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At least 19 records

Controllable X-ray Pulse Trains from Enhanced Self-Amplified Spontaneous Emission

We report the demonstration of optical compression of an electron beam and the production of controllable trains of femtosecond, soft x-ray pulses with the Linac Coherent Light Source (LCLS) freeelectron laser (FEL). This is achieved by enhanced self-amplified spontaneous emission with a 2 μm laser and a dechirper device. Optical compression was achieved by modulating the energy of an electron beam with the laser and then compressing with a chicane, resulting in high current spikes on the beam which we observe to lase. A dechirper was then used to selectively control the lasing region of the electron beam. Field autocorrelation measurements indicate a train of pulses, and we find that the number of pulses within the train can be controlled (from 1 to 5 pulses) by varying the dechirper position and undulator taper. These results are a step toward attosecond spectroscopy with x-ray FELs as well as future FEL schemes relying on optical compression of an electron beam.

Duris, Joseph P↗

On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr 3 Single Crystals

CsPbBr 3 is an all-inorganic halide perovskite with excellent photoluminescence (PL) properties for laser applications. Amplified spontaneous emission (ASE) is a prerequisite for lasing and typically observed from low-dimensional CsPbBr3 nanostructures, where quantum confinement enhances ASE. However, a gain medium for lasing should be prepared into a robust bulk form that works under intense light illumination. Here, we demonstrate that bulk CsPbBr 3 single crystals exhibit highly efficient ASE with a threshold of 46 MWcm -2 at 520 nm, if PL reabsorption via the indirect Rashba gap is properly suppressed by thickness control. Based on a series of spectroscopic and microscopic measurements, we show that this below-the-gap absorption can significantly alter the PL feature and even the apparent color of the crystal depending on the crystal size. Our results show that a thin CsPbBr 3 single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light–matter interaction.

36 MATERIALS SCIENCE↗

Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters

Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe 2+ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Furthermore, our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Stochastic modeling of x-ray superfluorescence

An approach to modeling the dynamics of x-ray amplified spontaneous emission and superfluorescence, the phenomenon of collective x-ray emission initiated by intense pulses of x-ray free-electron lasers, is developed based on stochastic partial differential equations. The equations are derived from first principles, and the relevant approximations, derivation steps, and extensions specific to stimulated x-ray emission are presented. The resulting equations take the form of three-dimensional generalized Maxwell-Bloch equations augmented with noise terms for both field and atomic variables. The derived noise terms possess specific correlation properties that enable the correct reconstruction of spontaneous emission. Consequently, the developed theoretical formalism is universally suitable for describing all stages of stimulated x-ray emission: spontaneous emission, amplified spontaneous emission, and superfluorescence. Here, we present numerical examples that illustrate various properties of the emitted field, including spatiotemporal coherence and spectral-angular and polarization characteristics. We anticipate that the proposed theoretical framework will establish a robust foundation for interpreting measurements in stimulated x-ray emission spectroscopy, modeling x-ray laser oscillators, and describing other experiments leveraging x-ray superfluorescence.

74 ATOMIC AND MOLECULAR PHYSICS↗

2-.mu.m fiber amplified spontaneous emission (ASE) source

A 2-.mu.m fiber Amplified Spontaneous Emission (ASE) source provides a wide emission bandwidth and improved spectral stability/purity for a given output power. The fiber ASE source is formed from a heavy metal oxide multicomponent glass selected from germanate, tellurite and bismuth oxides and doped with high concentrations, 0.5-15 wt. %, thulium oxides (Tm.sub.2O.sub.3) or 0.1-5 wt% holmium oxides (Ho.sub.2O.sub.3) or mixtures thereof. The high concentration of thulium dopants provide highly efficient pump absorption and high quantum efficiency. Co-doping of Tm and Ho can broaden the ASE spectrum.

Jiang, Shibin↗

Amplified spontaneous emission measurement of a line-narrowed, tunable, Ti:Al2O3 amplifier using rubidium absorption

Amplified spontaneous emission, ASE, generated by a Ti:Al2O3 laser amplifier has been measured as a function of pump energy, and thus gain, using the atomic absorption of rubidium, Rb, gas at 0.780 micron. By tuning the Ti:Al2O3 laser, the Rb cell could selectively absorb the narrow spectral bandwidth laser radiation while transmitting the wide spectral bandwidth ASE. Transmission of laser amplifier pulses through a Rb absorption cell, measured at various temperatures, thus allows the measurement of the weak ASE in the vicinity of the strong laser pulse. A model for the transmission of Rb as a function of temperature and wavelength has been developed. The measured transmissions are in good agreement with the transmission model predictions.

Barnes, James C.↗

Amplified spontaneous emission in solar-pumped iodine laser

The amplified spontaneous emission (ASE) from a long pulse, solar-simulating radiation pumped iodine laser amplifier is studied. The ASE threshold pump intensity is almost proportional to the inverse of the laser gain length when the gas pressure is constant in the laser tube.

