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Laboratory of the Spin Physics of Two-Dimensional Materials

Contract number
075-15-2021-598
Time span of the project
2021-2023

As of 01.11.2022

9
scientific publications
General information

Emerging goals of nanophotonics, optoelectronics and quantum technologies for processing and storage of information require the use of new materials. The project is devoted to the study of three emerging materials with extreme two-dimensionality: colloidal semiconductor nanoplatelets, monatomic layers of transition metal dichalcogenides and two-dimensional perovskites. These materials have common properties that make them attractive for both basic science and applications. These are large exciton binding energy of several tens and hundreds of millielectronvolts, high efficiency of luminescence in the visible and near-infrared range, an important role of the surface and the possibility of its functionalization, relatively simple synthesis of structures which does not require expensive equipment. Optical experimental methods will be used to study spin-dependent phenomena and nonlinear optical properties.

Name of the project: Spin physics of two-dimensional materials: colloidal nanoplatelets, transition metal dichalcogenides and perovskites

Goals and objectives

The main goal of the project is to develop spin physics of new two-dimensional materials. Application of known and development of new optical spectroscopy methods for investigation of spin-dependent effects, spin structure and spin dynamics of charge carriers and exciton complexes. Study of the role of extreme two-dimensionality, dielectric confinement, surface in two-dimensional materials and corresponding hybrid structures. Search for effects applicable in nanophotonics, optoelectronic devices and quantum information technologies. The Laboratory of Spin Physics of Two-Dimensional Materials will be established in P.N. Lebedev Physical Institute under the supervision of D.R. Yakovlev, an expert in spin physics of semiconductor nanostructures, who has extensive experience in organizing scientific research and international scientific cooperation. The goal is to set it as a world-class scientific center.

The practical value of the study

Scientific results:

  • Our researchers have determined the principal spin parameters of the CsPbBr3 perovskite nanocrystal: g factors of the electron and the hole, the spin dephasing times, the  longitudinal spin relaxation time.
  • In nanocrystals of CsPb(Cl,Br)3 perovskites in the matrix of fluorophosphate glass we have found a state with a very low value of the g factor (~0,07) related to the spatially indirect exciton. This state is characterized by a record-high longitudinal spin relaxation for perovskites that reaches a millisecond.
  • We have studied the main optical and spin parameters of hybrid organic-inorganic monocrystals of FA0.9Cs0.1PbI2.8Br0.2 perovskites. We measured the g factors and the spin dephasing times of the electrons and holes, investigated the ultra-thin interaction of electron (hole) and nuclear spins, demonstrated the dynamic nuclear polarization. It has been found that the nuclear field influencing electrons and holes have opposite signs and an ultra-thin interaction of nuclear spins and with electron spins is significantly weaker than with hole spins. We have researched longitudinal spin relaxation and determined the value of Т1, which reaches 80 ns.
  • In the two-dimensional perovskite (PEA)2PbI4 we have found intense photoluminescence that consists of several lines. Some lines are supposedly  attributed to excitons and trions. We have determined the g factors of the excitonic and the trionic component, g=-0.35 and 1.05 respectively. We have found the effect of linear arrangement for the excitonic component of photoluminescence and its dependence on the magnetic field in the case of the Voigt geometry.
  • Our researchers have determined the g factors of colloid nanoparticles of three and four monolayers (1.9 and 1.8 respectively  at room temperature). It has been shown that the  g factors slightly increase when the temperature increases: by 0.1 when the temperature changes from 10 to 300 К. We have determined the dephasing times of the T2* spin ensemble responsible for the attenuation of spin precession around the magnetic field. It has been found that the time of longitudinal spin relaxation T1 exceeds 10 ns even at room temperature.
  • We have mastered the production of monolayers of dichalcogenides of transition metals with high (thousands and tens of thousands μm2) area by delamination via a metallic mediator, the assemble of heterostructures of them, express photolithography on these materials. Since many of these materials decomposed in the air, we have assembled a device for the creation of heterostructures in a glove box, thus, in fact, creating competences that are unique in Russia.
  • We have assembled and characterized a microresonator made of macroscopic dielectric Bragg mirrors with a monolayer of WSe2 as the active medium. The disalignment between the photonic and the excitonic mode can be controlled using piezoelectric nanopositioners. In the case of non-resonance  photoexcitation,  in the luminescence spectrum of the microresonator it is possible to observe a lower polariton branch and radiation on the photonic mode in the weak coupling mode.
  • In a monolayer of MoS2 we have researched the spatiotemporal dynamics of free and bound excitons, it has been found that bound excitons have higher lifetimes (up to 1 μs) compared to free excitons (up to 30 ps). The propagation of bound excitons has a subdiffusional nature, while free excitons at room temperature have a diffusional natture of propagation. The behavior of bound excitons can be explained by a model based on accounting for Auger recombination of excitons.
  • Our researchers have developed a picoacoustic methodology for probing the elastic properties of two-dimensional crystals and heterostructures based on them, which was applied to structures with boron nitride and WSe2. We demonstrated the possibility of determining the number of monolayers and the two-dimensional mapping using this methodology. We demonstrated the high acoustic Q factor of the researched  heterostructures, which means that these structures are promising for acoustic field concentration.
Education and career development:

