Article
Physics, Multidisciplinary
Denitsa R. Baykusheva, Mona H. Kalthoff, Damian Hofmann, Martin Claassen, Dante M. Kennes, Michael A. Sentef, Matteo Mitrano
Summary: The applicability of using entanglement witnesses and operator-specific quantum bounds to diagnose many-body entanglement in condensed matter systems is investigated. The study focuses on detecting entangled states in quantum systems driven out of equilibrium. The dynamics of a fermion chain undergoing a time-dependent change of the Coulomb interaction is studied using the multipartite entanglement witness, the quantum Fisher information. The results show that the quantum Fisher information can witness distinct signatures of multipartite entanglement both near and far from equilibrium, and these signatures are robust against decoherence. The findings have implications for probing entanglement in light-driven quantum materials with time-resolved optical and x-ray scattering methods.
PHYSICAL REVIEW LETTERS
(2023)
Article
Multidisciplinary Sciences
Liguo Ma, Phuong X. Nguyen, Zefang Wang, Yongxin Zeng, Kenji Watanabe, Takashi Taniguchi, Allan H. MacDonald, Kin Fai Mak, Jie Shan
Summary: This study demonstrates a strongly correlated two-dimensional excitonic insulator ground state in transition metal dichalcogenide semiconductor double layers, providing direct thermodynamic evidence for the state. Capacitance measurements show that the exciton fluid is compressible but charge-incompressible. An exciton phase diagram reveals both the Mott transition and interaction-stabilized quasi-condensation.
Article
Chemistry, Physical
Jerzy Cioslowski, Berthold-Georg Englert, Martin-Isbjoern Trappe, Jun Hao Hue
Summary: At the limit of infinite confinement strength, the ground state of a system containing two interacting fermions or bosons in harmonic confinement remains strongly correlated. The natural orbitals of this system exhibit peculiar properties, such as nonzero collective occupancies for all angular momenta and a relationship with eigenfunctions and eigenvalues of a zero-energy Schrodinger equation with an attractive Gaussian potential. These properties have implications for the decay behavior and energy contributions of the system.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Lifu Zhang, Jie Jiang, Yao Cai, Shukai Yao, Bilal Azhar, Zhizhong Chen, Yang Hu, Saloni Pendse, Yuwei Guo, Ru Jia, Zhiting Tian, Chengliang Sun, Peilin Liao, Jian Shi
Summary: The study demonstrates the significant impact of hydrogenation on the electrical and optical properties of a quasi-2D perovskite niobate, suggesting that altering the orbital occupancy of Nb d orbitals could trigger on-site Coulomb interaction. The observed electrical plasticity induced by hydrogen doping is utilized for simulating neural synaptic activity, shedding light on the role of hydrogen in 4d transition metal oxides and proposing a new avenue for designing novel electronic phases.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Materials Science, Multidisciplinary
A. Shchepetilnikov, A. R. Khisameeva, G. A. Nikolaev, S. A. Lopatina, I. Kukushkin
Summary: We investigate the origin of the anomalous spin resonance detected in a strongly correlated two-dimensional electron system. This resonance is observed near nonmagnetic integer filling factors ν of the quantum Hall effect and is a result of strong electron-electron interactions. We demonstrate that the spin resonance at odd ν leads to an increase in the two-dimensional channel's longitudinal resistance due to radiation absorption-induced heating, while the anomalous resonance at even fillings is observed as a drop in resistance, as if the electron system is cooled.
Article
Materials Science, Multidisciplinary
S. Tsuchiya, H. Taniguchi, J. Yamada, Y. Toda, D. Mihailovic, T. Mertelj
Summary: The study investigates the quench and real-time formation of the Mott state and photoexcited carrier relaxation dynamics in two types of salts using femtosecond optical spectroscopy. The transient reflectivity amplitude gradually recovers over time after strong near-infrared pulse quench, indicating that the energy gap for charge excitations is filled by photoinduced carriers. The Mott state is re-formed on a picosecond timescale with the disappearance of in-gap photodoping-induced states.
Article
Materials Science, Multidisciplinary
Youngjae Kim
Summary: We used time-resolved transient absorption spectroscopy to investigate the ultrafast optical responses of condensed matter systems. We observed unconventional absorption spectra in Mott insulators that do not fully reflect the dynamical Franz-Keldysh effect, unlike in band insulators. These unconventional spectra, characterized by a negative difference absorption and a blueshift, are purely driven by electron correlations, as revealed by decomposed calculation.
