Discovery of ultrafast spontaneous spin switching in an antiferromagnet by femtosecond noise correlation spectroscopy.

Owing to their high magnon frequencies, antiferromagnets are key materials for future high-speed spintronics. Picosecond switching of antiferromagnetic spin systems has been viewed a milestone for decades and pursued only by using ultrafast external perturbations. Here, we show that picosecond spin switching occurs spontaneously due to thermal fluctuations in the antiferromagnetic orthoferrite Sm0.7Er0.3FeO3. By analysing the correlation between the pulse-to-pulse polarisation fluctuations of two femtosecond optical probes, we extract the autocorrelation of incoherent magnon fluctuations. We observe a strong enhancement of the magnon fluctuation amplitude and the coherence time around the critical temperature of the spin reorientation transition. The spectrum shows two distinct features, one corresponding to the quasi-ferromagnetic mode and another one which has not been previously reported in pump-probe experiments. Comparison to a stochastic spin dynamics simulation reveals this new mode as smoking gun of ultrafast spontaneous spin switching within the double-well anisotropy potential.

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.

Broadband interferometric subtraction of optical fields.

We present a Mach-Zehnder-like interferometer capable of simultaneous super-octave (950 - 2100 nm) destructive interference with an intensity extinction of 4 × 10-4. Achromatic nulling is achieved by unbalancing the number of Fresnel reflections off optically denser media in the two interferometer arms. With a methane gas sample in one interferometer arm, we isolate the coherent molecular vibrational emission from the broadband, impulsive excitation and quantitatively examine the potential improvement in detectable concentration, compared to direct transmission geometry. The novel concept will benefit sensing applications requiring high detection sensitivity and dynamic range, including time-domain and frequency-domain spectroscopy.

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.

High-power frequency comb at 2 µm wavelength emitted by a Tm-doped fiber laser system.

We report on the generation of a high-power frequency comb in the 2 µm wavelength regime featuring high amplitude and phase stability with unprecedented laser parameters, combining 60 W of average power with <30 fs pulse duration. The key components of the system are a mode-locked Er:fiber laser, a coherence-preserving nonlinear broadening stage, and a high-power Tm-doped fiber chirped-pulse amplifier with subsequent nonlinear self-compression of the pulses. Phase locking of the system resulted in a phase noise of less than 320 mrad measured within the 10 Hz-30 MHz band and 30 mrad in the band from 10 Hz to 1 MHz.

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.

Signatures of transient Wannier-Stark localization in bulk gallium arsenide.

Many properties of solids result from the fact that in a periodic crystal structure, electronic wave functions are delocalized over many lattice sites. Electrons should become increasingly localized when a strong electric field is applied. So far, this Wannier-Stark regime has been reached only in artificial superlattices. Here we show that extremely transient bias over the few-femtosecond period of phase-stable mid-infrared pulses may localize electrons even in a bulk semiconductor like GaAs. The complicated band structure of a three-dimensional crystal leads to a strong blurring of field-dependent steps in the Wannier-Stark ladder. Only the central step emerges strongly in interband electro-absorption because its energetic position is dictated by the electronic structure at an atomic level and therefore insensitive to the external bias. In this way, we demonstrate an extreme state of matter with potential applications due to e.g., its giant optical non-linearity or extremely high chemical reactivity.

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.

Below-gap excitation of semiconducting single-wall carbon nanotubes.

We investigate the optoelectronic properties of the semiconducting (6,5) species of single-walled carbon nanotubes by measuring ultrafast transient transmission changes with 20 fs time resolution. We demonstrate that photons with energy below the lowest exciton resonance efficiently lead to linear excitation of electronic states. This finding challenges the established picture of a vanishing optical absorption below the fundamental excitonic resonance. Our result points towards below-gap electronic states as an intrinsic property of semiconducting nanotubes.

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.

Nonperturbative interband response of a bulk InSb semiconductor driven off resonantly by terahertz electromagnetic few-cycle pulses.

