Ultrafast Emission Research Articles

Warm-White Light Emission of Lead-free CsAg2I3 Single Crystal Scintillator with a One-Dimensional Electronic Structure.

Presently, the exploration of novel inorganic lead-free perovskite scintillators has emerged as a prominent topic in the field of perovskite materials. Extensive attention has been garnered by materials such as Cs3Cu2I5 due to their notable advantage in scintillation intensity, but the response time constants in the microsecond or even millisecond range severely constrain their potential applications in scintillators. In this study, large-sized (5-6 mm) CsAg2I3 single crystals with an ultrafast warm-white light emission on a nanosecond time scale are presented. Specifically, upon X-ray excitation, the single crystal demonstrates a broad-spectrum white light emission with a color temperature as high as 5129 K, attributed to its self-trapped exciton emission. The 137Cs energy spectrum reveals that CsAg2I3 possesses an ultrafast response for γ rays with a time constant of 15 ns, which is significantly faster than that of Cs3Cu2I5. Furthermore, time-resolved photoluminescence unveils a subnanosecond component with a response time of 0.9 ns. The characteristics of ultrafast warm-white light emission exhibit the significant potential of CsAg2I3 in radiation scintillation detection and its probability of playing a pivotal role in future radiation detection technology.

Near-field strong coupling and entanglement of quantum emitters for room-temperature quantum technologies

In recent years, quantum nanophotonics has forged a rich nexus of nanotechnology with photonic quantum information processing, offering remarkable prospects for advancing quantum technologies beyond their current technical limits in terms of physical compactness, energy efficiency, operation speed, temperature robustness and scalability. In this perspective, we highlight a number of recent studies that reveal the especially compelling potential of nanoplasmonic cavity quantum electrodynamics for driving quantum technologies down to nanoscale spatial and ultrafast temporal regimes, whilst elevating them to ambient temperatures. Our perspective encompasses innovative proposals for quantum plasmonic biosensing, driving ultrafast single-photon emission and achieving near-field multipartite entanglement in the strong coupling regime, with a notable emphasis on the use of industry-grade devices. We conclude with an outlook emphasizing how the bespoke characteristics and functionalities of plasmonic devices are shaping contemporary research directives in ultrafast and room-temperature quantum nanotechnologies.

Significant Enhancement in THz Emission and Piezoelectricity in Atomically Thin Nb-Doped MoS2.

A significantly enhanced THz radiation generation from femtosecond photoexcited MoS2 layers due to Nb-doping is reported here. Different microscopic mechanisms involved in the THz photocurrent generation vary in their relative contributions in the two cases of photoexcitation, i.e., above and below the electronic bandgap of the layers. For a moderate Nb-doping level of just ∼0.05%, we have observed a multifold enhancement in the THz emission for the case of the above bandgap excitation, which is, though, nearly 1.5 times for the case of the below bandgap excitation of the monolayer MoS2. Alongside the difference in THz generation efficiency, the THz pulse polarity is also reversed at the above bandgap excitation of the Nb-doped layers, consequent to the reversed surface depletion field. Except for a slightly smaller difference in the THz enhancement factor, all the observations are reproducible in the bilayers as well to imply a weaker inversion symmetry and reduced screening of the surface depletion field due to Nb-doping. Furthermore, we employed pristine MoS2 and Nb-doped MoS2 monolayers to fabricate piezoelectric nanogenerator devices. Like enhancement in the ultrafast THz emission, the piezoelectric performance of the nanogenerator, fabricated with the Nb-doped MoS2 monolayer is also increased by a similar factor.

Ultrafast green single photon emission from an InGaN quantum dot-in-a-GaN nanowire at room temperature

Ultrafast green single photon emission from an InGaN quantum dot-in-a-GaN nanowire at room temperature

Timing limits of ultrafast cross-luminescence emission in CsZnCl-based crystals for TOF-CT and TOF-PET

