Felipe Herrera

Cavity-Controlled Chemistry in Molecular Ensembles.

The demonstration of strong and ultrastrong coupling regimes of cavity QED with polyatomic molecules has opened new routes to control chemical dynamics at the nanoscale. We show that strong resonant coupling of a cavity field with an electronic transition can effectively decouple collective electronic and nuclear degrees of freedom in a disordered molecular ensemble, even for molecules with high-frequency quantum vibrational modes having strong electron-vibration interactions. This type of polaron decoupling can be used to control chemical reactions. We show that the rate of electron transfer reactions in a cavity can be orders of magnitude larger than in free space for a wide class of organic molecular species.

External field control of collective spin excitations in an optical lattice of 2Σ molecules

We show that an ensemble of 2Σ molecules in the ro-vibrational ground state trapped on an optical lattice exhibits collective spin excitations that can be controlled by applying superimposed electric and magnetic fields. In particular, we show that the lowest energy excitation of the molecular ensemble at certain combinations of electric and magnetic fields leads to the formation of a magnetic Frenkel exciton. The exciton bandwidth can be tuned by varying the electric or magnetic fields. We show that the exciton states can be localized by creating vacancies in the optical lattice. The localization patterns of the magnetic exciton states are sensitive to the number and distribution of vacancies, which can be exploited for engineering many-body entangled spin states. We consider the dynamics of magnetic exciton wavepackets and show that the spin excitation transfer between molecules in an optical lattice can be accelerated or slowed down by tuning an external magnetic or electric field.

Investigating Polaron Transitions with Polar Molecules

We determine the phase diagram of a polaron model with mixed breathing-mode and Su-Schrieffer-Heeger couplings and show that it has two sharp transitions, in contrast to pure models which exhibit one (for Su-Schrieffer-Heeger coupling) or no (for breathing-mode coupling) transition. We then show that ultracold molecules trapped in optical lattices can be used as a quantum simulator to study precisely this mixed Hamiltonian, and that the relative contributions of the two couplings can be tuned with external electric fields. The parameters of current experiments place them in the region where one of the transitions occurs. We also propose a scheme to measure the polaron dispersion using stimulated Raman spectroscopy.

Dark Vibronic Polaritons and the Spectroscopy of Organic Microcavities

Organic microcavities are photonic nanostructures that strongly confine the electromagnetic field, allowing exotic quantum regimes of light-matter interaction with disordered organic semiconductors. The unambiguous interpretation of the spectra of organic microcavities has been a long-standing challenge due to several competing effects involving electrons, vibrations, and cavity photons. Here we present a theoretical framework that is able to describe the main spectroscopic features of organic microcavities consistently. We introduce a class of light-matter excitations called dark vibronic polaritons, which strongly emit but only weakly absorb light in the same frequency region of the bare electronic transition. A successful comparison with experimental data demonstrates the applicability of our theory. The proposed microscopic understanding of organic microcavities paves the way for the development of optoelectronic devices enhanced by quantum optics.

Absorption and Photoluminescence in Organic Cavity QED

Organic microcavities can be engineered to reach exotic quantum regimes of strong and ultrastrong light-matter coupling. However, the microscopic interpretation of their spectroscopic signals can be challenging due to the competition between coherent and dissipative processes involving electrons, vibrations and cavity photons. We develop here a theoretical framework based on the Holstein-Tavis-Cummings model and a Markovian treatment of dissipation to account for previously unexplained spectroscopic features of organic microcavities consistently. We identify conditions for the formation of dark vibronic polaritons, a new class of light-matter excitations that are not visible in absorption but lead to strong photoluminescence lines. We show that photon leakage from dark vibronic polaritons can be responsible for enhancing photoluminescence at the lower polariton frequency, and also explain the apparent breakdown of reciprocity between absorption and emission in the vicinity of the bare molecular transition frequency. Successful comparison with experimental data demonstrates the applicability of our theory.

Infrared-dressed entanglement of cold open-shell polar molecules for universal matchgate quantum computing

Implementing a scalable quantum information processor using polar molecules in optical lattices requires precise control over the long-range dipole–dipole interaction between molecules in selected lattice sites. We present here a scheme using trapped open-shell polar molecules that allows dipolar exchange processes between nearest and next-nearest neighbors to be controlled in order to construct a generalized transverse Ising spin Hamiltonian with tunable XX, YY and XY couplings in the rotating frame of the driving lasers. The scheme requires a moderately strong bias magnetic field together with near-infrared light to provide local tuning of the qubit energy gap, and mid-infrared pulses to perform rotational state transfer via stimulated Raman adiabatic passage. No interaction between qubits occurs in the absence of the infrared driving. We analyze the fidelity of the resulting two-qubit matchgate, and demonstrate its robustness as a function of the driving parameters. We discuss a realistic application of the system for universal matchgate quantum computing in optical lattices.

Collective effects in linear spectroscopy of dipole-coupled molecular arrays

Author(s): Kocherzhenko, AA; Dawlaty, J; Abolins, BP; Herrera, F; Abraham, DB; Whaley, KB | Abstract: