arXiv subjects

Stéphane Berciaud

Publications and source records attributed to Stéphane Berciaud.

At least 37 records · Page 2Linked to original sources

arXiv2016

Electrically-driven vibronic spectroscopy with sub-molecular resolution

A scanning tunneling microscope is used to generate the electroluminescence of phthalocyanine molecules deposited on NaCl/Ag(111). Photon spectra reveal an intense emission line at 1.9 eV that corresponds to the fluorescence of the molecules, and a series of weaker red-shifted lines. Based on a comparison with Raman spectra acquired on macroscopic molecular crystals, these spectroscopic features can be associated to the vibrational modes of the molecules and provide a detailed chemical fingerprint of the probed species. Maps of the vibronic features reveal sub- molecularly-resolved structures whose patterns are related to the symmetry of the probed vibrational modes.

cond-mat.mes-hall↗

arXiv2016

Monitoring Electrostatically-Induced Deflection, Strain and Doping in Suspended Graphene using Raman Spectroscopy

Electrostatic gating offers elegant ways to simultaneously strain and dope atomically thin membranes. Here, we report on a detailed \textit{in situ} Raman scattering study on graphene, suspended over a Si/SiO$_2$ substrate. In such a layered structure, the intensity of the Raman G- and 2D-mode features of graphene are strongly modulated by optical interference effects and allow an accurate determination of the electrostatically-induced membrane deflection, up to irreversible collapse. The membrane deflection is successfully described by an electromechanical model, which we also use to provide useful guidelines for device engineering. In addition, electrostatically-induced tensile strain is determined by examining the softening of the Raman features. Due to a small residual charge inhomogeneity $\sim 5\times 10^{10}~\rm cm^{-2}$, we find that non-adiabatic anomalous phonon softening is negligible compared to strain-induced phonon softening. These results open perspectives for innovative Raman scattering-based readout schemes in two-dimensional nanoreso

cond-mat.mes-hall↗

arXiv2016

Direct versus indirect band gap emission and exciton-exciton annihilation in atomically thin molybdenum ditelluride (MoTe$_2$)

We probe the room temperature photoluminescence of $N$-layer molybdenum ditelluride (MoTe$_2$) in the continuous wave (cw) regime. The photoluminescence quantum yield of monolayer MoTe$_2$ is three times larger than in bilayer MoTe$_2$ and forty times greater than in the bulk limit. Mono- and bilayer MoTe$_2$ display almost symmetric emission lines at $1.10~\rm eV$ and $1.07~\rm eV$, respectively, which predominantly arise from direct radiative recombination of the A exciton. In contrast, $N\geq3-$layer MoTe$_2$ exhibits a much reduced photoluminescence quantum yield and a broader, redshifted and seemingly bimodal photoluminescence spectrum. The low- and high-energy contributions are attributed to emission from the indirect and direct optical band gaps, respectively. Bulk MoTe$_2$ displays a broad emission line with a dominant contribution at 0.94~eV that is assigned to emission from the indirect optical band gap. As compared to related systems (such as MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$), the smaller energy difference between the monolayer direct optical band gap and the bulk indirect optical band gap leads to a smoother increase of the photoluminescence quantum yield as $N$ decreases. In addition, we study the evolution of the photoluminescence intensity in monolayer MoTe$_2$ as a function of the exciton formation rate $W_\mathrm{abs}$ up to $3.6\times 10^{22}~\rm{cm}^{-2} s^{-1}$. The lineshape of the photoluminescence spectrum remains largely independent of $W_\mathrm{abs}$, whereas the photoluminescence intensity grows sub-linearly above $W_\mathrm{abs}\sim 10^{21}~\rm cm^{-2} s^{-1}$. This behavior is assigned to exciton-exciton annihilation and is well-captured by an elementary rate equation model.

cond-mat.mes-hall↗

arXiv2016

Splitting of interlayer shear modes and photon energy dependent anisotropic Raman response in $N$-layer ReSe$_2$ and ReS$_2$

We investigate the interlayer phonon modes in $N$-layer rhenium diselenide (ReSe$_2$) and rhenium disulfide (ReS$_2$) by means of ultralow-frequency micro-Raman spectroscopy. These transition metal dichalcogenides exhibit a stable distorted octahedral (1T') phase with significant in-plane anisotropy, leading to sizable splitting of the (in-plane) layer shear modes. The fan-diagrams associated with the measured frequencies of the interlayer shear modes and the (out-of-plane) interlayer breathing modes are perfectly described by a finite linear chain model and allow the determination of the interlayer force constants. Nearly identical values are found for ReSe$_2$ and ReS$_2$. The latter are appreciably smaller than but on the same order of magnitude as the interlayer force constants reported in graphite and in trigonal prismatic (2Hc) transition metal dichalcogenides (such as MoS$_2$, MoSe$_2$, MoTe$_2$, WS$_2$, WSe$_2$), demonstrating the importance of van der Waals interactions in $N$-layer ReSe$_2$ and ReS$_2$. In-plane anisotropy results in a complex angular dependence of the intensity of all Raman modes, which can be empirically utilized to determine the crystal orientation. However, we also demonstrate that the angular dependence of the Raman response drastically depends on the incoming photon energy, shedding light on the importance of resonant exciton-phonon coupling in ReSe$_2$ and ReS$_2$.

cond-mat.mes-hall↗

arXiv2015

Unified description of the optical phonon modes in $N$-layer MoTe$_2$

$N$-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three dimensional) and monolayer (quasi two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the $Γ$-point optical phonons in $N$-layer $2H$-molybdenum ditelluride (MoTe$_2$). We observe a series of $N$-dependent low-frequency interlayer shear and breathing modes (below $40~\rm cm^{-1}$, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the range $100-200~\rm cm^{-1}$, denoted iX and oX), which solely involve displacements of the chalcogen atoms. In contrast, the high-frequency modes (in the range $200-300~\rm cm^{-1}$, denoted iMX and oMX), arising from displacements of both the metal and chalcogen atoms, exhibit considerably reduced splittings. The manifold of phonon modes associated with the in-plane and out-of-plane displacements are quantitatively described by a force constant model, including interactions up to the second nearest neighbor and surface effects as fitting parameters. The splittings for the iX and oX modes observed in $N$-layer crystals are directly correlated to the corresponding bulk Davydov splittings between the $E_{2u}/E_{1g}$ and $B_{1u}/A_{1g}$ modes, respectively, and provide a measurement of the frequencies of the bulk silent $E_{2u}$ and $B_{1u}$ optical phonon modes. Our analysis could readily be generalized to other layered crystals.

cond-mat.mes-hall↗

arXiv2015

Raman Spectroscopy of Electrochemically-Gated Graphene Transistors: Geometrical Capacitance, Electron-Phonon, Electron-Electron, and Electron-Defect Scattering

We report a comprehensive micro-Raman scattering study of electrochemically-gated graphene field-effect transistors. The geometrical capacitance of the electrochemical top-gates is accurately determined from dual-gated Raman measurements, allowing a quantitative analysis of the frequency, linewidth and integrated intensity of the main Raman features of graphene. The anomalous behavior observed for the G-mode phonon is in very good agreement with theoretical predictions and provides a measurement of the electron-phonon coupling constant for zone-center ($Γ$ point) optical phonons. In addition, the decrease of the integrated intensity of the 2D-mode feature with increasing doping, makes it possible to determine the electron-phonon coupling constant for near zone-edge (K and K' points) optical phonons. We find that the electron-phonon coupling strength at $Γ$ is five times weaker than at K (K'), in very good agreement with a direct measurement of the ratio of the integrated intensities of the resonant intra- (2D') and inter-valley (2D) Raman features. We also show that electrochemical reactions, occurring at large gate biases, can be harnessed to efficiently create defects in graphene, with concentrations up to approximately $1.4\times 10^{12}~\rm cm^{-2}$. At such defect concentrations, we estimate that the electron-defect scattering rate remains much smaller than the electron-phonon scattering rate. The evolution of the G- and 2D-mode features upon doping remain unaffected by the presence of defects and the doping dependence of the D mode closely follows that of its two-phonon (2D mode) overtone. Finally, the linewidth and frequency of the G-mode phonon as well as the frequencies of the G- and 2D-mode phonons in doped graphene follow sample-independent correlations that can be utilized for accurate estimations of the charge carrier density.

cond-mat.mes-hall↗

arXiv2015

Distance Dependence of the Energy Transfer Rate From a Single Semiconductor Nanostructure to Graphene

The near-field Coulomb interaction between a nano-emitter and a graphene monolayer results in strong Förster-type resonant energy transfer and subsequent fluorescence quenching. Here, we investigate the distance dependence of the energy transfer rate from individual, i) zero-dimensional CdSe/CdS nanocrystals and ii) two-dimensional CdSe/CdS/ZnS nanoplatelets to a graphene monolayer. For increasing distances $d$, the energy transfer rate from individual nanocrystals to graphene decays as $1/d^4$. In contrast, the distance dependence of the energy transfer rate from a two-dimensional nanoplatelet to graphene deviates from a simple power law, but is well described by a theoretical model, which considers a thermal distribution of free excitons in a two-dimensional quantum well. Our results show that accurate distance measurements can be performed at the single particle level using graphene-based molecular rulers and that energy transfer allows probing dimensionality effects at the nanoscale.

