Quantum physics rules the dynamics of small objects as they interact over microscopic length scales.Nevertheless,quantum correlations involving macroscopic distances can be observed between entangled photons as well a...Quantum physics rules the dynamics of small objects as they interact over microscopic length scales.Nevertheless,quantum correlations involving macroscopic distances can be observed between entangled photons as well as in atomic gases and matter waves at low temperatures.The long-range nature of the electromagnetic coupling between charged particles and extended objects could also trigger quantum phenomena over large distances.Here,we reveal a manifestation of quantum mechanics that involves macroscopic distances and results in a nearly complete depletion of coherence associated with which-way free-electron interference produced by electron-radiation coupling in the presence of distant extended objects.This is a ubiquitous effect that we illustrate through a rigorous theoretical analysis of a two-path electron beam interacting with a semi-infinite metallic plate and find the inter-path coherence to vanish proportionally to the path separation at zero temperature and exponentially at finite temperature.The investigated regime of large distances originates in the coupling of the electron to radiative modes assisted by diffraction at material structures but without any involvement of material excitations.Besides the fundamental interest of this macroscopic quantum phenomenon,our results suggest an approach to measuring the vacuum temperature and nondestructively sensing the presence of distant objects.展开更多
Luminescence constitutes a unique source of insight into hot carrier processes in metals,including those in plasmonic nanostructures used for sensing and energy applications.However,being weak in nature,metal luminesc...Luminescence constitutes a unique source of insight into hot carrier processes in metals,including those in plasmonic nanostructures used for sensing and energy applications.However,being weak in nature,metal luminescence remains poorly understood,its microscopic origin strongly debated,and its potential for unraveling nanoscale carrier dynamics largely unexploited.Here,we reveal quantum-mechanical effects in the luminescence emanating from thin monocrystalline gold flakes.Specifically,we present experimental evidence,supported by first-principles simulations,to demonstrate its photoluminescence origin(i.e.,radiative emission from electron/hole recombination)when exciting in the interband regime.Our model allows us to identify changes to the measured gold luminescence due to quantum-mechanical effects as the gold film thickness is reduced.Excitingly,such effects are observable in the luminescence signal from flakes up to 40 nm in thickness,associated with the out-of-plane discreteness of the electronic band structure near the Fermi level.We qualitatively reproduce the observations with first-principles modeling,thus establishing a unified description of luminescence in gold monocrystalline flakes and enabling its widespread application as a probe of carrier dynamics and light-matter interactions in this material.Our study paves the way for future explorations of hot carriers and charge-transfer dynamics in a multitude of material systems.展开更多
基金We thank Archie Howie and Morgan Mitchell for helpful and enjoyable discussions.This work has been supported in part by the European Research Council(Advanced Grant 789104-eNANO)the European Commission(Horizon 2020 Grants No.101017720 FET-Proactive EBEAM and No.964591-SMART-electron)+1 种基金the Spanish MICINN(PID2020-112625GB-I00 and Severo Ochoa CEX2019-000910-S)the Catalan CERCA Program,and Fundaciós Cellex and Mir-Puig.
文摘Quantum physics rules the dynamics of small objects as they interact over microscopic length scales.Nevertheless,quantum correlations involving macroscopic distances can be observed between entangled photons as well as in atomic gases and matter waves at low temperatures.The long-range nature of the electromagnetic coupling between charged particles and extended objects could also trigger quantum phenomena over large distances.Here,we reveal a manifestation of quantum mechanics that involves macroscopic distances and results in a nearly complete depletion of coherence associated with which-way free-electron interference produced by electron-radiation coupling in the presence of distant extended objects.This is a ubiquitous effect that we illustrate through a rigorous theoretical analysis of a two-path electron beam interacting with a semi-infinite metallic plate and find the inter-path coherence to vanish proportionally to the path separation at zero temperature and exponentially at finite temperature.The investigated regime of large distances originates in the coupling of the electron to radiative modes assisted by diffraction at material structures but without any involvement of material excitations.Besides the fundamental interest of this macroscopic quantum phenomenon,our results suggest an approach to measuring the vacuum temperature and nondestructively sensing the presence of distant objects.
基金ARB and FK acknowledge the support of SNSF Eccellenza Grant PCEGP2-194181ARB acknowledges SNSF Swiss Postdoctoral Fellowship TMPFP2_217040 and thanks Valeria Vento and Christophe Galland for the use of a commercial monocrystalline 200 nm gold sample,and Franky Esteban Bedoya Lora for the use of the Ocean Optics spectrometer.+5 种基金ARE,FI and FJGA acknowledge funding from the European Research Council(Advanced Grant No.789104-eNANO)the Spanish MICINN(PID2020-112625 GB-I00 and Severo Ochoa CEX2019-000910-S)the Catalan CERCA Program,and Fundacios Cellex and Mir-Puig.JDC is a Sapere Aude research leader supported by VILLUM FONDEN(Grant no.16498)Independent Research Fund Denmark(Grant no.0165-00051B)The Center for Polariton-driven Light-Matter Interactions(POLIMA)is funded by the Danish National Research Foundation(Project No.DNRF165)First-principles calculations were carried out at the Center for Computational Innovations at Rensselaer Polytechnic Institute.
文摘Luminescence constitutes a unique source of insight into hot carrier processes in metals,including those in plasmonic nanostructures used for sensing and energy applications.However,being weak in nature,metal luminescence remains poorly understood,its microscopic origin strongly debated,and its potential for unraveling nanoscale carrier dynamics largely unexploited.Here,we reveal quantum-mechanical effects in the luminescence emanating from thin monocrystalline gold flakes.Specifically,we present experimental evidence,supported by first-principles simulations,to demonstrate its photoluminescence origin(i.e.,radiative emission from electron/hole recombination)when exciting in the interband regime.Our model allows us to identify changes to the measured gold luminescence due to quantum-mechanical effects as the gold film thickness is reduced.Excitingly,such effects are observable in the luminescence signal from flakes up to 40 nm in thickness,associated with the out-of-plane discreteness of the electronic band structure near the Fermi level.We qualitatively reproduce the observations with first-principles modeling,thus establishing a unified description of luminescence in gold monocrystalline flakes and enabling its widespread application as a probe of carrier dynamics and light-matter interactions in this material.Our study paves the way for future explorations of hot carriers and charge-transfer dynamics in a multitude of material systems.