The field of topological mechanics has recently emerged due to the interest in robustly transporting various types of energy in a flaw and defect-insensitive fashion. While there have been a significant number of studies based on discovering and proposing topological materials and structures, very few have focused on tuning the resulting topological bandgaps, which is critical because the bandgap frequency is fixed once the structure has been fabricated. Here, we perform both lattice dynamical calculations and molecular dynamical simulations to investigate strain effects on the phononic topological bandgaps in two-dimensional monolayer hexagonal boron nitride. Our studies demonstrate that while the topologically protected phononic bandgaps are not closed even for severely deformed hexagonal boron nitride, and are relatively insensitive to uniaxial tension and shear strains, the position of the frequency gap can be efficiently tuned in a wide range through the application of biaxial strains. Overall, this work thus demonstrates that topological phonons are robust against the effects of mechanical strain engineering, and sheds light on the tunability of the topological bandgaps in nanomaterials.
This study investigates the programming of elastic wave propagation bandgaps in a kirigami material by intentionally sequencing its constitutive mechanical bits. Such sequencing exploits the multi-stable nature of the stretched kirigami, allowing each mechanical bit to switch between two stable equilibria with different external shapes (aka. "(0)" and "(1)" states). Therefore, by designing the sequence of (0) and (1) bits, one can fundamentally change the underlying periodicity and thus program the phononic bandgap frequencies. To this end, this study develops an algorithm to identify the uniq…
Using combination of Density Functional Theory and Monte Carlo simulation, we study the phase stability and electronic properties of two dimensional hexagonal composites of boron nitride and graphene, with a goal to uncover the role of the interface geometry formed between the two. Our study highlights that preferential creation of extended armchair interfaces may facilitate formation of solid solution of boron nitride and graphene within a certain temperature range. We further find that for band-gap engineering, armchair interfaces or patchy interfaces with mixed geometry are most suitable. E…
We present a tunable phononic crystal which undergoes a phase transition from mechanically insulating to mechanically transmissive (metallic). Specifically, in our simulations for a phononic lattice under biaxial tension ($σ_{xx} =σ_{yy}$ = 0.01 N$/$m), we find a bandgap for out-of-plane phonons in the range of 48.8 - 56.4 MHz, which we can close by increasing the degree of tension uniaxiality ($σ_{xx} / σ_{yy}$) to 1.7. To manipulate the tension distribution, we design a realistic device of finite size, where $σ_{xx} / σ_{yy}$ is tuned by applying a gate voltage to a phononic crystal made fro…
In the field of phononics, periodic patterning controls vibrations and thereby the flow of heat and sound in matter. Bandgaps arising in such phononic crystals realize low-dissipation vibrational modes and enable applications towards mechanical qubits, efficient waveguides, and state-of-the-art sensing. Here, we combine phononics and two-dimensional materials and explore the possibility of manipulating phononic crystals via applied mechanical pressure. To this end, we fabricate the thinnest possible phononic crystal from monolayer graphene and simulate its vibrational properties. We find a ban…
Phononic crystals exhibit Bragg bandgaps, frequency regions within which wave propagation is forbidden. In solid continua, bandgaps are the outcome of destructive interferences resulting from periodically alternating layers. Under certain conditions, natural frequencies emerge within these bandgaps in the form of high-amplitude localized vibrations near a structural boundary, referred to as truncation resonances. In this paper, we investigate the vibrational spectrum of finite phononic crystals which take the form of a one-dimensional rod, and explain the factors that contribute to the origina…
The light emission properties of color centers emitting in 3.3-4 eV region are investigated for hydrostatic pressures ranging up to 5GPa at liquid helium temperature. The light emission energy decreases with pressure less sensitively than the bandgap. This behavior at variance from the shift of the bandgap is typical of deep traps. Interestingly, hydrostatic pressure reveals the existence of levels that vary differently under pressure (smaller increase of the emission wavelength compared to the rest of the levels in this energy region or even decrease of it) with pressure. This discovery enric…
Group theory and density functional theory methods are combined to obtain compact and accurate $k\cdot p$ Hamiltonians that describe the bandstructures around the $K$ and $Γ$ points for the 2D material hexagonal boron arsenide (h-BAs) predicted to be an important low-bandgap material for electric, thermoelectric, and piezoelectric properties that supplements the well-studied 2D material hexagonal boron nitride. Hexagonal boron arsenide is a direct bandgap material with band extrema at the $K$ point. The bandgap becomes indirect with a conduction-band minimum at the $Γ$ point subject to a stron…
