We investigate the response of excitons in two-dimensional semiconductors subjected to controlled non-uniform strain fields. In our approach to non-uniform strain-engineering, a WS$_2$ monolayer is suspended over a triangular hole. Large ($>2\;\%$), strongly non-uniform ($>0.28\;\%/μm$), and in-situ tunable strain is induced in the monolayer by pressurizing it with inert gas. We observe peak shifts and spectral shape changes in the photoluminescence spectra of strained WS$_2$. We interpret these changes as a signature of increased free electron density and resulting conversion of neutral excitons to trions in the region of high strain. Our result establishes non-uniform strain engineering as a novel and useful experimental `knob' for tuning optoelectronic properties of 2D semiconductors.
Non-linear Zeeman splitting of neutral excitons is observed in composition engineered In(x)Ga(1-x)As self-assembled quantum dots and its microscopic origin is explained. Eight-band k.p simulations, performed using realistic dot parameters extracted from cross-sectional scanning tunneling microscopy, reveal that a quadratic contribution to the Zeeman energy originates from a spin dependent mixing of heavy and light hole orbital states in the dot. The dilute In-composition (x<0.35) and large lateral size (40-50 nm) of the quantum dots investigated is shown to strongly enhance the non-linear exci…
We show how the excitonic features of biaxial MoS2 flakes are very sensitive to biaxial strain. We find a lower bound for the gauge factors of the A exciton and B exciton of (-41 +- 2) meV/% and (-45 +- 2) meV/% respectively, which are larger than those found for single-layer MoS2. Interestingly, the interlayer exciton feature also shifts upon biaxial strain but with a gauge factor that is systematically larger than that found for the A exciton, (-48 +- 4) meV/%. We attribute this larger gauge factor for the interlayer exciton to the strain tunable van der Waals interaction due to the Poisson …
Monolayers of transition metal dichalcogenides (TMDs) have a remarkable excitonic landscape with deeply bound bright and dark exciton states. Their properties are strongly affected by lattice distortions that can be created in a controlled way via strain. Here, we perform a joint theory-experiment study investigating exciton diffusion in strained tungsten disulfide (WS$_2$) monolayers. We reveal a non-trivial and non-monotonic influence of strain. Lattice deformations give rise to different energy shifts for bright and dark excitons changing the excitonic landscape, the efficiency of intervall…
Transition metal dichalcogenides (TMDs) are layered materials that have a semiconducting phase with many advantageous optoelectronic properties, including tightly bound excitons and spin-valley locking. In Tungsten-based TMDs, spin and momentum forbidden transitions give rise to dark excitons that typically are optically inaccessible but represent the lowest excitonic states of the system. Dark excitons can deeply affect transport, dynamics and coherence of bright excitons, hampering device performance. Therefore, it is crucial to create conditions in which these excitonic states can be visual…
We investigate the formation of waveguides for Rydberg excitons in Cu$_\text{2}$O from cylindrical stressors as alternatives to optical traps. We show that the achievable potential depths can easily reach the meV and the trap frequencies the GHz regimes. For Rydberg excitons, we find that it is sufficient to consider only the shift of the band gap, whereas the excitonic binding energies remain almost unchanged.
The trend towards ever smaller high-performance devices in modern technology requires novel materials with new functionalities. The recent emergence of atomically thin two-dimensional (2D) materials has opened up possibilities for the design of ultra-thin and flexible nanoelectronic devices. As truly 2D materials, they exhibit an optimal surface-to-volume ratio, which results in an extremely high sensitivity to external changes. This makes these materials optimal candidates for sensing applications. Here, we exploit the remarkably diverse exciton landscape in monolayer transition metal dichalc…
We propose a simple, yet highly efficient and robust device for producing valley polarized current in graphene. The device comprises of two distinct components; a region of uniform uniaxial strain, adjacent to an out-of-plane magnetic barrier configuration formed by patterned ferromagnetic gates. We show that when the amount of strain, magnetic field strength, and Fermi level are properly tuned, the output current can be made to consist of only a single valley contribution. Perfect valley filtering is achievable within experimentally accessible parameters.
