Coherent interaction between free electrons and a photonic cavity.

Advances in the research of interactions between ultrafast free electrons and light have introduced a previously unknown kind of quantum matter, quantum free-electron wavepackets1-5. So far, studies of the interactions of cavity-confined light with quantum matter have focused on bound electron systems, such as atoms, quantum dots and quantum circuits, which are considerably limited by their fixed energy states, spectral range and selection rules. By contrast, quantum free-electron wavepackets have no such limits, but so far no experiment has shown the influence of a photonic cavity on quantum free-electron wavepackets. Here we develop a platform for multidimensional nanoscale imaging and spectroscopy of free-electron interactions with photonic cavities. We directly measure the cavity-photon lifetime via a coherent free-electron probe and observe an enhancement of more than an order of magnitude in the interaction strength relative to previous experiments of electron-photon interactions. Our free-electron probe resolves the spatiotemporal and energy-momentum information of the interaction. The quantum nature of the electrons is verified by spatially mapping Rabi oscillations of the electron spectrum. The interactions between free electrons and cavity photons could enable low-dose, ultrafast electron microscopy of soft matter or other beam-sensitive materials. Such interactions may also open paths towards using free electrons for quantum information processing and quantum sensing. Future studies could achieve free-electron strong coupling6,7, photon quantum state synthesis8 and quantum nonlinear phenomena such as cavity electro-optomechanics9.

Tunable photon-induced spatial modulation of free electrons.

Spatial modulation of electron beams is an essential tool for various applications such as nanolithography and imaging, yet its conventional implementations are severely limited and inherently non-tunable. Conversely, proposals of light-driven electron spatial modulation promise tunable electron wavefront shaping, for example, using the mechanism of photon-induced near-field electron microscopy. Here we present tunable photon-induced spatial modulation of electrons through their interaction with externally controlled surface plasmon polaritons (SPPs). Using recently developed methods of shaping SPP patterns, we demonstrate a dynamic control of the electron beam with a variety of electron distributions and verify their coherence through electron diffraction. Finally, the nonlinearity stemming from energy post-selection provides us with another avenue for controlling the electron shape, generating electron features far below the SPP wavelength. Our work paves the way to on-demand electron wavefront shaping at ultrafast timescales, with prospects for aberration correction, nanofabrication and material characterization.

Lossless Monochromator in an Ultrafast Electron Microscope Using Near-Field THz Radiation.

The ability to form monoenergetic electron beams is vital for high-resolution electron spectroscopy and imaging. Such capabilities are commonly achieved using an electron monochromator, which energy filters a dispersed electron beam, thus reducing the electron flux to yield down to meV energy resolution. This reduction in flux hinders the use of monochromators in many applications, such as ultrafast transmission electron microscopes (UTEMs). Here, we develop and demonstrate a mechanism for electron energy monochromation that does not reduce the flux-a lossless monochromator. The mechanism is based on the interaction of free-electron pulses with single-cycle THz near fields, created by nonlinear conversion of an optical laser pulse near the electron beam path inside a UTEM. Our experiment reduces the electron energy spread by a factor of up to 2.9 without compromising the beam flux. Moreover, as the electron-THz interaction takes place over an extended region of many tens of microns in free space, the realized technique is highly robust-granting uniform monochromation over a wide area, larger than the electron beam diameter. We further demonstrate the wide tunability of our method by monochromating the electron beam at multiple primary electron energies from 60 to 200 keV, studying the effect of various electron and THz parameters on its performance. Our findings have direct applications in the fast-growing field of ultrafast electron microscopy, allowing time- and energy-resolved studies of exciton physics, phononic vibrational resonances, charge transport effects, and optical excitations in the mid IR to the far IR.

Ultrafast Carrier Dynamics and Bandgap Renormalization in Layered PtSe2.

Carrier interactions in 2D nanostructures are of central importance not only in condensed-matter physics but also for a wide range of optoelectronic and photonic applications. Here, new insights into the behavior of photoinduced carriers in layered platinum diselenide (PtSe2 ) through ultrafast time-resolved pump-probe and nonlinear optical measurements are presented. The measurements reveal the temporal evolution of carrier relaxation, chemical potential and bandgap renormalization in PtSe2 . These results imply that few-layer PtSe2 has a semiconductor-like carrier relaxation instead of a metal-like one. The relaxation follows a triple-exponential decay process and exhibits thickness-dependent relaxation times. This occurs along with a band-filling effect, which can be controlled based on the number of layers and may be applied in saturable absorption for generating ultrafast laser pulses. The findings may provide means to study many-body physics in 2D materials as well as potentially leading to applications in the field of optoelectronics and ultrafast photonics.

