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result(s) for
"Pareek, Vivek"
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Structure of the moiré exciton captured by imaging its electron and hole
by
Pareek, Vivek
,
Zhu, Xing
,
Heinz, Tony F.
in
639/624/399
,
639/766/119/1000/1018
,
639/925/357/1018
2022
Interlayer excitons (ILXs) — electron–hole pairs bound across two atomically thin layered semiconductors — have emerged as attractive platforms to study exciton condensation
1
–
4
, single-photon emission and other quantum information applications
5
–
7
. Yet, despite extensive optical spectroscopic investigations
8
–
12
, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, in a WSe
2
/MoS
2
heterostructure, we captured images of the time-resolved and momentum-resolved distribution of both of the particles that bind to form the ILX: the electron and the hole. We thereby obtain a direct measurement of both the ILX diameter of around 5.2 nm, comparable with the moiré-unit-cell length of 6.1 nm, and the localization of its centre of mass. Surprisingly, this large ILX is found pinned to a region of only 1.8 nm diameter within the moiré cell, smaller than the size of the exciton itself. This high degree of localization of the ILX is backed by Bethe–Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, allowing the formation of extended arrays of localized excitations for quantum technology.
Imaging the electron and hole that bind to form interlayer excitons in a 2D moiré material enables direct measurement of its diameter and indicates the localization of its centre of mass.
Journal Article
A holistic view of the dynamics of long-lived valley polarized dark excitonic states in monolayer WS2
2025
With their long lifetime and protection against decoherence, dark excitons in monolayer semiconductors offer a promising route for quantum technologies. Optical techniques have previously observed dark excitons with a long-lived valley polarization. However, several aspects remain unknown, such as the populations and time evolution of the different valley-polarized dark excitons and the role of excitation conditions. Here, using time- and angle-resolved photoemission spectroscopy, we obtain a holistic view of the dynamics after valley-selective photoexcitation. By varying experimental conditions, we reconcile between the rapid valley depolarization previously reported in TR-ARPES, and the observation of long-lived valley polarized dark excitons in optical studies. For the latter, we find that momentum-dark excitons largely dominate at early times sustaining a 40% degree of valley polarization, while valley-polarized spin-dark states dominate at longer times. Our measurements provide the timescales and how the different dark excitons contribute to the previously observed long-lived valley polarization in optics.
The authors showcase the capabilities of time-resolved momentum microscopy to image spin- and valley-resolved excitons in monolayer WS₂ with high energy resolution, revealing distinct long-lived, valley-polarized dark excitons that dominate at different timescales.
Journal Article
High Pressure Experimental Studies on CuO: Indication of Re-entrant Multiferroicity at Room Temperature
by
Pareek, Vivek
,
Mukherjee, Goutam Dev
,
Kapri, Sutanu
in
140/133
,
639/301/119/996
,
639/766/119/996
2016
We have carried out detailed experimental investigations on polycrystalline CuO using dielectric constant, dc resistance, Raman spectroscopy and X-ray diffraction measurements at high pressures. Observation of anomalous changes both in dielectric constant and dielectric loss in the pressure range 3.7–4.4 GPa and reversal of piezoelectric current with reversal of poling field direction indicate to a change in ferroelectric order in CuO at high pressures. A sudden jump in Raman integrated intensity of
A
g
mode at 3.4 GPa and observation of Curie-Weiss type behaviour in dielectric constant below 3.7 GPa lends credibility to above ferroelectric transition. A slope change in the linear behaviour of the
A
g
mode and a minimum in the FWHM of the same indicate indirectly to a change in magnetic ordering. Since all the previous studies show a strong spin-lattice interaction in CuO, observed change in ferroic behaviour at high pressures can be related to a reentrant multiferroic ordering in the range 3.4 to 4.4 GPa, much earlier than predicted by theoretical studies. We argue that enhancement of spin frustration due to anisotropic compression that leads to change in internal lattice strain brings the multiferroic ordering to room temperature at high pressures.
Journal Article
Performance-limiting nanoscale trap clusters at grain junctions in halide perovskites
by
Pareek, Vivek
,
Doherty, Tiarnan A. S.
,
Tennyson, Elizabeth M.
in
Clusters
,
Correlation analysis
,
Crystal defects
2020
Halide perovskite materials have promising performance characteristics for low-cost optoelectronic applications. Photovoltaic devices fabricated from perovskite absorbers have reached power conversion efficiencies above 25 per cent in single-junction devices and 28 per cent in tandem devices
1
,
2
. This strong performance (albeit below the practical limits of about 30 per cent and 35 per cent, respectively
3
) is surprising in thin films processed from solution at low-temperature, a method that generally produces abundant crystalline defects
4
. Although point defects often induce only shallow electronic states in the perovskite bandgap that do not affect performance
5
, perovskite devices still have many states deep within the bandgap that trap charge carriers and cause them to recombine non-radiatively. These deep trap states thus induce local variations in photoluminescence and limit the device performance
6
. The origin and distribution of these trap states are unknown, but they have been associated with light-induced halide segregation in mixed-halide perovskite compositions
7
and with local strain
8
, both of which make devices less stable
9
. Here we use photoemission electron microscopy to image the trap distribution in state-of-the-art halide perovskite films. Instead of a relatively uniform distribution within regions of poor photoluminescence efficiency, we observe discrete, nanoscale trap clusters. By correlating microscopy measurements with scanning electron analytical techniques, we find that these trap clusters appear at the interfaces between crystallographically and compositionally distinct entities. Finally, by generating time-resolved photoemission sequences of the photo-excited carrier trapping process
10
,
11
, we reveal a hole-trapping character with the kinetics limited by diffusion of holes to the local trap clusters. Our approach shows that managing structure and composition on the nanoscale will be essential for optimal performance of halide perovskite devices.
