Cherenkov Radiation-Mediated In?Situ Excitation of Discrete Luminescent Lanthanide Complexes.
ABSTRACT: Lanthanide luminescence, while ideal for in?vivo applications owing to sharp emission bands within the optical window, requires high-intensity, short-wavelength excitation of small organic "antenna" chromophores in the vicinity of the lanthanide complex to access excited f-orbital states through intersystem crossing. Herein, we explored Cherenkov radiation of the radioisotopes 18 F and 89 Zr as an in?situ source of antenna excitation. The effective inter- and intramolecular excitation of the terbium(III) complexes of a macrocylic polyaminocarboxylate ligand (hydration number (q)=0, quantum yield (?)=47?%) as well as its analogue functionalized to append an intramolecular Cherenkov excitation source (q=0.07, ?=63?%) was achieved. Using conventional small-animal fluorescence imaging equipment, we have determined a detection limit of 2.5?nmol of Tb(III) complex in presence of 10??Ci of 18 F or 89 Zr. Our system is the first demonstration of the optical imaging of discrete luminescent lanthanide complexes without external short-wave excitation.
Project description:Reversed Cherenkov radiation is the exotic electromagnetic radiation that is emitted in the opposite direction of moving charged particles in a left-handed material. Reversed Cherenkov radiation has not previously been observed, mainly due to the absence of both suitable all-metal left-handed materials for beam transport and suitable couplers for extracting the reversed Cherenkov radiation signal. In this paper, we develop an all-metal metamaterial, consisting of a square waveguide loaded with complementary electric split ring resonators. We demonstrate that this metamaterial exhibits a left-handed behaviour, and we directly observe the Cherenkov radiation emitted predominantly near the opposite direction to the movement of a single sheet electron beam bunch in the experiment. These observations confirm the reversed behaviour of Cherenkov radiation. The reversed Cherenkov radiation has many possible applications, such as novel vacuum electronic devices, particle detectors, accelerators and new types of plasmonic couplers.
Project description:Conventionally the Cherenkov sound is governed by orbital degrees of freedom and is excited by supersonic particles. Additionally, it usually has a forward nature with a conic geometry known as the Cherenkov cone whose axis is oriented along the supersonic particle motion. Here we predict Cherenkov sound of a unique nature entirely resulting from the electronic spin degree of freedom and demonstrate a fundamentally distinct Cherenkov effect originating from essentially subsonic electrons in two-dimensional gases with both Bychkov-Rashba and Dresselhaus spin-orbit interactions. Specifically, we show that the axis of the conventional forward Cherenkov cone gets a nontrivial quarter-turn and at the same time the sound distribution strongly localizes around this rotated axis being now orthogonal to the subsonic particle motion. Apart from its fundamentally appealing nature, the orthogonal Cherenkov sound could have applications in planar semiconductor technology combining spin and acoustic phenomena to develop, e.g., acoustic amplifiers or sound sources with a flexible spin dependent orientation of the sound propagation.
Project description:We report a modified two-dimensional Cherenkov radiation, which occurs on a high-index dielectric nano-film driven by uniformly moving electron-beam. It is essentially different from the ordinary Cherenkov radiation in that, in the nondispersive medium, it shows unique dispersion characteristics-the waves with higher frequencies radiate at larger Cherenkov angles. Its radiation frequency and direction are essentially determined by structure parameters as well as the beam-velocity. By means of fully electromagnetic simulations and theoretical analyses, we explored the mechanism and requirements of this radiation. This new Cherenkov radiation may lead to promising applications in a broad range of fields.
Project description:PURPOSE:Patients have reported sensations of seeing light flashes during radiation therapy, even with their eyes closed. These observations have been attributed to either direct excitation of retinal pigments or generation of Cherenkov light inside the eye. Both in vivo human and ex vivo animal eye imaging was used to confirm light intensity and spectra to determine its origin and overall observability. METHODS AND MATERIALS:A time-gated and intensified camera was used to capture light exiting the eye of a patient undergoing stereotactic radiosurgery in real time, thereby verifying the detectability of light through the pupil. These data were compared with follow-up mechanistic imaging of ex vivo animal eyes with thin radiation beams to evaluate emission spectra and signal intensity variation with anatomic depth. Angular dependency of light emission from the eye was also measured. RESULTS:Patient imaging showed that light generation in the eye during radiation therapy can be captured with a signal-to-noise ratio of 68. Irradiation of ex vivo eye samples confirmed that the spectrum matched that of Cherenkov emission and that signal intensity was largely homogeneous throughout the entire eye, from the cornea to the retina, with a slight maximum near 10 mm depth. Observation of the signal external to the eye was possible through the pupil from 0° to 90°, with a detected emission near 2500 photons per millisecond (during peak emission of the ON cycle of the pulsed delivery), which is over 2 orders of magnitude higher than the visible detection threshold. CONCLUSIONS:By quantifying the spectra and magnitude of the signal, we now have direct experimental observations that Cherenkov light is generated in the eye during radiation therapy and can contribute to perceived light flashes. Furthermore, this technique can be used to further study and measure phosphenes in the radiation therapy clinic.
