Circularly Polarized Stimulated Emission from a Chiral Cavity Based on Apparent Circular Dichroism Organic Thin-Films
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Spatio-spectral quantum state estimation of photon pairs from optical fiber using stimulated emission
Developing a quantum light source that carries more than one bit per photon is pivotal for expanding quantum information applications. Characterizing a high-dimensional multiple-degree-of-freedom source at the single-photon level is challenging due to the large parameter space as well as limited emission rates and detection efficiencies. Here, we characterize photon pairs generated in optical fiber in the transverse-mode and frequency degrees of freedom by applying stimulated emission in both degrees of freedom while detecting in one of them at a time. This method may be useful in the quantum state estimation and optimization of various photon-pair source platforms in which complicated correlations across multiple degrees of freedom may be present.
Kim, Dong Beom (ORCID:0000000346887375)↗
Stimulated Emission from Below the Bandgap in Giant Quantum Shells
Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solution-processable optical gain media, with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (~14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton–exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle while the unusual sub-bandgap gain behaviour results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Altogether, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.
Absorption↗
Polariton spectra under the collective coupling regime. II. 2D non-linear spectra
In our previous work [Mondal et al., J. Chem. Phys. 162, 014114 (2025)], we developed several efficient computational approaches to simulate exciton–polariton dynamics described by the Holstein–Tavis–Cummings (HTC) Hamiltonian under the collective coupling regime. Here, we incorporated these strategies into the previously developed Lindblad-partially linearized density matrix ($\mathscr{L}$-PLDM) approach for simulating 2D electronic spectroscopy (2DES) of exciton–polariton under the collective coupling regime. In particular, we apply the efficient quantum dynamics propagation scheme developed in Paper I to both the forward and the backward propagations in the PLDM and develop an efficient importance sampling scheme and graphics processing unit vectorization scheme that allow us to reduce the computational costs from $\mathscr{O}$($\mathscr{K}$ 2 )$\mathscr{O}$(T 3 ) to $\mathscr{O}$($\mathscr{K}$)$\mathscr{O}$(T 0 ) for the 2DES simulation, where $\mathscr{K}$ is the number of states and T is the number of time steps of propagation. As a result, we further simulated the 2DES for an HTC Hamiltonian under the collective coupling regime and analyzed the signal from both rephasing and non-rephasing contributions of the ground state bleaching, excited state emission, and stimulated emission pathways.
2D non-linear spectra↗
Bound Exciton Complexes in Near-Infrared Emitting Quantum Shells
Near-infrared (NIR) light sources based on colloidal semiconductor nanocrystals (NCs) represent a scalable, low-cost alternative to epitaxial semiconductor platforms. However, their performance remains hindered by rapid Auger recombination, a problem that is particularly pronounced in narrow-bandgap materials. Here, we report on CdS/HgS/CdS and CdS/HgCdSe/ ZnS quantum shells (QSs), a class of spherical quantum wells specifically engineered for a suppression of nonradiative Auger processes. Fabricated QSs exhibit tunable NIR emission with photoluminescence quantum yields reaching ∼60% below 1000 nm and up to 30% near 1300 nm. Optical gain and stimulated emission were observed in CdS/HgS/CdS QSs. In contrast, CdS/HgCdSe/ZnS QSs displayed a photoinduced absorption in lieu of optical gain despite demonstrating a comparatively stronger Auger suppression. Transient absorption spectroscopy revealed that this phenomenon arises from the formation of bound multiexciton complexes that induce long-lived sub-bandgap multiexciton states. The observation of such bound excitonic clusters at room temperature offers a pathway toward nonlinear NIR photonic phenomena, including biexciton−exciton cascade emission, optical modulation, and singleexciton gain.
