arXiv subjects

Tony F. Heinz

Publications and source records attributed to Tony F. Heinz.

At least 55 records · Page 3Linked to original sources

arXiv2017

Approaching the Intrinsic Photoluminescence Linewidth in Transition Metal Dichalcogenide Monolayers

Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find that encapsulation in hexagonal boron nitride (h-BN) sharply reduces the PL linewidth, and that passivation of the oxide substrate by an alkyl monolayer further decreases the linewidth and also minimizes the charged exciton (trion) peak. The combination of these sample preparation methods results in much reduced spatial variation in the PL emission, with a full-width-at-half-maximum as low as 1.7 meV. Analysis of the PL line shape yields a homogeneous width of 1.43$\pm$0.08 meV and inhomogeneous broadening of 1.1$\pm$0.3 meV.

cond-mat.mtrl-sci↗

arXiv2017

Local polar fluctuations in lead halide perovskite crystals

Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in both hybrid (CH$_3$NH$_3$PbBr$_3$) and all-inorganic (CsPbBr$_3$) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations show that head-to-head Cs motion coupled to Br face expansion, on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr$_3$.

cond-mat.mtrl-sci↗

arXiv2017

Coulomb engineering of the bandgap in 2D semiconductors

The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment, we are able to tune the electronic bandgap in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behavior to present an in-plane dielectric heterostructure with a spatially dependent bandgap, illustrating the feasibility of our approach for the creation of lateral junctions with nanoscale resolution. This successful demonstration of bandgap engineering based on the non-invasive modification of the Coulomb interaction should enable the design of a new class of atomically thin devices to advance the limits of size and functionality for solid-state technologies.

cond-mat.mes-hall↗

arXiv2016

Magnetic brightening and control of dark excitons in monolayer WSe2

Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2016

Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2

We report a determination of the complex in-plane dielectric function of monolayers of four transition metal dichalcogenides: MoS2, MoSe2, WS2 and WSe2, for photon energies from 1.5 - 3 eV. The results were obtained from reflection spectra using a Kramers-Kronig constrained variational analysis. From the dielectric functions, we obtain the absolute absorbance of the monolayers. We also provide a comparison of the dielectric function for the monolayers with the corresponding bulk materials.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast Manipulation of Valley Pseudospin

The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including NMR, quantum communication, and quantum computation. Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics. Valley exciton polarization has been created in the transition metal dichalcogenide (TMDC) monolayers using excitation by circularly polarized light and has been detected both optically and electrically. In addition, the existence of coherence in the valley pseudospin has been identified experimentally. The manipulation of such valley coherence has, however, remained out of reach. Here we demonstrate an all-optical control of the valley coherence by means of the pseudomagnetic field associated with the optical Stark effect. Using below-bandgap circularly polarized light, we experimentally rotate the valley exciton pseudospin in monolayer WSe2 on the femtosecond time scale. Both the direction and speed of the rotation can be optically manipulated by tuning the dynamic phase of excitons in opposite valleys. This study completes the generation-manipulation-detection paradigm for valley pseudospin, enabling the platform of excitons in 2D materials for the control of this novel degree of freedom in solids.

cond-mat.mes-hall↗

arXiv2016

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS$_2$ and MoSe$_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS$_2$ through phonon emission at all temperatures.

cond-mat.mtrl-sci↗

arXiv2015

Photonic and plasmonic guiding modes in graphene-silicon photonic crystals

We report systematic studies of plasmonic and photonic guiding modes in large-area chemical-vapor-deposition-grown graphene on nanostructured silicon substrates. Light interaction in graphene with substrate photonic crystals can be classified into four distinct regimes depending on the photonic crystal lattice constant and the various modal wavelengths (i.e. plasmonic, photonic and free-space). By optimizing the design of the substrate, these resonant modes can magnify the graphene absorption in infrared wavelength, for efficient modulators, filters, sensors and photodetectors on silicon photonic platforms.

physics.optics↗

arXiv2014

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe2

We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $\mp$ 0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is modified by the magnetic field, reflecting the creation of field-induced valley polarization. At high doping levels, the Zeeman shift of the charged exciton increases to $\mp$ 0.18 meV/T. This enhancement is attributed to many-body effects on the binding energy of the charged excitons.

