arXiv subjects

A. Balocchi

Publications and source records attributed to A. Balocchi.

At least 19 recordsLinked to original sources

arXiv2026

Spin-Valley Relaxation of Rydberg Excitons

Rydberg excitons, characterized by large spatial extension and reduced electron-hole overlap, must have a spin-valley dynamics different from that of ground state excitons. Here we report a direct measurement of spin relaxation of Rydberg excitons in high-quality WSe2 monolayer using continuous-wave and time-resolved optical orientation experiments. Excited excitonic states exhibit exceptionally large photoluminescence circular polarization, approaching 90% for the 3s state. Time-resolved measurements reveal a strong increase of the spin relaxation time with the principal quantum number, from ~2 ps for the 1s exciton to ~75 ps for the 3s exciton. A microscopic model based on electron-hole exchange-driven spin relaxation quantitatively reproduces the observed trend, demonstrating that Rydberg excitons enable tunable spin-valley dynamics in two-dimensional semiconductors.

cond-mat.other↗

arXiv2025

Exciton Formation in Two-Dimensional Semiconductors

The optical properties of atomically thin semiconductors are dominated by excitons, tightly bound electron-hole pairs, which give rise to particularly rich and remarkable physics. Despite their importance, the microscopic formation mechanisms of excitons remain very poorly understood due to the complex interplay of concurrent phenomena occurring on an ultrafast timescale. Here, we investigate the exciton formation processes in 2D materials based on transition metal dichalcogenide (TMD) monolayers using a technique based on the control of excitation light polarization. It allows us to distinguish between the two competing models of exciton formation: geminate and bimolecular formation. The geminate process is the direct formation of the exciton from the initially photogenerated electron hole pair before the loss of correlation between them, whereas the bimolecular process corresponds to the random binding of free electron hole-pairs from the initially photogenerated plasma. These processes control the exciton formation time. Our findings reveal that the luminescence intensity is higher by up to 40% for circularly polarized excitation compared to linearly polarized excitation for laser energy above the free carrier gap. We show that this spin-dependent exciton emission is a fingerprint of the bimolecular formation process. Importantly, we observe that exciton linear polarization (valley coherence) persists even for laser excitation energies exceeding the gap. We demonstrate that it is the result of a fraction of excitons formed by a geminate process. This shows that two formation processes coexist for excitation energies above the gap, where both mechanisms operate concurrently.

cond-mat.mtrl-sci↗

arXiv2024

Efficient Electron Spin Relaxation by Chiral Phonons in WSe$_2$ Monolayers

In transition metal dichalcogenide semiconductor monolayers the spin dynamics of electrons is controlled by the original spin-valley locking effect resulting from the interplay between spin-orbit interaction and inversion asymmetry. As a consequence, for electrons occupying bottom conduction bands, a carrier spin flip occurs only if there is a simultaneous change of valley. However, very little is known about the intra-valley spin relaxation processes. In this work we have performed stationary and time-resolved photoluminescence measurements in high quality WSe$_2$ monolayers. Our experiments highlight an efficient relaxation from bright to dark excitons, due to a fast intra-valley electron transfer from the top to the bottom conduction band with opposite spins. A combination of experiments and theoretical analysis allows us to infer a spin relaxation time of about $\tau_s\sim10~$ps, driven by the interplay between $\Gamma$-valley chiral phonons and spin-orbit mixing.

cond-mat.mes-hall↗

arXiv2024

Brightened emission of dark trions in transition-metal dichalcogenide monolayers

The optical emission spectra of semiconducting transition-metal dichalcogenide monolayers highlight fascinating recombination processes of charged excitons (trions). When charge tunable WSe$_2$ monolayers are moderately doped with electrons, a strong luminescence peak emerges just below the well-understood spectral lines associated with the recombination of negatively charged bright and dark trions. Despite previous investigations, its origin remains elusive. Here, we demonstrate that this luminescence peak is the result of electron-electron assisted recombination that brightens the dark trion emission. Supporting evidence for this second-order recombination process comes from identifying the brightened emission of positively charged dark trions when the monolayer is electrostatically doped with holes. Remarkably, the discovered hole-hole assisted luminescence peak emerges in the near infrared, about 500 meV below the well-studied spectral region of excitons and trions. In magneto-photoluminescence experiments we find that the $g$-factor of this new transition ($g$ = +4) has an opposite sign compared to the well-known $g$-factor of neutral or charged excitons. This allows us to propose a mechanism of brightening of the positively charged dark trion involving the $\Gamma$ valence band.

