X-ray excited Mn^(2+)-doped persistent luminescence materials with biological window emission for in vivo bioimaging

In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity bioimaging.Transition metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window emission.Here,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence emission.After excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 h.More importantly.LYGM can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence emission.In addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in mice.After LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be achieved.After the persistent luminescence decays,LYGM can be re-excited for repeated imaging.Therefore,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.

Ultraviolet Super-Radiation Luminescence of Sputtering ZnO Film Under Cathode-Ray Excitation at Room Temperature

We report the observation of the cathode-ray(CR)pumped ultraviolet(UV)super-radiation luminescence in ZnO thin film at room temperature(RT).The dependence of UV(peak at about 390nm)and green(peak at about 520nm)luminescent peaks in ZnO thin film under CR excitation on excitation electron beam current has been investigated.With the increase of the density of excitation electron beam current,green peak relatively decreases and UV peak increases,resulting in a change of the luminescent color from green to blue-purple.The green peak intensity increases sublinearly with the increase of the electron beam current density and saturates at a relatively low density of electron beam current.But the intensity of 390nm UV peak increases superlinearly with the increase of the electron beam current density.This is a UV super-radiation luminescence of exciton in ZnO under high density pump.In this paper,three-dimensional atomic force microscope images of the surface of unannealled and annealled ZnO films are given.

Relaxation of Ne^(1+)1s^(0)2s^(2)2p^(6)np produced by resonant excitation of an ultraintense ultrafast x-ray pulse

The creation and relaxation of double K-hole states 1s^(0)2s^(2)2p^(6)np(n≥3)of Ne^(1+)in the interaction with ultraintense ultrafast x-ray pulses are theoretically investigated.The x-ray photon energies are selected so that x-rays first photoionize1s^(22)s^(22)p^(6) of a neon atom to create a single K-hole state of 1s2s^(22)p^(6) of Ne^(1+),which is further excited resonantly to double K-hole states of ls^(0)2s^(2)2p^(6)np(n≥3).A time-dependent rate equation is used to investigate the creation and relaxation processes of 1s^(0)2s^(2)2p^(6)np,where the primary microscopic atomic processes including photoexcitation,spontaneous radiation,photoionization and Auger decay are considered.The calculated Auger electron energy spectra are compared with recent experimental results,which shows good agreement.The relative intensity of Auger electrons is very sensitive to the photon energy and bandwidth of x-ray pulses,which could be used as a diagnostic tool for x-ray free electron laser and atom experiments.

Synthesis and Luminescence Properties of Ba2 MgSi2 O7 : Eu2+ under UV Excitation

Eu2+ activated pyrosilicate phosphor were prepared under a reducing atmosphere by solid-state reaction.The crystal structure of Ba2 MgSi2 O7: Eu2+ was analyzed by XRD method.The excitation spectrum of Ba2MgSi2 O7; Eu2+ is composed of two broad bands centered at about 310 nm and 395 nm respectively.In the emission spectra, the peak wavelength is at about 507 nm under 380 nm UV excitation.It was found that the introduction of Zn2+ into Ba2MgSi2O7: Eu2+ Can effectively increase its emission intensity without changing the position of emission peak.And the Eu2 + and Ce3 + codoped pyrosilicate phosphor is the efficient bluish green phosphor under the excitation of long UV light and its emission intensity is stronger than Eu2+ doped pyrosilicate phosphor.

Performance evaluation of the simpli¯ed spherical harmonics approximation for cone-beam X-ray luminescence computed tomography imaging

As an emerging molecular imaging modality,cone-beam X-ray luminescence computed tomog-raphy(CB-XLCT)uses X-ray-excitable probes to produce near-infrared(NIR)luminescence and then reconst ructs three-dimensional(3D)distribution of the probes from surface measurements.A proper photon-transportation model is critical to accuracy of XLCT.Here,we presented a systematic comparison between the common-used Monte Carlo model and simplified spherical harmonics(SPN).The performance of the two methods was evaluated over several main spec-trums using a known XLCT material.We designed both a global measurement based on the cosine similarity and a locally-averaged relative error,to quantitatively assess these methods.The results show that the SP_(3) could reach a good balance between the modeling accuracy and computational efficiency for all of the tested emission spectrums.Besides,the SP_(1)(which is equivalent to the difusion equation(DE))can be a reasonable alternative model for emission wavelength over 692nm.In vivo experiment further demonstrates the reconstruction perfor-mance of the SP:and DE.This study would provide a valuable guidance for modeling the photon-transportation in CB-XLCT.