BackgroundGood timing resolution in medical imaging applications such as TOF-CT or TOF-PET can boost image quality or patient comfort significantly by reducing the influence of background noise. However, the timing resolution of state-of-the-art detectors in CT and PET are limited by their light emission process. Core-valence cross-luminescence is an alternative, but well-known compounds (e.g. BaF2) pose several problems for medical imaging applications, such as their emission wavelength in the deep UV. CsZnCl-based materials show promise to solve this issue, as they provide fast decay times of 1–2 ns and an emission wavelength around 300 nm.ResultsIn this work, we investigated two CsZnCl-compounds: Cs2ZnCl4 and Cs3ZnCl5. We validated the previously published decay times on a time-correlated single-photon counting setup with 1.786 ± 0.016 ns for Cs2ZnCl4 and 1.034 ± 0.013 ns for Cs3ZnCl5. The setup’s high resolution enabled the discovery of an additional prompt emission component with a significant abundance of 98 ± 18 (Cs2ZnCl4) and 86 ± 14 (Cs3ZnCl5) photons/MeV energy deposit. In a PET coincidence experiment, we measured the best coincidence time resolution (CTR) of 62 ps (FWHM) for Cs2ZnCL4 coupled to FBK VUV SiPMs with silicon oil. To assess the CTR for lower energies, we filtered the energy along the Compton continuum and found a deteriorated CTR that seems to be mainly influenced by photon statistics. Furthermore, this study gave us a rough estimate of e.g. 150 ps (FWHM) CTR at 100 keV energy for Cs2ZnCL4. From measurements with high activity of 14 MBq to check for pile-up effects we assume that Cs2ZnCl4 is better suited for high-rate time-of-flight applications than lutetium-based oxides. Simulations demonstrated that the stopping power of Cs2ZnCl4 is lower than for LSO:Ce,Ca, meaning that a high amount of material would be needed for TOF-PET applications. However, the stopping power seems acceptable for applications in TOF-CT.ConclusionsThe fast decay time, state-of-the-art CTR in benchtop experiments and high-rate suitability make CsZnCl materials a promising candidate for time-of-flight experiments. We consider especially TOF-CT a suitable application due to its relatively low X-ray energies (~ 100 keV) and the thusly acceptable stopping power of Cs2ZnCl4. Currently, further exploration of the prompt emission and its creation mechanism is planned, as well as investigating the light transport of Cs2ZnCl4 in longer crystals.

Evidence of abnormal hot carrier thermalization at van Hove singularity of twisted bilayer graphene

Interlayer twist evokes revolutionary changes to the optical and electronic properties of twisted bilayer graphene (TBG) for electronics, photonics and optoelectronics. Although the ground state responses in TBG have been vastly and clearly studied, the dynamic process of its photoexcited carrier states mainly remains elusive. Here, we unveil the photoexcited hot carrier dynamics in TBG by time-resolved ultrafast photoluminescence (PL) autocorrelation spectroscopy. We demonstrate the unconventional ultrafast PL emission between the van Hove singularities (VHSs) with a ∼4 times prolonged relaxation lifetime. This intriguing photoexcited carrier behavior is ascribed to the abnormal hot carrier thermalization brought by bottleneck effects at VHSs and interlayer charge distribution process. Our study on hot carrier dynamics in TBG offers new insights into the excited states and correlated physics of graphene twistronics systems.

Triplet state photophysics of bis(dimethylphenanthroline)copper(I) might involve volume-changing molecular motion: Ultrafast absorption and emission studies

Study of triplet photophysics has remained a contemporary field for the last eight decades due to its wide-ranging applications. Many recent studies deciphered the influence of molecular vibrations on the electronic coupling for facile intersystem crossing (ISC) in numerous metal complexes. Through a combined analysis of steady-state and time-resolved spectroscopies, we identified the role of environmental rigidity on the triplet photophysics of bis(dimethylphenanthroline)copper(I) chloride ([Cu(dmphen)2]Cl). Our experiments suggest an involvement of volume-changing coordinate in ISC of [Cu(dmphen)2]Cl having an activation energy barrier of 5.9 kJ mol−1. This insight can be useful in the research and development of efficient triplets.

