arXiv subjects

Cherie R. Kagan

Publications and source records attributed to Cherie R. Kagan.

11 recordsLinked to original sources

arXiv2026

Quantum Dot Colloidosomes as Triggerable Microlasers

Quantum dot (QD) supraparticle lasers are promising platforms for microscale light sources and photonic labeling, yet their optical properties are set during assembly. Here we introduce QD colloidosomes, liquid-core/solid-shell supraparticles that combine whispering-gallery-mode optical feedback with stimulus-triggered structural collapse. Intact QD colloidosomes show cavity-defined lasing with fluence thresholds of ~2.8 mJ/cm2 and linewidths of 2.2-3.7 nm, demonstrating efficient light trapping without a solid core. We identify shell continuity as a critical determinant for whispering-gallery feedback and lasing by exploring a morphological continuum of suprastructures comprising solid supraparticles, colloidosomes, and microporous hollow shells. Intact colloidosomes support narrow cavity modes, whereas porous shells remain broadband even at high pump fluence. We show that colloidosomes can be driven to rupture and release payload through well-defined pathways, including meniscus-driven capillary failure, uniform heating, and localized near-infrared activation, thereby reconfiguring their optical response from cavity-defined lasing to broadband emission. These results establish QD colloidosomes as reconfigurable microlasers that couple optical-state switching and triggered release within a single self-assembled platform.

physics.optics↗

arXiv2026

Cavity-Mediated Radiative Energy Transfer Enables Stable, Low-Threshold Lasing in Hybrid Quantum Dot-Nanoplatelet Supraparticles

Colloidal semiconductor nanocrystals are promising building blocks for optoelectronics due to their solution processability, spectral tunability, and ability to self-assemble into complex architectures. However, their use in lasing application remains limited by high working thresholds, rapid nonradiative losses from Auger recombination, and sensitivity to environmental conditions. Here, we report hybrid microscale supraparticles composed of core/shell CdSe/ZnS quantum dots (QDs) and CdSe/CdxZn1-xS nanoplatelets (NPLs), which overcome these limitations through efficient, cavity-mediated energy funneling and coupling. Broadband absorbing QDs rapidly transfer excitation to narrow emitting NPLs, enabling stable whispering gallery mode lasing with a low threshold of 0.35 mJ/cm2. These supraparticles retain optical performance after prolonged exposure to air, water, and continuous irradiation, offering practical advantages for optoelectronic devices and advanced pigment technologies. Ultimately, our approach provides a versatile, programmable platform for optical amplification and tunable emission control within colloidal photonic architectures. Keywords

cond-mat.mtrl-sci↗

arXiv2025

Robotic Monitoring of Colorimetric Leaf Sensors for Precision Agriculture

Common remote sensing modalities (RGB, multispectral, hyperspectral imaging or LiDAR) are often used to indirectly measure crop health and do not directly capture plant stress indicators. Commercially available direct leaf sensors are bulky, powered electronics that are expensive and interfere with crop growth. In contrast, low-cost, passive and bio-degradable leaf sensors offer an opportunity to advance real-time monitoring as they directly interface with the crop surface while not interfering with crop growth. To this end, we co-design a sensor-detector system, where the sensor is a passive colorimetric leaf sensor that directly measures crop health in a precision agriculture setting, and the detector autonomously obtains optical signals from these leaf sensors. The detector comprises a low size weight and power (SWaP) mobile ground robot with an onboard monocular RGB camera and object detector to localize each leaf sensor, as well as a hyperspectral camera with a motorized mirror and halogen light to acquire hyperspectral images. The sensor's crop health-dependent optical signals can be extracted from the hyperspectral images. The proof-of-concept system is demonstrated in row-crop environments both indoors and outdoors where it is able to autonomously navigate, locate and obtain a hyperspectral image of all leaf sensors present, and acquire interpretable spectral resonance with 80 $\%$ accuracy within a required retrieval distance from the sensor.

cs.RO↗

arXiv2025

Hydrazine-Free Precursor for Solution-Processed All-Inorganic Se and Se1-xTex Photovoltaics

