Light-induced Interactions Research Articles

Impact of Nuclear Motion on Light-Induced Bimolecular Interaction Dynamics

In chemical reactions, the nuclear motion of the molecules plays a crucial role in determining the reaction rates and outcomes. Employing the cold target recoil ion momentum spectroscopy and femtosecond pump-probe techniques, we perform a molecular-level study into the influence of nuclear vibrations on light-induced bimolecular reactions within H2−D2 dimers. The study focuses on the formation dynamics of D2H+ and H2D+ cations, shedding light on the interplay between translational and vibrational motions of the nuclei steering the bimolecular reactions. Our observations reveal a notable yield ratio of 1:1.6 between H2D+ and D2H+ channels, accompanied with a faster formation of D2H+ compared to H2D+. Molecular dynamics simulations unveil that the faster vibrational motion of H2+ than that of D2+ upon single ionization within the dimer accounts for these differences. Our findings provide new insight into the time-resolved kinetic isotope effect on the bimolecular reactions, highlighting the critical relationship between nuclear vibrational motions and reaction dynamics. Published by the American Physical Society 2024

Photoexcited Cryptochrome 1 Interacts With SPCHLESS to Regulate Stomatal Development in Arabidopsis.

Stomata are epidermal openings that facilitate plant-atmosphere gas and water exchange during photosynthesis, respiration and water evaporation. SPEECHLESS (SPCH) is a master basic helix-loop-helix (bHLH) transcription factor that determines the initiation of stomatal development. It is known that blue light promotes stomatal development through the blue light photoreceptor cryptochromes (CRYs, CRY1 and CRY2). Whether CRYs regulate stomatal development through directly modulating SPCH is unknown. Here, we demonstrate by biochemical studies that CRY1 physically interacts with SPCH in a blue light-dependent manner. Genetic studies show that SPCH acts downstream of CRY1 to promote stomatal development in blue light. Furthermore, we show that CRY1 enhances the DNA-binding activity of SPCH and promotes the expression of its target genes in blue light. These results suggest that the mechanism by which CRY1 promotes stomatal development involves positive regulation of the DNA-binding activity of SPCH, which is likely mediated by blue light-induced CRY1-SPCH interaction. The precise regulation of SPCH DNA-binding activity by CRY1 may allow plants to optimize stomatal density and pattern according to ambient light conditions.

Light-Inducible Activation of TrkA for Probing Chronic Pain in Mice.

Chronic pain is a prevalent problem that plagues modern society, and better understanding its mechanisms is critical for developing effective therapeutics. Nerve growth factor (NGF) and its primary receptor, Tropomyosin receptor kinase A (TrkA), are known to be potent mediators of chronic pain, but there is a lack of established methods for precisely perturbing the NGF/TrkA signaling pathway in the study of pain and nociception. Optobiological tools that leverage light-induced protein-protein interactions allow for precise spatial and temporal control of receptor signaling. Previously, our lab reported a blue light-activated version of TrkA generated using light-induced dimerization of the intracellular TrkA domain, opto-iTrkA. In this work, we show that opto-iTrkA activation is able to activate endogenous ERK and Akt signaling pathways and causes the retrograde transduction of phospho-ERK signals in dorsal root ganglion (DRG) neurons. Opto-iTrkA activation also sensitizes the transient receptor potential vanilloid 1 (TRPV1) channel in cellular models, further corroborating the physiological relevance of the optobiological stimulus. Finally, we show that opto-iTrkA enables light-inducible potentiation of mechanical sensitization in mice. Light illumination enables nontraumatic and reversible (<2 days) sensitization of mechanical pain in mice transduced with opto-iTrkA, which provides a platform for dissecting TrkA pathways for nociception in vitro and in vivo.

The Birth of Picophotonics

Picometer-scale events in the nanoworld can be monitored with topologically structured light, while light-induced interactions and picometric movements can underpin time crystals—a new form of functional photonic material.

