We systematically study the impact of various electron-acoustic-phonon coupling mechanisms on valley physics in two-dimensional materials. In the static strain limit, we find that Dirac cone tilt and deformation potential have analogous valley Hall response since they fall into the same universality class of pseudospin structure. However, such argument fails for the coupling mechanism with position-dependent Fermi velocity. For the isotropic case, a significant valley Hall effect occurs near charge neutrality similar to the bond-length change, whereas for the anisotropic case, the geometric valley transport is suppressed, akin to the deformation potential. Gap opening mechanism by nonuniform strain is found to totally inhibit the valley Hall transport, even if the dynamics of strains are introduced. By varying gate voltage, a tunable phonon-assisted valley Hall response can be realized, which paves a way toward rich phenomena and new functionalities of valley acoustoelectronics.
Due to their possibility to encode information and realize low-energy-consumption quantum devices, control and manipulation of the valley degree of freedom have been widely studied in electronic systems. In contrast, the phononic counterpart--valley phononics--has been largely unexplored, despite the importance in both fundamental science and practical applications. In this work, we demonstrate that the control of "valleys" is also applicable for phonons in graphene by using a grain boundary. In particular, perfect valley filtering effect is observed at certain energy windows for flexural mode…
We observe a set of three replica luminescent peaks at ~21.4 meV below the dark exciton, negative and positive dark trions (or exciton-polarons) in monolayer WSe2. The replica redshift energy matches the energy of the zone-center E"-mode optical phonons. The phonon replicas exhibit parallel gate dependence and same g-factors as the dark excitonic states, but follow the valley selection rules of the bright excitonic states. While the dark states exhibit out-of-plane transition dipole and valley-independent linearly polarized emission in the in-plane directions, their phonon replicas exhibit in-…
Although single-layer transition-metal dichalcogenides with novel valley functionalities are promising candidate to realize valleytronic devices, the essential understanding of valley depolarization mechanisms is still incomplete. Based on pump-probe experiments performed for MoSe2 and WSe2 monolayers and corroborating analysis from density functional calculations, we demonstrate that coherent phonons at the K-point of the Brillouin zone can effectively mediate the valley transfer of electron carriers. In the MoSe2 monolayer case, we identify this mode as the flexural acoustic ZA(K) mode, whic…
We demonstrate significant modification of the electron-phonon energy loss rate in a many-valley semiconductor system due to lattice mismatch induced strain. We show that the thermal conductance from the electron system to the phonon bath in strained n + Si, at phonon temperatures between 200 mK and 450 mK, is more than an order of magnitude lower than that for a similar unstrained sample.
In monolayer hexagonal lattices, two inequivalent valleys appear in the Brillouin zone. With inversion symmetry breaking, we find chiral phonons with valley contrasting circular polarization and ionic magnetic moment. At valley centers, there is a three-fold rotational symmetry endowing phonons with a quantized pseudo angular momentum, which includes spin and orbital parts. From conservation of the pseudo angular momentum, crystal momentum and energy, selection rules in intervalley scattering of electrons by phonons are obtained. The chiral valley phonons are verified and the selection rules a…
We study the hybrid excitations due to the coupling between surface optical phonons of a polar insulator substrate and plasmons in the valley-spin-polarized metal phase of silicene under an exchange field. We perform the calculations within the generalized random-phase approximation where the plasmon-phonon coupling is taken into account by the long-range Fr$\ddot{\mathrm{o}}$hlich interaction. Our investigation on two hybridized plasmon branches in different spin and valley subbands shows distinct behavior compared to the uncoupled case. Interestingly, in one valley, it is found that while th…
Inversion symmetry breaking and three-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition metal dichalcogenides (TMDCs), which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, dark exciton could be long-lived but does not necessarily possess the valley degree of freedom. In this work, we report the identification of the momentum-dark, intervalley exciton in monolayer WSe2 through low-temperature magneto-photoluminescence (PL) spectra. I…
Distinct from the phononic valley pseudo-spin, the real physical spin of elastic waves adds a novel tool-kit capable of envisaging the valley-spin physics of topological valley phononic crystals from a local viewpoint. Here, we report the observation of local elastic valley spin as well as the hidden elastic spin-valley locking mechanism overlooked before. We demonstrate that the selective one-way routing of valley phonon states along the topological interface can be reversed by imposing the elastic spin meta-source at different interface locations with opposite valley-spin correspondence. We …
