Review
Chemistry, Multidisciplinary
Liang Li, Claudia R. R. Prindle, Wanzhuo Shi, Colin Nuckolls, Latha Venkataraman
Summary: Radicals, with their open-shell electronic structures, are unique molecular systems for electronic devices, capable of functioning as conductors and switches in molecular circuits and holding promise in molecular spintronics. However, creating stable and persistent radicals and understanding their properties in molecular junctions pose challenges. This Perspective provides design principles for synthesizing stable radicals relevant to molecular junctions and offers insight into the electronic properties of radicals in single-molecule devices, aiming to facilitate further exploration and development of radical-based molecular systems.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ryo Kawaguchi, Katsushi Hashimoto, Toshiyuki Kakudate, Keiichi Katoh, Masahiro Yamashita, Tadahiro Komeda
Summary: The spintronic properties of magnetic molecules have been widely studied, especially in the context of qubits for quantum information processing. This study focuses on the role of the delocalized pi-radical electron spin in the Pc ligand in reading and intermediating the localized Tb spin qubits. Using electron spin resonance (ESR) technique with a scanning tunneling microscope (STM), the researchers were able to measure the local ESR of a single TbPc2 molecule decoupled from the Cu(100) substrate by a two-monolayer NaCl film. The results indicate that the pi-radical electron is delocalized within the ligands and exhibits intramolecular coupling susceptible to the chemical environment.
Review
Chemistry, Multidisciplinary
Biao-Feng Zeng, Yu-Ling Zou, Gan Wang, Wenjing Hong, Zhong-Qun Tian, Yang Yang
Summary: Recent advances in single-molecule electronics have opened up new opportunities to investigate single-molecule chemistry. The focus has shifted towards quantitative analysis of the physical and chemical behavior of single molecules, including dynamic molecular configurations, redox states, single-molecule reactions, single-molecule sensing, and molecular adsorption behaviors.
Article
Chemistry, Multidisciplinary
Brecht G. Simon, Samer Kurdi, Joris J. Carmiggelt, Michael Borst, Allard J. Katan, Toeno van der Sar
Summary: Nitrogen-vacancy (NV) magnetometry is a new technique for imaging spin waves in magnetic materials. It uses microwave magnetic stray fields to detect spin waves, which decay evanescently on the scale of the spin-wavelength. In this study, nanoscale control of a single NV sensor is used as a wavelength filter to characterize frequency-degenerate spin waves excited by a microstrip in a thin-film magnetic insulator. The results show that despite the one-dimensional microstrip geometry, in-contact scans at low drive power occupy the entire isofrequency contour of the two-dimensional spin-wave dispersion.
Letter
Chemistry, Multidisciplinary
Yahia Chelli, Serena Sandhu, Abdalghani H. S. Daaoub, Sara Sangtarash, Hatef Sadeghi
Summary: It has been found that quantum interference in single molecules can be controlled by changing the spin state of stable open-shell organic radicals, resulting in a significant change in their electrical conductance. This discovery opens up new possibilities for spin interference-based molecular switches for energy storage and conversion applications.
Review
Nanoscience & Nanotechnology
Hongliang Chen, Chuancheng Jia, Xin Zhu, Chen Yang, Xuefeng Guo, J. Fraser Stoddart
Summary: Developing new materials is a long-standing goal in various fields, and understanding single-molecule reactions can deepen our understanding of chemical reactions and provide new frameworks in materials science. This review focuses on state-of-the-art chemical reactions in single-molecule junctions and highlights the advantages of real-time testbeds for studying reaction dynamics, intermediates, transition states, and solvent effects. The behavior of single-molecule reactions is compared with reactions in ensemble states, and the potential of leveraging single-molecule catalysis for large-scale materials production is explored.
