Monolayer transition-metal dichalcogenides possess a pair of degenerate helical valleys in the band structure that exhibit fascinating optical valley polarization. Optical valley polarization, however, is limited by carrier lifetimes of these materials. Lifting the valley degeneracy is therefore an attractive route for achieving valley polarization. It is very challenging to achieve appreciable valley degeneracy splitting with applied magnetic field. We propose a strategy to create giant splitting of the valley degeneracy by proximity-induced Zeeman effect. As a demonstration, our first principles calculations of monolayer MoTe$_2$ on a EuO substrate show that valley splitting over 300 meV can be generated. The proximity coupling also makes interband transition energies valley dependent, enabling valley selection by optical frequency tuning in addition to circular polarization. The valley splitting in the heterostructure is also continuously tunable by rotating substrate magnetization. The giant and tunable valley splitting adds a readily accessible dimension to the valley-spin physics with rich and interesting experimental consequences, and offers a practical avenue for exploring device paradigms based on the intrinsic degrees of freedom of electrons.
Berry phase plays an important role in determining many physical properties of quantum systems. However, a Berry phase altering energy spectrum of a quantum system is comparatively rare. Here, we report an unusual tunable valley polarized energy spectra induced by continuously tunable Berry phase in Bernal-stacked bilayer graphene quantum dots. In our experiment, the Berry phase of electron orbital states is continuously tuned from about pi to 2pi by perpendicular magnetic fields. When the Berry phase equals pi or 2pi, the electron states in the two inequivalent valleys are energetically degen…
The control and manipulation of the valley and spin degrees of freedom have received great interests in fundamental studies and advanced information technologies. Compared with magnetic means, it is highly desirable to realize more energy-efficient electric control of valley and spin. Using the first-principles calculations, we demonstrate tunable valley and spin degeneracy splittings in $\rm VSi_2N_4$ bilayers, with the aid of the layered structure and associated electric control. Depending on different interlayer magnetic couplings and stacking orders, the $\rm VSi_2N_4$ bilayers exhibit a v…
The relativistic Landau levels in the layered organic material alpha-(BEDT-TTF)_2I_3 [BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene] are sensitive to the tilt of the Dirac cones, which, as in the case of graphene, determine the low-energy electronic properties under appropriate pressure. We show that an applied inplane electric field, which happens to be in competition with the tilt of the cones, lifts the twofold valley degeneracy due to a different level spacing. The scenario may be tested in infrared transmission spectroscopy.
Atomically precise tailoring of graphene can enable unusual transport pathways and new nanometer-scale functional devices. Here we describe a recipe for the controlled production of highly regular "5-5-8" line defects in graphene by means of simultaneous electron irradiation and Joule heating by applied electric current. High-resolution transmission electron microscopy reveals individual steps of the growth process. Extending earlier theoretical work suggesting valley-discriminating capabilities of a graphene 5-5-8 line defect, we perform first-principles calculations of transport and find a s…
We have investigated the valley degeneracy of MoS2 multilayers and its effect on thermoelectric properties. By modulating the layer thickness and external electric field, the hole valleys at Γ and K points in the highest energy valence band and the electron valleys at K and Σmin points in the lowest energy conduction band are shifted differently. The hole valley degeneracy is observed in MoS2 monolayer, while that of electron valley is in MoS2 bilayer and monolayer under the external electric field. By tuning the valley degeneracy, the Seebeck coefficient and electrical conductivity can be sep…
Measuring degeneracy and broken-symmetry states of a system at nanoscale requires extremely high energy and spatial resolution, which has so far eluded direct observation. Here, we realize measurement of the degeneracy and subtle broken-symmetry states of graphene at nanoscale for the first time. By using edge-free graphene quantum dots, we are able to measure valley splitting and valley-contrasting spin splitting of graphene at the single-electron level. Our experiments detect large valley splitting around atomic defects of graphene due to the coexistence of sublattice symmetry breaking and t…
Various physical phenomena have been discovered by tuning degrees of freedom, among which there is the degree of freedom (DOF) -- "valley". The typical valley materials are characterized by two degenerate valley states protected by time-reversal symmetry (TS). These states indexed by valley DOF have been measured and manipulated for emergent valley-contrasting physics with the broken valley degeneracy. To achieve the valley splitting resulted from TS breaking, previous studies mainly focused on magnetic proximity effect provided by ferromagnetic (FM) layer. Nevertheless, the anti-ferromagnetic…