A direct band gap, remarkable light-matter coupling as well as strong spin-orbit and Coulomb interaction establish two-dimensional (2D) crystals of transition metal dichalcogenides (TMDs) as an emerging material class for fundamental studies as well as novel technological concepts. Valley selective optical excitation allows for optoelectronic applications based on the momentum of excitons. In addition to lattice imperfections and disorder, scattering by phonons is a significant mechanism for valley depolarization and decoherence in TMDs at elevated temperatures preventing high-temperature vall…
Two-dimensional (2D) semiconductors are promising channel materials for next-generation field-effect transistors (FETs) thanks to their unique mechanical properties and enhanced electrostatic control. However, the performance of these devices can be strongly limited by the scattering processes between carriers and phonons, usually occurring at high rates in 2D materials. Here, we use quantum transport simulations calibrated on first-principle computations to report on dissipative transport in antimonene and arsenene $n$-type FETs at the scaling limit. We show that the widely-used approximation…
This study investigates the occurrence of acoustic topological edge states in a 2D phononic elastic waveguide due to a phenomenon that is the acoustic analogue of the quantum valley Hall effect. We show that a topological transition takes place between two lattices having broken space inversion symmetry due to the application of a tunable strain field. This condition leads to the formation of gapless edge states at the domain walls, as further illustrated by the analysis of the bulk-edge correspondence and of the associated topological invariants. Although time reversal symmetry is still intac…
The topological quantum states in two-dimensional (2D) materials are fascinating subjects of research, which usually highlight electron-related systems. In this work, we present a recipe that leads to Dirac phonon states with quantized valley Berry phase in 2D hexagonal lattices by first-principles calculations. We show that candidates possessing the three-fold rotational symmetry at the corners of the hexagonal Brillouin zone host valley Dirac phonons, which are guaranteed to remain intact with respect to perturbations. We identify that such special topological features populated by Dirac pho…
We investigate the chirality of phonon modes in twisted bilayer WSe2 and demonstrate distinct chiral behavior of the $K/K^\prime$ valley phonons for twist angles close to $0^{\circ}$ and close to $60^{\circ}$. In particular, multiple chiral non-degenerate $K/K^\prime$ valley phonons are found for twist angles near $60^{\circ}$ whereas no non-degenerate chiral modes are found for twist angles close to $0^\circ$. Moreover, we discover two sets of emergent chiral valley modes that originate from an inversion symmetry breaking at the moiré scale and find similar modes in moiré patterns of strain-e…
Valley Hall effect is an appearance of the valley current in the direction transverse to the electric current. We develop the microscopic theory of the valley Hall effect in two-dimensional semiconductors where the electrons are dragged by the phonons or photons. We derive and analyze all relevant contributions to the valley current including the skew-scattering effects together with the anomalous contributions caused by the side-jumps and the anomalous velocity. The partial compensation of the anomalous contributions is studied in detail. The role of two-phonon and two-impurity scattering pro…
We present a symmetric double-sided pillared phononic crystals (PPnCs) that can emulate both quantum spin Hall effect (QSHE) and quantum valley Hall effect (QVHE) by solely imposing different geometric perturbations. Indeed, the Dirac cones can occur in the low (deep subwavelength) and high frequency regime by judiciously turning the parameters of the attached pillars and even a double Dirac cone can be achieved. We realize the valley-protected, the pseudospin-protected or the pseudospin-valley coupled edge states with the proposed platform. Besides, we show a variety of refraction phenomena (…
The valley degree of freedom and the possibility of spin-valley coupling of solid materials have attracted growing interest, and the relaxation dynamics of spin- and valley-polarized states has become an important focus of recent studies. In spin-orbit-coupled inversion-asymmetric two-dimensional materials, such as MoS_{2} it has been found that the spin randomization is characteristically faster than the time scales for inter- and intra-valley scatterings. In this study, we examined the ultrafast non-collinear spin dynamics of an electron valley in monolayer MoS_{2} by using real-time propaga…
Through a combined theoretical and experimental effort, we uncover a yet unidentified mechanism that strengthens considerably electron-phonon coupling in materials where electron accumulation leads to population of multiple valleys. Taking atomically-thin transition-metal dichalcogenides as prototypical examples, we establish that the mechanism results from a phonon-induced out-of-phase energy shift of the different valleys, which causes inter-valley charge transfer and reduces the effectiveness of electrostatic screening, thus enhancing electron-phonon interactions. The effect is physically r…
A double peak structure in the magneto-phonon resonance (MPR) spectrum of uniaxial strained graphene, under crossed electric and magnetic fields, is predicted. We focus on the $Γ$ point optical phonon modes coupled to the inter-Landau level transitions $0 \leftrightarrows \pm 1$ where MPR is expected to be more pronounced at high magnetic field. We derive the frequency shifts and the broadenings of the longitudinal (LO) and transverse (TO) optical phonon modes taking into account the effect of the strain modified electronic spectrum on the electron-phonon coupling. We show that the MPR lines a…
The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects because they possess unique spin-valley locking physics for hosting rich excitonic species and the reduced screening for strong Coulomb interactions. Here, we report the observation of multiple valley phonons, phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone, and the resulting exciton complexes…
We present time-resolved Kerr rotation measurements, showing spin lifetimes of over 100 ns at room temperature in monolayer MoSe$_2$. These long lifetimes are accompanied by an intriguing temperature dependence of the Kerr amplitude, which increases with temperature up to 50 K and then abruptly switches sign. Using ab initio simulations we explain the latter behavior in terms of the intrinsic electron-phonon coupling and the activation of transitions to secondary valleys. The phonon-assisted scattering of the photo-excited electron-hole pairs prepares a valley spin polarization within the firs…
Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic $B$ transition after optical excitation of the energetically lower excitonic $A$ transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a popul…
We study the relaxation of a single electron spin in a circular quantum dot in a transition-metal dichalcogenide monolayer defined by electrostatic gating. Transition-metal dichalcogenides provide an interesting and promising arena for quantum dot nano-structures due to the combination of a band gap, spin-valley physics and strong spin-orbit coupling. First we will discuss which bound state solutions in different B-field regimes can be used as the basis for qubits states. We find that at low B-fields combined spin-valley Kramers qubits to be suitable, while at large magnetic fields pure spin o…
We explore several microscopic mechanisms for breaking the $n=0$ fourfold Landau level degeneracy in a single-layer graphene. Valley-scattering random potential, Zeeman interaction, and electron-phonon coupling are considered in the presence of SU(4)-symmetric Coulomb exchange interaction. Among all the mechanisms considered, it is the electron-phonon coupling combined with the Zeeman interaction which leads to the full splitting of the $n=0$ Landau levels. A recent controversy of "valley-first" or "spin-first" breaking of SU(4) symmetry of the $n=0$ graphene Landau level is examined in light …
While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ va…
Topological phononics offers numerous opportunities in manipulating elastic waves that can propagate in solids without being backscattered. Due to the lack of nanoscale imaging tools that aid the system design, however, acoustic topological metamaterials have been mostly demonstrated in macroscale systems operating at low (kilohertz to megahertz) frequencies. Here, we report the realization of gigahertz topological valley Hall effect in nanoelectromechanical AlN membranes. Propagation of elastic wave through phononic crystals is directly visualized by microwave microscopy with unprecedented se…
Smoothly varying lattice strain in graphene affects the Dirac carriers through a synthetic gauge field. When the lattice strain is time dependent, as in connection with phononic excitations, the gauge field becomes time dependent and the synthetic vector potential is also associated with an electric field. We show that this synthetic electric field has observable consequences. Joule heating associated with the currents driven by the synthetic electric field dominates the intrinsic damping, caused by the electron-phonon interaction, of many acoustic phonon modes of graphene and metallic carbon …
We report on the effect of elastic intervalley scattering on the energy transport between electrons and phonons in many-valley semiconductors. We derive a general expression for the electron-phonon energy flow rate at the limit where elastic intervalley scattering dominates over diffusion. Electron heating experiments on heavily doped n-type Si samples with electron concentration in the range $3.5-16.0\times 10^{25}$ m$^{-3}$ are performed at sub-1 K temperatures. We find a good agreement between the theory and the experiment.
Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN en…
We investigate the possibility of using phonon-drag imaging for the study of 2D electrons in (110) AlAs quantum wells. Our numerical simulations show that direct information on the strain and quantum confinement dependent valley occupancy of the electrons, on the anisotropic effective mass tensor and on electron-phonon coupling parameters can be obtained.
We report the direct observation of intervalley exciton between the Q conduction valley and $Γ$ valence valley in bilayer WSe$_2$ by photoluminescence. The Q$Γ$ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe$_2$. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between Q$Γ$ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between Q$Γ$ and QK excitons. Both Q$Γ$ and QK excitons exhibit pronounced phonon re…
We present a comprehensive first-principles analysis of the non-adiabatic effects due to the electron-phonon interaction on the vibrational spectrum of the electron-doped monolayer MoS$_{2}$. Deep changes in the Fermi surface upon doping cause the linewidth broadening of the normal modes governing the spin-conserving inter-valley electronic scattering, which become unstable with the population of all the spin-split conduction valleys. We find that the non-adiabatic spectral effects modify dramatically the adiabatic dispersion of the long-wavelength optical phonon modes, responsible for intra-v…
An $\it{ab \,\, initio}$ based fully microscopic many-body approach is used to study the carrier relaxation dynamics in monolayer transition-metal dichalcogenides. Bandstructures and wavefunctions as well as phonon energies and coupling matrix elements are calculated using density functional theory. The resulting dipole and Coulomb matrix elements are implemented in the Dirac-Bloch equations to calculate carrier-carrier and carrier-phonon scatterings throughout the whole Brillouin zone. It is shown that carrier scatterings lead to a relaxation into hot quasi-Fermi distributions on a single fem…
Three-dimensional (3D) elastic phononic topological insulator, featuring two-dimensional (2D) surface states, which support the high-efficient and robust elastic wave propagation without backscattering in all spatial dimensions, remains a challenge due to the nature of multiple polarized elastic modes and their complex hybridization in 3D. Here, a 3D elastic phononic topological insulator is designed and observed experimentally by emulating the quantum valley Hall effects. The spatial inversion of adjacent atoms gives rise to a valley topological phase to an insulating regime with complete 3D …
The stability of valley polarized electron states is crucial for the development of valleytronics. A long relaxation time of the valley polarization is required to enable operations to be performed on the polarized states. Here we investigate the stability of valley polarized states in diamond, expressed as relaxation time. We have found that the stability of the states can be extremely long when we consider the symmetry determined electron-phonon scattering. By Time-of-Flight measurements and Monte Carlo simulations, we determine electron-phonon coupling constants and use these data in order …
We investigate the effect of the valley degree of freedom on Pauli-spin blockade readout of spin qubits in silicon. The valley splitting energy sets the singlet-triplet splitting and thereby constrains the detuning range. The valley phase difference controls the relative strength of the intra- and inter-valley tunnel couplings, which, in the proposed Pauli-spin blockade readout scheme, couple singlets and polarized triplets, respectively. We find that high-fidelity readout is possible for a wide range of phase differences, while taking into account experimentally observed valley splittings and…
