89 research outputs found
Ultrafast Charge Transfer in Atomically Thin MoS2/WS2 Heterostructures
Van der Waals heterostructures have recently emerged as a new class of
materials, where quantum coupling between stacked atomically thin
two-dimensional (2D) layers, including graphene, hexagonal-boron nitride, and
transition metal dichalcogenides (MX2), give rise to fascinating new phenomena.
MX2 heterostructures are particularly exciting for novel optoelectronic and
photovoltaic applications, because 2D MX2 monolayers can have an optical
bandgap in the near-infrared to visible spectral range and exhibit extremely
strong light-matter interactions. Theory predicts that many stacked MX2
heterostructures form type-II semiconductor heterojunctions that facilitate
efficient electron-hole separation for light detection and harvesting. Here we
report the first experimental observation of ultrafast charge transfer in
photo-excited MoS2/WS2 heterostructures using both photoluminescence mapping
and femtosecond (fs) pump-probe spectroscopy. We show that hole transfer from
the MoS2 layer to the WS2 layer takes place within 50 fs after optical
excitation, a remarkable rate for van der Waals coupled 2D layers. Such
ultrafast charge transfer in van der Waals heterostructures can enable novel 2D
devices for optoelectronics and light harvesting
Evolution of Interlayer Coupling in Twisted MoS2 Bilayers
Van der Waals (vdW) coupling is emerging as a powerful method to engineer and
tailor physical properties of atomically thin two-dimensional (2D) materials.
In graphene/graphene and graphene/boron-nitride structures it leads to
interesting physical phenomena ranging from new van Hove singularities1-4 and
Fermi velocity renormalization5, 6 to unconventional quantum Hall effects7 and
Hofstadter's butterfly pattern8-12. 2D transition metal dichalcogenides
(TMDCs), another system of predominantly vdW-coupled atomically thin layers13,
14, can also exhibit interesting but different coupling phenomena because TMDCs
can be direct or indirect bandgap semiconductors15, 16. Here, we present the
first study on the evolution of interlayer coupling with twist angles in
as-grown MoS2 bilayers. We find that an indirect bandgap emerges in bilayers
with any stacking configuration, but the bandgap size varies appreciably with
the twist angle: it shows the largest redshift for AA- and AB-stacked bilayers,
and a significantly smaller but constant redshift for all other twist angles.
The vibration frequency of the out-of-plane phonon in MoS2 shows similar twist
angle dependence. Our observations, together with ab initio calculations,
reveal that this evolution of interlayer coupling originates from the repulsive
steric effects, which leads to different interlayer separations between the two
MoS2 layers in different stacking configurations
Amplitude- and phase-resolved nano-spectral imaging of phonon polaritons in hexagonal boron nitride
Phonon polaritons are quasiparticles resulting from strong coupling of
photons with optical phonons. Excitation and control of these quasiparticles in
2D materials offer the opportunity to confine and transport light at the
nanoscale. Here, we image the phonon polariton (PhP) spectral response in thin
hexagonal boron nitride (hBN) crystals as a representative 2D material using
amplitude- and phase-resolved near-field interferometry with broadband mid-IR
synchrotron radiation. The large spectral bandwidth enables the simultaneous
measurement of both out-of-plane (780 cm-1) and in-plane (1370 cm-1) hBN phonon
modes. In contrast to the strong and dispersive in-plane mode, the out-of-plane
mode PhP response is weak. Measurements of the PhP wavelength reveal a
proportional dependence on sample thickness for thin hBN flakes, which can be
understood by a general model describing two-dimensional polariton excitation
in ultrathin materials
Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2
Strong Coulomb interactions in single-layer transition metal dichalcogenides
(TMDs) result in the emergence of strongly bound excitons, trions and
biexcitons. These excitonic complexes possess the valley degree of freedom,
which can be exploited for quantum optoelectronics. However, in contrast to the
good understanding of the exciton and trion properties, the binding energy of
the biexciton remains elusive, with theoretical calculations and experimental
studies reporting discrepant results. In this work, we resolve the conflict by
employing low-temperature photoluminescence spectroscopy to identify the
biexciton state in BN encapsulated single-layer WSe2. The biexciton state only
exists in charge neutral WSe2, which is realized through the control of
efficient electrostatic gating. In the lightly electron-doped WSe2, one free
electron binds to a biexciton and forms the trion-exciton complex. Improved
understanding of the biexciton and trion-exciton complexes paves the way for
exploiting the many-body physics in TMDs for novel optoelectronics
applications
A Unified Framework for Analyzing and Detecting Malicious Examples of DNN Models
Deep Neural Networks are well known to be vulnerable to adversarial attacks
and backdoor attacks, where minor modifications on the input can mislead the
models to give wrong results. Although defenses against adversarial attacks
have been widely studied, research on mitigating backdoor attacks is still at
an early stage. It is unknown whether there are any connections and common
characteristics between the defenses against these two attacks. In this paper,
we present a unified framework for detecting malicious examples and protecting
the inference results of Deep Learning models. This framework is based on our
observation that both adversarial examples and backdoor examples have anomalies
during the inference process, highly distinguishable from benign samples. As a
result, we repurpose and revise four existing adversarial defense methods for
detecting backdoor examples. Extensive evaluations indicate these approaches
provide reliable protection against backdoor attacks, with a higher accuracy
than detecting adversarial examples. These solutions also reveal the relations
of adversarial examples, backdoor examples and normal samples in model
sensitivity, activation space and feature space. This can enhance our
understanding about the inherent features of these two attacks, as well as the
defense opportunities
Systematic Determination of Absolute Absorption Cross-section of Individual Carbon Nanotubes
Determination of optical absorption cross-section is always among the central
importance of understanding a material. However its realization on individual
nanostructures, such as carbon nanotubes, is experimentally challenging due to
the small extinction signal using conventional transmission measurements. Here
we develop a technique based on polarization manipulation to enhance the
sensitivity of single-nanotube absorption spectroscopy by two-orders of
magnitude. We systematically determine absorption cross-section over broad
spectral range at single-tube level for more than 50 chirality-defined
single-walled nanotubes. Our data reveals chirality-dependent one-dimensional
photo-physics through the behaviours of exciton oscillator strength and
lifetime. We also establish an empirical formula to predict absorption spectrum
of any nanotube, which provides the foundation to determine quantum
efficiencies in important photoluminescence and photovoltaic processes
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