(111) Silicon quantum wells have been studied extensively, yet no convincing explanation exists for the experimentally observed breaking of 6 fold valley degeneracy into 2 and 4 fold degeneracies. Here, systematic sp3d5s* tight-binding and effective mass calculations are presented to show that a typical miscut modulates the energy levels which leads to breaking of 6 fold valley degeneracy into 2 lower and 4 raised valleys. An effective mass based valley-projection model is used to determine the directions of valley-minima in tight-binding calculations of large supercells. Tight-binding calcula…
Motivated by interesting recent experimental results, we consider theoretically charged-impurity scattering-limited 2D electronic transport in (100), (110), and (111)-Si inversion layers at low temperatures and carrier densities, where screening effects are important. We show conclusively that, given the same bare Coulomb disorder, the 2D mobility for a given system increases monotonically with increasing valley degeneracy. We also show that the temperature and the parallel magnetic field dependence of the 2D conductivity is strongly enhanced by increasing valley degeneracy. We analytically co…
Three-dimensional confinement allows semiconductor quantum dots (QDs) to exhibit size-tunable electronic and optical properties that enable a wide range of opto-electronic applications from displays, solar cells and bio-medical imaging to single-electron devices. Additional modalities such as spin and valley properties can provide further degrees of freedom requisite for quantum information and spintronics. When seeking to combine these material features into QD structures, however, confinement can cause hybridization that inhibits the robustness of these emergent properties for insertion into…
Electron spins in Si/SiGe quantum wells suffer from nearly degenerate conduction band valleys, which compete with the spin degree of freedom in the formation of qubits. Despite attempts to enhance the valley energy splitting deterministically, by engineering a sharp interface, valley splitting fluctuations remain a serious problem for qubit uniformity, needed to scale up to large quantum processors. Here, we elucidate and statistically predict the valley splitting by the holistic integration of 3D atomic-level properties, theory and transport. We find that the concentration fluctuations of Si …
Based on first-principles calculations, we find novel valley-polarized quantum anomalous Hall (VP-QAH) phases with a large gap-0.19 eV at an appropriate buckled angle and tunable topological phase transitions driven by the spontaneous magnetization within a half-hydrogenated Bi honeycomb monolayer. Depending on the magnetization orientation, four different phases can emerge, i.e., two VP-QAH phases, ferromagnetic insulating and metallic states. When the magnetization is reversed from the +$\mathbf{z}$ to -$\mathbf{z}$ directions, accompanying with a sign change in the Chern number (from -1 to …
The concept of ferrovalley materials has been proposed very recently. The existence of spontaneous valley polarization, resulting from ferromagnetism, in such hexagonal two-dimensional materials makes nonvolatile valleytronic applications realizable. Here, we introduce a new member of ferrovalley family with orthorhombic lattice, i.e. monolayer group-IV monochalcogenides (GIVMs), in which the intrinsic valley polarization originates from ferroelectricity, instead of ferromagnetism. Combining the group theory analysis and first-principles calculations, we demonstrate that, different from the va…
The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe$_2$/WSe$_2$ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned…
Strain-tunable multipiezo effects in Janus monolayer Cr2SSe: Selective reversal of valley polarization and single-spin-channel anomalous valley Hall effect
Breaking space-time symmetries in two-dimensional crystals (2D) can dramatically influence their macroscopic electronic properties. Monolayer transition-metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations, even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applicati…
We perform a comparative study on thermoelectric performance of antiperovskite oxides $Ae_3Tt$O and nitrides $Ae_3Pn$N ($Ae=$ Ca, Sr, Ba; $Tt=$ Ge, Sn, Pb; $Pn=$ As, Sb, Bi) by means of first-principles calculation. As for the oxides with the cubic structure, Ca$_3$GeO with a sizable band gap exhibits high thermoelectric performance at high temperatures, while Ba$_3$PbO with Dirac cones without the gap is favorable at low temperatures. The latter high performance owes to high valley degeneracy including the multiple Dirac cones and the valleys near the $Γ$ and R points. For the nitrides with t…
