Isotope Effects on Two-Photon Population Transfer Processes of HF and DF

The isotope effects of XF （X=H, D） on the population transfer process via two-photon resonance excitation are investigated by solving the time-dependent SchrSdinger equation. The vibrational levels v=0 and 2 of the ground electronic state are taken to be the initial and target states, respectively, for the two molecular systems. The influences of the field peak amplitude and pulse duration on the population transfer process are discussed in detail. The pulse duration is required to be longer than 860 fs for the DF molecule to achieve a relatively high transfer probability （more than 80%）, while the one for the HF molecule is just required to be longer than 460 fs. Moreover, the intermediate level v=1 and the higher level v=3 may play more important roles in the two-photon resonance process for the DF molecule, compared to the roles in the process for the HF molecule.

Solvent effects on optical properties of a newly synthesized two-photon polymerization initiator： BPYPA

Time-dependent hybrid density functional theory in combination with polarized continuum model is applied to study the solvent effects on the geometrical and electronic structures as well as one- and two-photon absorption processes, of a newly synthesized asymmetrical charge-transfer organic molecule bis-（4-bromo-phenyl）-[4-（2-pyridin-4-yl-vinyl）phenyl]-amine （BPYPA）. There exist two charge-transfer states for the compound in visible region. The two-photon absorption cross section calculated by a three-state model and solvatochromic shift of the charge-transfer states are found to be solvent-dependent, where a nonmonotonic behaviour with respect to the polarity of the solvents is observed. The numerical results show that the organic molecule exhibits a rather large two-photon absorption cross section as compared with the compound 4-trans-[p-（N, N-Di-n-butylamino）-p-stilbenyl vinyl] pyridine （DBASVP） reported previously, and is predicted to be a good two-photon polymerization initiator. The hydrogen-bond effect is analysed. The computational results are in good agreement with the measurements.

The aggregation effects on the two-photon absorption properties of para-nitroaniline polymers by hydrogen-bond interactions

This paper has theoretically designed a series of aggregate polymers on the basis of several para-nitroaniline monomers by hydrogen-bond interactions. At the level of time-dependent hybrid density functional theory, it has optimized their geometrical structures and studied their two-photon absorption （TPA） properties by using analytical response theory. The calculated results exhibit that the aggregation effects not only bring out the conaiderable red shift of the excited energies but also greatly enhance the TPA intensities of the aggregate polymers in comparison with the para-nitroaniline monomer. The aggregate configurations also have an important influence on the TPA abilities of the polymers; the trimer has the largest TPA cross section. The electron transitions between the molecular orbits involving the strong TPA excitations of the trimer are depicted to illuminate the relationship between the intermolecular charge transfer and the TPA property.

Effect of Substitution Site on Two-Photon Absorption and Excited States Properties of Lipid Droplets Detection NAPBr Dyes:a Theoretical Perspective

Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated in detail.In this work,a series of new lipid droplets detection dyes are designed and studied,molecular optical properties and non-radiative transitions are analyzed.The intramolecular weak interaction and electron-hole analysis reveal its inner mechanisms.All dyes are proven to possess excellent photophysical properties with high fluorescence quantum efficiency and large stokes shift as well as remarkable two-photon absorption cross section.Our work reasonably elucidates the experimental measurements and the effects of substitution site on two-photon absorption and excited states properties of lipid droplets detection NAPBr dyes are highlighted,which could provide a theoretical perspective for designing efficient organic dyes for lipid droplets detection in biology and medicine fields.

Two-Photon Interference Constructed by Two Hong–Ou–Mandel Effects in One Mach-Zehnder Interferometer

We present a two-photon interference experiment in a modified Mach-Zehnder （MZ） interferometer in which two Hong-Ou-Mandel effects occur in tandem and construct superposed two-photon states. The signal photons pass both the arms of the MZ interferometer while the idler photons pass one arm only. Interestingly, the probability of the idler photons emerging from any output port still shows a sine oscillation with the two-photon phase difference and it can be characterized only by the indistinguishability of the two-photon amplitudes. We also observe a two-photon interference pattern with a period being equal to the wavelength of the parametric photons instead of the two-photon photonie de Broglie wavelength due to the presence of two-photon phase difference, in particular, with complementary probabilities of finding the two-photon pairs in two output ports. The abundant observations can facilitate a more comprehensive understanding of the two-photon interference.

Incoherently Coupled Grey-Grey Spatial Soliton Pairs in Biased Two-Photon Photovoltaic Photorefractive Crystals

The incoherently coupled grey-grey screening-photovoltaic spatial soliton pairs are predicted in biased two-photon photovoltaic photorefractive crystals under steady-state conditions. These grey-grey screening-photovoltaic soliton pairs can be established provided that the incident beams have the same polarization, wavelength, and are mutually incoherent. The grey-grey screening-photovoltaic soliton pairs can be considered as the united form of grey- grey screening soliton pairs and open or closed-circuit grey-grey photovoltaic soliton pairs.

Two-photon absorption properties of aggregation systems on the basis of (E)-4-(2-nitrovinyl) benzenamine molecules

Aggregation effect caused by the intermolecular hydrogen-bonding interactions on two-photon absorption prop- erties of （E）-4-（2-nitrovinyl） benzenamine molecules is studied at a hybrid density functional level. The geometry optimization studies indicate that there exist two probable conformations for the dimers and three for the trimers. A strong red-shift of the charge-transfer states is shown. The two-photon absorption cross sections of the molecule for certain conformations are greatly enhanced by the aggregation effect, from which a ratio of 1.0：2.6：3.6 is found for the molecule and its dimer and trimer with nearly planar structures. Namely, a 30 or 20 percent increase of the two-photon absorption cross section is observed.

Temporal Behavior of Low-Amplitude Grey Spatial Solitons in Biased Two-Photon Photorefractive Crystals

The temporal property of grey screening spatial solitons due to two-photon photorefractive effect in lowamplitude regime is analyzed. The results indicate that a broad solitons is generated at the beginning, and as time evolves, the intensity width of grey solitons decreases monotonically to a minimum value toward steady state. In the same propagation time, the FWHM of solitons decreases with p increasing or m decreasing. Moreover, the formation time of solitons is independent of p and m. The time is close to a constant determined by the dielectric relaxation time.

Photoacoustic effect invokes auditory response in infrared neuron stimulation

Infrared neuron stimulation is regarded as an innovative approach for stimulating cochleae in animals while the exact mechanism still remains unknown.In this paper,we studied compound action potentials of guinea pig cochleae with chronic or acute deafness.We recorded optical compound action potentials and analyzed stretched cochlear preparations by fiuorescence microscopy.Photoacoustic signals were measured by hydrophone and microphone,respectively.In our experiment,we observed a switch response effect in vitro and in vivo experiments.Therefore,we proposed photoacoustic effect could invoke auditory response in infrared neuron stimulation.

Compensation of Finite Bandwidth Effect by Using an Optimal Filter in Photoacoustic Imaging

Most existing reconstruction algorithms for photoacoustic imaging (PAI) assume that transducers used to receive ultrasound signals have infinite bandwidth. When transducers with finite bandwidth are used, this assumption may result in reduction of the imaging contrast and distortions of reconstructed images. In this paper, we propose a novel method to compensate the finite bandwidth effect in PAI by using an optimal filter in the Fourier domain. Simulation results demonstrate that the use of this method can improve the contrast of the reconstructed images with finite-bandwidth ultrasound transducers.

An analysis of As_2S_3 chirped fiber grating formed by two-photon absorption effect

When femtosecond laser pulses interfere with chirped femtosecond laser pulses in As2S3 fiber, a chirped fiber grating is formed. An analytical expression is given to describe the chirped grating, and its Bragg reflectivity is calculated. Because of the high photosensitive effect of As2S3 material, the chirped fiber grating has a wide Bragg reflective spectrum and high reflectivity by choosing proper parameters. This indicates that the chirped fiber grating can be used as a stretcher in the femtosecond chirped pulse amplification (CPA) system.