Intensity-dependent nonlinear refraction of antimonene dispersions in the visible and near-infrared region.

Antimonene is a stable 2D allotrope of antimony that is predicted to have a direct bandgap, high third-order optical nonlinear susceptibility, and high electron mobility. These properties give it huge potential applications in photonics and optoelectronics. However, the nonlinear refractive response of antimonene dispersions, which is the key to nonlinear refraction-based devices, has not been fully investigated. In this work, we investigated the optical nonlinearities of the antimonene dispersions by spatial self-phase modulation (SSPM) at 405, 785, and 1064 nm wavelengths. The SSPM rings were observed at 405, 785, and 1064 nm, implying the broadband nonlinear optical response of antimonene dispersions from visible to near-infrared. The effective nonlinear refractive index, n2, and the third-order susceptibility, χ(3), of the antimonene dispersion were measured to be ∼10-5 cm2 W-1 and ∼10-8 esu, respectively. Furthermore, the nonlinearity of antimonene was demonstrated to be tuneable by the laser intensities. The relative change of the nonlinear refractive index, Δn2e/n2e, was observed to range from 14% to 63% for different intensities. Our results will be helpful for the photonic applications of antimonene in a broadband wavelength range, such as optical modulators and switchers.

Saturable absorption behavior of free-standing graphene polymer composite films over broad wavelength and time ranges.

A comparative research on saturable absorption (SA) behavior dependence on wavelength and pulse duration was performed for graphene polymer composites. Free-standing graphene-polyvinyl alcohol (PVA) composite films were fabricated by using solution cast method in combination of liquid phase exfoliation. SA responses were observed by using an open-aperture Z-scan technique for 340 fs pulses at 1030 nm and 515 nm from a mode-locked fiber laser, and 6 ns pulses at 1064 nm and 532 nm from a Q-switched Nd:YAG laser. The graphene films possess better SA property, i.e., larger SA coefficient and figure of merit (FOM), and lower saturation intensity I(s), for ns pulses than that for fs pulses at the similar near infrared (NIR) wavelength. For fs pulses, the films show better SA response at 1030 nm than that at 515 nm. By employing slow and fast SA modelling, the excited state and ground state absorption cross sections were estimated to be ~10(-17) cm(2), and the ratio was ~0.6 at NIR for both fs and ns pulses.

Algal-mediated nitrogen removal and sustainability of algal-derived dissolved organic matter supporting denitrification.

Algae-mediated nitrogen removal from low carbon vs. nitrogen (C/N) wastewater techniques has garnered significant attention due to its superior autotrophic assimilation properties. This study investigated the ammonium-N removal potential of four algae species from low C/N synthetic wastewater. Results showed that 95 % and 99 % of ammonium-N are eliminated at initial concentrations of 11.05 ±â€¯0.98 mg/L and 42.51 ±â€¯2.20 mg/L with little nitrate and nitrite accumulation. The compositions of secreted algal-derived dissolved organic matter varied as C/N decreased and showed better bioavailability for nitrate-N removal by Pseudomonas sp. SZF15 without pre-oxidation, achieving an efficiency of 99 %. High-throughput sequencing revealed that the aquatic microbial communities, dominated by Scenedesmus, Kalenjinia, and Micractinium, remain relatively stable across different C/N, aligning with the underlying metabolic pathways. These findings may provide valuable insights into the sustainable elimination of multiple nitrogen contaminants from low C/N wastewater.

Weak measurements and quantum-to-classical transitions in free electron-photon interactions.

How does the quantum-to-classical transition of measurement occur? This question is vital for both foundations and applications of quantum mechanics. Here, we develop a new measurement-based framework for characterizing the classical and quantum free electron-photon interactions and then experimentally test it. We first analyze the transition from projective to weak measurement in generic light-matter interactions and show that any classical electron-laser-beam interaction can be represented as an outcome of weak measurement. In particular, the appearance of classical point-particle acceleration is an example of an amplified weak value resulting from weak measurement. A universal factor, [Formula: see text], quantifies the measurement regimes and their transition from quantum to classical, where [Formula: see text] corresponds to the ratio between the electron wavepacket size and the optical wavelength. This measurement-based formulation is experimentally verified in both limits of photon-induced near-field electron microscopy and the classical acceleration regime using a DLA. Our results shed new light on the transition from quantum to classical electrodynamics, enabling us to employ the essence of the wave-particle duality of both light and electrons in quantum measurement for exploring and applying many quantum and classical light-matter interactions.

