Photon Excitation Research Articles

Laser-induced thermal grating spectroscopy based on femtosecond laser multi-photon absorption

Laser-induced grating spectroscopy (LIGS) is for the first time explored in a configuration based on the crossing of two focused femtosecond (fs) laser pulses (800-nm wavelength) and a focused continuous-wave (cw) laser beam (532-nm wavelength). A thermal grating was formed by multi-photon absorption of the fs-laser pulses by hbox {N}_{{2}} with a pulse energy around 700 upmu J (sim 45 TW/hbox {cm}^{2}). The feasibility of this LIGS configuration was investigated for thermometry in heated nitrogen gas flows. The temperature was varied from room temperature up to 750 K, producing strong single-shot LIGS signals. A model based on the solution of the linearized hydrodynamic equations was used to extract temperature information from single-shot experimental data, and the results show excellent agreement with the thermocouple measurements. Furthermore, the fluorescence produced by the fs-laser pulses was investigated. This study indicates an 8-photon absorption pathway for hbox {N}_{{2}} in order to reach the hbox {B}^{3}Pi _{g} state from the ground state, and 8 + 5 photon excitation to reach the hbox {B}^{2}Sigma _{u}^{+} state of the hbox {N}_{2}^{+} ion. At pulse energies higher than 1 mJ, the LIGS signal was disturbed due to the generation of plasma. Additionally, measurements in argon gas and air were performed, where the LIGS signal for argon shows lower intensity compared to air and hbox {N}_{{2}}.

Piezophototronic Effect in Nanosensors

The piezophototronic effect is the coupling of piezoelectricity, semiconductor behavior and photon excitation in wurtzite materials, which can enhance the performance of optoelectronic nano‐devices by regulating a series of processes of carrier injection, transport, and recombination. In recent years, many research results have been reported on the improvement of nanophotoelectric nano‐device efficiency by piezophototronic effect, such as photovoltaic devices, light‐emitting devices, transistors, etc. Herein, the research results of piezophototronic effect in the field of nanosensors, including enhancing the performance of traditional nanosensors and new types of pressure/deformation/tactile sensors based on piezophototronic effect are comprehensively summarized. Finally, the future development of piezophototronic effect in the field of nanosensors is discussed.

Direct Characterization of Thermal Nonequilibrium between Optical and Acoustic Phonons in Graphene Paper under Photon Excitation.

Raman spectroscopy has been widely used to measure thermophysical properties of 2D materials. The local intense photon heating induces strong thermal nonequilibrium between optical and acoustic phonons. Both first principle calculations and recent indirect Raman measurements prove this phenomenon. To date, no direct measurement of the thermal nonequilibrium between optical and acoustic phonons has been reported. Here, this physical phenomenon is directly characterized for the first time through a novel approach combining both electrothermal and optothermal techniques. While the optical phonon temperature is determined from Raman wavenumber, the acoustic phonon temperature is precisely determined using high‐precision thermal conductivity and laser power absorption that are measured with negligible nonequilibrium among energy carriers. For graphene paper, the energy coupling factor between in‐plane optical and overall acoustic phonons is found at (1.59–3.10) × 1015 W m−3 K−1, agreeing well with the quantum mechanical modeling result of 4.1 × 1015 W m−3 K−1. Under ≈1 µm diameter laser heating, the optical phonon temperature rise is over 80% higher than that of the acoustic phonons. This observation points out the importance of subtracting optical–acoustic phonon thermal nonequilibrium in Raman‐based thermal characterization.

Higher Harmonic Generation of Coherent Sub-THz Radiation at Lifshitz Transition in Gapped Bilayer Graphene

The microscopic quantum theory of nonlinear interaction of strong coherent electromagnetic radiation with gapped bilayer graphene is used for consideration of the high harmonic generation at low-energy photon excitation Lifshitz transition. The Liouville–von Neumann equation for the density matrix is solved numerically at the nonadiabatic multiphoton excitation regime. By numerical solutions, we examine the rates of the second and third harmonics generation at the particle-hole annihilation at Lifshitz transitions in the linearly polarized coherent electromagnetic wave. The obtained results show that the gapped bilayer graphene can serve as an effective medium for the generation of even and odd high harmonics in the sub-THz domain of frequencies.

