Publications

Sum-frequency generation (SFG) allows for coherent upconversion of an electromagnetic signal and has applications in mid-infrared vibrational spectroscopy of molecules. Recent experimental and theoretical studies have shown that plasmonic nanocavities, with their deep sub-wavelength mode volumes, may allow to obtain vibrational SFG signals from a single molecule. In this article, we compute the degree of second order coherence ($g^{(2)}(0)$) of the upconverted mid-infrared field under realistic parameters and accounting for the anharmonic potential that characterizes vibrational modes of individual molecules. On the one hand, we delineate the regime in which the device should operate in order to preserve the second-order coherence of the mid-infrared source, as required in quantum applications. On the other hand, we show that an anharmonic molecular potential can lead to antibunching of the upconverted photons under coherent, Poisson-distributed mid-infrared and visible drives. Our results therefore open a path toward a new kind of bright and tunable source of indistinguishable single photons by leveraging “vibrational blockade” in a resonantly and parametrically driven molecule, without the need for strong light-matter coupling.

Understanding the dynamical consequences of quantum phase transitions on thermodynamical quantities, such as work statistics and entropy production, is one of the most intriguing aspect of quantum many-body systems, pinpointing the emergence of irreversibility to critical features. In this work, we investigate the critical fingerprints appearing in these key thermodynamical quantities for a mean-field critical system undergoing a finite-time cycle, starting from a thermal state at a generic inverse temperature. In contrast to spatially extended systems, the presence of a mean-field critical point in a finite-time cycle leads to constant irreversible work even in the limit of infinitely slow driving. This links with the fact that a slow finite-time cycle results in a constant amount of squeezing, which enables us to derive analytical expressions for the work statistics and irreversible entropy, depending solely on the mean-field critical exponents and the functional form of the control parameter near the critical point. We find that the probability of observing negative work values, corresponding to negative irreversible entropy, is inversely proportional to the time the system remains near to the critical point, and this trend becomes less pronounced the lower the temperature of the initial thermal state. Finally, we determine the irreversibility traits under squeezing generation at zero-temperature using the relative entropy of coherence.