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Luis E. Parra López

Publications and source records attributed to Luis E. Parra López.

9 recordsLinked to original sources

Sub-nm range momentum-dependent exciton transfer from a 2D semiconductor to graphene

Heterostructures made from atomically thin semiconductors (here MoSe$_2$) and graphene are uniquely poised to investigate photoinduced charge and energy transfer in the 2D limit. Here, using picosecond time-resolved photoluminescence spectroscopy at cryogenic temperatures on two types of MoSe$_2$/graphene heterostrutures, we unveil key features of the underlying mechanisms. First, the shortening of the MoSe$_2$ bright exciton lifetime is marginally affected by the number of graphene layers to which MoSe$_2$ is coupled. Second, exciton transfer vanishes when a sub-nm thick spacer of hexagonal boron nitride decouples MoSe$_2$ from graphene. These results indicate that charge tunneling govern bright exciton relaxation in MoSe$_2$/graphene and that longer-range, Förster-type energy transfer (FRET) does not affect bright excitons. However, sub-ps FRET to graphene accelerates the relaxation of ``hot'' excitons formed upon optical excitation, leading to photoluminescence quenching factors that exceed expectations based on the shortening of the bright exciton lifetime. Our work has direct implications for energy harvesting and funneling using van der Waals heterostructures.

cond-mat.mes-hall↗

Ultrafast dynamics of local charge order in a THz-induced metastable quantum state

Controlling quantum materials with ultrafast light pulses enables access to transient and metastable states that are inaccessible under equilibrium conditions. Yet their local dynamics remain poorly understood due to the challenge of resolving ultrafast processes with angstrom-scale spatial resolution. Here, we use terahertz scanning tunnelling microscopy (THz-STM) to probe coherent collective dynamics within a THz-induced metastable state in the layered charge density wave (CDW) material 1T-TaS2. Following ultrafast photoexcitation, we locally resolve coherent oscillations of the CDW amplitude mode at 2.5 THz together with two previously unreported modes at 1.3 THz and 0.7 THz. Comparison with phonon calculations identifies these as interlayer breathing and shear vibrations that are sensitive to the stacking configuration. These coherent dynamics are observed within a THz-induced metastable state that exhibits long-lived and spatially inhomogeneous modifications of the local density of states within the insulating gap, while higher THz fields drive a local redistribution and disordering of Star-of-David clusters near defects and domain boundaries. Our results suggest that the THz-induced metastable state involves a modification of the local interlayer stacking configuration, and demonstrate the role of interlayer degrees of freedom in the ultrafast dynamics of light-induced phases in layered quantum materials.

cond-mat.mes-hall↗

Rotating spintronic terahertz emitter optimized for microjoule pump-pulse energies and megahertz repetition rates

Spintronic terahertz emitters (STEs) are powerful sources of ultra-broadband single-cycle terahertz (THz) field transients. They work with any pump wavelength, and their polarity and polarization direction are easily adjustable. However, at high pump powers and high repetition rates, STE operation is hampered by a significant increase in the local temperature. Here, we resolve this issue by rotating the STE at a few 100 Hz, thereby distributing the absorbed pump power over a larger area. Our approach permits stable STE operation at a fluence of ~1 mJ/cm$^2$ with up to 18 W pump power at megahertz repetition rates, corresponding to pump-pulse energies of a few 10 $μ$J and a power density far above the melting threshold of metallic films. The rotating STE is of interest for all ultra-broadband high-power THz applications requiring high repetition rates. As an example, we show that THz pulses with peak fields of 10 kV/cm can be coupled to a THz-lightwave-driven scanning tunneling microscope at 1 MHz repetition rate, demonstrating that the rotating STE can compete with standard THz sources such as LiNbO$_3$.

physics.optics↗

Symmetry-dependent dielectric screening of optical phonons in monolayer graphene

Quantised lattice vibrations (i.e., phonons) in solids are robust and unambiguous fingerprints of crystal structures and of their symmetry properties. In metals and semimetals, strong electron-phonon coupling may lead to so-called Kohn anomalies in the phonon dispersion, providing an image of the Fermi surface in a non-electronic observable. Kohn anomalies become prominent in low-dimensional systems, in particular in graphene, where they appear as sharp kinks in the in-plane optical phonon branches. However, in spite of intense research efforts on electron-phonon coupling in graphene and related van der Waals heterostructures, little is known regarding the links between the symmetry properties of optical phonons at and near Kohn anomalies and their sensitivity towards the local environment. Here, using inelastic light scattering (Raman) spectroscopy, we investigate a set of custom-designed graphene-based van der Waals heterostructures, wherein dielectric screening is finely controlled at the atomic layer level. We demonstrate experimentally and explain theoretically that, depending exclusively on their symmetry properties, the two main Raman modes of graphene react differently to the surrounding environment. While the Raman-active near-zone-edge optical phonons in graphene undergo changes in their frequencies due to the neighboring dielectric environment, the in-plane, zone-centre optical phonons are symmetry-protected from the influence of the latter. These results shed new light on the unique electron-phonon coupling properties in graphene and related systems and provide invaluable guidelines to characterise dielectric screening in van der Waals heterostructures and moiré superlattices.

cond-mat.mes-hall↗

Electroluminescence of monolayer WS$_2$ in a scanning tunneling microscope: the effect of bias polarity on the spectral and angular distribution of the emitted light