We investigate the optical response of the silicene and similar materials, such as germanene, in the presence of an electrically tunable band gap for variable doping. The interplay of spin orbit coupling, due to the buckled structure of these materials, and a perpendicular electric field gives rise to a rich variety of phases: a topological or quantum spin Hall insulator, a valley-spin-polarized metal and a band insulator. We show that the dynamical conductivity should reveal signatures of these different phases which would allow for their identification along with the determination of paramet…
In non-centrosymmetric metals, spin-orbit coupling (SOC) induces momentum-dependent spin polarization at the Fermi surfaces. This is exemplified by the valley-contrasting spin polarization in monolayer transition metal dichalcogenides (TMDCs) with in-plane inversion asymmetry. However, the valley configuration of massive Dirac fermions in TMDCs is fixed by the graphene-like structure, which limits the variety of spin-valley coupling. Here, we show that the layered polar metal BaMn$X_2$ ($X =$Bi, Sb) hosts tunable spin-valley-coupled Dirac fermions, which originate from the distorted $X$ square…
The valley degree of freedom is a sought-after quantum number in monolayer transition-metal dichalcogenides. Similar to optical spin orientation in semiconductors, the helicity of absorbed photons can be relayed to the valley (pseudospin) quantum number of photoexcited electrons and holes. Also similar to the quantum-mechanical spin, the valley quantum number is not a conserved quantity. Valley depolarization of excitons in monolayer transition-metal dichalcogenides due to long-range electron-hole exchange typically takes a few ps at low temperatures. Exceptions to this behavior are monolayers…
The valley splitting, which lifts the degeneracy of the lowest two valley states in a SiO$_2$/(100)Si/SiO$_2$ quantum well is examined through transport measurements. We demonstrate that the valley splitting can be observed directly as a step in the conductance defining a boundary between valley-unpolarized and polarized regions. This persists to well above liquid helium temperature and shows no dependence on magnetic field, indicating that single-particle valley splitting and valley-polarization exist in (100) silicon even at zero magnetic field.
A novel topological insulator with tunable edge states, called quantum spin-quantum anomalous Hall (QSQAH) insulator, is predicted in a heterostructure of a hydrogenated Sb (SbH) monolayer on a LaFeO3 substrate by using ab initio methods. The substrate induces a drastic staggered exchange field in the SbH film, which plays an important role to generate the QSQAH effect. A topologically nontrivial band gap (up to 35 meV) is opened by Rashba spin-orbit coupling, which can be enlarged by strain and electric field. To understand the underlying physical mechanism of the QSQAH effect, a tight-bindin…
Fractional quantum Hall states (FQHSs) at even-denominator Landau level filling factors ($ν$) are of prime interest as they are predicted to host exotic, topological states of matter. We report here the observation of a FQHS at $ν=1/2$ in a two-dimensional electron system of exceptionally high quality, confined to a wide AlAs quantum well, where the electrons can occupy multiple conduction-band valleys with an anisotropic effective mass. The anisotropy and multi-valley degree of freedom offer an unprecedented tunability of the $ν=1/2$ FQHS as we can control both the valley occupancy via the ap…
In this letter we study the valley degeneracy splitting of the transition-metal dichalcogenides monolayer by first-principles calculations. The local magnetic moments are introduced into the system when the transition-metal atoms are adsorbed to the monolayer surface. Zeeman effect arising from the local magnetic moment at transition-metal atom sites lifts the valley degeneracy. Anomalous charge, spin and valley Hall Effects can be accessed due to valley splitting when we can only excite carriers of one valley. The valley splitting depends on the direction of magnetization and thus can be tune…
The interplay between magnetism, band topology, and electronic correlation in low dimensions has been a fascinating subject of research. Here, we propose two-dimensional (2D) material systems which demonstrate such an interesting interplay. Based on first-principles calculations and structural search algorithms, we identify three lowest energy 2D CoSe structures, termed as the $α$-, $β$-, and $γ$-CoSe. {We show that $α$- and $β$-CoSe are two rare examples of 2D antiferromagnetic metals, which are related to their Fermi surfaces nesting features, and meanwhile, $γ$-CoSe is a ferromagnetic metal…
We apply a microscopic theory of exciton-polaritons in cavity-confined monolayer transition-metal dichalcogenides including both optical polarizations in the monolayer plane, allowing to describe how chiral cavity photons interact with the valley degrees of freedom of the active material. Upon polariton formation, the degenerate excitons inhabiting the two inequivalent valleys are shown to assume bonding and antibonding superpositions as a result of cavity-mediated intravalley interactions combined with intervalley Coulomb interactions. This is representative of a polariton-induced coherent mi…