Article
Materials Science, Multidisciplinary
A. Shchepetilnikov, A. R. Khisameeva, Yu A. Nefyodov, I. Kukushkin
Summary: The study investigates the spin relaxation of a strongly correlated electron system in a narrow AlAs quantum well near odd fillings of the integer quantum Hall effect. Results show that increasing tilt angle in the magnetic field leads to a significant decrease in relaxation time and alters the dependence of relaxation rate on filling factor at highest tilt angles. The observed effects are attributed to the renormalization of spin excitation spectra by strong electron-electron interactions.
Article
Multidisciplinary Sciences
Sami Dzsaber, Diego A. Zocco, Alix McCollam, Franziska Weickert, Ross McDonald, Mathieu Taupin, Gaku Eguchi, Xinlin Yan, Andrey Prokofiev, Lucas M. K. Tang, Bryan Vlaar, Laurel E. Winter, Marcelo Jaime, Qimiao Si, Silke Paschen
Summary: This paper demonstrates the manipulation of Weyl nodes in momentum space by means of the Zeeman effect in a topological semimetal, and successfully annihilates the nodes. This work is of great importance for systematic exploration of electronic topology and the development of topological quantum devices.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Abhishek Sarkar, Di Wang, Mohana Kante, Luis Eiselt, Vanessa Trouillet, Gleb Iankevich, Zhibo Zhao, Subramshu S. Bhattacharya, Horst Hahn, Robert Kruk
Summary: Technologically relevant strongly correlated phenomena exhibited by perovskite manganites are enhanced by the coexistence of multiple competing magneto-electronic phases. The recently discovered high entropy oxides exhibit indications of an inherent magneto-electronic phase separation encapsulated in a single crystallographic phase. Combining the high entropy concept with standard property control, the study demonstrates the potential for a synergetic development of strongly correlated oxides offered by the high entropy design approach.
ADVANCED MATERIALS
(2023)
Article
Physics, Multidisciplinary
R. J. Koch, R. Sinclair, M. T. McDonnelle, R. Yu, M. Abeykoon, M. G. Tucker, A. M. Tsvelik, S. J. L. Billinge, H. D. Zhou, W-G Yin, E. S. Bozin
Summary: Through examining the local structure of NaTiSi2O6, it was found that there is a preexisting local symmetry breaking before the Ti-dimerization orbital-assisted Peierls transition at 210 K. The dimers evolve into a short range orbital degeneracy lifted (ODL) state with dual orbital character as the temperature increases, persisting up to at least 490 K. The ODL state is correlated over a length scale spanning about 6 sites of the Ti zigzag chains, suggesting that the ODL phenomenology extends to strongly correlated electron systems.
PHYSICAL REVIEW LETTERS
(2021)
Article
Materials Science, Multidisciplinary
Z. E. Krix, O. P. Sushkov
Summary: Recent observations of superconductivity in moire graphene have sparked great interest in the system, and subsequent studies have revealed a more complex phase diagram. In this paper, we propose an alternate system using electrostatically patterned bilayer graphene to induce supermodulation. By varying the gap or modulation strength, we can tune the bilayer graphene into a strongly correlated regime, which is not possible in monolayer graphene. We also present a general technique for addressing Coulomb screening and demonstrate the feasibility of this system experimentally.
Article
Physics, Multidisciplinary
Sebastian Stumper, Michael Thoss, Junichi Okamoto
Summary: In this study, we investigate dynamical quantum phase transitions (DQPTs) in the extended Bose-Hubbard model. We demonstrate that interaction-driven DQPTs can occur after quenches between two topologically trivial insulating phases, which has previously only been studied between gapped and gapless phases. We define a new set of order parameters and find a close connection between DQPTs and these newly defined order parameters for both types of quenches. In addition, we examine the timescales of DQPTs and reveal different types of power laws for the topological and interaction-driven cases.
