DCA), nomogram, receiver operating characteristic (ROC), and survival curve analysis were further used to assess our risk model. All genes from TARGET-OS were used for gene set enrichment analysis (GSEA). Immune infiltration of osteosarcoma sample was calculated using CIBERSORT and ESTIMATE packages. The independent test data set GSE21257 from gene expression omnibus (GEO) was used to validate our risk model. RESULTS: 5 MAGs (MAP3K5, PML, WDR1, BAMBI, and GNPDA2) were screened based on protein-protein interaction (PPI), DGE, and survival analysis. A novel macrophage-associated risk model was constructed to predict a risk score based on multivariate Cox regression analysis. The high-risk group showed a worse prognosis of osteosarcoma (p < 0.001) while the low-risk group had higher immune and stromal scores. The risk score was identified as an independent prognostic factor for osteosarcoma. MAGs model for diagnosis of osteosarcoma had a better net clinical benefit based on DCA. The nomogram and ROC curve also effectively predicted the prognosis of osteosarcoma. Besides, the validation result was consistent with the result of TARGET-OS. CONCLUSIONS: A novel macrophage-associated risk score to differentiate low- and high-risk groups of osteosarcoma was constructed based on integrative bioinformatics analysis. Macrophages might affect the prognosis of osteosarcoma through macrophage differentiation pathways and bring novel sights for the progression and prognosis of osteosarcoma.
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Optically addressable solid-state color center spin qubits have become important platforms for quantum information processing, quantum networks and quantum sensing. The readout of color center spin states with optically detected magnetic resonance (ODMR) technology is traditionally based on Stokes excitation, where the energy of the exciting laser is higher than that of the emission photons. Here, we investigate an unconventional approach using anti-Stokes excitation to detect the ODMR signal of silicon vacancy defect spin in silicon carbide, where the exciting laser has lower energy than the emitted photons. Laser power, microwave power and temperature dependence of the anti-Stokes excited ODMR are systematically studied, in which the behavior of ODMR contrast and linewidth is shown to be similar to that of Stokes excitation. However, the ODMR contrast is several times that of the Stokes excitation. Coherent control of silicon vacancy spin under anti-Stokes excitation is then realized at room temperature. The spin coherence properties are the same as those of Stokes excitation, but with a signal contrast that is around three times greater. To illustrate the enhanced spin readout contrast under anti-Stokes excitation, we also provide a theoretical model. The experiments demonstrate that the current anti-Stokes excitation ODMR approach has promising applications in quantum information processing and quantum sensing.
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Heat stress as an environmental stressor causes abnormal bone remodeling and microarchitectural deterioration. The objective of this study was to investigate the effects of a Bacillus subtilis-based probiotic on bone mass of broilers subjected to cycling high ambient temperature. One hundred and twenty 1-day-old Ross 708 male broiler chicks were randomly assigned to 2 dietary treatments (12 pens per treatment): control diet and the control diet plus 250-ppm probiotic consisting of 3 strains of Bacillus subtilis. Room temperature was gradually decreased from 35°C on day 1 by 0.5°C/d until day 15, when ambient temperature was increased from 28°C to 32°C for 10 h (07:00 h-17:00 h) daily until day 44. Samples of blood, leg bones (tibia and femur), and brains (raphe nuclei and hypothalamus) were collected at day 43, while latency to lie test was conducted at day 44. Compared with controls, probiotic supplementation increased bone mineral content, weight, size, weight to length index, and reduced robusticity index in the tibia and femur (P < 0.05) of broilers subjected to heat stress. Serum concentrations of c-terminal telopeptide of type I collagen (CTX) were reduced (P = 0.02) by the probiotic supplementation, while ionized calcium, phosphate, and osteocalcin were not affected (P > 0.05). Moreover, tumor necrosis factor-α (TNF-α) in probiotic fed broilers was decreased (P = 0.003) without changes of plasma interleukin (IL)-6, IL-10, interferon-γ, and corticosterone concentrations. There were no treatment effects on the concentrations of peripheral serotonin and central serotonin and catecholamines (norepinephrine, epinephrine, and dopamine) as well as their metabolites. These results may indicate that dietary supplementation of Bacillus subtilis-based probiotic increases bone growth in broilers under a cyclic heating episode probably via inhibition of bone resorption, resulting from downregulation of the circulating TNF-α and CTX. Dietary probiotic supplementation may be a management strategy for increasing skeletal health of broilers under hot weather.