Auger recombination↗
Superradiant Neutrino Lasers from Radioactive Condensates
Superradiance emerges from collective spontaneous emission in optically pumped gases, and is characterized by photon emission enhancements of up to $\frac{1}{4}$𝑁 2 in an 𝑁 atom system. The gain mechanism derives from correlations developed within the decay medium rather than from stimulated emission as in lasing, so an analog of this process should be possible for fermionic final states. We introduce here the concept of superradiant neutrino emission from a radioactive Bose Einstein condensate, which can form the basis for a superradiant neutrino laser. A plausible experimental realization based on a condensate of electron-capture isotope 83 Rb could exhibit effective radioactive decay rates accelerated from 86.2 days to minutes in viably sized rubidium condensates of 10 6 atoms.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Laser-stimulated photodetachment of electrons from the negatively charged dielectric substrates
The photon-stimulated emission of bulk electrons has been extensively studied for various types of materials, while the photodetachment of surplus surface electrons has not been fully explored. The photodetachment barrier energy is commonly defined by the surface electron affinity of material, which is typically less than the work function and more pronounced for non-conducting substrates and in environments with a continuous flux of electrons to the surface, such as in gas discharge plasmas. Herein, it is experimentally shown that the photodetachment yield of surplus electrons created by plasma-induced charging of non-conductive surfaces of dielectric materials depends on the initial surface charge density and do not correlate with the tabulated affinity values of these materials under gas discharge charging conditions. In cocnclusion, this result obtained using laser-stimulated photodetachment for fused silica, boron nitride, and alumina, is critically important for the understanding of charging and discharging dynamics, secondary electron emission, and photo emission effects affecting plasma–wall interactions relevant to surface and capacitively coupled discharges, dusty plasmas, electrostatic probe diagnostics, and applications for plasma processing of materials, plasma propulsion, and gas breakdown.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Rapid RASER MRI
Conventional Magnetic Resonance Imaging (MRI) relies on high-power Radio-Frequency (RF) pulses to excite nuclear spins and in turn generate NMR signals. These pulses require large high-power RF-amplifiers and cause heat deposition in the tissue, which must be minimized for safety, presenting a growing problem when moving toward ever-higher field MRI. An alternative to RF-pulse excitation is self-excitation of nuclear spins using Radiofrequency Amplification by Stimulated Emission of Radiation (RASER), where the nuclear spins undergo spontaneous transition, without RF excitation, from an over-populated state to a ground state. Here, the feasibility of recording rapid proton RASER MRI images of pyrazine at low concentration (120 mM) with large matrix (128x128 pixels) in as little as 78 ms is demonstrated at 500 MHz (11.7 T). We also recorded a time-series of images using a single bolus hyperpolarized pyrazine highlighting the feasibility of dynamic tracking. Here, the demonstrated approach allows recording MRI scans without transmit-receive electronics of the MRI scanner, which is highly desirable for portable MRI as well as the emerging field of hyperpolarized MRI using, e.g., HP protons, 129 Xe gas or HP 13 C labeled biomolecules as molecular tracers and imaging agents.
MRI↗
Polariton Control of Molecular Charge Transfer in Perylene Diimide Semiconductors
We report the modulation of molecular charge transfer in a bay-substituted perylene diimide derivative embedded in a planar distributed Bragg reflector microcavity. Angle-resolved reflectance spectra confirm the formation of upper and lower polaritons with clear Rabi splitting, indicating strong coupling between the cavity mode and molecular excitons. Using broadband transient absorption spectroscopy, we compare the ultrafast dynamics of cavity and non-cavity films. While excited-state absorption and stimulated emission pathways remain largely unchanged, kinetic modeling reveals a moderate increase in the charge transfer rate and yield under strong coupling. This enhancement is attributed to a reduction in the effective driving force via the formation of the lower polariton, placing the system deeper into the Marcus inverted regime. Our results demonstrate a promising non-chemical method leveraging cavity quantum electrodynamics to modulate charge separation processes in molecular semiconductors.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Signatures of Antisymmetric Vibrations in the Ultrafast Dynamics of Quadrupolar Dyes
Antisymmetric molecular vibrations are central to ultrafast, nonadiabatic photophysical and photochemical processes such as conical intersection dynamics, Herzberg–Teller couplings and, potentially, singlet fission. Direct spectroscopic identification of such vibrations is, however, challenging, since they are typically Raman inactive and affect optical transitions only weakly. Here, we report experimental signatures of vibronic couplings to a high-frequency antisymmetric vibration in the excited state dynamics of a quasi-quadrupolar molecule by ultrafast two-dimensional electronic spectroscopy (2DES). The early time, sub-50 fs 2DES maps reveal an asymmetric peak pattern with characteristic low-energy cross-peaks. We show that these peaks arise from stimulated emission transitions from an anharmonic, double-minimum excited state potential energy surface formed by vibronic coupling to a high-frequency antisymmetric mode. Simulations based on a phenomenological essential state model support the results. Our findings offer a new approach for identifying antisymmetric vibrations in ultrafast 2DES and track excited state wavepacket motion before relaxation washes out the spectra.
36 MATERIALS SCIENCE↗
Nonlinear reversal of photoexcitation on the attosecond time scale improves ultrafast X-ray diffraction images
The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.
