Photoemission Process Research Articles

Freezing non-radiative recombination in high-performance CsPbBr3 single crystal x-ray detector

Though CsPbBr3 single crystals (SCs) possess intriguing photoelectronic properties for x/γ-ray detection, the serious ion migration and high thermally activated carrier concentration at room temperature (RT), typically associated with defect states in CsPbBr3 crystals, result in a high dark current and drift of baseline, hindering their potential applications. In this investigation, liquid nitrogen cooling is proposed to freeze deep-level defects in CsPbBr3 SCs, thereby suppressing the ion migrations and decreasing the thermally excited carrier concentration. Utilizing photoluminescence (PL) and time-resolved PL spectra, coupled with theoretical models for photoexcitation and photoemission processes, the freezing of deep-level defects at liquid nitrogen temperature (LNT) is confirmed, which is conducive to decreasing non-radiative recombination. At LNT, the CsPbBr3 SC exhibits a higher resistivity of 4.95 × 1011 Ω cm and a higher mobility–lifetime product of 9.54 × 10−3 cm2 V−1, in contrast to the RT values of 3.86 × 109 Ω cm and 3.67 × 10−3 cm2 V−1, respectively. Furthermore, the x-ray detector at LNT exhibits a high sensitivity of 9309 μC Gyair−1 cm−2 and an impressively low detection limit of 0.054 nGy s−1, which offers a route for obtaining highly sensitive x-ray detectors for applications including ultra-low dose radiation imaging.

Attosecond ionic photoionization spectroscopy.

Photoionization is one of the most fundamental processes in light-matter interaction. Advanced attosecond photoelectron spectroscopy provides the possibility to characterize the ultrafast photoemission process in an extremely short attosecond time scale. Following scattering symmetry rules, residual ions encode ultrafast photoionization prints at the instant of electron removal forming an alternative electron emission chronoscope. Here, we experimentally illustrate the attosecond ion reconstruction of attosecond beating by interference of two-photon transition (RABBIT)-like interferometry through the development of high-resolution ion momentum detection in atomic photoionization processes. Our ion interferometry presents identical momentum- and time-dependent scattering phase shift, as we observed in photoelectron spectroscopy, and thus demonstrates that ion interferometry can be a possible alternative attosecond approach to resolve the photoionization process, without the electron homogeneity limitation.

Electron Imaging of Nanoscale Charge Distributions Induced by Femtosecond Light Pulses.

Surface charging is ubiquitously observable during in situ transmission electron microscopy of nonconducting specimens as a result of electron beam/sample interactions or optical stimuli and often limits the achievable image stability and spatial or spectral resolution. Here, we report on the electron-optical imaging of surface charging on a nanostructured surface following femtosecond multiphoton photoemission. By quantitatively extracting the light-induced electrostatic potential and studying the charging dynamics on relevant time scales, we gain insights into the details of the multiphoton photoemission process in the presence of an electrostatic background field. We study the interaction of the charge distribution with the high-energy electron beam and secondary electrons and propose a simple model to describe the interplay of electron- and light-induced processes. In addition, we demonstrate how to mitigate sample charging by simultaneously optically illuminating the sample.

Structural design and photoelectron emission characteristics of a new Cs2Te photocathode based on surface plasmon polaritons

Surface plasmon polaritons (SPPs) have been introduced into Cu and K2CsSb photocathodes to substantially improve their quantum efficiency, while no similar studies have been reported on Cs2Te photocathode. In this paper, SPPs were introduced into Cs2Te photocathode by means of micro-nano grating structure, which successfully stimulated local enhanced field to improve photon absorption rate and regulate initial distribution of the excited photoelectrons. In order to explore the effect of SPPs on the performance of Cs2Te photocathode, Monte Carlo method was used to simulate the photoemission process of Cs2Te photocathode before and after the introduction of SPPs. The results showed that the quantum efficiency of Cs2Te photocathode with SPPs was improved by 60% while the thermal emittance remained basically unchanged. The results are of great significance for the development of high-brightness electron sources that are required in the field of particle accelerators.

