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Register a new userPolarized photoluminescence clocks ultrafast pseudospin relaxation in graphene
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Electronic states in 2D materials can exhibit pseudospin degrees of freedom, which allow for unique carrier-field interaction scenarios. Here, we investigate ultrafast sublattice pseudospin relaxation in graphene by means of polarization-resolved photoluminescence spectroscopy. Comparison with microscopic Boltzmann simulations allows to determine a lifetime of the optically aligned pseudospin distribution of $12pm 2,text{fs}$. This experimental approach extends the toolbox of graphene pseudospintronics, providing novel means to investigate pseudospin dynamics in active devices or under external fields.
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Interband optical transitions in graphene are subject to pseudospin selection rules. Impulsive excitation with linearly polarized light generates an anisotropic photocarrier occupation in momentum space that evolves at timescales shorter than 100fs. Here, we investigate the evolution of non-equilibrium charges towards an isotropic distribution by means of fluence-dependent ultrafast spectroscopy and develop an analytical model able to quantify the isotropization process. In contrast to conventional semiconductors, the isotropization is governed by optical phonon emission, rather than electron-electron scattering, which nevertheless contributes in shaping the anisotropic photocarrier occupation within the first few fs.
The possibility of transporting spin information over long distances in graphene, owing to its small intrinsic spin-orbit coupling (SOC) and the absence of hyperfine interaction, has led to intense research into spintronic applications. However, measured spin relaxation times are orders of magnitude smaller than initially predicted, while the main physical process for spin dephasing and its charge-density and disorder dependences remain unconvincingly described by conventional mechanisms. Here, we unravel a spin relaxation mechanism for nonmagnetic samples that follows from an entanglement between spin and pseudospin driven by random SOC, which makes it unique to graphene. The mixing between spin and pseudospin-related Berrys phases results in fast spin dephasing even when approaching the ballistic limit, with increasing relaxation times away from the Dirac point, as observed experimentally. The SOC can be caused by adatoms, ripples or even the substrate, suggesting novel spin manipulation strategies based on the pseudospin degree of freedom.
The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photo-excited electron-hole pairs. These interband excitations are in fact forbidden along the direction of the light polarization, and are maximum perpendicular to it. Here, we use time- and angle-resolved photoemission spectroscopy to investigate the resulting unconventional hot carrier dynamics, sampling carrier distributions as a function of energy and in-plane momentum. We first show that the rapidly-established quasi-thermal electron distribution initially exhibits an azimuth-dependent temperature, consistent with relaxation through collinear electron-electron scattering. Azimuthal thermalization is found to occur only at longer time delays, at a rate that depends on the substrate and the static doping level. Further, we observe pronounced differences in the electron and hole dynamics in n-doped samples. By simulating the Coulomb- and phonon-mediated carrier dynamics we are able to disentangle the influence of excitation fluence, screening, and doping, and develop a microscopic picture of the carrier dynamics in photo-excited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photo-control experiments and optoelectronic device applications.
For most optoelectronic applications of graphene a thorough understanding of the processes that govern energy relaxation of photoexcited carriers is essential. The ultrafast energy relaxation in graphene occurs through two competing pathways: carrier-carrier scattering -- creating an elevated carrier temperature -- and optical phonon emission. At present, it is not clear what determines the dominating relaxation pathway. Here we reach a unifying picture of the ultrafast energy relaxation by investigating the terahertz photoconductivity, while varying the Fermi energy, photon energy, and fluence over a wide range. We find that sufficiently low fluence ($lesssim$ 4 $mu$J/cm$^2$) in conjunction with sufficiently high Fermi energy ($gtrsim$ 0.1 eV) gives rise to energy relaxation that is dominated by carrier-carrier scattering, which leads to efficient carrier heating. Upon increasing the fluence or decreasing the Fermi energy, the carrier heating efficiency decreases, presumably due to energy relaxation that becomes increasingly dominated by phonon emission. Carrier heating through carrier-carrier scattering accounts for the negative photoconductivity for doped graphene observed at terahertz frequencies. We present a simple model that reproduces the data for a wide range of Fermi levels and excitation energies, and allows us to qualitatively assess how the branching ratio between the two distinct relaxation pathways depends on excitation fluence and Fermi energy.
We present a joint theory-experiment study on ultrafast photoluminescence from photoexcited graphene. Based on a microscopic theory, we reveal two distinct mechanisms behind the occurring photoluminescence: Besides the well-known incoherent contribution driven by non-equilibrium carrier occupations, we found a coherent part that spectrally shifts with the excitation energy. In our experiments, we demonstrate for the first time the predicted appearance and spectral shift of the coherent photoluminescence.
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