107 research outputs found
Observation of Hybrid Soliton Vortex-Ring Structures in Bose-Einstein Condensates
We present the experimental discovery of compound structures comprising
solitons and vortex rings in Bose-Einstein condensates (BECs). We examine both
their creation via soliton-vortex collisions and their subsequent development,
which is largely governed by the dynamics of interacting vortex rings. A
theoretical model in three-dimensional (3D) cylindrical symmetry is also
presented.Comment: 5 pages, 4 figures; submitted to PR
Non-Additive Interactions Unlock Small-Particle Mobility in Binary Colloidal Monolayers
We examine the organization and dynamics of binary colloidal monolayers
composed of micron-scale silica particles interspersed with smaller-diameter
silica particles that serve as minority component impurities. These binary
monolayers are prepared at the surface of ionic liquid droplets over a range of
size ratios () and are studied with low-dose minimally
perturbative scanning electron microscopy (SEM). The high resolution of SEM
imaging provides direct tracking of all particle coordinates over time,
enabling a complete description of the microscopic state. In these bidisperse
size mixtures, particle interactions are non-additive because interfacial
pinning to the droplet surface causes the equators of differently sized
particles to lie in separate planes. By varying the size ratio we control the
extent of non-additivity in order to achieve phase behavior inaccessible to
strictly 2D systems. Across the range of size ratios we tune the system from a
mobile small-particle phase (), to an interstitial solid
(). These distinct
phase regimes are classified through measurements of hexagonal ordering of the
large-particle host lattice and the lattice's capacity for small-particle
transport. Altogether, we explain these structural and dynamic trends by
considering the combined influence of interparticle interactions and the
colloidal packing geometry. Our measurements are reproduced in molecular
dynamics simulations of 2D non-additive hard disks, suggesting an efficient
method for describing confined systems with reduced dimensionality
representations.Comment: 12 pages, 7 figures, also see supplementary ancillary fil
Photoinduced phase separation in the lead halides is a polaronic effect
We present a perspective on recent observations of the photoinduced phase
separation of halides in multi-component lead-halide perovskites. The
spontaneous phase separation of an initial homogeneous solid solution under
steady-state illumination conditions is found experimentally to be reversible,
stochastic, weakly dependent on morphology, yet strongly dependent on
composition and thermodynamic state. Regions enriched in a specific halide
species that form upon phase separation are self-limiting in size, pinned to
specific compositions, and grow in number in proportion to the steady-state
carrier concentration until saturation. These empirical observations of
robustness rule out explanations based on specific defect structures and point
to the local modulation of an existing miscibility phase transition in the
presence of excess charge carriers. A model for rationalizing existing
observations based on the coupling between composition, strain and charge
density fluctuations through the formation of polarons is reviewed.Comment: Light edits for clarit
Charging-driven coarsening and melting of a colloidal nanoparticle monolayer at an ionic liquid-vacuum interface
We induce and investigate the coarsening and melting dynamics of an initially
static nanoparticle colloidal monolayer at an ionic liquid-vacuum interface,
driven by a focused, scanning electron beam. Coarsening occurs through grain
interface migration and larger-scale motions such as grain rotations, often
facilitated by sliding dislocations. The progressive decrease in area fraction
that drives melting of the monolayer is explained using an electrowetting model
whereby particles at the interface are solvated once their accumulating charge
recruits sufficient counterions to subsume the particle. Subject to stochastic
particle removal from the monolayer, melting is recapitulated in simulations
with a Lennard-Jones potential. This new driving mechanism for colloidal
systems, whose dynamical timescales we show can be controlled with the
accelerating voltage, opens the possibility to manipulate particle interactions
dynamically without need to vary particle intrinsic properties or surface
treatments. Furthermore, the decrease in particle size availed by electron
imaging presents opportunities to observe force and time scales in a
lesser-explored regime intermediate between typical colloidal and molecular
systems.Comment: 14 pages, 6 figures, also see supplementary ancilliary fil
Cathodoluminescence-based nanoscopic thermometry in a lanthanide-doped phosphor
Crucial to analyze phenomena as varied as plasmonic hot spots and the spread
of cancer in living tissue, nanoscale thermometry is challenging: probes are
usually larger than the sample under study, and contact techniques may alter
the sample temperature itself. Many photostable nanomaterials whose
luminescence is temperature-dependent, such as lanthanide-doped phosphors, have
been shown to be good non-contact thermometric sensors when optically excited.
Using such nanomaterials, in this work we accomplished the key milestone of
enabling far-field thermometry with a spatial resolution that is not
diffraction-limited at readout.
We explore thermal effects on the cathodoluminescence of lanthanide-doped
NaYF nanoparticles. Whereas cathodoluminescence from such lanthanide-doped
nanomaterials has been previously observed, here we use quantitative features
of such emission for the first time towards an application beyond localization.
We demonstrate a thermometry scheme that is based on cathodoluminescence
lifetime changes as a function of temperature that achieves 30 mK
sensitivity in sub-m nanoparticle patches. The scheme is robust against
spurious effects related to electron beam radiation damage and optical
alignment fluctuations.
We foresee the potential of single nanoparticles, of sheets of nanoparticles,
and also of thin films of lanthanide-doped NaYF to yield temperature
information via cathodoluminescence changes when in the vicinity of a sample of
interest; the phosphor may even protect the sample from direct contact to
damaging electron beam radiation. Cathodoluminescence-based thermometry is thus
a valuable novel tool towards temperature monitoring at the nanoscale, with
broad applications including heat dissipation in miniaturized electronics and
biological diagnostics.Comment: Main text: 30 pages + 4 figures; supplementary information: 22 pages
+ 8 figure
Detecting, distinguishing, and spatiotemporally tracking photogenerated charge and heat at the nanoscale
Since dissipative processes are ubiquitous in semiconductors, characterizing
how electronic and thermal energy transduce and transport at the nanoscale is
vital for understanding and leveraging their fundamental properties. For
example, in low-dimensional transition metal dichalcogenides (TMDCs), excess
heat generation upon photoexcitation is difficult to avoid since even with
modest injected exciton densities, exciton-exciton annihilation still occurs.
Both heat and photoexcited electronic species imprint transient changes in the
optical response of a semiconductor, yet the unique signatures of each are
difficult to disentangle in typical spectra due to overlapping resonances. In
response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to
simultaneously map both heat and exciton populations in few-layer \ch{MoS2} on
relevant nanometer and picosecond length- and time scales and with 100-mK
temperature sensitivity. We discern excitonic contributions to the signal from
heat by combining observations close to and far from exciton resonances,
characterizing photoinduced dynamics for each. Our approach is general and can
be applied to any electronic material, including thermoelectrics, where heat
and electronic observables spatially interplay, and lays the groundwork for
direct and quantitative discernment of different types of coexisting energy
without recourse to complex models or underlying assumptions.Comment: 22 pages, 4 figures, SI included as ancilliary fil
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