cond-mat.mes-hall↗

arXiv2014

All-Optical Blister Test of Suspended Graphene Using Micro-Raman Spectroscopy

We report a comprehensive micro-Raman study of a pressurized suspended graphene membrane that hermetically seals a circular pit, etched in a Si/SiO$_2$ substrate. Placing the sample under a uniform pressure load results in bulging of the graphene membrane and subsequent softening of the main Raman features, due to tensile strain. In such a microcavity, the intensity of the Raman features depends very sensitively on the distance between the graphene membrane and the Si substrate, which acts as the bottom mirror of the cavity. Thus, a spatially resolved analysis of the intensity of the G- and 2D-mode features as a function of the pressure load permits a direct reconstruction of the blister profile. An average strain is then deduced at each pressure load, and Grüneisen parameters of $1.8\pm0.2$ and $2.4\pm0.2$ are determined for the Raman G and 2D modes, respectively. In addition, the measured blister height is proportional to the cubic root of the pressure load, as predicted theoretically. The validation of this scaling provides a direct and accurate determination the Young's modulus of graphene with a purely optical, hence contactless and minimally invasive, approach. We find a Young's modulus of $(1.05\pm 0.10) \rm TPa$ for monolayer graphene, in a perfect match with previous nanoindentation measurements. This all-optical methodology opens avenues for pressure sensing using graphene and could readily be adapted to other emerging two-dimensional materials and nanoresonators.

cond-mat.mes-hall↗

arXiv2014

Probing electronic excitations in mono- to pentalayer graphene by micro-magneto-Raman spectroscopy

We probe electronic excitations between Landau levels in freestanding $N-$layer graphene over a broad energy range, with unprecedented spectral and spatial resolution, using micro-magneto Raman scattering spectroscopy. A characteristic evolution of electronic bands in up to five Bernal-stacked graphene layers is evidenced and shown to remarkably follow a simple theoretical approach, based on an effective bilayer model. $(N>3)$-layer graphene appear as appealing candidates in the quest for novel phenomena, particularly in the quantum Hall effect regime. Our work paves the way towards minimally-invasive investigations of magneto-excitons in other emerging low-dimensional systems, with a spatial resolution down to 1$~μ$m.

cond-mat.mes-hall↗

arXiv2013

Tunable electronic correlation effects in nanotube-light interactions

Electronic many-body correlation effects in one-dimensional (1D) systems such as carbon nanotubes have been predicted to modify strongly the nature of photoexcited states. Here we directly probe this effect using broadband elastic light scattering from individual suspended carbon nanotubes under electrostatic gating conditions. We observe significant shifts in optical transition energies, as well as line broadening, as the carrier density is increased. The results demonstrate the differing role of screening of many-body electronic interactions on the macroscopic and microscopic length scales, a feature inherent to quasi-1D systems. Our findings further demonstrate the possibility of electrical tuning of optical transitions and provide a basis for understanding of various optical phenomena in carbon nanotubes and other quasi-1D systems in the presence of charge carrier doping.

cond-mat.mes-hall↗

arXiv2013

Intrinsic lineshape of the Raman 2D-mode in freestanding graphene monolayers

We report a comprehensive study of the two-phonon inter-valley (2D) Raman mode in graphene monolayers, motivated by recent reports of asymmetric 2D-mode lineshapes in freestanding graphene. For photon energies in the range $1.53 \rm eV - 2.71 \rm eV$, the 2D-mode Raman response of freestanding samples appears as bimodal, in stark contrast with the Lorentzian approximation that is commonly used for supported monolayers. The transition between the freestanding and supported cases is mimicked by electrostatically doping freestanding graphene at carrier densities above $2\times 10^{11} \rm cm^{-2}$. This result quantitatively demonstrates that low levels of charging can obscure the intrinsically bimodal 2D-mode lineshape of monolayer graphene, which can be utilized as a signature of a quasi-neutral sample. In pristine freestanding graphene, we observe a broadening of the 2D-mode feature with decreasing photon energy that cannot be rationalized using a simple one-dimensional model based on resonant \textit{inner} and \textit{outer} processes. This indicates that phonon wavevectors away from the high-symmetry lines of the Brillouin zone must contribute to the 2D-mode, so that a full two-dimensional calculation is required to properly describe multiphonon-resonant Raman processes.