Properties and characteristics of the nanosecond discharge developing at the water–air interface: tracking evolution from a diffused streamer to a spark filament

The characteristics of nanosecond discharge propagating along the water–air interface in a unique dielectric-barrier discharge (DBD)-like configuration with coplanar electrodes submerged in deionised (DI)/tap water are studied by combining ultrafast imaging and emission spectra with electrical characteristics. Time-resolved images provide a clear signature of streamer channels excited on the water surface at either side of the blade (insulated plastic separating the anode/cathode) and propagating perpendicularly away from it towards the anode/cathode with different velocities. Later on, the streamer channels convert into a few discrete and bright discharge channels due to ionisation instability (spark phase). There is no distinctive dependence on water conductivity in the streamer phase, as the optical emission spectroscopy and images of discharges only showed an increase of the luminosity and no significant changes in morphology. However, in the spark phase, more numerous, brighter, and thicker filaments form in tap water. The time-resolved emission spectra reveal the dominance of the first and second positive system of N2 molecular bands in the streamer phase, followed by the appearance of atomic lines of hydrogen, nitrogen, and oxygen in the spark phase. The emission spectra are utilised to estimate several important parameters (gas temperature, reduced electric field ( E/N ), and electron density ( ne )). The streamer phase is characterised by a low gas temperature and a peak E/N amplitude between 700 and 850 Td. On the other hand, the subsequent spark phase is characterised by a gas temperature of ∼400/1100 K and a free electron density up to ne∼1017 –1018 cm−3 in DI/tap water.

Nanosecond pulse X-ray emission source based on ultrafast laser modulation

<sec>In response to the growing demand for miniaturized ultrafast pulsed X-ray sources in the fields of fundamental science and space applications, we design and develop an ultrafast pulsed X-ray generator based on a laser-modulated light source and a photoelectric cathode. This innovative technology addresses the limitations commonly encountered in traditional X-ray emission devices, such as low repetition rate, insufficient time stability, and suboptimal pulse characteristics.</sec><sec>Our effort is to study and develop the ultrafast modulation control module for the pulsed X-ray generator. This effort results in achieving high levels of time accuracy and stability in ultrafast time-varying photon signals. Moreover, we successfully generate nanosecond pulsed X-rays by using a laser-controlled light source.</sec><sec>Theoretically, we establish a comprehensive time response model for the pulsed X-ray generator in response to short pulses. This includes a thorough analysis of the time characteristics of the emitted pulsed X-rays in the time domain. Experimentally, we conduct a series of tests related to various time-related parameters of the laser-controlled light source. Additionally, we design and implemente an experimental test system for assessing the time characteristics of pulsed X-rays, by using an ultrafast scintillation detector.</sec><sec>The experimental results clearly demonstrate that our pulsed X-ray generator achieves impressive capabilities, including high repetition rates (12.5 MHz), ultrafast pulses (4 ns), and exceptional time stability (400 ps) in X-ray emission. These results closely align with our established theoretical model. Compared with traditional modulation techniques, our system exhibits significant improvement in pulse time parameters, thereby greatly expanding its potential applications.</sec><sec>This research provides a valuable insight into achieving ultra-high time stability and ultrafast pulsed X-ray emission sources. These advances will further enhance the capabilities of X-ray technology for scientific research and space applications.</sec>

Experimental capabilities for liquid jet samples at sub-MHz rates at the FXE Instrument at European XFEL.

The Femtosecond X-ray Experiments (FXE) instrument at the European X-ray Free-Electron Laser (EuXFEL) provides an optimized platform for investigations of ultrafast physical, chemical and biological processes. It operates in the energy range 4.7-20 keV accommodating flexible and versatile environments for a wide range of samples using diverse ultrafast X-ray spectroscopic, scattering and diffraction techniques. FXE is particularly suitable for experiments taking advantage of the sub-MHz repetition rates provided by the EuXFEL. In this paper a dedicated setup for studies on ultrafast biological and chemical dynamics in solution phase at sub-MHz rates at FXE is presented. Particular emphasis on the different liquid jet sample delivery options and their performance is given. Our portfolio of high-speed jets compatible with sub-MHz experiments includes cylindrical jets, gas dynamic virtual nozzles and flat jets. The capability to perform multi-color X-ray emission spectroscopy (XES) experiments is illustrated by a set of measurements using the dispersive X-ray spectrometer in von Hamos geometry. Static XES data collected using a multi-crystal scanning Johann-type spectrometer are also presented. A few examples of experimental results on ultrafast time-resolved X-ray emission spectroscopy and wide-angle X-ray scattering at sub-MHz pulse repetition rates are given.

