159 research outputs found
Ultrafast Electronic and Structural Phenomena in Graphite and Graphene
Extended abstract of a paper presented at Microscopy and Microanalysis 2010 in Portland, Oregon, USA, August 1 - August 5, 201
Ultrafast Light and Electrons: Imaging the Invisible
In this chapter, the evolutionary and revolutionary developments of microscopic imaging are overviewed with focus on ultrashort light and electrons pulses; for simplicity, we shall use the term “ultrafast” for both. From Alhazen’s camera obscura, to Hooke and van Leeuwenhoek’s optical micrography, and on to three- and four-dimensional (4D) electron microscopy, the developments over a millennium have transformed humans’ scope of visualization. The changes in the length and time scales involved are unimaginable, beginning with the visible shadows of candles at the centimeter and second scales, and ending with invisible atoms with space and time dimensions of sub-nanometer and femtosecond, respectively. With these advances it has become possible to determine the structures of matter and to observe their elementary dynamics as they fold and unfold in real time, providing the means for visualizing materials behavior and biological function, with the aim of understanding emergent phenomena in complex systems. Both light and light-generated electrons are now at the forefront of femtosecond and attosecond science and technology, and the scope of applications has reached beyond the nuclear motion as electron dynamics become accessible
Experimental Quantum Hamiltonian Learning
Efficiently characterising quantum systems, verifying operations of quantum
devices and validating underpinning physical models, are central challenges for
the development of quantum technologies and for our continued understanding of
foundational physics. Machine-learning enhanced by quantum simulators has been
proposed as a route to improve the computational cost of performing these
studies. Here we interface two different quantum systems through a classical
channel - a silicon-photonics quantum simulator and an electron spin in a
diamond nitrogen-vacancy centre - and use the former to learn the latter's
Hamiltonian via Bayesian inference. We learn the salient Hamiltonian parameter
with an uncertainty of approximately . Furthermore, an observed
saturation in the learning algorithm suggests deficiencies in the underlying
Hamiltonian model, which we exploit to further improve the model itself. We go
on to implement an interactive version of the protocol and experimentally show
its ability to characterise the operation of the quantum photonic device. This
work demonstrates powerful new quantum-enhanced techniques for investigating
foundational physical models and characterising quantum technologies
Single-nanoparticle phase transitions visualized by four-dimensional electron microscopy
The advancement of techniques that can probe the behaviour of individual nanoscopic objects is of paramount importance
in various disciplines, including photonics and electronics. As it provides images with a spatiotemporal resolution,
four-dimensional electron microscopy, in principle, should enable the visualization of single-nanoparticle structural
dynamics in real and reciprocal space. Here, we demonstrate the selectivity and sensitivity of the technique by visualizing
the spin crossover dynamics of single, isolated metal–organic framework nanocrystals. By introducing a small aperture in
the microscope, it was possible to follow the phase transition and the associated structural dynamics within a single
particle. Its behaviour was observed to be distinct from that imaged by averaging over ensembles of heterogeneous
nanoparticles. The approach reported here has potential applications in other nanosystems and those that undergo
(bio)chemical transformations
Femtosecond Coherence and Quantum Control of Single Molecules at Room Temperature
Quantum mechanical phenomena, such as electronic coherence and entanglement,
play a key role in achieving the unrivalled efficiencies of light-energy
conversion in natural photosynthetic light-harvesting complexes, and triggered
the growing interest in the possibility of organic quantum computing. Since
biological systems are intrinsically heterogeneous, clear relations between
structural and quantum-mechanical properties can only be obtained by
investigating individual assemblies. However, single-molecule techniques to
access ultrafast coherences at physiological conditions were not available so
far. Here we show by employing femtosecond pulse-shaping techniques that
quantum coherences in single organic molecules can be created, probed, and
manipulated at ambient conditions even in highly disordered solid environments.
We find broadly distributed coherence decay times for different individual
molecules giving direct insight into the structural heterogeneity of the local
surroundings. Most importantly, we induce Rabi-oscillations and control the
coherent superposition state in a single molecule, thus performing a basic
femtosecond single-qubit operation at room temperature
Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses
Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. Here, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light–matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light–matter) potentials in the strong light–matter coupling regime and bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a route towards ultrafast molecular spectroscopy with plasmonic nanocavitiesThis work has been funded by the European Research Council grant ERC-2016-STG-714870 and the Spanish Ministry for Science, Innovation, and Universities—AEI grants RTI2018-099737-B-I00, PCI2018-093145 (through the QuantERA program of the European Commission), and CEX2018-000805-M (through the María de Maeztu program for Units of Excellence in R&D
The Universal Plausibility Metric (UPM) & Principle (UPP)
<p>Abstract</p> <p>Background</p> <p>Mere possibility is not an adequate basis for asserting scientific plausibility. A precisely defined universal bound is needed beyond which the assertion of <it>plausibility</it>, particularly in life-origin models, can be considered operationally falsified. But can something so seemingly relative and subjective as plausibility ever be quantified? Amazingly, the answer is, "Yes." A method of objectively measuring the plausibility of any chance hypothesis (The Universal Plausibility Metric [UPM]) is presented. A numerical inequality is also provided whereby any chance hypothesis can be definitively falsified when its UPM metric of ξ is < 1 (The Universal Plausibility Principle [UPP]). Both UPM and UPP pre-exist and are independent of any experimental design and data set.</p> <p>Conclusion</p> <p>No low-probability hypothetical plausibility assertion should survive peer-review without subjection to the UPP inequality standard of formal falsification (ξ < 1).</p
Ultrafast-nonlinear ultraviolet pulse modulation in an AlInGaN polariton waveguide operating up to room temperature
Ultrafast nonlinear photonics enables a host of applications in advanced on-chip spectroscopy and information processing. These rely on a strong intensity dependent (nonlinear) refractive index capable of modulating optical pulses on sub-picosecond timescales and on length scales suitable for integrated photonics. Currently there is no platform that can provide this for the UV spectral range where broadband spectra generated by nonlinear modulation can pave the way to new on-chip ultrafast (bio-) chemical spectroscopy devices. We introduce an AlInGaN waveguide supporting highly nonlinear UV hybrid light-matter states (exciton-polaritons) up to room temperature. We experimentally demonstrate ultrafast nonlinear spectral broadening of UV pulses in a compact 100 micrometer long device and measure a nonlinearity 1000 times that in common UV nonlinear materials and comparable to non-UV polariton devices. Our demonstration, utilising the mature AlInGaN platform, promises to underpin a new generation of integrated UV nonlinear light sources for advanced spectroscopy and measurement
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