arXiv subjects

V. A. Apkarian

Publications and source records attributed to V. A. Apkarian.

3 recordsLinked to original sources

arXiv2023

Dynamics of molecular rotors in bulk superfluid helium

Molecules immersed in liquid helium are excellent probes of superfluidity. Their electronic, vibrational and rotational dynamics provide valuable clues about the superfluid at the nanoscale. Here we report on the experimental study of the laser-induced rotation of helium dimers inside the superfluid $^4\mathrm{He}$ bath at variable temperature. The coherent rotational dynamics of $\mathrm{He}_2^*$ is initiated in a controlled way by ultrashort laser pulses, and tracked by means of time-resolved laser-induced fluorescence. We detect the decay of rotational coherence on the nanosecond timescale and investigate the effects of temperature on the decoherence rate. The observed temperature dependence suggests a non-equilibrium evolution of the quantum bath, accompanied by the emission of the wave of second sound. The method offers new ways of studying superfluidity with molecular nano-probes under variable thermodynamic conditions.

quant-ph↗

arXiv2015

Observation and analysis of Fano-like lineshapes in the Raman spectra of molecules adsorbed at metal interfaces

Surface enhanced Raman spectra from molecules (bipyridyl ethylene) adsorbed on gold dumbells are observed to become increasingly asymmetric (Fano-like) at higher incident light intensity. The electronic temperature (inferred from the anti-Stokes (AS) electronic Raman signal increases at the same time while no vibrational AS scattering is seen. These observations are analyzed by assuming that the molecule-metal coupling contains an intensity dependent contribution (resulting from light-induced charge transfer transitions as well as renormalization of the molecule metal tunneling barrier). We find that interference between vibrational and electronic inelastic scattering routes is possible in the presence of strong enough electron-vibrational coupling and can in principle lead to the observed Fano-like feature in the Raman scattering profile. However the best fit to the observed results, including the dependence on incident light intensity and the associated thermal response is obtained from a model that disregards this coupling and accounts for the structure of the continuous electronic component of the Raman scattering signal. The temperatures inferred from the Raman signal are argued to be only of qualitative value.

cond-mat.mes-hall↗

arXiv2001

The manipulation of massive ro-vibronic superpositions using time-frequency-resolved coherent anti-Stokes Raman scattering (TFRCARS): from quantum control to quantum computing

Molecular ro-vibronic coherences, joint energy-time distributions of quantum amplitudes, are selectively prepared, manipulated, and imaged in Time-Frequency-Resolved Coherent Anti-Stokes Raman Scattering (TFRCARS) measurements using femtosecond laser pulses. The studies are implemented in iodine vapor, with its thermally occupied statistical ro-vibrational density serving as initial state. The evolution of the massive ro-vibronic superpositions, consisting of 1000 eigenstates, is followed through two-dimensional images. The first- and second-order coherences are captured using time-integrated frequency-resolved CARS, while the third-order coherence is captured using time-gated frequency-resolved CARS. The Fourier filtering provided by time integrated detection projects out single ro-vibronic transitions, while time-gated detection allows the projection of arbitrary ro-vibronic superpositions from the coherent third-order polarization. Beside the control and imaging of chemistry, the controlled manipulation of massive quantum coherences suggests the possibility of quantum computing. We argue that the universal logic gates necessary for arbitrary quantum computing - all single qubit operations and the two-qubit controlled-NOT (CNOT) gate - are available in time resolved four-wave mixing in a molecule. The molecular rotational manifold is naturally "wired" for carrying out all single qubit operations efficiently, and in parallel. We identify vibronic coherences as one example of a naturally available two-qubit CNOT gate, wherein the vibrational qubit controls the switching of the targeted electronic qubit.

physics.chem-ph↗