Ulmer, Anatoli [Universität Hamburg (Germany)] (OR↗
Quantum-Enhanced Dark-Matter Sensing with Large Photon Number Fock States in a High-Q SRF Cavity
Wave-like dark matter candidates such as axions or dark photons in the microwave frequency range can be probed using resonant superconducting cavities. We demonstrate a quantum-enhanced sensing approach based on a multimode, high-Q superconducting RF (SRF) cavity, where a large Fock state is prepared in the storage mode via sideband transitions mediated by a transmon ancilla and a measurement-based feedforward protocol, achieving high-fidelity Fock states [1]. The prepared |n⟩ state induces stimulated emission from the dark-matter field, providing an (n + 1) enhancement in transition probability and proportional boost in signal rate [2]. A secondary cavity mode functions as an in-situ reference to calibrate noise. We present the control sequence, noise-referencing strategy, and projected sensitivity improvements for axion and dark-photon detection. This multimode architecture combines large Fock state preparation with noise calibration, offering a practical path to increased scan rate in cavity-based dark-matter searches.
Kim, Taeyoon↗
MOD-Amp System Design Spring: Spring 2026 – Georgetown University, SYSM–5620
High-energy lasers (HELs) play an important role in both national defense and scientific research. In defense applications, HELs are used for target detection, tracking, and engagement. In research environments, they support studies of extreme physical conditions relevant to fusion energy and plasma science. These systems depend on the amplification of light through stimulated emission of radiation, allowing optical energy to be increased to the levels required for operation. This amplification occurs when light passes through an energized gain medium that receives energy from an external optical or electrical source. To achieve the desired output, laser systems often use multiple amplification stages, including high-gain preamplifiers and lower-gain power or booster amplifiers. At Lawrence Livermore National Laboratory (LLNL) and other national laboratories, many large-aperture laser amplifier systems are aging and rely on system-specific hardware, obsolete technologies, and incomplete documentation. These legacy systems create challenges for maintenance, supportability, and long-term operation. Their lack of standardization also increases the difficulty of sustaining reliable performance over time. As this infrastructure continues to age, the likelihood of unplanned downtime grows, which can negatively affect both national security missions and scientific research programs that depend on dependable HEL capabilities. The purpose of this document is to demonstrate the application of systems engineering fundamentals and design thinking through the development of a laser amplifier case study. The proposed system concept is intended as an academic exercise and not as a finalized engineering design. As a result, the development presented in this document is incomplete and may contain technical assumptions or errors that would require further investigation before any real-world implementation.
42 ENGINEERING↗
Multiplet lines in seeded stimulated Mn 𝐾𝛼 1 x-ray emission
We report the successful resolution of the multiplet structure of 𝐾𝛼 1 x-ray emission in manganese (Mn) complexes through seeded stimulated x-ray emission spectroscopy (seeded S-XES). Using a femtosecond pump pulse above the Mn 𝐾 edge to generate simultaneous 1𝑠 core holes, and a second-color tunable seed pulse to initiate the stimulated emission process, we were able to enhance individual lines within the 𝐾𝛼 1 emission. This approach allows to resolve the fine multiplet features that are obscured by lifetime broadening in conventional (spontaneous) Mn 𝐾𝛼 XES. The work builds on our previous observation that S-XES from Mn(II) and Mn(VII) complexes pumped at high intensities can exhibit stimulated emission without sacrificing the chemical sensitivity to oxidation states. Furthermore, this technique opens the door to controlled high-resolution electronic structure spectroscopy in transition-metal complexes beyond the core-hole lifetime, with potential applications in catalysis, inorganic chemistry, and materials science.
