arXiv subjects

Dinh Van Tuan

Publications and source records attributed to Dinh Van Tuan.

At least 37 records · Page 2Linked to original sources

arXiv2021

Relaxation and darkening of excitonic complexes in electrostatically-doped monolayer semiconductors: Roles of exciton-electron and trion-electron interactions

We present photoluminescence measurements in monolayer WSe$_2$, which point to the importance of the interaction between charged particles and excitonic complexes. The theoretical analysis highlights the key role played by exchange scattering, referring to cases wherein the particle composition of the complex changes after the interaction. For example, exchange scattering renders bright excitonic complexes dark in monolayer WSe$_2$ on accounts of the unique valley-spin configuration in this material. In addition to the ultrafast energy relaxation of hot excitonic complexes following their interaction with electrons or holes, our analysis sheds light on several key features that are commonly seen in the photoluminescence of this monolayer semiconductor. In particular, we can understand why the photoluminescence intensity of the neutral bright exciton is strongest when the monolayer is hole-doped rather than charge neutral or electron-doped. Or the reason for the dramatic increase of the photoluminescence intensity of negatively-charged excitons (trions) as soon as electrons are added to the monolayer. To self-consistently explain the findings, we further study the photoluminescence spectra at different excitation energies and analyze the behavior of the elusive indirect exciton.

cond-mat.mtrl-sci↗

arXiv2021

Spin/Valley pumping of resident electrons in WSe2 and WS2 monolayers

Monolayers of transition metal dichalcogenides are ideal materials to control both spin and valley degrees of freedom either electrically or optically. Nevertheless, optical excitation mostly generates excitons species with inherently short lifetime and spin/valley relaxation time. Here we demonstrate a very efficient spin/valley optical pumping of resident electrons in n-doped WSe2 and WS2 monolayers. We observe that, using a continuous wave laser and appropriate doping and excitation densities, negative trion doublet lines exhibit circular polarization of opposite sign and the photoluminescence intensity of the triplet trion is more than four times larger with circular excitation than with linear excitation. We interpret our results as a consequence of a large dynamic polarization of resident electrons using circular light.

cond-mat.mes-hall↗

arXiv2020

Valley Phonons and Exciton Complexes in a Monolayer Semiconductor

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 in the monolayer semiconductor WSe2. From Lande g-factor and polarization analyses of photoluminescence peaks, we find that these valley phonons lead to efficient intervalley scattering of quasi particles in both exciton formation and relaxation. This leads to a series of photoluminescence peaks as valley phonon replicas of dark trions. Using identified valley phonons, we also uncovered an intervalley exciton near charge neutrality, and extract its short-range electron-hole exchange interaction to be about 10 meV. Our work not only identifies a number of previously unknown 2D excitonic species, but also shows that monolayer WSe2 is a prime candidate for studying interactions between spin, pseudospin, and zone-edge phonons.

cond-mat.mes-hall↗

arXiv2019

Exciton valley depolarization in monolayer transition-metal dichalcogenides

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 MoSe$_2$ and MoTe$_2$ wherein the depolarization is much faster. We elucidate the enigmatic anomaly of these materials, finding that it originates from Rashba-induced coupling of the dark and bright exciton branches next to their degeneracy point. When photoexcited excitons scatter during their energy relaxation between states next to the degeneracy region, they reach the light cone after losing the initial helicity. The valley depolarization is not as fast in monolayers WSe$_2$, WS$_2$ and likely MoS$_2$ wherein the Rashba-induced coupling is negligible.

cond-mat.mes-hall↗

arXiv2019

Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe2

Monolayers of semiconducting transition metal dichalcogenides (TMDCs) with unique spin-valley contrasting properties and remarkably strong excitonic effects continue to be a subject of intense research interests. These model 2D semiconductors feature two fundamental intravalley excitons species - optically accessible ' bright' excitons with anti-parallel spins and optically inactive 'dark' excitons with parallel spins. For applications exploiting radiative recombination of bright excitons or long lifetime dark excitons, it is essential to understand the radiative character of the exciton ground state and establish the energy separation between the lowest energy bright and dark excitons. Here, we report a direct spectroscopic measure of dark excitons in monolayer MoSe$_2$ encapsulated in hexagonal boron nitride. By applying strong in-plane magnetic field, we induce mixing and splitting of bright and dark exciton branches, which enables an accurate spectroscopic determination of their energies. We confirm the bright character of the exciton ground state separated by a 1.5~meV gap from the higher energy dark exciton state, much smaller compared to the previous theoretical expectations. These findings provide critical information for further improvement of the accurate theoretical description of TMDCs electronic structure.