We study the effects of strain on the properties and dynamics of Wannier excitons in monolayer (phosphorene) and few-layer black phosphorus (BP), a promising two-dimensional material for optoelectronic applications due to its high mobility, mechanical strength and strain-tuneable direct band gap. We compare the results to the case of molybdenum disulphide (MoS$_2$) monolayers. We find that the so-called funnel effect, i.e. the possibility of controlling exciton motion by means of inhomogeneous strains, is much stronger in few-layer BP than in MoS$_2$ monolayers and, crucially, is of opposite s…
Strain can tune desirable electronic behavior in graphene, but there has been limited progress in controlling strain in graphene devices. In this paper, we study the mechanical response of graphene on substrates patterned with arrays of mesoscale pyramids. Using atomic force microscopy, we demonstrate that the morphology of graphene can be controlled from conformal to suspended depending on the arrangement of pyramids and the aspect ratio of the array. Non-uniform strains in graphene suspended across pyramids are revealed by Raman spectroscopy and supported by atomistic modeling, which also in…
The exciton states in strained (In,Ga)As nanorings embedded in a GaAs matrix are computed. The strain distribution is extracted from the continuum mechanical model, and the exact diagonalization approach is employed to compute the exciton states. Weak oscillations of the ground exciton state energy with the magnetic field normal to the ring are an expression of the excitonic Aharonov-Bohm effect. Those oscillations arise from anticrossings between the ground and the second exciton state and can be enhanced by increasing the ring width. Simultaneously, the oscillator strength for exciton recomb…
We study the effect of elastic anisotropic biaxial strain on the light emitted by neutral excitons confined in different kinds of semiconductor quantum dots (QDs). We find that the light polarization rotates by up to 80 degree and the excitonic fine structure splitting varies by several tens of $μ$eVs as the strain is varied. By means of a continuum model we mainly ascribe the observed effects to substantial changes of the hole wave function. These results show that strain-fields of a few permill magnitude are suffcient to dramatically modify the electronic structure of QDs.
Photoluminescence (PL) from excitons serves as a powerful tool to characterize the optoelectronic property and band structure of semiconductors, especially for atomically thin 2D transition metal chalcogenide (TMD) materials. However, PL quenches quickly when the thickness of TMD material increases from monolayer to few-layers, due to the change from direct to indirect band transition. Here we show that PL can be recovered by engineering multilayer heterostructures, with the band transition reserved to be direct type. We report emission from layer engineered interlayer excitons from these mult…
Neutral excitons in strained axially symmetric In(Ga)As/GaAs quantum dots with ringlike shape are investigated. Similar to experimental self-assembled quantum rings, the analyzed quantum dots have volcano-like shapes. The continuum mechanical model is employed to determine the strain distribution, and the single-band envelope function approach is adopted to compute the electron states. The hole states are determined by the axially symmetric multiband Luttinger-Kohn Hamiltonian, and the exciton states are obtained from an exact diagonalization. We found that the presence of the inner layer cove…
Reduced electron screening in two-dimension plays a fundamental role in determining exciton properties, which dictates optoelectronic and photonic device performances. Considering the explicit electron-hole interaction within the $GW-$Bethe-Salpeter formalism, we first study the excitonic properties of pristine phosphorene and investigate the effects of strain and impurity coverage. The calculations reveal strongly bound exciton in these systems with anisotropic spatial delocalization. Further, we present a simplified hydrogenic model with anisotropic exciton mass and effective electron screen…
Motivated by recent proposals on strain-engineering of graphene electronic circuits we calculate conductivity, shot-noise and the density of states in periodically deformed graphene. We provide the solution to the Dirac-Kronig-Penney model, which describes the phase-coherent transport in clean monolayer samples with an one-dimensional modulation of the strain and the electrostatic potentials. We compare the exact results to a qualitative band-structure analysis. We find that periodic strains induce large pseudo-gaps and suppress charge transport in the direction of strain modulation. The strai…
Nanoscale Mapping of Strain-engineered Excitons in Monolayer WSe$_2$
University of Arizona（亚利桑那大学）；Wyant College of Optical Sciences, University of Arizona（亚利桑那大学怀特光学学院）；United States Naval Research Laboratory（美国海军研究实验室）；Laboratory for Physical Sciences（物理科学实验室）；National Institute for Materials Science（物质材料研究机构）
Donor spin states in silicon are a promising candidate for quantum information processing. One possible donor spin readout mechanism is the bound exciton transition that can be excited optically and creates an electrical signal when it decays. This transition has been extensively studied in bulk, but in order to scale towards localized spin readout, microfabricated structures are needed for detection. As these electrodes will inevitably cause strain in the silicon lattice, it will be crucial to understand how strain affects the exciton transitions. Here we study the phosphorous donor bound exc…
The exciton ground state in strained quantum dots similar to those fabricated in article specified in the title is shortly discussed within a relevant model Hamiltonian. Some characteristics of the light--hole exciton ground state reached in a dot under the tensile biaxial strain appear to be sensitive to the strain anisotropy breaking a purity of this state. It refers in particular to a degree of the in--plane polarization of the emission and the fine structure of the ground state.
