Alfred Leitenstorfer

The properties of spin fluctuations in antiferromagnets are largely unexplored, in particular at ultrafast timescales. Here, we employ femtosecond noise correlation spectroscopy to experimentally study magnetization fluctuations in the canted antiferromagnet S m 0.7 E r 0.3 Fe O 3 across its spin-reorientation transition and under external magnetic fields. By comparing our measurements to atomistic spin noise and Monte Carlo simulations, we find that the amplitude of the spin noise is governed by the free energy, with stronger fluctuations in regions where the potential landscape softens. We furthermore demonstrate that external magnetic fields suppress spin fluctuations and enhance the quasiferromagnetic magnon frequency by effectively stiffening the potential. These results highlight an effective route for tuning ultrafast magnetization fluctuations via external parameters.

Lightwave-driven scanning tunnelling microscopy (STM) at near-IR frequencies promises an unprecedented combination of atomic spatial resolution and temporal resolution approaching the attosecond range. To achieve this goal, high-sensitivity optical control and detection of sub-cycle tunnelling currents must be achieved at the STM junction. Here, we demonstrate the generation and detection of coherent ultrafast currents across the junction of an STM illuminated by near-infrared single-cycle pulses. We introduce a modulation scheme that avoids time-dependent thermal loading while selectively isolating carrier-envelope phase (CEP)-dependent photocurrents. All artifacts arising from periodic modulation of laser power and thermal coupling are efficiently suppressed, enabling a clean readout of the coherent portion of the ultrafast tunneling current.

Spin fluctuations are an important issue for the design and operation of future spintronic devices. Femtosecond noise-correlation spectroscopy (FemNoC) was recently applied to detect ultrafast magnetization fluctuations. FemNoC gives direct access to the spontaneous fluctuations of magnetization in magnetically ordered materials. In FemNoC experiments, the magnetic fluctuations are imprinted on the polarization state of two independent femtosecond probe pulses upon transmission through a magnetic sample. Using a subharmonic demodulation scheme, the cross-correlation of the signals from both pulse trains is calculated. Here, we quantitatively link the FemNoC output signal to an optical polarization rotation, and then in turn to the magnitude of the inherent spin fluctuations. To this end, three different calibration protocols are presented and compared in accuracy. Ultimately, we quantitatively determine both the variance of optical polarization noise in rad 2 and that of the ultrafast magnetization fluctuations in ( A / m ) 2 .

Sustaining the growth of the data volume generated by artificial intelligence and the internet of things demands to develop schemes for data storage and processing operating at terahertz frequencies, unrestrained by thermal throttling. The optical drive of coherent magnetic collective excitations, namely magnons, represents a promising route. The ability to arbitrarily and nonthermally increase the magnon frequencies with laser pulses could enable this progress. However, this effect has not been reported to date. To achieve it, here, we explore the optical resonant excitation of high-momentum magnons, which experimentally are observed to couple to low-momentum magnons, modifying the frequencies and amplitudes thereof. This evidence, not caused by laser heating, is explained with a resonant light-scattering mechanism coupling high- and low-momentum eigenmodes across momentum space. Our results disclose routes to inducing instabilities and phase transitions via mode softening and potentially even light-driven Bose-Einstein condensation of magnons and superconductivity mediated by high-momentum spin-fluctuations.

Femtosecond frequency combs uniquely combine high frequency resolution, wide spectral coverage, and the ability to generate single‐cycle pulses, rendering them essential for fundamental research and applied photonics. However, effective dispersion management across vast bandwidths remains a major challenge, often requiring complex setups that compromise stability and efficiency. Here, a coherent comb spectrum is presented with an unprecedented bandwidth of 1 PHz, spanning from the deep ultraviolet (280 nm) to the mid‐infrared (2700 nm). This output is generated by a compact fiber device pumped by an ultrastable Er:fiber system. By integrating two highly nonlinear fibers with distinct germanium doping and waveguide design, a flat dispersion profile is achieved across the entire mid‐ and near‐infrared spectral region. This pulse purification technology facilitates efficient third‐harmonic generation within the same nonlinear device enabling the synthesis of ultrashort pulses with an exceptionally clean temporal envelope. Using a novel spectral filter and customized chirped mirrors, single‐cycle near‐infrared pulses with a duration of 3.56 fs are obtained. Beat signals between the fundamental dispersive wave and its third harmonic exhibit exceptional long‐term passive stability, underpinning the reliability of this concept. This compact and versatile approach marks a significant leap forward in the generation and control of coherent supercontinua.

Full characterization of electric-field waveforms in amplitude and phase is achieved across the terahertz to visible spectral range through interaction with an optical pulse shorter than a half-cycle period via the Pockels (linear electro-optic) effect. This technique of electro-optic sampling has become an indispensable tool in various areas, including ultrafast pump-probe, time-domain and frequency-comb spectroscopies, quantum optics, high-harmonic generation, and attosecond science, and holds great promise for further advances. Not only does it enable spectroscopic measurements with record dynamic range and temporal resolution, along with massively parallel real-time spectral data acquisition, but its remarkable sensitivity also allows the detection of vacuum fluctuations, i.e., “zero-point motion” of electric fields, profoundly impacting our understanding of the fundamental laws of nature.

Although often viewed as detrimental, fluctuations carry valuable information about the physical system from which they emerge. Femtosecond noise correlation spectroscopy (FemNoC) has recently been established to probe the ultrafast fluctuation dynamics of thermally populated magnons by measurement of their amplitude autocorrelation. Subharmonic lock-in detection is the key technique in this method, allowing us to extract the pulse-to-pulse polarization fluctuations of two femtosecond optical pulse trains transmitted through a magnetic sample. Here, we present a thorough technical description of the subharmonic demodulation technique and the FemNoC measurement system. We mathematically model the data acquisition process and identify the essential parameters that critically influence the signal-to-noise ratio of the signals. Comparing the model calculations to real datasets allows validating the predicted parameter dependences and provides a means to optimize FemNoC experiments.

Compact and broadband mid-infrared (MIR) sources are in high demand because of a wide range of potential applications such as molecular sensing in the fingerprint region. The generation of coherent MIR radiation at arbitrary frequencies typically requires nonlinear mixing between at least two input waves, which is often cumbersome to implement. We present an integrated and, therefore, adjustment-free solution combining few-femtosecond pulse compression in a germanosilicate optical fiber and optical rectification. To this end, a 16-μm-thin GaSe crystal is directly mounted on the end facet of a highly nonlinear fiber assembly exploiting a focused ion beam. With input pulses of a minute energy of 5 nJ and a duration of 120 fs at the telecom wavelength of 1.55 μm, we directly obtain ultrabroadband and phase-stable output transients. Electro-optic sampling in free space reveals single-cycle pulses with spectral components covering the entire MIR from 10 to 120 THz.

Electro-optic sampling of infrared electric fields has set sensitivity and dynamic-range records in broadband molecular vibrational spectroscopy. Yet, in these works, the 1-second-scale single-trace acquisition time leads to intra-scan noise accumulation and restricts the throughput in measurements of multiple samples and of dynamic processes. We present a dual-laser-oscillator approach capturing 2800 mid-infrared waveforms per second by scanning the relative delay between the sampled waveform and the gate pulses using a modulated repetition-frequency lock. The new technique of electro-optic delay tracking (EODT) provides delay calibration with down to few-attosecond precision and provides a general route to high-precision dual-oscillator spectroscopy with picosecond delay ranges. Our work has immediate applications in, e.g., precision electric-field metrology and high-speed biosensing.