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.

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.

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.

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.

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.

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.

Highly two-photon and X-ray excited long-persistent luminescence in a crystalline host-guest aggregate

As a unique type of supramolecular self-assemblies,crystalline host-guest aggregates have attracted extensive interests in multiple application fields.Herein,a crystalline host-guest aggregate LIFM-HG1 was obtained with curcubit[8]uril as the host and carboxypyridinium salt as the guest.Single-crystal structural analysis indicates that the presence of abundant weak interactions in LIFM-HG1 provides a rigid environment for the guest molecule and effectively blocks the external quenchers.Spectral analysis and theoretical calculations confirm the presence of robust triplet energy levels in LIFM-HG1.Even more impressively,the intersystem crossing channels of the guest molecules are greatly opened up after the formation of the crystalline host-guest aggregate,resulting in a large k_(isc)of 6.70×10^(7)s^(−1)at room temperature for LIFM-HG1(which is∼0 for pure guest),leading to fascinatingmultichannel(including one-photon,two-photon,and X-ray)excited LPL properties.In addition,the crystalline LIFM-HG1 has a much higher triplet state luminescence efficiency under X-ray and two-photon excitation than that under single-photon excitation(A_(P)/A_(F)=86.8,44.8,10.7 under the three circumstances,respectively).And the phosphorescent emission intensity of LIFM-HG1 is 27.6 times higher than that of the crystalline guest under X-ray excitation.As a result,LIFM-HG1 shows a long afterglow retention time under both single-and two-photon excitation,and an impressive afterglow retention time of 1 s under X-ray excitation.Furthermore,the excellent lysosomal targeting and low cytotoxicity by the formation of host-guest aggregate makes LIFM-HG1 promising to be used as a novel lysosomal-targeted two-photon excited phosphorescent tracer.

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.

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 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.

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.

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.

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

Er^3＋ doped SrTiO3 ultrafine powders were prepared by solid state reaction in a molten NaCl flux. The structural properties were characterized by X-ray diffraction, field emission scanning electron microscopy, and Fourier transform infrared spectroscopy. The Stokes emission spectra of Er^3＋ in SrTiO3：Er^3＋ ranging from green to near infrared region were investigated under 514.5 nm laser excitation. The green and red upconverted luminescence spectra of Er^3＋ were measured under excitation into the 419/2 level by 785 nm laser. The upconversion mechanisms were studied in detail through laser power dependence and Er^3＋ ion concentration dependence of upconverted emissions, and results show that excited state absorption and energy transfer process are the possible mechanisms for the upconversion. The upconversion properties indicate that SrTiO3：Er^3＋ may be used in upconversion phosphors.

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.

Bias-Polarity Dependent Electroluminescence from a Single Platinum Phthalocyanine Molecule

By using scanning tunneling microscope induced luminescence(STML)technique,we investigate systematically the bias-polarity dependent electroluminescence behavior of a single platinum phthalocyanine(PtPc)molecule and the electron excitation mechanisms behind.The molecule is found to emit light at both bias polarities but with different emission energies.At negative excitation bias,only the fluorescence at 637 nm is observed,which originates from the LUMOtHOMO transition of the neutral PtPc molecule and exhibits stepwise-like increase in emission intensities over three different excitation-voltage regions.Strong fluorescence in region(I)is excited by the carrier injection mechanism with holes injected into the HOMO state first;moderate fluorescence in region(II)is excited by the inelastic electron scattering mechanism;and weak fluorescence in region(III)is associated with an up-conversion process and excited by a combined carrier injection and inelastic electron scattering mechanism involving a spintriplet relay state.At positive excitation bias,more-than-one emission peaks are observed and the excitation and emission mechanisms become complicated.The sharp moleculespecific emission peak at〜911 nm is attributed to the anionic emission of PtPc-originated from the LUMO+1 tLUMO transition,whose excitation is dominated by a carrier injection mechanism with electrons first injected into the LUMO+1 or higher-lying empty orbitals.

Ultra-stable near-infrared Tm^(3+)-doped upconversion nanoparticles for in vivo wide-field two-photon angiography with a low excitation intensity

Two-photon luminescence with near-infrared(NIR)excitation of upconversion nanoparticles(NPs)is of great importance in biological imaging due to deep penetration in high-scattering tissues,low auto-luminescence and good sectioning ability.Unfortunately,common two-photon luminescence is in visible band with an extremely high exciation power density,which limits its application.Here,we synthesized NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs with strong twophoton NIR emission and a low excitation power density.Furthermore,NaYF_(4):Yb/Tm@NaYF_(4)@SiO_(2)@OTMS@F127 NPs with high chemical stability were obtained by a modified multilayer coating method which was applied to upconversion NPs for thefirst time.In addition,it is shown that the as-prepared hydrophillic upconversion NPs have great biocompatibility and kept stable for 6 hours during in vivo whole-body imaging.The vessels with two-photon luminescence were clear even under an excitation power density as low as 25mW/cm^(2).Vivid visualizations of capillaries and vessels in a mouse brain were also obtained with low background and high contrast.Because of cheaper instruments and safer power density,the NIR two-photon luminescence of NaYF_(4):Yb/Tm@NaYF_(4)upconversion NPs could promote wider application of two-photon technology.The modified multilayer coating method could be widely used for upconversion NPs to increase the stable time of the in vivo circulation.Our work possesses a great potential for deep imaging and imaging-guided treatment in the future.

Luminescence of Eu(MBA)_2NO_3Phen Complexes

At 77 K excitation spectra,luminescence and time-resolved spectra of Eu(o-MBA)2NO3 Phen and Eu(m-MBA)2NO3 Phen (MBA:methylbenzoate,Phen 1,10-phenanthroline) complexes were measured. Spectral data show that because of steric effect of ortho-methyl substituent there occur two Eu3+ sites with slightly different chemical environment in the Eu(o-MBA)2NO3Phen complex.The local symmetnes for the central metal ions are C2v and C1,C2 or Cs,respectively.However,there is only one Eu3+ site in the Eut(m-MBA)2NO3Phen complex which is similar to the C2v Eu3+ site of the previous complex.This demonstrates that the Eu3+ ion can be used as a conformational probe in the solid state compounds.

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.