Ultrafast Emission Research Articles

Electronic control of ultrafast field emission in carbon nanotube gaps

The electronic control of an ultrafast tunneling electron emission was demonstrated in the nanogap of a single-walled nanotube (SWNT) when irradiated by a femtosecond laser pulse. The SWNT apex possesses a nanoscale morphology with a large damage threshold and thus enabled the achievement of a large emission rate. More importantly, the DC field-emission characteristics varied when the gate bias was changed. This was analyzed in terms of the change in the effective barrier height and enhancement factors. Photoinduced electron emission was observed when the gap area was illuminated with a femtosecond laser centered at a wavelength of 800 nm. As the laser power was increased, a saturated tunneling current was observed, reaching more than 10 electrons per pulse. Finally, the photoelectron emission yield was tuned with the help of gate-induced variations in the electronic band structures of the SWNTs.

Far-Field Radiation of Three-Dimensional Plasmonic Gold Tapers near Apexes.

Three-dimensional plasmonic gold tapers are widely used structures in nano-optics for achieving imaging at the nanometer scale, enhanced spectroscopy, confined light sources, and ultrafast photoelectron emission. To understand their radiation properties further, especially in the proximity of the apex at the nanoscale, we employ cathodoluminescence spectroscopy with high spatial and energy resolution. The plasmon-induced radiation in the visible spectral range from three-dimensional gold tapers with opening angles of 13° and 47° is investigated under local electron excitation. We observe a much weaker radiation from the apex of the 13° taper than from that of the 47° taper. By means of finite-difference time-domain simulations we show that for small opening angles plasmon modes that are created at the apex are efficiently guided along the taper shaft. In contrast for tapers with larger opening angles, generated plasmon polaritons experience larger radiation damping. Interestingly, we find for both tapers that the most intense radiation comes from locations a few hundreds of nanometers behind the apexes, instead of exactly at the apexes. Our findings provide useful details for the design of plasmonic gold tapers as confined light sources or light absorbers.

Ultrafast deep-red emission fluorescent probe for highly selective imaging of endogenous cysteine in living cells and mice

It is still challenging how to selectively and sensitively detect cysteine in living systems which plays crucial roles in many physiological and biological processes. Here, we developed a deep-red emission fluorescent probe (DRP-Cys) for Cys based on a hemicyanine scaffold. A tailed malononitrile group could chromatically shift excitation/emission wavelengths to avoid the limitations such as photo-damage or auto-fluorescence in biological samples. Compared with other amino acids, Cys could trigger the Michael addition reaction to release a dramatic enhancement in fluorescence centering at around 645 nm in DMSO aqueous solution under physiological conditions with an ultrafast response time of about 1 min and a low limit of detection of 10 nM which significantly benefited from the introduction of the malononitrile moiety. The probe was also successfully applied for visualizing endogenous Cys in living HeLa cells and mice with low cytotoxicity and good cell-membrane permeability.

Gamma-ray emission from wakefield-accelerated electrons wiggling in a laser field

Ultra-fast synchrotron radiation emission can arise from the transverse betatron motion of an electron in a laser plasma wakefield, and the radiation spectral peak is limited to tens of keV. Here, we present a new method for achieving high-energy radiation via accelerated electrons wiggling in an additional laser field whose intensity is one order of magnitude higher than that for the self-generated transverse field of the bubble, resulting in an equivalent wiggler strength parameter K increase of approximately twenty times. By calculating synchrotron radiation, we acquired a peak brightness for the case of the laser wiggler field of 1.2 × 1023 ph/s/mrad2/mm2/0.1%BW at 1 MeV. Such a high brilliance and ultra-fast gamma-ray source could be applied to time-resolved probing of dense materials and the production of medical radioisotopes.

Subcycle interference in high-order harmonic generation from solids

Different from the high-order harmonic generation (HHG) from gases, we find that the yield of HHG from solids exhibits unexpected modulations as a function of the driving laser intensity and wavelength. Its mechanism can be unraveled by the interference between currents inside the solids induced by two adjacent Zener tunneling events. Our simulations agree well with the experimental measurements of HHG from ZnSe and solid Ar. We also find that the dephasing time plays a key role in this subcycle interference and can turn it on or off by controlling the overlap between the channels. It provides an avenue to optimize the ultrafast electron dynamics and HHG emission processes in solids, which will be useful for the compact ultrafast EUV light sources. We also propose an experimental scheme by using ultrashort lasers to explore this interference in other solid materials.

Bright and Ultrafast Photoelectron Emission from Aligned Single-Wall Carbon Nanotubes through Multiphoton Exciton Resonance.