One Doctor of Sciences and 2 Candidate of Sciences dissertations have been prepared and defended.

Postgraduate students of the Lebedev Physical Institute of the Russian Academy of Sciences have completed an internship at the leading scientist’s laboratory at TU Dortmund.

Collaborations:

  • TU Dortmund (Germany): joint research, visits by employees.
  • Ghent University (Belgium), ETH Zurich (Switzerland), Sorbonne University (France), ITMO University (Russia): production of samples for research.
  • Ioffe Institute, Saint Petersburg State University (Russia): joint research. 

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p.s. grigoryev, v.v. belykh, d.r. yakovlev, e. lhuillier, and m. bayer.
Coherent Spin Dynamics of Electrons and Holes in CsPbBr3 Colloidal Nanocrystals. Nano Lett. 2021 (21, 8481).
v. v. belykh, a. r. korotneva, and d. r. yakovlev.
Stimulated Resonant Spin Amplification Reveals Millisecond Electron Spin Coherence Time of Rare-Earth Ions in Solids. Phys. Rev. Lett. 2021 (127, 157401).
e. kirstein, d.r. yakovlev, m.m. glazov, e. evers, e.a. zhukov, v.v. belykh, n.e. kopteva, d. kudlacik, o. nazarenko, d.n. dirin, m.v. kovalenko, m. bayer
Lead-Dominated Hyperfine Interaction Impacting the Carrier Spin Dynamics in Halide Perovskites. Adv. Mater. 2021 (2105263).
m.v. pugachev, a.i. duleba, a.a. galiullin and a.y. kuntsevich.
Micromask Lithography for Cheap and Fast 2D Materials Microstructures Fabrication. Micromachines 2021 (12 (8), 850).
m. a. akmaev, m. m. glazov, m. v. kochiev, p. v. vinokurov, s. a. smagulova, and v. v. belykh
Spatiotemporal dynamics of free and bound excitons in CVD-grown MoS2 monolayer. Appl. Phys. Lett. 2021 (119, 113102).
v. v. belykh, m. l. skorikov, e. v. kulebyakina, e. v. kolobkova, m. s. kuznetsova, m. m. glazov, d. r. yakovlev
Submillisecond Spin Relaxation in CsPb(Cl,Br)3 Perovskite Nanocrystals in a Glass Matrix. Nano Lett. 2022, (22, 4583).
v. s. krivobok, e. a. ekimov, m. v. kondrin, s. n. nikolaev, m. a. chernopitssky, a. a. deeva , d. a. litvinov, and i. i. minaev.
Tin disulfide with bright near-IR luminescence centers obtained at high pressures. Phys. Rev. Mat. 2022 (6, 094605).
v. v. belykh and s. r. melyakov.
Selective measurement of the longitudinal electron spin relaxation time T1 of Ce3+ ions in a YAG lattice: Resonant spin inertia. Phys. Rev. B 2022 (105, 205129).
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