Symmetry analysis of light-induced magnetic interactions via Floquet engineering

Symmetry analysis of light-induced magnetic interactions via Floquet engineering

Crystalline phases of laser-driven dipolar Bose-Einstein condensates

Although crystallization is a ubiquitous phenomenon in nature, crystal formation and melting still remain fascinating processes with several open questions yet to be addressed. In this work, we study the emergent crystallization of a laser-driven dipolar Bose-Einstein condensate due to the interplay between long-range magnetic and effectively infinite-range light-induced interactions. The competition between these two interactions results in a collective excitation spectrum with two roton minima that introduce two different length scales at which crystalline order can emerge. In addition to the formation of regular crystals with simple periodic patterns due to the softening of one of the rotons, we find that both rotons can also soften simultaneously, resulting in the formation of exotic, complex periodic or aperiodic density patterns. We also demonstrate dynamic state-preparation schemes for achieving all the found crystalline ground states for experimentally relevant and feasible parameter regimes

Photo-thermal catalytic pyrolysis of waste plastics: Investigation into light-induced metal-support interaction

A novel photo-thermal catalytic pyrolysis of LDPE was conducted with a solar simulator for effective and energy-conserving production. Four photothermal catalysts, including TiO2, NiTi(Ni/TiO2), NiAl(Ni/Al2O3) and NiTiAl(Ni/TiO2/Al2O3), were prepared to study the performance on gas and carbonaceous production at variant temperatures (500 °C, 600 °C and 700 °C). NiTiAl reached carbon nanotubes(CNTs) yield of 280 mg/gplastics with simultaneous hydrogen yield of 54 mmol/g even at 700 °C. For the better understanding of light-induced carbon deposition and hydrogen evolution, pyrolysis in pure thermal mode was also carried out over NiTiAl for comparison, where H2 production of 28 mmol/g and little carbon product was found. It turns out that the introduction of irradiation together with support component deliberately mediated the metal-support interaction in NiTiAl by certain photoelectrons transfer, which was favorable for CNTs growth and hydrogen evolution. It is expected to provide a design strategy of catalysts in solar pyrolysis of carbonaceous feedstock.

Nature of the Anomalous Size Dependence of Resonance Red Shifts in Ultrafine Plasmonic Nanoparticles

Plasmonic red shifts of nanoparticles are commonly used in imaging technologies to probe the character of local environments, and the understanding of their dependence on size, shape, and surrounding media has therefore become an important target for research. The red shift of plasmon resonances changes character at about 8–10 nm of size for spherical gold nanoparticles─above this value, the red shift progresses linearly with particle size, while below this size, the red shift changes nonlinearly and more strongly with size. Using an atomistic discrete interaction model, we have studied the special properties of the nanoparticle surface layers and discovered its importance for ultrafine plasmonic nanoparticles and their red shifts. We find that the physical origin for the specific properties inherent to the surface layer of atoms near the nanoparticle boundary is related to the anisotropy of the local environment of atoms in this layer by other atoms. The anisotropy changes the conditions for light-induced nonlocal interactions of neighboring atoms with each other and with the incident radiation compared to the atoms located in the particle core with isotropic nearest surroundings by other atoms. The local anisotropy of the nanoparticle crystal lattice is a geometric factor that increases toward its boundary and that is the most fundamental factor underlying the physical differences between the nanoparticle surface layer and the core material. It is shown that the inflexion point at 8–10 nm is due to a change in the dominant physical origin of the red shift─from chaotization of atomically light-induced dipoles within the surface layer in the case of ultrafine nanoparticles to retardation effects for large nanoparticles in which the relative volume of the surface layer decreases rapidly to a negligible value with increasing nanoparticle size. The patterns revealed are the basis for predicting the manifestation of surface layer effects in ultrafine plasmonic nanoparticles of different shapes and composed of different plasmonic materials.

Purcell-enhanced dipolar interactions in nanostructures

Strong light-induced interactions between atoms are known to cause nonlinearities at a few-photon level, which are crucial for applications in quantum information processing. Compared to free space, the scattering and the light-induced dipolar interaction of atoms can be enhanced by a dielectric environment. For this Purcell effect, either a cavity or a waveguide can be used. Here, we combine the high densities achievable in thermal atomic vapors with an efficient coupling to a slot waveguide. In contrast to free-space interactions, atoms aligned within the slot exhibit repulsive interactions that are further enhanced by a factor of 8 due to the Purcell effect. The corresponding blueshift of the transition frequency of atoms arranged in the essentially one-dimensional geometry vanishes above the saturation, providing a controllable nonlinearity at the few-photon level. The experimental results are in good agreement with Monte Carlo simulations that include the dielectric environment, dipolar interactions, and motional effects. The results pave the way towards a robust scalable platform for quantum nonlinear optics and all-optical quantum information processing at room temperature.

Plasmon-induced excitation energy transfer in silver nanoparticle dimers: A real-time TDDFTB investigation.