Indocyanine green loaded graphene oxide for high-e±cient photoacoustic tumor therapy

Photoacoustic therapy,using the photoacoustic efect of agents for selectively kling tumor cells,has shown pronising for treat ing tumor.Utilization of high optical absorption probes can help to effectively improve the photoacoustic ther apy efficiency.Herein,we report a novel high-absorpt:ion photoacoustic probe that is composed of indocyanine green(ICG)and gr aphene oxide(GO),entitled GO-ICG,for photoacoustic ther apy.The attached ICG with narrow absorption spectral profile has strong optical absorption in the infrared region.The absorption spectrum of the GO-ICG solution reveals that the GO-ICG particles exhibited a 10-fold higher absorbance at 780 nm(its peak absorbance)as compared with GO.Importantly,ICG's fluorescence is quenched by GO via fuorescence resonance energy transfer.As a result,GO-ICG can high efficiently convert the absorbed light energy to acoustic wave under pulsed laser irradiation.We further demonstrate that GO-ICG can produce stronger photoacoustic wave than the GO and ICG alone.Moreover,we conjugate this contrast agent with integrin 0。As mono dlonal antibody to molecularly target the U87-MG human glioblastoma cells for selective tumor cell killing.Finally,our results testify that the photoacoustic therapy eficiency of GO-ICG is higher than the existing photoacoustic therapy agent.Our work demonstrates that GO-ICG is a high efficiency photo-acoustic therapy agent.This novel photoacoustic probe is likely to be an available candidate for tumor therapy.

Photoacoustic Detection in the Michelson Interferometer Cavity

For the first time, we report photoacoustic (PA) signal detection in a cell placed within the Michelson interferometer cavity in an attempt to relate photoacoustic effect to the Michelson fringe shift as a result of changes in the cell. Both detection schemes were investigated using IR absorption and their sensitivities compared. Signals related to Michelson interferometer fringe and PA effect have shown good correlations with each other using different samples including some essential oils and their corresponding plant part from which the essential oil is usually obtained. Results were encouraging and will open the door widely to use the combined Michelson interferometer-photoacoustic spectroscopy (PAS) in trace gas detection for different applications.

Interstitial photoacoustic technique and computational simulation for temperature distribution and tissue optical properties in interstitial laser photothermal interaction

Interstitial laser immunotherapy(ILIT)is designed to use photothermal and immunological inter-actions for treatment of metastatic cancers.The photothermal ffect is crucial in inducing anti-tumorimmune responses in the host.Tissue temperature and tssue optical properties are important factorsin this process.In this study,a device combining interstitial photoacoustic(PA)technique andinterstitial laser photothermal interaction is proposed.Together with computational simulation,thisdevice was designed to determine temperature distributions and tissue optical properties during lasertreatment.Experiments were performed usinger-ivoFporcine liver tissue.Our results demonstratedthat interstitial PA signal amplitude was linearly dependent on tisue temperature in the tempera-ture ranges of 20-60℃,as wll as 65-80℃,with a dfferent slope,due to the change of tissue opticalproperties.Using the directly measured temperature in the tissue around the interstitial optical fiberdiffusion tip for calibration,the theoretical temperature distribution predicted by the bioheatequation was used to extract optical properties of tssue.Finally,the three-dimensional temperature distribution was simulated to guide tumor destruction and immunological stimulation,Thus,thisnovel device and method could be used for monitoring and controlling ILIT for cancer treatment.

Detecting Photoacoustic Signals of Sulfur Hexafluoride at Varying Microphone Positions

Photoacoustic spectroscopy was used to test the photoacoustic properties of sulfur hexafluoride, an optically thick and potent greenhouse gas. While exploring the photoacoustic effect of sulfur hexafluoride, the effects of the position of the microphone within a gas cell were determined. Using a 35 cm gas cell, microphones were positioned at 17.5 cm, the middle of the gas cell, 12.5 cm, 7.5 cm, and 2.5 cm from the window of the cell. From the photoacoustic signal produced for each resonance frequency at each microphone position, the effects of acoustic pressure produced at each position on the signal recorded were observed. This is the first study done by experimentation with the photoacoustic effect to show that standing waves have different amplitudes at different microphone positions.

基于碳纳米管和聚二甲基硅氧烷的光声换能器研究

为探究激光参数、光声转换层厚度对光声换能器输出声压的影响,本研究通过COMSOL仿真软件建立了光声换能器的物理模型。首先,基于聚二甲基硅氧烷(polydimethylsiloxane, PDMS)和碳纳米管(carbon nanotube, CNT)分别建立CNT、CNT-PDMS转换层模型;其次,改变激光脉冲持续时间和转换层厚度,对转换层输出声压进行测量;最后,对激光脉冲持续时间和转换层厚度所引起换能器输出声压强度的改变进行分析。结果表明,当CNT和CNT-PDMS转换层的厚度均为200μm、激光脉冲持续时间分别在10~30 ns和50 ns左右时,换能器能输出较高声压强度的超声波。仿真结果对光声换能器的研究有一定的指导意义。