Defects induced by He+ irradiation in γ-Si3N4

Formation and evolution of defect levels in the electronic structure of silicon nitride with cubic spinel structure, γ-Si3N4, after the irradiation with He+ ions was investigated using spectroscopic techniques. Strong changes of cathodoluminescence (CL), photoluminescence (PL), photoluminescence excitation (PLE) and Raman spectra were detected. In particular, excitonic PL was significantly inhibited and a new near-IR band appeared with the band gap excitation hν≥Eg = 5.05 eV. This was explained by an effective trapping of photoinduced electrons and holes by charged defects. The spectral shift of PL with the excitation photon energy indicated heterogeneous nature of the defect sites. The energetic position of near-IR and visible PL bands correlate, suggesting an interaction with the common cation defect to be an origin. The visible PL of exciton bound to a neutral defect Si× was red shifted, which was attributed to the permutations between empty and occupied octahedral and tetrahedral sites, inherent to the spinel structure, after collisions with He+ ions. The positively charged cation sites in the spinel structure are compensated by VN‴ anion vacancies. The local deformation of the spinel lattice affects PL intensity of the self-trapped exciton at 4.35 eV.

Doped lanthanum cerate pyrochlore for multicolor luminescent phosphor: Decisive role of energy transfer and defects

Designing of efficient luminescent materials requires proper understanding of energy transfer, defect evolution and dopant local structure. The present work is a perfect amalgam wherein we have thoroughly investigated the concentration dependent host sensitized energy transfer, defect evolution and local structure of europium ion in La2Ce2O7 (LCO) pyrochlore material. Raman spectroscopy suggested stabilization of defect fluorite structure for LCO as well as LCO:Eu3+ (LCOE) but degree of structural distortion as well as oxygen vacancies (OVs) increases with increase in europium ion concentration. Diffuse reflectance spectroscopy suggested band gap narrowing at higher doping level owing to enhanced density of OVs. Positron annihilation lifetime spectroscopy suggested an increase in the formation of oxygen vacancies and vacancy clusters near the surfaces at higher doping. As a result, LCO, on irradiation with 250 nm ultraviolet photon showed visible emission due to OVs as well charge transfer transition. On Eu3+ doping emission spectra was rich in host as well as europium emission and host to europium energy transfer increases with increase in europium ion concentration. This get's reflected as violet blue emission at lower doping and yellowish white at higher doping level ≥7.5% under host excitation and orange-red emission under 471 nm dopant excitation. Europium ion emission spectral profiles in LCOE suggested stabilization of Eu3+ in CeO6 octahedra as is also confirmed using lifetime spectroscopy. Judd-Ofelt measurement further reflected higher branching ratio for 5D0→7F2, internal quantum yield ~48% and high Ω2 compared to Ω4. This work highlights the importance of local dopant site, HSET, excitation photon and defects in designing color tunable luminescent materials and is expected to play an important role in designing the phosphor converted light emitting diodes (pc-LEDs).

UV-A light-assisted gas-phase formic acid decomposition on photo-thermo Ru/TiO2 catalyst

Although solar energy is considered as one of the ideal abundant sources of renewable energy to be integrated into the catalytic processing, photonic and thermal excitations were perceived till recently as independent strategies in overcoming Arrhenius-type activation energy barriers in catalytic reactions. However, this dual-mode excitation of catalysts is receiving a growing interest nowadays due to promising evidence of synergy effects. A Ru/TiO2 photo-thermo- catalyst was prepared according to a UV-A light photo-assisted synthesis method allowing a fine control of the Ru nanoparticle size distribution, and the influence of a combined photonic (UV-A) and thermal activation on its performances in the gas phase decomposition of formic acid into hydrogen was studied. The results showed that a dual photonic/thermal excitation in a one-pot operation allows to increase the formic acid conversion and consequently the production of hydrogen vs. the reaction in the dark, the enhancement being all the more pronounced as the irradiance is high. The combined excitation allowed to drive the reaction at lower temperatures upon irradiation while maintaining a similar conversion level. This low-temperature shift was all the more marked as the irradiance was high, and was accompanied by a strong increase in the selectivity to hydrogen. The change in both conversion and selectivity patterns suggested the implication of the light-excited electrons in the non-plasmonic Ru nanoparticles for conducting the reaction through an alternative low-energy transition state, with a lowering of the apparent energy activation, rather than a mechanism of localized-heat delivery.

Exploring Heterostructured Upconversion Nanoparticles: From Rational Engineering to Diverse Applications.