cond-mat.mes-hall↗

arXiv2019

Localization-induced optical properties of monolayer transition-metal dichalcogenides

Impurities play an important role during recombination processes in semiconductors. Their important role is sharpened in atomically-thin transition-metal dichalcogenides whose two-dimensional character renders electrons and holes highly susceptible to localization caused by remote charged impurities. We study a multitude of phenomena that arise from the interaction of localized electrons with excitonic complexes. Emphasis is given to the amplification of the phonon-assisted recombination of biexcitons when it is mediated by localized electrons, showing that this mechanism can explain recent photoluminescence experiments in ML-WSe$_2$. In addition, the magnetic-field dependence of this mechanism is analyzed. The results of this work point to (i) an intriguing coupling between the longitudinal-optical and homopolar phonon modes that can further elucidate various experimental results, (ii) the physics behind a series of localization-induced optical transitions in tungsten-based materials, and (iii) the importance of localization centers in facilitating the creation of biexcitons and exciton-exciton annihilation processes.

cond-mat.mes-hall↗

arXiv2019

Probing Many-Body Interactions in Monolayer Transition-Metal Dichalcogenides

Many-body interactions in monolayer transition-metal dichalcogenides are strongly affected by their unique band structure. We study these interactions by measuring the energy shift of neutral excitons (bound electron-hole pairs) in gated WSe$_2$ and MoSe$_2$. Surprisingly, while the blueshift of the neutral exciton, $X^0$, in electron-doped samples can be more than 10~meV, the blueshift in hole-doped samples is nearly absent. Taking into account dynamical screening and local-field effects, we present a transparent and analytical model that elucidates the crucial role played by intervalley plasmons in electron-doped conditions. The energy shift of $X^0$ as a function of charge density is computed showing agreement with experiment, where the renormalization of $X^0$ by intervalley plasmons yields a stronger blueshift in MoSe$_2$ than in WSe$_2$ due to differences in their band ordering.

cond-mat.mtrl-sci↗

arXiv2019

Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum

Monolayer transition-metal dichalcogenides (ML-TMDs) offer exciting opportunities to test the manifestations of many-body interactions through changes in the charge density. Tuning the charge density by a gate voltage leads to profound changes in the optical spectra of excitons in ML-TMDs. We review the band-gap renormalization and dynamical screening as a function of charge density, and then incorporate these effects through various approximations that model long-wavelength charge excitations in the Bethe-Salpeter Equation (BSE). We then show that coupling between excitons and shortwave charge excitations is essential to resolve several experimental puzzles. Unlike ubiquitous and well-studied plasmons, driven by collective oscillations of the background charge density in the long-wavelength limit, we discuss the emergence of shortwave plasmons that originate from the short-range Coulomb interaction through which electrons transition between the $\mathbf{K}$ and $-\mathbf{K}$ valleys. We study the coupling between the shortwave plasmons and the neutral exciton through the self-energy of the latter. We then elucidate how this coupling as well as the spin ordering in the conduction band give rise to an experimentally observed optical sideband in electron-doped W-based MLs, conspicuously absent in electron-doped Mo-based MLs or any hole-doped ML-TMDs. While the focus of this review is on the optical manifestations of many-body effects in ML-TMDs, a systematic description of the dynamical screening and its various approximations allow one to revisit other phenomena, such as nonequilibrium transport or superconducting pairing, where the use of the BSE or the emergence of shortwave plasmons can play an important role.

cond-mat.mtrl-sci↗

arXiv2019

Intervalley plasmons in crystals

Collective charge excitations in solids have been the subject of intense research ever since the pioneering works of Bohm and Pines in the 1950s. Most of these studies focused on long-wavelength plasmons that involve charge excitations with a small crystal-momentum transfer, $q \ll G$, where $G$ is the wavenumber of a reciprocal lattice vector. Less emphasis was given to collective charge excitations that lead to shortwave plasmons in multivalley electronic systems (i.e., when $q \sim G$). We present a theory of intervalley plasmons, taking into account local-field effects in the dynamical dielectric function. Focusing on monolayer transition-metal dichalcogenides where each of the valleys is further spin-split, we derive the energy dispersion of these plasmons and their interaction with external charges. Emphasis in this work is given to sum rules from which we derive the interaction between intervalley plasmons and a test charge, as well as a compact single-plasmon pole expression for the dynamical Coulomb potential.