NATURE REVIEWS MATERIALS
(2023)
Article
Multidisciplinary Sciences
Qi Zhang, Yuhang Guo, Wentao Ji, Mengqi Wang, Jun Yin, Fei Kong, Yiheng Lin, Chunming Yin, Fazhan Shi, Ya Wang, Jiangfeng Du
Summary: The nitrogen-vacancy (NV) center in diamond is crucial for achieving high-fidelity single-shot readout of qubits, with a new spin-to-charge conversion method introduced to suppress spin-flip errors. This technique shows potential for exceeding fault-tolerant thresholds and may have applications in integrated optoelectronic devices.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Haochuan Mao, Ryan M. Young, Matthew D. Krzyaniak, Michael R. Wasielewski
Summary: This study investigates the spin-dependent dynamics of a covalent donor-acceptor-radical molecule D-A-R·, demonstrating different spin-selective reactions under different temperature and solvent conditions. Time-resolved EPR spectroscopy confirms the highly spin-polarized state of (3)*D-A-R·, highlighting the control of spin states in the same molecule through dielectric environment.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Physics, Multidisciplinary
Zheng-Zhong Zhang, Hao Liu
Summary: A theoretically proposed bias-controlled spin-filter and spin memory involves a single-molecule magnet sandwiched between nonmagnetic and ferromagnetic leads. By applying different voltage pulses, the spin direction of the single-molecule magnet can be controlled and read out using either magneto-resistance or spin current. The device has high spin current polarization (up to 100%) and can be manipulated in a full-electric manner, making it compatible with current technologies and suitable for high-density memory devices.
Article
Chemistry, Physical
Yi Ren, P. J. Hore
Summary: Chiral molecules can act as spin filters, preferentially transmitting electrons with spins polarized along their direction of travel. The magnetic properties of transient radical pairs can optimize the visibility of CISS polarization in time-resolved EPR spectra without the need for orientation or alignment of their precursors.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Nanoscience & Nanotechnology
Chen Yang, Weilin Hu, Xuefeng Guo
Summary: Chirality plays a crucial role in various processes and there is a need for accurate distinction among different chiralities. The article proposes a universal strategy for chirality detection and control by aligning the molecular frame with external stimuli.
NANO-MICRO LETTERS
(2023)
Article
Physics, Multidisciplinary
Fei Gao, Dongzhe Li, Cyrille Barreteau, Mads Brandbyge
Summary: All-electrical writing and reading of spin states can be achieved in molecular spinterfaces by depositing FeTPP molecules, and a feasible three-terminal setup to probe the spin state is proposed. In addition, we demonstrate how FeTPP modifies the quantum transport of non-spin polarized BG.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Haochuan Mao, Gediminas J. Pazera, Ryan M. Young, Matthew D. Krzyaniak, Michael R. Wasielewski
Summary: Researchers have addressed the challenges of achieving good spin-qubit addressability by using a D-A1-A2 molecule with reduced hyperfine couplings. They demonstrated the successful operation of a spin-qubit pair (SQP) in a liquid crystal, performing both single-qubit and two-qubit gate operations.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Environmental
Jin Li, Xia Long, Juexian Cao, Yong Hu
Summary: In this study, the authors achieved the in-situ label-free single-molecule detection of a thermal-reversible Diels-Alder reaction using scanning tunneling microscopy break junction technique. They found that external electric fields can selectively accelerate the forward reaction and stabilize the transition state dipole. The integration of reversible reactions into nanocircuits offers new opportunities for designing functional molecular-scale devices.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Physics, Applied
Jutarat Tanarom, Takuma Watanabe, Yoshinao Mizugaki, Hiroshi Shimada
Summary: We demonstrate that the supercurrent branch of a single Cooper-pair transistor can be used for sensitive phonon detection. The sensitivity of the SCPT detector is approximately 10^3 times higher than that of the traditional superconducting-tunnel-junction detector.