Project description:Luminescent lanthanides provide a promising alternative to organic chromophores for cellular bioimaging and bioassay applications; efficacy is closely governed by their respective quantum yields. Conventionally utilized quantum-yield measurements for lanthanides are laborious and not amenable to rapid relative comparison of compound performance. Here, we introduce a high-throughput optical imaging method to determine and directly compare relative quantum yield using Cherenkov-radiation-mediated excitation of luminescent lanthanide complexes.
Project description:This work explores the sensitization of luminescent lanthanide Tb(3+) and Eu(3+) cations by the electronic structure of zinc sulfide (ZnS) semiconductor nanoparticles. Excitation spectra collected while monitoring the lanthanide emission bands reveal that the ZnS nanoparticles act as an antenna for the sensitization of Tb(3+) and Eu(3+). The mechanism of lanthanide ion luminescence sensitization is rationalized in terms of an energy and charge transfer between trap sites and is based on a semiempirical model, proposed by Dorenbos and co-workers (Dorenbos, P. J. Phys.: Condens. Matter 2003, 15, 8417-8434; J. Lumin. 2004, 108, 301-305; J. Lumin. 2005, 111, 89-104. Dorenbos, P.; van der Kolk, E. Appl. Phys. Lett. 2006, 89, 061122-1-061122-3; Opt. Mater. 2008, 30, 1052-1057. Dorenbos, P. J. Alloys Compd. 2009, 488, 568-573; references 1-6.) to describe the energy level scheme. This model implies that the mechanisms of luminescence sensitization of Tb(3+) and Eu(3+) in ZnS nanoparticles are different; namely, Tb(3+) acts as a hole trap, whereas Eu(3+) acts as an electron trap. Further testing of this model is made by extending the studies from ZnS nanoparticles to other II-VI semiconductor materials; namely, CdSe, CdS, and ZnSe.
Project description:Low signal-to-noise ratios and limited imaging depths restrict the ability of optical-imaging modalities to detect and accurately quantify molecular emissions from tissue. Here, by using a scanning external X-ray beam from a clinical linear accelerator to induce Cherenkov excitation of luminescence in tissue, we demonstrate in vivo mapping of the oxygenation of tumours at depths of several millimetres, with submillimetre resolution and nanomolar sensitivity. This was achieved by scanning thin sheets of the X-ray beam orthogonally to the emission-detection plane, and by detecting the signal via a time-gated CCD camera synchronized to the radiation pulse. We also show with experiments using phantoms and with simulations that the performance of Cherenkov-excited luminescence scanned imaging (CELSI) is limited by beam size, scan geometry, probe concentration, radiation dose and tissue depth. CELSI might provide the highest sensitivity and resolution in the optical imaging of molecular tracers in vivo.
Project description:Cherenkov radiation is a ubiquitous phenomenon in nature. It describes electromagnetic radiation from a charged particle moving in a medium with a uniform velocity larger than the phase velocity of light in the same medium. Such a picture is typically adopted in the investigation of traditional Cherenkov radiation as well as its counterparts in different branches of physics, including nonlinear optics, spintronics and plasmonics. In these cases, the radiation emitted spreads along a "cone", making it impractical for most applications. Here, we employ a self-accelerating optical pump wave-packet to demonstrate controlled shaping of one type of generalized Cherenkov radiation - dispersive waves in optical fibers. We show that, by tuning the parameters of the wave-packet, the emitted waves can be judiciously compressed and focused at desired locations, paving the way to such control in any physical system.
Project description:The existence of reverse Cherenkov radiation for surface plasmons is demonstrated analytically. It is shown that in a metal-insulator-metal (MIM) waveguide, surface plasmon polaritons (SPPs) excited by an electron moving at a speed higher than the phase velocity of SPPs can generate Cherenkov radiation, which can be switched from forward to reverse direction by tuning the core thickness of the waveguide. Calculations are performed in both frequency and time domains, demonstrating that a radiation pattern with a backward-pointing radiation cone can be achieved at small waveguide core widths, with energy flow opposite to the wave vector of SPPs. Our study suggests the feasibility of generating and steering electron radiation in simple plasmonic systems, opening the gate for various applications such as velocity-selective particle detections.
Project description:Exciton-polaritons in semiconductor microcavities form a highly nonlinear platform to study a variety of effects interfacing optical, condensed matter, quantum and statistical physics. We show that the complex polariton patterns generated by picosecond pulses in microcavity wire waveguides can be understood as the Cherenkov radiation emitted by bright polariton solitons, which is enabled by the unique microcavity polariton dispersion, which has momentum intervals with positive and negative group velocities. Unlike in optical fibres and semiconductor waveguides, we observe that the microcavity wire Cherenkov radiation is predominantly emitted with negative group velocity and therefore propagates backwards relative to the propagation direction of the emitting soliton. We have developed a theory of the microcavity wire polariton solitons and of their Cherenkov radiation and conducted a series of experiments, where we have measured polariton-soliton pulse compression, pulse breaking and emission of the backward Cherenkov radiation.