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Spatiotemporal imaging of 2D polariton wave packet dynamics using free electrons.

Coherent optical excitations in two-dimensional (2D) materials, 2D polaritons, can generate a plethora of optical phenomena that arise from the extraordinary dispersion relations that do not exist in regular materials. Probing of the dynamical phenomena of 2D polaritons requires simultaneous spatial and temporal imaging capabilities and could reveal unknown coherent optical phenomena in 2D materials. Here, we present a spatiotemporal measurement of 2D wave packet dynamics, from its formation to its decay, using an ultrafast transmission electron microscope driven by femtosecond midinfrared pulses. The ability to coherently excite phonon-polariton wave packets and probe their evolution in a nondestructive manner reveals intriguing dispersion-dependent dynamics that includes splitting of multibranch wave packets and, unexpectedly, wave packet deceleration and acceleration. Having access to the full spatiotemporal dynamics of 2D wave packets can be used to illuminate puzzles in topological polaritons and discover exotic nonlinear optical phenomena in 2D materials.

Chemical Composition, Antimicrobial and Insecticidal Activities of Essential Oils of Discarded Perfume Lemon and Leaves (Citrus Limon (L.) Burm. F.) as Possible Sources of Functional Botanical Agents.

Two essential oils were isolated from discarded perfume lemon and leaves (Citrus limon (L.) Burm. F.) by hydro-distillation with good yield (0.044% for perfume lemon and 0.338% for leaves). Their biological activities were evaluated against five selected bacterial strains and Aedes albopictus (Ae. albopictus, Diptera: Culicidae). Chemical composition indicated that both essential oils were rich in essential phytochemicals including hydrocarbons, monoterpenes and sesquiterpene. These constituents revealed some variability among the oils displaying interesting chemotypes (R)-(+)-limonene (12.29-49.63%), citronellal (5.37-78.70%) and citronellol (2.98-7.18%). The biological assessments proved that the two essential oils had similar effect against bacterial (inhibition zones diameter ranging from 7.27 ± 0.06 to 10.37 ± 0.15 mm; MICs and MBCs ranging from 1.6 to 6.4 mg/mL); against Ae. albopictus larvae (LC50 ranging from 384.81 to 395.09 ppm) and adult mosquito (LD50 ranging from 133.059 to 218.962 µg/cm2); the activity of the two chemotypes ((R)-(+)-limonene and citronellal): larvae (LC50 ranging from 267.08 to 295.28 ppm), which were all presented in dose-dependent manners. Through this work, we have showcased that recycling and reusing of agriculture by-products, such as discarded perfume lemon and leaves can produce eco-friendly alternatives in bacterial disinfectants and mosquito control product.

Bacterially synthesized tellurium nanostructures for broadband ultrafast nonlinear optical applications.

Elementary tellurium is currently of great interest as an element with potential promise in nano-technology applications because of the recent discovery regarding its three two-dimensional phases and the existence of Weyl nodes around its Femi level. Here, we report on the unique nano-photonic properties of elemental tellurium particles [Te(0)], as harvest from a culture of a tellurium-oxyanion respiring bacteria. The bacterially-formed nano-crystals prove effective in the photonic applications tested compared to the chemically-formed nano-materials, suggesting a unique and environmentally friendly route of synthesis. Nonlinear optical measurements of this material reveal the strong saturable absorption and nonlinear optical extinctions induced by Mie scattering over broad temporal and wavelength ranges. In both cases, Te-nanoparticles exhibit superior optical nonlinearity compared to graphene. We demonstrate that biological tellurium can be used for a variety of photonic applications which include their proof-of-concept for employment as ultrafast mode-lockers and all-optical switches.

Optical identification of layered MoS2 via the characteristic matrix method.

It is demonstrated that the characteristic matrix method is effective and reliable for the optical identification of two-dimensional layered nanomaterials on different substrates. By using this method, the authors calculate the reflectivity and optical contrast of layered MoS2 crystallites prepared on quartz by chemical vapor deposition. It is found that the measured pixel intensity of an MoS2 optical image under continuous spectrum light is proportional to the calculated reflectivity, and that the theoretical optical contrast agrees well with the experimental results. This work provides a new way for the calculation of the optical contrast of the 2D nanomaterials and layered heterostructures on various substrates.

