Spatiotemporal Control of Ice Crystallization in Supercooled Water via an Ultrashort Laser Impulse

Takahashi H., Kono T., Sawada K., et al. Spatiotemporal Control of Ice Crystallization in Supercooled Water via an Ultrashort Laser Impulse. Journal of Physical Chemistry Letters, 14(19), 4394-4402, 18 May 2023: © 2023 American Chemical Society. DOI: 10.1021/acs.jpclett.3c00414.Focused irradiation with ultrashort laser pulses realized the fine spatiotemporal control of ice crystallization in supercooled water. An effective multiphoton excitation at the laser focus generated shockwaves and bubbles, which acted as an impulse for inducing ice crystal nucleation. The impulse that was localized close to the laser focus and accompanied by a small temperature elevation allowed the precise position control of ice crystallization and its observation with spatiotemporal resolution of micrometers and microseconds using a microscope. To verify the versatility of this laser method, we also applied it using various aqueous systems (e.g., plant extracts). The systematic study of crystallization probability revealed that laser-induced cavitation bubbles play a crucial role in inducing ice crystal nucleation. This method can be used as a tool for studying ice crystallization dynamics in various natural and biological phenomena

Effect of indium doping on the transient optical properties of GaN films

We have investigated the effects of In doping on the optical properties of GaN films grown by gas-source molecular-beam epitaxy. Time-resolved photoluminescence was carried out to study the transient optical properties of the epitaxial films. In comparison to the undoped GaN film, the spontaneous emission lifetime was prolonged from below 20 to 70 ps by doping with In. Under high-excitation density, stimulated emission was observed from both samples. The threshold excitation density was found to be reduced in the In-doped sample. These significant improvements of the optical properties are attributed to the effective suppression of the formation of the nonradiative recombination centers caused by a change of the growth kinetics induced by a small amount of In supplied during growth of the GaN films

Deterministic Single-Photon and Polarization-Correlated Photon Pair Generations From a Single InAlAs Quantum Dot

Photon emission with nonclassical photon statistics is discussed with a single InAlAs quantum dot. The deterministic single-photon generation in which the emitted photon wavelength matches well to the highly sensitive wavelength region of highly efficient, low-noise Si-single-photon detectors and also to an atmospheric transmission window is demonstrated. Competing transition processes between neutral and charged exciton species originating from an exclusive formation in the same single quantum dot are clarified. It was found that suppressing the charged exciton formation is possible by a quasi-resonant excitation for a deterministic monochromatic single-photon generation. Polarization-dependent photoluminescence spectroscopy clearly indicates the preservation of photon polarizations between photons emitted by biexciton/exciton recombinations. Furthermore, the deterministic polarization-correlated photon pair generation with biexciton-exciton cascaded transition occurring in a single quantum dot is directly confirmed by the polarized second-order photon correlation measurements. This indicates a longer polarization flip time than the exciton lifetime, which is an essential requirement for the deterministic Einstein-Podolsky-Rosen photon pair generation under the present biexciton-exciton cascaded transition scheme

Enhanced Photon Extraction from a Quantum Dot Induced by a Silver Microcolumnar Photon Reflector

We have fabricated silver microcolumnar photon reflectors to enhance the photon extraction efficiency from a quantum dot. The mechanically robust planar structure is favorable to couple to optical fibers for stable and efficient single-photon sources. A high photon extraction efficiency of up to 18% is achieved. Furthermore, strong suppression of multiphoton generation is confirmed. The proposed structure is quite promising toward the implementation of practical quantum key distribution systems with dot-fiber-coupled photon sources

Stable and efficient collection of single photons emitted from a semiconductor quantum dot into a single-mode optical fiber

We study stable and efficient coupling of single photons generated from a quantum dot (QD) into a single-mode fiber (SMF) prepared in a fiber couple module (FCM). We propose a method to focus the objective lens to a sample surface without imaging with the help of laser reflection. By assembling all the constituents, i.e., a pair of lenses, the SMF, and the optical alignment to the QD source, we demonstrate stable single-photon count rate and a high collection efficiency of 43.5% of the photons emitted in air from the QD into the collection lens in the FCM

Triggered single-photon emission and cross-correlation properties in InAlAs quantum dot

Triggered single-photon generation from InAlAs quantum dot (QD) was demonstrated for the first time. Emitted photon energy coincides with high detection efficiency range of Si single-photon detectors, which is highly suitable for free-space communication. Single-QD spectroscopy and crossed photon correlation measurements unambiguously revealed that several emitting lines observed in a single mesa structure originated from the identical QD, and two temporary competing decay processes associated with neutral states and charged states were identified. Presence of the competing process is also inferred from an analysis of steady-state photoluminescence intensities. Formation process of charged exciton in QD is also discussed

Photon Antibunching Observed from an InAlAs Single Quantum Dot

Single-photon emitters and detectors are the key devices to realize secure communications with single-photon-based quantum cryptography and single-photon-based quantum computing. InAlAs quantum dots (QDs) cover the wavelength range with high quantum efficiencies of Si-based single-photon detectors. Clear photon antibunching was observed from an InAlAs single QD under weak excitations. To realize single-photon emitters on demand, complete population of the QD energy states before the photon emission events is necessary, but the measured antibunching properties were dependent substantially on the photo-excitation powers. The physical origin of this problem is discussed and the criterion to distinguish the real deviation from the photon antibunching condition and the artifact of the measurements is clarified. The capability of single-photon emissions on demand will be demonstrated with photon antibunching under pulsed operations