Atomically-engineered nonlinear photonics with two-dimensional layered material superlattices

Project Information

ATOP

Grant agreement ID: 834742

DOI

10.3030/834742

Project closed

EC signature date 23 July 2019

Start date 1 September 2019

End date 31 August 2025

Funded under

• EXCELLENT SCIENCE - European Research Council (ERC)

Total cost

€ 2 442 448,00

EU contribution

€ 2 442 448,00

Coordinated by

AALTO KORKEAKOULUSAATIO SR
Finland

Periodic Reporting for period 3 - ATOP (Atomically-engineered nonlinear photonics with two-dimensional layered material superlattices)

Reporting period: 2022-09-01 to 2024-02-29

Summary of the context and overall objectives of the project

Now, we have already passed the middle point of the project and have 1.6 years left. We almost finished most of the scientific objectives of this ambitious project.
In this project, we have addressed the following problems/issues:
Objective 1 (Enabling technology development): (1.1) Design methods of 2D material integrated silicon waveguides and optical fibers; (1.2) Fabrication method for large-scale (e.g. inkjet printing) of 2D crystals and their twisted structures; (1.3) a deterministic optical modification method of 2D materials (MoS2 & MoTe2); (1.4) Single-step chemical vapour deposition method for MoS2/WS2 vertical heterostructure superlattices.

Objective 2 (Development of novel nonlinear optical devices with two-dimensional van der Waals superlattices): (2.1) Efficient modulation with van der Waals heterostructures with plasmonics and twist angle; (2.2) Electrical control of interband resonant nonlinear optics in monolayer MoS2; (2.3) ultrafast transient sub-bandgap absorption of monolayer MoS2; (2.4) efficient photonic and optoelectronic devices with other hybrid materials in mixed-dimensional heterostructures (e.g. extreme nonlinear strong-field photoemission from carbon nanotubes; single-nanowire spectrometers).

Objective 3 (Development of novel nonlinear optical devices with 2DSs): (3.1) Second-order parametric generation for the first time in monolayer MoS2; (3.2) ultrahigh optical nonlinearity with optical fibres with embedded two-dimensional materials; (3.3) Terahertz emission from 1D materials; (3.4) Photon pair generation in 2D materials; (3.5) Mid-infrared analogue polaritonic reversed Cherenkov radiation; (3.6) Chirality logic gates with 2D materials.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

Objective 1 Enabling technology development:
(1.1) designed methods of 2D material integrated silicon waveguides and optical fibers (Opt. Lett. 47, 734 (2022); Light:Adv. Manu.4,14(2023)).
(1.2) Fabrication method for large-scale (e.g. inkjet printing) of 2D crystals and their twisted structures (Sci. Adv.6,eaba502 (2020); Nat. Comm.11,2153(2020)).
(1.3) Deterministic optical modification method of 2D materials (Adv. Mater. Interf.2002119(2021); Adv. Funct. Mater.33,2302051(2023); 2D Mater. 10,045018(2023)).

Objective 2 Development of novel nonlinear optical devices with two-dimensional van der Waals superlattices:
(2.1) we report efficient modulation with van der Waals heterostructures with plasmonics and twist angle (Adv. Mater. 32,1907105 (2020); Adv. Funct. Mater.34,2310365(2024)).
(2.2) We report the ultrafast transient absorption of monolayer molybdenum disulfide in its sub-bandgap region from ~0.86 µm to 1.4 µm (Light: Sci. & Appl.10,27 (2021)).
(2.3) We report on an ultracompact microspectrometer design based on a single compositionally engineered nanowire (Science 365, 1017 (2019)) and heterostructures (Science,378,296(2022); Nat. Comm. 15, 571 (2024)).
(2.4) We demonstrate the gate-tunable interband resonant four-wave mixing and sum-frequency generation in monolayer MoS2 (ACS Nano 14, 8442 (2020)).