Upconversion nanoparticles (UCNPs) represent a class of optical nanomaterials that can convert low-energy excitation photons to high-energy fluorescence emissions. On the basis of UCNPs, heterostructured UCNPs, consisting of UCNPs and other functional counterparts (metals, semiconductors, polymers, etc.), present an intriguing system in which the physicochemical properties are largely influenced by the entire assembled particle and also by the morphology, dimension, and composition of each individual component. As multicomponent nanomaterials, heterostructured UCNPs can overcome challenges associated with a single component and exhibit bifunctional or multifunctional properties, which can further expand their applications in bioimaging, biodetection, and phototherapy. In this review, we provide a summary of recent achievements in the field of heterostructured UCNPs in the aspects of construction strategies, synthetic approaches, and types of heterostructured UCNPs. This review also summarizes the trends in biomedical applications of heterostructured UCNPs and discusses the challenges and potential solutions in this field.

Optical emission enhancement of bent InSe thin films

In contrast to the majority of two-dimensional semiconductors such as transition metal dichalcogenides, indium selenide (InSe) possesses an intrinsic large out-of-plane oriented band-edge luminescent dipole. This unique anisotropic feature of band-edge optical emissions can be exploited to achieve enhanced optical signal in bent regions of materials created by geometrical modification. We herein investigate based on first-principle calculations the mechanism of this optical emission enhancement by modelling the photoluminescence processes in bent and flat regions of the InSe thin film. We propose in our model that the shorter-wavelength interband transition, labelled as transition B′, between the second-highest valence band and the bottom of conduction band plays an important role in the enhancing process. Our model robustly describes the dependence of optical emission enhancement in the bent InSe thin films on thickness, incident light orientation, and excitation photon energy. In particular, we found that when excitation photon energy is lower than the energy of transition B′, strong enhancement up to hundreds of times can be obtained by applying an incident light at an angle less than 70° to the InSe layers. Our results provide useful references for modulating luminescent properties of InSe films toward flexible optoelectronic device applications.

Tuning Green to Red Color in Erbium Niobate Micro- and Nanoparticles.

Tetragonal Er0.5Nb0.5O2 and monoclinic ErNbO4 micro- and nanoparticles were prepared by the citrate sol–gel method and heat-treated at temperatures between 700 and 1600 °C. ErNbO4 revealed a spherical-shaped crystallite, whose size increased with heat treatment temperatures. To assess their optical properties at room temperature (RT), a thorough spectroscopic study was conducted. RT photoluminescence (PL) spectroscopy revealed that Er3+ optical activation was achieved in all samples. The photoluminescence spectra show the green/yellow 2H11/2, 4S3/2→4I15/2 and red 4F9/2→4I15/2 intraionic transitions as the main visible recombination, with the number of the crystal field splitting Er3+ multiplets reflecting the ion site symmetry in the crystalline phases. PL excitation allows the identification of Er3+ high-energy excited multiplets as the preferential population paths of the emitting levels. Independently of the crystalline structure, the intensity ratio between the green/yellow and red intraionic transitions was found to be strongly sensitive to the excitation energy. After pumping the samples with a resonant excitation into the 4G11/2 excited multiplet, a green/yellow transition stronger than the red one was observed, whereas the reverse occurred for higher excitation photon energies. Thus, a controllable selective excited tunable green to red color was achieved, which endows new opportunities for photonic and optoelectronic applications.

Distributed geometric quantum computation based on the optimized-control-technique in a cavity-atom system via exchanging virtual photons

We propose a scheme for quantum geometric computation on a fiber-cavity-fiber system, in which two atoms are located in two single-mode cavities, respectively, connected with each other by optical fiber. This scheme not only has the feature of virtual excitation of photons in the cavity quantum electrodynamics (CQED) that can reduce the effect of decay effectively but also has the advantage of geometric phase to withstand noises due to its built-in noise-resilience feature and robust merit. Specifically, our proposal combined with optimized-control-technology (OCT) can reduce gate operation error by adjusting the time-dependent amplitude and phase of the resonant field which further enhances the robustness of the quantum operation. The robustness against decoherence is demonstrated numerically and the scheme may be applied in the remote quantum information processing tasks and quantum computation.

Optical Tuning of Resistance Switching in Polycrystalline Gallium Phosphide Thin Films.

