Wavelength-and ellipticity-dependent photoelectron spectra from multiphoton ionization of atoms

We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schr ¨odinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the(2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.

Quantitative analysis of collagen morphology in breast cancer from millimeter scale using multiphoton microscopy

The tumor microenvironment(TME)is now recognized as an important participant of tumor progression.As the most abundant extracellular matrix component in TME,collagen plays an important role in tumor development.The imaging study of collagen morphological feature in TME is of great significance for understanding the state of tumor.Multiphoton microscopy(MPM),based on second harmonic generation(SHG)and two-photon excitation fluorescence(TPEF),can be used to monitor the morphological changes of biological tissues without labeling.In this study,we used MPM for large-scale imaging of early invasive breast cancer from the tumor center to normal tissues far from the tumor.We found that there were signi¯cant di®erences in collagen morphology between breast cancer tumor boundary,near tumor transition region and normal tissues far from the tumor.Furthermore,the morphological feature of eight collagen¯bers was extracted to quantify the variation trend of collagen in three regions.These results may provide a new perspective for the optimal negative margin width of breast-conserving surgery and the understanding of tumor metastasis.

Assessing pathological features of breast cancer via the multimodal information of multiphoton and Raman imaging

For unveiling the pathological evolution of breast cancer, nonlinear multiphoton microscopic(MPM) and confocal Raman microspectral imaging(CRMI) techniques were both utilized to address the structural and constitutional characteristics of healthy(H), ductal carcinoma in situ(DCIS), and invasive ductal carcinoma(IDC) tissues. MPM-based techniques,including two-photon excited fluorescence(TPEF) and second harmonic generation(SHG), visualized label-free and the fine structure of breast tissue. Meanwhile, CRMI not only presented the chemical images of investigated samples with the K-mean cluster analysis method(KCA), but also pictured the distribution of components in the scanned area through univariate imaging. MPM images illustrated that the cancer cells first arranged around the basement membrane of the duct,then proliferated to fill the lumens of the duct, and finally broke through the basement membrane to infiltrate into the stroma.Although the Raman imaging failed to visualize the cell structure with high resolution, it explained spectroscopically the gradual increase of nucleic acid and protein components inside the ducts as cancer cells proliferated, and displayed the distribution pattern of each biological component during the evolution of breast cancer. Thus, the combination of MPM and CRMI provided new insights into the on-site pathological diagnosis of malignant breast cancer, also ensured technical support for the development of multimodal optical imaging techniques for precise histopathological analysis.

Multiphoton microscopy for tumor regression grading after neoadjuvant treatment for colorectal carcinoma

AIM: To evaluate the feasibility of using multiphoton microscopy(MPM) to assess a tumor regression grading(TRG) system.METHODS: Fresh specimens from seven patients with colorectal carcinoma undergoing neoadjuvant radiochemotherapy at the Fujian Medical University Union Hospital were obtained immediately after proctectomy.Specimens were serially sectioned(10 μm thickness) and used for MPM or stained with hematoxylin and eosin for comparison.Sections were imaged by MPM using 810 nm excitation, and images were collected in two wavelength channels corresponding to second-harmonic generation(SHG) and two-photon excited fluorescence(TPEF) signals.The ratio of these signal intensities was used to distinguish fibrosis from normal mucosal and serosal tissues.RESULTS: TRG of specimens assessed by MPMwere in complete agreement with histologic grading performed by a consulting pathologist.SHG and TPEF images clearly revealed collagen fibers and fragmented elastic fibers in the muscularis propria specimens following neoadjuvant radiochemotherapy.Additionally, blood vessel hyperplasia was observed as thickening and fibrosis of the intima and media, which was accompanied by minimal inflammatory cell infiltration.Furthermore, the SHG/TPEF ratio in stromal fibrosis(4.15 ± 0.58) was significantly higher than those in the normal submucosal(2.31 ± 0.52) and serosal(1.47 ± 0.10) tissues(P < 0.001 for both).Analysis of emission spectra from cancerous tumor cells revealed two peaks corresponding to nicotinamide adenine dinucleotide hydrogen and flavin adenine dinucleotide signals; the ratio of these values was 1.19 ± 0.02, which is close to a normal metabolic state.CONCLUSION: MPM can be used to perform realtime diagnosis of tumor response after neoadjuvant treatment, and can be applied to evaluate TRG.

