Strain-Release-Controlled [4 + 2 + 1] Reaction of Cyclopropyl-Capped Diene-ynes/Diene-enes and Carbon Monoxide Catalyzed by Rhodium.

Achieving transition-metal-catalyzed reactions of diene-ynes/diene-enes and carbon monoxide (CO) to deliver [4 + 2 + 1] cycloadducts, rather than the kinetically favored [2 + 2 + 1] products, is challenging. Here, we report that this can be solved by adding a cyclopropyl (CP) cap to the diene moiety of the original substrates. The resulting CP-capped diene-ynes/diene-enes can react with CO under Rh catalysis to give [4 + 2 + 1] cycloadducts exclusively without forming [2 + 2 + 1] products. This reaction has a broad scope and can be used to synthesize useful 5/7 bicycles with a CP moiety. Of the same importance, the CP moiety in the [4 + 2 + 1] cycloadducts can act as an intermediate group for further transformations so that other challenging bicyclic 5/7 and tricyclic 5/7/5, 5/7/6, and 5/7/7 skeletons, some of which are widely found in natural products, can be accessed. The mechanism of this [4 + 2 + 1] reaction has been investigated by quantum chemical calculations, and the role of the CP group in avoiding the possible side [2 + 2 + 1] reaction has been identified, showing that the [4 + 2 + 1] is controlled by releasing the ring strain in the methylenecyclopropyl (MCP) group (about 7 kcal/mol) in the CP-capped dienes.

Proof-of-principle demonstration of compiled Shor's algorithm using a quantum dot single-photon source.

We report a proof-of-principle demonstration of Shor's algorithm with photons generated by an on-demand semiconductor quantum dot single-photon source for the first time. A fully compiled version of Shor's algorithm for factoring 15 has been accomplished with a significantly reduced resource requirement that employs the four-photon cluster state. Genuine multiparticle entanglement properties are confirmed to reveal the quantum character of the algorithm and circuit. The implementation realizes the Shor's algorithm with deterministic photonic qubits, which opens new applications for cluster state beyond one-way quantum computing.

Quantum Beat between Sunlight and Single Photons.

We demonstrate fourth-order quantum beat between sunlight and single photons from a quantum dot. With a fast time-resolved detection system, we observed high-visibility quantum beat between the independent photons of different frequencies from the two astronomically separated light sources. The temporal dynamics of the beat oscillation indicate the coherent behavior of the interfering photons, and the raw visibility of two-photon interference shows violation of the classical limit with a frequency mismatch of three-times the line width.