arXiv subjects

Andrea Balocchi

Publications and source records attributed to Andrea Balocchi.

14 recordsLinked to original sources

arXiv2026

Room temperature valley coherence in monolayer WSe2 mediated by chiral nematic liquid crystal

Valley coherence refers to a phase-coherent superposition of inequivalent momentum valleys, in which quantum information can be encoded in the relative valley phase. Chiral nematic liquid crystals, by imposing a flip of the spin angular momentum upon light reflection, provide an effective photonic environment for optically coupling excitons of the K and K' valleys in monolayer semiconducting transition-metal dichalcogenides. We experimentally demonstrate that using such liquid crystal as a substrate, it is possible through nearfield interaction to engineer a room temperature mechanism for inducing the intervalley coupling. Our results show that this approach provides a simple and scalable route toward valleytronic functionalities based on controlled coherent emission from valleys with opposite Berry curvature.

physics.optics↗

arXiv2026

Entangled Telecom Photon Generation using Twisted Van der Waals Crystals

Nanoscale quantum light sources are essential building blocks for integrated quantum photonic systems. Here, we report a wavelength-scale entangled-photon source based on van der Waals-engineered NbOBr$_2$, and benchmark its performance for telecom-wavelength quantum light generation. By exploiting the material's second-order nonlinearity, we generate quantum-correlated photon pairs via spontaneous parametric down-conversion. We then use a 90$^{\circ}$ twisted stacking to induce quantum interference in photon-pair generation, yielding polarization-entangled photons. This approach enables tunability of the quantum optical state via control of the excitation laser polarization. We experimentally obtain entanglement fidelities exceeding 95% for Bell states, along with a high coincidence-to-accidental ratio of $\sim$335, and a brightness approximately one order of magnitude higher than recently reported telecom sources based on transition metal dichalcogenide (TMD) 2D materials. These results establish twisted van der Waals engineering as a powerful platform for highly tunable, high-brightness quantum light sources at telecom wavelengths.

physics.optics↗

arXiv2025

Thermal assisted transport of biexcitons in monolayer WSe2

Studies of excitonic transport in transition metal dichalcogenide monolayers have attracted increasing interest in recent years in order to develop nano-optoelectronic devices made with 2D materials. These studies began with low to moderate optical excitation regimes, and more recently have focused on high injection regimes where nonlinear effects appear. This article is focused on the transport of biexcitons by spatially and temporally resolved photoluminescence spectroscopy at high excitation flux. The study is carried out on a high-quality WSe$_2$ monolayer encapsulated in hexagonal boron nitride. The results show that a Seebeck current affects transport in connection with the presence of hot biexcitons. In particular, we observe the formation of spatial rings, also called halos, which have been observed in other excitonic gases. These results tend to generalize the importance of high-energy populations in excitonic transport in TMD, even for complex and heavy excitonic particles.

cond-mat.mtrl-sci↗

arXiv2025

Carrier Thermalization and Biexciton Formation in a Polar ZnO/Zn$_{0.84}$Mg$_{0.16}$O Quantum Well Probed by Ultrafast Broadband Spectroscopy

We investigate the ultrafast dynamics of excitons in a 2.6 nm-thick $\mathrm{ZnO/Zn_{0.84}Mg_{0.16}O}$ quantum well grown on a c-axis sapphire substrate, using non-degenerate time-resolved pump-probe spectroscopy. A pump pulse at 266 nm generates photocarriers within the ZnMgO barriers, and their dynamics is monitored through time-resolved differential reflectance measurements using a supercontinuum probe spanning the 345-400 nm spectral range. Photocarriers generated in the barriers rapidly relax into the quantum well, where they form excitons within sub-picosecond timescales. These excitons quickly thermalize and become localized, likely due to interface disorder or well-width fluctuations, as supported by photoluminescence measurements showing a clear Stokes shift and the absence of free exciton emission. A phonon-assisted absorption process, leading to the effective thermalization of excitons, is observed and analyzed. We identify moreover a negative differential reflectance feature as a photoinduced absorption into a biexciton state, with a binding energy ranging from 18 to 22 meV depending on temperature.

