arXiv subjects

Dmitry Smirnov

Publications and source records attributed to Dmitry Smirnov.

At least 55 records · Page 3Linked to original sources

arXiv2020

Gate-tunable exciton-polaron Rydberg series with strong roton effect

The electronic exciton polaron is a hypothetical many-body quasiparticle formed by an exciton dressed with a polarized electron-hole cloud in the Fermi sea (FS). It is predicted to display rich many-body physics and unusual roton-like dispersion. Exciton polarons were recently evoked to explain the excitonic spectra of doped monolayer transition metal dichalcogenides (TMDs), but these studies are limited to the ground state. Excited-state exciton polarons can exhibit richer many-body physics due to their larger spatial extent, but detection is challenging due to their inherently weak signals. Here we observe gate-tunable exciton polarons for the 1s - 3s excitonic Rydberg series in ultraclean monolayer MoSe$_2$ devices by optical spectroscopy. When the FS expands, we observe increasingly severe suppression and steep energy shift from low to high Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Notably, the exciton-polaron absorption and emission bands are separated with an energy gap, which increases from ground to excited state. Such peculiar characteristics are attributed to the roton-like exciton-polaron dispersion, where energy minima occur at finite momenta. The roton effect increases from ground to excited state. Such exciton-polaron Rydberg series with progressively significant many-body and roton effect shall provide a new platform to explore complex many-body phenomena.

cond-mat.mes-hall↗

arXiv2019

Giant Valley-Zeeman Splitting from Spin-Singlet and Spin-Triplet Interlayer Excitons in WSe2/MoSe2 Heterostructure

Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and triplet interlayer excitons show giant valley-Zeeman splitting between the K and K' valleys, a result of the large Lande g-factor of the singlet interlayer exciton and triplet interlayer exciton, which are experimentally determined to be ~ 10.7 and ~ 15.2, respectively, in good agreement with theoretical expectation. The PL from the singlet and triplet interlayer excitons show opposite helicities, determined by the atomic registry. Helicity-resolved photoluminescence excitation (PLE) spectroscopy study shows that both singlet and triplet interlayer excitons are highly valley-polarized at the resonant excitation, with the valley polarization of the singlet interlayer exciton approaches unity at ~ 20 K. The highly valley-polarized singlet and triplet interlayer excitons with giant valley-Zeeman splitting inspire future applications in spintronics and valleytronics.

cond-mat.mes-hall↗

arXiv2019

Electrically controlled emission from triplet charged excitons in atomically thin heterostructures

Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular momentum to interlayer excitons, enabling emission from otherwise dark spin-triplet excitons. Employing magnetic field, we show that photons emitted by triplet and singlet excitons in the same valley have opposite chirality. We also measure effective exciton g-factors, presenting direct and quantitative evidence of triplet interlayer excitons. We further demonstrate gate tuning of the relative photoluminescence intensity between singlet and triplet charged excitons. Electrically controlled emission between singlet and triplet excitons enables a route for optoelectronic devices that can configure excitonic chiral, spin, and valley quantum states.

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arXiv2019

Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon

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. Interestingly, the intervalley exciton is brightened through the emission of a chiral phonon at the corners of the Brillouin zone (K point), and the pseudoangular momentum (PAM) of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be ~ 23 meV, based on the experimentally extracted exchange interaction (~ 7 meV), in excellent agreement with the theoretical expectation of 24.6 meV. The long-lived intervalley exciton with valley degree of freedom adds an exciting quasiparticle for valleytronics, and the coupling between the chiral phonon and intervalley exciton furnishes a venue for valley spin manipulation.

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arXiv2019

Probing the Electronic Structure of Graphene Near and Far from the Fermi Level via Planar Tunneling Spectroscopy

Scanning tunneling spectroscopy (STS) has yielded significant insight on the electronic structure of graphene and other two-dimensional (2D) materials. STS directly measures a fundamental and directly calculable quantity: the single particle density of states (SPDOS). Due to experimental setup limitations, however, STS has been unable to explore 2D materials in ultra-high magnetic fields where electron-electron interactions can drastically change the SPDOS. Recent developments in the assembly of heterostructures composed of graphene and hexagonal boron nitride have enabled a device-based alternative to potentially overcome these roadblocks. Thus far, however, these nascent efforts are incomplete in analyzing and understanding tunneling spectra and have yet to explore graphene at high magnetic fields. Here we report an experiment at magnetic fields up to 18 T that uses graphene tunneling field effect transistors (TFETs) to establish a clear benchmark for measurement and analysis of graphene planar tunneling spectroscopy. We acquire gate tunable tunneling spectra of graphene and then use these data and electrostatic arguments to develop a systematic analysis scheme. This analysis reveals that TFET devices directly probe electronic structure features near and far from the Fermi level. In particular, our study yields identification of the Dirac point and numerous Landau levels as they fill and empty with charge via application of a gate voltage. Our work demonstrates that TFET devices are a viable platform for directly probing the electronic structure of graphene and other 2D materials in high magnetic fields, where novel electronic states emerge.