Ultrashort bunches of electrons, emitted from solid surfaces through excitation by ultrashort laser pulses, are an essential ingredient in advanced X-ray sources, and ultrafast electron diffraction and spectroscopy. Multiphoton photoemission using a noble metal as the photocathode material is typically used but more brightness is desired. Artificially structured metal photocathodes have been shown to enhance optical absorption via surface plasmon resonance but such an approach severely reduces the damage threshold in addition to requiring state-of-the-art facilities for photocathode fabrication. Here, we report ultrafast photoelectron emission from sidewalls of aligned single-wall carbon nanotubes. We utilized strong exciton resonances inherent in this prototypical one-dimensional material, and its excellent thermal conductivity and mechanical rigidity leading to a high damage threshold. We obtained unambiguous evidence for resonance-enhanced multiphoton photoemission processes with definite power-law behaviors. In addition, we observed strong polarization dependence and ultrashort photoelectron response time, both of which can be quantitatively explained by our model. These results firmly establish aligned single-wall carbon nanotube films as novel and promising ultrafast photocathode material.

Ultrafast gamma-ray line emission driven by laser-accelerated ion beams

The Monte Carlo code Geant4 is used to demonstrate ultrafast gamma-ray line emission from the 12C +12C reaction driven by laser-accelerated ion beams. With carbon ions of the order of tens of MeV accelerated by laser-bombarding the carbon target, characteristic gamma-ray line emission is generated with durations as short as picoseconds through ultrafast gamma-ray transitions. Because the relative bandwidths of such gamma-ray lines can be reduced to less than 1% and the yield rate of gamma photons is around 10−5 for an incident carbon ion, this gamma-ray line emission can be used as an ultrafast monoenergetic gamma-ray source with a flux of 1.2 × 106 photons/J into 4π. We also show that the bremsstrahlung background induced by electrons accelerated simultaneously with the carbon ions can be mitigated by choosing a proper detection angle and an optimized target thickness.

Ultrafast strong-field photoelectron emission due to two-color laser fields

Electron emission from solids driven by two-color lasers provides great flexibility for the control of electron dynamics in ultrashort spatiotemporal scales due to the interference effect. Here, we construct an analytical model for the highly nonlinear photoelectron emission from a metal surface illuminated by two-color laser fields, by solving the time-dependent Schr\odinger equation. The exact solution is valid for arbitrary harmonic orders, laser intensities, phase difference between two lasers, and metal work function and Fermi level. We find two-color lasers can strongly modulate both the electron energy spectra and the emission current up to 99%. Using the same input parameters, our theoretical prediction for the photoemission current modulation depth (93.9%) is almost identical to the experimental result (94%) in [M. F\orster et al., Phys. Rev. Lett. 117, 217601 (2016)].

Unconventional Synthesis of a CuI Rotaxane with a Superacceptor Stopper: Ultrafast Excited‐State Dynamics and Near‐Infrared Luminescence

A CuI bis-phenanthroline rotaxane was prepared by using the [2+2] cycloaddition-retroelectrocyclization (CA-RE) reaction to graft a bulky dicyanoquinodimethane (DCNQ) stopper. The electronic properties were investigated with electrochemical and photophysical techniques, in parallel with three reference compounds, namely, the DCNQ derivative alone, the DCNQ-based phenanthroline ligand, and an analogue CuI complex lacking the DCNQ moiety. In all the systems containing the DCNQ unit, the lowest electronic excited states are centered thereon, with the singlet level (S1 ) located at about 1.0 eV, as suggested by TDDFT calculations. Accordingly, in the DCNQ-equipped rotaxane, the typical metal-to-ligand charge-transfer luminescence of the CuI center is totally quenched. Ultrafast transient absorption and emission studies show that, in the rotaxane, the final sink of photoinduced processes is the lowest singlet state of the DCNQ moiety (S1 ), which exhibits strong charge-transfer character and a lifetime of 0.4 ps. Its deactivation leads to population of another excited state with a lifetime of 1.3 ps, which can be the related triplet state (T1 ) or a vibrationally hot level (hot-S0 ). Notably, S1 also shows stimulated fluorescence in the near-infrared (NIR) region between 1100 and 1500 nm, corroborating the TDDFT prediction. This unusual finding opens up the study of ultrashort-lived NIR luminescence in organic donor-acceptor systems.