By using density functional theory, we have studied vibrational features, Raman activities, and electronic properties of ultrathin hydrogen-passivated diamond nanowires (H-DNWs). Confinement imposes the softening of transverse acoustic modes and the hardening of the low-optical modes. Higher frequencies optical modes are more influenced by the surface termination effect. Surface effect splits transverse (TO) and longitudinal (LO) optical modes with a redshift from the bulk diamond. Electronic inspection shows that the surface terminated hydrogen atoms have the main contribution to the conducti…
Using a new time-resolved cathodoluminescence system dedicated to the UV spectral range, we present a first estimate of the radiative lifetime of free excitons in hBN at room temperature. This is carried out from a single experiment giving both the absolute luminescence intensity under continuous excitation and the decay time of free excitons in the time domain. The radiative lifetime of indirect excitons in hBN is equal to 27 ns, which is much shorter than in other indirect bandgap semiconductors. This is explained by the close proximity of the electron and the hole in the exciton complex, an…
Two dimensional van der Waals crystals and their heterostructures provide an exciting alternative to bulk wide bandgap semiconductors as hosts of single photon emitters. Amongst different layered materials, bright and robust defect-based single photon emitters have been observed within hexagonal boron nitride, a layered wide-bandgap semiconductor. Despite research efforts to date, the identities of the deep defects responsible for quantum emissions in hexagonal boron nitride remain unknown. In this theoretical work, I demonstrate that the strain-induced changes in emission frequencies depend o…
Engineering the electronic bandgaps and band edge positions in carbon-substituted 2D boron nitride: a first-principles investigation
石墨烯的改性以在其电子光谱中打开一个强大的间隙对于其在场效应晶体管和光化学应用中的使用至关重要。受最近在制备石墨烯和氮化硼（BN）的均匀合金中的实验成功的启发，我们在这里考虑通过成分和构型修改来工程化C $_{2x}$ B $_{1-x}$ N $_{1-x}$合金的电子结构和带隙。我们从已经具有大带隙的BN端元开始，然后表明：（a）带隙原则上可以通过C $(x<0.25)$的适度取代降低到约2 eV;以及（b）C $_{2x}$ B $_{1-x}$ N $_{1-x}$的电子结构不仅可以通过组成$x$，而且可以通过BN基质中的C取代基所采用的构型来进一步调节。我们的分析，准确的筛选混合功能计算的基础上，提供了一个清晰的理解之间的相关性的带隙和聚集的C原子的水平：带隙减少最大时的C原子被最大限度地隔离，并增加与聚集的C原子由于形成的结合和反结合带与杂化的占据和空的缺陷状态。我们确定相对于真空的价带和导带边缘的位置，并讨论了2D C $_{2x}$ B $_{1-x}$ N $_{1-x}$合金在光催化应用中的潜在用途的影响。最后，我们评估这些合金的形成使用来自第一性原理的团簇膨胀模型的热力学限制。
Using machine learning (ML) approach, we unearthed a new III-V semiconducting material having an optimal bandgap for high efficient photovoltaics with the chemical composition of Gallium-Boron-Phosphide(GaBP$_2$, space group: Pna2$_1$). ML predictions are further validated by state of the art ab-initio density functional theory (DFT) simulations. The stoichiometric Heyd-Scuseria-Ernzerhof (HSE) bandgap of GaBP$_2$ is noted to 1.65 eV, a close ideal value (1.4-1.5 eV) to reach the theoretical Queisser-Shockley limit. The calculated electron mobility is similar to that of silicon. Unlike perovsk…
With the best overall electronic and thermal properties, single crystal diamond (SCD) is the extreme wide bandgap material that is expected to revolutionize power electronics and radio-frequency electronics in the future. However, turning SCD into useful semiconductors requires overcoming doping challenges, as conventional substitutional doping techniques, such as thermal diffusion and ion implantation, are not easily applicable to SCD. Here we report a simple and easily accessible doping strategy demonstrating that electrically activated, substitutional doping in SCD without inducing graphiti…
Stacking and Registry Effects in Layered Materials: The Case of Hexagonal Boron Nitride
采用van der Waals修正的密度泛函理论方法研究了六方氮化硼（h-BN）的层间滑移能谱.结果表明，范德华力的主要作用是将层间固定在一个固定的距离上，而静电力则决定了最佳的堆积模式和层间滑动能。一个几乎自由滑动的路径被确定，沿着该路径获得~0.6 eV的带隙调制。我们提出了一个简单的几何模型，量化层之间的注册表匹配，并捕捉波纹h-BN层间能量景观的本质。这种现象学模型的简单性为复杂的层状结构（如碳和氮化硼纳米管）的建模开辟了道路。
Hypersonic phononic bandgap structures confine acoustic vibrations whose wavelength is commensurate with that of light, and have been studied using either time- or frequency-domain optical spectroscopy. Pulsed pump-probe lasers are the preferred instruments for characterizing periodic multilayer stacks from common vacuum deposition techniques, but the detection mechanism requires the injected sound wave to maintain coherence during propagation. Beyond acoustic Bragg mirrors, frequency-domain studies using a tandem Fabry-Perot interferometer (TFPI) find dispersions of two- and three-dimensional…
Among a variety of layered materials used as building blocks in van der Waals heterostructures, hexagonal boron nitride (hBN) appears as an ideal platform for hosting optically-active defects owing to its large bandgap ($\sim 6$ eV). Here we study the optical response of a high-purity hBN crystal under green laser illumination. By means of photon correlation measurements, we identify individual defects emitting a highly photostable fluorescence under ambient conditions. A detailed analysis of the photophysical properties reveals a high quantum efficiency of the radiative transition, leading to…
Cubic boron arsenide (BAs) is attracting greater attention due to the recent experimental demonstration of ultrahigh thermal conductivity \k{appa} above 1000 W/mK. However, its bandgap has not been settled and a simple yet effective method to probe its crystal quality is missing. Furthermore, traditional \k{appa} measurement methods are destructive and time consuming, thus they cannot meet the urgent demand for fast screening of high \k{appa} materials. After we experimentally established 1.82 eV as the indirect bandgap of BAs and observed room-temperature band-edge photoluminescence, we devel…