Selenium (Se) has reemerged as a promising absorber material for indoor and tandem photovoltaics (PVs), and its alloys with Te (Se1-xTex) offer a widely tunable bandgap. Solution processing of this materials system offers a route to low-cost fabrication. However, solution processing of Se has, thus far, only used hydrazine, which is an extremely hazardous solvent. In this work, we prepare and isolate propylammonium poly-Se and poly-Se-Te precursors from a safer thiol-amine solvent system. We formulate molecular inks by dissolving the precursor n,n-dimethylformamide (DMF) with a monoethanolamine (EA) additive and process high-quality Se and Se1-xTex films with bandgaps ranging from 1.20 eV to 1.86 eV. We fabricate PVs from these films using TiO2 and MoO3 charge transport layers (CTLs) to achieve power conversion efficiencies as high as 2.73% for Se and 2.33% for Se0.7Te0.3 under solar simulation. Se devices show excellent stability with no degradation after 1 month in air, enabled by the excellent stability of Se and the use of inorganic CTLs. This work represents an important step towards low-cost solution-phase processing of Se and Se1-xTex alloys for PVs and photodetectors with low toxicity and high bandgap tunability.

cond-mat.mtrl-sci↗

arXiv2025

Room-temperature quantum emission from $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects in ZnS:Cu colloidal nanocrystals

We report room-temperature observations of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ quantum emitters in individual ZnS:Cu nanocrystals (NCs). Using time-gated imaging, we isolate the distinct, $\sim$3-$μ$s-long, red photoluminescence (PL) emission of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects, enabling their precise identification and statistical characterization. The emitters exhibit distinct blinking and photon antibunching, consistent with individual NCs containing two to four $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects. The quantum emitters' PL spectra show a pronounced blue shift compared to NC dispersions, likely due to photochemical and charging effects. Emission polarization measurements of quantum emitters are consistent with a $σ$-character optical dipole transition and the symmetry of the $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defect. These observations motivate further investigation of $\mathrm{Cu_{Zn}}$-$\mathrm{V_{S}}$ defects in ZnS NCs for use in quantum technologies.

cond-mat.mes-hall↗

arXiv2024

Crystallization of Binary Nanocrystal Superlattices and the Relevance of Short-Range Attraction

The synthesis of binary nanocrystal superlattices (BNSLs) enables the targeted integration of orthogonal physical properties, like photoluminescence and magnetism, into a single superstructure, unlocking a vast design space for multifunctional materials. Yet, the formation mechanism of BNSLs remains poorly understood, restricting the use of simulation to predict the structure and properties of the superlattices. Here, we use a combination of in situ scattering and molecular simulation to elucidate the self-assembly of two common BNSLs through emulsion templating. Our self-assembly experiments reveal that no intermediate structures precede the formation of the final binary phases, indicating that their formation proceeds through classical nucleation. Using simulations, we find that, despite the formation of AlB2 and NaZn13 typically being attributed to entropy, their self-assembly is most consistent with the nanocrystals possessing short-range interparticle attraction, which we find can dramatically accelerate nucleation kinetics in BNSLs. We also find homogenous, classical nucleation in simulation, corroborating our experiments. These results establish a robust correspondence between experiment and theory, paving the way towards a priori prediction of BNSLs.

cond-mat.mtrl-sci↗

arXiv2023

Nanodiamond emulsions for enhanced quantum sensing and click-chemistry conjugation

Nanodiamonds containing nitrogen-vacancy (NV) centers can serve as colloidal quantum sensors of local fields in biological and chemical environments. However, nanodiamond surfaces are challenging to modify without degrading their colloidal stability or the NV center's optical and spin properties. Here, we report a simple and general method to coat nanodiamonds with a thin emulsion layer that preserves their quantum features, enhances their colloidal stability, and provides functional groups for subsequent crosslinking and click-chemistry conjugation reactions. To demonstrate this technique, we decorate the nanodiamonds with combinations of carboxyl- and azide-terminated amphiphiles that enable conjugation using two different strategies. We study the effect of the emulsion layer on the NV center's spin lifetime, and we quantify the nanodiamonds' chemical sensitivity to paramagnetic ions using $T_1$ relaxometry. This general approach to nanodiamond surface functionalization will enable advances in quantum nanomedicine and biological sensing.