Green, orange, and red upconversion luminescence in Nd^(3+)/Yb^(3+): Cs_2NaGdCl_6 powders under 785 nm laser excitation

Nd^3＋：Cs2NaGdCl6 and Nd^3＋, Yb^3＋：Cs2NaGdCl6 polycrystalline powder samples were prepared by Morss method E. Under 785 nm semiconductor laser pumping, the upconversion luminescence of Nd^3＋ ions in Cs2NaGdCl6 was investigated at room temperature, and three upconversion emissions near 538 nm （Green）, 603 nm （Orange）, and 675 nm （Red） were observed and assigned to ^4G7/2→^4I9/2, （^4G7/2→^4I11/2; ^4G5/2→^4I9/2）, and （^4G7/2→^4I13/2; ^4G5/2→^4I11/2 ）, respectively. The dependences of these upconverted emissions on laser power and Nd^3＋ ion concentration were investigated, to explore the upconversion mechanism. The effect of doping Yb^3＋ ions on the upconversion luminescence of Nd^3＋ in Cs2NaGdCl6 was also studied under 785 nm laser excitation. The energy transfer processes were discussed as the possible mechanism for the above upconversion emissions.

Preparation of NaYF_4:Er^(3+)/TiO_2 composite and up-conversion luminescence properties under visible light excitation

The up-conversion luminescence composite NaYF4：Er3＋/TiO2 is prepared using the sol-gel method. The specimen has good crystallinity and two shapes, i.e., viereck and round, while the sizes of viereck and round particles are both micron-sized. The TiO2 has an anatase structure, while the NaYF4 has a hexagonal phase, which can be hardly obtained through the common sol-gel method. Due to the big particle size and the high crystallinity of pure NaYF4： Er3＋, the composite has a small specific surface area that is less than Degussa P25 TiO2. The NaYF4：Er3＋/TiO2 composite shows several emission peaks at 211, 237, and 251 nm under the excitation of 388 nm, at 395 nm and 411 nm under the excitation of 500 nm, and at 467, 481,492, and 508 nm under the excitation of 570 nm.

Blue-shift of Nano-Y_2O_3 : Eu^(3+) Emission Spectra Excited by X-ray

Nano-Y_2O_3:Eu^(3+) powder was prepared by the homogeneous precipitation. With controlling the conditions of the reaction, nano powders with different grain size were obtained. It is found that the blue-shift phenomena exist in the nano-Y2O3:Eu3+ emission spectra excited by X-ray. The wave lengths of the peak (5D0→7F2) are related with the grain size of the powder

X-ray luminescence computed tomography:an emerging molecular imaging modality

X-ray luminescence computed tomography(XLCT) is an emerging hybrid imaging modality that can be used as a new tool in molecular imaging. XLCT has the potential to achieve the high spatial resolution of X-ray imaging and the high sensitivity feature of optical imaging in deep tissues. In XLCT,high energy X-ray photons are used to excite X-ray excitable particles emitting optical photons to be measured for reconstruction of the particle distribution inside tissues. Numerical simulations and experimental studies have been performed and proved that XLCT is suitable for in vivo small animal imaging. The aim of this review paper is to introduce the background of XLCT and to detail the concept of XLCT,including a brief review of tw o types of XLCT imaging system designs. The major challenges in the development of XLCT are also described. Finally,the future applications and development directions of XLCT are discussed.

Efficient production of ligand-free microscintillators at gram-scale for high-resolution X-ray luminescence imaging

The efficient production of high-quality scintillators with long radioluminescence afterglow is crucial for high-performance X-ray luminescence extension imaging.However,scaling-up the synthesis of ligand-free scintillators to fabricate large-area X-ray imaging screens for industrial applications remains a challenge.In this study,we report an efficient method to synthesize ligand-free,lanthanide-doped microscintillators by a one-pot reaction via the concentrated hydrothermal method.The as-synthesized microscintillators exhibit prolonged persistent radioluminescence for up to 30 days after X-ray exposure and remain high stability in air or water for more than 18 months without deterioration.Monte Carlo simulations indicate that the size effect is responsible for the excellent afterglow performance of the microscintillators.We employ these high-quality lanthanide-doped microscintillators to fabricate a large-area X-ray imaging detector using a blade-coating method,a spatial resolution of 24.9 lp/mm for X-ray imaging.Our study offers a solution for scaling-up the synthesis of low-cost microscintillators for practical applications.