Using real-time quantum dynamics calculations, we perform theoretical investigations of light-induced interactions and electronic excitation transfer in a silver nanoparticle dimer. Real-time time-dependent density functional tight-binding (RT-TDDFTB) calculations provide details of the quantum dynamical processes at an electronic/atomistic level with attosecond resolution. The computational efficiency of RT-TDDFTB allows us to examine electronic dynamics up to picosecond time scales. With time scales varying over six orders of magnitude, we provide insight into interactions between the nanoparticle and laser and between nanoparticles. Our results show that the coupling between nanoparticle monomers is dependent on the separation distance between the nanoparticles in the dimer. As the interparticle distance is varied, the dipole-dipole interactions and electronic excitation transfer mechanisms are markedly different. At large distances (from 50 to 20 Å), the energy transfer from NP1 to NP2 becomes more efficient as the interparticle distance decreases. The total dipole moment of the Ag14 nanoparticle dimer increases linearly at an interparticle distance of 20 Å and reaches its maximum after 1.2ps. The electronic excitation transfer is also the most efficient at 20 Å. At short distances, back-transfer effects reduce the ability of the dimer and NP1 to accept energy from the incident electric field. We attribute the distance-dependent features of the nanoparticle dimer to the beating between the laser acting on NP1 and the back transfer from NP2 to NP1.

Effect of Photoreduction of Semiconducting Iron Mineral-Goethite on Microbial Community in the Marine Euphotic Zone.

Marine euphotic zone is the pivotal region for interplay of light-mineral–microorganism and elements cycle, in which semiconducting minerals exist widely and iron-bearing goethite is a typical and widespread one. In this work, we have conducted in-depth researches on the effect of ferrous [Fe(II)] ions dissolved by photoreduction of goethite on microbial community structure and diversity. The mineral phase, structure and morphology of synthesized goethite were characterized by Raman, X-ray diffraction (XRD), energy disperse spectroscopy (EDS), environmental scanning electron microscope (ESEM), and atomic force microscope (AFM). Photoelectrochemical measurements tested photoelectric response and redox activity of goethite, having proved its significant property of photoelectric response with 44.11% increment of the average photocurrent density relative to the dark current density. The photoreduction experiments of goethite were conducted under light condition in simulated seawater. It has suggested the photoreduction of goethite could occur and Fe(III) was reduced to Fe(II). The dissolved Fe(II) from the photoreduction of goethite under light condition was nearly 11 times than that group without light after a 10-day reaction. Furthermore, results of microbial community sequencing analysis indicated that dissolved Fe(II) could affect the structure and regulate the decrease of microbial community diversity. The emergence of dominant bacteria associated with iron oxidation and transport protein has suggested their obvious selectivity and adaptability in the environment with adding dissolved Fe(II). This work revealed the photoreduction process of semiconducting goethite was remarkable, giving rise to a non-negligible dissolved Fe(II) and its selective effect on the structure, diversity, as well as the function of microbial community. This light-induced interaction between minerals and microorganisms may also further regulate correlative metabolic pathways of carbon cycle in the marine euphotic zone.

Signaling Mechanisms by Arabidopsis Cryptochromes.

Cryptochromes (CRYs) are blue light photoreceptors that regulate growth, development, and metabolism in plants. In Arabidopsis thaliana (Arabidopsis), CRY1 and CRY2 possess partially redundant and overlapping functions. Upon exposure to blue light, the monomeric inactive CRYs undergo phosphorylation and oligomerization, which are crucial to CRY function. Both the N- and C-terminal domains of CRYs participate in light-induced interaction with multiple signaling proteins. These include the COP1/SPA E3 ubiquitin ligase, several transcription factors, hormone signaling intermediates and proteins involved in chromatin-remodeling and RNA N6 adenosine methylation. In this review, we discuss the mechanisms of Arabidopsis CRY signaling in photomorphogenesis and the recent breakthroughs in Arabidopsis CRY research.

Photo-Thermal Catalytic Pyrolysis of Waste Plastics: Investigation into Light-Induced Metal-Support Interaction

Photo-Thermal Catalytic Pyrolysis of Waste Plastics: Investigation into Light-Induced Metal-Support Interaction

Hybrid light-matter networks of Majorana zero modes

Topological excitations, such as Majorana zero modes, are a promising route for encoding quantum information. Topologically protected gates of Majorana qubits, based on their braiding, will require some form of network. Here, we propose to build such a network by entangling Majorana matter with light in a microwave cavity QED set-up. Our scheme exploits a light-induced interaction which is universal to all the Majorana nanoscale circuit platforms. This effect stems from a parametric drive of the light-matter coupling in a one-dimensional chain of physical Majorana modes. Our set-up enables all the basic operations needed in a Majorana quantum computing platform such as fusing, braiding, the crucial T-gate, the read-out, and importantly, the stabilization or correction of the physical Majorana modes.