Copper Surface Treatment with deep UV Ultrafast Laser for Improved Photocathode Photoemissive Properties

Cesium Telluride (Cs2Te) constitutes today the photoemissive semiconductor material of choice for electron accelerators due to its high quantum efficiency (QE) in the deep ultraviolet (DUV) spectral range, and capability to produce high charge over a long operation lifetime. Unfortunately, its chemical instability requires ultra-high vacuum (in the 10-10 mbar range). This inevitably complicates Cs2Te photocathode handling, and increases the overall cost compared to metallic counterparts. Copper photocathodes are alternative candidates, and although they are much more tolerant in terms of vacuum requirements, their use in high average current photo-injectors is limited due to their orders of magnitude lower QE (around 10-5 per unit). With the development of nanophotonics, plasmonic phenomena can now be exploited to tailor a new range of effects in the photoemission process. In this work, we focus on direct laser fabrication of nanostructures for plasmonic electric-field enhancement on copper, and study their potential for enhancing the quantum yield. We develop a methodology to fabricate the nanostructures by irradiating the Cu surface with 257 nm femtosecond pulses, well above copper’s work function. We directly obtained nanostructures 100-200 nm, matching the plasmonic resonance for photoinjector wavelengths. The study is accompanied by a parametric scan allowing to obtain the optimal laser machining parameters, and the analysis of the nanostructure morphologies obtained.

Performance of laser patterned copper plasmonic photocathodes

We study ultrafast laser surface nanopatterning as an alternative to improve the photo-emissive properties of metallic photocathodes. By tailoring the physical dimensions of these surface nanostructures, one can localize the optical field intensity and exploit plasmonic effects occurring in such nanostructures. As a result, this surface nanopatterning technique can become a great tool for improving metallic photocathodes photoemission behavior enabling their use for next generation high brightness electron sources. Our goal is to investigate such surface-plasmon assisted photoemission processes with a view on simplifying the photocathode production at CERN while extending the lifetime of existing photoinjectors. The performance of two different femtosecond laser nanopatterned plasmonic photocathodes was analyzed by measuring the quantum yield with a 65kV DC electron gun utilizing 266nm laser excitation generated by a nanosecond laser with 5ns pulse duration and 10Hz repetition rate. By comparing the electron emission of the copper surface nanostructured areas with that of a flat area, our results suggest quantum yield enhancements of up to a factor of 5.

Information hidden behind a single peak in the C 1s spectrum of graphene on Ir(111)

The energy resolution that can be achieved in x-ray photoelectron spectroscopy experiments allows to disentangle the contribution arising from the presence of a large variety of surface atoms in non-equivalent configurations which manifests itself not only with the appearance of different spectral components, but also as unusual lineshape.In the present work, we show that the fit of the C 1s core level spectrum of graphene grown on Ir(111) realized using 200 peaks based on ab initio calculations, accounting for the non-equivalent C atoms in the 10×10 moiré cell, does not improve the fit quality with respect to the use of a single component. On the contrary, the quantitative fit quality can be drastically increased by introducing a dependency of the Lorentzian width on the distance between C and Ir first-layer atoms. This result is associated to the different electronic properties, and in particular to the different density of states of the σ and π bands, of C atoms sitting on TOP (hills) or FCC (valleys) regions of graphene which affect the lifetimes of the core-holes generated during the photoemission process.

Discharge Randomness and Attraction Process of Epoxy Surface on Discharge Channel in SF6 Gas Under Uniform Electric Field

It is generally believed that due to the electric field distortion effect and the photoemission process of the solid surface, the discharge channel near the solid surface trends to develop along the surface than that in bulk gas. One way to improve insulation performance is to avoid the solid surface from participating in the gas discharge process. However, the mechanism of the solid surface’s effect on the gas discharge process is still unclear. In this paper, we recorded high-speed framing pictures of the discharge process in SF6 gas near the epoxy surface under lightning impulse voltage in the uniform electric field. The arc pictures show that the attraction effect of the solid surface to the discharge channel is related to the surface shape, gas gap height, and distance from the discharge channel to the solid surface. Besides, discharge randomness also plays a role, which is more obvious in the cylinder insulator than in the conical insulator, for the surface with conical shape could easily attract and arrest the discharge channel to its surface. According to the pictures of discharge process near the cylinder surface, we found that the photoemission process occurs in the streamer stage but has little effect on the attraction effect. The leader initiates after the streamer bridges the gas gap, and its random stepped walk could induce the attraction effect from the solid surface: only when the random stepped leader deflects close to the solid surface, the discharge channel could be further attracted to the solid surface by the electrostatic force, especially its normal component. The result indicates that there are three points to prevent the solid surface from participating in the gas discharge process and further improve insulation performance: choose a cylinder shape (avoid a conical shape), keep the surface away from the high electric field area where discharge may start, and reduce the normal component of the surface electric field.

Geometry-Induced Spin Filtering in Photoemission Maps from WTe_{2} Surface States.