Photoluminescent nickel(Ⅱ)carbene complexes with ligand-to-ligand charge-transfer excited states

While nickel(II)complexes have been widely used as catalysts for carbon-carbon coupling reactions,the exploration of their photophysical and photochemical properties is still in the infancy.Here,a series of square-planar Ni(II)complexes[(diNHC)NiX2]bearing chelating benzimidazole-based bis(N-heterocyclic carbene)ligands and varying anionic coligands(1,X=Cl;2,X=Br;3,X=I)are synthesized and structurally characterized.In solid state,both 1 and 2 exhibit orange-red photoluminescence under ambient conditions.The photophysical and electrochemical measurements along with density functional theory(DFT)calculations reveal that the low-energy emissions can be attributed to singlet excited states with ligand-to-ligand charge-transfer(LLCT)character.This work suggests that strong-field N-heterocyclic carbene ligands play a crucial role to achieve the luminescence of Ni(II)complexes.

Si _3O cluster:excited properties under external electric field and oxygen-deficient defect models

This paper investigates the excited states of Si3O molecule by using the single-excitation configuration interaction and density functional theory. It finds that the visible light absorption spectrum of Si3O molecule comprises the yellow and the purple light without external electric field, however all the visible light is included except the green light under the action of external electric field. Oxygen-deficient defects, which also can be found in Si3O molecule, have been used to explain the 1 from silicon-based materials but the microstructures of the materials are still uncertain Our results accord with the experimental values perfectly, this fact suggests that the structure of Si3O molecule is expected to be one of the main basic structures of the materials, so the oxygen-deficient defect structural model for Si3O molecule also has been provided to research the structures of materials.

Efficient and Fast X-Ray Luminescence in Organic Phosphors Through High-Level Triplet-Singlet Reverse Intersystem Crossing

Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation detection.However,the nature of triplet-singlet spinforbidden transitions in these materials often result in long-lived phosphorescence,which is undesirable for ultrafast X-ray detection and imaging.Here we demonstrate that the effect of hybridized local and charge-transfer(HLCT)excited states enables organic scintillators to exhibit highly efficient and fast radioluminescence(RL)in response to X-ray irradiation.Our experimental and theoretical investigation shows that the oxidized 1,8-naphthalimide-phenothiazine dyad(OMNI-PTZ 2)with HLCT-excited states has an enhanced overlap integral of the highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)on MNIπ-orbitals,and moderate donor–acceptor electron interactions.As a result,the RL of these crystals exhibits a 61-fold increase and its monoexponential decay lifetime is three orders of magnitude faster compared to its corresponding thermally activated delayed fluorescence(TADF)molecule MNI-PTZ 1.We further demonstrate the practical utility of the OMNI-PTZ 2(G)in high-performance X-ray detection and imaging,achieving an X-ray dose sensitivity of 97 nGy s−1 and an exceptional spatial resolution of 20 lp/mm.Our study provides a promising molecular design principle for utilizing triplet excitons to develop high-efficiency and fast X-ray scintillators for the development of next-generation flexible and stretchable X-ray imaging detectors.

Near Infrared Photoluminescence from Yb,Al Co-implanted SiO2 Films on Silicon

Intense room-temperature near infrared （NIR） photoluminescence （980 nm and 1032 nm） is observed from Yb,Al co-implanted SiO2 films on silicon. The optical transitions occur between the ^2F5/2 and ^2F7/2 levels of Yb^3＋ in SiO2. The additional Al-implantation into SiO2 films can effectively improve the concentration quenching effect of Yb^3＋ in SiO2. Photoluminescence excitation spectroscopy shows that the NIR photoluminescence is due to the non-radiative energy transfer from Al-implantation-induced non-bridging oxygen hole defects in SiO2 to Yb^3＋ in the Yb-related luminescent complexes. It is believed that the defect-mediated luminescence of rare-earth ions in SiO2 is very effective.