CMInject: Python framework for the numerical simulation of nanoparticle injection pipelines

CMInject simulates nanoparticle injection experiments of particles with diameters in the micrometer to nanometer-regime, e.g., for single-particle-imaging experiments. Particle-particle interactions and particle-induced changes in the surrounding fields are disregarded, due to low nanoparticle concentration in these experiments. CMInject's focus lies on the correct modeling of different forces on such particles, such as fluid-dynamics or light-induced interactions, to allow for simulations that further the scientific development of nanoparticle injection pipelines. To provide a usable basis for this framework and allow for a variety of experiments to be simulated, we implemented first specific force models: fluid drag forces, Brownian motion, and photophoretic forces. For verification, we benchmarked a drag-force-based simulation against a nanoparticle focusing experiment. We envision its use and further development by experimentalists, theorists, and software developers. Program summaryProgram Title: CMInjectCPC Library link to program files:https://doi.org/10.17632/rbpgn4fk3z.1Developer's repository link:https://github.com/cfel-cmi/cminjectCode Ocean capsule:https://codeocean.com/capsule/5146104Licensing provisions: GPLv3Programming language: Python 3Supplementary material: Code to reproduce and analyze simulation results, example input and output data, video files of trajectory moviesNature of problem: Well-defined, reproducible, and interchangeable simulation setups of experimental injection pipelines for biological and artificial nanoparticles, in particular such pipelines that aim to advance the field of single-particle imaging.Solution method: The definition and implementation of an extensible Python 3 framework to model and execute such simulation setups based on object-oriented software design, making use of parallelization facilities and modern numerical integration routines.Additional comments including restrictions and unusual features: Supplementary executable scripts for quantitative and visual analyses of result data are also part of the framework.

Manipulation of brightness and decay kinetics of LuAG: Ce3+ and YAG: Ce3+ by simple metal oxides in polymeric matrices

In this work, light-induced interactions among commercially available green and yellow garnets and wide range opto-emitters of ZnO and CuO have been investigated in terms of excitation, emission and decay kinetics. When the lutetium aluminum garnet (LuAG: Ce3+) is encapsulated along with the nanocrystalline metal oxides in a polymethylmethacrylate (PMMA) matrix, the absorption and emission efficiency of the phosphor enhanced 59-fold compared to its additive-free form. Similarly, when yttrium aluminum garnet (YAG: Ce3+) was incorporated with ZnO and ZnO-CuO nanoparticles, the composites exhibited 6- and 4-fold enhancement in the emission intensities, when excited by the blue light. In parallel to the emission intensities, the external quantum yield (EQY) of LuAG:Ce3+-ZnO-CuO enhanced from 88.4 to 116.4%, with respect to the additive-free-LuAG:Ce3+. Similarly, in YAG:Ce3 + based samples, the presence of the ZnO in the composite resulted in the enhancement of the EQE from 80.6 to 98.1.The steady-state and decay time based experimental studies have confirmed that metal oxides act like donors and phosphors as acceptors when encapsulated in a polymeric matrix at a critical concentration. The decay time of the LuAG: Ce3+ increased from 181to 397 microseconds when embedded along with the ZnO-CuO in the PMMA matrix. Similarly, the decay time of the YAG: Ce3+ extended from 49 to 477 microseconds for the YAG: Ce3+-ZnO composite films.

Optogenetic Control of the Canonical Wnt Signaling Pathway During Xenopus laevis Embryonic Development

Optogenetics uses light-inducible protein-protein interactions to precisely control the timing, localization, and intensity of signaling activity. The precise spatial and temporal resolution of this emerging technology has proven extremely attractive to the study of embryonic development, a program faithfully replicated to form the same organism from a single cell. We have previously performed a comparative study for optogenetic activation of receptor tyrosine kinases, where we found that the cytoplasm-to-membrane translocation-based optogenetic systems outperform the membrane-anchored dimerization systems in activating the receptor tyrosine kinase signaling in live Xenopus embryos. Here, we determine if this engineering strategy can be generalized to other signaling pathways involving membrane-bound receptors. As a proof of concept, we demonstrate that the cytoplasm-to-membrane translocation of the low-density lipoprotein receptor-related protein-6 (LRP6), a membrane-bound coreceptor for the canonical Wnt pathway, triggers Wnt activity. Optogenetic activation of LRP6 leads to axis duplication in developing Xenopus embryos, indicating that the cytoplasm-to-membrane translocation of the membrane-bound receptor could be a generalizable strategy for the construction of optogenetic systems.