cond-mat.mes-hall↗

arXiv2024

Using Light to Polarize and Detect Electron Spins in Silicon

Despite decades of research, demonstration of all-optical detection and control of free electron spins in silicon remains elusive. Here, we directly probe the electron spin properties in bulk silicon by measuring the polarization of luminescence following circularly polarized light excitation. The experiments performed for both direct and indirect gap excitation allow not only an experimental determination of the optical selection rules in silicon for the different phononassisted transitions but they also lead to the measurement of the spin relaxation of electrons in conditions which are not accessible using transport techniques. We also measure the spin properties of free excitons in bulk silicon, a very little explored field.

cond-mat.mtrl-sci↗

arXiv2021

Capacitively-coupled and inductively-coupled excitons in bilayer MoS$_2$

The interaction of intralayer and interlayer excitons is studied in a two-dimensional semiconductor, homobilayer MoS$_2$. It is shown that the measured optical susceptibility reveals both the magnitude and the sign of the coupling constants. The interlayer exciton interacts capacitively with the intralayer B-exciton (positive coupling constant) consistent with hole tunnelling from one monolayer to the other. Conversely, the interlayer exciton interacts inductively with the intralayer A-exciton (negative coupling constant). First-principles many-body calculations show that this coupling arises via an intravalley exchange-interaction of A- and B-excitons.

cond-mat.mes-hall↗

arXiv2021

Giant Stark splitting of an exciton in bilayer MoS$_2$

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to the quantum confined Stark effect, here the electron is localised to one of the layers yet the hole is delocalised across the bilayer. We optically probe the interaction between intra- and interlayer excitons as they are energetically tuned into resonance. This allows studying their mixing supported by beyond standard density functional theory calculations including excitonic effects. In MoS2 trilayers our experiments uncover two types of interlayer excitons with and without in-built electric dipoles, respectively. Highly tunable excitonic transitions with large oscillator strength and in-built dipoles, that lead to considerable exciton-exciton interactions, hold great promise for non-linear optics with polaritons.

cond-mat.mes-hall↗

arXiv2021

Interlayer exciton mediated second harmonic generation in bilayer MoS2

Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations.

cond-mat.mtrl-sci↗

arXiv2020

Magneto-optical determination of the carrier lifetime in coherent Ge(1-x)Sn(x)/Ge heterostructures

We present a magneto-optical study of the carrier dynamics in compressively strained Ge(1-x)Sn(x) films having Sn compositions up to 10% epitaxially grown on blanket Ge on Si (001) virtual substrates. We leverage the Hanle effect under steady-state excitation to study the spin-dependent optical transitions in presence of an external magnetic field. This allowed us to obtain direct access to the dynamics of the optically-induced carrier population. Our approach singled out that at cryogenic temperatures the effective lifetime of the photogenerated carriers in coherent Ge(1-x)Sn(x) occurs in the sub-ns time scale. Supported by a model estimate of the radiative lifetime, our measurements indicate that carrier recombination is dominated by non-radiative processes. Our results thus provide central information to advance the fundamental understanding of carrier kinetics in this novel direct-gap group-IV material system. Such knowledge can be a stepping stone in the quest for the implementation of Ge(1-x)Sn(x)-based functional devices.

physics.optics↗

arXiv2020

Electrical Detection of Light Helicity using a Quantum Dots based Hybrid Device at Zero Magnetic Field

Photon helicity-dependent photocurrent is measured at zero magnetic field on a device based on an ensemble of InGaAs/GaAs quantum dots that are embedded into a GaAs-based p-i-n diode. Our main goal is to take advantage of the long electron spin relaxation time expected in these nano-objects. In these experiments, no external magnetic field is required thanks to the use of an ultrathin magnetic CoFeB/MgO electrode, presenting perpendicular magnetic anisotropy (PMA). We observe a clear asymmetry of the photocurrent measured under respective right and left polarized light that follows the hysteresis of the magnetic layer. The amplitude of this asymmetry at zero magnetic field decreases with increasing temperatures and can be controlled with the bias. Polarization-resolved photoluminescence is detected in parallel while the device is operated as a photodetector. This demonstrates the multifunctional capabilities of the device and gives valuable insights into the spin relaxation of the electrons in the quantum dots.