MULTIPHOTON MICROSCOPY:A NEW APPROACH IN PHYSIOLOGICAL STUDIES AND PATHOLOGICAL DIAGNOSIS FOR OPHTHALMOLOGY

Multiphoton microscopy(MPM),with the advantages of improved penetration depth,decreased photo-damage,and optical sectioning capability,has become an indispensable tool for biomedical imaging.The combination of multiphoton fluorescence(MF)and second-harmonic generation(SHG)microscopy is particularly effective in imaging tissue structures of the ocular surface.This work is intended to be a review of advances that MPM has made in ophthalmic imaging.The MPM not only can be used for the label-free imaging of ocular structures,it can also be applied for investigating the morphological alterations in corneal pathologies,such as keratoconus,infected keratitis,and corneal scar.Furthermore,the corneal wound healing process after refractive surgical procedures such as conductive keratoplasty(CK)can also be studied with MPM.Finally,qualitative and quantitative SHG microscopy is effective for characterizing corneal thermal denaturation.With additional development,multiphoton imaging has the potential to be developed into an effective imaging technique for in vivo studies and clinical diagnosis in ophthalmology.

Understanding Tunneling Ionization of Atoms in Laser Fields using the Principle of Multiphoton Absorption

The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although great efforts have been carried out within semiclassical models, there are few discussions describing the multiphoton absorption process within a quantum framework. Comparing the results obtained with the time-dependent Schr?dinger equation(TDSE)and the Keldysh–Faisal–Reiss(KFR) theory, we study the nonperturbative effects of ionization dynamics beyond the KFR theory. The difference in momentum spectra between multiphoton and tunneling regimes is understood in a unified picture with virtual multiphoton absorption processes. For the multiphoton regime, the momentum spectra can be obtained by coherent interference of each periodic contribution. However, the interference of multiphoton absorption peaks will result in a complex structure of virtual multiphoton bands in the tunneling regime. It is shown that the virtual spectra will be almost continuous in the tunneling regime instead of the discrete levels found in the multiphoton regime. Finally, with a model combining the TDSE and the KFR theory,we try to understand the different effects of virtual multiphoton processes on ionization dynamics.

Multiphoton and tunneling ionization of atoms in an intense laser field

We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods, i.e., the numerical solution of the time-dependent SchrSdinger equation （TDSE）, the Perelomov-Popov Terent＇ev （PPT） theory, and the Ammosov-Delone-Krainov （ADK） theory. Our results show that laser intensity dependent ionization probabilities of several atoms （i.e., H, He, and Ne） obtained from the PPT theory accord quite well with the TDSE results both in the multiphoton and tunneling ionization regimes, while the ADK results fit well to the TDSE data only in the tunneling ionization regime. Our calculations also show that laser intensity dependent ionization probabilities of a H atom at three different laser wavelengths of 600 nm, 800 nm, and 1200 nm obtained from the PPT theory are also in good agreement with those from the TDSE, while the ADK theory fails to give the wavelength dependence of ionization probability. Only when the laser wavelength is long enough, will the results of ADK be close to those of TDSE.

Highly efficient avalanche multiphoton luminescence from coupled Au nanowires in the visible region

We report highly efficient avalanche multiphoton luminescence(MPL)from ordered-arrayed gold nanowires(NWs).The time-average excitation intensity I_(exc) is as low as 5.0-9.1 kW/cm^2.The intensity of avalanche MPL I_(MPL) is about 10~4 times larger than that of three-photon luminescence,the slope ■logI_(MPL)/■logI_(exc) of avalanche MPL reaches as high as 18.3 and the corresponding polarization dependence of I_(MPL) has a form of cos^(50)■_p.The emission dynamics of avalanche MPL and three-photon luminesc...