Heavy-atom engineered hypoxia-responsive probes for precisive photoacoustic imaging and cancer therapy

Photoacoustic agents combining photodynamic therapy(PDT) and photothermal therapy(PTT) functions have emerged as potent theranostic agents for combating cancer. The molecular approaches for enhancing the near-infrared(NIR)-absorption and maximizing non-radiative energy transfer are essential for effective photoacoustic imaging(PAI) and therapy applications. In addition, such molecules with high specificity and affinity to cancer cells are urgently needed, which would further decrease the side effect during treatments. In this study, we applied a heavy-atom engineering strategy and introduced p-aminophenol,-thio, and-seleno moieties into NIR heptamethine cyanine(Cy7) skeleton(Cy7-X-NH_(2), X = O, S, Se) to significantly increase photothermal conversion efficiency for PTT and promote intersystem crossing for PDT.Additionally, we designed a series of nitroreductase(NTR)-activated photoacoustic probes(Cy7-X-NO_(2),X = O, S, Se), and target hypoxic tumors with NTR overexpression. Our prostate cancer targeting probe,Cy7-Se-NO_(2)-KUE, exhibited specific tumor photoacoustic signals and effective tumor killing through outstanding synergistic PTT/PDT in vivo. These findings highlighted a versatile strategy for cancer photoacoustic diagnosis and enhanced phototherapy.

Ligand-dependent aggregation-enhanced photoacoustic of atomically precise metal nanocluster

Atomically precise metal nanoclusters(MNCs),as a potential type of photoacoustic(PA)contrast agent,are limited in application due to their low PA conversion efficiency(PACE).Here,with hydrophilic Au25SR18(SR=thiolate)as model NCs,we present a result that weakly polar solvent induces aggregation,which effectively enhances PA intensity and PACE.The PA intensity and PACE are highly dependent on the degree of aggregation,while the aggregation-enhanced PA intensity(AEPA)positively correlates to the protected ligands.Such an AEPA phenomenon indicates that aggregation actually accelerates the intramolecular motion of Au NCs,and enlarges the proportion of excited state energy dissipated through vibrational relaxation.This result conflicts with the restriction of intramolecular motion mechanism of aggregation-induced emission.Further experiments show that the increased energy of AEPA originates from the aggregation inhibiting the intermolecular energy transfer from excited Au NCs to their surrounding medium molecules,including solvent molecule and dissolved oxygen,rather than restricting radiative relaxations.This study develops a new strategy for enhancing the PA intensity of Au NCs,and contributes to a deeper understanding of the origin of the PA signal and the excited state energy dissipation processes for MNCs.

Responsive mechanism of three novel hypochlorous acid fluorescent probes and solvent effect on their sensing performance

Optical properties and responsive mechanisms of three newly synthesized fluorescent probes for hypochlorous acid （HOC1） are investigated by employing time-dependent density functional theory. The computational results show that the absorption and emission properties of these probes change obviously when they react with hypochlorous acid. It is found that the probe FHZ has the best performance according to the probing behavior. Moreover, the responsive mechanisms of the probes are studied by analyzing the distributions of molecular orbitals and charge transfer, which are shown as the photon- induced electron transfer （PET） for FHZ and the intramolecular charge transfer OCT） for the other two probes. Specially, solvent effect on optical properties of the probe FHZ before and after reaction is studied within the polarizable continuum model （PCM）. It is shown that performance of the probe depends crucially on the solvent polarity. Our computational results agree well with the experimental measurement, and provide information for design of efficient two-photon fluorescent probes.

Solvent effects on structure and optical properties of a D-π-A azobenzene dye

Time-dependent hybrid density functional theory in combination with Onsager reaction field model and super-molecular model has been applied to study solvent effects on the geometrical and electronic structures, as well as one/two-photon absorption properties, of 4-（N-（2-hydroxyethyl）-N-methyl）-amino-4＇-nitroazobenzene. It is found that the short-range interaction has a large effect on the electronic structure of the solute molecule, namely, large red-shift of the maximum one-photon absorption is induced by hydrogen bonding. The solute molecule has a large two-photon absorption cross section, which is enhanced by the solvent effect. The computational results are in good agreement with measurements.