Tunable ultrafast thermionic emission from femtosecond-laser hot spot on a metal surface by control of laser polarization and angle of incidence: A numerical investigation

Ultrafast laser induced thermionic emission from metal surfaces has several applications. Here, we investigate the role of laser polarization and angle of incidence on the ultrafast thermionic emission process from laser driven gold coated glass surface. The spatio-temporal evolution of electron and lattice temperatures are obtained using an improved three-dimensional (3D) two-temperature model (TTM) which takes into account the 3D laser pulse profile focused obliquely onto the surface. The associated thermionic emission features are described through the modified Richardson-Dushman equation, including dynamic space-charge effects and are included self-consistently in our numerical approach. We show that temperature-dependent reflectivity influences laser energy absorption. The resulting peak electron temperature on the metal surface monotonically increases with the angle of incidence for the P polarization, while for the S polarization it shows the opposite trend. We observe that thermionic emission duration shows a strong dependence on the angle of incidence and contrasting polarization dependent behavior. The duration of the thermionic current shows strong correlation to the intrinsic electron-lattice thermalization time, in a fluence regime well below the damage threshold of gold. The observations and insights have important consequences in designing ultrafast thermionic emitters using a metal based architecture.

Electrically-driven ultrafast out-of-equilibrium light emission from hot electrons in suspended graphene/hBN heterostructures

Nanoscale light sources with high speed of electrical modulation and low energy consumption are key components for nanophotonics and optoelectronics. The record-high carrier mobility and ultrafast carrier dynamics of graphene make it promising as an atomically thin light emitter, which can be further integrated into arbitrary platforms by van der Waals forces. However, due to the zero bandgap, graphene is difficult to emit light through the interband recombination of carriers like conventional semiconductors. Here, we demonstrate ultrafast thermal light emitters based on suspended graphene/hexagonal boron nitride (Gr/hBN) heterostructures. Electrons in biased graphene are significantly heated up to 2800 K at modest electric fields, emitting bright photons from the near-infrared to the visible spectral range. By eliminating the heat dissipation channel of the substrate, the radiation efficiency of the suspended Gr/hBN device is about two orders of magnitude greater than that of graphene devices supported on SiO2 or hBN. We further demonstrate that hot electrons and low-energy acoustic phonons in graphene are weakly coupled to each other and are not in full thermal equilibrium. Direct cooling of high-temperature hot electrons to low-temperature acoustic phonons is enabled by the significant near-field heat transfer at the highly localized Gr/hBN interface, resulting in ultrafast thermal emission with up to 1 GHz bandwidth under electrical excitation. It is found that suspending the Gr/hBN heterostructures on the SiO2 trenches significantly modifies the light emission due to the formation of the optical cavity and showed a ∼440% enhancement in intensity at the peak wavelength of 940 nm compared to the black-body thermal radiation. The demonstration of electrically driven ultrafast light emission from suspended Gr/hBN heterostructures sheds the light on applications of graphene heterostructures in photonic integrated circuits, such as broadband light sources and ultrafast thermo-optic phase modulators.

Revealing the ultrafast spontaneous emission in plasmon-enhanced monolayer semiconductor nano-light sources

Nanoscale spontaneous light sources are promising alternatives to lasers for high-speed optical communications and interconnections through energy-efficient integrated circuits. Yet, developing the spontaneous light sources faster than lasers is hampered by the detection means (e.g., time-resolved fluorescence spectroscopy). Here, by coupling monolayer WSe2 to individual plasmonic nanocavities, we achieved an efficient spontaneous light source with potential ultrafast modulation bandwidth and superior brightness. The ultrafast radiative decay rates can be determined and derived solely from the experimental parameters by combining the coupling strength and the photoluminescence enhancement in a single nanocavity-WSe2 hybrid. As a result, the hybrid light source has a radiative lifetime down to 350 fs, indicating a potential modulation bandwidth up to 440 GHz, which is 10 times of the traditional semiconductor lasers. Furthermore, the quantum yield is enhanced by a factor of over 300-folds up to 20.8% through making full use of the highly confined nanocavity mode. The nanocavity-WSe2 hybrid we built provides a promising approach for constructing high-speed light-emitting devices.

