Energy dissipation in water is very fast and more efficient than many other liquids. This behavior commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate dynamic energy flow bond network of liquid by a pump-probe experiment. We resonantly excite degrees freedom ultrashort single-cycle terahertz pulses monitor its Raman response. By using ultrathin sample cell windows, background-free bipolar signal whose tail relaxes monoexponentially...

Abstract The solvation of ions changes the physical, chemical and thermodynamic properties water, microscopic origin this behaviour is believed to be ion-induced perturbation water’s hydrogen-bonding network. Here we provide insights into process by monitoring dissipation energy in salt solutions using time-resolved terahertz–Raman spectroscopy. We resonantly drive low-frequency rotational dynamics water molecules intense terahertz pulses probe Raman response their intermolecular...

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging as a unique class of 2D electronic materials. However, intrinsically semiconducting c-MOFs with gaps in the Vis-NIR and high charge carrier mobility have been rare. Most reported metallic (i.e. gapless), which limits their use applications where larger band needed for logic devices. Herein, we design new D2h-geometric ligand, 2,3,6,7,11,12,15,16-octahydroxyphenanthro(9,10b)triphenylene (OHPTP), synthesize first...

Abstract Whereas there is increasing evidence for ion‐induced protein destabilization through direct ion–protein interactions, the strength of binding anions to proteins relative cation–protein has remained elusive. In this work, rotational mobility a model amide in aqueous solution was used as reporter interactions different with group. Protein‐stabilizing salts such KCl and KNO 3 do not affect amide. Conversely, denaturants KSCN KI markedly reduce orientational freedom Thus these results...

Abstract Despite the widespread use of aqueous electrolytes as conductors, molecular mechanism ionic conductivity at moderate to high electrolyte concentrations remains largely unresolved. Using a combination dielectric spectroscopy and dynamics simulations, we show that absorption ~0.3 THz sensitively reports on local environment ions. The magnitude these high-frequency motions scales linearly with for wide range ions concentrations. This scaling is rationalized within harmonic oscillator...

We report the electro-optic sampling (EOS) response and terahertz (THz) optical rectification (OR) of z-cut α-quartz. Due to its small effective second-order nonlinearity, large transparency window hardness, freestanding thin quartz plates can faithfully measure waveform intense THz pulses with MV/cm electric-field strength. show that both OR EOS responses are broad extension up ∼8 THz. Strikingly, latter independent crystal thickness, a plausible indication dominant surface contribution...

The air-water interface is a highly prevalent phase boundary impacting many natural and artificial processes. significance of this arises from the unique properties water molecules within interfacial region, with crucial parameter being thickness its structural anisotropy, or "healing depth". This quantity has been extensively assessed by various simulations which have converged to prediction remarkably short length ∼6 Å. Despite absence any direct experimental measurement quantity,...

Abstract We resolve the real-time coherent rotational motion of isolated water molecules encapsulated in fullerene-C 60 cages by time-domain terahertz (THz) spectroscopy. employ single-cycle THz pulses to excite low-frequency and measure subsequent emission electromagnetic waves molecules. At temperatures below ~ 100 K, C lattice vibrational damping is mitigated quantum dynamics confined are resolved with a markedly long coherence, extended beyond 10 ps. The observed transitions agree well...

Rotation of the plane polarization light in presence a magnetic field, known as Faraday rotation, is consequence electromagnetic nature and has been utilized many optical devices. Current efforts aim to realize ultrafast rotation on subpicosecond timescale. Thereby, medium should allow an process by which ultrashort intense rotates. We meet these criteria applying single cycle THz field simple molecular liquids demonstrate pulse traversing The effect attributed deflection optically induced...

The unique physical and chemical properties of interfaces are governed by a finite depth that describes the transition from topmost atomic layer to bulk material. Thus, understanding nature requires detailed insight into different structures, compositions, processes form this interfacial region. Such has traditionally been difficult obtain experiments, as it combination structural sensitivity with spatial resolution on nanometer scale. In contribution, we present vibrational spectroscopic...

The guanidinium cation interacts with amide groups, the interaction strength is – compared to other cations only intermediate.

Second-order nonlinear spectroscopy is becoming an increasingly important technique in the study of interfacial systems owing to its marked ability molecular structures and interactions. The properties such a system under investigation are contained within their intrinsic second-order susceptibilities which mapped onto measured signals (e.g. sum-frequency generation) through applied experimental settings. Despite this yielding plethora information, many crucial aspects typically remain...