Non-perturbative multiphoton excitation studies in an excitonic coupled quantum well system using high-intensity THz laser fields

Multiphoton excitations and nonlinear optical properties of exciton states in GaAs/AlxGa1-xAs coupled quantum well structure have been theoretically investigated under the influence of a time-varying high-intensity terahertz(THz)laser field.Non-perturbative Floquet theory is employed to solve the time-dependent equation of motion for the laser-driven excitonic quantum well system.The response to the field parameters,such as intensity and frequency of the laser electric field on the state populations,can be used in various optical semiconductor device applications,such as photodetectors,sensors,all-optical switches,and terahertz emitters.

Photoelectron imaging of resonance-enhanced multiphoton ionization and above-threshold ionization of ammonia molecules in a strong 800-nm laser pulse

In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.

Laser-manipulated the of a harmonically multiphoton transitions trapped particle

A single particle magneto-confined in a one-dimensional （1D） quantum wire experiences a harmonic potential, and imposing a sharply focused laser beam on an appropriate site shapes a δ potential. The theoretical investigation has demonstrated that for a sufficiently strong δ pulse the quantum motional stationary state of the particle is one of the eigenstates of the free harmonic oscillator, and it is determined by the site of the laser beam uniquely, namely a quantum state is admissible if and only if the laser site is one of its nodes. The numerical computation shows that all the nodes of the lower energy states with quantum numbers n ≤ 20, except the coordinate origin, are mutually different. So we can manipulate the multiphoton transitions between the quantum states by adjusting the position of the laser δ pulse and realize the transition from an unknown higher excitation state to a required lower energy state.

Two-colour coherent control of multiphoton ionization： a comparison between long-range and short-range potential model atoms

Using the numerical solution of the time-dependent SchrSdinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atomic multiphoton ionization. It is found that the photoelectron spectra are obviously different for the long-range （Coulomb-like） and short-range （with no excited bound states） potential model atoms, which are produced by two-colour coherent control of atomic multiphoton ionization in a few laser cycles. Our results indicate that two-colour coherent control of atomic multiphoton ionization can be observed in simulations, depending on the choice of the model potentials.

Multiphoton resonant ionization of hydrogen atom exposed to two-colour laser pulses

This paper studies the multiphoton resonant ionization by two-colour laser pulses in the hydrogen atom by solving the time-dependent Schroedinger equation. By fixing the parameters of fundamental laser field and scanning the frequency of second laser field, it finds that the ionization probability shows several resonance peaks and is also much larger than the linear superposition of probabilities by applying two lasers separately. The enhancement of the ionization happens when the system is resonantly pumped to the excited states by absorbing two or more colour photons non-sequentially.

Multiphoton ionization of the hydrogen atom exposed to circularly or linearly polarized laser pulses

This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent SchrSdinger equation. It finds that the ratio of the ionization probabilities by linearly and circularly polarized laser pulses varies with the numbers of absorbing photons. With the same laser intensity, the circularly polarized laser pulse favors to ionize the atom with more ease than the linearly polarized laser pulse if only two or three photons are necessary to be absorbed. For the higher order multiphoton ionization, the linearly polarized laser pulse has the advantage over circularly polarized laser pulse to ionize the atom.

The polarization effect of a laser in multiphoton Compton scattering

The multiphoton Compton scattering in a high-intensity laser beam is studied by using the laser-dressed quantum electrodynamics （QED） method, which is a non-perturbative theory for the interaction between a plane electromagnetic field and a charged particle. In order to analyze in the real experimental condition, a Lorentz transformation for the cross section of this process is derived between the laboratory frame and the initial rest frame of electrons. The energy of the scattered photon is analyzed, as well as the cross sections for different laser intensities and polarizations and different electron velocities. The angular distribution of the emitted photon is investigated in a special velocity of the electron, in which for a fixed number of absorbed photons, the electron energy will not change after the scattering in the lab frame. We obtain the conclusion that higher laser intensifies suppress few-laser-photon absorption and enhance more-laser-photon absorption. A comparison between different polarizations is also made, and we find that the linearly polarized laser is more suitable to generate nonlinear Compton scattering.