We demonstrate that an important quantum material WTe_{2} exhibits a new type of geometry-induced spin filtering effect in photoemission, stemming from low symmetry that is responsible for its exotic transport properties. Through the laser-driven spin-polarized angle-resolved photoemission Fermi surface mapping, we showcase highly asymmetric spin textures of electrons photoemitted from the surface states of WTe_{2}. Such asymmetries are not present in the initial state spin textures, which are bound by the time-reversal and crystal lattice mirror plane symmetries. The findings are reproduced qualitatively by theoretical modeling within the one-step model photoemission formalism. The effect could be understood within the free-electron final state model as an interference due to emission from different atomic sites. The observed effect is a manifestation of time-reversal symmetry breaking of the initial state in the photoemission process, and as such it cannot be eliminated, but only its magnitude influenced, by special experimental geometries.

Response to "Comment on 'Spin- and angle-resolved inverse photoemission setup with spin orientation independent from electron incidence angle'" [Rev. Sci. Instrum. 93, 093904 (2022)

We reply to the Comment by Donath et al. on our setup, which allows a total 3D control of the polarization direction of the electron beam in an inverse photoemission spectroscopy (IPES) experiment, a significant advance with respect to previous setups with partial polarization control. Donath et al. claim an incorrect operation of our setup after comparing their results, treated to enhance the spin asymmetry, with our spectra without the same treatment. They also equal spectra backgrounds instead of equaling peak intensities above the background. Thus, we compare our Cu(001) and Au(111) results with the literature. We reproduce previous results, including spin-up/spin-down spectral differences observed for Au and not observed for Cu. Also, spin-up/spin-down spectral differences appear at the expected reciprocal space regions. In the Comment, it is also stated that our tuning of the spin polarization misses the target because the spectra background changes when tuning the spin. We argue that the background change is irrelevant to IPES since the information is contained in peaks produced by primary electrons, those having conserved their energy in the inverse photoemission process. Second, our experiments agree with previous results from Donath et al. [Wissing et al., New J. Phys. 15, 105001 (2013)] and with a zero-order quantum-mechanical model of spins in vacuum. Deviations are explained by more realistic descriptions including the spin transmission through an interface. Consequently, the operation of our original setup is fully demonstrated. Our development corresponds to "the promising and rewarding angle-resolved IPES setup with the three-dimensional spin resolution," as indicated in the Comment, after our work.

Nanosecond Photoemission near the Potential Barrier of a Schottky Emitter

Nanosecond electron pulses are appealing for ultrafast imaging and electron-gating applications, where tunable currents and narrow energy spreads are desirable. Here, we demonstrate photoemission from a Schottky emitter triggered by nanosecond laser pulses. Using photon energies optimally tuned to the emission potential barrier, we generate pulses containing over ${10}^{5}$ electrons with energy spreads below 1 eV by means of a prompt single-photon photoemission process. These results are consistent with a theoretical model of laser-triggered electron emission and energetic broadening during propagation and can be widely implemented.

Wave Function of a Photoelectron and Its Collapse in the Photoemission Process

Wave Function of a Photoelectron and Its Collapse in the Photoemission Process

Multiple scattering description of multicenter coherent emission with applications to photoionization and electron scattering in diatomic molecules

In the light of a multiple scattering (MS) description of molecular photodiffraction and photoabsorption processes, we present an investigation of the interplay between initial state coherence and intramolecular scattering, leading to a reinterpretation of the molecular interference in diatomic molecules and in particular of the Cohen-Fano (CF) interference term in photoabsorption. Indeed, the delocalization of the initial state electron over different atoms at positions ${\mathbf{R}}_{n}$ introduces in the language of MS theory as many virtual emitters as there are atoms in the molecule, giving rise to new MS paths as compared to the case of a single emitter. Their emission amplitudes interfere via the usual phase factor ${e}^{i\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathbf{R}}_{n}}$ and in the case of two emitter photoemission describe how the usual picture of the microscopic Young's experiment is modified by the presence of intramolecular scattering. Photoabsorption follows from photoemission by integrating over the emission directions of the photoelectron and characterizes the CF oscillations as the remnants on the energy scale of the photoemission interference patterns introduced by the new paths joining the two centers, exactly like the extended x-ray absorption fine structure signals are the remnants of the closed paths that begin and end at the same atom. In the same context of initial state coherence we also show that the orientationally averaged scattering of electrons off small molecules can give access to CF type of oscillations, although in a more complicated way, due to the lack of site selectivity in comparison with the photoemission process and the absence of a dipole selection rule. It is shown that this type of modulation has the same physical origin as that found in photoabsorption.