Abstract Ion–protein interactions are important for protein function, yet challenging to rationalize owing the multitude of possible ion–protein interactions. To explore specific ion effects on binding sites, we investigate interaction different salts with zwitterionic peptide triglycine in solution. Dielectric spectroscopy shows that affect peptide's reorientational dynamics, a more pronounced effect denaturing cations (Li + , guanidinium (Gdm )) and anions (I − SCN ) than weakly ones (K Cl...

To understand specific ion effects on a molecular level we explore the effect of salts rotational mobility model amide using dielectric spectroscopy. Based our previous studies strong denaturing anions or cations, here study additivity anionic and cationic effect. Using consisting spherical cations find such to affect according what one expects based additive activity individual ions. The guanidinium (Gdm+) cation appears be notable exception, as results suggest that GdmI (and accordingly...

We report an approach in time-domain terahertz (THz) spectroscopy for measuring the dielectric response of liquids based on inherent properties spintronic THz emitters (STEs). The electric field radiated from STE is inversely proportional to sum complex refractive indices media surrounding thin metallic stack and stack's conductivity. demonstrate that by bringing a liquid contact with emitter, its index accordingly are imprinted into electromagnetic emitter. use water as test ascertain loss...

Abstract Trotz vermehrter Hinweise auf direkte Wechselwirkungen als Ursache für die Destabilisierung von Proteinen durch Ionen blieb Frage nach der Stärke Bindung Anionen zu im Vergleich jener Kationen offen. Die Rotation eines Modellamids wurde nun Maß Wechselwirkung verschiedener mit Amidgruppe verwendet. Untersuchungen zeigen, dass Protein‐stabilisierende Salze wie KCl und KNO 3 Rotationsmobilität des Amids nicht beeinflussen. Umgekehrt reduzieren denaturierende KSCN KI...

Abstract Terahertz time-domain and infrared Fourier-transform spectroscopy techniques are used to investigate the properties of H 2 O@C 60 endofullerene in 6 K – 300 temperature interval. A number absorption lines associated with rotational transitions water molecule entrapped inside C cages observed assigned. Fitting resonances Lorenzian lineshapes allowed us obtain dependencies parameters frequency, strength damping.

We show scalable and complete suppression of the recently reported terahertz-pulse-induced switching between different resistance states antiferromagnetic $\mathrm{Cu}\mathrm{Mn}\mathrm{As}$ thin films by ultrafast gating. The gating functionality is achieved an optically generated transiently conductive parallel channel in semiconducting substrate underneath metallic layer. photocarrier lifetime determines timescale suppression. As we do not observe a direct impact optical pulse on state...

The air-water interface is a highly prevalent phase boundary with far-reaching impact on natural and industrial processes. Water molecules behave differently at the compared to bulk, exhibiting anisotropic orientational distributions, reduced intermolecular connectivity in hydrogen bond network, significantly slower dynamics. Despite many decades of research, thickness structural anisotropy interfacial layer remains controversial, direct experimental measurement being absent. In this study,...

The burgeoning field of 2D heterostructures targets the combination materials with 3D, 1D, or 0D nanomaterials. Among most popular materials, 2H polytype molybdenum disulfide (MoS

Abstract Solvation of ions changes the physical, chemical and thermodynamic properties water. The microscopic origin this process is believed to be ion-induced perturbation in structure dynamics hydrogen (H)-bonding network Here, we provide insight on local structural deformation H-bonding water by ions, via investigating dissipation external energy salt solutions a novel time-resolved terahertz (THz)-Raman spectroscopy. We resonantly drive low-frequency rotational molecules intense THz...

Abstract Zweidimensionale konjugierte metallorganische Gerüstverbindungen (2D c‐ MOFs) gehören zu einer einzigartigen Gruppe elektronischer Materialien. 2D MOFs mit Bandlücken im sichtbaren oder nahen IR‐Bereich und hohen Ladungsträger‐mobilitäten sind jedoch rar. Die meisten literaturbekannten halbleitenden metallisch, was ihre Verwendung in logischen Bauelementen stark einschränkt. Im Folgenden konzipieren wir einen Phenanthrotriphenylen basierten, D 2h ‐symmetrischen, π‐konjugierten...