cond-mat.mes-hall↗

arXiv2014

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2

We have experimentally determined the energies of the ground and first four excited excitonic states of the fundamental optical transition in monolayer WS2, a model system for the growing class of atomically thin two-dimensional semiconductor crystals. From the spectra, we establish a large exciton binding energy of 0.32 eV and a pronounced deviation from the usual hydrogenic Rydberg series of energy levels of the excitonic states. We explain both of these results using a microscopic theory in which the non-local nature of the effective dielectric screening modifies the functional form of the Coulomb interaction. These strong but unconventional electron-hole interactions are expected to be ubiquitous in atomically thin materials.

cond-mat.mtrl-sci↗

arXiv2014

Atomically thin p-n junctions with van der Waals heterointerfaces

Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this region. With the advent of atomically thin van der Waals (vdW) materials and their heterostructures, we are now able to realize a p-n junction at the ultimate quantum limit. In particular, vdW junctions composed of p- and n-type semiconductors each just one unit cell thick are predicted to exhibit completely different charge transport characteristics than bulk junctions. Here we report the electronic and optoelectronic characterization of atomically thin p-n heterojunctions fabricated using vdW assembly of transition metal dichalcogenides (TMDCs). Across the p-n interface, we observe gate-tuneable diode-like current rectification and photovoltaic response. We find that the tunnelling-assisted interlayer recombination of the majority carriers is responsible for the tunability of the electronic and optoelectronic processes. Sandwiching an atomic p-n junction between graphene layers enhances collection of the photoexcited carriers. The atomically scaled vdW p-n heterostructures presented here constitute the ultimate quantum limit for functional electronic and optoelectronic components.

cond-mat.mes-hall↗

arXiv2013

Tuning many-body interactions in graphene: The effects of doping on excitons and carrier lifetimes

The optical properties of graphene are strongly affected by electron-electron (e-e) and electron-hole (e-h) interactions. Here we tune these many-body interactions through varying the density of free charge carriers. Measurements from the infrared to the ultraviolet reveal significant changes in the optical conductivity of graphene for both electron and hole doping. The shift, broadening, and modification in shape of the saddle-point exciton resonance reflect strong screening of the many-body interactions by the carriers, as well as changes in quasi-particle lifetimes. Ab initio calculations by the GW Bethe-Salpeter equation (GW-BSE), which take into account modification of both the repulsive e-e and the attractive e-h interactions, provide excellent agreement with experiment. Understanding the optical properties and high-energy carrier dynamics of graphene over a wide range of doping is crucial for both fundamental graphene physics and for emerging applications of graphene in photonics.

cond-mat.mtrl-sci↗

arXiv2013

Competing thermodynamic and dynamic factors select molecular assemblies on a gold surface

Controlling the self-assembly of surface-adsorbed molecules into nanostructures requires understanding physical mechanisms that act across multiple length and time scales. By combining scanning tunneling microscopy with hierarchical ab initio and statistical mechanical modeling of 1,4-substituted benzenediamine (BDA) molecules adsorbed on a gold (111) surface, we demonstrate that apparently simple nanostructures are selected by a subtle competition of thermodynamics and dynamics. Of the collection of possible BDA nanostructures mechanically stabilized by hydrogen bonding, the interplay of intermolecular forces, surface modulation, and assembly dynamics select at low temperature a particular subset: low free energy oriented linear chains of monomers, and high free energy branched chains.

cond-mat.mes-hall↗

arXiv2013

Controlling the Spontaneous Emission Rate of Monolayer MoS$_2$ in a Photonic Crystal Nanocavity

We report on controlling the spontaneous emission (SE) rate of a molybdenum disulfide (MoS$_2$) monolayer coupled with a planar photonic crystal (PPC) nanocavity. Spatially resolved photoluminescence (PL) mapping shows strong variations of emission when the MoS$_2$ monolayer is on the PPC cavity, on the PPC lattice, on the air gap, and on the unpatterned gallium phosphide substrate. Polarization dependences of the cavity-coupled MoS$_2$ emission show a more than 5 times stronger extracted PL intensity than the un-coupled emission, which indicates an underlying cavity mode Purcell enhancement of MoS$_2$ SE rate exceeding a factor of 70.

