Ultrafast Photophysics of Single-Walled Carbon Nanotubes

Single-walled carbon nanotubes (SWNTs) are nanocylinders obtained by wrapping one layer of graphene; due to their very high aspect ratio, they are the prototypical quantum confined one-dimensional systems. The unique mechanical, electronic, and optical properties of SWNTs open up transversal application possibilities in many fields of science and technology, with particular emphasis on optoelectronics and photonics. A prerequisite for many of these applications is a thorough understanding of the nature and dynamics of their elementary excitations. This review aims at summarizing the current understanding of the ultrafast photophysics of SWNTs, based on two decades of experimental investigations. After discussing the morphological and electronic properties of SWNTs and introducing the different photogenerated species, we will briefly describe the ultrafast spectroscopic techniques most commonly used for their characterization. Finally, we present the experimental evidence that has led to establish the nature (singlet and triplet excitons, bi-excitons, trions, and free charges) and the relaxation pathways of photoexcitations in SWNTs

Fourier transform spectroscopy in the vibrational fingerprint region with a birefringent interferometer

We introduce a birefringent interferometer for Fourier transform (FT) spectroscopy in the mid-infrared, covering the vibrational fingerprint region (5-10 μm, 1000-2000 cm-1), which is crucial for molecular identification. Our interferometer employs the crystal calomel (Hg2Cl2), which combines high birefringence (ne-no≈0.55) with a broad transparency range (0.38-20 μm). We adopt a design based on birefringent wedges, which is simple and compact and guarantees excellent delay accuracy and long-term stability. We demonstrate FTIR spectroscopy, with a frequency resolution of 3 cm-1, as well as two-dimensional IR (2DIR) spectroscopy. Our setup can be extended to other spectroscopic modalities such as vibrational circular dichroism and step-scan FT spectroscopy

Double waveguide couplers produced by simultaneous femtosecond writing

We report on a novel method to create waveguide coupler devices in fused silica by combining the technique of beam shaping with femtosecond laser writing. The method is based on a programmable phase modulator and a dynamic variation of the phase-pattern during the writing process. The major advantage is the possibility to create complex devices in a single sweep by simultaneously writing two or more waveguides with changing separation. The guiding properties and the coupling behavior between the waveguides are investigated

Standoff detection of bacterial spores by field deployable coherent Raman spectroscopy

: Vibrational spectroscopies offer great potential for standoff detection of chemical and biological warfare agents, avoiding contamination to the operator and equipment. Among them, particularly promising is Coherent anti-Stokes Raman scattering (CARS) spectroscopy, using synchronized pump/Stokes laser pulses to set up a vibrational coherence of target molecules at a laser focus, which is read by further interaction with a probe pulse, resulting in the emission of a coherent beam detectable at a distance. CARS has previously demonstrated the capability to detect bacterial spores based on the Raman spectrum of the characteristic molecule calcium dipicolinate (CaDPA); however, a complex and bulky laser technology, which is only suitable for a laboratory environment, was employed. Here we develop a broadband CARS setup based on a compact, industrial grade ytterbium laser system. We demonstrate high signal-to-noise ratio detection of Bacillus atrophaeus spores at a concentration of 105 cfu/mm2, at a standoff distance of 1 m, and an acquisition time of 1 s. Our system, which combines chemical specificity and sensitivity along with improved ruggedness and portability, paves the way to a new generation of instruments for real-world standoff detection of chemical and biological threats

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF 3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain

Tunable 30 fs light pulses at 1 W power level from a Yb-pumped optical parametric oscillator

We report on a Yb-pumped optical parametric oscillator (OPO) that delivers 30 fs pulses with spectral coverage from 680 to 910 nm and an average output power of up to 1.1 W. The resulting peak power is â\u88¼0.5 MW, which is, to the best of our knowledge, the highest ever demonstrated in a femtosecond OPO. The intensity noise remains at a level of 0.2% rms, and rapid wavelength tuning is obtained by simply scanning the resonator length. The performances of the OPO are promising for a variety of applications in nonlinear microscopy and ultrafast spectroscopy

Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium

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Excitation-emission Fourier-transform spectroscopy based on a birefringent interferometer

The correlation of molecular excitation and emission events provides a powerful multidimensional spectroscopy tool, by relating transitions from electronic ground and excited states through two-dimensional excitation-emission maps. Here we present a compact, fast and versatile Fourier-transform spectrometer, combining absorption and excitation-emission fluorescence spectroscopy in the visible. We generate phase-locked excitation pulse pairs via an inherently stable birefringent wedge-based common-path interferometer, retaining all the advantages of Fourier-transform spectroscopy but avoiding active stabilization or auxiliary tracking beams. We employ both coherent and incoherent excitation sources on dye molecules in solution, with data acquisition times in the range of seconds and minutes, respectively