The ground state of quantum systems is characterized by zero-point motion. This motion, in the form of vacuum fluctuations, is generally considered to be an elusive phenomenon that manifests itself only indirectly. Here, we report direct detection of the vacuum fl uctuations of electromagnetic radiation in free space. The ground·state electric-field variance is inversely proportional to the four-dimensional space·time volume, which we sampled electro-optically with tightly focused laser pulses lasting a few femtoseconds. Subcycle temporal readout and nonlinear coupling far from resonance provide signals from purely virtual photons without amplification. Our findings enable an extreme time-domain approach to quantum physics, with nondestructive access to the quantum state of light. Operating at multiterahertz frequencies, such techniques might also allow time-resolved studies of intrinsic fluctuations of elementarY excitations in condensed matter. The quantum properties of light (10) are typi calJy analyzed either by phcton oorrelation (11 14), bomodyning (15 18), or hybrid measurements (19). In those approaches, information is averaged over multiple cycles, and aocessing the vacuum state requires amplification. Femtnsecond studies still rely on pulse envelopes that vary slowly relative tn the carrier frequency (20 23). In our work, we directly probed the varuum noise of the electric field on a subcycle time scale using laser pulses lasting a few femtnseoonds. In ultrabroad band electro optic sampling (24 27), a horizon tally polarized electric field waveform (red in Fig. lA) propagates through an electro optic crystal (EOX), inducing a change Lln of the linear re fractive index 11.o that is proportional to its local amplitude Em:. (Fig. lA and fig. SI). The geometty is adjusted so that a new index ellipsoid emerges under46°tothe polarization of Ern., with nv and nr = 11.o :1:: !!:.n. An ultrashort optical probe pulse at a much higher carrier frequency vp (green in Fig. 1A; intensity, I p, electric field, E.J coprop~ with Em~ at a variable delay time td. The envelope ·of!Pbastn be on theorderofhalfacycle oflightat the highest frequencies il/2rt of En~ that are detected. We used probe pulses as short as tp = 5.8 fs, oorresponding tn Jess than L5 optical cycles at vp = 255 1Hz ( fig. 82). Upon passage through the EOX, the a! andy' components of Ep acquire a relative phase delay proportional to Lln and Eml.,td). The final polarizatim state of the probe is analyzed with ellipsometry. The differential photn rurrent 111/I is proportional tn the electric field Eml.,t,V. We used a radio frequency lock in ampli tier (R.FLA) for readout.We a
'Blinking', or 'fluorescence intermittency', refers to a random switching between 'ON' (bright) and 'OFF' (dark) states of an emitter; it has been studied widely in zero-dimensional quantum dots and molecules, and scarcely in one-dimensional systems. A generally accepted mechanism for blinking in quantum dots involves random switching between neutral and charged states (or is accompanied by fluctuations in charge-carrier traps), which substantially alters the dynamics of radiative and non-radiative decay. Here, we uncover a new type of blinking effect in vertically stacked, two-dimensional semiconductor heterostructures, which consist of two distinct monolayers of transition metal dichalcogenides (TMDs) that are weakly coupled by van der Waals forces. Unlike zero-dimensional or one-dimensional systems, two-dimensional TMD heterostructures show a correlated blinking effect, comprising randomly switching bright, neutral and dark states. Fluorescence cross-correlation spectroscopy analyses show that a bright state occurring in one monolayer will simultaneously lead to a dark state in the other monolayer, owing to an intermittent interlayer carrier-transfer process. Our findings suggest that bilayer van der Waals heterostructures provide unique platforms for the study of charge-transfer dynamics and non-equilibrium-state physics, and could see application as correlated light emitters in quantum technology.
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