arXiv subjects

Xuedan Ma

Publications and source records attributed to Xuedan Ma.

15 recordsLinked to original sources

arXiv2025

Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films

Colloidal perovskite quantum dots (PQDs) are an exciting platform for on-demand quantum, and classical optoelectronic and photonic devices. However, their potential success is limited by the extreme sensitivity and low stability arising from their weak intrinsic lattice bond energy and complex surface chemistry. Here we report a novel platform of buried perovskite quantum dots (b-PQDs) in a three-dimensional perovskite thin-film, fabricated using one-step, flash annealing, which overcomes surface related instabilities in colloidal perovskite dots. The b-PQDs demonstrate ultrabright and stable single-dot emission, with resolution-limited linewidths below 130 {\mu}eV, photon-antibunching (g^2(0)=0.1), no blinking, suppressed spectral diffusion, and high photon count rates of 10^4/s, consistent with unity quantum yield. The ultrasharp linewidth resolves exciton fine-structures (dark and triplet excitons) and their dynamics under a magnetic field. Additionally, b-PQDs can be electrically driven to emit single photons with 1 meV linewidth and photon-antibunching (g^2(0)=0.4). These results pave the way for on-chip, low-cost single-photon sources for next generation quantum optical communication and sensing.

physics.optics↗

arXiv2024

Sulfur and sulfur-oxide compounds as potential optically active defects on SWCNTs

Semiconducting single-walled carbon nanotubes (SWCNT) functionalized with covalent defects are a promising class of optoelectronic materials with strong, tunable photoluminescence and demonstrated single photon emission (SPE). Here, we investigate sulfur-oxide containing compounds as a new class of optically active dopants on (6,5) SWCNT. Experimentally, it has been found that when the SWCNT is exposed to sodium dithionite, the resulting compound displays a red-shifted and bright photoluminescence peak that is characteristic of doping with covalent defects. We perform density functional theory calculations on the possible adsorbed compounds that may be the source of doping (S, SO, SO2 and SO3). We predict that the two smallest molecules strongly bind to the SWCNT with binding energies of ~ 1.5-1.8 eV and 0.56 eV for S and SO, respectively, and introduce in-gap electronic states into the bandstructure of the tube consistent with the measured red-shift of (0.1-0.3) eV, consistent with measurements. In contrast, the larger compounds are found to be either unbound or weakly physisorbed with no appreciable impact on the electronic structure of the tube, indicating that they are unlikely to occur. Overall, our study suggests that sulfur-based compounds are promising new dopants for (6,5) SWCNT with tunable electronic properties.

cond-mat.mtrl-sci↗

arXiv2023

Excitation protocols for non-linear phononics in bismuth and antimony

We study the optical generation and control of coherent phonons in elemental bismuth (Bi) and antimony (Sb) using a classical equation of motion informed by first-principles calculations of the potential energy surface and the frequency-dependent macroscopic dielectric function along the zone-centered optical phonons coordinates. Using this approach, we demonstrate that phonons with the largest optomechanical couplings, also have the strongest degree of anharmonicity among the zone-centered modes, a result of the broken symmetry structural ground state of Bi and Sb. We show how this anharmonicity, explaining the light-induced phonon softening observed in experiments, prevents the application of standard phonon-amplification and annihilation protocols. We introduce a simple linearization protocol that extends the use of such protocols to the case of anharmonic phonons in broken symmetry materials, and demonstrate its efficiency at high displacement amplitudes. Our formalism and results provide a path for improving optical control in non-linear phononics.

cond-mat.mtrl-sci↗

arXiv2023

Intersubband Transitions in Lead Halide Perovskite-Based Quantum Wells for Mid-Infrared Detectors

Due to their excellent optical and electrical properties as well as versatile growth and fabrication processes, lead halide perovskites have been widely considered as promising candidates for green energy and opto-electronic related applications. Here, we investigate their potential applications at infrared wavelengths by modeling the intersubband transitions in lead halide perovskite-based quantum well systems. Both single-well and double-well structures are studied and their energy levels as well as the corresponding wavefunctions and intersubband transition energies are calculated by solving the one-dimensional Schrödinger equations. By adjusting the quantum well and barrier thicknesses, we are able to tune the intersubband transition energies to cover a broad range of infrared wavelengths. We also find that the lead-halide perovskite-based quantum wells possess high absorption coefficients, which are beneficial for their potential applications in infrared photodetectors. The widely tunable transition energies and high absorption coefficients of the perovskite-based quantum well systems, combined with their unique material and electrical properties, may enable an alternative material system for the development of infrared photodetectors.

cond-mat.mtrl-sci↗

arXiv2023

Demonstration of an AI-driven workflow for autonomous high-resolution scanning microscopy