Intense multiterahertz pulses are used to study the coherent nonlinear response of bulk InSb by means of field-resolved four-wave mixing spectroscopy. At amplitudes above 5 MV/cm the signals show a clear temporal substructure which is unexpected in perturbative nonlinear optics. Simulations based on a model of a two-level quantum system demonstrate that in spite of the strongly off-resonant character of the excitation the high-field few-cycle pulses drive the interband resonances into a nonperturbative regime of Rabi flopping. The rotating wave approximation breaks down in this case and the system reaches a complete population inversion.

Pulse synthesis in the single-cycle regime from independent mode-locked lasers using attosecond-precision feedback.

We report the synthesis of a nearly single-cycle (3.7 fs), ultrafast optical pulse train at 78 MHz from the coherent combination of a passively mode-locked Ti:sapphire laser (6 fs pulses) and a fiber supercontinuum (1-1.4 µm, with 8 fs pulses). The coherent combination is achieved via orthogonal, attosecond-precision synchronization of both pulse envelope timing and carrier envelope phase using balanced optical cross-correlation and balanced homodyne detection, respectively. The resulting pulse envelope, which is only 1.1 optical cycles in duration, is retrieved with two-dimensional spectral shearing interferometry (2DSI). To our knowledge, this work represents the first stable synthesis of few-cycle pulses from independent laser sources.

Optimum photoluminescence excitation and recharging cycle of single nitrogen-vacancy centers in ultrapure diamond.

Important features in the spectral and temporal photoluminescence excitation of single nitrogen-vacancy (NV) centers in diamond are reported at conditions relevant for quantum applications. Bidirectional switching occurs between the neutral (NV(0)) and negatively charged (NV(-)) states. Luminescence of NV(-) is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of NV(0). The dark state of NV(-) is identified as NV(0). A narrow resonance is observed in the excitation spectra at 521 nm, which mediates efficient conversion to NV(0).

Ultrafast transient generation of spin-density-wave order in the normal state of BaFe2As2 driven by coherent lattice vibrations.

The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing order. Here, we employ few-cycle multi-terahertz pulses to resonantly probe the evolution of the spin-density-wave (SDW) gap of the pnictide compound BaFe(2)As(2) following excitation with a femtosecond optical pulse. When starting in the low-temperature ground state, optical excitation results in a melting of the SDW order, followed by ultrafast recovery. In contrast, the SDW gap is induced when we excite the normal state above the transition temperature. Very surprisingly, the transient ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. Our results attest to a pronounced spin-phonon coupling in pnictides that supports rapid development of a macroscopic order on small vibrational displacement even without breaking the symmetry of the crystal.

Ultrashort pulse characterization with a terahertz streak camera.

A phase-locked terahertz transient is exploited as an ultrafast phase gate for femtosecond optical pulses. We directly map out the group delay dispersion of a low-power near-infrared pulse by measuring the electro-optically induced polarization rotation as a function of wavelength. Our experiment covers the spectral window from 1.0 to 1.4 µm and reaches a temporal precision better than 1 fs. A quantitative analysis of the detector response confirms that this streaking technique requires no reconstruction algorithm and is also well suited for the characterization of pulses spanning more than one optical octave.

Femtosecond response of quasiparticles and phonons in superconducting YBa(2)Cu(3)O(7-δ) studied by wideband terahertz spectroscopy.

We measure the anisotropic midinfrared response of electrons and phonons in bulk YBa(2)Cu(3)O(7-δ) after femtosecond photoexcitation. A line shape analysis of specific lattice modes reveals their transient occupation and coupling to the superconducting condensate. The apex oxygen vibration is strongly excited within 150 fs, demonstrating that the lattice absorbs a major portion of the pump energy before the quasiparticles are thermalized. Our results attest to substantial electron-phonon scattering and introduce a powerful concept probing electron-lattice interactions in a variety of complex materials.

Single-cycle multiterahertz transients with peak fields above 10 MV/cm.

Phase-locked single-cycle transients with frequency components between 1 and 60THz and peak fields of up to 12MV/cm are generated as the idler wave of a parametric amplifier. To achieve broadband conversion in GaSe nonlinear crystals, we match the group velocities of signal and idler components. The influence of group-velocity dispersion is minimized by long-wavelength pumping at 1.18mum. Free-space electro-optic sampling monitors the multiterahertz waveforms with direct field resolution.