APPLIED PHYSICS EXPRESS
(2022)
Article
Chemistry, Physical
Clemens Vittmann, R. Kevin Kessing, James Lim, Susana F. Huelga, Martin B. Plenio
Summary: This study investigates the nonequilibrium dynamics of electron transmission from a straight waveguide to a helix with spin-orbit coupling. Transmission is found to be spin-selective, leading to large spin polarizations of the itinerant electrons. The degree of spin selectivity depends on the width of the interface region, and no polarization is observed for single-point couplings. The study identifies interface structure and conservation of momentum as crucial factors for chiral-induced spin selectivity, and confirms the robustness of this mechanism against static disorder.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Physics, Multidisciplinary
Eldad Bettelheim, Aditya Banerjee, Martin B. Plenio, Susana F. Huelga
Summary: The statistical mechanics characterization of finite subsystems embedded in an infinite system is a fundamental question in quantum physics. In this study, a mathematical framework based on the Riemann-Hilbert approach is developed to address this problem in the one-dimensional case, where the finite system consists of two disjoint intervals and is analyzed in the thermodynamic limit. The method is demonstrated to be useful for computing the change in the entanglement and negativity spectra, providing insights into the quantum correlation structure and extent in fermionic systems subject to local environments.
JOURNAL OF PHYSICS A-MATHEMATICAL AND THEORETICAL
(2022)
Article
Astronomy & Astrophysics
Kirill Streltsov, Julen Simon Pedernales, Martin Bodo Plenio
Summary: In this study, we investigate the interaction between a harmonic oscillator and a two-level test mass mediated by a local operations and classical communication channel. We demonstrate that a signature, claimed to be exclusive to channels that can transmit quantum information, is generated. By providing an explicit example based on a measurement-and-feedback channel, we explain the failure of the previous proof and discuss the potential applications of setups of this type in testing the nature of gravitational interaction and the fundamental implications an LOCC model of gravity may have in black hole physics.
Article
Quantum Science & Technology
Min Yu, Yu Liu, Pengcheng Yang, Musang Gong, Qingyun Cao, Shaoliang Zhang, Haibin Liu, Markus Heyl, Tomoki Ozawa, Nathan Goldman, Jianming Cai
Summary: This study experimentally demonstrates near saturation of the quantum Cramer-Rao bound in phase estimation of a solid-state spin system. By comparing the experimental uncertainty in phase estimation with the related quantum Fisher information, the researchers provide evidence for the accuracy limit set by the Cramer-Rao bound. This method offers a versatile and powerful tool to explore the Cramer-Rao bound and quantum Fisher information in systems of higher complexity.
NPJ QUANTUM INFORMATION
(2022)
Article
Physics, Multidisciplinary
Evan Meyer-Scott, Nidhin Prasannan, Ish Dhand, Christof Eigner, Viktor Quiring, Sonja Barkhofen, Benjamin Brecht, Martin B. Plenio, Christine Silberhorn
Summary: This study demonstrates the scalable generation of multiphoton entangled states by utilizing active feed-forward and multiplexing, increasing the generation rates and facilitating practical multiphoton protocols for photonic quantum technologies.
PHYSICAL REVIEW LETTERS
(2022)
Article
Physics, Mathematical
Giovanni Ferrari, Ludovico Lami, Thomas Theurer, Martin B. Plenio
Summary: In this study, we examine asymptotic state transformations in continuous variable quantum resource theories. We prove that lower semicontinuity and strong superadditivity can be used to bound asymptotic transformation rates in these settings. We provide applications to optical nonclassicality, entanglement, and quantum thermodynamics resource theories. Our findings offer computable upper bounds for asymptotic transformation rates, including those achievable with linear optical elements.
COMMUNICATIONS IN MATHEMATICAL PHYSICS
(2023)
Article
Chemistry, Physical
Clemens Vittmann, James Lim, Dario Tamascelli, Susana F. Huelga, Martin B. Plenio
Summary: This study examines the role of delocalized phonon modes in electron transport in chiral structures and demonstrates that spin selectivity can originate from spin-dependent energy and momentum conservation in electron-phonon scattering events. The degree of spin polarization, however, depends on environmental factors and the presence of external driving fields. The parametric dependence allows for experimentally testable predictions of the model.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Mathematics, Applied
Andrea Smirne, Dario Tamascelli, James Lim, Martin B. Plenio, Susana F. Huelga
Summary: In this study, we determine the conditions for the equivalence between the multi-time expectation values of a general finite-dimensional open quantum system when interacting with different environments. This non-perturbative evaluation of multi-time expectation values allows for the investigation of open-system multi-time quantities in fully general regimes.