cond-mat.mtrl-sci↗

arXiv2018

The Coulomb interaction in monolayer transition-metal dichalcogenides

Recently, the celebrated Keldysh potential has been widely used to describe the Coulomb interaction of few-body complexes in monolayer transition-metal dichalcogenides. Using this potential to model charged excitons (trions), one finds a strong dependence of the binding energy on whether the monolayer is suspended in air, supported on SiO$_2$, or encapsulated in hexagonal boron-nitride. However, empirical values of the trion binding energies show weak dependence on the monolayer configuration. This deficiency indicates that the description of the Coulomb potential is still lacking in this important class of materials. We address this problem and derive a new potential form, which takes into account the three atomic sheets that compose a monolayer of transition-metal dichalcogenides. The new potential self-consistently supports (i) the non-hydrogenic Rydberg series of neutral excitons, and (ii) the weak dependence of the trion binding energy on the environment. Furthermore, we identify an important trion-lattice coupling due to the phonon cloud in the vicinity of charged complexes. Neutral excitons, on the other hand, have weaker coupling to the lattice due to the confluence of their charge neutrality and small Bohr radius.

cond-mat.mtrl-sci↗

arXiv2018

Virtual trions in the photoluminescence of monolayer transition-metal dichalcogenides

Photoluminescence experiments from monolayer transition-metal dichalcogenides often show that the binding energy of trions is conspicuously similar to the energy of optical phonons. This enigmatic coincidence calls into question whether phonons are involved in the radiative recombination process. We address this problem, unraveling an intriguing optical transition mechanism. Its initial state is a localized charge (electron or hole) and delocalized exciton. The final state is the localized charge, phonon and photon. In between, the intermediate state of the system is a virtual trion formed when the localized charge captures the exciton through emission of the phonon. We analyze the difference between radiative recombinations that involve real and virtual trions (i.e., with and without a phonon), providing useful ways to distinguish between the two in experiment.

cond-mat.mtrl-sci↗

arXiv2018

Pseudospin-driven spin relaxation mechanism in graphene

The possibility of transporting spin information over long distances in graphene, owing to its small intrinsic spin-orbit coupling (SOC) and the absence of hyperfine interaction, has led to intense research into spintronic applications. However, measured spin relaxation times are orders of magnitude smaller than initially predicted, while the main physical process for spin dephasing and its charge-density and disorder dependences remain unconvincingly described by conventional mechanisms. Here, we unravel a spin relaxation mechanism for nonmagnetic samples that follows from an entanglement between spin and pseudospin driven by random SOC, which makes it unique to graphene. The mixing between spin and pseudospin-related Berry's phases results in fast spin dephasing even when approaching the ballistic limit, with increasing relaxation times away from the Dirac point, as observed experimentally. The SOC can be caused by adatoms, ripples or even the substrate, suggesting novel spin manipulation strategies based on the pseudospin degree of freedom.

cond-mat.mes-hall↗

arXiv2017

Marrying excitons and plasmons in monolayer transition-metal dichalcogenides

Just as photons are the quanta of light, plasmons are the quanta of orchestrated charge-density oscillations in conducting media. Plasmon phenomena in normal metals, superconductors and doped semiconductors are often driven by long-wavelength Coulomb interactions. However, in crystals whose Fermi surface is comprised of disconnected pockets in the Brillouin zone, collective electron excitations can also attain a shortwave component when electrons transition between these pockets. Here, we show that the band structure of monolayer transition-metal dichalcogenides gives rise to an intriguing mechanism through which shortwave plasmons are paired up with excitons. The coupling elucidates the origin for the optical side band that is observed repeatedly in monolayers of WSe$_2$ and WS$_2$ but not understood. The theory makes it clear why exciton-plasmon coupling has the right conditions to manifest itself distinctly only in the optical spectra of electron-doped tungsten-based monolayers.

