Toward quantum processing in molecules: A THz-bandwidth coherent memory for light

The unusual features of quantum mechanics are enabling the development of technologies not possible with classical physics. These devices utilize nonclassical phenomena in the states of atoms, ions, and solid-state media as the basis for many prototypes. Here we investigate molecular states as a distinct alternative. We demonstrate a memory for light based on storing photons in the vibrations of hydrogen molecules. The THz-bandwidth molecular memory is used to store 100-fs pulses for durations up to 1ns, enabling 10,000 operational time bins. The results demonstrate the promise of molecules for constructing compact ultrafast quantum photonic technologies.Comment: 5 pages, 3 figures, 1 tabl

Ultrafast slow-light: Raman-induced delay of THz-bandwidth pulses

We propose and experimentally demonstrate a scheme to generate optically-controlled delays based on off-resonant Raman absorption. Dispersion in a transparency window between two neighboring, optically-activated Raman absorption lines is used to reduce the group velocity of broadband 765 nm pulses. We implement this approach in a potassium titanyl phosphate (KTP) waveguide at room temperature, and demonstrate Raman-induced delays of up to 140 fs for a 650-fs duration, 1.8-THz bandwidth, signal pulse; the available delay-bandwidth product is $\approx1$. Our approach is applicable to single photon signals, offers wavelength tunability, and is a step toward processing ultrafast photons.Comment: 5+4 pages, 4+2 figure

Time-bin to Polarization Conversion of Ultrafast Photonic Qubits

The encoding of quantum information in photonic time-bin qubits is apt for long distance quantum communication schemes. In practice, due to technical constraints such as detector response time, or the speed with which co-polarized time-bins can be switched, other encodings, e.g. polarization, are often preferred for operations like state detection. Here, we present the conversion of qubits between polarization and time-bin encodings using a method that is based on an ultrafast optical Kerr shutter and attain efficiencies of 97% and an average fidelity of 0.827+/-0.003 with shutter speeds near 1 ps. Our demonstration delineates an essential requirement for the development of hybrid and high-rate optical quantum networks

Quantum optical signal processing in diamond

Controlling the properties of single photons is essential for a wide array of emerging optical quantum technologies spanning quantum sensing, quantum computing, and quantum communications. Essential components for these technologies include single photon sources, quantum memories, waveguides, and detectors. The ideal spectral operating parameters (wavelength and bandwidth) of these components are rarely similar; thus, frequency conversion and spectral control are key enabling steps for component hybridization. Here we perform signal processing of single photons by coherently manipulating their spectra via a modified quantum memory. We store 723.5 nm photons, with 4.1 nm bandwidth, in a room-temperature diamond crystal; upon retrieval we demonstrate centre frequency tunability over 4.2 times the input bandwidth, and bandwidth modulation between 0.5 to 1.9 times the input bandwidth. Our results demonstrate the potential for diamond, and Raman memories in general, to be an integrated platform for photon storage and spectral conversion.Comment: 6 pages, 4 figure

Time-resolved photoelectron imaging of excited state relaxation dynamics in phenol, catechol, resorcinol and hydroquinone

Time-resolved photoelectron imaging was used to investigate the dynamical evolution of the initially prepared S1 (\u3c0\u3c0*) excited state of phenol (hydroxybenzene), catechol (1,2-dihydroxybenzene), resorcinol (1,3-dihydroxybenzene), and hydroquinone (1,4-dihydroxybenzene) following excitation at 267 nm. Our analysis was supported by ab initio calculations at the coupled-cluster and CASSCF levels of theory. In all cases, we observe rapid (<1 ps) intramolecular vibrational redistribution on the S1potential surface. In catechol, the overall S1 state lifetime was observed to be 12.1 ps, which is 1\u20132 orders of magnitude shorter than in the other three molecules studied. This may be attributed to differences in the H atom tunnelling rate under the barrier formed by a conical intersection between the S1 state and the close lying S2 (\u3c0\u3c3*) state, which is dissociative along the O\u2013H stretching coordinate. Further evidence of this S1/S2 interaction is also seen in the time-dependent anisotropy of the photoelectron angular distributions we have observed. Our data analysis was assisted by a matrix inversion method for processing photoelectron images that is significantly faster than most other previously reported approaches and is extremely quick and easy to implement.Peer reviewed: YesNRC publication: Ye

Storage and retrieval of ultrafast single photons using a room-temperature diamond quantum memory

We report the storage and retrieval of single photons, via a quantum memory, in the optical phonons of room-temperature bulk diamond. The THz-bandwidth heralded photons are generated by spontaneous parametric downconversion and mapped to phonons via a Raman transition, stored for a variable delay, and released on demand. The second-order correlation of the memory output is $g^{(2)}(0) = 0.65 \pm 0.07$, demonstrating preservation of non-classical photon statistics throughout storage and retrieval. The memory is low-noise, high-speed and broadly tunable; it therefore promises to be a versatile light-matter interface for local quantum processing applications.Comment: 6 pages, 4 figure

Storage of polarization-entangled THz-bandwidth photons in a diamond quantum memory

Bulk diamond phonons have been shown to be a versatile platform for the generation, storage, and manipulation of high-bandwidth quantum states of light. Here we demonstrate a diamond quantum memory that stores, and releases on demand, an arbitrarily polarized $\sim$250 fs duration photonic qubit. The single-mode nature of the memory is overcome by mapping the two degrees of polarization of the qubit, via Raman transitions, onto two spatially distinct optical phonon modes located in the same diamond crystal. The two modes are coherently recombined upon retrieval and quantum process tomography confirms that the memory faithfully reproduces the input state with average fidelity $0.784\pm0.004$ with a total memory efficiency of $(0.76\pm0.03)\%$. In an additional demonstration, one photon of a polarization-entangled pair is stored in the memory. We report that entanglement persists in the retrieved state for up to 1.3 ps of storage time. These results demonstrate that the diamond phonon platform can be used in concert with polarization qubits, a key requirement for polarization-encoded photonic processing