Light-induced degradation of SPA2 via its N-terminal kinase domain is required for photomorphogenesis.

Arabidopsis (Arabidopsis thaliana) CONSTITUTIVELY PHOTOMORPHOGENIC1 (COP1) and members of the SUPPRESSOR OF PHYTOCHROMEA-105 (SPA) protein family form an E3 ubiquitin ligase that suppresses light signaling in darkness by polyubiquitinating positive regulators of the light response. COP1/SPA is inactivated by light to allow photomorphogenesis to proceed. Mechanisms of inactivation include light-induced degradation of SPA1 and, in particular, SPA2, corresponding to a particularly efficient inactivation of COP1/SPA2 by light. Here, we show that SPA3 and SPA4 proteins are stable in the light, indicating that light-induced destabilization is specific to SPA1 and SPA2, possibly related to the predominant function of SPA1 and SPA2 in dark-grown etiolating seedlings. SPA2 degradation involves cullin and the COP10-DEETIOLATED-DAMAGED-DNA BINDING PROTEIN (DDB1) CDD complex, besides COP1. Consistent with this finding, light-induced SPA2 degradation required the DDB1-interacting Trp-Asp (WD)-repeat domain of SPA2. Deletion of the N-terminus of SPA2 containing the kinase domain led to strong stabilization of SPA2 in darkness and fully abolished light-induced degradation of SPA2. This prevented seedling de-etiolation even in very strong far-red and blue light and reduced de-etiolation in red light, indicating destabilization of SPA2 through its N-terminal domain is essential for light response. SPA2 is exclusively destabilized by phytochrome A in far-red and blue light. However, deletion of the N-terminal domain of SPA2 did not abolish SPA2-phytochrome A interaction in yeast nor in vivo. Our domain mapping suggests there are two SPA2-phytochrome A interacting domains, the N-terminal domain and the WD-repeat domain. Conferring a light-induced SPA2-phyA interaction only via the WD-repeat domain may thus not lead to COP1/SPA2 inactivation.

Preparation of one-dimensional chains and dense cold atomic clouds with a high numerical aperture four-lens system

We report the efficient and fast ($\sim 2\mathrm{Hz}$) preparation of randomly loaded 1D chains of individual $^{87}$Rb atoms and of dense atomic clouds trapped in optical tweezers using a new experimental platform. This platform is designed for the study of both structured and disordered atomic systems in free space. It is composed of two high-resolution optical systems perpendicular to each other, enhancing observation and manipulation capabilities. The setup includes a dynamically controllable telescope, which we use to vary the tweezer beam waist. A D1 $\Lambda$-enhanced gray molasses enhances the loading of the traps from a magneto-optical trap. Using these tools, we prepare chains of up to $\sim 100$ atoms separated by $\sim 1 \mathrm{\mu m}$ by retro-reflecting the tweezer light, hence producing a 1D optical lattice with strong transverse confinement. Dense atomic clouds with peak densities up to $n_0 = 10^{15}\:\mathrm{at}/\mathrm{cm}^3$ are obtained by compression of an initial cloud. This high density results into interatomic distances smaller than $\lambda/(2\pi)$ for the D2 optical transitions, making it ideal to study light-induced interactions in dense samples.

Enhancing optical properties of Lu3Al5O12:Ce3+ by cost-effective silica-based photonic crystals

Light-induced interactions between a commercially available green phosphor; Lu3Al5O12:Ce3+ (LuAG:Ce3+); and silica photonic crystals (PC) have been investigated in terms of absorption, excitation- and emission-based properties, respectively. The composites were prepared by embedding the phosphorus and other additives homogeneously in a polymethyl methacrylate (PMMA) matrix in form of thin films. When entrapped in the polymer, the additive-free LuAG:Ce3+ exhibited two efficient absorption bands centered at 346 and 450 nm, respectively. A broadband emission at 538 nm and a Stoke’s Shift of 88 nm were observed when excited by blue light; at 450 nm. When the Ce-free and Ce-doped photonic crystals were utilized along with the LuAG:Ce3+, the emission intensities of the composites were enhanced at 19- and 18-fold with respect to the PC-free forms. Additionally, average decay times of the individual phosphor and silica-modified phosphor composites were measured as 64, 550, 772, and 830 µs, respectively.