physics.optics↗

arXiv2013

Tunable electronic correlation effects in nanotube-light interactions

Electronic many-body correlation effects in one-dimensional (1D) systems such as carbon nanotubes have been predicted to modify strongly the nature of photoexcited states. Here we directly probe this effect using broadband elastic light scattering from individual suspended carbon nanotubes under electrostatic gating conditions. We observe significant shifts in optical transition energies, as well as line broadening, as the carrier density is increased. The results demonstrate the differing role of screening of many-body electronic interactions on the macroscopic and microscopic length scales, a feature inherent to quasi-1D systems. Our findings further demonstrate the possibility of electrical tuning of optical transitions and provide a basis for understanding of various optical phenomena in carbon nanotubes and other quasi-1D systems in the presence of charge carrier doping.

cond-mat.mes-hall↗

arXiv2013

Intrinsic lineshape of the Raman 2D-mode in freestanding graphene monolayers

We report a comprehensive study of the two-phonon inter-valley (2D) Raman mode in graphene monolayers, motivated by recent reports of asymmetric 2D-mode lineshapes in freestanding graphene. For photon energies in the range $1.53 \rm eV - 2.71 \rm eV$, the 2D-mode Raman response of freestanding samples appears as bimodal, in stark contrast with the Lorentzian approximation that is commonly used for supported monolayers. The transition between the freestanding and supported cases is mimicked by electrostatically doping freestanding graphene at carrier densities above $2\times 10^{11} \rm cm^{-2}$. This result quantitatively demonstrates that low levels of charging can obscure the intrinsically bimodal 2D-mode lineshape of monolayer graphene, which can be utilized as a signature of a quasi-neutral sample. In pristine freestanding graphene, we observe a broadening of the 2D-mode feature with decreasing photon energy that cannot be rationalized using a simple one-dimensional model based on resonant \textit{inner} and \textit{outer} processes. This indicates that phonon wavevectors away from the high-symmetry lines of the Brillouin zone must contribute to the 2D-mode, so that a full two-dimensional calculation is required to properly describe multiphonon-resonant Raman processes.

cond-mat.mes-hall↗

arXiv2013

Tunable Infrared Phonon Anomalies in Trilayer Graphene

Trilayer graphene in both ABA (Bernal) and ABC (rhombohedral) stacking sequences is shown to exhibit intense infrared absorption from in-plane optical phonons. The feature, lying at ~1580 cm-1, changes strongly with electrostatic gating. For ABC-stacked graphene trilayers, we observed a large enhancement in phonon absorption amplitude, as well as softening of the phonon mode, as the Fermi level is tuned away from charge neutrality. A similar, but substantially weaker effect is seen in samples with the more common ABA stacking order. The strong infrared response of the optical phonons and the pronounced variation with electrostatic gating and stacking-order reflect the interactions of the phonons and electronic excitations in the two systems. The key experimental findings can be reproduced within a simplified charged-phonon model that considers the influence of charging through Pauli blocking of the electronic transitions.

cond-mat.mes-hall↗

arXiv2013

Grains and grain boundaries in highly crystalline monolayer molybdenum disulfide

Recent progress in large-area synthesis of monolayer molybdenum disulfide, a new two-dimensional direct-bandgap semiconductor, is paving the way for applications in atomically thin electronics. Little is known, however, about the microstructure of this material. Here we have refined chemical vapor deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulfide up to 120 um in size with optical and electrical properties comparable or superior to exfoliated samples. Using transmission electron microscopy, we correlate lattice orientation, edge morphology, and crystallinity with island shape to demonstrate that triangular islands are single crystals. The crystals merge to form faceted tilt and mirror boundaries that are stitched together by lines of 8- and 4- membered rings. Density functional theory reveals localized mid-gap states arising from these 8-4 defects. We find that mirror boundaries cause strong photoluminescence quenching while tilt boundaries cause strong enhancement. In contrast, the boundaries only slightly increase the measured in-plane electrical conductivity.

cond-mat.mtrl-sci↗