arXiv subjects

V. Jindal

Publications and source records attributed to V. Jindal.

5 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↗

arXiv2025

Spin-valley polarization control in WSe$_2$ monolayers using photochemical doping

We report on the influence of a photochemical doping method on the spin-valley polarization degree ($P_{c}$) of excitons in WSe$_2$ monolayers. By varying the carrier density and transitioning from an excess of electrons (n-type) to an excess of holes (p-type), we observe a non-monotonic dependence of $P_{c}$ on the doping level. Using controlled, single-shot photochlorination steps, we unveil this non-monotonic behavior, with $P_{c}$ reaching a minimum value of less than 10$\%$ at 78 K near the charge neutrality point, while increasing by a factor of three at a hole density of $5 \times 10^{11} \,\mathrm{cm^{-2}}$. The impact of the doping on $P_{c}$ is explained using a phenomenological model that accounts for various mechanisms influencing exciton polarization dynamics, including exciton-carrier scattering processes and exciton-to-trion conversion rates. Among these, exciton-carrier collisions emerge as the dominant mechanism driving the observed variations in $P_{c}$, while the exciton effective lifetime remains nearly independent of doping. These findings highlight the potential of photochemical methods for investigating valley physics and for effectively tuning the exciton polarization degree in transition metal dichalcogenide monolayers.

cond-mat.mes-hall↗

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↗