The valley degeneracy of electron states in graphene stimulates intensive research of valley-related optical and transport phenomena. While many proposals on how to manipulate valley states have been put forward, experimental access to the valley polarization in graphene is still a challenge. Here, we develop a theory of the second optical harmonic generation in graphene and show that this effect can be used to measure the degree and sign of the valley polarization. We show that, at the normal incidence of radiation, the second harmonic generation stems from imbalance of carrier populations in…
We examine energy spectra of Si quantum dots embedded into Si_{0.75}Ge_{0.25} buffers using atomistic numerical calculations for dimensions relevant to qubit implementations. The valley degeneracy of the lowest orbital state is lifted and valley splitting fluctuates with monolayer frequency as a function of the dot thickness. For dot thicknesses <6 nm valley splitting is found to be >150 ueV. Using the unique advantage of atomistic calculations we analyze the effect of buffer disorder on valley splitting. Disorder in the buffer leads to the suppression of valley splitting by a factor of 2.5, t…
Electrons are offered a valley degree of freedom in presence of particular lattice structures. Manipulating valley degeneracy is the subject matter of an emerging field of investigation, mostly focused on charge transport in graphene. In bulk bismuth, electrons are known to present a threefold valley degeneracy and a Dirac dispersion in each valley. Here we show that because of their huge in-plane mass anisotropy, a flow of Dirac electrons along the trigonal axis is extremely sensitive to the orientation of in-plane magnetic field. Thus, a rotatable magnetic field can be used as a valley valve…
The electronic topology is generally related to the Berry curvature, which can induce the anomalous Hall effect in time-reversal symmetry breaking systems. Intrinsic monolayer transition metal dichalcogenides possesses two nonequivalent K and K' valleys, having Berry curvatures with opposite signs, and thus vanishing anomalous Hall effect in this system. Here we report the experimental realization of asymmetrical distribution of Berry curvature in a single valley in monolayer WSe2 through applying uniaxial strain to break C3v symmetry. As a result, although the Berry curvature itself is still …
The lifting of the two-fold degeneracy of the conduction valleys in a strained silicon quantum well is critical for spin quantum computing. Here, we obtain an accurate measurement of the splitting of the valley states in the low-field region of interest, using the microwave spectroscopy technique of electron valley resonance (EVR). We compare our results with conventional methods, observing a linear magnetic field dependence of the valley splitting, and a strong low-field suppression, consistent with recent theory. The resonance linewidth shows a marked enhancement above $T\simeq 300$ mK.
In transition-metal dichalcogenides, electrons in the K-valleys can experience both Ising and Rashba spin-orbit couplings. In this work, we show that the coexistence of Ising and Rashba spin-orbit couplings leads to a special type of valley Hall effect, which we call spin-orbit coupling induced valley Hall effect. Importantly, near the conduction band edge, the valley-dependent Berry curvatures generated by spin-orbit couplings are highly tunable by external gates and dominate over the intrinsic Berry curvatures originating from orbital degrees of freedom under accessible experimental conditio…
Strain-Tunable Spin Filtering and Valley Splitting Coexisting with Anomalous Hall Effect in 2D Half-Metallic VSe2/VN Heterostructure: Toward a Unified Spintronic-Valleytronic Platform
Compared with direct-gap semiconductors, the valley degeneracy of silicon and germanium opens up new channels for spin relaxation that counteract the spin degeneracy of the inversion-symmetric system. Here the symmetries of the electron-phonon interaction for silicon and germanium are identified and the resulting spin lifetimes are calculated. Room-temperature spin lifetimes of electrons in silicon are found to be comparable to those in gallium arsenide, however, the spin lifetimes in silicon or germanium can be tuned by reducing the valley degeneracy through strain or quantum confinement. The…
Two-dimensional transition metal dichalcogenides show great potential as promising thermoelectric materials due to their lower dimensionality, the unique density of states and quantum confinement of carriers. The effect of mechanical strain on the thermoelectric performances of monolayer WS 2 has been investigated using density functional theory associated with semiclassical Boltzmann transport theory. The variation of Seebeck coefficient and band gap with applied strain has followed the same type of trend. For n-type material the relaxation time scaled power factor(S 2 σ/τ) increases by the a…