Benzothioxanthene Dicarboximide as a Tuneable Electrogenerated Chemiluminescence Dye

AbstractOverlooked for years, the promising benzothioxanthene dicarboximide (BTXI) structure is nonetheless known to be an excellent fluorophore. As a further step towards the exploration of this rylene structure, the generation of electrochemiluminescence (ECL) in acetonitrile solutions is investigated herein as well as its direct comparison with a diphenylamine (DPA) derivative. Electrochemical characterization shows that the bare BTXI can be reversibly reduced or oxidized, characteristics which suggest the possibility that the electrogenerated reactive species can be exploited in the context of ECL. As a result, the BTXI moiety was found to be ECL‐active in both annihilation and co‐reactant mechanisms. Tri‐n‐propylamine (TPA) and benzoyl peroxide (BPO) were selected as sacrificial co‐reactants for promoting ECL. An ECL efficiency of 13 % (BTXI) and 6 % (BTXI‐DPA) compared to that of Ru(bpy)32+ was found when using TPA in oxidative ECL. Moreover, the ECL efficiency increased to 75 % and 55 % of Ru(bpy)32+ with BPO (i. e. reductive‐oxidation ECL) for BTXI and BTXI‐DPA, respectively. These results can be understood by calculating the free enthalpy of the redox reactions associated with each ECL pathway. Although the BTXI‐DPA red emitter exhibits more suitable thermodynamic properties, the BTXI green emitter is nonetheless more effective in combination with a co‐reactant due to a much larger photoluminescence quantum yield. The ECL spectra of the two molecules are compared to their photoluminescence spectra, revealing the involvement of the same excited states in the two different photoemission processes. In turn, the chemical engineering of BTXI is shown to be an effective platform for achieving tuneable ECL generation.

Electric field control of photoluminescence response in lanthanide doped ferroelectric materials: A brief review

Tuning the photoluminescence (PL) properties of lanthanide ions not only provides a deeper understanding of the luminescence mechanism, but also promotes its potential applications in lighting industry, volumetric 3 D display, biological assaying, and medical imaging. The traditional chemical strategies, such as changing the types or concentration of doped ions, changing the composition of host materials, changing the preparation process, etc, can easily adjust the photo excitation, energy transfer and emission processes, which have been widely employed. In spite of the strong ability to tune luminescence intensity and wavelength, these chemical methods are irreversible, which is difficult to observe the dynamic luminescence process and unfavorable for real applications. Recently, enabling in-situ, real-time and reversibly control PL response by the application of electric field has been realized through doping lanthanide ions into ferroelectric host materials. Herein, the electric field control of PL response in lanthanide doped ferroelectric bulks and thin films is summarized. The intrinsic luminescence mechanism under electric field and possible application directions in the future are discussed.

Influence of an atomic resonance on the coherent control of the photoionization process

In coherent control schemes, pathways connecting an initial and a final state can be independently controlled by manipulating the complex amplitudes of their transition matrix elements. For paths characterized by the absorption of multiple photons, these quantities depend on the magnitude and phase between the intermediate steps, and are expected to be strongly affected by the presence of resonances. We investigate the coherent control of the photoemission process in neon using a phase-controlled two-color extreme ultraviolet pulse with frequency in proximity of an excited energy state. Using helium as a reference, we show that the presence of such a resonance in neon modifies the amplitude and phase of the asymmetric emission of photoelectrons. Theoretical simulations based on perturbation theory are in fair agreement with the experimental observations.Received 25 July 2021Revised 1 August 2022Accepted 5 August 2022DOI:https://doi.org/10.1103/PhysRevResearch.4.033231Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasMultiphoton or tunneling ionization & excitationPhotoemissionSingle- and few-photon ionization & excitationUltrafast phenomenaUltrashort pulsesAtomic, Molecular & Optical

Plasmonic internal-photoemission-based Si photodetector design suitable for optical communication.

We propose a high-performance plasmonic photodetector based on the internal photoemission (IPE) process for the C-band communication wavelength. This photodetector takes advantage of an embedded nanohole array in Schottky metal. Owing to localized surface plasmon resonance, the absorption of the active metal layer increases, which results in the generation of more hot carriers and subsequently compensates for the low efficiency of IPE-based photodetectors. Simulations show that for the proposed photodetector with 2-nm-thick Au, Cu, and Ag Schottky contacts, the absorptance dramatically enhances to 95.1%, 93.2%, and 98.2%, respectively, at the wavelength of 1.55 µm. For the detector based on Au, the highest external quantum efficiency of 25.3% and responsivity of 0.32 A/W are achieved at a reverse bias voltage of 1 V. Furthermore, the 3 dB bandwidth can exceed 369 GHz owing to the low capacitance of the structure and the fast transit time of carriers from the thin p-Si layer. Finally, by studying the current-voltage characteristics of the photodetector, it is shown that under the reverse bias voltage of 1 V, the dark current is 665 nA at room temperature, and by reducing the temperature to 200 K, it improves three orders of magnitude and decreases to 810 pA.