Time-resolved characteristics and chemical kinetics of non-oxidative methane conversion in repetitively pulsed dielectric barrier discharge plasmas

Repetitively pulsed discharge is an emerging non-thermal plasma technology in the chemistry field given its advantages of high electron energy and moderate gas temperature. The focus of this paper is on the temporal evolution of physical and chemical processes in the plasma-assisted non-oxidative conversion of methane (CH4). Positive and negative streamer discharge plasmas were generated by a microsecond-pulse power source (pulse rising time ~500 ns and full width at half maximum ~8 μs) in a well-designed dielectric barrier discharge reactor. The performance of CH4 conversion (conversion rate, product yield, energy conversion efficiency, etc) was investigated in the first instance. A CH4 conversion rate of 6.2%–9.6% was acquired in the negative streamer discharges, which is on average 6% higher than that in the positive streamer discharges. To explain this phenomenon, the temporal evolution of voltage–current waveforms and ultrafast ICCD photographs and optical emission spectra were recorded. As expected, significant differences between the two different forms of discharges were found. Compared with those of the positive streamer discharges, characteristics of only one, big breakdown, higher initial voltage and current peak, a more stable and nearly uniform luminescent process, and higher CH (A2Δ − X2Π) emission intensity and rotational temperature were observed in the negative streamer discharges, which coincide with the promotion of CH4 conversion performance. A simplified chemical kinetics analysis of CH4 discharge was also implemented to demonstrate the influence of characteristic differences on CH4 conversion performance.

Multichannel high-order harmonic generation from solids

We studied the ultrafast dynamics of high-order harmonic generation (HHG) from solids numerically. It is found that a superposition of Bloch oscillation in the same band and Zenner tunneling to its neighboring conduction band (i.e., Bloch-Zener oscillation effect) play significant roles in HHG when the Bloch electrons cross the boundary of the first Brillouin zone. It increases the number of the harmonic emission channels. These multichannel signals extend the cutoff energy of the plateau in the HHG spectra and enhance both the intra- and interband contributions. The interference of different channels makes the structure of the HHG spectra complex. The multichannel dynamics in the monochromatic and two-color laser fields are demonstrated in a periodic potential model and single-crystal MgO, respectively. It provides an alternative way to control the ultrafast electron dynamics and HHG emission processes in solids.

Multi-watt, multi-octave, mid-infrared femtosecond source.

Spectroscopy in the wavelength range from 2 to 11 μm (900 to 5000 cm-1) implies a multitude of applications in fundamental physics, chemistry, as well as environmental and life sciences. The related vibrational transitions, which all infrared-active small molecules, the most common functional groups, as well as biomolecules like proteins, lipids, nucleic acids, and carbohydrates exhibit, reveal information about molecular structure and composition. However, light sources and detectors in the mid-infrared have been inferior to those in the visible or near-infrared, in terms of power, bandwidth, and sensitivity, severely limiting the performance of infrared experimental techniques. This article demonstrates the generation of femtosecond radiation with up to 5 W at 4.1 μm and 1.3 W at 8.5 μm, corresponding to an order-of-magnitude average power increase for ultrafast light sources operating at wavelengths longer than 5 μm. The presented concept is based on power-scalable near-infrared lasers emitting at a wavelength near 1 μm, which pump optical parametric amplifiers. In addition, both wavelength tunability and supercontinuum generation are reported, resulting in spectral coverage from 1.6 to 10.2 μm with power densities exceeding state-of-the-art synchrotron sources over the entire range. The flexible frequency conversion scheme is highly attractive for both up-conversion and frequency comb spectroscopy, as well as for a variety of time-domain applications.

Nanoantenna-Enhanced Radiative and Anisotropic Decay Rates in Monolayer-Quantum Dots

Nanoantenna-enhanced ultrafast emission from colloidal quantum dots as quantum emitters is required for fast quantum communications. On-chip integration of such devices requires a scalable and high-throughput technology. We report self-assembly lithography technique of preparing hybrid of gold nanorods antenna over a compact CdSe quantum dot monolayer. We demonstrate resonant and nonresonant gold nanorod antenna-enhanced radiative and anisotropic decay. Extensive simulations explain the mechanism of the decay rates and the role of antenna in both random and compact monolayers of quantum dots. The study could find applications in quantum dot display and quantum communication devices.

Plasmon-Enhanced Ultrasensitive Surface Analysis Using Ag Nanoantenna.

Raman scattering and fluorescence spectroscopy permeate analytic science and are featured in the plasmon-enhanced spectroscopy (PES) family. However, the modest enhancement of plasmon-enhanced fluorescence (PEF) significantly limits the sensitivity in surface analysis and material characterization. Herein, we report a Ag nanoantenna platform, which simultaneously fulfills very strong emission (an optimum average enhancement of 105-fold) and an ultrafast emission rate (∼280-fold) in PES. For applications in surface science, this platform has been examined with a diverse array of fluorophores. Meanwhile, we utilized a finite-element method (FEM) and time-dependent density functional theory (TD-DFT) to comprehensively investigate the mechanism of largely enhanced radiative decay. PES with a shell-isolated Ag nanoantenna will open a wealth of advanced scenarios for ultrasensitive surface analysis.