Chemical Physics & Physical Chemistry↗
Manipulating Excitonic Quantum Droplets in Two-Dimensional CdSe Nanoplatelets via Thickness and Core/Shell Morphology
Recently, photoexcitation of high-density 4 or 5 monolayer (ML) thick CdSe nanoplatelet films at temperatures below ~200K was observed to produce pump-intensitydependent, superlinear, progressively red-shifted light output due to amplified spontaneous emission (ASE) from polyexcitonic species, distinct from biexcitonic ASE. These polyexcitonic species comprise Coulombically bound multiexciton states, termed “quantum droplets”, that form when multiexciton binding energy exceeds thermal energy fluctuations. In this work, we investigate thinner samples as well as core/shell nanoplatelet films and find that the 3 ML sample supports quantum droplet ASE up to higher temperatures than the 4 or 5 ML whereas core/shell structures suppress this form of ASE even at very low sample temperatures despite observable biexcitonic ASE, suggesting that the reduced or repulsive Coulomb binding energy of multiple excitons suppresses quantum droplets. These findings help to add understanding of routes to harness quantum droplet optical nonlinearities.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Ligand‐Induced Crystallization Control in MAPbBr 3 Hybrid Perovskites for High Quality Nanostructured Films
AbstractControlling the formation of hybrid perovskite thin films is crucial in obtaining high‐performance optoelectronic devices, since factors like morphology and film thickness have a profound impact on a film's functionality. For light‐emitting applications grain sizes in the sub‐micrometer‐range have previously shown enhanced brightness. It is therefore crucial to develop simple, yet reliable methods to produce such films. Here, a solution‐based synthesis protocol for the on‐substrate formation of MAPbBr3 (MA = methylammonium) nanostructures by adding the bifunctional rac‐3‐aminobutyric acid to the precursor solution is reported. This synthesis route improves key optical properties such as photoluminescence quantum yields and life times of excited states by inducing a controlled slow‐down of the film formation and suppressing agglomeration effects. In situ spectroscopy reveals a delayed and slowed down crystallization process, which achieves synthesis of perovskite structures with much reduced defect densities. Further, aggregation can be controlled by the amount of amino acid added and adjusting the synthesis protocol allows to produce cubic crystallites with targeted size from nanometer to micrometer scales. The nanocrystalline MAPbBr3 samples show enhanced amplified spontaneous emission (ASE) intensities, reduced ASE thresholds and purer ASE signals, compared to pristine films, even under intense optical driving, making them promising structures for lasing applications.
36 MATERIALS SCIENCE↗
2D Semiconductor Nanosheets Supported on Colloidal Quantum Cubes
Two-dimensional (2D) colloidal nanocrystals bridge the physics of epitaxial quantum wells with the synthetic scalability of solution-processed nanomaterials, making them an attractive platform for future LEDs, lasers, and photodetectors. However, their strongly anisotropic 2D morphology complicates the formation of close-packed films required for electrically interfaced devices. Here, we address this limitation by introducing semiconductor quantum cubes (QCs) in which 2D CdSe nanosheets are conformally grown on six faces of CdS cubic scaffolds. This architecture preserves excitonic physics of quasi-2D nanosheets while leveraging the mechanical rigidity and self-assembly of nanocubes, enabling close-packed films with improved electronic coupling and electrical conductivity. By extending CdS/CdSe QCs into a CdS/CdSe/CdS core/shell/shell structure, we realize 2D quantum wells that exhibit unusual multiexciton behavior. In particular, CdS/CdSe/CdS QCs show repulsive exciton–exciton interactions, which decouple CdSe facets into quasi-independent emitters. This leads to the suppressed Auger recombination, long multiexciton lifetimes, and broadband optical gain. The demonstrated combination of unusual multiexciton photophysics and favorable film self-assembly characteristics in QCs presents opportunities for solution-processed optoelectronic devices.
perovskites↗
Optimizing HAARP Beam Pattern for Generation of Strong F‐Region Field‐Aligned Irregularities
Field-aligned irregularities (FAIs) are the signatures of plasma turbulence and convection in the mid- and high-latitude F-region ionosphere, and also provide coherent backscatter targets for HF radars. To serve irregularity generation and characterization studies, we conducted experiments at the High-frequency Active Auroral Research Program (HAARP) in August 2023 with the goal of identifying the optimal HAARP beam pattern for reliable generation of intense FAIs over a large geographic region. The HAARP beam patterns we tested were the commonly-used narrow beam, also known as L0, as well as the wider L1 and L2 “twisted” beam patterns. The size and intensity of the FAI region generated by each HAARP beam pattern was quantified using the Kodiak Island Super Dual Auroral Radar Network (SuperDARN) radar. Stimulated electromagnetic emissions (SEE) from heater wave-FAI scattering were also recorded using a receiver located near HAARP. The L1 beam pattern was found to produce the strongest SuperDARN backscatter over the largest region. Although the heater frequency was intended to be tuned a few hundred kHz below the F-region critical frequency (foF2) during each experiment, difficulty in estimating foF2 during the campaign likely resulted in HAARP heating at significantly different frequency ranges around foF2 during each experiment. Although this additional free parameter complicated data analysis for this study, the SuperDARN and SEE measurements have led to further inquiry into the role heater frequency plays in the artificial generation of FAIs.
58 GEOSCIENCES↗