Ultrafast Nonlinear Excitation Dynamics of Black Phosphorus Nanosheets from Visible to Mid-Infrared.

The recent progress on black phosphorus makes it a promising candidate material for broadband nanophotonic devices, especially operating in the mid-infrared spectral region. Here, the excited carrier dynamics and nonlinear optical response of unoxidized black phosphorus nanosheets and their wavelength dependence were systematically studied from 800 nm to 2.1 µm. The wavelength-dependent relaxation times of black phosphorus nanosheets are determined to be 360 fs to 1.36 ps with photon energies from 1.55 to 0.61 eV. In a comparative study with graphene, we found that black phosphorus has a faster carrier relaxation in near- and mid-infrared region. With regard to nonlinear optical absorption, the response of black phosphorus significantly increases from near- to mid-infrared, and black phosphorus is also confirmed to be better as saturable absorber to MoS2 in infrared region.

Slow and fast absorption saturation of black phosphorus: experiment and modelling.

According to the excited-state decay time, a slow saturable absorber model was employed to obtain the ground-state absorption and excited-state absorption cross sections σgs and σes of black phosphorus (BP) nanosheets, which are (1.25 ± 0.07) × 10-16 cm2 and (2.97 ± 0.21) × 10-17 cm2 at 515 nm, and (5.95 ± 0.17) × 10-18 cm2 and (5.19 ± 0.71) × 10-19 cm2 at 1030 nm, respectively. In comparison, the σgs and σes of MoS2 and graphene were also obtained with the same model. The ratio σes/σgs of BP is the smallest (only 0.24 ± 0.03 at 515 nm and 0.09 ± 0.01 at 1030 nm) among the three two-dimensional layered materials both at 515 nm and 1030 nm. Relatively large ground-state transition probability and weak loss of excited-state absorption result in good saturable absorption performance. In comparison with MoS2 and graphene, the much lower saturation intensity of BP can be well explained from this perspective.

Facile fabrication of wafer-scale MoS2 neat films with enhanced third-order nonlinear optical performance.

Wafer-scale MoS2 neat films with controllable thicknesses were successfully fabricated by vacuum filtering liquid-exfoliated MoS2 dispersions. The obtained MoS2 filtered thin films were systematically characterized by UV-Vis spectroscopy, Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, atomic force microscopy (AFM) and scanning electron microscopy (SEM). It was found that the fabricated scalable MoS2 films have a smooth surface and high optical homogeneity verified by AFM and a collimated 532 nm beam, respectively. We investigated the ultrafast nonlinear optical (NLO) properties of the filtered films by an open aperture Z-scan method using 515 and 1030 nm femtosecond laser pulses. Saturable absorption was observed at both 515 and 1030 nm with the figure of merit (FOM) values as ∼3.3 × 10(-12) esu cm and ∼3.4 × 10(-14) esu cm, respectively. The observation of ultrafast NLO performance of the MoS2 filtered films indicates that vacuum filtration is a feasible method for the fabrication of optical thin films, which can be expanded to fabricate other two-dimensional films from the corresponding dispersions. This easy film fabrication technology will greatly enlarge the application of graphene analogues including graphene in photonic devices, especially of MoS2 as a saturable absorber.

Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics.

Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement.

Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors.

A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10,000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.

Ultrafast saturable absorption of two-dimensional MoS2 nanosheets.

Employing high-yield production of layered materials by liquid-phase exfoliation, molybdenum disulfide (MoS2) dispersions with large populations of single and few layers were prepared. Electron microscopy verified the high quality of the two-dimensional MoS2 nanostructures. Atomic force microscopy analysis revealed that ~39% of the MoS2 flakes had thicknesses of less than 5 nm. Linewidth and frequency difference of the E(1)2g and A1g Raman modes confirmed the effective reduction of flake thicknesses from the bulk MoS2 to the dispersions. Ultrafast nonlinear optical (NLO) properties were investigated using an open-aperture Z-scan technique. All experiments were performed using 100 fs pulses at 800 nm from a mode-locked Ti:sapphire laser. The MoS2 nanosheets exhibited significant saturable absorption (SA) for the femtosecond pulses, resulting in the third-order NLO susceptibility Imχ((3)) ~ 10(-15) esu, figure of merit ~10(-15) esu cm, and free-carrier absorption cross section ~10(-17) cm(2). Induced free carrier density and the relaxation time were estimated to be ~10(16) cm(-3) and ~30 fs, respectively. At the same excitation condition, the MoS2 dispersions show better SA response than the graphene dispersions.