With the continuing advances in scientific instrumentation, scanning microscopes are now able to image physical systems with up to sub-atomic-level spatial resolutions and sub-picosecond time resolutions. Commensurately, they are generating ever-increasing volumes of data, storing and analysis of which is becoming an increasingly difficult prospect. One approach to address this challenge is through self-driving experimentation techniques that can actively analyze the data being collected and use this information to make on-the-fly measurement choices, such that the data collected is sparse but representative of the sample and sufficiently informative. Here, we report the Fast Autonomous Scanning Toolkit (FAST) that combines a trained neural network, a route optimization technique, and efficient hardware control methods to enable a self-driving scanning microscopy experiment. The key features of our method are that: it does not require any prior information about the sample, it has a very low computational cost, and that it uses generic hardware controls with minimal experiment-specific wrapping. We test this toolkit in numerical experiments and a scanning dark-field x-ray microscopy experiment of a $WSe_2$ thin film, where our experiments show that a FAST scan of <25% of the sample is sufficient to produce both a high-fidelity image and a quantitative analysis of the surface distortions in the sample. We show that FAST can autonomously identify all features of interest in the sample while significantly reducing the scan time, the volume of data acquired, and dose on the sample. The FAST toolkit is easy to apply for any scanning microscopy modalities and we anticipate adoption of this technique will empower broader multi-level studies of the evolution of physical phenomena with respect to time, temperature, or other experimental parameters.

physics.app-ph↗

arXiv2022

Noisy detectors with unmatched detection efficiency thwart identification of single photon emitters via photon coincidence correlation

Single photon emitters (SPEs) are often identified with a Hanbury Brown and Twiss intensity interferometer (HBTII) consisting of a 50:50 beamsplitter and two time-correlated single photon counters. For an SPE, the cross-correlation of photon arrival time between the two detectors, $g^{(2)}(τ)$, shows a hallmark dip to zero at $τ=0$. One common heuristic for identifying SPEs is by measuring a system to have $g^{(2)}(0)<1/2$. Here in, we use stochastic methods to simulate the case of a SPE observed with non-ideal detectors and optics. We show that identification of SPEs is thwarted when the detectors have asymmetric detection efficiency, and when detector background noise is more than half the true SPE signal rate.

quant-ph↗

arXiv2022

Thermal Hysteresis Behavior of Skyrmion Lattices in the van der Waals Ferromagnet Fe3GeTe2

Understanding the physics of phase transitions in two-dimensional (2D) systems underpins the research in diverse fields including statistical mechanics, quantum systems, nanomagnetism, and soft condensed matter. However, many fundamental aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions, which are non-trivial chiral spin structures, can be considered as quasi-particles that form two-dimensional lattices. Here we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. Our quantitative analysis explains this behavior based on the energy landscape of skyrmions and demonstrates the potential to control the lattice order in 2D phase transitions.

cond-mat.mtrl-sci↗

arXiv2022

Field-Dependent Magnetic Domain Behavior in van der Waals Fe$_3$GeTe$_2$

Two-dimensional magnetic van der Waals (vdW) materials can show a variety of topological nontrivial spin textures, such as Bloch- or Néel-type stripe, skyrmion or bubble domains under certain external stimuli. It is critical to understand the magnetic domain behavior in vdW materials in order to control their size, and density in response to external stimuli such as electric and magnetic fields. Here we examine the magnetic field dependence of topologically non-trivial magnetization spin textures in vdW Fe$_3$GeTe$_2$. Néel-type stripe domains and skyrmions are formed depending on the magnetic field-cooling protocol used during in-situ Lorentz transmission electron microscopy (LTEM) experiments. Use of quantitative reconstruction of magnetic induction maps, and micromagnetic simulations, allow for understanding the LTEM results of Néel-type stripe domains as well as skyrmions. In addition, the deformation of skyrmion contrast is observed as a result of the introduction of an in-plane magnetic field. We demonstrate the stability of the stripe domains and skyrmions in response to externally applied magnetic field due to energy barrier for domain wall annihilation. Our results establish an understanding of the energy landscape that governs the behavior of the topologically non-trivial spin textures in vdW materials which can be harnessed for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2022

Rapid and facile reconstruction of time-resolved fluorescence data with exponentially modified Gaussians

Analyte response is convoluted with instrument response in time resolved fluorescence data. Decoding the desired analyte information from the measurement usually requires iterative numerical convolutions. Here in, we show that time resolved data can be completely, analytically reconstructed without numerical convolutions. Our strategy relies on a summation of exponentially modified Gaussians which encode all convolutions within easily evaluated complementary error functions. Compared to a numerical convolution strategy implemented with Python, this new method is computationally cheaper and scales less steeply with the number of temporal points in the experimental dataset.

physics.data-an↗

arXiv2021

Trapping Interlayer Excitons in van der Waals Heterostructures by Potential Arrays

Transition metal dichalcogenide heterostructures can host interlayer excitons (IXs), which consist of electrons and holes spatially separated in different layers. IXs possess permanent dipoles and have proven to offer a wealth of novel physics. We develop a discrete, random-walk model which includes annihilation and repulsion interactions among IXs. Using this model, we simulate the trapping of IXs in traps of different depths, densities, and shapes. Our results show that dipole-dipole interactions play an important role in regulating IX trapping. The effects of dipole interactions can be mitigated with small, deep traps which are realizable with atomic defects and moire potentials.