Subject(s)
Bacillus subtilis , Bone Development , Chickens , Heating , Inflammation , Probiotics , Animal Feed/analysis , Animals , Bacillus subtilis/physiology , Chickens/growth & development , Chickens/microbiology , Diet/veterinary , Inflammation/microbiology , Inflammation/veterinary , Male , Random AllocationABSTRACT
Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration sixfold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature, and the coherence time T_{2} can be reached to around 17.1 µs. Furthermore, an investigation of fluorescence properties of single NV centers shows that they are room-temperature photostable single-photon sources at telecom range. Taking advantage of technologically mature materials, the experiment demonstrates that the NV centers in silicon carbide are promising platforms for large-scale integrated quantum photonics and long-distance quantum networks.
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OBJECTIVE: The present study aimed to evaluate the short-term clinical performance and safety of percutaneous microwave ablation (MWA) techniques for the treatment of bone tumors. METHODS: This single-institution retrospective study investigated 47 cases of bone tumors treated by MWA from June 2015 to June 2018. The study included 26 patients (55.3%) with benign bone tumors and 21 patients (44.7%) with malignant bone tumors. The tumors were located in the spine or sacrum (15, 31.9%), the upper extremities (6, 12.8%), the lower extremities (17, 36.2%) and the pelvis (9, 19.1%). Outcomes regarding clinical efficacy, including pain relief, quality of life, and intervention-related complications, were evaluated before and after MWA using the visual analog scale (VAS) and the 36-item Short-Form Health Survey (SF-36) scoring system. RESULTS: Of the 47 patients included in this study, all of them completed follow-up examinations, with a mean follow-up duration of 4.8 ± 1.6 months (range, 2-9 months). Significantly improved VAS and SF-36 scores were recorded after the initial treatment (P<0.001), suggesting that almost 100% of patients experienced pain relief and an improved quality of life following surgery. No major intervention-related complications (e.g., serious neurovascular injury or infection) occurred during or after the treatment. We recorded only three minor posttreatment complications (6.4%, 3/47), which were related to thermal injury that caused myofasciitis and affected wound healing. CONCLUSION: In our study, the short-term efficacy of MWA was considerably favorable, with a relatively low rate of complications. Our results also showed that MWA was effective for pain relief and improved patients' quality of life, making it a feasible treatment alternative for bone tumors.
Subject(s)
Bone Neoplasms/therapy , Microwaves/therapeutic use , Radiofrequency Ablation/methods , Adult , Female , Humans , Male , Middle Aged , Quality of Life , Treatment OutcomeABSTRACT
Color centers in silicon carbide have recently attracted broad interest as high bright single photon sources and defect spins with long coherence time at room temperature. There have been several methods to generate silicon vacancy defects with excellent spin properties in silicon carbide, such as electron irradiation and ion implantation. However, little is known about the depth distribution and nanoscale depth control of the shallow defects. Here, a method is presented to precisely control the depths of the ion implantation induced shallow silicon vacancy defects in silicon carbide by using reactive ion etching with little surface damage. After optimizing the major etching parameters, a slow and stable etching rate of about 5.5 ± 0.5 nm min-1 can be obtained. By successive nanoscale plasma etching, the shallow defects are brought close to the surface step by step. The photoluminescence spectrum and optically detected magnetic resonance spectra are measured, which confirm that there were no plasma-induced optical and spin property changes of the defects. By tracing the mean counts of the remaining defects after each etching process, the depth distribution of the defects can be obtained for various implantation conditions. Moreover, the spin coherence time T2* of the generated VSi defects is detected at different etch depths, which greatly decreases when the depth is less than 25 nm. The method of nanoscale depth control of silicon vacancies would pave the way for investigating the surface spin properties and the applications in nanoscale sensing and quantum photonics.