arXiv subjects

Ryan A. DeCrescent

Publications and source records attributed to Ryan A. DeCrescent.

9 recordsLinked to original sources

arXiv2026

Electrochemical reactions under reverse bias create additional mobile ions that enable hole tunneling in metal halide perovskite diodes

Gradual reverse-bias breakdown in metal-halide perovskite diodes and solar cells is thought to originate from hole tunneling through steep bands in an ionic depletion region near the electron transport layer after positively charged iodine vacancies accumulate near the hole-transport layer (HTL). However, typical reported mobile ion concentrations near $1\times10^{17}$ cm$^{-3}$ are too small to quantitatively explain significant tunneling current densities and (Zener) breakdown observed near $-5$ V. Here, we show that inferred mobile ion concentrations increase by more than 100$\times$, to over $1\times10^{18}$ cm$^{-3}$, within just three minutes of reverse bias at $-6.0$ V in p-i-n perovskite diodes. We attribute the increase in mobile ion concentration to iodide oxidation and the resulting iodine vacancy creation which must be balanced by reduction reactions near the HTL. Thin and sub-optimal HTL coverage leads to direct contact between the transparent conducting electrode and perovskite and facilitates electron transfer and reduction, enabling the creation of even larger inferred mobile ion concentrations ($\sim1\times10^{19}$ cm$^{-3}$) and leading to faster degradation under reverse bias. This explains previous work that showed increased breakdown voltages and improved reverse-bias stability by implementing thick, uniform HTLs.

physics.app-ph↗

arXiv2026

Degradation Dynamics of Perovskite Solar Cells Under Fixed Reverse Current Injection

Previous studies of reverse-bias stability in perovskite solar cells have focused primarily on voltage controlled reverse-bias tests. Here we instead present an investigation of perovskite solar cell degradation under well-defined, constant reverse-current stress. We show that the choice of hole-transport layer dictates the dominant degradation pathway: cells using thick poly(triphenylamine) (PTAA) layers with better indium-doped tin oxide (ITO) coverage can tolerate high reverse bias but quickly undergo catastrophic breakdown under fixed reverse current near their one-sun maximum power-point. In contrast, cells modified with the phosphonic-acid interface layer MeO-2PACz, with poorer ITO coverage compared to PTAA, exhibit soft, gradual, and largely recoverable degradation, regardless of the shading conditions. For MeO-2PACz devices, degradation increases with both current magnitude and duration. Importantly, when normalized by injected charge (current times duration), lower currents applied over longer times cause more severe degradation than higher currents over shorter periods. Combining electrical measurements with spatially resolved photoluminescence imaging, we argue against shunt formation and instead support an ion- and charge-mediated interfacial electrochemical degradation mode.

physics.app-ph↗

arXiv2024

Gated InAs quantum dots embedded in surface acoustic wave cavities for low-noise optomechanics

Self-assembled InAs quantum dots (QDs) are promising optomechanical elements due to their excellent photonic properties and sensitivity to local strain fields. Microwave-frequency modulation of photons scattered from these efficient quantum emitters has been recently demonstrated using surface acoustic wave (SAW) cavities. However, for optimal performance, a gate structure is required to deterministically control the charge state and reduce charge noise of the QDs. Here, we integrate gated QDs and SAW cavities using molecular beam epitaxy and nanofabrication. We demonstrate that with careful design of the substrate layer structure, integration of the two systems can be accomplished while retaining the optimal performance of each subsystem. These results mark a critical step toward efficient and low-noise optomechanical systems for microwave-to-optical quantum transduction.

quant-ph↗

arXiv2023

Monolithic Polarizing Circular Dielectric Gratings on Bulk Substrates for Improved Photon Collection from InAs Quantum Dots

III-V semiconductor quantum dots (QDs) are near-ideal and versatile single-photon sources. Because of the capacity for monolithic integration with photonic structures as well as optoelectronic and optomechanical systems, they are proving useful in an increasingly broad application space. Here, we develop monolithic circular dielectric gratings on bulk substrates -- as opposed to suspended or wafer-bonded substrates -- for greatly improved photon collection from InAs quantum dots. The structures utilize a unique two-tiered distributed Bragg reflector (DBR) structure for vertical electric field confinement over a broad angular range. Opposing ``openings" in the cavities induce strongly polarized QD luminescence without harming collection efficiencies. We describe how measured enhancements depend critically on the choice of collection optics. This is important to consider when evaluating the performance of any photonic structure that concentrates farfield emission intensity. Our cavity designs are useful for integrating QDs with other quantum systems that require bulk substrates, such as surface acoustic wave phonons.

physics.optics↗

arXiv2022

Large Single-Phonon Optomechanical Coupling between Quantum Dots and Tightly Confined Surface Acoustic Waves in the Quantum Regime