cond-mat.mtrl-sci↗

arXiv2017

Spin Hall Effect and Origins of Nonlocal Resistance in Adatom-Decorated Graphene

Recent experiments reporting unexpectedly large spin Hall effect (SHE) in graphene decorated with adatoms have raised a fierce controversy. We apply numerically exact Kubo and Landauer- Buttiker formulas to realistic models of gold-decorated disordered graphene (including adatom clustering) to obtain the spin Hall conductivity and spin Hall angle, as well as the nonlocal resistance as a quantity accessible to experiments. Large spin Hall angles of 0.1 are obtained at zero-temperature, but their dependence on adatom clustering differs from the predictions of semiclassical transport theories. Furthermore, we find multiple background contributions to the nonlocal resistance, some of which are unrelated to SHE or any other spin-dependent origin, as well as a strong suppression of SHE at room temperature. This motivates us to design a multiterminal graphene geometry which suppresses these background contributions and could, therefore, quantify the upper limit for spin current generation in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2016

Spin Dynamics in Bilayer Graphene : Role of Electron-Hole Puddles and the Dyakonov-Perel Mechanism

We report on spin transport features which are unique to high quality bilayer graphene, in absence of magnetic contaminants and strong intervalley mixing. The time-dependent spin polarization of propagating wavepacket is computed using an efficient quantum transport method. In the limit of vanishing effects of substrate and disorder, the energy-dependence of spin lifetime is similar to monolayer graphene with a M-shape profile and minimum value at the charge neutrality point, but with an electron-hole asymmetry fingerprint. In sharp contrast, the incorporation of substrate-induced electron-hole puddles (characteristics of supported graphene either on SiO2 orhBN) surprisingly results in a large enhancement of the low-energy spin lifetime and a lowering of its high-energy values. Such feature, unique to bilayer, is explained in terms of a reinforced Dyakonov-Perel mechanism at the Dirac point, whereas spin relaxation at higher energies is driven by pure dephasing effects. This suggests further electrostatic control of the spin transport length scales in graphene devices.

cond-mat.mes-hall↗

arXiv2016

Spin Manipulation in Graphene by Chemically-Induced Sublattice Pseudospin Polarization

Spin manipulation is one of the most critical challenges to realize spin-based logic devices and spintronic circuits. Graphene has been heralded as an ideal material to achieve spin manipulation but so far new paradigms and demonstrators are limited. Here we show that certain impurities such as fluorine ad-atoms, which locally break sublattice symmetry without the formation of strong magnetic moment, could result in a remarkable variability of spin transport characteristics. The impurity resonance level is found to be associated with a long range sublattice pseudospin polarization, which by locally decoupling spin and pseudospin dynamics, provokes a huge spin lifetime electron-hole asymmetry. In the dilute impurity limit, spin lifetimes could be tuned electrostatically from hundred picoseconds to several nanoseconds, providing a protocol to chemically engineer an unprecedented spin device functionality.

cond-mat.mes-hall↗

arXiv2015

Spin Dynamics and Relaxation in Graphene Dictated by Electron-hole Puddles

The understanding of spin dynamics and relaxation mechanisms in clean graphene and the upper time and length scales on which spin devices can operate are prerequisites to realizing graphene spintronic technologies. Here we theoretically reveal the nature of fundamental spin relaxation mechanisms in clean graphene on different substrates with spin-orbit Rashba fields as low as a few tens of micron eV. Spin lifetimes ranging from 50 picoseconds up to several nanoseconds are found to be dictated by substrate-induced electron-hole characteristics. A crossover in the spin relaxation mechanism from a Dyakonov-Perel type for SiO2 substrates to a broadening-induced dephasing for hBN substrates is described. The energy dependence of spin lifetimes, their ratio for spins pointing out-of-plane and in-plane, and the scaling with disorder provide a global picture about spin dynamics and relaxation in ultraclean graphene in presence of electron-hole puddles.

cond-mat.mes-hall↗

arXiv2015

Anomalous Ballistic Transport in Disordered Bilayer Graphene: Dimer Vacancies induced Dirac Semimetal

We report anomalous quantum transport features in bilayer graphene in presence of a random distribution of structural vacancies. By using an efficient real-space Kubo-Greenwood transport methodology, the impact of a varying density of dimer versus non-dimer vacancies is investigated in very large scale disordered models. While non-dimer vacancies are shown to induce localization regimes, dimer vacancies result in an unexpected ballistic regime whose energy window surprisingly enlarges with increasing impurity density. Such counterintuitive phenomenon is explained by the formation of an effective linear dispersion in the bilayer bandstructure, which roots in the symmetry breaking effects driven by dimer vacancies, and provides a novel realization of Dirac semimetals in high dimension.

cond-mat.mes-hall↗