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Register a new userExcited-state relaxations and Franck-Condon shift in Si quantum dots
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Added by
Alberto Franceschetti
Publication date
2002
fields
Physics
and research's language is
English
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Excited-state relaxations in molecules are responsible for a red shift of the absorption peak with respect to the emission peak (Franck-Condon shift). The magnitude of this shift in semiconductor quantum dots is still unknown. Here we report first-principle calculations of excited-state relaxations in small (diameter < 2.2 nm) Si nanocrystals, showing that the Franck-Condon shift is surprisingly large (~60 meV for a 2.2 nm-diameter nanocrystal). The physical mechanism of the excited-state relaxations changes abruptly around 1 nanoeter in size, providing a clear demarcation between ``molecules and ``nanocrystals.
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Understanding the influence of vibrational motion of the atoms on electronic transitions in molecules constitutes a cornerstone of quantum physics, as epitomized by the Franck-Condon principle of spectroscopy. Recent advances in building molecular-electronics devices and nanoelectromechanical systems open a new arena for studying the interaction between mechanical and electronic degrees of freedom in transport at the single-molecule level. The tunneling of electrons through molecules or suspended quantum dots has been shown to excite vibrational modes, or vibrons. Beyond this effect, theory predicts that strong electron-vibron coupling dramatically suppresses the current flow at low biases, a collective behaviour known as Franck-Condon blockade. Here we show measurements on quantum dots formed in suspended single-wall carbon nanotubes revealing a remarkably large electron-vibron coupling and, due to the high quality and unprecedented tunability of our samples, admit a quantitative analysis of vibron-mediated electronic transport in the regime of strong electron-vibron coupling. This allows us to unambiguously demonstrate the Franck-Condon blockade in a suspended nanostructure. The large observed electron-vibron coupling could ultimately be a key ingredient for the detection of quantized mechanical motion. It also emphasizes the unique potential for nanoelectromechanical device applications based on suspended graphene sheets and carbon nanotubes.
Electronic states and vibrons in carbon nanotube quantum dots have in general different location and size. As a consequence, the conventional Anderson-Holstein model, coupling vibrons to the dot total charge only, may no longer be appropriated in general. Here we explicitly address the role of the spatial fluctuations of the electronic density, yielding space-dependent Franck-Condon factors. We discuss the consequent marked effects on transport which are compatible with recent measurements. This picture can be relevant for tunneling experiments in generic nano-electromechanical systems.
We study the quantum transitions of a central spin surrounded by a collective-spin environment. It is found that the influence of the environmental spins on the absorption spectrum of the central spin can be explained with the analog of the Franck-Condon (FC) effect in conventional electron-phonon interaction system. Here, the collective spins of the environment behave as the vibrational mode, which makes the electron to be transitioned mainly with the so-called vertical transitions in the conventional FC effect. The vertical transition for the central spin in the spin environment manifests as, the certain collective spin states of the environment is favored, which corresponds to the minimal change in the average of the total spin angular momentum.
We show that for a quantum system coupled to both vibrational and electromagnetic environments, enforcing additivity of their combined influences results in non-equilibrium dynamics that does not respect the Franck-Condon principle. We overcome this shortcoming by employing a collective coordinate representation of the vibrational environment, which permits the derivation of a non-additive master equation. When applied to a two-level emitter our treatment predicts decreasing photon emission rates with increasing vibrational coupling, consistent with Franck-Condon physics. In contrast, the additive approximation predicts the emission rate to be completely insensitive to vibrations. We find that non-additivity also plays a key role in the stationary non-equilibrium model behaviour, enabling two-level population inversion under incoherent electromagnetic excitation.
We report on a new approach to detect excitonic qubits in semiconductor quantum dots by observing spontaneous emissions from the relevant qubit level. The ground state of excitons is resonantly excited by picosecond optical pulses. Emissions from the same state are temporally resolved with picosecond time resolution. To capture weak emissions, we greatly suppress the elastic scattering of excitation beams, by applying obliquely incident geometry to the micro photoluminescence set-up. Rabi oscillations of the ground-state excitons appear to be involved in the dependence of emission intensity on excitation amplitude.
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