Deep learning enhanced ultra-fast SPECT/CT bone scan in patients with suspected malignancy: quantitative assessment and clinical performance

Objectives. To evaluate the clinical performance of deep learning-enhanced ultrafast single photon emission computed tomography/computed tomography (SPECT/CT) bone scans in patients with suspected malignancy. Approach. In this prospective study, 102 patients with potential malignancy were enrolled and underwent a 20 min SPECT/CT and a 3 min SPECT scan. A deep learning model was applied to generate algorithm-enhanced images (3 min DL SPECT). The reference modality was the 20 min SPECT/CT scan. Two reviewers independently evaluated general image quality, Tc-99m MDP distribution, artifacts, and diagnostic confidence of 20 min SPECT/CT, 3 min SPECT/CT, and 3 min DL SPECT/CT images. The sensitivity, specificity, accuracy, and interobserver agreement were calculated. The lesion maximum standard uptake value (SUVmax) of the 3 min DL and 20 min SPECT/CT images was analyzed. The peak signal-to-noise ratio (PSNR) and structure similarity index measure (SSIM) were evaluated. Main results. The 3 min DL SPECT/CT images showed significantly superior general image quality, Tc-99m MDP distribution, artifacts, and diagnostic confidence than the 20 min SPECT/CT images (P < 0.0001). The diagnostic performance of the 20 min and 3 min DL SPECT/CT images was similar for reviewer 1 (paired X 2 = 0.333, P = 0.564) and reviewer 2 (paired X 2 = 0.05, P = 0.823). The diagnosis results for the 20 min (kappa = 0.822) and 3 min DL (kappa = 0.732) SPECT/CT images showed high interobserver agreement. The 3 min DL SPECT/CT images had significantly higher PSNR and SSIM than the 3 min SPECT/CT images (51.44 versus 38.44, P < 0.0001; 0.863 versus 0.752, P < 0.0001). The SUVmax of the 3 min DL and 20 min SPECT/CT images showed a strong linear relationship (r = 0.991; P < 0.0001). Significance. Ultrafast SPECT/CT with a 1/7 acquisition time can be enhanced by a deep learning method to achieve comparable image quality and diagnostic value to those of standard acquisition.

Ultrafast Jahn-Teller Photoswitching in Cobalt Single-Ion Magnets.

Single-ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering breakthroughs in quantum information and communication technologies could be alleviated by new generations of SIMs displaying multifunctionality. Here, ultrafast optical absorption spectroscopy and X-ray emission spectroscopy are employed to track the photoinduced spin-state switching of the prototypical complex [Co(terpy)2 ]2+ (terpy=2,2':6',2″-terpyridine) in solution phase. The combined measurements and their analysis supported by density functional theory (DFT), time-dependent-DFT (TD-DFT) and multireference quantum chemistry calculations reveal that the complex undergoes a spin-state transition from a tetragonally elongated doublet state to a tetragonally compressed quartet state on the femtosecond timescale, i.e., it sustains ultrafast Jahn-Teller (JT) photoswitching between two different spin multiplicities. Adding new Co-based complexes as possible contenders in the search for JT photoswitching SIMs will greatly widen the possibilities for implementing magnetic multifunctionality and eventually controlling ultrafast magnetization with optical photons.

Excitation wavelength-dependent ultrafast THz emission from surface and bulk of three-dimensional topological insulators

Three-dimensional topological insulators possess various interesting properties that are promising for various modern applications, including in the recently emerging fields of ultrafast THz photonics and spintronics. Their gapless spin-momentum-locked topological surface states with the presence of chiral spin structure are relevant for the development of light helicity-sensitive THz emitters and detectors. In this paper, we report femtosecond excitation pulse wavelength and helicity-dependent response of Bi2Te3 and Bi2Se3 for an enhanced broadband THz pulse emission from the surface and bulk states. Specifically, the excitation wavelength has been varied in a large range from near UV to near IR, where it was observed that the photoexcitation at shorter wavelengths enhances the THz emission from both the surface and bulk states but more rapidly from the surface states. These results will be highly relevant for developing chirality-sensitive efficient THz emitters and detectors.