The nanoscale resistive switching characteristics of gallium phosphide (GaP) thin films directly grown on Si are investigated as a function of incident light. The formation of conductive channels along the grain boundaries is attributed to the presence of point defects and structural disorder, which provide the ideal environment to enable the filamentary switching process. Both first-principles calculations and UV-vis and photoluminescence spectroscopy strongly point to the possibility of mid-gap electronic states in the polycrystalline GaP film due to such defects. To study the photonic excitation, photoconductive atomic force microscopy (phAFM) measurement is conducted. We observe photocurrents even for incident photon energies lower than the band gap, consistent with the presence of mid-gap electronic states; the photocurrents increase in direct proportion to the incident photon energy with a concomitant decrease in the filament resistance. This demonstrates GaP directly integrated on Si can be a promising photonic resistive switching materials system.

Optical Characterization of Gallium Oxide α and β Polymorph Thin-Films Grown on c-Plane Sapphire

In this work, the optical properties of thin-film α-Ga2O3 are examined and contrasted with those of β-Ga2O3 thin films grown on similar substrates. Thin films of α-Ga2O3 were synthesized employing mist chemical vapor deposition (mist CVD) on double-side polished c-plane sapphire. Optical properties were studied through absorbance, photoluminescence (PL), and photoluminescence excitation (PLE). Absorbance measurements showed spectra consistent with that previously reported in the literature, with Eg ~ 5.19 eV for α-Ga2O3. Despite an absorption edge laying at higher energies, the PL spectra in α-Ga2O3 films yield similar features to those of metal-organic chemical vapor deposition (MOCVD) grown β-Ga2O3 thin-films. In both cases, when excited above the band gap, the PL spectra consist of UV, UV′, blue and green broad bands. As the excitation photon energy was varied, the relative intensity of these PL bands changed. This is attributed to a non-uniform defect concentration distribution across the sample depth. With smaller concentration of defects associated with blue and green emission in the bulk compared to the surface in the α-phase films.

Cooling and diffusion characteristics of a hot carrier in the monolayer WS2.

The characteristics of a hot carrier distributed in the C excitonic state of the monolayer WS2 is investigated by exploiting the transient absorption (TA) spectroscopy. The hot carrier cooling lifetime gradually prolongs from 0.58 ps to 2.68 ps with the absorbed photon flux owing to the hot phonon bottleneck effect, as the excitation photon energy is 2.03 eV. Meanwhile, the normalized TA spectra shows that the spectral feature of hot carriers is different from that of normal carriers. Based on the modified Lennard-Jones model, the average distance among hot carriers can be estimated according to the peak shift of TA spectra and the diffusion velocity can also be calculated simultaneously. The hot carrier limits the diffusion of the photo-generated carrier at the initial several picoseconds. These results help people to elucidate the hot carrier dynamics in 2D TMDCs and give guidance on the designing and optimizing the TMDC-based electronic devices of high performance.

Electron pair emission from surfaces: Photon versus electron excitation

We have studied the electron pair emission process from a Cu(111) surface excited by a primary electron or photon beam. Although the photon energy was 30 eV the primary electron beam had an energy of 25 eV. We will discuss the energy and momentum distributions. The experiments with the electron beam demonstrate that the contributions from the Shockley surface state can be clearly identified. This is not the case for the work with photons which we ascribe to the low spectral weight of the contribution from two Shockley state electrons compared to two $3d$ electrons. The momentum distributions reveal a close similarity between the two types of excitation despite the fact that the microscopic origin of the pair emission is very different. There is a distinctive energy dependence of these curves which we describe by an empirical three-parameter polynomial. The numerical values of these parameters are close for both pathways. Additional measurements with different primary electron energies reveals the importance of the initial state on the momentum distributions.

Ultrafast dynamics of photoexcited carriers in perovskite semiconductor nanocrystals

Abstract Perovskite semiconductor nanocrystals have emerged as a promising family of materials for optoelectronic applications including light-emitting diodes, lasers, light-to-electricity convertors and quantum light emitters. The performances of these devices are fundamentally dependent on different aspects of the excited-state dynamics in nanocrystals. Herein, we summarize the recent progress on the photoinduced carrier dynamics studied by a variety of time-resolved spectroscopic methods in perovskite nanocrystals. We review the dynamics of carrier generation, recombination and transport under different excitation densities and photon energies to show the pathways that underpin the photophysics for light-emitting diodes and solar cells. Then, we highlight the up-to-date spin dynamics and coherent exciton dynamics being manifested with the exciton fine levels in perovskite semiconductor nanocrystals which are essential for potential applications in quantum information technology. We also discuss the controversial results and the possible origins yet to be resolved. In-depth study toward a comprehensive picture of the excited-state dynamics in perovskite nanocrystals may provide the key knowledge of the device operation mechanism, enlighten the direction for device optimization and stimulate the adventure of new conceptual devices.