The relative orientation of successive sheets, i.e. the stacking sequence, in layered two-dimensional materials is central to the electronic, thermal, and mechanical properties of the material. Often different stacking sequences have comparable cohesive energy, leading to alternative stable crystal structures. Here we theoretically and experimentally explore different stacking sequences in the van der Waals bonded material hexagonal boron nitride (h-BN). We examine the total energy, electronic bandgap, and dielectric response tensor for five distinct high symmetry stacking sequences for both b…
Hexagonal boron nitride (h-BN) is an attractive van der Waals material for studying fluorescent defects due to its large bandgap. In this work, we demonstrate enhanced pink color due to neutron irradiation and perform electron paramagnetic resonance (EPR) measurements. The new point defects are tentatively assigned to doubly- occupied nitrogen vacancies with (S = 1) and a zero-field splitting (D = 1.2 GHz). These defects are associated with a broad visible optical absorption band and near infrared photoluminescence band centered at ~ 490 nm and 820 nm, respectively. The EPR signal intensities …
Quantum emitters in layered materials are promising candidates for applications in nanophotonics. Here we present a technique based on charge transfer to graphene for measuring the charge transition levels ($\rm E_t$) of fluorescent defects in a wide bandgap 2D material, and apply it to quantum emitters in hexagonal boron nitride (hBN). Our results will aid in identifying the atomic structures of quantum emitters in hBN, as well as practical applications since $\rm E_t$ determines defect charge states and plays a key role in photodynamics.
Inverse design of materials with desired properties is currently laborious and heavily relies on intuition of researchers through a trial-and-error process. The massive combinational spaces due to the constituent elements and their structural configurations are too overwhelming to be all searched even by high-throughput computations. Herein, we demonstrated a novel regressional generative adversarial network (RGAN) for inverse design of representative two-dimensional materials, graphene and boron-nitride (BN) hybrids. A significant novelty of the proposed RGAN is that it combines the supervise…
Cubic boron nitride (cBN) is an ultra-wide bandgap, super-hard material with potential for extreme-temperature and -pressure applications. A proof-of-principle p-n junction using cBN was demonstrated almost three decades ago. However, to date, there remain two unresolved challenges that prevent its practical use in technologies: (i) it is difficult to produce high-quality cBN films and (ii) it is difficult to controllably n- and p-dope its matrix. In this theoretical work, we study the reasons for doping-limitations, which is an acute issue in realizing cBN-based electronics. In particular, we…
Atom-layered hexagonal boron nitride (hBN), with excellent stability, flat surface and large bandgap, has been reported to be the best 2D insulator to open up the great possibilities for exciting potential applications in electronics, optoelectronics and photovoltaics. The ability to grow high-quality large single crystals of hBN is at the heart for those applications, but the size of single-crystal 2D BN is less than a millimetre till now. Here, we report the first epitaxial growth of a 10*10 cm2 single-crystal hBN monolayer on a low symmetry Cu(110) "vicinal surface". The growth kinetics, un…
Heat management becomes more and more critical, especially in miniaturized modern devices, so the exploration of highly thermally conductive materials with electrical insulation and favorable mechanical properties is of great importance. Here, we report that high-quality monolayer boron nitride (BN) has a thermal conductivity (\k{appa}) of 751 W/mK at room temperature. Though smaller than that of graphene, this value is larger than that of cubic boron nitride (cBN) and only second to those of diamond and lately discovered cubic boron arsenide (BAs). Monolayer BN has the second largest \k{appa}…
Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using sub-bandgap optical excitation. Quantum emission from defects is observed at room temperature and characterized in detail. Our results advance the use of hBN in quantum nanophotonics technologies and en…
Since the rising of graphene, boron nitride monolayers have been deeply studied due to their structural similarity with the former. A hexagonal graphene-like boron-carbon-nitrogen (h-BCN) monolayer was synthesized recently using bis-BN cyclohexane (B2N2C2H12) as a precursor molecule. Herein, we investigated the electronic and structural properties of this novel BCN material, in the presence of single-atom (boron, carbon, or nitrogen) vacancies, by employing density functional theory calculations. The stability of these vacancy-endowed structures is verified from cohesion energy calculations. R…
Interlayer electron transport through a graphene / hexagonal boron-nitride (h-BN) / graphene heterostructure is strongly affected by the misorientation angle $θ$ of the h-BN with respect to the graphene layers with different physical mechanisms governing the transport in different regimes of angle, Fermi level, and bias. The different mechanisms and their resulting signatures in resistance and current are analyzed using two different models, a tight-binding, non-equilibrium Green function model and an effective continuum model, and the qualitative features resulting from the two different mode…