The electronic states at the direct band gap of monolayer WSe2 at the $K^+$ and $K^-$ valleys are related by time reversal and may be viewed as pseudo-spins. The corresponding optical interband transitions are governed by robust excitons. In double resonant Raman spectroscopy, we uncover that the 2s exciton state energy differs from the 1s state energy by exactly the energy of the combination of several prominent phonons. Superimposed on the exciton photoluminescence (PL) we observe the double resonant Raman signal. This spectrally narrow peak shifts with the excitation laser energy as incomin…
The presence of degenerate conduction band valleys and how they are mixed by interfaces play critical roles in determining electron interaction and spectrum in a silicon nanostructure. Here we investigate how the valley phases affect the exchange interaction in a symmetric two-electron silicon double quantum dot. Through a configuration interaction calculation, we find that exchange splitting is suppressed at a finite value of valley phase difference between the two dots, and reaches its minimum value ({\sim} 0) when the phase difference is π. Such a suppression can be explained using the Hubb…
When graphene is deformed in a dynamical manner, a time-dependent potential is induced for the electrons. The potential is antisymmetric with respect to valleys, and some straightforward applications are found for Raman spectroscopy. We show that a valley-antisymmetric potential broadens Raman $D$ band but does not affect $2D$ band, which is already observed by recent experiments. The space derivative of the valley antisymmetric potential gives a force field that accelerates intervalley phonons, while it corresponds to the longitudinal component of the previously discussed pseudoelectric field…
Calculations combining first-principles electron-phonon ($e$-ph) interactions with the Boltzmann equation enable studies of ultrafast carrier and phonon dynamics. However, in materials with weak Coulomb screening, electrons and holes form bound excitons and their scattering processes become correlated, posing additional challenges for modeling nonequilibrium physics. Here we show calculations of ultrafast exciton dynamics and related time-domain spectroscopies using $ab~initio$ exciton-phonon (ex-ph) interactions together with an excitonic Boltzmann equation. Starting from the nonequilibrium e…
Valley splitting is a key figure of silicon-based spin qubits. Quantum dots in Si/SiGe heterostructures reportedly suffer from a relatively low valley splitting, limiting the operation temperature and the scalability of such qubit devices. Here, we demonstrate a robust and large valley splitting exceeding 200 $μ$eV in a gate-defined single quantum dot, hosted in molecular-beam epitaxy-grown $^{28}$Si/SiGe. The valley splitting is monotonically and reproducibly tunable up to 15 % by gate voltages, originating from a 6 nm lateral displacement of the quantum dot. We observe static spin relaxation…
Excitons and trions (or exciton-polarons) in transition metal dichalcogenides (TMDs) are known to decay predominantly through intravalley transitions. Electron-hole recombination across different valleys can also play a significant role in the excitonic dynamics, but intervalley transitions are rarely observed in monolayer TMDs, because they violate the conservation of momentum. Here we reveal the intervalley recombination of dark excitons and trions through more than one path in monolayer WSe$_2$. We observe the intervalley dark excitons, which can recombine by the assistance of defect scatte…
In single-layer WSe$_2$, a paradigmatic semiconducting transition metal dichalcogenide, a circularly polarized laser field can selectively excite electronic transitions in one of the inequivalent $K^{\pm}$ valleys. Such selective valley population corresponds to a pseudospin polarization. This can be used as a degree of freedom in a valleytronic device provided that the time scale for its depolarization is sufficiently large. Yet, the mechanism behind the valley depolarization still remains heavily debated. Recent time-dependent Kerr experiments have provided an accurate way to visualize the v…