Sub-picosecond steering of ultrafast incoherent emission from semiconductor metasurfaces

Sub-picosecond steering of ultrafast incoherent emission from semiconductor metasurfaces

Noncollinear antiferromagnetic textures driven high-harmonic generation from magnetic dynamics in the absence of spin-orbit coupling

We demonstrate the generation of high order harmonics in carrier pumping from precessing ferromagnetic or antiferromagnetic orders, excited via magnetic resonance, in the presence of topological antiferromagnetic textures. This results in an enhancement of the carrier dynamics by orders of magnitude, enabling for an emission deep in the THz frequency range. Interestingly, the generation process occurs in an intrinsic manner, and is solely governed by the interplay between the s-d exchange coupling underlying the noncollinear antiferromagnetic order and the dynamical s-d exchange constant of the magnetic drive. Therefore, the relativistic spin–orbit interaction is not required for the emergence of high harmonics in the pumped currents. Accordingly, the noncollinear topological antiferromagnetic order is presented as an alternative to spin–orbit interaction for the purpose of harnessing high harmonic emission in carrier pumping. Furthermore, we demonstrate the emergence of high harmonics from random magnetic impurities. This suggests the universality of the magnetically induced high harmonic emission in the presence of real and/or momentum space noncollinear textures. Our proposal initiates a tantalizing prospect for the utilization of topological textures in the context of the highly active domains of ultrafast spintronics and THz emission.

Structural change dynamics of heteroleptic Cu(I) complexes observed by ultrafast emission spectroscopy.

[Cu(I)(dmp)(P)2]+ (dmp = 2,9-dimethyl-1,10-phenanthroline derivatives; P = phosphine ligand) is one of the most promising photosensitizers used in a photo-catalytic system for reducing CO2, for which the quantum yield is as high as 57%. In this work, time-resolved emission spectra of Cu(I) complexes in solutions were investigated using femtosecond fluorescence up-conversion and nanosecond time-resolved emission spectroscopic systems. The temporal profiles of emission intensities less than 10 ps in acetonitrile solution were reproduced using a tri-exponential function with three-time constants of 0.040 ps, 0.78 ps and 8.0 ps. We found that only the second time constant is dependent on the solvent (acetonitrile: 0.78 ps, butyronitrile: 1.4 ps), indicating that the 0.78 ps spectral change is attributed to the structural change of the Cu(I) complex. The oscillator strengths of transition species are derived from the intensities in the time-resolved emission spectra (species-associated spectra). Based on the oscillator strengths, we concluded that the 0.040 ps process is the Sn → S1 internal conversion and the 0.78 ps process is a structural change in the S1 state. The final time constant of 8.0 ps is assigned to the S1 → T1 intersystem crossing because the 3MLCT state (τT1 = 97 ns) is generated after the decay. The DFT calculation showed that the 0.78 ps spectral change (∼600 cm-1 redshift) is attributed to Jahn-Teller distortion around the metal center, and there is a large structural change in the ligand, which results in a large Stokes shift in the Sn state (7.3 × 103 cm-1).

Single-shot measurement of wavelength-resolved state of polarization dynamics in ultrafast lasers using dispersed division-of-amplitude

Characterization of the state of polarization (SOP) of ultrafast laser emission is relevant in several application fields such as field manipulation, pulse shaping, testing of sample characteristics, and biomedical imaging. Nevertheless, since high-speed detection and wavelength-resolved measurements cannot be simultaneously achieved by commercial polarization analyzers, single-shot measurements of the wavelength-resolved SOP of ultrafast laser pulses have rarely been reported. Here, we propose a method for single-shot, wavelength-resolved SOP measurements that exploits the method of division-of-amplitude under far-field transformation. A large accumulated chromatic dispersion is utilized to time-stretch the laser pulses via dispersive Fourier transform, so that spectral information is mapped into a temporal waveform. By calibrating our test matrix with different wavelengths, wavelength-resolved SOP measurements are achieved, based on the division-of-amplitude approach, combined with high-speed opto-electronic processing. As a proof-of-concept demonstration, we reveal the complex wavelength-dependent SOP dynamics in the build-up of dissipative solitons. The experimental results show that the dissipative soliton exhibits far more complex wavelength-related polarization dynamics, which are not shown in single-shot spectrum measurement. Our method paves the way for single-shot measurement and intelligent control of ultrafast lasers with wavelength-resolved SOP structures, which could promote further investigations of polarization-related optical signal processing techniques, such as pulse shaping and hyperspectral polarization imaging.