cond-mat.mes-hall↗

arXiv2022

Non-linear diffusion of negatively charged excitons in WSe2 monolayer

We investigate the diffusion process of negatively charged excitons (trions) in WSe2 transition metal dichalcogenide monolayer. We measure time-resolved photoluminescence spatial profiles of these excitonic complexes which exhibit a non-linear diffusion process with an effective negative diffusion behavior. Specifically, we examine the dynamics of the two negatively charged bright excitons (intervalley and intravalley trion) as well as the dark trion. The time evolution allows us to identify the interplay of different excitonic species: the trionic species appear after the neutral excitonic ones, consistent with a bimolecular formation mechanism. Using the experimental observations, we propose a phenomenological model suggesting the coexistence of two populations: a first one exhibiting a fast and efficient diffusion mechanism and a second one with a slower dynamics and a less efficient diffusion process. These two contributions could be attributed to hot and cold trion populations.

cond-mat.mtrl-sci↗

arXiv2022

Optical manipulation of the Rashba effect in germanium quantum wells

The Rashba effect in Ge/Si$_{0.15}$Ge$_{0.85}$ multiple quantum wells embedded in a p-i-n diode is studied through polarization and time-resolved photoluminescence. In addition to a sizeable redshift arising from the quantum-confined Stark effect, a threefold enhancement of the circular polarization degree of the direct transition is obtained by increasing the pump power over a 2kW/cm$^2$ range. This marked variation reflects an efficient modulation of the spin population and is further supported by dedicated investigations of the indirect gap transition. This study demonstrates a viable strategy to engineer the spin-orbit Hamiltonian through contactless optical excitation and opens the way towards the electro-optical manipulation of spins in quantum devices based on group-IV heterostructures.

cond-mat.mes-hall↗

arXiv2021

Machine learning assisted GaAsN circular polarimeter

We demonstrate the application of a two stage machine learning algorithm that enables to correlate the electrical signals from a GaAs$_x$N$_{1-x}$ circular polarimeter with the intensity, degree of circular polarization and handedness of an incident light beam. Specifically, we employ a multimodal logistic regression to discriminate the handedness of light and a 6-layer neural network to establish the relationship between the input voltages, the intensity and degree of circular polarization. We have developed a particular neural network training strategy that substantially improves the accuracy of the device. The algorithm was trained and tested on theoretically generated photoconductivity and on photoluminescence experimental results. Even for a small training experimental dataset (70 instances), it is shown that the proposed algorithm correctly predicts linear, right and left circularly polarized light misclassifying less than $1.5\%$ of the cases and attains an accuracy larger than $97\%$ in the vast majority of the predictions ($92\%$) for intensity and degree of circular polarization. These numbers are significantly improved for the larger theoretically generated datasets (4851 instances). The algorithm is versatile enough that it can be easily adjusted to other device configurations where a map needs to be established between the input parameters and the device response. Training and testing data files as well as the algorithm are provided as supplementary material.

cond-mat.other↗

arXiv2021

Chiral photodetector based on GaAsN

The detection of light helicity is key to several research and industrial applications from drugs production to optical communications. However, the direct measurement of the light helicity is inherently impossible with conventional photodetectors based on III-V or IV-VI semiconductors, being naturally non-chiral. The prior polarization analysis of the light by a series of often moving optical elements is necessary before light is sent to the detector. A method is here presented to effectively give to the conventional dilute nitride GaAs-based semiconductor epilayer a chiral photoconductivity in paramagnetic-defect-engineered samples. The detection scheme relies on the giant spin-dependent recombination of conduction electrons and the accompanying spin polarization of the engineered defects to control the conduction band population via the electrons' spin polarization. As the conduction electron spin polarization is, in turn, intimately linked to the excitation light polarization, the light polarization state can be determined by a simple conductivity measurement. This effectively gives the GaAsN epilayer a chiral photoconductivity capable of discriminating the handedness of an incident excitation light in addition to its intensity. This approach, removing the need of any optical elements in front of a non-chiral detector, could offer easier integration and miniaturisation. This new chiral photodetector could potentially operate in a spectral range from the visible to the infra-red using (In)(Al)GaAsN alloys or ion-implanted nitrogen-free III-V compounds.

physics.app-ph↗

arXiv2021

Polarization sensitive photodectector based on GaAsN

We propose and numerically simulate an optoelectronic compact circular polarimeter. It allows to electrically measure the degree of circular polarization and light intensity at room temperature for a wide range of incidence angles in a single shot. The device, being based on GaAsN, is easy to integrate into standard electronics and does not require bulky movable parts nor extra detectors. Its operation hinges mainly on two phenomena: the spin dependent capture of electrons and the hyperfine interaction between bound electrons and nuclei on Ga$^{2+}$ paramagnetic centers in GaAsN. The first phenomenon confers the device with sensitivity to the degree of circular polarization and the latter allows to discriminate the handedness of the incident light.