cond-mat.mes-hall↗

arXiv2019

Dirac energy spectrum and inverted band gap in metamorphic InAsSb/InSb superlattices

A Dirac-type energy spectrum was demonstrated in gapless ultra-short-period metamorphic InAsSb/InSb superlattices by angle-resolved photoemission spectroscopy (ARPES_ measurements. The Fermi velocity value 7.4x10^5 m/s in a gapless superlattice with a period of 6.2nm is in a good agreement with the results of magneto-absorption experiments. An "inverted" bandgap opens in the center of the Brillouin zone at higher temperatures and in the SL with a larger period. The ARPES data indicate the presence of a surface electron accumulation layer

cond-mat.mtrl-sci↗

arXiv2019

Direct Observation of Gate Tunable Dark Trions in Monolayer WSe2

Spin-forbidden intravalley dark exciton in tungsten-based transition metal dichalcogenides (TMDCs), owing to its unique spin texture and long lifetime, has attracted intense research interest. Here, we show that we can control the dark exciton electrostatically by dressing it with one free electron or free hole, forming the dark trions. The existence of the dark trions is suggested by the unique magneto-photoluminescence spectroscopy pattern of the boron nitride (BN) encapsulated monolayer WSe2 device at low temperature. The unambiguous evidence of the dark trions is further obtained by directly resolving the radiation pattern of the dark trions through back focal plane imaging. The dark trions possess binding energy of ~ 15 meV, and it inherits the long lifetime and large g-factor from the dark exciton. Interestingly, under the out-of-plane magnetic field, dressing the dark exciton with one free electron or hole results in distinctively different valley polarization of the emitted phonon, a result of the different intervalley scattering mechanism for the electron and hole. Finally, the lifetime of the positive dark trion can be further tuned from ~ 50 to ~ 215 ps by controlling the gate voltage. The gate tunable dark trions ushers in new opportunities for excitonic optoelectronics and valleytronics.

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.

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arXiv2019

Melting of charge order in the low-temperature state of an electronic ferroelectric

Strong electronic interactions can drive a system into a state with a symmetry breaking. Lattice frustration or competing interactions tend to prevent a symmetry breaking, leading to quantum disordered phases. In spin systems frustration can produce a spin liquid state. Frustration of a charge degree of freedom also can result in various exotic states, however, experimental data on these effects is scarce. In this work we demonstrate how a charge ordered ferroelectric looses the order on cooling to low temperatures using an example of a Mott insulator on a weakly anisotropic triangular lattice $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl. Typically, a low temperature ordered state is a ground state of a system, and the demonstrated re-entrant behavior is unique. Raman scattering spectroscopy finds that this material enters an insulating ferroelectric `dipole solid' state at $T=30~K$, but below $T=15~K$ the order melts, while preserving the insulating energy gap. The resulting phase diagram is relevant to other quantum paraelectric materials.

cond-mat.str-el↗

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.

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arXiv2019

Emerging Photoluminescence from the Dark-Exciton Phonon Replica in Monolayer WSe2

Tungsten-based monolayer transition metal dichalcogenides host a long-lived dark exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E" phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin.

cond-mat.mes-hall↗

arXiv2019

Enhanced Optoelectronic Response in Bilayer Lateral Heterostructures of Transition Metal Dichalcogenides

Two-dimensional lateral heterojunctions are basic components for low-power and flexible optoelectronics. In contrast to monolayers, devices based on few-layer lateral heterostructures could offer superior performance due to their lower susceptibility to environmental conditions. Here, we report the controlled synthesis of multi-junction bilayer lateral heterostructures based on MoS2-WS2 and MoSe2-WSe2, where the hetero-junctions are created via sequential lateral edge-epitaxy that happens simultaneously in both the first and the second layer. With respect to their monolayer counterparts, bilayer lateral heterostructures yield nearly one order of magnitude higher rectification currents. They also display a clear photovoltaic response, with short circuit currents ~103 times larger than those extracted from the monolayers, in addition to room-temperature electroluminescence. The superior performance of bilayer heterostructures significantly expands the functionalities of 2D crystals.

cond-mat.mtrl-sci↗

arXiv2019

Luminescent emission of excited Rydberg excitons from monolayer WSe2

We report the experimental observation of radiative recombination from Rydberg excitons in a two-dimensional semiconductor, monolayer WSe2, encapsulated in hexagonal boron nitride. Excitonic emission up to the 4s excited state is directly observed in photoluminescence spectroscopy in an out-of-plane magnetic field up to 31 Tesla. We confirm the progressively larger exciton size for higher energy excited states through diamagnetic shift measurements. This also enables us to estimate the 1s exciton binding energy to be about 170 meV, which is significantly smaller than most previous reports. The Zeeman shift of the 1s to 3s states, from both luminescence and absorption measurements, exhibits a monotonic increase of g-factor, reflecting nontrivial magnetic-dipole-moment differences between ground and excited exciton states. This systematic evolution of magnetic dipole moments is theoretically explained from the spreading of the Rydberg states in momentum space.