Research of Luminescence Properties on MO-RE2 O3 -B2 O3: Eu, Mn(M=Mg, Ca, Sr; RE=Y, La, Gd)

A series of phosphor of MO-RE2 O3-B2 O3: Eu, Mn ( M = Mg, Ca, Sr; RE = Y, La, Gd) were prepared and studied.Excitation spectra exhibited high absorption in UV region (370 ～ 400 nm).There existed two valence states for europium ions Eu2+ and Eu 3+, the broad emission band peaking at 515 nm correspond to the 5d-4f emission transition of Eu2+ , the sharp emission peaking at 590 and 610 nm correspond to the 5D0→7FJ(J = 1,2,3,4) emission transition of Eu 3 + By the introduction of Mg and Y into MO-RE2O3-B2O3: Eu, blue-green emission was restrained ultimately and red emission peaking at 610 nm was enhanced strongly, intensity and colorimetric purity of red light were both enhanced.Furthermore, Mg1-xSrxO-Y2O3-B2O3: Eu was also researched, the introduction of Sr into MgO-Y2O3-B2O3:Eu gives rise to a shift to longer wavelengths of the position of the excitation peak, and the emission spectra varies with the increasing of x simultaneously.

Luminescence property of Eu-doped fluorochlorozirconate glass-ceramics

A series of Eu2＋-doped fluorochlorozirconate glass-ceramics were prepared by solid state reaction method. X-ray diffraction, pho- toluminescence, photo-stimulated luminescence （PSL） and the turbidity of fluorozirconate glass containing BaCl2 nano- and micro-crystals were measured for the samples annealed at 290℃ for 10 rain The PSL was attributed to the characteristic emission of Eu2＋ in nano-crystallites of BaCI2, which formed in the glass upon annealing. The PSL efficiency of the glass ceramic was increased by increasing the concentration of BaCl2, which, however, resulted in the decreasing in the transparency of the sample. The sample turned to a semi-transparent glass ceramic or even an opaque and milky white one from a near-transparent glass. The trade-off between optical transparency and PSL intensity over different concentrations of BaCl2 for X-ray imaging plate applications was briefly discussed.

Upconversion Luminescence of SrTiO3：Er^3＋ Ultrafine Powders Produced by 785 nm Laser

Er3+ 做的 SrTiO3 极其细小的粉末被稳固的州的反应在熔融的 NaCl 流动准备。结构的性质被 X 光检查衍射，地排放扫描电子显微镜学，和 Fourier 变换描绘红外线的光谱学。在 SrTiO3 的 Er3+ 的 Stokes 排放系列：从绿色接近红外线的区域的 Er3+ 在 514.5 nm 激光刺激下面被调查。Er3+ 的绿、红的 upconverted 光系列被 785 nm 激光在刺激下面测量进 4I9/2 水平。upconversion 机制通过激光力量依赖和 upconverted 排出物的 Er3+ 离子集中依赖详细被学习，并且结果证明激动的州的吸收和精力转移过程是为 upconversion 的可能的机制。upconversion 性质显示那 SrTiO3 :Er3+ 可以在 upconversion 黄磷被使用。

Triangle Type Trinuclear Copper Complexes with Triplet-excitation Luminescent Property, an Ab Initio Study

The luminescent mechanism and properties of a triangular Cu（I） complex, （CuPz）3. have been studied by CIS method. The ground and lowest triplet excitation state geometries were optimized at MP2/SBKJC and CIS/SBKJC levels, respectively. A remarkable geometry distortion of the lowest triplet state was found and believed to cause the emission spectra to red shift.

Photoluminescence from Erbium-Implanted Silicon-Rich SiO_(2)

Si-rich SiO_(2) films were deposited by plasma-enhanced chemical vapor deposition on the silicon substrates,and then implanted with 1×10^(15)cm^(-2) 400 keV Er ions.After annealing at 800℃ for 5 min,the samples show room temperature luminescence around 1.54μm,characteristic of intra-4f emission from Er^(3+),upon excitation using an Ar ion laser.

Low thermal expansion and broad band photoluminescence of Zr0.1Al1.9Mo2.9V0.1O12

A new material of Zr0.1Al1.9Mo2.9V0.1O12 is synthesized by the traditional solid state synthesis method.The phase transition,coefficient of thermal expansion,and luminescence properties of Zr0.1Al1.9Mo2.9V0.1O12 are explored with Raman spectrometer,dilatometer,and x-ray diffraction(XRD)diffractometer.The results show that the Zr0.1Al1.9Mo2.9V0.1O12 possesses the strong broad-band luminescence characteristics almost in the whole visible region.The sample is crystallized in a monoclinic structure group of P21/a(No.14)crystallized at room temperature(RT).The crystal is changed from monoclinic to orthorhombic structure when the temperature increases to 463 K.The material has very low thermal expansion performance in a wide temperature range.Its excellent low thermal expansion and strong pale green light properties in a wide temperature range suggest its potential applications in light-emitting diode(LED)and other optoelectronic devices.