cond-mat.mes-hall↗

arXiv2013

Biexciton, single carrier, and trion generation dynamics in single-walled carbon nanotubes

We present a study of free carrier photo-generation and multi-carrier bound states, such as biexcitons and trions (ionized excitons), in semiconducting single-walled carbon nanotubes. Pump-and-probe measurements performed with fs pulses reveal the effects of strong Coulomb interactions between carriers on their dynamics. Biexciton formation by optical transition from exciton population results in an induced absorption line (binding energy 130 meV). Exciton-exciton annihilation process is shown to evolve at high densities towards an Auger process that can expel carriers from nanotubes. The remaining carriers give rise to an induced absorption due to trion formation (binding energy 190 meV). These features show the dynamics of exciton and free carriers populations.

cond-mat.mes-hall↗

arXiv2011

All-optical trion generation in single walled carbon nanotubes

We present evidence of all optical trion generation and emission in undoped single walled carbon nanotubes (SWCNTs). Luminescence spectra, recorded on individual SWCNTs over a large CW excitation intensity range, show trion emission peaks red-shifted with respect to the bright exciton peak. Clear chirality dependence is observed for 22 separate SWCNT species, allowing for determination of electron-hole exchange interaction and trion binding energy contributions. Luminescence data together with ultrafast pump probe experiments on chirality sorted bulk samples suggest that exciton-exciton annihilation processes generate dissociated carriers that allow for trion creation upon a subsequent photon absorption event.

cond-mat.mes-hall↗

arXiv2011

Temperature dependence of the anharmonic decay of optical phonons in carbon nanotubes and graphite

We report on the temperature dependence of the anharmonic decay rate of zone-center (G mode) optical phonons in both single-walled carbon nanotubes and graphite. The measurements are performed using a pump-probe Raman scattering scheme with femtosecond laser pulses. For nanotubes, measured over a temperature range of 6 K-700 K, we observe little temperature dependence of the decay rate below room temperature. Above 300 K, the decay rate increases from 0.8 to 1.7 ps-1. The decay rates observed for graphite range from 0.5 to 0.8 ps-1 for temperatures from 300 K-700 K. We compare the behavior observed in carbon nanotubes and graphite and discuss the implications of our results for the mechanism of the anharmonic decay of optical phonons in both systems.

cond-mat.mtrl-sci↗

arXiv2010

Electron and optical phonon temperatures in electrically biased graphene

We examine the intrinsic energy dissipation steps in electrically biased graphene channels. By combining in-situ measurements of the spontaneous optical emission with a Raman spectroscopy study of the graphene sample under conditions of current flow, we obtain independent information on the energy distribution of the electrons and phonons. The electrons and holes contributing to light emission are found to obey a thermal distribution, with temperatures in excess of 1500 K in the regime of current saturation. The zone-center optical phonons are also highly excited and are found to be in equilibrium with the electrons. For a given optical phonon temperature, the anharmonic downshift of the Raman G-mode is smaller than expected under equilibrium conditions, suggesting that the electrons and high-energy optical phonons are not fully equilibrated with all of the phonon modes.

cond-mat.mes-hall↗

arXiv2010

Energy Transfer from Individual Semiconductor Nanocrystals to Graphene

Energy transfer from photoexcited zero-dimensional systems to metallic systems plays a prominent role in modern day materials science. A situation of particular interest concerns the interaction between a photoexcited dipole and an atomically thin metal. The recent discovery of graphene layers permits investigation of this phenomenon. Here we report a study of fluorescence from individual CdSe/ZnS nanocrystals in contact with single- and few-layer graphene sheets. The rate of energy transfer is determined from the strong quenching of the nanocrystal fluorescence. For single-layer graphene, we find a rate of ~ 4ns-1, in agreement with a model based on the dipole approximation and a tight-binding description of graphene. This rate increases significantly with the number of graphene layers, before approaching the bulk limit. Our study quantifies energy transfer to and fluorescence quenching by graphene, critical properties for novel applications in photovoltaic devices and as a molecular ruler.

physics.chem-ph↗

arXiv2007

Observation of intrinsic size effects in the optical response of individual gold nanoparticles

The Photothermal Heterodyne Imaging method is used to study for the first time the absorption spectra of individual gold nanoparticles with diameters down to 5 nm. Intrinsic size effects wich result in a broadening of the Surface Plasmon resonance are unambiguously observed. Dispersions in the peak energies and homogeneous widths of the single particle resonances are revealed. The experimental results are analysed within the frame of Mie theory.

physics.optics↗

arXiv2007

Photothermal heterodyne imaging of individual nonfluorescent nanoclusters and nanocrystals

We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle.

physics.optics↗