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result(s) for
"Shi, Zhiwen"
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Spontaneous broken-symmetry insulator and metals in tetralayer rhombohedral graphene
2024
Interactions among charge carriers in graphene can lead to the spontaneous breaking of multiple degeneracies. When increasing the number of graphene layers following rhombohedral stacking, the dominant role of Coulomb interactions becomes pronounced due to the significant reduction in kinetic energy. In this study, we employ phonon–polariton-assisted near-field infrared imaging to determine the stacking orders of tetralayer graphene devices. Through quantum transport measurements, we observe a range of spontaneous broken-symmetry states and their transitions, which can be finely tuned by carrier density
n
and electric displacement field
D
. Specifically, we observe a layer-antiferromagnetic insulator at
n
=
D
= 0 with a gap of approximately 15 meV. Increasing
D
allows for a continuous phase transition from a layer-antiferromagnetic insulator to a layer-polarized insulator. By simultaneously tuning
n
and
D
, we observe isospin-polarized metals, including spin–valley-polarized and spin-polarized metals. These transitions are associated with changes in the Fermi surface topology and are consistent with the Stoner criteria. Our findings highlight the efficient fabrication of specially stacked multilayer graphene devices and demonstrate that crystalline multilayer graphene is an ideal platform for investigating a wide range of broken symmetries driven by Coulomb interactions.
Stacking graphene in the rhombohedral order to the tetralayer yields stronger Coulomb interactions, which results in insulating and metallic states with spontaneous symmetry breaking in spin, valley and layer degrees of freedom.
Journal Article
Graphene nanoribbons grown in hBN stacks for high-performance electronics
2024
Van der Waals encapsulation of two-dimensional materials in hexagonal boron nitride (hBN) stacks is a promising way to create ultrahigh-performance electronic devices
1
–
4
. However, contemporary approaches for achieving van der Waals encapsulation, which involve artificial layer stacking using mechanical transfer techniques, are difficult to control, prone to contamination and unscalable. Here we report the transfer-free direct growth of high-quality graphene nanoribbons (GNRs) in hBN stacks. The as-grown embedded GNRs exhibit highly desirable features being ultralong (up to 0.25 mm), ultranarrow (<5 nm) and homochiral with zigzag edges. Our atomistic simulations show that the mechanism underlying the embedded growth involves ultralow GNR friction when sliding between AA′-stacked hBN layers. Using the grown structures, we demonstrate the transfer-free fabrication of embedded GNR field-effect devices that exhibit excellent performance at room temperature with mobilities of up to 4,600 cm
2
V
–1
s
–1
and on–off ratios of up to 10
6
. This paves the way for the bottom-up fabrication of high-performance electronic devices based on embedded layered materials.
A strategy for the transfer-free direct growth of ultralong, high-quality graphene nanoribbons, which have desirable electronic properties, between layers of a boron nitride insulator is reported.
Journal Article
Atomically precise photothermal nanomachines
2024
Interfacing molecular machines to inorganic nanoparticles can, in principle, lead to hybrid nanomachines with extended functions. Here we demonstrate a ligand engineering approach to develop atomically precise hybrid nanomachines by interfacing gold nanoclusters with tetraphenylethylene molecular rotors. When gold nanoclusters are irradiated with near-infrared light, the rotation of surface-decorated tetraphenylethylene moieties actively dissipates the absorbed energy to sustain the photothermal nanomachine with an intact structure and steady efficiency. Solid-state nuclear magnetic resonance and femtosecond transient absorption spectroscopy reveal that the photogenerated hot electrons are rapidly cooled down within picoseconds via electron–phonon coupling in the nanomachine. We find that the nanomachine remains structurally and functionally intact in mammalian cells and in vivo. A single dose of near-infrared irradiation can effectively ablate tumours without recurrence in tumour-bearing mice, which shows promise in the development of nanomachine-based theranostics.
Gold nanoclusters show promise as photothermal materials, but are often thermally unstable. Here ligand engineering is used to integrate molecular rotors with gold nanoclusters to dissipate thermal energy and improve photothermal therapy performance.