We study the effect of a uniform pseudomagnetic field, induced by a strain in a monolayer and double layer of gapped graphene, acting on excitons. For our analysis it is crucial that the pseudomagnetic field acts on the charges of the constituent particles of the excitons, i.e., the electrons and holes, the same way in contrast to a magnetic field. Moreover, using a circularly polarized laser field, the electrons and the holes can be excited only in one valley of the honeycomb lattice of gapped graphene. This breaks the time-reversal symmetry and provides the possibility to observe the various…
Recent experiments showed that non-uniform strain can be produced by depositing graphene over pillars. We employed atomistic calculations to study the non-uniform strain and the induced pseudo-magnetic field up to 5000 Tesla in graphene on top of nano-pillars. By decreasing the distance between the nano-pillars a complex distribution for the pseudo-magnetic field can be generated. Furthermore, we performed tight-binding calculations of the local density of states (LDOS) by using the relaxed graphene configuration obtained from the atomistic calculations. We find that the quasiparticle LDOS are…
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
Polarization-dependent two-dimensional Fourier-transform spectroscopy (2DFTS) is performed on excitons in strained bulk GaAs layers probing the coherent response for differing amounts of strain. Biaxial tensile strain lifts the degeneracy of heavy-hole (HH) and light-hole (LH) valence states, leading to an observed splitting of the associated excitons at low temperature. Increasing the strain increases the magnitude of the HH/LH exciton peak splitting, induces an asymmetry in the off-diagonal coherences, increases the difference in the HH and LH exciton homogenous linewidths, and increases the…
We study theoretically effects of an anisotropic elastic strain on the exciton energy spectrum fine structure and optical selection rules in atom-thin crystals based on transition-metal dichalcogenides. The presence of strain breaks the chiral selection rules at the $\bm K$-points of the Brillouin zone and makes optical transitions linearly polarized. The orientation of the induced linear polarization is related to the main axes of the strain tensor. Elastic strain provides an additive contribution to the exciton fine structure splitting in agreement with experimental evidence obtained from un…
We investigate the effects of point charge defects on the single particle electronic structure, emission energies, fine structure splitting and oscillator strengths of excitonic transitions in strained In$_{0.6}$Ga$_{0.4}$As/GaAs and strain-free GaAs/Al$_{0.3}$Ga$_{0.7}$As quantum dots. We find that the charged defects significantly modify the single particle electronic structure and excitonic spectra in both strained and strain-free structures. However, the excitonic fine structure splitting, polarization anisotropy and polarization direction in strained quantum dots remain nearly unaffected,…
The strain induced pseudo-magnetic field in supported graphene deposited on top of a nanostructured substrate is investigated by using atomistic simulations. Step, elongated trench, one dimensional barrier, spherical bubbles, Gaussian bump and Gaussian depression are considered as support structures for graphene. From the obtained optimum configurations we found very strong induced pseudo-magnetic fields which can reach up to $\sim$ 1000\,T due to the strain-induced deformations in the supported graphene. Different magnetic confinements with controllable geometries are found by tuning the patt…
Mechanical strain is a powerful tuning knob for excitons, Coulomb-bound electron-hole complexes dominating optical properties of two-dimensional semiconductors. While the strain response of bright free excitons is broadly understood, the behavior of dark free excitons (long-lived excitations that generally do not couple to light due to spin and momentum conservation) or localized excitons related to defects remains mostly unexplored. Here, we develop a technique capable of straining pristine suspended WSe2 kept at cryogenic temperatures up to 3\% to study the strain behavior of these fragile m…
We demonstrate mechanical modulations of the exciton lifetime by using vibrational strain of a gallium arsenide (GaAs) resonator. The strain-induced modulations have anisotropic dependences on the crystal orientation, which reveals the origin of these modulations to be the piezoelectric effect. Numerical analyses based on the tunneling model clarify that the mechanical strain modulates the internal electric field and spatially separates the electrons and holes, leading to non-radiative exciton decomposition. This carrier separation also generates an optomechanical back-action force from the ph…