Theory of multiphoton photoemission disclosing excited states in conduction band of individual TiO_(2) nanoparticles

A theory of multiphoton photoemission is derived to explain the experimentally observed monotonic decrease with the wavelength in the electron yield of TiO_(2) nanoparticles(NPs)by as large as four orders of magnitude.It is found that the fitting parameter corresponds to the energy position of Ti3d e_(g) and t_(2g) states,and the derived theory is a novel diagnostic of excited states in the conduction band,very importantly,applicable to individual NPs.The difference between four-photon slope NPs and three-photon slope NPs is attributed to the difference in defect density.The success of the theory in solving the puzzling result shows that thermal emission from high-lying levels may dominate over direct multiphoton ionization in solids when the photon number larger than four is required.

Utilizing multiphoton imaging and integrative clearing to reveal sex differences in neuroimmune interactions after nerve injury

With the constant development of multiphoton microscopy,our ability to observe complex and dynamic biological processes deeper within living tissue,is steadily improving.Researchers use multiphoton microscopy,because experiments can be conducted with little to no invasiveness or tissue damage over a long period of time with no photodamage(Mancuso et al.,2009).This allows for the introduction of tissue into the context of a three-dimensional 3D environment in which visualization of cellular activation and interaction is viable.By circumventing a distorted reconstruction with limited z-stacks,multiphoton imaging provides enhanced spatiotemporal resolution.

Scanless multitarget-matching multiphoton excitation fluorescence microscopy

Using the combination of a refective blazed grating and a reflective phase-only difractive spatiallight modulator(SLM),scanless multitarget-matching multiphoton excitation fuorescence mi.croscopy(SMTM-MP M)was achieved.The SLM shaped an incoming mode-locked,near-infraredTi:sapphire laser beam into an excitation pattern with addressable shapes and sizes that matchedthe samples of interest in the field of view.Temporal and spatial focusing were simultaneouslyrealized by combining an objective lens and a blazed grating.The fluorescence signal fromilluminated areas was recorded by a two-dimensional sCMOS camera.Compared with a conventional temporal focusing multiphoton microscope,our microscope achieved effective use of thelaser power and decreased photodamage with higher axial resolution.

MULTIPHOTON MICROSCOPIC IMAGING OF MOUSE INTESTINAL MUCOSA BASED ON TWO-PHOTON EXCITED FLUORESCENCE AND SECOND HARMONIC GENERATION

Multiphoton microscopy(MPM),based on two-photon excited fuorescence and second harmonic generation,enables direct noninvasive visualization of tissue architecture and cell morphology in live tissues without the administration of exogenous contrast agents.In this paper,we used MPM to image the microstructures of the mucosa in fresh,unfixed,and unstained intestinal tissue of mouse.The morphology and distribution of the main components in mucosa layer such as columnar cells,goblet cells,intestinal glands,and a little collagen fibers were clearly observed in MPM images,and then compared with standard H&:E images from paired specimens.Our results indicate that MPM combined with endoscopy and miniaturization probes has the potential application in the clinical diagnosis and in vivo monitoring of early intestinal cancer.

DIAGNOSTIC APPLICATION OF MULTIPHOTON MICROSCOPY IN EPITHELIAL TISSUES

Epithelial cancer comprises more than 85%of human cancers.The detection and treatment at the early stage has been demonstrated to apparently improve patient survival.In this review,we summarize our recent research works on the diagnostic application of epithelial tissue based on multiphoton microscopy(MPM),including identification of the layered structures of esophagus,oral cavity,skin and bronchus tissues,establishment of the diagnostic features for distinguishing gastric normal tissue from cancerous tissue,linking collagen alteration and ectocervical epithelial tumor progression for evaluating epithelial tumor progression,and differentiating normal,inflammatory,and dysplastic ectocervical epithelial tissues.These results provide the groundwork for developing MPM into clinical multiphoton endoscopy.