Photonic and plasmonic transition radiation from graphene

We theoretically study the transition radiation in the framework of full Maxwell equations, when a swift electron crosses a monolayer graphene. Based on the Sommerfeld integration, we demonstrate in the frequency domain the spatial distribution of this free-electron radiation, which clearly shows the broadband excitation of both photons and graphene plasmons. Moreover, the radiation spectra for photons and graphene plasmons are analytically derived. We find that the excitation of photons and graphene plasmons favors different particle velocities. To be specific, a higher particle velocity gives rise to the excitation of photons with better directivity and higher intensity, while a lower particle velocity enables the efficient excitation of graphene plasmons in a broader frequency range. Our work indicates that the interaction between swift charged particles and various 2D materials or van der Waals heterostructures is promising for the design of terahertz on-chip radiation sources.

Bridging nano-optics and condensed matter formalisms in a unified description of inelastic scattering of relativistic electron beams

In the last decades, the blossoming of experimental breakthroughs in the domain of electron energy loss spectroscopy (EELS) has triggered a variety of theoretical developments. Those have to deal with completely different situations, from atomically resolved phonon mapping to electron circular dichroism passing by surface plasmon mapping. All of them rely on very different physical approximations and have not yet been reconciled, despite early attempts to do so. As an effort in that direction, we report on the development of a scalar relativistic quantum electrodynamic (QED) approach of the inelastic scattering of fast electrons. This theory can be adapted to describe all modern EELS experiments, and under the relevant approximations, can be reduced to most of the last EELS theories. In that aim, we present in this paper the state of the art and the basics of scalar relativistic QED relevant to the electron inelastic scattering. We then give a clear relation between the two once antagonist descriptions of the EELS, the retarded dyadic Green function, usually applied to describe photonic excitations and the quasi-static mixed dynamic form factor (MDFF), more adapted to describe core electronic excitations of material. Using the photon propagator in a material, expressed in the relevant gauges, as a tool to understand the interaction between a fast electron and a material, we extend this relation to a newly defined quantity, the relativistic MDFF. The relation between the dyadic Green function and the relativistic MDFF does depend only on the photon propagator and not on the specifics of the particle (here, a fast electron) probing the target. Therefore, it can be adapted to any spectroscopy where a relation between the electromagnetic and electronic properties of a material is needed. We then use this theory to establish two important EELS-related equations. The first one relates the spatially resolved EELS to the imaginary part of the photon propagator and the incoming and outgoing electron beam wavefunction, synthesizing the most common theories developed for analyzing spatially resolved EELS experiments. The second one shows that the evolution of the electron beam density matrix is proportional to the mutual coherence tensor, proving that quite universally, the electromagnetic correlations in the target are imprinted in the coherence properties of the probing electron beam.

Maximally entangled and gigahertz-clocked on-demand photon pair source

We present a 1 GHz-clocked, maximally entangled and on-demand photon pair source based on droplet etched GaAs quantum dots using two-photon excitation. By employing these GaP microlensenhanced devices in conjunction with their substantial brightness, raw entanglement fidelities of up to $0.95 \pm 0.01$ and post-selected photon indistinguishabilities of up to $0.93 \pm 0.01$, the suitability for quantum repeater based long range quantum entanglement distribution schemes is shown. Comprehensive investigations of a complete set of polarization selective two-photon correlations as well as time resolved Hong-Ou-Mandel interferences facilitate innovative methods that determine quantities such as photon extraction and excitation efficiencies as well as pure dephasing directly - opposed to commonly employed indirect techniques.

Femtosecond Lasers in Cornea & Refractive Surgery

Since the introduction of femtosecond laser (FS) systems for corneal flap creation in laser-assisted in-situ keratomileusis there have been numerous applications for FS laser in corneal surgery. This manuscript details the utility of FS lasers in corneal surgical procedures including refractive laser surgeries, intracorneal ring segment tunnels, presbyopic treatments, and FS-assisted keratoplasty. We also review the role of FS lasers in diagnostic procedures such as two photon excitation fluorescence and second harmonic generation.