Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopy
arXiv:2207.06517 · doi:10.1002/adma.202107104
Abstract
Electronic states and their dynamics are of critical importance for electronic and optoelectronic applications. Here, we probe various relevant electronic states in monolayer MoS2, such as multiple excitonic Rydberg states and free-particle energy bands, with a high relative contrast of up to >200 via broadband (from ~1.79 to 3.10 eV) static third-harmonic spectroscopy, which is further supported by theoretical calculations. Moreover, we introduce transient third-harmonic spectroscopy to demonstrate that third-harmonic generation can be all-optically modulated with a modulation depth exceeding ~94% at ~2.18 eV, providing direct evidence of dominant carrier relaxation processes, associated with carrier-exciton and carrier-phonon interactions. Our results indicate that static and transient third-harmonic spectroscopies are not only promising techniques for the characterization of monolayer semiconductors and their heterostructures, but also a potential platform for disruptive photonic and optoelectronic applications, including all-optical modulation and imaging.
arXiv comment17 pages, 4 figures
References in corpus (22)
- Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
- Excitons in atomically thin transition metal dichalcogenides
- Moiré Excitons in Van der Waals Heterostructures
- Tightly bound excitons in monolayer WSe2
- Observation of Moiré Excitons in WSe2/WS2 Heterostructure Superlattices
- Probing Excitonic Dark States in Single-layer Tungsten Disulfide
- Observation of Intense Second Harmonic Generation from MoS Atomic Crystals
- Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
- Halide-Assisted Atmospheric Pressure Growth of Large WSe2 and WS2 Monolayer Crystals
- Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2
- Engineering symmetry breaking in two-dimensional layered materials
- Third harmonic generation in graphene and few-layer graphite films
- Broadband, electrically tuneable, third harmonic generation in graphene
- Gate tunable third-order nonlinear optical response of massless Dirac fermions in graphene
- Ultra-strong nonlinear optical processes and trigonal warping in MoS layers
- Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe
- Optical harmonic generation in monolayer group-VI transition metal dichalcogenides
- All-optical polarization and amplitude modulation of second-harmonic generation in atomically thin semiconductors
- Optical Selection Rule based on Valley-Exciton Locking for 2D Valleytronics
- Hot electrons modulation of third harmonic generation in graphene
- Dielectrics in a time-dependent electric field: a real-time approach based on density-polarization functional theory
- Pump-triple sum-frequency-probe spectroscopy of transition metal dichalcogenides