Cho, Yong S.↗

Amplified spontaneous emission from europium-based molecular complexes coupled to photonic crystal cavities

Rare-earth ion-based materials bear many remarkable optical properties that render them highly appealing for lighting and quantum-related applications. However, their small oscillator strength and weak emission often pose limitations. Here, in this work, we synthesize and couple Eu(III)-based molecular complexes to nanobeam photonic crystals supporting air modes. A reasonable spatial overlap between the molecular complexes and cavity modes leads to an average spontaneous emission coupling efficiency of 0.19. Our pump power-dependent photoluminescence measurements evidence amplified spontaneous emission from the molecular complexes with an amplification threshold as low as 4.4 W/cm 2 , likely benefiting from the efficient coupling. These findings suggest that integrating rare-earth ion-based molecular complexes with photonic structures could be a viable approach for regulating their emission characteristics for particular applications.

36 MATERIALS SCIENCE↗

Development of a High Min-Entropy Quantum Random Number Generator Based on Amplified Spontaneous Emission

We present the theory, architecture, and performance characteristics of a quantum random number generator (QRNG) which operates in a PCI express form factor-compatible plug-and-play design. The QRNG relies on a thermal light source (in this case, amplified spontaneous emission), which exhibits photon bunching according to the Bose–Einstein (BE) statistics. We demonstrate that 98.7% of the unprocessed random bit stream min-entropy is traceable to the BE (quantum) signal. The classical component is then removed using a non-reuse shift-XOR protocol, and the final random numbers are generated at a 200 Mbps rate and shown to pass the statistical randomness test suites FIPS 140-2, Alphabit, SmallCrush, DIEHARD, and Rabbit of the TestU01 library.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Band Edge Excitons and Amplified Spontaneous Emission of Mercury Chalcogenide Nanoplatelets

Colloidal nanoplatelets of HgSe and HgTe prepared indirectly through cation exchange reactions can transfer many of the advantageous properties of atomically precise, 2D cadmium chalcogenides to the near-infrared (NIR) spectral window. In this work, HgSe and HgTe nanoplatelets are studied to understand their fundamental photophysical properties, particularly those areas of similarity and difference from cadmium-based NPLs, and to examine their potential as optical gain media. Similar to cadmium chalcogenide NPLs, low-temperature photoluminescence of HgTe NPLs displays two-color emission that depends on temperature, sample, fluence, excitation frequency, and irradiation time. Both HgTe and HgSe show nanosecond emission dynamics at temperatures as low as 2.5 K, with no indication that bright-dark excitonic splitting governs the low-temperature photoluminescence. Collectively, experimental data is most consistent with emission from a negative trion state at low temperature. Although the mercury chalcogenide nanoplatelets are shown to have broadened optical resonances compared to the cadmium chalcogenides from which they are derived, they retain slow Auger recombination and can display low-threshold amplified spontaneous emission in the NIR spectral window. Optical pumping thresholds for HgTe NPLs are observed as low as 4.4 µJ cm -2 and highlight the potential 2D nanoplatelets as gain medium in the near-infrared.

36 MATERIALS SCIENCE↗

Amplified Spontaneous Emission from Electron–Hole Quantum Droplets in Colloidal CdSe Nanoplatelets

Two-dimensional cadmium selenide nanoplatelets (NPLs) exhibit large absorption cross sections and homogeneously broadened band-edge transitions that offer utility in wide-ranging optoelectronic applications. Here, we examine the temperature-dependence of amplified spontaneous emission (ASE) in 4- and 5-monolayer thick NPLs and show that the threshold for close-packed (neat) films decreases with decreasing temperature by a factor of 2-10 relative to ambient temperature owing to extrinsic (trapping) and intrinsic (phonon-derived line width) factors. Interestingly, for pump intensities that exceed the ASE threshold, we find development of intense emission to lower energy in particular provided that the film temperature is <= 200 K. For NPLs diluted in an inert polymer, both biexcitonic ASE and low-energy emission are suppressed, suggesting that described neat-film observables rely upon high chromophore density and rapid, collective processes. Transient emission spectra reveal ultrafast red-shifting with the time of the lower energy emission. Taken together, these findings indicate a previously unreported process of amplified stimulated emission from polyexciton states that is consistent with quantum droplets and constitutes a form of exciton condensate. For studied samples, quantum droplets form provided that roughly 17 meV or less of thermal energy is available, which we hypothesize relates to polyexciton binding energy. Polyexciton ASE can produce pump-fluence-tunable red-shifted ASE even 120 meV lower in energy than biexciton ASE. Finally, our findings convey the importance of biexciton and polyexciton populations in nanoplatelets and show that quantum droplets can exhibit light amplification at significantly lower photon energies than biexcitonic ASE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanowire implosion under laser amplified spontaneous emission pedestal irradiation

Nanowire array targets exhibit high optical absorption when interacting with short, intense laser pulses. This leads to an increased yield in the production of accelerated particles for a variety of applications. However, these interactions are sensitive to the laser prepulse and could be significantly affected. Here, we show that an array of aligned nanowires is imploded when irradiated by an Amplified Spontaneous Emission pedestal of a 1 PW laser with an intensity on the order of 10 11 W cm –2 . Using radiation hydrodynamics simulations, we demonstrate that the electron density profile is radially compressed at the tip by the rocket-like propulsion of the ablated plasma. The mass density compression increases up to 2.9x when a more dense nanowire array is used. This is due to the ablation pressure from the neighboring nanowires. These findings offer valuable information for selecting an appropriate target design for experiments aimed at enhancing production of accelerated particles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Electrically driven amplified spontaneous emission from colloidal quantum dots