Journal Article
Genomic and molecular landscape of homologous recombination deficiency across multiple cancer types
2023
Homologous recombination deficiency (HRD) causes faulty double-strand break repair and is a prevalent cause of tumorigenesis. However, the incidence of HRD and its clinical significance in pan-cancer patients remain unknown. Using computational analysis of Single-nucleotide polymorphism array data from 10,619 cancer patients, we demonstrate that HRD frequently occurs across multiple cancer types. Analysis of the pan-cancer cohort revealed that HRD is not only a biomarker for ovarian cancer and triple-negative breast cancer, but also has clinical prognostic value in numerous cancer types, including adrenocortical cancer and thymoma. We discovered that homologous recombination–related genes have a high mutation or deletion frequency. Pathway analysis shows HRD is positively correlated with the DNA damage response and the immune-related signaling pathways. Single cell RNA sequencing of tumor-infiltrating lymphocytes reveals a significantly higher proportion of exhausted T cells in HRD patients, indicating pre-existing immunity. Finally, HRD could be utilized to predict pan-cancer patients’ responses to Programmed cell death protein 1 immunotherapy. In summary, our work establishes a comprehensive map of HRD in pan-cancer. The findings have significant implications for expanding the scope of Poly ADP-ribose polymerase inhibitor therapy and, possibly, immunotherapy.
Journal Article
Epitaxial growth of single-domain graphene on hexagonal boron nitride
by
Zhang, Guangyu
,
Taniguchi, Takashi
,
Zhang, Yuanbo
in
639/301/119/995
,
639/301/357/918
,
639/301/930/1032
2013
The epitaxial growth of large-area single-domain graphene on hexagonal boron nitride by plasma-assisted deposition is now reported. New sets of Dirac points are produced as a result of a trigonal superlattice potential, while Dirac fermion physics near the original Dirac point remain unperturbed. This growth approach could enable band engineering in graphene through epitaxy on different substrates.
Hexagonal boron nitride (h-BN) has recently emerged as an excellent substrate for graphene nanodevices, owing to its atomically flat surface and its potential to engineer graphene’s electronic structure
1
,
2
. Thus far, graphene/h-BN heterostructures have been obtained only through a transfer process
1
, which introduces structural uncertainties due to the random stacking between graphene and h-BN substrate
2
,
3
. Here we report the epitaxial growth of single-domain graphene on h-BN by a plasma-assisted deposition method. Large-area graphene single crystals were successfully grown for the first time on h-BN with a fixed stacking orientation. A two-dimensional (2D) superlattice of trigonal moiré pattern was observed on graphene by atomic force microscopy. Extra sets of Dirac points are produced as a result of the trigonal superlattice potential and the quantum Hall effect is observed with the 2D-superlattice-related feature developed in the fan diagram of longitudinal and Hall resistance, and the Dirac fermion physics near the original Dirac point is unperturbed. The macroscopic epitaxial graphene is in principle limited only by the size of the h-BN substrate and our synthesis method is potentially applicable on other flat surfaces. Our growth approach could thus open new ways of graphene band engineering through epitaxy on different substrates.
Journal Article
Observation of an intrinsic bandgap and Landau level renormalization in graphene/boron-nitride heterostructures
2014
Van der Waals heterostructures formed by assembling different two-dimensional atomic crystals into stacks can lead to many new phenomena and device functionalities. In particular, graphene/boron-nitride heterostructures have emerged as a very promising system for band engineering of graphene. However, the intrinsic value and origin of the bandgap in such heterostructures remain unresolved. Here we report the observation of an intrinsic bandgap in epitaxial graphene/boron-nitride heterostructures with zero crystallographic alignment angle. Magneto-optical spectroscopy provides a direct probe of the Landau level transitions in this system and reveals a bandgap of ~38 meV (440 K). Moreover, the Landau level transitions are characterized by effective Fermi velocities with a critical dependence on specific transitions and magnetic field. These findings highlight the important role of many-body interactions in determining the fundamental properties of graphene heterostructures.
The unusual electronic properties of graphene can be modified by placing it on a boron-nitride substrate with a small crystallographic alignment angle. Chen
et al.
now reveal that such heterostructures grown by epitaxy have a large bandgap, useful for applications using magneto-optical spectroscopy.
Journal Article
Catalyst-Free Growth of Nanographene Films on Various Substrates
by
Lianchang Zhang Zhiwen Shi Yi Wang Rong Yang Dongxia Shi Guangyu Zhang
in
Atomic/Molecular Structure and Spectra
,
Atoms & subatomic particles
,
Biomedicine
2011
We have developed a new method to grow uniform graphene films directly on various substrates, such as insulators, semiconductors, and even metals, without using any catalyst. The growth was carried out using a remote plasma enhancement chemical vapor deposition (r-PECVD) system at relatively low temperatures, enabling the deposition of graphene films up to 4-inch wafer scale. Scanning tunneling microscopy (STM) confirmed that the films are made up of nanocrystalline graphene particles of tens of nanometers in lateral size. The growth mechanism for the nanographene is analogous to that for diamond grown by PECVD methods, in spite of sp2 carbon atoms being formed in the case of graphene rather than sp3 carbon atoms as in diamond. This growth approach is simple, low-cost, and scalable, and might have potential applications in fields such as thin film resistors, gas sensors, electrode materials, and transparent conductive films.