Enhanced Directional Emission from Monolayer WSe2 Integrated onto a Multiresonant Silicon-Based Photonic Structure

Two-dimensional transition-metal dichalcogenides such as WSe2 show great promise as versatile atomic-scale light sources for on-chip applications due to their advanced optoelectronic properties and compatibility with a silicon photonics platform. However, the sub-nanometer thickness of such active materials limits their emission efficiency. Hence, new approaches to simultaneously enhance the emission and control its directionality are required. Here, we demonstrate enhanced and directional emission from a WSe2 monolayer integrated onto a silicon photonic structure. This is achieved by coupling of the WSe2 layer to a multiresonant silicon grating-waveguide structure. The interaction with the multiple resonant modes supported by the structure provides simultaneous excitation and emission enhancement, while the dispersion of the modes further routes the emission into specified directions. In addition, our hybrid structure offers the opportunity for ultrafast emission modulation, owing to the reduced emission...

Relaxation Oscillations and Ultrafast Emission Pulses in a Disordered Expanding Polariton Condensate

Semiconductor microcavities are often influenced by structural imperfections, which can disturb the flow and dynamics of exciton-polariton condensates. Additionally, in exciton-polariton condensates there is a variety of dynamical scenarios and instabilities, owing to the properties of the incoherent excitonic reservoir. We investigate the dynamics of an exciton-polariton condensate which emerges in semiconductor microcavity subject to disorder, which determines its spatial and temporal behaviour. Our experimental data revealed complex burst-like time evolution under non-resonant optical pulsed excitation. The temporal patterns of the condensate emission result from the intrinsic disorder and are driven by properties of the excitonic reservoir, which decay in time much slower with respect to the polariton condensate lifetime. This feature entails a relaxation oscillation in polariton condensate formation, resulting in ultrafast emission pulses of coherent polariton field. The experimental data can be well reproduced by numerical simulations, where the condensate is coupled to the excitonic reservoir described by a set of rate equations. Theory suggests the existence of slow reservoir temporarily emptied by stimulated scattering to the condensate, generating ultrashort pulses of the condensate emission.

Development of an ultrafast electron source based on a cold-field emission gun for ultrafast coherent TEM

We report on the design of a femtosecond laser-driven electron source for ultrafast coherent transmission electron microscopy. The proposed architecture allows introducing an ultrafast laser beam inside the cold field emission source of a commercial TEM, aligning and focusing the laser spot on the apex of the nanoemitter. The modifications of the gun assembly do not deteriorate the performances of the electron source in conventional DC mode and allow easy switching between the conventional and ultrafast laser-driven emission modes. We describe here this ultrafast electron source and discuss its properties.

Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy.

The multifunctional protein cytochrome c (cyt c) plays key roles in electron transport and apoptosis, switching function by modulating bonding between a heme iron and the sulfur in a methionine residue. This Fe-S(Met) bond is too weak to persist in the absence of protein constraints. We ruptured the bond in ferrous cyt c using an optical laser pulse and monitored the bond reformation within the protein active site using ultrafast x-ray pulses from an x-ray free-electron laser, determining that the Fe-S(Met) bond enthalpy is ~4 kcal/mol stronger than in the absence of protein constraints. The 4 kcal/mol is comparable with calculations of stabilization effects in other systems, demonstrating how biological systems use an entatic state for modest yet accessible energetics to modulate chemical function.

Ultrafast emission decay with high emission efficiency of quantum dots in plasmonic–dielectric metasubstrates

We report on the ultrafast decay of quantum dots that reaches nearly 430 ps without reduction in the emission intensity when near a metasubstrate of simple geometry. By implementing a layered structure of amorphous silicon sandwiched between two gold layers, the balance between plasmonic near field enhancement and energy transfer of the quantum dots has been shifted. This is achieved by tailoring the amount of Förster resonance energy transfer (FRET) to the top Au layer and plasmonic near field enhancement by the bottom Au layer. We also study the impact of deposition of Al oxide on the top Au layer, forming a charge barrier junction that can suppress Auger recombination of quantum dots. The results show that such a barrier can increase emission efficiency of the metastructure without significant reduction in the decay rate. We study the impact of formation of small nanoislands to contiguous islands via variation of the thickness of the top Au layer, and discuss how such morphologies determine the amount of FRET, screening of plasmonic field from the bottom Au layer, and enhancement of emission due to their own plasmonic fields.

Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency.

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field-driven photoemission from metal tips provides high light-phase synchronization, but suffers large electron energy spreads (3-100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field-driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube-based ultrafast electron source opens exciting prospects for extending current characterization to sub-femtosecond temporal resolution as well as sub-nanometer spatial resolution.