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Semiconducting single-walled carbon nanotubes (SWCNT) containing sp3-type defects are a promising class of optoelectronic materials, demonstrating single photon emission and long-lived spins. The defect introduces new optical transitions due to both symmetry breaking induced band splitting and introduction of in-gap electronic states. We investigate sulfur-oxide containing compounds as a new class of optically active dopants on (6,5) SWCNT. The SWCNT is exposed to sodium dodecyl sulfate with the resulting compound displaying a red-shifted and bright photoluminescence peak that is characteristic of sp3 doping. Density functional theory calculations are then performed on the adsorbed compounds that may arise (S, SO, SO2 and SO3). These calculations indicate that the two smallest molecules strongly bind to the SWCNT with binding energies of ~ 1.5-1.7 eV and 0.56 eV for S and SO, respectively. Moreover, these adsorbates introduce in-gap electronic states into the bandstructure of the tube consistent with the measured red-shift of (0.1-0.3) eV. Our study suggests that sulfur-based compounds are promising new dopants for (6,5) SWCNT with tunable electronic properties., Comment: 6 pages, 4 figures, 1 SI pdf

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.

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 Schr\"odinger 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., Comment: 24 pages, 5 figures

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.

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, $g^{(2)}(\tau)$, shows a hallmark dip to zero at $\tau=0$. 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.

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 N\'eel 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.

Two-dimensional magnetic van der Waals (vdW) materials can show a variety of topological nontrivial spin textures, such as Bloch- or N\'eel-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$_2$. N\'eel-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 N\'eel-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., Comment: 16 pages, 5 figures

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.

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.

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., Comment: 24 pages, 4 figures

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, $G^{(2)}(\tau)$, as a function of time delay $\tau$ 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., Comment: 5 pages, 3 figures

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., Comment: 38 pages, report of the first workshop on Quantum Sensing for High Energy Physics, held at Argonne National Laboratory, December 12-14, 2017

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., Comment: 12 pages, 10 figures

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., Comment: Revised version (30 pages, 11 figures) accepted for publication in Phys. Rev. Lett. including Supplementary materials