Colloidal quantum dots (QDs) are attractive materials for realizing solution-processable laser diodes that could benefit from size-controlled emission wavelengths, low optical-gain thresholds and ease of integration with photonic and electronic circuits. However, the implementation of such devices has been hampered by fast Auger recombination of gain-active multicarrier states, poor stability of QD films at high current densities and the difficulty to obtain net optical gain in a complex device stack wherein a thin electroluminescent QD layer is combined with optically lossy charge-conducting layers. Here we resolve these challenges and achieve amplified spontaneous emission (ASE) from electrically pumped colloidal QDs. The developed devices use compact, continuously graded QDs with suppressed Auger recombination incorporated into a pulsed, high-current-density charge-injection structure supplemented by a low-loss photonic waveguide. These colloidal QD ASE diodes exhibit strong, broadband optical gain and demonstrate bright edge emission with instantaneous power of up to 170 μW.

36 MATERIALS SCIENCE↗

Two‐Color Amplified Spontaneous Emission from Auger‐Suppressed Quantum Dots in Liquids

Abstract Colloidal quantum‐dot (QD) lasing is normally achieved in close‐packed solid‐state films, as a high QD volume fraction is required for stimulated emission to outcompete fast Auger decay of optical‐gain‐active multiexciton states. Here a new type of liquid optical‐gain medium is demonstrated, in which compact compositionally‐graded QDs (ccg‐QDs) that feature strong suppression of Auger decay are liquefied using a small amount of solvent. Transient absorption measurements of ccg‐QD liquid suspensions reveal broad‐band optical gain spanning a wide spectral range from 560 (green) to 675 nm (red). The gain magnitude is sufficient to realize a two‐color amplified spontaneous emission (ASE) at 637 and 594 nm due to the band‐edge (1S) and the excited‐state (1P) transition, respectively. Importantly, the ASE regime is achieved using quasicontinuous excitation with nanosecond pulses. Furthermore, the ASE is highly stable under prolonged excitation, which stands in contrast to traditional dyes that exhibit strong degradation under identical excitation conditions. These observations point toward a considerable potential of high‐density ccg‐QD suspensions as liquid, dye‐like optical gain media that feature readily achievable spectral tunability and stable operation under intense photoexcitation.

Li, Xueyang↗

Synthesis of Thick Hg x Cd 1– x Se Nanoplatelets by Cation Exchange Catalyzed by Silver Ions, Showing Amplified Spontaneous Emission

II-VI semiconductor nanoplatelets have emerged as promising candidates for various applications, owing to their tunable optical properties dictated by their thickness and compositions. In the realm of infrared technology, mercury chalcogenides stand out as particularly promising materials for optoelectronic applications. However, the direct synthesis of 2D particles in this category remains challenging, thus prompting the exploration of alternative methods such as cation exchange. Here, we demonstrate that the cation exchange process from cadmium to mercury can be effectively catalyzed by monovalent Ag + cations. Further, this catalysis facilitates the formation of alloyed Hg x Cd 1-x Se nanoplatelets with tunable optical properties, with the photoluminescence peak ranging from 1.23 eV for the thinnest three-monolayer (ML) nanoplatelets to 0.92 eV for the thickest 7 ML nanoplatelets. The Ag + ions reduce the activation energy of the cation exchange process by a factor of 2, enabling enhanced penetration of mercury atoms deep into the native CdSe nanoplatelets. Moreover, these nanoplatelets exhibit optical gain in the infrared spectrum, including the 1.3 μm telecommunication band, with a fluence threshold at 80 K of 50 μJ∙cm -2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental demonstration of enhanced self-amplified spontaneous emission by photocathode temporal shaping and self-compression in a magnetic wiggler

In this paper we demonstrate experimentally the generation of attosecond soft X-ray free-electron laser (XFEL) pulses based on a novel approach to enhanced self-amplfied spontaneous emission. Instead of utilizing an external laser, we shape the electron beam at the cathode by laser pulse stacking. We enhance the high-current spike in the beam profile through a self-compression process which uses short-range coherent synchrotron radiation in a wiggler and a downstream magnetic chicane. The undulator taper is then matched with the energy chirp along the beam for attosecond XFEL generation. Start-to-end simulations are performed to demonstrate the proposed method. The measured spectra suggest that a ~250 as pulse duration is achieved at ~940 eV in the experiment.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Stochastic Maxwell-Bloch equations for modeling amplified spontaneous emission

An approach for studying atom-radiation interaction has been developed, associating quantum operators with stochastic variables governed by discrete Heisenberg equations. This framework models general multilevel atomic systems using the paraxial approximation in both single- and multipass configurations. Simulation results for x-ray laser oscillators with parameters of interest are presented. Finally, the stochastic model is efficient to solve, as the required computational resources scale linearly with the number of emitters, and it may be applicable to various other quantum systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