cond-mat.mes-hall↗

arXiv2019

Gate tunable dark trions in monolayer WSe$_2$

We report the observation and gate manipulation of intrinsic dark trions in monolayer WSe$_2$. By using ultraclean WSe$_2$ devices encapsulated by boron nitride, we directly resolve the weak photoluminescence of dark trions. The dark trions can be tuned continuously between negative and positive charged trions with electrostatic gating. We also reveal their spin triplet configuration and distinct valley optical emission by their characteristic Zeeman splitting under magnetic field. The dark trions exhibit large binding energy (14-16 meV). Their lifetime (~1.3 ns) is two orders of magnitude longer than the bright trion lifetime (~10 ps) and can be tuned between 0.4 to 1.3 ns by electrostatic gating. Such robust, optically detectable, and gate tunable dark trions provide a new path to realize electrically controllable trion transport in two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2019

Quantum Parity Hall effect in ABA Graphene

The celebrated phenomenon of quantum Hall effect has recently been generalized from transport of conserved charges to that of other approximately conserved state variables, including spin and valley, which are characterized by spin- or valley-polarized boundary states with different chiralities. Here, we report a new class of quantum Hall effect in ABA-stacked graphene trilayers (TLG), the quantum parity Hall (QPH) effect, in which boundary channels are distinguished by even or odd parity under the systems mirror reflection symmetry. At the charge neutrality point and a small perpendicular magnetic field $B_{\perp}$, the longitudinal conductance $σ_{xx}$ is first quantized to $4e^2/h$, establishing the presence of four edge channels. As $B_{\perp}$ increases, $σ_{xx}$ first decreases to $2e^2/h$, indicating spin-polarized counter-propagating edge states, and then to approximately $0$. These behaviors arise from level crossings between even and odd parity bulk Landau levels, driven by exchange interactions with the underlying Fermi sea, which favor an ordinary insulator ground state in the strong $B_{\perp}$ limit, and a spin-polarized state at intermediate fields. The transitions between spin-polarized and unpolarized states can be tuned by varying Zeeman energy. Our findings demonstrate a topological phase that is protected by a gate-controllable symmetry and sensitive to Coulomb interactions.

cond-mat.mes-hall↗

arXiv2018

Narrow photoluminescence peak of epitaxial MoS$_2$ on graphene/Ir(111)

We report on the observation of photoluminescence (PL) with a narrow 18 meV peak width from molecular beam epitaxy grown MoS$_2$ on graphene/Ir(111). This observation is explained in terms of a weak graphene-MoS$_2$ interaction that prevents PL quenching expected for a metallic substrate. The weak interaction of MoS$_2$ with the graphene is highlighted by angle-resolved photoemission spectroscopy and temperature dependent Raman spectroscopy. These methods reveal that there is no hybridization between electronic states of graphene and MoS$_2$ and a different thermal expansion of graphene and MoS$_2$. Molecular beam epitaxy grown MoS2 on graphene is therefore an important platform for optoelectronics which allows for large area growth with controlled properties.

cond-mat.mes-hall↗

arXiv2018

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2

Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to identify the biexciton state in BN encapsulated single-layer WSe2. The biexciton state only exists in charge neutral WSe2, which is realized through the control of efficient electrostatic gating. In the lightly electron-doped WSe2, one free electron binds to a biexciton and forms the trion-exciton complex. Improved understanding of the biexciton and trion-exciton complexes paves the way for exploiting the many-body physics in TMDs for novel optoelectronics applications.

cond-mat.mes-hall↗

arXiv2018

Chiral Landau levels in Weyl semimetal NbAs with multiple topological carriers

Recently, Weyl semimetals have been experimentally discovered in both inversion-symmetry-breaking and time-reversal-symmetry-breaking crystals. The non-trivial topology in Weyl semimetals can manifest itself with exotic phenomena which have been extensively investigated by photoemission and transport measurements. Despite the numerous experimental efforts on Fermi arcs and chiral anomaly, the existence of unconventional zeroth Landau levels, as a unique hallmark of Weyl fermions which is highly related to chiral anomaly, remains elusive owing to the stringent experimental requirements. Here, we report the magneto-optical study of Landau quantization in Weyl semimetal NbAs. High magnetic fields drive the system towards the quantum limit which leads to the observation of zeroth chiral Landau levels in two inequivalent Weyl nodes. As compared to other Landau levels, the zeroth chiral Landau level exhibits a distinct linear dispersion in z momentum direction and allows the optical transitions without the limitation of zero z momentum or square root of magnetic field evolution. The magnetic field dependence of the zeroth Landau levels further verifies the predicted particle-hole asymmetry of the Weyl cones. Meanwhile, the optical transitions from the normal Landau levels exhibit the coexistence of multiple carriers including an unexpected massive Dirac fermion, pointing to a more complex topological nature in inversion-symmetry-breaking Weyl semimetals. Our results provide insights into the Landau quantization of Weyl fermions and demonstrate an effective tool for studying complex topological systems.

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