Photoemission electron microscopy images of trap states in halide peroskites, spatially correlated with their structural and compositional factors, may help in managing power losses in optoelectronic applications.
Journal Article
A holistic view of the dynamics of long-lived valley polarized dark excitonic states in monolayer WS 2
2025
With their long lifetime and protection against decoherence, dark excitons in monolayer semiconductors offer a promising route for quantum technologies. Optical techniques have previously observed dark excitons with a long-lived valley polarization. However, several aspects remain unknown, such as the populations and time evolution of the different valley-polarized dark excitons and the role of excitation conditions. Here, using time- and angle-resolved photoemission spectroscopy, we obtain a holistic view of the dynamics after valley-selective photoexcitation. By varying experimental conditions, we reconcile between the rapid valley depolarization previously reported in TR-ARPES, and the observation of long-lived valley polarized dark excitons in optical studies. For the latter, we find that momentum-dark excitons largely dominate at early times sustaining a 40% degree of valley polarization, while valley-polarized spin-dark states dominate at longer times. Our measurements provide the timescales and how the different dark excitons contribute to the previously observed long-lived valley polarization in optics.
Journal Article
Visualizing superconductivity in an inversion-symmetry-broken doped Weyl semimetal
by
Olivares, Jorge
,
Pareek, Vivek
,
Dani, Keshav
in
Coherence length
,
Critical field (superconductivity)
,
Elementary excitations
2021
The Weyl semimetal MoTe\\(_2\\) offers a rare opportunity to study the interplay between Weyl physics and superconductivity. Recent studies have found that Se substitution can boost the superconductivity up to 1.5K, but suppress the Td structure phase that is essential for the emergence of Weyl state. A microscopic understanding of possible coexistence of enhanced superconductivity and the Td phase has not been established so far. Here, we use scanning tunneling microscopy (STM) to study a optimally doped new superconductor MoTe\\(_{1.85}\\)Se\\(_{0.15}\\) with bulk Tc ~ 1.5K. By means of quasiparticle interference imaging, we identify the existence of low temperature Td phase with broken inversion symmetry where superconductivity globally coexists. Consistently, we find that the superconducting coherence length, extracted from both the upper critical field and the decay of density of states near a vortex, is much larger than the characteristic length scale of existing dopant derived chemical disorder. Our findings of robust superconductivity arising from a Weyl semimetal normal phase in MoTe\\(_{1.85}\\)Se\\(_{0.15}\\), makes it a promising candidate for realizing topological superconductivity.
Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors
by
Pareek, Vivek
,
E Laine Wong
,
Abdullah Al Mahboob
in
Excitons
,
Holes (electron deficiencies)
,
Momentum
2020
Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of the momentum forbidden dark excitons, and study their properties, including their near-degeneracy with bright excitons and their formation pathways in the energy-momentum landscape. These dark excitons dominate the excited state distribution - a surprising finding that highlights their importance in atomically thin semiconductors.
Driving non-trivial quantum phases in conventional semiconductors with intense excitonic fields
by
Pareek, Vivek
,
Zhu, Xing
,
Bussolotti, Fabio
in
Boson fields
,
Condensed matter physics
,
Cooper pairs
2024
Inducing novel quantum phases and topologies in materials using intense light fields is a key objective of modern condensed matter physics, but nonetheless faces significant experimental challenges. Alternately, theory predicts that in the dense limit, excitons - collective excitations composed of Coulomb-bound electron-hole pairs - could also drive exotic quantum phenomena. However, the direct observation of these phenomena requires the resolution of electronic structure in momentum space in the presence of excitons, which became possible only recently. Here, using time- and angle-resolved photoemission spectroscopy of an atomically thin semiconductor in the presence of a high-density of resonantly and coherently photoexcited excitons, we observe the Bardeen-Cooper-Schrieffer (BCS) excitonic state - analogous to the Cooper pairs of superconductivity. We see the valence band transform from a conventional paraboloid into a Mexican-hat like Bogoliubov dispersion - a hallmark of the excitonic insulator phase; and we observe the recently predicted giant exciton-driven Floquet effects. Our work realizes the promise that intense bosonic fields, other than photons, can also drive novel quantum phenomena and phases in materials.
Moiré-localized interlayer exciton wavefunctions captured by imaging its electron and hole constituents
2021
Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, we captured images of the time- and momentum-resolved distribution of both the electron and the hole that bind to form the ILX in a WSe2/MoS2 heterostructure. We thereby obtain a direct measurement of the interlayer exciton diameter of ~5.4 nm, comparable to the moiré unit-cell length of 6.1 nm. Surprisingly, this large ILX is well localized within the moiré cell to a region of only 1.8 nm - smaller than the size of the exciton itself. This high degree of localization of the interlayer exciton is backed by Bethe-Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, thus allowing the formation of extended arrays of localized excitations for quantum technology.
Experimental measurement of the intrinsic excitonic wavefunction
by
Pareek, Vivek
,
Zhu, Xing
,
E Laine Wong
in
Condensed matter physics
,
Conduction bands
,
Electrons
2020
An exciton, a two-body composite quasiparticle formed of an electron and hole, is a fundamental optical excitation in condensed-matter systems. Since its discovery nearly a century ago, a measurement of the excitonic wavefunction has remained beyond experimental reach. Here, we directly image the excitonic wavefunction in reciprocal space by measuring the momentum distribution of electrons photoemitted from excitons in monolayer WSe2. By transforming to real space, we obtain a visual of the distribution of the electron around the hole in an exciton. Further, by also resolving the energy coordinate, we confirm the elusive theoretical prediction that the photoemitted electron exhibits an inverted energy-momentum dispersion relationship reflecting the valence band where the partner hole remains, rather than that of conduction-band states of the electron.