cond-mat.mes-hall↗

arXiv2019

Electron-nucleus spin correlation conservation of the spin dependent recombination in Ga$^{2+}$ centers

Spin dependent recombination in GaAsN offers many interesting possibilities in the design of spintronic devices mostly due to its astounding capability to reach conduction band electron spin polarizations close to 100% at room temperature. The mechanism behind the spin selective capture of electrons in Ga$^{2+}$ paramagnetic centers is revisited in this paper to address inconsistencies common to most previously presented models. Primarily, these errors manifest themselves as major disagreements with the experimental observations of two key characteristics of this phenomenon: the effective Overhauser-like magnetic field and the width of the photoluminescence Lorentzian-like curves as a function of the illumination power. These features are not only essential to understand the spin dependent recombination in GaAsN, but are also key to the design of novel spintronic devices. Here we demonstrate that the particular structure of the electron capture expressions introduces spurious electron-nucleus correlations that artificially alter the balance between the hyperfine and the Zeeman contributions. This imbalance strongly distorts the effective magnetic field and width characteristics. In this work we propose an alternative recombination mechanism that preserves the electron-nucleus correlations and, at the same time, keeps the essential properties of the spin selective capture of electrons. This mechanism yields a significant improvement to the agreement between experimental and theoretical results. In particular, our model gives results in very good accord with the experimental effective Overhauser-like magnetic field and width data, and with the degree of circular polarization under oblique magnetic fields.

cond-mat.mes-hall↗

arXiv2018

Exciton-phonon coupling in MoSe2 monolayers

We study experimentally and theoretically the exciton-phonon interaction in MoSe2 monolayers encapsulated in hexagonal BN, which has an important impact on both optical absorption and emission processes. The exciton transition linewidth down to 1 meV at low temperatures makes it possible to observe high energy tails in absorption and emission extending over several meV, not masked by inhomogeneous broadening. We develop an analytical theory of the exciton-phonon interaction accounting for the deformation potential induced by the longitudinal acoustic phonons, which plays an important role in exciton formation. The theory allows fitting absorption and emission spectra and permits estimating the deformation potential in MoSe2 monolayers. We underline the reasons why exciton-phonon coupling is much stronger in two-dimensional transition metal dichalcodenides as compared to conventional quantum well structures. The importance of exciton-phonon interactions is further highlighted by the observation of a multitude of Raman features in the photoluminescence excitation experiments.

cond-mat.mtrl-sci↗

arXiv2018

Electrically tunable dynamic nuclear spin polarization in GaAs quantum dots at zero magnetic field

In III-V semiconductor nano-structures the electron and nuclear spin dynamics are strongly coupled. Both spin systems can be controlled optically. The nuclear spin dynamics is widely studied, but little is known about the initialization mechanisms. Here we investigate optical pumping of carrier and nuclear spins in charge tunable GaAs dots grown on 111A substrates. We demonstrate dynamic nuclear polarization (DNP) at zero magnetic field in a single quantum dot for the positively charged exciton X$^+$ state transition. We tune the DNP in both amplitude and sign by variation of an applied bias voltage V$_g$. Variation of $Δ$V$_g$ of the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from -30 $μ$eV (-22 %) to +10 $μ$eV (+7 %), although the X$^+$ photoluminescence polarization does not change sign over this voltage range. This indicates that absorption in the structure and energy relaxation towards the X$^+$ ground state might provide favourable scenarios for efficient electron-nuclear spin flip-flops, generating DNP during the first tens of ps of the X$^+$ lifetime which is of the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments.

cond-mat.mes-hall↗

arXiv2018

Electrical initialization of electron and nuclear spins in a single quantum dot at zero magnetic field

The emission of circularly polarized light from a single quantum dot relies on the injection of carriers with well-defined spin polarization. Here we demonstrate single dot electroluminescence (EL) with a circular polarization degree up to 35% at zero applied magnetic field. The injection of spin polarized electrons is achieved by combining ultrathin CoFeB electrodes on top of a spin-LED device with p-type InGaAs quantum dots in the active region. We measure an Overhauser shift of several $μ$eV at zero magnetic field for the positively charged exciton (trion X$^+$) EL emission, which changes sign as we reverse the injected electron spin orientation. This is a signature of dynamic polarization of the nuclear spins in the quantum dot induced by the hyperfine interaction with the electrically injected electron spin. This study paves the way for electrical control of nuclear spin polarization in a single quantum dot without any external magnetic field.