physics.app-ph↗

arXiv2020

Mo Thio and Oxo-Thio Molecular Complexes Film as Self-Healing Catalyst for Photocatalytic Hydrogen Evolution on 2D Materials

2D semiconducting nanosheets of Transition Metal Dichalcogenides are attractive materials for solar energy conversion because of their unique absorption properties. Here, we propose Mo thio- and oxo-thio-complexes anchored on 2D p-WSe2 nanosheets for efficient water splitting under visible light irradiation with photocurrent density up to 2.0 mA cm-2 at -0.2 V/NHE. Besides developing high electro-catalytic activity, the Mo complexe films were shown to display ability to heal surface defects. We propose that the observed healing of surface defects arises from the strong adsorption on point defects of the 2D WSe2 substrate of Mo complexes such as (MoS4)2-, (MoOS3)2-, (Mo2S6O2)2- as shown from DFT calculations. In addition to display catalytic and healing effects, the thio-, oxo-thio Mo complexes films were shown to enhance charge carrier separation and migration for the hydrogen evolution reaction, thus representing an example of multicomponent passivation layer exhibiting multiple properties.

physics.app-ph↗

arXiv2019

Interlayer excitons in bilayer MoS2 with strong oscillator strength up to room temperature

Coulomb bound electron-hole pairs, excitons, govern the optical properties of semi-conducting transition metal dichalcogenides like MoS$_2$ and WSe$_2$. We study optical transitions at the K-point for 2H homobilayer MoS$_2$ in Density Functional Theory (DFT) including excitonic effects and compare with reflectivity measurements in high quality samples encapsulated in hexagonal BN. In both calculated and measured spectra we find a strong interlayer exciton transition in energy between A and B intralayer excitons, observable for T$=4 -300$ K, whereas no such transition is observed for the monolayer in the same structure in this energy range. The interlayer excitons consist of an electron localized in one layer and a hole state delocalized over the bilayer, which results in the unusual combination of high oscillator strength and a static dipole moment. We also find signatures of interlayer excitons involving the second highest valence band (B) and compare absorption calculations for different bilayer stackings. For homotrilayer MoS$_2$ we also observe interlayer excitons and an energy splitting between different intralayer A-excitons originating from the middle and outer layers, respectively.

cond-mat.mtrl-sci↗

arXiv2017

Carrier and Spin Coherent Dynamics in Strained Germanium-Tin Semiconductor on Silicon

Germanium-Tin is emerging as a material exhibiting excellent photonic properties. Here we demonstrate optical initialization and readout of spins in this intriguing group IV semiconductor alloy and report on spin quantum beats between Zeeman-split levels under an external magnetic field. Our optical experiments reveal robust spin orientation in a wide temperature range and a persistent spin lifetime that approaches the ns regime at room temperature. Besides important insights into nonradiative recombination pathways, our findings disclose a rich spin physics in novel epitaxial structures directly grown on a conventional Si substrate. This introduces a viable route towards the synergic enrichment of the group IV semiconductor toolbox with advanced spintronics and photonic capabilities.

cond-mat.mtrl-sci↗

arXiv2015

Optical orientation of electron spins and valence band spectroscopy in germanium

We have investigated optical orientation in the vicinity of the direct gap of bulk germanium. The electron spin polarization is studied via polarization-resolved photoluminescence excitation spectroscopy unfolding the interplay between doping and ultrafast electron transfer from the center of the Brillouin zone towards its edge. As a result, the direct-gap photoluminescence circular polarisation can vary from 30% to -60% when the excitation laser energy increases. This study provides also simultaneous access to the resonant electronic Raman scattering due to inter-valence band excitations of spin-polarized holes, yielding a fast and versatile spectroscopic approach for the determination of the energy spectrum of holes in semiconducting materials.

cond-mat.mes-hall↗