Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.W...Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.展开更多
The negatively charged nitrogen vacancy(NV^(−))center ensemble in as-grown chemical vapor deposition(CVD)diamond is a promising candidate for quantum sensing due to its long coherence time and excellent optical proper...The negatively charged nitrogen vacancy(NV^(−))center ensemble in as-grown chemical vapor deposition(CVD)diamond is a promising candidate for quantum sensing due to its long coherence time and excellent optical properties.However,achieving a high concentration of NV^(−)centers in as-grown CVD diamond remains a critical challenge,which constrains the performance of NV^(−)based sensors.In this study,we observe that NV^(−)center formation efficiency is significantly enhanced during the initial growth phase,with a coherence time T_(2)^(*)of 1.1μs.These findings demonstrate that high-concentration NV^(−)centers can be achieved in as-grown diamonds,greatly enhancing their utility in high-performance magnetometers and quantum sensing.展开更多
文摘Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.11374280 and 50772110).
文摘The negatively charged nitrogen vacancy(NV^(−))center ensemble in as-grown chemical vapor deposition(CVD)diamond is a promising candidate for quantum sensing due to its long coherence time and excellent optical properties.However,achieving a high concentration of NV^(−)centers in as-grown CVD diamond remains a critical challenge,which constrains the performance of NV^(−)based sensors.In this study,we observe that NV^(−)center formation efficiency is significantly enhanced during the initial growth phase,with a coherence time T_(2)^(*)of 1.1μs.These findings demonstrate that high-concentration NV^(−)centers can be achieved in as-grown diamonds,greatly enhancing their utility in high-performance magnetometers and quantum sensing.