Objective 3 Development of novel nonlinear optical devices with 2DSs:
(3.1) we demonstrate difference frequency generation down to atomic thickness in molybdenum disulfide for the first time (Nanoscale 12, 19638 (2020)).
(3.2) we report the direct growth of MoS2, a highly nonlinear two-dimensional material, onto the internal walls of a SiO2 optical fibre. By using the as-fabricated 25-cm-long fibre, both second- and third-harmonic generation could be enhanced by ~300 times compared with monolayer MoS2/silica. (Nat. Nano.15 987 (2020)).
(3.3) We report enhanced terahertz emission from mushroom shaped InAs nanowire network (Nanotechnology,33,085207(2022)).
(3.4) We demonstrate mid-infrared analogue polaritonic reversed Cherenkov radiation in 2D materials (Nat. Comm.14,2532(2023)).
(3.5) We report chirality logic gates with 2D materials (Sci. Adv.,8, 49 (2022); Appl. Phys. Lett.123,240501(2023)).

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

(1) A general fabrication method for wafer-scale inkjet printing of 2D crystals. This general formulation supports uniform deposition of 2D crystals and their derivatives, enabling scalable and even wafer-scale device fabrication, moving them closer to industrial-level additive manufacturing.
(2) A deterministic optical modification method to tune the topography and optical properties of monolayer MoS2. The findings improve the applicability of monolayer transition metal dichalcogenides and shed light on modifying their physical properties.
(3) A fabrication strategy to precisely control the interlayer twist angle in large scale MoS2 homostructures. Our work provides a firm basis for the development of twistronics.
(4) A single-step chemical vapour deposition method for MoS2/WS2vertical heterostructure superlattices. This strategy for synthesizing anti-pyramid structures unveils a new synthesis route for the products of two-dimensional heterostructures and their devices for application.
(5) Efficient all-optical plasmonic modulation with van der Waals heterostructures. Plasmonic modulation of 44 cm−1 is demonstrated by an LED with light intensity down to 0.15 mW/cm2, which is four orders of magnitude smaller than the prevailing graphene nonlinear all‐optical modulators (≈103 mW/cm^2).
(6) Electrical control of interband resonant nonlinear optics in monolayer MoS2 for the first time. Up to 80% modulation depth in four-wave mixing is achieved when the generated signal is resonant with the A exciton at room temperature, corresponding to an effective third-order optical nonlinearity tuning.
(7) Ultrafast transient sub-bandgap absorption of monolayer MoS2. Our results elucidate the fundamental understanding regarding the optical properties, excited carrier states, and carrier dynamics in the technologically important near-infrared region, which potentially leads to various photonic and optoelectronic applications of 2D materials and their heterostructures.
(8) We report on an ultracompact microspectrometer design based on a single compositionally engineered nanowire. Our devices are capable of accurate, visible-range monochromatic and broadband light reconstruction, as well as spectral imaging.
(9) Second-order parametric generation for the first time in monolayer MoS2. mixing femtosecond optical pulses at wavelength of 406 nm with tunable pulses, we generate tunable pulses across the spectral range of 550–590 nm with frequency conversion efficiency up to ∼2 × 10^−4.
(10) We report a high-performance computational spectrometer based on a single van der Waals junction with an electrically tunable transport-mediated spectral response. We achieve high peak wavelength accuracy (∼0.36 nm), high spectral resolution (∼3 nm), broad operation bandwidth (from ∼405 to 845 nm), and proof-of-concept spectral imaging.
(11) We propose polaritonic negative refraction as a promising platform for infrared applications such as electrically tunable super-resolution imaging, Nanoscale thermal manipulation, enhanced molecular sensing, and on-chip optical circuitry.
(12) We also validate the unique advantages of chirality gates by realizing multiple gates with simultaneous operation in a single device and electrical control. Our first demonstrations of logic gates using chiral selection rules suggest that optical chirality could provide a powerful degree of freedom for future optical computing.

The photo about the optical modification of topographical and properties of monolayer 2D materials