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Springer series in chemical physics

Chromophore Interacting with Phonons and TLSs Which Are not in Thermal Equilibrium

Игорь Сергеевич Осадько

Published Jan 1, 2003• 1 citation
Publisher
DOI
10.1007/978-3-662-05248-8_20

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Quantum two-level systems (TLSs) intrinsic to glasses induce decoherence in many modern quantum devices, such as superconducting qubits. Although the low-temperature physics of these TLSs is usually well-explained by a phenomenological standard tunneling model of independent TLSs, the nature of these TLSs, as well as their behavior out of equilibrium and at high energies above 1 K, remain inconclusive. Here we measure the non-equilibrium dielectric loss of TLSs in amorphous silicon using a superconducting resonator, where energies of TLSs are varied in time using a swept electric field. Our results show the existence of two distinct ensembles of TLSs, interacting weakly and strongly with phonons, where the latter also possesses anomalously large electric dipole moment. These results may shed new light on the low temperature characteristics of amorphous solids, and hold implications to experiments and applications in quantum devices using time-varying electric fields.
We have carried out a theoretical and numerical study of disorder-induced changes in the absorption line shape of a chromophore embedded in a host matrix. The stochastic sudden jump model is employed wherein the host matrix molecules are treated as noninteracting two-level systems (TLSs) occupying points on a three-dimensional lattice with randomly oriented dipole moments. By systematically controlling the degree of positional disorder (α) attributed to them, a perfectly crystalline (α = 0) or a glassy environment (α = 1) or a combination of the two is obtained. The interaction between the chromophore and the TLSs is assumed to be of the dipole-dipole form. With an increase in α, the broadening of the absorption line shape was found to follow a power-law behavior. More importantly, it is revealed in the long-time limit that the resultant line shape is Gaussian in the absence of disorder but transforms to Lorentzian for a completely disordered environment. For an arbitrarily intermediate value of α, the resultant line shape can be approximately fitted by a linear combination of Gaussian and Lorentzian components. The Lorentzian profile for the disordered medium is attributed to the chomophore-TLS pairs with vanishingly small separation between them.
We present experimental evidence of a thermally-driven amplitude-frequency nonlinearity in a thin-film quartz phononic crystal resonator at millikelvin temperatures. The nonlinear response arises from the coupling of the mechanical mode to an ensemble of microscopic two-level system defects driven out of equilibrium by a microwave drive. In contrast to the conventional Duffing oscillator, the observed nonlinearity exhibits a mixed reactive-dissipative character. Notably, the reactive effect can manifest as either a softening or hardening of the mechanical resonance, depending on the ratio of thermal to phonon energy. By combining the standard TLS theory with a thermal conductance model, the measured power-dependent response is quantitatively reproduced and readout-enhanced relaxation damping from off-resonant TLSs is identified as the primary mechanism limiting mechanical coherence. Within this framework, we delineate the conditions under which similar systems will realize this nonlinearity.