scholarly journals Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Erfu Liu ◽  
Jeremiah van Baren ◽  
Zhengguang Lu ◽  
Takashi Taniguchi ◽  
Kenji Watanabe ◽  
...  

AbstractExciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe2 and WSe2 gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because the trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe2 and WSe2.

Nanophotonics ◽  
2020 ◽  
Vol 9 (7) ◽  
pp. 1811-1829 ◽  
Author(s):  
Zhipeng Li ◽  
Tianmeng Wang ◽  
Shengnan Miao ◽  
Zhen Lian ◽  
Su-Fei Shi

AbstractMonolayer transitional metal dichalcogenides (TMDCs), a new class of atomically thin semiconductor, respond to optical excitation strongly with robust excitons, which stem from the reduced screening in two dimensions. These excitons also possess a new quantum degree of freedom known as valley spin, which has inspired the field of valleytronics. The strongly enhanced Coulomb interaction allows the exciton to bind with other particles to form new excitonic states. However, despite the discovery of trions, most of the excitonic states in monolayer TMDCs remain elusive until recently, when new light was shed into the fascinating excitonic fine structures with drastically improved sample quality through boron nitride encapsulation. Here, we review the latest research progress on fine structures of excitonic states in monolayer TMDCs, with a focus on tungsten-based TMDCs and related alloy. Many of the new excitonic complexes inherit the valley degree of freedom, and the valley-polarized dark excitonic states are of particular interest because of their long lifetime and possible long valley coherence time. The capability of resolving the excitonic fine structures also enables the investigation of exciton–phonon interactions. The knowledge of the interlayer between excitons and other particles not only advances our understanding of many-body effects in the monolayer TMDCs but also provides guidance on future applications based on TMDCs.


NANO ◽  
2021 ◽  
Author(s):  
Arslan Usman ◽  
Abdul Sattar ◽  
Hamid Latif ◽  
Muhammad Imran

The impact of phonon and their surrounding environment on exciton and its complexes were investigated in monolayer WSe2 semiconductor. Phonon up-conversion has been studied in past for conventional III–V semiconductors, but its role in two-dimensional layered transition metal dichalcogenides has rarely been explored. We investigated the photoluminescence up-conversion mechanism in WSe2 monolayer and found that a lower energy photon gain energy upto 64[Formula: see text]meV to be up-converted to emission photon at room temperature. Moreover, the phonon-exciton coupling mechanism has also been investigated and the role of dielectric screening has been explored to get complete insight of coulomb’s interaction in these electron-hole pairs. Investigations of charge carrier’s lifetime reveal that boron nitride encapsulated monolayer has shorter recombination time as low as 41 ps as compared to a bare monolayer on SiO2 substrate. These results are very promising for realizing spintronics-based application from two-dimensional layered semiconductors.


2020 ◽  
Vol 10 ◽  
pp. 184798042095509
Author(s):  
Ankit Kumar Verma ◽  
Federico Raffone ◽  
Giancarlo Cicero

Two-dimensional transition metal dichalcogenides have gained great attention because of their peculiar physical properties that make them interesting for a wide range of applications. Lately, alloying between different transition metal dichalcogenides has been proposed as an approach to control two-dimensional phase stability and to obtain compounds with tailored characteristics. In this theoretical study, we predict the phase diagram and the electronic properties of Mo xTi1− xS2 at varying stoichiometry and show how the material is metallic, when titanium is the predominant species, while it behaves as a p-doped semiconductor, when approaching pure MoS2 composition. Correspondingly, the thermodynamically most stable phase switches from the tetragonal to the hexagonal one. Further, we present an example which shows how the proposed alloys can be used to obtain new vertical two-dimensional heterostructures achieving effective electron/hole separation.


2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Chiara Trovatello ◽  
Florian Katsch ◽  
Nicholas J. Borys ◽  
Malte Selig ◽  
Kaiyuan Yao ◽  
...  

Abstract The equilibrium and non-equilibrium optical properties of single-layer transition metal dichalcogenides (TMDs) are determined by strongly bound excitons. Exciton relaxation dynamics in TMDs have been extensively studied by time-domain optical spectroscopies. However, the formation dynamics of excitons following non-resonant photoexcitation of free electron-hole pairs have been challenging to directly probe because of their inherently fast timescales. Here, we use extremely short optical pulses to non-resonantly excite an electron-hole plasma and show the formation of two-dimensional excitons in single-layer MoS2 on the timescale of 30 fs via the induced changes to photo-absorption. These formation dynamics are significantly faster than in conventional 2D quantum wells and are attributed to the intense Coulombic interactions present in 2D TMDs. A theoretical model of a coherent polarization that dephases and relaxes to an incoherent exciton population reproduces the experimental dynamics on the sub-100-fs timescale and sheds light into the underlying mechanism of how the lowest-energy excitons, which are the most important for optoelectronic applications, form from higher-energy excitations. Importantly, a phonon-mediated exciton cascade from higher energy states to the ground excitonic state is found to be the rate-limiting process. These results set an ultimate timescale of the exciton formation in TMDs and elucidate the exceptionally fast physical mechanism behind this process.


2020 ◽  
Vol 10 ◽  
pp. 184798042090256 ◽  
Author(s):  
Sara Postorino ◽  
Davide Grassano ◽  
Marco D’Alessandro ◽  
Andrea Pianetti ◽  
Olivia Pulci ◽  
...  

Thanks to the ultrahigh flexibility of 2D materials and to their extreme sensitivity to applied strain, there is currently a strong interest in studying and understanding how their electronic properties can be modulated by applying a uniform or nonuniform strain. In this work, using density functional theory (DFT) calculations, we discuss how uniform biaxial strain affects the electronic properties, such as ionization potential, electron affinity, electronic gap, and work function, of different classes of 2D materials from X-enes to nitrides and transition metal dichalcogenides. The analysis of the states in terms of atomic orbitals allows to explain the observed trends and to highlight similarities and differences among the various materials. Moreover, the role of many-body effects on the predicted electronic properties is discussed in one of the studied systems. We show that the trends with strain, calculated at the GW level of approximation, are qualitatively similar to the DFT ones solely when there is no change in the character of the valence and conduction states near the gap.


Nanoscale ◽  
2019 ◽  
Vol 11 (25) ◽  
pp. 12381-12387 ◽  
Author(s):  
Samuel Brem ◽  
Jonas Zipfel ◽  
Malte Selig ◽  
Archana Raja ◽  
Lutz Waldecker ◽  
...  

The reduced dielectric screening in atomically thin transition metal dichalcogenides allows to study the hydrogen-like series of higher exciton states in optical spectra even at room temperature.


2020 ◽  
Vol 5 (2) ◽  
pp. 331-335 ◽  
Author(s):  
Viviana Jehová González ◽  
Antonio M. Rodríguez ◽  
Ismael Payo ◽  
Ester Vázquez

Different 2D-layered materials of transition metal dichalcogenides (TMDCs) such as boron nitride (BN) or molybdenum disulphide (MoS2) have been theorised to have piezoelectric behaviour.


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