cond-mat.mes-hall↗

arXiv2017

Electron-nuclear coherent spin oscillations probed by spin dependent recombination

We demonstrate the detection of coherent electron-nuclear spin oscillations related to the hyperfine interaction and revealed by the band-to-band photoluminescence (PL) in zero external magnetic field. On the base of a pump-probe PL experiment we measure, directly in the temporal domain, the hyperfine constant of an electron coupled to a gallium defect in GaAsN by tracing the dynamical behavior of the conduction electron spin-dependent recombination to the defect site. The hyperfine constants and the relative abundance of the nuclei isotopes involved can be determined without the need of electron spin resonance technique and in the absence of any magnetic field. Information on the nuclear and electron spin relaxation damping parameters can also be estimated from the oscillations damping and the long delay behavior.

cond-mat.mes-hall↗

arXiv2016

Electron-nuclear spin dynamics of Ga$^{2+}$ paramagnetic centers probed by spin dependent recombination: A master equation approach

Similar to nitrogen-vacancy centers in diamond and impurity atoms in silicon, interstitial gallium deep paramagnetic centers in GaAsN have been proven to have useful characteristics for the development of spintronic devices. Among other interesting properties, under circularly polarized light, gallium centers in GaAsN act as spin filters that dynamically polarize free and bound electrons reaching record spin polarizations (100\%). Furthermore, the recent observation of the amplification of the spin filtering effect under a Faraday configuration magnetic field has suggested that the hyperfine interaction that couples bound electrons and nuclei permits the optical manipulation of its nuclear spin polarization. Even though the mechanisms behind the nuclear spin polarization in gallium centers are fairly well understood, the origin of nuclear spin relaxation and the formation of an Overhauser-like magnetic field remain elusive. In this work we develop a model based on the master equation approach to describe the evolution of electronic and nuclear spin polarizations of gallium centers interacting with free electrons and holes. Our results are in good agreement with existing experimental observations. In regard to the nuclear spin relaxation, the roles of nuclear dipolar and quadrupolar interactions are discussed. Our findings show that, besides the hyperfine interaction, the spin relaxation mechanisms are key to understand the amplification of the spin filtering effect and the appearance of the Overhauser-like magnetic field. Based on our model's results we propose an experimental protocol based on time resolved spectroscopy. It consists of a pump-probe photoluminescence scheme that would allow the detection and the tracing of the electron-nucleus flip-flops through time resolved PL measurements.

cond-mat.other↗

arXiv2016

Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers

We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $τ_{rad}=1.8\pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $\leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.

cond-mat.mtrl-sci↗

arXiv2015

Exciton states in monolayer MoSe2: impact on interband transitions

We combine linear and non-linear optical spectroscopy at 4K with ab initio calculations to study the electronic bandstructure of MoSe2 monolayers. In 1-photon photoluminescence excitation (PLE) and reflectivity we measure a separation between the A- and B-exciton emission of 220 meV. In 2-photon PLE we detect for the A- and B-exciton the 2p state 180meV above the respective 1s state. In second harmonic generation (SHG) spectroscopy we record an enhancement by more than 2 orders of magnitude of the SHG signal at resonances of the charged exciton and the 1s and 2p neutral A- and B-exciton. Our post-Density Functional Theory calculations show in the conduction band along the $K-Γ$ direction a local minimum that is energetically and in k-space close to the global minimum at the K-point. This has a potentially strong impact on the polarization and energy of the excitonic states that govern the interband transitions and marks an important difference to MoS2 and WSe2 monolayers.

cond-mat.mtrl-sci↗

arXiv2014

Exciton dynamics in WSe2 bilayers

We investigate exciton dynamics in 2H-WSe2 bilayers in time-resolved photoluminescence (PL) spectroscopy. Fast PL emission times are recorded for both the direct exciton with $τ_{D}$ ~ 3 ps and the indirect optical transition with $τ_{i}$ ~ 25 ps. For temperatures between 4 to 150 K $τ_{i}$ remains constant. Following polarized laser excitation, we observe for the direct exciton transition at the K point of the Brillouin zone efficient optical orientation and alignment during the short emission time $τ_{D}$. The evolution of the direct exciton polarization and intensity as a function of excitation laser energy is monitored in PL excitation (PLE) experiments.

cond-mat.mtrl-sci↗