Optical whispering gallery microcavities with high-quality factors have shown great potential toward achieveing ultrahigh-sensitivity sensing up to a single molecule or nanoparticle, which raises a huge demand on a de...Optical whispering gallery microcavities with high-quality factors have shown great potential toward achieveing ultrahigh-sensitivity sensing up to a single molecule or nanoparticle, which raises a huge demand on a deep theoretical insight into the crucial phenomena such as the mode shift, mode splitting, and mode broadening in sensing experiments. Here we propose an intuitive model to analyze these phenomena from the viewpoint of the nanoparticle-induced multiple scattering of the azimuthally propagating mode(APM). The model unveils explicit relations between these phenomena and the phase change and energy loss of the APM when scattered at the nanoparticle; the model also explains the observed polarization-dependent preservation of one resonance and the particle-dependent redshift or blueshift. The model indicates that the particle-induced coupling between the pair of unperturbed degenerate whispering gallery modes(WGMs) and the coupling between the WGMs and the free-space radiation modes, which are widely adopted in current theoretical formalisms, are realized via the reflection and scattering-induced free-space radiation of the APM, respectively, and additionally exhibits the contribution of cross coupling between the unperturbed WGMs and other different WGMs to forming the splittingresonant modes, especially for large particles.展开更多
The chiral coupling of an emitter to waveguide mode, i.e., the propagation direction of the excited waveguide mode is locked to the transverse spin(T-spin) of a circularly polarized emitter, has exhibited unprecedente...The chiral coupling of an emitter to waveguide mode, i.e., the propagation direction of the excited waveguide mode is locked to the transverse spin(T-spin) of a circularly polarized emitter, has exhibited unprecedented applications in nanophotonics and quantum information processing. This chiral coupling can be largely enhanced in terms of unidirectivity, efficiency, and spontaneous emission rate by introducing resonant modes as coupling interfaces. However, this indirect chiral coupling still undergoes limitations in flexibility and miniaturization, and the underlying physical mechanisms are to be clarified. Here, we present an intuitive and rigorous approach for analyzing the direct/indirect chiral coupling, and thereout, derive some general relations between the chiralcoupling directionality and the T-spin of the field or emitter. Based on the theories, we propose an indirect chiral-coupling system on the platform of surface plasmon polariton(SPP), with a nanocavity supporting Fabry–Perot(FP) resonance of dual SPP modes serving as a novel coupling interface. The FP resonance provides flexible design freedoms which can modulate the chirality of the T-spin(and the resultant chiral-coupling directionality) to flip or disappear. A unidirectivity up to 99.9% along with a high coupling efficiency and enhancement of spontaneous emission rate is achieved. Two first-principles-based SPP models for the reciprocal and original problems are built up to verify the decisive role of the FP resonance in achieving the chiral coupling.The proposed theories and novel chiral-coupling interface will be beneficial to the design of more compact and flexible chiral-coupling systems for diverse applications.展开更多
Photo-corrosion is one of the major obstacles for CdS application in wet chemical fields, and atomic layer deposition (ALD) has been proposed as an effective way to suppress the corrosion. Here, prior to ALD coating...Photo-corrosion is one of the major obstacles for CdS application in wet chemical fields, and atomic layer deposition (ALD) has been proposed as an effective way to suppress the corrosion. Here, prior to ALD coating, CdS, one facilely corrosive photocatalyst, was synthesized via hydrothermal synthesis to access the fundamental corrosion mechanism and the according corrosive sites. X-ray photoelectron spectros- copy (XPS) and X-ray diffraction (XRD) demonstrated that the failure of catalytic decomposition of methylene blue originated from the formation of soluble CdSO4 by oxidizing S2 of as-prepared CdS. High resolu- tion transmission electron microscopy (HRTEM) further identified the active sites in the V-shaped regions ofCdS nanoparticles, confirmed by the simulated electric field distribution. To rationally coat oxides on CdS, the right candidates and their thicknesses have been considered by our tunneling model with trans- fer matrix method based on quantum mechanism, upon which the thickness of protective layer should be less than 0.5 nm to maintain a high tunneling probability, and thus one cycle of ALD TiO2 or AbO3 was proposed to passivate the CdS powder to balance the carrier transportation and corrosion suppres- sion. Based on HRTEM results, we found that the active V-shaped region was covered by ALD oxides (TiO2 or AbO3). For each case, no soluble CdSO4 has been found before and after photocatalytic reactions based XPS measurements. Importantly, we noticed that with the passivation of one cycle of ALD, the catalyst's lifetime was elongated up to 〉14 times higher than that of the as-prepared CdS.展开更多
基金National Key Basic Research Program of China(2013CB328701)National Natural Science Foundation of China(NSFC)(61322508,11504270)
文摘Optical whispering gallery microcavities with high-quality factors have shown great potential toward achieveing ultrahigh-sensitivity sensing up to a single molecule or nanoparticle, which raises a huge demand on a deep theoretical insight into the crucial phenomena such as the mode shift, mode splitting, and mode broadening in sensing experiments. Here we propose an intuitive model to analyze these phenomena from the viewpoint of the nanoparticle-induced multiple scattering of the azimuthally propagating mode(APM). The model unveils explicit relations between these phenomena and the phase change and energy loss of the APM when scattered at the nanoparticle; the model also explains the observed polarization-dependent preservation of one resonance and the particle-dependent redshift or blueshift. The model indicates that the particle-induced coupling between the pair of unperturbed degenerate whispering gallery modes(WGMs) and the coupling between the WGMs and the free-space radiation modes, which are widely adopted in current theoretical formalisms, are realized via the reflection and scattering-induced free-space radiation of the APM, respectively, and additionally exhibits the contribution of cross coupling between the unperturbed WGMs and other different WGMs to forming the splittingresonant modes, especially for large particles.