Inelastic electron tunneling in a scanning tunneling microscope (STM) is used to generate excitons in monolayer tungsten disulfide (WS$_2$). Excitonic electroluminescence is measured both at positive and negative sample bias. Using optical spectroscopy and Fourier-space optical microscopy, we show that the bias polarity of the tunnel junction determines the spectral and angular distribution of the emitted light. At positive sample bias, only emission from excitonic species featuring an in-plane transition dipole moment is detected. Based on the spectral distribution of the emitted light, we infer that the dominant contribution is from charged excitons, i.e., trions. At negative sample bias, additional contributions from lower-energy excitonic species are evidenced in the emission spectra and the angular distribution of the emitted light reveals a mixed character of in-plane and out-of-plane transition dipole moments.

cond-mat.mes-hall↗

Tip-induced excitonic luminescence nanoscopy of an atomically-resolved van der Waals heterostructure

Low-temperature scanning tunneling microscopy is used to probe, with atomic-scale spatial resolution, the intrinsic luminescence of a van der Waals heterostructure, made of a transition metal dichalcogenide monolayer stacked onto a few-layer graphene flake supported by an Au(111) substrate. Sharp emission lines arising from neutral, charged and localised excitons are reported. Their intensities and emission energies vary as a function of the nanoscale environment of the van der Waals heterostructure, explaining the variability of the emission properties observed with diffraction-limited approaches. Our work paves the way towards understanding and control of optoelectronic phenomena in moiré superlattices with atomic-scale resolution.

cond-mat.mes-hall↗

Picosecond energy transfer in a transition metal dichalcogenide-graphene heterostructure revealed by transient Raman spectroscopy

Intense light-matter interactions and unique structural and electrical properties make Van der Waals heterostructures composed by Graphene (Gr) and monolayer transition metal dichalcogenides (TMD) promising building blocks for tunnelling transistors, flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and quantum light emitting devices (QLEDs), bright and narrow-line emitters using minimal amounts of active absorber material. The performance of such devices is critically ruled by interlayer interactions which are still poorly understood in many respects. Specifically, two classes of coupling mechanisms have been proposed: charge transfer (CT) and energy transfer (ET), but their relative efficiency and the underlying physics is an open question. Here, building on a time resolved Raman scattering experiment, we determine the electronic temperature profile of Gr in response to TMD photo-excitation, tracking the picosecond dynamics of the G and 2D bands. Compelling evidence for a dominant role ET process accomplished within a characteristic time of ~ 4 ps is provided. Our results suggest the existence of an intermediate process between the observed picosecond ET and the generation of a net charge underlying the slower electric signals detected in optoelectronic applications.

cond-mat.mes-hall↗

Single- and narrow-line photoluminescence in a boron nitride-supported MoSe$_2$/graphene heterostructure

Heterostructures made from van der Waals materials provide a template to investigate proximity effects at atomically sharp heterointerfaces. In particular, near-field charge and energy transfer in heterostructures made from semiconducting transition metal dichalcogenides (TMD) have attracted interest to design model 2D "donor-acceptor" systems and new optoelectronic components. Here, using of Raman scattering and photoluminescence spectroscopies, we report a comprehensive characterization of a molybedenum diselenide (MoSe$_2$) monolayer deposited onto hexagonal boron nitride (hBN) and capped by mono- and bilayer graphene. Along with the atomically flat hBN susbstrate, a single graphene epilayer is sufficient to passivate the MoSe$_2$ layer and provides a homogenous environment without the need for an extra capping layer. As a result, we do not observe photo-induced doping in our heterostructure and the MoSe$_2$ excitonic linewidth gets as narrow as 1.6~meV, hence approaching the homogeneous limit. The semi-metallic graphene layer neutralizes the 2D semiconductor and enables picosecond non-radiative energy transfer that quenches radiative recombination from long-lived states. Hence, emission from the neutral band edge exciton largely dominates the photoluminescence spectrum of the MoSe$_2$/graphene heterostructure. Since this exciton has a picosecond radiative lifetime at low temperature, comparable with the energy transfer time, its low-temperature photoluminescence is only quenched by a factor of $3.3 \pm 1$ and $4.4 \pm 1$ in the presence of mono- and bilayer graphene, respectively. Finally, while our bare MoSe$_2$ on hBN exhibits negligible valley polarization at low temperature and under near-resonant excitation, we show that interfacing MoSe$_2$ with graphene yields a single-line emitter with degrees of valley polarization and coherence up to $\sim 15\,\%$.

cond-mat.mes-hall↗

Filtering the photoluminescence spectra of atomically thin semiconductors with graphene

Atomically thin semiconductors made from transition metal dichalcogenides (TMDs) are model systems for investigations of strong light-matter interactions and applications in nanophotonics, opto-electronics and valley-tronics. However, the photoluminescence spectra of TMD monolayers display a large number of features that are particularly challenging to decipher. On a practical level, monochromatic TMD-based emitters would be beneficial for low-dimensional devices but this challenge is yet to be resolved. Here, we show that graphene, directly stacked onto TMD monolayers enables single and narrow-line photoluminescence arising solely from TMD neutral excitons. This filtering effect stems from complete neutralization of the TMD by graphene combined with selective non-radiative transfer of long-lived excitonic species to graphene. Our approach is applied to four tungsten and molybdenum-based TMDs and establishes TMD/graphene heterostructures as a unique set of opto-electronic building blocks, suitable for electroluminescent systems emitting visible and near-infrared photons at near THz rate with linewidths approaching the lifetime limit.

cond-mat.mes-hall↗