cond-mat.mes-hall↗

arXiv2023

Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals

Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for bio-sensing and opto-electronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the Cu$_{Zn}$-V$_S$ complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First principles calculations confirm the thermodynamic stability and electronic structure of Cu$_{Zn}$-V$_S$. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and an anomalous plateau in the intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally-activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of Cu$_{Zn}$-V$_S$ and related complexes as quantum point defects in ZnS.

cond-mat.mtrl-sci↗

arXiv2021

Template-Assisted Self Assembly of Fluorescent Nanodiamonds for Scalable Quantum Technologies

Milled nanodiamonds containing nitrogen-vacancy (NV) centers provide an excellent platform for sensing applications as they are optically robust, have nanoscale quantum sensitivity, and form colloidal dispersions which enable bottom-up assembly techniques for device integration. However, variations in their size, shape, and surface chemistry limit the ability to position individual nanodiamonds and statistically study properties that affect their optical and quantum characteristics. Here, we present a scalable strategy to form ordered arrays of nanodiamonds using capillary-driven, template-assisted self assembly. This method enables the precise spatial arrangement of isolated nanodiamonds with diameters below 50 nm across millimeter-scale areas. Measurements of over 200 assembled nanodiamonds yield a statistical understanding of their structural, optical, and quantum properties. The NV centers' spin and charge properties are uncorrelated with nanodiamond size, but rather are consistent with heterogeneity in their nanoscale environment. This flexible assembly method, together with improved understanding of the material, will enable the integration of nanodiamonds into future quantum photonic and electronic devices.

cond-mat.mes-hall↗

arXiv2021

Photophysics of Two-Dimensional Semiconducting Organic-Inorganic Metal-Halide Perovskites

2D organic-inorganic hybrid perovskites (2DHPs) consist of alternating anionic metal-halide and cationic organic layers. They have widely tunable structural and optical properties. We review the role of the organic cation in defining the structural and optical properties of 2DHPs through example lead iodide 2DHPs. Even though excitons reside in the metal halide layers, the organic and inorganic frameworks cannot be separated-they must be considered as a single unit to fully understand the photophysics of 2DHPs. We correlate cation-induced distortion and disorder in the inorganic lattice with the resulting optical properties. We also discuss the role of the cation in creating and altering the discrete excitonic structure that appears at cryogenic temperatures in some 2DHPs, including the cation-dependent presence of hot exciton photoluminescence. We conclude our review with an outlook for 2DHPs, highlighting existing gaps in fundamental knowledge as well as potential future applications.

cond-mat.mtrl-sci↗

arXiv2020

Tailoring Hot Exciton Dynamics in 2D Hybrid Perovskites through Cation Modification

We report a family of two-dimensional hybrid perovskites (2DHPs) based on phenethylammonium lead iodide ((PEA)$_2$PbI$_4$) that show complex structure in their low-temperature excitonic absorption and photoluminescence (PL) spectra as well as hot exciton PL. We replace the 2-position (ortho) H on the phenyl group of the PEA cation with F, Cl, or Br to systematically increase the cation's cross-sectional area and mass and study changes in the excitonic structure. These single atom substitutions substantially change the observable number of and spacing between discrete resonances in the excitonic absorption and PL spectra and drastically increase the amount of hot exciton PL that violates Kasha's rule by over an order of magnitude. To fit the progressively larger cations, the inorganic framework distorts and is strained, reducing the Pb-I-Pb bond angles and increasing the 2DHP band gap. Correlation between the 2DHP structure and steady-state and time-resolved spectra suggests the complex structure of resonances arises from one or two manifolds of states, depending on the 2DHP Pb-I-Pb bond angle (as)symmetry, and the resonances within a manifold are regularly spaced with an energy separation that decreases as the mass of the cation increases. The uniform separation between resonances and the dynamics that show excitons can only relax to the next-lowest state are consistent with a vibronic progression caused by a vibrational mode on the cation. These results demonstrate that simple changes to the structure of the cation can be used to tailor the properties and dynamics of the confined excitons without directly modifying the inorganic framework.

physics.app-ph↗