基金National Natural Science Foundation of China(62075104,61775105).
文摘The chiral coupling of an emitter to waveguide mode, i.e., the propagation direction of the excited waveguide mode is locked to the transverse spin(T-spin) of a circularly polarized emitter, has exhibited unprecedented applications in nanophotonics and quantum information processing. This chiral coupling can be largely enhanced in terms of unidirectivity, efficiency, and spontaneous emission rate by introducing resonant modes as coupling interfaces. However, this indirect chiral coupling still undergoes limitations in flexibility and miniaturization, and the underlying physical mechanisms are to be clarified. Here, we present an intuitive and rigorous approach for analyzing the direct/indirect chiral coupling, and thereout, derive some general relations between the chiralcoupling directionality and the T-spin of the field or emitter. Based on the theories, we propose an indirect chiral-coupling system on the platform of surface plasmon polariton(SPP), with a nanocavity supporting Fabry–Perot(FP) resonance of dual SPP modes serving as a novel coupling interface. The FP resonance provides flexible design freedoms which can modulate the chirality of the T-spin(and the resultant chiral-coupling directionality) to flip or disappear. A unidirectivity up to 99.9% along with a high coupling efficiency and enhancement of spontaneous emission rate is achieved. Two first-principles-based SPP models for the reciprocal and original problems are built up to verify the decisive role of the FP resonance in achieving the chiral coupling.The proposed theories and novel chiral-coupling interface will be beneficial to the design of more compact and flexible chiral-coupling systems for diverse applications.
基金supported by the National Natural Science Foundation of China(Nos.11304161,11104148,21573117,51171082,11404172 and 61322508)the 1000 Youth Talents Plan+2 种基金the Tianjin Natural Science Foundation(Nos.13JCYBJC41100 and 14JCZDJC37700)the National Basic Research Program of China(973 Program,Nos.2014CB931703 and 2013CB328701)the Fundamental Research Funds for the Central Universities
文摘Photo-corrosion is one of the major obstacles for CdS application in wet chemical fields, and atomic layer deposition (ALD) has been proposed as an effective way to suppress the corrosion. Here, prior to ALD coating, CdS, one facilely corrosive photocatalyst, was synthesized via hydrothermal synthesis to access the fundamental corrosion mechanism and the according corrosive sites. X-ray photoelectron spectros- copy (XPS) and X-ray diffraction (XRD) demonstrated that the failure of catalytic decomposition of methylene blue originated from the formation of soluble CdSO4 by oxidizing S2 of as-prepared CdS. High resolu- tion transmission electron microscopy (HRTEM) further identified the active sites in the V-shaped regions ofCdS nanoparticles, confirmed by the simulated electric field distribution. To rationally coat oxides on CdS, the right candidates and their thicknesses have been considered by our tunneling model with trans- fer matrix method based on quantum mechanism, upon which the thickness of protective layer should be less than 0.5 nm to maintain a high tunneling probability, and thus one cycle of ALD TiO2 or AbO3 was proposed to passivate the CdS powder to balance the carrier transportation and corrosion suppres- sion. Based on HRTEM results, we found that the active V-shaped region was covered by ALD oxides (TiO2 or AbO3). For each case, no soluble CdSO4 has been found before and after photocatalytic reactions based XPS measurements. Importantly, we noticed that with the passivation of one cycle of ALD, the catalyst's lifetime was elongated up to 〉14 times higher than that of the as-prepared CdS.