Femtosecond Transfer and Manipulation of Persistent Hot-Trion Coherence in a Single CdSe/ZnSe Quantum Dot.

Ultrafast transmission changes around the fundamental trion resonance are studied after exciting a p-shell exciton in a negatively charged II-VI quantum dot. The biexcitonic induced absorption reveals quantum beats between hot-trion states at 133 GHz. While interband dephasing is dominated by relaxation of the P-shell hole within 390 fs, trionic coherence remains stored in the spin system for 85 ps due to Pauli blocking of the triplet electron. The complex spectrotemporal evolution of transmission is explained analytically by solving the Maxwell-Liouville equations. Pump and probe polarizations provide full control over amplitude and phase of the quantum beats.

Deterministic Nonlinear Transformations of Phase Noise in Quantum-Limited Frequency Combs.

Optical phase noise of femtosecond lasers is analyzed over various steps of broadband nonlinear frequency conversion. The intrinsic phase jitter of our system originates from quantum statistics in the mode-locked oscillator. Supercontinuum generation by four-wave-mixing processes preserves a noise minimum at the optical carrier frequency. From there, a quadratic increase of the comb linewidth results with mutually anticorrelated phase fluctuations of both spectral wings. Passive phase locking by difference frequency generation strongly enhances the optical phase noise to a level equaling the carrier-envelope phase jitter of the fundamental comb. The same value results from quadratic extrapolation of the optical phase noise to radio frequencies. Our findings are consistent with a fully deterministic transformation of phase noise according to the elastic tape model.

Spectra of Ultrabroadband Squeezed Pulses and the Finite-Time Unruh-Davies Effect.

We study spectral properties of quantum radiation of ultimately short duration. In particular, we introduce a continuous multimode squeezing operator for the description of subcycle pulses of entangled photons generated by coherent-field driving in a thin nonlinear crystal with second-order susceptibility. We find the ultrabroadband spectra of the emitted quantum radiation perturbatively in the strength of the driving field. They can be related to the spectra expected in an Unruh-Davies experiment with a finite time of acceleration. In the time domain, we describe the corresponding behavior of the normally ordered electric field variance.

Multicolor femtosecond pump-probe system with single-electron sensitivity at low temperatures and high magnetic fields.

We present an ultrafast spectroscopy system designed for temporal and spectral resolution of transient transmission changes after excitation of single electrons in solid-state quantum structures. The system is designed for optimum long-term stability, offering the option of hands-off operation over several days. Pump and probe pulses are generated in a versatile Er:fiber laser system where visible photon energies may be tuned independently from 1.90 eV to 2.51 eV in three parallel branches. Bandwidth-limited pulse durations between 100 fs and 10 ps are available. The solid-state quantum systems under investigation are mounted in a closed-cycle superconducting magnet cryostat providing temperatures down to 1.6 K and magnetic fields of up to 9 T. The free-standing cryomagnet is coupled to the laser system by means of a high-bandwidth active beam steering unit to eliminate residual low-frequency mechanical vibrations of the pulse tube coolers. High-NA objective lenses inside the sample chamber are employed for focusing femtosecond laser pulses onto the sample and recollection of the transmission signal. The transmitted probe light is dispersed in a grating monochromator equipped with a liquid nitrogen-cooled CCD camera, enabling a frame rate of 559 Hz. In order to eliminate spurious background effects due to low-frequency changes in the thermal equilibrium of the sample, we operate with a lock-in scheme where, instead of the pump amplitude, the pump-probe timing is modulated. This feature is provided without any mechanical action by an electro-optic timing unit inside the femtosecond Er:fiber system. The performance of the instrument is tested with spectrally resolved pump-probe measurements on a single negatively charged CdSe/ZnSe quantum dot under a magnetic field of 9 T. Selective initialization and readout of charge and spin states is carried out via two different femtosecond laser pulses. High-quality results on subpicosecond intraband relaxation dynamics after single-electron excitation motivate a broad variety of future experiments in ultrafast quantum optics and few-fermion quantum dynamics.

Efficient Emission Enhancement of Single CdSe/CdS/PMMA Quantum Dots through Controlled Near-Field Coupling to Plasmonic Bullseye Resonators.

A strong increase of spontaneous radiative emission from colloidally synthesized CdSe/CdS/PMMA hybrid particles is achieved when manipulated into plasmonic bullseye resonators with the tip of an atomic force microscope (AFM). This type of antenna provides a broadband resonance, which may be precisely matched to the exciton ground state energy in the inorganic cores. Statistically analyzing the spectral photoluminescence (PL) of a large number of individual coupled and uncoupled CdSe/CdS/PMMA quantum dots, we find an order of magnitude of intensity enhancement due to the Purcell effect. Time-resolved PL shows a commensurate increase of the spontaneous emission rate with radiative lifetimes below 230 ps for the bright exciton transition. The combination of AFM and PL imaging allows for sub-200 nm localization of the particle position inside the plasmonic antenna. This capability unveils a different coupling behavior of dark excitonic states: even stronger PL enhancement occurs at positions with maximum spatial gradient of the nearfield, effectively adding a dipolar component to original quadrupole transitions. The broadband maximization of light-matter interaction provided by our nanoengineered compound systems enables an attractive class of future experiments in ultrafast quantum optics.

Subcycle quantum electrodynamics.

Squeezed states of electromagnetic radiation have quantum fluctuations below those of the vacuum field. They offer a unique resource for quantum information systems and precision metrology, including gravitational wave detectors, which require unprecedented sensitivity. Since the first experiments on this non-classical form of light, quantum analysis has been based on homodyning techniques and photon correlation measurements. These methods currently function in the visible to near-infrared and microwave spectral ranges. They require a well-defined carrier frequency, and photons contained in a quantum state need to be absorbed or amplified. Quantum non-demolition experiments may be performed to avoid the influence of a measurement in one quadrature, but this procedure comes at the expense of increased uncertainty in another quadrature. Here we generate mid-infrared time-locked patterns of squeezed vacuum noise. After propagation through free space, the quantum fluctuations of the electric field are studied in the time domain using electro-optic sampling with few-femtosecond laser pulses. We directly compare the local noise amplitude to that of bare (that is, unperturbed) vacuum. Our nonlinear approach operates off resonance and, unlike homodyning or photon correlation techniques, without absorption or amplification of the field that is investigated. We find subcycle intervals with noise levels that are substantially less than the amplitude of the vacuum field. As a consequence, there are enhanced fluctuations in adjacent time intervals, owing to Heisenberg's uncertainty principle, which indicate generation of highly correlated quantum radiation. Together with efforts in the far infrared, this work enables the study of elementary quantum dynamics of light and matter in an energy range at the boundary between vacuum and thermal background conditions.

Direct sampling of electric-field vacuum fluctuations.

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 fluctuations 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.

Paraxial Theory of Direct Electro-optic Sampling of the Quantum Vacuum.

Direct detection of vacuum fluctuations and analysis of subcycle quantum properties of the electric field are explored by a paraxial quantum theory of ultrafast electro-optic sampling. The feasibility of such experiments is demonstrated by realistic calculations adopting a thin ZnTe electro-optic crystal and stable few-femtosecond laser pulses. We show that nonlinear mixing of a short near-infrared probe pulse with the multiterahertz vacuum field leads to an increase of the signal variance with respect to the shot noise level. The vacuum contribution increases significantly for appropriate length of the nonlinear crystal, short pulse duration, tight focusing, and a sufficiently large number of photons per probe pulse. If the vacuum input is squeezed, the signal variance depends on the probe delay. Temporal positions with a noise level below the pure vacuum may be traced with subcycle resolution.