We develop a model of the coherent exciton spin-valley dynamics in two-dimensional transition metal dichalcogenides under elastic strain. The strain splits the exciton radiative doublet in linearly polarized states. Consequently, it induces an effective magnetic field acting on the exciton pseudospin and causes its precession. As a result, under circularly polarized excitation, the circular polarization of excitons oscillates with time, also a time-oscillating linear polarization appears. We study competition of the strain-induced effective magnetic field with the field caused by the exciton l…
In monolayer transition metal dichalcogenides, quantum emitters are associated with localized strain that can be deterministically applied to create designer nano-arrays of single photon sources. Despite an overwhelming empirical correlation with local strain, the nanoscale interplay between strain, excitons, defects and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopy of excitons in nanobubbles of localized strain in monolayer WSe2 with atomistic structural models to elucidate ho…
We investigate the transport of excitons and trions in monolayer semiconductor WS$_2$ subjected to controlled non-uniform mechanical strain. We actively control and tune the strain profiles with an AFM-based setup in which the monolayer is indented by an AFM tip. Optical spectroscopy is used to reveal the dynamics of the excited carriers. The non-uniform strain configuration locally changes the valence and conduction bands of WS$_2$, giving rise to effective forces attracting excitons and trions towards the point of maximum strain underneath the AFM tip. We observe large changes in the photolu…
Monolayers of transition metal dichalcogenides (TMDs) have recently emerged as a promising optoelectronic platform. To leverage their full potential, however, it is important to understand and engineer the properties of the different exciton species that exist in these monolayers, as well as to control their transport through the material. A promising approach relies on engineering strain landscapes in atomically thin semiconductors that excitons navigate. In WSe$_2$ monolayers, for example, localized strain has been used to control the emission wavelength of excitons, induce exciton funneling…
We study the effect of uniaxial strain on the band structure of ZrSe$_3$, a semiconducting material with a marked in-plane structural anisotropy. By using a modified 3-point bending test apparatus, thin ZrSe$_3$ flakes were subjected to uniaxial strain along different crystalline orientations monitoring the effect of strain on their optical properties through micro-reflectance spectroscopy. The obtained spectra showed excitonic features that blueshift upon uniaxial tension. This shift is strongly dependent on the direction along which the strain is being applied. When the flakes are strained a…
Strain presents a straightforward tool to tune electronic properties of atomically thin nanomaterials that are highly sensitive to lattice deformations. While the influence of strain on the electronic band structure has been intensively studied, there are only few works on its impact on optical properties of monolayer transition metal dichalcogenides (TMDs). Combining microscopic theory based on Wannier and Bloch equations with nearestneighbor tight-binding approximation, we present an analytical view on how uni- and biaxial strain influences the optical fingerprint of TMDs including their exc…
Raman scattering is a ubiquitous phenomenon in light-matter interactions which reveals a material's electronic, structural and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe2 monolayer with materials such as SiO2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons …
Magneto transmission spectroscopy was employed to study the valley Zeeman effect in large-area monolayer MoS$_{2}$ and MoSe$_{2}$. The extracted values of the valley g-factors for both A- and B-exciton were found be similar with $g_v \simeq -4.5$. The samples are expected to be strained due to the CVD growth on sapphire at high temperature ($700^\circ$C). However, the estimated strain, which is maximum at low temperature, is only $\simeq 0.2\%$. Theoretical considerations suggest that the strain is too small to significantly influence the electronic properties. This is confirmed by the measure…