Surface acoustic waves (SAWs) coupled to quantum dots (QDs), trapped atoms and ions, and point defects have been proposed as quantum transduction platforms, yet the requisite coupling rates and cavity lifetimes have not been experimentally established. Although the interaction mechanism varies, small acoustic cavities with large zero-point motion are required for high efficiencies. We experimentally establish the feasibility of this platform through electro- and opto-mechanical characterization of tightly focusing, single-mode Gaussian SAW cavities at $\sim$3.6 GHz on GaAs. We explore the performance limits of the platform by fabricating SAW cavities with mode volumes approaching 6$λ^3$ and linewidths $\leq$1 MHz. Employing strain-coupled single InAs QDs as optomechanical intermediaries, we measure single-phonon optomechanical coupling rates $g_0 \approx 2π\times 1.2$ MHz. Sideband scattering rates thus exceed intrinsic phonon loss, indicating the potential for quantum optical readout and transduction of cavity phonon states. To demonstrate the feasibility of this platform for low-noise ground-state quantum transduction, we develop a fiber-based confocal microscope in a dilution refrigerator and perform single-QD resonance fluorescence sideband spectroscopy at mK temperatures. These measurements show conversion between microwave phonons and optical photons with sub-natural linewidths.

physics.app-ph↗

arXiv2020

Ferroelastic Hysteresis in Thin Films of Methylammonium Lead Iodide

Mechanical strain can modify the structural and electronic properties of methylammonium lead iodide MAPbI3. The consequences of ferroelastic hysteresis, which involves the retention of structural memory upon cycles of deformation, in polycrystalline thin films of MAPbI3 are reported. Repeatedly bent films of MAPbI3 on flexible polyimide substrates were examined using Grazing Incidence Wide-Angle X-ray Scattering (GIWAXS) to quantitatively characterize the strain state, populations, and minimum sizes of twin domains. Approximate locations for the coercive stress and saturation on the ferroelastic stress-strain curve are identified, and domains from differently-strained twin sets in the films are found to interact with each other. The presence of specific twin domains is found to correlate to reports of the heterogeneity of strain states with defect content. Long-term stability testing reveals that domain walls are highly immobile over extended periods. Nucleation of new domain walls occurs for specific mechanical strains and correlates closely with degradation of the films. These results help to explain the behavior of ion migration, degradation rate, and photoluminescence in thin films under compressive and tensile strain.

cond-mat.mtrl-sci↗

arXiv2020

Tamm plasmons in metal/nanoporous GaN distributed Bragg reflector cavities for active and passive optoelectronics

We investigate Tamm plasmon (TP) modes in a metal/semiconductor distributed Bragg reflector (DBR) interface. A thin Ag (silver) layer with an optimized thickness (~ 55 nm from simulation) was deposited on nanoporous GaN DBRs fabricated using electrochemical etching on freestanding semipolar GaN substrates. The reflectivity spectra of the DBRs are compared before and after the Ag deposition and with that of a blanket Ag layer deposited on GaN. The results indicate presence of a TP mode at ~ 455 nm on the structure after the Ag deposition. An active medium can also be accommodated within the mode for optoelectronics and photonics. Moreover, the simulation results predict a sensitivity of the TP mode wavelength to the ambient (~ 4 nm shift when changing the ambient within the pores from air with n = 1 to isopropanol n = 1.3) , suggesting an application of the nanoporous GaN based TP structure for optical sensing.

physics.optics↗

arXiv2019

Unidirectional Luminescence from Quantum Well Metasurfaces

III-Nitride light emitting diodes (LEDs) are the backbone of ubiquitous lighting and display applications. Imparting directional emission is an essential requirement for many LED implementations. Although optical packaging, nano-patterning and surface roughening techniques can enhance LED extraction, directing the emitted light requires bulky optical components. Optical metasurfaces provide precise control over transmitted and reflected waveforms, suggesting a new route for directing light emission. However, it is difficult to adapt metasurface concepts for incoherent light emission, due to the lack of a phase-locking incident wave. In this Letter, we demonstrate metasurface-based design of InGaN/GaN quantum-well structures that generate narrow, unidirectional transmission and emission lobes at arbitrary engineered angles. We show that the directions and polarization of emission differ significantly from transmission, in agreement with an analytical Local Density of Optical States (LDOS) model. The results presented in this Letter open a new paradigm for exploiting metasurface functionality in light emitting devices.

physics.optics↗

arXiv2019

Bright magnetic dipole radiation from two-dimensional lead-halide perovskites

Light-matter interactions in semiconductor systems are uniformly treated within the electric dipole (ED) approximation, as multipolar interactions are considered "forbidden". Here, we demonstrate that this approximation inadequately describes light emission in novel two-dimensional hybrid organic-inorganic perovskite materials (2D HOIPs) --- a class of solution processable layered semiconductor with promising optoelectronic properties. Consequently, photoluminescence (PL) spectra become strongly dependent on the experimental geometry, a fact that is often overlooked, though critical for correct optical characterization of materials. Using energy-momentum and time-resolved spectroscopies, we experimentally demonstrate that low-energy sideband emission in 2D HOIPs exhibits a highly unusual, multipolar polarization and angle dependence. Using combined electromagnetic and quantum-mechanical analyses, we attribute this radiation pattern to an out-of-plane oriented magnetic dipole transition arising from the 2D character of the excited and ground state orbitals. Symmetry arguments point toward the presence of significant inversion symmetry-breaking mechanisms that are currently under great debate. These results provide a new perspective on the origins of unexpected sideband emission in HOIPs, clarify discrepancies in previous literature, and generally challenge the paradigm of ED-dominated light-matter interactions in novel optoelectronic materials.

cond-mat.mtrl-sci↗