Journal Article
Nonlinear Luttinger liquid plasmons in semiconducting single-walled carbon nanotubes
2020
Interacting electrons confined in one dimension are generally described by the Luttinger liquid formalism, where the low-energy electronic dispersion is assumed to be linear and the resulting plasmonic excitations are non-interacting. Instead, a Luttinger liquid in one-dimensional materials with nonlinear electronic bands is expected to show strong plasmon–plasmon interactions, but an experimental demonstration of this behaviour has been lacking. Here, we combine infrared nano-imaging and electronic transport to investigate the behaviour of plasmonic excitations in semiconducting single-walled carbon nanotubes with carrier density controlled by electrostatic gating. We show that both the propagation velocity and the dynamic damping of plasmons can be tuned continuously, which is well captured by the nonlinear Luttinger liquid theory. These results contrast with the gate-independent plasmons observed in metallic nanotubes, as expected for a linear Luttinger liquid. Our findings provide an experimental demonstration of one-dimensional electron dynamics beyond the conventional linear Luttinger liquid paradigm and are important for understanding excited-state properties in one dimension.
Electric-field tunable plasmonic excitations in semiconducting carbon nanotubes are shown to behave consistently with the nonlinear Luttinger liquid theory, providing a platform to study non-conventional one-dimensional electron dynamics and realize integrated nanophotonic devices.
Journal Article
Collapse of carbon nanotubes due to local high-pressure from van der Waals encapsulation
2024
Van der Waals (vdW) assembly of low-dimensional materials has proven the capability of creating structures with on-demand properties. It is predicted that the vdW encapsulation can induce a local high-pressure of a few GPa, which will strongly modify the structure and property of trapped materials. Here, we report on the structural collapse of carbon nanotubes (CNTs) induced by the vdW encapsulation. By simply covering CNTs with a hexagonal boron nitride flake, most of the CNTs (≈77%) convert from a tubular structure to a collapsed flat structure. Regardless of their original diameters, all the collapsed CNTs exhibit a uniform height of ≈0.7 nm, which is roughly the thickness of bilayer graphene. Such structural collapse is further confirmed by Raman spectroscopy, which shows a prominent broadening and blue shift in the Raman G-peak. The vdW encapsulation-induced collapse of CNTs is fully captured by molecular dynamics simulations of the local vdW pressure. Further near-field optical characterization reveals a metal-semiconductor transition in accompany with the CNT structural collapse. Our study provides not only a convenient approach to generate local high-pressure for fundamental research, but also a collapsed-CNT semiconductor for nanoelectronic applications.
vdW assembly of low-dimensional materials has proven the capability of creating structures with on-demand properties. Here, the authors report on the structural collapse of CNTs in conjunction with a metal-semiconductor junction induced by the VdW encapsulation.
Journal Article
Observation of a Luttinger-liquid plasmon in metallic single-walled carbon nanotubes
by
Zeng, Bo
,
Shen, Yuen-Ron
,
Taniguchi, Takashi
in
147/136
,
639/624/400/1021
,
Applied and Technical Physics
2015
The authors report the observation of plasmons that exhibit quantized velocities in carbon nanotubes.
Surface plasmons
1
, collective oscillations of conduction electrons, hold great promise for the nanoscale integration of photonics and electronics
1
,
2
,
3
,
4
. However, nanophotonic circuits based on plasmons have been significantly hampered by the difficulty in achieving broadband plasmonic waveguides that simultaneously exhibit strong spatial confinement, a high quality factor and low dispersion. Quantum plasmons, where the quantum mechanical effects of electrons play a dominant role, such as plasmons in very small metal nanoparticles
5
,
6
and plasmons affected by tunnelling effects
7
, can lead to novel plasmonic phenomena in nanostructures. Here, we show that a Luttinger liquid
8
,
9
of one-dimensional Dirac electrons in carbon nanotubes
10
,
11
,
12
,
13
exhibits quantum plasmons that behave qualitatively differently from classical plasmon excitations. The Luttinger-liquid plasmons propagate at ‘quantized’ velocities that are independent of carrier concentration or excitation wavelength, and simultaneously exhibit extraordinary spatial confinement and high quality factor. Such Luttinger-liquid plasmons could enable novel low-loss plasmonic circuits for the subwavelength manipulation of light.
Journal Article