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Following the emergence of many novel two-dimensional (2-D) materials beyond graphene, interest has grown in exploring implications for fundamental physics and practical applications, ranging from electronics, photonics, phononics, to thermal management and energy storage. In this Colloquium, we first summarize and compare the phonon properties, such as phonon dispersion and relaxation time, of pristine 2-D materials with single layer graphene to understand the role of crystal structure and dimension on thermal conductivity. We then compare the phonon properties, contrasting idealized 2-D crystals, realistic 2-D crystals, and 3-D crystals, and synthesizing this to develop a physical picture of how the sample size of 2-D materials affects their thermal conductivity. The effects of geometry, such as number of layers, and nanoribbon width, together with the presence of defects, mechanical strain, and substrate interactions, on the thermal properties of 2-D materials are discussed. Intercalation affects both the group velocities and phonon relaxation times of layered crystals and thus tunes the thermal conductivity along both the through-plane and basal-plane directions. We conclude with a discussion of the challenges in theoretical and experimental studies of thermal transport in 2-D materials. The rich and special phonon physics in 2-D materials make them promising candidates for exploring novel phenomena such as topological phonon effects and applications such as phononic quantum devices., Comment: This article has been accepted by Reviews of Modern Physics

Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter. This is especially true for high frequency heat carrying phonons, which are intrinsic lattice vibrations experiencing many decoherence events with the environment, and are thus generally assumed to be incoherent. Two photon interference techniques, especially coherent population trapping (CPT) and electromagnetically induced transparency (EIT), have led to extremely sensitive detection, spectroscopy and metrology. Here, we propose the use of two photon interference in a three level system to sense coherent phonons. Unlike prior works which have treated phonon coupling as damping, we account for coherent phonon coupling using a full quantum-mechanical treatment. We observe strong asymmetry in absorption spectrum in CPT and negative dispersion in EIT susceptibility in the presence of coherent phonon coupling which cannot be accounted for if only pure phonon damping is considered. Our proposal has application in sensing heat carrying coherent phonons effects and understanding coherent bosonic multi-pathway interference effects in three coupled oscillator systems.

Generating and detection coherent high-frequency heat-carrying phonons has been a great topic of interest in recent years. While there have been successful attempts in generating and observing coherent phonons, rigorous techniques to characterize and detect these phonon coherence in a crystalline material have been lagging compared to what has been achieved for photons. One main challenge is a lack of detailed understanding of how detection signals for phonons can be related to coherence. The quantum theory of photoelectric detection has greatly advanced the ability to characterize photon coherence in the last century and a similar theory for phonon detection is necessary. Here, we re-examine the optical sideband fluorescence technique that has been used detect high frequency phonons in materials with optically active defects. We apply the quantum theory of photodetection to the sideband technique and propose signatures in sideband photon-counting statistics and second-order correlation measurement of sideband signals that indicates the degree of phonon coherence. Our theory can be implemented in recently performed experiments to bridge the gap of determining phonon coherence to be on par with that of photons., Comment: 3 Figures

Piezoelectricity offers precise and robust conversion between electricity and mechanical force. Here we report the first experimental evidence of piezoelectricity in a single layer of molybdenum disulfide (MoS2) crystal as a result of inversion symmetry breaking of the atomic structure, with measured piezoelectric coefficient e11 = 2.9e-10 C/m. Through the angular dependence of electro-mechanical coupling, we uniquely determined the two-dimensional (2D) crystal orientation. We observed that only MoS2 membranes with odd number of layers exhibited piezoelectricity, in sharp contrast to the conventional materials. The piezoelectricity discovered in single molecular membrane promises scaling down of nano-electro-mechanical systems (NEMS) to single atomic unit cell - the ultimate material limit.

Transition metal dichalcogenide (TMDC) monolayer has recently emerged as an important two-dimensional semiconductor with promising potentials for electronic and optoelectronic devices. Unlike semi-metallic graphene, layered TMDC has a sizable band gap. More interestingly, when thinned down to a monolayer, TMDC transforms from an indirect bandgap to a direct bandgap semiconductor, exhibiting a number of intriguing optical phenomena such as valley selective circular dichroism, doping dependent charged excitons, and strong photocurrent responses. However, the fundamental mechanism underlying such a strong light-matter interaction is still under intensive investigation. The observed optical resonance was initially considered to be band-to-band transitions. In contrast, first-principle calculations predicted a much larger quasiparticle band gap size and an optical response that is dominated by excitonic effects. Here, we report experimental evidence of the exciton dominance mechanism by discovering a series of excitonic dark states in single-layer WS2 using two-photon excitation spectroscopy. In combination with GW-BSE theory, we find the excitons are Wannier excitons in nature but possess extraordinarily large binding energy (~0.7 eV), leading to a quasiparticle band gap of 2.7 eV. These strongly bound exciton states are observed stable even at room temperature. We reveal an exciton series in significant deviation from hydrogen models, with a novel inverse energy dependence on the orbital angular momentum. These excitonic energy levels are experimentally found robust against environmental perturbations. The discovery of excitonic dark states and exceptionally large binding energy not only sheds light on the importance of many-electron effects in this two-dimensional gapped system, but also holds exciting potentials for the device application of TMDC monolayers and their heterostructures.

Heat flow control is essential for widespread applications of heating, cooling, energy conversion and utilization. Here we demonstrate the first observation of temperature-gated thermal rectification in vanadium dioxide beams, in which an environment temperature actively modulates asymmetric heat flow. In this three terminal device, there are two switchable states, which can be accessed by global heating: Rectifier state and Resistor state. In the Rectifier state, up to 28% thermal rectification is observed. In the Resistor state, the thermal rectification is significantly suppressed (below 4%). This temperature-gated rectifier can have substantial implications ranging from autonomous thermal management of micro/nanoscale devices to thermal energy conversion and storage.

Excitons in MoS2 dominate the absorption and emission properties of the two-dimensional system. Here, we study the microscopic origin of the electroluminescence from monolayer MoS2 fabricated on a heavily p-type doped silicon substrate. By comparing the photoluminescence and electroluminescence of a MoS2 diode, direct-exciton and bound-exciton related recombination processes can be identified. Auger recombination of the exciton-exciton annihilation of bound exciton emission is observed under a high electron-hole pair injection rate at room temperature. We expect the direct exciton-exciton annihilation lifetime to exceed the carrier lifetime, due to the absence of any noticeable direct exciton saturation. We believe that our method of electrical injection opens a new route to understand the microscopic nature of the exciton recombination and facilitate the control of valley and spin excitation in MoS2., Comment: 12 pages, 3 figures