Versatile Dicyanomethylene-Based Fluorescent Probes for the Detection of β-Amyloid in Alzheimer's Disease: A Theoretical Perspective.

Motivated by the growing demand for target chemosensors designed with diagnostic or therapeutic capability for fibrils related to amyloidosis diseases, we investigated in the present work the response mechanism of dicyanomethylene-based fluorescent probes for amyloid fibril using a combined approach, including molecular docking, quantum mechanics/molecular mechanics (QM/MM), and the quantum chemical method. Various binding modes for the probes in β-amyloid (Aβ) are discussed, and the fibril environment-induced molecular optical changes at the most stable site are compared to the fibril-free situation in aqueous environments. The results reveal that the fluorescence enhancement for the probes in Aβ observed experimentally is an average consequence over multiple binding sites. In particular, the conformational difference, including conjugation length and donor effect, significantly contributes to the optical property of the studied probes both in water and fibril. To further estimate the transition nature of the molecular photoabsorption and photoemission processes, the hole-electron distribution and the structural variation on the first excited state of the probes are investigated in detail. On the basis of the calculations, structure–property relationships for the studied chemosensors are established. Our computational approach with the ability to elucidate the available experimental results can be used for designing novel molecular probes with applications to Aβ imaging and the early diagnosis of Alzheimer’s disease.

Retrieval of photoionization group delay in chirped-attosecond pulses photoelectron streaking experiments

Photoionization time delays have been investigated in many streaking experiments in which an extreme ultraviolet (XUV) attosecond pulse is used to ionize the target in the presence of a dressing infrared laser field. The discrepancies between the photoionization time delays thus experiment measured and those from many sophisticated theoretical simulations have generated a great deal of controversy in recent years. The difficulty of achieving an accuracy of the retrieved time delays comes from two facts: a so-called wavepacket approximation is introduced to construct the photoionization electron wavepacket, this approximation is invalid if atto-chirp of XUV is non-zero; the other one is that the lower sensitivity of the streaking spectra to the phase of the photoionization transition dipole. Here we present a time delay retrieval method born from our recently proposed ‘phase retrieval of broadband pulses auto correlation’ (PROBP-AC) technology to overcome above limitations. We carefully exam the validity of our method and make a few compare with some other common used retrieval codes, and the simulations demonstrate that more accurate results can be retrieved using PROBP AC. Based on the present method, the angular dependent photoionization time delays can also be retrieved. Our investigation casts doubts on the measured group time delays in previous streaking experiments. We also mention here that a single photoionization group time delay at the XUV peak energy is not enough to represent a complete photoemission process; instead, a fully characterization of the photoionization group time delay over the whole bandwidth of the wave packet is required.

The surface flashover process under positive lightning impulse voltage: initial stage and evolution

Surface flashover is a crucial issue in the field of electrical insulation, and it involves many complex physical processes. In this paper, the development process of the surface flashover was studied from different methods. The initial process of positive surface streamers in different gas environments (air, N2, CO2) was studied by photoelectric observation. The evolution of positive surface streamers in the air was described based on a 2D fluid model. The influence of the surface trap energy level on flashover development and the relationship between gas adsorption and surface trap energy level was discussed by density functional theory calculation preliminarily. The results showed that the initial ionization process of surface flashover is considered as the collision ionization between the initial electrons and gas molecules and photoionization of high-energy photons. Some of the high-energy photons can not only ionize some gas molecules but also cause the surface of the insulator to emit electrons (photoemission process), which could promote the development of the streamer. Both the ionization of the gas molecules and the photoelectric emission of the insulator surface may determine the initial development of surface flashover. During the process of the flashover, the electron density of the surface streamer (∼1021 m−3) is high and the main streamer tends to develop towards the insulator surface. The attraction of surface streamers changes with the position of the initial electron, and the positive surface charge brings the stronger ionization process, and the negative surface charge has the opposite effect. The band gap of the insulator surface is affected by the adsorption of gas molecules, which is considered as introducing shallow traps on the surface. For impulse voltage, the charge accumulation and internal charge migration may be not evident, the initial photoionization process and initial surface charge distribution affect the flashover process primarily.