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arXiv:0805.1633 · Physical Review Letters

Vibronic Spectroscopy of an Artificial Molecule

David Gunnarsson, Jani Tuorila, Antti Paila, Jayanta Sarkar, E. V. Thuneberg, Yuriy Makhlin, Pertti Juhani Hakonen

Published Dec 19, 2008• 13 citations
arXivHTMLPDF

Abstract

We have performed microwave reflection experiments on a charge-phase qubit coupled to an LC oscillator. We find that the system behaves like an artificial molecule showing vibronic sideband transitions. The reflected signal is determined by a combination of the Franck-Condon principle and resolved-sideband cooling or heating of the oscillator.

DOI
10.1103/physrevlett.101.256806

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We have performed microwave reflection experiments on a charge-phase qubit coupled to an LC oscillator. We find that the system behaves like an artificial molecule showing vibronic sideband transitions. The reflected signal is determined by a combination of the Franck-Condon principle and resolved-sideband cooling or heating of the oscillator.
This thesis is a compilation of several works in the area of condensed matter physics, and with devices based on superconducting Josephson junctions (JJ) as the common denominator for the presented projects apart from the work on diffusive systems. Microwave measurements were conducted on a Superconducting Cooper pair transistor to explore its current-phase relationship. Measurements on a JJ-based qubit coupled to a LC resonator revealed the vibronic transitions obeying the Franck-Condon principle. The main body of the thesis is the work done on the Bloch Oscillating Transistor (BOT), an ultra low noise quantum amplifier. In the present work, we investigated the dynamics of the BOT near the bifurcation threshold as well as implemented differential BOTs to check its capability to reject common mode signals. To account for our studies of quantum features in mesoscopic systems other than JJs, we performed an experiment similar to the Hanbury-Brown and Twiss interferometry in optics. For this mesoscopic interference experiment we selected a multiterminal diffusive system. We developed a low temperature noise measurement scheme to study current-current correlations in the GHz frequency range. In our experiments we found a small positive HBT exchange correction factor in the non-interacting limit at low bias voltage in the presence of quantum interference. We found negative exchange correction factor in the hot electron case for similar structures, which agrees well with the theory. Altogether, our experiments demonstrated the theoretically predicted HBT exchange effects in non-interacting and interacting regime of electron transport in a diffusive mesoscopic system.
In addition to the exciting fundamental questions of quantum computing and implementation possibilities of quantum computers, it is important to look for application areas of quantum computing, to point out practical cases which justify the need for this technology. Besides the wellknown qubit-based quantum computers, there are also devices based on other foundations that can surpass the capabilities of classical computers. Among these, devices operating on the basis of boson sampling have a naturally occurring application: the approximate calculation of the vibrational spectrum of molecules. Two separate research groups, Huh et al. [14] and Wang et al. [22] created quantum simulators based on boson sampling, which were successfully used to calculate the transition probabilities between specific states of small molecules. Following the methodology found in these two articles, this paper presents how the calculations of transition probabilities can be performed on a classical computer using a quantum computer simulator which is based on Gaussian boson sampling.
When non-adiabatic coupling mixes electronic states of a molecule, vibronic states of different electronic symmetry become interleaved across the same spectral region. The symmetry of these states cannot be accessed in conventional spectroscopy due to orientation averaging. We show that molecular-frame angular signatures, which are preserved even when states with different symmetry overlap in energy, can be used to resolve them. Using vacuum-ultraviolet transient absorption spectroscopy of aligned carbon dioxide molecules, we separate two electronically distinct classes of vibronic states (A′A^{'}A′ and A′′A^{''}A′′) that arise from Renner-Teller splitting of the 1Δu^1Δ_u1Δu​ state. We reconstruct molecular-frame anisotropy continuously across the vibronic manifold showing that the anisotropy crosses over from perpendicular to parallel transition character and maps the interleaved electronic symmetry landscape. By scanning the femtosecond delay between the VUV and a near-infrared pulse through temporal overlap, we measure symmetry-dependent coherence dephasing times of these states and find that the parallel (A′A^{'}A′) states dephase faster than the perpendicular (A′′A^{''}A′′) states. We attribute this to faster departure of the A′A^{'}A′ wavepacket from the Franck-Condon region due to the distinct topology of the A′A^{'}A′ excited-state surface. These measurements probe symmetry-resolved ultrafast wavepacket dynamics on the coupled excited-state potential energy surfaces.
The absorption spectrum of a system of NNN atoms interacting with a single mode of the quantized radiation field is exactly calculated. Such a spectrum shows vacuum-field Rabi splittings, and thus microwave absorption by Rydberg atoms in a cavity should be a useful way to observe these splittings.
We propose a way to explore the Franck–Condon (FC) physics using a single ion confined in a spin-dependent potential, formed by the combination of a Paul trap and a magnetic field gradient. A correlation between electronic and vibrational degrees of freedom, called electron–vibron coupling, is induced by a non-zero gradient. In the case of a sufficiently strong electron–vibron coupling, FC blockade of low-lying vibronic transitions takes place. We examine the feasibility of observing FC physics in a single trapped ion and demonstrate many potential applications of ionic FC physics in quantum state engineering and quantum information processing.