2,375,822 research outputs found
Real-time observation of epitaxial graphene domain reorientation.
Graphene films grown by vapour deposition tend to be polycrystalline due to the nucleation and growth of islands with different in-plane orientations. Here, using low-energy electron microscopy, we find that micron-sized graphene islands on Ir(111) rotate to a preferred orientation during thermal annealing. We observe three alignment mechanisms: the simultaneous growth of aligned domains and dissolution of rotated domains, that is, 'ripening'; domain boundary motion within islands; and continuous lattice rotation of entire domains. By measuring the relative growth velocity of domains during ripening, we estimate that the driving force for alignment is on the order of 0.1 meV per C atom and increases with rotation angle. A simple model of the orientation-dependent energy associated with the moiré corrugation of the graphene sheet due to local variations in the graphene-substrate interaction reproduces the results. This work suggests new strategies for improving the van der Waals epitaxy of 2D materials
Real-time observation of interfering crystal electrons in high-harmonic generation
Accelerating and colliding particles has been a key strategy to explore the
texture of matter. Strong lightwaves can control and recollide electronic
wavepackets, generating high-harmonic (HH) radiation which encodes the
structure and dynamics of atoms and molecules and lays the foundations of
attosecond science. The recent discovery of HH generation in bulk solids
combines the idea of ultrafast acceleration with complex condensed matter
systems and sparks hope for compact solid-state attosecond sources and
electronics at optical frequencies. Yet the underlying quantum motion has not
been observable in real time. Here, we study HH generation in a bulk solid
directly in the time-domain, revealing a new quality of strong-field
excitations in the crystal. Unlike established atomic sources, our solid emits
HH radiation as a sequence of subcycle bursts which coincide temporally with
the field crests of one polarity of the driving terahertz waveform. We show
that these features hallmark a novel non-perturbative quantum interference
involving electrons from multiple valence bands. The results identify key
mechanisms for future solid-state attosecond sources and next-generation
lightwave electronics. The new quantum interference justifies the hope for
all-optical bandstructure reconstruction and lays the foundation for possible
quantum logic operations at optical clock rates
Real-time interactive 3D manipulation of particles viewed in two orthogonal observation planes
Real-time observation of a coherent lattice transformation into a high-symmetry phase
Excursions far from their equilibrium structures can bring crystalline solids
through collective transformations including transitions into new phases that
may be transient or long-lived. Direct spectroscopic observation of
far-from-equilibrium rearrangements provides fundamental mechanistic insight
into chemical and structural transformations, and a potential route to
practical applications, including ultrafast optical control over material
structure and properties. However, in many cases photoinduced transitions are
irreversible or only slowly reversible, or the light fluence required exceeds
material damage thresholds. This precludes conventional ultrafast spectroscopy
in which optical excitation and probe pulses irradiate the sample many times,
each measurement providing information about the sample response at just one
probe delay time following excitation, with each measurement at a high
repetition rate and with the sample fully recovering its initial state in
between measurements. Using a single-shot, real-time measurement method, we
were able to observe the photoinduced phase transition from the semimetallic,
low-symmetry phase of crystalline bismuth into a high-symmetry phase whose
existence at high electronic excitation densities was predicted based on
earlier measurements at moderate excitation densities below the damage
threshold. Our observations indicate that coherent lattice vibrational motion
launched upon photoexcitation with an incident fluence above 10 mJ/cm2 in bulk
bismuth brings the lattice structure directly into the high-symmetry
configuration for tens of picoseconds, after which carrier relaxation and
diffusion restore the equilibrium lattice configuration.Comment: 22 pages, 4 figure
Observation of molecular vibrations in real time
Journal ArticleIn a recent Letter Rosker, Wise, and Tang1 have reported ultrafast optical measurements on two large dye molecules, malachite green and nile blue 690. Using the transmission-correlation technique with 40-fs light pulses, they measured photoinduced changes in optical transmission and found a response consisting of damped oscillations superimposed on two exponential decays. They tentatively interpreted the oscillations as quantum beats between two eigenstates of the isolated molecule. In this Comment we report Raman and infrared measurements on the same molecules and discuss the implications these measurements have for the interpretation of the data of Rosker, Wise, and Tang
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