PHYSICAL REVIEW RESEARCH
(2022)
Article
Chemistry, Physical
Matthew S. Church, Brenda M. Rubenstein
Summary: This article introduces an Auxiliary Field Quantum Monte Carlo (AFQMC) method for real-time modeling of correlated electron dynamics, demonstrating its ability to accurately capture long-lived electronic coherences and showing that simulation times can be lengthened through importance sampling and adaptive active space sampling techniques.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Multidisciplinary Sciences
Shingo Kaneta-Takada, Miho Kitamura, Shoma Arai, Takuma Arai, Ryo Okano, Le Duc Anh, Tatsuro Endo, Koji Horiba, Hiroshi Kumigashira, Masaki Kobayashi, Munetoshi Seki, Hitoshi Tabata, Masaaki Tanaka, Shinobu Ohya
Summary: Researchers have achieved efficient spin-charge current conversion by using a two-dimensional electron gas (2DEG) formed at the interface between SrTiO3 (STO) and oxide insulating layers. The introduction of a strongly correlated perovskite oxide LaTiO3+delta (LTO) interlayer has enabled giant spin-to-charge current conversion efficiencies, highlighting the potential of oxide interfaces for spin-orbitronics applications.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
M. Marini, A. Nardini, R. Martinez Vazquez, C. Conci, M. Bouzin, M. Collini, R. Osellame, G. Cerullo, B. S. Kariman, M. Farsari, E. Kabouraki, M. T. Raimondi, G. Chirico
Summary: Non-linear excitation microscopy has advantages over conventional confocal techniques for in-vivo imaging, but tissue penetration can still be problematic. This study develops and tests fibroblast cell culture plano-convex microlenses for non-linear imaging of biological tissue. The microlenses can be used individually or in an array, and they provide magnified fluorescence images without substantially affecting the signal-to-noise ratio. These results pave the way for optical in-vivo inspection of biological processes using implanted micro-optics.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Saptarshi Chakraborty, Payel Mondal, Mahima Makkar, Luca Moretti, Giulio Cerullo, Ranjani Viswanatha
Summary: Transition metal doping in II-VI semiconductor quantum dots introduces midgap states and adds previously unavailable properties. This study investigates CdS quantum dots doped with different transition metal ions using X-ray absorption fine structure spectroscopy and transient absorption spectroscopy, providing evidence for the origin of magnetization and the importance of ion radius and oxidation state in dopant-anion bond lengths. Based on ultrafast transient absorption spectroscopy, the study proposes photoinduced switching between multiple oxidation states in some dopants.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Vasilis Petropoulos, Ioannis Georgoulis, Chrisovalantou Vourdaki, Peter Hrobarik, Ivica Sigmundova, Jela Nociarova, Margherita Maiuri, Giulio Cerullo, Mihalis Fakis
Summary: This study compares the photophysics and ultrafast dynamics of dipolar and octupolar molecules with benzothiazole acceptors having matched or mismatched orientation. The results show that derivatives with mismatched geometry exhibit stronger fluorescence solvatochromism and faster excited state dynamics. However, introducing an auxiliary acceptor enhances the intramolecular charge transfer for molecules with matched geometry. These findings confirm the crucial role of the relative orientation of the heteroaromatic unit in tuning optical properties and excited state dynamics.
Article
Chemistry, Physical
Samylla Boazegevski, Jeferson Ferreira de Deus, Denis Augusto Turchetti, Leni Campus Akcelrud, Samim Sardar, Cosimo D'Andrea, Franco V. A. Camargo, Giulio Cerullo, Giovanni Bressan, Stephen R. Meech, Ismael A. Heisler
Summary: A detailed photophysical study was conducted on a polymer based on a fluorene derivative using ultrafast nonlinear spectroscopy. The study found significant differences in the photophysical behavior of the polymer in solution and as a film, suggesting a near absence of self-collapsed chain conformations in solution. In the film, interchain interactions promote efficient energy transfer, resulting in faster excited state relaxation compared to solution. The time scales of exciton dynamics revealed in this study are useful for designing blends for optoelectronic and electro-optical devices.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Marco Lamperti, Lucile Rutkowski, Davide Gatti, Riccardo Gotti, Luca Moretti, Dario Polli, Giulio Cerullo, Marco Marangoni
Summary: We discuss the layout and performance of a newly developed high-resolution Stimulated Raman Loss spectrometer for accurate studies of hydrogen isotopologues and Raman active transitions. The spectrometer achieves a frequency accuracy of 50 kHz thanks to frequency comb calibration and active alignment. It allows for shot-noise limited detection, signal enhancement, active flattening of the spectral baseline, and efficient averaging of Raman spectra over long measurement times.
Article
Multidisciplinary Sciences
Fabio Novelli, Kaixuan Chen, Adrian Buchmann, Thorsten Ockelmann, Claudius Hoberg, Teresa Head-Gordon, Martina Havenith
Summary: The study investigates the photo-induced radiolysis of water using an optical-pump terahertz-probe spectroscopy setup, revealing three distinct spectral responses. These responses correspond to the initial diffuse electron, the mass rearrangement of solvent molecules, and the weakening of the solvent cage characterized by the localized electron.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Multidisciplinary
Mattia Trama, Vittorio Cataudella, Carmine Antonio Perroni, Francesco Romeo, Roberta Citro
Summary: The electronic structure of the (111) LaAlO3/SrTiO3 interface was calculated using a tight binding supercell approach. The confinement potential at the interface was evaluated through the iterative solution of a discrete Poisson equation. Local Hubbard electron-electron terms were included at the mean-field level within a fully self-consistent procedure. The calculation accurately described the formation of a two-dimensional electron gas near the interface due to quantum confinement and showed agreement with experimental results.