OPEN SYSTEMS & INFORMATION DYNAMICS
(2022)
Article
Quantum Science & Technology
C. Munuera-Javaloy, R. Puebla, B. D'Anjou, M. B. Plenio, J. Casanova
Summary: This article presents a new method for detecting molecular conformational changes using nitroxide electron-spin labels and a nitrogen-vacancy center in diamond. By applying microwave and radiofrequency pulses carefully, stable nitroxide resonances can be achieved. The article also proposes an optimized scheme by using nitroxides with distinct nitrogen isotopes. Additionally, a simple theoretical model is developed and combined with Bayesian inference techniques to demonstrate the ability to detect conformational changes in ambient conditions and extract inter-label distances using the residual effect of random molecular tumbling.
NPJ QUANTUM INFORMATION
(2022)
Article
Physics, Multidisciplinary
Patrick Barthel, Patrick H. Huber, Jorge Casanova, Inigo Arrazola, Dorna Niroomand, Theeraphot Sriarunothai, Martin B. Plenio, Christof Wunderlich
Summary: We demonstrate the experimental implementation of a two-qubit phase gate using a radio frequency controlled trapped-ion quantum processor. The gate is generated by applying a pulsed dynamical decoupling sequence to the ions' carrier transitions, allowing for tunable and high-fidelity phase shift. The gate's performance is robust against various sources of error and holds potential for fast gate speeds.
NEW JOURNAL OF PHYSICS
(2023)
Article
Physics, Multidisciplinary
Alejandro D. Somoza, Nicola Lorenzoni, James Lim, Susana F. Huelga, Martin B. Plenio
Summary: The role of vibrational motion in the charge dynamics of donor-acceptor networks in organic photovoltaics is investigated using non-perturbative simulations. The study addresses the challenge of simulating large electronic-vibrational systems and identifies conditions under which underdamped vibrational motion induces efficient charge separation. The results provide insights into coupling mechanisms and the role of entropic effects, offering a toolbox for designing efficient charge separation pathways in artificial nanostructures.
COMMUNICATIONS PHYSICS
(2023)
Article
Physics, Multidisciplinary
Alastair Marshall, Thomas Reisser, Phila Rembold, Christoph Mueller, Jochen Scheuer, Martin Gierse, Tim Eichhorn, Jakob M. Steiner, Patrick Hautle, Tommaso Calarco, Fedor Jelezko, Martin B. Plenio, Simone Montangero, Ilai Schwartz, Matthias M. Mueller, Philipp Neumann
Summary: This paper utilizes photoexcited triplet state of pentacene-doped naphthalene crystals to polarize surrounding protons and enhance nuclear magnetic resonance signals. Optimal control pulses designed with REDCRAB and a strategy called ARISE are introduced to improve the performance of hyperpolarization sequences.
PHYSICAL REVIEW RESEARCH
(2022)
Article
Optics
Julen S. Pedernales, Martin B. Plenio
Summary: This study designs a method that utilizes spatial correlations to reduce the impact of perturbations from distant sources on the visibility of matter-wave interference patterns, and develops a general framework for correcting the multipole expansion of environmental potential fields. This method works for stochastic field fluctuations at any timescale and does not require quantum correlations.
Article
Quantum Science & Technology
Theodoros Ilias, Dayou Yang, Susana F. Huelga, Martin B. Plenio
Summary: This study proposes a protocol for criticality-enhanced sensing by continuously observing the emitted radiation quanta. The study establishes a scaling theory for the global quantum Fisher information and derives universal scaling laws related to critical exponents. The findings suggest that the precision scaling of continuous detection of emitted quanta exceeds that of direct measurement, indicating the metrological value of this approach in dissipative criticality.
Article
Optics
Giovanni Spaventa, Susana F. Huelga, Martin B. Plenio
Summary: This study combines the concepts of quantum resource theory and divisibility classes of quantum channels to prove that memory effects can increase the efficiency of photoisomerization, which is not achievable under purely thermal Markovian evolution. This provides rigorous evidence that memory effects can serve as a resource in quantum thermodynamics at the nanoscale.