cond-mat.mtrl-sci↗

arXiv2021

Room temperature single-photon superfluorescence from a single epitaxial cuboid nano-heterostructure

Single-photon superradiance can emerge when a collection of identical emitters are spatially separated by distances much less than the wavelength of the light they emit, and is characterized by the formation of a superradiant state that spontaneously emits light with a rate that scales linearly with the number of emitters. This collective phenomena has only been demonstrated in a few nanomaterial systems, all requiring temperatures below 10K. Here, we rationally design a single colloidal nanomaterial that hosts multiple (nearly) identical emitters that are impervious to the fluctuations which typically inhibit room temperature superradiance in other systems such as molecular aggregates. Specifically, by combining molecular dynamics, atomistic electronic structure calculations, and model Hamiltonian methods, we show that the faces of a heterostructure nanocuboid mimic individual quasi-2D nanoplatelets and can serve as the robust emitters required to realize superradiant phenomena at room temperature. Leveraging layer-by-layer colloidal growth techniques to synthesize a nanocuboid, we demonstrate single-photon superfluorescence via single-particle time-resolved photoluminescence measurements at room temperature. This robust observation of both superradiant and subradiant states in single nanocuboids opens the door to ultrafast single-photon emitters and provides an avenue to entangled multi-photon states via superradiant cascades.

physics.optics↗

arXiv2020

Accelerating quantum optics experiments with statistical learning

Quantum optics experiments, involving the measurement of low-probability photon events, are known to be extremely time-consuming. We present a new methodology for accelerating such experiments using physically-motivated ansatzes together with simple statistical learning techniques such as Bayesian maximum a posteriori estimation based on few-shot data. We show that it is possible to reconstruct time-dependent data using a small number of detected photons, allowing for fast estimates in under a minute and providing a one-to-two order of magnitude speed up in data acquisition time. We test our approach using real experimental data to retrieve the second order intensity correlation function, $G^{(2)}(τ)$, as a function of time delay $τ$ between detector counts, for thermal light as well as anti-bunched light emitted by a quantum dot driven by periodic laser pulses. The proposed methodology has a wide range of applicability and has the potential to impact the scientific discovery process across a multitude of domains.

quant-ph↗

arXiv2018

Quantum Sensing for High Energy Physics

Report of the first workshop to identify approaches and techniques in the domain of quantum sensing that can be utilized by future High Energy Physics applications to further the scientific goals of High Energy Physics.

hep-ex↗

arXiv2017

Confinement Effect Emission from Infiltrated ZnO in PS-b-PMMA Nanostructures

We have characterized the growth of ZnO using sequential infiltration synthesis (SiS) on PS-b-PMMA block copolymers (BCP) of spherical and cylindrical sub-20nm morphologies and studied how the photoluminescence of these nanostructures varies per its seed layer. Investigation of these structures was done using atomic force microscopy (AFM), spectrofluorometry, Raman spectroscopy, and scanning electron microscopy (SEM). We report blue-shifted photoemission at 335 nm (3.70 eV), suggesting quantum confinement effects. This UV-photoluminescence can be translated into emitter sizes of roughly 1.5nm in radius. Furthermore, samples of ZnO prepared with an alumina seed layer showed additional defect state photoemission at 470 nm and 520 nm for spherical and cylindrical BCP morphologies, respectively. Defect photoemission was not observed in samples prepared without a seed layer. Raman and EXAFS data suggest lack of long range order between the ZnO nanostructures during early stages of infiltrated ZnO growth and therefore supports the blue shift emission is due to confinement. Our work demonstrates that ZnO nanostructures grown on PS-b-PMMA via infiltration are advantageous in uniformity and size, and exhibit unique fluorescence properties. These observations suggest that infiltrated ZnO in PS-b-PMMA nanostructures lends itself to a new regime of applications in photonics and quantum materials.

cond-mat.mtrl-sci↗

arXiv2015

Influences of Exciton Diffusion and Exciton-Exciton Annihilation on Photon Emission Statistics of Carbon Nanotubes

Pump-dependent photoluminescence imaging and 2nd order photon correlation studies have been performed on individual single-walled carbon nanotubes (SWCNTs) at room temperature that enable the extraction of both the exciton diffusion constant and the Auger recombination coefficient. A linear correlation between these is attributed to the effect of environmental disorder in setting the exciton mean free-path and capture-limited Auger recombination at this lengthscale. A suppression of photon antibunching is attributed to creation of multiple spatially non-overlapping excitons in SWCNTs whose diffusion length is shorter than the laser spot size. We conclude that complete antibunching at room temperature requires an enhancement of exciton-exciton annihilation rate that may become realizable in SWCNTs allowing for strong exciton localization.

cond-mat.mes-hall↗