Article
Chemistry, Physical
Thorsten Ockelmann, Claudius Hoberg, Adrian Buchmann, Fabio Novelli, Martina Havenith
Summary: This study investigates the energy dissipation mechanism in the hydrogen-bonded network of water upon photoexcitation of a photoacid, revealing that energy transfer occurs through acoustic phonon propagation. It is found that the propagation in the water network exhibits long-range correlation with a constant group velocity within the first 10 ps, followed by thermalization and a temperature increase of ΔT = 0.5 degrees C after 300 ps.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Angela Montanaro, Kyu Hyung Park, Francesca Fassioli, Francesca Giusti, Daniele Fausti, Gregory D. Scholes
Summary: In organic bulk heterojunction materials, charge delocalization plays a vital role in generating free carriers. Pump-push-probe experiments with mid-infrared push pulses were performed and identified three types of charge transfer excitons (CTXs): delocalized, localized, and trapped. Delocalized CTXs can be promoted by resonant mid-infrared push pulses, while trapped CTXs are non-responsive. The presence of delocalized CTXs emphasizes the importance of engineering the microstructure and energetics of the donor-acceptor interface in photovoltaic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Vasilis Petropoulos, Lorenzo Uboldi, Margherita Maiuri, Giulio Cerullo, Lara Martinez-Fernandez, Evangelos Balanikas, Dimitra Markovitsi
Summary: The polarity of DNA has been found to have an impact on the relaxation of DNA electronic excited states, with different nucleotide sequences leading to different optical properties.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Piotr Kabacinski, Pietro Marabotti, Daniele Fazzi, Vasilis Petropoulos, Andrea Iudica, Patrick Serafini, Giulio Cerullo, Carlo S. S. Casari, Margherita Zavelani-Rossi
Summary: Investigated the photophysics of one-dimensional linear nanostructures and revealed their excellent mechanical, thermal, and electronic properties. Studied the excited state relaxation processes using experimental and computational methods, providing important insights into photoinduced events in low-dimensional carbon-based materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Multidisciplinary
Andrea Schirato, Mychel G. Silva, Danielle C. Teles-Ferreira, Cristian Manzoni, Ana Maria de Paula, Giulio Cerullo, Giuseppe Della Valle, Marcel Di Vece
Summary: The photoexcitation of plasmonic nanostructures with ultrashort laser pulses allows for understanding the ultrafast nonlinear optical response and fundamental processes triggered by light absorption. The effects of photoexcitation on plasmonic nanostructures are studied using broadband transient absorption spectroscopy and semiclassical nonlinear simulations. The results provide a comprehensive understanding of the thermo-modulational nonlinearities of plasmonic nanostructures exhibiting resonances close to the interband transition threshold.
ADVANCED PHOTONICS RESEARCH
(2023)
Proceedings Paper
Engineering, Electrical & Electronic
Armando Genco, Cristina Cruciano, Matteo Corti, Kirsty E. Mcghee, Benedetto Ardini, Tersilla Virgili, David G. Lidzey, Andrea Bassi, Gianluca Valentini, Giulio Cerullo, Cristian Manzoni
Summary: Fourier-plane optical microscopy is a powerful technique for studying the angularly-resolved optical properties of materials and devices. By combining it with an innovative hyperspectral imaging system, this study provides a new approach for characterizing planar organic microcavities. The system is able to extract angle-resolved hyperspectral information, revealing the parabolic cavity dispersion across the whole Fourier space.
PHOTONIC INSTRUMENTATION ENGINEERING X
(2023)
Article
Chemistry, Multidisciplinary
Claudius Hoberg, Justin J. Talbot, James Shee, Thorsten Ockelmann, Debasish Das Mahanta, Fabio Novelli, Martin Head-Gordon, Martina Havenith
Summary: Photo-induced excited-state proton transfer (ESPT) reactions are important in biological and chemical processes. In this study, optical pump THz probe spectroscopy and molecular dynamics simulations were used to investigate solvation environment changes in different derivatives of pyranine. The results suggest efficient sub-ps energy transfer into a specific solvent mode, promoting proton transfer. Furthermore, damped oscillations in the THz signal indicated vibrational energy transfer between the photoexcited chromophore and solvent molecules.
Article
Materials Science, Multidisciplinary
C. A. Perroni, A. De Canada, V. Cataudella, R. Faizo, G. De Filippis
Summary: This study shows that changing the dissipative environment can alter the characteristics of continuous quantum phase transitions and induce first-order transitions in ferromagnetic spin chains. By coupling the spins to local quantum boson baths, the transition from the second to the first order can be driven even at low dissipation strength. The effective magnetic field induced by dissipation can switch the sign of magnetization and has implications for quantum sensing.
