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Register a new userMicroscopic mechanism for transient population inversion and optical gain in graphene
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A transient femtosecond population inversion in graphene was recently reported by Li et al., Phys. Rev. Lett. 108, 167401 (2012). Based on a microscopic theory we clarify the underlying microscopic mechanism: Transient gain and population inversion in graphene occurs due to a complex interplay of strong optical pumping and carrier cooling that fills states close to the Dirac point giving rise to a relaxation bottleneck. The subsequent femtosecond decay of the optical gain is mainly driven by Coulomb-induced Auger recombination.
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The recent demonstration of saturable absorption and negative optical conductivity in the Terahertz range in graphene has opened up new opportunities for optoelectronic applications based on this and other low dimensional materials. Recently, population inversion across the Dirac point has been observed directly by time- and angle-resolved photoemission spectroscopy (tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This severely limits the applicability of single layer graphene to, for example, Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived population inversion in bilayer graphene. The effect is attributed to the small band gap found in this compound. We propose a microscopic model for these observations and speculate that an enhancement of both the pump photon energy and the pump fluence may further increase this lifetime.
We theoretically study the population inversion and negative dynamic conductivity in intrinsic graphene in the terahertz (THz) frequency range upon pulse photoexcitation with near-/mid-infrared wavelength. The threshold pulse energy required for the population inversion and negative dynamic conductivity can be orders-of-magnitude lower when the pulse photon energy is lower, due to the inverse proportionality of the photoexcited carrier concentration to the pulse photon energy and to the weaker carrier heating. We also investigate the dependence of the dynamic conductivity on the momentum relaxation time. The negative dynamic conductivity takes place either in high- or low-quality graphene, where the Drude absorption by carriers in the THz frequency is weak.
We present a microscopic explanation of the controversially discussed transient negative differential transmission observed in degenerate optical pump-probe measurements in graphene. Our approach is based on the density matrix formalism allowing a time- and momentum-resolved study of carrier-light, carrier-carrier, and carrier-phonon interaction on microscopic footing. We show that phonon-assisted optical intraband transitions give rise to transient absorption in the optically excited hot carrier system counteracting pure absorption bleaching of interband transitions. While interband transition bleaching is relevant in the first hundreds of fs after the excitation, intraband absorption sets in at later times. In particular, in the low excitation regime, these intraband absorption processes prevail over the absorption bleaching resulting in a zero-crossing of the differential transmission. Our findings are in good agreement with recent experimental pump-probe studies.
When graphene is close to charge neutrality, its energy landscape is highly inhomogeneous, forming a sea of electron-like and hole-like puddles, which determine the properties of graphene at low carrier density. However, the details of the puddle formation have remained elusive. We demonstrate numerically that in sharp contrast to monolayer graphene, the normalized autocorrelation function for the puddle landscape in bilayer graphene depends only on the distance between the graphene and the source of the long-ranged impurity potential. By comparing with available experimental data, we find quantitative evidence for the implied differences in scanning tunneling microscopy measurements of electron and hole puddles for monolayer and bilayer graphene in nominally the same disorder potential.
In contrast to conventional structures, efficient non-radiative carrier recombination counteracts the appearance of optical gain in graphene. Based on a microscopic and fully quantum-mechanical study of the coupled carrier, phonon, and photon dynamics in graphene, we present a strategy to obtain a long-lived gain: Integrating graphene into a photonic crystal nanocavity and applying a high-dielectric substrate gives rise to pronounced coherent light emission suggesting the design of graphene-based laser devices covering a broad spectral range.
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